Showing papers by "Christoph J. Brabec published in 2023"

Conformally bonded molecular interface retarded iodine migration for durable perovskite solar cells

Abstract: State-of-the-art n-i-p perovskite solar cells (PSCs) suffer from stability issues due to ionic interdiffusion. Herein, by enlarging indacenodithiophene -bridge donor (D’) to combine with methoxy triphenylamine donor (D) and benzothiadiazole...

Highly Luminescent Transparent Cs2AgxNa1–xBiyIn1–yCl6 Perovskite Films Produced by Single-Source Vacuum Deposition

Abstract: Thermal deposition of halide perovskites as a universal and scalable route to transparent thin films becomes highly challenging in the case of lead-free double perovskites, requiring the evaporation dynamics of multiple metal halide sources to be balanced or a single-phase precursor preliminary synthesized to achieve a reliable control over the composition and the phase of the final films. In the present Letter, the feasibility of the single-source vacuum deposition of microcrystalline Cs2AgxNa1–xBiyIn1–yCl6 double perovskites into corresponding transparent nanocrystalline films while preserving the bulk spectral and structural properties is shown. The perovskite films produced from the most emissive powders with x = 0.40 and y = 0.01 revealed a photoluminescence quantum yield of 85%, highlighting thermal evaporation as a promising approach to functional perovskite-based optical materials.

Autonomous Optimization of an Organic Solar Cell in a 4-dimensional Parameter Space

Abstract: Optimizing solution-processed organic solar cells is a complex task due to the vast parameter space in organic photovoltaics (OPV). Classical Edisonian or one-variable-at-a-time (OVAT) optimization approaches are laborious, time-consuming, and may not find the optimal parameter set in multidimensional design spaces. To tackle this problem, we demonstrate here for the first time artificial intelligence (AI) guided closed-loop autonomous optimization for fully functional organic solar cells. We empower our LineOne, an automated materials and device acceleration platform with a Bayesian Optimizer (BO) to enable autonomous operation for solving complex optimization problems without human interference. The system is able to fabricate and characterize complete OPV devices and navigate efficiently through the design space spanned by composition and processing parameters. In addition, a Gaussian Progress Regression (GPR) based early prediction model is employed to predict the efficiency of the cells from cheap proxy measurements, in our case, thin film absorption spectra, which are analyzed using a spectral model based on physical properties to generate microstructure features as input for the GPR. We demonstrate our generic and complete autonomous approach by optimizing composition and processing conditions of a ternary OPV system (PM6:Y12:PC70BM) in a four-dimensional parameter space. We identify the best parameter set for our system and obtain a precise objective function over the whole parameter space with a minimal number of samples. We demonstrate autonomous optimization of a complex opto-electronic device within 40 samples only, whereas an Edisonian approach would have required about 1000 samples. This raises an important discussion on the necessity of autonomous platforms to accelerate Material science.

A Digital Twin to overcome long-time challenges in Photovoltaics

Abstract: The recent successes of emerging photovoltaics (PV) such as organic and perovskite solar cells are largely driven by innovations in material science. However, closing the gap to commercialization still requires significant innovation to match contradicting requirements such as performance, longevity and recyclability. The rate of innovation, as of today, is limited by a lack of design principles linking chemical motifs to functional microscopic structures, and by an incapacity to experimentally access microscopic structures from investigating macroscopic device properties. In this work, we envision a layout of a Digital Twin for PV materials aimed at removing both limitations. The layout combines machine learning approaches, as performed in materials acceleration platforms (MAPs), with mathematical models derived from the underlying physics and digital twin concepts from the engineering world. This layout will allow using high-throughput (HT) experimentation in MAPs to improve the parametrization of quantum chemical and solid-state models. In turn, the improved and generalized models can be used to obtain the crucial structural parameters from HT data. HT experimentation will thus yield a detailed understanding of generally valid structure-property relationships, enabling inverse molecular design, that is, predicting the optimal chemical structure and process conditions to build PV devices satisfying a multitude of requirements at the same time. After motivating our proposed layout of the digital twin with causal relationships in material science, we discuss the current state of the enabling technologies, already being able to yield insight from HT data today. We identify open challenges with respect to the multiscale nature of PV materials and the needed volume and diversity of data, and mention promising approaches to address these challenges.

