Carrier Loss Research Articles

Efficient and Stable Wide‐Bandgap Methylammonium‐Free Perovskite Solar Cells by Simultaneous Passivation and Cleaning with Diamine

Wide‐bandgap perovskite solar cells (WBG‐PSCs) are pivotal in achieving high‐performance tandem solar cells. However, their power conversion efficiency (PCE) is limited by the losses from the interfacial charge transfer barrier and nonradiative recombination. In this investigation, 1,4‐bis(aminomethyl)benzene (PDMA) is employed as a defect passivator for fabricating methylammonium (MA)‐free perovskite solar cells (PSCs), thus effectively mitigating nonradiative recombination losses of charge carriers. Meanwhile, PDMA molecules chemically rinse the perovskite film to create a grooved surface, leading to the increase of contact area between the perovskite and electron transport layer to further improve the interfacial charge transfer. As a result, the PSCs based on these surface‐passivated and chemically cleaned perovskite films present a champion PCE of 21.23% (Eg = 1.68 eV) compared to the control devices with a PCE of 18.23%, while maintaining over 80% efficiency after 800 h storage in ambient air. This study presents a highly effective approach for one‐step passivation and chemical cleaning of wide‐bandgap perovskite for efficient and stable solar cells, offering valuable insights for future research in this field.

Design and Simulation for Minimizing Non-Radiative Recombination Losses in CsGeI2Br Perovskite Solar Cells.

CsGeI2Br-based perovskites, with their favorable band gap and high absorption coefficient, are promising candidates for the development of efficient lead-free perovskite solar cells (PSCs). However, bulk and interfacial carrier non-radiative recombination losses hinder the further improvement of power conversion efficiency and stability in PSCs. To overcome this challenge, the photovoltaic potential of the device is unlocked by optimizing the optical and electronic parameters through rigorous numerical simulation, which include tuning perovskite thickness, bulk defect density, and series and shunt resistance. Additionally, to make the simulation data as realistic as possible, recombination processes, such as Auger recombination, must be considered. In this simulation, when the Auger capture coefficient is increased to 10-29 cm6 s-1, the efficiency drops from 31.62% (without taking Auger recombination into account) to 29.10%. Since Auger recombination is unavoidable in experiments, carrier losses due to Auger recombination should be included in the analysis of the efficiency limit to avoid significantly overestimating the simulated device performance. Therefore, this paper provides valuable insights for designing realistic and efficient lead-free PSCs.

Intercalation Electrode and Grain Reconstruction Induce Significant Sensitivity Enhancement for Perovskite X-ray Detectors.

Organic-inorganic hybrid perovskites have been recognized as potential candidates in direct X-ray detectors and have triggered tremendous interest in the past years. The blade coating method meets the requirements of large area and low cost for perovskite X-ray detectors, while the low compactness resulting from solvent evaporation limits the charge collection efficiency (CCE) and device sensitivity. Most of the reports are focused on the melioration of perovskite films to increase device sensitivity; there are still problems of low CCE. Herein, we introduce an intercalation-electrode device structure and achieve a ∼20-fold sensitivity enhancement. Carrier distribution throughout the thick films is simulated, and the electrode intercalating site can be optimized according to the mobility-lifetime factor to achieve the highest CCE. A methylamine thiocyanate (MASCN) additive-assisted coating strategy is developed, and pinhole free thick films with regrown particles are obtained without frequently used hot/soft pressing. A sensitivity level of ∼105 μC Gyair-1 cm-2 as well as a detection limit of 77 nGyair s-1 is achieved under low bias, which is among the best performance for polycrystalline perovskite direct X-ray detectors. This work provides a universal device structure design to overcome carrier loss through a long transport distance and enhances the CCE for ultrahigh sensitivity.

Flexible Soft X-Ray Image Sensors based on Metal Halide Perovskites With High Quantum Efficiency.

