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We describe a path-integral molecular dynamics implementation of our recently developed golden-rule quantum transition-state theory (GR-QTST). The method is applied to compute the reaction rate in various models of electron transfer and…

Chemical Physics · Physics 2020-01-08 Wei Fang , Manish J. Thapa , Jeremy O. Richardson

A shortcut-to-adiabatic protocol for the realization of a fast and high-fidelity controlled-phase gate in Rydberg atoms is developed. The adiabatic state transfer, driven in the high-blockade limit, is sped up by compensating nonadiabatic…

Quantum Physics · Physics 2025-11-04 Luis S. Yagüe Bosch , Tim Ehret , Francesco Petiziol , Ennio Arimondo , Sandro Wimberger

A novel and readily understandable derivation of the Golden Rule of time dependent perturbation theory is presented. The derivation is based on adiabatic turning on of the perturbation as used, for instance, in some formal developments of…

Quantum Physics · Physics 2020-06-24 M G Burt

There is currently much interest in the development of improved trajectory-based methods for the simulation of nonadiabatic processes in complex systems. An important goal for such methods is the accurate calculation of the rate constant…

Chemical Physics · Physics 2014-09-04 Jeremy O. Richardson , Michael Thoss

The quantum phase transition in iron-based superconductors with 'half-Dirac' node at the electron Fermi surface as a $T=0$ structural phase transition described in terms of nematic order is discussed. An effective low energy theory that…

Strongly Correlated Electrons · Physics 2015-10-21 Imam Makhfudz

The crossover from nonadiabatic to adiabatic electron transfer has been theoretically studied under a spin-boson model (dissipative two-state system) description. We present numerically exact data for the thermal transfer rate and the…

Condensed Matter · Physics 2009-11-07 L. Muehlbacher , R. Egger

Instanton theory is an established method to calculate rate constants of chemical reactions including atom tunneling. Technical and methodological improvements increased its applicability. Still, a large number of energy and gradient…

Chemical Physics · Physics 2020-09-10 Jan Meisner , Johannes Kästner

At present, several models for quantum computation have been proposed. Adiabatic quantum computation scheme particularly offers this possibility and is based on a slow enough time evolution of the system, where no transitions take place. In…

Quantum Physics · Physics 2012-10-12 P. J. Salas Peralta

Using the idea of the instanton approach to quantum tunneling we try to obtain a method of calculating spontaneous fission rates for nuclei with the odd number of neutrons or protons. This problem has its origin in the failure of the…

Nuclear Theory · Physics 2020-11-11 W. Brodziński , J. Skalski

We investigate a simple and robust scheme for choosing the phases of adiabatic electronic states smoothly (as a function of geometry) so as to maximize the performance of ab initio non-adiabatic dynamics methods. Our approach is based upon…

Chemical Physics · Physics 2019-09-26 Zeyu Zhou , Zuxin Jin , Tian Qiu , Andrew M. Rappe , Joseph Eli Subotnik

Reactions involving adsorbates on metallic surfaces and impurities in bulk metals are ubiquitous in a wide range of technological applications. The theoretical modelling of such reactions presents a formidable challenge for theory because…

Chemical Physics · Physics 2022-05-17 Y. Litman , E. S. Pós , C. L. Box , R. Martinazzo , R. J. Maurer , M. Rossi

The Nonequilibrium Fermi's Golden Rule (NE-FGR) provides a convenient theoretical framework for calculating the charge transfer rate between a photoexcited bright donor electronic state and a dark acceptor electronic state, when the nuclear…

Quantum Physics · Physics 2025-09-17 Pouya Khazaei , Eitan Geva

The problem of escape of a Brownian particle in a cusp-shaped metastable potential is of special importance in nonadiabatic and weakly-adiabatic rate theory for electron transfer (ET) reactions. Especially, for the weakly-adiabatic…

Statistical Mechanics · Physics 2009-11-07 Bartlomiej Dybiec , Ewa Gudowska-Nowak , Pawel F. Gora

Transition State Theory is a central cornerstone in reaction dynamics. Its key step is the identification of a dividing surface that is crossed only once by all reactive trajectories. This assumption is often badly violated, especially when…

Chemical Physics · Physics 2015-05-07 F. Revuelta , Thomas Bartsch , R. M. Benito , F. Borondo

Ring-polymer instanton theory has been developed to simulate the quantum dynamics of molecular systems at low temperatures. Chemical reaction rates can be obtained by locating the dominant tunneling pathway and analyzing fluctuations around…

Chemical Physics · Physics 2019-03-25 Pierre Winter , Jeremy O. Richardson

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

The adiabatic approximation is a natural approach for the description of phenomena induced by low frequency laser radiation because the ratio of the laser frequency to the characteristic frequency of an atom or a molecule is a small…

Atomic Physics · Physics 2010-12-27 Denys Bondar

We propose a scheme which can produce desired nonadiabatic passages for the stimulated Raman transition in three-level systems. The state transfer in the protocol is realized by following the evolution of the dynamical basis itself and no…

Quantum Physics · Physics 2019-11-27 Hong Cao , Shao-Wu Yao , Li-Xiang Cen

Non-adiabatic decay rates for a radio-frequency dressed magnetic trap are calculated using Fermi's Golden Rule: that is, we examine the probability for a single atom to make transitions out of the dressed trap and into a continuum in the…

Atomic Physics · Physics 2017-09-06 Kathryn A Burrows , Barry M Garraway , Hélène Perrin

The passage through a critical point of a many-body quantum system leads to abundant nonadiabatic excitations. Here, we explore a regime, in which the critical point is not crossed although the system is passing slowly very close to it. We…

Statistical Mechanics · Physics 2024-02-19 Nikolai A. Sinitsyn , Vijay Ganesh Sadhasivam , Fumika Suzuki