Integrated System Built for Small-Molecule Semiconductors via High-Throughput Approaches.

Abstract: High-throughput synthesis of solution-processable structurally variable small-molecule semiconductors is both an opportunity and a challenge. A large number of diverse molecules provide a possibility for quick material discovery and machine learning based on experimental data. However, the diversity of the molecular structure leads to the complexity of molecular properties, such as solubility, polarity, and crystallinity, which poses great challenges to solution processing and purification. Here, we first report an integrated system for the high-throughput synthesis, purification, and characterization of molecules with a large variety. Based on the principle "Like dissolves like," we combine theoretical calculations and a robotic platform to accelerate the purification of those molecules. With this platform, a material library containing 125 molecules and their optical-electronic properties was built within a timeframe of weeks. More importantly, the high repeatability of recrystallization we design is a reliable approach to further upgrading and industrial production.

Overcoming Moisture‐induced Degradation in Organic Solar Cells

Abstract: Unencapsulated organic solar cells are prone to severe performance losses in the presence of moisture. We present accelerated damp heat (85 oC/85% RH) studies and show that the hygroscopic hole-transporting PEDOT:PSS layer is the origin of device failure in the case of prototypical inverted solar cells. Complementary measurements unveil that under these conditions a decreased PEDOT:PSS work function along with areas of reduced electrical contact between active layer and hole-transport layer are the main factors for device degradation rather than a chemical reaction of water with the active layer. We further explore replacements for PEDOT:PSS and find that tungsten oxide (WO3) or phosphomolybdic acid (PMA) – materials that can be processed from benign solvents at room temperature – yield comparable performance as PEDOT:PSS and enhance the resilience of solar cells under damp heat. The stability trend follows the order PEDOT:PSS << WO3 < PMA, with PEDOT:PSS based devices failing after few minutes, while PMA based devices remain nearly pristine over several hours. PMA is thus proposed as a robust, solution processable hole-extraction layer that can act as a one to one replacement of PEDOT:PSS to achieve organic solar cells with significantly improved longevity. This article is protected by copyright. All rights reserved.

Influence of tin oxide decoration on the junction conductivity of silver nanowires

Abstract: Flexible electrodes using nanowires (NWs) suffer from challenges of long-term stability and high junction resistance which limit their fields of applications. Welding via thermal annealing is a common strategy to enhance the conductivity of percolated NW networks, however, it affects the structural and mechanical integrity of the NWs. In this study we show that the decoration of NWs with an ultrathin metal oxide is a potential alternative procedure which not only enhances the thermal and chemical stability but, moreover, provides a totally different mechanism to reduce the junction resistance upon heat treatment. Here, we analyze the effect of SnO x decoration on the conductance of silver NWs and NW junctions by using a four-probe measurement setup inside a scanning electron microscope. Dedicated transmission electron microscopy analysis in plan-view and cross-section geometry are carried out to characterize the nanowires and the microstructure of the junctions. Upon heat treatment the junction resistance of both plain silver NWs and SnO x -decorated NWs is reduced by around 80%. While plain silver NWs show characteristic junction welding during annealing, the SnO x -decoration reduces junction resistance by a solder-like process which does not affect the mechanical integrity of the NW junction and is therefore expected to be superior for applications.

All Printed Photoanode/Photovoltaic Mini-Module for Water Splitting.

