Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package

Abstract Optical second harmonic generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. Closed-form analytical solution of the nonlinear optical responses is essential for evaluating materials whose optical properties are unknown a...

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Main Authors: Rui Zu, Bo Wang, Jingyang He, Lincoln Weber, Akash Saha, Long-Qing Chen, Venkatraman Gopalan
Format: Article
Language:English
Published: Nature Portfolio 2024-03-01
Series:npj Computational Materials
Online Access:https://doi.org/10.1038/s41524-024-01229-2
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author Rui Zu
Bo Wang
Jingyang He
Lincoln Weber
Akash Saha
Long-Qing Chen
Venkatraman Gopalan
author_facet Rui Zu
Bo Wang
Jingyang He
Lincoln Weber
Akash Saha
Long-Qing Chen
Venkatraman Gopalan
author_sort Rui Zu
collection DOAJ
description Abstract Optical second harmonic generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. Closed-form analytical solution of the nonlinear optical responses is essential for evaluating materials whose optical properties are unknown a priori. A recent open-source code, ♯SHAARP.si, can provide such closed form solutions for crystals with arbitrary symmetries, orientations, and anisotropic properties at a single interface. However, optical components are often in the form of slabs, thin films on substrates, and multilayer heterostructures with multiple reflections of both the fundamental and up to ten different SHG waves at each interface, adding significant complexity. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry in Multilayers (♯SHAARP.ml). The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes using standard and commonly used nonlinear optical materials as well as twisted 2-dimensional heterostructures.
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spelling doaj.art-7d95919fc34c4d4c8779a4e24673b4592024-03-31T11:26:43ZengNature Portfolionpj Computational Materials2057-39602024-03-0110111510.1038/s41524-024-01229-2Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml packageRui Zu0Bo Wang1Jingyang He2Lincoln Weber3Akash Saha4Long-Qing Chen5Venkatraman Gopalan6Department of Materials Science and Engineering, The Pennsylvania State UniversityDepartment of Materials Science and Engineering, The Pennsylvania State UniversityDepartment of Materials Science and Engineering, The Pennsylvania State UniversityDepartment of Materials Science and Engineering, The Pennsylvania State UniversityDepartment of Materials Science and Engineering, The Pennsylvania State UniversityDepartment of Materials Science and Engineering, The Pennsylvania State UniversityDepartment of Materials Science and Engineering, The Pennsylvania State UniversityAbstract Optical second harmonic generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. Closed-form analytical solution of the nonlinear optical responses is essential for evaluating materials whose optical properties are unknown a priori. A recent open-source code, ♯SHAARP.si, can provide such closed form solutions for crystals with arbitrary symmetries, orientations, and anisotropic properties at a single interface. However, optical components are often in the form of slabs, thin films on substrates, and multilayer heterostructures with multiple reflections of both the fundamental and up to ten different SHG waves at each interface, adding significant complexity. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry in Multilayers (♯SHAARP.ml). The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes using standard and commonly used nonlinear optical materials as well as twisted 2-dimensional heterostructures.https://doi.org/10.1038/s41524-024-01229-2
spellingShingle Rui Zu
Bo Wang
Jingyang He
Lincoln Weber
Akash Saha
Long-Qing Chen
Venkatraman Gopalan
Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package
npj Computational Materials
title Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package
title_full Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package
title_fullStr Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package
title_full_unstemmed Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package
title_short Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package
title_sort optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯shaarp ml package
url https://doi.org/10.1038/s41524-024-01229-2
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