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Photopyroelectric‐based circularly polarized light (CPL) detection, coupling the pyro‐phototronic effect and chiroptical phenomena, has provided a promising platform for high‐performance CPL detectors. However, as a novel detection strategy, photopyroelectric‐based CPL detection is currently restricted by the short‐wave optical response, underscoring the urgent need to extend its response range. Herein, visible‐to‐near‐infrared CPL detection induced by the pyro‐phototronic effect is first realized in chiral‐polar perovskites. Specifically, chiral‐polar multilayered perovskites (S‐BPEA)2FAPb2I7 (1‐S, S‐BPEA = (S)‐1‐4‐Bromophenylethylammonium, FA = formamidinium) with spontaneous polarization shows intrinsic pyroelectric and photopyroelectric performance. Strikingly, combining its merits of the pyro‐phototronic effect and intrinsic wide‐spectrum spin‐selective effect, chiral multilayered 1‐S presents efficient photopyroelectric‐based broadband CPL detection performance spanning 405–785 nm. This research first realizes photopyroelectric‐based infrared CPL detection and also sheds light on developing high‐performance broadband CPL detectors based on the pyro‐phototronic effect in the fields of optics, optoelectronics, and spintronics. [ABSTRACT FROM AUTHOR]

Circularly polarized light (CPL) detection has wide applications in many fields, where the anisotropy factor (gIph) is an important indicator to characterize the CPL detection performance. So far, many materials with high gIph have been reported, however, the exploration of the regulation of gIph is still in its infancy. Herein, two novel alternating chiral‐achiral cations intercalation‐type chiral hybrid perovskites (CHPs), named (R/S‐1‐phenylpropylamine)(propylamine)PbBr4 (1‐R/S), exhibit above room‐temperature (RT) polar‐phase transition, which greatly regulates the gIph value. The gIph of 1‐R is 0.04 in high‐temperature phase chiral non‐polar (P212121) by applying 5 V bias, interestingly, with the temperature decrease, the gIph value in low‐temperature phase chiral polar (P21) gradually increases (0.22@360K, 0.40@340K, 0.47@320K), and finally reaches a maximum of 0.5 at RT. Such value is not only the highest among 2D CHPs to date, but presents a 12.5‐fold amplification compared with 0.04. Further, this rare phenomenon should be attributed to the built‐in electric field induced by the polar photovoltaic effect, which sheds light on further obtaining CHPs with large gIph. [ABSTRACT FROM AUTHOR]