Quo Vadis Nonlinear Optics? An Alternative and Simple Approach to Third Rank Tensors in Semiconductors

It is well understood that nonlinear optical (NLO) phenomena are deeply related to the material’s symmetry. Mathematically, the material symmetry can be described in terms of the nonzero parameters in the nonlinear susceptibility tensors. Generally, more complex structures involve more nonzero parameters in the tensor. The number of parameters increases rapidly if higher NLO orders are considered, complicating the physical analysis. Conventionally, these parameters are obtained via abstract symmetry analysis, e.g., group theory (GT). This work presents a novel theoretical analysis to approach the nonlinear tensor using the simplified bond hyperpolarizability model (SBHM) and compare it with GT. Our analysis is based on a light–matter interaction classical phenomenological physical framework. Rather than just looking at the symmetry of the crystal, the model applies physical considerations requiring fewer independent parameters in the tensor than GT. Such a simplification significantly improves the determination of the surface–bulk SHG contribution factors, which cannot be extracted from the experiment alone. We also show for the case of perovskite that the SHG contribution can be addressed solely from their surface dipoles with only one independent component in the tensor. Therefore, this work may open the path for a similar analysis in other complicated semiconductor surfaces and structures in the future, with potential applications to nanoscale surface characterization and real-time surface deposition monitoring.

Nonlinear optical single crystals for terahertz generation and detection

Nonlinear optical (NLO) single crystals with high quality are the pillars for the development of new devices that fulfil the demands of society. Nowadays, NLO single crystals are very attractive for the photonic applications particularly for terahertz (THz) photonics. The reason for their popularity is that these crystals can produce very powerful and ultra wideband THz waves due to their high nonlinear susceptibility. In this review paper, we deal with the challenges and progresses in the evolution of NLO single crystals for THz wave generation and detection. Here, we review the single crystal growth that how and by which method single crystal is grown. We summarize the structures, intermolecular and intramolecular interactions, their properties and how they generate and detect the THz waves. Widely used single crystals at present are DAST, BNA, OH1, amino acid-based single crystals, etc.

A monoclinic semiorganic molecular crystal GUHP for terahertz photonics and optoelectronics

In this paper we describe the properties of the crystal of guanylurea hydrogen phosphate (NH$$_2$$ 2 )$$_2$$ 2 CNHCO(NH$$_2$$ 2 )H$$_2$$ 2 PO$$_3$$ 3 (GUHP) and propose its application in terahertz photonics and optoelectronics. GUHP crystal has a wide window of transparency and a high optical threshold in the visible and NIR spectral regions and narrow absorption bands in the terahertz frequency range. The spectral characteristics of absorption and refraction in the THz range were found to be strongly dependent on crystal temperature and orientation. Computer simulations made it possible to link the nature of the resonant response of the medium at THz frequencies with the molecular structure of the crystal, in particular, with intermolecular hydrogen bonds and the layered structure of the lattice. The possibility of application of the crystal under study for the conversion of femtosecond laser radiation from visible an NIR to terahertz range was demonstrated. It was shown that dispersion properties of the crystal allow the generation of narrow band terahertz radiation, whose spectral properties are determined by conditions close to phase matching. The properties of the generated terahertz radiation under various temperatures suggest the possibility of phonon mechanism of enhancement for nonlinear susceptibility of the second order.

Label-free imaging of collagen fibers in tissue slices using phase imaging with computational specificity

Evaluating the tissue collagen content in addition to the epithelial morphology has been proven to offer complementary information in histopathology, especially in disease stratification and patient survivability prediction. One imaging modality widely used for this purpose is second harmonic generation microscopy (SHGM), which reports on the nonlinear susceptibility associated with the collagen fibers. Another method is polarization light microscopy (PLM) combined with picrosirius-red (PSR) tissue staining. However, SHGM requires expensive equipment and provides limited throughput, while PLM and PSR staining are not part of the routine pathology workflow. Here, we advance phase imaging with computational specificity (PICS) to computationally infer the collagen distribution of unlabeled tissue, with high specificity. PICS utilizes deep learning to translate quantitative phase images (QPI) into corresponding PSR images with high accuracy and speed. Our results indicate that the distributions of collagen fiber orientation, length, and straightness reported by PICS closely match the ones from ground truth.

