Abstract Inspired by the urgent demand for novel multifunctional materials in advanced technology applications, herein, first-principles calculations are utilized to construct new two-dimensional GaSiX 2 (X = N, P, As) monolayers. After optimizing the GaSiX 2 crystal structures, their stabilities, Raman responses, piezoelectricity, and electronic/transport characteristics are systematically studied. Results from phonon dispersions, ab initio molecular dynamics simulations, elastic constants, and cohesive energies confirm the good dynamic, thermal, energetic, and mechanical stabilities of the proposed GaSiX 2 monolayers. Based on the Heyd–Scuseria–Ernzerhof approach, the GaSiX 2 exhibit semiconductor behaviors with favorable bandgaps for absorption of the visible spectrum of 1.82 for GaSiP2 and 1.43 eV for GaSiAs2 monolayer. In addition, the GaSiX 2 monolayers also show piezoelectric effects, and high in-plane piezoelectric coefficients d 11 are found for the GaSiP2 (−1.16 pm V − 1 ) and GaSiAs2 (−1.26 pm V − 1 ). The carrier mobilities of the GaSiX 2 are estimated by the deformation potential method for their transport properties. Along two in-plane transport directions, the carrier mobilities of the GaSiX 2 are anisotropy for holes and electrons. GaSiP2 and GaSiAs2 show large electron mobilities along the x axis of 2816.99 and 1211.41 cm2V−1s−1, respectively. Thus, the GaSiP2 and GaSiAs2 monolayers not only have high anisotropic electron mobilities but also favorable bandgaps and large piezoelectric coefficients, indicating potential applications of GaSiP2 and GaSiAs2 in electronic, photovoltaic, and piezoelectric devices. The findings of this study may provide insights into the GaSiX 2 monolayers for multifunctional applications.
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