Non-artificial Layered Heterostructure as Inch-size Single Crystal for Shortwave Polarized-Light Array Detector

Layered heterostructures of different 2D building blocks have invigorated the booming of 2D materials toward high-performance optoelectronic devices. However, contrary to the typical artificial multi-component form, the engineering of non-artificial layered heterostructure into single-phase crystals and resultant properties are largely overlooked. Here, for the first time, an inch-sized single crystal of a non-artificial layered heterostructure is exploited, (PbBr₂)₂(AMTP)₂PbBr₄ ( 1 , AMTP is 4-ammoniomethyltetrahydropyran), serving as polarization-sensitive candidate. Notably, it adopts an interleaved architecture of 2D perovskite slabs with the distinct non-perovskite lattice, thus forming a self-assembled perovskite-intergrowth layered heterostructure. This motif leads to new electronic transitions distributed across two sublattices and affords an inherent in-plane anisotropy ratio of ≈1.6, beyond some known inorganic materials (e.g., GeSe: 1.44; GeAs: 1.49). Combining this in-plane anisotropy and wide bandgap (≈2.9 eV), lateral crystal array of 1 enables shortwave polarized-light detection with ultrahigh responsivity and detectivity under weak illumination compared to some inorganic polarized detectors. As the first demonstration of inch-sized single crystals of non-artificial layered heterostructure, this study affords a new platform to explore candidates toward high-performance optoelectronic devices.     

2D Antiferroelectric Hybrid Perovskite with a Large Breakdown Electric Field And Energy Storage Density

Energy conversion and storage devices are highly desirable for the sustainable development of human society. Hybrid organic–inorganic perovskites have shown great potential in energy conversion devices including solar cells and photodetectors. However, its potential in energy storage has seldom been explored. Here the crystal structure and electrical properties of the 2D hybrid perovskite (benzylammonium)₂PbBr₄ (PVK-Br) are investigated, and the consecutive ferroelectric-I (FE1) to ferroelectric-II (FE2) then to antiferroelectric (AFE) transitions that are driven by the orderly alignment of benzylamine and the distortion of [PbBr₆] octahedra are found. Furthermore, accompanied by field-induced AFE to FE transition near room temperature, a large energy storage density of ≈1.7 J cm⁻³ and a wide working temperature span of ≈70 K are obtained; both of which are among the best in hybrid AFEs. This good energy storage performance is attributed to the large polarization of ≈7.6 µC cm⁻² and the high maximum electric field of over 1000 kV cm⁻¹, which, as revealed by theoretical calculations, originate from the cooperative coupling between the [PbBr₆] octahedral framework and the benzylamine molecules. The research clarifies the discrepancy in the phase transition character of PVK-Br and shed light on developing high-performance energy storage devices based on 2D hybrid perovskite.     

Hybrid Organic–Inorganic Halide Post-Perovskite 3-Cyanopyridinium Lead Tribromide for Optoelectronic Applications

2D halide perovskite-like semiconductors are attractive materials for various optoelectronic applications, from photovoltaics to lasing. To date, the most studied families of such low-dimensional halide perovskite-like compounds are Ruddlesden–Popper, Dion–Jacobson, and other phases that can be derived from 3D halide perovskites by slicing along different crystallographic directions, which leads to the spatially isotropic corner-sharing connectivity type of metal-halide octahedra in the 2D layer plane. In this work, a new family of hybrid organic–inorganic 2D lead halides is introduced, by reporting the first example of the hybrid organic–inorganic post-perovskite 3-cyanopyridinium lead tribromide (3cp)PbBr₃. The post-perovskite structure has unique octahedra connectivity type in the layer plane: a typical “perovskite-like” corner-sharing connectivity pattern in one direction, and the rare edge-sharing connectivity pattern in the other. Such connectivity leads to significant anisotropy in the material properties within the inorganic layer plane. Moreover, the dense organic cation packing results in the formation of 1D fully organic bands in the electronic structure, offering the prospects of the involvement of the organic subsystem into material's optoelectronic properties. The (3cp)PbBr₃ clearly shows the 2D quantum size effect with a bandgap around 3.2 eV and typical broadband self-trapped excitonic photoluminescence at temperatures below 200 K.     

