CHARGE TRANSPORT IN BISMUTH Jamal Derakhshan, West Virginia University Arthur F. Hebard, University of Florida This paper explains preliminary measurements and analysis of magnetoresistance (change in resistance induced by a magnetic field) studies on two pieces of single crystal bismuth. The bismuth is cut such that the current flows parallel to the binary axis. Both samples have purities better than 99.999%. The measurements include temperature sweeps between 2K and 300K and field sweeps between –7T and +7T. We use curve fitting to the data to create a phenomenological model for the observed magnetoresistance. We find that the magnetoresistance varies as T2 instead of the predicted T. In addition, the field dependence approaches the expected quadratic form at low fields. Introduction The aim of this project is to gain an understanding of how the charge carriers, both positive and negative, behave at low temperatures and high magnetic fields in this semimetal. Bismuth is unique among elements because of its low intrinsic carrier density compared with metals and because it is compensated (i.e., it has the same number of electrons as holes). Pure samples (see Table I below) have less elastic scattering of the charge carriers (off vibrating ions or static impurities) and a longer scattering length (distance traveled between collisions) compared with their impure counterparts. The long scattering length causes a dramatic decrease in resistivity ρ= RA . l 1 R is the resistance, A is the cross-sectional area of the sample, and l is the distance between the voltage leads (see Fig. 1). Bismuth reacts unusually to the presence of magnetic fields, exhibiting a change in resistance of 5 orders of magnitude at low temperatures in a field of 7T (see Fig. 2). Past studies of bismuth [1-3] have concentrated on resistivity as a function of magnetic field at a given temperature, with particular attention paid to the Shubnikov-de Haas effect, i.e., the existence of magnetic-field-dependent oscillations in the resistivity at high magnetic fields and low temperatures. Although we have pursued similar analyses, we focused primarily on measuring resistivity as a function of temperature at fixed magnetic field. It is beyond the scope of this paper to describe in detail the crystal structure of bismuth; however, it is necessary to mention that bismuth has one of the most complex crystal structures of any element. It has both a binary and a bisectrix axes lying in a common plane and a trigonal axis perpendicular to that plane. We used magnetoresistance measurements to characterize two samples of crystalline bismuth cut such that the current flowed in the binary direction with varying magnetic fields (-7T to +7T) applied in the trigonal direction at temperatures between 2K and 300K. From the magnetoresistance measurements, we determined our own model for resistivity as a function of temperature and magnetic field. We started by fitting the data to very simple models, which we then generalized to explain all of our low-field data. The measurements described above were then compared with the theoretical 2-band model of resistivity in bismuth. 2 Methods We cut crystals of bismuth in specific orientations and measured their electrical responses in the geometry shown in Fig. 1. Table I lists the characteristics of the two crystals which we analyzed. L W I+ V+ V- V- I- Transverse Longitudinal FIG. 1. Schematic view from top of sample showing placement of voltage and current leads and the labeling of the dimensions and directions. The applied magnetic field comes out of the paper. Sample Sample 1 (BiRGB2) Sample 2 (BiXuJd01) Orientation binary binary Dimensions 1.471mm-1.548mm-1.548mm 2.8mm-3.6mm-4.0mm Measured using microscope Measured using calipers 99.9995% 99.9999% W-H-L (see Fig. 2) Purity TABLE. I. Properties of analyzed samples. The measurements were taken in the Physical Property Measurement System (PPMS) manufactured by Quantum Design Inc. The sample space consisted of a 1-inch diameter cylinder kept at 1 torr pressure of helium exchange gas. This cylinder is enclosed by a liquid helium Dewar (thermos for cryogenic materials) which itself is enclosed by another Dewar filled with liquid nitrogen. The sample space is cooled either by the flow of gaseous helium (above 4K) or by pumping on liquid helium (between 2K and 4K). 