A monolithic chiral perovskite crystal enables self-powered, full-Stokes detection of ultra-weak light

Abstract

Accurate and chip-integrated full-Stokes polarization detection is essential for advancing multifunctional optoelectronic systems. However, conventional approaches relying on optical filters often suffer from significant optical losses and poor sensitivity under weak-light conditions. Here, we report an efficient full-Stokes polarimeter based on a 1D chiral-polar perovskite, (R/S-NEA)PbI₃. The intrinsic anisotropic and chiral structure of the (R/S-NEA)PbI₃ single crystal enables both high linear and circular polarization sensitivity. Moreover, the polar structure induces a giant bulk photovoltaic effect (BPVE) of up to 8 V, enabling efficient carrier extraction under zero bias and significantly suppressing noise currents to the ∼fA level, resulting in an exceptional specific detectivity of 4.1 × 10¹³ Jones. These combined properties enable accurate, self-powered full-Stokes polarization detection, with the fabricated single-crystal-based polarimeter achieving an average Stokes parameter error (ΔS_1–3) of less than 3%. Notably, the polarimeter demonstrates an ultra-low detection limit of 0.4 μW cm⁻², representing the highest sensitivity among comparable polarimeters reported to date. With easy on-chip integration, the polarimeter showcases precise full-Stokes imaging capabilities.

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Introduction

The state of polarization (SoP), which describes the oscillation direction of the electric field, is a fundamental parameter in optics, playing a critical role in diverse applications such as quantum optics, remote sensing, and astronomy.^1–4 Current state-of-the-art SoP detection technologies rely on full-Stokes polarimeters that integrate metasurfaces or diffraction gratings. However, these components often introduce significant optical losses and fabrication complexity, which in turn limit the detection sensitivity—particularly under low-light conditions—thereby restricting their practical applicability in weak-light polarization sensing.

An ideal approach to overcoming these challenges is to develop semiconducting materials with intrinsic polarization sensitivity. Among the candidates, hybrid metal–halide perovskites stand out due to their outstanding optoelectronic properties and rich chemical tunability.^5–9 For instance, dimensional engineering can induce anisotropic lattice structures, while the incorporation of chiral organic ligands can transfer chirality to the inorganic framework, enabling selective responses to both linearly polarized light (LPL) and circularly polarized light (CPL).^10,11 These structural features endow perovskites with inherent polarization sensitivity. Moreover, the tunable polar structures of perovskites offer another promising pathway to realize ultra-sensitive full-Stokes polarimetry. By breaking inversion symmetry—achievable through specific polar point groups—perovskites can exhibit bulk photovoltaic effects (BPVEs),^12,13 which allows polarimeters to operate under zero-bias conditions with minimal noise current, while enhancing polarization sensitivity under low-light illumination.

Recent progress has demonstrated the feasibility of using chiral perovskites for full-Stokes photodetection. While high-performance SoP polarimeters have been realized using patterned 2D and 3D chiral perovskites with aligned nanowires,^14–19 the complex and costly fabrication processes involved present significant drawbacks. Consequently, a more streamlined approach of integrating anisotropy and chirality directly into the perovskite crystal lattice has become a promising strategy for high-performance detection.^20–22 Despite this progress, a fundamental limitation persists. Most intrinsically polarization-sensitive perovskites are plagued by large noise currents, which restrict their detection capabilities to optical intensities above the microwatt-per-square-centimeter (μW cm⁻²) threshold. This limitation poses a significant barrier for applications requiring the detection of weak signals or subtle polarization variations, highlighting the urgent need for more promising materials.