Abstract: Printing a large-area bismuth vanadate photoanode offers a promising approach for cost-effective photoelectrochemical (PEC) water splitting. However, the light absorption trade-off with charge transfer, as well as stability issues always lead to poor PEC efficiency. Here, the solution-processed recipe is advanced with BiI3 dopant for the printed deposition with controllable crystal growth. The resultant BiVO4 films prefer (001) orientation with nanorod feature on substrate, allowing a faster charge transfer and improved photocurrent. The BiVO4 photoanode in tandem with perovskite solar module delivers an operating photocurrent density of 5.88 mA cm-2 at zero bias in 3.11 cm2 active area under AM 1.5 G illumination, yielding a solar-to-hydrogen efficiency as high as 7.02% for unbiased water splitting. Equally important, the stability of the aged BiVO4 rods has been addressed to distinguish phase segregation at surface. The photocatalysis degradation composes of vanadium loss and Bi2 O3 enriching at the surface, opening a lid on the long-term stability of BiVO4 photoanodes.

Cutting 'lab-to fab' short: High Throughput Optimization and Process Assessment in Roll-to-Roll Slot Die Coating of Printed Photovoltaics

Abstract: Commercialization of printed photovoltaics requires knowledge of the optimal composition and microstructure of the single layers, and the ability to control these properties over large areas under industrial conditions. While microstructure optimization can be readily achieved by lab scale methods, the transfer from laboratory scale to a pilot production line ('lab to fab') is a slow and cumbersome process. Here, we show how we can optimize the performance of organic solar cells and at the same time assess process performance in a 2D combinatorial approach directly on an industrially relevant slot die coating line. This is enabled by a multi-nozzle slot die coating head allowing parameter variations along and across the web. This modification allows us to generate and analyze 3750 devices in a single coating run, varying the active layer donor:acceptor ratio and the thickness of the electron transport layer (ETL). We use Gaussian Process Regression (GPR) to exploit the whole dataset for precise determination of the optimal parameter combination. Performance-relevant features of the active layer morphology are inferred from UV-Vis absorption spectra. By mapping morphology in this way, small undesired gradients of process conditions (extrusion rates, annealing temperatures) are detected and their effect on device performance is quantified. The correlation between process parameters, morphology and performance obtained by GPR provides hints to the underlying physics, which are finally quantified by automated high-throughput drift-diffusion simulations. This leads to the conclusion that voltage losses which are observed for very thin ETL coatings are due to incomplete coverage of the electrode by the ETL, which cause enhanced surface recombination.

Highly Stable n–i–p Structured Formamidinium Tin Triiodide Solar Cells through the Stabilization of Surface Sn2+ Cations

Abstract: Improving the performance, reproducibility, and stability of Sn‐based perovskite solar cells (PSCs) with n–i–p structures is an important challenge. Spiro‐OMeTAD [2,2′,7,7′‐tetrakis(N,N‐di‐p‐methoxyphenyl‐amine)9,9′‐spirobifluorene], a hole transporting material (HTM) with n–i–p structure, requires the oxygen exposure after addition of Li‐TFSI [Lithium bis(trifluoromethanesulfonyl)imide] as a dopant to increase the hole concentration. In Sn‐based PSC, Sn2+ is easily oxidized to Sn4+ under such a condition, resulting in a sharp decrease in efficiency. Herein, a formamidinium tin triiodide (FASnI3)‐based PSCs fabricated using DPI‐TPFB [4‐Isopropyl‐4′‐methyldiphenyliodonium tetrakis(pentafluorophenyl)borate] instead of Li‐TFSI are reported as a dopant in Spiro‐OMeTAD. The DPI‐TPFB enables the fabrication of PSCs with an efficiency of up to 10.9%, the highest among FASnI3‐based PSCs with n–i–p structures. Moreover, ≈80% of the initial efficiency is maintained even after 1,597 h under maximum power point tracking conditions. In particular, the encapsulated device does not show any decrease in efficiency even after holding for 50 h in the 85 °C/85% RH condition. The high efficiency and excellent stability of PSCs prepared by doping with DPI‐TPFB are attributed to not only increasing electrical conductivity by acting as a Lewis acid, but also stabilizing Sn2+ through coordination with Sn2+ on the surface of FASnI3.

