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The nonlinear susceptibility in the terahertz region is expected to have a non-negligible imaginary part originating from the momentum-dependent scattering time of free carriers, but it has been scarcely reported. By utilizing an intense 4 THz beam from a terahertz free electron laser, we investigated the azimuth angle dependence of the third harmonic generation (THG) from semiconductors. The observed angular anisotropy of THG revealed the contribution of the imaginary part of the nonlinear susceptibility originating from the momentum-scattering time relation in addition to its real part originating from the band nonparabolicity. The results provide a deeper understanding of nonlinear optics in the terahertz region.
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http://dx.doi.org/10.1364/OL.532646 | DOI Listing |
J Phys Chem Lett
September 2025
Hunan Key Laboratory of Nanophotonics and Devices, School of Physics, Central South University, Changsha 410083, People's Republic of China.
NbOCl has garnered interest owing to its second-order nonlinear optical properties, but the influence of thickness on its third-harmonic generation (THG) and excited-state dynamics has not been fully investigated. Here, mechanically exfoliated NbOCl flakes were found to produce THG and second-harmonic generation (SHG), simultaneously, and to show a nonmonotonic dependence on sample thickness. The increase in thickness leads to a decrease in the bandgap.
View Article and Find Full Text PDFJ Phys Chem B
September 2025
CNRS, Bordeaux INP, ISM, UMR 5255, University of Bordeaux, F-33405 Cedex Talence, France.
A computational protocol is developed to evaluate the second- and third-order nonlinear optical (NLO) properties of donor-acceptor benzene derivatives, incorporating ab initio electron correlation, frequency dispersion, and solvent effects, with the aim of achieving high predictive accuracy. The computational scheme encompasses (i) high-level CCSD(T) calculations of the static first (β) and second (γ) hyperpolarizabilities, (ii) the assessment of the performance of the CAM-B3LYP and M06-2X exchange-correlation DFT functionals to evaluate β and γ values, (iii) the use, after assessment of its effectiveness, of the multiplicative scheme to evaluate second harmonic generation responses, (iv) the evaluation of the frequency dispersion factors on β and γ by using Bishop's frequency-dispersion polynomials, and their use, in combination with the multiplicative correction scheme, to evaluate third harmonic generation second hyperpolarizabilities. This hybrid approach is shown to closely reproduce the experimental trends, although systematic quantitative deviations still remain with respect to experimental values.
View Article and Find Full Text PDFYing Yong Sheng Tai Xue Bao
August 2025
Guangdong Eco-Engineering Polytechnic, Guangzhou 510520, China.
, a monotypic relict tree species endemic to China, has extremely sparse populations in the wild. The world's largest natural forest is distributed in the Zhuzhou Island Forest Nature Reserve, Zhuhai, Guangdong Province. However, artificial plantations of currently exhibit significant decline.
View Article and Find Full Text PDFWe achieve merging mirror-coupled bound states in the continuum (BICs) at THz frequency in the metasurface consisting of Si block arrays on an Au mirror with SiO as a spacer. Compared with the conventional mirror-coupled BIC, the merging BIC exhibits a higher Q-factor and local field enhancement at the same in-plane wavevector . Further, merging mirror-coupled BICs can combine the advantage of mirror-coupled BICs without breaking the symmetry of the nanostructure and the superiority of merging BICs, which is robust to imperfections of the nanostructure.
View Article and Find Full Text PDFClin Transl Allergy
August 2025
Division of Respirology, Department of Medicine, Faculty of Health Sciences, McMaster University, Hamilton, Ontario, Canada.