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We develop and implement an exact conical intersection nonadiabatic wave packet dynamics method that combines the local diabatic representation, Strang splitting for the total molecular propagator, and discrete variable representation with…

Chemical Physics · Physics 2024-04-23 Bing Gu

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 (stationary) Schr\"{o}dinger equation for atomistic systems is solved using the adiabatic potential energy curves (PECs) and the associated adiabatic approximation. Despite being very simplistic, this approach is very powerful and used…

Chemical Physics · Physics 2023-12-22 Ryan P. Brady , Charlie Drury , Sergei N. Yurchenko , Jonathan Tennyson

We propose to measure nonadiabaticity of molecular quantum dynamics rigorously with the quantum fidelity between the Born-Oppenheimer and fully nonadiabatic dynamics. It is shown that this measure of nonadiabaticity applies in situations…

Chemical Physics · Physics 2012-06-28 Tomas Zimmermann , Jiri Vanicek

A classical approach for solving discrete time nonlinear control on a finite horizon consists in repeatedly minimizing linear quadratic approximations of the original problem around current candidate solutions. While widely popular in many…

Optimization and Control · Mathematics 2025-07-08 Vincent Roulet , Siddhartha Srinivasa , Maryam Fazel , Zaid Harchaoui

We build on the concept of eigenvector continuation to develop an efficient multi-state method for the rigorous and smooth interpolation of a small training set of many-body wavefunctions through chemical space at mean-field cost. The…

Chemical Physics · Physics 2024-05-02 Kemal Atalar , Yannic Rath , Rachel Crespo-Otero , George H. Booth

The global many-electron wave function overlap matrix accounts for all effects beyond the Born-Oppenheimer approximation in the discrete variable local diabatic representation, a numerically exact framework for modeling nonadiabatic conical…

Chemical Physics · Physics 2025-01-10 Yujuan Xie , Bing Gu

We perform model calculations for a stretched LiF molecule, demonstrating that nonadiabatic charge transfer effects can be accurately and seamlessly described within a density functional framework. In alkali halides like LiF, there is an…

Chemical Physics · Physics 2018-03-01 Chen Li , Ryan Requist , E. K. U. Gross

This report presents a new approach for treating the coupling of electrons and nuclei in quantum mechanical calculations for molecules and condensed matter. It includes the standard "Born-Oppenheimer approximation" as a special case but…

Chemical Physics · Physics 2013-06-28 Gerald I. Kerley

We develop a nondirect product discrete variable representation (npDVR) for treating quantum dynamical problems which involve nonseparable angular variables. The npDVR basis is constructed on spherical functions orthogonalized on the grids…

Computational Physics · Physics 2020-01-07 Sara Shadmehri , Shahpoor Saeidian , Vladimir S. Melezhik

Given the prevalence of superconducting platforms for uses in quantum computing and quantum sensing, the simulation of quantum superconducting circuits has become increasingly important for identifying system characteristics and modeling…

Quantum Physics · Physics 2026-03-09 Brittany Richman , C. J. Lobb , Jacob M. Taylor

We propose an approximate method for evaluating the importance of non-Born-Oppenheimer effects on the quantum dynamics of nuclei. The method uses a generalization of the dephasing representation (DR) of quantum fidelity to several diabatic…

Chemical Physics · Physics 2013-01-15 Tomas Zimmermann , Jiri Vanicek

Real-time simulations of laser-driven electron dynamics contain information about molecular optical properties through all orders in response theory. These properties can be extracted by assuming convergence of the power series expansion of…

A novel treatment of non-adiabatic couplings is proposed. The derivation starts from the long-known, but not well-known, fact that the wave function of the complete system of elctrons and nuclei can be written, without approximation, as a…

Materials Science · Physics 2007-05-23 Nikitas I. Gidopoulos , E. K. U. Gross

This thesis develops a general theoretical and numerical framework for achieving high-contrast atom interferometry based on double Bragg diffraction (DBD). While DBD offers intrinsic symmetry, reduced sensitivity to internal-state…

Quantum Physics · Physics 2026-03-25 Rui Li

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

We investigate the efficiency of approximate counterdiabatic driving (CD) in accelerating adiabatic passage through exponentially small gaps. First, we analyze a minimal spin-glass bottleneck model that is analytically tractable and…

Quantum Physics · Physics 2025-10-14 András Grabarits , Federico Balducci , Adolfo del Campo

A new methodology of simulating nonadiabatic dynamics using frozen-width Gaussian wavepackets within the moving crude adiabatic representation with the on-the-fly evaluation of electronic structure is presented. The main feature of the new…

Chemical Physics · Physics 2018-04-04 Loïc Joubert-Doriol , Artur F. Izmaylov

Excited-state molecular dynamics (ESMD) simulations near conical intersections (CIs) pose significant challenges when using machine learning potentials (MLPs). Although MLPs have gained recognition for their integration into mixed…

Chemical Physics · Physics 2025-01-17 Sung Wook Moon , Soohaeng Yoo Willow , Tae Hyeon Park , Seung Kyu Min , Chang Woo Myung

We study the generation of electronic ring currents in the presence of nonadiabatic coupling using circularly polarized light. For this, we introduce a solvable model consisting of an electron and a nucleus rotating around a common center…

Chemical Physics · Physics 2021-02-03 Krishna R. Nandipati , Oriol Vendrell
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