Chiral-Polar Photovoltage-Driven Efficient Self-Powered Circularly Polarized Light Detection in Three-Dimensional Hybrid Perovskites.

The chiral-polar photovoltaic effect (CPPE), widely present in chiral hybrid perovskites, has brought an unprecedented opportunity for self-powered circularly polarized light (CPL) detection. However, on account of spatial limitations of the crystal structure, currently reported CPPE primarily focuses on low-dimensional hybrid perovskites, which have a low CPL photoresponse restricted by lower carrier transport efficiency compared to three-dimensional perovskites. For the first time, we reported chiral-polar photovoltage-driven efficient self-powered CPL detection in three-dimensional chiral-polar perovskites, MHyPbBr (MHy = Methylhydrazinium).

Stable self-powered X-ray detection with a low detection limit using a green halide hybrid perovskite ferroelectric crystal.

Lead halide hybrid perovskite ferroelectrics show great potential in the field of self-powered X-ray detection due to their excellent X-ray absorption, high carrier mobility, large carrier lifetime, and interesting ferroelectricity. Nonetheless, the toxicity of lead raises concerns regarding safety for humans and the environment, which limits their practical applicability. Herein, we successfully realized stable self-powered X-ray detection with a low detection limit using a lead-free halide hybrid perovskite ferroelectric crystal, [Hmdap]BiBr (1, Hmdap = -methyl-1,3-diaminopropanium), driven by the switchable spontaneous polarization ( ).

Unprecedented Ultraviolet Circularly Polarized Light-Dependent Anomalous Photovoltaics in Chiral Hybrid Perovskites.

Circularly Polarized Light (CPL)-dependent anomalous photovoltaic effect (APVE), characterized by light helicity-manipulated steady photocurrent and above-bandgap photovoltage, has demonstrated significant potential in the fields of photoelectronic and photovoltaics. However, exploiting CPL-dependent APVE in chiral hybrid perovskites, a promising family with intrinsic chiroptical activity and non-centrosymmetric structure, remains challenging. Here, leveraging the flexible structural design of chiral alternating cations intercalation-type perovskites, CPL-dependent APV, for the first time, is achieved in chiral perovskites.

Chiral-Polar Alternating Cation Intercalation-Type Perovskite Enables Sensitive Self-Driven X-ray Detection with an Ultralow Detection Limit.

Metal halide perovskites (MHPs) have shown great potential for direct X-ray detection, but achieving high sensitivity without external bias remains challenging. Chiral-polar alternating cation intercalation (ACI)-type MHPs, with excellent optoelectronic properties and a robust chirality-induced bulk photovoltaic effect (BPVE), offer a promising platform for self-driven X-ray detection. Herein, impressive self-driven X-ray detection performance was achieved by utilizing chiral-polar 2D ACI-type perovskite single crystals of (-PPA)PAPbBr (; -PPA = -1-phenylpropylamine; PA = propylamine).

Self-Powered Broadband Photodetection Ranging from X-ray to UV-Vis Light in a Polar Perovskite Induced by Bulk Photovoltaic Effect.

Self-powered broadband photodetection has evoked increased interest in next-generation photoelectronic devices. However, realizing self-powered broadband photodetection in a single material is still a challenge because of the harsh requirements, including powerful built-in field, excellent charge transport behaviors, as well as the broad absorption. Herein, we first realize broadband photodetection in the range from X-ray to UV-vis light in a polar two-dimensional perovskite (2-FBA)MAPbI (2-FBA = 2-fluorobenzylamine, MA = methylamine) by incorporating an aromatic spacer into a three-dimensional prototype.

Indium-Assisted Construction of {SiNbO}-Based Aggregates and Their Assembly into Extended Polyoxoniobate Architectures.

