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Organic THz Generators: A Design Strategy for Organic Crystals with Ultralarge Macroscopic Hyperpolarizability
  • Seok, Jin Hong ;
  • Kim, Deokjoong ;
  • Kim, Won Tae ;
  • Kim, Seung Jun ;
  • Yoon, Woojin ;
  • Yoon, Ga Eun ;
  • Yu, In Cheol ;
  • Jazbinsek, Mojca ;
  • Kim, Sang Wook ;
  • Yun, Hoseop ;
  • Kim, Dongwook ;
  • Rotermund, Fabian ;
  • Kwon, O. Pil
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dc.contributor.authorSeok, Jin Hong-
dc.contributor.authorKim, Deokjoong-
dc.contributor.authorKim, Won Tae-
dc.contributor.authorKim, Seung Jun-
dc.contributor.authorYoon, Woojin-
dc.contributor.authorYoon, Ga Eun-
dc.contributor.authorYu, In Cheol-
dc.contributor.authorJazbinsek, Mojca-
dc.contributor.authorKim, Sang Wook-
dc.contributor.authorYun, Hoseop-
dc.contributor.authorKim, Dongwook-
dc.contributor.authorRotermund, Fabian-
dc.contributor.authorKwon, O. Pil-
dc.date.issued2021-10-01-
dc.identifier.issn2195-1071-
dc.identifier.urihttps://aurora.ajou.ac.kr/handle/2018.oak/32085-
dc.identifier.urihttps://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=85107974989&origin=inward-
dc.description.abstractNewly designed halogenated organic quinolinium crystals proposed in this work provide fully optimized molecular ordering for maximizing the optical nonlinearity and high-performance broadband terahertz (THz) wave generation. The ultralarge diagonal optical nonlinearity (almost 300 × 10−30 esu) of the new halogenated crystals is approximately two times larger than that of state-of-the-art pyridinium-based crystals. In contrast, nonhalogenated analogous crystals exhibit very low (or vanishing) diagonal optical nonlinearity. This is attributed to halogen-induced unique interionic interactions and fine-tuning of the space-filling characteristics. In addition, the halogenated crystals show a good ability for bulk crystal growth of few millimeters lateral size with plate-like morphology and high thermal stability that are finally required for real-world applications. The new halogenated quinolinium crystals exhibit excellent THz wave generation characteristics, significantly surpassing the limit of conversion efficiency and spectral bandwidth of inorganic benchmark crystals. A 0.16 mm thick chlorinated crystal generates a 29-times larger THz field than 1.0 mm thick inorganic ZnTe crystals at 1500 nm pump wavelength with a flat and broadband spectrum extending up to ≈8 THz. Therefore, introducing halogen substituents is a potential design strategy for designing new organic crystals showing ultralarge macroscopic hyperpolarizability and high-performance THz wave generation.-
dc.description.sponsorshipJ.H.S., D.K., and W.T.K. 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 (Nos. 2021R1A5A6002853, 2021R1A2C1005012, 2019K1A3A1A14057973, 2019R1A2C3003504, and 2020R1A4A2002828) 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 (No. 2019R1I1A2A01058066).-
dc.language.isoeng-
dc.publisherJohn Wiley and Sons Inc-
dc.subject.meshBroad-band spectrum-
dc.subject.meshBroadband terahertz-
dc.subject.meshBulk crystal growth-
dc.subject.meshHigh thermal stability-
dc.subject.meshHyper-polarizability-
dc.subject.meshInterionic interactions-
dc.subject.meshOptical nonlinearity-
dc.subject.meshPlate-like morphology-
dc.titleOrganic THz Generators: A Design Strategy for Organic Crystals with Ultralarge Macroscopic Hyperpolarizability-
dc.typeArticle-
dc.citation.number19-
dc.citation.titleAdvanced Optical Materials-
dc.citation.volume9-
dc.identifier.bibliographicCitationAdvanced Optical Materials, Vol.9 No.19-
dc.identifier.doi10.1002/adom.202100324-
dc.identifier.scopusid2-s2.0-85107974989-
dc.identifier.urlhttp://onlinelibrary.wiley.com/journal/10.1002/(ISSN)2195-1071-
dc.subject.keywordelectro-optic crystals-
dc.subject.keywordhalogenated organic crystals-
dc.subject.keywordnonlinear optics-
dc.subject.keywordTHz photonics-
dc.type.otherArticle-
dc.description.isoafalse-
dc.subject.subareaElectronic, Optical and Magnetic Materials-
dc.subject.subareaAtomic and Molecular Physics, and Optics-
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