In perovskite solar cells, photovoltaic action is created by charge transport layers (CTLs) either side of the light-absorbing metal halide perovskite semiconductor. Hence, the rates for desirable charge extraction and unwanted interfacial recombination at the perovskite-CTL interfaces play a critical role for device efficiency. Here, the electrical properties of perovskite-CTL bilayer heterostructures are obtained using ultrafast terahertz and optical studies of the charge carrier dynamics after pulsed photoexcitation, combined with a physical model of charge carrier transport that includes the prominent Coulombic forces that arise after selective charge extraction into a CTL, and cross-interfacial recombination. The charge extraction velocity at the interface and the ambipolar diffusion coefficient within the perovskite are determined from the experimental decay profiles for heterostructures with three of the highest-performing CTLs, namely C60, PCBM and Spiro-OMeTAD. Definitive targets for the further improvement of devices are deduced: fullerenes deliver fast electron extraction, but suffer from a large rate constant for cross-interface recombination or hole extraction. Conversely, Spiro-OMeTAD exhibits slow hole extraction but does not increase the perovskite’s surface recombination rate, likely contributing to its success in solar cell devices.

Improved knowledge of the influence of temperature upon layered perovskites is essential to enable perovskite-based devices to operate over a broad temperature range and to elucidate the impact of structural changes upon the optoelectronic properties. We examined the Ruddlesden–Popper layered perovskite 2-thiophenemethylammonium lead iodide (ThMA2PbI4) and observed a structural phase transition between a high- and a low-temperature phase at 220 K using temperature-dependent X-ray diffraction, UV–visible absorption, and photoluminescence (PL) spectroscopy. The structural phase transition altered the tilt pattern of the inorganic octahedra layer, modifying the absorption and PL spectra. Further, we found a narrow and intense additional PL peak in the low-temperature phase, which we assigned to radiative emission from a defect-bound exciton state. In both phases we determined the thermal expansion coefficient and found values similar to those of cubic 3D perovskites, i.e., larger than those of typical substrates such as glass. These results demonstrate that the organic spacer plays a critical role in controlling the temperature-dependent structural and optoelectronic properties of layered perovskites and suggests more widely that strain management strategies may be needed to fully utilize layered perovskites in device applications.

Monolayer molybdenum disulfide (MoS2) is a promising candidate for inclusion in optoelectronic technologies, owing to its two-dimensional (2D) nature and resultant novel photoluminescence (PL). Chemical vapour deposition (CVD) is an important method for the preparation of large-area films of monolayer MoS2. The PL character of as-prepared monolayer MoS2 must be well understood to facilitate detailed evaluation of any process-induced effects during device fabrication. We comparatively explore the PL emission from four different commercially available CVD-grown MoS2 monolayer films. We characterize the samples via Raman and PL spectroscopy, using both single-spot and mapping techniques, while atomic force microscopy (AFM) is applied to map the surface structure. Via multipeak fitting, we decompose the PL spectra into constituent exciton and trion contributions, enabling an assessment of the quality of the MoS2 monolayers. We find that the PL character varies significantly from sample to sample. We also reveal substantial inhomogeneity of the PL signal across each individual MoS2 film. We attribute the PL variation to non-uniform MoS2 film morphologies that result from the nucleation and coalescence processes during the CVD film development. Understanding the large variability in starting PL behaviour is vital to optimize the optoelectronic properties for MoS2-based devices.

Light-emitting diodes (LEDs) are ubiquitous in modern society, with applications spanning from lighting and displays to medical diagnostics and data communications. Metal-halide perovskites are promising materials for LEDs because of their excellent optoelectronic properties and solution processability. Although research has progressed substantially in optimizing their external quantum efficiency, the modulation characteristics of perovskite LEDs remain unclear. Here we report a holistic approach for realizing fast perovskite photonic sources on silicon based on tailoring alkylammonium cations in perovskite systems. We reveal the recombination behaviour of charged species at various carrier density regimes relevant for their modulation performance. By integrating a Fabry–Pérot microcavity on silicon, we demonstrate perovskite devices with efficient light outcoupling. We achieve device modulation bandwidths of up to 42.6 MHz and data rates above 50 Mbps, with further analysis suggesting that the bandwidth may exceed gigahertz levels. The principles developed here will support the development of perovskite light sources for next-generation data-communication architectures. The demonstration of solution-processed perovskite emitters on silicon substrates also opens up the possibility of integration with micro-electronics platforms.