Semiconductor nanocrystals are receiving increased interest as narrow-band emitters for display applications. Here, we investigate the underlying photoluminescence (PL) linewidth broadening mechanisms in thickness-tunable 2D halide perovskite (Csn−1PbnBr3n+1) nanoplatelets (NPLs). Temperature-dependent PL spectroscopy on NPL thin films reveals a blue-shift of the PL maximum for thicker NPLs, no shift for three monolayer (ML) thick NPLs, and a red-shift for the thinnest (2 ML) NPLs with increasing temperature. Emission linewidths also strongly depend on NPL thickness, with the thinnest NPLs showing the smallest temperature-induced broadening. We determine the combined interaction of exciton–phonon coupling and thermal lattice expansion to be responsible for both effects. Additionally, the 2 ML NPLs exhibit a significantly larger Fröhlich coupling constant and optical phonon energy, possibly due to an inversion in the exciton fine structure. These results illustrate that ultrathin halide perovskite NPLs could illuminate the next generation of displays, provided a slightly greater sample homogeneity and improved stability.

Two-dimensional halide perovskite nanoplatelets (NPLs) have exceptional light-emitting properties, including wide spectral tunability, ultrafast radiative decays, high quantum yields (QY), and oriented emission. To realize efficient devices, it is imperative to understand how exciton 2 transport progresses in NPL thin films. Due to the high binding energies of electron-hole pairs, excitons are generally considered the dominant species responsible for carrier transfer. We employ spatially and temporally resolved optical microscopy to map exciton diffusion in perovskite nanocrystal (NC) thin films between 15 °𝐶 and 50 °𝐶. At room temperature (RT), we find the diffusion length to be inversely correlated to the thickness of the nanocrystals (NCs). With increasing temperatures, exciton diffusion declines for all NC films, but at different rates. This leads to specific temperature turnover points, at which thinner NPLs exhibit higher diffusion lengths. We attribute this anomalous diffusion behavior to the coexistence of excitons and free electron hole-pairs inside the individual NCs within our temperature range. The organic ligand shell surrounding the NCs prevents charge transfer. Accordingly, any time an electron-hole pair spends in the unbound state reduces the FRET-mediated inter-NC transfer rates and consequently the overall diffusion. These results clarify how exciton diffusion progresses in strongly confined halide perovskite NC films, emphasizing critical considerations for optoelectronic devices.

Trap states of the semiconductor/gate dielectric interface give rise to a pronounced subthreshold behavior in field‐effect transistors (FETs) diminishing and masking intrinsic properties of 2D materials. To reduce the well‐known detrimental effect of SiO2 surface traps, this work spin‐coated an ultrathin (≈5 nm) cyclic olefin copolymer (COC) layer onto the oxide and this hydrophobic layer acts as a surface passivator. The chemical resistance of COC allows to fabricate monolayer MoS2 FETs on SiO2 by standard cleanroom processes. This way, the interface trap density is lowered and stabilized almost fivefold, to around 5 × 1011 cm−2 eV−1, which enables low‐voltage FETs even on 300 nm thick SiO2. In addition to this superior electrical performance, the photoresponsivity of the MoS2 devices on passivated oxide is also enhanced by four orders of magnitude compared to nonpassivated MoS2 FETs. Under these conditions, negative photoconductivity and a photoresponsivity of 3 × 107 A W−1 is observed which is a new highest value for MoS2. These findings indicate that the ultrathin COC passivation of the gate dielectric enables to probe exciting properties of the atomically thin 2D semiconductor, rather than interface trap dominated effects.