Axel F. Palmstrom

Nickel oxide (NiO _x ) is a common hole transport layer (HTL) in perovskite photovoltaics, but the chemical reactivity of NiOx surfaces accelerates degradation when contacting perovskites. We developed an ultrathin, conformal tin oxide (SnO _x ) interlayer to suppress interfacial reactivity between NiO _x and perovskite. SnO _x is typically an electron transport layer, but we show that the energy alignment can be modified for hole extraction using molecules with dipoles. This synergy yielded high efficiency in perovskite photovoltaic devices and showed an ~10x improvement in T 90 lifetime in open-circuit conditions under AM1.5G at 65°C. This structure also improves resilience to thermomechanical durability, as minimodules retained 95.7% of their initial performance after 1000 thermal cycles (−65° to 85°C), highlighting the importance of interfaces for robust perovskite photovoltaic modules.

Current encapsulation architectures for thin‐film metal halide perovskite do not adequately eliminate all ambient stressors. Here, we develop low transmission rate barrier layers using atomic layer deposited (ALD) aluminum oxide grown directly on the completed photovoltaic (PV) device stack to provide an additional seal, prior to full packaging. We investigate the effect of deposition temperature and oxidant chemistries on the barrier growth for protection of perovskite photovoltaic devices. We characterize the layers individually, then integrate into devices to detail the tradeoff between protection and deposition compatibility. To enhance compatibility and impermeability, we present an approach using water as the aluminum oxidant during nucleation and switching from water to ozone for the remainder of the growth. At 50 nm, the barrier results in a water vapor transmission rate (WVTR) of 4.5·10 ⁻⁴ g/m ² /day, and 1,000‐hour device stability under 45°C with 85% relative humidity without further packaging. This barrier provides sufficient protection to enable minimal degradation of the perovskite solar cells while completely submerged in water for 140 minutes. Additionally, we characterize the oxygen transmission rate (OTR) to be 0.49 cm ³ /m ² /day at 23°C and 0% relative humidity, which is 1.5 orders of magnitude improvement over the OTR of the current encapsulation.

The stability of metal-halide-perovskite (MHP) solar cells must be understood and improved for the commercial viability of MHP technologies. Here, we apply multiscale characterization methods to study degradation modes, specifically electrode corrosion, for p-i-n MHP partial device stacks and full devices that are stored in the dark under an inert atmosphere. Our multiscale characterization approaches include full-device electro-optical performance using current–voltage (JV) curves and spatial imaging with electroluminescence (EL) and photoluminescence (PL). We further correlate interface properties using cross-sectional Kelvin probe force microscopy, which maps the nanoscale electric field properties, and electron microscopy, which demonstrates structural and chemical features. Devices stored as a full device stack degrade primarily by metal (Ag) electrode diffusion into the absorber, with formation of AgI byproducts and Ag accumulation near the indium tin oxide (ITO) contact. This causes decomposition of the perovskite absorber domains, loss of the potential drop at the electron transport layer (ETL)/perovskite interface near the metal contact, and increased equivalent resistance at the perovskite/hole transport layer (HTL) interface near the ITO contact. The devices stored without metal show a different degradation pathway dominated by corrosion of the ITO, creating voids at the ITO electrode surface with diffusion of In and Sn into the absorber. We conclude that metal electrode-induced degradation is the most severe degradation pathway under dark storage, but that ITO corrosion and absorber instability must also be mitigated. We further demonstrate mitigation of these degradation pathways by changes to the device stack, including a SnO _x blocking layer at the ETL side and replacing ITO with FTO at the HTL side. These results provide a useful demonstration of specific dark degradation pathways at each electrode interface, as well as a unique multiscale example that links degradation of chemical, structural, and electrical interface properties to the full-device electro-optical characteristics.

An in situ electrical bias was placed on a perovskite device through the device thickness while under investigation with time-of-flight secondary ion mass spectrometry. The applied bias resulted in an observed reversible migration of halide and lithium ions on the timescale of minutes. The results show a framework that can be used for further study of ion migration in perovskite materials and devices. Graphical abstract

Though power conversion is an important metric for photovoltaic windows, it must be balanced with visible transmittance, aesthetics (color and haze), and thermal performance. Optical properties are often reported, but thermal performance is typically neglected entirely in photovoltaic window design. Here, we introduce the strategy of using laminate layers to improve the thermo-optical performance of perovskite-based photovoltaic insulating glass units. We design the laminates and insulating glass units by coupling a transfer matrix method optical model to a 1D heat transfer model. We validate our models with experimental fabrication of one-dimensional photonic crystal layers that are deposited on glass and laminated to the perovskite photovoltaic device. The holistic designs neutralize the inherent transmissive red color, and the "red low-e" design dramatically reduce emissivity of the glass surface to significantly improve thermal insulation and boost the photocurrent of the device.