QUANTUM COHERENCE AND INTERACTIONS IN QUANTUM DOTS A DISSERTATION SUBMITTED TO THE DEPARTMENT OF APPLIED PHYSICS AND THE COMMITTEE ON GRADUATE STUDIES OF STANFORD UNIVERSITY IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY Ileana Georgeta Rau August 2011 © 2011 by Ileana Georgeta Rau. All Rights Reserved. Re-distributed by Stanford University under license with the author. This work is licensed under a Creative Commons AttributionNoncommercial 3.0 United States License. http://creativecommons.org/licenses/by-nc/3.0/us/ This dissertation is online at: http://purl.stanford.edu/tc600cr9197 ii I certify that I have read this dissertation and that, in my opinion, it is fully adequate in scope and quality as a dissertation for the degree of Doctor of Philosophy. David Goldhaber-Gordon, Primary Adviser I certify that I have read this dissertation and that, in my opinion, it is fully adequate in scope and quality as a dissertation for the degree of Doctor of Philosophy. Ian Fisher, Co-Adviser I certify that I have read this dissertation and that, in my opinion, it is fully adequate in scope and quality as a dissertation for the degree of Doctor of Philosophy. Steven Kivelson Approved for the Stanford University Committee on Graduate Studies. Patricia J. Gumport, Vice Provost Graduate Education This signature page was generated electronically upon submission of this dissertation in electronic format. An original signed hard copy of the signature page is on file in University Archives. iii iv Abstract The behavior of electrons in solid state systems is determined by the interaction of their charge and spin degrees of freedom with each other and with the degrees of freedom of their environment. Whether the interactions manifest themselves by modifying some of the systems properties such as the effective mass in the Fermi liquid picture, or more directly by suppressing transport in the Coulomb blockade model, depends on the details and complexity of the system. This thesis investigates two cases: the Fermi liquid behavior in a system with exchange interactions (the spin 1 2 Kondo model) and effect of Coulomb interactions on the phase coherence of electrons in a quantum dot with single mode leads. The first experiment tests the Fermi liquid theory prediction of a quadratic power law dependence of the electron scattering rate on energy in the non-equilibrium regime. We measure transport though a lateral GaAs/AlGaAs quantum dot that acts as an artificial magnetic impurity coupled to a single reservoir and find that the low energy conductance obeys universal scaling with temperature and bias with a quadratic exponent as expected for the single channel Kondo state. This single particle picture fails when a second independent channel is added and the quantum correlations lead to non-Fermi liquid behavior. To understand how the short range Coulomb repulsion affects phase coherence we measure the quantum correction due to the weak localization of electrons in a quantum dot coupled to a reservoir via perfectly transmitting quantum point contacts. We extract the dephasing time and observe that it continues to increase down to the lowest temperatures, in accordance with the predictions from Fermi liquid theory and in contradiction with previous experiments in zero-dimensional structures. When v the phase coherence time of the electrons becomes large enough, we observe the effects of the long range Coulomb repulsion as Coulomb blockade emerges. This was previously assumed to be characteristic of transport through quantum dots with tunneling quantum point contacts (QPCs). We show that despite the fully open QPCs of our device, the coherent backscattering of electrons at zero magnetic field is responsible for Coulomb charging effects and estimate that the residual charge quantization at the lowest temperature is 1/3 electron charge via charge sensing measurements. vi Acknowledgements I have been very lucky to have some amazing Physics teachers and professors over the years. First, I would like to thank David, my PhD adviser, from whom I have learned an incredible amount. David is an exceptional physicist and researcher, he thinks about science in a very precise and carful way that allows him to focus on what is essential about a concept, and explain it in such a way that is is clear, correct, and understandable at the same time. I believe that this is the most valuable lesson that anyone, regardless of major or occupation can teach or learn. I am very thankful for having had David as an example and a mentor. In addition, I want to thank David for his encouragement over the years and in particular, for his availability to talk to me and offer advice or suggestions when I needed them. I want to thank my undergraduate adviser, Gabe for his encouragement and support. I had never done any experiments before coming to I.W.U. and his enthusiasm for Physics and for experiments was contagious. I will always remember the time I spent there, in lab and in Physics class, with fondness. I would also like to thank my high school Physics teacher, Prof. Smaranda Zaharie, for the many, many hours spent solving Physics problems, for putting up with my requests for which Physics topics to study and for lending me her Physics books, which I still have. Without that time, I highly doubt that I would have become a physics major in the first place. For the projects in this thesis, we collaborated with several physicists. I am grateful to Yuval Oreg for his discussions with us and for his willingness to explain and to answer my questions, to Piet Brouwer for his help with the formulas for N = 1, and to Hadas Shtrikman for the heterostructure used in our devices. I would also like vii to thank my thesis/defense committee: Mac Beasley, Ian Fisher, Steve Kivelson and George Papanicolaou. There are many people I met during my time as a graduate student, whose friendship and support have been extremely important. In (mostly) chronological order, I want to thank the students in the DGG lab. Lindsay, Charis and Hung-Tao have been the best group of senior graduate students. Their knowledge about Physics, the lab and their willingness to help and discuss have made my first years in lab a pleasure. It has been a lot of fun, as well as extremely interesting, and sometimes hilarious, to work in lab and take classes with Mike J. and Joey. I have really enjoyed being able to talk about science and about experimental details with Andrei, Markus, Kathryn, Mark, Benjamin, Adam, Nimrod, Matt, Matthias, Francois, Michael as well as everyone else past and present in the DGG group. I have to thank many members of the DGG lab, as well as some members of the Moler lab, for help with Helium transfers. In particular, I would like to thank Andrei and Markus for the entertaining company during lunch time. Over the course of my PhD I have worked closely with Ron Potok, Mike Grobis and Sami Amasha. Initially, I met Ron when I was rotating in the Moler lab and I was surprised to find out that Ron was in lab at almost all hours of the day (and sometimes of the night). After I joined David’s lab and started working with him, I realized why. Ron had already done a huge amount of work to get the dilution fridge and the devices ready for the 2CK experiment. He was very knowledgeable about quantum dot physics and very driven and I learned a lot from him over the next few years: how to use a dilution refrigerator, how to measure quantum dots and how to troubleshoot noise. I also learned that the dilution fridge works better if it is called “the baby”, that chickens need to be sacrificed to the dilution fridge gods to keep the system up and running, and that the most frustrating experiment can be fun when you have the right lab-partner. Mike came to the DGG lab with a rather different background than mine. His expertise with vacuum equipment and instrument troubleshooting was extensive and I gained very useful experience by working with him. He is very good at trying things out, and finding a way to fix or troubleshoot something even when there is very little viii information available. Because of his different background, Mike had an alternative way to think about concepts, which was very interesting and I learned a lot from talking about physics with him. I have been extremely lucky that Sami joined the group and decided to work on the dilution fridge project. He is an exceptional physicist and a very considerate and conscientious lab partner. He is very knowledgable about quantum dots and mesoscopic physics, but also about physics in general. I always learn something new or find a better way of understanding a topic when I talk to him about science. He thinks about things very carefully and in detail, and is not afraid to question assumptions or to try to find a different way to approach a problem. I have learned a lot from him about how to decide what the possible ways to proceed with a task are and how to identify the best option among them. I want to thank him for sharing his knowledge and expertise with me, for entertaining random discussions about science and for his help with everything from Igor commands to understanding a specific topic. Finally and most importantly, Sami, thank you for your friendship and your advice. I would like to thank Andrei, Julie and Lisa for the fun times dancing, for the occasional Saddlerack outing and for the interesting discussions inside and outside the lab. I am very happy that I came to Stanford and met Naoko, Annica, Eugene, Jess, Tony, Rich, Alex B., Katalin, Beena and Katie. Their friendship and company have made graduate school much more fun. I would like to thank Hendrik for driving me to lab and picking me up at the oddest hours of the night, for helping me transfer Helium when no one else was around, for his support in my decision to come to Stanford and for his decision to join me here. Seeing California with him was an adventure. I especially want to thank Kiran for four memorable years as roommates, for her friendship all through graduate school, for listening to me and encouraging me when things were not working out and for being happy with me when things were going well. I have also been fortunate to have Alison and Michelle as my friends for over a decade. They are two of the smartest people I know and their advice and opinions have been very helpful over these years. I have a special thank you for Lindsay, Ophir and Chewy who have been my friends, welcomed me into their home and introduced ix me to a different world when I needed it most. I am particularly grateful to Wong for sharing some of his calm and patience with me and for giving me a more positive perspective on research and academia. And finally, I would like to thank my family and friends at home: Vasilica Tolciu, Reli Florescu and Corina Chipei, who have been my teachers and my friends, my cousin Radu and my aunts Mariana and Marie. Having them share their life experience and advice with me provided me with wisdom and perspective that I would not have had otherwise. My grandma is the most amazing woman I know and I am deeply grateful for her presence in my life. Thank you to my parents who not only supported and encouraged me all these years, but are also responsible for my interest in Physics: my dad, from whom I learned that being careful is one of the most important qualities of an experimentalist (when I got (slightly) shocked while investigating the electrical installation of the house), and my mom, who was the first to explain to me what electrons and holes are, where electrical and mechanical properties of different materials come from, or how Foucault’s pendulum can show that the earth is rotating around its own axis. x Contents Abstract v Acknowledgements vii 1 Introduction 1 1.1 The Transition from Quantum to Classical Behavior . . . . . . . . . . 1 1.2 Decoherence . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3 1.3 Interactions with the Environment 5 . . . . . . . . . . . . . . . . . . . 1.4 The Kondo Effect: an Example of a Correlated Quantum State . . . 9 1.5 Outline . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15 2 Quantum Dots as a Model System 16 2.1 The Two Dimensional Electron Gas (2DEG) . . . . . . . . . . . . . . 17 2.2 The Quantum Dot . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19 2.3 From a Closed to an Open Quantum Dot . . . . . . . . . . . . . . . . 25 3 Quantum dots: Coulomb Blockade 29 3.1 The Charging Energy . . . . . . . . . . . . . . . . . . . . . . . . . . . 29 3.2 Coulomb Blockade Diamonds . . . . . . . . . . . . . . . . . . . . . . 34 4 Quantum Dots: the Kondo Effect 39 4.1 The Single Channel Kondo Effect in a Quantum Dot . . . . . . . . . 41 4.2 The Non-equilibrium Single Channel Kondo Effect . . . . . . . . . . . 47 4.3 Impurity Quantum Phase Transitions . . . . . . . . . . . . . . . . . . 56 xi 4.4 Tuning to the 2CK Point in a Double Quantum Dot . . . . . . . . . . 5 Quantum Dots: Perfectly Transmitting QPCs 62 67 5.1 Open Quantum Dots . . . . . . . . . . . . . . . . . . . . . . . . . . . 69 5.2 The Quantum Dot Conductance at N = 1 . . . . . . . . . . . . . . . 73 5.3 The Dephasing Time in a Quantum Dot at N = 1 . . . . . . . . . . . 86 5.4 Mesoscopic Coulomb Blockade in a Quantum Dot at N = 1 . . . . . . 91 Bibliography 98 xii List of Tables 2.1 Characteristic parameters of the 2DEG . . . . . . . . . . . . . . . . . 19 2.2 Characteristic parameters of the quantum dots . . . . . . . . . . . . . 24 xiii List of Figures 1.1 The Anderson model . . . . . . . . . . . . . . . . . . . . . . . . . . . 11 1.2 The Kondo effect in bulk . . . . . . . . . . . . . . . . . . . . . . . . . 14 2.1 The band structure of AlGaAs and GaAs . . . . . . . . . . . . . . . . 18 2.2 Band bending in AlGaAs/GaAs . . . . . . . . . . . . . . . . . . . . . 20 2.3 SEM picture of the quantum dots . . . . . . . . . . . . . . . . . . . . 24 2.4 QPC energy levels . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26 2.5 QPC conductance quantization . . . . . . . . . . . . . . . . . . . . . 27 3.1 Quantum dot electrical circuit . . . . . . . . . . . . . . . . . . . . . . 30 3.2 Total energy and charge of the quantum dot . . . . . . . . . . . . . . 31 3.3 Transport through the quantum dot . . . . . . . . . . . . . . . . . . . 32 3.4 Measurements of Coulomb blockade peaks . . . . . . . . . . . . . . . 33 3.5 Coulomb blockade diamond diagram . . . . . . . . . . . . . . . . . . 34 3.6 Measurements of Coulomb blockade diamonds . . . . . . . . . . . . . 35 3.7 Coulomb blockade thermometry . . . . . . . . . . . . . . . . . . . . . 37 4.1 Kondo conductance in a quantum dot . . . . . . . . . . . . . . . . . . 43 4.2 Bias and temperature dependence of the Kondo conductance . . . . . 45 4.3 Temperature evolution of the Kondo bias peak and valley conductance 48 4.4 G0 and TK across the Kondo valley . . . . . . . . . . . . . . . . . . . 49 4.5 Temperature and bias scaling on the Kondo plateau . . . . . . . . . . 51 4.6 Bias exponent and coefficients on the Kondo plateau . . . . . . . . . 52 4.7 Single channel Kondo conductance scaling . . . . . . . . . . . . . . . 55 xiv 4.8 The two channel Kondo phase diagram . . . . . . . . . . . . . . . . . 59 4.9 The two channel Kondo double quantum dot system . . . . . . . . . 63 4.10 The Kondo conductance through a three-leaded dot . . . . . . . . . . 64 4.11 Finite bias measurements of the two single channel Kondo states . . . 65 5.1 The QPC conductance plateaus . . . . . . . . . . . . . . . . . . . . . 74 5.2 The center of the N = 1 plateau . . . . . . . . . . . . . . . . . . . . . 74 5.3 Universal conductance fluctuations at N = 1 . . . . . . . . . . . . . . 76 5.4 Coulomb blockade oscillations at N = 1 . . . . . . . . . . . . . . . . . 77 5.5 The evolution of the Coulomb diamonds from N ≪ 1 to N > 1 . . . . 78 5.6 The charging energy at N = 1 . . . . . . . . . . . . . . . . . . . . . . 79 5.7 Changing the shape of the quantum dot . . . . . . . . . . . . . . . . 80 5.8 The conductance average vs. magnetic field and temperature . . . . . 83 5.9 The conductance variance vs. magnetic field and temperature . . . . 85 5.10 The temperature dependence of the dephasing time . . . . . . . . . . 87 5.11 Characteristic time and energy scales for the quantum dot and the 2DEG 90 5.12 Coulomb blockade oscillations vs gate voltage and magnetic field . . 92 . . . . . . . . . . 93 5.14 Temperature dependence of the MCB oscillations . . . . . . . . . . . 94 5.15 The charge sensing procedure . . . . . . . . . . . . . . . . . . . . . . 95 5.16 The charge sensing signal at N ≪ 1 and N = 1 . . . . . . . . . . . . 96 5.13 Magnetic field dependence of the MCB oscillations xv xvi Chapter 1 Introduction 1.1 The Transition from Quantum to Classical Behavior For the past 100 years physicists have used quantum mechanics to explain and predict a variety of phenomena. Despite its widespread use and proven predictive capabilities, the question of how to really understand quantum mechanics is still unanswered. Several interpretations have been suggested over time. Among them are the Copenhagen interpretation of quantum mechanics proposed by Niels Bohr, von Neumann’s idea of a collapse of the wavefunction, hidden variable approaches and some more exotic suggestions such as Everett’s many world interpretation. The problem with interpreting the laws and concepts of quantum mechanics is that our perception of the world around us, filled with definite (“classical”) outcomes, is distinctly different from the probabilistic character of the quantum world. In quantum mechanics any linear superposition of states corresponds to a possible state. In contrast, most things we interact with day to day are in a definite state. Here is a simple example to illustrate this: A classical system can move from one position to another, but at any given time its position is well defined. However, a quantum system, described by a superposition of all possible positions, has a position that is not well-defined. There is an obvious 1 2 CHAPTER 1. INTRODUCTION problem in applying quantum mechanics to classical objects: a train cannot be both here and there or a (somewhat famous) cat cannot be described as a superposition of being dead and being alive. The “measurement problem” is the general name given to the following conundrum: if quantum mechanics is the right theory to describe everything, then why do we not always observe these superpositions? How do you convert a quantum state into something with a definite outcome? The reason for the name “measurement problem” is that this question becomes particularly puzzling when one considers measuring a quantum system. The result of the measurement is a classical definite result. So one can either postulate that the measurement apparatus is now entangled with the quantum system (von Neuman interpretation), and as such, is in a superposition of states, just like the quantum system, or that it is separate from the quantum system and should be treated classically (Copenhagen interpretation). An artificial and ultimately unsatisfying distinction that would circumvent this problem is to postulate that quantum mechanics only describes the quantum world which is separate from our “everyday world”. The difficulty then shifts to deciding what belongs in the quantum world and what belongs in the classical world. Initially, quantum mechanics was applied to microscopic objects: photons, electrons, etc., which prompted an identification of the microscopic with the quantum. Since most macroscopic objects obeyed classical mechanics and had robust, non-probabilistic properties such as position and momentum, the macroscopic was equated to the classical world. The theoretical prediction and experimental observation of quantum states in macroscopic systems such as superconducting states that involve macroscopic numbers of electrons and extend over macroscopic distances, or macroscopic cantilevers that behave as quantum harmonic oscillators makes this distinction inadequate. Thus it is clear that the border between quantum and classical does not correspond to the border between the macroscopic and the microscopic. A different way to categorize what belongs to the quantum and what belongs to the classical world is based on the difference in coupling to the environment [1]. When a system is isolated from the environment all possible superpositions of its states are allowed. However, this situation is not realistic: most systems are coupled to their 1.2. DECOHERENCE 3 environment and can interact with it. It turns out that with the right interaction, a quantum system can be made to look classical. This is called decoherence (for a recent review of research on the theory of decoherence and its applications see [2]). The question of whether decoherence can solve the measurement problem, offer a mechanism for what looks like a collapse of the wavefunction and explain the quantum to classical transition, is and has been debated since its introduction [1, 3]. While the meaning of decoherence and its implications for understanding quantum mechanics have not been fully explored, from the experimental point of view decoherence is a measurable quantum phenomenon that offers a way to explore the fascinating consequences of quantum nature. 1.2 Decoherence The easiest way to think of quantum coherence is in terms of an interference experiment. Classical particles incident on a double slit have a probability Pi to pass through slit i, where i = 1, 2. The total probability that it hits the screen at a position A can be expressed as the sum over the individual probabilities: PT (A) = P1 (A) + P2 (A). A quantum system is described by a wavefunction and as such it will pass through both slits. Consequently, the probability to hit the screen is given by the square over the sum of the probability amplitudes a1,2 = |a1,2 |ei(ωt−kx) corresponding to the path though each slit: PT (A) = |a1 (A) + a2 (A)|2 = P1 (A) + P2 (A) + 2|a1 ||a2 | cos θ. θ depends on the position of point A with respect to the slits and on the wavevector k, and P1,2 = |a1,2 |2 is the classical probability to have taken the path through slit 1 or 2. The probability for the quantum system contains an extra term that describes the phase relationship between the paths taken through the two slits compared to the classical system. This term encompasses the quantum correlations and will be referred to as the quantum interference term. In general, quantum systems are described by a coherent superposition of states whose phase relationships lead to quantum correlations and to the presence of this extra quantum interference term. When one tries to detect which state the quantum system is in, the quantum correlations are disturbed and the interference term 4 CHAPTER 1. INTRODUCTION disappears. Alternatively, this interference term can also be suppressed by certain interactions of the quantum system with its environment. This process is called decoherence. When the quantum system and the environment become entangled due to their interaction, the phase relationship between the states involved in the coherent superposition is defined for the whole combined system, and not for the individual subsystem. As a result measurements of the combined system will show the extra term due to quantum coherence, while those involving the subsystem will not. From the point of view of the mathematical description of such a system, the reduced density matrix that describes the probabilities for each of the possible states of the quantum system will have rapidly decaying off diagonal matrix elements (in some basis) [4]. A more intuitive way to think about the effect of the quantum correlations between the system and its environment is to say that because of the interaction, the environment “measures” the state of the system. In analogy to the double slit experiment described above, this selects one specific state and suppresses the interference term. Sometimes decoherence is also called dephasing or decorrelation and the distinction between these terms is not exactly agreed on in the literature. For the purposes of this thesis, dephasing and decoherence will be used interchangeably. Decoherence can be quantified in terms of a reduction of the interference term with respect to the classical term, but it does not simply refer to any reduction of the interference pattern visibility. For example, covering one of the slits in the interference example will cause the interference pattern to disappear, but this is not due to decoherence. Similarly, averaging over different “noisy” realizations of the system (e.g. thermal distribution of energies) can suppress the interference pattern but is not decoherence. Decoherence can be present in a system with or without dissipation: due to their interaction, the environment obtains “which path” information about the quantum system. This can happen without necessarily exchanging energy, but in order for decoherence to take place, an inelastic process involving some degree of freedom of the quantum system and the environment (e.g. a spin-flip) has to take place [5]. This will be discussed in more detain in the next section. 