Three-dimensional excitonic dipole anisotropy enables ultrabroadband polarization photodetection in CrCl3

Abstract

Simultaneous detection of the spectral and polarization properties of light is highly desirable for integrated imaging and photonic technologies but typically requires complex multi-component architectures. Here, we demonstrate that the intrinsic dielectric anisotropy of layered insulating CrCl3 enables ultrabroadband polarization-resolved photodetection spanning wavelengths from 300 to 1700 nm. The photoresponse is governed by long-lived ligand-field excitons, whose microsecond-scale lifetime produces a photoconductive gain exceeding 4.5 x 10^4. By combining wavelength-, polarization-, and angle-resolved optoelectronic measurements, we reveal that distinct ligand-field and higher-energy excitonic transitions possess different optical dipole orientations, leading to excitation-energy-dependent rotation of the in-plane polarization axis. Furthermore, oblique illumination activates out-of-plane optical dipoles, while competing excitonic transitions with distinct dipole orientations drive wavelength-dependent rotation and reversal of the polarization anisotropy. Together, these effects produce a highly tunable degree of polarization ranging from -90% to +75%, establishing intrinsic three-dimensional vectorial light-matter interactions in a layered magnetic van der Waals insulator. These findings establish dielectric anisotropy and excitonic dipole engineering as powerful design principles for compact ultrabroadband polarization-sensitive photodetectors and multifunctional van der Waals photonic systems.