Benzothiazolium Single Crystals: A New Class of Nonlinear Optical Crystals with Efficient THz Wave Generation

Lee, Seung‐Heon; Lu, Jian; Lee, Seung‐Jun; Han, Jae-Hyun; Jeong, Chan-Uk; Lee, Seung‐Chul; Liang, Xian; Jazbinšek, Mojca; Yoon, Woojin; Yun, Hoseop; Kang, Bong Joo; Rotermund, Fabıan; Nelson, Keith A.; Kwon, O‐Pil

doi:10.1002/adma.201701748

Cited by 67 publications

(47 citation statements)

References 52 publications

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“…1(a). HMB-TMS crystals with large sizes that is essential for intense THz generation can be routinely grown by solution growth methods [28]. A photograph of a cleaved HMB-TMS crystal is shown in Fig.…”

Section: Phase Matching Condition For Thz Generationmentioning

confidence: 99%

“…In general, the polar axis of nonlinear optical crystals is defined as the average direction of the maximal first-order hyperpolarizability β max of the nonlinear optical molecules [23]. The polar axis of HMB-TMS crystals is defined as the average direction of the maximal first-order hyperpolarizability β max of HMB (2-(4-hydroxy-3-methoxystyryl)-3-methylbenzo[d]thiazol-3-ium) molecular cations [28]. HMB-TMS crystals have a large diagonal component of the macroscopic second-order nonlinear optical response…”

Section: Phase Matching Condition For Thz Generationmentioning

confidence: 99%

“…111 ≥ 162 × 10 −30 esu or 679 × 10 −40 m 4 /V) [28], which is very promising for highly efficient THz generation with pump light polarized along the crystal polar axis.…”

Section: (β Effmentioning

confidence: 99%

“…These achievements have stimulated considerable efforts in the development of new organic crystals by chemical modifications for intense THz generation [27]. Recently, we have reported a new class of organic crystals based on a benzothiazolium electronacceptor which proves stronger nonlinearity than the two classes of benchmark organic crystals based on either pyridinium (e.g., DAST and DSTMS) or quinolinium (e.g., HMQ-TMS) [28]. When pumped by laser pulses at 800 nm, the newly developed HMB-TMS (2-(4-hydroxy-3methoxystyryl)-3-methylbenzo[d]thiazol-3-ium 2,4,6-trimethylbenzenesulfonate) crystals with a small clear aperture (2 mm) are capable of generating THz pulses that have an order of magnitude higher field strength (up to 100 kV/cm) and broader bandwidth (up to 5.3 THz) than the inorganic ZnTe crystals under the same condition [28].…”

Section: Introductionmentioning

confidence: 99%

“…Recently, we have reported a new class of organic crystals based on a benzothiazolium electronacceptor which proves stronger nonlinearity than the two classes of benchmark organic crystals based on either pyridinium (e.g., DAST and DSTMS) or quinolinium (e.g., HMQ-TMS) [28]. When pumped by laser pulses at 800 nm, the newly developed HMB-TMS (2-(4-hydroxy-3methoxystyryl)-3-methylbenzo[d]thiazol-3-ium 2,4,6-trimethylbenzenesulfonate) crystals with a small clear aperture (2 mm) are capable of generating THz pulses that have an order of magnitude higher field strength (up to 100 kV/cm) and broader bandwidth (up to 5.3 THz) than the inorganic ZnTe crystals under the same condition [28]. The THz generation efficiency of HMB-TMS crystals might be improved with better phase matching condition between optical and THz frequencies by controlling the pump frequencies and crystal thicknesses.…”

Section: Introductionmentioning

confidence: 99%

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Efficient terahertz generation in highly nonlinear organic crystal HMB-TMS