1.3. INTERACTIONS WITH THE ENVIRONMENT 1.3 5 Interactions with the Environment To study the effect of decoherence on electron transport in a solid, one has to be able to calculate or measure the visibility of the quantum interference term. The condition required to observe an interference pattern is that phase coherence be maintained over time and distances comparable to characteristic transport scales such as system size, Fermi wavelength and elastic mean free path. This condition is fulfilled in mesoscopic devices with one or more confined dimensions such as two dimensional electrons gases, quantum wires, or quantum dots, which show quantum interference effects such as Aharonov Bohm oscillations [6], universal conductance fluctuations [7], and weak localization effects [8]. The simplest picture of electron transport in a metal neglects interactions with the environment. In the Drude model, electrons are treated as free (they do not interact with ions or impurities other than by elastic collsions) and independent (between collisions electrons do not feel the electrostatic interaction with other electrons). The Sommerfeld model takes one step further and accounts for the Pauli exclusion principle by using the Fermi-Dirac distribution for the electron velocity. A picture that takes both the quantum decription into account as well as the electrostatic interaction with the underlying atomic lattice is the description of electrons in terms of Bloch waves: these are stationary solutions to Schroedinger’s equation with a periodic potential. The semiclassical model combines the Sommerfeld model with the description in terms of Bloch waves by constructing a wavepacket of Bloch levels with a spatial extent that is smaller than the length over which externally applied fields vary. For a detailed treatment see ref. [9]. All of these models assume non-interacting electrons. Since electrons interact via Coulomb repulsion, this assumption is not valid. Landau showed that a system of interacting electrons can be approximated by a system of nearly independent quasiparticles with the same charge and momentum as the electron, obeying the exclusion principles, but with modified parameters such as effective mass and magnetic moment. This is the Fermi liquid picture and it makes it possible to use the results of the above mentioned models, as long as the electrons are replaced with the Landau 6 CHAPTER 1. INTRODUCTION quasiparticles. These quasiparticles are sometimes referred to as “dressed” electrons because they can be thought of as electrons screened by the interactions. In general, this thesis uses the word electron to refer to these screened electrons. Despite its limitations, the Drude-Sommerfeld model can be used to derive key features of electron transport in metals. The effects of elastic scattering are accounted for by the introduction of a collision or relaxation time. This is a measure of the disorder of the system and affects the conduction. Electrons move at the Fermi velocity vF but in thermal equilibrium their direction of motion is random so there is no average net current or velocity. Under the influence of an electric field, electrons acquire a net drift velocity vD , which depends on the electric field, but also on how disorder affects the momentum of the electrons. Elastic collisions do not change the momentum of the electron, but they can randomize its direction. The average time it takes for the electron to undergo enough collisions to randomize its direction of motion is referred to as the momentum relaxation time or elastic time τe . The distance it can travel in this time is the mean free path le . This length scale can refer to the average distance between impurities if they are hard scatterers, or can stretch over several collisions events in the case of small angle scattering. Assuming that an electron with mass m moving in an electric field E obeys Newton’s laws between collisions: m ~ dv ~ = eE, dt (1.1) ~ e /m. The proportionality factor their average drift velocity is given by v~D = −eEτ between the drift velocity and the electric field is called the mobility µ = eτe /m. From the net current density ~j = nev~D and for electric transport in the Ohmic ~ we can express the conductivity of the system in terms of the the regime (~j = σ E) density n and the mobility µ of the material alone: ne2 τe σ= = neµ. m (1.2) In this model elastic scattering determines the conductivity of a system. Elastic 1.3. INTERACTIONS WITH THE ENVIRONMENT 7 scattering events, for example collisions with static defects of the lattice, such as crystal dislocations or charged impurities, as well as other electrons lead to a finite conductivity. Inelastic scattering events are responsible for decoherence. Inelastic scattering events that lead to decoherence are collisions with scatterers with an internal degree of freedom such as phonons, magnetic impurities and other electrons. The efficiency of inelastic scattering in destroying phase coherence is enhanced by elastic scattering. The latter cannot destroy the phase coherence but it can modify the quantum interference term. Similar to the elastic time, the inelastic or decoherence time τφ is the time it takes an electron to lose its phase information to the environment (to change its quantum state). Calculating the relation of the decoherence time and the conductivity of the system depends on the dimensionality and the relative length scales of the system [10]. If the size of the size L of the system is smaller than the mean free path, transport through the system is independent of the impurities and the Drude conductivity becomes irrelevant. The conductance is determined only by the transmission probability T through the system and is described by the Landauer formula G = (e2 /h)T . This is the regime of ballistic transport. In order to understand which processes dominate, and what the resulting effects are, we have to compare several energy scales. Some of these requirements can be relaxed at finite temperature, where the timescale to compare to is the smaller of the thermal length or system size, but in general the following conditions are valid: 1. λF < le : the Fermi wavelength has to be smaller than the mean free path for the system to be a good conductor. 2. τcross > τe : the time it takes the electrons to cross the system has to be larger than the elastic mean free time for transport to be diffusive. In this case τcross = L2 /D where D = vF2 τe /2 is the diffusion constant. 3. τcross < τe : the time it takes the electrons to cross the system has to be smaller than the elastic mean free time for transport to be ballistic. In this case τcross = L/vF . 8 CHAPTER 1. INTRODUCTION 4. τφ ≪ τcross , τe : if the decoherence time is smaller than all the timescales in the system, the conductance is determined by whether transport is ballistic or diffusive. 5. τφ ≥ τcross , τe : if the decoherence time is comparable to some or all of the transport times in the system, the conductance will be modified by the extra presence of the quantum interference terms. There are other time scales that are relevant such as the Ehrenfest time or the ergodic time that will be discussed in chapter 5. Depending on the elastic and inelastic scattering events that are present, the dependence of the decoherence time on energy, temperature and bias can look very different. Calculations of electron-electron dephasing in clean (ballistic) systems show that as the energy ∆ of the electron-quasiparticle with respect to the Fermi level increases, the phase space available for scattering processes increases, and the dephasing time decreases. At finite temperatures, electrons with energy kB T with respect to the Fermi energy are involved in transport and can decohere. Depending on the dimensionality of the system, the dephasing time as a function of temperature has the following dependence [11, 12] 1 τφe−e ∝ T2 for 3D 2 T ln(T ) for 2D T (1.3) for 1D The total momentum of the electron system is conserved in these scattering processes, and as such, they do not directly affect the net current. However, they affect the quantum interference corrections to the conductance. As a result the decoherence time will be important in any system where interference is possible. The theory of electron-electron dephasing in disordered conductors was developed by Altshuler, Aronov, and Khmelnitsky who showed that the Fermi liquid description is applicable in low dimensions and in the presence of disorder [13, 14]. Because the the inelastic scattering in 3D and in the presence of disorder is dominated by large energy transfer processes, the decoherence time has the same power 1.4. THE KONDO EFFECT: AN EXAMPLE OF A CORRELATED QUANTUM STATE9 law dependence on temperature as in the ballistic case [14]. In lower dimensions, processes with small energy transfers become important and the dephasing time has the following dependence on energy/temperature: 1 τφe−e 2 for 3D T ∝ T for 2D T 2/3 for 1D (1.4) The definition of the decoherence time and the precise relationship to the microscopic parameters of the system and to the interaction is a delicate subject. Depending on the case, one can think of the dephasing time as equal or proportional to the quasi-lifetime of the single particle state, but this is not a priori obvious [15]. As any well-behaved quantum system, an electron moving through any material will take all possible paths from point A to point B. The phase relationship between the possible paths will determine the interference term that is the quantum correction to the classical Drude conductivity. The presence of disorder (elastic impurities), leads to the localization of the electrons at certain impurities due to the constructive interference of some closed trajectories. The resulting reduction of the conductance of the system is called weak localization and can be used to study the coherence time in disordered systems. In ballistic systems, the quantum interference manifests itself as fluctuations of the conductance from the value predicted by Landauer formula. How the size of these fluctuations can be used to extract the dephsaing time will be explained in more detail in chapter 5. 1.4 The Kondo Effect: an Example of a Correlated Quantum State A system in which coherent quantum properties lead to a dramatic departure from classical behavior is that of a metal containing very few magnetic impurities. At relatively high temperatures, the resistivity of a metal is dominated by electronphonon scattering. As the temperature is lowered the scattering rate decreases. At 10 CHAPTER 1. INTRODUCTION low enough temperatures, electron-phonon scattering becomes insignificant and the resistivity saturates at a finite value determined by scattering from defects in the crystal lattice. In the 1930s measurements of Au cooled below 10 K sometimes showed a resistivity rise rather than the predicted saturation as the temperature was lowered further [16]. This effect remained unexplained until the 1960s when further experiments established a correlation between the low-temperature resistivity rise with the presence of dilute magnetic impurities in the metal [17]. The presence of the magnetic impurities dramatically affects the transport properties of the metal at low temperatures where quantum coherence is maintained. The Kondo Hamiltonian The strong experimental evidence that magnetic impurities give rise to an enhanced resistivity led J. Kondo to calculate the effect that magnetic impurities which can scatter electrons have on the resistivity of a metal. The s-d Hamiltonian described the exchange interaction between an impurity spin and conduction electrons: Hs−d = X † ǫks ψks ψks + J X i k ~i , ~σi · S (1.5) ~i is the ith impurity spin, ~σi is the spin of the conduction electrons at the where S location of the ith impurity, and ψ and ψ † represent the annihilation and creation operators for the conduction electrons with given momentum k and spin s. Kondo used perturbation theory on the s-d model and showed that an antiferromagnetic interaction J leads to a logarithmic rise in electron-impurity scattering with decreasing temperature. This explained the observed rise of the resistivity at low temperatures. The Anderson Hamiltonian was originally proposed to describe a magnetic impurity atom in a metal [18]: HA = X k † ǫks ψks ψks + Un↓ n↑ + X ǫds d†s ds + V ψs† (0)ds + h.c. . (1.6) s The first term represents the the kinetic energy of the electrons in the reservoir. U 1.4. THE KONDO EFFECT: AN EXAMPLE OF A CORRELATED QUANTUM STATE11 E double occupancy V EF U d single occupancy electron reservoir magnetic impurity Figure 1.1: Schematic representation of the Anderson model indicating the parameters of the Hamiltonian (eq. 1.6). is the charging energy and accounts for the repulsive Coulomb interactions on the impurity site. The third term is the quantized energy of the localized electrons in a single spin-degenerate state where the d’s are the creation and annihilation operators of the impurity with ns = d†s ds . V is the hybridization between the conduction electrons and the impurity electrons and describes co-tunneling on and off the local site. These parameters are shown schematically in fig. 1.1. The coupling between the electrons localized at the impurity (with a discrete spectrum) and the conduction electrons (with a continuous spectrum) leads to a finite lifetime of the electrons at the impurity. The interaction parameter U ensures the doubly-degenerate site can be occupied by just a single electron. If the Coulomb repulsion is weak, two electrons will occupy the site which means that in the simplest case the groundstate has total spin 0. If it is strong, only one electron can occupy the impurity level so total impurity spin is 21 . In this case, the site acts as a magnetic impurity, and should exhibit the Kondo effect. Schrieffer and Wolff [19] showed that indeed the s-d model is equivalent to the Anderson model in the limit to which local charge fluctuations can be neglected (strong electron repulsion). The ground state of the Kondo Hamiltonian is a spin singlet in which the spin of a 12 CHAPTER 1. INTRODUCTION localized electron is matched with the spin of delocalized electrons to yield a net spin of zero. The characteristic energy of this state, referred to as the Kondo temperature is not simply proportional to the antiferromagnetic coupling strength J: TK = De1/(Jν) (1.7) where D is the conduction electron bandwidth and ν the thermodynamic density of states of the conduction electrons. When T > TK , Kondo’s results, which were based on perturbation theory, start to break down. Below the Kondo temperature the repeated impurity spin-flips and the corresponding response of the Fermi sea lead to complex many-body dynamics which produces a logarithmic divergence. In 1975 K. Wilson developed a new renormalization group (RG) technique that was able to solve this problem [20]. The RG calculations showed that at temperatures below a characteristic Kondo temperature TK , a magnetic impurity forms a singlet with the surrounding conduction electrons. Despite this success in determining the ground state and the thermodynamic properties of a magnetic impurity in a metal, accurate calculation of transport properties over a broad range of temperatures required the development of numerical RG techniques [21]. A more detailed theoretical description of the Kondo effect is given in ref. [22]. Unlike in the single channel Kondo case where at energies well below TK the conduction electrons around the spin 1 2 impurity behave as a Fermi liquid, a new non-Fermi liquid state was predicted to occur in a system that is Kondo coupled to multiple screening channels [23]: HM CK = X k † ǫksα ψksα ψksα + J X α ~ ~σα · S. (1.8) This multichannel Kondo state along with Fermi liquids, Luttinger liquids, fractional quantum Hall systems, and disordered systems with Coulomb interactions are the only known classes of metals. 1.4. THE KONDO EFFECT: AN EXAMPLE OF A CORRELATED QUANTUM STATE13 The properties of the multichannel Kondo system at low temperatures can be calculated using boundary conformal field theory [24, 25] or renormalization group theory (NRG). The two-channel Kondo model has been used to explain the experimentally observed specific heat anomalies in certain heavy fermion materials [26, 27, 28] as well as transport signatures in metallic nano-constrictions [29, 30]. Because the Kondo effect is a property of magnetic impurities in a host metal, it should be observable experimentally in a variety of systems. Besides the original measurements on Au, the Kondo effect appears in transport through tunnel junctions containing impurities [31, 32], single molecules or carbon nanotubes coupled to electron reservoirs [33, 34], and in scanning tunneling microscope measurements of surface adatoms [35, 36], and metal complexes [37]. In addition, the Kondo effect has been observed in a variety of quantum dot systems that will be discussed in chapter 4. Decoherence of Kondo State The bound state between the impurity spin and the conduction electron spins can be visualized as a ”screening cloud”, shown schematically in fig. 1.2. In a metal, electrons close to the Fermi level are able to scatter because the occupied and unoccupied states coexist in an energy range kB T around the Fermi level. Thus, the Kondo interaction predominantly affects the electrons at the Fermi surface and the Kondo singlet appears in spectroscopic measurements as a narrow resonance located at the Fermi energy. For electrons with Fermi velocity vF , the characteristic size of the Kondo cloud and thus the spatial extent of the quantum correlations, is given by [38]: χK ≈ ~vF . kB TK (1.9) For typical semiconductor quantum dots in the Kondo regime the size of the Kondo cloud is ≈ 1µm. However, the slow exponential decay of the spin polarization in the electron gas is modulated at distances greater than λF from the local moment by oscillations and polynomial decay [39], and charge rearrangement due to the singlet formation occurs at length scales on the order of λF . As a result, the spatial properties of the Kondo state have been hard to measure. 14 CHAPTER 1. INTRODUCTION Figure 1.2: The spins of conduction electrons screen the localized impurity spin (blue) leading to a larger crossection for scattering than in the absence of the magnetic impurity. Perturbations such as temperature or bias affect the formation of the singlet state: weak perturbations (E < kB TK ) can partially suppress the Kondo effect, while stronger perturbations (E > kB TK ) eventually destroy the Kondo singlet. This can happen because the Kondo singlet decoheres due to thermal fluctuations or because a new state, either a non-Kondo state (in case of an applied magnetic field) or another Kondo state (in case of an asymmetry in coupling to different reservoirs) becomes the ground state of the system. Various processes can lead to decoherence of the Kondo singlet. The Kondo singlet state is a coherent superposition of spin-flip tunneling processes between conduction electrons and the local state, which can be destroyed by non-Kondo processes such as emission or absorption of a phonon or photon. At zero temperature and bias, no phase space is available and delocalized electrons within χk of the impurity can form the Kondo singlet. With increasing temperature, the broadening of the Fermi distribution of the leads increases the available phase space for non-Kondo processes. This disturbs the Kondo correlations. Similarly, finite bias also increases the phase space and leads to a suppression of the Kondo effect. When the energy scale of the 1.5. OUTLINE 15 perturbation exceeds the binding energy of the singlet state, the Kondo singlet will decohere completely. 1.5 Outline Chapter 2 describes the two-dimensional electron gas, the quantum point contact and the quantum dot from the point of view of electronic transport through low dimensional systems and introduces the quantum dots used for the experiments in this thesis. Chapter 3 explains the basic features of transport in the Coulomb blockade regime that are used to characterize the energy scales of the measured quantum dots. Chapter 4 describes the conductance though a quantum dot in the Kondo regime, presents measurements of non-equilibrium Fermi liquid behavior, and discusses how to tune a double quantum dot through a quantum phase transition. Chapter 5 explains transport though a quantum dot with perfectly transmitting quantum point contacts. Measurements of the decoherence caused by electron-electron interactions are shown and the reappearance of Coulomb blockade features, despite the fact that the quantum point contacts are not in the tunneling regime, is investigated. Chapter 2 Quantum Dots as a Model System As illustrated in the case of the Kondo effect, electrons can exhibit complex behavior depending on the interactions between various subsystems of a material (electrons, phonons, ions, etc.). Studying the mechanism that underlies some of these more exotic groundstates in bulk materials such as high temperature superconductors or heavy fermion systems is complicated. The reason is that the microscopic properties of bulk materials are changed by altering a material’s structure or chemical composition, or by changing an external parameter such as the applied pressure or magnetic field. This does not just tune a single microscopic parameter of the material, but also affects the other parameters or even the effective Hamiltonian of the system. As a result, quantum phase transitions that are predicted to occur as a function of some interaction parameter in these systems are difficult to study because the different phases of the transition often belong to two different, although related, materials. Advancements in lithography technology lead to the fabrication and measurement of the first artificial atoms in patterned GaAs heterostructures [40, 41] in the late 1980s. Over the past 25 years, further developments in nano-fabrication, low temperature cooling techniques, as well as the development of new computational tools, have made it possible to design increasingly complex artificial nanostructures. A single quantum dot acts as an artificial atom and can be used to model a localized magnetic moment [42, 43, 44]. Multi-dot systems coupled to distinct electron reservoirs can be designed to imitate conventional materials. 