3 The measurements were computer-controlled and did not require constant intervention by an operator. This set-up enabled us to take many data points and analyze them as soon as they became available. We used two types of sequences to analyze the samples. The first was a temperature sweep between 2K and 300K holding the magnetic field constant at a value between 0T and +7T. Then the magnetic field was set to another constant value and another temperature sweep was performed. The second type of sequence was a magnetic field sweep from –7T to +7T while holding the temperature constant. The temperature was set to another constant value and the measurement repeated. We chose the following temperatures for field sweeps: 2, 5, 10, 15, 20, 30, 50, 80, 130, 210, and 300K. Although this paper is limited to the measurement, analysis, and results of the longitudinal resistivity, measurements of the longitudinal and transverse (or Hall) voltages were simultaneously taken (see Fig. 1). These measurements were necessary in order to understand the principles underlying the behavior of the longitudinal resistivity. The Hall voltage is a potential difference caused by accumulation of charge at the sides of the crystal due to currents flowing in the presence of a magnetic field perpendicular to the longitudinal current. Results Figure 2 shows the results of temperature sweeps of the longitudinal resistivity taken for both samples. 4 0-0.1T in 0.01T steps 0-0.1T in 0.01T steps 1E-5 resistivity (ohm-m) resistivity (ohm-m) 1E-5 1E-6 1E-7 sample: BiRGB2 1E-8 1E-6 1E-7 sample: BiXuJd01 1E-8 0 50 100 0 temperature (K) 50 100 temperature (K) FIG. 2. Log-linear plot of longitudinal resistivity of each sample as a function of temperature at various magnetic fields. Data were taken from 2K to 300 K; however, they are shown only up to 100 K for clarity. In each graph, the bottom curve corresponds to B=0. We modeled these data in the following way. The normalized resistivity [resistivity – resistivity (B=0)] at some finite field was plotted against temperature. These curves were then individually fit to the following simple equation: ρ − ρ ( B = 0) = P1 . 1 + P2T 2 The fitting program iterated until chi squared was no longer reduced. In this way, the best values for P1 and P2 were determined. Our values of R2 varied from 0.9911 to 0.99829 for sample 1 and from 0.99339 to 0.99986 for sample 2 (R is the correlation coefficient). The data were fitted only from 5K-300K in this part of the experiment due to the flattening out of the data below 5K. The T2 term in the denominator was chosen because it surprisingly fit the temperature sweeps 5 much better than the T-dependence predicted by 2-band conduction theory (See discussion section). To determine the dependence of P1 and P2 on the applied magnetic field, we plotted these coefficients vs. B on log-log axes and found that both parameters had a power-law dependence on B. The slope of the resulting line determined the power-law exponent for each parameter. This procedure is illustrated for both samples in Figs. 3 and 4. Interestingly, the coefficients obey relationships of the form P1 ∝ B n−η and P2 ∝ B −η , where η is different for sample 1 and C o e ffic ie n t 2 .5 2 .0 1 .5 1 .0 P 2 P 1 C o e ffic ie n t sample 2; however, n = 1.95 ≈ 2 in both cases. 0 .5 0 .0 - 0 .5 0 .0 2 6 0 .0 2 4 0 .0 2 2 0 .0 2 0 0 .0 1 8 0 .0 0 0 0 .0 0 6 0 .0 1 2 0 .0 1 4 0 .0 1 8 (T ^ 1 .7 1 ) 1 .6 1 .8 2 .0 2 .2 2 .4 C o e ffic ie n t 1 / F ie ld ^ 0 .2 3 6 1 2 .6 2 .8 3 .0 3 .2 (1 / T ^ 0 .2 3 6 ) 0 .0 5 0 .0 4 0 .0 3 0 .0 2 P 2 C o e ffic ie n t 0 .0 2 8 0 .0 1 6 F ie ld ^ 1 .7 1 P 1 0 .0 3 0 0 .1 0 .0 1 0 .0 2 5 F ie ld 0 . 0 5 0 . 0 7 50 . 1 0 .0 1 0 .2 5 (T e s la ) FIG. 3. Coefficients for sample 1. P1 is proportional to 0 .0 1 0 .0 2 5 F ie ld B1.71±0.01 and P2 to B −0.24±0.01 . 6 0 . 0 5 0 . 0 7 50 . 1 (T e s la ) 0 .2 5 C o e f f ic ie n t c o e f f ic ie n t 1 2 .5 2 .0 1 .5 P 1 P 1 1 .0 0 .1 0 . 0 00 . 80 1 0 .0 0 .0 2 0 . 0 4 0 . 0 06 . 0 08 . 1 0 .2 0 .0 0 0 0 .0 0 5 0 .0 1 0 0 .0 1 5 0 .0 2 0 0 .0 2 5 F ie ld ^ 1 . 5 4 7 C o e f f ic ie n t ( T e s la ) 0 .0 6 0 .0 5 0 .0 4 0 .0 3 0 .0 2 P 2 C o e f f ic ie n t F ie ld P 2 0 .5 ( T e s la ^ 1 .5 4 7 ) 0 .0 4 5 0 .0 4 0 0 .0 3 5 0 .0 3 0 0 .0 2 5 0 .0 2 0 0 .0 1 5 0 .0 1 0 0 .0 0 5 0 .0 0 0 -0 .0 0 5 0 .0 1 0 . 00 0. 060 0. 0 8 1 0 .0 2 0 . 0 40 . 00 6. 008. 1 F ie ld 0 .2 0 .4 -0 .0 1 0 ( T e s la ) FIG. 4. Coefficients for sample 2. P1 is proportional to -2 -1 0 1 2 3 1 /( F ie ld ^ 0 . 4 0 9 ) 4 5 6 7 8 (1 /(T ^ 0 .4 0 9 )) B1.55±0.01 and P2 to B −0.41±0.01 . As a final test of our fitting equations, we superimposed our parameterization of the normalized resistivity on our original data. As can be seen from Fig. 5, the agreement is excellent over the entire range of temperatures and from 0.01T-0.1T. 7 Resistivity - Resistivity (B=0) R=((130)*(B^1.711)*(10^-5))/(1+0.00963*(B^-0.236)*(T^2)) 0.000016 0.01-0.09 T in 0.01 T Steps 0.000014 0.000012 0.000010 0.000008 0.000006 0.000004 sample: BiRGB2 0.000002 0.000000 0 20 40 60 80 100 Temperature (K) Resistivity- Resistivity (B=0) R=(103*(B^1.547)*(10^-5))/(1+0.00532*(B^-0.409)*(T^2)) 0.000018 0.000016 0.000014 0.01T-0.09T in 0.01T steps 0.000012 0.000010 0.000008 0.000006 0.000004 Sample: BiXuJd01 0.000002 0.000000 0 20 40 60 80 100 Temperature (K) FIG. 5. Normalized resistivity of each bismuth sample vs. temperature at various magnetic fields. Points show measured values, red lines plot the result of the fitting