Orthogonal molecular assembly : eliminating intrinsic phonon modes in organic THz generators

Kim, Seung‐Jun; Seok, Jin‐Hong; Yu, In Cheol; Lee, Jeong Hyeon; Kim, Won Tae; Shin, Bong‐Rim; Yoon, Ga‐Eun; Lee, Yun‐Sang; Kim, Jin Chul; Yoon, Woojin; Yun, Hoseop; Jazbinsek, Mojca; Kwak, Sang Kyu; Rotermund, Fabian; Kwon, O‐Pil

doi:10.1002/adom.202102654

Publication type:	Article in scientific journal
Type of review:	Peer review (publication)
Title:	Orthogonal molecular assembly : eliminating intrinsic phonon modes in organic THz generators
Authors:	Kim, Seung‐Jun Seok, Jin‐Hong Yu, In Cheol Lee, Jeong Hyeon Kim, Won Tae Shin, Bong‐Rim Yoon, Ga‐Eun Lee, Yun‐Sang Kim, Jin Chul Yoon, Woojin Yun, Hoseop Jazbinsek, Mojca Kwak, Sang Kyu Rotermund, Fabian Kwon, O‐Pil
et. al:	No
DOI:	10.1002/adom.202102654
Published in:	Advanced Optical Materials
Volume(Issue):	10
Issue:	23
Page(s):	2102654
Issue Date:	2022
Publisher / Ed. Institution:	Wiley
ISSN:	2195-1071
Language:	English
Subject (DDC):	621.3: Electrical, communications, control engineering
Abstract:	This work reports a series of new organic electro-optic salt crystals possessing unusual orthogonal dipole-coupling assembly that act as dimple-free THz generators. In the new crystals, optically anisotropic aromatic anions introducing highly electronegative fluorinated substituents are orthogonally assembled with optically anisotropic nonlinear optical benzothiazolium cations. These orthogonal cation–anion assembled crystals exhibit strong suppression of intrinsic THz phonon modes along the polar axis, which results in a wide THz absorption-free range from 1.5 to 4.0 THz without substantial absorption peaks. This is sharply in contrast to previous benchmark crystals with parallel cation–anion assembly; for example, in analogous crystals, several strong absorption peaks appear in this frequency range. This absence of strong absorption peaks is attributed to the orthogonal cation–anion dipole coupling assembly, the formation of fluorinate-induced strong interionic interactions, and a high packing ability of uniaxial anions. With top-level macroscopic optical nonlinearity, new orthogonal-dipole assembled crystals make dimple-free THz wave generation possible in the range of about 1.5–4.0 THz, which is very beneficial for characterizing signature peaks related to molecular phonon motions of analytes in THz spectroscopy. Therefore, orthogonal molecular assembly of optically highly anisotropic molecules provides an efficient way to substantially reduce and control intrinsic THz phonon modes.
URI:	https://digitalcollection.zhaw.ch/handle/11475/27000
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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Kim, S.-J., Seok, J.-H., Yu, I. C., Lee, J. H., Kim, W. T., Shin, B.-R., Yoon, G.-E., Lee, Y.-S., Kim, J. C., Yoon, W., Yun, H., Jazbinsek, M., Kwak, S. K., Rotermund, F., & Kwon, O.-P. (2022). Orthogonal molecular assembly : eliminating intrinsic phonon modes in organic THz generators. Advanced Optical Materials, 10(23), 2102654. https://doi.org/10.1002/adom.202102654

Kim, S.-J. et al. (2022) ‘Orthogonal molecular assembly : eliminating intrinsic phonon modes in organic THz generators’, Advanced Optical Materials, 10(23), p. 2102654. Available at: https://doi.org/10.1002/adom.202102654.

S.-J. Kim et al., “Orthogonal molecular assembly : eliminating intrinsic phonon modes in organic THz generators,” Advanced Optical Materials, vol. 10, no. 23, p. 2102654, 2022, doi: 10.1002/adom.202102654.

KIM, Seung‐Jun, Jin‐Hong SEOK, In Cheol YU, Jeong Hyeon LEE, Won Tae KIM, Bong‐Rim SHIN, Ga‐Eun YOON, Yun‐Sang LEE, Jin Chul KIM, Woojin YOON, Hoseop YUN, Mojca JAZBINSEK, Sang Kyu KWAK, Fabian ROTERMUND und O‐Pil KWON, 2022. Orthogonal molecular assembly : eliminating intrinsic phonon modes in organic THz generators. Advanced Optical Materials. 2022. Bd. 10, Nr. 23, S. 2102654. DOI 10.1002/adom.202102654

Kim, Seung‐Jun, Jin‐Hong Seok, In Cheol Yu, Jeong Hyeon Lee, Won Tae Kim, Bong‐Rim Shin, Ga‐Eun Yoon, et al. 2022. “Orthogonal Molecular Assembly : Eliminating Intrinsic Phonon Modes in Organic THz Generators.” Advanced Optical Materials 10 (23): 2102654. https://doi.org/10.1002/adom.202102654.

Kim, Seung-Jun, et al. “Orthogonal Molecular Assembly : Eliminating Intrinsic Phonon Modes in Organic THz Generators.” Advanced Optical Materials, vol. 10, no. 23, 2022, p. 2102654, https://doi.org/10.1002/adom.202102654.