Computationally-driven discovery of second harmonic generation in EuBa 3 (B 3 O 6 ) 3 through inversion symmetry breaking

He, Jingyang; Alaerts, Louis; Wang, Yu; Trinquet, Victor; Yoshida, Suguru; Yennawar, Hemant; Sanni, Victor; Claes, Romain; Katzbaer, Rowan; Krysko, Evan; Sarker, Saugata; Schaak, Raymond E.; Rignanese, Gian-Marco; Hautier, Geoffroy; Mao, Zhiqiang; Gopalan, Venkatraman

doi:10.1364/OME.497727

Computationally-driven discovery of second harmonic generation in EuBa ₃ (B ₃ O ₆ ) ₃ through inversion symmetry breaking

Journal Article · Mon Nov 06 00:00:00 EST 2023 · Optical Materials Express

DOI:https://doi.org/10.1364/OME.497727· OSTI ID:2204805

; ; Wang, Yu; Trinquet, Victor; ; Yennawar, Hemant; Sanni, Victor; Claes, Romain; Katzbaer, Rowan; Krysko, Evan; ; Schaak, Raymond E.; Rignanese, Gian-Marco; Hautier, Geoffroy; Mao, Zhiqiang;

Nonlinear optical (NLO) crystals with superior properties are significant for advancing laser technologies and applications. Introducing rare earth metals to borates is a promising and effective way to modify the electronic structure of a crystal to improve its optical properties in the visible and ultraviolet range. In this work, we computationally discover inversion symmetry breaking in EuBa ₃ (B ₃ O ₆ ) ₃ , which was previously identified as centric, and demonstrate noncentrosymmetry via synthesizing single crystals for the first time by the floating zone method. We determine the correct space group to be P 6¯. The material has a large direct bandgap of 5.56 eV and is transparent down to 250 nm. The complete anisotropic linear and nonlinear optical properties were also investigated with a d ₁₁ of ∼0.52 pm/V for optical second harmonic generation. Further, it is Type I and Type II phase matchable. This work suggests that rare earth metal borates are an excellent crystal family for exploring future deep ultraviolet (DUV) NLO crystals. It also highlights how first principles computations combined with experiments can be used to identify noncentrosymmetric materials that have been wrongly assigned to be centrosymmetric.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2204805

Alternate ID(s):: OSTI ID: 2582875

Journal Information:: Optical Materials Express, Journal Name: Optical Materials Express Journal Issue: 12 Vol. 13; ISSN 2159-3930

Publisher:: Optical Society of AmericaCopyright Statement

Country of Publication:: United States

Language:: English

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