Charge Carrier Dynamics Research Articles

Characterization of Intrinsic Charge Carrier Dynamics in Lead Halide Perovskite Films Using Time-Resolved Terahertz Spectroscopy

Characterization of Intrinsic Charge Carrier Dynamics in Lead Halide Perovskite Films Using Time-Resolved Terahertz Spectroscopy

Photoexcited charge carrier dynamics and electronic properties of two-dimensional MXene, Nb2CT x

Two-dimensional, 2D, niobium carbide MXene, Nb2CT x , has attracted attention due to its extraordinarily high photothermal conversion efficiency that has applications ranging from medicine, for tumor ablation, to solar energy conversion. Here, we characterize its electronic properties and investigate the ultrafast dynamics of its photoexcitations with a goal of shedding light onto the origins of its unique properties. Through density functional theory, DFT, calculations, we find that Nb2CT x is metallic, with a small but finite DOS at the Fermi level for all experimentally relevant terminations that can be achieved using HF or molten salt etching of the parent MAX phase, including –OH, –O, –F, –Cl, –Br, –I. In agreement with this prediction, THz spectroscopy reveals an intrinsic long-range conductivity of ∼60 Ω−1 cm−1, with significant charge carrier localization and a charge carrier density (∼1020 cm−3) comparable to Mo-based MXenes. Excitation with 800 nm pulses results in a rapid enhancement in photoconductivity, which decays to less than 25% of its peak value within several picoseconds, underlying efficient photothermal conversion. At the same time, a small fraction of photoinjected excess carriers persists for hundreds of picoseconds, and can potentially be utilized in photocatalysis or other energy conversion applications.

Providing a Review of Hot Carrier (HC) Relaxation Dynamics and Strategies of HC Extraction in Perovskites Nanocrystals

AbstractMetal halide perovskite (MHPs) nanocrystals (NCs) have recently emerged as promising materials for optoelectronic applications due to their exceptional photophysical properties. A comprehensive understanding of the underlying principles and key challenges associated with controlling the hot carrier (HC) cooling dynamics in MHPs is pivotal for the design of efficient perovskite‐based optoelectronic applications. This review highlights the general carrier cooling mechanism and identifies influencing crucial controlling parameters for carrier dynamics. The discussion includes strategies for manipulating HC cooling dynamics through carrier‐phonon and carrier‐carrier interactions. Notably, recent advancements in HC extraction with suitable acceptors are explored, as efficient HC extraction is imperative for the advancement of optoelectronic applications. The objective of this review is to outline potential pathways for strategically modifying carrier cooling processes to align with specific optoelectronic applications. A profound comprehension of charge carrier dynamics in MHPs NCs will pave the way for the development of highly efficient optoelectronic applications.

Insights into dielectric and electrical conductivity dynamics in sol-gel synthesized Ba0.75Ni0.25Tc0.88Mn0.12O3 perovskite ceramic

This study presents a comprehensive investigation into the structural, morphological, and electrical properties of sol-gel synthesized Ba0.75Ni0.25Tc0.88Mn0.12O3 perovskite ceramic (BNTMO). The meticulous preparation protocol, involving solvating various precursors, was followed by an extensive characterization employing X-ray diffraction, scanning electron microscopy, and dielectric studies. XRD analysis affirmed the single-phase single-phase cubic structure with Pm-3m space, while SEM revealed a well-defined morphology with an average particle size of 243 nm. The electrical conductivity exploration, elucidated through Jonscher’s universal power law, provided insights into charge carrier dynamics, exhibiting semiconductor behavior. Impedance spectroscopy unraveled a distinctive relaxation peak, corroborated by Cole-Cole plots, unveiling a unique charge carrier mechanism. Dielectric studies showcased intriguing polarization dynamics, indicating promising applications in energy storage. The convergence of activation energy values from various analyses underscores the coherence in the charge carrier relaxation process. Overall, our findings contribute to a nuanced understanding of the electrical intricacies of BNTMO, presenting avenues for its utilization in advanced technological applications.Graphical

Synergizing perovskite solar cell and thermally regenerative thermocapacitive cycle toward full-spectrum solar energy conversion

