Large bulk photovoltaic effect and second-harmonic generation in few-layer pentagonal semiconductors PdS${}_2$ and PdSe${}_2$

Abstract

Recently, atomically thin PdSe${}_2$ semiconductors with rare pentagonal Se-Pd-Se monolayers were synthesized and were also found to possess superior properties such as ultrahigh air stability, and high carrier mobility, thus offering a new family of two-dimensional (2D) materials for exploration of 2D semiconductor physics and for applications in advanced opto-electronic and nonlinear photonic devices. In this work, we systematically study the nonlinear optical (NLO) responses [namely, bulk photovoltaic effect (BPVE), second-harmonic generation (SHG) and linear electric-optic (LEO) effect] of noncentrosymmetric bilayer (BL) and four-layer (FL) PdS${}_2$ and PdSe${}_2$ by applying the first-principles density functional theory with the generalized gradient approximation plus scissors-correction. First of all, the shift current conductivity is in the order of 130 $\mu$A/V${}^2$, being very high compared to known BPVE materials. Similarly, their injection current susceptibilities are in the order of 100$\times$10${}^8$A/V${}^2$s, again being large. Secondly, the SHG coefficients (${\chi }^{(2)}$) of these materials are also large, being one order higher than that of the best-known few-layer group 6B transition metal dichalcogenides. For example, the maximum magnitude of ${\chi }^{(2)}$ can reach 1.4$\times$10${}^3$ pm/V for BL PdSe${}_2$ at 1.9 eV and 1.2$\times$10${}^3$ pm/V at 3.1 eV for BL PdS${}_2$. Thirdly we find significant LEO coefficients for these structures in the low photon energy. All these indicate that 2D PdX${}_2$ semiconductors will find promising NLO applications. Fourthly, we find that the large BPVE and SHG of the few-layer PdX${}_2$ structures are due to strong intralayer directional covalent bonding and also 2D quantum confinement.

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Cited by in corpus (2)

• Magnetism-induced second-order nonlinear optical responses in multiferroic BiFeO${}_3$
• Topological bands in the PdSe${}_2$ pentagonal monolayer