Ultrafast Control of Excitonic Rashba Fine Structure by Phonon Coherence in the Metal Halide Perovskite CH3NH3PbI3

被引:33
作者
Liu, Z. [1 ,2 ]
Vaswani, C. [1 ,2 ]
Yang, X. [1 ,2 ]
Zhao, X. [1 ,2 ]
Yao, Y. [1 ,2 ]
Song, Z. [3 ,4 ]
Cheng, D. [1 ,2 ]
Shi, Y. [5 ,6 ]
Luo, L. [1 ,2 ]
Mudiyanselage, D-H [1 ,2 ]
Huang, C. [1 ,2 ]
Park, J-M [1 ,2 ]
Kim, R. H. J. [1 ,2 ]
Zhao, J. [5 ,6 ]
Yan, Y. [3 ,4 ]
Ho, K-M [1 ,2 ]
Wang, J. [1 ,2 ]
机构
[1] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA
[2] Iowa State Univ, Ames Lab, US DOE, Ames, IA 50011 USA
[3] Univ Toledo, Dept Phys & Astron, Toledo, OH 43606 USA
[4] Univ Toledo, Wright Ctr Photovolta Innovat & Commercializat, Toledo, OH 43606 USA
[5] Univ Sci & Technol China, Chinese Acad Sci, ICQD Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
[6] Univ Sci & Technol China, Chinese Acad Sci, Key Lab Strongly Coupled Quantum Matter Phys, Hefei 230026, Anhui, Peoples R China
基金
美国国家科学基金会; 国家重点研发计划; 中国国家自然科学基金;
关键词
CARRIER DYNAMICS;
D O I
10.1103/PhysRevLett.124.157401
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
We discover hidden Rashba fine structure in CH3NH3PbI3 and demonstrate its quantum control by vibrational coherence through symmetry-selective vibronic (electron-phonon) coupling. Above a critical threshold of a single-cycle terahertz pump field, a Raman phonon mode distinctly modulates the middle excitonic states with persistent coherence for more than ten times longer than the ones on two sides that predominately couple to infrared phonons. These vibronic quantum beats, together with first-principles modeling of phonon periodically modulated Rashba parameters, identify a threefold excitonic fine structure splitting, i.e., optically forbidden, degenerate dark states in between two bright ones with a narrow, similar to 3 nm splitting. Harnessing of vibronic quantum coherence and symmetry inspires light-perovskite quantum control and sub-THz-cycle "Rashba engineering" of spin-split bands for ultimate multifunction device.
引用
收藏
页数:6
相关论文
共 38 条
[1]   Optical properties of semiconductors using projector-augmented waves -: art. no. 125108 [J].
Adolph, B ;
Furthmüller, J ;
Bechstedt, F .
PHYSICAL REVIEW B, 2001, 63 (12)
[2]   Bright triplet excitons in caesium lead halide perovskites [J].
Becker, Michael A. ;
Vaxenburg, Roman ;
Nedelcu, Georgian ;
Sercel, Peter C. ;
Shabaev, Andrew ;
Mehl, Michael J. ;
Michopoulos, John G. ;
Lambrakos, Samuel G. ;
Bernstein, Noam ;
Lyons, John L. ;
Stoferle, Thilo ;
Mahrt, Rainer F. ;
Kovalenko, Maksym V. ;
Norris, David J. ;
Raino, Gabriele ;
Efros, Alexander L. .
NATURE, 2018, 553 (7687) :189-+
[3]   Direct Observation of Dynamic Symmetry Breaking above Room Temperature in Methylammonium Lead Iodide Perovskite [J].
Beecheri, Alexander N. ;
Semonin, Octavi E. ;
Skelton, Jonathan M. ;
Frost, Jarvist M. ;
Terban, Maxwell W. ;
Zhai, Haowei ;
Alatas, Ahmet ;
Owen, Jonathan S. ;
Walsh, Aron ;
Billinge, Simon J. L. .
ACS ENERGY LETTERS, 2016, 1 (04) :880-887
[4]   Helicity-dependent terahertz photocurrent and phonon dynamics in hybrid metal halide perovskites [J].
Cheng, D. ;
Liu, Z. ;
Luo, L. ;
Vaswani, C. ;
Park, J. -M. ;
Yao, Y. ;
Song, Z. ;
Huang, C. ;
Mudiyanselage, D. -H. ;
Kim, R. H. J. ;
Yan, Y. ;
Ho, K. -M. ;
Wang, J. .
JOURNAL OF CHEMICAL PHYSICS, 2019, 151 (24)
[5]   Excitons versus free charges in organo-lead tri-halide perovskites [J].
D'Innocenzo, Valerio ;
Grancini, Giulia ;
Alcocer, Marcelo J. P. ;
Kandada, Ajay Ram Srimath ;
Stranks, Samuel D. ;
Lee, Michael M. ;
Lanzani, Guglielmo ;
Snaith, Henry J. ;
Petrozza, Annamaria .
NATURE COMMUNICATIONS, 2014, 5
[6]   Inversion symmetry and bulk Rashba effect in methylammonium lead iodide perovskite single crystals [J].
Frohna, Kyle ;
Deshpande, Tejas ;
Harter, John ;
Peng, Wei ;
Barker, Bradford A. ;
Neaton, Jeffrey B. ;
Louie, Steven G. ;
Bakr, Osman M. ;
Hsieh, David ;
Bernardi, Marco .
NATURE COMMUNICATIONS, 2018, 9
[7]   Neutral and Charged Exciton Fine Structure in Single Lead Halide Perovskite Nanocrystals Revealed by Magneto-optical Spectroscopy [J].
Fu, Ming ;
Tamarat, Philippe ;
Huang, He ;
Even, Jacky ;
Rogach, Andrey L. ;
Lounis, Brahim .
NANO LETTERS, 2017, 17 (05) :2895-2901
[8]   Free Carrier Emergence and Onset of Electron-Phonon Coupling in Methylammonium Lead Halide Perovskite Films [J].
Ghosh, Tufan ;
Aharon, Sigalit ;
Etgar, Lioz ;
Ruhman, Sanford .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (50) :18262-18270
[9]   Highly Spin-Polarized Carrier Dynamics and Ultra large Photoinduced Magnetization in CH3NH3Pbl3 Perovskite Thin Films [J].
Giovanni, David ;
Ma, Hong ;
Chua, Julianto ;
Graetzel, Michael ;
Ramesh, Ramamoorthy ;
Mhaisalkar, Subodh ;
Mathews, Nripan ;
Sum, Tze Chien .
NANO LETTERS, 2015, 15 (03) :1553-1558
[10]   Semiempirical GGA-type density functional constructed with a long-range dispersion correction [J].
Grimme, Stefan .
JOURNAL OF COMPUTATIONAL CHEMISTRY, 2006, 27 (15) :1787-1799