Centimeter-Sized Single Crystals of Two-Dimensional Hybrid Iodide Double Perovskite (4,4-Difluoropiperidinium)4AgBiI8 for High-Temperature Ferroelectricity and Efficient X-Ray Detection

Ferroelectricity and X-ray detection property have been recently implemented for the first time in hybrid bromide double perovskites. It sheds a light on achieving photosensitive and ferroelectric multifunctional materials based on 2D lead-free hybrid halide double perovskites. However, the low T_c, small P_s, and relatively low X-ray sensitivity in the reported bromide double perovskites hinder practical applications. Herein, the authors demonstrate a novel 2D lead-free iodide double perovskite (4,4-difluoropiperidinium)₄AgBiI₈ (1) for high-performance X-ray sensitive ferroelectric devices. Centimeter-sized single crystal of 1 is obtained and exhibits an excellent ferroelectricity including a high T_c up to 422 K and a large P_s of 10.5 μC cm⁻². Moreover, due to a large X-ray attenuation and efficient charge carrier mobility (μ)–charge carrier lifetime (τ) product, the crystal 1 also exhibits promising X-ray response with a high sensitivity up to 188 μC·Gy_air⁻¹ cm⁻² and a detection limit below 3.13 μGy_air·s⁻¹. Therefore, this finding is a step further toward practical applications of lead-free halide perovskite in high-performance photoelectronic devices. It will afford a promising platform for exploring novel photosensitive ferroelectric multifunctional materials based on lead-free double perovskites.     

Fluorinated Organic A-Cation Enabling High-Performance Hysteresis-Free 2D/3D Hybrid Tin Perovskite Transistors

2D tin-based perovskites have gained considerable attention for use in diverse optoelectronic applications, such as solar cells, lasers, and thin-film transistors (TFTs), owing to their good stability and optoelectronic properties. However, their intrinsic charge-transport properties are limited, and the insulating bulky organic ligands hinder the achievement of high-mobility electronics. Blending 3D counterparts into 2D perovskites to form 2D/3D hybrid structures is a synergistic approach that combine the high mobility and stability of 3D and 2D perovskites, respectively. In this study, reliable p-channel 2D/3D tin-based hybrid perovskite TFTs comprising 3D formamidinium tin iodide (FASnI₃) and 2D fluorinated 4-fluoro-phenethylammonium tin iodide ((4-FPEA)₂SnI₄) are reported. The optimized FPEA-incorporated TFTs show a high hole mobility of 12 cm² V⁻¹ s⁻¹, an on/off current ratio of over 10⁸, and a subthreshold swing of 0.09 V dec⁻¹ with negligible hysteresis. This excellent p-type characteristic is compatible with n-type metal-oxide TFT for constructing complementary electronics. Two procedures of antisolvent engineering and device patterning are further proposed to address the key concern of low-performance reproducibility of perovskite TFTs. This study provides an alternative A-cation engineering method for achieving high-performance and reliable tin-halide perovskite electronics.     

In Situ Embedding Synthesis of Highly Stable CsPbBr3/CsPb2Br5@PbBr(OH) Nano/Microspheres through Water Assisted Strategy

