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We show how vibronic spectra in molecular systems can be simulated in an efficient and accurate way using first principles approaches without relying on the explicit use of multiple Born-Oppenheimer potential energy surfaces. We demonstrate…

Chemical Physics · Physics 2024-03-01 Kevin Lively , Guillermo Albareda , Shunsuke A. Sato , Aaron Kelly , Angel Rubio

We present a comparison between Fe K-edge x-ray absorption spectra of carbonmonoxy-myoglobin and its simulation based on density-functional theory determination of the structure and vibrations and spectral simulation with…

Soft Condensed Matter · Physics 2010-08-04 G. Veronesi , C. Degli Esposti Boschi , L. Ferrari , G. Venturoli , F. Boscherini , F. D. Vila , J. J. Rehr

We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…

Chemical Physics · Physics 2016-12-04 Ralph Gebauer , Morrel H. Cohen , Roberto Car

Recently, several works have analysed the efficiency of photosynthetic complexes in a transient scenario and how that efficiency is affected by environmental noise. Here, following a quantum master equation approach, we study the energy and…

Biomolecules · Quantitative Biology 2013-02-28 Daniel Manzano

Organic molecules store the energy of absorbed light in the form of charge-neutral molecular excitations -- Frenkel excitons. Usually, in amorphous organic materials, excitons are viewed as quasiparticles, localized on single molecules,…

Mesoscale and Nanoscale Physics · Physics 2013-04-02 Semion K. Saikin , Alexander Eisfeld , Stéphanie Valleau , Alán Aspuru-Guzik

We study the geometric properties of the energy landscape of coarse-grained, off-lattice models of polymers by endowing the configuration space with a suitable metric, depending on the potential energy function, such that the dynamical…

Statistical Mechanics · Physics 2007-05-23 Lorenzo N. Mazzoni , Lapo Casetti

The use of eco-friendly materials for the environment has been addressed as a critical issue in the development of systems for renewable energy applications. In this regard, the investigation of organic photovoltaic (OPV) molecules for the…

Chemical Physics · Physics 2017-01-13 Alfredo Guillén-López , Miguel Robles , Jesús Muñiz

The electronic transport properties and switching mechanism of single photochromic diarylethene derivatives sandwiched between two gold surfaces with closed and open configurations are investigated by a fully self-consistent nonequilibrium…

Other Condensed Matter · Physics 2009-11-13 Jing Huang , Qunxiang Li , Hao Ren , Haibin Su , Q. W. Shi , Jinlong Yang

Quantum beats in nonlinear spectroscopy of molecular aggregates are often attributed to electronic phenomena of excitonic systems, while nuclear degrees of freedom are commonly included into models as overdamped oscillations of bath…

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

We propose a local, O(N) molecular dynamics algorithm for the simulation of charged systems. The long ranged Coulomb potential is generated by a propagating electric field that obeys modified Maxwell equations. On coupling the…

Soft Condensed Matter · Physics 2009-11-10 Jörg Rottler , A. C. Maggs

Spectral density functions are central to the simulation of complex many body systems. Their determination requires to make approximations not only to the dynamics but also to the underlying electronic structure theory. Here, blending…

Chemical Physics · Physics 2018-05-23 Per-Arno Plötz , Jörg Megow , Thomas Niehaus , Oliver Kühn

A theoretical description of local absorption is proposed in order to investigate spectral variations on a length scale comparable with the extension of the relevant quantum states. A general formulation is derived within the density-matrix…

Materials Science · Physics 2009-10-31 O. Mauritz , G. Goldoni , F. Rossi , E. Molinari

The Feynman-Vernon path integral formalism is used to derive the density matrix of a quantum oscillator that is linearly coupled to an environmental reservoir. Although low-temperature reservoirs thermalize the oscillator to the usual…

General Physics · Physics 2014-12-15 George E. Cragg

We explore various design principles for efficient excitation energy transport in complex quantum systems. We investigate energy transfer efficiency in randomly disordered geometries consisting of up to 20 chromophores to explore spatial…

Quantum Physics · Physics 2014-02-25 M. Mohseni , A. Shabani , S. Lloyd , Y. Omar , H. Rabitz

Numerous studies have identified large quantum mechanical effects in the dynamics of liquid water. In this paper, we suggest that these effects may have been overestimated due to the use of rigid water models and flexible models in which…

Soft Condensed Matter · Physics 2010-11-05 Scott Habershon , Thomas E. Markland , David E. Manolopoulos

We present a machine learning (ML) framework for predicting Green's functions of molecular systems, from which photoemission spectra and quasiparticle energies at quantum many-body level can be obtained. Kernel ridge regression is adopted…

Chemical Physics · Physics 2023-12-05 Christian Venturella , Christopher Hillenbrand , Jiachen Li , Tianyu Zhu

We propose a new method for the evaluation of the particle density and kinetic pressure profiles in inhomogeneous one-dimensional systems of non-interacting fermions, and apply it to harmonically confined systems of up to N=1000 fermions.…

Statistical Mechanics · Physics 2009-10-31 Patrizia Vignolo , Anna Minguzzi , M. P. Tosi

In this article, we explore the dynamical decoherence of the chromophores within a green fluorescent protein when coupled to a finite-temperature dielectric environment. Such systems are of significant interest due to their anomalously long…

Chemical Physics · Physics 2024-05-08 Adam Burgess , Marian Florescu

Biomolecular thermodynamics and spectroscopy depend on relative conformer energies, local curvatures, and collective dipole fluctuations on the potential-energy surface. Conventional molecular mechanics force fields enable large-scale…

The light-harvesting is a problem of long interest. It becomes active again in recent years stimulated by suggestions of quantum effects in energy transport. Recent experiments found evidence that BChla 1 and BChla 6 are the first to be…

Biological Physics · Physics 2015-06-04 B. Cui , X. X. Yi , C. H. Oh