Soft X-ray imaging is a powerful tool to explore the structure of cells, probe material with nanometer resolution, and investigate the energetic phenomena in the universe. Conventional soft X-ray image sensors are by and large Si-based charge coupled devices that suffer from low frame rates, complex fabrication processes, mechanical inflexibility, and required cooling below -60°C. Here, a soft X-ray photodiode is reported based on low-cost metal halide perovskite with comparable performance to commercial Si-based device. Nanothrough network electrodeminimized the optical loss due to the shadowing of insensitive layers, while a multidimensional perovskite heterojunctionis generated to reduce the photo-generated carrier loss. This strategy promoted a record quantum efficiency of 8×103% without cooling, several orders of magnitude greater than the previously achieved. Flexible and curved soft X-ray imaging arrays are fabricated based on this high-performance device structure, demonstrating stable soft X-ray response and sharp imaging capabilities. This work highlights the low-cost and efficient perovskite photodiode as a strong candidate for the next-generation soft X-ray image sensors.

Microstructural Passivation of Patterned Al2O3 Back Contacts on CdS/CdTe Solar Cells

AbstractPatterned aluminum oxide (Al2O3) back contact on cadmium telluride (CdTe) solar cells can effectively mitigate the loss of the majority carriers while retaining the passivation benefits for minority carriers. This study investigates the impact of the point‐contact geometry on cell performance, where the spacing of the microholes is systematically varied at a constant microhole diameter (≈16 µm). Microhole arrays are created on an evaporated Al2O3 layer (≈30 nm) on CdTe using laser‐beam lithography and selective wet etching processes. Comparative analysis indicates a significant decrease in fill factor (FF) and short‐circuit current (ISC) when the contact fraction falls below 30%, likely due to the Al2O3 barrier impeding majority carriers. Above this fraction, FF and ISC are comparable to those of baseline CdTe cells without Al2O3. Open‐circuit voltage (VOC) shows a gradual decrease as Al2O3 coverage is reduced but exhibits a slight increase (<15 mV) when the contact fraction exceeds 30%. Cathodoluminescence (CL) characterization reveals that significantly improved radiative recombination occurs within the CdTe grain bulk with Al2O3, whereas this effect on grain boundaries is minimal. The findings imply complex local carrier dynamics in the patterned back‐contact region, closely tied to the microstructural properties of CdTe‐based solar cells.

Interface-Centric Strategies in Kesterite Solar Cells: Addressing Challenges, solutions, and Future Directions for Efficient Solar-Harvesting Technologies.

As reserves of non-renewable energy sources decline, the search for sustainable alternatives becomes increasingly critical. Next-generation energy materials play a key role in this quest by enabling the manipulation of properties for effective energy solutions and understanding interfaces to enhance energy yield. Studying these interfaces is essential for managing charge transport in optoelectronic devices, yet it presents significant challenges. This review emphasizes the critical role of interfaces in kesterite solar cells (KSCs), focusing on interfacial architecture, carrier losses, and non-radiative recombination. This review highlights the importance of addressing interface issues and utilizing advanced characterization tools to reveal interface properties. Current interface problems are addressed, recent advancements in interface engineering are summarized, and perspectives on future challenges and prospects are offered. The goal is to illuminate the nature of interfaces and tackle interface losses, which are crucial for improving device design and performance. Despite their pivotal role in device operation, comprehensive reviews on interfaces are lacking, underscoring the relevance of the work for researchers in material interfaces and device engineering. It is hoped that this article will spark interest and inspire further research into interface studies and the mitigation of interface losses.

