Colloidal perovskite nanoplatelets are a promising class of semiconductor nanomaterials-exhibiting bright luminescence, tunable and spectrally narrow absorption and emission features, strongly confined excitonic states, and facile colloidal synthesis. Here, we demonstrate the high degree of spectral tunability achievable through variation of the cation, metal, and halide composition as well as nanoplatelet thickness. We synthesize nanoplatelets of the form L2[ABX3]n-1BX4, where L is an organic ligand (octylammonium, butylammonium), A is a monovalent metal or organic molecular cation (cesium, methylammonium, formamidinium), B is a divalent metal cation (lead, tin), X is a halide anion (chloride, bromide, iodide), and n-1 is the number of unit cells in thickness. We show that variation of n, B, and X leads to large changes in the absorption and emission energy, while variation of the A cation leads to only subtle changes but can significantly impact the nanoplatelet stability and photoluminescence quantum yield (with values over 20%). Furthermore, mixed halide nanoplatelets exhibit continuous spectral tunability over a 1.5 eV spectral range, from 2.2 to 3.7 eV. The nanoplatelets have relatively large lateral dimensions (100 nm to 1 μm), which promote self-assembly into stacked superlattice structures-the periodicity of which can be adjusted based on the nanoplatelet surface ligand length. These results demonstrate the versatility of colloidal perovskite nanoplatelets as a material platform, with tunability extending from the deep-UV, across the visible, into the near-IR. In particular, the tin-containing nanoplatelets represent a significant addition to the small but increasingly important family of lead- and cadmium-free colloidal semiconductors.

Two-dimensional perovskites, in which inorganic layers are stabilized by organic spacer molecules, are attracting increasing attention as a more robust analogue to the conventional three-dimensional metal-halide perovskites. However, reducing the perovskite dimensionality alters their optoelectronic properties dramatically, yielding excited states that are dominated by bound electron-hole pairs known as excitons, rather than by free charge carriers common to their bulk counterparts. Despite the growing interest in two-dimensional perovskites for both light harvesting and light emitting applications, the full impact of the excitonic nature on their optoelectronic properties remains unclear, particularly regarding the spatial dynamics of the excitons within the two-dimensional (2D) plane.Here, we present direct measurements of in-plane exciton transport in single-crystalline layered perovskites. Using time-resolved fluorescence microscopy, we show that excitons undergo an initial fast, intrinsic normal diffusion through the crystalline plane, followed by a transition to a slower subdiffusive regime as excitons get trapped. Interestingly, the early intrinsic exciton diffusivity depends sensitively on the choice of organic spacer. We find a clear correlation between the stiffness of the lattice and the diffusivity, suggesting exciton-phonon interactions to be dominant in determining the spatial dynamics of the excitons in these materials. Our findings provide a clear design strategy to optimize exciton transport in these systems. lead, tin), X is a halide anion (chloride, bromide, iodide), L is a long organic spacer molecule, and n is the number of octahedra that make up the thickness of the inorganic layer. The separation into fewatom thick inorganic layers yields strong quantum and dielectric confinement effects. 38 As a result, the exciton binding energies in 2D perovskites can be as high as several hundreds of meVs, which is around an order of magnitude larger than those found in bulk perovskites. [39][40][41] The excitonic character of the excited state is accompanied by an effective widening of the bandgap, an increase in the oscillator strength, and a narrowing of the emission spectrum. [40][41][42] The strongest confinement effects are observed for n = 1, where the excited state is confined to a single B-X-octahedral layer (see Figure 1a).Light harvesting using 2D perovskites relies on the efficient transport of excitons and their subsequent separation into free charges. 43 This stands in contrast to bulk perovskites in which free charges are generated instantaneously thanks to the small exciton binding energy. 39 Particularly, with excitons being neutral quasi-particles, the charge extraction becomes significantly more challenging as they cannot be guided to the electrodes through an external electric field. 44 Excitons need to diffuse to an interface before the electron and hole can be efficiently separated into free charges. 45 On the other hand, for light emitting applications the spatial displacement is ...

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Organic−inorganic perovskites have been shown to have excellent optoelectronic properties. Further, layered perovskites have been demonstrated, utilizing quantum confinement to achieve emission blueshifted from the bulk band gap. Here, we tune this blue-shift to build LEDs that span the visible spectrum. We demonstrate that electroluminescence from red-shifted layers dominates emission from mixed-thickness devices and that the addition of excess ligand is necessary to drive emission toward blue-shifted layers. By tuning the thickness of the layers, we build LEDs with blue emission utilizing the lead bromide system and orange emission utilizing the lead iodide system. Finally, we demonstrate that these materials suffer reversible degradation under an applied electric field. The spectrally narrow emission, combined with the favorable electronic properties of perovskite materials and access to shorter emission wavelengths through quantum confinement, demonstrates the promise of these materials as a new platform for low-cost, high-performance light-emitting devices.

Is there a way to describe pedestrian movement with simple rules, as in a cellular automaton, but without being restricted to a cellular grid? Inspired by the natural stepwise movement of humans, we develop a model that uses local discretization on a circle around virtual pedestrians. This allows for movement in arbitrary directions, only limited by the chosen optimization algorithm and numerical resolution. The radii of the circles correspond to the step lengths of pedestrians and thus are model parameters, which must be derived from empirical observation. Therefore, we conducted a controlled experiment, collected empirical data for step lengths in relation with different speeds, and used the findings in our model. We complement the model with a simple calibration algorithm that allows reproducing known density-velocity relations, which constitutes a proof of concept. Further validation of the model is achieved by reenacting an evacuation scenario from experimental research. The simulated egress times match the values reported for the experiment very well. A new normalized measure for space occupancy serves to visualize the results.

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Using light to control matter has captured the imagination of scientists for generations, as there is an abundance of photons at our disposal. Yet delivering photons beyond the surface to many photoresponsive systems has proven challenging, particularly at scale, due to light attenuation via absorption and scattering losses. Triplet−triplet annihilation upconversion (TTA-UC), a process which allows for low energy photons to be converted to high energy photons, is poised to overcome these challenges by allowing for precise spatial generation of high energy photons due to its nonlinear nature. With a wide range of sensitizer and annihilator motifs available for TTA-UC, many researchers seek to integrate these materials in solution or solid-state applications. In this Review, we discuss nanoengineering deployment strategies and highlight their uses in recent state-of-the-art examples of TTA-UC integrated in both solution and solid-state applications. Considering both implementation tactics and application-specific requirements, we identify critical needs to push TTA-UC-based applications from an academic curiosity to a scalable technology.

Two-dimensional layered perovskites are attracting increasing attention as more robust analogues to the conventional three-dimensional metal-halide perovskites for both light harvesting and light emitting applications. However, the impact of the reduced dimensionality on the optoelectronic properties remains unclear, particularly regarding the spatial dynamics of the excitonic excited state within the two-dimensional plane. Here, we present direct measurements of exciton transport in single-crystalline layered perovskites. Using transient photoluminescence microscopy, we show that excitons undergo an initial fast diffusion through the crystalline plane, followed by a slower subdiffusive regime as excitons get trapped. Interestingly, the early intrinsic diffusivity depends sensitively on the choice of organic spacer. A clear correlation between lattice stiffness and diffusivity is found, suggesting exciton-phonon interactions to be dominant in the spatial dynamics of the excitons in perovskites, consistent with the formation of exciton-polarons. Our findings provide a clear design strategy to optimize exciton transport in these systems.