In this research, indium ions were introduced into polyoxoniobates (PONbs) reaction systems to facilitate the construction of different {SiNbO}-based aggregates, including an {In(en){SiNbO}} (en = ethylenediamine) dimer, an {[InO][In(en)O]{SiNbO}} trimer, and an {[In(en)][InO][In(en)O]{SiNbO}} tetramer. Interestingly, these aggregates were further assembled into three uncommon extended PONb architectures in the presence of [Cu(en)] complexes, namely, H[Cu(en)(HO)][Cu(en)][Cu(en)]{[In(en)][K{SiNbO}(HO)]}·1.5en·16HO, H{[Cu(en)]{[Cu(en)][Cu(en)(HO)][In(HO)][In(en)(HO)(OH)]{SiNbO}}·5en·29HO, and H[Cu(en)][Cu(en)(HO)]{[Cu(en)]{[Cu(en)][Cu(en)(HO)][K(HO)][In(HO)][In(en)][In(OH)(en)]{SiNbO}}·7en·39HO.

Building High-Density Polar Hybrid Perovskites via Intercalation of Cs and Aromatic Diamine for Passive X-ray Detection.

2D organic-inorganic hybrid perovskites (OIHPs) have shown great promise in direct X-ray detection. The development of high-performance passive X-ray detectors in 2D OIHPs calls for an increase in material density while maintaining structural polarity, which is becoming quite challenging. Here, a high-density, polar 2D alternating-cation-intercalated (ACI) perovskite, (4-AP)CsPbI (, 4-AP = 4-amidinopyridinium), capable of addressing this problem is successfully constructed by introducing heavy Cs into the interlayer space of an aromatic Dion-Jacobson (DJ) perovskite (4-AP)PbI ().

Multi-Axial Self-Driven X-Ray Detection by a Two-Dimensional Biaxial Hybrid Organic-Inorganic Perovskite Ferroelectric.

Metal halide perovskite ferroelectrics combining spontaneous polarization and excellent semiconducting properties is an ideal platform for enabling self-driven X-ray detection. However, achievements to date have been only based on uniaxiality, which increases the complexity of device fabrication. Multi-axial ferroelectric materials have multiple equivalent polarization directions, making them potentially amenable to multi-axial self-driven X-ray detection, but the report on these types of materials is still a huge blank.

Pyro-Phototronic Effect Induced Circularly Polarized Light Detection with a Broadband Response.

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.

Multiple Interlayer Interactions Enable Highly Stable X-ray Detection in 2D Hybrid Perovskites.

Metal halide perovskites have outperformed conventional inorganic semiconductors in direct X-ray detection due to their ease of synthesis and intriguing photoelectric properties. However, the operational instability caused by severe ion migration under a high external electric field is still a big concern for the practical application of perovskite detectors. Here, we report a 2D (BPEA)PbI (BPEA = -1-(4-bromophenyl)ethylammonium) perovskite with Br-substituted aromatic spacer capable of introducing abundant interactions, e.

Dion-Jacobson Type Lead-Free Double Perovskite with Ultra-Narrow Aromatic Interlayer Spacing for Highly Sensitive and Stable X-ray Detection.

The low-toxic and environmentally friendly 2D lead-free perovskite has made significant progress in the exploration of "green" X-ray detectors. However, the gap in detection performance between them and their lead-based analogues remains a matter of concern that cannot be ignored. To reduce this gap, shortening the interlayer spacing to accelerate the migration and collection of X-ray carriers is a promising strategy.

Borosilicate-Based Framework: Synthesis, Single-Crystal Structure Study, and Physical Properties.

Herein, we report the synthesis, crystal structure, and optical properties of a metal-free three-dimensional (3D) inorganic covalent framework ((Hen)[Si(BO)], named , where Hen is the abbreviation for ethanediamine). With the assistance of a tiny amount of F ions and the selection of SiO as Si sources, single crystals of can be successfully prepared under solvothermal conditions. The precise structure information on has been disclosed through both single-crystal X-ray diffraction (SCXRD) and low-dose high-resolution transmission electron microscopy (LD-HRTEM).

