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We theoretically propose a multidimensional high-harmonic echo spectroscopy technique which utilizes strong optical fields to resolve coherent electron dynamics spanning an energy range of multiple electron Volts. Using our recently…

Electronic coherences can be leveraged to control molecular dynamics, but such control is limited by ultrafast decoherence driven by coupling between electronic excitations and molecular vibrations. With the goal of understanding and…

Chemical Physics · Physics 2025-05-27 Jiří Suchan , Benjamin G. Levine

We analyze electronically excited nuclear wave functions and their coherence when subjecting a molecule to the action of natural, pulsed incoherent solar-like light, and to that of ultrashort coherent light assumed to have the same center…

Quantum Physics · Physics 2015-06-12 Alex C. Han , Moshe Shapiro , Paul Brumer

Photoionization using attosecond pulses can lead to the formation of coherent superpositions of the electronic states of the parent ion. However, ultrafast electron ejection triggers not only electronic but also nuclear dynamics---leading…

Chemical Physics · Physics 2017-03-29 Caroline Arnold , Oriol Vendrell , Robin Santra

Molecular polaritons have become an emerging platform for remotely controlling molecular properties through strong light-matter interactions. Herein, a semiclassical approach is developed for describing molecular polaritons by…

Chemical Physics · Physics 2022-04-19 Tao E. Li , Zhen Tao , Sharon Hammes-Schiffer

Attochemistry aims to exploit the properties of coherent electronic wavepackets excited via attosecond pulses, to control the formation of photoproducts. Such molecular processes can in principle be simulated with various nonadiabatic…

Chemical Physics · Physics 2024-05-28 Thierry Tran , Anthony Ferté , Morgane Vacher

We propose mixed quantum-classical equations of motion that unify electronic coherence and phase evolution simultaneously within the exact factorization framework. Our derivation shows that incorporating the second-order electron-nuclear…

Chemical Physics · Physics 2026-03-03 Jong-Kwon Ha , Seong Ho Kim , Seung Kyu Min

Revealing possible long-living coherence in ultrafast processes allows detecting genuine quantum mechanical effects in molecules. To investigate such effects from a quantum chemistry perspective, we have developed a method for simulating…

Chemical Physics · Physics 2018-07-04 Emanuele Coccia , Filippo Troiani , Stefano Corni

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 coherence is highly involved in photochemical functioning of complex molecular systems. Co-existence and intermixing of electronic and/or vibrational coherences, while never unambiguously identified experimentally, has been proposed…

We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a…

Optics · Physics 2018-12-11 Daria Popova-Gorelova , Jochen Küpper , Robin Santra

With a semiclassical quasi-static model we achieve an insight into the complex dynamics of two correlated electrons under the combined influence of a two-center Coulomb potential and an intense laser field. The model calculation is able to…

Atomic and Molecular Clusters · Physics 2009-11-13 J. Liu , D. F. Ye , J. Chen , X. liu

Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as…

Chemical Physics · Physics 2016-05-24 Alexander White , Sergei Tretiak , Dmitry Mozyrsky

Understanding the reactivity and spectroscopy of aqueous solutions at the atomistic level is crucial for the elucidation and design of chemical processes. However, the simulation of these systems requires addressing the formidable…

Chemical Physics · Physics 2017-02-28 Ondrej Marsalek , Thomas E. Markland

Molecular structure is often considered as emerging from the decoherence effect of the environment. Electrons are part of the environment of the nuclei in a molecule. In this work, their contribution to the classical-like geometrical…

Chemical Physics · Physics 2021-11-10 Patrick Cassam-Chenaï , Edit Mátyus

A new approach for describing the effective electronic states of "atoms in compounds" to study the properties of molecules and condensed matter which are circumscribed by the operators heavily concentrated in atomic cores is proposed. Among…

Chemical Physics · Physics 2014-12-02 Anatoly V. Titov , Yuriy V. Lomachuk , Leonid V. Skripnikov

Coherent emission of light by free charged particles is ubiquitous in many areas of physics and engineering, with the light's properties believed to be successfully captured by classical electromagnetism in all relevant experimental…

Quantum Physics · Physics 2021-12-07 Aviv Karnieli , Nicholas Rivera , Ady Arie , Ido Kaminer

Quantum mechanical phenomena, such as electronic coherence and entanglement, play a key role in achieving the unrivalled efficiencies of light-energy conversion in natural photosynthetic light-harvesting complexes, and triggered the growing…

Quantum Physics · Physics 2011-02-02 Richard Hildner , Daan Brinks , Niek F. van Hulst

A new concept of the molecular structure optimization method based on quantum dynamics computations is presented. Nuclei are treated as quantum mechanical particles, as are electrons, and the many-body wave function of the system is…

Hyperfine interaction of electron spins with nuclear spins, in coupled double quantum dots is studied. Results of successive electron spin measurements exhibit bunching due to correlations induced via the nuclear spins. Further nuclear…

Mesoscale and Nanoscale Physics · Physics 2009-11-11 Ozgur Cakir , Toshihide Takagahara