In this work, we report 1D chiral-polar (R/S-NEA)PbI₃ (R-NEA = R-(+)-1-(1-naphthyl)ethylamine, S-NEA = S-(−)-1-(1-naphthyl)ethylamine) that exhibits a big BPVE of up to 8 V. This intrinsic BPVE enables efficient carrier extraction under zero bias and suppresses noise currents to the ∼fA level, yielding a high specific detectivity of 4.1 × 10¹³ Jones. The intrinsic anisotropic and chiral structure of (R/S-NEA)PbI₃ enables high linear polarization sensitivity, with a polarization ratio (ω) of 1.99 and a robust CPL anisotropic factor (g_cpl) of 0.57. These combined properties enable accurate, self-powered full-Stokes polarization detection, with the fabricated single-crystal-based polarimeter achieving an average Stokes parameter error (ΔS_1–3) of less than 3%. Remarkably, the polarimeter achieves an ultra-low detection limit of 0.4 μW cm⁻², representing the highest sensitivity reported to date among comparable systems. Benefiting from facile on-chip integration, the polarimeter further enables precise full-Stokes polarization imaging.

Results and discussion

We use temperature-cooling methods to grow the centimeter-sized (R/S-NEA)PbI₃ single crystal (SC), as shown in Fig. S1. The crystallographic structure presents that the chiral NEA⁺ cations surround face-sharing [PbI₆]⁴⁻ octahedral chains via hydrogen bonding (Fig. 1a). This interaction induces chirality transfer from the organic cations to the inorganic framework, forming helically arranged [PbI₆]⁴⁻ chains along the a-axis—a structural motif that promotes strong light–matter interactions with CPL. Moreover, these [PbI₆]⁴⁻ chains exhibit anisotropic topological arrangement along intrachain (a-axis) and out-of-chain (b- or c-axis) directions, thereby imparting structural features favorable for LPL detection (Fig. 1b).

Fig. 1 The schematic illustration of (R-NEA)PbI₃ and (S-NEA)PbI₃: (a) chiral and polar crystallographic structures; (b) anisotropic crystallographic structure. (c) GIWAX pattern of the (R-NEA)PbI₃ SC powder. (d) Possible second-rank axial tensor forms for 16 non-centrosymmetric space groups with chiral and polar characteristics, among which only five exhibit both chiral and polar properties.

Notably, (R/S-NEA)PbI₃ breaks the structural inversion symmetry into a special polar characteristic. Grazing-incidence wide-angle X-ray scattering (GIWAXS) measurements of (R-NEA)PbI₃ reveal distinct (010) and (012) diffraction peaks belonging to the C₂ space group (Fig. 1c). This observation aligns with prior studies and confirms that the synthesized crystals belong to one of the 16 chiral polar point groups—non-centrosymmetric groups that possess nonzero gyration tensors in the helical [PbI₆]⁴⁻ chain direction (as shown in Fig. 1d). The chiral-polar structure is expected to facilitate the BPVE, which enables spontaneous photocarrier separation and extraction under zero bias—an essential mechanism for enhancing polarization sensitivity under weak-light conditions.^23,24

We perform azimuth-dependent reflectance difference microscopy (ADRDM) to quantitatively investigate the anisotropic optical properties of (R/S-NEA)PbI₃ SC. This technique assesses the normalized reflectance difference (ΔR/R) along two orthogonal in-plane directions under linearly polarized light. For (R/S-NEA)PbI₃ SCs with arbitrary in-plane orientations, the angular dependence of ΔR/R(θ) can be modeled as follows:²⁵

ΔR/R(θ) = ΔR/R_ab cos 2(θ − θ₀) (1)

Here, ΔR/R_ab is calculated as ΔR/R_ab = 2(R_a − R_b)/(R_a + R_b), where R_a and R_b denote the reflectance along the a-axis and the b-axis, respectively. θ is the azimuthal angle of the incident polarization relative to the lab frame, and θ₀ is the angle between the a-axis of the crystal and the initial reference direction. Fig. 2a displays the optical image of the (R-NEA)PbI₃ crystal measured by ADRDM, with a black Cartesian coordinate system indicating the azimuthal angle θ. In the initial measurement, the polarization direction of the incident light is aligned with the a-axis of the crystal. During image recording, the angle is rotated counterclockwise in 15° increments. ADRDM images at angles varying from 0° to 180° reveal significant brightness variations across the surface of the (R-NEA)PbI₃ SC (Fig. 2b). The ΔR/R values extracted from each ADRDM image exhibit a clear sinusoidal trend, as shown in Fig. 2c. Notably, ΔR/R reaches a maximum of 0.16 and a minimum of −0.15 at azimuthal angles of approximately 180° and 90°, corresponding closely to the crystallographic a- and b-axis directions, respectively.