Bypassing the single junction limit with advanced photovoltaic architectures

Abstract: In single-junction photovoltaic (PV) devices, the maximum achievable power conversion efficiency (PCE) is mainly limited by thermalization and transmission losses, because polychromatic solar irradiation cannot be matched to a single bandgap. Several concepts are being investigated to reduce these losses, such as the classical vertical multijunction cells, 'lateral' tandem cells, and multi-exciton generation in the form of photon up- and down-conversion. While in theory, efficiencies exceeding 90% are possible (Landsberg or thermodynamic limit), there are severe practical limitations in terms of processability, cost, and spectral sensitivity. Here, we present a simulation environment based on Bayesian Optimization that is able to predict and optimize the electrical performance of multi-junction architectures, both vertical and lateral, in combination with multi-exciton materials. With respect to vertical stacks, we show that by optimizing bandgap energies of multi-exciton generation (MEG) layers, double junctions can reach efficiencies beyond those of five-junction tandem devices (57%). Moreover, such combinations of MEG and double junction devices would be highly resilient against spectral changes of the incoming sunlight. We point out three main challenges for PV material science to realize such devices. With respect to lateral architectures, we show that MEG layers might allow reducing nonradiative voltage losses following the Energy Gap Law. Finally, we show that the simulation environment is able to use machine learned quantitative structure-property relationships obtained from high-throughput experiments to virtually optimise the active layer (such as, the film thickness and the donor-acceptor ratio) for a given architecture. The simulation environment thus represents an important building block towards a digital twin of PV materials.

Impact of 2D Ligands on Lattice Strain and Energy Losses in Narrow‐Bandgap Lead–Tin Perovskite Solar Cells

Abstract: Mixed lead and tin (Pb/Sn) hybrid perovskites exhibit a great potential in fabricating all-perovskite tandem devices due to their easily tunable bandgaps. However, the energy deficit and instability in Pb/Sn perovskite solar cells (PSCs) constrain their practical applications, which renders defect passivation engineering indispensable to develop highly efficient and long-term stable PSCs. Herein, the mechanisms of strain tailoring and defect passivation in Pb/Sn PSCs by 2D ligands are investigated. The 2D ligands include electroneutral cations with long alkyl chain (LAC), iodates with relatively short alkyl chain (SAC) and their mixtures. This study reveals that LAC ligands facilitate the relaxation of tensile strain in perovskite films while SAC ligands cause strain buildup. By mixing LAC/SAC ligands, tensile strain in perovskite films can be balanced which improves solar cell performance. PSCs with admixed β-guanidinopropionic acid (GUA)/phenethylammonium iodide (PEAI) exhibit enhanced open circuit voltage and fill factor, which is attributed to reduced nonradiative recombination losses in the bulk and at the interfaces. Furthermore, the operational stability of PSCs is slightly improved by the mixed 2D ligands. This work reveals the mechanisms of 2D ligands in strain tailoring and defect passivation toward efficient and stable narrow-bandgap PSCs.

CO2 snow jet cleaning as a roll-to-roll compatible method for deburring IMI substrates after laser patterning

Abstract: Burring is commonly encountered upon patterning of dielectric-metal-dielectric (DMD) transparent electrodes by laser ablation. These burrs are conductive and thus lead to shunting of the (opto-)electronic devices built upon these electrodes. In this work, CO2 snow jet blasting is presented as a convenient and reliable method for deburring laser-patterned DMD electrodes during roll-to-roll manufacturing of organic solar modules. As CO2 snow jet blasting significantly reduces the extent of shunting and concomitantly avoids scratching the electrode, the photoelectrical conversion efficiencies of the solar modules thus produced are higher than those obtained for traditional deburring techniques.

