One of distinguishing features of metal halide perovskites is their long (up to microseconds) photoluminescence (PL) lifetimes, which are regularly observed for this class of semiconductors in spite of their direct gap origin. It is difficult to explain this contradiction in the framework of usual two-level Jablonski photophysical diagram because the absorption coefficient (i.e., the oscillator strength of the direct optical transition) is too high in perovskites to hold such long PL lifetimes. In this paper, we describe practical steps how the PL decay kinetics of perovskites in the forms of (1) passivated nanocrystals and (2) thin multicrystalline films can be described. In case of nanocrystals, the three-level delayed luminescence model is described by including shallow non-quenching traps providing multiple trapping and de-trapping of carriers and thus essentially lengthening the observed PL lifetime. In the case of perovskite thin films limited by interfacial recombination, the PL decay kinetics is usually determined by the non-radiative recombination on the film surfaces and can be satisfactorily described in terms of one-dimensional diffusion equation. The limits of applicability of such approaches are discussed.
Manipulation of the exciton emission
rate in nanocrystals of lead
halide perovskites (LHPs) was demonstrated by means of coupling of
excitons with a hyperbolic metamaterial (HMM) consisting of alternating
thin metal (Ag) and dielectric (LiF) layers. Such a coupling is found
to induce an increase of the exciton radiative recombination rate
by more than a factor of three due to the Purcell effect when the
distance between the quantum emitter and HMM is nominally as small
as 10 nm, which coincides well with the results of our theoretical
analysis. Besides, an effect of the coupling-induced long wavelength
shift of the exciton emission spectrum is detected and modeled. These
results can be of interest for quantum information applications of
single emitters on the basis of perovskite nanocrystals with high
photon emission rates.
Nanocrystals surface chemistry engineering offers a direct approach to tune charge carrier dynamics in nanocrystals-based photodetectors. For this purpose, we have investigated the effects of altering the surface chemistry of thin films of CsPbBr3 perovskite nanocrystals produced by the doctor blading technique, via solid state ligand-exchange using 3-mercaptopropionic acid (MPA). The electrical and electro-optical properties of photovoltaic and photoconductor devices were improved after the MPA ligand exchange, mainly because of a mobility increase up to 5 × 10−3 cm 2 / Vs . The same technology was developed to build a tandem photovoltaic device based on a bilayer of PbS quantum dots (QDs) and CsPbBr3 perovskite nanocrystals. Here, the ligand exchange was successfully carried out in a single step after the deposition of these two layers. The photodetector device showed responsivities around 40 and 20 mA/W at visible and near infrared wavelengths, respectively. This strategy can be of interest for future visible-NIR cameras, optical sensors, or receivers in photonic devices for future Internet-of-Things technology.
Self‐assembled nanocrystals (NCs) into superlattices (SLs) are alternative materials to polycrystalline films and single crystals, which can behave very differently from their constituents, especially when they interact coherently with each other. This work concentrates on the Superradiance (SR) emission observed in SLs formed by CsPbBr3 and CsPbBrI2 NCs. Micro‐Photoluminescence spectra and transients in the temperature range 4–100 K are measured in SLs to extract information about the SR states and uncoupled domains of NCs. For CsPbBr3 SLs with mostly homogeneous SR lines (linewidth 1–5 meV), this work measures lifetimes as short as 160 ps, 10 times lower than the value measured in a thin film made with the same NCs, which is due to domains of near identical NCs formed by 1000 to 40 000 NCs coupled by dipole–dipole interaction. The thermal decoherence of the SR exciton state is evident above 25 K due to its coupling with an effective phonon energy of ≈8 meV. These findings are an important step toward understanding the SR emission enhancement factor and the thermal dephasing process in perovskite SLs.
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