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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Contracted, Not Converted: Photoluminescence Thermochromism in Ultrabright Pure Blue Emissive Hybrid Copper(I) Halide

Thermochromic luminescent materials are promising for applications such as sensors or display technologies. Understanding the mechanism of thermochromic luminescence in these materials plays an important role for their targeted applications. Here, a 0D copper(I) halide (TMP)2CuBr3 and 1D (TMP)Ag2Br3 (TMP = tetramethylphosphonium) are reported. While (TMP)Ag2Br3 is a weak light emitter, (TMP)2CuBr3 demonstrates ultrabright pure blue emission with photoluminescence (PL) quantum yield exceeding 90% within the temperature range 300–80 K. The emission in (TMP)2CuBr3 is attributed to the radiative recombination of self-trapped excitons (STEs) that arise localized on [CuBr3]2− anions. (TMP)2CuBr3 demonstrates excitation-selective PL thermochromism at low temperatures. In the literature, the origin of multiple STEs is often unclear in luminescent metal halides. Here, a detailed temperature-dependent spectroscopic and structural analysis suggests that the PL thermochromism in (TMP)2CuBr3 is associated with the appearance of a second STE state. The appearance of second STE is expected to have a structural origin, and it may be associated with the observed anomaly in thermal contraction near 200 K. The distinct PL features of melt-processible (TMP)2CuBr3 coupled with its remarkable photo- and thermal stability allow its consideration for practical optical applications, including temperature sensing.

Popy, Dilruba [University of Oklahoma, Norman]↗
DOE OSTI2025

Full Device Evaluation of Metal Halide Perovskite Solar Cells in Low Earth Orbit Aboard the International Space Station

This study investigates how sustained low Earth orbit (LEO) exposure affects metal halide perovskite (MHP) thin films and perovskite solar cells (PSCs). It examines samples deployed on the Materials International Space Station Experiment (MISSE) 15 and 16 missions. Five methylammonium lead iodide (MAPI) thin films are deployed on MISSE-16, each with distinct UV filters to selectively attenuate AM0 spectral bands. While post-flight optical analysis reveals that the least UV-exposed film exhibits the highest emission and lowest non-radiative recombination rate, no clear correlation is observed among the rest, and all MAPI films maintained excellent integrity throughout the mission. MISSE-15 deployed eight PSCs with diverse structures, MHP compositions, and contact materials. Post-flight analysis reveals stable, highly emissive MHPs, but damaged contacts due to ion migration, which caused loss of electrical response. The MISSE missions demonstrate MHPs' suitability for space applications, while highlighting the need for improved interfacial layers and contact materials to enhance charge carrier mobility, prevent ion migration, and improve charge carrier extraction efficiency.

14 SOLAR ENERGY↗
DOE OSTI2026

Single-Particle Insights Into the Electronic Structure and Enhanced Stability of CsPbBr 3 /FAPbBr 3 Core/Crown Nanoplatelets at the Nanometer Scale

Colloidal perovskite nanoplatelets (NPLs), despite their exceptional optoelectronic properties, face significant challenges due to their intrinsic instability and trap-assisted non-radiative recombination. Although many studies employing surface engineering, such as selecting ligands or coating to passivate defects, have demonstrated improved optoelectronic properties, these enhancements are typically inferred from bulk-ensemble measurements; the effects at the single-particle level remain elusive. Here, we conduct single-particle-level studies using scanning tunneling spectroscopy (STS) on a unique core–crown system, CsPbBr 3 @FAPbBr 3 NPLs, where the lateral surfaces of the CsPbBr 3 core are coated with an FAPbBr 3 crown. Experimental density-of-states (DOS) analysis reveals a 47% reduction in deep-trap states in core-crown NPLs compared to core-only NPLs, consistent with nearly two-fold enhancements in photoluminescence quantum yields. Progressive I–V sweep measurements demonstrate superior electrical stability in core-crown NPLs, preserving band structure with minimal degradation, while core-only NPLs exhibit rapid bandgap shrinkage and trap formation. Density functional theory (DFT) calculations indicate that FA incorporation distorts Pb octahedral lattice, widening the bandgap. This study elucidates how surface engineering modulates charge localization, passivates defects, and enhances stability at the single-particle level. Moreover, by uncovering bias-induced trap states in single unpassivated NPLs, this study establishes a precise, robust approach for characterizing emerging perovskite nanocrystals.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Nanoscale Strain and Octahedral Tilting Removes Structural and Nonradiative Defects in 2D-Templated FAPbI 3

