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Molecular electronics is a rapidly developing field focused on using molecules as the structural basis for electronic components. It is common in such devices for the system of interest to couple simultaneously to multiple environments.…

Mesoscale and Nanoscale Physics · Physics 2019-08-27 Conor McConnell , Ahsan Nazir

Determining the spectral density of a molecular system immersed in a proteomic scaffold and in contact to a solvent is a fundamental challenge in the coarse-grained description of, e.g., electron and energy transfer dynamics. Once the…

Quantum Physics · Physics 2014-11-04 Leonardo A. Pachon , Paul Brumer

Vibrational spectroscopy is a powerful technique to characterize the near-equilibrium dynamics of molecules in the gas- and the condensed-phase. This contribution summarizes efforts from computer-based methods to gain insight into the…

Chemical Physics · Physics 2022-04-15 Markus Meuwly

Conducting precise electronic-vibrational dynamics simulations of molecular systems poses significant challenges when dealing with realistic environments composed of numerous vibrational modes. Here, we introduce a technique for the…

Two-dimensional electronic spectroscopy has become one of the main experimental tools for analyzing the dynamics of excitonic energy transfer in large molecular complexes. Simplified theoretical models are usually employed to extract model…

Chemical Physics · Physics 2019-01-17 Mirta Rodríguez , Tobias Kramer

We present a general two-dimensional model of conical intersection between metastable states that are vibronically coupled not only directly but also indirectly through a virtual electron in the autodetachment continuum. This model is used…

Chemical Physics · Physics 2023-07-26 Martina Ćosićová , Jan Dvořák , Martin Čížek

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…

Experimental auto- and cross-correlation functions and their corresponding spectral density functions are extracted from measured sweep data of mode-stirred fields. These are compared with theoretical models derived in part I, using…

Classical Physics · Physics 2024-04-05 Luk R. Arnaut , John M. Ladbury

Coherent dynamics of coupled molecules are effectively characterized by the two-dimensional (2D) electronic coherent spectroscopy. Depending on the coupling between electronic and vibrational states, oscillating signals of purely…

Chemical Physics · Physics 2013-10-17 Vytautas Butkus , Donatas Zigmantas , Darius Abramavicius , Leonas Valkunas

Ultra-fast and multi-dimensional spectroscopy gives a powerful looking glass into the dynamics of molecular systems. In particular two-dimensional electronic spectroscopy (2DES) provides a probe of coherence and the flow of energy within…

Quantum Physics · Physics 2021-03-31 André Anda , Jared H. Cole

Two-dimensional electronic spectroscopy (2DES) provides a detailed picture of electronically nonadiabatic dynamics that can be interpreted with the aid of simulations. Here, we develop and contrast trajectory-based nonadiabatic dynamics…

Spectroscopic methods involving the sudden injection or ejection of electrons in materials are a powerful probe of electronic structure and interactions. These techniques, such as photoemission and tunneling, yield measurements of the…

Mesoscale and Nanoscale Physics · Physics 2007-07-12 O. E. Dial , R. C. Ashoori , L. N. Pfeiffer , K. W. West

We show that individual vibrational modes in single-molecule junctions with asymmetric molecule-lead coupling can be selectively excited by applying an external bias voltage. Thereby, a non-statistical distribution of vibrational energy can…

Mesoscale and Nanoscale Physics · Physics 2017-09-13 R. Volkovich , R. Härtle , M. Thoss , U. Peskin

The recent development of multidimensional ultrafast spectroscopy techniques calls for the introduction of computational schemes that allow for the simulation of such experiments and the interpretation of the corresponding results from a…

Mesoscale and Nanoscale Physics · Physics 2023-10-30 Jannis Krumland , Michele Guerrini , Antonietta De Sio , Christoph Lienau , Caterina Cocchi

Photoemission and tunneling spectroscopies measure the energies at which single electrons can be added to or removed from an electronic system. Features observed in such spectra have revealed electrons coupling to vibrational modes of ions…

Strongly Correlated Electrons · Physics 2017-05-09 Joonho Jang , Benjamin Hunt , Loren N. Pfeiffer , Kenneth W. West , Raymond C. Ashoori

Two-dimensional electronic spectroscopy provides information on coupling and energy transfer between excited states on ultrafast timescales. Only recently, incoherent fluorescence detection has made it possible to combine this method with…

Optics · Physics 2025-05-14 Sanchayeeta Jana , Simon Durst , Lucas Ludwig , Markus Lippitz

We present a theory of vibrational modulation of two-dimensional coherent Fourier transformed electronic spectra. Based on an expansion of the system's energy gap correlation function in terms of Huang-Rhys factors, we explain the…

Experimental and theoretical evidence point out to the crucial role of specific resonant intramolecular vibrational modes in the interpretation of long-lived coherences observed in two-dimensional spectra of some natural and synthetic light…

Chemical Physics · Physics 2020-07-15 Leonardo F. Calderón , Leonardo A. Pachón

The potential of mean-field decomposition techniques in interpreting electronic transitions in molecules is explored, particularly, the usefulness of these for offering computational signatures of different classes of such excitations. When…

Chemical Physics · Physics 2022-02-14 Janus J. Eriksen

The study of electronic transitions within a molecule connected to the absorption or emission of light is a common task in the process of the design of new materials. The transitions are complex quantum mechanical processes and a detailed…

Human-Computer Interaction · Computer Science 2021-06-03 Talha Bin Masood , Signe Sidwall Thygesen , Mathieu Linares , Alexei I. Abrikosov , Vijay Natarajan , Ingrid Hotz