Sub-picosecond, strain-tunable, polarization-selective optical switching via anisotropic exciton dynamics in quasi-1D ZrSe3.

In cutting-edge optical technologies, polarization is a key for encoding and transmitting vast information, highlighting the importance of selectively switching and modulating polarized light. Recently, anisotropic two-dimensional materials have emerged for ultrafast switching of polarization-multiplexed optical signals, but face challenges with low polarization ratios and limited spectral ranges. Here, we apply strain to quasi-one-dimensional layered ZrSe₃ to enhance polarization selectivity and tune operational energies in ultrafast all-optical switching. Initially, transient absorption on unstrained ZrSe₃ reveals a sub-picosecond switching response in polarization along a specific crystal axis, attributed to shifting-recovery dynamics of an anisotropic exciton. However, its polarization selectivity is weakened by a slow non-excitonic response in the perpendicular polarization. To overcome this limitation, we apply strain to ZrSe₃ by bending its flexible substrate. The compressive strain spectrally decouples the excitonic and non-excitonic components, doubling the polarization selectivity of the sub-picosecond switching and tripling it compared to that in the tensile-strained ZrSe₃. It also effectively tunes the switching energy at a shift rate of ~93 meV %^-1. This strain-tunable switching is repeatable, reversible, and robustly maintains the sub-picosecond operation. First-principles calculations reveal that the strain control is enabled by momentum- and band-dependent modulations of the electronic band structure, causing opposite shifts in the excitonic and non-excitonic transitions. Our findings offer a novel approach for high-performance, wavelength-tunable, polarization-selective ultrafast optical switching.