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The interaction of electronic spin and molecular vibrations mediated by spin-orbit coupling governs spin relaxation in molecular qubits. I derive an extended molecular spin Hamiltonian that includes both adiabatic and non-adiabatic…

Chemical Physics · Physics 2024-01-31 Philip Shushkov

We extend the Mixed Quantum-Classical Initial Value Representation (MQC-IVR), a semiclassical method for computing real-time correlation functions, to electronically nonadiabatic systems using the Meyer-Miller-Stock-Thoss (MMST) Hamiltonian…

Chemical Physics · Physics 2018-01-17 Matthew S. Church , Timothy J. H. Hele , Gregory S. Ezra , Nandini Ananth

We propose the multi-state complete-active-space second-order perturbation theory spin-orbit method (MS-CASPT2-SO) for electronic structure calculations. It is a two-step spin-orbit coupling method that does not make use of energy shifts…

Chemical Physics · Physics 2010-12-30 Zoila Barandiaran , Luis Seijo

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

We study the asymptotic dynamics of a driven spin-boson system where the environment is formed by a broadened localized mode. Upon exploiting an exact mapping, an equivalent formulation of the problem in terms of a quantum two-state system…

Mesoscale and Nanoscale Physics · Physics 2009-11-10 M. C. Goorden , M. Thorwart , M. Grifoni

The mapping approach addresses the mismatch between the continuous nuclear phase space and discrete electronic states by creating an extended, fully continuous phase space using a set of harmonic oscillators to encode the populations and…

Chemical Physics · Physics 2019-09-30 Maximilian A. C. Saller , Aaron Kelly , Jeremy O. Richardson

Nonadiabatic dynamics methods are an essential tool for investigating photochemical processes. In the context of employing first principles electronic structure techniques, such simulations can be carried out in a practical manner using…

Chemical Physics · Physics 2024-05-08 Jonathan R. Mannouch , Aaron Kelly

We develop a semi-classical method to simulate the motion of atoms in a dissipative optical lattice. Our method treats the internal states of the atom quantum mechanically, including all nonadiabatic couplings, while position and momentum…

Atomic Physics · Physics 2009-11-11 S. Jonsell , C. M. Dion , M. Nylén , S. J. H. Petra , P. Sjölund , A. Kastberg

The quantum dynamics of open many-body systems poses a challenge for computational approaches. Here we develop a stochastic scheme based on the positive P phase-space representation to study the nonequilibrium dynamics of coupled spin-boson…

Quantum Physics · Physics 2015-06-11 Stephan Mandt , Darius Sadri , Andrew A. Houck , Hakan E. Türeci

Under the spin-position decoupling approximation, a vector with a phase in 3D orientation space endowed with geometric algebra, substitutes the vector-matrix spin model built on the Pauli spin operator. The standard quantum operator-state…

Quantum Physics · Physics 2022-12-20 Sokol Andoni

The powerful molecular dynamics (MD) simulation is basically based on a picture that the atoms experience classical-like trajectories under the exertion of classical force field determined by the quantum mechanically solved electronic…

Chemical Physics · Physics 2013-12-16 Wei Feng , Luting Xu , Xin-Qi Li , Weihai Fang

The microscopic control available over cold atoms in optical lattices has opened new opportunities to study the properties of quantum spin models. While a lot of attention is focussed on experimentally realizing ground or thermal states via…

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 introduce mapping-variable ring polymer molecular dynamics (MV-RPMD), a model dynamics for the direct simulation of multi-electron processes. An extension of the RPMD idea, this method is based on an exact, imaginary time path-integral…

Statistical Mechanics · Physics 2015-06-17 Nandini Ananth

We introduce a novel methodology for simulating the excited-state dynamics of extensive molecular aggregates in the framework of the long-range corrected time-dependent density-functional tight-binding fragment molecular orbital method…

Chemical Physics · Physics 2024-04-23 Richard Einsele , Roland Mitrić

We describe an efficient numerical method for simulating the dynamics and steady states of collective spin systems in the presence of dephasing and decay. The method is based on the Schwinger boson representation of spin operators and uses…

Quantum Physics · Physics 2021-05-18 Julian Huber , Peter Kirton , Peter Rabl

Quantum molecular dynamics requires an accurate representation of the molecular potential energy surface from a minimal number of electronic structure calculations, particularly for nonadiabatic dynamics where excited states are required.…

Chemical Physics · Physics 2016-08-24 Charles W. Heaps , David A. Mazziotti

We propose a simple construction of shortcuts to adiabaticity tracking instantaneous stationary states in classical spin systems without knowing tracked stationary states. In our construction, control fields of counter-diabatic driving are…

Quantum Physics · Physics 2018-09-28 Takuya Hatomura , Takashi Mori

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 use the effective Hamiltonian that we recently fitted against the first 306 experimentally observed vibronic transitions of NO2 [J. Chem. Phys. 119, 5923 (2003)] to investigate the time domain nonadiabatic dynamics of this molecule on…

Chemical Physics · Physics 2011-11-09 Michaël Sanrey , Marc Joyeux