Theoretical Understanding of Nonlinear Optical Properties in Solids: A Perspective.

Nonlinear optical (NLO) crystals have become a hot topic in chemical science and material physics, due to their essential role in laser technology, optical information, optoelectronics, and precision measurements. In this Perspective, we provide an overview of recent advances in second-order nonlinear optics, with a focus on two critical topics: second harmonic generation (SHG) and the bulk photovoltaic effect (BPVE). For SHG, we discuss recent progress in deep-ultraviolet (DUV) materials, highlighting their structural characteristics and nonlinear groups that contribute to their exceptional performance. For BPVE, we concentrate on the emerging field of low-dimensional materials, emphasizing their potential in a shift current. Additionally, we discuss the development of regulation approaches for NLO materials, which is vital for their practical application. Finally, we address the outlook for the field, including the challenges that must be overcome to further advance NLO materials research.

Manipulation of nonlinear optical responses in layered ferroelectric niobium oxide dihalides.

Realization of highly tunable second-order nonlinear optical responses, e.g., second-harmonic generation and bulk photovoltaic effect, is critical for developing modern optical and optoelectronic devices. Recently, the van der Waals niobium oxide dihalides are discovered to exhibit unusually large second-harmonic generation. However, the physical origin and possible tunability of nonlinear optical responses in these materials remain to be unclear. In this article, we reveal that the large second-harmonic generation in NbOX2 (X = Cl, Br, and I) may be partially contributed by the large band nesting effect in different Brillouin zone. Interestingly, the NbOCl2 can exhibit dramatically different strain-dependent bulk photovoltaic effect under different polarized light, originating from the light-polarization-dependent orbital transitions. Importantly, we achieve a reversible ferroelectric-to-antiferroelectric phase transition in NbOCl2 and a reversible ferroelectric-to-paraelectric phase transition in NbOI2 under a certain region of external pressure, accompanied by the greatly tunable nonlinear optical responses but with different microscopic mechanisms. Our study establishes the interesting external-field tunability of NbOX2 for nonlinear optical device applications.