Multiconfigurational Surface Hopping: a Time-Dependent Variational Approach with Momentum-Jump Trajectories DOI
Guijie Li, Zhecun Shi, Lei Huang

и другие.

Journal of Chemical Theory and Computation, Год журнала: 2024, Номер unknown

Опубликована: Авг. 31, 2024

The Ehrenfest mean field dynamics and trajectory surface hopping have been widely used in nonadiabatic simulations. Based on the time-dependent variational principle (TDVP), multiconfigurational (MCE) method has also developed can be regarded as a extension of traditional dynamics. However, it is not straightforward to apply TDVP trajectories because there exists momentum jump during hops. To solve this problem, we here propose (MCSH) method, where continuous momenta are obtained by linear interpolation interpolated construct basis functions for postprocessing manner. As demonstrated series representative spin-boson models, MCSH achieves high accuracy with only several hundred bases uniformly improve performance hopping. In principle, combined all kinds mixed quantum-classical thus potential properly describe general

Язык: Английский

Machine learning accelerated nonadiabatic dynamics simulations of materials with excitonic effects DOI Open Access

Sheng-Ze Wang,

Fang Qiu, Xiang‐Yang Liu

и другие.

The Journal of Chemical Physics, Год журнала: 2025, Номер 162(2)

Опубликована: Янв. 8, 2025

This study presents an efficient methodology for simulating nonadiabatic dynamics of complex materials with excitonic effects by integrating machine learning (ML) models simplified Tamm–Dancoff approximation (sTDA) calculations. By leveraging ML models, we accurately predict ground-state wavefunctions using unconverged Kohn–Sham (KS) Hamiltonians. These ML-predicted KS Hamiltonians are then employed sTDA-based excited-state calculations (sTDA/ML). The results demonstrate that energies, time-derivative couplings, and absorption spectra from sTDA/ML accurate enough compared those conventional density functional theory based sTDA (sTDA/DFT) Furthermore, sTDA/ML-based molecular simulations on two different systems, namely chloro-substituted silicon quantum dot monolayer black phosphorus, achieve more than 100 times speedup the linear response time-dependent DFT simulations. work highlights potential ML-accelerated studying complicated photoinduced large offering significant computational savings without compromising accuracy.

Язык: Английский

Процитировано

1
Detailed Complementary Consistency: Wave Function Tells Particle How to Hop, Particle Tells Wave Function How to Collapse DOI
Lei Huang, Zhecun Shi, Linjun Wang

и другие.

The Journal of Physical Chemistry Letters, Год журнала: 2024, Номер 15(26), С. 6771 - 6781

Опубликована: Июнь 24, 2024

In mixed quantum-classical dynamics, the quantum subsystem can have both wave function and particle-like descriptions. However, they may yield inconsistent results for expectation value of same physical quantity. We here propose a novel detailed complementary consistency (DCC) method based on principle internal consistency. Namely, along each trajectory tells particle how to hop, while collapse active states in ensemble. As benchmarked diverse array representative models with localized nonadiabatic couplings, DCC not only achieves fully consistent (i.e., identical populations calculated functions states) but also closely reproduces exact results. Due high performance, our new has great potential give accurate description general dynamics after further development.

Язык: Английский

Процитировано

7
Coupled-trajectory surface hopping with sign consistency DOI

Rixin Xie,

Zhecun Shi, Linjun Wang

и другие.

The Journal of Chemical Physics, Год журнала: 2025, Номер 162(16)

Опубликована: Апрель 22, 2025

The framework of exact factorization (XF) has inspired a series trajectory-based nonadiabatic dynamics methods by introducing different approximations. Recently, the coupled-trajectory surface hopping (CTSH) method been proposed to combine key advantages mixed quantum–classical based on XF and fewest switches hopping. We here present novel variant CTSH, namely, sign-consistent CTSH (SC-CTSH), which considers proper trajectory clustering reconstruct nuclear density distribution consistency between wave function active states introduce decoherence. Using quantum solutions as references, high performance SC-CTSH is benchmarked in widely studied scattering models compared with other related XF-based methods. Due incorporation new sign algorithms, obtains more accurate momentum decoherence during dynamics, makes combination consistent reliable. This study further highlights significance internal states, important development

Язык: Английский

Процитировано

0
Detailed Complementary Consistency: Wave Function Tells Particle How to Hop, Particle Tells Wave Function How to Collapse DOI Creative Commons
Lei Huang, Zhecun Shi, Linjun Wang

и другие.

Опубликована: Апрель 5, 2024

In mixed quantum-classical dynamics, the time evolution of quantum subsystem can involve both wave function and particle-like descriptions, which may yield inconsistent results for expectation value same physical quantity. this study, we propose a novel detailed complementary consistency (DCC) method, achieves fully consistent based only on principle internal in nonadiabatic dynamics. Namely, tells particle how to hop along each trajectory, while collapse occupation active states. As benchmarked diverse array representative models, DCC not gives identical populations functions states, but also closely systematically reproduces exact Due high performance, our new method provides promising approach toward more description dynamics with much better reliability efficiency general applications.

Язык: Английский

Процитировано

1
Multiconfigurational Surface Hopping: A Time-Dependent Variational Approach with Momentum-Jump Trajectories DOI Creative Commons
Guijie Li, Zhecun Shi, Lei Huang

и другие.

Опубликована: Июнь 21, 2024

The Ehrenfest mean field dynamics and trajectory surface hopping have been widely used in nonadiabatic simulations. Based on the time-dependent variational principle (TDVP), multiconfigurational (MCE) method has also developed can be regarded as a extension of traditional dynamics. However, it is not straightforward to apply TDVP trajectories because there exists momentum jump during hops. To solve this problem, we here propose (MCSH) method, where continuous momenta are obtained by linear interpolation interpolated construct basis functions for post-processing manner. As demonstrated series representative spin-boson models, MCSH achieves high accuracy with only several hundred bases uniformly improve performance hopping. In principle, combined all kinds mixed quantum-classical trajectories, thus potential properly describe general

Язык: Английский

Процитировано

1
Multiconfigurational Surface Hopping: a Time-Dependent Variational Approach with Momentum-Jump Trajectories DOI
Guijie Li, Zhecun Shi, Lei Huang

и другие.

Journal of Chemical Theory and Computation, Год журнала: 2024, Номер unknown

Опубликована: Авг. 31, 2024

The Ehrenfest mean field dynamics and trajectory surface hopping have been widely used in nonadiabatic simulations. Based on the time-dependent variational principle (TDVP), multiconfigurational (MCE) method has also developed can be regarded as a extension of traditional dynamics. However, it is not straightforward to apply TDVP trajectories because there exists momentum jump during hops. To solve this problem, we here propose (MCSH) method, where continuous momenta are obtained by linear interpolation interpolated construct basis functions for postprocessing manner. As demonstrated series representative spin-boson models, MCSH achieves high accuracy with only several hundred bases uniformly improve performance hopping. In principle, combined all kinds mixed quantum-classical thus potential properly describe general

Язык: Английский

Процитировано

1