Tailoring Interfacial Dipole Molecules to Mitigate Carrier and Energy Losses in Perovskite Solar Cells

Tailoring Interfacial Dipole Molecules to Mitigate Carrier and Energy Losses in Perovskite Solar Cells

Hierarchical ultra-thin porous Co3O4 nanosheets derived from mixed phase α- and β-Co(OH)2 for high sensitivity and ppb-level acetone sensing

Addressing the energy loss of carriers during transmission and achieving high sensitivity detection of target gases facilitates the synthesis of trace-level acetone sensors, which is of great significance in the fields of air quality early warning, health monitoring, and industrial safety monitoring. Here, we propose a strategy where, under hydrothermal conditions, the content of mixed-phase α- and β-Co(OH)2 is regulated by varying the protonation level of 2-methylimidazole in different solutions, leading to the formation of porous monocrystalline Co3O4 microflower structure. The microflower is assembled from ultrathin nanosheets, and the 3D-interconnected macroporous and mesoporous structure provides high surface area and gas diffusion channels. The monocrystalline and two-dimensional structures favor high carrier mobility, enhancing the signal-to-noise ratio. Furthermore, the thickness of the Co3O4 nanosheets is less than twice the Debye length, making their electrical properties completely dependent on surface. DFT calculations also indicate that the few layers Co3O4 model is conducive to acetone adsorption. The Co3O4 sensor exhibits exceptional gas sensing performance towards acetone, with favourable sensitivity (16.83 to 10 ppm), selectivity, and stability, as well as an ultra-low practical detection limit of 10 ppb. Rich point defects and line defects play a significant role in improving the surface activity of the sensitive material as well. This research offers a pathway for designing sensors with exceptional gas sensitivity by employing a straightforward method to control the morphology of sensitive materials, combined with defect engineering to enhance sensing activity.

InGaAs/GaAs nano-ridge laser with an amorphous silicon grating monolithically grown on a 300 mm Si wafer.

The monolithic growth of direct-bandgap III-V materials directly on a Si substrate is a promising approach for the fabrication of complex silicon photonic integrated circuits including light sources and amplifiers. It remains challenging to realize practical, reliable, and efficient light emitters due to misfit defect formation during the epitaxial growth. Exploiting nano-ridge engineering (NRE), III-V nano-ridges with high crystal quality were achieved based on aspect ratio defect trapping inside narrow trenches. In an earlier work, we used an etched grating to create distributed feedback lasers from these nano-ridges. Here we deposited an amorphous silicon grating on the top of the nano-ridge. Under pulsed optical pumping, a ∼7.84 kW/cm2 lasing threshold was observed, ∼5 times smaller compared to devices with an etched grating inside the nano-ridge. Compared to the etched grating, the amorphous silicon grating introduces no extra carrier loss channels through surface state defects, which is believed to be the origin of the lower threshold. This low threshold again demonstrates the high quality of the epitaxial deposited material and may provide a route toward further optimizing the electrically driven devices.

Random lasers with controlled emission modes by colloidal semiconductor quantum dots coupled to plasmonic nanorod arrays

Random lasers based on scattering for light amplification have gained extensive attention due to their simple structures. Colloidal semiconductor quantum dots (CSQDs) are excellent candidates as active media for random lasing. However, achieving CSQDs-based random lasers is challenging because the non-radiative Auger recombination produces a remarkable carrier loss. Here, we report random lasers with low thresholds based on the CSQDs coupled to the plasmonic nanorod arrays. The random lasers result from the enhancing excitation and emission rates of the CSQDs through plasmon resonance energy transfer induced by the spectral overlap between the resonant cavity modes of the plasmonic nanorod arrays and the excitons of the CSQDs, which reduces the carrier loss and establishes the optical gain in the CSQDs. Moreover, the incoherent and coherent emission modes can be controlled by varying the filling configurations (i.e., full-filling and partial-filling) of the plasmonic nanorods embedded in anodic aluminum oxide templates. Consequently, the incoherent random laser with a threshold of 19.3 μJ/mm2 and coherent random lasers with a threshold of 13.5 μJ/mm2 are performed, respectively. The proposed system provides a feasible method for low-threshold CSQDs-based random lasers with controlled emission modes, showing a promising avenue for potential applications.

