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Sb2Se3 has become a promising absorber layer material for photovoltaic applications because of its attractive optical properties and rapid improvement in Sb2Se3 solar cell efficiency in recent years. The indirect bandgap and Urbach energy of Sb2Se3 have been determined to be 1.12 eV and 21.1 meV, respectively, using photothermal deflection spectroscopy. Above bandgap critical points at 1.48, 2.00, 2.35, 2.87, and 3.86 eV are identified from the complex dielectric function (e = e1 + ie2) spectra of thin film Sb2Se3 obtained from spectroscopic ellipsometry. Spectra in e serve as input for external quantum efficiency (EQE) simulations of substrate type Sb2Se3 solar cells. Comparison of experimental and simulated EQE quantifies carrier collection losses and identifies a carrier collection length in the absorber layer of 439 ± 4 nm and a 96.4 ± 0.2 % carrier collection probability near the heterojunction.

Perovskite solar cell device performance is affected by optical and electronic losses. To minimize these losses in solar cells, it is important to identify their sources. Here, we report the optical and electronic losses arising from physically mixed interfacial layers between the adjacent component materials in highly efficient two terminal (2T) all-perovskite tandem, single-junction wide-bandgap, and single-junction narrow-bandgap perovskite-based solar cells. Physically mixed interfacial layers as the sources of optical and electronic losses are identified from spectroscopic ellipsometry measurements and data analysis followed by comparisons of simulated and measured external quantum efficiency spectra. Parasitic absorbance in the physically mixed regions between silver metal electrical contacts and electron transport layers (ETLs) near the back contact and a physical mixture of commercial indium tin oxide and hole transport layers (HTL) near the front electrical contact lead to substantial optical loss. A lower-density void + perovskite nucleation layer formed during perovskite deposition at the interface between the perovskite absorber layer and the HTL causes electronic losses because of incomplete collection of photogenerated carriers likely originating from poor coverage and passivation of the initially nucleating grains.

High-performance perovskite/perovskite tandem solar cells require high-efficiency and stable low-bandgap perovskite subcells. State-of-the-art low-bandgap mixed tin–lead iodide perovskite solar cells exhibit either a high power-conversion efficiency or improved stability, but not both. Here we report a two-step bilayer interdiffusion growth process to simultaneously meet both requirements for formamidinium-based low-bandgap mixed tin–lead iodide perovskite solar cells. The bilayer interdiffusion growth process allows for the formation of high-quality and large-grained perovskite films with only 10 mol% volatile methylammonium. Additionally, one-dimensional pyrrolidinium perovskite was applied to passivate the perovskite film and improve the junction quality, which resulted in a carrier lifetime of 1.1 μs and an open circuit voltage of 0.865 V for our perovskite film and device with a bandgap of 1.28 eV. Our strategies enabled a power-conversion efficiency of 20.4% for low-bandgap perovskite solar cells under AM 1.5G illumination. More importantly, an encapsulated device can retain 92% of its initial efficiency after 450 h of continuous 1 sun illumination. Low-bandgap tin–lead perovskites are key to all-perovskite tandem solar cells but simultaneous improvement in efficiency and stability has proven challenging. Now, Li et al. fabricate tin–lead perovskite cells with reduced methylammonium content that are 20.4% efficient and stable under illumination for 450 h.

The Urbach energy indicating the width of the exponentially decaying sub-bandgap absorption tail is commonly used as the indicator of electronic quality of thin-film materials used as absorbers in solar cells. Urbach energies of hybrid inorganic-organic metal halide perovskites with various anion-cation compositions are measured by photothermal deflection spectroscopy. The variation in anion-cation composition has a substantial effect on the measured Urbach energy and hence the electronic quality of the perovskite. Depending upon the compositions, the Urbach energy varies from 18 to 65 meV for perovskite films with similar bandgap energies. For most of the perovskite compositions studied here including methylammonium (MA) + formamidinium (FA)-based Pb iodides, mixed Sn + Pb narrow-bandgap perovskites with low or intermediate Sn contents, and wide-bandgap FA + Cs- and I + Br-based perovskites, the correlation between the Urbach energy of the perovskite thin film and open-circuit voltage (

Optical characterization and simulations have been applied to study formamidinium + cesium lead triiodide (FA1-xCsxPbI3) perovskite based thin films and solar cells. Near infrared to ultraviolet complex dielectric function (e = e1 + ie2) spectra of varying cesium-to-formamidinium ratios in solution processed perovskite thin films have been extracted. Analysis of these e spectra track changes in the positions of critical point (CP) energies, including band gaps and above band gap transitions, with increasing cesium contents. Band gap values are identified as the lowest energy CP, with additional sub-gap features attributed to the presence of defects. Absorption onset values, for which absorption coefficient (α) = 4000 cm−1, are extracted, with x = 0.2 showing the sharpest absorption edge and the least contribution to absorption from defects below the band gap. External quantum efficiency (EQE) simulations of solar cells using e spectra as input are compared to experimental results and corroborate that the observed sub-gap absorption is due to defects as it does not contribute to EQE.

