2D Free-Standing GeS<sub>1-x</sub>Se<sub>x</sub> with Composition-Tunable Bandgap for Tailored Polarimetric Optoelectronics.

Zheng, Tao; Pan, Yuan; Yang, Mengmeng; Li, Zhongming; Zheng, Zhaoqiang; Li, Ling; Sun, Yiming; He, Yingbo et al. · Adv Mater · 2024

basic_science · Level V

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Abstract

Germanium-based monochalcogenides (i.e., GeS and GeSe) with desirable properties are promising candidates for the development of next-generation optoelectronic devices. However, they are still stuck with challenges, such as relatively fixed electronic band structure, unconfigurable optoelectronic characteristics, and difficulty in achieving free-standing growth. Herein, it is demonstrated that two-dimensional (2D) free-standing GeS<sub>1-x</sub>Se<sub>x</sub> (0 ≤ x ≤ 1) nanoplates can be grown by low-pressure rapid physical vapor deposition (LPRPVD), fulfilling a continuously composition-tunable optical bandgap and electronic band structure. By leveraging the synergistic effect of composition-dependent modulation and free-standing growth, GeS<sub>1-x</sub>Se<sub>x</sub>-based optoelectronic devices exhibit significantly configurable hole mobility from 6.22 × 10<sup>-4</sup> to 1.24 cm<sup>2</sup>V<sup>-1</sup>s⁻<sup>1</sup> and tunable responsivity from 8.6 to 311 A W<sup>-1</sup> (635 nm), as x varies from 0 to 1. Furthermore, the polarimetric sensitivity can be tailored from 4.3 (GeS<sub>0.29</sub>Se<sub>0.71</sub>) to 1.8 (GeSe) benefiting from alloy engineering. Finally, the tailored imaging capability is also demonstrated to show the application potential of GeS<sub>1-x</sub>Se<sub>x</sub> alloy nanoplates. This work broadens the functionality of conventional binary materials and motivates the development of tailored polarimetric optoelectronic devices.