Suppressing leakage current and charge accumulation via perovskite interface morphology regulation for efficient light-emitting diodes

Charge carriers will recombine outside the emitting layer (EML) in non-ideal perovskite light-emitting diodes (PeLEDs), which can lead to parasitic loss and be detrimental to the performance of PeLEDs. Here, we have subtly utilized the property of perovskite nanocrystals (NCs) to design and optimize the homogeneity and optical property of EML, thereby suppressing the undesired carrier loss behavior in system. Photoluminescence (PL) spectra with transmission electron microscopy (TEM) images show that smaller and more homogeneous NCs in size are obtained by temperature-controlled (TC) method. Atomic force microscopy (AFM) images and temperature-dependent PL spectra show that EML with better optical property and uniformity is fabricated. The multiscale capacitance characterization shows that the device with modified EML exhibits significantly reduced leakage current, while the increased specific surface area between electron transport layer (ETL) and EML substantially reduces charge accumulation. Additionally, multiscale reactance, impedance and phase angle responses, reveal that the carrier oscillation behavior in the optimized device is suppressed compared to control group, leading to less energy loss. Consequently, the optimized devices exhibit lower leakage current and superior electroluminescent properties. The luminance is increased from 31650 cd/m2 to 72941 cd/m2, current efficiency (CE) is improved from 59.9 cd/A to 94.3 cd/A, and the external quantum efficiency (EQE) rises from 12.6 % to 19.7 %, corresponding to improvement of 230 %, 157 %, and 156 %, respectively. This research provides valuable insight into the impact of functional layer morphology on carrier dynamic behavior in PeLEDs.

Ion-Exchange Polymer Network Enhanced Interfacial Compatibility for Stable and Efficient Inverted Perovskite Solar Cells.

Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) as a low-cost and water-processable hole transport material has been widely used in various optoelectronic devices. Although the incorporation of anionic polyelectrolyte PSS in PEDOT contributes to superior water solubility, the trade-off between efficiency and stability remains a challenging issue, limiting its reliable application in perovskite solar cells (PSCs). Herein, we proposed an ion-exchange (IE) strategy to effectively control the doping degree, interfacial charge dynamics, and reliability of PEDOT:PSS in PSCs. This IE approach based on hard cation-soft anion rules enabled effective anion exchange between PEDOT:PSS and lithium bis(trifluoromethylsulfonyl)imide (LiTFSI), which favored enhancing the film conductivity, regulating the perovskite crystallization, and reducing the carrier losses at the interfaces. Consequently, a notable increase of the open-circuit voltage from 0.88 to 1.02 V was realized, resulting in a champion efficiency of 18.7% compared to the control (15.4%) in inverted PSCs. More encouragingly, this IE strategy significantly promoted the thermal and environmental stability of unsealed devices by maintaining over 80% of initial efficiencies after 2000 h. This work provides an effective way to regulate the doping state of the PEDOT-based hole transport material and guides the development of robust polymeric conducting materials for efficient perovskite photovoltaics.

Reaction Mechanism of Hydrogen Generation and Nitrogen Fixation at Carbon Nitride/Double Perovskite Heterojunctions

Photocatalytically active heterojunctions based on metal halide perovskites (MHPs) are drawing significant interest for their chameleon ability to foster several redox reactions. The lack of mechanistic insights into their performance, however, limits the ability of engineering novel and optimized materials. Herein, a report is made on a composite system including a double perovskite, Cs2AgBiCl6/g‐C3N4, used in parallel for solar‐driven hydrogen generation and nitrogen reduction, quantified by a rigorous analytical approach. The composite efficiently promotes the two reactions, but its activity strongly depends on the perovskite/carbon nitride relative amounts. Through advanced spectroscopic investigation and density function theory (DFT) modeling the H2 and NH3 production reaction mechanisms are studied, finding perovskite halide vacancies as the primary reactive sites for hydrogen generation together with a positive contribution of low loaded g‐C3N4 in reducing carrier recombination. For nitrogen reduction, instead, the active sites are g‐C3N4 nitrogen vacancies, and the heterojunction best performs at low perovskites loadings where the composites maximize light absorption and reduce carrier losses. It is believed that these insights are important add‐ons toward universal exploitation of MHPs in contemporary photocatalysis.