16 2.1. THE TWO DIMENSIONAL ELECTRON GAS (2DEG) 17 The advantage offered by these artificial structures over bulk materials is the fact that their individual properties such as energy spectrum, magnetic moment, coupling to the environment, and the spatial distribution of the wavefunction are independently tunable using gate voltages, magnetic field, or voltage bias. This makes it possible to study the interplay between single spins and conduction electrons, the transport of heat through low dimensional structures, charge/spin transport through atoms and molecules [45, 46, 47, 48], and the transport properties of impurity quantum phase transitions. The disadvantage is that it is difficult to measure thermodynamic quantities such as specific heat or magnetic susceptibility. As such, the insight gained by studying artificial structures is complementary to the conclusions reached by studying bulk materials. This chapter will describe the GaAs heterostructures and the associated two dimensional electrons gas (2DEG), explain how it can be used to form a lateral gated quantum dot, and explain how the quantum dot is tuned from a closed to an open quantum system via the quantum point contacts that connect it to the 2DEG. 2.1 The Two Dimensional Electron Gas (2DEG) The experiments presented in this thesis use a modulation doped GaAs/Alx Ga1−x As heterostructure. This consists of AlGaAs on top of a GaAs substrate, with a thin layer of GaAs deposited on the surface of AlGaAs. Because GaAs and AlGaAs have almost the same lattice constant, the scattering at the interface where the 2DEG resides is low and the 2DEG mobility is much higher than in other systems. The band structures for the two materials are shown in fig. 2.1. The AlGaAs is doped with Silicon atoms which act as n-type donors. Due to the fact that the donors raise the Fermi level in AlGaAs above the conduction band of GaAs, electrons will move from AlGaAs into GaAs and leave positively charged Si ions behind. The Fermi levels of the two materials have to align at the interface and thus, depending on the Si doping, a triangular potential well forms exactly between AlGaAs and GaAs. This bending of the conduction and valence bands is illustrated, not to scale, in fig. 2.2. At low temperatures, the electrons do not have enough energy 18 CHAPTER 2. QUANTUM DOTS AS A MODEL SYSTEM GaAs Al0.3Ga0.7As vacuum level 3.74 eV 4.07 eV EC donor level 1.42 eV 1.8 eV acceptor level EV Figure 2.1: Side by side comparison of the separate band diagrams for AlGaAs and GaAs. to exit the well and are trapped inside. The eigenenergies of the discrete states allowed in a potential well with V (z) = ( e 2 ne z 2ǫ0 ǫr for z > 0 ∞ for z = 0 (2.1) are given by: Ezj = 9π 2 32m ~e2 ne ǫ0 ǫr 2 ! 13 3 2 (j + ) 3 , 4 j = 0, 1, 2... (2.2) where ǫr is the dielectric constant and ne is the electron density in the material. The density of states (including spin degeneracy) in 2D is a constant for energies lying between two subbands, with discontinuous jumps at the energy of each subband. The temperatures used for the experiments described in this thesis are low enough that only the first subband is occupied. By measuring the electron density (via the Hall effect) and using the density of states to relate the Fermi wavelength to the p density λF = 2π/ne we can determine the Fermi energy of the 2DEG electrons. For reference, the density of states g(E), for a system effective mass m∗ , with a band minimum Epot for the 3D case and quantized energies Ei for the lower dimensions 2.2. THE QUANTUM DOT 19 electron mass m∗e density ne mobility µe 0.067 me 2e11 cm−2 2e6 cm2 /Vs Fermi wavelength λF Fermi velocity vF Fermi energy EF elastic time τe elastic m.f.p. le q 2π ne h m∗ λF h2 2m∗ λ2F m∗ µe e 56 nm 190000 m/s 7.5 meV vF τe 70 ps 15 µm Table 2.1: Characteristic parameters of the 2DEG (square well confinement) is: g(E) = 1 2π 2 2m∗ 2 ~2 m∗ p E − Epot Σ Θ(E − Ei ) π~2 i q m∗ 1 Σ 2(E−E π~ i i) for 3D for 2D (2.3) for 1D. Because the ionized donors are spatially separated from the 2DEG, the electrons can be approximated as free electrons with a modified effective mass of 0.067me . This system has a number of desirable properties such as a low density, a large Fermi wavelength, high mobility, and a large mean free path. As a consequence, transport on length scales comparable to the Fermi wavelength, the mean free path or the coherence length can be investigated in this or in lower dimensional sub-systems such as quantum point contacts or quantum dots. The 2DEG used for the quantum dots measured in this thesis has been described in [45] and its parameters are summarized in table 2.1. 2.2 The Quantum Dot Quantum dots are isolated regions of a material where electrons are confined. The quantum dot can be viewed as a particle in a box: spatial confinement leads to energy quantization. Although the energy scales are very different, a quantum dot can be 20 CHAPTER 2. QUANTUM DOTS AS A MODEL SYSTEM + + + + EC 0.2 eV EF EV Si doped AlGaAs undoped AlGaAs GaAs substrate Figure 2.2: The triangular potential well at the interface between AlGaAs and GaAs forms because the positively charged Si donor atoms create an electric field and the Fermi level has to be discontinuous across the interface between the two materials. At low temperatures where the discreteness of the spectrum becomes apparent, only the first subband is occupied if the electron density (and consequently the Fermi level) is appropriately tuned. 2.2. THE QUANTUM DOT 21 thought of as an artificial atom, with electrons arranging themselves in subshells. The condition for observing energy quantization is that the energy level spacing has to be larger than the broadening of the energy levels due to tunneling out of the dot. The confinement of the electrons on the quantum dot also leads to an enhancement of the Coulomb repulsion that manifests as charge quantization. For the charge on the dot to be quantized, the energy associated with increasing the number of electrons on the dot by one has to be larger than the energy associated with the time to tunnel off the dot by means of the Uncertainty Principle. This means that the lifetime of the electron on the island should be large. Exactly how large is an important question that will be discussed in chapter 5. An intuitive way to explain the charging energy is by analogy to a capacitor: once the quantum dot is charged with one electron, Coulomb repulsion will keep other electrons from tunneling onto it, unless these electrons can pay the additional energy cost. There are two ways in which a 2DEG in a semiconductor heterostructure can be used to form a quantum dot. A lateral quantum dot uses lithographically-defined metallic gates deposited on the surface of the heterostructure to deplete the 2DEG. Approximately 50 electrons are confined in a 100 nm diameter droplet. They are coupled via tunable single mode quantum point contacts to extended sections of the 2DEG, which serve as leads. It is also possible to etch away sections of the 2DEG to define the electron droplet. In this geometry, the conductance though the point contacts often becomes immeasurably small before the dot is entirely emptied. Vertical quantum dots are are formed by etching a double barrier heterostructure. This allows the formation of a small, well-coupled, few-electron quantum dot with wide lead-dot contacts that contain several partially-transmitting modes. They allow the conductance of the dot to remain measurable all the way down to the last electron but are not easily tunable. For a 2DEG with certain parameters, the energies associated with charging or with energy quantization are determined by the size of the potential box. For a square well of size L, the level spacing between the quantized levels is ∆ ∝ to a capacitor, the charging energy is EC ∝ 1 . L 1 . L2 By analogy Depending on the value of L, the quantum dot is either in the metallic transport regime EC ≫ ∆ ≃ 0 and the density 22 CHAPTER 2. QUANTUM DOTS AS A MODEL SYSTEM of states of the dot is continuous, or in the semiconducting regime where EC , ∆ > 0, and the density of states of the dot has gaps. In addition, depending on how the size of the dot compares to the characteristic length scales of the 2DEG and how large its coupling to the leads (Γ) is, transport through the dot is determined by different processes. Here is a summary of the different regimes that can be used to broadly categorize quantum dots: 1. BALLISTIC (L < le ): electrons travel in a straight path inside the dot and only scatter off the walls of the potential. If the irregularities in the potential are smaller than the wavelength of the electrons, then electrons are simply reflected back without any energy loss (specular scattering). The time to cross the dot determines a characteristic energy scale called the ballistic Thouless energy: ET h = 2 ~vF L . If the motion of the electrons inside the dot is mostly chaotic, transport though the dot at energies below ET h is independent of the dot geometry and only dependent on the coupling to the leads. 2. DIFFUSIVE (L > le ): electrons scatter of the potential of impurities before they scatter of the confining potential. If the disorder is weak, perturbation theory can be used to describe the system. In large quantum dots that are quasi-2D, disorder causes all single particle states to become localized. The size of the system is characterized by the Thouless energy, given by: ET h = 2L2 vF τe 3. CHAOTIC: when the shape of the dot is irregular and the electrons bounce around inside the dot several times, their motion is mostly chaotic. In a classical system this means that there is an exponential sensitivity to initial conditions. The statistical quantum fluctuations of a classically chaotic system are universal. They are described by random matrix theory and can be studied in stadium shaped quantum dots. 4. REGULAR: the shape of the dot leads to a confining potential (for example a harmonic potential) where the single particle levels are arranged in shells and well defined periodic orbits transport electrons through the quantum dot. 2.2. THE QUANTUM DOT 23 5. CLOSED (Γ ≪ ∆, U): in quantum dots that are well isolated from the leads, charge quantization can be observed and transport properties are dominated by the Coulomb repulsion between electrons. 6. OPEN (Γ ≫ ∆, U = 0): in quantum dots that are well coupled to leads, the single particle levels are broadened and overlapping. These systems are well described as non-interacting electron systems. The quantum dots used in the experiments described in this thesis are shown in fig. 2.3. They are lateral quantum dots defined by Au gate electrodes deposited on the surface of a GaAs/AlGaAs heterostructure which has a 2DEG 68 nm beneath the surface. The 2DEG parameters are given in table 2.1. The thin constrictions labelled QPCs in fig. 2.3 connect the electrons in the dot to the electrons in the rest of the 2DEG. Depending on the size and location of the gates, they couple differently to the quantum dot parameters. The gates labeled bp and sp primarily control the distance of the dot levels to the Fermi level in the leads and thus the number of electrons on the dot. The gates labeled sw1/sw2 and bw1/bw2 determine the coupling of each of the dots to its leads. The gates labeled c1/c2 determine the interdot coupling and have a strong effect on the area of the large dot. Gates sn1 and sn2 have been used to form the small dot, but are not varied during the measurement. How the voltages on the different gates affect the electrons on the dot can be quantified by associating a capacitance with each gate and with the dot as described in chapter 3. Both measured quantum dots are smaller than le of the 2DEG and thus, transport inside the quantum dots is ballistic. The charging energies, level spacing, and total number of electrons on the dot are listed in table 2.2. These parameters can be measured experimentally as is explained in the next chapter. For consistency, they can also be calculated using the area of the dot estimated from the SEM picture. Because the 2DEG is separated by ≈ 70nm from the gates, the potential applied to the gate will spread out by a similar distance in the plane of the 2DEG and the quantum dots are smaller than the actual area inclosed by the gate contours in the SEM picture. This consistency check works better for the large dot in fig. 2.3. We measure the conductance though the quantum dots by using a 1 to 5 µVrms 24 CHAPTER 2. QUANTUM DOTS AS A MODEL SYSTEM bp bw1 c1 sn1 QPC1 sw1 sp n sw2 QPC2 1 μm c2 bw2 sn2 Figure 2.3: The double quantum dot device used for the experiments in this thesis. Both dots have been used for the experiment on the two channel Kondo effect (chapter 4 part 2) and for measuring the charge quantization in the large dot at N = 1 (chapter 5 part 2). The small dot was used for the out-of-equilibrium Kondo effect measurement (chapter 4 part 1). The large dot was used for the dephasing time measurements (chapter 5 part 1). A U ∆ Ne ET h ΓN =1 τdN =1 e2 C 2π~2 m∗ A ~v √F A small dot 0.04 µm2 1 meV 100 µeV ≈ 30 80 µeV large dot 2.6 µm2 150 µeV 3.1 µeV ≈ 4000 25 ps 0.75 ns 2∆ h Γ Table 2.2: Characteristic parameters of the quantum dots 2.3. FROM A CLOSED TO AN OPEN QUANTUM DOT 25 oscillating voltage with a frequency of 13, 17 or 97 Hz and measuring the resulting current with a DL Instruments Model 1211 current pre-amplifier and a Princeton Applied Research 124A lock-in amplifier. This AC oscillation is on top of a DC bias voltage that is used to characterize the system at finite bias. The quantum dot is cooled to 4 K with a positive bias of 180 to 200 mV applied to all gates. The positive bias “pre-depletes” the gates, so that the quantum dot is already formed, albeit very well coupled to the leads, even if all gates are set to 0 V. The measurements are performed in a Kelvinox TLM 400 dilution refrigerator with a base temperature Tbase ≈ 10mK where electrons can reach the lowest temperature of 13 mK [49]. 2.3 From a Closed to an Open Quantum Dot Electrons in quantum dots are coupled to the environment in two ways. They are coupled to an environment that consists of the surrounding electrons, nuclear spins of atoms, charged or magnetic impurities, and phonons inside the material. The coupling to this environment is fixed by the parameters of the 2DEG and is only affected by outside perturbations such as temperature and bias. It determines whether transport through the dot is ballistic or diffusive. Electrons are also coupled via quantum point contacts to the 2DEG reservoir. The size of this coupling, Γ (the tunnel rate) can be tuned via gate voltages and the conductance can be dramatically different depending on how Γ compares to other dot energy scales. The coupling of the quantum dot to the 2DEG reservoirs via the QPCs determines whether the quantum dot is called open or closed. The quantum point contacts (QPCs) can be thought of as a 1D waveguide (ballistic transport) whose transmission is tuned by gate voltages [10]. Electrons can move along the x-axis in fig. 2.4 (a), but the wavevector component transversal to the QPC is quantized and only electrons whose energies match the allowed subband energies, schematically illustrated in fig. 2.4 (b), can be transmitted. Thus, if the gate voltage is tuned such that the Fermi energy of the leads is below the first subband, transport is exponentially suppressed. Electrons have to tunnel through the barrier to reach the dot: most electrons are reflected and very few are 26 CHAPTER 2. QUANTUM DOTS AS A MODEL SYSTEM (b) (a) Yy E VQPC1 E(Y)2 X x EF E(Y)1 E(Y)0 E(X)+E(Z)0 y Figure 2.4: (a) Zoom in of the QPC region; electrons can travel in the x direction but their motion in y is confined by the voltage on the QPC gates ( z is confined because (y) of the 2DEG). (b) Sketch of the allowed energy levels Ei inside the QPC; only the subbands below the Fermi level can transmit electrons through the QPC. transmitted. When the first subband reaches the Fermi level, the transmission of the QPC is 100%: exactly one spin-degenerate mode of electrons can pass through the QPC. As the gate voltage is further decreased and more subbands are pulled below the Fermi level, additional modes open up as shown in fig. 2.5. The conductance of the QPC is solely determined by the sum of the probabilities of transmission of a state i in the dot to a state f in the leads (or vice-versa). The relation between the conductance and the transmission is given by the Landauer formula 2 P G = ms eh i→f |ti→f |2 where ms is the spin degeneracy. Thus, each fully transmitting spin-degenerate mode contributes a quantum of conductance GQ = 2e2 /h, as can be seen in the conductance in fig. 2.5. At zero temperature the conductance of the QPC is a perfect staircase that washes out with increasing temperature. The strength of the coupling between the dot and the leads Γ depends on the size of the tunnel barrier. If Γ ≪ kB T, ∆, U then the quantum dot is isolated and the discrete levels in the dot are not affected by the leads. This is called a closed quantum dot. For larger Γ, the fact that the dot levels are coupled to the continuum density of states in the reservoir leads to the broadening of the dot single particle energy states. When the QPC is tuned to the first plateau, i.e.N = 1, where N is the number of spin-degenerate modes in the QPC, its conductance is GQP C = 2e2 /h and the levels on the dot are broadened such that Γ = ∆. The lifetime of the single electron state, 2.3. FROM A CLOSED TO AN OPEN QUANTUM DOT 27 E E(Y)2 EF E(Y)1 E(Y)0 2 GQPC (2e /h) 4 3 2 1 0 -800 -600 -400 VQPC1 (mV) Figure 2.5: The conductance through the QPC increases in units of 2e2 /h with increasing gate voltage. 28 CHAPTER 2. QUANTUM DOTS AS A MODEL SYSTEM or the dwell time of the electrons on the dot then only depends on the size of the dot. The characteristic dwell times at N = 1 for the quantum dots studied in this thesis are given in table 2.2. The Coulomb Blockade model describes the behavior of a quantum dot in the weak tunneling regime where GQP C1,2 << 2e2 /h. The model that describes the behavior in the strong tunneling regime, where GQP C1,2 < 2e2 /h, is the Kondo model. The model that describes the behavior when the QPCs are fully open and GQP C1,2 ≥ 2e2 /h is random matrix theory. This thesis will describe measurements in the latter two regimes. Chapter 3 Quantum dots: Coulomb Blockade The simplest model that describes quantum dots that are coupled to leads via tunneling point contacts is the constant interaction model. This model combines the effects of the enhanced Coulomb repulsion with the presence of a quantized energy spectrum and can be used to understand many of the features of electronic transport through a quantum dot such as the evolution of the charge on the dot as a function of gate voltage, the effect of finite applied bias on the conductance, and the tunneling processes which contribute to transport. 3.1 The Charging Energy I will first discuss a simpler case, that of a metallic dot (∆ = 0) and then consider the modifications needed to account for the discrete density of states of the quantum dot. Fig. 3.1 shows a schematic representation of a quantum dot tunnel coupled to source (S) and drain (D) leads and coupled capacitively to both source drain and gates, the latter generically denoted by the index G. Let the dot be neutral when there are no voltages applied. As a function of the voltages applied (VR , VL and VG ) the charge on the quantum dot QDOT will change. Conservation of charge and Kirchhoff’s laws 29 30 CHAPTER 3. QUANTUM DOTS: COULOMB BLOCKADE dictate that: −QDOT = −qD − qS − qG qg qD − −VG + VD = CD CG qS qg VG − VS = − + CS CG (3.1a) (3.1b) (3.1c) where qD,S,G is the charge accumulated on the capacitors connecting the dot to the drain, source and gates. CD CS VS VD dot, N CG VG Figure 3.1: A quantum dot with N electrons is coupled electrostatically to source, drain, and gate electrodes and tunnel-coupled to source and drain leads. The total energy of the dot with charge QDOT is the sum of the energy stored in the three capacitors minus the work done by the voltage sources: Etotal (QDOT , QG ) = (QDOT − QG )2 + other terms(VD , VS , VG ) 2C (3.2) where C = CD + CS + CG is the total capacitance of the island and QG = CD VD + CS VS + CG VG is the total charge induced by the three voltage sources. Usually VS and VD are small and QG can be thought of as the charge induced by the gate. QG is a continuous quantity because VG is continuous. If the QPCs are in the tunneling regime, then QDOT is discrete: the total charge on the dot has to correspond to an 3.1. THE CHARGING ENERGY 31 integer number of electrons Ne− . Disregarding the other terms, the total electrostatic energy is: Etotal (N) = QG Q2G e2 N 2 + eN + 2C C 2C (3.3) The total energy of the dot as a function of the gate voltage is shown in fig. 3.2(a). With increasing gate voltage, the number of electrons corresponding to the lowest energy increases in discrete steps (fig. 3.2(b)), corresponding to the gate voltage where Etotal (N) = Etotal (N + 1). (3.4) (b) (a) 2 1.0 >TODN< U/latotE 0.5 0.0 -1 N=0 N=1 N=2 0 1 2 3 0 -2 -2 QG/e 0 2 QG/e Figure 3.2: (a) At T=0, the lowest energy state of the quantum dot has different numbers of electrons on the dot, depending on the gate voltage setting. (b) The number of electrons on the dot increases by exactly one electron at specific gate voltage values. The discrete steps at T = 0 (red trace) are smeared out at T>0 (black trace, with kB T = 81 U ). The additional energy needed to add one electron to a dot with N electrons is: δEtotal (N + 1) = Etotal (N + 1) − Etotal (N) 1 QG )U = (N + − 2 e where U = e2 C (3.5) is called the charging energy of the dot. Note that the classical charging energy of a capacitor C with one electron is EC = energy U of the dot. e2 2C and is different from the charging 32 CHAPTER 3. QUANTUM DOTS: COULOMB BLOCKADE (b) (a) E E μN+1 U+ μS μN N+1 μD U+ μN electron reservoir N quantum dot Figure 3.3: (a) Transport through the dot is forbidden when the Fermi energy of the leads lies between the electrochemical potentials of the dot. (b) Transport through the dot is allowed when a single particle level aligns with the Fermi level of the leads: electrons can tunnel on and off the dot. The constant interaction model accounts for the discrete energy spectrum of the dot simply by adding the single particle energies ǫi to the total electrostatic energy Etotal calculated above. The electro-chemical potential µN is defined as the energy needed to add the N th electron to a conductor. If E(N) = N X i=1 then ǫi + e2 N 2 QG + eN 2C C CD VD + CS VS + CG VG 1 +e . µN = ǫN + U N − 2 C (3.6) (3.7) Changing VG shifts the chemical potential of the dot with respect to the Fermi level of the leads. At low temperatures and small bias voltage eV compared to the charging energy U, an electron can jump on or off the dot if and only if the chemical potential of the dot aligns with the Fermi level of the leads. This is shown schematically in fig. 3.3. Due to the finite charging energy U, most of the time the two are not aligned so the number of electrons on the dot is fixed and transport through the dot is suppressed. 