Contactless Detection of Giant Helicity‐Dependent Photovoltage in Chiral 2D Perovskites

ABSTRACT

Chiral‐induced spin selectivity (CISS) provides a direct route for spin filtering without magnetic fields, yet directly probing spin‐dependent charge separation in low‐dimensional hybrid perovskite systems remains elusive. Here, we systematically investigate helicity‐dependent charge‐carrier separation in chiral 2D perovskites using a novel contactless approach that employs a dynamic long‐range organization strategy to enhance the chiroptical response. By employing contactless circularly polarized time‐resolved surface photovoltage (CP‐TRSPV), we directly monitor the interplay between chirality and charge separation dynamics across multiple timescales. While typical chiro‐optical absorption in these materials is minimal, we observe a giant photovoltage anisotropy factor g _SPV of −0.7 and 0.17 for the R‐ and S‐enantiomers, respectively. This significant anisotropy, persisting from nanoseconds to milliseconds, indicates that the response is not merely a surface optical effect and is consistent with CISS‐associated spin‐polarized transport. The successful contactless demonstration of giant helicity‐dependent photovoltage substantially expands our understanding of chirality‐controlled charge dynamics and their application in spin‐optoelectronic devices.