Publication Date

7-5-2019

Department

Ames Laboratory; Chemistry

Campus Units

Chemistry, Ames Laboratory

OSTI ID+

1556110

Report Number

IS-J 9971

DOI

10.1021/jacs.9b04653

Journal Title

Journal of the American Chemical Society

Volume Number

141

Issue Number

30

First Page

11976

Last Page

11983

Abstract

A novel barium silicon phosphide was synthesized and characterized. Ba2Si3P6 crystallizes in the noncentrosymmetric space group Pna21 (No. 33) and exhibits a unique bonding connectivity in the Si–P polyanion not found in other compounds. The crystal structure is composed of SiP4 tetrahedra connected into one-dimensional double-tetrahedra chains through corner sharing, edge sharing, and covalent P–P bonds. Chains are surrounded by Ba cations to achieve an electron balance. The novel compound exhibits semiconducting properties with a calculated bandgap of 1.6 eV and experimental optical bandgap of 1.88 eV. The complex pseudo-one-dimensional structure manifests itself in the transport and optical properties of Ba2Si3P6, demonstrating ultralow thermal conductivity (0.56 W m–1 K–1 at 300 K), promising second harmonic generation signal (0.9 × AgGaS2), as well as high laser damage threshold (1.6 × AgGaS2, 48.5 MW/cm2) when compared to the benchmark material AgGaS2. Differential scanning calorimetry reveals that Ba2Si3P6 melts congruently at 1373 K, suggesting that large single crystal growth may be possible.

DOE Contract Number(s)

AC02-07CH11358

Language

en

Publisher

Iowa State University Digital Repository, Ames IA (United States)

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