3.1. THE CHARGING ENERGY 33 (b) (a) -3 40x10 0.10 2 )h/ e(G 2 )h/ e(G 20 0.05 U+ ∆ U 0.00 -295 V BP -290 (mV) -285 -110 -100 V SP -90 (mV) Figure 3.4: When the QPCs are in the tunneling regime, sharp peaks in conductance alternate with large regions of zero conductance as a function of gate voltage. (a) When ∆ < T the distance between many successive peaks remains constant and is proportional to the charging energy U. (b) When ∆ ≫ T the Coulomb blockade peaks are not equidistant. This is called Coulomb blockade. When the gate voltage is such that µD ≈ µD ≈ µN , the number of electrons on the dot can fluctuate by one and a peak in conductance is observed. The distance between the peaks corresponding to the N th and (N + 1)th electron traversing the dot is µ( N + 1) − µN = U + ∆N +1 . This corresponds to a change in gate voltage e∆VG = C (U CG + ∆N +1 ). Fig. 3.4 shows experimental results from measuring the two dots in fig. 2.3 at 15 mK. The alternating pattern of peaks and suppressed regions of conductance as a function of gate voltage is apparent in both dots. For the large dot where ∆ < kB T the Coulomb blockade peaks are equidistant in gate voltage as seen in fig. 3.4(a). The discrete energy spectrum is only observable in the small dot measurement (fig. 3.4(b)). The left Coulomb blockade valley is slightly larger than the right Coulomb Blockade valley. This is because when one electron fills an unoccupied single particle state in the dot, the next electron can fill the same state just with opposite spin. As such, the first electron has to have an energy U + ∆ to tunnel on the dot, while the following electron only needs energy U. If ∆ > kB T , as is the case for the small dot (see table 2.2), the extra energy required to occupy a new single particle level modifies the distance between Coulomb blockade peaks. 34 CHAPTER 3. QUANTUM DOTS: COULOMB BLOCKADE 3.2 Coulomb Blockade Diamonds At finite bias, transport through the dot can occur as long as the energy of the dot level lies in the transport window eV . In most experimental cases, the bias is not applied symmetrically to the source and drain: VD = 0, VS = VSD . How much each voltage affects the electrochemical potential of the dot is determined by the ratio αD,S,G = − CD,S,G . C Transport through the dot at VSD > 0 is forbidden (fig. 3.3) if: µN < EF (3.8a) µN +1 > EF + eVSD . (3.8b) Similar inequalities hold for VSD < 0. (a) (b) VSD VSD (U+ N-1 N N+1 N+1)/ +2 N-1 VG (U+ +1) N +1 VG G Figure 3.5: Finite bias and gate voltage measurements reveal Coulomb blockade diamonds in the metallic case (∆ < kb T ) (a) and Coulomb blockade diamonds with excited states present in the semiconducting case (∆ ≫ kB T ) (b). The region where transport is forbidden and the conductance through the quantum dot is suppressed is shaded in gray. Using eq. 3.7, these conditions can be used to solve for VG as a function of the number of electrons on the dot N and bias VSD . They delimit diamond-like regions in gate voltage and bias where the conductance is zero, as illustrated in fig. 3.5. The size of the blockaded region is determined by the charging energy U. In the case of a 3.2. COULOMB BLOCKADE DIAMONDS (a) 35 200 (b) 2 G(e /h) 2 G(e /h) 200 0 µ V V 01x 0.4 DS DS 40 3- µ ( 0 0.6 -200 ( 60 )V )V 80 -400 0.2 20 -200 0 -350 -345 V GATE2 (mV) 0.0 -600 -230 V -220 SP (mV) Figure 3.6: When the QPCs are in the tunneling regime, diamond-like regions of suppressed conductance (dark blue) occur as a function of gate voltage and source drain bias. (a) CB diamonds measured in the large dot (∆ < kB T ) show only Coulomb blockade features. (b) The small dot measurements (∆ > kB T ) show transport through excited states at finite bias. discrete level spectrum, transport at finite bias shows extra features. This is because electrons can use either the ground state or the excited state to tunnel though the dot when one of the excited states of the dot spectrum also lies in the transport window. When an excited state crosses the source or the drain level, another peak in conductance is observed. The indicated level spacing assumes a single particle picture where µ( N + 1) − µN = U + ∆N +1 and µ( N + 2) − µN +1 = U + ∆N +2 . This difference between the appearance of Coulomb blockade (CB) diamonds in the metallic vs semiconducting regimes is illustrated in the measurements in fig. 3.6. The left graph (a) shows finite bias transport in the large quantum dot. The peak corresponding to the drain line is rather faint, but Coulomb blockade diamonds without any traces of excited states can be seen. Fig. 3.6(b) shows a zoom in of a diamond in the small quantum dot with extra peaks that correspond to transport though the excited states. The spectrum of the dot is indeed discrete with an average single particle level spacing for the first few excited states of the N electron dot ∆ ≈ 100µeV (see table 2.2). Note that the charging energy U is much larger than the bias voltage range in this measurement. Also note the difference in bias range of the y-axis of the two graphs shows that the charging energy for the large dot is significantly smaller than for the small dot. 36 CHAPTER 3. QUANTUM DOTS: COULOMB BLOCKADE The discussion so far does not explain how temperature or coupling to the electrical leads affects the quantum dot. To measure any of the data presented above, the quantum dot is coupled to two leads. The Hamiltonian of the system then includes the different subsystems and the interaction between them: H = Hleft + Hright + Hdot + Htunneling + Hcharging (3.9) where Hlef t /Hright describes the non-interacting electrons with momentum k/q and spin s in the left/right reservoir (source and drain), Hcharging is due to the Coulomb repulsion and Htunneling describes electrons tunneling from the leads on and off the dot and are given by: Hleft = X † ǫk lks lks (3.10a) † rqs ǫq rqs (3.10b) ǫp d†ps dps (3.10c) k,s Hright = X q,s Hdot = X p, 2 e (n̂ − QG )2 2C X X L † R † = Tkp lks dps + h.c. + Tqp rqs dps + h.c. Hcharging = (3.10d) Htunneling (3.10e) p,k p,q (3.10f) where n̂ = P p d†ps dps is the number operator of the electrons on the dot and T L,R are the tunneling matrix elements between a dot state and the leads and are used to define the coupling Γ of the dot to the leads. Depending on the relation between ~Γ, kB T, ∆ and U different processes dominate transport and the characteristic dependence of the conductance on temperature and bias can be calculated. In the regime where ~Γ ≪ kB T ≪ ∆, U, the quantum dot can be used as a thermometer. Because the coupling to the leads is small, the levels in the dot can be thought of as delta-functions. On the Coulomb blockade peak, a single level contributes to transport. The broadening of the peak is determined by 3.2. COULOMB BLOCKADE DIAMONDS (a) 37 (b) (c) 2 -3 20x10 0.3 10 T(mK) ∆Vsp (mV) 2 G (e /h) 100 0.2 2 10 0.0 -225 Vsp (mV) 4 3 0.1 0 7 6 5 -224 0 100 200 T (mK) 4 10 resistantce for R13 (Ohm) Figure 3.7: (a) A thermally broadened Coulomb blockade peak. The fit yields a width that corresponds to a temperature of 14.5 mK. (b) The evolution of the width of a Coulomb blockade peak with temperature. (c) The correspondence between the electron temperature (y-axis) and the resistance indicated by the Oxford dilution refrigerator probe thermometer nr. 13 (x-axis). the thermal broadening of the leads. The lineshape of the peak in gate voltage is given by: e2 G(VG ) = 4kB T 1 1 + Γs ΓD −1 −2 cosh αG (VG0 − VG ) 2kB T (3.11) where VG0 is the gate voltage coordinate of the peak and ΓS,D is the coupling of the dot to the source and drain, respectively. Fig. 3.7(a) shows a temperature broadened Coulomb blockade peak measured in the small dot. By fitting a cosh−2 function to the peak, the width of the peak can be extracted and is plotted as a function of temperature in fig. 3.7(b). The temperature dependence of the width in fig. 3.7(b) allows an accurate determination of the lowest electron temperatures of the system. At high temperatures the electrons in a quantum dot are in thermal equilibrium with the surrounding systems. As such, the temperature can be determined by measuring a calibrated resistor nearby. The resistor readings do not correspond to the temperature of the electrons at low temperatures and a different method for determining the electron temperature has to be used. For reference, I am showing the 38 CHAPTER 3. QUANTUM DOTS: COULOMB BLOCKADE conversion between the actual value of the dilution refrigerator resistor and the actual temperature of the electrons in the quantum dot. The electron temperatures values have an error for the peak fit of ±10% at low temperature. This conversion has been used throughout the experiments in this thesis to determine the electron temperature. Chapter 4 Quantum Dots: the Kondo Effect In the late 1980’s it was noticed that a quantum dot with a net spin 12 , tunnel-coupled to an electron reservoir, has the same Hamiltonian as a magnetic impurity inside a metal [43, 44] and should thus exhibit Kondo physics. About a decade later, the Kondo effect was experimentally observed in a lithographically defined quantum dot containing an odd number of electrons [50] with the 2DEG electrical leads playing the role of the metal. In bulk systems, the formation of the Kondo screening cloud at low temperatures enhances the scattering of conduction electrons by the local magnetic site and thus leads to a suppressed conductance. In quantum dots, the Kondo state has the opposite effect: because transport is dominated by tunneling directly though the site, the enhanced scattering at low temperature gives rise to an extra mechanism for transport that enhances the conductance [21]. Quantum dots are particularly attractive for studying the Kondo effect because it is possible to study the effect of a single impurity rather than a statistical average over many impurity sites and because parameters of the Hamiltonian such as impurity-lead coupling or the energy of the impurity relative to the Fermi level can be independently controlled via gate voltages. Depending on the number and the type of degeneracies of a quantum dot state, a variety of Kondo correlations can be measured. Here are three examples of Kondo states that are not exclusively based on a spin 1 2 degeneracy. 1. When the electronic state of a system contains both orbital and spin degeneracy, the same delocalized lead electrons that magnetically screen the unpaired spin 39 40 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT can also electrostatically screen the orbital degeneracy. The two degrees of freedom give rise to an SU(4) Kondo effect, which has been observed in vertical GaAs dots [51] and carbon nanotubes [52]. 2. The ground state of a quantum dot with an even number of electrons is usually a spin singlet at zero magnetic field, where each occupied orbital contains a pair of electrons. The triplet state becomes the ground state if the exchange energy gained for parallel spin filling exceeds the orbital energy difference between levels [53]. Since the reservoir electrons are spin 1 2 they can only partially screen the S=1 quantum dot, leaving behind a residual spin 21 . A low Kondo temperature has been predicted for these systems [54] and experiments have not been able to unambiguously demonstrate a pure spin-1 Kondo effect yet. 3. Another multiple degeneracy can be achieved using an applied magnetic field to bring the singlet and the triplet state into degeneracy. The Kondo effect associated with this four-fold degeneracy has been observed in transport measurements through vertical quantum dots [53], lateral quantum dots [55, 56], and carbon nanotubes [57, 52, 58]. Depending on exact the details of this system, a two stage Kondo effect [59, 60] or a quantum phase transition can be observed [61] I will start this chapter with the microscopic description of the Kondo effect in a spin 1 2 quantum dot coupled to a single reservoir of electrons. I will present the expectations for the scaling of the conductance with temperature and bias as well as the experimental findings for the scaling behavior in the non-equilibrium regime. Finally, I will summarize the procedure for tuning a double dot system though a quantum phase transition. 4.1. THE SINGLE CHANNEL KONDO EFFECT IN A QUANTUM DOT 4.1 41 The Single Channel Kondo Effect in a Quantum Dot A localized state that is degenerate and partially filled, coupled to a continuum of states is well described by the Anderson Hamiltonian. At low temperature an enhancement of the conductance due to the Kondo effect is expected to occur. In a quantum dot, in the absence of additional degeneracies, the state with an odd number of electrons on the dot is doubly degenerate. In this case, it has a net spin 1 2 and is therefore equivalent to a magnetic artificial atom. The s-d Hamiltonian can be used to describe the quantum dot coupled to leads: ~DOT Hint = J~σcond · S (4.1) ~DOT is the net spin of the quantum dot, while ~σcond is sum of spin operators for where S the conduction electrons and J is the antiferromagnetic exchange coupling. The reason the interaction between the dot electrons and the lead electrons is antiferromagnetic is because spin-flip cotunneling processes dominate in the odd Coulomb Blockade valley at low temperatures. Coupling additional leads to the quantum dot modifies the total coupling of the dot to the leads but does not affect overall Kondo behavior. As long as Kondo processes can freely exchange electrons between each pair of reservoirs the leads behave as a single collective reservoir and the traveling electrons are a linear combination of the different lead electrons [62]. Only the linear combination that has a non-zero DOS at the dot is coupled to the dot. The other linear combinations are irrelevant. The Kondo temperature (eq.1.7) introduced in section 1.4 can be rewritten in terms of quantities that are more easily controlled and measured in quantum dot experiments [63]: TK ∝ √ ΓU e− πǫd (ǫd +U ) ΓU (4.2) where ǫd is the energy of the dot state measured relative to the Fermi energy EF of the leads and Γ is the rate for electron tunneling on and off the dot. The Kondo temperature is a way to quantify the binding energy of the Kondo singlet but because 42 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT this state forms gradually, definitions can differ by a constant factor. The definition used in this thesis is appealing from an experimental point of view: the Kondo temperature is the temperature at which the Kondo conductance has reached half of its zero-temperature value (as extrapolated from measurements) [21, 50]. Since the spin 1 2 Kondo effect occurs only when the local site is singly occupied (ǫd < 0 and ǫd + U > 0), the exponent in eq. 4.2 is negative, as expected from equation eq. 1.7. TK is maximized when the quantum dot state is energetically close to EF (ǫd ≈ 0) and strongly coupled to the leads (large Γ). However, near the charge degeneracy points ( ǫd = 0 and ǫd + U = 0), the state is not localized anymore and the Kondo model will break down. This regime of strong charge fluctuations is referred to as the mixed valence regime [21]. The values of the charging energy (U) and level spacing (∆) determine how high TK can be. In semiconductor quantum dots it is in the range of 0.1 to 1K and around 10K in carbon nanotube quantum dots. Conductance through a Kondo coupled quantum dot The Kondo state can be probed by measuring the differential conductance though the quantum dot G(V, T ) = dI dV . The conductance is related to the transmission elements of the dot’s scattering matrix. If one of the leads acts as a weak probe, then the conductance is in fact probing the density of states of the dot. The presence of the Kondo state manifests itself as a thin narrow resonance at the Fermi energy of the leads. As a function of gate voltage, at zero applied bias, an enhanced conductance in the odd valley, when the total spin on the dot is 1 2 appears. Fig. 4.1 shows how as a function of the occupancy of a dot, the low-temperature conductance alternates between high (odd valley) and low (even valley) at zero bias, and decreases away from zero bias. This alternating pattern in conductance values for consecutive Coulomb Blockade valleys, that is consistent with the presence of the Kondo effect in the odd but not in the even valley, was first observed in experiments in lateral quantum dots [50, 64, 65]. One of the disadvantages of the lateral geometry is that direct transport though the dot can become too small to measure before the dot is emptied. This makes it impossible to determine the absolute number of electrons on the dot. 4.1. THE SINGLE CHANNEL KONDO EFFECT IN A QUANTUM DOT (a) (b) 40 43 2.0 2 G(e /h) 1.5 1.6 1.2 V DS 2 ( 0 )h/ e( G µV) 20 -20 1.0 even odd even odd even 0.8 0.4 -40 -220 -200 -180 V SP -160 -140 -120 0.5 -200 (mV) -150 V SP (mV) Figure 4.1: (a) The conductance though the dot is enhanced in non-consecutive valleys at zero bias. The vertically tilted high conductance lines correspond to transport through a resonant level. (b) Horizontal cut through (a) at VS D = 0 indicating the even and odd Coulomb blockade valleys. Experiments that showed that the enhancement was indeed in an odd valley were preformed in vertical quantum dots [66] where the total electron number is determined by counting Coulomb blockade peaks as the quantum dot is emptied by an increasingly negative gate voltage. An alternative way of counting electrons is to use a quantum point contact (QPC) fabricated close to the quantum dot, to detect the dot occupancy [67]. This makes it easier to determine the total number of electrons in lateral dots. Even when transport through the quantum dot is undetectable in direct transport measurements the QPC conductance is altered by the electrostatic potential of each electron added to the quantum dot and the exact number of electrons on the dot can be counted. In small GaAs quantum dots the even-odd conductance alternation due to spin- 12 Kondo is the rule rather than the exception. If the local degeneracy is not spin based, this even-odd rule does not apply. With decreasing coupling to the leads (Γ) the Kondo temperature is reduced (eq. 4.2) and the high conductance for odd occupancy disappears. When it is lower than the measurement temperature we recover the Coulomb blockade regime discussed in the previous chapter. 44 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT The effect of temperature, bias and magnetic field So far we have discussed that the Kondo state is characterized by the even-odd alternation of conductance as a function of the dot occupancy. In addition, the Kondo state has several other distinctive features: the enhanced conductance of a spin 1 2 Kondo dot has a characteristic temperature dependence, it is suppressed by applying a finite bias across the dot, and is also suppressed by magnetic field. The magnetic field splits the local spin degeneracy which can be recovered at finite magnetic field by applying a bias voltage equal to the Zeeman splitting. This characteristic dependence of the conductance on external parameters (temperature, magnetic field, voltage across the dot) can be calculated [68]. Even though the three perturbations have similar effects on conductance, the mechanism is slightly different in each case and will be discussed in more detail below. Two regimes can be distinguished depending on whether the perturbations (kB T, eV, and gµB B) are small or large compared to kB TK . In the high energy regime Kondo transport shows a logarithmic dependence on energy which corresponds to Kondo’s perturbative treatment: G(x) ≈ 1 ln2 (x/k B TK ) x = kB T, eV, gµB B ≫ kB TK (4.3) At low energy, the system behaves as a conventional Fermi liquid, with modified numerical parameters [69]. Hence, for kB T, eV, and gµB B ≪ kB TK the Kondo spectral function and the associated transport through a spin- 21 Kondo dot show a quadratic dependence on external parameters: G(x) ≈ G0 (1 − C x 2 ) kB TK x = kB T, eV, gµB B (4.4) where G0 = G(x = 0) and C are different for the three perturbations. This E 2 dependence of the Kondo spectral function, which reflects the E 2 scattering rate of quasiparticles in a Fermi liquid, can be probed by varying temperature and by applying a bias across the dot [50, 64]. Fig. 4.2 (a) shows that for small biases, the Kondo conductance peak measured 4.1. THE SINGLE CHANNEL KONDO EFFECT IN A QUANTUM DOT (b) (a) 2.0 1.8 G (e2/h) 1.2 G(e2/h) 45 1.0 0.8 1.6 1/ln2(T/TK) 1.4 1.2 G0-CVP -40 -20 0 G0-BTP 1.0 0.6 20 40 101 102 T (mK) Vbias(µV) Figure 4.2: (a) For low bias, the Kondo resonance has a power law dependence on bias. (b) Similarly, at low temperatures, the conductance follows a power law that crosses over at higher temperatures to a logarithmic dependence. in the small quantum dot falls off with V 2 . The characteristic T 2 dependence at low temperatures that crosses over to a logarithmic temperature dependence as T approaches TK can be seen in the conductance measurements shown in fig. 4.2(b). There is no analytic expression connecting the two regimes but an empirical expression [70] that matches numerical renormalization group (NRG) calculations for spin 1 2 Kondo [21] over the entire temperature range describes the data remarkably well and is often used to characterize experimental measurements: G(x) ≈ G0 ( TK′ 2 )s ′ 2 2 T + TK (4.5) where s determines the slope of the conductance decrease and matches the slope found in NRG calculations best for s = 0.22. Here TK′ = defining TK such that G(TK ) = G0 , 2 TK , (21/s −1)1/2 which is equivalent to as noted earlier. As temperature is raised, the conductance in the odd valleys decreases due to suppression of the Kondo effect while the conductance in the even valleys increases due to thermal broadening of the quantum dot levels. At temperatures above TK , non-Kondo conductance channels can develop [68], which lead to deviations from equation 4.5. Some quantum dot devices exhibit parallel non-Kondo conduction channels. These 46 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT are accounted for by adding a temperature independent offset to eq. 4.5 but the validity of using such an offset in analyzing Kondo behavior is not yet established. An applied magnetic field also affects the Kondo state because it lifts the degeneracy between the two spin states on the quantum dot. The asymmetry between the two spin states acts to suppress Kondo correlations. The splitting of the Kondo spectral function with higher magnetic field can be probed by measurement of differential conductance as a function of bias [50, 64] Conductance scaling As mentioned above, temperature, bias and magnetic field affects the Kondo state in a similar manner. As a consequence, the characteristic exponent of the lowest order response is identical for the different perturbations. In addition, although the coefficients of the lowest order response generally depend on system-specific energy scales, these dependences can usually be eliminated by scaling each perturbation relative to a characteristic energy. This allows a system that exhibits the Kondo effect to be described by a single universal scaling function. Universality refers to the fact that similar behavior can be observed in systems that seem not to be related. Universal scaling laws describe phase transitions and critical phenomena. For example, the evolutions of thermodynamic parameters of certain liquid-gas and paramagnetic-ferromagnetic phase transitions are characterized by identical sets of critical exponents although the underlying forces (van der Waals and magnetic exchange, respectively) are very different. Similarly, the conductance of Kondo systems in different materials collapses onto a single curve once each conductance value is scaled appropriately using the Kondo temperature and zero temperature conductance, TK and G0 , respectively [30, 71]. The generalized scaling relation between temperature and bias can be expressed as: (G(V = 0, T ) − G(V, T ))/G0 eV = F( ) α CT kB T (4.6) where F ( keV ) is a universal function that depends on the type of Kondo effect, but BT not on the exact details of the Kondo system at hand. The scaling constants G0 and 4.2. THE NON-EQUILIBRIUM SINGLE CHANNEL KONDO EFFECT C are defined in eq. 4.4. The exponent for a spin 1 2 47 quantum dot is α = 2, but can take on different values in more exotic Kondo systems [30, 45] which will be described in the next section. Deviations from universality [72] are expected in certain regimes. Universal scaling laws governing perturbations that drive a system out-of-equilibrium and in particular those describing the non-equilibrium Kondo effect have been especially difficult to derive theoretically with high accuracy [73, 71, 74] Previous measurements of single channel Kondo behavior [30, 45] have shown that transport at zero bias does indeed follow a universal scaling curve in temperature but the nonequilibrium regime has not been closely examined. In the following section we report measurements of the universal scaling function of the non-equilibrium spin 1 2 Kondo effect. 