> 2eph03 < 1 Fabrication and characterization of epitaxial NbN/TaN/NbN Josephson junctions grown by pulsed laser ablation M. R. Nevala, I. J. Maasilta, K. Senapati and R. C. Budhani Abstract—We report fabrication and characterization of epitaxial NbN/TaN/NbN Josephson junctions grown by pulsed laser ablation. These SNS junctions can be used as elements of rapid-single-flux-quantum (RSFQ) logic, which is a promising technology for high speed digital electronic devices. The NbN/TaN/NbN trilayer films were prepared on a single crystal MgO substrate by pulsed laser ablation, and patterned into junctions using a novel process utilizing e-beam lithography, chemical vapor deposition and e-beam evaporation. The quality of junctions was tested by measuring the temperature dependence of the junctions’ IcRn values, observed to be quite close to theoretical values. Index Terms—Josephson junctions, Pulsed laser deposition, Superconducting device fabrication, Superconductor-normalsuperconductor devices. form SNS Josephson junctions. TaN was chosen as barrier material because of the tunability of its resistivity by varying growth conditions (e.g pressure) and its observed high resistivity [4], [5], [6] which results in higher resistance and therefore possibly higher IcRn product. Another reason is that its thermal, chemical and mechanical properties are quite similar to NbN [5]. NbN was chosen because of its high critical temperature (Tc) when fabricated by pulsed laser ablation (up to ~17 K), and because of its good stability against strain, mechanical and chemical attacks [5], [7]. Here, we have developed a simple new fabrication process based on electron-beam lithography, plasma-enhanced chemical vapor deposition (PECVD) and ebeam evaporation, which is shown to produce high-quality junctions with a simple insulator alignment process, and which could directly be extended to the submicron scale. I. INTRODUCTION II. LIKHAREV’S THEORY single flux quantum (RSFQ) logic is a promising technology for high speed digital electronic devices [1]. Devices with superconductor/normal conductor/superconductor (SNS) junctions have nonhysteretic [2] current I vs. voltage V characteristics required for RSFQ logic. These kind of SNS devices have several advantages. For example they can be packed closely, their intrinsic switching speed is high, and their fabrication is simpler than semiconductor transistors with similar design [1]. In RSFQ circuitry the appropriate figure of merit of a SNS junction is the product of the critical current Ic and the normal resistance of the junction Rn, since it is inversely proportional to SFQ pulse width [3], [4]. If we want to operate at 30-50 GHz frequency, the product IcRn should be greater than ~0.3 mV [3], [4]. We have used a tantalum nitride (TaN) barrier sandwiched between superconducting niobium nitride (NbN) electrodes to The density of Cooper pairs decreases with distance from the superconductor in an SNS junction when electron pairs are leaking from a superconductor to a normal conductor [2]. The rate of decay is approximately exponential, and the distance where the density has decreased by a factor 1/e is the coherence length of the normal conductor [2] ξ n , expressed as R APID Manuscript received 16 August 2008. This work was supported by the Academy of Finland and the Technological foundation of Finland. M. R. Nevala and I. J. Maasilta are with Nanoscience Center, Department of Physics, University of Jyväskylä P.O. Box 35, FIN-40014 University of Jyväskylä, Finland (phone: +358 14 260 4720; fax: +358 14 260 4756; e-mail: minna.nevala@phys.jyu.fi). K. Senapati, was with the Department of Physics, Indian Institute of Technology Kanpur, Kanpur 208016, India. He is now with the Department of Materials Science and Metallurgy, University of Pembroke Street, Cambridge, UK (e-mail: ks485@cam.ac.uk ). Cambridge, R. C. Budhani is with the Department of Physics, Indian Institute of Technology Kanpur, Kanpur 208016, India (rcb@iitk.ac.in). 1/ 2 hD (1) 2π kT where D is the diffusion constant D = 1 /( e 2 g (ε F ) ρ ) , e is the electron charge, g (ε F ) is the density of states at Fermi ξn = energy ε F , ρ is the resistivity and h is the Planck’s constant devided by 2π, k is the Boltzmann’s constant and T is temperature. Likharev developed a theory [8] for SNS junctions in the temperature range 0.3Tc < T < Tc. Within that range and with the condition [9] for N layer thickness L > 2ξ n (T c ) Likharev’s predictions follow quite closely the earlier de Gennes’ theory [10] for SNS junctions. Likharev’s theoretical prediction for the critical current Ic of the junction when 0.3Tc < T < Tc can be approximated by 4 ∆ L exp (− L / ξ n ) π eR n kT c ξ n where ∆ is the energy gap parameter. 