To overcome the heat generation issues in a perovskite solar cell (PSC) and enhance overall energy conversion efficiency, a pioneering full-spectrum solar power hybrid system seamlessly synergizing a PSC, a thermally regenerative thermocapacitive cycle (TRTC) and a solar selective absorber (SSA) is proposed. By developing a mathematical model grounded in charge carrier dynamics and thermodynamics, operational restraints and key performance indicators are derived. Through exhaustive parametric studies, the coefficient of thermal conductance between SSA and TRTC, proportional coefficient of regenerator, absorption layer thickness of PSC, absorption layer (AL)/hole transport layer interface defect density, and electron transport layer/AL interface defect density are identified optimizable factors. Meanwhile, elevating the coefficient of thermal conductance between TRTC and environment, charging endpoint voltage can effectively enhance performance. Besides, the operating temperature of PSC within different interval leads to different impacts on performance. Predictive optimization reveals remarkable maximum efficiencies of energy and exergy for the optimized hybrid system (i.e., 28.64 % and 30.80 %), surpassing unoptimized PSCs by 44.56 % and 45.56 %, respectively. These findings not only demonstrate the potential of the hybrid system but also provide valuable insights for enhancing solar energy conversion in real-world applications.

Modulating the Structure and Optoelectronic Properties of Solution-Processed Bismuth-Based Nanocrystals.

Bismuth-based chalcogenides have emerged as promising candidates for next-generation, solution-processable semiconductors, mainly benefiting from their facile fabrication, low cost, excellent stability, and tunable optoelectronic properties. Particularly, the recently developed AgBiS2 solar cells have shown striking power conversion efficiencies. High performance bismuth-based photodetectors have also been extensively studied in the past few years. However, the fundamental properties of these Bi-based semiconductors have not been sufficiently investigated, which is crucial for further improving the device performance. Here, we introduce multiple time-resolved and steady-state techniques to fully characterize the charge carrier dynamics and charge transport of solution-processed Bi-based nanocrystals. It was found that the Ag-Bi ratio plays a critical role in charge transport. For Ag-deficient samples, silver bismuth sulfide thin films behave as localized state induced hopping charge transport, and the Ag-excess samples present band-like charge transport. This finding is crucial for developing more efficient Bi-based semiconductors and optoelectronic devices.

Investigation into charge carrier dynamics in organic light-emitting diodes

Investigation into charge carrier dynamics in organic light-emitting diodes

Impact of nuclear effects on the ultrafast dynamics of an organic/inorganic mixed-dimensional interface

Electron dynamics at weakly bound interfaces of organic/inorganic materials are easily influenced by large-amplitude nuclear motion. In this work, we investigate the effects of different approximations to the equilibrium nuclear distributions on the ultrafast charge-carrier dynamics of a laser-excited hybrid organic/inorganic interface. By considering a prototypical system consisting of pyrene physisorbed on a MoSe2 monolayer, we analyze linear absorption spectra, electronic density currents, and charge-transfer dynamics induced by a femtosecond pulse in resonance with the frontier-orbital transition in the molecule. The calculations are based on ab initio molecular dynamics with classical and quantum thermostats, followed by time-dependent density-functional theory coupled to multi-trajectory Ehrenfest dynamics. We impinge the system with a femtosecond (fs) pulse of a few hundred GW cm−2 intensity and propagate it for 100 fs. We find that the optical spectrum is insensitive to different nuclear distributions in the energy range dominated by the excitations localized on the monolayer. The pyrene resonance, in contrast, shows a small blue shift at finite temperatures, hinting at an electron-phonon-induced vibrational-level renormalization. The electronic current density following the excitation is affected by classical and quantum nuclear sampling through suppression of beating patterns and faster decay times. Interestingly, finite temperature leads to a longer stability of the ultrafast charge transfer after excitation. Overall, the results show that the ultrafast charge-carrier dynamics are dominated by electronic rather than by nuclear effects at the field strengths and time scales considered in this work.

Surface evolution of thermoelectric material KCu4Se3 explored by scanning tunneling microscopy

Abstract Novel two-dimensional thermoelectric materials have attracted significant attention in the field of thermoelectric due to their low lattice thermal conductivity. A comprehensive understanding of their microscopic structures is crucial for driving further the optimization of materials properties and developing novel functional materials. Here, by using in situ scanning tunneling microscopy, we report the atomic layer evolution and surface reconstruction on the cleaved thermoelectric material KCu4Se3 for the first time. We clearly revealed each atomic layer, including the naturally cleaved K atomic layer, the intermediate Se2− atomic layer, and the Se− atomic layer that emerges in the thermodynamic-stable state. Departing from the majority of studies that predominantly concentrate on macroscopic measurements of the charge transport, our results reveal the coexistence of potassium disorder and complex reconstructed patterns of selenium, which potentially influences charge carrier and lattice dynamics. These results provide direct insight into the surface microstructures and evolution of KCu4Se3, and shed useful light on designing functional materials with superior performance.

