Pure Perovskites Research Articles

Effects of adding copper to bismuth titanate for photocatalytic hydrogen production

In this work, pure and copper-doped bismuth titanate perovskites were synthesized using the modified amorphous citrate method to evaluate the influence of the dopant on the material's structure and its efficiency as a catalyst. X-ray diffraction method has been employed for the analysis of the crystal structure while scanning electron microscopy (SEM) and transmission electron microscopy (TEM) techniques were used to examine the material's morphology. Electron dispersion spectroscopy (EDS) was also employed to confirm the doping of the material. The doped material exhibited a bandgap within the visible region calculated using the Tauc plot from UV-Vis diffuse reflectance spectroscopy. The dopant influenced the emergence of secondary bandgaps with considerably lower values than the pure materials, directly impacting the photocatalytic performance of hydrogen gas (H2) production. The highest H2 gas production occurred in the doped and more crystalline sample. Comparing these results with other studies, it can be concluded that copper is a metal with great potential as a dopant for the development of bismuth titanate-based catalysts.

Blue Light-Emitting Diodes Based on Pure Bromide Perovskites.

Blue perovskite light-emitting diodes (LEDs) are essential for the creation of full-color displays and white-light illumination, and some significant progress is made in recent years. However, most high-performance blue perovskite LEDs are currently based on mixed-halide perovskites and suffer from unstable spectra due to inevitable halide phase segregation, which is unfavorable for the application of blue perovskite LEDs. In contrast, blue emissions from pure bromide perovskites generally exhibit stable spectra (consistent emission peak positions and spectral shapes) and are worthy of attention. In this review, the recent advances in blue LEDs based on pure bromide perovskites according to different strategies are classified and summarized. Moreover, the challenges related to poor charge injection, high defect-state density, lack of high-performance in the deeper blue region, and inferior operational stability are addressed. Finally, an outlook is provided on feasible future research directions for highly bright, efficient, and stable blue perovskite LEDs.

Preparation and surface photovoltage regulation of (Cs/MA)3Bi2I9 double A-site cation mixed-phase perovskite nanocrystal structure

This paper reports a novel (Cs/MA)3Bi2I9 double A-site cations perovskite nanostructured photoelectrode and its fabrication method, utilizing a stoichiometric dissolution of MAI, CsI, and BiI3 solutes in DMF solvent. The (Cs/MA)3Bi2I9 perovskite electrodes are then prepared on FTO glass substrates using the spin-coating technique. Furthermore, by adjusting the molar ratio x of Cs+ to the total moles of Cs+ and MA+ in precursor, the morphology and size of the (Cs/MA)3Bi2I9 perovskite nanostructures can be effectively modulated, thereby tuning their photoelectrical properties. (Cs/MA)3Bi2I9 consists of two phases: (CsMA)3Bi2I9 formed by substituting Cs+ with MA+, and (MACs)3Bi2I9 formed by substituting MA+ with Cs+. The surface photovoltage performance of the (Cs/MA)3Bi2I9 perovskites prepared at different x values surpasses that of pure MA3Bi2I9 and Cs3Bi2I9 bismuth-based perovskites. Particularly noteworthy is that at x = 0.6, the surface photovoltage performance of (Cs/MA)3Bi2I9 perovskite is nearly double that of the pure MA3Bi2I9 and Cs3Bi2I9 perovskites.

Dynamics of glassy state in MAPbBr3-xClx mixed lead halide perovskites

Mixed lead halide perovskites have shown remarkable performance in photovoltaic and optoelectronic applications. Pure hybrid halide perovskites undergo clear phase transitions, however, the phase transitions in mixed perovskites are less studied. We present a contrasting behavior of the phase transition dynamics of MAPbBr3-xClx (MA = CH3NH3+) mixed halide perovskites compared to the pure MAPbX3 (X = Cl, Br) counterparts, which typically exhibit order-disorder phase transitions through a series of distinct structural phases. We have employed several spectroscopic techniques including temperature-dependent PXRD, Raman, dielectric and Brillouin spectroscopy. The results demonstrate that the mixed halide perovskite MAPbBr1.5Cl1.5 does not undergo any structural phase transition typically observed in pure halide perovskites. We observed signatures of glassy behavior in mixed compositions of this system. In addition, we also explored the effects of replacing A-site cation on the phase transition behaviors. The results contribute to the understanding of phase transition mechanisms in perovskites and have implications for their stability and optoelectronic properties.

