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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

While rigorous quantum dynamical simulations of many-body systems are extremely difficult (or impossible) due to the exponential scaling with dimensionality, corresponding classical simulations completely ignore quantum effects.…

Quantum Physics · Physics 2015-05-30 Cesare Mollica , Jiri Vanicek

Engineering, controlling, and simulating quantum dynamics is a strenuous task. However, these techniques are crucial to develop quantum technologies, preserve quantum properties, and engineer decoherence. Earlier results have demonstrated…

Accurate simulations of molecules require high-level electronic-structure theory in combination with rigorous methods for approximating the quantum dynamics. Machine-learning approaches can significantly reduce the computational expense of…

Chemical Physics · Physics 2026-02-24 Valerii Andreichev , Jindra Dušek , Markus Meuwly , Jeremy O. Richardson

Owing to the computational complexity of electronic structure algorithms running on classical digital computers, the range of molecular systems amenable to simulation remains tightly circumscribed even after many decades of work. Quantum…

Quantum Physics · Physics 2022-05-18 Alexis Ralli , Michael I. Williams , Peter V. Coveney

Molecular dynamics simulations are indispensable for exploring the behavior of atoms and molecules. Grounded in quantum mechanical principles, quantum molecular dynamics provides high predictive power but its computational cost is dominated…

Chemical Physics · Physics 2025-09-10 Siu Wun Cheung , Youngsoo Choi , Jean-Luc Fattebert , Daniel Osei-Kuffuor

Due to the Heisenberg uncertainty principle, various classical systems differing only on the scale smaller than Planck's cell correspond to the same quantum system. This fact is used to find a unique semiclassical representation without the…

Quantum Physics · Physics 2009-11-10 Jiri Vanicek

Characterizing quantum dynamics is essential for quantifying arbitrary properties of a quantum process -- such as its ability to exhibit quantum-mechanical dynamics or generate entanglement. However, current methods require a number of…

While most work on the quantum simulation of chemistry has focused on computing energy surfaces, a similarly important application requiring subtly different algorithms is the computation of energy derivatives. Almost all molecular…

One of the central problems in quantum theory is to characterize, detect, and quantify quantumness in terms of classical strategies. Dephasing processes, caused by non-dissipative information exchange between quantum systems and…

Quantum Physics · Physics 2019-08-23 Hong-Bin Chen , Ping-Yuan Lo , Clemens Gneiting , Joonwoo Bae , Yueh-Nan Chen , Franco Nori

Quantum computers hold promise to enable efficient simulations of the properties of molecules and materials; however, at present they only permit ab initio calculations of a few atoms, due to a limited number of qubits. In order to harness…

Materials Science · Physics 2020-07-07 He Ma , Marco Govoni , Giulia Galli

The molecular energies of chemical systems have been successfully calculated on quantum computers, however, more attention has been paid to the dynamic process of chemical reactions in practical application, especially in catalyst design,…

Quantum Physics · Physics 2023-03-28 Qiankun Gong , Qingmin Man , Ye Li , Menghan Dou , Qingchun Wang , Yu-Chun Wu , Guo-Ping Guo

Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…

Chemical Physics · Physics 2024-04-11 Nikolay V. Golubev , Jiří Vaníček

We have developed and implemented a new quantum molecular dynamics approximation that allows fast and accurate simulations of dense plasmas from cold to hot conditions. The method is based on a carefully designed orbital-free implementation…

Plasma Physics · Physics 2015-06-22 Travis Sjostrom , Jerome Daligault

General semiclassical expression for quantum fidelity (Loschmidt echo) of arbitrary pure and mixed states is derived. It expresses fidelity as an interference sum of dephasing trajectories weighed by the Wigner function of the initial…

Quantum Physics · Physics 2007-05-23 Jiri Vanicek

We present an efficient \textit{ab initio} algorithm for quantum dynamics simulations of interacting systems that is based on the conditional decomposition of the many-body wavefunction [Phys. Rev. Lett. 113, 083003 (2014)]. Starting with…

Mesoscale and Nanoscale Physics · Physics 2019-02-27 Guillermo Albareda , Aaron Kelly , Angel Rubio

Theoretical concepts in condensed matter physics are typically verified and also developed by exploiting computer simulations mostly in simple models. Predictions based on these usually isotropic models are often at odds with measurement…

Soft Condensed Matter · Physics 2020-11-13 K. Koperwas , A. Grzybowski , M. Paluch

Molecular dynamics simulation is now a widespread approach for understanding complex systems on the atomistic scale. It finds applications from physics and chemistry to engineering, life and medical science. In the last decade, the approach…

Computational Physics · Physics 2021-04-28 Shunzhou Wan , Robert C. Sinclair , Peter V. Coveney

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

Molecular dynamics simulations at a constant electric potential are an essential tool to study electrochemical processes, providing microscopic information on the structural, thermodynamic, and dynamical properties. Despite the numerous…

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