Identification and Dynamics of Microsecond Long-Lived Charge Carriers for CsPbBr3 Perovskite Quantum Dots, Featuring Ambient Long-Term Stability.

We analyze the stability and photophysical dynamics of CsPbBr3 perovskite quantum dots (PeQDs), fabricated under mild synthetic conditions and embedded in an amorphous silica (SiOx) matrix (CsPbBr3@SiOx), underscoring their sustained performance in ambient conditions for over 300 days with minimal optical degradation. However, this stability comes at the cost of a reduced photoluminescence efficiency. Time-resolved spectroscopic analyses, including flash-photolysis time-resolved microwave conductivity and time-resolved photoluminescence, show that excitons in CsPbBr3@SiOx films decay within 2.5 ns, while charge carriers recombine over approximately 230 ns. This longevity of the charge carriers is due to photoinduced electron transfer to the SiOx matrix, enabling hole retention. The measured hole mobility in these PeQDs is 0.880 cm2 V-1 s-1, underscoring their potential in optoelectronic applications. This study highlights the role of the silica matrix in enhancing the durability of PeQDs in humid environments and modifying exciton dynamics and photoluminescence, providing valuable insights for developing robust optoelectronic materials.

Charge carrier dynamics and relaxation in highly conducting gel polymer electrolytes added with adiponitrile and dual redox

The fundamental understanding of the relationship between ion transport and segmental dynamics of polymer chains in polymer electrolytes is crucial for achieving high ionic conductivity at room temperature for technological applications in supercapacitors, batteries, etc. In this work, the ion dynamics and relaxation have been studied for gel polymer electrolytes (GPEs) containing P(VdF-HFP) as host polymer, adiponitrile as a plasticizer, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide as ionic liquid, and diphenylamine and copper iodide redox additives as fillers. The crystallization temperature of the ionic liquid and the melting temperature of the plasticizer play important roles in ion dynamics. The highest room-temperature ionic conductivity (3.3 × 10−3 S/cm) was obtained for the GPE filled with dual redox additives. The broadband ac conductivity spectra have been analyzed by using the Universal Power law model coupled with the Poisson–Nernst–Planck (PNP) model. The solid–solid phase transition of the ionic liquid affects the grain and grain boundary regions of the GPEs due to the presence of redox fillers. The temperature dependence of the dielectric spectra of the GPEs containing redox fillers confirms the phase transition at the crystallization temperature. The electric modulus and dielectric spectra have been analyzed by using the Havrilliak–Nigami, Kohlrausch–Williams–Watts, and derivative dielectric constant functions. The scaling of ac conductivity and modulus spectra confirms a common ion conduction and relaxation mechanism for the GPEs. The influence of dual redox additives is clearly observed in the values of ionic conductivity, ion diffusivity, and relaxation time.

Nitrogen Configuration Effects on Charge Carrier Dynamics in CsPbBr3/Carbon Dots S-Scheme Heterojunction for Photocatalytic CO2 Reduction.

Nitrogen-doped carbon dots (NCDs) featuring primary pyrrolic N and pyridinic N dominated configurations were prepared using hydrothermal (H-NCDs) and microwave (M-NCDs) methods, respectively. These H-NCDs and M-NCDs were subsequently applied to decorate CsPbBr3 nanocrystals (CPB NCs) individually, using a ligand-assisted reprecipitation process. Both CPB/M-NCDs and CPB/H-NCDs nanoheterostructures (NHSs) exhibited S-scheme charge transfer behavior, which enhanced their performance in photocatalytic CO2 reduction and selectivity of CO2-to-CH4 conversion, compared to pristine CPB NCs. The presence of pyrrolic N configuration at the heterojunction of CPB/H-NCDs facilitated efficient S-scheme charge transfer, leading to a remarkable 43-fold increase in photoactivity. In contrast, CPB/M-NCDs showed only a modest 3-fold enhancement in photoactivity, which was attributed to electron trapping by pyridinic N at the heterojunction. The study offers crucial insights into charge carrier dynamics within perovskite/carbon NHSs at the molecular level to advance the understanding of solar fuel generation.

