Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 26, Pages 30853-30860Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c07442
Keywords
deep ultraviolet; nonlinear optical material; fluoroaluminoborate; second harmonic generation; birefringence
Funding
- National Natural Science Foundation of China [21975062]
- Hebei Province Outstanding Youth Fund [E2020201003]
- Science and Technology Project of Hebei Education Department [BJ2020020]
- Key Project of Hebei Natural Science Foundation [E2020201030]
- Advanced Talents Incubation Program of the Hebei University [521000981271]
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Deep-UV nonlinear optical (NLO) materials are crucial for demanding DUV laser applications, and the two synthesized fluoroaluminoborates exhibit NLO activity with short UV cutoff edges. Despite having the same fundamental structural units, their crystal structures and second harmonic generation (SHG) responses differ significantly due to the cation effect.
Deep-UV (DUV) nonlinear optical (NLO) materials are of vital importance to demanding DUV laser applications; however, those with a large NLO coefficient, wide band gap, and sufficient phase-matching ability are rare. In this work, by combining p-conjugated B3O6 groups and distort AlO3F tetrahedra, we successfully designed and synthesized two fluoroaluminoborates, RbAlB3O6F (RABF) and Cs0.5Rb0.5AlB3O6F (CRABF). In addition, the solid solution CsxRb1-xAlB3O6F (0.2 < x < 0.8) polycrystalline samples were obtained by the standard solid-state reaction. It was shown that all these compounds are NLO-active and possess short UV cutoff edges (<200 nm). Interestingly, although they have the same fundamental structural units, their crystal structures and second harmonic generation (SHG) responses are significantly different owing to the cation effect. Theoretical calculations reveal that both B3O6 and AlO3F groups contribute to the SHG responses. Remarkably, it also indicates that RABF exhibits a large birefringence (Delta n = 0.0946 at 1064 nm), which is capable of realizing deep-UV phase matching down to 174 nm. The exploration of fluoroaluminoborates provides a new perspective for searching excellent deep-UV NLO materials.
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