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.     

Suppression of Ionic and Electronic Conductivity by Multilayer Heterojunctions Passivation Toward Sensitive and Stable Perovskite X-Ray Detectors

Organic-inorganic hybrid perovskites are promising candidates for direct X-ray detection and imaging. The relatively high dark current in perovskite single crystals (SCs) is a major limiting factor hindering the pursuit of performance and stability enhancement. In this study, the contribution of dark current is disentangled from electronic (σ_e) and ionic conductivity (σ_i) and shows that the high σ_i dominates the dark current of MAPbBr₃ SCs. A multilayer heterojunctions passivation strategy is developed that suppresses not only the σ_i by two orders of magnitude but also σ_e by a factor of 1.6. The multilayer heterojunctions passivate the halide vacancy defects and increase the electron and hole injection barrier by inducing surface p-type doping of MAPbBr₃. This enables the MAPbBr₃ SC X-ray detectors to obtain a high sensitivity of 19 370 µC Gy_air⁻¹ cm⁻² under a high electric field of 100 V cm⁻¹, a record high sensitivity for bromine self-powered devices, and a low detection limit of 42.3 nGy_air s⁻¹. The unencapsulated detectors demonstrate a stable baseline after storage for 210 days and outstanding operational stability upon irradiation with an accumulated dose of up to 1944 mGy_air.     

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.     

2D-Layered Manganese Perovskite with High Mobility

2D perovskite is an organic–inorganic hybrid material with good photoelectric properties, generally prepared by using organic groups as isolation molecules. In this study, using manganese chloride and potassium halide as raw materials, all-inorganic 2D lead-free perovskites are prepared by the Bridgeman melting and cooling method. Different from the 2D perovskites synthesized by organic spacer molecules, the prepared all-inorganic 2D perovskites have smaller layer spacings and good crystallization performance due to the use of potassium halide as spacer molecules. They are direct bandgap semiconductors and their energy bandgaps are tuned by the different types of potassium halides. High degree orientation crystal thin films with (001) lattice plane parallel to silicon wafer substrate are prepared by double-source evaporation. The physical morphology of the films is characterized by grazing angle X-ray diffraction, transmission electron microscopy, and electron diffraction. The field effect transistors prepared from these 2D films show excellent electronic characteristics. The mobility of the optimized device is ≈24 cm² v⁻¹ s⁻¹ and the on/off ratio reaches 10⁵. This study reveals the potential of lead-free manganese 2D perovskite as a high-performance perovskite field effect transistor.     

A Large Bandgap Organic Salt Dopant for Sn-Based Perovskite Thin-Film Transistor

Metal halide perovskite optoelectronic devices have made significant progress over the past few years, but precise control of charge carrier density through doping is essential for optimizing these devices. In this study, the potential of using an organic salt, N,N-dimethylanilinium tetrakis(pentafluorophenyl)borate, as a dopant for Sn-based perovskite devices, is explored. Under optimized conditions, the thin film transistors based on the doped 2D/3D perovskite PEAFASnI₃ demonstrate remarkable improvement in hole mobility, reaching 7.45 cm²V⁻¹s⁻¹ with a low subthreshold swing and the smallest sweep hysteresis (ΔV_hysteresis = 2.27 V) and exceptional bias stability with the lowest contact resistance (2.2 kΩ cm). The bulky chemical structure of the dopant prevents it from penetrating the perovskite lattice and also surface passivation against Sn oxidation due to its hydrophobic nature surface. This improvement is attributed to the bifunctional effect of the dopant, which simultaneously passivates defects and improves crystal orientation. These findings provide new insights into potential molecular dopants that can be used in metal halide perovskite devices.     

