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In the spirit of the fewest switches surface hopping, the frozen Gaussian approximation with surface hopping (FGA-SH) method samples a path integral representation of the non-adiabatic dynamics in the semiclassical regime. An improved…

Chemical Physics · Physics 2016-10-12 Jianfeng Lu , Zhennan Zhou

We use the effective Hamiltonian that we recently fitted against the first 306 experimentally observed vibronic transitions of NO2 [J. Chem. Phys. 119, 5923 (2003)] to investigate the time domain nonadiabatic dynamics of this molecule on…

Chemical Physics · Physics 2011-11-09 Michaël Sanrey , Marc Joyeux

We present a comprehensive computational framework for simulating nonadiabatic molecular dynamics with explicit inclusion of geometric phase (GP) effects. Our approach is based on a generalized two-level Hamiltonian model that can represent…

Mesoscale and Nanoscale Physics · Physics 2025-10-17 Dhruv Sharma

Nuclear Berry curvature effects emerge from electronic spin degeneracy and canlead to non-trivial spin-dependent (nonadiabatic) nuclear dynamics. However, such effects are completely neglected in all current mixed quantum-classical methods…

Chemical Physics · Physics 2022-08-29 Xuezhi Bian , Yanze Wu , Jonathan Rawlinson , Robert G. Littlejohn , Joseph E. Subotnik

We investigate a simple and robust scheme for choosing the phases of adiabatic electronic states smoothly (as a function of geometry) so as to maximize the performance of ab initio non-adiabatic dynamics methods. Our approach is based upon…

Chemical Physics · Physics 2019-09-26 Zeyu Zhou , Zuxin Jin , Tian Qiu , Andrew M. Rappe , Joseph Eli Subotnik

Conical intersections serve as critical gateways in photochemical reactions, enabling rapid nonradiative transitions between potential energy surfaces that underpin fundamental processes such as photosynthesis or vision. Their calculation…

Chemical Physics · Physics 2025-02-19 Rhyan Barrett , Christoph Ortner , Julia Westermayr

Physically accurate and mathematically tractable models are presented to characterize scattering and reflection properties of reconfigurable intelligent surfaces (RISs). We take continuous and discrete strategies to model a single patch and…

Systems and Control · Electrical Eng. & Systems 2022-08-31 Tiebin Mi , Jianan Zhang , Rujing Xiong , Zhengyu Wang , Robert Caiming Qiu

Probing vibronic coherence in molecules has been a central topic in ultrafast science, as it is an essential prerequisite to monitoring electronic motion. While experiments have demonstrated that attosecond transient absorption spectroscopy…

Atomic Physics · Physics 2023-08-02 C. H. Yuen , C. D. Lin

Coarse-grained (CG) conformational surface hopping (SH) adapts the concept of multisurface dynamics, initially developed to describe electronic transitions in chemical reactions, to accurately describe classical molecular dynamics at a…

Soft Condensed Matter · Physics 2021-02-03 Joseph F. Rudzinski , Tristan Bereau

We present the simulation of the photochemical dynamics of cyclobutanone induced by the excitation of the 3s Rydberg state. For this purpose, we apply the complete active space self-consistent field method together with spin-orbit…

Chemical Physics · Physics 2024-01-15 Xincheng Miao , Kira Diemer , Roland Mitrić

The global many-electron wave function overlap matrix accounts for all effects beyond the Born-Oppenheimer approximation in the discrete variable local diabatic representation, a numerically exact framework for modeling nonadiabatic conical…

Chemical Physics · Physics 2025-01-10 Yujuan Xie , Bing Gu

In this work, we present the computational realization of holographic metasurfaces to generation of the non-diffracting waves. These holographic metasurfaces (HMS) are simulated by modeling a periodic lattice of metallic patches on…

Classical Physics · Physics 2019-08-27 Santiago R. C. Fernandez , Marcos R. R. Gesualdi

Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…

Chemical Physics · Physics 2024-04-11 Nikolay V. Golubev , Jiří Vaníček

We present a perturbation approach rooted in time-dependent density-functional theory to calculate electron hole (eh)-pair excitation spectra during the non-adiabatic vibrational damping of adsorbates on metal surfaces. Our analysis for the…

Chemical Physics · Physics 2017-11-22 Simon P. Rittmeyer , Jörg Meyer , Karsten Reuter

A new methodology of simulating nonadiabatic dynamics using frozen-width Gaussian wavepackets within the moving crude adiabatic representation with the on-the-fly evaluation of electronic structure is presented. The main feature of the new…

Chemical Physics · Physics 2018-04-04 Loïc Joubert-Doriol , Artur F. Izmaylov

We present a framework for simulating relaxation dynamics through a conical intersection of an open quantum system that combines methods to approximate the motion of degrees of freedom with disparate time and energy scales. In the vicinity…

Statistical Mechanics · Physics 2019-07-24 Addison J. Schile , David T. Limmer

Aligning theoretical atomistic structural models of materials with available experimental data presents a significant challenge for disordered systems. The configurational space to navigate is vast, and faithful realizations require large…

Materials Science · Physics 2025-09-29 Tigany Zarrouk , Miguel A. Caro

In this paper, we investigate coherent control of nonadiabatic dynamics at a conical intersection (CI) using engineered ultrafast laser pulses. Within a model vibronic system, we tailor pulse chirp and temporal profile and compute the…

We have previously demonstrated that in the context of two-dimensional (2D) coherent electronic spectroscopy measured by phase modulation and phase-sensitive detection, an \emph{incoherent} nonlinear response, due to pairs of…

Quantitative photoacoustic tomography (qPAT) is an imaging technique aimed at estimating chromophore concentrations inside tissues from photoacoustic images, which are formed by combining optical information and ultrasonic propagation. The…

Computational Physics · Physics 2019-12-23 Hwan Goh , Timo Lahivaara , Tanja Tarvainen , Aki Pulkkinen , Owen Dillon , Ruanui Nicholson , Jari Kaipio