equations (shown above each graph). Resistivities are given in units of ohm-m. In each graph the bottom curve corresponds to B=0.01T. 8 Before discussing our results, we should explain why we have parameterized the normalized resistivity instead of the resistivity ρ (B) itself. The reason for this is that ρ (0) has significant deviations from a linear-in-temperature behavior. There is enough of a deviation from a straight line that our experimentally determined equations do not describe the total resistivity as closely as they fit the normalized data. We therefore chose to fit just the magnetically induced resistance at each temperature—the quantity we were immediately concerned with. A better approximation to the resistance at zero field can be calculated by the Bloch-Grüneisen method; however, this analysis was not performed here. Discussion We found that the normalized magnetoresistance varies as T-2 –a fact that is completely unexpected. The theoretical 2-band model for a compensated metal predicts a longitudinal resistivity ρ ( B) = ρ1 ρ 2 R2 B2 , + ρ1 + ρ 2 ρ1 + ρ 2 where ρ1, 2 are the resistivities of the electrons and holes, and R is the Hall coefficient. According to this model, if ρ1, 2 are linearly dependent on T, then in the absence of a magnetic field the resistivity is linear in T. This result is confirmed in our experiment. However, this model also predicts a magnetoresistivity of the form A1 B 2 . ρ − ρ ( B = 0) = 1 + A2T Our experiment rules out this functional form; both our samples obey ρ − ρ ( B = 0) = A1B 2−η A1B 2 . ≡ 1 + A2T 2 B −η Bη + A2T 2 9 Note that as B approaches zero, a B2 dependence is recovered. This is important for three reasons. First, it agrees with the fundamental symmetry expected for the parabolicity of the magnetoresistance at low fields. Secondly, it fits all our data. This is surprising because we could not have seen it without doing our temperature sweeps. If we simply tried to fit the field sweeps, we saw different exponents of the magnetic field and obtained fits that were not nearly as good. Finally, this model may explain why previous researchers have seen deviations from parabolicy at low fields: they may not have looked at low enough fields to see the B2 dependence [4]. Our results seem to indicate that the magnetoresistance of bismuth is not well described by the straightforward application of 2-band theory. We speculate that the reason may be a difference between the temperature-dependent scattering rates of the electrons and of the holes (i.e., that one type of carrier dominates the conductivity). However, we do not yet have a complete theory to support this picture. More work is needed in this direction. Understanding how bismuth acts in moderate magnetic fields ( ≤ 7T ) and at low temperatures ( T ≥ 2 K ) is the preliminary step before considering quantum effects predicted at high magnetic fields (30T) and very low temperatures (20mK). At those extremes, the charge carriers in a low-carrier-density material such as bismuth or graphite are predicted to behave in a one-dimensional manner because they travel in cyclotron orbits in the presence of large magnetic fields [5]. At high enough magnetic fields, the diameter of these orbits can become smaller than the distance between charge carriers. The charged particles still interact via the Coulomb interaction; however, they can be treated as one-dimensional objects. This phase is analogous to having separated conducting “wires” within the three-dimensional object. In this state, the charge carriers may comprise a postulated “Luttinger-liquid phase.” Understanding the response 10 of bismuth to magnetic fields and temperatures in a classical regime will enable us to proceed to the next level of experimentation. We hope to perform measurements at the National High Magnetic Field Laboratory where it is possible to test samples at magnetic fields up to 30T and temperatures in the 20mK range. Acknowledgments The REU program is sponsored and supported by the National Science Foundation (NSF). One big thank you to all members of Dr. Hebard’s laboratory: Quentin Hudspeth, Kevin McCarthy, Nikoletta Theodoropoulou, Rick Piciullo, Jeremy Nesbitt, Dr. Steven Arnason for explaining much of the material, and Xu Du for preparing the bismuth samples. Dr. Dmitri Maslov and Gregory Martin worked out the theoretical 2-band model. Drs. Kevin Ingersent and Alan Dorsey organized and administered the Research Experiences for Undergraduates (REU) program at the University of Florida. References [1] Y. Iye, L. E. McNeal, and G. Dresselhaus, Phys. Rev. 135, 1118 (1964). [2] R. D. Brown III, Phys. Rev. B 2, 928 (1970). [3] E. M. Lifshitz, and L. P. Pitaevskii, Physical Kinetics (Nauka, Moscow, 1979). [4] A. B. Pippard, Magnetoresistance in Metals (Cambridge University Press, New York, 1989). [5] C. Biagini, D. L. Maslov, M. Yu. Reizer, and L. I. Glazman, preprint (cond-mat/0006407). 11