Role of Environmental Dynamic Polarizability in Static Excited State Properties of Embedded Molecular Systems: Application to Disordered Fluorographene Systems

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F23%3A10475187" target="_blank" >RIV/00216208:11320/23:10475187 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=5845iOQsks" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=5845iOQsks</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jpcc.2c06779" target="_blank" >10.1021/acs.jpcc.2c06779</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Role of Environmental Dynamic Polarizability in Static Excited State Properties of Embedded Molecular Systems: Application to Disordered Fluorographene Systems

Popis výsledku v původním jazyce

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 full quantum description of the environment using perturbation theory for the system-environment coupling. Our model provides a more general description of the environment, including frequency-dependent atomic polarizabilities, without the loss of computational simplicity of the QM/MM approach. The classical polarizable atom description, used in the polarizable QM/ MM approach, can be obtained as a limiting case of the present model. This result enables us to pinpoint approximations and assumptions about the system inherent to a classical polarizable atom description of the environment. We apply our method to fluorographene (FG)-based systems to investigate the effects of the FG sheet on excited state properties of impurities on the FG surface. The comparison to full quantum chemistry calculations and to the standard polarizable QM/MM approach on disordered fluorographene clusters reveals the importance of the frequency dependence of atomic polarizabilities for a proper treatment of the effects of the environment on both the transition energy shifts and the interaction energies.

Název v anglickém jazyce

Role of Environmental Dynamic Polarizability in Static Excited State Properties of Embedded Molecular Systems: Application to Disordered Fluorographene Systems

Popis výsledku anglicky

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 full quantum description of the environment using perturbation theory for the system-environment coupling. Our model provides a more general description of the environment, including frequency-dependent atomic polarizabilities, without the loss of computational simplicity of the QM/MM approach. The classical polarizable atom description, used in the polarizable QM/ MM approach, can be obtained as a limiting case of the present model. This result enables us to pinpoint approximations and assumptions about the system inherent to a classical polarizable atom description of the environment. We apply our method to fluorographene (FG)-based systems to investigate the effects of the FG sheet on excited state properties of impurities on the FG surface. The comparison to full quantum chemistry calculations and to the standard polarizable QM/MM approach on disordered fluorographene clusters reveals the importance of the frequency dependence of atomic polarizabilities for a proper treatment of the effects of the environment on both the transition energy shifts and the interaction energies.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)

Projekt

<a href="/cs/project/GA18-18022S" target="_blank" >GA18-18022S: Bioinspirované světlosběrné systémy na bázi grafenu</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2023

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Journal of Physical Chemistry C

ISSN

1932-7447

e-ISSN

1932-7455

Svazek periodika

127

Číslo periodika v rámci svazku

1

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

12

Strana od-do

381-392

Kód UT WoS článku

000907825600001

EID výsledku v databázi Scopus

2-s2.0-85145467277