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We introduce a novel methodology for simulating the excited-state dynamics of extensive molecular aggregates in the framework of the long-range corrected time-dependent density-functional tight-binding fragment molecular orbital method…

Chemical Physics · Physics 2024-04-23 Richard Einsele , Roland Mitrić

The time-development of photoexcitations in molecular aggregates exhibits specific dynamics of electronic states and vibrational wavefunction. We discuss the dynamical formation of entanglement between electronic and vibrational degrees of…

Quantum Physics · Physics 2007-05-23 Dmitri S. Kilin , Jeffrey A. Cina , Oleg V. Prezhdo

An ultra-strong photovoltaic effect has recently been reported for electrons trapped on a liquid Helium surface under a microwave excitation tuned at intersubband resonance [D. Konstantinov et. al. : J. Phys. Soc. Jpn. 81, 093601 (2012) ].…

Mesoscale and Nanoscale Physics · Physics 2013-07-24 F. Closa , E. Raphael , A. D. Chepelianskii

A procedure is developed to rigorously decompose experimental loss spectra of medium-energy electrons reflected from solid surfaces into contributions due to surface and volume electronic excitations. This can be achieved by analysis of two…

Materials Science · Physics 2009-11-11 Wolfgang S. M. Werner

We use a simple generic model to study the desorption of atoms from a solid surface in contact with a liquid, by using a combination of Monte Carlo and molecular dynamics simulations. The behavior of the system depends on two parameters:…

Chemical Physics · Physics 2022-11-16 Krishna Jaiswal , Horia Metiu , Vishal Agarwal

Density functional theory (DFT) based modeling of electronic excited states is of importance for investigation of the photophysical/photochemical properties and spectroscopic characterization of large systems. The widely used linear…

Chemical Physics · Physics 2021-05-11 Diptarka Hait , Martin Head-Gordon

We simulate the femtosecond laser induced desorption dynamics of a diatomic molecule from a metal surface by including the effect of the electron and phonon excitations created by the laser pulse. Following previous models, the laser…

Materials Science · Physics 2016-01-14 Ivor Lončarić , M. Alducin , P. Saalfrank , J. I. Juaristi

The interaction of hydrogen with many transition metal surfaces is characterized by a coexistence of activated with non-activated paths to adsorption with a broad distribution of barrier heights. By performing six-dimensional quantum…

Condensed Matter · Physics 2007-05-23 Axel Gross , Matthias Scheffler

We study the rotational and vibrational heating of diatomic molecules placed near a surface at finite temperature on the basis of macroscopic quantum electrodynamics. The internal molecular evolution is governed by transition rates that…

Quantum Physics · Physics 2009-12-14 Stefan Yoshi Buhmann , M. R. Tarbutt , Stefan Scheel , E. A. Hinds

During the exothermic adsorption of molecules at solid surfaces dissipation of the released energy occurs via the excitation of electronic and phononic degrees of freedom. For metallic substrates the role of the nonadiabatic electronic…

Materials Science · Physics 2015-03-19 Jörg Meyer , Karsten Reuter

The potential energy surface (PES) of dissociative adsorption of H_2 on Pd(100) is investigated using density functional theory and the full-potential linear augmented plane wave (FP-LAPW) method. Several dissociation pathways are…

mtrl-th · Physics 2009-10-28 Steffen Wilke , Matthias Scheffler

Density matrix embedding theory (DMET) provides a framework to describe ground-state expectation values in strongly correlated systems, but its extension to dynamical quantities is still an open problem. We show one route to obtaining…

Strongly Correlated Electrons · Physics 2025-11-13 Shuoxue Li , Chenghan Li , Huanchen Zhai , Garnet Kin-Lic Chan

We theoretically study hot electron generation through the emission of a dipole source coupled to a nanoresonator on a metal surface. In our hybrid approach, we solve the time-harmonic Maxwell's equations numerically and apply a quantum…

We present a state-space-based path integral method to calculate the rate of electron transfer (ET) in multi-state, multi-electron condensed-phase processes. We employ an exact path integral in discrete electronic states and continuous…

Chemical Physics · Physics 2016-06-07 Jessica Ryan Duke , Nandini Ananth

Heterogeneous catalysis of adsorbates on metallic surfaces mediated by plasmon has potential high photoelectric conversion efficiency and controllable reaction selectivity. Theoretical modeling of dynamical reaction processes provides…

Chemical Physics · Physics 2023-06-05 Xiaoyan Wu , Tammo van der Heide , Thomas Frauenheim , Sergei Tretiak , ChiYung Yam , Yu Zhang

We present a real-time path integral theory for the rate of electron transfer reactions. Using graph theoretic techniques, the dynamics is expressed in a formally exact way as a set of integral equations. With a simple approximation for the…

chem-ph · Physics 2009-10-28 Juergen T. Stockburger , C. H. Mak

Excited-state intramolecular proton transfer (ESIPT) is a fundamental photochemical process in which photoexcitation induces proton transfer within a molecule, leading to the formation of a tautomeric excited state. It was observed…

Chemical Physics · Physics 2026-03-03 Alessandro Nicola Nardi , Morgane Vacher

We investigate the time an electronic excitation travels in a supermolecular setup using a measurement process in an open quantum-system framework. The approach is based on the stochastic Schr\"odinger equation and uses a Hamiltonian from…

Materials Science · Physics 2013-12-09 Dirk Hofmann , Heiko Appel , Massimiliano Di Ventra , Stephan Kümmel

We propose a method using reduced size of Hilbert space to describe an electron dynamics in molecule and aggregate based on our previous theoretical scheme [ T. Yonehara and T. Nakajima, J. Chem. Phys. \textbf{147}, 074110 (2017) ]. The…

Chemical Physics · Physics 2019-09-09 Takehiro Yonehara , Takahito Nakajima

At the Mott transition, electron-electron interaction changes a metal, in which electrons are itinerant, to an insulator, in which electrons are localized. This phenomenon is central to quantum materials. Here we contribute to its…

Strongly Correlated Electrons · Physics 2019-02-20 C. Walsh , P. Sémon , D. Poulin , G. Sordi , A. -M. S. Tremblay