Chirality Inducing Polar Photovoltage in a 2D Lead-Free Double Perovskite toward Self-Powered X-ray Detection

ACS Energy Letters, Год журнала: 2023, Номер 8(6), С. 2809 - 2816

Опубликована: Май 31, 2023

Lead-free halide double perovskites (HDPs) have sparked broad interest in developing "green" photodetectors; however, self-powered X-ray detectors this family remain elusive. Here, by exploiting the chirality-induced polar photovoltaic effect a chiral-polar 2D HDP, (R-MPA)4AgBiI8 (1, R-MPA = R-β-methylphenethylammonium), we successfully realized detection. The significant spontaneous electric polarization 1 gives it large photovoltage of 0.36 V, which drives separation and transport X-ray-generated carriers, thus acquiring capability Consequently, based on high-quality single crystals exhibit high sensitivity 46.3 μC Gy–1 cm–2 an ultralow detection limit 85 nGy s–1 at zero bias. can be further increased to 949.6 50 V bias, outperforming all current HDP detectors. Our work is first demonstrate single-phase lead-free HDPs, enlightening future design radiation

Язык: Английский

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Inch‐Size Single Crystals of Lead‐Free Chiral Perovskites with Bulk Photovoltaic Effect for Stable Self‐Driven X‐Ray Detection

Advanced Functional Materials, Год журнала: 2023, Номер 33(36)

Опубликована: Май 8, 2023

Abstract Lead halide perovskites have made great advance in direct X‐ray detection, however the presence of toxic lead and requirement high working voltages severely limit their applicability operational stability. Thus, exploring “green” lead‐free hybrid capable detecting X‐rays at zero bias is crucial but remains toughly challenging. Here, utilizing chiral R / S ‐1‐phenylpropylamine ( ‐PPA) cations, a pair 0D chiral‐polar perovskites, 2 BiI 5 1 ) are constructed. Their intrinsic spontaneous electric polarization induces large bulk photovoltage 0.63 V, which acts as driving force to separate transport photogenerated carriers, thus endowing them with capability self‐driven detection. Consequently, detectors low detection 270 nGy s −1 successfully constructed based on high‐quality, inch‐sized single crystals . Notably, they show suppressed baseline drift under mode, exhibiting superior This study realizes single‐phase perovskite by exploiting photovoltaic effect, sheds light future explorations toward radiation performance.

Язык: Английский

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Spintronic Phenomena and Applications in Hybrid Organic–Inorganic Perovskites

Advanced Functional Materials, Год журнала: 2024, Номер 34(27)

Опубликована: Март 1, 2024

Abstract The spin degree of freedom in hybrid organic–inorganic perovskites (HOIPs) has become a rapidly growing research topic both HOIPs and spintronics fields due to its fundamental scientific significance tight relevance with optoelectronics. flourishing achievements HOIP call for timely review summarize the key progress guide future developments. In this review, classical spintronic phenomena based on spin‐orbit coupling (SOC) are discussed, especially Rashba splitting related applications such as spin‐charge conversion. Owing unique chirality‐spin coupling, chiral particularly focused on, including chirality‐induced selectivity (CISS). Based complex band structure carrier/exciton, dynamics is also widely investigated constitutes an indispensable part spintronics. Aside from three main threads, other magneto‐optical device exploration involved promising opportunities. Despite continuous breakthroughs spintronics, more efforts required expand material systems, explore new physics, optimize configurations enhanced performance high integration. A deep understanding behaviors will create platform beyond conventional optoelectronic photovoltaic applications.

Язык: Английский

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Hafnium-Based Chiral 2D Organic–Inorganic Hybrid Metal Halides: Engineering Polarity and Nonlinear Optical Properties via Para-Substituent Effects

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 8, 2025

Two-dimensional (2D) organic–inorganic hybrid metal halides (OIMHs), characterized by noncentrosymmetric structures arising from the incorporation of chiral organic molecules that break inversion symmetry, have attracted significant attention. Particularly, chiral-polar 2D OIMHs offer a unique platform for multifunctional applications, as coexistence chirality and polarity enables simultaneous manifestation distinct properties such nonlinear optical (NLO) effects, circular dichroism (CD), ferroelectricity. In this study, we report first synthesis hafnium (Hf)-based OIMHs, achieved through strategic para-substituents on benzene ring components. By tuning substituents, successfully modulate crystal structures, resulting in both chiral-nonpolar systems. Our analysis structural properties, supported density functional theory calculations, demonstrates these materials can be systematically tuned, enabling adjustable band gaps CD UV range (200–280 nm). Notably, halogen substitution at para-position layer produces tunable ranging 4.33 to 4.48 eV, widest reported date OIMHs. Furthermore, exhibit enhanced NLO including remarkable 3.3-fold increase second-harmonic generation intensity compounds compared their counterparts. These findings position Hf-based promising candidates UV-region devices self-driven circularly polarized light detectors, offering new opportunities designing optoelectronic harnessing interplay between polarity.

