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A novel method of coherent manipulation of the electron tunneling in quantum-dots is proposed, which utilizes the quantum interference in nonadiabatic double-crossing of the discrete energy levels. In this method, we need only a smoothly…

Mesoscale and Nanoscale Physics · Physics 2009-11-10 Keiji Saito , Yosuke Kayanuma

Nonadiabatic ring-polymer molecular dynamics employs the mapping approach to describe nonadiabatic effects within the ring-polymer ansatz. In this paper, it is generalized to allow for the nuclear and electronic degrees of freedom to be…

Chemical Physics · Physics 2017-08-23 Jeremy O. Richardson , Philipp Meyer , Marc-Oliver Pleinert , Michael Thoss

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

We present a detailed derivation and numerical tests of a new mixed quantum-classical scheme to deal with non-adiabatic processes. The method is presented as the zero-th order approximation to the exact coupled dynamics of electrons and…

Chemical Physics · Physics 2015-06-22 Federica Agostini , Ali Abedi , E. K. U. Gross

Electron transfer is an important and fundamental process in chemistry, biology and physics, and has received significant attention in recent years. Perhaps one of the most intriguing questions concerns with the realization of the…

Mesoscale and Nanoscale Physics · Physics 2023-05-30 Bokang Hou , Michael Thoss , Uri Banin , Eran Rabani

A derivation of non-adiabatic coupling vectors for the density functional based tight binding method (DFTB) between ground and excited states is presented. The analytical result is valid both for semi-local and long-range corrected DFTB and…

Chemical Physics · Physics 2020-10-29 Thomas A. Niehaus

A relativistic version of the coupled-cluster single-double (CCSD) method is developed for atoms with a single valence electron. In earlier work, a linearized version of the CCSD method (with extensions to include a dominant class of triple…

Atomic Physics · Physics 2009-11-13 Rupsi Pal , M. S. Safronova , W. R. Johnson , Andrei Derevianko , Sergey G. Porsev

A cluster state cannot be a unique ground state of a two-body interacting Hamiltonian. Here, we propose the creation of a cluster state of logical qubits encoded in spin-1/2 particles by adiabatically weakening two-body interactions. The…

Quantum Physics · Physics 2014-10-30 Thi Ha Kyaw , Ying Li , Leong Chuan Kwek

Non-adiabatic coupling matrix elements (NACMEs) are important in quantum chemistry, particularly for molecular dynamics methods such as surface hopping. However, NACMEs are gauge dependent. This presents a difficulty for their calculation…

Chemical Physics · Physics 2024-07-23 Tanner Culpitt , Erik I. Tellgren , Laurens D. M. Peters , Trygve Helgaker

We analyze the electric dipole moments (PDMs) and static electric dipole polarizabilities of the alkali--alkaline-earth (Alk-AlkE) dimers by employing finite-field coupled-cluster methods, both in the frameworks of non-relativistic and…

Atomic Physics · Physics 2022-06-29 R. Mitra , V. S. Prasannaa , B. K. Sahoo

This work identifies geometric effects on dynamics due to nonadiabatic couplings in Born Oppenheimer systems and provides a systematic method for deriving corrections to mixed quantum-classical methods. Specifically, an exact path integral…

Chemical Physics · Physics 2007-05-23 Vinod Krishna

Nonadiabatic molecular dynamics is an effective method for modeling nonradiative decay in electronically excited molecules. Its accuracy depends strongly on the quality of the potential energy surfaces, and its affordability for long…

Chemical Physics · Physics 2024-10-11 Matthew R. Hennefarth , Donald G. Truhlar , Laura Gagliardi

We study non-adiabatic two-parameter charge and spin pumping through a single-level quantum dot with Coulomb interaction. For the limit of weak tunnel coupling and in the regime of pumping frequencies up to the tunneling rates, $\Omega…

Mesoscale and Nanoscale Physics · Physics 2011-10-10 Fabio Cavaliere , Michele Governale , Jürgen König

A software package, called DFTBaby, is published, which provides the electronic structure needed for running non-adiabatic molecular dynamics simulations at the level of charge-consistent tight-binding DFT. A long-range correction is…

Chemical Physics · Physics 2017-10-25 Alexander Humeniuk , Roland Mitric

Theoretical investigation of the dissociative recombination (DR) of NeH+ with low-energy electrons in the regime where the process occurs without direct potential energy curve crossings is presented. The calculations are performed using…

Atomic and Molecular Clusters · Physics 2025-09-09 Riyad Hassaine , Janos Zsolt Mezei , Dahbia Talbi , Jonathan Tennyson , Ioan F. Schneider

We analyze a mixed quantum-classical algorithm recently derived from the exact factorization equations [Min, Agostini, Gross, PRL {\bf 115}, 073001 (2015)] to show the role of the different terms in the algorithm in bringing about…

Chemical Physics · Physics 2018-05-10 Graeme H. Gossel , Federica Agostini , Neepa T. Maitra

The coupling of electronic and vibrational motion is studied by two canonical transformations namely normal coordinate transformation and momentum transformation on molecular Hamiltonian. It is shown that by these transformations we can…

Chemical Physics · Physics 2007-05-23 Ivan Hubac , Peter Babinec , Martin Polasek , Jan Urban , Pavel Mach , Jozef Masik , Jerzy Leszczynski

We introduce an approach to improve single-reference coupled cluster theory in settings where the Aufbau determinant is absent from or plays only a small role in the true wave function. Using a de-excitation operator that can be efficiently…

Chemical Physics · Physics 2024-07-03 Harrison Tuckman , Eric Neuscamman

In this work we present a coupled cluster based approach to the computation of the spin orbit coupling matrix elements. The working expressions are derived from the quadratic response function with the coupled cluster parametrization, using…

Chemical Physics · Physics 2023-01-11 Aleksandra Maria Tucholska , Michał Lesiuk , Robert Moszynski

We propose a new formulation of time-dependent coupled cluster with adaptive basis functions and division of the one-particle space into active and secondary subspaces. The formalism is fully bivariational in the sense of a real-valued…

Chemical Physics · Physics 2024-02-20 Mads Greisen Højlund , Ove Christiansen