Lead-Free Cs2AgBiCl6 Double Perovskite: Experimental and Theoretical Insights into the Self-Trapping for Optoelectronic Applications.

Lead-free double perovskites (DPs) will emerge as viable and environmentally safe substitutes for Pb-halide perovskites, demonstrating stability and nontoxicity if their optoelectronic property is greatly improved. Doping has been experimentally validated as a powerful tool for enhancing optoelectronic properties and concurrently reducing the defect state density in DP materials. Fundamental understanding of the optical properties of DPs, particularly the self-trapped exciton (STEs) dynamics, plays a critical role in a range of optoelectronic applications. Our study investigates how Fe doping influences the structural and optical properties of Cs2AgBiCl6 DPs by understanding their STEs dynamics, which is currently lacking in the literature. A combined experimental-computational approach is employed to investigate the optoelectronic properties of pure and doped Cs2AgBiCl6 (Fe-Cs2AgBiCl6) perovskites. Successful incorporation of Fe3+ ions is confirmed by X-ray diffraction and Raman spectroscopy. Moreover, the Fe-Cs2AgBiCl6 DPs exhibit strong absorption from below 400 nm up to 700 nm, indicating sub-band gap state transitions originating from surface defects. Photoluminescence (PL) analysis demonstrates a significant enhancement in the PL intensity, attributed to an increased radiative recombination rate and higher STE density. The radiative kinetics and average lifetime are investigated by the time-resolved PL (TRPL) method; in addition, temperature-dependent PL measurements provide valuable insights into activation energy and exciton-phonon coupling strength. Our findings will not only deepen our understanding of charge carrier dynamics associated with STEs but also pave the way for the design of some promising perovskite materials for use in optoelectronics and photocatalysis.

La-based Transition Metal Oxide Perovskites as Electrocatalysts for Electrochemical Carbon Dioxide Reduction

We report here the feasibility of using LaTMO3-based perovskites (TM = Co, Cr, Fe, Mn, Ni, i.e., non-Cu 3d transition metals) as electrocatalysts for electrochemical CO2 reduction reaction (eCO2RR). Phase pure LaTMO3 perovskites, having TM-ions in multiple oxidation states for all and O-defects for LaFeO3 and LaNiO3, have been synthesized and tested as electrocatalysts for eCO2RR in flow cell type set-up. The above characteristics of the La-TM-oxides have been found to influence the current densities during eCO2RR at the various applied potentials, with favorable effects of the presence of O-defects (as for LaFeO3 and LaNiO3). Upon eCO2RR, both C1 and C2 liquid products have been obtained, including ethanol, with a partial current density of −2.66 mA cm−2 at −1.2 V vs RHE (for LaFeO3). The types of products and the faradic efficiencies have been found to depend on the TM-ion present (in the LaTMO3); in particular, the oxidation state(s), associated O-defect(s) and electronic conductivity. Furthermore, the electrocatalysts have been found to be stable during eCO2RR. Overall, the present work highlights the potential of La-TM-oxide perovskites for usage as stable electrocatalysts for eCO2RR, and also provides insights into the proper selection of “TM” and reaction conditions for obtaining the desired product(s).

Alloy [FA,Cs]PbI3 perovskite surfaces: The role of surface cesium composition in stability and tolerance to defect formation

Halide-perovskite alloys that include cesium have achieved records of stability and efficiency in solar cells. Controlling the surface composition, defects, and electronic properties guarantees interface stability and improves performance. By using density functional theory and molecular dynamic simulations, we analyzed which surface compositions of the formamidinium (FA) and cesium (Cs) lead iodide perovskite FA1−xCsxPbI3 with 25 and 50% of Cs become more stable than pure perovskites. Structural and electronic properties and tolerance to defect formation were also evaluated. Surface energy calculations show that only the alloys with 25% Cs and FAI-enriched surfaces are more stable than pure FAPbI3 ones. The most stable alloy surface shows electronic energy levels similar to the FAPbI3 perovskite, suggesting that this alloy may also be efficient for charge transport in the cell. However, the presence of Cs on the alloy surface, although low, favors the formation of FAI vacancies, which is detrimental to the stability of the perovskite. These results suggest evaluating FA1−xCsxPbI3 alloys with small Cs compositions to mitigate the formation of defects or using a passivation scheme. This study delivers valuable information for efficiency device improvement from the perspective of interface stability.

