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Reliable trajectory-based nonadiabatic quantum dynamics methods at the atomic level are critical for understanding many important processes in real systems. The paper reports latest progress of nonadiabatic field (NaF), a conceptually novel…

Chemical Physics · Physics 2025-04-14 Baihua Wu , Bingqi Li , Xin He , Xiangsong Cheng , Jiajun Ren , Jian Liu

The constraint coordinate-momentum \textit{phase space} (CPS) has recently been developed to study nonadiabatic dynamics in gas-phase and condensed-phase molecular systems. Although the CPS formulation is exact for describing the discrete…

Chemical Physics · Physics 2026-05-19 Jiaji Zhang , Jian Liu , Lipeng Chen

Isomorphism of the two-state system is heuristic in understanding the dynamical or statistical behavior of the simplest yet most quantum system that has no classical counterpart. We use the constraint phase space developed in J. Chem. Phys.…

Quantum Physics · Physics 2024-05-22 Xiangsong Cheng , Xin He , Jian Liu

Nonadiabatic transition dynamics lies at the core of many electron/hole transfer, photoactivated, and vacuum field-coupled processes. About a century after Ehrenfest proposed "Phasenraum" and the Ehrenfest theorem, we report a conceptually…

Quantum Physics · Physics 2024-04-09 Baihua Wu , Xin He , Jian Liu

We have recently developed the \textit{constraint} coordinate-momentum \textit{phase space} (CPS) formulation for finite-state quantum systems. It has been implemented for the electronic subsystem in nonadiabatic transition dynamics to…

Quantum Physics · Physics 2025-03-21 Youhao Shang , Xiangsong Cheng , Jian Liu

On-the-fly quantum nonadiabatic dynamics for large systems greatly benefits from the adiabatic representation readily available from the electronic structure programs. However, frequently occurring in this representation conical…

Nonadiabatic dynamical processes are one of the most important quantum mechanical phenomena in chemical, materials, biological, and environmental molecular systems, where the coupling between different electronic states is either inherent…

Chemical Physics · Physics 2022-05-24 Jian Liu , Xin He , Baihua Wu

The standard model of classical Density Functional Theory for pair potentials consists of a hard-sphere functional plus a mean-field term accounting for long ranged attraction. However, most implementations using sophisticated Fundamental…

Computational Physics · Physics 2021-01-04 James F. Lutsko , Cédric Schoonen

We present a rare event sampling scheme applicable to coupled electronic excited states. In particular, we extend the forward flux sampling (FFS) method for rare event sampling to a nonadiabatic version (NAFFS) that uses the trajectory…

Nonadiabatic molecular dynamics (NAMD) is widely used to describe hot electron relaxation and nonradiative recombination processes, but high computational costs limit its application to large supercells. Here, we implement a nonadiabatic…

Chemical Physics · Physics 2026-05-26 Xiaoke He , Hsiao-Yi Tsai , Ziwei Chai , Junwen Yin , Zhongfei Xu , Li-Min Liu

A new scheme of realizing the nonadiabatic conditional geometric phase shift via a noncoplanar (and coiled) fiber system is presented in this Letter. It is shown that the effective Hamiltonian that describes the interaction of polarized…

Quantum Physics · Physics 2007-05-23 Jian Qi Shen

Nonadiabatic molecular dynamics is an effective method for modeling nonradiative decay in electronically excited molecules. Its accuracy depends strongly on the quality of the potential energy surfaces, and its affordability for long…

Chemical Physics · Physics 2024-10-11 Matthew R. Hennefarth , Donald G. Truhlar , Laura Gagliardi

We review techniques for simulating fully quantum nonadiabatic dynamics using the frozen-width moving Gaussian basis functions to represent the nuclear wavefunction. A choice of these basis functions is primarily motivated by the idea of…

Chemical Physics · Physics 2018-09-05 Loïc Joubert-Doriol , Artur F. Izmaylov

We present an efficient \textit{ab initio} algorithm for quantum dynamics simulations of interacting systems that is based on the conditional decomposition of the many-body wavefunction [Phys. Rev. Lett. 113, 083003 (2014)]. Starting with…

Mesoscale and Nanoscale Physics · Physics 2019-02-27 Guillermo Albareda , Aaron Kelly , Angel Rubio

We derive and implement analytic nuclear gradients and derivative couplings for a constrained Complete Active Space Self-Consistent Field with a small active space designed to model electron or hole transfer. Using a Lagrangian formalism,…

Computational Physics · Physics 2025-09-01 Tian Qiu , Joseph E. Subotnik

An approximate method based on adiabatic time dependent density functional theory (TDDFT) is presented, that allows for the description of the electron dynamics in nanoscale junctions under arbitrary time dependent external potentials. In…

Mesoscale and Nanoscale Physics · Physics 2015-05-27 Y. Wang , C. -Y. Yam , G. H. Chen , Th. Frauenheim , T. A. Niehaus

A full quantum treatment of coherent population trapping (CPT) is given for a system of resonantly coupled atoms and electromagnetic field. We develop a regular analytical method of the construction of generalized dark states (GDS). It…

Quantum Physics · Physics 2009-11-11 A. V. Taichenachev , A. M. Tumaikin , V. I. Yudin

Simulation of conditional master equations is important to describe systems under continuous measurement and for the design of control strategies in quantum systems. For large bosonic systems, such as BEC and atom lasers, full quantum field…

Quantum Physics · Physics 2013-05-30 M. R. Hush , A. R. R. Carvalho , J. J. Hope

In this work we give a comprehensive derivation of an exact and numerically feasible method to perform ab-initio calculations of quantum particles interacting with a quantized electromagnetic field. We present a hierachy of…

Rare nonadiabatic events play a central role in photochemistry but remain difficult to simulate because excited-state dynamics is computationally demanding and often stochastic. Here we introduce a deterministic and time-reversible…

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