Supercritical CH3OH-Triggered Isotype Heterojunction and Groups in g-C3N4 for Enhanced Photocatalytic H2 Evolution.

The structure tuning of bulk graphitic carbon nitride (g-C3N4) is a critical way to promote the charge carriers dynamics for enhancing photocatalytic H2-evolution activity. Exploring feasible post-treatment strategies can lead to effective structure tuning, but it still remains a great challenge. Herein, a supercritical CH3OH (ScMeOH) post-treatment strategy (250-300 °C, 8.1-11.8 MPa) is developed for the structure tuning of bulk g-C3N4. This strategy presented advantages of time-saving (less than 10 min), high yield (over 80%), and scalability due to the enhanced mass transfer and high reactivity of ScMeOH. During the ScMeOH post-treatment process, CH3OH molecules diffused into the interlayers of g-C3N4 and subsequently participated in N-methylation and hydroxylation reactions with the intralayers, resulting in a partial phase transformation from g-C3N4 into carbon nitride with a poly(heptazine imide)-like structure (Q-PHI) as well as abundant methyl and hydroxyl groups. The modified g-C3N4 showed enhanced photocatalytic activity with an H2-evolution rate 7.2 times that of pristine g-C3N4, which was attributed to the synergistic effects of the g-C3N4/Q-PHI isotype heterojunction construction, group modulation, and surface area increase. This work presents a post-treatment strategy for structure tuning of bulk g-C3N4 and serves as a case for the application of supercritical fluid technology in photocatalyst synthesis.

Managing Interfacial Defects and Charge-Carriers Dynamics by a Cesium-Doped SnO2 for Air Stable Perovskite Solar Cells.

A high-quality nanostructured tin oxide (SnO2) has garnered massive attention as an electron transport layer (ETL) for efficient perovskite solar cells (PSCs). SnO2 is considered the most effective alternative to titanium oxide (TiO2) as ETL because of its low-temperature processing and promising optical and electrical characteristics. However, some essential modifications are still required to further improve the intrinsic characteristics of SnO2, such as mismatch band alignments, charge extraction, transportation, conductivity, and interfacial recombination losses. Herein, an inorganic-based cesium (Cs) dopant is used to modify the SnO2 ETL and to investigate the impact of Cs-dopant in curing interfacial defects, charge-carrier dynamics, and improving the optoelectronic characteristics of PSCs. The incorporation of Cs contents efficiently improves the perovskite film quality by enhancing the transparency, crystallinity, grain size, and light absorption and reduces the defect states and trap densities, resulting in an improved power conversion efficiency (PCE) of ≈22.1% with Cs:SnO2 ETL, in-contrast to pristine SnO2-based PSCs (20.23%). Moreover, the Cs-modified SnO2-based PSCs exhibit remarkable environmental stability in a relatively higher relative humidity environment (>65%) and without encapsulation. Therefore, this work suggests that Cs-doped SnO2 is a highly favorable electron extraction material for preparing highly efficient and air-stable planar PSCs.

Point-junction and alkali-assisted surface selenium diffusion: Unveiling a two-step method for enhancing the efficiency of VTD-SnS thin-film solar cells

Surface and interface engineering in thin-film solar cells (TFSCs) is vital for optimizing charge carrier dynamics, reducing recombination, enhancing material properties, and ultimately improving efficiency and overall performance. In this study, e-beam evaporation was used to deposit selenium (Se) onto tin sulfide (SnS) absorber layers with a thickness of 10 nm to 50 nm. The Se layer optimization was validated using various characterization techniques, which confirmed the formation of micro-sized openings via Se droplet deposition. This Se passivation-plus-local opening geometry plays a crucial role in forming point-junctions with the n-type CdS during cell fabrication, presenting a novel approach in state-of-the-art technology. The results revealed a significant enhancement in the conversion efficiency of the SLG/Mo/SnS/Se/CdS/i-ZnO/AZO/Al device to 3.01 % (VOC = 0.326 V, JSC = 20.21 mA cm−2, and FF = 0.45) with 30 nm Se layer deposition. Furthermore, a 30 nm-thick NaF-assisted Se layer was deposited to improve device performance. The diffusion of both Se and Na into the SnS substrate was validated using XRD, SEM, EDS, AFM, and XPS. The power conversion efficiency (PCE) of the SLG/Mo/SnSSe-NaF/CdS/i-ZnO/AZO/Al device was further enhanced to 3.70 % (VOC = 0.340 V, JSC = 22.56 mA cm−2, and FF = 0.48). This enhancement is attributed to the creation of localized junctions via Se surface passivation, and the concurrent SnSSe formation induces band gap tuning and increases the grain size, contributing to additional PCE improvement during Na-assisted Se diffusion.