Ultrahigh Energy Density of Antiferroelectric PbZrO3-Based Films at Low Electric Field

Dielectric capacitors play a vital role in advanced electronics and power systems as a medium of energy storage and conversion. Achieving ultrahigh energy density at low electric field/voltage, however, remains a challenge for insulating dielectric materials. Taking advantage of the phase transition in antiferroelectric (AFE) film PbZrO₃ (PZO), a small amount of isovalent (Sr²⁺) / aliovalent (La³⁺) dopants are introduced to form a hierarchical domain structure to increase the polarization and enhance the backward switching field E_A simultaneously, while maintaining a stable forward switching field E_F. An ultrahigh energy density of 50 J cm⁻³ is achieved for the nominal Pb_0.925La_0.05ZrO₃ (PLZ5) films at low electric fields of 1 MV cm⁻¹, exceeding the current dielectric energy storage films at similar electric field. This study opens a new avenue to enhance energy density of AFE materials at low field/voltage based on a gradient-relaxor AFE strategy, which has significant implications for the development of new dielectric materials that can operate at low field/voltage while still delivering high energy density.     

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

Lead halide perovskites have made great advance in direct X-ray detection, however the presence of toxic lead and the requirement of high working voltages severely limit their applicability and operational stability. Thus, exploring “green” lead-free hybrid perovskites capable of detecting X-rays at zero bias is crucial but remains toughly challenging. Here, utilizing chiral R/S-1-phenylpropylamine (R/S-PPA) cations, a pair of 0D chiral-polar perovskites, (R/S-PPA)₂BiI₅ ( 1 R / 1 S ) are constructed. Their intrinsic spontaneous electric polarization induces a large bulk photovoltage of 0.63 V, which acts as a driving force to separate and transport photogenerated carriers, thus endowing them with the capability of self-driven detection. Consequently, self-driven X-ray detectors with a low detection limit of 270 nGy s⁻¹ are successfully constructed based on high-quality, inch-sized single crystals of 1 R . Notably, they show suppressed baseline drift under the self-driven mode, exhibiting superior operational stability. This study realizes self-driven X-ray detection in a single-phase lead-free hybrid perovskite by exploiting the intrinsic bulk photovoltaic effect, which sheds light on future explorations of lead-free hybrid perovskites toward “green” self-driven radiation detectors with high performance.     

High-Tc Realization of Lead-Free Halide Hybrid Ferroelectrics via Steric Confinement Modulation

Hybrid organic–inorganic perovskite (HOIP) ferroelectrics with high Curie temperature (T_c), typified by the lead halide hybrid perovskite ferroelectrics, are developing rapidly owing to their maneuverable ferroelectricity at high temperatures. However, acquiring high-T_c lead-free HOIP ferroelectrics via rational strategy still needs development. In this study, a brand-new program by modulating the steric confinement in a cuplike cavity to design high-T_c bismuth-halide ferroelectrics [H₂mdap]BiX₅ (H₂mdap = N-Methyl-1,3-Propanediamine, X = Cl ( 1 ), Br ( 2 ), I( 3 )) is proposed. Emphatically, the T_c enhanced dramatically from 264 K of 3 to 318 K of 2 and 377 K of 1 , induced by the substitution of Br and Cl to I, accompanied with an interesting transition from second-order phase transition (for 3 ) to the first-order one (for 1 and 2 ). The extent of T_c increase is up to 113 K, which far outweighs that of reported Pb-halide hybrid ferroelectrics. Structural and computational analyses elucidate that this unprecedented improvement of T_c is due to the higher phase transition energy barriers induced by modulating the steric confinement of cuplike cavity via halogen substitution. These results will provide new inspiration for designing high-T_c lead-free HOIP ferroelectrics.     

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

2D chiral hybrid perovskites have recently emerged as outstanding semiconductor materials. However, most of the reported 2D chiral perovskites have limited structural types and contain high levels of toxic lead, which severely hinders their further applications. Herein, by using a mixed-cation strategy, an unprecedented type of lead-free cluster-based 2D chiral hybrid double perovskite derivatives are successfully obtained, [(R/S-PPA)₄(IPA)₆Ag₂Bi₄I₂₄]·2H₂O ( 1-R and 1-S ), and [(R/S-PPA)₄(n-BA)₆Ag₂Bi₄I₂₄]·2H₂O ( 2-R and 2-S ) (R/S-PPA=R/S–1-phenylpropylamine; IPA=isopentylamine; n-BA=n-butylamine). Their inorganic skeletons are linked by binuclear {Bi₂I₁₀} and infinite chain {Ag₂Bi₂I₁₄}_∞, in which bismuth clusters and multiple coordination modes (e.g., tetrahedral AgI₄ and octahedral AgI₆) are introduced into the double perovskite system for the first time. This introduction induces distortion of the inorganic layer, which may facilitate the transfer of chirality from the chiral cations into achiral double perovskite skeletons. Further, circular dichroism measurements and circularly polarized light detection confirm their inherent chiral optical activities. In addition, 1-S exhibits an ultralow X-ray detection limit of 129.5 nGy s⁻¹, which is 42-fold lower than that of demands in regular medical diagnosis (5.5 µGy s⁻¹). This study provides a pathway to construct novel type of lead-free cluster-based double perovskite derivatives.     

