Strain-Tunable Opto-electronics in PdS2 Monolayer: the Role of Band Nesting and Carrier-Phonon Scattering

Abstract

Strain engineering is a powerful strategy for tuning the optoelectronic properties in two-dimensional materials, yet the underlying mechanisms governing their strain response are often not fully elucidated. In this work, our first-principles calculations show that the penta-orthorhombic PdS2 monolayer exhibits two key strain-tunable properties: a continuous redshift of its main optical absorption peak from ∼2.0 to ∼1.6 eV and enhancement in carrier mobility, with a more than threefold increase for electron under 0-4% biaxial tensile strain. Subsequent analysis reveals that the tunable optical response originates from a robust band nesting feature between the highest valence and lowest conduction bands, which is preserved across the Brillouin zone under biaxial strain. For the carrier transport, deformation potential theory predicts mobility increasing with strain, strongly correlating with the reduction of carrier effective mass. Our first-principles calculations show a strain-induced monotonic decrease in carrier linewidths near the band edges, indicating suppressed carrier-phonon scattering and longer carrier lifetime as the origin of the mobility enhancement. Our work establishes a pathway for engineering the optoelectronic response in 2D semiconductors where strong band nesting governs the optical properties and paves the way for the rational design of continuously tunable flexible optoelectronic devices.