Computationally-driven discovery of second harmonic generation in EuBa3(B3O6)3 through inversion symmetry breaking

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

Research output: Contribution to journalArticlepeer-review


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 EuBa3(B3O6)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 P6̄. 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 d11 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.

Original languageEnglish (US)
Pages (from-to)3416-3427
Number of pages12
JournalOptical Materials Express
Issue number12
StatePublished - Dec 1 2023

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials

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