Structural and superconducting properties of low-temperature ultrathin PbBi3 films

Bismuth (Bi), as a stable heaviest element in the periodic table of elements, has strong spin-orbit coupling, which has attracted a lot of attention as the parent material of various known topological insulators. Previous calculations predicted that Bi(111) with a thickness less than eight bilayers and the ultrathin black-phosphorus-like Bi(110) films are single-element two-dimensional (2D) topological insulators. However, it is generally believed that these crystalline bismuth phases are not superconducting or their transition temperature should be lower than 0.5 mK. Lead (Pb) is a good superconducting elementary material, and there is a relatively small difference in radius between the Bi atom and Pb atom. According to the Hume-Rothery rule, it is expected that Pb/Bi alloys in an arbitrary ratio should be superconducting. One may thus expect to form crystalline Bi based superconductors by Pb substitution, which might host intriguing topological superconductivity. While our previous work has demonstrated a low-temperature stable Pb1-xBix (x similar to 0.1) alloy phase in which Pb in the Pb(111) structure is partially replaced by Bi, the Bi crystalline structure-based phases of the superconducting alloys still lack in-depth research. Here, we report a new low-temperature phase of Pb-Bi alloy thin film, namely PbBi3, on the Si(111)-(7 x 7) substrate, by co-depositing Pb and Bi at a low temperature of about 100 K followed by an annealing treatment of 200 K for 2 h. Using low-temperature scanning tunneling microscopy and spectroscopy (STM/STS), we characterize in situ the surface structure and superconducting properties of the Pb-Bi alloy film with a nominal thickness of about 4.8 nm. Two spatially separated phases with quasitetragonal structure are observed in the surface of the Pb-Bi alloy film, which can be identified as the pure Bi(110) phase and the PbBi3 phase, respectively, based on their distinct atomic structures, step heights and STS spectra. The PbBi3 film has a base structure similar to Bi(110), where about 25% of the Bi atoms are replaced by Pb, and the surface shows a root 2 x root 2R45 degrees reconstructed structure. The superconducting behavior of the PbBi3 phase is characterized using variable-temperature STS spectra. We obtain that the superconducting transition temperature of PbBi3 is about 6.13 K, and the 2 Delta(0)/k(B)T(c) ratio is about 4.62 using the fitting parameter of Delta(0) = 1.22 meV at 0 K. By measuring the magnetic field dependent superconducting coherence length, the critical field is estimated at larger than 0.92 T. We further investigate the superconducting proximity effect in the normal metal-superconductor (N-S) heterojunction consisting of the non-superconducting Bi(110) domain and the superconducting PbBi3 domain. The N-S heterojunctions with both in-plane configuration and step-like configuration are measured, which suggest that the atomic connection and the area of the quasi-2D Josephson junctions and the external magnetic field can affect the lateral superconducting penetration length. We also observe the zero-bias conductance peaks (ZBCPs) in the superconducting gap of the PbBi3 surface in some cases at zero magnetic field. By measuring dI/dV spectra at various temperatures and by adopting a superconducting Nb tip, we identify that the ZBCP originates from the superconductor-insulator-superconductor (S-I-S) junction formed between a superconducting tip and the sample. Nevertheless, the Bi(110)-based PbBi3 phase may provide a possible platform to explore the intriguing topological superconducting behaviors at the vortexes under magnetic fields, or in the vicinity of the potentially topological superconducting Bi(110) islands by considering the proximity effect.

Automated summary

This study reports a new low-temperature phase of Pb-Bi alloy thin film, namely PbBi3. Through in situ characterization of surface structure and superconducting properties, it is found that the superconducting transition temperature of PbBi3 is about 6.13K. By studying the heterojunctions of non-superconducting and superconducting regions with different structures, the lateral superconducting penetration length is found to be influenced by atomic connection, Josephson junctions, and external magnetic field. Furthermore, the observed topological superconducting behaviors on the PbBi3 surface may occur in the vortex regions under magnetic fields or near the topological superconducting Bi(110) islands considering the proximity effect.