Scanning Transmission Ion Microscopy Time-of-Flight Spectroscopy Using 20 keV Helium Ions.

Scanning transmission ion microscopy imaging was performed whilst using a delay-line detector to record the impact position and arrival time of transmitted ions or neutrals. The incident helium ion beam had an energy of 20 keV and the arrival time measurements were used to calculate the energy loss after transmission through the sample. The 5D dataset thus produced (2D position in the sample plane, 2D position in the detector plane, and energy) is analyzed by collection into energy spectra or images. It is demonstrated that ion energy loss maps can identify regions of identical materials in the sample plane. The behavior of the energy loss with respect to the scattering angle is calculated and these simulations agree with the experimentally measured results. This experiment demonstrates the capability of keV helium ions to be successfully used in energy loss imaging experiments. This is the first step in the development of keV scanning transmission ion microscopy energy loss techniques.

Alleviating nanostructural phase impurities enhances the optoelectronic properties, device performance and stability of cesium-formamidinium metal-halide perovskites.

The technique of alloying FA+ with Cs+ is often used to promote structural stabilization of the desirable α-FAPbI3 phase in halide perovskite devices. However, the precise mechanisms by which these alloying approaches improve the optoelectronic quality and enhance the stability have remained elusive. In this study, we advance that understanding by investigating the effect of cationic alloying in CsxFA1-xPbI3 perovskite thin-films and solar-cell devices. Selected-area electron diffraction patterns combined with microwave conductivity measurements reveal that fine Cs+ tuning (Cs0.15FA0.85PbI3) leads to a minimization of stacking faults and an increase in the photoconductivity of the perovskite films. Ultra-sensitive external quantum efficiency, kelvin-probe force microscopy and photoluminescence quantum yield measurements demonstrate similar Urbach energy values, comparable surface potential fluctuations and marginal impact on radiative emission yields, respectively, irrespective of Cs content. Despite this, these nanoscopic defects appear to have a detrimental impact on inter-grains'/domains' carrier transport, as evidenced by conductive-atomic force microscopy and corroborated by drastically reduced solar cell performance. Importantly, encapsulated Cs0.15FA0.85PbI3 devices show robust operational stability retaining 85% of the initial steady-state power conversion efficiency for 1400 hours under continuous 1 sun illumination at 35 °C, in open-circuit conditions. Our findings provide nuance to the famous defect tolerance of halide perovskites while providing solid evidence about the detrimental impact of these subtle structural imperfections on the long-term operational stability.

Interface passivation for 31.25%-efficient perovskite/silicon tandem solar cells.

Silicon solar cells are approaching their theoretical efficiency limit of 29%. This limitation can be exceeded with advanced device architectures, where two or more solar cells are stacked to improve the harvesting of solar energy. In this work, we devise a tandem device with a perovskite layer conformally coated on a silicon bottom cell featuring micrometric pyramids-the industry standard-to improve its photocurrent. Using an additive in the processing sequence, we regulate the perovskite crystallization process and alleviate recombination losses occurring at the perovskite top surface interfacing the electron-selective contact [buckminsterfullerene (C60)]. We demonstrate a device with an active area of 1.17 square centimeters, reaching a certified power conversion efficiency of 31.25%.

Quantitative nanoscale imaging using transmission He ion channelling contrast: Proof-of-concept and application to study isolated crystalline defects.

A newly developed microscope prototype, namely npSCOPE, consisting of a Gas Field Ion Source (GFIS) column and a position sensitive Delay-line Detector (DLD) was used to perform Scanning Transmission Ion Microscopy (STIM) using keV He+ ions. One experiment used 25 keV ions and a second experiment used 30 keV ions. STIM imaging of a 50 nm thick free-standing gold membrane exhibited excellent contrast due to ion channelling and revealed rich microstructural features including isolated nanoscale twin bands which matched well with the contrast in the conventional ion-induced Secondary Electron (SE) imaging mode. Transmission Kikuchi Diffraction (TKD) and Backscattered Electron (BSE) imaging were performed on the same areas to correlate and confirm the microstructural features observed in STIM. Monte Carlo simulations of the ion and electron trajectories were performed with parameters similar to the experimental conditions to derive insights related to beam broadening and its effect in the degradation of transmission image resolution. For the experimental conditions used, STIM imaging showed a lateral resolution close to30 nm. Dark twin bands in bright grains as well as bright twin bands in dark grains were observed in STIM. Some of the twin bands were invisible in STIM. For the specific experimental conditions used, the ion transmission efficiency across a particular twin band was found to decrease by a factor of 2.8. Surprisingly, some grains showed contrast reversal when the Field of View (FOV) was changed indicating the sensitivity of the channelling contrast to even small changes in illumination conditions. These observations are discussed using ion channelling conditions and crystallographic orientations of the grains and twin bands. This study demonstrates for the first time the potential of STIM imaging using keV He+ ions to quantitatively investigate channelling in nanoscale structures including isolated crystalline defects.