Recently, some organic–inorganic hybrid perovskites (OIHPs) have been reported to exhibit strong subgap broadband luminescence. While the origin of such luminescence has been proposed by several groups, a strategy to prepare OIHP with the desired subgap emission properties has remained elusive. Here, we report controlled synthesis of a broadband-emitting single-crystal 2D OIHP with an average quantum yield of >80 %. We demonstrate that the intensity of broadband emission can be tuned by controlling the excess iodine ion concentration during the synthesis in hydroiodic acid. We show that the emitters exhibit characteristics of localized defects such as limited mobility and saturation at high excitation power. Using density functional theory calculations, we show that bond-state iodine interstitials are responsible for the observed long-lived luminescence.

Semiconducting transition metal dichalcogenides (TMDs) have been applied as the active layer in photodetectors and solar cells, displaying substantial charge photogeneration yields. However, their large exciton binding energy, which increases with decreasing thickness (number of layers), as well as the strong resonance peaks in the absorption spectra suggest that excitons are the primary photoexcited states. Detailed time-domain studies of the photoexcitation dynamics in TMDs exist mostly for MoS2. Here, we use femtosecond optical spectroscopy to study the exciton and charge dynamics following impulsive photoexcitation in few-layer WS2. We confirm excitons as the primary photoexcitation species and find that they dissociate into charge pairs with a time constant of about 1.3 ps. The better separation of the spectral features compared to MoS2 allows us to resolve a previously undetected process: these charges diffuse through the samples and get trapped at defects, such as flake edges or grain boundaries, causing an appreciable change of their transient absorption spectra. This finding opens the way to further studies of traps in TMD samples with different defect contents.

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We report a straightforward chemical methodology for controlling the thickness of black phosphorus flakes down to the monolayer limit by layer-by-layer oxidation and thinning, using water as solubilizing agent.

Monolayer semiconductors are atomically thin quantum wells with strong confinement of electrons in two-dimensional (2D) plane. Here, we experimentally study the out-of-plane polarizability of excitons in hBN-encapsulated monolayer WSe2 in strong electric fields of up to 1.6 V/nm (16 MV/cm). We monitor free and bound exciton photoluminescence peaks with increasing electric fields at a constant carrier density, carefully compensating for unintentional photodoping in our double-gated device at 4K. We show that the Stark shift is < 0.4 meV despite the large electric fields applied, yielding an upper limit of polarizability αz to be ~ 10 -11 Dm/V. Such a small polarizability, which is nearly two orders of magnitude smaller than the previously reported value for MoS2, indicates strong atomic confinement of electrons in this 2D system and highlights the unusual robustness of free excitons against surface potential fluctuations.

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The optoelectronic properties of a material are determined by the processes following light-matter interaction. Here we use femtosecond optical spectroscopy to systematically study photoexcited carrier relaxation in few-layer MoS 2 flakes as a function of excitation density and sample thickness. We find bimolecular coalescence of charges into indirect excitons as the dominant relaxation process in two-to three-layer flakes while thicker flakes show a much higher density of defects, which efficiently trap charges before they can coalesce.

Signal modulation in optoelectronics is obtained by modulation of either the refractive index or the absorbance by an electric field. However, electromodulators have not kept up with the miniaturization of other electronic and optical components. Here we show a strong transverse electroabsorption signal in a monolayer of the 2D semiconductor MoS2. The electroabsorption spectrum is dominated by an apparent linewidth broadening of around 15% at a modulated voltage of only Vpp  =  0.5 V. Contrary to known variants of the Stark effect, the broadening increases linearly with the applied field strength and arises from a linear variation of the distance between the strongly overlapping exciton and trion resonances. The achievable modulation depths exceeding 0.1 dB nm−1 bear the scope for extremely compact, ultrafast, energy-efficient electroabsorption modulators for integrated photonics, including on-chip optical communication.