A Lead Mixed Halide with Three Different Coordinated Anions and Strong Second‐Harmonic Generation Response. Issue 4 (5th November 2021)

• Record Type: Journal Article
• Authors: Shui, Qi‐Rui; Fu, Rui‐Biao; Zhou, Zi‐Qi; Ma, Zu‐Ju; Tang, Hong‐Xin; Wu, Xin‐Tao
• Is Part Of: Chemistry. Volume 28:Issue 4(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-11-05
• Subjects: mixed halides -- non-centrosymmetric -- nonlinear optical crystals -- precise synthesis -- second harmonic generation; Chemistry -- Periodicals; 540
• DOI: 10.1002/chem.202103687
• Languages: English
• ISSNs: 0947-6539

Abstract

Abstract: Nonlinear optical (NLO) crystals are widely applied in information technology, micro‐manufacturing and medical treatment. Herein, a new lead mixed halide with strong second‐harmonic generation (SHG) response, Cs3 Pb2 (CH3 COO)2 Br3 I2, has been designed and rationally synthesized. Cs3 Pb2 (CH3 COO)2 Br3 I2 represents the rare NLO crystal featuring that three different anions (I −, Br − and O 2− ) simultaneously coordinate the Pb(II) atom to form a severely distorted [PbBr2 I2 O2 ] polyhedron with a large polarizability. Remarkably, Cs3 Pb2 (CH3 COO)2 Br3 I2 not only exhibits a very strong phase‐matching SHG response of 9×KH2 PO4 (KDP), but also possesses a large birefringence (0.27@1064 nm) and high laser damage threshold (LDT). The strong SHG effect of Cs3 Pb2 (CH3 COO)2 Br3 I2 mainly originates from the oriented arrangement of [Pb2 Br3 I2 ] chains. This study points out an effective strategy to develop new NLO crystals with strong SHG response. Abstract : A new lead mixed halide, Cs3 Pb2 (CH3 COO)2 Br3 I2, has been designed and rationally synthesized. Cs3 Pb2 (CH3 COO)2 Br3 I2 featuring that three different anions (I −, Br − and O 2− ) simultaneously coordinate the Pb(II) atom into a severely distorted [PbBr2 I2 O2 ] polyhedron, exhibits a very strong phase‐matching second‐harmonic generation (SHG) response of 9×KH2 PO4 (KDP) and a large birefringence (0.27@1064 nm). Systematic theoretical calculations demonstrate that the strong SHG effect of Cs3 Pb2 (CH3 COO)2 Br3 I2 mainly originates from the oriented arrangement of [Pb2 Br3 I2 ] chains.