Three-Dimensional Polar Perovskites for Highly Sensitive Self-Driven X-Ray Detection.

Three-dimensional (3D) organic-inorganic hybrid perovskites (OIHPs) have achieved tremendous success in direct X-ray detection due to their high absorption coefficient and excellent carrier transport. However, owing to the centrosymmetry of classic 3D structures, these reported X-ray detectors mostly require external electrical fields to run, resulting in bulky overall circuitry, high energy consumption, and operational instability. Herein, we first report the unprecedented radiation photovoltage in 3D OIHP for efficient self-driven X-ray detection.

Regulating Circularly Polarized Light Detection via Polar-Phase Transition in Alternating Chiral-Achiral Cations Intercalation-Type Hybrid Perovskites.

Circularly polarized light (CPL) detection has wide applications in many fields, where the anisotropy factor (g ) is an important indicator to characterize the CPL detection performance. So far, many materials with high g have been reported, however, the exploration of the regulation of g is still in its infancy. Herein, two novel alternating chiral-achiral cations intercalation-type chiral hybrid perovskites (CHPs), named (R/S-1-phenylpropylamine)(propylamine)PbBr (1-R/S), exhibit above room-temperature (RT) polar-phase transition, which greatly regulates the g value.

A Metal-Free Helical Covalent Inorganic Polymer: Preparation, Crystal Structure and Optical Properties.

Helical morphologies are widely observed in nature, however, it is very challenging to prepare artificial helical polymers. Especially, precisely understanding the structure information of artificial metal-free helical covalent inorganic polymers via single-crystal X-ray diffraction (SCXRD) analysis is rarely explored. Here, we successfully prepare a novel metal-free helical covalent inorganic polymer ({[Te(C H ) ] [PO (OH)]} , named CityU-10) by introducing angular anions (HOPO ) into traditional tellurium-oxygen chains.

Unique Perovskitizer N─Pb Bond Switching Induced Polar Photovoltaic Effect in Trilayered Hybrid Perovskite.

Polar photovoltaic effect (PPE) has attracted great attention in regulating desired optoelectronic properties, which can be driven by order-disorder and displacive phase transitions. Bond-switching is also a feasible method to induce PPE, but such investigation is very rare. Lead-halide hybrid perovskite (LHHP) is an outstanding photodetection material; lead atoms possess rich coordination modes to provide possibilities to construct switchable bonds.

Radiation Photovoltaics in a 2D Multilayered Chiral-Polar Halide Perovskite toward Efficient Self-Driven X-Ray Detection.

2D multilayered organic-inorganic hybrid perovskites (OIHPs) have exhibited bright prospects for high-performance self-driven X-ray detection due to their strong radiation absorption and long carrier transport. However, as an effective tool for self-driven X-ray detection, radiation photovoltaics remain rare, and underdeveloped in multilayered OIHPs. Herein, chirality to induce radiation photovoltaics in 2D multilayered chiral OIHPs is first utilized for efficient self-driven X-ray detection.

Circularly Polarized Light-Dependent Pyro-Phototronic Effect from 2D Chiral-Polar Double Perovskites.

Chiral hybrid perovskites combine the advantages of chiral materials and halide perovskites, offering an ideal platform for the design of circularly polarized light (CPL) detectors. The pyro-phototronic effect, as a special mechanism of the photoexcited pyroelectric signal, can significantly improve the performance of photodetectors, whereas it remains a great challenge to achieve pyroelectricity-based CPL detection. In this work, the chiroptical phenomena and the pyro-phototronic effect are combined in chiral-polar perovskites to achieve unprecedented pyroelectric-based CPL detection.

Chiral-Achiral Cations Intercalation Induced Lead-Free Chiral-Polar Hybrid Perovskites Enable Self-Powered X-Ray and Ultraviolet-Visible-Near-Infrared Photo Detection.

