Novel Quaternary TlGaSn2Se6 Single Crystal as Promising Material for Laser Operated Infrared Nonlinear Optical Modulators

Oleh Parasyuk,Oksana Tsisar,Oleg Khyzhun,Volodymyr Babizhetskyy,Artur Maciag,Lyudmyla Piskach,Michal Piasecki,Galyna Myronchuk,Jaroslaw Jedryka,Volodymyr Levytskyy,Iwan Kityk

doi:10.3390/cryst7110341

Oleh Parasyuk, Oksana Tsisar + Show 9 more

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https://doi.org/10.3390/cryst7110341

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Abstract

The studies of the laser operated third order nonlinear optical features of novel TlGaSn2Se6 crystal were done. The main efforts were devoted to a search of a possibility to apply these crystals as laser operated optoelectronic material. For this reason, the third harmonic generation of the Nd:YAG pulse laser 1064 nm as the fundamental beam with varied energy density of up to 200 J/m2 was studied. As a source of laser operated light, we have used the cw laser (532 nm), exciting the material above the energy gap. Additionally, the influence of middle-energy Ar+ ions on the XPS spectra of the TlInSn2Se6 surface has been explored. We have shown that the main contribution of the Se4p states is manifested in the upper part of the valence band of TlInSn2Se6 We have established that for the TlGaSn2Se6 crystal there exists a possibility of variation of the third harmonic generation efficiency using illumination by external continuous wave laser beam. The discovered effect makes it possible to utilize TlGaSn2Se6 crystal in advanced optoelectronic laser operated devices.

Highlights

Before the consideration of the TlGaSn2 Se6 compound, it is necessary to discuss the similar well studied ternary thallium gallium selenide TlGaSe2, which belongs to a known class of TlCIII XVI 2 ferroelectrics semiconductors with layered structure
It is well known that the improvement of the parameters of such kinds of compounds and their wider application can be attained by the modification with various dopants. This is best achieved by the systematic studies of phase diagrams based on these compounds. When such an approach was applied to the systems AgGaS2 –GeS2 and AgGaSe2 –GeSe2 [10,11,12,13,14,15] to improve non-linear optical parameters of the ternary compounds AgGaS2 and AgGaSe2, it resulted in the synthesis of quaternary chalcogenides AgGaGeS4 and Agx Gax Ge1–x Se2
We present the results of investigations of crystal structure for TlGaSn2 Se6 performed by the X-ray powder method, its electronic structure using X-ray spectroscopy methods, as well as its optical and non-linear optical properties

Summary

Introduction

Before the consideration of the TlGaSn2 Se6 compound, it is necessary to discuss the similar well studied ternary thallium gallium selenide TlGaSe2 , which belongs to a known class of TlCIII XVI 2 ferroelectrics semiconductors with layered structure. This is best achieved by the systematic studies of phase diagrams based on these compounds When such an approach was applied to the systems AgGaS2 –GeS2 and AgGaSe2 –GeSe2 [10,11,12,13,14,15] to improve non-linear optical parameters of the ternary compounds AgGaS2 and AgGaSe2 , it resulted in the synthesis of quaternary chalcogenides AgGaGeS4 and Agx Gax Ge1–x Se2. Like their ternary analog, they crystallize in the acentric structure, but they have wider transparency windows, higher laser damage threshold (which is important as they are intended for the operating range of the powerful CO- and CO2 -pulsed lasers), and a simpler crystal growth technique

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