A new class of organic crystals with extremely large hyperpolarizability : efficient THz wave generation with wide flat‐spectral‐band

Kim, Seung‐Jun; Yu, In Cheol; Kim, Dong‐Joo; Jazbinsek, Mojca; Yoon, Woojin; Yun, Hoseop; Kim, Dongwook; Rotermund, Fabian; Kwon, O‐Pil

doi:10.1002/adfm.202209915

Please use this identifier to cite or link to this item: https://doi.org/10.21256/zhaw-30289

Publication type:	Article in scientific journal
Type of review:	Peer review (publication)
Title:	A new class of organic crystals with extremely large hyperpolarizability : efficient THz wave generation with wide flat‐spectral‐band
Authors:	Kim, Seung‐Jun Yu, In Cheol Kim, Dong‐Joo Jazbinsek, Mojca Yoon, Woojin Yun, Hoseop Kim, Dongwook Rotermund, Fabian Kwon, O‐Pil
et. al:	No
DOI:	10.1002/adfm.202209915 10.21256/zhaw-30289
Published in:	Advanced Functional Materials
Volume(Issue):	33
Issue:	1
Page(s):	2209915
Issue Date:	Jan-2023
Publisher / Ed. Institution:	Wiley
ISSN:	1616-301X 1616-3028
Language:	English
Subjects:	THz Photonics; Organic nonlinear optics; Organic crystal
Subject (DDC):	621.3: Electrical, communications, control engineering
Abstract:	In organic π-conjugated crystals, enhancing molecular optical nonlinearity of chromophores (e.g., first hyperpolarizability β ≥ 300 × 10−30 esu) in most cases unfortunately results in zero macroscopic optical nonlinearity, which is a bottleneck in organic nonlinear optics. In this study, a new class of nonlinear optical organic crystals introducing a chromophore possessing an extremely large first hyperpolarizability is reported. With newly designed 4-(4-(4-(hydroxymethyl)piperidin-1-yl)styryl)-1-(pyrimidin-2-yl)pyridin-1-ium (PMPR) chromophore, incorporating a head-to-tail cation-anion O-H⋯O hydrogen-bonding synthon and an optimal selection of molecular anion into crystals results in extremely large macroscopic optical nonlinearity with effective first hyperpolarizability of 335 × 10−30 esu. This is in sharp contrast to zero value for previously reported analogous crystals. An ultrathin PMPR crystal with a thickness of ≈10 µm exhibits excellent terahertz (THz) wave generation performance. Both i) broadband THz wave generation with a wide flat-spectral-band in the range of 0.7–3.4 THz defined at −3 dB and high upper cut-off generation frequency of > 7 THz as well as ii) high-generation efficiency (5 times higher THz amplitude than ZnTe crystal with a mm-scale thickness) are simultaneously achieved. Therefore, new PMPR crystals are highly promising materials for diverse applications in nonlinear optics and THz photonics.
URI:	https://digitalcollection.zhaw.ch/handle/11475/30289
Fulltext version:	Accepted version
License (according to publishing contract):	Licence according to publishing contract
Departement:	School of Engineering
Organisational Unit:	Institute of Computational Physics (ICP)
Appears in collections:	Publikationen School of Engineering

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Kim, S.-J., Yu, I. C., Kim, D.-J., Jazbinsek, M., Yoon, W., Yun, H., Kim, D., Rotermund, F., & Kwon, O.-P. (2023). A new class of organic crystals with extremely large hyperpolarizability : efficient THz wave generation with wide flat‐spectral‐band. Advanced Functional Materials, 33(1), 2209915. https://doi.org/10.1002/adfm.202209915

Kim, S.-J. et al. (2023) ‘A new class of organic crystals with extremely large hyperpolarizability : efficient THz wave generation with wide flat‐spectral‐band’, Advanced Functional Materials, 33(1), p. 2209915. Available at: https://doi.org/10.1002/adfm.202209915.

S.-J. Kim et al., “A new class of organic crystals with extremely large hyperpolarizability : efficient THz wave generation with wide flat‐spectral‐band,” Advanced Functional Materials, vol. 33, no. 1, p. 2209915, Jan. 2023, doi: 10.1002/adfm.202209915.

KIM, Seung‐Jun, In Cheol YU, Dong‐Joo KIM, Mojca JAZBINSEK, Woojin YOON, Hoseop YUN, Dongwook KIM, Fabian ROTERMUND und O‐Pil KWON, 2023. A new class of organic crystals with extremely large hyperpolarizability : efficient THz wave generation with wide flat‐spectral‐band. Advanced Functional Materials. Januar 2023. Bd. 33, Nr. 1, S. 2209915. DOI 10.1002/adfm.202209915

Kim, Seung‐Jun, In Cheol Yu, Dong‐Joo Kim, Mojca Jazbinsek, Woojin Yoon, Hoseop Yun, Dongwook Kim, Fabian Rotermund, and O‐Pil Kwon. 2023. “A New Class of Organic Crystals with Extremely Large Hyperpolarizability : Efficient THz Wave Generation with Wide Flat‐Spectral‐Band.” Advanced Functional Materials 33 (1): 2209915. https://doi.org/10.1002/adfm.202209915.

Kim, Seung-Jun, et al. “A New Class of Organic Crystals with Extremely Large Hyperpolarizability : Efficient THz Wave Generation with Wide Flat‐Spectral‐Band.” Advanced Functional Materials, vol. 33, no. 1, Jan. 2023, p. 2209915, https://doi.org/10.1002/adfm.202209915.