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Cross-sectional transmission electron microscopy has been widely used to investigate organic-inorganic hybrid halide perovskite-based optoelectronic devices. Electron-transparent specimens (lamellae) used in such studies are often prepared using focused ion beam (FIB) milling. However, the gallium ions used in FIB milling may severely degrade the structure and composition of halide perovskites in the lamellae, potentially invalidating studies performed on them. In this work, the close relationship between perovskite structure and luminescence is exploited to examine the structural quality of perovskite solar cell lamellae prepared by FIB milling. Through hyperspectral cathodoluminescence (CL) mapping, the perovskite layer was found to remain optically active with a slightly blue-shifted luminescence. This finding indicates that the perovskite structure is largely preserved upon the lamella fabrication process although some surface amorphisation occurred. Further changes in CL due to electron beam irradiation were also recorded, confirming that electron dose management is essential in electron microscopy studies of carefully prepared halide perovskite-based device lamellae. RESEARCH HIGHLIGHTS: Cathodoluminescence is used to study the emission of focused ion beam milled perovskite solar cell lamellae. The perovskite remained optically active with a slightly blue-shifted luminescence, indicating that the perovskite structure is mostly preserved.

Bulk heterojunction (BHJ) nonfullerene organic solar cells prepared from sequentially deposited donor and acceptor layers (sq-BHJ) have recently been shown to be highly efficient, environmentally friendly, and compatible with large area and roll-to-roll fabrication. However, the related photophysics at donor-acceptor interface and the vertical heterogeneity of donor-acceptor distribution, critical for exciton dissociation and device performance, have been largely unexplored. Herein, steady-state and time-resolved optical and electrical techniques are employed to characterize the interfacial trap states. Correlating with the luminescent efficiency of interfacial states and its nonradiative recombination, interfacial trap states are characterized to be about 40% more populated in the sq-BHJ devices than the as-cast BHJ (c-BHJ), which probably limits the device voltage output. Cross-sectional energy-dispersive X-ray spectroscopy and ultraviolet photoemission spectroscopy depth profiling directly visualize the donor–acceptor vertical stratification with a precision of 1–2 nm. From the proposed “needle” model, the high exciton dissociation efficiency is rationalized. This study highlights the promise of sequential deposition to fabricate efficient solar cells, and points toward improving the voltage output and overall device performance via eliminating interfacial trap states.

The upscaling of perovskite solar cells is one of the challenges that must be addressed to pave the way toward the commercial development of this technology. As for other thin-film photovoltaic technologies, upscaling requires the fabrication of modules composed of series-connected cells. In this work we demonstrate for the first time the interconnection of inverted modules with NiOx using a UV ns laser, obtaining a 10.2 cm2 minimodule with a 15.9% efficiency on the active area, the highest for a NiOx based perovskite module. We use optical microscopy, energy-dispersive X-ray spectroscopy, and transfer length measurement to optimize the interconnection. The results are implemented in a complete electrical simulation of the cell-to-module losses to evaluate the experimental results and to provide an outlook on further development of single junction and multijunction perovskite modules.

Halide perovskite materials have promising performance characteristics for low-cost optoelectronic applications. Photovoltaic devices fabricated from perovskite absorbers have reached power conversion efficiencies above 25 per cent in single-junction devices and 28 per cent in tandem devices1,2. This strong performance (albeit below the practical limits of about 30 per cent and 35 per cent, respectively3) is surprising in thin films processed from solution at low-temperature, a method that generally produces abundant crystalline defects4. Although point defects often induce only shallow electronic states in the perovskite bandgap that do not affect performance5, perovskite devices still have many states deep within the bandgap that trap charge carriers and cause them to recombine non-radiatively. These deep trap states thus induce local variations in photoluminescence and limit the device performance6. The origin and distribution of these trap states are unknown, but they have been associated with light-induced halide segregation in mixed-halide perovskite compositions7 and with local strain8, both of which make devices less stable9. Here we use photoemission electron microscopy to image the trap distribution in state-of-the-art halide perovskite films. Instead of a relatively uniform distribution within regions of poor photoluminescence efficiency, we observe discrete, nanoscale trap clusters. By correlating microscopy measurements with scanning electron analytical techniques, we find that these trap clusters appear at the interfaces between crystallographically and compositionally distinct entities. Finally, by generating time-resolved photoemission sequences of the photo-excited carrier trapping process10,11, we reveal a hole-trapping character with the kinetics limited by diffusion of holes to the local trap clusters. Our approach shows that managing structure and composition on the nanoscale will be essential for optimal performance of halide perovskite devices.

The upscaling of perovskite solar cells is one of the challenges that must be addressed to pave the way toward the commercial development of this technology. As for other thin-film photovoltaic technologies, upscaling requires the fabrication of modules composed of series-connected cells. In this work we demonstrate for the first time the interconnection of inverted modules with NiOx using a UV ns laser, obtaining a 10.2 cm2 minimodule with a 15.9% efficiency on the active area, the highest for a NiOx based perovskite module. We use optical microscopy, energy-dispersive X-ray spectroscopy, and transfer length measurement to optimize the interconnection. The results are implemented in a complete electrical simulation of the cell-to-module losses to evaluate the experimental results and to provide an outlook on further development of single junction and multijunction perovskite modules.

The upscaling of perovskite solar cells is one of the challenges that must be addressed to pave the way toward the commercial development of this technology. As for other thin-film photovoltaic technologies, upscaling requires the fabrication of modules composed of series-connected cells. In this work we demonstrate for the first time the interconnection of inverted modules with NiOx using a UV ns laser, obtaining a 10.2 cm2 minimodule with a 15.9% efficiency on the active area, the highest for a NiOx based perovskite module. We use optical microscopy, energy-dispersive X-ray spectroscopy, and transfer length measurement to optimize the interconnection. The results are implemented in a complete electrical simulation of the cell-to-module losses to evaluate the experimental results and to provide an outlook on further development of single junction and multijunction perovskite modules.

Halide perovskite materials have promising performance characteristics for low-cost optoelectronic applications. Photovoltaic devices fabricated from perovskite absorbers have reached power conversion efficiencies above 25 per cent in single-junction devices and 28 per cent in tandem devices1,2. This strong performance (albeit below the practical limits of about 30 per cent and 35 per cent, respectively3) is surprising in thin films processed from solution at low-temperature, a method that generally produces abundant crystalline defects4. Although point defects often induce only shallow electronic states in the perovskite bandgap that do not affect performance5, perovskite devices still have many states deep within the bandgap that trap charge carriers and cause them to recombine non-radiatively. These deep trap states thus induce local variations in photoluminescence and limit the device performance6. The origin and distribution of these trap states are unknown, but they have been associated with light-induced halide segregation in mixed-halide perovskite compositions7 and with local strain8, both of which make devices less stable9. Here we use photoemission electron microscopy to image the trap distribution in state-of-the-art halide perovskite films. Instead of a relatively uniform distribution within regions of poor photoluminescence efficiency, we observe discrete, nanoscale trap clusters. By correlating microscopy measurements with scanning electron analytical techniques, we find that these trap clusters appear at the interfaces between crystallographically and compositionally distinct entities. Finally, by generating time-resolved photoemission sequences of the photo-excited carrier trapping process10,11, we reveal a hole-trapping character with the kinetics limited by diffusion of holes to the local trap clusters. Our approach shows that managing structure and composition on the nanoscale will be essential for optimal performance of halide perovskite devices. Photoemission electron microscopy images of trap states in halide peroskites, spatially correlated with their structural and compositional factors, may help in managing power losses in optoelectronic applications.