Synthesis of 0D Manganese-Based Organic–Inorganic Hybrid Perovskite and Its Application in Lead-Free Red Light-Emitting Diode

Lead-based perovskite light-emitting diodes (PeLEDs) have exhibited excellent purity, high efficiency, and good brightness. In order to develop nontoxic, highly luminescent metal halide perovskite materials, tin, copper, germanium, zinc, bismuth, and other lead-free perovskites have been developed. Here, a novel 0D manganese-based (Mn-based) organic–inorganic hybrid perovskite with the red emission located at 629 nm, high photoluminescence quantum yield of 80%, and millisecond level triplet lifetime is reported. When applied as the emissive layer in the PeLEDs, the maximum recording brightness of devices after optimization is 4700 cd m⁻², and the peak external quantum efficiency is 9.8%. The half-life of the device reaches 5.5 h at 5 V. The performance and stability of Mn-based PeLEDs are one order of magnitude higher than those of other lead-free PeLEDs. This work clearly shows that the Mn-based perovskite will provide another route to fabricate stable and high-performance lead-free PeLEDs.     

Flexible Piezoelectric Nanocomposite Generators Based on Formamidinium Lead Halide Perovskite Nanoparticles

Organic–inorganic lead halide perovskite materials have recently attracted much attention in the field of optoelectronic devices. Here, a hybrid piezoelectric nanogenerator based on a composite of piezoelectric formamidinium lead halide perovskite (FAPbBr₃) nanoparticles and polydimethylsiloxane polymer is fabricated. Piezoresponse force spectroscopy measurements reveal that the FAPbBr₃ nanoparticles contain well‐developed ferroelectric properties with high piezoelectric charge coefficient (d₃₃) of 25 pmV⁻¹. The flexible device exhibits high performance with a maximum recordable piezoelectric output voltage of 8.5 V and current density of 3.8 μA cm⁻² under periodically vertical compression and release operations. The alternating energy generated from nanogenerators can be used to charge a capacitor and light up a red light‐emitting diode through a bridge rectifier. This result innovatively expands the feasibility of organic–inorganic lead halide perovskite materials for application in a wide variety of high‐performance energy harvesting devices.     

Integrating Low-Cost Earth-Abundant Co-Catalysts with Encapsulated Perovskite Solar Cells for Efficient and Stable Overall Solar Water Splitting

Metal halide perovskite solar cells have an appropriate bandgap (1.5–1.6 eV), and thus output voltage (>1 V), to directly drive solar water splitting. Despite significant progress, their moisture sensitivity still hampers their application for integrated monolithic devices. Furthermore, the prevalence of the use of noble metals as co-catalysts for existing perovskite-based devices undermines their use for low-cost H₂ production. Here, a monolithic architecture for stable perovskite-based devices with earth-abundant co-catalysts is reported, demonstrating an unassisted overall solar-to-hydrogen efficiency of 8.54%. The device layout consists of two monolithically encapsulated perovskite (FA_0.80MA_0.15Cs_0.05PbI_2.55Br_0.45) solar cells with low-cost earth-abundant CoP and FeNi(OH)_x co-catalysts as the photocathode and photoanode, respectively. The CoP-based photocathode demonstrates more than 17 h of continuous operation, with a photocurrent density of 12.4 mA cm⁻² at 0 V and an onset potential as positive as ≈1 V versus reversible hydrogen electrode (RHE). The FeNi(OH)_x-based photoanode achieves a photocurrent of 11 mA cm⁻² at 1.23 V versus RHE for more than 13 h continuous operation. These excellent stability and performance demonstrate the potential for monolithic integration of perovskite solar cells and low-cost earth-abundant co-catalysts for efficient direct solar H₂ production.     