Elucidating How Low Energy Offset Matters to Performance of Nonfullerene Acceptor-Based Solar Cells

Abstract: The energetic offset between the highest occupied molecular orbitals of the donor and acceptor components of organic photovoltaic blends is well-known to affect the device efficiency. It is well-established that a decreasing offset increases the open-circuit voltage but reduces the short-circuit current, which has been explained by insufficient exciton dissociation. However, the impact of the offset on the fill factor and underlying processes is less clear. Here, we study free charge generation and recombination in three different nonfullerene acceptors, Y6, ITIC, and o-IDBTR, blended with the same donor polymer PM6. We demonstrate that a diminishing offset results in field-dependent charge generation related to field-assisted exciton dissociation. On the other hand, reformation of excitons from free charges is identified as an additional channel for charge recombination, which goes along with a substantial rise in the bimolecular recombination coefficient. In combination of these two effects, the fill factor drops considerably with a decreasing energy offset. Using the comparison between PM6:ITIC and PM6:o-IDBTR, we show that bulk properties such as morphology and carrier mobilities can not fully explain the observed difference in performance, highlighting the importance of interfacial kinetics and thermodynamics in controlling the device efficiency, both through generation and recombination of charge carriers.

Understanding causalities in organic photovoltaics device degradation in a machine learning driven high-throughput platform.

Abstract: AAAA. This article is protected by copyright. All rights reserved.

Enhancing Planar Inverted Perovskite Solar Cells with Innovative Dumbbell‐Shaped HTMs: A Study of Hexabenzocoronene and Pyrene‐BODIPY‐Triarylamine Derivatives

Abstract: Dumbbell-shaped systems based on PAHs-BODIPY-triarylamine hybrids TM-(01-04) are designed as novel and highly efficient hole-transporting materials for usage in planar inverted perovskite solar cells. BODIPY is employed as a bridge between the PAH units, and the effects of the conjugated π-system's covalent attachment and size are investigated. Fluorescence quenching, 3D fluorescence heat maps, and theoretical studies support energy transfer within the moieties. The systems are extremely resistant to UVC 254 nm germicidal light sources and present remarkable thermal stability at degradation temperatures exceeding 350 °C. Integrating these systems into perovskite solar cells results in outstanding power conversion efficiency (PCE), with TM-02-based devices exhibiting a PCE of 20.26%. The devices base on TM-01, TM-03, and TM-04 achieve PCE values of 16.98%, 17.58%, and 18.80%, respectively. The long-term stability of these devices is measured for 600 h, with initial efficiency retention between 94% and 86%. The TM-04-based device presents noticeable stability of 94%, better than the reference polymer PTAA with 91%. These findings highlight the exciting potential of dumbbell-shaped systems based on PAHs-BODIPY-triarylamine derivatives for next-generation photovoltaics.

Quasi-2D Lead-Tin Perovskite Memory Devices Fabricated by Blade Coating.

Abstract: Two terminal passive devices are regarded as one of the promising candidates to solve the processor-memory bottleneck in the Von Neumann computing architectures. Many different materials are used to fabricate memory devices, which have the potential to act as synapses in future neuromorphic electronics. Metal halide perovskites are attractive for memory devices as they display high density of defects with a low migration barrier. However, to become promising for a future neuromorphic technology, attention should be paid on non-toxic materials and scalable deposition processes. Herein, it is reported for the first time the successful fabrication of resistive memory devices using quasi-2D tin-lead perovskite of composition (BA)2 MA4 (Pb0.5 Sn0.5 )5 I16 by blade coating. The devices show typical memory characteristics with excellent endurance (2000 cycles), retention (105 s), and storage stability (3 months). Importantly, the memory devices successfully emulate synaptic behaviors such as spike-timing-dependent plasticity, paired-pulse facilitation, short-term potentiation, and long-term potentiation. A mix of slow (ionic) transport and fast (electronic) transport (charge trapping and de-trapping) is proven to be responsible for the observed resistive switching behavior.

