Key Takeaways & Executive Findings
- •• • Achieved a photocurrent dissymmetry factor (g_Iph) of 0.5 at zero bias, surpassing the typical <0.3 for most CHP-based detectors, enabling reliable discrimination of left- and right-handed circularly polarized light for secure quantum communication and spin-optoelectronics. • • Demonstrated self-powered CPL detection at an ultralow light intensity of 62 nW cm−2, with a responsivity of 71 mA W−1 and detectivity of 6×10^12 Jones, outperforming prior CHP detectors (e.g., (S-MBA)2PbI4: 2.2×10^11 Jones; (R-α-PEA)PbI3: ~7.1×10^11 Jones; (R-BPEA)2PbI4: ~3×10^11 Jones), enabling weak-signal detection in low-photon-flux environments. • • The multilayered Cs-based chiral-polar perovskite (R-β-MPA)PACsPb2Br7 crystallizes in a polar space group, exhibiting a chiral-polar photovoltaic effect that facilitates spin-selective carrier separation and collection, effectively decoupling chiroptical activity from charge transport. • • The device operates at zero bias (self-powered), significantly suppressing dark current and maintaining polarization selectivity down to 62 nW cm−2, which is critical for energy-efficient, miniaturized CPL sensors in satellite communication and biomedical imaging.
Abstract
Detection of circularly polarized light (CPL) is crucial for advancing next-generation chiral optoelectronic applications, where a large photocurrent dissymmetry factor (g_Iph) is essential for accurate polarization discrimination. Chiral hybrid perovskites (CHPs) have emerged as promising CPL-active materials owing to their intrinsic spin-orbit coupling and chiroptical properties. However, an intrinsic conflict between g_Iph and photocurrent response remains a major bottleneck in current CHP-based devices. Low-dimensional CHPs typically suffer from limited carrier mobility, while multilayered structures improve carrier transport but generally reduce the chiral component, thereby reducing chiroptical activity and g_Iph. Herein, we report a Cs-based multilayered chiral-polar perovskite, (R-β-MPA)PACsPb2Br7 (1R, MPA=methylphenethylammonium, PA=propylammonium). The distinctive chiral-polar photovoltaic effect in 1R benefits spin-selective carrier separation and collection, and the resulting device achieves self-powered CPL detection with a high g_Iph of 0.5 and maintains excellent polarization selectivity even at ultralow light intensities of 62 nW cm−2. Meanwhile, the multilayered framework enables high responsivity of 71 mA W−1 and detectivity of 6×10^12 Jones (1 Jones = 1 cm Hz^(1/2) W−1) even at zero bias. This work provides a rational design strategy to achieve chiral optoelectronic materials with a high dissymmetry factor and photocurrent response.
1. Introduction
Conventional circularly polarized light (CPL) photodetectors rely on bulky optical components such as quarter-wave plates and polarizers to distinguish left- and right-handed circular polarization, leading to low sensitivity, complex integration, and high cost. Chiral hybrid perovskites (CHPs) offer intrinsic chiroptical activity and spin-dependent carrier transport, but their performance is hindered by a fundamental trade-off: low-dimensional CHPs exhibit high chirality but poor carrier mobility, while multilayered structures improve transport at the expense of chiral content, reducing the photocurrent dissymmetry factor (g_Iph). This bottleneck has limited the practical deployment of CHP-based CPL detectors.
To address this, we introduce alternating chiral and achiral spacer cations into a CsPbBr3-derived framework, forming a multilayered chiral-polar perovskite (R-β-MPA)PACsPb2Br7. This design exploits the chiral-polar photovoltaic effect (CPPE) to achieve helicity-sensitive charge separation, while the multilayered inorganic framework ensures efficient carrier transport. The resulting device attains a high g_Iph of 0.5 and a detectivity of 6×10^12 Jones at zero bias, even under ultralow light intensities of 62 nW cm−2, thereby overcoming the long-standing trade-off and offering a viable route for next-generation CPL detection.
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Xin Dong, Zhijin Xu, Yaru Geng, Lina Li, Junhua Luo, Zhihua Sun (2026). Overcoming the chiroptical activity-photoelectricity trade-off via the construction of multilayered Cs-based chiral-polar perovskite. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3931-6
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Frequently Asked Questions
What is the physical origin of the high photocurrent dissymmetry factor (g_Iph = 0.5) in (R-β-MPA)PACsPb2Br7, and how does the chiral-polar photovoltaic effect (CPPE) contribute to spin-selective carrier separation?
The high g_Iph arises from the intrinsic chiral-polar photovoltaic effect (CPPE) in the polar space group of the material. The alternating chiral (R-β-MPA) and achiral (PA) cations create structural asymmetry, which, combined with the polar nature, induces helicity-dependent charge separation. Under CPL illumination, spin-selective carrier collection is enhanced, leading to a large difference in photocurrent between left- and right-handed CPL, yielding g_Iph = 0.5 at zero bias.
How does the device maintain high detectivity (6×10^12 Jones) and responsivity (71 mA W−1) at zero bias, and what is the role of the multilayered inorganic framework?
The multilayered CsPbBr3-derived framework provides efficient carrier transport and high absorption, enabling high responsivity even without external bias. The self-powered operation is achieved via the chiral-polar photovoltaic effect, which generates a built-in electric field that separates carriers. The suppressed dark current at zero bias contributes to the high detectivity, allowing detection of weak signals down to 62 nW cm−2.
What are the key performance metrics compared to previously reported chiral perovskite CPL detectors, and how does this material overcome the trade-off between chiroptical activity and photocurrent response?
The device exhibits a g_Iph of 0.5, responsivity of 71 mA W−1, and detectivity of 6×10^12 Jones, outperforming prior CHP detectors such as (S-MBA)2PbI4 (2.2×10^11 Jones), (R-α-PEA)PbI3 (~7.1×10^11 Jones), and (R-BPEA)2PbI4 (~3×10^11 Jones). The multilayered structure retains sufficient chiral content while ensuring efficient charge transport, effectively decoupling the two conflicting factors.
What is the operational stability of the device under continuous illumination or varying light intensities, and are there any degradation mechanisms observed?
The paper does not provide explicit long-term stability data, but the self-powered operation at zero bias reduces dark current and potential degradation from bias-induced ion migration. The material's polar structure and robust inorganic framework suggest good thermal and environmental stability, though further studies are needed to assess operational lifetime.
What are the scalability prospects for this material in practical CPL detection applications, considering synthesis complexity and cost?
The synthesis involves solution processing of CsPbBr3-derived frameworks with alternating organic cations, which is scalable using standard perovskite fabrication techniques. The use of earth-abundant cesium and lead may raise toxicity concerns, but the high performance at ultralow light intensities could enable applications where sensitivity is paramount, such as in quantum communication and biomedical imaging, justifying the material cost.
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