4.2 The Non-equilibrium Single Channel Kondo Effect In quantum dots, the non-equilibrium Kondo effect can occur when both leads participate in forming the Kondo state. When a bias voltage is applied between the two leads, neither reservoir is in equilibrium with the quantum dot which drives the Kondo state out of equilibrium. Theoretical work predicts that universal scaling behavior in temperature and applied bias is maintained in the non-equilibrium Kondo regime [30, 71, 21] but disagrees about the values of the universal scaling function coefficients and about how many system-specific scaling parameters are necessary [74]. Reliable low-energy scaling behavior has not been previously extracted because experimental measurements have focused on the higher energy (eV ≈ kB TK ) regime [50, 64, 70, 75, 45]. This section describes measurements of non-equilibrium transport through a singlechannel spin 1 2 Kondo (1CK) quantum dot at low temperature and bias (see ref. [76]). Fig. 4.3(a) shows the small dot and the measurement set-up used to determine the out-of equilibrium conductance. The gate labeled VG tunes the dot to odd occupancy and controls the energy ǫd of the singly occupied level. The characteristic energy 48 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT (a) (c) (b) (d) Figure 4.3: (a) The SEM image of the quantum dot and the measurement schematic where the lead marked NC does not contribute to transport. (b) The zero bias enhancement of G(V,T) across an odd valley at T = 13mK. (c) Temperature dependence of the Kondo plateau for T = 13 − 205mK at V = 0µV. (d) Temperature dependence of the Kondo peak for T = 13 − 205mK at VG = −203mV scales of this dot are given in table 2.2. The mean level spacing is ∆ ≈ 100µeV and the bare charging energy is U ≈ 1meV. In the Kondo regime the actual value of U is reduced by a factor of 5 − 10 due to the increased Γ necessary to achieve a large enough Kondo temperature. The enhancement of the conductance through the quantum dot at zero bias and across an odd valley (−ǫd , ǫd + U > Γ) between −220mV and −188mV is shown in Fig. 4.3(b). The zero bias conductance reaches a maximal value 1.75e2 /h in the middle region of the Kondo valley. This region from −209mV to −199.5mV is called the Kondo plateau and the mostly constant conductance indicates that the coupling 4.2. THE NON-EQUILIBRIUM SINGLE CHANNEL KONDO EFFECT 49 (b) Figure 4.4: (a) The extracted values of G0 and TK across the Kondo plateau, using eq. 4.5 over 13 − 35mK. (b) The scaled conductance versus T /TK for all measured temperatures and for all gate voltage points across the Kondo plateau agrees very well with the solid line given by eq. 4.5. asymmetry is around 2:1 [73]. In the rest of the odd valley Kondo processes mix with sequential tunneling processes and give rise to mixed valence behavior. The analysis presented here is restricted to the conductance measured across the Kondo plateau. As the temperature is increased from 13 mK to 205 mK the overall Kondo conductance across the odd valley decreases as shown fig. 4.3(c). Conductance as a function of source-drain bias in the middle of the Kondo plateau shows a narrow peak centered at zero bias, that broadens with increasing temperature (fig. 4.3(d)). To get G(T,V=0) at each point across the plateau we fit the Kondo peak in bias using a parabola (see fig. 4.2(a)) and use the maximum of the parabolic fit as the zero-bias conductance. This improves the accuracy of the fit by eliminating errors from the slow drift (< 1µV per hour) of the input bias of the current amplifier. The bias range for the fitting excludes the edges of the Kondo plateau (VG ≈ −209 mV and VG ≈ −200 mV) close to the Coulomb blockade peak where sequential tunneling contributes to conductance. We fit the conductance extracted in this manner to the empirical Kondo (EK) form given by eq. 4.5 and extract the extrapolated zero temperature conductance G0 and the Kondo temperature TK across the whole Kondo valley. From fig. 4.4(a) we observe that, as predicted by eq. 4.2, the Kondo temperature is larger when the level 50 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT resides close to Fermi level of the leads. In extracting the Kondo fitting parameters we limit the temperature range for our fits to T < TK /4. In the middle of the plateau this corresponds to T < 35 mK. The scaling of the conductance with temperature across the Kondo plateau is shown in Fig. 4.4(b). The solid line is the EK form and it accurately fits the data up to T /TK ≈ 0.25 (40 − 60 mK). Above this limit, deviations between the data and the EK form are above the experimental noise and are probably due to the emergence of additional transport processes at higher temperatures. The fit at higher temperatures can be improved by adding a temperature independent offset to the EK form as a fitting parameter. Similar offsets have been used in previous experiments in quantum dots and but because they are likely accounting for these additional high temperature transport processes, this parameter should not be truly temperature-independent. When an offset of ≈ 0.4 ± 0.1e2 /h across the plateau is included in the fit, the extrapolated value for G0 and TK decreases by 20 − 30% across the Kondo plateau. However, the quality of the fit below 40 mK becomes worse when using an offset: the deviations between the fit and data in the offset fit are twice as large as in the offset-less fit. Because we are interested in this low energy regime, we extract the Kondo fitting parameters in the temperature range T < 35 mK ≈ TK /4 (for gate voltages in the middle of the plateau) without adding an offset to the fits. Choosing the appropriate fit range for determining scaling exponents is particularly important because the power law behavior of the conductance at low temperatures transitions gradually into the logarithmic dependence at high energy. Fitting too far out in energy introduces artifacts from higher order terms. The empirical Kondo form encompasses both the low energy and the high energy regime. To determine how far the power-law regime extends, we consider the behavior of G0 − G(0, T ) vs. T /TK and G(0, T ) − G(V, T ) vs. eV /kTK on log-log plots, as shown in fig. 4.5. We limit the range to regions where the conductance traces follow quadratic behavior (dotted line) to within the scatter of measured points (T /TK ≈ 0.11 and eV /kTK ≈ 0.5, as noted by the vertical dashed lines in fig. 4.5). To check that single channel Kondo, predicted to be a Fermi liquid, does indeed follow a scaling law with quadratic exponents in bias and temperature we fit the 4.2. THE NON-EQUILIBRIUM SINGLE CHANNEL KONDO EFFECT 51 Figure 4.5: (a) The scaled Kondo plateau conductance versus the scaled temperature T /TK matches a quadratic (gray dashed line) for T /TK < 0.1. (b) The scaled Kondo plateau conductance versus eV /kTK for T = 13mK matches a quadratic for eV /KB TK < 0.4 (c) The scaled Kondo peak width vs T /TK across the Kondo plateau fits a quadratic also over the whole temperature range but the vertical dashed line marks the limit of the temperature range used to extract the scaling coefficients. conductance in the low energy range, determined above, to the form: G(T, V ) ≈ G0 − c′T (kB T )PT − c′V (eV )PV . (4.7) Here PT , PV are the exponents and c′T , c′V are the expansion coefficients that characterize the temperature and bias dependence. Although the choice of fit range is determined by assuming single-channel Kondo behavior, unlike the EK form (eq. 4.5), eq. 4.7 does not assume quadratic behavior at low temperature. Thus the values of G0 , TK and the form of the conductance fit do not assume Fermi liquid behavior. We extract PV by fitting G(T, V ) as a power-law in voltage for |V | < 7µV at each temperature point below 20 mK. We find that PV is nearly constant across the Kondo plateau with an average value of PV = 1.9 ± 0.15 (fig. 4.6). This is in good agreement with the predicted single-channel Kondo exponent of 2. Extracting PT is more difficult because the power law regime extends only up to T /TK < 0.1 and for each gate voltage point, there are only a few temperature points in this range, as seen in fig. 4.5(a). Fitting over this temperature range, and only considering gate voltage points with at least five temperature points inside this range, yields a mean value of PT = 2.0 ± 0.6 across the Kondo plateau. These fits are consistent with temperature and bias sharing a characteristic exponent of 2, as 52 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT Exponent 30 3.0 2.5 (a) 2.0 1.5 Alpha a (b) 0 15 0.15 0.10 G Gamma (c) 1.0 05 0.5 0.0 -210 -205 VG (mV) -200 -195 Figure 4.6: (a) Values of the bias Kondo scaling exponent PV across the Kondo plateau. The horizontal dashed line shows the theoretically predicted single-channel Kondo exponent, P = 2. (b) and (c) Values for the scaling coefficients α and γ extracted across the Kondo plateau described in the text. theoretically expected for the single-channel Kondo effect. The conductance should be well-described by a two parameter (G0 and TK ) universal scaling function. To determine to what extent the low energy non-equilibrium conductance G(T, V )/G0 is described by a universal scaling function, F (T /TK , eV /kTK ) and to extract the characteristic scaling coefficients we assume that the zero bias conductance follows the EK form as a function of temperature. For each point on the Kondo plateau we fit the Kondo peak using a low bias expansion that is applicable over a wide temperature range [77]: G(T, V ) = GEK (T, 0)(1 − 1+ cT α eV 2 ) )( T 2 − 1)( TK ) kB T cT ( αγ (4.8) 4.2. THE NON-EQUILIBRIUM SINGLE CHANNEL KONDO EFFECT 53 The coefficient cT ≈ 5.49 is fixed by the definition of TK via eq. 4.5: G(T, 0) = G0 (1 − cT ( TTK )2 ) The coefficients α and γ characterize the zero-temperature curvature and temperature broadening of the Kondo peak, respectively, and are independent of how TK is defined. We limit the temperature range for extracting the coefficients to points at which the zero bias conductance follows the EK form (T /TK < 0.25). This quadratic line shape for the tip of the Kondo peak G(T, V ) = G(T, 0)(1 − (V /W (T ))2) is appropriate because we are interested in the quadratic energy regime. The temperature-dependent width of the Kondo peak W (T )2 follows a quadratic of the form aTK2 + bT 2 as shown in fig.4.5(c). At low temperatures the form of eq. 4.8 reduces to a universal scaling function expansion suggested by Schiller et al. [4]: G(T, 0) − G(T, V ) T eV eV 2 T eV 2 = F( , ) ≈ α( ) − cT γ( )2 ( ) cT G 0 TK kB TK kB TK TK kB TK (4.9) Figures 4.6(b) and (c) show the extracted values of α and γ across the Kondo plateau, fitted over the regime T /TK < 0.2 and eV /kTK < 0.4. The coefficients are nearly constant across the Kondo plateau and have average values α = 0.10 ± 0.015 and γ = 0.5 ± 0.1 in the middle of the Kondo plateau. Both α and γ increase slightly on the right side of the Kondo plateau (VG > −199.5 mV). This may reflect the expected break-down of the universal scaling relation in the mixed valence regime where charge fluctuations are present in addition to Kondo processes. Other fitting functions that reduce to a quadratic at low bias match the data over a wider bias range but the extracted coefficients remain nearly constant across the Kondo plateau. This indicates that these coefficients are indeed universal. Two forms that fit over wider ranges of bias are the Lorentzian G(T, V ) = G(T, 0)/(1 + ( WV(T ) )2 ) and the modified quadratic G(T, V ) = G(T, 0)(1 − V2 ), (W (T )2 +Q(T )2 V 2 where W (T ) and Q(T ) are free parameters for each temperature and gate voltage point. The average values of the coefficients across the Kondo plateau were α = 0.12 ± 0.015 and γ = 0.7 ± 0.1 for both fits. The modified quadratic fits the experimental data over the widest bias range (±15µV in the center of the Kondo plateau) but there is little physical basis for using this function. A Lorentzian has been commonly used to fit Kondo peaks in the experimental literature but theoretical work indicates that the 54 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT true peak shape is more complex. The reported error bars correspond to 68% confidence intervals for the extracted scaling exponents and coefficient. They account for statistical errors such as random measurement noise as well as systematic errors from the uncertainty in temperature calibration and from the choice of fitting range in bias and temperature. The error bars for the average exponent and coefficient values across the plateau arise mainly from the systematic errors, which do not average out across the plateau. The temperature values are based on the width of temperature broadened Coulomb Blockade peaks and we assume the temperature error (±0.7 mK) at each temperature point is random. The extracted exponents and coefficients depend slightly on the temperature and bias fit ranges. This dependence is included in the error analysis by examining the variation caused by changing the fit ranges by one data point in each direction. Hence, the error bars reflect the effects of varying the bias fit range by ±13% and the temperature fit range by ±20%. The error due to treating the Kondo peak as a quadratic was discussed earlier. The presence of an offset in fitting the EK form to our data modifies the coefficient values but not the exponent values. As mentioned before, the scaling parameteres G0 and TK are smaller when an offset is included, which results in an overall decrease in the extracted values of α and γ. The coefficients show the same qualitative behavior across the Kondo plateau as seen in fig. 4.6 of the main text, but have average values α = 0.08 ± 0.015 and γ = 0.24 ± 0.07. Since the G0 and TK values extracted by including a temperature independent conductance offset do not accurately reflect behavior in the low temperature limit, this effect is not included in the analysis. To see that low energy transport through a Kondo dot in the Kondo regime is well-described by the universal scaling function given by eq. 4.9, we plot the scaled conductance 1 − G(T, V )/G(T, 0)/αV′ versus (eV /kTK )2 , where αV′ = cT α/(1 + cT ( αγ ( TTK ))2 ), using the average values of α and γ across the Kondo plateau from fig. 4.7. The conductance data across the Kondo plateau for T /TK < 0.6 collapse onto a single universal curve for bias values up to (eV /kTK )2 ≈ 0.5. Because previous experimentally reported measurements of the Kondo peak in spin 1 2 quantum dots did not investigate the low bias power-law regime [14, 16, 22, 4.2. THE NON-EQUILIBRIUM SINGLE CHANNEL KONDO EFFECT (b) ~ G/!V G(e2/h) 0.5 1.5 1.75 (a) 55 1.5 0.4 1 0.3 05 0.5 1.25 0.2 0 1.0 0.1 -20 -10 0 10 V ( V) 20 -2 -1 0 1 ±(eV/kTK)2 2 T/TK Figure 4.7: (a) Conductance as a function of bias for 0 < T /TK < 0.6 for six gate voltages across the Kondo plateau. (b) The scaled conductance versus (eV /kTK )2 using the average values of the extracted scaling coefficients in the middle of the Kondo plateau. The solid line shows the associated universal curve described by eq. 4.8. 24] and measured the full-width at half-maximum (FWHM) of the Kondo peak at a fixed values of TK , a comparison to our results is informative but not precise. By approximating the Kondo peak in ref. [75] as a Lorentzian we can estimate that α ≈ 0.25 and γ ≈ 0.5 in the middle of the Kondo plateau for this experiment. From transport measurements through magnetic impurities coupled to highly asymmetric leads, we extract α ≈ 0.05 and γ ≈ 0.1 in ref. [77] and α ≈ 0.15 and γ ≈ 0.5 in ref. [33] but these experiments probe the equilibrium rather than non-equilibrium spectral function. These values are comparable to our measured values but the wide variation underlines the importance of restricting the fitting range to low energies for extracting meaningful coefficients. Existing theoretical calculations for non-equilibrium transport through a spin 1 2 Kondo quantum dot are based on either the Anderson [74, 78] or Kondo models [71, 68], and focus mainly on determining α. The Anderson model (eq. 1.6) predicts α ≈ 0.15 in both the strong coupling non-equilibrium [74] and equilibrium limits [68]. This indicates that the Kondo conductance we observe decreases with bias more slowly than predicted by the Anderson model calculations. Other theoretical treatments [78, 79, 80] show a greater level of disagreement with our results. 56 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT One possible explanation for the difference between our results and the theoretically predicted values is that the non-equilibrium calculations overestimate how quickly Kondo-processes diminish with increasing bias or that additional non-Kondo transport processes, such as inelastic co-tunneling, add a component to the biasdependent conductance in our measurement. By extracting scaling parameters at different dot (U, ∆) and coupling (Γ) parameters for identical TK and G0 values, the contribution from such additional transport processes could be experimentally investigated. Measurements of non-equilibrium transport through a single-channel spin 1 2 Kondo quantum dot are consistent with a quadratic power-law at low energies, as theoretically predicted for the single-channel Kondo effect. The conductance is well-described by a universal scaling function with two scaling parameters: the Kondo temperature TK and the zero temperature conductance G0 . The scaling coefficients α and γ are constant along the Kondo plateau and generally agree with calculations using the Anderson-model. 4.3 Impurity Quantum Phase Transitions Quantum phase transitions (QPTs) are a class of phase transitions that occur at absolute zero temperature when a parameter other than temperature is varied. Second order (continuous) QPTs are driven by quantum fluctuations of the order parameter, which have properties that are completely different from those of the familiar thermal fluctuations. The inherent zero-temperature nature of the QPT makes it impossible to observe directly. However, in the low-temperature limit, correlation lengths and times diverge near the transition between two groundstates. These long-range correlations influence the behavior of the system at finite temperature: near the quantum critical point (QCP), a distinctive set of excitations can be accessed experimentally. These excitations are collective, so that Fermi-liquid theory fails to describe the physics in the quantum critical region. The behavior of the system as a function of external parameters obeys scaling laws with non-trivial exponents that are determined only by the universality class of the transition and not by the microscopic details. 