PMID- 33591761 OWN - NLM STAT- PubMed-not-MEDLINE LR - 20210225 IS - 1948-7185 (Electronic) IS - 1948-7185 (Linking) VI - 12 IP - 7 DP - 2021 Feb 25 TI - Tunable Rashba Spin Splitting in Two-Dimensional Polar Perovskites. PG - 1932-1939 LID - 10.1021/acs.jpclett.0c03668 [doi] AB - Two-dimensional (2D) Rashba semiconductors with structure inversion asymmetry and a spin-orbit coupling (SOC) effect show promising applications in nanospintronics, such as spin field effect transistors (FETs). Here, we systematically investigate the electronic structures and Rashba effect of 2D polar perovskites ABX(3) (A = Cs(+) or Rb(+); B = Pb(2+) or Sn(2+); X = Cl, Br, or I) by first-principles density functional theory calculations. We demonstrate that, except for the cubic case, 2D polar perovskites from tetragonal and orthorhombic three-dimensional (3D) bulks exhibit a strong intrinsic Rashba effect around the Gamma point, due to their structure inversion asymmetry and the strong SOC effect of heavy atoms. In particular, 2D orthorhombic RbSnI(3) shows the largest Rashba constant of 1.176 eV A among these polar perovskites, which is comparable to that of 3D bulk perovskites previously reported in experiments and theory. Furthermore, several 2D polar perovskites also show a strong electric field response. In particular, 2D tetragonal RbPbI(3) and tetragonal CsPbI(3) have strong electric field responses of >0.5 e A(2). Therefore, 2D polar perovskites as promising Rashba semiconductors possess large Rashba constants and strong electric field responses, resulting in a short spin channel length of tens of nanometers to preserve the spin coherence in spin FETs, superior to conventional 3D micrometer spin FETs. FAU - Chen, Jiajia AU - Chen J AUID- ORCID: 0000-0001-5182-0904 AD - Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China. FAU - Wu, Kai AU - Wu K AUID- ORCID: 0000-0003-4321-7819 AD - Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China. FAU - Hu, Wei AU - Hu W AUID- ORCID: 0000-0001-9629-2121 AD - Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China. FAU - Yang, Jinlong AU - Yang J AUID- ORCID: 0000-0002-5651-5340 AD - Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China. LA - eng PT - Journal Article DEP - 20210216 PL - United States TA - J Phys Chem Lett JT - The journal of physical chemistry letters JID - 101526034 SB - IM EDAT- 2021/02/17 06:00 MHDA- 2021/02/17 06:01 CRDT- 2021/02/16 17:09 PHST- 2021/02/17 06:00 [pubmed] PHST- 2021/02/17 06:01 [medline] PHST- 2021/02/16 17:09 [entrez] AID - 10.1021/acs.jpclett.0c03668 [doi] PST - ppublish SO - J Phys Chem Lett. 2021 Feb 25;12(7):1932-1939. doi: 10.1021/acs.jpclett.0c03668. Epub 2021 Feb 16.