RT Journal Article
T1 Charge delocalization and hyperpolarizability in ionic liquids
A1 Rodríguez-Fernández, Carlos Damián
A1 Varela Cabo, Luis Miguel
A1 Schröder, Christian
A1 López Lago, María Elena
K1 Ionic Liquids (ILs)
K1 Hyperpolarizability
K1 Non-linear Susceptibility
K1 Second Harmonic Generation (SHG)
K1 Electro-Optical Kerr-Effect (EOKE)
K1 Charge delocalization
K1 Density functional theory (DFT)
AB In this work the role that charge delocalization plays in the non-linear optical response of ionic liquids is evaluated. The first hyperpolarizability for the non-linear process of second harmonic generation (SHG) and second hyperpolarizability for the non-linear process of electro-optical Kerr-Effect (EOKE) of a large number of ionic liquid forming ions were estimated by means of density functional theory calculations. The results point to that both charge delocalization and molecular geometry are the key features that govern their hyperpolarizabilities. Our findings show that some of the most commonly used anions in ionic liquids are expected to present strong non-linear responses while common cations present a much more limited performance. However, this limitation can be overcome by a proper tailoring of cations to present charge delocalization over large molecular regions. The hypothesis of additivity of hyperpolarizabilities in ionic liquids is tested and exploited to obtain a map of second and third order non-linear susceptibilities of 1496 ion combinations. This map is intended to be a guide for future works on the hyperpolarizability of ILs
PB Elsevier
YR 2022
FD 2022
LK http://hdl.handle.net/10347/27901
UL http://hdl.handle.net/10347/27901
LA eng
NO Journal of Molecular Liquids 349 (2022) 118153. https://doi.org/10.1016/j.molliq.2021.118153
NO This work was supported by Ministerio de Economia y Competitividad (MINECO) and FEDER 17 Program through the projects (MAT2017-89239-C2-1-P); Xunta de Galicia and FEDER (GRC ED431C 2016/001, ED431D 2017/06, ED431E2018/08). C. D. R. F. thanks the support of Xunta de Galicia through the grant ED481A-2018/032. We also thank the Centro de Supercomputacion de Galicia (CESGA) facility, Santiago de Compostela, Galicia, Spain, for providing the computational resources employed in this work
DS Minerva
RD 28 abr 2026