Significance of Formamidinium Incorporation in Perovskite Composition and Its Impact on Solar Cell Efficiency: A Mini‐Review

Perovskite solar cells (PSCs) have gained tremendous research interest recently owing to several advantages, including low material cost, facile solution processability, bandgap tunability, and alluring device efficiency. The organic formamidinium (FA) cation‐based perovskites are mainly considered as one of the potential candidates for charge carrier generation due to their excellent properties, such as bandgap and thermal stability than traditional perovskites. However, the inevitable unfavorable polymorphism (i.e., α to δ) at room temperature still forms the basis for numerous research works to allow the fabrication of a high‐quality absorber and enhances the PSCs performance. The studies to resolve the polymorphism and several contemporary techniques (e.g., passivation strategy) with several recent novel fabrication methods presented in this review form the essence of the improvements in PSCs. The absorber morphology also influences the charge‐transfer behavior and the device's lifetime. Therefore, understanding these properties is essential to improve the absorber quality and avoid many defects. This review focuses on the structure and properties of pure and mixed FA perovskites with various halides, mainly the FA cation's role in the absorber composition. And a comprehensive overview of recent FA cation‐based double, triple, and quadrupole PSCs results with proper scientific explanations to understand the device physics.

Impact of photoinduced phase segregation in mixed-halide perovskite absorbers on their material and device stability

Mixed-halide perovskites enable bandgap engineering for tandem solar cell and light-emitting diode applications. However, photoinduced halide phase segregation introduces a compositional instability, that is, formation of I-rich and Br-rich phases, which compromises photovoltaic efficiency and stability. While optical and structural studies of the photoinduced phase segregation in mixed-halide perovskites have been reported, its impact on the material stability is missing. Here, a detailed compositional analysis of mixed-halide perovskite films using x-ray and ultraviolet photoelectron spectroscopy (UPS) was carried out to determine how their stability in various environments depends on the halide ratio. A series of perovskite thin films were fabricated with the composition CH3NH3Pb(IxBr1−x)3, where x = 0.00, 0.25, 0.50, 0.75, and 1.00, and analyzed under different conditions, such as exposure to light in ambient and in nitrogen atmosphere, as well as storage in the dark. From the spectroscopy results, complemented with structural and optical properties, it was found that the deletion of halide ions from the surface is facilitated in mixed-halide perovskites in comparison with pure halide perovskites. A higher stability was found for the mixed-halide perovskite containing less than 25% Br, and it decreases with increasing Br content. This study also established the effect of the Br/I ratio on the energy landscape of the materials. The UPS spectra reveal that photoinduced degradation results in a mismatch of the energy levels at the perovskite/transport layer interface, which may limit the collection of charge carriers. These findings correlate well with the photovoltaic device stability under similar degradation conditions.

Synergetic Near- and Far-Field Plasmonic Effects for Optimal All-Perovskite Tandem Solar Cells with Maximized Infrared Absorption.

The efficiency and reliability of perovskite solar cells have rapidly increased in conjunction with the proposition of advanced single-junction and multi-junction designs that allow light harvesting to be maximized. However, Sn-based compositions required for optimized all-perovskite tandem devices have reduced absorption coefficients, as opposed to pure Pb perovskites. To overcome this, we investigate near- and far-field plasmonic effects to locally enhance the light absorption of infrared photons. Through optimization of the metal type, particle size, and volume concentration, we maximize effective light harvesting while minimizing parasitic absorption in all-perovskite tandem devices. Interestingly, incorporating 240 nm silver particles into the Pb-Sn perovskite layer with a volume concentration of 3.1% indicates an absolute power conversion efficiency enhancement of 2% in the tandem system. We present a promising avenue for experimentalists to realize ultrathin all-perovskite tandem devices with optimized charge carrier collection, diminishing the weight and the use of Pb.

Element Regulation and Dimensional Engineering Co-Optimization of Perovskite Memristors for Synaptic Plasticity Applications.

