Replica symmetry breaking in a colloidal plasmonic random laser with gold-coated triangular silver nanostructures.

Plasmonic random lasers have drawn significant attention recently due to their versatility, low threshold, and the possibility of achieving tunable and coherent/incoherent outputs. However, in this Letter, the phenomenon of replica symmetry breaking is reported in intensity fluctuations of a rarely used colloidal plasmonic random laser (RL) illumination. Triangular nanosilver scatter particles produced incoherent RL action when used in a dimethylformamide (DMF) environment in a Rhodamine-6G gain medium. The use of gold-coated triangular nanosilver as the scatterer in place of triangular nanosilver offered a dual contribution of scattering and lower photo-reabsorption, which caused a reduction in the lasing threshold energy of 39% compared to that obtained with the latter. Further, due to its long-term photostability and chemical properties, a phase transition from the photonic paramagnetic to the glassy phase is observed experimentally in the RL system used. Interestingly, the transition occurs at approximately the lasing threshold value, which is a consequence of stronger correlation of modal behaviors at high input pump energies.

Transition metal dichalcogenides nanomaterials based piezocatalytic activity: recent progresses and outlook.

Piezoelectric materials have drawn significant attention from researchers in the recent past as the piezo-potential, induced by applied external stress, generates an electric field, which paves the way for the creation and transfer of electrons and holes. After the theoretical prediction of the existence of the piezoelectric effect in transition metal dichalcogenides (TMDCs) semiconductors, intense research efforts have been made by various researchers to demonstrate the effect experimentally. In addition 2D TMDCs exhibit layer-dependent tunable electronic structure, strongly bound excitons, enhanced catalytic activity at their edges, and novel spin/pseudospin degrees of freedom. The edge sites and activated basal planes of 2D TMDCs are shown to be highly active toward catalysis of the hydrogen evolution reaction (HER). However, as compared to electrocatalytic or even photocatalytic performances, TMDC materials exhibit poorer piezocatalytic activity, in general. Therefore, a numbers of research strategies have been made to intensify the piezoelectric effect by synthesizing different types of TMDC nanostructures, by coupling the piezoelectric effect with the photocatalytic effect, by doping with other materials, etc. This review discusses various techniques of synthesis of TMDCs nanostructures and the recent progresses in applications of TMDC nanomaterials in piezocatalysis. In the present article, the piezocatalytic dye degradation performances and HER activity using different TMDCs have been reviewed in detail. Different methods of increasing the piezocatalytic activity of various TMDCs nanostructures have been illustrated. Here, it has also been attempted to systematically summarize and provide an outlook of the charge transfer behaviour and catalytic mechanisms in large varieties of TMDC piezocatalysts and piezo-photocatalysts. In addition, advanced applications of TMDC piezocatalytic materials as piezoelectric nanogenerator, piezocatalytic dye degradation, piezo-phototronic dye degradation and HER studies have been highlighted.

Utilization of DNA and 2D metal oxide interaction for an optical biosensor.

The efficient monitoring and early detection of viruses may provide essential information about diseases. In this work, we have highlighted the interaction between DNA and a two-dimensional (2D) metal oxide for developing biosensors for further detection of viral infections. Spectroscopic measurements have been used to probe the efficient interactions between single-stranded DNA (ssDNA) and the 2D metal oxide and make them ideal candidates for detecting viral infections. We have also used fully atomistic molecular dynamics (MD) simulation to give a microscopic understanding of the experimentally observed ssDNA-metal oxide interaction. The adsorption of ssDNA on the inorganic surface was found to be driven by favourable enthalpy change, and 5'-guanine was identified as the interacting nucleotide base. Additionally, the in silico assessment of the conformational changes of the ssDNA chain during the adsorption process was also performed in a quantitative manner. Finally, we comment on the practical implications of these developments for sensing that could help design advanced systems for preventing virus-related pandemics.

Identification of aggregated 2D cobalt tellurides using a spatial self-phase modulation technique.