2 I c (T ; L ) ≅ (2) > 2eph03 < 2 III. SAMPLE FABRICATION NbN-TaN-NbN trilayers were fabricated on single crystal (100) MgO substrates by pulsed laser ablation of high purity Nb and Ta targets using a KrF excimer laser (λ=248 nm) in high purity N2 environment. The turbo molecular pump based deposition chamber was equipped with a multi-target carousel for automated in-situ target exchange, to facilitate multilayer depositions. Both NbN and TaN layers were deposited at a substrate temperature of 600 °C and ~80 mTorr N2 pressure. Pulse energy of the laser was kept fixed at ~145 mJ. The size of laser spot on the target and the target-to-substrate distance were optimized to achieve a deposition rate of 0.4 nm/sec for NbN and ~0.5 nm/sec for TaN. Thickness of the top and base NbN layers was kept constant at 200 nm while the thickness of TaN was ~10 nm for all samples in this study. Several NbN/TaN/NbN trilayer films were pattered by ebeam lithography as squares of different sizes from 3 micrometer × 3 micrometer to 10 micrometer × 10 micrometer, and reactive ion etched by a mixture of CHF3 and O2 [11] to form the electrodes of SNS Josephson junctions. The etching rate was ~10 nm/min at 55 mTorr and 150 W. A thin layer of aluminum was used as an etch mask. The lateral size and height of the etched pillars were checked with an atomic force microscope. E-beam lithography was again used for patterning the SiO2 insulator for the top Nb contact layer (Fig. 1). The growth of SiO2 was done in a plasma enhanced chemical vapor deposition (PECVD) reactor using a mixture of Silane/Argon (5%SiH4/Ar) and nitrous oxide (N2O), after the surface was cleaned gently with N2 plasma. The insulator deposition was done in two steps: first at 150 °C for regions around the devices, and then at 300 °C for areas below the bond pads, both followed by a lift-off. Two steps were needed because only the 300 °C SiO2 can withstand bonding, whereas accurate small scale lift-off was only possible for the 150 °C SiO2. Also, 150 °C is about the maximum temperature that could be used to avoid burning the thinner e-beam resists around the device active area. By using this unconventional technique (ebeam patterned PECVD lift-off), we achieved highly aligned SiO2 patterns. The top contact Nb layer was again pattered by e-beam lithography and evaporated (2 Å/s) on top of the device with an UHV ( ~ 9 × 10 − 9 mbar) e-beam evaporator. Before the Nb deposition, we used a gentle O2 plasma cleaning and 1 kV Arion sputtering in situ to remove impurities and a possible thin oxide layer from the NbN surface. The thickness of a possible natural oxide on the NbN surface could be about 2 nm thick [7]. In previous studies, Ar-ion cleaning has been shown to reduce the NbN surface contact resistance [12], and was observed to be necessary to make a good contact with the top NbN layer also in this work. A direct bond far from the device area served as the bottom NbN layer contact. A schematic illustration of the final device structure is presented in Fig. 1. Fig. 1. A schematic cross section of the device geometry. The NbN/TaN/NbN trilayer was grown by pulsed laser ablation on single crystal (100) MgO. Devices were pattered by e-beam lithography as squares and reactive ion etched to form the electrodes of the SNS Josephson junctions. The growth of highly aligned SiO2 insulator was performed by PECVD after e-beam lithography patterning. The top contact Nb layer was e-beam evaporated in an UHV chamber. Fig. 2. Resistance versus temperature of a 8 micrometer × 8 micrometer NbN/TaN/NbN Josephson junction. Inset shows a zoom-in of the Nb transition. Critical temperature of NbN was ~15.7 K and for Nb ~ 8.8 K. The high quality of the NbN film is reflected in its high transition temperature. IV. EXPERIMENTAL RESULTS Junction resistance (R) vs. temperature (T) was measured for all samples, with a typical result shown in Fig. 2. Typically critical temperatures of NbN (Tc ~15.7 K) and Nb (Tc ~ 8.8 K) were observed. The high quality of the NbN film is reflected in its high transition temperature. The I-V measurements of the junctions were performed at several different temperatures from 4.2 K upwards. The 3 micrometer × 3 micrometer junctions were not sputter cleaned before the Nb deposition, which resulted in resistive behavior even at zero bias. However, those 8 micrometer × 8 micrometer junctions that were cleaned showed a large supercurrent branch, as exemplified in Figs. 3 and 4. In Fig. 3 we can notice a rounding of the I-V characteristics, possibly due to thermal fluctuations [2]. In Fig. 4 less pronounced rounding is seen; however, the critical currents are clearly lower compared to Fig. 3. The difference between these two devices (and others) is not well understood at the moment, as fairly large variations were observed between devices fabricated on the same substrate, with nominally identical trilayer films. The Rn values obtained from the I-V characteristics were observed to be as high as 180 mΩ and relatively