Язык: Английский

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Integrating Achiral and Chiral Organic Ligands in Zero‐Dimensional Hybrid Metal Halides to Boost Circularly Polarized Luminescence

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(37)

Опубликована: Июль 24, 2023

Chiral zero-dimensional hybrid metal halides (0D HMHs) could combine excellent optical properties and chirality, making them promising for circularly polarized luminescence (CPL). However, chiral 0D HMHs with efficient CPL have been rarely reported. Here, we propose an strategy to achieve simultaneously high photoluminescence quantum yield (PLQY) large dissymmetry factor (glum ), by integrating achiral ligands into HMHs. Specifically, three pairs of indium-antimony chlorides are synthesized combing guanidine types methylbenzylammonium-based derivatives as the organic cations. These exhibit near-unity PLQY glum values up around ±1×10-2 . The ligand is not only essential crystallize these PLQYs, but also greatly enhances chirality induction from inorganic units in Furthermore, choice different can modify strength hydrogen bonding interactions HMHs, maximize their values. Overall, this study provides a robust way realize expanding applications chiroptical fields.

Язык: Английский

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

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(46), С. 25134 - 25142

Опубликована: Ноя. 13, 2023

Chiral hybrid perovskites combine the advantages of chiral materials and halide perovskites, offering an ideal platform for design circularly polarized light (CPL) detectors. The pyro-phototronic effect, as a special mechanism photoexcited pyroelectric signal, can significantly improve performance photodetectors, whereas it remains great challenge to achieve pyroelectricity-based CPL detection. In this work, chiroptical phenomena effect are combined in chiral-polar unprecedented pyroelectric-based Two novel two-dimensional (2D) lead-free double S/R-[(4-aminophenyl)ethylamine]2AgBiI8·0.5H2O, successfully designed synthesized by introducing organic ligands into metal frameworks. Strikingly, photoresponse is substantially boosted with support showing increased current that 40 times greater than photovoltaic current. Furthermore, detector possesses excellent detection capacity distinguish different polarization states photons, which impressive glph up 0.27 at zero bias. This study provides brand new process utilizing opens avenue optoelectronic applications.

Язык: Английский

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Resonant Second Harmonic Generation in Proline Hybrid Lead Halide Perovskites

Advanced Optical Materials, Год журнала: 2023, Номер 11(8)

Опубликована: Фев. 8, 2023

Abstract Chiral hybrid organic−inorganic perovskites (HOIPs) with intrinsic noncentrosymmetry have shown great potentials for chiroptoelectronic applications including second‐order nonlinear optics (NLO). Ideal NLO materials should simultaneously feature a large coefficient, wide optical transparency, high laser damage threshold, and physicochemical stability. However, the development of applicable has been largely restricted due to their strict requirement on structural noncentrosymmetry. Here, chiral amino acids abundant in nature adopted synthesize lead halide ( D ‐/ L ‐Pro)PbI 3 ·H 2 O (Pro = Proline) resonance enhanced second‐harmonic generation (SHG). Their crystals balanced performances transparent region, polarization ratio. This work demonstrates promise naturally construction metal next optoelectronic materials.

Язык: Английский

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Discovering New Type of Lead‐Free Cluster‐Based Hybrid Double Perovskite Derivatives with Chiral Optical Activities and Low X‐Ray Detection Limit

Advanced Functional Materials, Год журнала: 2023, Номер 33(26)

Опубликована: Март 24, 2023

Abstract 2D chiral hybrid perovskites have recently emerged as outstanding semiconductor materials. However, most of the reported limited structural types and contain high levels toxic lead, which severely hinders their further applications. Herein, by using a mixed‐cation strategy, an unprecedented type lead‐free cluster‐based double perovskite derivatives are successfully obtained, [( R / S ‐PPA) 4 (IPA) 6 Ag 2 Bi I 24 ]·2H O ( 1‐R 1‐S ), n ‐BA) 2‐R 2‐S ) ‐PPA= –1‐phenylpropylamine; IPA=isopentylamine; ‐BA= ‐butylamine). Their inorganic skeletons linked binuclear {Bi 10 } infinite chain {Ag 14 ∞ , in bismuth clusters multiple coordination modes (e.g., tetrahedral AgI octahedral introduced into system for first time. This introduction induces distortion layer, may facilitate transfer chirality from cations achiral skeletons. Further, circular dichroism measurements circularly polarized light detection confirm inherent optical activities. In addition, exhibits ultralow X‐ray limit 129.5 nGy s −1 is 42‐fold lower than that demands regular medical diagnosis (5.5 µGy ). study provides pathway to construct novel derivatives.

Язык: Английский

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

Advanced Science, Год журнала: 2023, Номер 10(21)

Опубликована: Май 10, 2023

Broadband photodetectors (PDs) with low detection limits hold significant importance to next-generation optoelectronic devices. However, simultaneously detecting broadband (i.e., X-ray visible regimes) and weak lights in a single semiconducting material remains highly challenging. Here, by alloying iodine-substituted short-chain cations into the 3D FAPbI

Язык: Английский

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

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(11)

Опубликована: Янв. 10, 2024

Abstract 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 the centrosymmetry of classic 3D structures, these reported detectors mostly require external electrical fields run, resulting bulky overall circuitry, energy consumption, operational instability. Herein, we first report unprecedented radiation photovoltage OIHP for efficient self‐driven detection. Specifically, polar MhyPbBr 3 ( 1 , Mhy=methylhydrazine) shows an intrinsic (0.47 V) large mobility‐lifetime product (1.1×10 −3 cm 2 V −1 ) under irradiation. Strikingly, physical characteristics endow with sensitive performance, showing a considerable sensitivity 220 μC Gy −2 which surpasses those most detectors. This work explores highly OIHPs, shedding light on future practical applications.

Язык: Английский

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