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Dichlorinated Organic-Salt Terahertz Sources for THz Spectroscopy
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Publication Year
2023-02-17
Journal
Advanced Optical Materials
Publisher
John Wiley and Sons Inc
Citation
Advanced Optical Materials, Vol.11 No.4
Keyword
halogen bondsnonlinear opticsorganic crystalsself-assemblyterahertz waves
Mesh Keyword
Counter anionsHalogen bondsMolecular anionsOrganic crystalOrganic saltPerformanceSource materialTera HertzTerahertz generationTerahertz sources
All Science Classification Codes (ASJC)
Electronic, Optical and Magnetic MaterialsAtomic and Molecular Physics, and Optics
Abstract
Although in terahertz (THz) source materials molecular anions significantly influence the performance of THz generation, only limited classes of molecular counter anions have been reported. Here, utilizing dichlorinated molecular anions in THz generators is reported for the first time, to the best of our knowledge. In these new crystals, two dichlorinated molecular anions with different molecular symmetries, asymmetric 3,4-dichlorobenzenesulfonate (34DCS) and symmetric 3,5-dichlorobenzenesulfonate (35DCS), are incorporated with a 2-(4-hydroxystyryl)-1-methylquinolinium (OHQ) cation possessing top-level molecular optical nonlinearity. OHQ-34DCS exhibits a strong nonlinear optical response, in contrast to OHQ-35DCS. In OHQ-34DCS crystals, the dichlorinated groups form strong halogen bonds (XBs) and hydrogen bonds (HBs), which are beneficial for suppressing molecular (phonon) vibrations. The optical-to-THz conversion efficiency of the OHQ-34DCS crystals is extremely high, comparable to that of the benchmark organic THz generators. Moreover, the THz emission spectra from the OHQ-34DCS crystals, compared to those of previously reported benchmark analogous crystals, are stronger modulated toward a flatter shape, but possess substantially reduced spectral dimples. Therefore, the introduction of dichlorinated molecular anions is an efficient approach for the design of highly efficient electro-optic salt crystals as efficient broadband THz wave sources.
ISSN
2195-1071
Language
eng
URI
https://aurora.ajou.ac.kr/handle/2018.oak/33129
https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=85144100748&origin=inward
DOI
https://doi.org/10.1002/adom.202202027
Journal URL
http://onlinelibrary.wiley.com/journal/10.1002/(ISSN)2195-1071
Type
Article
Funding
B.R.S. and I.C.Y. contributed equally to this work. This work has been supported by the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT & Future Planning, Korea (No. 2021R1A2C1005012, 2021R1A5A6002853, 2019K1A3A1A14057973, 2019R1A2C3003504), Institute of Information & communications Technology Planning & Evaluation (IITP) grant funded by the Korea government (MSIT) (No. 2022\u20100\u201000624) and Swiss National Science Foundation (SNSF), Switzerland (No. IZKSZ2_188194). X\u2010ray structural analysis was supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (2019R1I1A2A01058066).
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Yun, Hoseop윤호섭
Department of Chemistry
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