Optical and Defect Properties of Mid-IR Laser Crystal Dy3+: PbGa2S4: a DFT and XPS Study

Abstract

Dy3+: PbGa2S4 crystal with low phonon energy has been used to achieve direct lasing of 4.3-4.7μm lasers. High quality PbGa2S4 crystal is difficult to be fabricated due to the component volatilization. In this work, the influence of component condition on the intrinsic defects and optical absorption in Dy3+: PbGa2S4 crystal were investigated through first-principles calculations and crystal growth experiments. We found that PbGa2S4 was prone to decompose out Ga2S3 at its growth temperature, usually resulting in a PbS-rich (Ga2S3-deficient) growth condition. The calculated results of defect formation energy indicate that the PbGa and VGa defects play a dominant role in PbGa2S4 under the PbS-rich growth condition. The Ga2S3-rich growth condition can increase the defect formation energy and may lower the defect density. Our post-growth annealing and crystal growth experiments proved that the Ga2S3-rich condition did improve the optical quality of Dy3+: PbGa2S4 crystal. The structure and composition of PGS were analyzed by the XRD and EDS. The XRC result showed the crystal has a high crystalline quality.The changes of bond length were studied through the XPS characterizations and DFT calculated results. The VGa and PbGa defects result in the different XPS peaks of PbGa2S4 crystals fabricated under PbS-rich and Ga2S3-rich growth conditions.

Article information

Article type
Paper
Submitted
07 Apr 2022
Accepted
23 May 2022
First published
25 May 2022

CrystEngComm, 2022, Accepted Manuscript

Optical and Defect Properties of Mid-IR Laser Crystal Dy3+: PbGa2S4: a DFT and XPS Study

X. Yu, Ch. B. Huang, Y. Ni, Z. Wang and H. Wu, CrystEngComm, 2022, Accepted Manuscript , DOI: 10.1039/D2CE00486K

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