TY - JOUR
T1 - Organic Kainate Single Crystals for Second-Harmonic and Broadband THz Generation
AU - Barhum, Hani
AU - McDonnell, Cormac
AU - Alon, Tmiron
AU - Hammad, Raheel
AU - Attrash, Mohammed
AU - Ellenbogen, Tal
AU - Ginzburg, Pavel
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/2/15
Y1 - 2023/2/15
N2 - Organic crystals with unique nonlinear optical properties have been attracting attention owing to their capability to outperform their conventional nonorganic counterparts. Since nonlinear material responses are linked to a crystal’s internal microscopic structure, molecular engineering of maximally unharmonic quantum potentials can boost macromolecular susceptibilities. Here, large-scale kainic acid (kainate) single crystals were synthesized, and their linear and nonlinear optical properties were studied in a broad spectral range, spanning the visible to THz spectral regions. The non-centrosymmetric zwitterionic crystallization, molecular structure, and intermolecular arrangement were found to act as additive donor-acceptor domains, enhancing the efficiency of the intrinsic second-order optical nonlinearity of this pure enantiomeric crystal. Molecular simulations and experimental analysis were performed to retrieve the crystals’ properties. The crystals were predicted and found to have good transparency in a broad spectral range from the UV to the infrared (0.2-20 μm). Second-harmonic generation was measured for ultrashort pumping wavelengths between 800 and 2400 nm, showing an enhanced response around 600 nm. Broadband THz generation was demonstrated with a detection limited bandwidth of >8 THz along with emission efficiencies comparable to and prevailing those of commercial ZnTe crystals. The broadband nonlinear response and high transparency make kainate crystals extremely attractive for realizing a range of nonlinear optical devices.
AB - Organic crystals with unique nonlinear optical properties have been attracting attention owing to their capability to outperform their conventional nonorganic counterparts. Since nonlinear material responses are linked to a crystal’s internal microscopic structure, molecular engineering of maximally unharmonic quantum potentials can boost macromolecular susceptibilities. Here, large-scale kainic acid (kainate) single crystals were synthesized, and their linear and nonlinear optical properties were studied in a broad spectral range, spanning the visible to THz spectral regions. The non-centrosymmetric zwitterionic crystallization, molecular structure, and intermolecular arrangement were found to act as additive donor-acceptor domains, enhancing the efficiency of the intrinsic second-order optical nonlinearity of this pure enantiomeric crystal. Molecular simulations and experimental analysis were performed to retrieve the crystals’ properties. The crystals were predicted and found to have good transparency in a broad spectral range from the UV to the infrared (0.2-20 μm). Second-harmonic generation was measured for ultrashort pumping wavelengths between 800 and 2400 nm, showing an enhanced response around 600 nm. Broadband THz generation was demonstrated with a detection limited bandwidth of >8 THz along with emission efficiencies comparable to and prevailing those of commercial ZnTe crystals. The broadband nonlinear response and high transparency make kainate crystals extremely attractive for realizing a range of nonlinear optical devices.
KW - THz
KW - hyperpolarizability
KW - nonlinear organic crystal
KW - second-harmonic generation
KW - zwitterionic crystal
UR - http://www.scopus.com/inward/record.url?scp=85147565481&partnerID=8YFLogxK
U2 - 10.1021/acsami.2c18454
DO - 10.1021/acsami.2c18454
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C2 - 36729720
AN - SCOPUS:85147565481
SN - 1944-8244
VL - 15
SP - 8590
EP - 8600
JO - ACS applied materials & interfaces
JF - ACS applied materials & interfaces
IS - 6
ER -