Circularly Polarized Photoluminescence in Chiral Hybrid Organic–Inorganic Manganese Halide Perovskites: From Bulk Materials to Exfoliated Flakes

Abstract Layered hybrid organic–inorganic metal‐halide perovskites (HOIPs) can acquire chirality from molecules incorporated into their structure showing exciting possibilities in optoelectronics and spintronics. However, researchers have focused their attention on the study of bulk compounds, namely unstable and toxic Pb HOIPs. Herein, the chiroptical properties of R‐ and S‐β‐methylphenethylammonium Mn chloride HOIPs are reported in both the bulk and the few‐layer limit as exfoliated flakes. Red photoluminescence (PL) emission originating from the octahedrally coordinated Mn 2+ is observed, with a PL shift to longer wavelengths when passing from bulk to flakes. Circular dichroism and circularly polarized PL mirrored‐signals for enantiomers are found in bulk samples, while in flakes, a degree of circularly polarized emission (P) of up to 17% at 80 K is achieved, comparable to Pb‐based HOIPs. Moreover, angle‐resolved PL measurements on flakes show that the PL emission and P are isotropic. These findings highlight the potential of these HOIPs from bulk to flakes for spin‐optoelectronic applications.