We report a previously unreported application of the spatial self-phase modulation (SSPM) technique for recognizing solute-solvent interaction in a suspension of 2D material. Broadband optical absorption of the 2D Co2Te3 leads to a nonlinear optical (NLO) susceptibility for the monolayer, i.e., χ M o n o(3) of 1.5 ×10-9 (3.3 ×10-9) esu at 532 (632) nm, which is 1-2 orders higher than for the 2D CoTe and CoTe2. The fine structure of the SSPM patterns is analyzed to explore the foundations of the observed NLO effects. With increasing polarity of the liquid media, a change of 2D Co2Te3 from homophonous dispersion to aggregation occurs, as confirmed from in situ optical microscopy and UV-vis absorption spectroscopy. As a result, type-I (thickest outer ring) SSPM ring patterns are converted to type-II (thinnest outer ring) SSPM ring patterns. Therefore, using SSPM with a CW laser as an optical tool to identify solvent-polarity-induced aggregation in 2D materials is possible.

Dye-Derived Red-Emitting Carbon Dots for Lasing and Solid-State Lighting.

Carbon dots are carbon-based nanoparticles renowned for their intense light-emitting capabilities covering the whole visible light range. Achieving carbon dots emitting in the red region with high efficiency is extremely relevant due to their huge potential in biological applications and in optoelectronics. Currently, photoluminescence in such an energy interval is often associated with polyheterocyclic molecular domains forming during the synthesis that, however, present low emission efficiency and issues in controlling the optical features. Here, we overcome these problems by solvothermally synthesizing carbon dots starting from Neutral Red, a common red-emitting dye, as a molecular precursor. As a result of the synthesis, such molecular fluorophore is incorporated into a carbonaceous core while retaining its original optical properties. The obtained nanoparticles are highly luminescent in the red region, with a quantum yield comparable to that of the starting dye. Most importantly, the nanoparticle carbogenic matrix protects the Neutral Red molecules from photobleaching under ultraviolet excitation while preventing aggregation-induced quenching, thus allowing solid-state emission. These advantages have been exploited to develop a fluorescence-based color conversion layer by fabricating polymer-based highly concentrated solid-state carbon dot nanocomposites. Finally, the dye-based carbon dots demonstrate both stable Fabry-Perot lasing and efficient random lasing emission in the red region.

Syntheses of flower and tube-like MoSe2 nanostructures for ultrafast piezocatalytic degradation of organic dyes on cotton fabrics.

The synthesis of few-layered transition metal dichalcogenides (TMDCs) with abundant exposure of the active site, viz., is an important key to achieve excellent dye degradation performance. Here, we have reported synthesis and ultrafast dye degradation performance of flowers-like MoSe2 nanostructure (FMN) with ~230 nm in diameter and its transformation to tube-like MoSe2 microstructure (~1 µm in length) by tuning the solvothermal reaction time. The piezoelectric devices are developed using the FMNs delivers the highest open-circuit voltage of ~ 2.12 V, which is ~21 times higher than that of the developed device with the tube-like MoSe2 microstructure. The piezoelectric property of the synthesized samples has been judiciously utilized further for ultrafast degradation of organic dyes within 60-120 s only under the low-frequency (40 kHz) ultrasonication vibration in the dark. The estimated dye degradation efficiencies of the FMNs-based piezocatalyst are found to be ∼86% and 85% for degradation of Rhodamine B (RhB) and methylene blue (MB) dye within the 60 s, respectively. Also, the FMN has exhibited an excellent piezocatalytic dye degradation capability for RhB-MB dye mixture and dye loaded on a cotton fabric with an efficiency of ~98% (60 s) and 84% (120 s), respectively. The piezocatalytic dye degradation mechanism of FMNs has also been explained theoretically.

Self-Assembly of Solvent-Stabilized Au Nanocluster as Efficient Förster Resonance Energy-Transfer Initiator for White Light Generation.

Aggregation-induced enhancement (AIE) in the photoluminescence quantum yield (PLQY) from 12.5 to 51% in the N,N-dimethylformamide (DMF)-stabilized Au nanocluster (AuNC) system is reported here. The self-assembling of AuNC has been achieved via hydrogen bonding interaction, which is further utilized in designing the AuNC_DCM system for realizing a Förster resonance energy transfer (FRET)-based white LED (WLED), having CIE coordinates of (0.35, 0.29). The solution-processed fabrication strategy used, has given us the liberty to optimize its components for optimal full-spectrum light output. The CIE coordinates of the designed WLED have been improved further to (0.33, 0.32), with a high color rendering index of 93 and correlated color temperature of 5620 K by incorporating a green emitter, namely nitrogen-doped graphene quantum dots (NGQD), in the AuNC_DCM system. The excellent spectral quality of the as-designed WLED and the repeatability of the proposed fabrication method will make the developed AuNCs_DCM FRET conjugate useful in practical photonic applications.