The halide perovskite formamidinium lead iodide (FAPbI 3 ) is a prime candidate for photovoltaics due to its excellent optoelectronic properties, but its application has been limited due to its structural instability. The large size of the FA cation results in metastability of the photoactive cubic phase and a facile degradation into thermodynamically stable hexagonal phases at room temperature. Recently, the incorporation of two-dimensional (2D) Ruddlesden-Popper halide perovskite seeds into a FAPbI 3 precursor solution was shown to template the growth of and stabilize cubic FAPbI 3 . Here, in this study, we investigate the nanoscale structural and optoelectronic mechanisms behind the observed bulk stabilization using synchrotron-based X-ray microscopies. Nanoprobe X-ray diffraction reveals 2D-templated FAPbI 3 films exhibit an average compressive strain normal to the substrate of -3.3%, 2-fold larger than that of MACl-stabilized FAPbI 3 . This compression creates locally templated regions composed of tetragonal-phase FAPbI 3 distributed nonuniformly throughout the film with fewer crystalline defects than purely cubic regions. Scanning X-ray excited optical luminescence (X-ray analog of photoluminescence) reveals that this local templating results in increased radiative recombination and red-shifted band edge and emission. Our results provide insight into the microscopic mechanism for the phase stabilization of FAPbI 3 using 2D perovskites as templates.

X-ray diffraction↗
DOE OSTI2024

Grain engineering for efficient near-infrared perovskite light-emitting diodes

Metal halide perovskites show promise for next-generation light-emitting diodes, particularly in the near-infrared range, where they outperform organic and quantum-dot counterparts. However, they still fall short of costly III-V semiconductor devices, which achieve external quantum efficiencies above 30% with high brightness. Among several factors, controlling grain growth and nanoscale morphology is crucial for further enhancing device performance. This study presents a grain engineering methodology that combines solvent engineering and heterostructure construction to improve light outcoupling efficiency and defect passivation. Solvent engineering enables precise control over grain size and distribution, increasing light outcoupling to ~40%. Constructing 2D/3D heterostructures with a conjugated cation reduces defect densities and accelerates radiative recombination. The resulting near-infrared perovskite light-emitting diodes achieve a peak external quantum efficiency of 31.4% and demonstrate a maximum brightness of 929 W sr -1 m -2 . These findings indicate that perovskite light-emitting diodes have potential as cost-effective, high-performance near-infrared light sources for practical applications.

42 ENGINEERING↗
DOE OSTI2024

Diamine chelates for increased stability in mixed Sn–Pb and all-perovskite tandem solar cells

Perovskite tandem solar cells show promising performance but non-radiative recombination and its progressive worsening with time, especially in the mixed Sn–Pb low-bandgap layer, limit performance and stability. Here, in this study, we find that mixed Sn–Pb perovskite thin films exhibit a compositional gradient, with an excess of Sn on the surface – and we show this gradient exacerbates oxidation and increases the recombination rate. We find that diamines preferentially chelate Sn atoms, removing them from the film surface and achieving a more balanced Sn:Pb stoichiometry, making the surface of the film resistive to the oxidation of Sn. The process forms an electrically resistive low-dimensional barrier layer, passivating defects and reducing interface recombination. Further improving the homogeneity of the barrier layer using 1,2-diaminopropane results in more uniform distribution and passivation. Tandems achieve a power conversion efficiency of 28.8%. As a result, encapsulated tandems retain 90% of initial efficiency following 1000 hours of operating at the maximum power point under simulated one-sun illumination in air without cooling.

