Phase-Sensitive Vibrational SFG Spectra from Simple Classical Force Field Molecular Dynamics Simulations

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60076658%3A12310%2F20%3A43901133" target="_blank" >RIV/60076658:12310/20:43901133 - isvavai.cz</a>

Výsledek na webu

<a href="https://pubs.acs.org/doi/10.1021/acs.jpcc.0c03576" target="_blank" >https://pubs.acs.org/doi/10.1021/acs.jpcc.0c03576</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jpcc.0c03576" target="_blank" >10.1021/acs.jpcc.0c03576</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Phase-Sensitive Vibrational SFG Spectra from Simple Classical Force Field Molecular Dynamics Simulations

Popis výsledku v původním jazyce

We show that phase-sensitive vibrational sum frequency generation (SFG) spectra of solid/water and air/water interfaces, neutral and charged, can be successfully predicted using classical molecular dynamics (CMD) simulations in combination with simple nonpolarizable force fields (FFs). This can be achieved when employing velocity-velocity autocorrelation functions weighted by parameterized Raman and atomic polar tensors for the computation of the SFG. This procedure avoids computing polarizability tensors and dipole moments using either costly ab initio molecular dynamics (AIMD) simulations or CMD simulations with more complex and computationally demanding FFs. Such a methodology paves the way to a broad usage and computationally low-cost theoretical SFG spectroscopy, as even flexible nonpolarizable water models and common FFs for inorganic surfaces can provide good predictions of the SFG spectra, in rather good qualitative agreement with AIMD and/or experiments. The strongly reduced computational cost in our approach opens the possibility to study larger systems for long periods of time, for example, allowing a detailed characterization of the electric double-layer formation at interfaces with &quot;environmentally relevant&quot; ionic concentrations (mM), extracting fingerprints by theoretical CMD-SFG spectroscopy.

Název v anglickém jazyce

Phase-Sensitive Vibrational SFG Spectra from Simple Classical Force Field Molecular Dynamics Simulations

Popis výsledku anglicky

We show that phase-sensitive vibrational sum frequency generation (SFG) spectra of solid/water and air/water interfaces, neutral and charged, can be successfully predicted using classical molecular dynamics (CMD) simulations in combination with simple nonpolarizable force fields (FFs). This can be achieved when employing velocity-velocity autocorrelation functions weighted by parameterized Raman and atomic polar tensors for the computation of the SFG. This procedure avoids computing polarizability tensors and dipole moments using either costly ab initio molecular dynamics (AIMD) simulations or CMD simulations with more complex and computationally demanding FFs. Such a methodology paves the way to a broad usage and computationally low-cost theoretical SFG spectroscopy, as even flexible nonpolarizable water models and common FFs for inorganic surfaces can provide good predictions of the SFG spectra, in rather good qualitative agreement with AIMD and/or experiments. The strongly reduced computational cost in our approach opens the possibility to study larger systems for long periods of time, for example, allowing a detailed characterization of the electric double-layer formation at interfaces with &quot;environmentally relevant&quot; ionic concentrations (mM), extracting fingerprints by theoretical CMD-SFG spectroscopy.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/GA17-10734S" target="_blank" >GA17-10734S: Molekulární popis jevů v elektrické dvojvrstvě - predikce a interpretace experimentálních dat počítačovými simulacemi</a><br>

Návaznosti

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

Rok uplatnění

2020

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

—

Svazek periodika

124

Číslo periodika v rámci svazku

28

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

11

Strana od-do

15253-15263

Kód UT WoS článku

000551543800033

EID výsledku v databázi Scopus

2-s2.0-85089263723