Lu¹,

Lee²,

Liang³

et al. 2018

Opt. Express

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We report on generation of strong and broadband terahertz (THz) pulses via collinearly phase-matched optical rectification of near-infrared femtosecond pulses in the organic nonlinear optical HMB-TMS (2-(4-hydroxy-3-methoxystyryl)-3-methylbenzo[d]thiazol-3-ium 2,4,6-trimethylbenzenesulfonate) single crystals which exhibit optimal molecular orientation and large macroscopic optical nonlinearity for efficient THz wave generation. Single-cycle THz pulses with a peak electric field strength of 0.66 MV/cm and a bandwidth from 0.1 to 5.4 THz are achieved from an HMB-TMS crystal with only a 2-mm clear aperture pumped by 1350 nm pulses at moderate fluences. The generated THz energy is about 1 µJ and the corresponding pump-to-THz energy conversion efficiency reaches 0.23%.

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Section: Phase Matching Condition For Thz Generationmentioning

confidence: 99%

Section: Phase Matching Condition For Thz Generationmentioning

confidence: 99%

“…111 ≥ 162 × 10 −30 esu or 679 × 10 −40 m 4 /V) [28], which is very promising for highly efficient THz generation with pump light polarized along the crystal polar axis.…”

Section: (β Effmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Efficient terahertz generation in highly nonlinear organic crystal HMB-TMS

Lu¹,

Lee²,

Liang³

et al. 2018

Opt. Express

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Designing Non‐Centrosymmetric Molecular Crystals: Optimal Packing May Be Just One Carbon Away

Valdivia‐Berroeta

Jackson

Kenney

et al. 2019

Adv Funct Materials

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Molecular nonlinear optical (NLO) crystals feature important advantages compared to inorganic counterparts, such as low dielectric constants, ultrafast response times, and large electro‐optic coefficients. Conjugated push–pull chromophores connecting electron‐donating with accepting groups are often employed in the design of these crystals. However, associated large molecular dipole moments induce antiparallel or centrosymmetric conformations in the solid‐state, which leads to NLO inactivity. The cation–anion hydrogen bond interactions of a hydroxy‐piperidino electron donor group are combined with increased van der Waals volume effects induced by an ethyl modification of the electron‐accepting moiety. This produces non‐centrosymmetric packing in the organic salt EHPSI‐4NBS ((E)‐1‐ethyl‐2‐(4‐(4‐(hydroxymethyl)piperidin‐1‐yl)styryl)‐3,3‐dimethyl‐3H‐indol‐1‐ium 4‐nitrobenzenesulfonate). Converting a methyl group into ethyl changes the packing symmetry in the molecular crystal to switch on NLO activity. This behavior is attributed to the increased size of the ethyl group, which pushes apart the van der Waals contacts of the cation that lead to centrosymmetric packing in the methyl derivative. To test the NLO properties of EHPSI‐4NBS, THz generation experiments are performed at 1200 nm pump wavelength. Spectral amplitude similar to DAST ((E)‐4‐(4‐(dimethylamino)styryl)‐1‐methylpyridin‐1‐ium tosylate) crystal is observed with generation profile from 0 to 3.8 THz.

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A New Class of Organic Crystals with Extremely Large Hyperpolarizability: Efficient THz Wave Generation with Wide Flat‐Spectral‐Band

Kim

et al. 2022

Adv Funct Materials

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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 β iii eff of 335 × 10 −30 esu. This is in sharp contrast to zero β iii eff 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.

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Benzothiazolium Single Crystals: A New Class of Nonlinear Optical Crystals with Efficient THz Wave Generation

Cited by 67 publications

References 52 publications

Efficient terahertz generation in highly nonlinear organic crystal HMB-TMS

Efficient terahertz generation in highly nonlinear organic crystal HMB-TMS

Designing Non‐Centrosymmetric Molecular Crystals: Optimal Packing May Be Just One Carbon Away

A New Class of Organic Crystals with Extremely Large Hyperpolarizability: Efficient THz Wave Generation with Wide Flat‐Spectral‐Band

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