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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

An accurate description of nonadiabatic dynamics of molecular species on metallic surfaces poses a serious computational challenge associated with a multitude of closely-spaced electronic states. We propose a mixed quantum-classical scheme…

Chemical Physics · Physics 2017-01-10 Ilya G. Ryabinkin , Artur F. Izmaylov

Attochemistry aims to exploit the properties of coherent electronic wavepackets excited via attosecond pulses, to control the formation of photoproducts. Such molecular processes can in principle be simulated with various nonadiabatic…

Chemical Physics · Physics 2024-05-28 Thierry Tran , Anthony Ferté , Morgane Vacher

Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as…

Chemical Physics · Physics 2016-05-24 Alexander White , Sergei Tretiak , Dmitry Mozyrsky

We developed a general theoretical approach and a user-ready computer code that permit to study the dynamics of collisional energy transfer and ro-vibrational energy exchange in complex molecule-molecule collisions. The method is a mixture…

Chemical Physics · Physics 2024-02-06 Carolin Joy , Bikramaditya Mandal , Dulat Bostan , Marie-Lise Dubernet , Dmitri Babikov

The ever-growing intersection of quantum electrodynamics (QED) and molecular processes has shown remarkable and unanticipated advancements in altering molecular properties and reactivity by exploiting light-matter couplings. In recent…

Chemical Physics · Physics 2023-11-09 Xinyang Li , Yu Zhang

The development of emerging technologies in quantum optics demands accurate models that faithfully capture genuine quantum effects. Mature semiclassical approaches reach their limits when confronted with quantized electromagnetic fields,…

Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…

Chemical Physics · Physics 2014-08-08 Wei Feng , Luting Xu , Xin-Qi Li , Weihai Fang , YiJing Yan

Mixed-quantum classical (MQC) methods for simulating the dynamics of molecules at metal surfaces have the potential to accurately and efficiently provide mechanistic insight into reactive processes. Here, we introduce simple two-dimensional…

Chemical Physics · Physics 2023-08-02 James Gardner , Scott Habershon , Reinhard J. Maurer

Trajectory-based mixed quantum-classical approaches to coupled electron-nuclear dynamics suffer from well-studied problems such as the lack of (or incorrect account for) decoherence in the trajectory surface hopping method and the inability…

Quantum Physics · Physics 2016-02-29 Federica Agostini , Seung Kyu Min , Ali Abedi , E. K. U. Gross

Mixed quantum-classical dynamics is a set of methods often used to understand systems too complex to treat fully quantum mechanically. Many techniques exist for full quantum mechanical evolution on quantum computers, but mixed…

Quantum Physics · Physics 2023-08-22 Daniel Bultrini , Oriol Vendrell

We develop a density matrix formalism to describe coupled electron-nuclear dynamics. To this end we introduce an effective Hamiltonian formalism that describes electronic transitions and small (quantum) nuclear fluctuations along a…

Chemical Physics · Physics 2020-09-07 Eugene Stolyarov , Alexander White , Dmitry Mozyrsky

We study the collective optical response of an atomic ensemble confined within a single-mode optical cavity by stochastic electrodynamics simulations that include the effects of atomic position correlations, internal level structure, and…

Quantum Physics · Physics 2017-08-28 Mark D. Lee , Stewart D. Jenkins , Yael Bronstein , Janne Ruostekoski

We extent the recently developed Multi-Layer Multi-Configuration Time-Dependent Hartree method for Bosons (ML-MCTDHB) for simulating the correlated quantum dynamics of bosonic mixtures to the fermionic sector and establish a unifying…

Quantum Physics · Physics 2017-10-31 L. Cao , V. Bolsinger , S. I. Mistakidis , G. M. Koutentakis , S. Krönke , J. M. Schurer , P. Schmelcher

We benchmark a selection of semiclassical and perturbative dynamics techniques by investigating the correlated evolution of a cavity-bound atomic system to assess their applicability to study problems involving strong light-matter…

Quantum Physics · Physics 2020-01-29 Norah M. Hoffmann , Christian Schäfer , Niko Säkkinen , Angel Rubio , Heiko Appel , Aaron Kelly

The dynamics of an electronic two-level system coupled to an electromagnetic field are simulated explicitly for one and three dimensional systems through semiclassical propagation of the Maxwell-Liouville equations. We consider three…

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

We consider the dynamics of interacting quantum and classical systems in the Heisenberg representation. Unlike the usual construction in standard quantum mechanics, mixed quantum-classical systems involve the interplay of unitary operators…

Chemical Physics · Physics 2025-05-26 David Martínez-Crespo , Cesare Tronci

We investigate detailed balance for a quantum system interacting with thermal radiation within mixed quantum-classical theory. For a two-level system coupled to classical radiation fields, three semiclassical methods are benchmarked: (1)…

Chemical Physics · Physics 2019-07-17 Hsing-Ta Chen , Tao E. Li , Abraham Nitzan , Joseph E. Subotnik

We develop and experimentally demonstrate a methodology for a full molecular frame quantum tomography (MFQT) of dynamical polyatomic systems. We exemplify this approach through the complete characterization of an electronically…

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