Fig. 2 (a) Optical image of (R-NEA)PbI₃ SC on a silicon substrate. The black Cartesian coordinate frame defined along the a- and b-axes is used as the reference for the azimuthal angle (θ). (b) ADRDM images acquired at azimuthal angles from 15° to 180°. (c) Polar plot of ΔR/R as a function of the azimuthal angle θ, extracted from the ADRDM images. (d) CD spectra of (R-/S-NEA)PbI₃ films. (e) Corresponding g_CD spectra of (R-/S-NEA)PbI₃ films.

To gain deeper insight into the anisotropic light–matter interactions, we performed angle-resolved polarized Raman spectroscopy on the crystal's ab-plane. The resulting spectra, shown in Fig. S2a and b, distinctly reveal that the Raman intensity is strongly dependent on the polarization angle of the incident laser. In particular, the prominent low-frequency mode at 53 cm⁻¹, which is attributed to the stretching vibration of the [PbI₆]⁴⁻ octahedra, is analyzed. As plotted in the inset of Fig. S2b, the intensity of this mode follows a clear sinusoidal pattern as a function of polarization angle. This periodic variation is a direct signature of an anisotropic vibrational mode, confirming that the crystal lattice exhibits an asymmetric response to LPL along the a- and b-axes.

The chiroptical properties of the material are further characterized using circular dichroism (CD) spectroscopy. To eliminate interference from linear birefringence (LB) and linear dichroism (LD), we measure CD signals from both the front and back sides of the crystal and apply calibration based on established protocols.²⁶ As shown in Fig. 2d, (R-NEA)PbI₃ and (S-NEA)PbI₃ exhibit strong and opposite CD signals near the exciton resonance (Fig. S3). The corresponding CD anisotropy factor (g_CD) extracted from the spectrum is estimated to be approximately 0.044 (Fig. 2e), which exceeds the values reported for previously studied chiral perovskites.^27–31 This suggests a strong intrinsic response to CPL-vector detection.

To investigate the photoelectronic properties of (R-NEA)PbI₃, we fabricated a lateral-configuration device, as illustrated in Fig. 3a. We first explored the BPVE in 1D (R-NEA)PbI₃ SC by measuring the photocurrent–voltage (I–V) characteristics along the a- and b-axis directions, which correspond to the intrachain and out-of-chain directions, respectively. As shown in Fig. 3b, a pronounced BPVE is observed along the a-axis, characterized by a short-circuit current of approximately 0.5 nA and an open-circuit voltage (V_oc) as high as 8 V. Critically, the magnitude of V_oc scaled linearly with increasing electrode distance (Fig. S4a and b), which points to a uniform electric field originating from the BPVE.³¹ For comparison, almost no BPVE photocurrent is observed along the b-axis due to the centrosymmetric nature in the out-of-plane direction (Fig. 3b inset). Moreover, an opposite negative current signal is observed in the (S-NEA)PbI₃ SC device (Fig. 3c), confirming that the BPVE originates from the intrinsic chiral polar structure rather than measurement artifacts.^9,32–36 These results suggest the presence of a strong internal electric field along the intrachain direction, which is advantageous for efficient carrier separation and extraction.