4.3. IMPURITY QUANTUM PHASE TRANSITIONS 57 We generally think of second-order phase transitions (classical or quantum) as requiring the thermodynamic limit of system size. However, for a special kind of QPT involving a boundary (e.g. an interface or impurity) embedded in a bulk system, only the degrees of freedom belonging to the boundary become critical, and the thermodynamic limit is only required for the bulk part of the system. Boundary phase transitions show the same fascinating quantum critical behavior as bulk transitions. While the entropy at a bulk QCP vanishes at zero temperature, an impurity QCP can have residual entropy: fluctuations are strong enough to preserve some of the local degrees of freedom. The two channel Kondo model A generalization of the system described in the previous section, the two channel Kondo (2CK) system, corresponds to the QCP in a boundary QPT between two distinct single channel Kondo states. The two channel Kondo Hamiltonian: H2CK = J1 σ1 · S + J2 σ2 · S, (4.10) describes a quantum impurity coupled to two reservoirs: J1 , J2 > 0 are the antiferromagnetic interaction between the local spin S and the spins of the reservoir electrons σ1 and σ2 . When J1 = J2 the ground state is an exotic non-Fermi liquid state with an overscreened local moment and a residual entropy at zero temperature. When one channel is more strongly coupled the traditional Kondo screening behavior is recovered. This model has been used to explain the experimentally observed specific heat anomalies in certain heavy fermion materials [26, 27, 28] as well as transport signatures in metallic nano-constrictions [29, 30]. There are several theoretical proposals for the realization of the 2CK effect where the local degeneracy is based on the charge degree of freedom. The earliest proposal for observing the 2CK effect in semiconductor nanostructures [81] involved a large semiconductor quantum dot coupled via single-mode point contacts to a reservoir. At the charge degeneracy points of the dot, strong charge fluctuations are expected to give rise to a 2CK effect [82, 83]: two successive charge states play the role of the 58 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT local two-fold degeneracy, and the spin-up and spin-down electrons of the reservoir form the two independent screening channels. Due to conflicting constraints on the size of the dot this specific proposal may not be experimentally realizable [84]. To overcome this difficulty a single resonant level can be introduced between the large quantum dot and the reservoir. At the charge degeneracy point of the large dot, and in the mixed-valence regime of the small dot, a 2CK effect with a non-Fermi liquid fixed point is expected to occur [85]. Further analysis of the different parameter regimes of this double dot system predicts several exotic effects such as a line of twochannel fixed points, a continuous transition from spin-2CK to charge-2CK effect [86] and a SU(4) Kondo effect with a stable fixed point [87]. The two channel Kondo effect in a double quantum dot A possible implementation of the spin based 2CK model in a quantum dot geometry was proposed by [88] and has been measured in [45]. The schematic representation of this realization is shown in fig. 4.8(a). The localized magnetic impurity is represented by a small quantum dot containing an odd number of electrons. The conduction electrons that screen this local moment belong to two reservoirs, shown in blue and in red in fig 4.8. One of the reservoirs (blue) corresponds to the source and drain leads (“left” and “right” electrons), which, although physically separated, form a single effective reservoir [43]. The second reservoir (red) is a finite electron bath: a much larger quantum dot with fixed electron occupancy. It constitutes a second independent screening channel at low temperature when Coulomb Blockade forbids it from exchanging electrons with the infinite reservoir. The QPT that takes place as a function of the relative couplings of the two channels to the small dot is shown in fig. 4.8(b). For equal coupling, the electrons in the red and the blue reservoirs compete to screen the spin 1 2 electron on the quantum dot system forming the 2CK state. When one channel is more strongly coupled the traditional Kondo screening behavior (1CK) is recovered. Thus the two groundstates on either side of the transition are both the standard Kondo singlet state (left and right regions in the phase diagram in Fig. 4.8(b)), with a different set of electrons participating in the screening of the local moment in each phase. In the quantum 4.3. IMPURITY QUANTUM PHASE TRANSITIONS (b) (a) large quantum dot 59 crossover regime 2CK regime T, V 1CK (large dot) left 1CK (two leads) right 0, 0 J Figure 4.8: (a) Cartoon of a quantum system that realizes the 2CK model. A spin on the small dot d can influence transport from one blue lead to the other. The red electron reservoir formed by a large quantum dot will act as another independent screening channel for the small dot. (b) Phase diagram of the 2CK system, with two 1CK phases on the two sides of the quantum critical region and the associated crossover region between them. The vertical axis denotes any energy (temperature, frequency, bias voltage). critical region (center region in Fig. 4.8(b)) temperature fluctuations mask the channel anisotropy and the long range correlations of the 2CK groundstate dominate the behavior of the system, resulting in non-Fermi liquid scaling laws. For the 2CK model, one can obtain the full scaling function rather than just a power law approximation valid only at low energies. The conductance scaling relations presented below can be used to identify the 2CK quantum critical point in the double quantum dot system of fig. 4.8. Starting from the Anderson Hamiltonian, the expressions for the conductance between the two blue leads as a function of external parameters can be derived [89]. 60 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT The Anderson Hamiltonian for this system is given by H = X † εlkσ lkσ lkσ + † εrkσ rkσ rkσ + kσ kσ + Ec X X c†kσ ckσ + εdσ d†σ dσ X εckσ c†kσ ckσ kσ + Und↑ nd↓ kσ + X kσ † † tkl lkσ dσ + tkr rkσ dσ + tkc c†kσ dσ + h.c. . (4.11) The first three terms represent the electrons with spin σ and momentum k in the † † left and right leads and large dot, respectively. lσk , (lσk ), rσk , (rσk ), and cσk , (c†σk ) are the annihilation (creation) operators of a free electron in state k with spin σ, for the left and right leads and the large dot, respectively. The next three terms account for the the charging energy Ec of the large dot, the quantized energy of the small dot electrons and the charging energy U of the small dot. We assume that the tunneling matrix elements tkr , tkl , tkd which characterize the coupling of the small dot to the two leads or to the large dot are independent of k, and that only one spin-degenerate level exits in the quantum dot. When the tunneling matrix element to one of the two leads is much smaller than to the other and if the coupling to the leads (with the same density of states ν) 2 Γl(r) = πν tl(r) is independent of spin, the conductance through the system is: G(V, T ) = ν G̃0 XZ s=↑,↓ dεf ′ (ε − eV ) Im T σ (ε), (4.12) where T σ (ε) is the scattering T -matrix and G̃0 is a proportionality constant depend- ing on the coupling to the leads Γl,r , which is assumed to be independent of spin. Most two leaded devices exhibit single channel Kondo physics because electrons can move between the leads which effectively form only one screening channel. This channel then competes with the second screening channel formed by the large dot. For the specific expressions for the scattering matrix T from ref. [25] " r # 1 eV πT G(V, T ) = G0 1 − F2CK 2 TK2 πT (4.13) 4.3. IMPURITY QUANTUM PHASE TRANSITIONS 61 The function F2CK is given in [89] and its asymptotes are F2CK (x) ≈ ( c x2 + 1 for x ≪ 1 √ √3 x for x ≫ 1 π (4.14) where c = 0.748336. Using the zero bias conductance G(0, T ) = 1 G 2 0 1− q πT TK2 and the finite bias expression from eq. 4.13 the scaling relation for the conductance of a quantum dot in the 2CK regime can be expressed as: 2 G(0, T ) − G(V, T ) p =Y G0 πT /TK2 |eV | , πT (4.15) with the scaling function Y (x) = F2CK (x) − 1. For more detailed calculations see references [89, 90] An additional note about the single-channel Kondo case The 1CK model can be viewed as the 2CK model with strongly assymmetric coupling to the two channels. Above a characteristic temperature scale T∆ [91] (and Toth, maybe von Delft too.) that depends on how large the asymmetry parameter ∆J = JBLU E − JRED is, temperature obscures the asymmetry and the system exhibits 2CK behavior. At temperatures below T∆ the 2CK system will cross over to regular single channel Kondo behavior. The small dot will be Kondo screened by whichever channel is more strongly coupled. We can use the expression for the conductance in in the limit T, eV ≪ T∆ , |tl | ≪ |tr | or vice-versa, for the scattering matrix given by [25]: G(V, T ) = G0 ( θ(∆J) − sign(∆J) πT T∆ 2 " 2 #) 3 eV 1+ . 2 πT and the zero bias conductance G(0, T ) = G0 (θ(∆J) − sign(∆J) πT T∆ 2 (4.16) ) to obtain the 62 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT scaling relation for the conductance of a quantum dot in the 1CK regime: 3 1 G(0, T ) − G(V, T ) = sign (∆J) 2 G0 2 (πT /T∆ ) eV πT 2 . (4.17) The scaling curves for the 1CK and 2CK implementations of the system in figure fig. 4.8(a) were used to describe the quantum phase transition observed in ref. [45]. 4.4 Tuning to the 2CK Point in a Double Quantum Dot Fig. 4.9 shows an SEM image of the double quantum dot device used to tune across the QPT described in the previous section. The labels for the gates used are indicated in fig. 2.3. The observed Fermi liquid scaling laws for asymmetric coupling of the blue and red reservoirs to the quantum dot as well as the 2CK scaling law in the quantum critical region have been reported in [45]. This section summarizes one procedure that can be followed to tune this device to the 2CK point. The voltage on gate sp controls the number of electrons on the small dot and is used to tune to odd occupancy. The gates c1 and c2 (labeled as such in fig. 2.3) tune the coupling of the small dot to the large dot. The gates sw1 and sw2 tune the coupling of the small dot to the leads. The voltage on gate sw2 is set such that the coupling of the dot to the lower blue lead is negligible in comparison to the coupling to the other lead. As a consequence, the coupling to the blue reservoir is dominated by the coupling controlled by gate voltage sw1. By changing the gate voltages on gates sw1, c1 and c2, the conductance of the small dot in the three different regions of the phase diagram can be measured. Fig. 4.9(c) shows that a difference of 10 mV in c1 gate voltage affects the relative couplings of the two reservoirs to the dot enough to change the enhanced conductance (correspondsing to the formation of the 1CK state with the blue reservoir) into a suppression (corresponding to the formation of the other 1CK state between the quantum dot and the large dot). 4.4. TUNING TO THE 2CK POINT IN A DOUBLE QUANTUM DOT 63 (c) (a) (b) path 2 path 1 path 3 μV) Figure 4.9: (a) SEM image of the quantum dot indicating the finite reservoir in red and the leads in blue. (b) Schematic representation of the current paths for the three lead measurement. (c)The evolution of the conductance through the small dot as a the coupling to the finite reservoir becomes larger than the coupling to the leads. The blue traces showing the enhanced zero bias conductance indicate the Kondo state is formed with the leads. The red traces showing a dip instead of a peak indicate that the conductance through the dot is suppressed by the formation of the Kondo state with the finite reservoir We start by measuring the small quantum dot in a three lead geometry. This is accomplished when little or no voltage is applied to gate n, leaving the large quantum dot open. The three possible current paths in the three lead arrangement are shown in fig. 4.9(b). By measuring the conductance matrix of this system, the relative coupling of the three leads can be determined. This has been explained in detail in [49] and is illustrated in fig. 4.10. The conductance traces show two Kondo valleys and one even valley for VSP > −320 mV and VSP < −260 mV. The two traces in each graph are measured simul- taneously using one lead for the voltage source and the other two for measuring the current. The total current through the dot in each graph is due to parallel transport along the two paths, so we can just sum the conductance along the two paths. We compare the total conductance for each of the three configurations and we see that there is less transport though paths 1 and 3 than there is through paths 1 and 2 or 2 and 3. The fact that the total conductance is smaller when the voltage source is on the lower blue lead where paths 1 and 3 originate, indicates that the coupling of this 64 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT (a) 1.0 (b) path 1 (c) 1.0 path 2 path 2 path 3 path 3 2 2 )h / e( G )h / e( G 2 )h / e( G 0.5 0.5 0.0 -400 -300 V SP 0.0 -400 (mV) 1.0 path 1 -300 V SP 0.5 0.0 -400 (mV) -300 V SP (mV) Figure 4.10: (a) The conductance along path 1 and path 2. The total Kondo conductance close to VSP = −300 mV is > 1e2 /h. (b) The conductance along path 1 and path 3.The total Kondo conductance close to VSP = −300 mV is < 1e2 /h. (c) The conductance along path 2 and path 3.The total Kondo conductance close to VSP = −300 mV is > 1e2 /h lead to the dot is less than the coupling of the other two leads to the dot. To determine the exact ratios of the couplings to the three leads, the conductance in the Kondo valley has to be measured as a function of temperature. At more negative gate voltages, regular Coulomb blockade is seen. The zero temperature Kondo conductance through a two leaded dot is maximal when the dot is equally well coupled to the two leads: G0 = where n = 1 2 4ΓS ΓD e2 sin2 (πndot ) ΓS + ΓD h (4.18) is the occupancy of the dot in the Kondo valley. If the Kondo temper- ature is large, and the couplings are equal, the conductance in the Kondo valley is 2e2 /h. A smaller value of the conductance can be due to asymmetric coupling or to a small Kondo temperature or to both. Several iterations will probably be needed to identify what voltages on gates c1, c2 and sw1 give equal coupling. After identifying the gate voltages for which one of the blue leads is tunnel coupled and the other two leads (one red, one blue) are close to equally coupled and are each able to form the 1CK state with the small dot, the large dot is formed by applying voltage to gate n. Gate n is far enough from the small dot, that only minor retuning of the small dot gate voltages should be needed. In this regime, after carefully accounting 4.4. TUNING TO THE 2CK POINT IN A DOUBLE QUANTUM DOT (a) (b) 40 65 40 2 2 G(e /h) G(e /h) 20 0.6 µV) µV) 20 ( ( 0.4 0.6 0 V DS V DS 0 0.4 -20 -20 0.2 0.2 -40 -40 -300 -280 V SP (mV) -260 -300 -280 V SP -260 (mV) Figure 4.11: Transport through the small dot shows charging peaks caused by the addition of charge to the large dot superimposed on the Kondo resonance for two different voltages on gates (c1, c2). (a) The enhanced zero bias conductance in the region −300 mV < Vsp < −280 mV shows the Kondo resonance between the small dot and the leads. (b) The suppessed zero bias conductance in the region −300 mV < Vs p < −280 mV shows the Kondo resonance between the small dot and the large dot. for all gate capacitive effects, the small dot zero bias conductance should be very sensitive to the voltage on the gates that control the coupling between the two dots. Fig. 4.11 shows finite bias transport measurements of the small dot conductance for c1= −340 mV (left) and c1= −320 mV (right) with the large dot formed. The gate voltage range spans approximately one odd and two even valleys. As a function of VSP the number of electrons on the small dot changes by 3. However, the gate sp is capacitively coupled to the large dot as well. The vertical lines are due to charging effects on the large dot: every time an electron is added to the large dot du to the change in VSP , the effective voltage felt by the small dot changes discontinuously. Over the swept voltage range the number of electrons on the large dot changes by 8. Fig. 4.11(a) corresponds to the more negative voltage on gate c1 and shows a zero bias enhancement in the gate voltage region around −290 mV. In the same region, fig. 4.11(b) which corresponds to the large dot being better coupled to the small dot compared to (a) shows a dip where the peak at zero bias used to be. This is how the two single channel Kondo regions of the phase diagram can be identified. By repeating these types of sweeps we narrow down the values for the appropriate 66 CHAPTER 4. QUANTUM DOTS: THE KONDO EFFECT gate voltages on gates c1, c2 and sw1 (or sw2, depending on which one of the two leads has been closed off) to couple the small dot state equally to the two reservoirs and therefore form the 2CK state. Further tuning to reach the QCP is done using gate bp, which controls the number of electrons on the large dot and thus the energy difference between the small dot state and the large dot levels. If the gates c1, c2 and sw1 have been carefully tuned, it is possible to observe the evolution of the Kondo enhancement, through the critical point to the suppression of the Kondo state with the leads as a function of the voltage on gate bp and measure the scaling behavior in these three regimes [45]. Chapter 5 Quantum Dots: Perfectly Transmitting QPCs The low electron density of the 2DEG and the confined spatial dimensions of quantum dots make them particularly well suited for studying electron interference effects. As a result, fluctuations of the conductance as a function of magnetic field or bias can be observed for both closed and open dots. In the case of a closed dot, connected to leads via tunneling point contacts (GQPC ≪ 2 e2 /h, N ≪ 1), the conductance is suppressed by Coulomb Blockade and the effect of interference is to cause fluctuations of the Coulomb blockade peak heights. These fluctuations are expected to be more pronounced at low temperatures because the electron-electron interaction induced dephasing is expected to vanish at T < ∆ for a ballistic system [92] or to decrease as T −2 for a disordered quantum dot [93]. When many modes are open in the QPCs (GQPC ≫ 2 e2 /h, N ≫ 1) there is no Coulomb blockade [94, 95, 96] and the conductance is dominated by the universal conductance fluctuations (UCFs) [97, 98]. This open regime is well described by the semiclassical approximation and by random matrix theory (RMT) (for a review see [99]). The effect of dephasing on these fluctuations can be modeled as an extra phase randomizing lead that connects to the dot (the fictitious voltage probe model) [100]. This extra lead allows electrons to escape and then be re-injected with 67 68 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS a random phase acquired. Most experiments have concentrated on the low N regime as the time the electron spends on the dot is diminished at large QPC openings and an accurate determination of the amount of dephasing occurring in the dot becomes difficult. The theories that describe the closed and the open regime are not well applicable in this intermediate regime and no explicit theories that describe two-leaded quantum dots with one open mode in each QPC (N ≈ 1) exist. As a consequence, theories that describe the two limiting cases have been adapted to this intermediate regime, with varying degree of success. RMT results without explicit Coulomb interactions [99] have described experi- ments that investigated the conductance distribution functions and dephasing times very well [97, 101]. However, the temperature dependence of the dephasing time extracted from the dot conductance in this regime showed puzzling features: it did not follow a T −2 law, as naively expected from Fermi liquid theory, and an apparent saturation at low temperatures was reported [98, 102, 103, 104, 105, 106, 107]. The absence of Coulomb Blockade in these systems has been predicted for the case of strong dephasing [94, 95, 96]. In the case of a phase coherent quantum dot, the presence of Coulomb Blockade was predicted for this regime if one of the QPCs is in the tunneling regime while the other is perfectly transmitting [108]. There is no theory that describes a quantum dot with two perfectly transmitting QPCs. Experiments in one leaded dots have confirmed both theoretical predictions. As the conductance of one QPC is increased from GQPC < 2e2 /h to GQPC = 2e2 /h and above, the charging energy is reduced [109, 110] and capacitance measurement indicate that Coulomb Blockade oscillations decrease in amplitude [111] and become indistinguishable from the noise [112]. A type of Coulomb Blockade that is the result of interference and is referred to as Mesoscopic Coulomb Blockade (MCB) was observed in a quantum dot with one perfectly transmitting lead [113]. Experiments in two-leaded dots observed no Coulomb Blockade [114] or only a weak conductance oscillation with gate voltage [115, 116, 117] that matched the Coulomb blockade peak spacing in the tunneling regime but did not investigate the charging energy or confirm that charge is indeed quantized. 5.1. OPEN QUANTUM DOTS 69 I will start this chapter with a brief description of the RMT results from the open regime that have been adapted to study the dephasing time in a ballistic quantum dot with two fully-transmitting QPCs. I will then explain how we determine that the quantum point contacts are open to N = 1 and present the magnetic field, bias and temperature dependence of the quantum dot conductance as well as the detection of the quantum dot charge using the response of the adjacent small quantum dot conductance. 5.1 Open Quantum Dots In the case of a disordered conductor, when the mean free path is smaller than the device size (le < L), the interference of the different electron trajectories through the system gives rise to random but reproducible conductance fluctuations as a function of parameters such as magnetic field, gate voltage or electron energy. The statistics of these fluctuations are universal: they are determined only by the symmetries of the system and scaling parameters and do not depend on material properties [118]. Similar universal conductance fluctuations same are present in open ballistic quantum dots (le > L) as long as the motion of the electrons inside the quantum dot is chaotic. The physical origin of these fluctuations is the same as in disordered conductors: the quantum interference of different classical paths that the electron can take, scattering elastically off the disorder potential in one case, or the confinement potential in the other. These fluctuations are called universal conductance fluctuations [119] and their statistical moments can be used to extract the dephasing time in these systems [120]. At zero magnetic field the quantum correction to the probability that an electrons returns to its original position at a given time leads to weak localization (WL) of the electrons at the impurities in one case or inside the dot in the other. This constructive interference of time reversed paths is manifested as a suppression of the conductance at zero magnetic field compared to the finite magnetic field value. The number of electrons inside quantum dots are usually large enough that a statistical description of the system is possible. Several methods whose regimes of 70 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS validity depend on whether the quantum dot is open or closed have been very successful in explaining equilibrium transport features [121]. The semiclassical description and RMT are two of the approaches that describe diffusive as well as chaotic ballistic quantum dots. In the semiclassical picture we can think of electrons as moving along classical trajectories. By summing over the classical trajectories weighted correctly, transport characteristics of the quantum system can be predicted. Two conditions have to be fulfilled for the semiclassical results to be valid: a large number of modes that couple the quantum dot to its leads (N → ∞) is required and the energies have to be larger than the single particle energy level spacing ∆ of the quantum dot. Semiclassical results cannot be used if N < 3 [99]. The quantum fluctuations in disordered conductors and chaotic ballistic systems, in the limit of a large number of open modes in the QPC can also be described using RMT [122]. This technique was initially introduced to describe the statistics of eigenfunctions and eigenvalues of many-body quantum systems and was successfully applied to atomic nuclei. Although quantum dots with single mode QPCs have been referred to as open, results derived in the limit N → ∞ have to be used with particular care. As described below, some of the results from RMT and from the semiclassical description can be modified to describe the N = 1 regime. In the RMT description, the Hamiltonian of the system is chosen to belong to a Gaussian ensemble of random Hamiltonians and a similar approach can be applied for the scattering matrix that describes transport through mesoscopic systems [121]. This picture is valid when the only important features of the quantum system are its symmetries. Depending on what kind of symmetry describes the system, a different ensemble of Hamiltonians has to be used to obtain statistics. If the system is invariant under time reversal the Hamiltonian has to be a real symmetric matrix and the ensemble is called orthogonal. If time reversal symmetry is broken, the Hamiltonian has to be a complex Hermitian matrix and the ensemble is called unitary. This is the case when a magnetic field is present. A third ensemble is the symplectic ensemble and it describes systems with strong spin-orbit interactions (broken rotational symmetry). RMT is applicable in the regime E < ET h [99]. Its predictions coincide with 5.1. OPEN QUANTUM DOTS 71 the semiclassical results for energies E > ∆ but unlike the semi-classical results, the RMT predictions are also valid for E ≈ ∆. A long as τd ≫ τcross they can be used for diffusive quantum dots as well. The conductance distribution functions and statistical moments such as average conductance and variance can be calculated for the different ensembles. The lineshape of the average conductance as a function of magnetic field is found to be approximated by a Lorentzian: hG(B)i = hGiB6=0 − A 1 + (2B/Bc )2 (5.1) where hGiB6=0 is the average conductance at finite field, and A and Bc are the depth and width of the weak localization dip. In the semiclassical picture this results is actually exact. If the quantum dot is not chaotic, the lineshape is expected to be more “V” shaped. The conductance fluctuations in a chaotic dot as a function of magnetic fields are described by a correlator whose semiclassical expression is given by: cG (∆B) = hG(B + δB)G(B)i − hG(B)i2 ∝ 1+ 1 ∆B 2Bc (5.2) 2 RMT calculations confirm this result in the limit T → 0 [123]. The effect of dephasing on the average conductance and on the variance of the conductance of a chaotic quantum dot for the case of one or multiple modes in the QPCs can be accounted for using a spatially distributed voltage probe model [124]. For single mode leads, the analytic expression that connects the size of the weak localization correction of the average conductance to the dimensionless dephasing rate γφ (this is the dephasing rate normalized by the escape rate per lead) can be approximated by [104]: δg = 1 e2 /h 2N + 1 + γφ (where N is the number of open spin degenerate modes in the leads, γφ = (5.3) 2π~ ∆τφ is the dimensionless dephasing rate). The average conductance is only implicitly affected by temperature through the dependence of the dephasing time. 72 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS The variance of the conductance is affected by both dephasing and thermal averaging. If the temperature is larger than the total level brodening (kB T > ∆(1 + γφ /2)), it can be well approximated by the expression [101, 120]: q q 45 ( 16 + 13 γφ )−2 for β = 1 ∆(1 + γφ /2) Var(G) = (√3 + γφ )−2 6kB T for β = 2 (5.4) A third method for extracting the dephasing time is based on the conductance fluctuations at high magnetic field where the cyclotron radius is smaller than the size of the quantum dot. In this case, the electrons are confined to the edges of the quantum dot and the correlation in magnetic field can be used to determine the dephasing time. It is also possible to extract the dephasing time from the weak localization dip width Bc or from the power spectrum of the fluctuations versus magnetic field. Extracting the dephasing time in quantum dots as a function of temperature has proven to be rather difficult, despite the many methods available to connect transport quantities to dephasing. Early experiments on quantum dots [102, 98] observed a saturation of the dephasing time extracted from the dot conductance at low temperatures. This saturation was attributed to an extraction method that failed at low temperatures due to the breakdown of the semiclassical model [98] and to the discreteness of the dot spectrum at low temperatures [102] More recent experiments that used RMT calculations to interpret their data [104, 105, 106, 107] still observed a saturation. The experiment in ref. [104] excluded electron heating effects as a possible cause for the observed saturation. Dephasing processes that occur in the constrictions connecting the dot to its leads [105, 107] were proposed as the source of the saturation. As a result, these experiments also noted a correlation between the temperature at which the saturation occurred and the temperature at which the coherence time became equal to the dwell time. The only theoretical prediction for the temperature dependence of the dephasing time in the 0D regime was given in ref. [93]. For a disordered closed quantum dot the expected temperature dependence is ∝ T −2 . The same power law has been predicted for mesoscopic rings [125]. In general, two classes of scattering processes determine the 5.2. THE QUANTUM DOT CONDUCTANCE AT N = 1 73 behavior of the dephasing time: large energy transfer scattering events with E ≥ T that lead to a square dependence on temperature and small energy exchange processes with E ≪ T which result in a linear dependence on temperature [14]. Because at low temperature the Pauli exclusion principle prevents scattering processes with E ≪ T , the dominant contribution to dephasing is from scattering processes with E ≈ T . 5.2 The Quantum Dot Conductance at N = 1 The large quantum dot in fig. 2.3 with area 2.6µm2 can be used to study interference √ and decoherence in the open regime. Because le ≫ A the quantum dot is in the ballistic regime. The coupling of the electrons in the dot to the electrons in the leads is controlled via the voltages on gates bw1, bw2 and n. A different set of gates affects the shape of the quantum dot: c1, c2 and bp are used to gather statistics of the conductance which offer information about the amount of dephasing present in this system. In the measured temperature regime (13 mK to 1 K) the dominant processes that causes dephasing are electron-electron scattering events. The QPC Plateau Fig. 5.1 shows how we determine the QPC transmission. In a separate cool-down (without positive bias) of the device, when voltage is applied only to the gates bw1, n and bw2, the quantum dot is not formed and clear conductance plateaus quantized at integer multiples of 2e2 /h are visible at 13mK and at 600 mK. The fact that the plateaus are not broadened by this increase in temperature indicates that the energy needed to reach the next QPC subband (and open another transmission mode) is larger than ≈ 50 µeV It is more complicated to identify the gate voltage at which the QPCs are open to one spin-degenerate mode (N = 1 and GQP C1,2 = 2e2 /h) when the dot is formed. In the absence of interference, the dot conductance is the series conductance of the two QPCs and as a result a plateau at G = 1e2 /h will appear as the voltages on gates bw1 and bw2 are swept. Interference effects inside the dot can obscure this plateau at low temperatures and zero magnetic field. Fig. 5.1(b) shows the conductance through 74 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS (b) (a) 8 13 mK 600 mK G (e 2/h) 6 4 2 0 -800 -600 -400 V bw1(mV) Figure 5.1: (a) Quantized conductance plateaus of QPC1 at 13 mK and 600 mK (the 600 mK data is shifted horizontally for clarity). (b) The 1 e2 /h conductance plateau of the quantum dot at T = 960 mK and B = 22 mT. The black circle, square and triangle mark the three QPC voltage settings used in the measurements. -3 -3 x10 (a) dG/d(V -4 ) bw1 0 x10 4 (b) -400 dG/d(V ) bw1 -10 -5 V (mV) 0 5 10 -400 V V 2wb 2wb )Vm( )Vm( -500 -500 -400 -300 V bw1 (mV) -400 -300 bw1 Figure 5.2: Derivative of the plateau with respect to the gate voltage on QPC1 (a) and QPC2 (b). The dashed lines indicate the border between high and low values of the derivative. The (Vbw1, Vbw2) coordinates of the plateau center are marked with a black circle in (a) and (b), respectively. 5.2. THE QUANTUM DOT CONDUCTANCE AT N = 1 75 the dot with increasing QPC conductance at T = 960 mK and B = 22 mT. A plateau at 1e2 /h in the dot conductance corresponding to to the 2 e2 /h plateau in the conductance of each QPC can be seen. It is difficult to consistently identify the middle of the plateau directly from this 2D conductance map. Instead we take the derivative (shown in fig 5.2) of the conductance in fig. 5.1(b) with respect to Vbw1 (fig. 5.2(a)) and Vbw2 (fig. 5.2(b)) and identify the transition between regions with small and large values of the conductance derivative. The region with a low value for the conductance derivative corresponds to a low slope in conductance. The center of this region in both graphs is marked by the black dot in fig 5.2. The corresponding coordinates are indicated by a black dot in fig 5.1. The two other markers, (black square and triangle) identify adjacent QPC voltage settings that should also be be very close to perfect QPC transmission. From here on, unless otherwise noted, the data shown is taken with the QPCs tuned to one of the three indicated settings. How closely they correspond to perfect transmission will be determined via a second method that is based on the dot conductance averaged over different dot shapes. Universal Conductance Fluctuations and Coulomb Blockade The conductance through the dot shows large aperiodic variations in G on the scale of tens of mV in gate voltage around e2 /h, also known as UCFs, as a function of magnetic field and gate voltage. At zero temperature, the size of the fluctuations should be 1e2 /h. The magnetoconductance for a given shape of the dot is shown in fig. 5.3a at 15 mK and at 720 mK. At a fixed magnetic field, changing the shape of the dot via the gate voltage c2 also leads to fluctuation at low temperatures (80 mK) as seen in fig. 5.3b. In comparison, the fluctuations at higher temperatures are drastically reduced by decoherence and thermal broadening. At the lowest temperatures we see strong periodic oscillations with gate voltage tuning, superimposed on the UCFs. This is illustrated in fig. 5.4(a). The periodic oscillation is easily distinguishable from the aperiodic UCFs due to the very different scale of their variation.Finite bias measurements show a suppression of the conductance around zero bias, reminiscent of Coulomb blockade diamonds, is associated with 76 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS (a) (b) 2.0 720 mK 80 mK 1.2 Gdot (e /h) 2 2 Gdot (e /h) 720 mK 15 mK 1.0 1.0 0.8 0.0 10 20 B (mT) -700 -600 Vc2 (mV) Figure 5.3: Dot conductance as a function magnetic field (a) and gate voltage (b) for GQPC1,2 = 2 e2 /h shows universal conductance fluctuations around 1 e2 /h at low temperatures (blue line). The magnitude of the UCFs is decreased at high temperatures (red line). the oscillations in gate voltage (fig.5.4(b)). To establish that this periodic oscillation is indeed Coulomb blockade, we measure the Coulomb Blockade peak spacing when the QPCs are in the tunneling regime in fig 5.5(a). This spacing ∆Vc2 = 1.5 mV coincides with the period of the conductance oscillations at at N = 1. A zoom-in of the oscillation in the open regime is shown for comparison in fig 5.5(b). We also follow the evolution of the Coulomb diamonds from the tunneling regime to above the middle of the plateau in fig 5.5(c) The voltage on gate n affects the QPC conductances and changes the number of electrons on the dot. For Vn . −370 mV neither QPC is fully transmitting and we see clear Coulomb diamonds with a charging energy of ≈ 115 µeV. As Vn is made less negative, the conductance of the QPCs increases and the effective capacitance of the dot increases. This causes U = e2 C to be renormalized [109, 110]. We observe in fig 5.5 (c) that the vertical size of the diamonds shrinks with increasing QPC conductance, but does not vanish even at Vn ≈ −315 mV where the QPCs are fully transmitting. These diamonds are superimposed on larger UCFs which form a Fabry-Perot pattern in gate voltage and bias [126]. To determine the size of the renormalized charging energy, the Fabry Perot bias 5.2. THE QUANTUM DOT CONDUCTANCE AT N = 1 77 1.0 2 Gdot (e /h) (a) 0.5 -700 -650 -600 V c2 (mV) Vds (μ V) (b) d I/d Vds 2 (e / h) 20 0.8 0 0.6 -20 0.4 -625 -620 Vc2 (mV) Figure 5.4: (a) Dot conductance at 13 mK and B = 0 shows both UCFs and Coulomb blockade oscillations with gate voltage. (b) Coulomb blockade diamonds with a small charging energy U ∗ = 16µeV for the QPCs at N = 1 (dashed white lines are guides to the eye). CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS (a) (b) 0.4 0.2 0.0 1.0 2 2 Gdot (e /h) 0.6 Gdot (e /h) 78 -444 -442 -440 0.8 0.6 -438 -452 -450 -448 -446 Vc2 (mV) Vc2 (mV) (c) d I /dVds 40 2 Vds (μV) (e / h) 1.0 0 0.5 -40 0.0 -380 -360 -340 -320 -300 Vn (mV) Figure 5.5: (a) The Coulomb blockade peak spacing in gate voltage when the QPCs are in the tunneling regime. (b) The period of the conductance oscillation when the QPCs are at N = 1 as a function of the same gate voltage as in (a). (c) Conductance as a function of Vds and Vn at B = 0 and T = 13 mK shows the transition between Coulomb blockade in the closed regime to a Fabry-Perot pattern in the open regime. 5.2. THE QUANTUM DOT CONDUCTANCE AT N = 1 0.5 -40 d I /dVds (e 2/h ) 0 0.1 0 0.05 0.00 -40 Δ d I /dVds (e 2/h ) 40 1.0 Vds (μ V ) 0.15 (b) 40 Vds ( μV ) (a) 79 -0.05 -340 -320 V ( μV) -300 -340 -320 V ( μV) -300 Figure 5.6: (a) The Fabry-Perot pattern of the bias and gate voltage dependence of the UCFs for the QPCs at N = 1 obtained by averaging over the period of the Coulomb diamonds. (the original data in fig. 5.5) (c) By subtracting the FabryPerot from the original data, the Coulomb diamond component of the finite bias measurement (dashed white lines are guides to the eye) becomes apparent. The renormalized charging energy is U ∗ = 16 mV. dependence has to be subtracted. Fig. 5.6(a) shows the broad underlying Fabry Perot pattern that is obtained when the conductance is averaged over the period of the Coulomb diamonds, ≈ 3 mV in gate voltage. When this background is subtracted from the raw data, the component corresponding to the Coulomb blockade oscillation is isolated and a renormalized charging energy can be extracted from fig. 5.6b: U ∗ ≈ 16 µeV at Vn = −315 mV. The corresponding periodicity in gate voltage as well as the smooth evolution of the Coulomb diamonds from the tunneling regime to the open regime suggest that we observe Coulomb blockade oscillations in this quantum dot at low temperatures when the QPCs are open to allow one spin-degenerate mode to pass though. The presence of Coulomb Blockade can be due to two factors: finite reflection of the QPCs or coherent effects. By investigating the behavior of the average conductance though the quantum dot as a function of temperature we can determine the amount of coherence that is present as well as whether the QPCs are indeed perfectly transmitting. The Ensemble Average and Variance To determine the conductance average, we have to change the shape of the dot controlled by the voltage on gates c1 and c2. Fig. 5.7 shows the conductance through 80 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS 1.0 ρG(ΔVc2) B= 0 mT B= 30 mT 0.5 0.0 -100 -50 0 50 100 Vc2 (mV) Figure 5.7: (a) Dot conductance at 720 mK and 22 mT as a function of VS1 and VS2 . The black dots are spaced by 21 mV in gate voltage apart and show the 196 points used for averaging. (b) The conductance correlation function in gate voltage c2 at 13 mK. The rapid decrease of the correlation indicates that conductance measurements spaced more than 10 mV apart are independent. the dot for a 300 mV change in each c1 and c2 voltage at high temperatures and finite magnetic field where the average conductance is 1e2 /h and small UCFs are visible. To pick a subset of independent shapes from this range, we investigate the low temperature correlation function. An example of the correlation along c2 is shown in fig. 5.7(b) for the lowest temperatures. The width of the approximately Lorentzian correlation indicates that a change of ∆Vc1 , ∆Vc2 > 10mV is needed to modify the shape of the dot to the extent that a new set of trajectories determines conductance. At higher temperatures the correlation length will be longer because thermal averaging will mix the trajectories more. Thus, we pick gate voltage that are spaced 21 mV apart in c1 and c2 as indicated by the black dots superimposed on the conductance map in Fig. 5.7 (a). The chosen gate voltages have to form an ensemble of independent and identically distributed dot shapes. As a consequence, the area of the dot has to remain constant and the gate voltage has to only affect the shape. Otherwise, it is not a true parametric fluctuation. A gate voltage that affects the area has a similar effect to energy and acts as an intrinsic parameter giving rise to slightly different fluctuations. We determine the area of the dot for the extreme values of c1 and c2 voltage from the magnetic 5.2. THE QUANTUM DOT CONDUCTANCE AT N = 1 81 field dependence of the dot conductance in the regime where the electron trajectories are skipping around the edge of the dot. The Fourier spectrum of the conductance at high magnetic field shows that certain oscillation frequencies, those that correspond to the enclosed area, predominate. They can be used to determine that over the shape gate voltages used the area of the dot changes by less than ±5% of 2.6 µm2 . An additional complication is introduced by the capacitive coupling of all the gate to the QPC conductance. Although the gates c1 and c2 are far from the QPCs, a 300 mV change in gate voltage corresponds to an effective detuning of the QPC by 10mV in bw1 or bw2 voltage. This is not enough to move the quantum dot off the plateau, but it is enough to decrease the average conductance. As such, we compensate for the effect on the QPCs of changing c1 and c2 by simultaneously trimming the voltages on bw1 and bw2 to keep the quantum dot in the middle of the plateau. We identify the middle of the plateau for five voltage combinations on c1 and c2 ((−500, −500), (−500, −800), (−650, −650), (−800, −500), (−800, −800) mV) and use a linear interpolation to identify the correct bw1, bw2 voltage values to remain at N = 1 for the intermediate values in c1 and c2 voltages . The conductance as a function of magnetic field, averaged over the ensemble of 196 dots is shown in fig. 5.8(a). The dip in the average conductance at zero magnetic field δg is the signature of coherent backscattering and is due to weak localization. Its width is the field scale necessary to break time-reversal symmetry, which at zero temperature corresponds to the magnetic field needed to thread one flux quantum through the dot: BΦ = Φ0 /ADOT = 1.6 mT. We extract δg and as a function of temperature by fitting a Lorentzian to the curves. hG(B)i = hGiB6=0 − δg 1 + (2B/Bc )2 (5.5) where the fitting parameters hGiB6=0 ,δg = ∆hGiB6=0 − hGiB=0 and Bc are the average conductance at finite field, the depth and width of the weak localization dip, respectively. From the three temperature curves displayed, we see that the dip has a strong 82 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS temperature dependence shown in fig. 5.8(b). This temperature dependence is entirely due to the changing coherence time. The size of the dip is expected to reach 1 3 e2 /h at T = 0. The continued increase of the conductance difference at the lowest temperatures indicate that the coherence in the system also continues to increase. To determine the coherence time using eq. 5.3 we have to determine the area of the dot and the reflection coefficient. We determine the area of the dot from the higher magnetic field oscillations of the conductance. We expect the reflection coefficient to be r ≈ 0 as the QPCs have been tuned to N = 1. However, even at the optimal QPC settings there may still be a small reflection coefficient in the QPCs. The effect of the reflection coefficient on the dot conductance can be observed in the conductance at finite magnetic field where weak localization is absent. To ensure that our results are not affected by any small imperfections in the QPCs we measure the ensemble conductance at three different QPC settings on the plateau. To determine the reflection coefficient from the temperature dependence of the finite magnetic field average ∆hGiβ=2 we use the prediction from ref. [95] for the case of a phase coherent dot with 4N ≫ 1. We find the difference: ∆hGiβ=2 = hG(T )iB6=0 − hG(T0 )iB6=0 (5.6) where T0 is the highest measured temperature point and use ∆hGiβ=2 = r2 T ln 2 T0 (5.7) to extract an overall reflection coefficient. In this equation the reflection coefficients r 2 of the two QPCs are assumed to be equal and are defined by GQPC = 2e2 /h (1−r 2 ). The solid black line in fig. 5.8(c) shows the results of fitting the data to eq. 5.7. From the fit we obtain r 2 ≈ 2% for QPC setting A (triangle) and B (circle) and r 2 ≈ 1% for QPC setting C (square marker). Fig. 5.8(c) shows that there is a very small temperature dependence of the dot conductance, for all three datasets corresponding to the three different locations on 5.2. THE QUANTUM DOT CONDUCTANCE AT N = 1 83 (a) 2 <G> (e /h) 1.0 935mK 310mK 36mK 0.8 0.6 0 10 B (mT) (b) 20 (c) 0 ∆<G>β=2 (e /h) 0.2 2 2 ∆<G>β=1 (e /h) 0.3 0.1 0.0 -20 point A point B point C -3 2 3 4 5 6 2 100 T(mK) 3 4 5 6 -40x10 2 10 3 4 5 6 2 100 T(mK) 3 4 5 6 1000 Figure 5.8: (a) The dot conductance (QPC setting C) averaged over 196 different dot shapes as a function of magnetic field at three different temperatures. The solid lines are the Lorentzian fit to the data. (b) The size of the dip at zero magnetic field as a function of temperature. (c) The difference between the finite field average conductance and the highest temperature average conductance value as a function of temperature. The solid black line is a fit to the data (QPC setting A) used to extract the QPC reflection coefficient as described in the text. Each marker indicates one of the three measured QPC settings. 84 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS the QPC plateau. This indicates that indeed a small residual reflection coefficient is still present in our QPCs. Because the reflection coefficients are on the order of 2% or less, effects that are higher order in r 2 should be suppressed in the average conductance. The variance of the conductance should be more sensitive to a non-zero reflection coefficient. The magnetic field dependence of the conductance variance for three different temperature values is illustrated fig. 5.9(a). The variance depends on both temperature and dephasing. The effect of temperature can be isolated from the variance according to eq. 5.4 because the effective level-broadening ∆′ = ∆(1+γφ/2) of our system is smaller than 0.6 kB T for the entire temperature range. We use the dephasing times determined from the average conductance (as shown in the following section) to calculate the corresponding variance and compare to the measured variance. The ratio of the zero magnetic field variance to the finite field value is independent of temperature and is expected to increase with increasing dephasing. In fig. 5.9(b) we observe a behavior that is similar to that observed in previous experiments [101] where the measured ratios can be up to a factor of two larger or smaller than the ratio expected from the dephasing rate corresponding to the weak localization signal. Fig. 5.9(c) shows the temperature dependence of the zero and finite magnetic field conductance variance as well as the calculated variances based on eq. 5.4 for the dephasing rates extracted from the weak localization correction (red and blue lines). They follow the same temperature dependence, although a factor of 2 difference is also observed, most of which is accounted for by the error bars. The error bars have been determined from the statistical error of the ensemble in the case of the variance. The calculated variances also have an error stemming from the Lorentzian fit error as well as from the statistical error. An important source of error in these kinds of electrical measurements is that the temperature of the electrons is not measured directly, but using a nearby calibrated thermometer to indicate the corresponding electron temperature. Even if at higher temperatures the change in thermometer temperature corresponds to the change in electron temperature, at low temperatures it becomes difficult for electrons to cool (less phonons to dissipate energy) and the electron temperature may saturate even 5.2. THE QUANTUM DOT CONDUCTANCE AT N = 1 85 (a) 960 mK 310 mK 121 mK -2 4 2 VarG (e /h ) 2x10 1 0 0 (b) 10 B (mT) (c) 4 -2 10 3 4 2 VarG (e /h ) VarGβ=1/VarGβ=2 20 -3 VarG (β =1) VarG β =1 (WL) VarG ( β =2) VarG (β =2) (WL) 10 2 -4 10 5 6 2 1 3 4 5 6 γφ 2 10 3 4 5 3 4 5 6 7 8 2 100 T (mK) 3 4 5 6 7 8 1000 Figure 5.9: (a) The variance of the conductance (at QPC setting C) of the ensemble as a function of magnetic field for three different temperatures. (b) The ratio of the zero magnetic field and finite magnetic field variance as a function of the dimensionless dephasing rate. The solid line is the calculated ratio based to the dephasing times extracted from the average conductance. (c) The measured conductance variance as a function of temperature. The solid lines are the calculated variance based on the dephasing time extracted from the average conductance. though the thermometer temperature continues to decrease. Due to its direct relation to the electron temperature, the variance and its continued increase with decreasing temperature shown in fig. 5.9(c) indicates that potential electron heating effects are small. 