Field-Effect Transistors Based on Formamidinium Tin Triiodide Perovskite

To date, there are no reports of 3D tin perovskite being used as a semiconducting channel in field-effect transistors (FETs). This is probably due to the large amount of trap states and high p-doping typical of this material. Here, the first top-gate bottom-contact FET using formamidinium tin triiodide perovskite films is reported as a semiconducting channel. These FET devices show a hole mobility of up to 0.21 cm² V⁻¹ s⁻¹, an I_ON/OFF ratio of 10⁴, and a relatively small threshold voltage (V_TH) of 2.8 V. Besides the device geometry, the key factor explaining this performance is the reduced doping level of the active layer. In fact, by adding a small amount of the 2D material in the 3D tin perovskite, the crystallinity of FASnI₃ is enhanced, and the trap density and hole carrier density are reduced by one order of magnitude. Importantly, these transistors show enhanced parameters after 20 months of storage in a N₂ atmosphere.     

Solution-processed field-effect transistors based on polyfluorene –cesium lead halide nanocrystals composite films with small hysteresis of output and transfer characteristics

We have designed and investigated electrical and optical properties of solution-processed organic field-effect transistors (OFETs) based on conjugated polymer PFO and perovskite –cesium lead halide nanocrystals (CsPbI₃) composite films. It was shown that OFETs based on PFO:CsPbI₃ films exhibit current-voltage (I-V) characteristics of OFETs with dominant hole transport and saturation current behavior at temperatures 200–300 K. It was found that PFO:CsPbI₃ OFETs have a negligible hysteresis of output and transfer characteristics especially at temperatures below 250 K. The values of the hole mobility estimated from I-Vs of PFO:CsPbI₃ OFETs were found to be ∼2.4 10⁻¹ cm²/Vs and ∼1.9 10⁻¹ cm²/Vs in saturation and low fields regimes respectively at 300 K; the hole mobility dropped down to ∼6 10⁻³ cm²/Vs and 2.8 10⁻³ cm²/Vs respectively at 200 K, and then down to 5.5 10⁻⁵ cm²/Vs at 100 K (in low field regime), which is characteristic of hopping conduction. The effect of sensitivity to light and light-emitting effect were found under application of negative source-drain and gate pulse voltages to PFO:CsPbI₃ OFETs at 300 K. The mechanism of charge carrier transport in OFETs based on PFO:CsPbI₃ hybrid films is discussed.     

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.     

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.     

Multilevel Structure Engineered Lead-Free Piezoceramics Enabling Breakthrough in Energy Harvesting Performance for Bioelectronics

The prevalence of wearable/implantable medical electronics together with the rapid development of the Internet of Medicine Things call for the advancement of biocompatible, reliable, and high-efficiency energy harvesters. However, most current harvesters are based on toxic lead-based piezoelectric materials, raising biological safety concerns. What hinders the application of lead-free piezoelectric energy harvesters (PEHs) is the low power output, where the key challenge lies in obtaining a high piezoelectric voltage constant (g₃₃) and harvesting figure of merit (d₃₃ × g₃₃). Here, micron pores are introduced into phased boundary engineered high-performance (K, Na)NbO₃-based ceramic matrix, resulting in the state-of-the-art g₃₃ and the highest d₃₃ × g₃₃ values of 57.3 × 10⁻³ Vm N⁻¹ and 20887 × 10⁻¹⁵ m² N⁻¹ in lead-free piezoceramics, respectively. Concomitantly, ultrahigh energy harvesting performances are obtained in porous ceramic PEHs, with output voltage and power density of 200 V and 11.6 mW cm⁻² under instantaneous force impact and an average charging rate of 14.1 µW under high-frequency (1 MHz) ultrasound excitation, far outperforming previously reported PEHs. Porous ceramic PEHs are further developed into wearable and bio-implantable devices for human motion sensing and percutaneous ultrasound power transmission, opening avenues for the design of next-generation eco-friendly WIMEs.     

