W.D. Chen, D. C. Rodenberger, R. Shi, Q. Zhou, A. Garito
{"title":"Excited State Dynamics of the Third Order Nonlinear Optical Susceptibility in Conjugated Linear Chains","authors":"W.D. Chen, D. C. Rodenberger, R. Shi, Q. Zhou, A. Garito","doi":"10.1364/otfa.1993.tha.1","DOIUrl":null,"url":null,"abstract":"We have earlier presented theoretical and experimental results demonstrating that the nonresonant third order optical susceptibility χ(3)(−ω;ω,ω,−ω) can be enhanced for nonlinear optical processes originating from real population of electronic excited states in conjugated linear chains[1,2]. Compared with the ground state, χ(3)(−ω;ω,ω,−ω) of π-conjugated linear chains can be enhanced by orders of magnitude when the first S1 or second S2 π-electron excited state is optically pumped and then populated for times long enough to perform nonresonant measurements of χ(3)(−ω;ω,ω,−ω) at frequencies different from the resonant pump frequency. In this paper, a dynamical model is developed for the time evolution of the nonresonant microscoopic degenerate four wave mixing (DFWM) susceptibility γ(-ω;ω,ω,-ω) for the excited state enhancement mechanism. The model is applied to the case of the six site chain, diphenylhexatriene (DPH).","PeriodicalId":246676,"journal":{"name":"Organic Thin Films for Photonic Applications","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Organic Thin Films for Photonic Applications","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1364/otfa.1993.tha.1","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0
Abstract
We have earlier presented theoretical and experimental results demonstrating that the nonresonant third order optical susceptibility χ(3)(−ω;ω,ω,−ω) can be enhanced for nonlinear optical processes originating from real population of electronic excited states in conjugated linear chains[1,2]. Compared with the ground state, χ(3)(−ω;ω,ω,−ω) of π-conjugated linear chains can be enhanced by orders of magnitude when the first S1 or second S2 π-electron excited state is optically pumped and then populated for times long enough to perform nonresonant measurements of χ(3)(−ω;ω,ω,−ω) at frequencies different from the resonant pump frequency. In this paper, a dynamical model is developed for the time evolution of the nonresonant microscoopic degenerate four wave mixing (DFWM) susceptibility γ(-ω;ω,ω,-ω) for the excited state enhancement mechanism. The model is applied to the case of the six site chain, diphenylhexatriene (DPH).