Capitalizing on rapid carrier migration characteristics and outstanding photoelectric conversion performance, halide perovskite memristors demonstrate an exceptional resistive switching performance. However, they have consistently faced constraints due to material stability issues. This study systematically employs elemental modulation and dimension engineering to effectively control perovskite memristors with different dimensions and A-site elements. Compared to pure 3D and 2D perovskites, the quasi-2D perovskite memristor, specifically BA0.15MA0.85PbI3, is identified as the optimal choice through observations of resistive switching (HRS current < 10-5 A, ON/OFF ratio > 103, endurance cycles > 1000, and retention time > 104 s) and synaptic plasticity characteristics. Subsequently, a comprehensive investigation into various synaptic plasticity aspects, including paired-pulse facilitation (PPF), spike-variability-dependent plasticity (SVDP), spike-rate-dependent plasticity (SRDP), and spike-timing-dependent plasticity (STDP), is conducted. Practical applications, such as memory-forgetting-memory and recognition of the Modified National Institute of Standards and Technology (MNIST) database handwritten data set (accuracy rate reaching 94.8%), are explored and successfully realized. This article provides good theoretical guidance for synaptic-like simulation in perovskite memristors.

ZIF-8@CsPbBr3 Nanocrystals Formed by Conversion of Pb to CsPbBr3 in Bimetallic MOFs for Enhanced Photocatalytic CO2 Reduction.

Perovskite nanocrystals are embedded into metal-organic frameworks (MOFs) to create composites with high light absorption coefficients, tunable electronic properties, high specific surface area, and metal atom tunability for enhanced photocatalytic carban dioxide (CO2) reduction. However, existing perovskite-MOF structures with a large particle size are achieved based on Pb source adsorption into the pores of MOFs, which can significantly break down the porous structure, thereby resulting in a decreased specific surface area and impacting CO2 adsorption. Herein, a novel perovskite-MOF structure based on the synthesis of bimetallic Pb-containing MOFs and post-processing to convert Pb to CsPbBr3 nanocrystals (NCs) is proposed. It is discovered that the additional Pb is not introduced by adsorption, but instead engages in coordination and generates Pb-N. The produced ZIF-8@CsPbBr3 NCs are ≈40nm and have an ultra-high specific surface area of 1325.08 m2g-1, and excellent photovoltaic characteristics, which are beneficial for photocatalytic CO2 reduction. The electronic conversion rate of composites is 450mol g-1h-1, which is more than three times that of pure perovskites. Additionally, the superior reduction capacity is sustained after undergoing four cycles. Density Functional Thoery (DFT) simulations are used to explore the 3D charge density at the ZIF-8@CsPbBr3 NCs interface to better understand the electrical structure.

Deep insight into structural and optoelectronic properties of mixed anion perovskites

Abstract Here we present the optoelectronic properties of pure inorganic lead-free halide perovskites in the form of Cs2AgBiX 6 (X = Br, Cl, F, I) using the density functional theory calculations on cubic phase (Fm 3 ̅ m) and tetragonal phase (I4/m). First, all the structures of the two phases were optimized at the PBE level. Structural, electronic, optical properties, phonon, and thermal properties of Cs2AgBiX 6 in cubic (Fm 3 ̅ m) and tetragonal phases (I4/m) were obtained using the VASP code. Tetragonal phases of all compounds of the form Cs2AgBiX 6, except Cs2AgBiBr6, are reported here for the very first time. Among all the Cs2AgBiX 6 (X = F, Cl, Br, I) structures, the cubic phase of Cs2AgBiBr6 was seen to have the highest absorption coefficient along with prominent electronic features that are favorable for optoelectronic applications. Thus, the cubic phase of Cs2AgBiBr6 was selected as the host lattice and bromine atoms were partly replaced with chlorine and iodine atoms. Electronic and optical properties of these mixed halide compounds of Cs2AgBiBr6−xFx, Cs2AgBiBr6−xClx, and Cs2AgBiBr6−xIx where x = 1, 2, 3, 4, 5 are investigated with hybrid functional HSE06 level. The electronic structure revealed that these mixed compounds exhibited indirect band gap nature regardless of the halide substitution (different x concentration) and the band gap of Cs2AgBiBr6 could be varied with the substitutions of fluorine, chlorine, and iodine atoms. Our in-depth analysis shows that Cs2AgBiBr6 and their mixed halides have the potential to become active double perovskite materials for photovoltaic applications and as photocatalysts for water splitting.

All-inorganic lead halide perovskites for photocatalysis: a review.