Fig. 3 (a) Schematic illustration of the experimental configuration for the polarization measurements; the polarization states are modulated using the λ/2 or λ/4 plates. Photocurrent versus voltage (I–V) measurements under 396 nm UV illumination: (b) electrodes assessed parallel to the a-axis and b-axis (inset) of (R-NEA)PbI₃ SC; (c) electrodes assessed parallel to the a-axis of (S-NEA)PbI₃ SC. (d) Photocurrent and responsivity of the (R-NEA)PbI₃ SC polarimeter measured under various light irradiation intensities at zero bias; and (e) corresponding detectivity extracted from responsivity. (f) Frequency photocurrent responses. (g) On–off photocurrent measurements. (h) LPL-dependent and (i) CPL-dependent photocurrent measurements under 396 nm illumination with intensities of 0.4 μW cm⁻² and 300 μW cm⁻².

Encouraged by the strong BPVE, we fabricate a self-powered polarimeter by depositing lateral electrodes along the a-axis of (R-NEA)PbI₃. The photoresponse is characterized under 396 nm irradiation at various light intensities. The polarimeter exhibits a broad linear dynamic range (LDR) of 96 dB (Fig. 3d), with a calculated responsivity (R) of 744 mA W⁻¹ and a corresponding External Quantum Efficiency (EQE) of 233% (Fig. S5). Due to the BPVE-driven carrier extraction, the polarimeter operates without an external bias, significantly reducing dark current fluctuations.^33,37–41 Correspondingly, the equivalent noise current under zero bias is estimated to be as low as 2.4 fA Hz⁻¹ (Fig. S6). Owing to its high responsivity and ultra-low noise, the specific detectivity (D*) of the polarimeter is determined to be 4.1 × 10¹³ Jones (and Fig. 3e), surpassing that (∼10¹² Jones) of commercial silicon photodetectors. This high detectivity is especially beneficial for detecting weak polarization signals buried in noise. Frequency-dependent photocurrent analysis reveals a high response bandwidth of up to 821 Hz (Fig. 3f). Also, the polarimeter demonstrates a fast temporal response, with rise and fall times of 142 μs and 144 μs (Fig. 3g), indicating that the (R-NEA)PbI₃ SC-based polarimeter is capable of high-speed optical sensing. Taken together, the combination of low noise, high detectivity, and fast response makes this chiral perovskite-based polarimeter a highly promising candidate for efficient polarization-sensitive photodetectors.

We further investigated the polarization discrimination capabilities of the (R-NEA)PbI₃ SC polarimeter. First, to optimize the device for LPL detection, we systematically varied the lateral electrode distance and selected 50 μm as the optimal channel width for fabrication (Fig. S7a and b). Using this optimized configuration, the device was illuminated with 396 nm light whose polarization state was controlled using a linear polarizer, a half-wave (λ/2), and a quarter-wave (λ/4) plate. As shown in Fig. 3h and Fig. S8, the (R-NEA)PbI₃ polarimeter exhibits a distinct periodic modulation in photocurrent under zero bias across a wide range of illumination intensities from 0.4 μW cm⁻² to 300 μW cm⁻². Specifically, the polarization ratio (ω = I_max/I_min, where I_max and I_min represent the maximum and minimum photocurrent responses under different polarization angles) is calculated to be 1.99 under 300 μW cm⁻² illumination. Remarkably, even at ultra-low illumination of 0.4 μW cm⁻², the polarization ratio remains at 1.89, indicating minimal performance degradation. This high LPL discrimination surpasses that of most previously reported perovskite polarimeters.^40–42 The helical arrangement of the 1D inorganic framework generates a strong electric field, along with anisotropic absorbance in both intrachain and out-of-chain directions, which excludes the excellent polarization-sensitive performance.

Next, we assess the capability of (R-NEA)PbI₃ for CPL detection by analyzing the photocurrent difference under right-handed (RCP) and left-handed (LCP) circularly polarized illumination. Across the range of incident powers (0.4–300 μW cm⁻²), the polarimeter demonstrates an almost consistent discrimination in photocurrent response between LCP and RCP (Fig. 3i and Fig. S9). By evaluating the photocurrent anisotropy factor (g_cpl) for CPL:

g_cpl = 2(I_L − I_R)/(I_L + I_R) (2)

where I_L and I_R mean the photocurrent under LCP and RCP illumination, respectively. We obtain a g_cpl of 0.57 at 300 μW cm⁻² and retain a high value of 0.41 even under weak illumination of 0.4 μW cm⁻². These results indicate that the robust BPVE in (R-NEA)PbI₃ enables efficient spin-dependent carrier extraction under zero bias, enabling reliable CPL discrimination even under ultra-weak light conditions.

