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Modern X-ray spectroscopy has proven itself as a robust tool for probing the electronic structure of atoms in complex environments. Despite working on energy scales that are much larger than those corresponding to nuclear motions, taking…

Chemical Physics · Physics 2017-06-28 Sven Karsten , Sergey I. Bokarev , Saadullah G. Aziz , Sergei D. Ivanov , Oliver Kühn

Vibrational-excitation cross sections of ground electronic state of carbon dioxide molecule by electron-impact through the CO2-(2\Pi) shape resonance is considered in the separation of the normal modes approximation. Resonance curves and…

Chemical Physics · Physics 2016-11-01 V. Laporta , J. Tennyson , R. Celiberto

We study the relation between the microscopic properties of a many-body system and the electron spectra, experimentally accessible by photoemission. In a recent paper [Phys. Rev. Lett. 114, 236402 (2015)], we introduced the "fluctuation…

Strongly Correlated Electrons · Physics 2018-03-28 O. Gunnarsson , J. Merino , T. Schäfer , G. Sangiovanni , G. Rohringer , A. Toschi

This is the first in a series of two papers investigating the effect of electron-phonon coupling in two-dimensional Fourier transformed electronic spectroscopy. We present a series of one- and two-dimensional nonlinear spectroscopic…

Two-dimensional (2D) spectroscopy provides information about dissipative processes subsequent to electronic excitation, which play a functional role in energy harvesting materials and devices. This technique is particularly sensitive to…

Chemical Physics · Physics 2014-06-05 Joachim Seibt , Tonu Pullerits

With advanced fabrication techniques it is possible to make nanoscale electronic structures that have discrete energy levels. Such structures are called artificial atoms because of analogy with true atoms. Examples of such atoms are quantum…

Mesoscale and Nanoscale Physics · Physics 2012-06-07 David Gunnarsson , Jani Tuorila , Antti Paila , Jayanta Sarkar , Erkki Thuneberg , Yuriy Makhlin , Pertti Hakonen

We investigate the time evolution process of one selected (initially prepared by optical pumping) vibrational molecular state, coupled to all other intra-molecular vibrational states of the same molecule, and also to its environment.…

Mesoscale and Nanoscale Physics · Physics 2015-05-13 V. A. Benderskii , E. I. Kats

Atomic vibrations control all thermally activated processes in materials including diffusion, heat transport, phase transformations, and surface chemistry. Recent developments in monochromated, aberration-corrected scanning transmission…

Materials Science · Physics 2020-01-08 Kartik Venkatraman , Barnaby D. A. Levin , Katia March , Peter Rez , Peter A. Crozier

The electronic band structure, describing the periodic dependence of electronic quantum states on lattice momentum in reciprocal space, is a fundamental concept in solid-state physics. However, it's only well-defined for static nuclei. To…

The two-dimensional spectroscopy has recently revealed oscillatory behavior of excitation dynamics in molecular systems. However, in the majority of cases it is strongly debated if excitonic or vibrational wavepackets, or evidences of…

Chemical Physics · Physics 2012-11-27 Vytautas Butkus , Donatas Zigmantas , Leonas Valkunas , Darius Abramavicius

We present a methodology for simulating multi-dimensional electronic spectra of molecular aggregates with coupling of electronic excitation to a structured environment using the stochastic non-Markovian quantum state diffusion (NMQSD)…

Quantum Physics · Physics 2022-09-28 Lipeng Chen , Doran I. G. Bennett , Alexander Eisfeld

The spectra (rotational, rotation-vibrational or electronic) of diatomic molecules due to transitions involving only closed-shell ($^1\Sigma$) electronic states follow very regular, simple patterns and their theoretical analysis is usually…

Chemical Physics · Physics 2016-05-10 Jonathan Tennyson , Lorenzo Lodi , Laura K. McKemmish , Sergei N Yurchenko

Ultrafast laser excitation can create coherent superpositions of electronic states in molecules and trigger ultrafast flow of electron density on few- to sub-femtosecond time scales. While recent attosecond experiments have addressed…

Chemical Physics · Physics 2020-11-18 Yuki Kobayashi , Daniel M. Neumark , Stephen R. Leone

In the construction of diabatic vibronic Hamiltonians for quantum dynamics in the excited-state manifold of molecules, the coupling constants are often extracted solely from information on the excited-state energies. Here, a new protocol is…

Chemical Physics · Physics 2018-04-02 Maria Fumanal , Felix Plasser , Sebastian Mai , Chantal Daniel , Etienne Gindensperger

Fully numerical mesh solutions of 2D and 3D quantum equations of Schroedinger and Hartree-Fock type allow us to work with wavefunctions which possess a very flexible geometry. This flexibility is especially important for calculations of…

Atomic Physics · Physics 2007-05-23 Mikhail V. Ivanov

Calculations of highly excited and delocalized molecular vibrational states are computationally challenging tasks, which strongly depends on the choice of coordinates for describing vibrational motions. We introduce a new method that…

We study resonant optical excitations of strongly-interacting Rydberg states of atoms in the presence of relaxations. We employ the quantum stochastic (Monte Carlo) wavefunctions to simulate the dissipative dynamics of tens of atoms in…

Quantum Physics · Physics 2013-06-25 David Petrosyan

We discuss an integral equation approach that enables fast computation of the response of nonlinear multi-degree-of-freedom mechanical systems under periodic and quasi-periodic external excitation. The kernel of this integral equation is a…

Dynamical Systems · Mathematics 2019-05-10 Shobhit Jain , Thomas Breunung , George Haller

A novel quantum dynamical method to simulate vibronic reaction dynamics in molecules at metal surfaces is proposed. The method is based on the hierarchical quantum master equation approach and uses a discrete variable representation of the…

Chemical Physics · Physics 2019-12-05 A. Erpenbeck , M. Thoss

In this work, we present a proof-of-concept investigation of non-equilibrium chemical reaction dynamics at a molecule-electrode interface, driven out of equilibrium by an applied votage bias and mediated by a confined, enhanced vacuum…

Chemical Physics · Physics 2025-12-15 Yaling Ke