Aerosol‐Jet‐Printed Encapsulation of Organic Photovoltaics

Abstract: Organic electronic devices (OEDs) are prone to oxygen- and water-induced degradation and therefore need to be encapsulated with barrier materials. In this work, we develop an aerosol jet (AJ) printing process to coat perhydropolysilazane (PHPS) directly onto OEDs by adapting the print setup and systematically optimizing the process parameters. Furthermore, we develop a novel curing process that converts PHPS to silica barrier layers by combining damp heat exposure with subsequent vacuum-UV irradiation. This two-step treatment is shown to be considerably faster and gentler than the state-of-the-art curing processes and also yields a quantitatively higher conversion. Both the printing and the conversion process are fully compatible with OED devices, which is demonstrated by a damage-free direct encapsulation of organic solar cells. The encapsulated cells show a significant reduction of degradation in damp heat conditions (65 °C/ 85% r.h.), maintaining >95% of their initial performance for >100 h. Complementary electroluminescence measurements reveal that the AJ-printed barrier layers effectively prevent lateral water ingress into the devices. This work provides the proof of principle that AJ printing can be used to print barrier layers directly onto OEDs and is thus an industrially highly relevant technology to precisely encapsulate such devices even on 3D objects. This article is protected by copyright. All rights reserved.

Practical limits of multijunction solar cells

Abstract: Multijunction solar cells offer a path to very high conversion efficiency, exceeding 60% in theory. Under ideal conditions, efficiency increases monotonically with the number of junctions. In this study, we explore technical and economic mechanisms acting on tandem solar cells. We find that these mechanisms produce limitations that are the more pronounced the greater the number of junction is and, hence, limit the ideal number of junctions, as well as the corresponding efficiencies. Spectral variations induce current losses in series-connected tandem solar cells. For Denver, we find that these losses reduce achievable harvesting efficiencies to 51% for non-concentrated light, and that they restrict the ideal number of junctions to less than nine. Independently operated solar cells suffer from optical losses with similar consequences. Optical efficiencies of 99% restrict the ideal number of junctions to below ten, and reduce achievable efficiencies by more than 10%. Only architectures with a sequential cell illumination are more resilient to these losses. Restricting available materials reveals that a sufficiently low band gap for the bottom cell of 0.9 eV or below is expedient to realize high efficiencies. Economic considerations show that five junctions or less are economically ideal for most conceivable applications. Hosted file pip-22-458-File001.docx available at https://authorea.com/users/563094/articles/610294practical-limits-of-multijunction-solar-cells

Double-Cable Conjugated Polymers Based on Simple Non-Fused Electron Acceptors for Single-Component Organic Solar Cells

Abstract: In this work, a non-fused electron acceptor with near-infrared absorption was introduced into double-cable conjugated polymers for single-component organic solar cells (SCOSCs). The non-fused electron acceptor contains a simple thienyl-phenyl-thienyl core with 2-(3-oxo-2,3-dihydroinden-1-ylidene)malononitrile (IC) as the end group, which was used as the side unit to create double-cable conjugated polymers. In addition, poly(benzodithiophene) was selected as the conjugated backbone, in which the number of chlorine (Cl) atoms was varied to tune the optical and electronic properties. The new double-cable polymers were successfully applied in SCOSCs, providing an efficiency of over 8% with a broad photoresponse from 300 to 800 nm. When the number of Cl atoms on the repeat unit was increased from 2 to 3, the open-circuit voltage was enhanced to 1.01 V, yielding a low voltage loss of 0.59 eV, while the efficiency was reduced to 5.28%. The reduced performance is explained by the increased charge recombination in this polymer, as observed by transient absorption spectroscopy. This work reports a set of IC-based NIR double-cable conjugated polymers, which inspire material design toward more efficient SCOSCs.

Unraveling the Role of Non-Fullerene Acceptor with High Dielectric Constant in Organic Solar Cells.