14 SOLAR ENERGY↗
DOE OSTI2024

Two-dimensional-lattice-confined single-molecule-like aggregates

Intermolecular distance largely determines the optoelectronic properties of organic matter. Conventional organic luminescent molecules are commonly used either as aggregates or as single molecules that are diluted in a foreigner matrix. They have garnered great research interest in recent decades for a variety of applications, including light-emitting diodes, lasers and quantum technologies, among others. However, there is still a knowledge gap on how these molecules behave between the aggregation and dilution states. Here we report an unprecedented phase of molecular aggregate that forms in a two-dimensional hybrid perovskite superlattice with a near-equilibrium distance, which we refer to as a single-molecule-like aggregate (SMA). By implementing two-dimensional superlattices, the organic emitters are held in proximity, but, surprisingly, remain electronically isolated, thereby resulting in a near-unity photoluminescence quantum yield, akin to that of single molecules. Moreover, the emitters within the perovskite superlattices demonstrate strong alignment and dense packing resembling aggregates, allowing for the observation of robust directional emission, substantially enhanced radiative recombination and efficient lasing. Molecular dynamics simulations together with single-crystal structure analysis emphasize the critical role of the internal rotational and vibrational degrees of freedom of the molecules in the two-dimensional lattice for creating the exclusive SMA phase. Furthermore, this two-dimensional superlattice unifies the paradoxical properties of single molecules and aggregates, thus offering exciting possibilities for advanced spectroscopic and photonic applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

A type-I van der Waals heterostructure formed by monolayer WS 2 and trilayer PdSe 2

Two-dimensional (2D) heterostructures, formed by stacking 2D semiconductors through the van der Waals force, have been extensively studied recently. However, the majority of the heterostructures discovered so far possess type-II interfaces that facilitate interlayer charge separation. Type-I interfaces, on the other hand, confine both electrons and holes in one layer, which is beneficial for optical applications that utilize electron–hole radiative recombination. So far, only a few type-I 2D heterostructures have been achieved, which has limited the construction of multilayer heterostructures with sophisticated band landscapes. Here, we report experimental evidence of a type-I interface between monolayer WS 2 and trilayer PdSe 2 . Two-dimensional PdSe 2 has emerged as a promising material for infrared optoelectronic and other applications. We fabricated the heterostructure by stacking an exfoliated monolayer WS 2 flake on top of a trilayer PdSe 2 film, synthesized by chemical vapor deposition. Photoluminescence spectroscopy measurements revealed that the WS 2 exciton peak is significantly quenched in the heterostructure, confirming efficient excitation transfer from WS 2 to PdSe 2 . Femtosecond transient absorption measurements with various pump/probe configurations showed that both electrons and holes photoexcited in the WS 2 layer of the heterostructure can efficiently transfer to PdSe 2 , while neither type of carriers excited in PdSe 2 can transfer to WS 2 . These experimental findings establish a type-I band alignment between monolayer WS 2 and trilayer PdSe 2 . Furthermore, our results further highlight PdSe 2 as an important 2D material for constructing van der Waals heterostructures with emergent electronic and optoelectronic properties.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Enhanced charge carrier extraction and transport with interface modification for efficient tin-based perovskite solar cells

Interface modification improves charge carrier extraction in tin-based perovskite solar cells. Tin-based perovskites have become the most promising non-lead perovskites due to their ideal band gap and low toxicity. Although the open circuit voltage of tin-based perovskite solar cells (TPSCs) continues to approach the theoretical value, the short-circuit current is still far from the theoretical value. Here, we describe an interface modification method by regulating the property of hole transport layer, PEDOT:PSS, which improves the surface molecular morphology and the energy level alignment of PEDOT:PSS/perovskite interface. Advanced GIWAXS and IR s-SNOM characterization are conducted to achieve multi-dimensional characterization of nanoscale surface morphology and chemical distribution of PEDOT:PSS. With the multi-attribute optimization, charge carrier extraction and non-radiative recombination are also improved. The resultant TPSCs exhibit a higher power conversion efficiency of 13.32% in compared with the control device of 10.50%, accompanied with an increase in the short-circuit current from 18.10 to 20.50 mA cm −2 and FF from 68.23% to 76.43%. This work demonstrates a reliable strategy for improving charge carrier extraction and device performance for lead-free TPSCs.

Zhao, Zhenzhu↗
DOE OSTI2025

Optimizing 2D passivation for enhancing performance of fully air-processed carbon electrode-based perovskite solar cells

Air-processed carbon-based perovskite solar cells (C-PSCs) offer scalable and cost-effective photovoltaic manufacturing but face efficiency loss compared to metal-contact perovskite solar cells. Surface passivation of three-dimensional (3D) perovskites with two-dimensional (2D) perovskite layers has emerged as a promising strategy to enhance device performance. However, the mechanisms by which 2D perovskites more effectively improve C-PSC efficiency and stability remain underexplored. This study investigates the efficacy of 2D/3D heterostructures using n-hexylammonium bromide (C6Br), phenethylammonium iodide (PEAI), and n-octylammonium iodide (OAI) as surface passivators for C-PSCs. C-PSCs treated with C 6 Br achieved a champion power conversion efficiency (PCE) of 21.0%. This enhancement is attributed to superior defect passivation, improved charge extraction, and suppressed non-radiative recombination. Transient ion-drift characterization demonstrates that C 6 Br and OAI reduce ionic conductivity by 2–3 orders of magnitude, correlating with enhanced operational stability under continuous illumination. Our findings highlight the role of short-chain bromide cations (C 6 Br) in optimizing halide-mediated defect healing and interfacial band alignment, positioning 2D-passivated C-PSCs as viable competitors to conventional metal-contact perovskite solar cells.