Exploring the charge carrier dynamics in carbon nanotubes-TiO2 composites for water photooxidation

Composite materials consisting of stable metal oxides and functionalized carbonaceous nanomaterials are attractive for application in a range of photocatalytic systems. Carbon nanotubes/titanium dioxide (CNTs/TiO2) composites have been shown to outperform TiO2 in photoelectrochemical applications, which has been attributed to efficient electron extraction from TiO2 by CNTs and subsequent fast electron transport. However, the underlying mechanisms need to be clarified. In this work, we present a systematic study varying the CNTs content and comprehensively analyze the composite structure, morphology, crystallinity, light harvesting properties, and photoelectrochemical charge carrier dynamics. We show that the performance improvement observed for the composites depends in a complex manner on several parameters, including the CNTs content, the thickness of the TiO2 overlayer, the chemical capacitance of CNTs, and the hole transfer efficiency. Using intensity-modulated photocurrent spectroscopy in aqueous electrolyte solution both without and with 0.1 M Na2SO3 as hole capturing agent, we show that electron extraction and transport compete with the hole trapping, recombination, and transfer dynamics at the CNTs/TiO2 and TiO2/electrolyte interfaces. We show that the optimal performance is related to the change in charge extraction mechanism from a trap-limited diffusion scenario in TiO2 to a direct charge extraction in CNTs/TiO2 composite with optimal CNTs content and TiO2 thickness. These insights provide valuable guidance for the design and optimization of CNTs/TiO2 and similar composites for photoelectrochemical applications.

Enhanced photovoltaic performance of dye sensitized solar cells using cesium bromide modified TiO2 electron transport layer

TiO2 is one of the most widely explored materials as an electron transport layer (ETL) in dye sensitized solar cells (DSSCs) due to its excellent physical and chemical properties. However, recombination at the device's interface slackens the charge carrier movement, adversely affecting their device performance. Rapid extraction of photogenerated charge carriers plays a vital role in developing high efficiency DSSCs. The conduction band alignment of TiO2 ETL and N719 dye light absorber plays a crucial role in charge carrier dynamics of DSSCs. Herein, the band structure of TiO2 ETL is finely tuned by the incorporation of cesium bromide (CsBr). At the optimal concentration (0.4 Wt. %), DSSCs achieved the best power conversion efficiency (PCE) of 9.28 % compared to 7.61 % for pristine TiO2. The modified TiO2–CsBr ETL induced a negative shift in flat band potential (Vfb) from −0.46 to −0.50 V, which improved the open circuit voltage (VOC), its work function (ɸ) from −4.71 to −3.75 eV and increased conduction band minimum (CBM) from −3.58 to −2.42 eV. CsBr incorporation increased electron density in TiO2 matrix, indicating the suppression of trap state and significantly improved the overall photovoltaic performance of DSSCs.

Construction of TiO2@Cu2O-CuS heterostructures integrating RGO for enhanced full-spectrum photocatalytic degradation of organic pollutants