Forster resonance energy transfer assisted white light generation and luminescence tuning in a colloidal graphene quantum dot-dye system.

The development of white light-emitting LED (WLED) is now one of the important demands of present society due to its energy saving feature. However, in this work, an ingenious strategy has been employed to develop Forster resonance energy transfer (FRET) based and rare-earth material free luminescent duo (LD) for the generation of white light. A colloidal LD, consisting of nitrogen-doped graphene quantum dots (N-GQDs) and DCM dye (DCM@N-GQDs), is employed for demonstrating the FRET. The band-gap is engineered by nitrogen (N) doping in GQDs, and an energy transfer efficiency of ~30% for white light generation is attained. The widely tunable PL emission from blue to the red region has been obtained by changing the D-A ratio. Therefore, the present work has provided an alternate approach to widen the light emission band of a conventional laser dye, which is otherwise restricted within a limited region of the visible spectrum. FRET-based WLED (F-WLEDs) with colour rendering index of 70 and correlated colour temperature of 4690 K have also been fabricated. The F-WLED exhibits an emission overlapping of 56% with the solar spectrum (AM 1.5) in visible region, which is doubled in compared to that of a commercial WLED. The present report of rapid synthesis of highly luminescent N doped GQDs and the strategy used here for generation of FRET based colloidal DCM-GQDs luminescent duo may also be extended further with other suitable laser dyes for further widening as well as tuning the spectral range of light emissions of different commercially available laser dyes and GQDs for their different photonic applications.

In-situ synthesis of rGO-ZnO nanocomposite for demonstration of sunlight driven enhanced photocatalytic and self-cleaning of organic dyes and tea stains of cotton fabrics.

Recently, research activities are focused on development of 2D reduced graphene oxide (rGO) based semiconductor nanocomposite materials for boosting up its catalytic applications. In this work, a rarely reported green synthesis approach has been envisioned to synthesize in-situ 2D rGO-ZnO (rGZn) nanocomposites from Apple juice and zinc acetate. Also the composition of the samples has been optimized to achieve high photocatalytic and self-cleaning properties by the formation of reactive oxidation species. The samples are characterized for their microstructural, optical absorption and photoluminescence properties. It has been tested that rGZn nanocomposites are capable of removing a test dye, namely methylene blue (MB) from water and achieved the highest dye degradation efficiency of ∼91% within only 60 min under UV-vis light irradiation. A smart cotton fabric (CF) coated with rGZn has been prepared and demonstrated its photocatalytic self-cleaning property by degradation of MB, rhodamine B dyes and tea stains on it even under sunlight irradiation, which is scarcely available in the literature. Therefore, this work may open a new avenue of research for low cost and easy synthesis of rGO-semiconductor nanocomposites with high photocatalytic properties for industrial applications as well as for development of rGO based smart fabric for real-life applications.

Colloidal N-Doped Graphene Quantum Dots with Tailored Luminescent Downshifting and Detection of UVA Radiation with Enhanced Responsivity.

Luminescent downshifting (LDS) materials are in great demand for their applications in light conversion devices. In this work, by an ingenious chemical approach of in situ doping, N-doped graphene quantum dots (N-GQDs) have been synthesized with tailored green photoluminescence (PL) under ultraviolet (UV) light excitation. The incorporation of N atoms in the form of pyridinic and graphitic C-N bonding into the sp2-hybridized graphitic framework of N-GQDs has led to tailored LDS via PL emissions. The LDS property of synthesized N-GQDs has been advantageously utilized to demonstrate enhanced responsivity (R) of a low-cost commercially available photoconductive cell (PC) for detection of UVA radiation through an indigenous technique. The linear optical responses of samples are optimized by varying the concentration and the dispersing medium. Also the N-GQDs are shown to be photostable in poly(vinyl alcohol) (PVA) hydrogel. A 60% enhancement in photocurrent of the PC-based photodetector under UV radiation has been obtained here by using N-GQDs/PVA as LDS material. Thus, detection of UVA radiation with a high specific detectivity (D*) of 9 × 1013 Jones and responsivity (R) of 3 A W-1 has been demonstrated, which might open the opportunity of using this material in future energy conversion devices.