The disappointing stability of perovskites, especially in water, remains a key issue hindering their further commercialization. Here, CsPbBr₃/CsPb₂Br₅@PbBr(OH) (PQDs@PbBr(OH)) nano/microspheres with superior stability and outstanding photoluminescence quantum yield (PLQY, ≈98%) are fabricated through a water-assisted process. The nano/microspheres can maintain excellent photoluminescence (PL) intensity and high PLQY (≈90%) when immersed in water for more than 18 months. By changing the water content in the reaction mixture, the phase, particle size, and PL peaks of the nano/microspheres will change. Compared with CsPbBr₃/Cs₄PbBr₆ nanocrystals synthesized without water, PQDs@PbBr(OH) nano/microspheres exhibit better thermal stability, photostability, and superior stability in water. Based on the first-principles calculations, the enhanced stability results from PbBr(OH) with high decomposition enthalpy in water, which can effectively prevent water from contacting PQDs embedded in it. Moreover, white light-emitting diodes are fabricated by mixing green-emitting PQDs@PbBr(OH) powder and K₂SiF₆:Mn⁴⁺ (KSF) red phosphor on a 460 nm blue chip and the device shows a high luminous efficacy of 101.27 lm W⁻¹ at 10 mA. This work not only provides a reliable method for the facile preparation of ultrastable perovskites, but also has great potentials for future practical applications.     

Polarization-Resolved Broadband MoS2/Black Phosphorus/MoS2 Optoelectronic Memory with Ultralong Retention Time and Ultrahigh Switching Ratio

The rapidly emerging requirement for device miniaturization and structural flexibility make 2D semiconductors and their van der Waals (vdWs) heterostructures extremely attractive for nonvolatile optoelectronic memory (NOM) applications. Although several concepts for 2D NOM have been demonstrated, multi-heterojunction devices capable of further improving storage performance have received little attention. This work reports a concept for MoS₂/black phosphorus (BP)/MoS₂ multi-heterojunction NOM with artificial trap sites through the BP oxidation, in which the trapped holes at BP/PO_x interface intrigue a persistent photoconductivity that hardly recovers within the experimental time scales (exceeding 10⁴ s). As a result of the interfacial trap-controlled charge injection, the device exhibits excellent photoresponsive memory characteristics, including a record high detectivity of ≈1.2 × 10¹⁶ Jones, a large light-to-dark switching ratio of ≈1.5 × 10⁷_, an ultralow off-state current of ≈1.2 pA, and an outstanding multi-bit storage capacity (11 storage states, 546 nC state^–1). In addition, the middle BP layer in the multi-heterojunction enables broadband spectrum distinction (375–1064 nm), together with a high polarization ratio of 8.4. The obtained results represent the significant step toward the high-density integration of optoelectronic memories with 2D vdWs heterostructures.     

Enhancing Resistive Switching Performance and Ambient Stability of Hybrid Perovskite Single Crystals via Embedding Colloidal Quantum Dots

Hybrid organic‐inorganic halide perovskites are actively pursued for optoelectronic technologies, but the poor stability is the Achilles’ heel of these materials that hinders their applications. Very recently, it has been shown that lead sulfide (PbS) quantum dots (QDs) can form epitaxial interfaces with the perovskite matrix and enhance the overall stability. In this work, it is demonstrated that embedding QDs can significantly modify the transport property of pristine perovskite single crystals, endowing them with new functionalities besides being structurally robust and free from grain boundaries. Resistive switching memory devices are constructed using solution‐processed CH₃NH₃PbBr₃ (MAPbBr₃) perovskite single crystals and the QD‐embedded counterparts. It is found that QDs could significantly enhance the charge transport and reduce the current–voltage hysteresis. The pristine singe crystal device exhibits negative differential resistance, while the QD‐embedded crystals are featured with filament‐type switching behavior and much improved device stability. This study underscores the potential of QD‐embedded hybrid perovskites as a new media for advanced electronic devices.     