High Optical Gain of Solution-Processed Mixed-Cation CsPbBr3 Thin Films towards Enhanced Amplified Spontaneous Emission

A solution-processed thin film made of all-inorganic CsPbBr₃ perovskite is a promising candidate for low-cost and flexible green-color lasers. However, the amplified spontaneous emission (ASE) of solution-processed CsPbBr₃ films still experiences a high threshold owing to poor morphology and insufficient optical gain. Here, a multiple-cation doping strategy is demonstrated to develop compact, smooth thin films of Cs_0.87(FAMA)_0.13PbBr₃/(NMA)₂PbBr₄ (FA: formamidinium; MA: methylammonium; NMA: naphthylmethylammonium) with a record high net modal optical gain of ≈ 3030 cm⁻¹ and low propagation loss of 1.0 cm⁻¹. The FA and MA cations improve the crystallization kinetics to form continuous films, and the NMA cations reduce the grain dimension, increase film dispersibility/uniformity, and enhance spatial confinement to promote optical gain. Room-temperature ASE is demonstrated under a low threshold of ≈ 3.8  µ J cm⁻² without degradation after four months of storage in glove box or excitation by 3 × 10⁷ laser pulses. These findings provide insights into enhancing the optical gain and lowering the threshold of perovskite lasers in terms of molecular synthesis and microstructure engineering.     

Piezoelectric Nanogenerator Based on In Situ Growth All-Inorganic CsPbBr3 Perovskite Nanocrystals in PVDF Fibers with Long-Term Stability

Inorganic lead halide perovskite has become an emerging material for modern photoelectric and electronic nanodevices due to its excellent optical and electronic properties. In view of its huge dielectric and electrical properties, inorganic CsPbBr₃ perovskite is introduced into the piezoelectric nanogenerator (PENG). Based on one-step electrospinning of solutions containing CsPbBr₃ precursors and polyvinylidene difluoride (PVDF), in situ growth of CsPbBr₃ nanocrystals in PVDF fibers (CsPbBr₃@PVDF composite fibers) with highly uniform size and spatial distribution are synthesized. The CsPbBr₃@PVDF composite fibers based PENG reveals an open-circuit voltage (V_oc) of 103 V and a density of short-circuit current (I_sc) of 170  µ A cm⁻², where the V_oc is comparable to the state-of-the-art hybrid composite piezoelectric nanogenerators (PENGs) and the density of I_sc is 4.86 times higher than that of lead halide perovskites counterpart ever reported. Moreover, CsPbBr₃@PVDF composite fibers based PENG exhibits fundamentally improved thermal/water/acid–base stabilities. This study suggests that the CsPbBr₃@PVDF composite fiber is a good candidate for fabricating high-performance PENGs, promising application potentials in mechanical energy harvesting and motion sensing technologies.     

Vapor Phase Growth of Centimeter-Sized Band Gap Engineered Cesium Lead Halide Perovskite Single-Crystal Thin Films with Color-tunable Stimulated Emission

Single crystal metal halide perovskites thin films are considered to be a promising optical, optoelectronic materials with extraordinary performance due to their low defect densities. However, it is still difficult to achieve large-scale perovskite single-crystal thin films (SCTFs) with tunable bandgap by vapor-phase deposition method. Herein, the synthesis of CsPbCl_3(1–x)Br_3x SCTFs with centimeter size (1 cm × 1 cm) via vapor-phase deposition is reported. The Br composition of CsPbCl_3(1–x)Br_3x SCTFs can be gradually tuned from x = 0 to x = 1, leading the corresponding bandgap to change from 2.29 to 2.91 eV. Additionally, an low-threshold (≈23.9 µJ cm⁻²) amplified spontaneous emission is achieved based on CsPbCl_3(1–x)Br_3x SCTFs at room temperature, and the wavelength is tuned from 432 to 547 nm by varying the Cl/Br ratio. Importantly, the high-quality CsPbCl_3(1–x)Br_3x SCTFs are ideal optical gain medium with high gain up to 1369.8 ± 101.2 cm⁻¹. This study not only provides a versatile method to fabricate high quality CsPbCl_3(1–x)Br_3x SCTFs with different Cl/Br ratio, but also paves the way for further research of color-tunable perovskite lasing.