insensitive to temperature below 7 K. The I-V data in Figs. 3 and 4 corresponds to values ~25 mΩ and ~ 42 mΩ, respectively. At T ~11 K where Rn is dominated by the Nb contact Figs. 2, 3 > 2eph03 < and 4 all give a consistent value ~100 mΩ. Using the I-V data, we determined the IcRn values of four similar (nominally the same trilayers) 8 micrometer × 8 micrometer devices at several different temperatures from 4.2 K to 8.7 K. The results are shown in Fig. 5. Measurements above 9 K were prohibited by the finite resistance of the Nb lead. 3 the obtained D, 2 ξ n (T c ) ~ 2 nm < 10 nm = L, so that we are well within the range of validity of Eq. (2). The dashed curve shows the same analysis but with n = 2 × 10 21 cm-3, giving a D ~ 7 . 5 × 10 − 6 m2s-1. We also checked that with these values 2 ξ n (T c ) ~ 1.5 nm < 10 nm = L. From Fig. 5 we can notice that the theoretical curves follow fairly well the measured values. However, one of the samples showed clearly lower IcRn values, most likely due to a bad quality Nb-NbN interface. Fig. 3. The I-V characteristic for a 8 micrometer × 8 micrometer NbN/TaN/NbN Josephson junction at eight different temperatures from 4.2 K to 11.0 K with a TaN barrier of 10 nm. The critical current at 4.2 K was ~3.2 mA. Fig. 4. The I-V characteristic for a 8 micrometer × 8 micrometer NbN/TaN/NbN Josephson junction at eight different temperatures from 4.2 K to 11.8 K with a TaN barrier of 10 nm. The critical current at 4.2 K was ~1.2 mA. Using the normal state resistance (~ 25 mΩ) of the junction from Fig. 3 at 4.2 K we can estimate the resistivity of a 8 micrometer × 8 micrometer junction, giving ~16 mOhms cm. To estimate a value for the diffusion constant D, we need in addition a reliable value for the carrier density n. As it can vary a lot as a function of the TaN composition [13], we have to leave it as a fit parameter for our theoretical analysis. In Fig. 5 we show two different theoretical curves based on Eq. (2) with n as a parameter and L kept fixed at 10 nm. The solid curve has n = 1× 10 21 cm-3, corresponding to a diffusion constant D is ~ 9 . 5 × 10 − 6 m2s-1. In addition, we fixed a value 2 ∆ / kT c ≈ 4 .0 as observed for high quality NbN [14]. With Fig. 5. The measured values of critical current Ic times normal layer resistance Rn with different temperatures for four 8 micrometer × 8 micrometer junctions and two theoretical curves with different carrier density n according to Likharev’s theory of SNS junctions. The product IcRn is the appropriate figure of the merit for SNS junction and measured data follows quite closely Likharev’s theory. We also made I-V measurements at several different values of magnetic flux density B from 0 T to 3.2 T at a temperature 4.2 K. The junctions were placed in the magnetic field so that the field lines are along the N layer (90 degrees from the direction of the current flow). A typical measured curve of critical current Ic vs. magnetic flux density B is presented in Fig. 6. Although the measured curve in Fig. 6 does not show the Fraunhofer pattern of a clean and small Josephson junction [2], it is clearly seen that increasing magnetic field suppresses critical current Ic to zero at ~3 T. The absence of the Fraunhofer pattern is the result of a nonuniform critical current density at the junction area, likely caused by the fact that the junction dimension (8 µm) is slightly larger that the Josephson penetration depth, estimated to be ~ 3 µm. > 2eph03 < 4 Likharev’s theory of SNS junctions followed quite closely the measurements, showing that this simple proximity effect based model is likely a good enough design guide for NbN based junctions. REFERENCES [1] [2] [3] [4] Fig. 6. The critical current (Ic) vs. magnetic flux density (B) for a 8 micrometer × 8 micrometer NbN/TaN/NbN Josephson junction with a TaN barrier of 10 nm at the temperature 4.2 K. [5] [6] V. CONCLUSIONS We have grown high quality NbN/TaN/NbN trilayer films with high critical temperature (~16 K) with the pulsed laser ablation method, and developed an unconventional e-beam lithography-based technique that uses lift-off of a high-quality PECVD-grown SiO2 insulator layer to produce high alignment accuracy. The method may allow a close packed structure on a small area and a material friendly fabrication process for submicron devices in the future. Ar-ion sputtering of the NbN surface before the top wiring deposition improved the quality of the junctions significantly by removing the native oxide and surface contaminants from the NbN surface, proving to be necessary for high quality junctions. The I-V characteristics of the devices showed sharp features at 4.2 K. However, the IcRn products were slightly smaller although comparable to values measured before for sputtered NbN films [4], and showed scatter between nominally identical devices. 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