TY - JOUR
T1 - Toward Large Second-Harmonic Generation and Deep-UV Transparency in Strongly Electropositive Transition Metal Sulfates
AU - Wu, Chao
AU - Jiang, Chunbo
AU - Wei, Guangfeng
AU - Jiang, Xingxing
AU - Wang, Zujian
AU - Lin, Zheshuai
AU - Huang, Zhipeng
AU - Humphrey, Mark G.
AU - Zhang, Chi
N1 - © 2023 The Author(s)
PY - 2023
Y1 - 2023
N2 - The development of deep-ultraviolet (DUV)/solar-blind UV nonlinear optical (NLO) crystals simultaneously possessing wide UV transparency, strong second-harmonic generation (SHG) response, and suitable birefringence is a major challenge in advanced laser technology. We herein propose a “cation compensation” strategy for strong optical nonlinearity in inorganic solids that is exemplified by the introduction of strongly electropositive transition metals (TMs). Following this strategy, the first d0 TM UV-transparent NLO sulfates, MF2(SO4) (M = Zr (ZFSO), Hf (HFSO)), have been synthesized. Short UV cutoff edges of 206 nm and below 190 nm are observed for bulk ZFSO and HFSO crystals, respectively, together with the strongest powder SHG responses (3.2 × (ZFSO) and 2.5 × KDP (HFSO)) for solar-blind UV/DUV NLO sulfates, as well as suitable birefringence. This work provides a new and efficient approach to the development of urgently needed high-performance NLO materials for applications in the short-wavelength UV region.
AB - The development of deep-ultraviolet (DUV)/solar-blind UV nonlinear optical (NLO) crystals simultaneously possessing wide UV transparency, strong second-harmonic generation (SHG) response, and suitable birefringence is a major challenge in advanced laser technology. We herein propose a “cation compensation” strategy for strong optical nonlinearity in inorganic solids that is exemplified by the introduction of strongly electropositive transition metals (TMs). Following this strategy, the first d0 TM UV-transparent NLO sulfates, MF2(SO4) (M = Zr (ZFSO), Hf (HFSO)), have been synthesized. Short UV cutoff edges of 206 nm and below 190 nm are observed for bulk ZFSO and HFSO crystals, respectively, together with the strongest powder SHG responses (3.2 × (ZFSO) and 2.5 × KDP (HFSO)) for solar-blind UV/DUV NLO sulfates, as well as suitable birefringence. This work provides a new and efficient approach to the development of urgently needed high-performance NLO materials for applications in the short-wavelength UV region.
UR - http://www.scopus.com/inward/record.url?scp=85146355733&partnerID=8YFLogxK
U2 - 10.1021/jacs.2c11645
DO - 10.1021/jacs.2c11645
M3 - Article
SN - 0002-7863
VL - 145
SP - 3040
EP - 3046
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 5
ER -