Centimeter-Sized Molecular Perovskite Crystal for Efficient X-Ray Detection

Molecular perovskites have demonstrated great potential for ferroelectrics and nonlinear optics; however, their charge transport properties for optoelectronics have rarely been explored. Here, understanding of charge transport behavior of molecular perovskite under X-ray excitation based on centimeter-scale TMCM-CdCl₃ (TMCM⁺, trimethylchloromethyl ammonium) single crystal is demonstrated. The crystal is fabricated from an aqueous solution and exhibits a large bandgap of 5.51 eV, with the valence band maximum mainly dominated by the Cl-p/Cd-d states and the conduction band minimum primarily by Cd-s/Cl-p states. Charge mobility exceeding 40 cm² V⁻¹ s⁻¹ and mobility–lifetime (µτ) product on the order of 10⁻⁴ cm² V⁻¹ for the crystal are observed. These excellent optoelectronic properties translate to an efficient photoresponse under X-ray excitation, with the sensitivity reaching 128.9 ± 4.64 µC Gy_air⁻¹ cm⁻² [fivefold higher than that of the commercialized amorphous selenium (α-Se)] and a low detection limit of 1.06 μC Gy_air⁻¹ s⁻¹ (10 V bias). This work pioneers a superior metal-based molecular perovskite single-crystal based paradigm for optoelectronic investigation, which may lead to the discovery of a new generation of X-ray detection and imaging materials.     

Zero‐Dimensional Perovskite Nanocrystals for Efficient Luminescent Solar Concentrators

Luminescent solar concentrators (LSCs) are able to efficiently harvest solar energy through large‐area photovoltaic windows, where fluorophores are delicately embedded. Among various types of fluorophores, all‐inorganic perovskite nanocrystals (NCs) are emerging candidates as absorbers/emitters in LSCs due to their size/composition/dimensionality tunable optical properties and high photoluminescence quantum yield (PL QY). However, due to the large overlap between absorption and emission spectra, it is still challenging to fabricate high‐efficiency LSCs. Intriguingly, zero‐dimensional (0D) perovskites provide a number of features that meet the requirements for a potential LSC absorber, including i) small absorption/emission spectral overlap (Stokes shift up to 1.5 eV); ii) high PL QY (>95% for bulk crystal); iii) robust stability as a result of its large exciton binding energy; and iv) ease of synthesis. In this work, as a proof‐of‐concept experiment, Cs₄PbBr₆ perovskite NCs are used to fabricate semi‐transparent large‐area LSCs. Cs₄PbBr₆ perovskite film exhibits green emission with a high PL QY of ≈58% and a small absorption/emission spectral overlap. The optimized LSCs exhibit an external optical efficiency of as high as 2.4% and a power conversion efficiency of 1.8% (100 cm²). These results indicate that 0D perovskite NCs are excellent candidates for high‐efficiency LSCs compared to 3D perovskite NCs.     

Controlled Growth and Reliable Thickness‐Dependent Properties of Organic–Inorganic Perovskite Platelet Crystal

Organolead halide perovskites (e.g., CH₃NH₃PbI₃) have caught tremendous attention for their excellent optoelectronic properties and applications, especially as the active material for solar cells. Perovskite crystal quality and dimension is crucial for the fabrication of high‐performance optoelectronic and photovoltaic devices. Herein the controlled synthesis of organolead halide perovskite CH₃NH₃PbI₃ nanoplatelets on SiO₂/Si substrates is investigated via a convenient two‐step vapor transport deposition technique. The thickness and size of the perovskite can be well‐controlled from few‐layers to hundred nanometers by altering the synthesis time and temperature. Raman characterizations reveal that the evolutions of Raman peaks are sensitive to the thickness. Furthermore, from the time‐resolved photoluminescence measurements, the best optoelectronic performance of the perovskite platelet is attributed with thickness of ≈30 nm to its dominant longest lifetime (≈4.5 ns) of perovskite excitons, which means lower surface traps or defects. This work supplies an alternative to the synthesis of high‐quality organic perovskite and their possible optoelectronic applications with the most suitable materials.     

