期刊
CHEMISTRY OF MATERIALS
卷 34, 期 11, 页码 5283-5293出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.2c00962
关键词
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资金
- Air Force Office of Scientific Research [FA9550-18-S-0003]
- Soft and Hybrid Nano-technology Experimental (SHyNE) Resource [NSF ECCS-2025633]
- Northwestern University
- National Science Foundation (NSF) [DMR-2011208]
- National Research Foundation of Korea (NRF) - Korean government [2020R1F1A1069646, 2021R1A2C2013625]
- National Research Foundation of Korea [2021R1A2C2013625, 2020R1F1A1069646] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
Noncentrosymmetric chalcogenides containing stereochemically active lone pair elements can tune the band gap and enhance the second harmonic generation (SHG) response. These compounds with a three-dimensional structure show significantly improved SHG behavior and are attractive for commercial applications.
Noncentrosymmetric chalcogenides containing stereochemically active lone pair elements, such as As, Sb, and Bi, offer a useful way to tune the band gap and enhance the second harmonic generation (SHG) response. Ba(2)As(2-x)Sb(x)Q(5), Ba(2)As(2-x)Bi(x)Q(5) (Q = S and Se), and Ba2As2S4.8Se0.2 are new chalcoarsenates that crystallize in the noncentrosymmetric monoclinic space group P2(1). These five new compounds crystallized with a three-dimensional (3D) Ba2As2Se5-type structure, containing AsQ(3) units and [As(2)Q(4)](2-) dimeric units. The [As(2)Q(4)](2-) dimeric unit can be tuned by replacing As with Sb or Bi and Se with S. In contrast Ba2As2S5 crystallizes in the orthorhombic space group Pca2(1). Differential thermal analysis suggested that Ba2As2S5, Ba2As2Se5, Ba2AsSbSe5, and Ba2As1.25Bi0.75Se5 melt congruently. The [M(2)Q(4)](2-) unit plays a significant role in tuning the band gap of these compounds, decreasing from 2.02 eV in Ba2As2S5 to 1.37 eV in Ba2As1.25Bi0.75Se5. Powder SHG measurements showed all the compounds are essentially phase-matchable at 3300 nm. Ba2AsSbSe5 exhibits the highest chi((2)) of 36 pm/V and a laser-induced damage threshold of 0.10 GW/cm(2), comparable to that of AgGaQ(2). These materials show significantly improved SHG behavior response to BaGa(4)Q(7) compounds, making them attractive for commercial applications.
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