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8 result(s) for "Simmonds, Maxim"
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Tailored Crystallization Dynamics for Efficient and Stable DMSO‐Free Tin Perovskite Solar Cells
Tin perovskite solar cells are emerging as a sustainable lead‐free alternative in thin film photovoltaics. DMSO‐free processed tin perovskites are gaining interest due to the detrimental effects of DMSO on tin oxidation. However, replacing DMSO with other solvents remains challenging due to the accelerated crystallization dynamics in non‐DMSO systems. In this study, the crystallization process in a DMSO‐free solvent system is regulated by managing the transition from the sol‐gel phase to the solid film. Specifically, piperazine dihydriodide (PDAI) and 4‐tert‐butylpyridine (tBP) are utilized to coordinately tune the colloidal chemistry through forming large pre‐nucleation clusters in perovskite ink, further, facilitating the film formation process. By combining tBP and PDAI, a controllable crystallization rate is achieved as evidenced by in situ photoluminescence (PL) measurement during spin‐coating. As a result, tin perovskite films show high crystallinity and improved microstructure. Devices treated with tBP+PDAI exhibit a champion power conversion efficiency of 7.8% and excellent stability without observable degradation for over 3000 h stored in the N2 glovebox. These findings advance understanding and managing crystallization in DMSO‐free solvents processed tin perovskite solar cells. In this work, the authors investigated the crystallization process of tin perovskites in a DMSO‐free solvent system using in situ PL technique. The authors discovered that a synergistic approach effectively facilitates the formation of high‐quality DMSO‐free tin perovskite films by modulating the emergence of crystallites and the aggregation process. As a result, they achieved efficient and stable tin devices without DMSO.
Photodegradation of 2D Ruddlesden‐Popper Perovskites: Consequences and Design Principles for Photoelectrochemical Applications
Halide perovskites (HaP), with their exceptional optoelectronic properties and high‐power conversion efficiencies in photovoltaic devices, hold promise for photoelectrochemical (PEC) applications in green fuel and chemical production. However, their stability in aqueous environments remains a challenge. This study investigates the stability and degradation mechanisms of the 2D Ruddlesden‐Popper phase phenylethyl ammonium lead iodide (PEA(+)2PbI4) thin films in aqueous electrolytes under dark and illuminated conditions. While PEA(+)2PbI4 thin films appear to be thermodynamically stable in an aqueous electrolyte with phenylethyl ammonium iodide (PEAI), illumination causes significant photodegradation generating a deprotonated and dehalogenated 2D intercalation product: phenylethylamine‐lead iodide, 2PEA(0)‐PbI2. The degradation of the 2D semiconductor leads to substantial reduction in the photovoltage, adversely impacting the material performance in photoelectrochemical (PEC) devices. To intercept photo‐excited charge carriers in the 2D semiconductor, the I3−/I− redox is added, which reduced photodegradation. The findings underscore that while catalytic reactions at halide perovskite electrodes in aqueous electrolytes are feasible, reversible and irreversible photodegradation remains a critical limitation that must be addressed in the design of PEC devices employing metal halide semiconductor layers for direct electrochemical energy conversion. In this study, we examined the structural and morphological stability of the 2D perovskite‐phenylethylammonium lead iodide PEA(+)2PbI4 thin films in aqueous electrolytes of phenylethylammonium iodide (PEA(+)I), both in the dark and under illumination. In dark conditions, the material remains stable due to dynamic equilibrium with the species in solution. However, under illumination, we demonstrate the formation of an intercalated phase 2PEA(0)−PbI2, which affects device performance. This work presents insightful design principles for utilizing 2D perovskite materials in photoelectrochemical applications.