The First Improper Ferroelectric of 2D Multilayered Hybrid Perovskite Enabling Strong Tunable Polarization-Directed Second Harmonic Generation Effect

2D organometallic halide perovskites are recently emerging as a robust family of ferroelectrics, of which their inherent spontaneous polarization (P_s) endows fascinating quadratic nonlinear optical properties. However, up to date, few studies are reported to tune and control the second harmonic generation (SHG) effect in this ferroelectric branch. Herein, the first improper ferroelectric of 2D multilayered hybrid perovskites, (IA)₂(EA)₂Pb₃Br₁₀ ( 1 , where IA is isoamylammonium and EA is ethylammonium), which exhibits a high Curie temperature ( ≈ 371 K) and biaxial ferroelectricity with P_s of 2.2  µ C cm⁻² is reported. Strikingly, its unique in-plane ferroelectricity allows strong tunable SHG properties under the polarized-light. That is, the maximum SHG signals are observed with polarized-light parallel to P_s, while the minimum SHG appears along the vertical direction. This SHG anisotropy creates an extremely large dichroism ratio of ≈ 12, as visualized by 2D color mapping, which is the record-high merit for this type of SHG systems. To the best knowledge, this is the first time to achieve tunable SHG effects through ferroelectric polarization. As a pioneering study, the coupling between the SHG effect and ferroelectricity paves a new direction of 2D hybrid perovskite ferroelectrics toward smart optical device applications.     

Flexible Transparent Bifunctional Capacitive Sensors with Superior Areal Capacitance and Sensing Capability based on PEDOT:PSS/MXene/Ag Grid Hybrid Electrodes

Flexible transparent supercapacitors (FTSs) have aroused considerable attention. Nonetheless, balancing energy storage capability and transparency remains challenging. Herein, a new type of FTSs with both excellent energy storage and superior transparency is developed based on PEDOT:PSS/MXene/Ag grid ternary hybrid electrodes. The hybrid electrodes can synergistically utilize the high optoelectronic properties of Ag grids, the excellent capacitive performance of MXenes, and the superior chemical stability of PEDOT:PSS, thus, simultaneously demonstrating excellent optoelectronic properties (T: ≈89%, R_s: ≈39 Ω sq⁻¹), high areal specific capacitance, superior mechanical softness, and excellent anti-oxidation capability. Due to the excellent comprehensive performances of the hybrid electrodes, the resulting FTSs exhibit both high optical transparency (≈71% and ≈60%) and large areal specific capacitance (≈3.7 and ≈12 mF cm⁻²) besides superior energy storage capacity (P: 200.93, E: 0.24 µWh cm⁻²). Notably, the FTSs show not only excellent energy storage but also exceptional sensing capability, viable for human activity recognition. This is the first time to achieve FTSs that combine high transparency, excellent energy storage and good sensing all-in-one, which make them stand out from conventional flexible supercapacitors and promising for next-generation smart flexible energy storage devices.     

Synergy of Organic and Inorganic Sites in 2D Perovskite for Fast Neutron and X-Ray Imaging

Fast neutron and X-ray imaging are considered complementary nondestructive detection technologies. However, due to their opposite cross-sections, development of a scintillator that is sensitive to both fast neutrons and X-rays within a single-material framework remains challenging. Herein, an organic–inorganic hybrid perovskite (C₄H₉NH₃)₂PbBr₄ (BPB) is demonstrated as a scintillator that fully meets the requirements for both fast neutron and X-ray detection. The hydrogen-rich organic component acts as a fast neutron converter and produces detectable recoil protons. The heavy atom-rich inorganic fraction efficiently deposits the energy of charged recoil protons and directly provides a large X-ray cross-section. Due to the synergy of these organic and inorganic components, the BPB scintillator exhibits high light yields (86% of the brightness of a commercial ZnS (Ag)/⁶LiF scintillator for fast neutrons; 22 000 photons per MeV for X-rays) and fast response times (τ_decay = 10.3 ns). More importantly, energy-selective fast neutron and X-ray imaging are also demonstrated, with high resolutions of ≈1 lp mm⁻¹ for fast neutrons and 17.3 lp mm⁻¹ for X-rays; these are among the highest resolution levels for 2D perovskite scintillators. This study highlights the potential of 2D perovskite materials for use in combined fast neutron and X-ray imaging applications.     

