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Carbon monoxide (CO) and nitrous oxide (N2O) both undergo profound structural and chemical transformations when compressed. While their individual high-P/T phase diagrams have been mapped in considerable detail, comparatively little…

Materials Science · Physics 2025-08-19 Reetam Paul , Jonathan C. Crowhurst , Stanimir Bonev

Many recent experimental ultrafast spectroscopy studies have hinted at non-adiabatic dynamics indicating the existence of conical intersections, but their direct observation remains a challenge. The rapid change of the energy gap between…

Chemical Physics · Physics 2021-05-05 Deependra Jadoun , Mahesh Gudem , Markus Kowalewski

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 novel method to describe realistically ionization processes with absorbing boundary conditions in basis expansion within the formalism of the so-called Non-Adiabatic Quantum Molecular Dynamics. This theory couples…

Quantum Physics · Physics 2015-06-26 Mathias Uhlmann , Thomas Kunert , Ruediger Schmidt

Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…

Chemical Physics · Physics 2014-08-08 Wei Feng , Luting Xu , Xin-Qi Li , Weihai Fang , YiJing Yan

We propose an approach to probe coherent spin-state dynamics of molecules using circularly polarized hard x-ray pulses. For the dynamically aligned nitric oxide molecules in a coherent superposition spin-orbit coupled electronic state that…

Optics · Physics 2024-01-02 Xiaoyu Mi , Ming Zhang , Zheng Li

An approach to non-adiabatic dynamics of atoms in molecular and condensed matter systems under general non-equilibrium conditions is proposed. In this method interaction between nuclei and electrons is considered explicitly up to the second…

Materials Science · Physics 2018-08-01 L. Kantorovich

Time-resolved ultrafast x-ray scattering is an emerging approach to probe the temporally evolving electronic charge distribution in real-space and in real-time. In this contribution, time-resolved ultrafast x-ray scattering from an…

Atomic Physics · Physics 2015-06-18 Gopal Dixit , Robin Santra

A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees…

Mesoscale and Nanoscale Physics · Physics 2024-05-06 Samuel L. Rudge , Christoph Kaspar , Robin L. Grether , Steffen Wolf , Gerhard Stock , Michael Thoss

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 have employed non-adiabatic molecular dynamics based on time-dependent density-functional theory to characterize the scattering behaviour of a proton with the Li$_4$ cluster. This technique assumes a classical approximation for the…

Atomic and Molecular Clusters · Physics 2015-05-27 Alberto Castro , Miguel Isla , Jose I. Martinez , Julio A. Alonso

Quantum material systems upon applying ultrashort laser pulses provide a rich platform to access excited material phases and their transformations that are not entirely like their equilibrium counterparts. The addressability and potential…

Strongly Correlated Electrons · Physics 2021-08-19 Xiaoyi Sun , Shuaishuai Sun , Chong-Yu Ruan

Technological advancements in generation of ultrafast and intense laser pulses have enabled the real-time observation and control of charge migration in molecules on their natural timescale, which ranges from few femtoseconds to several…

Optics · Physics 2025-02-25 Sucharita Giri

Nonadiabatic effects appear due to avoided crossings or conical intersections that are either intrinsic properties in field-free space or induced by a classical laser field in a molecule. It was demonstrated that avoided crossings in…

Chemical Physics · Physics 2019-11-12 András Csehi , Markus Kowalewski , Gábor J. Halász , Ágnes Vibók

We demonstrate the existence of a strictly non-adiabatic control pathway in deprotonation of the acetylene dication. This pathway is identified experimentally by measuring a kinetic energy shift in an ion coincidence experiment. We use a…

For years, theoretical calculations and scalable computer simulations have complemented ultrafast experiments as they offer the advantage to overcome experimental restrictions and have access to the whole dynamics. This synergy between…

Chemical Physics · Physics 2024-02-20 Patricia Vindel-Zandbergen , Jesús González-Vázquez

Non-adiabatic quantum effects, often experimentally observed in semiconductors nano-devices such as single-electron pumps operating at high frequencies, can result in undesirable and uncontrollable behaviour. However, when combined with the…

Mesoscale and Nanoscale Physics · Physics 2022-02-16 Alan Gardin , Ross D. Monaghan , Tyler Whittaker , Rajib Rahman , Giuseppe C. Tettamanzi

X-ray diffraction from molecules in the ground state produces an image of their charge density, and time-resolved X-ray diffraction can thus monitor the motion of the nuclei. However, the density change of excited valence electrons upon…

Chemical Physics · Physics 2018-06-15 Jérémy R. Rouxel , Markus Kowalewski , Kochise Bennett , Shaul Mukamel

We formulate a rigorous method for calculating a nonadiabatic (frequency-dependent) exchange-correlation (XC) kernel required for correct description of both equilibrium and nonequilibrium properties of strongly correlated systems within…

Strongly Correlated Electrons · Physics 2014-10-13 Volodymyr Turkowski , Talat S. Rahman