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Development of ab initio time-dependent GW+BSE method based on surface hopping scheme in nonadiabatic molecular dynamics

EMSL Project ID
50834
Award DOI
https://dx.doi.org/10.46936/lser.proj.2019.50834/60000117

Abstract

 An exciton is a quasiparticle formed by an electron and a hole, which interact through the Coulomb interaction. It generally describes optically excited states in insulators, semiconductors, and liquids. The dynamics of excitons, including the hot exciton relaxation and electron-hole recombination, play crucial roles in the energy transfer processes for sustainable energy generation. Calculating the electronic structure of excited states in solids requires many-body perturbation theory approaches such as green's function based many-body perturbation and Bethe-Salpeter equation (GW+BSE). In this project, we plan to develop the ab initio time-dependent GW+BSE (TDGW+BSE) method based on the classical path approximation (CPA) and surface hopping scheme in nonadiabatic molecular dynamics (NAMD). The spin-orbit coupling (SOC) will be included in order to investigate spin dynamics of the electron/hole in the exciton. We expect the proposed TDGW+BSE method will become an important tool to investigate the ultrafast exciton dynamics in condensed matter systems. With the collaboration with the time-resolved multi-photon photoemission (TR-mPP) spectroscopy experiments at the University of Pittsburgh, we will try to reach the benchmarks of the newly developed TDGW+BSE method.

Project Details

Project type
Large-Scale EMSL Research
Start Date
2019-10-01
End Date
2021-12-31
Status
Closed
Released Data Link
https://search.emsl.pnnl.gov/?project_id_search=50834

Team

Principal Investigator

Jin Zhao
Institution
University of Science and Technology of China, Chinese Academy of Sciences

Team Members

Linjie Chen
Institution
University of Science and Technology of China, Chinese Academy of Sciences

Atreyie Ghosh
Institution
University of Pittsburgh

Jiawei Zhan
Institution
University of Chicago

Zhaorui Xia
Institution
University of Science and Technology of China, Chinese Academy of Sciences

Zehua Wang
Institution
University of Pittsburgh

Chuanyu Zhao
Institution
Tencent Quantum Laboratory

Zhenfa Zheng
Institution
University of Science and Technology of China, Chinese Academy of Sciences

Aolei Wang
Institution
University of Science and Technology of China, Chinese Academy of Sciences

Yunzhe Tian
Institution
University of Science and Technology of China, Chinese Academy of Sciences

Xiang Jiang
Institution
University of Science and Technology of China, Chinese Academy of Sciences

Yongliang Shi
Institution
University of Science and Technology of China, Chinese Academy of Sciences

Hongli Guo
Institution
California State University, Northridge

Qijing Zheng
Institution
University of Science and Technology of China, Chinese Academy of Sciences

Hrvoje Petek
Institution
University of Pittsburgh

Related Publications

CO2 Photoreduction on Metal Oxide Surface is Driven by Tran-sient Capture of Hot Electrons: Ab initio Quantum Dynamics Simulation W. Chu, Q. Zheng, O. V. Prezhdo, J. Zhao* J. Am. Chem. Soc. , 142, 3214, (2020)
Coherent Electron Transfer at the Ag/Graphite Heterojunction Interface S. Tan, Y. Dai, S. Zhang, L. Liu, J. Zhao* and H. Petek* Phys. Rev. Lett., 120, 126801, (2018)
Delocalized Impurity Phonon Induced Electron-Hole Recombination in Doped Semiconductors L. Zhang, Q. Zheng, Y. Xie, Z. Lan, O.V. Prezhdo, W. A. Saidi, and J. Zhao* Nano Lett., 18, 1592, (2018)
Dynamics of Photoexcited Small Polarons in Transition Metal Oxides L. Zhang, W. Chu, C. Zhao, Q. Zheng*, O. V. Prezhdo and J. Zhao J. Phys. Chem. Lett.,12, 2191(2021)
Electronic Structure , 1, 034001, (2019)
Highly Dispersive Nearly Free Electron Bands at a 2D-Assembled C60 Monolayer Masahiro Shibuta, Kazuo Yamamoto, Hongli Guo, J. Zhao and Atsushi Nakajima* J. Phys. Chem. C , 124, 1734, (2020)
Hongli Guo, Wissam A. Saidi, Yanan Wang, Jin Zhao, Qijing Zheng. 2018. "Tuning Solvated Electrons by Polar–Nonpolar Oxide Heterostructure." The Journal of Physical Chemistry Letters 9 (11):3049-3056. https://doi.org/10.1021/acs.jpclett.8b00938
Hongli Guo, Zhenggang Lan, Oleg V. Prezhdo, Wissam A. Saidi, Chuanyu Zhao, Jin Zhao, Qijing Zheng. 2018. "Superatom Molecular Orbital as an Interfacial Charge Separation State." The Journal of Physical Chemistry Letters 9 (12):3485-3490. https://doi.org/10.1021/acs.jpclett.8b01302
Interlayer Polarization Explains Slow Charge Recombination in Two-Dimensional Halide Perovskites by Nonadiabatic Molecular Dynamics Simulation J. Su, Q. Zheng, Y. Shi*, and J. Zhao*
Iodine and Sulfur Vacancy Cooperation Promotes Ultrafast Charge Extraction at MAPbI3/MoS2 Interface Y. Shi, O. V. Prezhdo, J. Zhao* and W. A. Saidi* ACS Energy Lett. , 5, 1346, (2020)
J. Phys. Chem. Lett. , 10, 6151-6158, (2019)
J. Phys. Chem. Lett. , 11, 9032, (2020)
J. Phys. Chem. Lett. , 12, 3960, (2021)
Low-Frequency Lattice Phonons in Halide Perovskites Explain High Defect Tolerance Towards Electron-Hole Recombination W. Chu, Q. Zheng, O. V. Prezhdo, J. Zhao* and W. A. Saidi* Sci. Adv. , 6, eaaw7453, (2020)
Mono-Elemental Properties of 2D Black Phosphorus Ensure Extended Charge Carrier Lifetimes under Oxidation: Time-Domain Ab Initio Analysis L. Zhang, A. S. Vasenko, J. Zhao* and O. V. Prezhdo* J. Phys. Chem. Lett. , 10, 1083, (2019)
Real-time GW-BSE Investigations on Spin-Valley Exciton Dynamics in Monolayer Transition Metal Dichalcogenide. X. Jiang, Q. Zheng, Z. Lan, W. A. Saidi, X. Ren and J. Zhao* Sci. Adv. , 7, eabf3759, (2021)
Tensile Strain-Controlled PhotoGenerated Carrier Dynamics at van der Waals Heterostructure Interface Y. Tian, Q. Zheng,* J. Zhao* J. Phys. Chem. Lett. , 11, 586, (2020)
Tuning the Carrier Lifetime in Black Phosphorene through Family Atom Doping H. Guo, W. Chu, Q. Zheng and J. Zhao* J. Phys. Chem. Lett. , 11, 4662, (2020)
Wissam A. Saidi, Reza Shahbazian-Yassar, Yongliang Shi, Boao Song, Jin Zhao. 2018. "Experimentally Validated Structures of Supported Metal Nanoclusters on MoS2." The Journal of Physical Chemistry Letters 9 (11):2972-2978. https://doi.org/10.1021/acs.jpclett.8b01233