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We present a general computational protocol for the evaluation of extensive molecular response properties in complex environments within a polarizable quantum embedding framework. The approach extends multilevel density functional theory…

Chemical Physics · Physics 2026-02-11 Alberto Barlini , Julien Bloino , Henrik Koch , Tommaso Giovannini

Fully polarizable QM/MM approach based on fluctuating charges and fluctuating dipoles, named QM/FQF{\mu} (J. Chem. Theory Comput. 2019, 15 2233-2245), is extended to the calculation of vertical excitation energies of solvated molecular…

The derivation of linear response theory within polarizable embedding is carried out from a rigorous quantum-mechanical treatment of a composite system. Two different subsystem decompositions (symmetric and nonsymmetric) of the linear…

Chemical Physics · Physics 2017-10-09 Nanna Holmgaard List , Patrick Norman , Jacob Kongsted , Hans Jørgen Aagaard Jensen

We investigate the coupling of different quantum-embedding approaches with a third molecular-mechanics layer, which can be either polarizable or non-polarizable. In particular, such a coupling is discussed for the multilevel families of…

Chemical Physics · Physics 2020-12-11 Linda Goletto , Tommaso Giovannini , Sarai D. Folkestad , Henrik Koch

We present an extension of the standard polarizable quantum mechanic/molecular mechanics (QM/MM) approach for treating environmental effects on excited state properties of embedded systems. A quantum polarizable atom model is derived from a…

Chemical Physics · Physics 2018-08-08 Vladislav Sláma , Frank Müh , Thomas Renger , Tomáš Mančal

We present the theoretical derivation and numerical implementation of the linear response equations for relativistic quantum electrodynamical density functional theory (QEDFT). In contrast to previous works based on the Pauli-Fierz…

Chemical Physics · Physics 2024-07-09 Lukas Konecny , Valeriia P. Kosheleva , Heiko Appel , Michael Ruggenthaler , Angel Rubio

Accurately predicting response properties of molecules such as the dynamic polarizability and hyperpolarizability using quantum mechanics has been a long-standing challenge with widespread applications in material and drug design. Classical…

Chemical Physics · Physics 2020-09-01 Xiaoxia Cai , Wei-Hai Fang , Heng Fan , Zhendong Li

Implicit electron-density solvation models based on joint density-functional theory offer a computationally efficient solution to the problem of calculating thermodynamic quantities of solvated systems from firstprinciples quantum…

Chemical Physics · Physics 2015-02-12 Deniz Gunceler , T. A. Arias

A multiscale model based on the coupling of the multiconfigurational self-consistent field (MCSCF) method and the classical atomistic polarizable Fluctuating Charges (FQ) force field is presented. The resulting MCSCF/FQ approach is…

Non-local electrostatic interactions associated with the finite solvent size and ion polarizability are investigated within the mean-field linear response theory. To this end, we introduce a field theoretic model of a polar liquid composed…

Soft Condensed Matter · Physics 2015-06-15 Sahin Buyukdagli , Tapio Ala-Nissila

Polarizable Quantum Mechanics/Molecular Mechanics (QM/MM) approaches based on fluctuating charges and dipoles (QM/FQ(F$\mu$)) are formulated within the state-specific Vertical Excitation Model (VEM) to compute vertical excitation energies…

Chemical Physics · Physics 2025-11-05 Chiara Sepali , Piero Lafiosca , Linda Goletto , Tommaso Giovannini , Chiara Cappelli

Delivering the full benefits of first principles calculations to battery materials demands the development of accurate and computationally-efficient electronic structure methods that incorporate the effects of the electrolyte environment…

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

Quantum computing presents a promising avenue for solving complex problems, particularly in quantum chemistry, where it could accelerate the computation of molecular properties and excited states. This work focuses on hybrid…

The nonlinear response is investigated for a space-fractional quantum mechanical system subject to a static electric field. Expressions for the polarizability and hyperpolarizability are derived from the fractional Schr\"{o}dinger equation…

Quantum Physics · Physics 2016-09-29 Nathan J. Dawson

The dynamics of the electrons for a molecule in solution is coupled to the dynamics of its polarizable environment, i.e., the solvent. To theoretically investigate such electronic dynamics, we have recently developed equations of motion…

Chemical Physics · Physics 2017-02-16 Silvio Pipolo , Stefano Corni , Roberto Cammi

Electronic polarization and dispersion are decisive actors in determining interaction energies between molecules. These interactions have a particularly profound effect on excitation energies of molecules in complex environments, especially…

Chemical Physics · Physics 2024-12-13 Thomas P. Fay , Nicolas Ferré , Miquel Huix-Rotllant

The Polarizable Continuum Model (PCM) can be used in conjunction with Density Functional Theory (DFT) and its time-dependent extension (TDDFT) to simulate the electronic and optical properties of molecules and nanoparticles immersed in a…

Materials Science · Physics 2015-10-28 Alain Delgado , Stefano Corni , Stefano Pittalis , Carlo Andrea Rozzi

We present the extension of the quantum/classical polarizable fluctuating charge model to the calculation of single residues of quadratic response functions, as required for the computational modeling of two-photon absorption…

Computational Physics · Physics 2022-10-28 Roberto Di Remigio , Tommaso Giovannini , Matteo Ambrosetti , Chiara Cappelli , Luca Frediani

We present the development and implementation of the relativistic coupled cluster linear response theory (CC-LR) which allows the determination of molecular properties arising from time-dependent or time-independent electric, magnetic, or…

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