Formation of a potential barrier by a ZnSXSe1−X electron-blocking layer to improve the efficiency of CdSe0.3S0.7/CdSe quantum dot sensitized solar cells

We designed and fabricated multilayer quantum dots sensitized solar cells (QDSCs) with TiO2 NPs/CdSe0.3S0.7/CdSe/ZnSXSe1−X, X = S/S + Se = 0, 0.7, 0.8, 0.9, and 1 photoelectrodes to achieve optimum power conversion efficiency (PCE). In the corresponding structure, incoming light is absorbed by the CdSe0.3S0.7 and CdSe quantum dots (QDs), while the ZnSXSe1−X QDs act as an electron blocking layer or passivation layer, forming an energy barrier that restricts electron mobility from the light absorbers to the polysulfide electrolyte. The beneficial effect of the alloyed ZnSXSe1−X layer is the adjustability of its nanoparticle size/bandgap energy proportional to variations in the concentration of anionic precursors X, according to optical results. The PCE value of the reference cell with the TiO2 NPs/CdSe0.3S0.7/CdSe photoanode is 4.15 %. Following the coating of ZnSe, ZnS0.7Se0.3, ZnS0.8Se0.2, ZnS0.9Se0.1, and ZnS QDs via two successive ionic layer adsorption and reaction (SILAR) cycles (2Sc) on the CdSe0.3S0.7/CdSe co-sensitized photoelectrode increasing stability and improving the PCE value to 4.9 %, 5.40 %, 5.70, 5.25 %, and 5.05 %, respectively. Next, by modifying the thickness of the champion cell's passivation layer, the QDSCs with TiO2 NPs/CdSe0.3S0.7/CdSe/ZnS0.8Se0.2 (3Sc) photoelectrode exhibit maximum photovoltaic performance parameters of short circuit current density (JSC) = 26.25 mA/cm2, open circuit voltage (VOC) = 560 mV, fill factor (FF) = 0.42 % and PCE = 6.15 %. This improvement in performance is the result of decreased internal energy loss and recombination of charge carriers at the interface between the electrolyte and photoelectrode, which increases electron collection efficiency and electron injection efficiency in the visible region according to the external and internal quantum efficiency curves.

Side Chain Functional Molecule Additives for Efficient and Stable Perovskite Solar Cells

AbstractIn the commercial development of perovskite solar cells, the main challenge lies in achieving efficient devices with high stability. Additive engineering in polycrystalline perovskites is considered as an effective approach to address this challenge by passivating surface defects and reducing carrier losses associated with these defects. In this work, the passivation effect of molecules with different side chain groups on perovskites and the role of binding energy in mitigating carrier loss are studied. The findings reveal that the thiophene group is particularly effective in passivating defects and enhancing hole transport. Consequently, devices treated with 2‐thienylmethylamine hydrochloride (TMAC) demonstrate a champion power conversion efficiency (PCE) of 24.63%. Furthermore, these TMAC‐treated devices exhibit remarkable stability, maintaining over 93.13% of their initial efficiencies after 1200 h of continuous illumination under maximum power point tracking (MPPT). This research presents a pathway to enhance the optoelectronic performance and stability of perovskite solar cells.

TiO2 Electron Transport Layer with p–n Homojunctions for Efficient and Stable Perovskite Solar Cells

HighlightsDeveloping a universal strategy of the p–n homojunction engineering that could significantly boost electron mobility of electron transport layer (ETL) by two orders of magnitude.Proposing a new mechanism based on p–n homojunction to explain inhibited carrier loss at buried interface.Setting a new performance benchmark as high as 25.50% for planar perovskite solar cells employing TiO2 as ETLs.

Photo Luminescence and Radiative Carrier Losses in Monolayer Transition Metal Dichalcogenides.