Nowadays, environmental pollution and the energy crisis are two significant concerns in the world, and photocatalysis is seen as a key solution to these issues. All-inorganic lead halide perovskites have been extensively utilized in photocatalysis and have become one of the most promising materials in recent years. The superior performance of all-inorganic lead halide perovskites distinguish them from other photocatalysts. Since pure lead halide perovskites typically have shortcomings, such as low stability, poor active sites, and ineffective carrier extraction, that restrict their use in photocatalytic reactions, it is crucial to enhance their photocatalytic activity and stability. Huge progress has been made to deal with these critical issues to enhance the effects of all-inorganic lead halide perovskites as efficient photocatalysts in a wide range of applications. In this manuscript, the synthesis methods of all-inorganic lead halide perovskites are discussed, and promising strategies are proposed for superior photocatalytic performance. Moreover, the research progress of photocatalysis applications are summarized; finally, the issues of all-inorganic lead halide perovskite photocatalytic materials at the current state and future research directions are also analyzed and discussed. We hope that this manuscript will provide novel insights to researchers to further promote the research on photocatalysis based on all-inorganic lead halide perovskites.

Phase distribution regulation of formamidinium-based quasi-2D perovskites through solution engineering.

Quasi-2D perovskites have attracted attention as potential solar energy absorber materials due to their balanced efficiency and stability and their unique quantum-well structures. In order to facilitate directional excitons and charge carrier transport and preferential energy transfer landscape in photovoltaic thin films, the phase distribution formed by different types of microstructural domains should be regulated. In this work, the Dion-Jacobson-type spacer 1,4-phenylenedimethanammonium (PDMA) was used, and different strategies were pursued to control the phase distribution in formamidinium-based (FA) quasi-2D perovskites based on the composition of (PDMA)FA4Pb5I16. In general, doping with FACl modulated the crystallization kinetics, forming 2D low-n crystals on the top surface or a reversed-gradient phase distribution, depending on whether excess or substitutional doping was employed. Alternatively, mixing with a Ruddlesden-Popper spacer helped bridging to adjacent octahedra in pure PDMA-based perovskites and improved crystallization, while regulating the quantum-well structures to give a normal-gradient phase distribution, where 2D domains resided on the bottom side. By combining FACl doping and spacer mixing, the film showed both a reversed-gradient phase distribution and larger vertically aligned grains. This work contributes to the knowledge of how to manipulate and regulate the phase distribution in FA-based quasi-2D perovskites and further paves the way for fabricating corresponding devices with high efficiency and stability.

Copper Modulated Lead‐Free Cs4MnSb2Cl12 Double Perovskite Microcrystals for Photocatalytic Reduction of CO2

AbstractIn order to deal with the global energy crisis and environmental problems, reducing carbon dioxide through artificial photosynthesis has become a hot topic. Lead halide perovskite is attracted people's attention because of its excellent photoelectric properties, but the toxicity and long‐term instability prompt people to search for new photocatalysts. Herein, a series of &lt;111&gt; inorganic double perovskites Cs4Mn1‐xCuxSb2Cl12 microcrystals (x = 0, 0.1, 0.2, 0.3, 0.4, and 0.5) are synthesized and characterized. Among them, Cs4Mn0.7Cu0.3Sb2Cl12 microcrystals have the best photocatalytic performance, and the yields of CO and CH4 are 503.86 and 68.35 µmol g−1, respectively, after 3 h irradiation, which are the highest among pure phase perovskites reported so far. In addition, in situ Fourier transform infrared (FT‐IR) spectroscopy and electron spin resonance (ESR) spectroscopy are used to explore the mechanism of the photocatalytic reaction. The results highlight the potential of this class of materials for photocatalytic reduction reactions.

On the Origin of Energetic Disorder in Mixed Halides Lead Perovskites

AbstractMixed halide perovskites are emerging as promising candidates for wide‐bandgap components in tandem solar cells and color‐tunable light‐emitting diodes. Yet, halide mixing poses a fundamental question of whether the inhomogeneous halide distribution impacts the intrinsic electronic disorder in these materials. To address this point, density functional theory (DFT)‐based molecular dynamics (MD) simulations are performed for pure and mixed halide perovskites, accounting for disorder stemming from inhomogeneous chemical composition associated with the halide component and from finite temperature effects. For pure halide perovskites, finite‐temperature band gap fluctuations from the MD simulations are in good agreement with the broadening measured using photoluminescence. Furthermore, these calculations confirm the natively modest inhomogeneous disorder in the electronic structure of these materials. Most notably, such a low degree of electronic disorder is preserved in models mimicking finely intermixed Br/I solid‐state solutions. In contrast, models featuring halide segregation show comparably wider band gap fluctuations, with a sizable contribution from inhomogeneous (static) broadening, which is associated, at least in part, with structural distortions stemming from lattice mismatch.

