Explicit versus implicit solvation effects on the first hyperpolarizability of an organic biphotochrome

Jean Quertinmont, Benoit Champagne, Frédéric Castet, Marcelo Hidalgo Cardenuto

Research output: Contribution to journalArticle

Abstract

The first hyperpolarizability of the four trans forms of a dithienylethene indolinooxazolidine biphotochrome in acetonitrile solution has been evaluated by using two solvation models, an explicit and an implicit one. The implicit solvation model is the integral equation formalism of the polarizable continuum model (IEF-PCM), whereas in the explicit one, the solvent molecules are represented by point charges, of which the positions have been generated by Monte Carlo simulations whereas the solute is treated quantum mechanically. At optical frequencies, first hyperpolarizabilities calculated with the implicit solvation model are usually larger than those obtained with the multiscale approach. However, both approaches predict similar contrasts, indicating that implicit solvation models such as IEF-PCM are well-suited to describe the variations in the NLO responses of molecular switches. In addition, the analysis of the contrasts of first hyperpolarizabilities shows that the biphotochrome can act as a three-state NLO switch.

Original languageEnglish
Pages (from-to)5496-5503
Number of pages8
JournalJournal of physical chemistry A
Volume119
Issue number21
DOIs
Publication statusPublished - 28 May 2015

Fingerprint

Solvation
solvation
Integral equations
integral equations
switches
Switches
formalism
continuums
acetonitrile
solutes
Molecules
molecules
simulation

Cite this

@article{11fcdf258ee249fdb1146f2b6a639926,
title = "Explicit versus implicit solvation effects on the first hyperpolarizability of an organic biphotochrome",
abstract = "The first hyperpolarizability of the four trans forms of a dithienylethene indolinooxazolidine biphotochrome in acetonitrile solution has been evaluated by using two solvation models, an explicit and an implicit one. The implicit solvation model is the integral equation formalism of the polarizable continuum model (IEF-PCM), whereas in the explicit one, the solvent molecules are represented by point charges, of which the positions have been generated by Monte Carlo simulations whereas the solute is treated quantum mechanically. At optical frequencies, first hyperpolarizabilities calculated with the implicit solvation model are usually larger than those obtained with the multiscale approach. However, both approaches predict similar contrasts, indicating that implicit solvation models such as IEF-PCM are well-suited to describe the variations in the NLO responses of molecular switches. In addition, the analysis of the contrasts of first hyperpolarizabilities shows that the biphotochrome can act as a three-state NLO switch.",
author = "Jean Quertinmont and Benoit Champagne and Fr{\'e}d{\'e}ric Castet and {Hidalgo Cardenuto}, Marcelo",
year = "2015",
month = "5",
day = "28",
doi = "10.1021/acs.jpca.5b00631",
language = "English",
volume = "119",
pages = "5496--5503",
journal = "The journal of physical chemistry. A",
issn = "1089-5639",
publisher = "American Chemical Society",
number = "21",

}

Explicit versus implicit solvation effects on the first hyperpolarizability of an organic biphotochrome. / Quertinmont, Jean; Champagne, Benoit; Castet, Frédéric; Hidalgo Cardenuto, Marcelo.

In: Journal of physical chemistry A, Vol. 119, No. 21, 28.05.2015, p. 5496-5503.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Explicit versus implicit solvation effects on the first hyperpolarizability of an organic biphotochrome

AU - Quertinmont, Jean

AU - Champagne, Benoit

AU - Castet, Frédéric

AU - Hidalgo Cardenuto, Marcelo

PY - 2015/5/28

Y1 - 2015/5/28

N2 - The first hyperpolarizability of the four trans forms of a dithienylethene indolinooxazolidine biphotochrome in acetonitrile solution has been evaluated by using two solvation models, an explicit and an implicit one. The implicit solvation model is the integral equation formalism of the polarizable continuum model (IEF-PCM), whereas in the explicit one, the solvent molecules are represented by point charges, of which the positions have been generated by Monte Carlo simulations whereas the solute is treated quantum mechanically. At optical frequencies, first hyperpolarizabilities calculated with the implicit solvation model are usually larger than those obtained with the multiscale approach. However, both approaches predict similar contrasts, indicating that implicit solvation models such as IEF-PCM are well-suited to describe the variations in the NLO responses of molecular switches. In addition, the analysis of the contrasts of first hyperpolarizabilities shows that the biphotochrome can act as a three-state NLO switch.

AB - The first hyperpolarizability of the four trans forms of a dithienylethene indolinooxazolidine biphotochrome in acetonitrile solution has been evaluated by using two solvation models, an explicit and an implicit one. The implicit solvation model is the integral equation formalism of the polarizable continuum model (IEF-PCM), whereas in the explicit one, the solvent molecules are represented by point charges, of which the positions have been generated by Monte Carlo simulations whereas the solute is treated quantum mechanically. At optical frequencies, first hyperpolarizabilities calculated with the implicit solvation model are usually larger than those obtained with the multiscale approach. However, both approaches predict similar contrasts, indicating that implicit solvation models such as IEF-PCM are well-suited to describe the variations in the NLO responses of molecular switches. In addition, the analysis of the contrasts of first hyperpolarizabilities shows that the biphotochrome can act as a three-state NLO switch.

UR - http://www.scopus.com/inward/record.url?scp=84930663744&partnerID=8YFLogxK

U2 - 10.1021/acs.jpca.5b00631

DO - 10.1021/acs.jpca.5b00631

M3 - Article

VL - 119

SP - 5496

EP - 5503

JO - The journal of physical chemistry. A

JF - The journal of physical chemistry. A

SN - 1089-5639

IS - 21

ER -