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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

Nonadiabatic geometric quantum computation provides a means to perform fast and robust quantum gates. It has been implemented in various physical systems, such as trapped ions, nuclear magnetic resonance and superconducting circuits.…

Quantum Physics · Physics 2017-12-06 P. Z. Zhao , Xiao-Dan Cui , G. F. Xu , Erik Sjöqvist , D. M. Tong

Accurate and efficient methods to simulate nonadiabatic and quantum nuclear effects in high-dimensional and dissipative systems are crucial for the prediction of chemical dynamics in condensed phase. To facilitate effective development,…

The recent improvement in experimental capabilities for interrogating and controlling molecular systems with ultrafast coherent light sources calls for the development of theoretical approaches that can accurately and efficiently treat…

Chemical Physics · Physics 2024-08-20 Jonathan R. Mannouch , Aaron Kelly

We developed a method which performs the coupled adiabatic spin and lattice dynamics based on the tight-binding electronic structure model, where the intrinsic magnetic field and ionic forces are calculated from the converged…

In this study, two different simple and intuitive semiempirical schemes for computing approximate non-adiabatic coupling vectors (NACVs) between the ground and excited electronic states are presented. The first approximation makes use of…

Chemical Physics · Physics 2019-08-02 Alexander Humeniuk , Roland Mitrić

Rabi oscillations have long been thought to be out of reach in simulations using time-dependent density functional theory (TDDFT), a prominent symptom of the failure of the adiabatic approximation for non-perturbative dynamics. We present a…

Chemical Physics · Physics 2024-06-21 Davood B. Dar , Anna Baranova , Neepa T. Maitra

The simulation of adiabatic evolution has deep connections with Adiabatic Quantum Computation, the Quantum Approximate Optimization Algorithm and adiabatic state preparation. Here we address the error analysis problem in quantum simulation…

Quantum Physics · Physics 2022-02-09 Changhao Yi

The applicability of the density functional based tight binding (DFTB) method to the description of hydrogen bond dynamics and infrared spectroscopy is addressed for the exemplary protic ionic liquid triethylammonium nitrate. Potential…

Chemical Physics · Physics 2017-01-04 Tobias Zentel , Oliver Kühn

A generalized formalism of the so-called non-adiabatic quantum molecular dynamics is presented, which applies for atomic many-body systems in external laser fields. The theory treats the nuclear dynamics and electronic transitions…

Atomic Physics · Physics 2007-05-23 Thomas Kunert , Ruediger Schmidt

An extension of the CCS-method [Chem. Phys. 2004, 304, p. 103-120] for simulating non-adiabatic dynamics with quantum effects of the nuclei is put forward. The time-dependent Schr\"{o}dinger equation for the motion of the nuclei is solved…

Chemical Physics · Physics 2016-07-27 Alexander Humeniuk , Roland Mitrić

In silico materials design is hampered by the computational complexity of Kohn-Sham DFT, which scales cubically with the system size. Owing to the development of new-generation kinetic energy density functionals (KEDFs), orbital-free DFT…

Computational Physics · Physics 2020-08-24 Xuecheng Shao , Kaili Jiang , Wenhui Mi , Alessandro Genova , Michele Pavanello

The non-radiative electron-relaxation dynamics in C$_{60}$ molecule is studied after selective initial photoexcitations. The methodology includes nonadibabtic molecular simulation combined with time-dependent density functional theory (DFT)…

Atomic and Molecular Clusters · Physics 2023-06-29 Esam Ali , Mohamed El-Amine Madjet , Ruma De , Thomas Frauenheim , Himadri S. Chakraborty

Time-dependent density-functional theory (TDDFT) treats dynamical exchange and correlation (xc) via a single-particle potential, Vxc(r,t), defined as a nonlocal functional of the density n(r',t'). The popular adiabatic local-density…

Mesoscale and Nanoscale Physics · Physics 2009-11-11 C. A. Ullrich , I. V. Tokatly

The high-speed implementation and robustness against of non-adiabatic holonomic quantum computation provide a new idea for overcoming the difficulty of quantum system interacting with the environment easily decoherence, which realizing…

Quantum Physics · Physics 2020-03-31 Guo-An Yan , Jia-Xin Chen , Hua Lu , Ai-Xi Chen

Molecular dynamics (MD) simulations play a crucial role in resolving the underlying conformational dynamics of molecular systems. However, their capability to correctly reproduce and predict dynamics in agreement with experiments is limited…

Chemical Physics · Physics 2025-05-19 Ivan Gilardoni , Valerio Piomponi , Thorben Fröhlking , Giovanni Bussi

Recently, nonadiabatic geometric quantum computation has been received great attentions, due to its fast operation and intrinsic error resilience. However, compared with the corresponding dynamical gates, the robustness of implemented…

Quantum Physics · Physics 2023-07-12 Cheng-Yun Ding , Li Chen , Li-Hua Zhang , Zheng-Yuan Xue

Microscopic methods and tools to describe nuclear dynamics have considerably been improved in the past few years. They are based on the time-dependent Hartree-Fock (TDHF) theory and its extensions to include pairing correlations and quantum…

Nuclear Theory · Physics 2018-09-13 C. Simenel , A. S. Umar

Most applications of time-dependent density-functional theory (TDDFT) use the adiabatic local-density approximation (ALDA) for the dynamical exchange-correlation potential Vxc(r,t). An exact (i.e., nonadiabatic) extension of the…

Mesoscale and Nanoscale Physics · Physics 2015-06-25 C. A. Ullrich

We develop a trajectory-based approach for excited-state molecular dynamics simulations of systems subject to an external periodic drive. We combine the exact-factorization formalism, allowing to treat electron-nuclear systems in…

Chemical Physics · Physics 2021-03-31 Marco Schirò , Florian G. Eich , Federica Agostini
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