# Microwave-induced constant voltage steps in surface junctions of Bi2Sr2CaCu2O8+δ single crystals

## Abstract

We have observed the zero-crossing steps in a surface junction of a mesa structure micro-fabricated on the surface of a Bi<sub>2</sub>Sr<sub>2</sub>CaCu<sub>2</sub>O<sub>8+δ</sub> single crystal. With the application of microwave of frequencies 76 and 94 GHz, the current-voltage characteristics show clear voltage steps satisfying the ac Josephson relation. Increasing the microwave power, the heights of the steps show the Bessel-function behavior up to step number $`n=4`$. We confirm that the intrinsic surface junction meets the criterion for the observation of zero-crossing steps.

Irradiated with a microwave of frequency $`f`$, Josephson tunnel junctions can spontaneously exhibit quantized dc voltages of $`V_n=nhf/2e`$ in the absence of a bias current, where $`n`$ is an integer and $`h`$ is the Planck’s constant. In current-voltage ($`I`$-$`V`$) characteristics, this effect manifests itself as constant voltage steps crossing the zero-current axis. The occurrence of these voltage steps is a direct consequence of the ac Josephson effect and the phase-coherent pair tunneling in response to an external electromagnetic excitation. Since no voltages other than the quantized values $`V_n`$ are present for zero current bias, Josephson tunnel junctions are ideal as voltage standards which require constant voltage output independent of environmental parameters such as temperature or humidity. Thus, most Josephson voltage standards currently in use consist of several thousands of Nb/AlO<sub>x</sub>/Nb tunnel junctions connected in series, with each junction exhibiting highly hysteretic $`I`$-$`V`$ characteristics.

The highly anisotropic high-$`T_c`$ superconductors (HTSCs) with layered structures, such as Bi<sub>2</sub>Sr<sub>2</sub>CaCu<sub>2</sub>O<sub>8+δ</sub> (Bi-2212) and Tl<sub>2</sub>Ba<sub>2</sub>Ca<sub>2</sub>Cu<sub>3</sub>O<sub>10+δ</sub> (Tl-2223), can be considered as series arrays of Josephson tunnel junctions along the $`c`$-axis. For Bi-2212 single crystals the superconducting order parameter tends to be localized in $`3`$-Å-thick Cu-O bilayers and the transport along the $`c`$-axis occurs mainly via Josephson tunneling between the neighboring Cu-O bilayers, which are $`12`$ Å apart from each other. The $`c`$-axis dc $`I`$-$`V`$ characteristics of a Bi-2212 single crystal usually show multiple quasiparticle branches with very large hysteresis, where the number of branches corresponds to the number of intrinsic Josephson junctions (IJJs) in the crystal. In spite of the general consensus for dc $`I`$-$`V`$ characteristics, the microwave response of a stack of IJJs in HTSCs is unclear. Applied with a microwave, a stack of IJJs has been observed to exhibit constant voltage steps. However, their values do not satisfy the Josephson frequency-voltage relation and strongly depend on the microwave power. Thus, the authors of Ref.  have attributed their results to the microwave-induced phase-locked fluxon motion in a series stack of IJJs, rather than the ac Josephson effect. Although Shapiro steps or zero-crossing steps are observed in the studies, the measured interval between the voltage steps, $`\mathrm{\Delta }V`$, shows a large difference from the expected value $`Nhf/2e`$ and depends sensitively on the frequency and power of the applied microwave. Here, $`N`$ is the total number of IJJs in a measuring stack. This discrepancy is ascribed to other coupling mechanisms which give rise to the phase locking of IJJs in addition to the ac Josephson effect.

In this paper, we report an observation of clear zero-crossing voltage steps in $`I`$-$`V`$ characteristics of stacks of IJJs in Bi-2212 single crystals, irradiated with a microwave of frequency $`f=76`$ and $`94`$ GHz. The voltage steps are believed to be from a single intrinsic Josephson junction formed on the top surface of the stack in contact with a metallic (Au) electrode. The voltage difference between the successive steps coincides with the expected value of $`hf/2e`$. The magnitude of the voltage steps follows the Bessel-function dependence on the applied microwave power up to the order of $`n=4`$. This implies that the observed voltage steps are genuine zero-crossing voltage steps. The critical current of the surface intrinsic Josephson junction is significantly suppressed due to the proximity contact to the normal-metal electrode. This severe reduction of the critical current allows one to isolate the microwave response of the “surface junction” from that of the rest of the “inner junctions” in a stack of Bi-2212 single crystals. From our experimental results we were able to confirm the necessary condition for observing zero-crossing steps in an intrinsic Josephson junction of highly anisotropic high-$`T_c`$ superconductors.

