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This paper presents the first implementation of a coupling between advanced wave function theories and molecular density functional theory (MDFT). This method enables the modeling of solvent effect into quantum mechanical (QM) calculations…

Chemical Physics · Physics 2024-04-12 Maxime Labat , Emmanuel Giner , Guillaume Jeanmairet

A comprehensive description of molecular electron transfer reactions is essential for our understanding of fundamental phenomena in bio-energetics and molecular electronics. Experimental studies of molecular systems in condensed-phase…

Quantum Physics · Physics 2021-02-04 Frank Schlawin , Manuel Gessner , Andreas Buchleitner , Tobias Schaetz , Spiros S Skourtis

Quantum-chemical processes in liquid environments impact broad areas of science, from molecular biology to geology to electrochemistry. While density-functional theory (DFT) has enabled efficient quantum-mechanical calculations which…

Chemical Physics · Physics 2017-10-16 Kendra Letchworth-Weaver , Ravishankar Sundararaman , T. A. Arias

We perform model calculations for a stretched LiF molecule, demonstrating that nonadiabatic charge transfer effects can be accurately and seamlessly described within a density functional framework. In alkali halides like LiF, there is an…

Chemical Physics · Physics 2018-03-01 Chen Li , Ryan Requist , E. K. U. Gross

Many chemical systems cannot be described by quantum chemistry methods based on a singlereference wave function. Accurate predictions of energetic and spectroscopic properties require a delicate balance between describing the most important…

Chemical Physics · Physics 2018-06-12 Erik Donovan Hedegård , Julien Toulouse , Hans Jørgen Aagaard Jensen

We have developed and implemented a new quantum molecular dynamics approximation that allows fast and accurate simulations of dense plasmas from cold to hot conditions. The method is based on a carefully designed orbital-free implementation…

Plasma Physics · Physics 2015-06-22 Travis Sjostrom , Jerome Daligault

We propose a new molecular simulation framework that combines the transferability, robustness and chemical flexibility of an ab initio method with the accuracy and efficiency of a machine learned force field. The key to achieve this mix is…

Computational Physics · Physics 2020-01-08 Sebastian Dick , Marivi Fernandez-Serra

Classical density functional theory (cDFT) and dynamical density functional theory (DDFT) are modern statistical mechanical theories for modeling many-body colloidal systems at the one-body density level. The theories hinge on knowing the…

A fundamental assumption of the dynamical density functional theory (DDFT) of colloidal systems is that a grand-canonical free energy functional may be employed to generate the thermodynamic driving forces. Using one-dimensional hard-rods…

Soft Condensed Matter · Physics 2013-06-04 Johannes Reinhardt , Joseph Michael Brader

The non-radiative electron-relaxation dynamics in C$_{60}$ molecule is studied after selective initial photoexcitations. The methodology includes nonadibabtic molecular simulation combined with time-dependent density functional theory (DFT)…

Atomic and Molecular Clusters · Physics 2023-06-29 Esam Ali , Mohamed El-Amine Madjet , Ruma De , Thomas Frauenheim , Himadri S. Chakraborty

The stationary functional of the all-electron density functional plus dynamical mean field theory (DFT+DMFT) formalism to perform free energy calculations and structural relaxations is implemented for the first time. Here, the first order…

Strongly Correlated Electrons · Physics 2015-12-23 Kristjan Haule , Turan Birol

Achieving chemical accuracy for molecular simulations remains a central challenge in computational chemistry. Here, we present an embedded correlated wavefunction transfer learning (ECW-TL) framework for accurately simulating molecular…

Chemical Physics · Physics 2026-03-18 Xuezhi Bian , Emily A. Carter

Plane-wave electronic-structure predictions based upon orbital-dependent density-functional theory (OD-DFT) approximations, such as hybrid density-functional methods and self-interaction density-functional corrections, are severely affected…

Materials Science · Physics 2011-10-19 Yanli Li , Ismaila Dabo

Multideterminant calculations have been performed on model systems to emphasize the role of many-body effects in the general description of charge quantization experiments. We show numerically and derive analytically that a closed-shell…

Mesoscale and Nanoscale Physics · Physics 2015-05-13 V. Geskin , R. Stadler , J. Cornil

Density Functional Theory (DFT) is one of the most widely used methods for "ab initio" calculations of the structure of atoms, molecules, crystals, surfaces, and their interactions. Unfortunately, the customary introduction to DFT is often…

Physics Education · Physics 2010-12-07 Nathan Argaman , Guy Makov

Calculating charge transfer (CT) excitation energies with high accuracy and low computational cost is a challenging task. Kohn-Sham density functional theory (KS-DFT), due to its efficiency and accuracy, has achieved great success in…

Chemical Physics · Physics 2019-05-01 Yuncai Mei , Weitao Yang

Time-Dependent Density Functional Theory (TDDFT) has recently been extended to describe many-body open quantum systems (OQS) evolving under non-unitary dynamics according to a quantum master equation. In the master equation approach,…

Chemical Physics · Physics 2015-05-18 David G. Tempel , Mark A. Watson , Roberto Olivares-Amaya , Alán Aspuru-Guzik

We investigate the time an electronic excitation travels in a supermolecular setup using a measurement process in an open quantum-system framework. The approach is based on the stochastic Schr\"odinger equation and uses a Hamiltonian from…

Materials Science · Physics 2013-12-09 Dirk Hofmann , Heiko Appel , Massimiliano Di Ventra , Stephan Kümmel

Static electric response properties of atoms and molecules are reported within the real-space Cartesian grid implementation of pseudopotential Kohn-Sham (KS) density functional theory (DFT). A detailed systematic investigation is made for a…

Chemical Physics · Physics 2019-04-26 Tanmay Mandal , Abhisek Ghosal , Amlan K. Roy

Traditional finite-temperature Kohn-Sham density functional theory (KSDFT) has an unfavorable scaling with respect to the electron number or at high temperatures. The evaluation of the ground-state density in KSDFT can be replaced by the…

Computational Physics · Physics 2022-10-05 Qianrui Liu , Mohan Chen
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