Abstract
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.
Sign-in/Register to access full text options 
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