We then explore the detection of the SoPs. Here, we use four Stokes parameters—total intensity S₀, two linear components S₁ and S₂, and the circular component S₃—to describe SoPs. Eight representative SoPs on the Poincaré sphere (modulated using λ/2 and λ/4 wave plates, as depicted in Fig. 4a) are inputted to evaluate detection accuracy. During the measurement process, the polarimeter is rotated at five angles (0°, 45°, 90°, 135°, and 180°) to record the photocurrent. As shown in Fig. 4b, the angle-dependent photocurrent fits well to sinusoidal functions and displays clear dependence on input polarization. By calibrating the photocurrent data according to established methods,^22,43 we extract the Stokes parameters (ΔS_1–3) and compare them with theoretical inputs. As illustrated in Fig. 4c, the measured parameters show excellent agreement with the expected values. The corresponding detection errors under 300 μW cm⁻² illumination are ΔS₁ = 1.3%, ΔS₂ = 2.6%, and ΔS₃ = 2.5% (Fig. 4d). This performance significantly surpasses that of a recently reported polarimeter utilizing an analogous (R-NEA)PbI₃ polycrystalline thin film (see comparison in Table S1).^19,21 We attribute this enhancement to the pronounced BPVE present in single-crystal devices. Notably, at a low-light intensity of 0.4 μW cm⁻², the polarimeter still achieves high accuracy with detection errors of ΔS₁ = 2.0%, ΔS₂ = 3.1%, and ΔS₃ = 3.6% (Fig. S10), enabling full-Stokes polarization detection under ultra-weak illumination conditions that are challenging for conventional optical-filter-based systems. Furthermore, the device shows outstanding long-term stability; its detection accuracy is maintained after 120 days of storage under ambient conditions, with errors for S_1–3 remaining below 4% (Fig. S11a–c).

Fig. 4 (a) Poincaré sphere showing representative SoPs. (b) Measured photocurrent of the (R-NEA)PbI₃ polarimeter under eight distinct input polarization states, recorded with the rotation stage set to 0°, 45°, 90°, 135°, and 180°; the incident wavelength is 396 nm with an illumination intensity of 300 μW cm⁻². (c) Detection errors for the Stokes parameters (S₀–S₃) extracted from the eight input SoPs. (d) Average detection errors for the S₁–S₃ parameters. (e) Schematic illustration of the full-Stokes imaging test: the procedure involved transmitting modulated SoPs through an N-shaped pattern, followed by a step-by-step process to generate a 20 × 20 pixel image array. (f–h) Full-Stokes imaging results for the S₁–S₃ parameters and their corresponding average detection errors.

To demonstrate practical applications, we perform full-Stokes imaging using a patterned “N” mask illuminated with a known SoP (Fig. 4e). By spatially resolving the Stokes parameters across a 20 × 20 pixel array, we reconstruct high-resolution images corresponding to S₁, S₂, and S₃ (Fig. 4f–h), each exhibiting uniform intensity distribution and clear edge definition. The average detection errors across the array are ΔS₁ = 5.2%, ΔS₂ = 5.9%, and ΔS₃ = 7.1%, confirming the system's reliability in pixel-level polarization imaging. Furthermore, from the pixel-wise Stokes data, we extract the Degree of Linear Polarization and Degree of Circular Polarization (DOCP = |S₃|/S₀), yielding DOLP = 0.74 and DOCP = 0.67 from the image recording. This ability to simultaneously capture both linear and circular polarization components demonstrates the polarimeter's robustness for real-time polarization imaging. Notably, unlike conventional division-of-focal-plane polarimeters which require complex optical splitting and at least four detectors per pixel, our filter-less polarimeter offers a compact, monolithic design. This highlights its potential for next-generation in-chip, high-resolution, and energy-efficient full-Stokes imaging systems.