Lead halide hybrid perovskites have made great progress in direct X-ray detection and broadband photodetection, but the existence of toxic Pb and the demand for external operating voltage have severely limited their further applications and operational stability improvements. Therefore, exploring "green" lead-free hybrid perovskite that can both achieve X-ray detection and broadband photodetection without external voltage is of great importance, but remains severely challenging. Herein, using centrosymmetric (BZA)BiI (1, BZA = benzylamine) as a template, a pair of chiral-polar lead-free perovskites, (BZA)(R/S-PPA)BiI (2-R/S, R/S-PPA = (R/S)-1-Phenylpropylamine) are successfully obtained by introducing chiral aryl cations of (R/S)-1-Phenylpropylamine.

Alternating chiral and achiral spacers for constructing two-dimensional chiral hybrid perovskites toward circular-polarization-sensitive photodetection.

The intrinsic integration of structural flexibility, chiroptical activity, and photoelectric properties endows the two-dimensional (2D) chiral hybrid perovskites (CHPs) with significant application potential in chiroptoelectronics and spintronics. However, the scarcity of suitable chiral organic ligands severely hinders their extensive construction, necessitating the development of new strategies for designing 2D CHPs. Herein, by exploiting a half substitution method, we created a pair of 2D CHPs with alternating cations in the interlayer space (ACI), (/-PPA)(PA)PbBr (2/2, PPA = 1-phenylpropylamine, PA = -pentylamine), from the achiral Ruddlesden-Popper (RP) (PA)PbBr (1).

Unprecedented Chiral Three-dimensional Hybrid Organic-Inorganic Perovskitoids.

Chiral three-dimensional hybrid organic-inorganic perovskites (3D HOIPs) would show unique chiroptoelectronic performance due to the combination of chirality and 3D structure. However, the synthesis of 3D chiral HOIPs remains a significant challenge. Herein, we constructed a pair of unprecedented 3D chiral halide perovskitoids (R/S-BPEA)EA Pb Cl (1-R/S) (R/S-BPEA=(R/S)-1-4-Bromophenylethylammonium, EA=ethylammonium), in which the large chiral cations can be contained in the big "hollow" inorganic frameworks induced by mixing cations.

Weak X-Ray to Visible Lights Detection Enabled by a 2D Multilayered Lead Iodide Perovskite with Iodine-Substituted Spacer.

Broadband photodetectors (PDs) with low detection limits hold significant importance to next-generation optoelectronic devices. However, simultaneously detecting broadband (i.e.

Low Detection Limit Circularly Polarized Light Detection Realized by Constructing Chiral Perovskite/Si Heterostructures.

Chiral perovskites have been demonstrated as promising candidates for direct circularly polarized light (CPL) detection due to their intrinsic chirality and excellent charge transport ability. However, chiral perovskite-based CPL detectors with both high distinguishability of left- and right-handed optical signals and low detection limit remain unexplored. Here, a heterostructure, (R-MPA) MAPb I /Si (MPA = methylphenethylamine, MA = methylammonium) is constructed, to achieve high-sensitive and low-limit CPL detection.

Proton-Conductive Polyoxometalate Architectures Constructed from Lanthanide-Incorporated Polyoxoniobate Cages.

Two new extended polyoxometalate (POM) architectures based on lanthanide-incorporated polyoxoniobate (Ln-incorporated PONb) cages, namely, H[Cu(en)]{K(HO)[Cu(en)][Cu(trz)(en)(OH)][DyCu(en)(CO)(HO)(OH)][Dy(HO)][DyNbO(HO)]}·60HO (, en = ethylenediamine) and H[Cu(en)]{[Cu(en)][Dy(CO)(HO)][(Nb(OH)(HO)O]}·54HO (), have been successfully synthesized and structurally characterized, demonstrating a feasible strategy to develop functional POM materials. In addition, the proton conductivity and magnetic behaviors of both and were studied.