14 SOLAR ENERGY↗
DOE OSTI2026

Thin Film Synthesis of SrZn2P2 with SrI2 Post-Annealing for Enhanced Crystallinity and Optoelectronic Quality

Ternary Zintl phosphides are promising light-absorbing semiconductors for thin-film optoelectronic applications, but strategies for controlling their microstructure and optoelectronic quality remain underexplored. Here, we report the synthesis of phase-pure SrZn2P2 thin films using radio-frequency co-sputtering in a PH3 + Ar atmosphere and investigate the impact of post-growth processing on their structural and optical properties. Grazing-incidence X-ray scattering and Raman spectroscopy confirm the formation of crystalline SrZn2P2 films over a finite compositional window. Optical measurements reveal clear absorption near the direct-band-gap energy (~1.8 eV) and near-band-edge photoluminescence. Further, we have studied the effects of chemically compatible halide-assisted annealing. It is found that SrI2 treatments lead to pronounced grain growth and reduced diffraction peak broadening while preserving phase purity, in contrast to rapid thermal or forming-gas annealing. Notably, annealing with SrI2 at 450 degrees C significantly enhances both the intensity and spatial uniformity of the photoluminescence, thus connecting the observed microstructural consolidation with improved radiative recombination. Our study demonstrates that halide-assisted annealing provides an effective pathway for microstructural control in SrZn2P2 thin films and highlights a generalizable processing strategy for advancing Zintl phosphide semiconductors toward optoelectronic applications.

14 SOLAR ENERGY↗
DOE OSTI2025

Thermoradiative energy conversion in infrared interband cascade InAs/GaSb/AlInSb/GaSb type-II superlattice diodes

Thermoradiative energy conversion presents a means for the direct conversion of thermal energy through radiative transfer to a cold scene. However, much of the study of thermoradiative principles has been based on theory and simulations, with only sparse reports on the experimental demonstration of the concept. This work studies thermoradiative energy conversion in InAs/GaSb/AlInSb/GaSb type-II superlattice cascade devices. The devices exhibit a cutoff wavelength of 3.2 μm at 300 K, corresponding to a bandgap of 0.39 eV. Testing under a temperature-controlled chamber and scene demonstrates a maximum power density of 2.9 mW/m2 at a cell temperature of 121 °C. It is consistent with expected values for device operation limited by Shockley–Read–Hall non-radiative recombination. This result is a significant step in providing an experimental demonstration of thermoradiative energy conversion and a means to characterize cell performance, providing a foundation for further development to achieve practical values for power generation.

Islam, Md Toriqul (ORCID:0000000249871320)↗
DOE OSTI2025

The effects of antimony incorporation on the optoelectronic properties of Cd(Se,Te) photovoltaics

One historical limitation of CdTe PV devices has been the open circuit voltage (VOC) deficit (difference between theoretical maximum VOC and measured values). While non-radiative recombination at extended structural defects and interfaces negatively impacts VOC, intentionally adding impurities (dopants) to increase the concentration of free carriers in the photovoltaic (PV) absorber material can increase the VOC. In this contribution we present a detailed analysis of the Sb doped CdTe and the Cd(Se,Te) alloy system via electron beam induced current (EBIC) measurements and the presence as well as spatial distribution of defect levels through cathodoluminescence spectrum imaging (CLSI).