Nonlinear Absorption Applications of CH3NH3PbBr3 Perovskite Crystals

Researchers have recently revealed that hybrid lead halide perovskites exhibit ferroelectricity, which is often associated with other physical characteristics, such as a large nonlinear optical response. In this work, the nonlinear optical properties of single crystal inorganic–organic hybrid perovskite CH₃NH₃PbBr₃ are studied. By exciting the material with a 1044 nm laser, strong two‐photon absorption‐induced photoluminescence in the green spectral region is observed. Using the transmission open‐aperture Z‐scan technique, the values of the two‐photon absorption coefficient are observed to be 8.5 cm GW^?1, which is much higher than that of standard two‐photon absorbing materials that are industrially used in nonlinear optical applications, such as lithium niobate (LiNbO₃), LiTaO₃, KTiOPO₄, and KH₂PO₄. Such a strong two‐photon absorption effect in CH₃NH₃PbBr₃ can be used to modulate the spectral and spatial profiles of laser pulses, as well as to reduce noise, and can be used to strongly control the intensity of incident light. In this study, the superior optical limiting, pulse reshaping, and stabilization properties of CH₃NH₃PbBr₃ are demonstrated, opening new applications for perovskites in nonlinear optics.     

Quantitative Correlation of Perovskite Film Morphology to Light Emitting Diodes Efficiency Parameters

This paper reports quantitative correlation of CH₃NH₃PbBr₃ (MAPbBr₃) thin film morphology to light emitting diode efficiency parameters. Sequential (spin coating) deposition is used for highly reproducible and dense film morphology of MAPbBr₃ thin‐film. In this fabrication process using an orthogonal solvent approach, control of morphology, coverage, thickness, and optical properties in these compact thin‐films is demonstrated. Optical studies show direct correlation between morphology to dynamics of photoluminescence (PL) and absolute PL yield. Perovskite light emitting diodes (PeLEDs) are fabricated from these films to find the best ratio of PbBr₂ versus MABr for optimal performance. This study demonstrates PeLEDs with high brightness, ≈1050 cd m^?2 at 4.7 V (luminance efficiency ≈0.1 cd A^?1), for optimal thin‐film process with state‐of‐the‐art device performance. This quantitative analysis suggests that these state‐of‐the‐art PeLEDs suffer from poor charge carrier balance (≈2%) and out‐coupling efficiency (≈6%). Interestingly, charge carrier balance and PL yield together can explain the change in PeLED efficiency modulation with film morphology. Studies on single carrier devices show that these PeLEDs are electron current dominated and charge carrier balance increases with operating bias voltage.     

High Q-Factor and Low Threshold Continuous-Wave Near-Infrared Lasing with Quasi-2D Perovskites

Quasi-2D perovskites have shown great potential in achieving solution-processed electrically pumped laser diodes due to their multiple-quantum-well structure, which induces a carrier cascade process that can significantly enhance population inversion. However, continuous-wave (CW) optically pumped lasing has yet to be achieved with near-infrared (NIR) quasi-2D perovskites due to the challenges in obtaining high-quality quasi-2D films with suitable phase distribution and morphology. This study regulates the crystallization of a NIR quasi-2D perovskite ((NMA)₂FA_n−1Pb_nI_3n+1) using an 18-crown-6 additive, resulting in a compact and smooth film with a largely improved carrier cascade efficiency. The amplified spontaneous emission threshold of the film is reduced from 47.2 to 35.9 µJ cm⁻². Furthermore, by combining the film with a high-quality distributed feedback grating, this study successfully realizes a CW NIR laser of 809 nm at 110 K, with a high Q-factor of 4794 and a low threshold of 911.6 W cm⁻². These findings provide an important foundation for achieving electrically pumped laser diodes based on the unique quasi-2D perovskites.     

