Abstract
We investigated the mechanism of the third-order nonlinear optical (NLO) response of liquid CS2 by molecular dynamics simulation from both qualitative and quantitative aspects. The time-dependent relative importance of the orientational and collision-induced dynamics of the molecules to the fluctuation of polarizability was analyzed in order to understand the relation between the dynamics of the molecules and the third-order NLO response. Our analysis shows that the fluctuation of polarizability associated with the orientational dynamics of the molecules is responsible for 81% of the total NLO response. We calculated the values of the third-order NLO coefficients and they were found to be in semiquantitative agreement with the experimental values. We discuss the validity of fitting semiempirical theoretical models to the experimental signals as a means to analyze the mechanism of the NLO response.
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.