Abstract: Increasing the relative dielectric constant is a constant pursuit of organic semiconductors, but it often leads to multiple changes in device characteristics, hindering the establishment of a reliable relationship between dielectric constant and photovoltaic performance. Herein, a new non-fullerene acceptor named BTP-OE is reported by replacing the branched alkyl chains on Y6-BO with branched oligoethylene oxide chains. This replacement successfully increases the relative dielectric constant from 3.28 to 4.62. To surprise, BTP-OE offers consistently lower device performance relative to Y6-BO in organic solar cells (16.27% vs 17.44%) due to the losses in open-circuit voltage and fill factor. Further investigations unravel that BTP-OE has resulted in reduced electron mobility, increased trap density, enhanced first order recombination, and enlarged energetic disorder. These results demonstrate the complex relationship between dielectric constant and device performance, which provide valuable implications for the development of organic semiconductors with high dielectric constant for photovoltaic application.

Aerial photoluminescence imaging of photovoltaic modules

Abstract: On-site imaging of modules in photovoltaic systems requires contact-free techniques with high-throughput and low-cost for commercial relevance. Photoluminescence imaging satisfies these requirements, but it has so far not been used for aerial imaging. Such a system faces unique engineering and operating challenges, including the need to mount a light source on the drone and identifying module defects from images taken under low- and non-uniform irradiance. In this study, we present our in-house developed PLAI (photoluminescence aerial imaging) setup and we demonstrate that it can be used to identify defects even with a difference of excitation intensity of up to 50%. The setup consists of a hexa-copter aerial drone equipped with an illumination unit and a near-infrared camera. The unit is capable of partially illuminating full size modules at night and capturing the photoluminescence response. In the maiden flight, we achieved a throughput of 13.6 PV modules per minute, and we estimate that a throughput of 300 PV modules per minute is feasible. We show that the setup can be used to detect and identify cracks and potential-induced-degradation with high levels of confidence. We verify these findings by cross correlation and comparing captured photoluminescence images to electroluminescence images taken indoors. This article is protected by copyright. All rights reserved.

Highly Efficient Bilayer Polymer Solar Cells Using the Method of Sequential Processing with Additive Bilayer

Abstract: Despite the research value of bilayer organic solar cells (OSCs) for commercialization in the future, the bulk‐heterojunction (BHJ) structure dominates the fabrication of OSCs because of its higher power conversion efficiency (PCE) compared with bilayer OSCs. Herein, four different types of bilayer OSC structures using sequential processing (SP) with an additive bilayer are investigated and considerably enhanced device performance is demonstrated. The performance of our bilayer devices based on a wide bandgap (PBDT‐DPPD‐TPD; P2) polymer and [6,6]‐phenyl C61‐butyric acid methyl ester (PCBM) is improved from 2.88% for the conventional bilayer structure to 6.62%. More importantly, remarkable PCEs of 8.78% and 15.16% for PTB7‐Th/PCBM and PM6/Y6 bilayer OSCs, respectively, using the SP with additive bilayer method are achieved and the inhomogeneity issues of the BHJ structure are successfully addressed. Herein, a novel way to overcome the low efficiency of bilayer OSCs is suggested and an unprecedented possibility of renovation, breaking the standardization of OSC research, is presented.

An Insight into Temperature Dependence of Photoluminescence of a Highly-Emissive Cs-Ag(Na)Bi(In)Cl6 Perovskite

Abstract: THE TEMPERATURE-DEPENDENT EVOLUTION OF PHOTOLUMINESCENCE (PL) PROPERTIES OF HIGHLY EMISSIVE CS2AG0.35NA0.65BI0.02IN0.98CL6 PEROVSKITE WAS EXAMINED IN THE RANGE OF 80-340 K. THE PL MAXIMUM EXHIBITED SHIFTED TO HIGHER ENERGIES WITH AN...

Rationale for Highly Efficient and Outdoor-Stable Terpolymer Solar Cells

Abstract: Random terpolymerization is an effective approach to achieving highly efficient and outdoor-stable terpolymer photovoltaics. However, the working principle behind this remains unclear. Herein, we report spectroscopic, morphological, and computational results...