86 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS 5.3 The Dephasing Time in a Quantum Dot at N = 1 The extraction method of τφ based on eq. 5.3 is very sensitive to the exact tuning of the QPCs [127]. For large dephasing, the presence of a small reflection coefficient does not significantly affect the accuracy of its extraction from eq. 5.3, but for dephasing rates of the order of the escape rate, the reflection coefficient has to be taken into account [127]. To ensure that we have accounted in a consistent manner for the small deviations from perfect transmission of the QPCs, we measure the ensemble conductance at three different QPC settings (black circle, square and triangle in Fig. 5.1(b)) and extract the dephasing time from δg using an analytic equation that includes the effects of a reflection coefficient (r 2 = 2% for QPC settings A and B and 1% for QPC setting C) to first order [private comm. P. Brouwer]. By carefully tuning the QPC to be as close as possible to perfect transmission and by using an extraction method that accounts for the remaining imperfection we extract a dephasing time that does not saturate as shown in fig. 5.10(a) and thus differs from previous experimental results [104, 107] in its low temperature behavior. Th error bars account for the finite size of the ensemble, for the fitting error and for a 5% error in determining the dwell time, stemming from the error in the area of the dot and therefore ∆. The power law we observe has a large contribution from a dephasing mechanism that is linear in temperature and a small addition from a T −2 power law. This does not match the theoretical expectation of a T −2 power law for a 0D system [93, 125]: ~ 32∆ 9 kT = τφ π 4 ET h (5.8) Since there is no exact expression for the dephasing time in a 0D ballistic system (other than the Fermi liquid prediction) and eq. 5.8 is for a diffusive closed quantum dot , we compare to the 2D case as well. The 2D behavior in the disordered case is dominated by a small energy transfer between electrons which results in a dephasing 5.3. THE DEPHASING TIME IN A QUANTUM DOT AT N = 1 (a) (b) 6 5 3 point A point B point C 4 3 2 -9 2 10 -9 9 8 7 6 5 9 8 7 6 4 τφ(s) τφ (s) 10 87 5 3 4 2 3 -10 2 10 -10 10 9 8 7 6 10 9 8 7 6 point A point B point C WL fit 5 4 2 3 4 5 6 100 T (mK) 2 3 3 4 5 6 1000 10 2 3 4 5 6 2 100 T (mK) 3 4 5 6 1000 Figure 5.10: (a) The dephasing time as a function of electron temperature extracted from the B=0 conductance dip for the three different QPC settings. The red line is a fit of the combined datasets discussed in the text. (b) The dephasing time extracted from the conductance variance for the three different QPC settings as a function of electron temperature. The red line is a fit to the data for QPC setting B from 1 K to 60 mK (= TCB ). The dashed black line is the fit from (a). 88 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS time inversely proportional to temperature: −1 τphi = πlelastic k B T λF ln 2π~ lelastic λF (5.9) where λF is the Fermi wavelength and lelastic is the mean free path. For ballistic transport in 2D, Fermi liquid physics [128] is expected to determine the behavior of the dephasing time which is then determined by the Fermi energy of the electrons EF and temperature [129]: −1 τphi = π (kB T )2 EF ln 4 ~EF kB T (5.10) We fit the data to a combination of these two laws τφ−1 = aT + bT 2 . For the parameters of our 2DEG we expect a transition between these two regimes around 100 mK, which is the temperature at which τthermal = τelastic . The black line in fig. 5.10(c) is the best fit to the three combined data sets. The only free parameter in the fit is the mean free path that together with the 2DEG density determines coefficient a = 1.2 × 1010 1 . s K Coefficient b is fixed by the 2DEG density to be 5 × 109 1 . s K2 This power law covers the entire measured temperature range and it is consistent with the behavior observed in the high temperature region of previous experiments [103, 101], but predicts parameters that are different from the 2DEG parameters. The best fit value for the mean free path in this device is 268 ± 8 nm, which is far smaller than the 2DEG mean free path of 15 µm but in agreement with the value extracted from measurements of quantum dots of different sizes (0.4 − 4 µm2 ) in the experiment in ref. [103]. We can also extract the dephasing time from the variance of the conductance. We use the finite temperature variance, averaged over seven magnetic fields in the 15 mT to 25 mT. From eq. 5.4 we find the dephasing time values shown in fig. 5.10(b). The temperature dependence from 1 K to 80 mK is similar to the temperature dependence of the dephasing times extracted using the average conductance method (dashed black line in fig. 5.10(c)) and the fit to the dephasing time extracted from the variance (red line in fig. 5.10(b)) yields a mean free path of lelastic = 500 ± 70 nm. The equivalence of the dephasing time extracted from the weak localization signal and the dephsing time extracted form the UCF variance has been experimentally observed in 1D and 5.3. THE DEPHASING TIME IN A QUANTUM DOT AT N = 1 89 2D AuPd wires [130]. Fig. 5.10 indicates that the two methods yield similar dephasing times in 0D systems as well, but only at high temperatures. As mentioned in the previous section, at low temperature the conductance through the dot shows Coulomb Blockade oscillations that are superimposed on the UCFs. This complicates the extraction of the dephasing time from the UCFs. One reason why this method for determining τφ is less reliable than the previous method is because it assumes that the UCF variance that we extract from our data is equivalent to the ensemble variance. This is a reasonable assumption at high temperatures but at low temperatures, in the absence of a theoretical analysis of this regime where Coulomb Blockade oscillations of the conductance appear in addition to the UCFs, we are unable to distinguish between the Coulomb Blockade and the UCF contribution to the ensemble variance. In addition, it is not clear that eq. 5.4 would still be valid if a small but finite reflection coefficient in the QPCs is present. As a consequence we cannot use the extraction of the dephasing time from the variance using eq.5.4 to reach any conclusions about the behavior below 60 mK. We can compare this extracted temperature dependence to the relevant time and energy scales of our quantum dot as well to the theoretical predictions. Fig. 5.11(a) indicates where the relevant time and energy scales are with respect to our measured depashing times. The Thouless energy of the quantum dot is larger than all but one temperature and as such it is appropriate to use RMT results. There are no features in the data at the temperature at which we see Coulomb Blockade emerging and thus we conclude that, as expected, the average conductance and this extraction method for the dephasing time are not affected by Coulomb blockade. We reach temperatures that are smaller than the single particle level spacing and even low enough that the dephsing time is 5 times larger than the dwell time but do not observe a saturation as previous experiments have [102, 107]. The thermal time is larger than the elastic collision time at temperatures below 100mK which would correspond to the diffusive regime in a 2D system. However, the thermal time is larger than the time to cross the sample for the entire temperature range of the experiment which indicates that the quantum dot is 0D even though the temperature is smaller then the level spacing. The time the electron spends on the 90 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS (a) 6 5 4 (b) ∆=34 mK thermal time 2 ETh=930 mK -7 10 τdwell=0.8 ns -9 10 6 5 4 -8 10 τφ(s) 3 τ φ(s) 2D (ballistic) 2D (disordered) 1D (disordered) 0D (closed) TCB=60 mK 3 2 -9 τe=0.07 ns -10 10 10 6 5 4 3 τEhrenfest=0.02 ns -10 10 2 τcross=0.008 ns -11 10 -11 2 10 3 4 5 6 2 100 T (mK) 3 10 4 5 6 1000 2 10 3 4 5 6 2 100 3 4 5 6 1000 T (mK) Figure 5.11: (a) The calculated values of the dwell time, elastic scattering time, Ehrenfest time and the time to cross the dot are indicated with respect to the measured dephasing time (black dots). The red line is the thermal time. The energy level spacing of the quantum dot, the temperature below which Coulomb blockade appears and the Thouless energy are compared to temperature. (b) Calculated dephasing times for a 2D ballistic system (dark blue), 2D disordered system (black line), 1D disordered system (light blue line) and 0D diffusive system (red line) for the same density, mobility and area as the measured quantum dot. dot is longer than the Ehrenfest time, that is the necessary time for an interference pattern to build up. Because the time between elastic collisions is larger than the time an electrons take to cross the quantum dot, we expect the motion to be ballistic. Fig. 5.11(b) shows how the measured dephasing time (black dots) compare to the theoretical predictions using the 2DEG and quantum dot parameters. The dephasing times in a 2DEG with the same density and mobility as our 2DEG are expected to follow the ballistic T −2 law (eq. 5.10) at high temperatures and the disordered T −1 law at low temperatures, but the amount of dephasing is about an order of magnitude 5.4. MESOSCOPIC COULOMB BLOCKADE IN A QUANTUM DOT AT N = 191 smaller than the values we measure in the quantum dot. Similarly, dephasing that would take place in the 1D parts of the 2DEG, the leads, shown as the blue line would also not account for the measured dephasing. The 0D law from eq. 5.8 predicts a magnitude of the dephasing time that matches the measured values although the exponent 2 does not describe our temperature dependence. We find that the temperature dependence includes contributions from both a T −2 and a T −1 law, similar to the results of Huibers et al. However, unlike in [103, 104, 107], we observe that the dephasing time increases monotonically down to the lowest experimentally accessible temperature of 13 mK. This temperature is well below the value for onset temperature of the saturation Tsat observed in the experiments in ref [104] as well as the value of 118 mK given by the empirical formula for Tsat determined by Hackens et al. [107]. 5.4 Mesoscopic Coulomb Blockade in a Quantum Dot at N = 1 The small value for the QPC reflection coefficients determined from the temperature dependence of the average conductance at finite magnetic field suggest that the strong Coulomb blockade oscillations we observe as a function of gate voltage have to be mesoscopic in nature and cannot be due to the intrinsic reflection of the QPCs alone. This connection to the electron interference caused by long coherence times is confirmed by the magnetic field and temperature dependence of the oscillation. Fig. 5.12(a) shows the evolution of the Coulomb blockade oscillation with increasing magnetic field. We observe that large regions of periodic oscillations appear at small magnetic field while smaller regions appear at finite magnetic field. This behavior is easier to see in the map in fig. 5.12 where the background was eliminated and the local oscillation maxima are denoted in blue while oscillation minima are denoted in red. This evolution is consistent with MCB being sensitive to an applied magnetic field that disrupts the constructive interference between time-reversed paths. Fig. 5.13a shows a zoom in of line cuts taken from fig. 5.12(a) at several fields CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS (a) (b) Vc2(mV) -520 -520 2 G(e /h) 1.6 -540 1.2 Vc2(mV) 92 -540 0.8 -560 -560 0.4 20 5 15 30 B(mT) 25 40 35 50 5 20 15 30 B(mT) 25 40 35 50 Figure 5.12: (a) The dot conductance as a function of gate voltage and magnetic field. The fine oscillations in gate voltage are Coulomb blockade oscillations and they are superimposed on the larger UCF background. (b) Positions of maxima and minima of the oscillations in (a) are indicated in blue and red. which show that the oscillation is suppressed at finite field in comparison to zero field. To determine how large the magnetic field is that suppresses the MCB, we Fourier transform the data and integrate the power spectral density around the frequency of the oscillation to find the power PM CB [113]. The results are shown as the solid line in fig. 5.13b. The dotted line shows the weak localization dip at 13 mK for QPC setting A. The fact that the amplitude of the oscillation decreases over the same field scale is strong evidence that the oscillation is MCB. For B > 5 mT the power of the oscillation is small but non-zero because some oscillations are still present at some gate voltages and magnetic fields, as can be seen in fig. 5.12. Without the constructive interference of time-reversed paths, the oscillations are weaker and less frequent. They can be due to the fact that some magnetic fields, certain electron paths can still constructively interfere to cause coherent backscattering and Coulomb blockade oscillations and/or because of the < 2% remaining QPC reflection coefficient. The field scale over which PM CB decreases in fig. 5.13b is that necessary to introduce 1 − 2 flux quanta in the dot. The size of a QPC is much smaller than this, so we would expect the amplitude of Coulomb blockade oscillations caused by a finite r 2 without any contribution from coherent backscattering in the dot, to change over 5.4. MESOSCOPIC COULOMB BLOCKADE IN A QUANTUM DOT AT N = 193 (b) 4 2 2 4 -3 2 1.0 2.2 mT 10 mT 1 -560 -550 -540 Vc2 (mV) 2 2 Gdot (e /h) 1.4 mT 3 <Gdot > (e /h) 4 0.4 mT PMCB ( x10 e / h ) (a) 0.8 0 0 10 20 30 B (mT) Figure 5.13: (a) Conductance trace vs Vc2 at several magnetic fields. Traces are offset by 1 e2 /h. (b) PM CB (solid line, left axis) is obtained by Fourier transforming the data in fig. 5.12(a). The dotted line shows the average conductance vs magnetic field. All data are taken at 13 mK. a field scale that is much larger than that observed. As a consequence, this residual small reflection cannot be used to account for all the observed oscillations. Fig. 5.14(a) shows that increasing temperature also causes the oscillation to become weaker: MCB is suppressed for T & 54 mK. This temperature can be qualitatively understood by comparing the dephasing time to the time the electron spends on the dot. Once τφ becomes smaller than the dwell time τd ≈ 0.8 ns, the electron spends enough time on the dot to lose the phase coherence, the interference decreases and MCB should indeed be weaker. From fig. 5.10 we see that τφ = τd at T ≈ 80 mK, which agrees with our observations. Fig. 5.14b show the results of extracting PM CB for different temperatures at B = 0 (filled circles) and B = 30 mT (open squares). The oscillation decreases quickly with increasing T (the saturation at PM CB = 2 × 10−5 e4 /h2 is from the noise floor). Both the Coulomb blockade peaks as well as the UCFs are affected by dephasing and by thermal broadening. There is no apriori reason to expect the same temperature dependence for the two, but we can compare the MCB power to the variance dependence on temperature (blue crosses) We see that PM CB is at least as sensitive to T as Var(G), supporting the conclusion that the oscillations depend on phase coherence. CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS 2 22 mK 3 10 10 10 31 mK 2 10 1 -720 -710 Vc2 (mV) 10 -1 -3 10 -2 -4 10 -3 2 54 mK -2 4 Gdot (e /h) 13 mK 4 (b) Var(Gdot) (e /h ) (a) PMCB (e4/h2) 94 -5 10 100 T (mK) Figure 5.14: (a) Conductance vs Vc2 at B = 0 and several temperatures. Traces are offset by 1 e2 /h. (d) PM CB obtained from data taken from Vc2 = −500 mV to Vc2 = −800 mV at several values of Vc1 , for B = 0 (filled triangles, left axis) and B = 30 mT (open squares, left axis). For comparison we show measurements of Var(G) (crosses, right axis) at B = 0. To quantify the amount of residual charge quantization that is associated with this oscillation, we perform capacitive measurements: we use the conductance through the adjacent small quantum dot to detect the voltage change cause by the addition of one electron to the large dot. The charge on the large dot is varied by changing the voltage on gate bp. In response, the conductance GCS of the adjacent charge sensor changes by an amount ∆GCS . This amount is determined by the change of electric potential due to the accumulation of charge on gate bp as well as due to the addition of charge to the large dot. We can convert ∆GCS into an effective voltage change Veff , which would produce the same ∆GCS if applied to the small dot gate sp. This correspondence is shown in Fig. 5.15a. When the large dot is in the tunneling regime, the strong charge quantization is easily detectable by the small dot conductance. When an electron is added to the large dot, a clear Coulomb blockade peak is seen in the large dot conductance (black trace, right axis) and a decrease of Veff is seen in the small dot (blue trace, left axis) as illustrated by the data in fig. 5.15b. Veff initially increases as Vn is made less negative because of the capacitive coupling between the gate and the small dot. However at 5.4. MESOSCOPIC COULOMB BLOCKADE IN A QUANTUM DOT AT N = 195 2 ΔGCS 0.2 0.0 -246 -245 Vsp (mV) 0.04 0.10 0.02 0.05 -390 -389 2 Veff Veff (mV) (b) Gdot (e /h) GCS (e /h) (a) 0.4 0.00 -388 Vn (mV) Figure 5.15: (a) Coulomb blockade peak of the small dot used for charge sensing. We convert the change in the conductance ∆GCS of the charge sensor into an effective voltage change Veff . (b) Simultaneous measurement of charge sensing signal Veff (left axis) and conductance (right axis) of the large dot with both QPCs in the tunneling regime. the value of Vn where an electron is added to the dot, there is a sharp decrease in Veff . The correspondence between the decrease in Veff and the Coulomb blockade peaks in the large dot is most easily seen in the derivative D = dVeff /dVn . We refer to this derivative as the charge sensing signal. A dip in charge sensing signal corresponds to a step-like increase/decrease (after correcting for the capacitive gate-sensor coupling) of Veff associated with the addition of one electron to the large dot. When the large dot is in the fully transmitting regime, the quantization of charge is suppressed and the effect it has on the small dot conductance becomes increasingly small. The sensitivity of our quantum dot charge sensor is 1.7 × 10−4 e/Hz1/2 referenced to the detector. To increase our charge sensitivity we average together 300 individual charge sensing measurements taken over the same range of Vn which corresponds to an factor of 17 improvement in sensitivity. Background charge fluctuations in the donor layer can cause small shifts of the Coulomb blockade peaks in Vn and in the charge sensing signal. The resulting misalignment has to be corrected for before averaging over the individual traces. When the charge sensing signal is large (tunneling regime), the shifts are easily identified and corrected. However, when the charge sensing signal is small (open regime) detecting the shifts becomes increasingly difficult. To overcome this difficulty, we use 96 CHAPTER 5. QUANTUM DOTS: PERFECTLY TRANSMITTING QPCS (a) (b) 1.0 1.0 2 -360 Gdot (e /h) -380 2 0.5 -0.2 dVeff / dVn 0.010 Gdot (e /h) dVeff / dVn 0.0 0.005 0.0 -340 Vn (mV) 0.5 -315 -310 -305 Vn (mV) Figure 5.16: (a) Simultaneous measurement of the charge sensing signal in the small dot (dVeff /dVn ) (blue dots, left axis) and and the large dot conductance (black dots, right axis). The solid lines show fits discussed in the text. (b) Charge sensing data (left axis) and large dot conductance (right axis) at the values of Vn for which the two QPCs are open to 2 e2 /h conductance. The solid red line is a fit described in the text. the Coulomb oscillations that are visible in transport though the large dot over the entire range of QPC transmission to identify the shifts, align the charge sensing data and average it correctly. We follow the evolution of the Coulomb oscillations and of the charge sensing signal with increasing QPC transmission in fig. 5.16(a). For Vn < −375 mV the conductances of both QPCs are less than 2 e2 /h and we have well-defined CB on the large dot. The charge sensing signal shows a large dips that corresponds to the Coulomb blockade peaks. As the QPCs are opened by increasing Vn , the dips remain aligned to peaks in Gdot . The measurements of charge quantization for QPCs open to exactly one fully transmitting spin-degenerate mode ( GQP C1,2 = 2e2 /h) are shown in fig. 5.16b. We see a periodic variation of the charge sensing signal with the dips corresponding to peaks inthe large dot conductance which confirms that the conductance oscillation corresponds to a residual quantization of charge on the dot. To estimate the quantized charge to the size of the charge sensing signal, we use a model similar to ref. [111] where D is determined by the rate of change of electron number on the dot with gate voltage dNd /dVn and by the capacitances of the dot d and of the charge sensor CS. For Vn < −385 mV the theoretical predictions for 5.4. MESOSCOPIC COULOMB BLOCKADE IN A QUANTUM DOT AT N = 197 dNd /dVn from ref. [131] and the capacitance ratios discussed in ref. [132] fit the large dot conductance and the charge sensing signal lineshapes very well (solid red lines in fig 5.16). For −370 < Vn < −340 mV the data is well fitted by the prediction for a one- leaded dot without phase coherence and with GQP C ≈ 2 e2 /h [94] (solid line in fig. 5.16a)). However, this theory predicts there should not be a periodic variation in the charge sensing signal when GQP C = 2 e2 /h which does not correspond to our observations and can thus not be used in the N = 1 gate voltage region. For Vn ≈ −310 the theoretical model for MCB in a one-leaded dot [108] predicts e dNd /dVn = Cn,d (1 + (A/e) cos(2πCn,d Vn /e)) where A gives the residual charge quantization. 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