Nikolaj A. Zhestkij, Anastasiia S. Efimova, Maria Timofeeva, Alexander S. Novikov, Irina A. Gorbunova, Daria A. Shipilovskikh, Maksim V. Dmitriev, Sergei A. Shipilovskikh, Valentin A. Milichko
{"title":"Chemical Tuning of Second Harmonic Generation Efficiency in Aminothiophene-Based Molecular Microcrystals","authors":"Nikolaj A. Zhestkij, Anastasiia S. Efimova, Maria Timofeeva, Alexander S. Novikov, Irina A. Gorbunova, Daria A. Shipilovskikh, Maksim V. Dmitriev, Sergei A. Shipilovskikh, Valentin A. Milichko","doi":"10.1021/acs.jpcc.4c04885","DOIUrl":null,"url":null,"abstract":"We report on a chemical way to tune the efficiency of second harmonic generation (SHG) by aminothiophene-based molecular crystals (MCs) of a fixed noncentrosymmetric crystal structure. Through the multistep synthesis of three substituted pyrrolo[1,2-<i>a</i>]thieno[3,2-<i>e</i>]pyrimidines, we design a set of MCs of a similar <i>Pna</i>21 space group, providing stable (over 30 min of continuous generation) SHG in a controlled visible spectral range. Substitution of the donor methyl component of the MC with neutral hydrogen and acceptor chlorine leads to an approximately 400-fold increase in SHG efficiency due to 70% growth of the MC's hyperpolarizability. The reported chemical strategy, thereby, opens the way to design MCs and tune their SHG efficiency, being competitive with commercial nonlinear optical crystals.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":3.3000,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry C","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpcc.4c04885","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
We report on a chemical way to tune the efficiency of second harmonic generation (SHG) by aminothiophene-based molecular crystals (MCs) of a fixed noncentrosymmetric crystal structure. Through the multistep synthesis of three substituted pyrrolo[1,2-a]thieno[3,2-e]pyrimidines, we design a set of MCs of a similar Pna21 space group, providing stable (over 30 min of continuous generation) SHG in a controlled visible spectral range. Substitution of the donor methyl component of the MC with neutral hydrogen and acceptor chlorine leads to an approximately 400-fold increase in SHG efficiency due to 70% growth of the MC's hyperpolarizability. The reported chemical strategy, thereby, opens the way to design MCs and tune their SHG efficiency, being competitive with commercial nonlinear optical crystals.
期刊介绍:
The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.