This study presents the development and optimization of TiO2@Cu2O-CuS heterostructures, enhanced with reduced graphene oxide (RGO), for efficient photocatalytic degradation of organic pollutants, focusing on imidacloprid. Two configurations, TiO2/RGO/Cu2O-CuS and Cu2O-CuS/RGO/TiO2, are explored to highlight the impact of material layering on photocatalytic efficiency. The strategic integration of RGO optimizes charge transfer, crucial for photocatalysis. Comprehensive characterization techniques, such as X-ray diffraction (XRD), Transmission Electron Microscopy (TEM), X-ray Photoelectron Spectroscopy (XPS), Raman spectroscopy, and Nitrogen adsorption-desorption isotherms, provide insights into the crystalline structure, morphology, surface chemistry, and textural properties of the heterostructures. The TiO2/RGO/Cu2O-CuS configuration significantly outperforms its counterpart in photocatalytic activity under full-spectrum (UV–VIS–IR) illumination, due to improved charge carrier dynamics and synergistic interactions between the composite materials. Remarkably, the TiO2/RGO/Cu2O-CuS assembly achieved over 95 % degradation of imidacloprid under simulated solar irradiation, marking a breakthrough in solar spectrum utilization for photocatalysis and exhibits promising recyclability, maintaining its high photocatalytic efficiency even after multiple degradation cycles, highlighting its potential for sustainable pollutant removal applications. Additionally, this configuration demonstrates a twofold increase in degradation efficiency compared to separate UV and VIS irradiations, emphasizing its rapid pollutant removal capability. This research underscores the critical role of material layer sequencing in developing high-efficiency photocatalytic systems and marks a significant advancement in environmental remediation technologies that harness renewable energy sources.

Atomically‐Scattered Active Centers Accelerating Photocatalytic Evolution of Ammonia

AbstractPhotocatalytic N2 reduction to ammonia rises as a cost‐effective, environmentally benign, and efficient route to generate ammonia as a transportable/storable energy carrier and essential fertilizer. Recently, photocatalysts anchored with various atomically scattered active centers (ASACs), such as Ru, Fe, Au, Pt, Cu, Mo, and La, are extensively explored in photocatalytic N2‐to‐ammonia transformation. This review critically summarizes the current achievements in the synthesis of various photocatalyst supports (such as metal oxide, carbon nitride, metal‐organic framework, and covalent organic framework) anchored with the above‐mentioned ASACs for N2 reduction to form ammonia. The synthesis routes, structural/compositional characteristics, and performances of these ASACs anchored photocatalysts are summarized and introduced. Furthermore, the atomic‐scale relationship between the structure/composition and performance of these ASACs anchored photocatalysts is also introduced. The reaction mechanism including the reaction kinetics/thermodynamics, reaction pathways, and charge carrier kinetics, especially those revealed by various state‐of‐art characterization techniques, have been highlighted. This review also outlines the basic principles for the synthesis of novel photocatalysts aimed at ammonia evolution. Finally, the current challenges, opportunities, and future outlooks of ASACs anchored photocatalysts for ammonia evolution are introduced.

Elucidating Interfacial Hole Extraction and Recombination Kinetics in Perovskite Thin Films

Hybrid organic–inorganic perovskite solar cells (PSCs) are receiving huge attention owing to their marvelous advantages, such as low cost, high efficiency, and superior optoelectronics characteristics. Despite their promising potential, charge-carrier dynamics at the interfaces are still ambiguous, causing carrier recombination and hindering carrier transport, thus lowering the open-circuit voltages (Voc) of PSCs. To unveil this ambiguous phenomenon, we intensively performed various optoelectronic measurements to investigate the impact of interfacial charge-carrier dynamics of PSCs under various light intensities. This is because the charge density can exhibit different mobility and charge transport properties depending on the characteristics of the charge transport layers. We explored the influence of the hole transport layer (HTL) by investigating charge transport properties using photoluminescence (PL) and time-resolved (TRPL) to unveil interfacial recombination phenomena and optoelectronic characteristics. We specifically investigated the impact of various thicknesses of HTLs, such as 2,2′,7,7′-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9′-spirobifluorene (spiro-OMeTAD), and poly(triaryl)amine (PTAA), on FA0.83MA0.17Pb(Br0.05I0.95)3 perovskite films. The HTLs are coated on perovskite film by altering the HTL’s concentration and using F4-TCNQ and 4-tert-butylpyridine (tBP) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSi) as dopants both for spiro-OMeTAD and PTAA. These HTLs diversified the charge concentration gradients in the absorption layer, thus leading to different recombination rates based on the employed laser intensities. At the same time, the generated charge carriers are rapidly transferred to the interface of the HTL/absorption layer and accumulate holes at the interface because of inefficient capacitance and mobility differences caused by differently doped HTL thicknesses. Notably, the charge concentration gradient is low at lower light intensities and did not accumulate holes at the HTL/absorption layer interface, even though they have high charge mobility. Therefore, this study highlights the importance of interfacial charge recombination and charge transport phenomena to achieve highly efficient and stable PSCs.