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We present a dynamical simulation scheme to model the highly correlated excited state dynamics of linear polyenes. We apply it to investigate the internal conversion processes of carotenoids following their photoexcitation. We use the…

Chemical Physics · Physics 2023-07-19 Dilhan Manawadu , Darren J. Valentine , William Barford

Mixed quantum-classical mechanics descriptions are critical to modeling coupled electron-nuclear dynamics, i.e. non-adiabatic molecular dynamics, relevant to photochemical and photophysical processes. We argue that, for polyatomic…

Chemical Physics · Physics 2018-08-21 Roman Baskov , Alexander White , Dmitry Mozyrsky

We employ the time-dependent Hartree-Fock (TDHF) method to study various aspects of the reactions utilized in searches for superheavy elements. These include capture cross-sections, quasifission, prediction of $P_{\mathrm{CN}}$, and other…

Nuclear Theory · Physics 2016-04-12 A. S. Umar , V. E. Oberacker

Time-dependent density-functional theory (TDDFT) is widely used to describe electronic excitations in complex finite systems with large numbers of atoms, such as biomolecules and nanocrystals. The first part of this paper will give a simple…

Materials Science · Physics 2008-08-15 C. A. Ullrich , V. Turkowski

We investigate optical absorption spectra obtained through time-dependent density functional theory (TD-DFT) based on nonempirical hybrid functionals that are designed to correctly reproduce the dielectric function. The comparison with…

Materials Science · Physics 2020-08-17 Alexey Tal , Peitao Liu , Georg Kresse , Alfredo Pasquarello

We present an application of our new theoretical formulation of quantum dynamics, moment propagation theory (MPT) (Boyer et al., J. Chem. Phys. 160, 064113 (2024)), for employing machine-learning techniques to simulate the quantum dynamics…

Chemical Physics · Physics 2024-12-09 Nicholas J. Boyer , Christopher Shepard , Ruiyi Zhou , Jianhang Xu , Yosuke Kanai

We present the molecular hyperdynamics algorithm and its implementation to the nonorthogonal tight-binding model NTBM and the corresponding software. Due to its multiscale structure, the proposed approach provides the long time scale…

Spectroscopy is an indispensable tool in understanding the structures and dynamics of molecular systems. However computational modelling of spectroscopy is challenging due to the exponential scaling of computational complexity with system…

Quantum Physics · Physics 2021-06-22 Chee-Kong Lee , Chang-Yu Hsieh , Shengyu Zhang , Liang Shi

Despite the variety of available computational approaches, state-of-the-art methods for calculating excitation energies such as time-dependent density functional theory (TDDFT), are computationally demanding and thus limited to moderate…

Chemical Physics · Physics 2022-03-10 Martina Stella , Kritam Thapa , Luigi Genovese , Laura E. Ratcliff

We implemented various DFT+U schemes, including the ACBN0 self-consistent density-functional version of the DFT+U method [Phys. Rev. X 5, 011006 (2015)] within the massively parallel real-space time-dependent density functional theory…

Strongly Correlated Electrons · Physics 2017-12-27 Nicolas Tancogne-Dejean , Micael J. T. Oliveira , Angel Rubio

Time-dependent density functional theory is widely used to describe excitations of many-fermion systems. In its many applications, 3D coordinate-space representation is used, and infinite-domain calculations are limited to a finite volume…

Nuclear Theory · Physics 2016-05-11 B. Schuetrumpf , W. Nazarewicz , P. -G. Reinhard

The non-radiative electron-relaxation dynamics in C$_{60}$ molecule is studied after selective initial photoexcitations. The methodology includes nonadibabtic molecular simulation combined with time-dependent density functional theory (DFT)…

Atomic and Molecular Clusters · Physics 2023-06-29 Esam Ali , Mohamed El-Amine Madjet , Ruma De , Thomas Frauenheim , Himadri S. Chakraborty

We propose a framework to learn the time-dependent Hartree-Fock (TDHF) inter-electronic potential of a molecule from its electron density dynamics. Though the entire TDHF Hamiltonian, including the inter-electronic potential, can be…

Chemical Physics · Physics 2024-12-05 Harish S. Bhat , Prachi Gupta , Christine M. Isborn

Recent advances in laser technology allow us to follow electronic motion at its natural time-scale with ultra-fast time resolution, leading the way towards attosecond physics experiments of extreme precision. In this work, we assess the use…

Other Condensed Matter · Physics 2016-06-22 Jessica Walkenhorst , Umberto De Giovannini , Alberto Castro , Angel Rubio

To explore whether the density-functional theory non-equilibrium Green's function formalism (DFT-NEGF) provides a rigorous framework for quantum transport, we carried out time-dependent density functional theory (TDDFT) calculations of the…

Materials Science · Physics 2011-07-01 ChiYung Yam , Xiao Zheng , GuanHua Chen , Yong Wang , Thomas Frauenheim , Thomas A. Niehaus

The time-dependent density functional theory (TDDFT) provides a unified description of the structure and reaction. The linear approximation leads to the random-phase approximation (RPA) which is capable of describing a variety of collective…

Nuclear Theory · Physics 2016-05-09 Kai Wen , Kouhei Washiyama , Ni Fang , Takashi Nakatsukasa

We present the basic concepts and recent developments in the time-dependent density functional theory (TDDFT) for describing nuclear dynamics at low energy. The symmetry breaking is inherent in nuclear energy density functionals (EDFs),…

Nuclear Theory · Physics 2016-12-21 Takashi Nakatsukasa , Kenichi Matsuyanagi , Masayuki Matsuo , Kazuhiro Yabana

We benchmark a set of quantum-chemistry methods, including multitrajectory Ehrenfest, fewest-switches surface-hopping, and multiconfigurational-Ehrenfest dynamics, against exact quantum-many-body techniques by studying real-time dynamics in…

We introduce real-time density matrix embedding theory (DMET), a dynamical quantum embedding theory for computing non-equilibrium electron dynamics in strongly correlated systems. As in the previously developed static DMET, real-time DMET…

Chemical Physics · Physics 2017-11-03 Joshua S. Kretchmer , Garnet Kin-Lic Chan

Recent advances in numerically exact quantum dynamics methods have brought the dream of accurately modeling the dynamics of chemically complex open systems within reach. Path-integral-based methods, hierarchical equations of motion (HEOM)…

Chemical Physics · Physics 2025-04-08 Roman Korol , Xinxian Chen , Ignacio Franco