Sudipta Seth

Fluorescence Blinking and Photoactivation of All-Inorganic Perovskite Nanocrystals CsPbBr3 and CsPbBr2I

Study of the emission behavior of all-inorganic perovskite nanocrystals CsPbBr3 and CsPbBr2I as a function of the excitation power employing fluorescence correlation spectroscopy and conventional techniques reveals fluorescence blinking in the microsecond time scale and photoinduced emission enhancement. The observation provides insight into the radiative and nonradiative deactivation pathways of these promising substances. Because both blinking and photoactivation processes are intimately linked to the charge separation efficiency and dynamics of the nanocrystals, these key findings are likely to be helpful in realizing the true potential of these substances in photovoltaic and optoelectronic applications.

A Facile Methodology for Engineering the Morphology of CsPbX3 Perovskite Nanocrystals under Ambient Condition

A facile and highly reproducible room temperature, open atmosphere synthesis of cesium lead halide perovskite nanocrystals of six different morphologies is reported just by varying the solvent, ligand and reaction time. Sequential evolution of the quantum dots, nanoplates and nanobars in one medium and nanocubes, nanorods and nanowires in another medium is demonstrated. These perovskite nanoparticles are shown to be of excellent crystalline quality with high fluorescence quantum yield. A mechanism of the formation of nanoparticles of different shapes and sizes is proposed. Considering the key role of morphology in nanotechnology, this simple method of fabrication of a wide range of high quality nanocrystals of different shapes and sizes of all-inorganic lead halide perovskites, whose potential is already demonstrated in light emitting and photovoltaic applications, is likely to help widening the scope and utility of these materials in optoelectronic devices.

Fluorescent Phase-Pure Zero-Dimensional Perovskite-Related Cs4PbBr6 Microdisks: Synthesis and Single-Particle Imaging Study

Quantum-confined perovskites are a new class of promising materials in optoelectronic applications. In this context, a zero-dimensional perovskite-related substance, Cs4PbBr6, having high exciton binding energy can be an important candidate, but its photoluminescence (PL) is a topic of recent debate. Herein, we report an ambient condition controlled synthesis of Cs4PbBr6 microdisks of different shapes and dimensions which exhibit fairly strong green PL (quantum yield up to 38%, band gap ∼2.43 eV) in the solid state. Using confocal fluorescence microscopy imaging of the single particles, we show that the fluorescence of Cs4PbBr6 microdisks is inherent to these particles. Fluorescence intensity and lifetime imaging of the microdisks reveals significant spatial heterogeneity with a bright central area and somewhat dimmer edges. This intensity and lifetime distribution is attributed to enhanced trap-mediated nonradiative deactivation at the edges compared to the central region of the microdisks. Our results, which unambiguously establish the PL of these Cs4PbBr6 and suggest its possible origin, brighten the potential of these materials in photon-emitting applications.

Contrasting Response of Two Dipolar Fluorescence Probes in a Leucine‐Based Organogel and Its Implications

The microenvironments of a leucine-based organogel are probed by monitoring the fluorescence behavior of coumarin 153 (C153) and 4-aminophthalimide (AP). The steady-state data reveals distinctly different locations of the two molecules in the gel. Whereas AP resides close to the hydroxyl moieties of the gelator and engages in hydrogen-bonding interactions, C153 is found in bulk-toluene-like regions. In contrast to C153, AP exhibits excitation-wavelength-dependent emission, indicating that the environments of the hydrogen-bonded AP molecules are not all identical. A two-component fluorescence decay of AP in gel, unlike C153, supports this model. A time-resolved fluorescence anisotropy study of the rotational motion of the molecules also reveals the strong association of only AP with the gelator. That AP influences the critical gelation concentration implies its direct involvement in the gel-formation process. The results highlight the importance of guest-gelator interactions in gels containing guest molecules.

Effect of Controlled Deposition of ZnS Shell on the Photostability of CdTe Quantum Dots as Studied by Conventional Fluorescence and FCS Techniques

The effect of one and two monolayers of ZnS shells on the photostability of CdTe quantum dots (QDs) in aqueous and nonaqueous media has been studied by monitoring the fluorescence behavior of the QDs under ensemble and single-molecule conditions. ZnS capping of the CdTe QDs leads to significant enhancement of the fluorescence brightness of these QDs. Considerable enhancement of the photostability of the shell-protected QDs, including the suppression of photoactivation, is also observed. Fluorescence correlation spectroscopy measurements reveal an increase in the number of particles undergoing reversible fluorescent on-off transitions in the volume under observation with increasing excitation power; this effect is found to be more pronounced in the case of core-only QDs than for core-shell QDs.

Photoluminescence of Zero-Dimensional Perovskites and Perovskite-Related Materials

Zero-dimensional (0-D) perovskites and perovskite-related materials are an emerging class of optoelectronic materials exhibiting strong excitonic properties and, quite often, high photoluminescence (PL) in the solid state. Here we highlight two different classes of 0-D perovskites with contrasting structural and optical properties, focusing mainly on the less explored but rapidly growing bulk quantum materials termed as 0-D perovskite-related materials (0-D PRMs), whose PL properties are quite intriguing and a topic of recent debate. We attempt to present here a comprehensive picture to rationalize the contrasting properties of the 0-D PRMs and provide an understanding of the mechanism of exciton dynamics and PL of this class of materials. We hope that exciting PL and tunable composition of these systems will help design of new materials with versatile optical properties suited for practical applications.

Nucleation and self-assembly of CsPbX3 perovskite nanocrystals

In recent years lead halide perovskites have become a burgeoning topic of research due to their promising optoelectronic applications. As optical and electronic properties of the nanocrystals (NCs) are determined largely by their shape and size, the morphologies of the NCs are crucial to their applications. Unlike tedious hot injection technique, ambient condition, antisolvent precipitation is a facile and cost effective method for nanoparticle synthesis. CsPbX3 perovskite NCs of six different morphologies are synthesized just by varying the solvent, ligand and reaction time. NCs with dot and cubic shapes are formed as the nucleation product in two solvents of different polarity, namely toluene and ethyl acetate. We have systematically studied the self-assembly of these NCs yielding nanoplates and nanobars in one medium and nanorods and nanowires in another medium by controlling the time interval and ligand concentration. Our findings suggest that polarity of the environment has a major role in determining the shape and size of the resulting NCs. These perovskite nanoparticles are shown to be of excellent crystalline quality with high fluorescence quantum yield. Considering the key role of morphology in nanotechnology, this simple method of fabrication of a wide range of high quality nanocrystals of different shapes and sizes of all-inorganic lead halide perovskites, is likely to help widening the scope and utility of these materials in optoelectronic devices. Seth. S. & Samanta. A. (2016). Sci. Rep. 6, 37693.