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A first principles quantum formalism to describe the non-adiabatic dynamics of electrons and nuclei based on a second quantization representation (SQR) of the electronic motion combined with the usual representation of the nuclear…

Chemical Physics · Physics 2020-11-06 Sudip Sasmal , Oriol Vendrell

The nonadiabatic photodissociation dynamics of alkali halide molecules excited by a femtosecond laser pulse in the gas phase are investigated theoretically, and it is shown that the population of the photoexcited molecules exhibits…

Chemical Physics · Physics 2018-11-30 Yuta Mizuno , Koji Hukushima

Multiconfiguration pair-density functional theory (MC-PFDT) has previously been applied successfully to carry out ground-state and excited-state calculations. However, because it includes no interaction between electronic states, MC-PDFT…

We have employed non-adiabatic molecular dynamics based on time-dependent density-functional theory to characterize the scattering behaviour of a proton with the Li$_4$ cluster. This technique assumes a classical approximation for the…

Atomic and Molecular Clusters · Physics 2015-05-27 Alberto Castro , Miguel Isla , Jose I. Martinez , Julio A. Alonso

We compare two recently developed strategies, implemented in open source software packages, for computing linear optical spectra in condensed phase environments in the presence of nonadiabatic effects. Both approaches rely on computing…

Chemical Physics · Physics 2024-08-14 Evan Lambertson , Dayana Bashirova , Kye E. Hunter , Benhardt Hansen , Tim J. Zuehlsdorff

Coupled cluster theory is one of the most accurate electronic structure methods for predicting ground and excited state chemistry. However, the presence of numerical artifacts at electronic degeneracies, such as complex energies, has made…

Chemical Physics · Physics 2024-05-16 Eirik F. Kjønstad , Sara Angelico , Henrik Koch

Due to their small size and unique properties, single-molecule electronics have long seen research interest from experimentalists and theoreticians alike. From a theoretical standpoint, modeling these systems using electronic structure…

Chemical Physics · Physics 2021-10-04 Andrew M. Sand , Justin T. Malme , Erik P. Hoy

Multiconfiguration pair-density functional theory (MC-PDFT) is a post-MCSCF multireference electronic-structure method that explicitly models strong electron correlation, and linearized pair-density functional theory (L-PDFT) is a recently…

For classical many-body systems subject to Brownian dynamics we develop a superadiabatic dynamical density functional theory (DDFT) for the description of inhomogeneous fluids out-of-equilibrium. By explicitly incorporating the dynamics of…

Soft Condensed Matter · Physics 2022-12-20 S. M. Tschopp , J. M. Brader

We show that the time dependent single electron, nuclear density matrix of an interacting electronic system coupled to nuclear degrees of freedom can be exactly reproduced by that of an electronic system with arbitrarily specified…

Materials Science · Physics 2009-02-07 Vinod Krishna

Time-dependent orbital-free density functional theory (TD-OFDFT) is an efficient ab-initio method for calculating the electronic dynamics of large systems. In comparison to standard TD-DFT, it computes only a single electronic state…

Chemical Physics · Physics 2021-12-15 Kaili Jiang , Xuecheng Shao , Michele Pavanello

Singlet fission (SF) is a very significant photophysical phenomenon and possesses potential applications. In this work, we try to give the rather detailed theoretical investigation of the SF process in the stacked polyacene dimer by…

Chemical Physics · Physics 2023-09-01 Jiawei Peng , Deping Hu , Hong Liu , Qiang Shi , Peng Bao , Zhenggang Lan

We present a new partially linearized mapping-based approach for approximating real-time quantum correlation functions in condensed-phase nonadiabatic systems, called spin-PLDM. Within a classical trajectory picture, partially linearized…

Chemical Physics · Physics 2021-02-03 J. R. Mannouch , J. O. Richardson

Analytic gradient routines are a desirable feature for quantum mechanical methods, allowing for efficient determination of equilibrium and transition state structures and several other molecular properties. In this work, we present…

Nonadiabatic ring-polymer molecular dynamics employs the mapping approach to describe nonadiabatic effects within the ring-polymer ansatz. In this paper, it is generalized to allow for the nuclear and electronic degrees of freedom to be…

Chemical Physics · Physics 2017-08-23 Jeremy O. Richardson , Philipp Meyer , Marc-Oliver Pleinert , Michael Thoss

In this contribution, we extend our framework for analyzing and visualizing correlated many-electron dynamics to non-variational, highly scalable electronic structure method. Specifically, an explicitly time-dependent electronic wave packet…

Chemical Physics · Physics 2017-04-27 Gunter Hermann , Vincent Pohl , Jean Christophe Tremblay

Multielectron tunneling ionization creates ionic coherence crucial for lasing and driving electron motion in molecules. While tunneling is well understood as a single active electron process, less emphasis has been placed on theoretical…

Quantum Physics · Physics 2026-04-23 Chi-Hong Yuen

Nonadiabatic coupling between electrons and molecular motion at metal surfaces leads to energy dissipation and dynamical steering effects during chemical surface dynamics. We present a theoretical approach to the scattering of molecules…

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

Electron-positron interactions have been utilized in various fields of science. Here we develop time-dependent multi-component density functional theory to study the coupled electron-positron dynamics from first principles. We prove that…

Chemical Physics · Physics 2018-10-03 Yasumitsu Suzuki , Satoshi Hagiwara , Kazuyuki Watanabe