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The effect of nuclear dynamics and conical intersections on electronic coherences is investigated employing a two-state, two-mode linear vibronic coupling model. Exact quantum dynamical calculations are performed using the…

Chemical Physics · Physics 2018-08-22 Caroline Arnold , Oriol Vendrell , Ralph Welsch , Robin Santra

We examine structural and dynamical properties of quantum resonances associated with an avoided crossing and identify the parameter shifts where these properties attain maximal or extreme values, first at a general level, and then for a…

Quantum Physics · Physics 2015-05-13 I. Lizuain , E. Hernandez-Concepcion , J. G. Muga

In molecular systems containing conical intersections (CIs), a nontrivial geometric phase (GP) appears in the nuclear and electronic wave-functions in the adiabatic representation. We study GP effects in nuclear dynamics of an N-dimensional…

Quantum Physics · Physics 2015-01-12 Loic Joubert-Doriol , Ilya G. Ryabinkin , Artur F. Izmaylov

Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections (CIs), which generate coherences between electronic…

Phase separation, crucial for spatially segregating biomolecules in cells, is well-understood in the simple case of a few components with pairwise interactions. Yet, biological cells challenge the simple picture in at least two ways: First,…

Soft Condensed Matter · Physics 2024-03-12 Chengjie Luo , Yicheng Qiang , David Zwicker

We use extreme-ultraviolet interferometry to measure the phase of high-order harmonic generation from transiently aligned CO2 molecules. We unambiguously observe a reversal in phase of the high order harmonic emission for higher harmonic…

Atomic Physics · Physics 2009-11-13 Xibin Zhou , Robynne Lock , Wen Li , Nick Wagner , Margaret. M. Murnane , Henry C. Kapteyn

Preserving quantum coherence with the increase of a system's size and complexity is a major challenge. Molecules, with their diverse sizes and complexities and many degrees of freedom, are an excellent platform for studying the transition…

Quantum Physics · Physics 2024-09-23 Tamar Levin , Ziv Meir

Nonadiabaticity, i.e., the effect of mixing electronic states by nuclear motion, is a central phenomenon in molecular science. The strongest nonadiabatic effects arise due to the presence of conical intersections of electronic energy…

Chemical Physics · Physics 2020-04-01 Csaba Fábri , Benjamin Lasorne , Gábor J. Halász , Lorenz S. Cederbaum , Ágnes Vibók

Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an…

Chemical Physics · Physics 2016-07-27 Markus Kowalewski , Kochise Bennett , Jérémy R. Rouxel , Shaul Mukamel

We investigate the role of the geometric phase (GP) in an internal conversion process when the system changes its electronic state by passing through a conical intersection (CI). Local analysis of a two-dimensional linear vibronic coupling…

Chemical Physics · Physics 2015-01-12 Ilya G. Ryabinkin , Loic Joubert-Doriol , Artur F. Izmaylov

We introduce multistate metadynamics for automatic exploration of conical intersection seams between adiabatic Born-Oppenheimer potential energy surfaces in molecular systems. By choosing the energy gap between the electronic states as a…

Chemical Physics · Physics 2018-05-10 Joachim O. Lindner , Merle I. S. Röhr , Roland Mitrić

We present a framework for simulating relaxation dynamics through a conical intersection of an open quantum system that combines methods to approximate the motion of degrees of freedom with disparate time and energy scales. In the vicinity…

Statistical Mechanics · Physics 2019-07-24 Addison J. Schile , David T. Limmer

We show that time-resolved x-ray scattering from molecules prepared in a superposition of electronic states moving through an avoided crossing has new features not found in diffraction from the corresponding classical mixed state.…

In this letter we study dynamical tunneling in highly excited symmetric molecules. The role of classical phase space structures like resonances and chaos on the tunneling splittings are illustrated using the water molecule as an example. It…

Chaotic Dynamics · Physics 2009-11-07 Srihari Keshavamurthy

We show that finite systems with conical intersections can exhibit spontaneous symmetry breaking which manifests itself in spatial localization of eigenstates. This localization has a geometric phase origin and is robust against variation…

Quantum Physics · Physics 2015-01-12 Ilya G. Ryabinkin , Artur F. Izmaylov

The geometric phase effect arises from the dependence on the nuclear coordinates in the electronic Hamiltonian, leading to sign changes of the electronic wave functions upon traversal of certain paths in nuclear configuration space. The…

Chemical Physics · Physics 2025-08-15 Eirik F. Kjønstad , Henrik Koch

The effect of conical intersections (CIs) on electronic relaxation, transitions from excited states to ground states, is well studied, but their influence on hyperfine quenching in a reactant molecule is not known. Here, we report on…

Chemical Physics · Physics 2021-01-29 Ming Li , Jacek Klos , Alexander Petrov , Hui Li , Svetlana Kotochigova

Sub-laser cycle time scale of electronic response to strong laser fields enables attosecond dynamical imaging in atoms, molecules and solids. Optical tunneling and high harmonic generation are the hallmarks of attosecond imaging in optical…

Optics · Physics 2019-10-22 R. E. F. Silva , Á. Jiménez-Galán , B. Amorim , O. Smirnova , M. Ivanov

Quantum interference between multiple pathways in molecular photodissociation often results in angular momentum polarization of atomic products and this can give deep insight into fundamental physical processes. For dissociation of diatomic…

Chemical Physics · Physics 2022-04-26 Chaya Weeraratna , Arthur G. Suits , Oleg S. Vasyutinskii

We report on the new non--linear optical signatures of quantum phase transitions in the high-temperature superconductor YBCO, observed through high harmonic generation. While the linear optical response of the material is largely unchanged…