Co‐Doping Approach for Enhanced Electron Extraction to TiO2 for Stable Inorganic Perovskite Solar Cells
Inorganic perovskite CsPbI3 solar cells hold great potential for improving the operational stability of perovskite photovoltaics. However, electron extraction is limited by the low conductivity of TiO2, representing a bottleneck for achieving stable performance. In this study, a co‐doping strategy for TiO2 using Nb(V) and Sn(IV), which reduces the material's work function by 80 meV compared to Nb(V) mono‐doped TiO2, is introduced. To gain fundamental understanding of the processes at the interfaces between the perovskite and charge‐selective layer, transient surface photovoltage measurements are applied, revealing the beneficial effect of the energetic and structural modification on electron extraction across the CsPbI3/TiO2 interface. Using 2D drift‐diffusion simulations, it is found that co‐doping reduces the interface hole recombination velocity by two orders of magnitude, increasing the concentration of extracted electrons by 20%. When integrated into n–i–p solar cells, co‐doped TiO2 enhances the projected TS80 lifetimes under continuous AM1.5G illumination by a factor of 25 compared to mono‐doped TiO2. This study provides fundamental insights into interfacial charge extraction and its correlation with operational stability of perovskite solar cells, offering potential applications for other charge‐selective contacts. TiO2 is highly relevant in photoelectrochemistry, (photo)catalysis, and sensor applications, where high conductivity is crucial. Herein, a co‐doping strategy for TiO2 using Nb(V) and Sn(IV) is developed, enhancing electron extraction from perovskite and improving solar cell efficiency and stability. Using transient surface photovoltage and drift‐diffusion simulations, buried interfaces are characterized and critical charge transport parameters for optoelectronic advancements are extracted.
Co‐Doping Approach for Enhanced Electron Extraction to TiO 2 for Stable Inorganic Perovskite Solar Cells
Inorganic perovskite CsPbI 3 solar cells hold great potential for improving the operational stability of perovskite photovoltaics. However, electron extraction is limited by the low conductivity of TiO 2 , representing a bottleneck for achieving stable performance. In this study, a co‐doping strategy for TiO 2 using Nb(V) and Sn(IV), which reduces the material's work function by 80 meV compared to Nb(V) mono‐doped TiO 2 , is introduced. To gain fundamental understanding of the processes at the interfaces between the perovskite and charge‐selective layer, transient surface photovoltage measurements are applied, revealing the beneficial effect of the energetic and structural modification on electron extraction across the CsPbI 3 /TiO 2 interface. Using 2D drift‐diffusion simulations, it is found that co‐doping reduces the interface hole recombination velocity by two orders of magnitude, increasing the concentration of extracted electrons by 20%. When integrated into n–i–p solar cells, co‐doped TiO 2 enhances the projected T S80 lifetimes under continuous AM1.5G illumination by a factor of 25 compared to mono‐doped TiO 2 . This study provides fundamental insights into interfacial charge extraction and its correlation with operational stability of perovskite solar cells, offering potential applications for other charge‐selective contacts.
Monitoring charge separation of individual cells in perovskite/silicon tandems via transient surface photovoltage spectroscopy
Identification of charge carrier separation processes in perovskite/silicon tandem solar cells and recombination at buried interfaces of charge selective contacts is crucial for photovoltaic research. Here, intensity- and wavelength- dependent transient surface photovoltage (tr-SPV) is used to investigate slot-die-coated perovskite top layers deposited on n-type Heterojunction Silicon bottom cells. We show that using an appropriate combination of photon energy and/or bottom cell polarity, one can individually probe the buried interfaces of the bottom silicon cell or the perovskite`s buried interfaces of a tandem solar cell: For excitation with higher energy photons, time delays before the onset of a strong SPV signal indicate significant hole minority drift before separation in the silicon bottom cells. Furthermore, symmetric bottom Si heterojunction solar cell stacks can serve to investigate the top perovskite stack including its junction to the bottom cell, unhampered by photovoltages from the silicon substrate. Thus, investigation of the buried interfaces in tandem devices using time-resolved surface photovoltage is found to yield valuable information on charge carrier extraction at buried interfaces and demonstrates its unique potential compared to more conventional approaches that rely on photoluminescence decay kinetics.
Unlocking High-Throughput Heterojunction Discovery
Photoluminescence (PL) is a ubiquitous proxy for material quality in optoelectronic devices, widely used for high-throughput materials discovery. However, we demonstrate that in the presence of charge-selective contacts, PL loses its predictive reliability and can exhibit strong quenching even in highly efficient photovoltaic devices under open-circuit conditions. By combining steady-state and transient PL with contactless transient surface photovoltage measurements we disentangle the intertwined processes of extraction and recombination, clarifying the physical origin of this phenomenon. This joint approach reveals extraction dynamics not captured by PL alone. A digital replica of the interface shows that Coulomb attraction and interfacial recombination are the fundamental mechanisms driving quenching after charge extraction. Based on these insights, we present a decision tree for heterojunction classification and PL interpretation applicable across diverse optoelectronic systems, including photovoltaics, photodetectors, and LEDs. Our approach supports systematic screening and optimization of half-devices, bridging the gap between accelerated materials discovery and accelerated device discovery.
