Structural fluctuations cause spin-split states in tetragonal (CH3NH3)PbI3 as evidenced by the circular photogalvanic effect

被引:112
作者
Niesner, Daniel [1 ]
Hauck, Martin [2 ]
Shrestha, Shreetu [3 ]
Levchuk, Ievgen [3 ]
Matt, Gebhard J. [3 ]
Osvet, Andres [3 ]
Batentschuk, Miroslaw [3 ]
Brabec, Christoph [3 ,4 ]
Weber, Heiko B. [2 ]
Fauster, Thomas [1 ]
机构
[1] Friedrich Alexander Univ Erlangen Nurnberg, Lehrstuhl Festkorperphys, D-91058 Erlangen, Germany
[2] Friedrich Alexander Univ Erlangen Nurnberg, Lehrstuhl Angew Phys, D-91058 Erlangen, Germany
[3] Friedrich Alexander Univ Erlangen Nurnberg, Inst Mat Elect & Energy Technol, Dept Mat Sci & Engn, D-91058 Erlangen, Germany
[4] Bavarian Ctr Appl Energy Res, D-91058 Erlangen, Germany
关键词
organic-inorganic perovskite; lead halide perovskite; circular photogalvanic effect; dynamical Rashba; Rashba effect; METHYLAMMONIUM LEAD IODIDE; CHARGE-CARRIER LIFETIMES; EXCITON BINDING-ENERGY; CH3NH3PBI3; CRYSTALS; RECOMBINATION; PEROVSKITES; TRANSITION; DYNAMICS; PHOTOLUMINESCENCE;
D O I
10.1073/pnas.1805422115
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Lead halide perovskites are used in thin-film solar cells, which owe their high efficiency to the long lifetimes of photocarriers. Various calculations find that a dynamical Rashba effect could significantly contribute to these long lifetimes. This effect is predicted to cause a spin splitting of the electronic bands of inversion-symmetric crystalline materials at finite temperatures, resulting in a slightly indirect band gap. Direct experimental evidence of the existence or the strength of the spin splitting is lacking. Here, we resonantly excite photocurrents in single crystalline (CH3NH3)PbI3 with circularly polarized light to clarify the existence of spin splittings in the band structure. We observe a circular photogalvanic effect, i.e., the photocurrent depends on the light helicity, in both orthorhombic and tetragonal (CH3NH3)PbI3. At room temperature, the effect peaks for excitation photon energies Delta E = 110 meV below the direct optical band gap. Temperature-dependent measurements reveal a sign change of the effect at the orthorhombic-tetragonal phase transition, indicating different microscopic origins in the two phases. Within the tetragonal phase, both Delta E and the amplitude of the circular photogalvanic effect increase with temperature. Our findings support a dynamical Rashba effect in this phase, i.e., a spin splitting caused by thermally induced structural fluctuations which break inversion symmetry.
引用
收藏
页码:9509 / 9514
页数:6
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