Structural analysis and photocatalytic activities of bismuth-lanthanide oxide perovskites

A series of pure bismuth-lanthanide oxide perovskites of the formula of BiLnO3 (Ln = Sm, Eu, Tb, Er and Ho) has been synthesized via simple sol-gel methods. The elemental compositions and valence states of these materials were confirmed by X-ray photoelectron spectroscopy (XPS). Powder X-ray diffraction spectroscopy (PXRD) revealed an isostructural cubic system of BiEuO3, BiTbO3 BiErO3 and BiHoO3, whereas BiSmO3 adapted a rhombohedral system. Scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDX) were employed to further characterize and analyze the structure of these mixed metal oxides. Band gap measurements obtained using diffuse reflectance spectroscopy (DRS) revealed potential photocatalytic activities of BiLnO3 in the visible light region (2.14 eV, 2.23 eV, 1.50 eV, 2.10 eV and 2.13 for BiSmO3, BiEuO3, BiTbO3, BiErO3 and BiHoO3 respectively). Accordingly, the photocatalytic performances of BiLnO3 were investigated for the cyclic carbonate formation by CO2 cycloaddition reaction to multiple epoxides. Reaction yields of the reported photocatalysts varied up to 99.9% depending on the epoxide substrate used. The simple sol-gel route explained in this report offers an easy, low-cost, environmentally friendly synthesis of highly efficient photocatalysts for a potential variety of photochemical reactions.

Investigations of electronic, elastic, and optical properties of (Ag, Cd)-doped LaAlO3: a computational insight

In this study, we used density functional theory to examine how the wide band gap optoelectronic properties of pure, silver-, and cadmium-doped LaAlO3 perovskites changed. Structural, electrical, elastic, and mechanical properties were calculated using generalized gradient approximation. Silver and cadmium incorporated at Al site demonstrated a decreasing trend in the band gap. Both impurities showed the reduction in band gap from 2.98 to 0.468 eV and from 2.98 to 2.0238 eV. The density of states was examined for pristine and doped structures to understand behavioral change of LaAlO3. It was observed that p states in upper valance band and d states in lower conduction band were contributing toward the reduction of band gap. Elastic properties were computed. Elastic parameters were used to calculate Born’s stability and it is predicted that the material is stable mechanically for both pristine and doped forms. Mechanical properties were also predicted and brittle nature was found for both pristine and doped materials. Optical responses such as dielectric function, absorption, and refractive index were also predicted. The impurity inclusion in pristine structure not only reduces the bad gap but also alters the optical behavior. Absorption edge shifted toward lower energy shows a clear redshift, whereas refractive index also reduces from 2.4 to 1.9, making the material more transparent. The absorption spectrum as well as electronic band gap makes this material more useful for solar cell application as well as photocatalytic applications.

Resolving the Ultrafast Charge Carrier Dynamics of 2D and 3D Domains within a Mixed 2D/3D Lead‐Tin Perovskite

AbstractMixed 2D/3D perovskite materials are of particular interest to the photovoltaics and light‐ emitting diode (LED) communities due to their impressive opto‐electronic properties alongside improved moisture stability compared to conventional 3D perovskite absorbers. Here, a mixed lead‐tin perovskite containing distinct, self‐assembled domains of either 3D structures or highly phase‐pure Ruddlesden–Popper 2D structures is studied. The complex energy landscape of the material is revealed with ultrafast optical transient absorption measurements. It is shown that charge transfer between these microscale domains only occurs on nanosecond timescales, consistent with the large size of the domains. Using optical pump‐terahertz probe spectroscopy, the effective charge‐carrier mobility is shown to be an intermediary between analogous pure 2D and 3D perovskites. Furthermore, detailed analysis of the free carrier recombination dynamics is presented. By combining results from a range of excitation wavelengths within a full dynamic model of the photoexcited carrier population, it is shown that the 2D domains in the film exhibit remarkably similar carrier dynamics to the 3D domains, suggesting that long‐range charge‐transport should not be impeded by the heterogeneous structure of the material.