14 SOLAR ENERGY↗
DOE OSTI2026

Incident excitation effects on ZnO-based photoluminescence

Zinc oxide (ZnO) is an attractive semiconductor material owing to a wide band gap, large exciton binding energy, and strong luminescent properties. Two distinct spectral regions are present in the room temperature emission of this material: a narrow line in the UV/near-UV region that is excitonic in nature and a lower energy broad emission band centered in the green/yellow region. Commercially available ZnO particles containing excess Zn and oxygen vacancy defect sites (referred to as ZnO:Zn) were excited using three light sources to study different radiative recombination regimes of the as-received powders. First, a UV LED at a center wavelength of 365 nm provided low irradiance (0.02–0.08 W/cm 2 ) with varying pulse widths (continuous operation to 16 ns). Second, the third harmonic of a pulsed Nd:YAG laser provided high irradiances (∼10 4 –10 6 W/cm 2 ) at a fixed nominal pulse width of 5 ns. Finally, a continuous polychromatic synchrotron X-ray source was also used to excite the ZnO:Zn powders. During UV LED excitation, a low number of carriers are created in the material, leading to an anticipated linear relationship between luminescence and irradiance. This held true for defect luminescence; however, there was an observed enhancement of exciton emission relative to the UV LED intensity as the pulse width was decreased, independent of irradiance. During UV laser excitation, the number of carriers was significantly increased, raising the material into a bimolecular recombination regime, which produced exciton emission much stronger than visible band emission. Finally, spectra obtained during synchrotron X-ray excitation, whose continuous illumination and higher penetration depth yielded higher emission from defect sites relative to exciton emission. A redshift in the exciton emission was also observed as excitation pulse width and sample temperature were varied, and is discussed.

Westphal, Eric Robert [Sandia National Lab. (SNL-N↗
DOE OSTI2026

Solutions to Droop and the Green Gap by Novel Carrier Injection

Long-wavelength (green, yellow, red) visible light-emitting diodes (LEDs) have historically been inefficient compared to blue light-emitters in the III-nitrides. This is due to many factors, including poor material quality due to the low growth temperatures required for high Incomposition InGaN quantum wells (QWs), and the polar nature of the III-nitride crystal structure. Spontaneous and piezoelectric polarization in the III-nitrides causes enhanced quantum-confined Stark effect (QCSE), which spatially separates electrons and holes and reduces radiative recombination (ie: light output) from the devices. Polarization in the crystal also induces additional potential barriers that electrons and holes must cross over before entering the QWs where they can recombine to emit light. Both of these polarization effects worsen as emission wavelength increases, making blue III-nitride LEDs are the most efficient and red III-nitride LEDs the least efficient. The focus of this project has been solving the latter polarization-related issue through the implementation of V-defects in long wavelength LEDs. V-defects are morphological defects which are commonly observed in c-plane III-nitrides. They are observed as hexagonal pyramid-shaped depressions on the c-plane surface, with six semipolar sidewalls. They typically form at the apex of threading dislocations (TDs) under conditions of kinetically-limited growth and low growth-temperature. They were initially thought to be detrimental to LED performance and much early work focused on eliminating them entirely from III-nitride devices. However, over the past decade work has emerged that indicate that they can improve LED performance by allowing electrons and holes to bypass the polarization-induced barriers present in the c-plane and directly enter the QWs of an LED. This is due to the semipolar nature of the V-defect sidewall: these sidewalls are thin and lack the polarization-induced barriers which prevent carriers easily moving between layers. V-defects have since been determined to be an efficient avenue by which to inject electrons and holes into the c-plane QWs where they can recombine to emit light. Throughout this project we have explored lateral injection through a variety of methods: simulation (Task 2), epitaxial growth of V-defect and non-V-defect LEDs (Tasks 1, 3, 4, 5, 6), and advanced characterization methods (Task 7). All tasks have been completed. A description of each task completed follows from this section.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2025

The Influence of Structural Dynamics in Two-Dimensional Hybrid Organic–Inorganic Perovskites on Their Photoluminescence Efficiency — Neutron Scattering Analysis

Two-dimensional hybrid organic–inorganic perovskites (HOIPs) have emerged as promising materials for light-emitting diode applications. In this study, by using time-of-flight neutron spectroscopy we identified and quantitatively separated the lattice vibrational and molecular rotational dynamics of two perovskites, butylammonium lead iodide (BA)2PbI4 and phenethyl-ammonium lead iodide (PEA) 2 PbI 4 . By examining the corresponding temperature dependence, we found that the lattice vibrations, as evidenced by neutron spectra, are consistent with the lattice dynamics obtained from Raman scattering. We revealed that the rotational dynamics of organic molecules in these materials tend to suppress their photoluminescence quantum yield (PLQY) while the vibrational dynamics did not show predominant correlations with the same. Additionally, we observed photoluminescence emission peak splitting for both systems, which becomes prominent above certain critical temperatures where the suppression of PLQY begins. This study suggests that the rotational motions of polarized molecules may lead to a reduction in exciton binding energy or the breaking of degeneracy in exciton binding energy levels, enhancing non-radiative recombination rates, and consequently reducing photoluminescence yield. These findings offer a deeper understanding of fundamental interactions in 2D HOIPs and could guide the design of more efficient light-emitting materials for advanced technological applications.