Stacks of IJJs were fabricated on the surface of a Bi-2212 single crystal using photolithography and Ar-ion etching. The Bi-2212 single crystal, grown by standard solid-state-reaction method, was glued onto a MgO substrate using negative photoresist and was cleaved using pieces of Scotch tape until an optically smooth surface appeared. A thin ($``$ 50 nm) Au film was evaporated on top of the crystal immediately after cleaving to protect the crystal surface from any contamination during further fabrication processes. Then a large base mesa ($`450\times 20\times 1.2`$ $`\mu `$m<sup>3</sup>) was formed by photolithography and ion-beam etching, using the beam voltage $`V_{\mathrm{beam}}=300`$ V and the beam current $`I_{\mathrm{beam}}=0.8`$ mA/cm<sup>2</sup>. The ash of photoresist was removed by oxygen plasma etching. To prevent the regions of the specimen other than the top surface of the base mesa from being shorted to the contact electrodes, an insulation layer of photoresist was placed around the base mesa. Then a 400-nm-thick Au film was further evaporated and patterned afterwards by photolithography and ion-beam etching to form electrical extension pads and small stacks ($`18\times 20\times 0.04`$ $`\mu `$m<sup>3</sup>) on top of the base mesa. The lateral dimensions of a small stack were determined by the narrow width of the base mesa and the breadth of the electrode, which also acted as a mask for the fabrication of the small stack. The thickness of the measuring stack, which corresponded to the number of junctions in it, was controlled by adjusting the ion-beam etching time. The fabrication procedure was completed by removing the remnant photoresist by oxygen plasma etching. The heat treatment of the specimen was limited to $`T<`$ 120 <sup>o</sup>C during the entire microfabrication process.

The microwave response of the specimen was measured at $`T=4.2`$ K. The microwave generated by a Gunn diode was transmitted through a waveguide and coupled inductively to the specimen placed at $`\lambda `$/4 distance from the end of the waveguide. The maximum available microwave power was 100 mW for $`f=76`$ GHz and 50 mW for $`f=94`$ GHz. The power coupled to the specimen was tuned by using a level set attenuator.

Transport measurements were carried out using a three-terminal measurement method (see the inset in Fig. 1). Shown in Fig. 1 is a typical $`c`$-axis resistance vs temperature, $`R_c(T)`$. The resistance shows a weak semiconducting behavior above $`T_c87`$ K, indicating that the crystal is in a slightly overdoped regime. One also notices that the resistance remains finite below $`T_c`$ with a secondary peak appearing far below $`T_c`$. It is attributed to a weak intrisic Josephson junction formed at the surface of a measuring stack in contact with a Au normal-metal electrode. The superconductivity of the topmost Cu-O bilayer of a stack is suppressed by the proximity contact to a normal metal (Au) pad rather than by a degradation effect of the surface layer. Thus, the surface Cu-O bilayer has a superconducting transition temperature $`T_c^{}31`$ K far below the bulk $`T_c`$. In the temperature range of $`T_c^{}<T<T_c`$, the surface junction can be considered as a normal metal/insulator/$`d_{x^2y^2}`$-wave-superconductor (NID) junction consisting of the surface Cu-O bilayer in the normal state and the adjacent inner bilayer in the superconducting state. Thus, $`R_c(T)`$ corresponds to a quasiparticle tunneling resistance of the NID junction with a junction resistance $`R_n^{}=R_c(T_c)=3.9`$ $`\mathrm{\Omega }`$. As the surface junction becomes Josephson coupled below $`T_c^{}`$, $`R_c(T)`$, which is essentially the contact resistance between Au pad and the topmost Cu-O bilayer, becomes less than 40 m$`\mathrm{\Omega }`$ in our specimen.

Figure 2 shows the $`I`$-$`V`$ characteristics of IJJs in a stack below $`T_c^{}`$ in the absence of an exteranl rf field. With increasing bias current just above the critical current of each intrinsic Josephson junction in a stack, periodic voltage jumps occur in units of $`V_c23`$ mV, and the $`I`$-$`V`$ curves show highly hysteretic behavior. Although not apparent in the figure, the number of quasiparticle branches in the $`I`$-$`V`$ characteristics indicates that 28 IJJs are contained in the measuring stack. The average critical current $`I_c`$ is about $`4.5`$ mA and the normal state junction resistance of the inner junctions, estimated from the linear portion of the $`I`$-$`V`$ curves, is $`R_n=0.7`$ $`\mathrm{\Omega }`$. The inset of Fig. 2 shows the enlarged view of the $`I`$-$`V`$ curves in the low bias region. One notices that the weak surface junction shows a much smaller critical current $`I_c^{}130`$ $`\mu `$A with clear hysteresis. The reduced critical current of the surface junction, compared to the ones of the inner junctions, is due to the suppressed superconductivity of the surface layer. This result is consistent with the finite-resistance behavior of the $`R_c(T)`$ curve in Fig. 1.

Figure 3(a) shows the $`I`$-$`V`$ characteristics of the specimen with the application of a microwave of frequency $`f=94`$ GHz. Clearly seen are the two steps of height $`\mathrm{\Delta }I_1=120`$ $`\mu `$A. The voltage difference between the two steps is about $`400\pm 20`$ $`\mu `$V in agreement with the expected value of $`\mathrm{\Delta }V=2hf/2e=389`$ $`\mu `$V, implying that these steps are genuine zero-crossing steps corresponding to the step number $`n=\pm 1`$. Due to the weakness of the transmitted microwave power, we could not observe other steps of $`n>3`$ for $`f=94`$ GHz.

