Author Correction: Maximizing and stabilizing luminescence from halide perovskites with potassium passivation.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Visualizing Buried Local Carrier Diffusion in Halide Perovskite Crystals via Two-Photon Microscopy.

Halide perovskites have shown great potential for light emission and photovoltaic applications due to their remarkable electronic properties. Although the device performances are promising, they are still limited by microscale heterogeneities in their photophysical properties. Here, we study the impact of these heterogeneities on the diffusion of charge carriers, which are processes crucial for efficient collection of charges in light-harvesting devices. A photoluminescence tomography technique is developed in a confocal microscope using one- and two-photon excitation to distinguish between local surface and bulk diffusion of charge carriers in methylammonium lead bromide single crystals. We observe a large dispersion of local diffusion coefficients with values between 0.3 and 2 cm2·s-1 depending on the trap density and the morphological environment-a distribution that would be missed from analogous macroscopic or surface measurements. This work reveals a new framework to understand diffusion pathways, which are extremely sensitive to local properties and buried defects.

Controlling the coherence of a diamond spin qubit through its strain environment.

The uncontrolled interaction of a quantum system with its environment is detrimental for quantum coherence. For quantum bits in the solid state, decoherence from thermal vibrations of the surrounding lattice can typically only be suppressed by lowering the temperature of operation. Here, we use a nano-electro-mechanical system to mitigate the effect of thermal phonons on a spin qubit - the silicon-vacancy colour centre in diamond - without changing the system temperature. By controlling the strain environment of the colour centre, we tune its electronic levels to probe, control, and eventually suppress the interaction of its spin with the thermal bath. Strain control provides both large tunability of the optical transitions and significantly improved spin coherence. Finally, our findings indicate the possibility to achieve strong coupling between the silicon-vacancy spin and single phonons, which can lead to the realisation of phonon-mediated quantum gates and nonlinear quantum phononics.

Maximizing and stabilizing luminescence from halide perovskites with potassium passivation.

Metal halide perovskites are of great interest for various high-performance optoelectronic applications. The ability to tune the perovskite bandgap continuously by modifying the chemical composition opens up applications for perovskites as coloured emitters, in building-integrated photovoltaics, and as components of tandem photovoltaics to increase the power conversion efficiency. Nevertheless, performance is limited by non-radiative losses, with luminescence yields in state-of-the-art perovskite solar cells still far from 100 per cent under standard solar illumination conditions. Furthermore, in mixed halide perovskite systems designed for continuous bandgap tunability (bandgaps of approximately 1.7 to 1.9 electronvolts), photoinduced ion segregation leads to bandgap instabilities. Here we demonstrate substantial mitigation of both non-radiative losses and photoinduced ion migration in perovskite films and interfaces by decorating the surfaces and grain boundaries with passivating potassium halide layers. We demonstrate external photoluminescence quantum yields of 66 per cent, which translate to internal yields that exceed 95 per cent. The high luminescence yields are achieved while maintaining high mobilities of more than 40 square centimetres per volt per second, providing the elusive combination of both high luminescence and excellent charge transport. When interfaced with electrodes in a solar cell device stack, the external luminescence yield-a quantity that must be maximized to obtain high efficiency-remains as high as 15 per cent, indicating very clean interfaces. We also demonstrate the inhibition of transient photoinduced ion-migration processes across a wide range of mixed halide perovskite bandgaps in materials that exhibit bandgap instabilities when unpassivated. We validate these results in fully operating solar cells. Our work represents an important advance in the construction of tunable metal halide perovskite films and interfaces that can approach the efficiency limits in tandem solar cells, coloured-light-emitting diodes and other optoelectronic applications.

Probing buried recombination pathways in perovskite structures using 3D photoluminescence tomography.

Perovskite solar cells and light-emission devices are yet to achieve their full potential owing in part to microscale inhomogeneities and defects that act as non-radiative loss pathways. These sites have been revealed using local photoluminescence mapping techniques but the short absorption depth of photons with energies above the bandgap means that conventional one-photon excitation primarily probes the surface recombination. Here, we use two-photon time-resolved confocal photoluminescence microscopy to explore the surface and bulk recombination properties of methylammonium lead halide perovskite structures. By acquiring 2D maps at different depths, we form 3D photoluminescence tomography images to visualise the charge carrier recombination kinetics. The technique unveils buried recombination pathways in both thin film and micro-crystal structures that aren't captured in conventional one-photon mapping experiments. Specifically, we reveal that light-induced passivation approaches are primarily surface-sensitive and that nominal single crystals still contain heterogeneous defects that impact charge-carrier recombination. Our work opens a new route to sensitively probe defects and associated non-radiative processes in perovskites, highlighting additional loss pathways in these materials that will need to be addressed through improved sample processing or passivation treatments.