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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

In this article we show how Ehrenfest mean field theory can be made both a more accurate and efficient method to treat nonadiabatic quantum dynamics by combining it with the generalized quantum master equation framework. The resulting mean…

Chemical Physics · Physics 2015-06-23 Aaron Kelly , Nora Brackbill , Thomas E. Markland

Nonadiabatic quantum-classical mapping approaches have significantly gained in popularity in the past several decades because they have acceptable accuracy while remaining numerically tractable even for large system sizes. In the recent few…

Chemical Physics · Physics 2024-10-03 Haifeng Lang , Philipp Hauke

Quantum dynamics (i.e., the Schr\"odinger equation) and classical dynamics (i.e., Hamilton equations) can both be formulated in equal geometric terms: a Poisson bracket defined on a manifold. In this paper we first show that the hybrid…

Chemical Physics · Physics 2013-06-21 J. L. Alonso , A. Castro , J. Clemente-Gallardo , J. C. Cuchí , P. Echenique , F. Falceto

Ehrenfest urns with interaction that are connected in a ring is considered as a paradigm model for non-equilibrium thermodynamics and is shown to exhibit two distinct non-equilibrium steady states (NESS) of uniform and non-uniform particle…

Statistical Mechanics · Physics 2021-06-03 Chi-Ho Cheng , Pik-Yin Lai

We present a Lagrangian-based implementation of Ehrenfest dynamics with nuclear-electronic orbital (NEO) theory and real-time time-dependent density functional theory (RT-TDDFT) for extended periodic systems. In addition to a quantum…

Chemical Physics · Physics 2024-07-29 Jianhang Xu , Ruiyi Zhou , Tao E. Li , Sharon Hammes-Schiffer , Yosuke Kanai

We present a novel quantum-classical approach to non-adiabatic dynamics, deduced from the coupled electronic and nuclear equations in the framework of the exact factorization of the electron-nuclear wave function. The method is based on the…

Chemical Physics · Physics 2015-08-19 Seung Kyu Min , Federica Agostini , E. K. U. Gross

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

Conical intersections are common in molecular physics and photochemistry, and are often invoked to explain observed reaction products. A conical intersection can occur when an excited electronic potential energy surface intersects with the…

Quantum Physics · Physics 2023-02-06 Jacob Whitlow , Zhubing Jia , Ye Wang , Chao Fang , Jungsang Kim , Kenneth R. Brown

We propose a numerical method which embeds the variational non-Gaussian wavefunction approach within exact diagonalization, allowing for efficient treatment of correlated systems with both electron-electron and electron-phonon interactions.…

Strongly Correlated Electrons · Physics 2020-11-24 Yao Wang , Ilya Esterlis , Tao Shi , J. Ignacio Cirac , Eugene Demler

The violation of detailed balance poses a serious problem for the majority of current quasiclassical methods for simulating nonadiabatic dynamics. In order to analyze the severity of the problem, we predict the long-time limits of the…

Quantum Physics · Physics 2023-11-20 Graziano Amati , Jonathan R. Mannouch , Jeremy O. Richardson

Choosing an appropriate representation of the molecular Hamiltonian is one of the challenges faced by simulations of the nonadiabatic quantum dynamics around a conical intersection. The adiabatic, exact quasidiabatic, and strictly diabatic…

Chemical Physics · Physics 2024-09-26 Seonghoon Choi , Jiří Vaníček

Conical intersections are ubiquitous in polyatomic molecules and responsible for a wide range of phenomena in chemistry and physics. We introduce and implement a local diabatic representation for the correlated electron-nuclear dynamics…

Quantum Physics · Physics 2023-10-18 Bing Gu

The dynamics of quantum expectation values is considered in a geometric setting. First, expectation values of the canonical operators are shown to be equivariant momentum maps for the action of the Heisenberg group on quantum states. Then,…

Mathematical Physics · Physics 2016-05-18 Esther Bonet-Luz , Cesare Tronci

We study the mean-field dynamics and the reduced-dimension character of two-mode Bose-Einstein condensates (BECs) in highly anisotropic traps. By means of perturbative techniques, we show that the tightly confined (transverse) degrees of…

Quantum Gases · Physics 2013-02-07 Alexandre B. Tacla , Carlton M. Caves

We investigate the accuracy and efficiency of the semiclassical Frozen Gaussian method in describing electron dynamics in real time. Model systems of two soft-Coulomb-interacting electrons are used to study correlated dynamics under…

Chemical Physics · Physics 2015-05-30 Peter Elliott , Neepa T. Maitra

Quantum embedding approaches involve the self-consistent optimization of a local fragment of a strongly correlated system, entangled with the wider environment. The `energy-weighted' density matrix embedding theory (EwDMET) was established…

Strongly Correlated Electrons · Physics 2021-02-23 P. V. Sriluckshmy , Max Nusspickel , Edoardo Fertitta , George H. Booth

Conical intersections are ubiquitous in chemistry and physics, often governing processes such as light harvesting, vision, photocatalysis, and chemical reactivity. They act as funnels between electronic states of molecules, allowing rapid…

Processes involving ultrafast laser driven electron-phonon dynamics play a fundamental role in the response of quantum systems in a growing number of situations of interest, as evidenced by phenomena such as strongly driven phase…

Materials Science · Physics 2024-03-01 Kevin Lively , Shunsuke A. Sato , Guillermo Albareda , Angel Rubio , Aaron Kelly

We study quantum circuits consisting of unitary gates, projective measurements, and control operations that steer the system towards a pure absorbing state. Two types of phase transition occur as the rate of these control operations is…

Quantum Physics · Physics 2023-06-07 Lorenzo Piroli , Yaodong Li , Romain Vasseur , Adam Nahum