Conclusions

In summary, we developed a high-performance, self-powered full-Stokes polarimeter based on the chiral polar 1D perovskite (R/S-NEA)PbI₃ SC. The intrinsic BPVE enables efficient photocarrier extraction under zero bias, effectively minimizing the influence of noise currents. As a result, the polarimeter achieves a high D* of 4.1 × 10¹³ Jones. The strong linear and circular dichroism endows the polarimeter with excellent sensitivity to both LPL and CPL, with a ω of 1.99 and a g_cpl of 0.57. These characteristics enable accurate full-Stokes polarization detection, achieving an average error in the Stokes parameters (ΔS_1–3) of less than 3%. Remarkably, the polarimeter maintains detection errors below 4% even at an ultra-low light intensity of 0.4 μW cm⁻², surpassing the lowest detectable power reported for comparable polarimeters. Furthermore, we demonstrate full-Stokes imaging with clearly resolved S_1–3 parameter extraction across the image matrix, enabling precise and uniform polarization-resolved imaging.

Experimental section

Materials

Lead(II) oxide (PbO, 99.9%), hydroiodic acid solution (HI, 57% wt/wt), hydrochloric acid solution (H₃PO₄, 37% wt/wt), and R-(+)- or S-(−)-1-(1-naphthyl)ethylamine were purchased from Aladdin (Shanghai, China).

Syntheses

The prescribed stoichiometric quantities of (R or S)-NEA (3 mmol), Pb(Ac)₂·3H₂O (3 mmol) and hydriodic acid (48 wt%, 12 ml) were used in the experiment. First, 3 mmol of Pb(Ac)₂·3H₂O was dissolved in 12 mL of hydriodic acid under continuous stirring. The mixture was gradually heated to 373 K and maintained at this temperature until the solution became completely clear (approximately 10 minutes). Next, 3 mmol of (R or S)-NEA was added to the clear solution, which was then stirred and heated continuously for an additional 15 minutes. After full dissolution, the solution was slowly cooled to room temperature at a rate of 2 K per hour. Orange-colored rod-like crystals of (R or S)-NEAPbI₃ were obtained upon completion of the cooling process.

Device fabrication

Planar structured photoconductive detectors were fabricated by thermally evaporating Au electrodes onto single crystals, and the channel between neighboring electrodes had a width of 0.5 mm, with lengths of 50, 70, 100, 130, and 180 μm.

Author contributions

Quanlin Chen: writing – original draft, methodology, experiment, and data curation. Yangbin Xu: experiment. Qingming Wu: experiment. Yanxing Feng: review and editing. Zhiqiang Huang: review and editing. Hai Jia: review and editing. Shaoming Ying: supervision, conceptualization and formal analysis – review & editing. Xiaohui Huang: supervision, conceptualization and formal analysis – review & editing.

Conflicts of interest

There are no conflicts to declare.

Data availability

The data supporting this article have been included as part of the supplementary information (SI). Supplementary information: experimental and characterization details including XRD, UV-Vis absorption spectra, CD spectra, Raman spectra and POM image recording. The details of photoelectric studies and polarimetric measurements. See DOI: https://doi.org/10.1039/d5qi01944c.

Acknowledgements

Q. Chen acknowledges financial support from the Research Projects of Ningde Normal University (Grant No. 2024Y10), the Foundation for Cultivated Young Talents of Fujian Province, China (Grant No. 2025350147), and the Young and Middle-aged Teacher Education Research Project of Fujian Province of China (Grant No. JAT241161). This work was also supported by the Natural Science Foundation of Fujian Province of China (Grant No. 2024J08226 and 2023J05203) and the Project of Scientific Research of Ningde Normal University (Grant No. 2024ZX01, 2024T02, and 2023Y09).

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