Mars Science Laboratory Mission and Science Investigation
Scheduled to land in August of 2012, the Mars Science Laboratory (MSL) Mission was initiated to explore the habitability of Mars. This includes both modern environments as well as ancient environments recorded by the stratigraphic rock record preserved at the Gale crater landing site. The Curiosity rover has a designed lifetime of at least one Mars year (∼23 months), and drive capability of at least 20 km. Curiosity ’s science payload was specifically assembled to assess habitability and includes a gas chromatograph-mass spectrometer and gas analyzer that will search for organic carbon in rocks, regolith fines, and the atmosphere (SAM instrument); an x-ray diffractometer that will determine mineralogical diversity (CheMin instrument); focusable cameras that can image landscapes and rock/regolith textures in natural color (MAHLI, MARDI, and Mastcam instruments); an alpha-particle x-ray spectrometer for in situ determination of rock and soil chemistry (APXS instrument); a laser-induced breakdown spectrometer to remotely sense the chemical composition of rocks and minerals (ChemCam instrument); an active neutron spectrometer designed to search for water in rocks/regolith (DAN instrument); a weather station to measure modern-day environmental variables (REMS instrument); and a sensor designed for continuous monitoring of background solar and cosmic radiation (RAD instrument). The various payload elements will work together to detect and study potential sampling targets with remote and in situ measurements; to acquire samples of rock, soil, and atmosphere and analyze them in onboard analytical instruments; and to observe the environment around the rover. The 155-km diameter Gale crater was chosen as Curiosity’s field site based on several attributes: an interior mountain of ancient flat-lying strata extending almost 5 km above the elevation of the landing site; the lower few hundred meters of the mountain show a progression with relative age from clay-bearing to sulfate-bearing strata, separated by an unconformity from overlying likely anhydrous strata; the landing ellipse is characterized by a mixture of alluvial fan and high thermal inertia/high albedo stratified deposits; and a number of stratigraphically/geomorphically distinct fluvial features. Samples of the crater wall and rim rock, and more recent to currently active surface materials also may be studied. Gale has a well-defined regional context and strong evidence for a progression through multiple potentially habitable environments. These environments are represented by a stratigraphic record of extraordinary extent, and insure preservation of a rich record of the environmental history of early Mars. The interior mountain of Gale Crater has been informally designated at Mount Sharp, in honor of the pioneering planetary scientist Robert Sharp. The major subsystems of the MSL Project consist of a single rover (with science payload), a Multi-Mission Radioisotope Thermoelectric Generator, an Earth-Mars cruise stage, an entry, descent, and landing system, a launch vehicle, and the mission operations and ground data systems. The primary communication path for downlink is relay through the Mars Reconnaissance Orbiter. The primary path for uplink to the rover is Direct-from-Earth. The secondary paths for downlink are Direct-to-Earth and relay through the Mars Odyssey orbiter. Curiosity is a scaled version of the 6-wheel drive, 4-wheel steering, rocker bogie system from the Mars Exploration Rovers (MER) Spirit and Opportunity and the Mars Pathfinder Sojourner . Like Spirit and Opportunity , Curiosity offers three primary modes of navigation: blind-drive, visual odometry, and visual odometry with hazard avoidance. Creation of terrain maps based on HiRISE (High Resolution Imaging Science Experiment) and other remote sensing data were used to conduct simulated driving with Curiosity in these various modes, and allowed selection of the Gale crater landing site which requires climbing the base of a mountain to achieve its primary science goals. The Sample Acquisition, Processing, and Handling (SA/SPaH) subsystem is responsible for the acquisition of rock and soil samples from the Martian surface and the processing of these samples into fine particles that are then distributed to the analytical science instruments. The SA/SPaH subsystem is also responsible for the placement of the two contact instruments (APXS, MAHLI) on rock and soil targets. SA/SPaH consists of a robotic arm and turret-mounted devices on the end of the arm, which include a drill, brush, soil scoop, sample processing device, and the mechanical and electrical interfaces to the two contact science instruments. SA/SPaH also includes drill bit boxes, the organic check material, and an observation tray, which are all mounted on the front of the rover, and inlet cover mechanisms that are placed over the SAM and CheMin solid sample inlet tubes on the rover top deck.