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Cation exchange has been investigated in a wide range of nanocrystals of varying composition, size, and shape. Complete and fully reversible exchange occurs, and the rates of the reactions are much faster than in bulk cation exchange processes. A critical size has been identified below which the shapes of complex nanocrystals evolve toward the equilibrium shape with lowest energy during the exchange reaction. Above the critical size, the anion sublattice remains intact and the basic shapes of th

Cesium lead halide (CsPbX₃) nanocrystals have emerged as a new family of materials that can outperform the existing semiconductor nanocrystals due to their superb optical and charge-transport properties. However, the lack of a robust method for producing quantum dots with controlled size and high ensemble uniformity has been one of the major obstacles in exploring the useful properties of excitons in zero-dimensional nanostructures of CsPbX₃. Here, we report a new synthesis

We report the direct hot-injection synthesis of Mn-doped cesium lead bromide (CsPbBr3) perovskite nanocrystals. In contrast to Mn-doped CsPbCl3 nanocrystals, where doping of Mn under typical hot-injection synthesis condition has been relatively straightforward, extending the same approach to CsPbBr3 has been very difficult. Here, we achieved the synthesis of Mn-doped CsPbBr3 nanocrystals via the formation of an intermediate structure (L2[Pb1–xMnx]Br4, L = ligand) before the hot-injection of the

We report the strong light-induced activation of forbidden exciton transition in CsPbBr₃ perovskite quantum dots mediated by the symmetry-breaking polaron that modifies the optical selection rule of the confined exciton transition. The activated forbidden transition results in an intense pump-induced absorption in the transient absorption spectra above the bandgap, where the original parity-forbidden transition was located. In contrast to many other semiconductor quantum dots, photoex

Lead-halide perovskite nanocrystals (NCs) are receiving much attention as a potential high-quality source of photons due to their superior luminescence properties in comparison to other semiconductor NCs. To date, research has focused mostly on NCs with little or no quantum confinement. Here, we measured the size- and temperature-dependent photoluminescence (PL) from strongly confined CsPbBr₃ quantum dots (QDs) with highly uniform size distributions, and examined the factors determini

ConspectusSemiconducting metal halide perovskite (MHP) nanocrystals have emerged as an important new class of materials as the source of photons and charges for various applications that can outperform many other semiconductor nanocrystals utilized for the same purposes. However, the majority of the studies of MHP nanocrystals focused on weakly or nonconfined systems, where the quantum confinement giving rise to various size-dependent and confinement-enhanced photophysical properties cannot be e

Dark exciton as the lowest-energy (ground) exciton state in metal halide perovskite nanocrystals is a subject of much interest. This is because the superior performance of perovskites as the photon source combined with long lifetime of dark exciton can be attractive for many applications of exciton. However, the direct observation of the intense and long-lived dark exciton emission, indicating facile access to dark ground exciton state, has remained elusive. Here, we report the intense photolumi

Femtosecond multicolor pump−probe spectroscopy on the prototypical intramolecular electron-transfer compound ([(NH3)5RuNCRu(CN)5]-; RuRu) in aqueous solution is reported for the first time with sufficient time resolution and spectral coverage to monitor the complete spectral dynamics. From the dynamic absorption spectrum, constructed from the pump−probe data obtained over a wide range of probe wavelengths (570−1300 nm), accurate measurement of the electron transfer (ET) time (1/kET) have been ob

Chemiluminescence immunoassays have been widely employed for diagnosing various diseases. However, because of the extremely low intensity chemiluminescence signals, highly sensitive transducers, such as photomultiplier tubes and image sensors with cooling devices, are required to overcome this drawback. In this study, a hypersensitive photosensor was developed based on cesium lead bromide (CsPbBr₃) perovskite quantum dots (QDs) with sufficient high sensitivity for chemiluminescence im

We report the photoinduced post-synthesis method of Mn doping in colloidal perovskite nanocrystals, which can produce Mn-doped CsPbX3 (X = Cl, Br) nanocrystals with preserved size and anisotropic morphology. Photoinduced Mn doping occurs through cation exchange driven by the facile photoinduced halide exchange in dihalomethane (CH2X2, X = Cl, Br) solvent taking advantage of in situ photogeneration of halide ions from the solvent molecules. In the presence of a small amount of Mn acetate dissolve

Experimental information on the spatial extent of the putative p and conduction band states of the hydrated electron (eeq) has been obtained by monitoring and controlling the electron/hole spatial separation of a photogenerated eeq/hole pair using a femtosecond laser pulse sequence. Optical excitation of eeq with two photons is observed to dramatically alter its spatial distribution and geminate recombination yield with the hole. One-photon excitation, in contrast, has no effect on the spatial d

We report a ratiometric temperature imaging method based on Mn luminescence from Mn-doped CdS-ZnS nanocrystals (NCs) with controlled doping location, which is designed to exhibit strong temperature dependence of the spectral lineshape while being insensitive to the surrounding chemical environment. Ratiometric thermometry on the Mn luminescence spectrum was performed by using Mn-doped CdS-ZnS core-shell NCs that have a large local lattice strain on the Mn site, which results in the enhanced temp

The fine structure of the band edge exciton and the dark exciton photoluminescence (PL) are topics of significant interest in the research of semiconducting metal halide perovskite nanocrystals, with several conflicting reports on the level ordering of the bright and dark states and the accessibility of the emitting dark states. Recently, we observed the intense dark exciton PL in strongly confined CsPbBr₃ nanocrystals at cryogenic temperatures, in contrast to weakly confined nanocrys

The photo-induced enhancement of second harmonic generation and the effect of nanocrystal shape and pump intensity on confined acoustic phonons in semiconductor nanocrystals have been investigated with time-resolved scattering and absorption measurements. The second harmonic signal showed a sublinear increase of the second-order susceptibility with respect to the pump pulse energy, indicating a reduction of the effective one-electron second-order nonlinearity with increasing electron-hole densit