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Diabatization of the molecular Hamiltonian is a standard approach to removing the singularities of nonadiabatic couplings at conical intersections of adiabatic potential energy surfaces. In general, it is impossible to eliminate the…

Chemical Physics · Physics 2021-03-26 Seonghoon Choi , Jiří Vaníček

Chemical relaxation phenomena, including photochemistry and electron transfer processes, form a vigorous area of research in which nonadiabatic dynamics plays a fundamental role. Here, we show that for nonadiabatic dynamics with two…

Chemical Physics · Physics 2022-07-20 Yanze Wu , Xuezhi Bian , Jonathan Rawlinson , Robert G. Littlejohn , Joseph E. Subotnik

Applying time-dependent driving is a basic way of quantum control. Driven systems show various dynamics as its time scale is changed due to the different amount of nonadiabatic transitions. The fast-forward scaling theory enables us to…

Quantum Physics · Physics 2023-07-19 Takuya Hatomura

We present a framework for simulating the open dynamics of spin-boson systems by combining variational non-Gaussian states with a quantum trajectories approach. We apply this method to a generic spin-boson Hamiltonian that has both…

We present an efficient \textit{ab initio} algorithm for quantum dynamics simulations of interacting systems that is based on the conditional decomposition of the many-body wavefunction [Phys. Rev. Lett. 113, 083003 (2014)]. Starting with…

Mesoscale and Nanoscale Physics · Physics 2019-02-27 Guillermo Albareda , Aaron Kelly , Angel Rubio

We propose a trajectory-based method for simulating nonadiabatic dynamics in molecular systems with two coupled electronic states. Employing a quantum-mechanically exact mapping of the two-level problem to a spin-1/2 coherent state, we…

Chemical Physics · Physics 2020-03-03 Johan E. Runeson , Jeremy O. Richardson

The theoretical investigation of non-adiabatic processes is hampered by the complexity of the coupled electron-nuclear dynamics beyond the Born-Oppenheimer approximation. Classically, the simulation of such reactions is limited by the…

Quantum Physics · Physics 2021-01-06 Pauline J. Ollitrault , Guglielmo Mazzola , Ivano Tavernelli

We present an overview of the role of quantum coherence in influencing nonadiabatic processes in the condensed phase. Equations of motion for mixed quantum-classical dynamics are derived from the Consistent Histories interpretation of…

Chemical Physics · Physics 2008-02-03 Eric R. Bittner

We introduce and apply a numerically exact method for investigating the real-time dissipative dynamics of quantum impurities embedded in a macroscopic environment beyond the weak-coupling limit. We focus on the spin-boson Hamiltonian that…

Strongly Correlated Electrons · Physics 2013-02-04 Peter P. Orth , Adilet Imambekov , Karyn Le Hur

A stochastic representation of the dynamics of open quantum systems, suitable for non-perturbative system-reservoir interaction, non-Markovian effects and arbitrarily driven systems is presented. It includes the case of driving on…

Statistical Mechanics · Physics 2016-10-05 Jürgen T. Stockburger

Fast nonadiabatic control protocols known as shortcuts to adiabaticity have found a plethora of applications, but their use has been severely limited to speeding up the dynamics of isolated quantum systems. We introduce shortcuts for open…

Quantum Physics · Physics 2020-08-06 L. Dupays , I. L. Egusquiza , A. del Campo , A. Chenu

Following on from our recent work, we investigate a stochastic approach to non-equilibrium quantum spin systems. We show how the method can be applied to a variety of physical observables and for different initial conditions. We provide…

Statistical Mechanics · Physics 2020-01-24 S. De Nicola , B. Doyon , M. J. Bhaseen

On-the-fly quantum nonadiabatic dynamics for large systems greatly benefits from the adiabatic representation readily available from the electronic structure programs. However, frequently occurring in this representation conical…

The quantum-classical Liouville equation offers a rigorous approach to nonadiabatic quantum dynamics based on surface hopping type trajectories. However, in practice the applicability of this approach has been limited to short times owing…

Chemical Physics · Physics 2015-06-16 Aaron Kelly , Thomas E. Markland

The study of non-equilibrium dynamics is one of the most important challenges of modern quantum many-body physics, in relationship with fundamental questions in quantum statistical mechanics, as well as with the fields of quantum simulation…

Quantum Gases · Physics 2023-06-14 Raphaël Menu , Tommaso Roscilde

We study a number of filtering schemes for the reduction of the statistical error in non-adiabatic calculations by means of the quantum-classical Liouville equation. In particular, we focus on a scheme based on setting a threshold value on…

Quantum Physics · Physics 2016-10-21 Daniel Uken , Alessandro Sergi , Francesco Petruccione

The dynamics of spin-boson systems at very low temperatures has been studied using a real-time path-integral simulation technique which combines a stochastic Monte Carlo sampling over the quantum fluctuations with an exact treatment of the…

chem-ph · Physics 2009-10-22 Reinhold Egger , C. H. Mak

We study nonadiabatic electron transfer within the biased spin-boson model. We calculate the incoherent transfer rate in analytic form at all temperatures for a power law form of the spectral density of the solvent coupling. In the Ohmic…

Statistical Mechanics · Physics 2009-10-31 G. Lang , E. Paladino , U. Weiss

We present a method to study rare nonadiabatic dynamics in open quantum systems using transition path sampling and quantum jump trajectories. As with applications of transition path sampling to classical dynamics, the method does not rely…

Statistical Mechanics · Physics 2021-12-08 Addison J. Schile , David T. Limmer

We provide a general formula of quantum transfer that includes the non-adiabatic effect under periodic environmental modulation by using full counting statistics in Hilbert-Schmidt space. Applying the formula to an anharmonic junction model…

Quantum Physics · Physics 2014-05-09 Chikako Uchiyama