The carrier losses due to radiative recombination in monolayer transition metal dichalcogenides are studied using fully microscopic many-body models. The density- and temperature-dependent losses in various Mo- and W-based materials are shown to be dominated by Coulomb correlations beyond the Hartree-Fock level. Despite the much stronger Coulomb interaction in 2D materials, the radiative losses are comparable-if not weaker-than in conventional III-V materials. A strong dependence on the dielectric environment is found in agreement with experimental results.

Stability and kinetic insights for ibuprofen removal from aquaculture wastewater using green supported ionic liquid membranes

Pharmaceutical residues in aquaculture effluent have become a growing environmental concern due to their potential ecological impacts. Supported ionic liquid membranes (SILM) offer a promising solution for extracting micropollutants from contaminated sources. SILM was developed using Aliquat 336 in sunflower oil (SFO) as a carrier solution, specifically targeting ibuprofen (IBP) in aquaculture wastewater. Different solid supports are fabricated through the nonsolvent-induced phase separation (NIPS) process and characterized by SEM, EDX, contact angle, FTIR and porosimeter. PVDF support is selected as solid support for immobilization of the carrier solution owing to its properties of having an asymmetrical shape, thickness of 48.8 µm, porosity of 72% and contact angle of 89.0° (feed side) and 85.3° (stripping side). The percentage of carrier loss obtained was only 1.10%. The optimal conditions for IBP removal were obtained at 0.50 M Aliquat 336, with a feed phase pH of 5.5 and stripping phase pH of 8. Further tests on real aquaculture wastewater affirmed the system’s efficacy in removing IBP and maintaining the stability at least the fifth cycle of membrane reusability. This study underscores the viability of proposed SILM system in mitigating IBP from aquaculture sector.

Cross-examination of photoinitiated carrier and structural dynamics of black phosphorus at elevated fluences.

Revived attention in black phosphorus (bP) has been tremendous in the past decade. While many photoinitiated experiments have been conducted, a cross-examination of bP's photocarrier and structural dynamics is still lacking. In this article, we provide such analysis by examining time-resolved data acquired using optical transient reflectivity and reflection ultrafast electron diffraction, two complementary methods under the same experimental conditions. At elevated excitation fluences, we find that more than 90% of the photoinjected carriers are annihilated within the first picosecond (ps) and transfer their energy to phonons in a nonthermal, anisotropic fashion. Electronically, the remaining carrier density around the band edges induces a significant interaction that leads to an interlayer lattice contraction in a few ps but soon diminishes as a result of the continuing loss of carriers. Structurally, phonon-phonon scattering redistributes the energy in the lattice and results in the generation of out-of-plane coherent acoustic phonons and thermal lattice expansion. Their onset times at ∼6ps are found to be in good agreement. Later, a thermalized quasi-equilibrium state is reached following a period of about 40-50ps. Hence, we propose a picture with five temporal regimes for bP's photodynamics.

Revealing the Loss Mechanism of Chemically-Induced Hot Electron Transport.

Hot electrons are crucial for unraveling the intrinsic relationship between chemical reactions and charge transfer in heterogeneous catalysis. Significant research focused on real-time detection of reaction-driven hot electron flow (chemicurrent) to elucidate the energy conversion mechanisms, but it remains elusive because carrier generation contributes to only part of the entire process. Here, a theoretical model for quantifying the chemicurrent yield is presented by clarifying the contributions of hot carrier losses from the internal emission and multiple reflections. The experimental chemicurrent yield verifies our model with a reliable mean free path of hot electrons, emphasizing the importance of comprehensive consideration of the transport process besides hot electron generation. Moreover, Pt nanoparticles (NPs)-decorated Au/TiO2 is examined, showing the role of NPs-induced carrier losses in the performance of catalytic nanodiodes. These findings are expected to contribute to understanding the hot electron detection efficiency and designing nanodiodes with enhanced hot carrier flow and catalytic activity.