The Photochemistry of Organic Materials for Photonic Devices

<p>Optically active organic chromophores have attracted much interest in recent years for their potential for use in photonic devices. Chromophores such as compound (1) have been found to have a very high second order nonlinear susceptibility ( β ) value of 650 × 10⁻³⁰esu in dimethyl formamide.¹ The performance of 1 in a polymer film is much lower than this due to the formation of aggregates which hinder the poling process necessary to ensure a noncentrosymmetric arrangement of the molecules in order to display second order nonlinear behaviour. The molecular aggregation behaviour of a set of second order nonlinear compounds based on compound 1 have been studied in this thesis. These compounds share the backbone shown in figure 1 with pendant groups added to the R₁ R₂ and R₃ positions, with the aim of finding substituent groups that can be added to the optically active merocyanine backbone that reduce the aggregation and increase the solubility of the compounds. This in turn will make them more suitable for use in photonics devices. It was found that a C₁₁H₂₃ alkyl chain added to the R₃ position made the largest contribution to decreasing aggregation. Bulky groups on the R₁ and R₂ positions also reduced aggregation. As a result compounds 5 and 8, with R₃ = C₁₁H₂₃ and bulky groups attached displayed the least aggregation of the compounds studied. ¹ See Figure 1 (pg. i): Merocyanine backbone with substituent positions marked.</p>

The Photochemistry of Organic Materials for Photonic Devices

<p>Optically active organic chromophores have attracted much interest in recent years for their potential for use in photonic devices. Chromophores such as compound (1) have been found to have a very high second order nonlinear susceptibility ( β ) value of 650 × 10⁻³⁰esu in dimethyl formamide.¹ The performance of 1 in a polymer film is much lower than this due to the formation of aggregates which hinder the poling process necessary to ensure a noncentrosymmetric arrangement of the molecules in order to display second order nonlinear behaviour. The molecular aggregation behaviour of a set of second order nonlinear compounds based on compound 1 have been studied in this thesis. These compounds share the backbone shown in figure 1 with pendant groups added to the R₁ R₂ and R₃ positions, with the aim of finding substituent groups that can be added to the optically active merocyanine backbone that reduce the aggregation and increase the solubility of the compounds. This in turn will make them more suitable for use in photonics devices. It was found that a C₁₁H₂₃ alkyl chain added to the R₃ position made the largest contribution to decreasing aggregation. Bulky groups on the R₁ and R₂ positions also reduced aggregation. As a result compounds 5 and 8, with R₃ = C₁₁H₂₃ and bulky groups attached displayed the least aggregation of the compounds studied. ¹ See Figure 1 (pg. i): Merocyanine backbone with substituent positions marked.</p>

Anisotropic optical responses of layered thallium arsenic sulfosalt gillulyite

Multi-element two-dimensional (2D) materials hold great promise in the context of tailoring the physical and chemical properties of the materials via stoichiometric engineering. However, the rational and controllable synthesis of complex 2D materials remains a challenge. Herein, we demonstrate the preparation of large-area thin quaternary 2D material flakes via mechanical exfoliation from a naturally occurring bulk crystal named gillulyite. Furthermore, the anisotropic linear and nonlinear optical properties including anisotropic Raman scattering, linear dichroism, and anisotropic third-harmonic generation (THG) of the exfoliated gillulyite flakes are investigated. The observed highly anisotropic optical properties originate from the reduced in-plane crystal symmetry. Additionally, the third-order nonlinear susceptibility of gillulyite crystal is retrieved from the measured thickness-dependent THG emission. We anticipate that the demonstrated strong anisotropic linear and nonlinear optical responses of gillulyite crystal will facilitate the better understanding of light-matter interaction in quaternary 2D materials and its implications in technological innovations such as photodetectors, frequency modulators, nonlinear optical signal processors, and solar cell applications.

Polarization-dependent optical responses in natural 2D layered mineral teallite

Multi-element layered materials enable the use of stoichiometric variation to engineer their optical responses at subwavelength scale. In this regard, naturally occurring van der Waals minerals allow us to harness a wide range of chemical compositions, crystal structures and lattice symmetries for layered materials under atomically thin limit. Recently, one type of naturally occurring sulfide mineral, ternary teallite has attained significant interest in the context of thermoelectric, optoelectronic, and photovoltaic applications, but understanding of light-matter interactions in such ternary teallite crystals is scarcely available. Herein, polarization-dependent linear and nonlinear optical responses in mechanically exfoliated teallite crystals are investigated including anisotropic Raman modes, wavelength-dependent linear dichroism, optical band gap evolution, and anisotropic third-harmonic generation (THG). Furthermore, the third-order nonlinear susceptibility of teallite crystal is estimated using the thickness-dependent THG emission process. We anticipate that our findings will open the avenue to a better understanding of the tailored light-matter interactions in complex multi-element layered materials and their implications in optical sensors, frequency modulators, integrated photonic circuits, and other nonlinear signal processing applications.