Multi-junction all-perovskite tandem solar cells are a promising choice for next-generation solar cells with high efficiency and low fabrication cost. However, the lack of high-quality low-bandgap perovskite absorber layers seriously hampers the development of efficient and stable two-terminal monolithic all-perovskite tandem solar cells. Here, we report a bulk-passivation strategy via incorporation of chlorine, to enlarge grains and reduce electronic disorder in mixed tin–lead low-bandgap (~1.25 eV) perovskite absorber layers. This enables the fabrication of efficient low-bandgap perovskite solar cells using thick absorber layers (~750 nm), which is a requisite for efficient tandem solar cells. Such improvement enables the fabrication of two-terminal all-perovskite tandem solar cells with a champion power conversion efficiency of 21% and steady-state efficiency of 20.7%. The efficiency is retained to 85% of its initial performance after 80 h of operation under continuous illumination. Two-terminal monolithic all-perovskite tandem solar cells are attractive due to their flexible nature and low-cost fabrication. Here the authors develop a process to obtain high-quality Sn–Pb perovskite thin films by incorporating chlorine. Such layers are employed to fabricate 20.7%-efficient tandem cells with 80 h operational stability.

Narrow bandgap mixed tin (Sn) + lead (Pb) perovskites are necessary for the bottom sub-cell absorber in high efficiency all-perovskite polycrystalline tandem solar cells. We report on the impact of mixed cation composition and atmospheric exposure of perovskite films on sub-gap absorption in films and performance of solar cells based on narrow bandgap mixed formamidinium (FA) + methylammonium (MA) and Sn + Pb halide perovskites, (FASnI

In situ real-time spectroscopic ellipsometry (RTSE) measurements have been conducted on MAPbI3, MA0.7FA0.3PbI3, and (FAPbI3)0.95(MAPbBr3)0.05 perovskite thin films when exposed to different levels of relative humidity at given temperatures over time. Analysis of RTSE measurements track changes in the complex dielectric function spectra and structure, which indicate variations in stability influenced by the underlying material, preparation method, and perovskite composition. MAPbI3 and MA0.7FA0.3PbI3 films deposited on commercial fluorine-doped tin oxide coated glass are more stable than corresponding films deposited on soda lime glass directly. (FAPbI3)0.95(MAPbBr3)0.05 films on soda lime glass showed improved stability over the other compositions regardless of the substrate, and this is attributed to the preparation method as well as the final composition.

Optical characterization and simulations have been applied to study formamidinium + cesium lead triiodide (FA}1}$X \mathbf{Cs} X$textbf{PbI3}\textbf{) perovskite thin films and solar cells. Near infrared to ultraviolet complex index of refraction ($N = n +_{\mathbf{\, }} ik$) spectra of varying cesium-to-formamidinium ratios in solution processed perovskite thin films have been extracted. Critical point transitions and the absorption onset are extracted, with $x =$ 0.2 showing the sharpest absorption edge and least contribution from defects to absorption near the band edge. External quantum efficiency simulations of perovskite based solar cells using optical properties as input are performed and compared to experimental device results.

The phenomenon of spontaneously growing metal whiskers (MW) raises significant reliability concerns due to its related arcing and shorting in electric equipment. The growth kinetics of MW remains poorly predictable. Here we present a theory describing the earlier observed intermittent growth of MW as caused by local energy barriers related to variations in the random electric fields generated by surface imperfections. We find the probabilistic distribution of MW stopping times, during which MW growth halts, which is important for reliability projections., 4 pages, 3 figures

Narrow bandgap mixed tin (Sn) + lead (Pb) perovskites are necessary for the bottom sub-cell absorber in high efficiency all-perovskite polycrystalline tandem solar cells. We report on the impact of mixed cation composition and atmospheric exposure of perovskite films on sub-gap absorption in films and performance of solar cells based on narrow bandgap mixed formamidinium (FA) + methylammonium (MA) and Sn + Pb halide perovskites, (FASnI3)x(MAPbI3)1-x. Structural and optical properties of 0.3 ≤ x ≤ 0.8 (FASnI3)x(MAPbI3)1-x perovskite thin film absorbers with bandgaps ranging from 1.25 eV (x = 0.6) to 1.34 eV (x = 0.3) are probed with and without atmospheric exposure. Urbach energy, which quantifies the amount of sub-gap absorption, is tracked for pristine perovskite films as a function of composition, with x = 0.6 and 0.3 demonstrating the lowest and highest Urbach energies of 23 meV and 36 meV, respectively. Films with x = 0.5 and 0.6 compositions show less degradation upon atmospheric exposure than higher or lower Sn-content films having greater sub-gap absorption. The corresponding solar cells based on the x = 0.6 absorber show the highest device performance. Despite having a low Urbach energy, higher Sn-content solar cells show reduced device performances as the amount of degradation via oxidation is the most substantial.

The tunable bandgaps and facile fabrication of perovskites make them attractive for multi-junction photovoltaics(1,2). However, light-induced phase segregation limits their efficiency and stability(3-5): this occurs in wide-bandgap (>1.65 electron volts) iodide/bromide mixed perovskite absorbers, and becomes even more acute in the top cells of triple-junction solar photovoltaics that require a fully 2.0-electron-volt bandgap absorber(2,6). Here we report that lattice distortion in iodide/bromide mixed perovskites is correlated with the suppression of phase segregation, generating an increased ion-migration energy barrier arising from the decreased average interatomic distance between the A-site cation and iodide. Using an approximately 2.0-electron-volt rubidium/caesium mixed-cation inorganic perovskite with large lattice distortion in the top subcell, we fabricated all-perovskite triple-junction solar cells and achieved an efficiency of 24.3 per cent (23.3 per cent certified quasi-steady-state efficiency) with an open-circuit voltage of 3.21 volts. This is, to our knowledge, the first reported certified efficiency for perovskite-based triple-junction solar cells. The triple-junction devices retain 80 per cent of their initial efficiency following 420 hours of operation at the maximum power point.