Non-convergence of the blinking timescale of twelve-faceted perovskite nanocrystals observed through an advanced fluorescence correlation spectroscopy study.

Single-particle photoluminescence measurements have been extensively utilized to investigate the charge carrier dynamics in quantum dots (QDs). Among these techniques, single dot blinking studies are effective for probing relatively slower processes with timescales >10 ms, whereas fluorescence correlation spectroscopy (FCS) studies are suited for recording faster processes with timescales typically <1 ms. In this study, we utilized scanning FCS (sFCS) to bridge the ms gap, thereby enabling the tracking of carrier dynamics across an extended temporal window ranging from μs to subsecond.

Evidence of carrier diffusion between emission states in CdSe/ZnS core-shell quantum dots: a comprehensive investigation combining fluorescence lifetime correlation spectroscopy (FLCS) and single dot photoluminescence studies.

Investigation of carrier dynamics in CdSe/ZnS core-shell quantum dots (QDs) is performed using fluorescence-lifetime-correlation-spectroscopy (FLCS) and single-dot PL blinking studies. The origin of an emitted photon from a QD in an FLCS study is assigned to either an exciton state or trap state based on its excited state lifetime (). Subsequently, two intrastate autocorrelation functions (ACFs) representing the exciton and trap states and one cross-correlation function (CCF) coupling these two states are constructed.

Unveiling the Influence of Brightness Heterogeneity in Fluorescence Correlation Spectroscopy of Perovskite Nanocrystals.

Nanoparticles (NPs), including perovskite nanocrystals (PNCs) with single photon purity, present challenges in fluorescence correlation spectroscopy (FCS) studies due to their distinct photoluminescence (PL) behaviors. In particular, the zero-time correlation amplitude [g(0)] and the associated diffusion timescale (τ) of their FCS curves show substantial dependency on pump intensity (I). Optical saturation inadequately explains the origin of this FCS phenomenon in NPs, thus setting them apart from conventional dye molecules, which do not manifest such behavior.

Facet Dependent Photoluminescence Blinking from Perovskite Nanocrystals.

Photoluminescence (PL) blinking of nanoparticles, while detrimental to their imaging applications, may benefit next-generation displays if the blinking is precisely controlled by reversible electron/hole injections from an external source. Considerable efforts are made to create well-characterized charged excitons within nanoparticles through electrochemical charging, which has led to enhanced control over PL-blinking in numerous instances. Manipulating the photocharging/discharging rates in nanoparticles by surface engineering can represent a straightforward method for regulating their blinking behaviors, an area largely unexplored for perovskite nanocrystals (PNCs).

Dodecahedron CsPbBr Perovskite Nanocrystals Enable Facile Harvesting of Hot Electrons and Holes.

This Letter reports the facile harvesting of hot carriers (HCs) in a composite of 12-faceted dodecahedron CsPbBr nanocrystal (NC) and a scavenger molecule. We recorded ∼3.3 × 10 s HC cooling rate in NC when excited with ∼1.

Facet Engineering for Decelerated Carrier Cooling in Polyhedral Perovskite Nanocrystals.

We report here the hot carrier (HC) cooling time scales within polyhedral CsPbBr nanocrystals (NCs) characterized by different numbers of facets (6 to 26) utilizing a femtosecond upconversion setup. Interestingly, the observed cooling time scale slows many-fold (>10 times) upon opening the new facets on the NC surface. Furthermore, a temperature-dependent study reveals that cooling in multifaceted NCs is polaron mediated, where newly opened polar facets and the soft lattice of CsPbBr NCs play pivotal roles.