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Phosphorene, a well-studied 2D allotrope of phosphorus, features uniqueproperties such as widely tunable bandgap, high carrier mobility, andremarkable intrinsic in-plane anisotropy. Utilizing these structural andelectronic properties, we investigate ultrafast electron dynamics and highharmonic generation (HHG) from phosphorene subject to band structureengineering through external strain, based on ab initio time-dependentdensity-functional theory approach. We show that strong field processes in suchsystems can be optimized and controlled by biaxial tensile and compressivestrain engineering, that results in electronic structure modification. While-10% strain resulted in closing of band gap, 2% strain increased the gap by 22%with respect to 0.9 eV in pristine phosphorene, consequently affecting the highharmonic yield. With reduction of gap, by applying strain from 2% to -10%, thevalence band near $\Gamma-$point becomes more flat and discreet, resulting inlarge electronic density of states and enhanced electronic excitation, whichreflects in their ultrafast sub-cycle dynamics under laser excitation.Moreover, due to its intrinsic in-plane anisotropy, harmonic yield with laserpolarization along the armchair (AC) direction is found to be higher than thatof the zigzag (ZZ) direction for all the strain cases. Nearly, an order ofmagnitude enhancement of harmonic intensity is achieved for -10% strain alongAC direction. The current study expands the research possibilities ofphosphorene into a previously unexplored domain, indicating its potential forfuture utilization in extreme-ultraviolet and attosecond nanophotonics, andalso for efficient table-top HHG sources.

Controlling high-harmonic generation from strain engineered monolayer phosphorene