Polar enhancement of optical nonlinearities and domain-driven second harmonic contrast in bismuth telluro-halide van der Waals crystals

Fuente: arXiv
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Hauptverfasser: Kwock, Kevin W. C., Norden, Tenzin, Darlington, Thomas P., Yao, Kaiyuan, Du, Kai, Nedić, Ana-Marija, Trevisan, Thaís V., Dolgopolova, Ekaterina, Orth, Peter P., Prasankumar, Rohit P., Schuck, P. James, Cheong, Sang-Wook, Kort-Kamp, Wilton J. M., Padmanabhan, Prashant
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Veröffentlicht: 2026
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author Kwock, Kevin W. C.
Norden, Tenzin
Darlington, Thomas P.
Yao, Kaiyuan
Du, Kai
Nedić, Ana-Marija
Trevisan, Thaís V.
Dolgopolova, Ekaterina
Orth, Peter P.
Prasankumar, Rohit P.
Schuck, P. James
Cheong, Sang-Wook
Kort-Kamp, Wilton J. M.
Padmanabhan, Prashant
author_facet Kwock, Kevin W. C.
Norden, Tenzin
Darlington, Thomas P.
Yao, Kaiyuan
Du, Kai
Nedić, Ana-Marija
Trevisan, Thaís V.
Dolgopolova, Ekaterina
Orth, Peter P.
Prasankumar, Rohit P.
Schuck, P. James
Cheong, Sang-Wook
Kort-Kamp, Wilton J. M.
Padmanabhan, Prashant
contents The BiTeX family of polar van der Waals (vdW) semiconductors offers a unique platform for exploring the interplay between polar crystalline structure and nonlinear optical phenomena. Here, we utilize second harmonic generation (SHG) polarimetry to demonstrate giant anisotropic optical nonlinearities in BiTeBr and BiTeI driven by contributions to the crystals' nonlinear polarizability originating from their permanent dipole moment. In addition, using SHG microscopy, we show that BiTeI displays a distinctive SHG spatial texture consisting of thread-like regions of reduced harmonic intensity. These features demark the boundaries between phase and anti-phase polar domains, confirmed via piezoresponse force microscopy and are attributable to disorder-driven restoration of inversion symmetry and concomitant optical interference effects. Our results unveil the power of polarization-resolved SHG microscopy in elucidating the intricate relationship between structure, symmetry, and nonlinear optical responses in polar vdW materials and highlight the promise of BiTeX as a material platform for domain-engineered nanoscale nonlinear photonics.
format Preprint
id arxiv_https___arxiv_org_abs_2601_00195
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Polar enhancement of optical nonlinearities and domain-driven second harmonic contrast in bismuth telluro-halide van der Waals crystals
Kwock, Kevin W. C.
Norden, Tenzin
Darlington, Thomas P.
Yao, Kaiyuan
Du, Kai
Nedić, Ana-Marija
Trevisan, Thaís V.
Dolgopolova, Ekaterina
Orth, Peter P.
Prasankumar, Rohit P.
Schuck, P. James
Cheong, Sang-Wook
Kort-Kamp, Wilton J. M.
Padmanabhan, Prashant
Optics
Mesoscale and Nanoscale Physics
The BiTeX family of polar van der Waals (vdW) semiconductors offers a unique platform for exploring the interplay between polar crystalline structure and nonlinear optical phenomena. Here, we utilize second harmonic generation (SHG) polarimetry to demonstrate giant anisotropic optical nonlinearities in BiTeBr and BiTeI driven by contributions to the crystals' nonlinear polarizability originating from their permanent dipole moment. In addition, using SHG microscopy, we show that BiTeI displays a distinctive SHG spatial texture consisting of thread-like regions of reduced harmonic intensity. These features demark the boundaries between phase and anti-phase polar domains, confirmed via piezoresponse force microscopy and are attributable to disorder-driven restoration of inversion symmetry and concomitant optical interference effects. Our results unveil the power of polarization-resolved SHG microscopy in elucidating the intricate relationship between structure, symmetry, and nonlinear optical responses in polar vdW materials and highlight the promise of BiTeX as a material platform for domain-engineered nanoscale nonlinear photonics.
title Polar enhancement of optical nonlinearities and domain-driven second harmonic contrast in bismuth telluro-halide van der Waals crystals
topic Optics
Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2601.00195