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Due to their abundant use in all-solid-state lasers, nonlinear optical (NLO) crystals are needed for many applications across diverse fields such as medicine and communication. However, because of conflicting requirements, the design of…

Materials Science · Physics 2025-08-13 Victor Trinquet , Matthew L. Evans , Gian-Marco Rignanese

Second harmonic generation (SHG) microscopy is a valuable tool for optical microscopy. SHG microscopy is normally performed as a point scanning imaging method, which lacks phase information and is limited in spatial resolution by the…

Understanding the mechanisms and spatial correlations of crystallographic symmetry breaking in ferroelectric materials is essential to tuning their functional properties. While optical second harmonic generation (SHG) has long been utilized…

Materials Science · Physics 2022-08-10 Wei Li , Yunpeng Ma , Tianyi Feng , Sergei V. Kalinin , Jing-Feng Li , Qian Li

Coherent nonlinear optical micro-spectroscopy is a frequently used tool in modern material science, as it is sensitive to many different local observables, which comprise, among others, crystal symmetry and vibrational properties. The…

Optics · Physics 2023-04-12 Kai J. Spychala , Zeeshan H. Amber , Lukas M. Eng , Michael Rüsing

We develop a multipolar theory of second-harmonic generation (SHG) by dielectric nanoparticles made of noncentrosymmetric materials with bulk quadratic nonlinearity. We specifically analyze two regimes of optical excitation: illumination by…

We conduct a theoretical and numerical study on the second-harmonic (SH) optical response of a nano-structured metamaterial composed of a periodic array of inclusions. Both the inclusions and their surrounding matrix are made of…

Mesoscale and Nanoscale Physics · Physics 2019-03-13 Ulises R. Meza , Bernardo S. Mendoza , W. Luis Mochán

Second-order nonlinear optical materials enable frequency doubling of light (second-harmonic generation, SHG), which is essential for optoelectronic applications ranging from materials characterization to quantum technologies. However,…

Materials Science · Physics 2026-03-25 Aubrey G. J. Nyiri , Michael J. Waters , James M. Rondinelli

Noble metals with well-defined crystallographic orientation constitute an appealing class of materials for controlling light-matter interactions on the nanoscale. Nonlinear optical processes, being particularly sensitive to anisotropy, are…

The phasing problem of heterodyne-detected nonlinear spectroscopy states that the relative time delay between the exciting pulses and a local oscillator must be known with subcycle precision to separate absorptive and dispersive…

Second harmonic generation (SHG) spectroscopy ubiquitously enables the investigation of surface chemistry, interfacial chemistry as well as symmetry properties in solids. Polarization-resolved SHG spectroscopy in the visible to infrared…

A very efficient method for the calculation of the effective optical response of nano-structured composite systems allows the design of metamaterials tailored for specific optical polarization properties. We use our method to design 2D…

Optics · Physics 2019-09-24 Bernardo S. Mendoza , W. Luis Mochán

Nonlinear optics is essential for many recent photonic technologies. Here, we introduce a novel multi-scale approach to simulate the nonlinear optical response of molecular nanomaterials combining ab initio quantum-chemical and classical…

Second harmonic generation (SHG) is forbidden in centrosymmetric molecular materials. However, a signal is frequently observed from interfaces where the symmetry is broken. Whereas the effect can be phenomenologically accommodated, an ab…

Wavefront shaping has revolutionized imaging deep in scattering media, being able to spatially and temporally refocus light through or inside the medium. However, wavefront shaping is not compatible yet with polarization-resolved microscopy…

Optics · Physics 2018-11-26 Hilton B. de Aguiar , Sylvain Gigan , Sophie Brasselet

In the currently accepted models of the nonlinear optics, the nonlinear radiation was treated as the result of an infinitesimally thin polarization sheet layer, and a three layer model was generally employed. The direct consequence of this…

Chemical Physics · Physics 2016-08-29 De-sheng Zheng , Yuan Wang , An-an Liu , Hong-fei Wang

Optical second-harmonic generation (SHG) is a nonlinear parametric process that doubles the frequency of incoming light. Only allowed in non-centrosymmetric materials, it has been widely used in frequency modulation of lasers, surface…

Materials Science · Physics 2021-01-05 Wontaek Kim , Je Yhoung Ahn , Juseung Oh , Ji Hoon Shim , Sunmin Ryu

We use second and third harmonic generation microscopy to investigate the nonlinear optical response of GaAs nanocavities embedded in a gold film and compare them to bare GaAs nanocavities. Our results reveal that the surrounding metallic…

Optical second-harmonic generation (SHG) enables orientational polarimetry for crystallographic analysis and domain imaging of various materials. However, conventional intensity polarimetry, which neglects phase information, fails to…

The controlled assembly of twisted 2D structures requires precise determination of the crystal orientation of their component layers. In the established procedure, the second-harmonic generation (SHG) intensity of a noncentrosymmetric layer…

Using symmetry arguments we show how optical second harmonic generation (SHG) can be used to detect antiferromagnetism at surfaces and in thin films. Based on the group theoretical analysis of the nonlinear electric susceptibility we…

Condensed Matter · Physics 2007-05-23 A. Daehn , W. Huebner , K. H. Bennemann