Shown in Fig. 3(b) are the $`I`$-$`V`$ characteristics of the same stack at a microwave frequency $`f=76`$ GHz. Compared to the case of $`f=94`$ GHz, the height of the $`n=1`$ step becomes reduced while the steps of higher orders $`n=\pm 2,\pm 3`$ are seen more clearly. The steps of $`n3`$ do not cross the zero-current line, possibly due to a large leakage current. The remarkably large leakage current for the $`c`$-axis tunneling in Bi-2212 high-$`T_c`$ superconductors is attributed to the existence of the gapless node for the $`d_{x^2y^2}`$-wave order parameter. By increasing the microwave power, we were able to identify other voltage steps up to the order of $`n=4`$. Further increase of the microwave power caused a noticeable slope in the voltage steps, possibly due to chaotic switching of the surface junction between a Josephson-tunneling state and a resistive one. Once any of the Josephson junctions in the stack becomes resistive, all the steps are bound to exhibit a finite resistive slope, making it difficult to identify the steps at high bias voltages.

Figure 4 shows the measured step heights as a function of the square root of the applied microwave power, $`P^{1/2}`$. Varying the step order from $`n=0`$ to 4, the measured step heights are in qualitative agreement with the relation of $`\mathrm{\Delta }I_n=I_c^{}|J_n(I_{ac}f_c^{}/I_c^{}f)|`$, where $`I_c^{}`$ is the critical current of the surface junction at $`T=4.2`$ K, $`J_n`$ the $`n`$-th order Bessel function, $`I_{ac}`$ the applied rf current, and $`f_c^{}=2eI_c^{}R_n^{}/h`$ the characteristic frequency of the surface junction. We obtained the fitting parameter $`I_c^{}`$ (4.2 K) to be $`180`$ $`\mu `$A, which corresponds to the critical current density of 50 A/cm<sup>2</sup>. This value is consistent with the ones observed in the surface junctions of other specimens at 4.2 K. To reveal the Bessel-function behavior, a Josephson junction is required to satisfy the condition of $`\mathrm{\Omega }^2\beta =(f/f_p)^21`$, where $`\mathrm{\Omega }=f/f_c`$ is the frequency reduced with the characteristic frequency of a junction, $`\beta =2eI_cR_n^2C/\mathrm{}`$ the hysteresis parameter, and $`f_p=\sqrt{eI_c/\pi hC}`$ the Josephson plasma frequency. $`C`$ is the capacitance of the Josephson junction. This criterion is not satisfied with the inner IJJs in the stack but is satisfied with the surface junction (see Table I). Thus we infer that the observed zero-crossing steps should originate from the weak surface junction. As shown in Table I, specimens used by other groups concerning the microwave-induced fluxon motion or collective behavior of the IJJs do not meet the above criterion. Nonetheless, one can notice that the typical parameters of Josephson junctions currently used for Nb-based voltage standards are similar to the ones of the surface junction. Although the observing conditon for the zero-crossing steps was originally proposed for Josephson tunnel junctions made of conventional superconductors, our results indicate that the IJJs in HTSCs provide high potential for observing the same phenomenon.

The observing condition for the zero-crossing steps can be rewritten as $`\mathrm{\Omega }^2\beta =(\pi h/e)(ϵf^2/dJ_c)1`$, where $`ϵ`$ is a dielectric constant of the blocking layer between adjacent conducting bilayers, $`d`$ a inter-bilayer distance, and $`J_c`$ a critical current density of the intrinsic Josephson junction. For our specimen in this study, the critical current density of the inner junctions is 24 times larger than that of the surface junction. An inner junction thus has the Josephson plasma frequency $`f_p`$ about five times larger than that of the surface junction. IJJs with larger critical current densities require higher microwave frequencies and higher power to produce stable zero-crossing steps. Reducing the tunneling critical current density is, therefore, required to obtain the stable voltage steps from the inner IJJs in a stack. In addition, to prohibit any nonuniform rf-current flow into the junction, which becomes more probable at higher microwave frequencies, one needs to reduce the junction size. These requirements may be fulfilled with ultra-small IJJs in Bi-2212 single crystals or with IJJs in Bi-2212 single crystals intercalated with guest molecules such as HgI<sub>2</sub> or HgBr<sub>2</sub>.

In summary, we have studied the inverse ac Josephson effect from a intrinsic Josephson junction located in the surface of Bi-2212 single crystals irradiated with the external microwave of $`f=76`$ and $`94`$ GHz. The surface weak Josephson junction shows clear voltage steps satisfying the ac Josephson relation and the step heights follow the Bessel-function behavior with increasing microwave power, up to the step number $`n=4`$. Our results indicate that the intrinsic Josephson junctions in highly anisotropic HTSCs with very low tunneling critical current density may be a promising candidate for the observation of zero-crossing steps.

This work was supported in part by KRISS Project No. 98-0502-102. This work was also supported by BSRI under Contract No. 1NH9825602, MARC under Contract No. 1MC9801301, and POSTECH under Contract No. 1UD9900801.