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

doi:10.1002/adom.202100324

Publication type:	Article in scientific journal
Type of review:	Peer review (publication)
Title:	Organic THz generators : a design strategy for organic crystals with ultralarge macroscopic hyperpolarizability
Authors:	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
et. al:	No
DOI:	10.1002/adom.202100324
Published in:	Advanced Optical Materials
Volume(Issue):	9
Issue:	19
Page(s):	2100324
Issue Date:	2021
Publisher / Ed. Institution:	Wiley
ISSN:	2195-1071
Language:	English
Subjects:	THz photonics; Nonlinear optics; Electro-optic crystal; Halogenated organic crystal
Subject (DDC):	621.3: Electrical, communications, control engineering
Abstract:	Newly 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 millimetres 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.
URI:	https://digitalcollection.zhaw.ch/handle/11475/24340
Fulltext version:	Published version
License (according to publishing contract):	Licence according to publishing contract
Departement:	School of Engineering
Organisational Unit:	Institute of Computational Physics (ICP)
Published as part of the ZHAW project:	Molecular Phonon-Mode Engineering for All-Organic Gap-Free THz Photonics
Appears in collections:	Publikationen School of Engineering

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Seok, J.-H., Kim, D., Kim, W. T., Kim, S.-J., Yoon, W., Yoon, G.-E., Yu, I. C., Jazbinsek, M., Kim, S.-W., Yun, H., Kim, D., Rotermund, F., & Kwon, O.-P. (2021). Organic THz generators : a design strategy for organic crystals with ultralarge macroscopic hyperpolarizability. Advanced Optical Materials, 9(19), 2100324. https://doi.org/10.1002/adom.202100324

Seok, J.-H. et al. (2021) ‘Organic THz generators : a design strategy for organic crystals with ultralarge macroscopic hyperpolarizability’, Advanced Optical Materials, 9(19), p. 2100324. Available at: https://doi.org/10.1002/adom.202100324.

J.-H. Seok et al., “Organic THz generators : a design strategy for organic crystals with ultralarge macroscopic hyperpolarizability,” Advanced Optical Materials, vol. 9, no. 19, p. 2100324, 2021, doi: 10.1002/adom.202100324.

SEOK, Jin‐Hong, Deokjoong KIM, Won Tae KIM, Seung‐Jun KIM, Woojin YOON, Ga‐Eun YOON, In Cheol YU, Mojca JAZBINSEK, Sang‐Wook KIM, Hoseop YUN, Dongwook KIM, Fabian ROTERMUND und O‐Pil KWON, 2021. Organic THz generators : a design strategy for organic crystals with ultralarge macroscopic hyperpolarizability. Advanced Optical Materials. 2021. Bd. 9, Nr. 19, S. 2100324. DOI 10.1002/adom.202100324

Seok, Jin‐Hong, Deokjoong Kim, Won Tae Kim, Seung‐Jun Kim, Woojin Yoon, Ga‐Eun Yoon, In Cheol Yu, et al. 2021. “Organic THz Generators : A Design Strategy for Organic Crystals with Ultralarge Macroscopic Hyperpolarizability.” Advanced Optical Materials 9 (19): 2100324. https://doi.org/10.1002/adom.202100324.

Seok, Jin-Hong, et al. “Organic THz Generators : A Design Strategy for Organic Crystals with Ultralarge Macroscopic Hyperpolarizability.” Advanced Optical Materials, vol. 9, no. 19, 2021, p. 2100324, https://doi.org/10.1002/adom.202100324.