Abstract
Low-dimensional materials with charge density waves (CDW) are attractive for their potential to exhibit superconductivity and nontrivial topological electronic features. Here we report the two-dimensional (2D) chalcogenide, BaSbTe2S which acts as a new platform hosting these phenomena. The crystal structure of BaSbTe2S is composed of alternating atomically thin Te square-net layers and double rock-salt type [(SbTeS)2]2- slabs separated with Ba2+ atoms. Due to the electronic instability of the Te square net, an incommensurately modulated structure is triggered and confirmed by both single-crystal X-ray diffraction, electron diffraction, and the presence of an energy bandgap in this compound. Our first-principles electronic structure analysis and investigation of structural dynamical instability suggest that the Te network plays a dominant role in its origin. The incommensurate structure is refined with a modulation vector of q = 0.351(1)b* using an orthorhombic cell of a = 4.4696(5) Å, b = 4.4680(5) Å, and c = 15.999(2) Å under superspace group Pmm2(0β0)000 at 293 K. The modulation vector q varies as a function of both occupancy of Te in the square net and temperature, indicating the CDW order can be modulated by local distortions. The CDW can be suppressed by pressure, leading to the emergence of superconductivity with a Tc up to 7.5 K at 13.6 GPa, suggesting a competition between the CDW order and superconductivity. Furthermore, electrical transport under the magnetic field reveals the existence of compensated high mobility electron- and hole-bands near the Fermi surface (μ ∼600-3500 cm2V-1s-1), suggesting Dirac-like band dispersion.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 6753-6762 |
| Number of pages | 10 |
| Journal | Journal of the American Chemical Society |
| Volume | 147 |
| Issue number | 8 |
| DOIs | |
| State | Published - Feb 26 2025 |
Funding
The work is primarily supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences, and the Engineering Division (synthesis, physical property measurements, Hall and multiband analysis, synchrotron data analysis, and writing manuscript) at Argonne National Laboratory. The work was partially supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357. This work was supported in part by the National Key Research and Development Program of China (2020YFA0710303). At Northwestern, work was supported in part by the Department of Energy, Office of Science, Basic Energy Sciences under grant DE-SC0014520 (sample synthesis, TEM measurements, and DFT calculations), and by the Department of Energy, Office of Science, National Quantum Information Science Research Centers, Superconducting Quantum Materials and Systems Center (SQMS) under the contract No. DE-AC02-07CH11359 as well as the National Science Foundation under the MRSEC grant DMR-1720139, and funding from Leslie and Mac McQuown (electronic transport measurements). This study was supported in part by the National Natural Science Foundation of China (12204298, 52102218, U1905215, and 52072076) and the Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China (2021ZZ127). Z.Z.L acknowledges the Minjiang Scholar Professorship (GXRC-21004). S.S., S.H. and C.W. acknowledge the Department of Energy, Office of Science, Basic Energy Sciences under grant DE-SC0014520; the computational resources of the Bridges-2 supercomputer at the Pittsburgh Supercomputing Center (PSC) under grant DMR-160112; and the Quest high-performance computing facility at Northwestern University. The experimental research at the University of Utah received support from the National Science Foundation Division of Materials Research Award No. 2132692. This work was also supported by the U.S. Department of Energy (DOE) Office of Science, Fusion Energy Sciences funding award entitled High Energy Density Quantum Matter, Award No DE-SC0020340 (S.D., W.Z.C, J.B. and T.B.). S.C. and V.P.D. acknowledge that this work made use of the EPIC facility of Northwestern University\u2019s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633); the MRSEC program (NSF DMR-2308691) at the Materials Research Center; the International Institute for Nanotechnology (IIN). Research conducted at the Center for High-Energy X-ray Science (CHEXS) is supported by the NSF (BIO, ENG, and MPS Directorates) under award DMR-2342336. S.D. thanks Prof. Vikram Deshpande for providing guidance for magnetic measurements under pressure.
ASJC Scopus subject areas
- Catalysis
- General Chemistry
- Biochemistry
- Colloid and Surface Chemistry