Fast Photoresponse from 1T Tin Diselenide Atomic Layers

Atomically layered 2D crystals such as transitional metal dichalcogenides (TMDs) provide an enchanting landscape for optoelectronic applications due to their unique atomic structures. They have been most intensively studied with 2H phase for easy fabrication and manipulation. 1T phase material could possess better electrocatalytic and photocatalytic properties, while they are difficult to fabricate. Herein, for the first time, the atomically layered 1T phase tin diselenides (SnSe₂, III‐IV compound) are successfully exfoliated by the method of mechanical exfoliation from bulk single crystals, grown via the chemical vapor transport method without transport gas. More attractively, the high performance atomically layered SnSe₂ photodetector has been first successfully fabricated, which displays a good responsivity of 0.5 A W^?1 and a fast photoresponse down to ≈2 ms at room temperature, one of the fastest response times among all types of 2D photodetectors. It makes SnSe₂ a promising candidate for high performance optoelectronic devices. Moreover, high performance bilayered SnSe₂ field‐effect transistors are also demonstrated with a mobility of ≈4 cm² V^?1 s^?1 and an on/off ratio of 10³ at room temperature. The results demonstrate that few layered 1T TMD materials are relatively stable in air and can be exploited for various electrical and optical applications.     

Activation of Self-Trapped Emission in Stable Bismuth-Halide Perovskite by Suppressing Strong Exciton–Phonon Coupling

All-inorganic bismuth-halide perovskites are promising alternatives for lead halide perovskites due to their admirable chemical stability and optoelectronic properties; however, these materials deliver inferior photoluminescence (PL) properties, severely hindering their prospects in lighting applications. Here, a novel air-stable but non-emissive perovskite Rb₃BiCl₆ is synthesized, and the material is used as a prototype to uncover origin of the poor optical performance in bismuth-halide perovskite. It is found that the extremely strong exciton–phonon interactions with a large coupling constant up to 693 meV leads to the seriously nonradiative recombination, which, however, can be effectively suppressed to 347 meV by introducing Sb³⁺ ions. As a result, Sb³⁺-doped Rb₃BiCl₆ exhibits a stable yellow emission with unprecedented PL quantum yield up to 33.6% from self-trapped excitons. Systematic spectroscopic characterizations and theoretical calculations are carried out to unveil the intriguing photophysical mechanisms. This work reveals the effect of exciton–phonon interaction, that is often underemphasized, on a material's photophysical properties.     

Record‐Low‐Threshold Lasers Based on Atomically Smooth Triangular Nanoplatelet Perovskite

Single‐crystalline perovskites are ideal candidates for lasing and other optoelectronic applications. Although significant efforts have been made to grow both bulk single‐crystalline perovskites in liquid solution, their dimensions are still too large to make nanoscale whispering‐gallery‐mode (WGM) resonator based lasers that possess high quality (Q) factor and small volume. Besides, most reported perovskite resonators do not possess atomically smooth surfaces and facets, which limits the Q and thereby increases the lasing threshold. Here, atomically smooth triangular PbI₂ templates are fabricated on a mica substrate by the vapor phase deposition method and are converted to atomically smooth perovskites which have regular and unwrinkled facets with average surface roughness less than 2 nm. By using a CH₃NH₃PbI₃ nanoplatelet with a side length of 27 µm and thickness of 80 nm, room temperature WGM lasing with a Q up to 2600 is demonstrated, the highest reported for hybrid organic–inorganic perovskite nanoplatelets. In addition, the volume of the WGM mode is reduced significantly in comparison with the prior reports. The realized high‐quality triangular CH₃NH₃PbI₃ perovskite nanoplatelets with high Q factor and small volume are expected to perform as ideal cavities for long pulse durations lasers and would find potential applications in integrated optoelectronic devices.