Chiral Rashba Ferroelectrics for Circularly Polarized Light Detection

Abstract

Direct detection of circularly polarized light (CPL) is a challenging task due to limited materials and ambiguous structure–property relationships that lead to low distinguishability of the light helicities. Perovskite ferroelectric semiconductors incorporating chirality provide new opportunities in dealing with this issue. Herein, a pair of 2D chiral perovskite ferroelectrics is reported, which have enhanced CPL detection performance due to interplays among lattice, photon, charge, spin, and orbit. The chirality‐transfer‐induced chiral&polar ferroelectric phase enhances the asymmetric nature of the photoactive sublattice and achieves a switchable self‐powered detection via the bulk photovoltaic effect. The single‐crystal‐based device exhibits a CPL‐sensitive detection performance under 430 nm with an asymmetric factor of 0.20 for left‐ and right‐CPL differentiation, about two times that of the pure chiral counterparts. The enhanced CPL detection performance is ascribed to the Rashba–Dresselhaus effect that originates from the bulk inversion asymmetry and strong spin–orbit coupling, shown with a large Rashba coefficient, which is demonstrated by density functional theory calculation and circularly polarized light excited photoluminescence measurement. These results provide new perspectives on chiral Rashba ferroelectric semiconductors for direct CPL detection and ferroelectrics‐based chiroptics and spintronics.

Stable organic lead iodides with three-dimensional crystallographic and electronic structures showing high photoresponse

“…The large dielectric change suggests the potential for developing ferroelectrics by introducing chirality or H/F substitution. 41–43…”

“…The large dielectric change suggests the potential for developing ferroelectrics by introducing chirality or H/F substitution. [41][42][43] Compared with (M 2 pda)Pb 2 I 6 , (Mpda)Pb 2 I 6 has a relatively low phase transition temperature (Fig. 4e).…”

Incorporating an Aromatic Diammonium To Assemble Bilayered Dion–Jacobson Perovskite Crystals for Weak Light Detection

“…At present, the research of DJ hybrid perovskites in the form of a thin film is more than that of its single crystal, which limits the fundamental study of its structure–activity relationship. , Recently, the research of using DJ hybrid perovskite bulk single crystals for photodetection has attracted increasing attention, which is due to the single-crystal materials have significant advantages compared to polycrystalline materials, such as no grain boundaries, few defect states, and high carrier mobility. − For example, Liu’s group reported a monolayer DJ hybrid perovskite (DGA)­PbI 4 crystal with the tiniest lattice distortion, which is used for high-performance X-ray detection and exhibited a pronounced sensitivity of 4869.0 μC Gy air –1 cm –2 . In addition, a bilayered DJ hybrid perovskite crystal (HDA)­CsPb 2 Br 7 (HAD is 1,6-hexamethylenediammonium) was developed by Sun’s group, who studied its photoactivities under 3 mW/cm 2 polarized light, with the detectivity of 1.5 × 10 9 Jones achieved in the crystal-based device .…”

Circularly polarized luminescence enlargement from crystals to oriented films of enantiopure 2D hybrid perovskites

“…20 The reported luminescent C-2D-OIHPs also have small g lum values of the magnitude of 10 −3 . 9–13 How to simultaneously enlarge the emission efficiency and the g lum remains overwhelmingly challenging in C-2D-OIHPs.Films of C-2D-OIHPs usually orientedly grow on some specific substrates, 7,21–24 which have been used to detect circularly polarized light. However, no studies of the enlargement of the optical activities of the oriented C-2D-OIHP films have been reported.…”

“…Films of C-2D-OIHPs usually orientedly grow on some specific substrates, 7,[21][22][23][24] which have been used to detect circularly polarized light. However, no studies of the enlargement of the optical activities of the oriented C-2D-OIHP films have been reported.…”