Rajeev, Haritha Sindhu [Univ. of Virginia, Charlot↗
DOE OSTI2025

Effect of growth dynamics on the structural, photophysical and pseudocapacitance properties of famatinite copper antimony sulphide colloidal nanostructures (including nanosheets)

Facile phase selective synthesis of copper antimony sulphide (CAS) nanostructures is important because of their tunable photoconductive and electrochemical properties. In this study, off-stoichiometric famatinite phase CAS (fCAS) quasi-spherical and quasi-hexagonal colloidal nanostructures (including nanosheets) of sizes, 2.4–18.0 nm were grown under variable conditions of temperature (60–200 °C), time and oleylamine capping ligand concentration using copper(II) acetylacetonate and antimony(III) diethyldithiocarbamate precursors. Data from powder X-ray diffraction, Raman spectroscopy and high-resolution scanning/transmission electron microscopy confirm the tetragonal structure of the famatinite phase. X-ray photoelectron spectroscopy, transmission electron microscopy and scanning electron microscopy-energy dispersive X-ray spectroscopy data suggest a correlation of particle size, morphology and composition of the off-stoichiometric fCAS nanostructures with growth temperature and time, and oleylamine concentration. The off-stoichiometric Cu 3-a Sb 1+b S 4±c (a, b, c – mole fractions) nanostructures being severely copper-deficient and antimony-rich, exhibit shallow-lying acceptor copper vacancy states, deep-lying donor states of antimony interstitials, sulphur vacancies and antimony-copper antisites and shallow-lying acceptor surface trapping states. Further, these electronic states are likely implicated in tunable UV-visible absorption and bandgaps between 2.3 and 2.8 eV, and broad visible-NIR photoluminescence with fast recombination of radiative lifetimes between 0.2 and 6.2 ns, confirmed from absorption, steady-state and time-resolved photoluminescence spectroscopies. Additionally, cyclic voltammetry and electrochemical impedance spectroscopy confirm that electrodes of the fCAS nanostructures display slightly variable pseudocapacitance of charge-storage primarily via possible sodium ion intercalation with a high specific capacitance of ~84 F g -1 obtained at a scan rate of 5 mV s -1 . Overall, these results show the influence of composition, in particular point defects, phase quality and morphology on the optical and pseudocapacitance properties of fCAS nanostructures, suitable as solar absorbers or electrodes for energy storage devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Unveiling the role of halide mixing in the crystallization kinetics and charge transfer mechanisms of wide-bandgap organic–inorganic halide perovskites

Understanding the crystallization kinetics of Br–I mixed-halide WBG perovskite films, and their correlation to the crystallographic structure and charge transfer dynamics, is critical for advancing WBG perovskite devices. Despite many efforts to increase the photovoltaic performances of wide-bandgap (WBG, with a Br content above 20%) perovskite solar cells based on bromine–iodine (Br–I) mixed-halide perovskites, understanding the crystallization kinetics of WBG perovskite films, as well as the role of Br mixing in the crystallization kinetics, is still lacking. Furthermore, an overlooked aspect is the correlation of the halide compositions, crystallization kinetics, crystallographic structure, and charge transfer dynamics. Here, we unveil that Br–I mixed-halide WBG perovskite films undergo two intrinsically different crystallization kinetic processes. One is the intermediate solvent-complex phase-assisted growth (I-rich), and the other is top-to-bottom downward growth (Br-rich). Such downward growth (including high Br concentrations) correlates with the formation of a highly vertically oriented perovskite film, which is accompanied by defect formation caused by a dissolving and recrystallization process coupled with halide homogenization. Consequently, Br-rich WBG perovskite films exhibit enhanced charge carrier transport, but are concurrently plagued by non-radiative charge recombination. Addressing this fundamental perspective is critical to precisely tailor Br-related crystallization, which significantly affects the structure and optoelectronic properties of WBG perovskite films and devices.

Li, Nian↗