Eco-friendly luminescent solar concentrators with low reabsorption losses and resistance to concentration quenching based on aqueous-solution-processed thiolate-gold nanoclusters.

Heavy-metal-containing quantum dots (QDs) with engineered electronic states have been served as luminophores in luminescent solar concentrators (LSCs) with impressive optical efficiency. Unfortunately, those QDs involve toxic elements and need to be synthesized in a hazardous solvent. Recently, biocompatible, eco-friendly gold nanoclusters (AuNCs), which can be directly synthesized in an aqueous solution, have gained much attention for promising applications in 'green photonics'. Here, we explored the solid-state photophysical properties of aqueous-solution-processed, glutathione-stabilized gold nanoclusters (GSH-AuNCs) with a ligand-to-metal charge-transfer (LMCT) state for developing 'green' LSCs. We found that such GSH-AuNCs exhibit a large Stokes shift with almost no spectral overlap between the optical absorption and PL emission due to the LMCT states, thus, suppressing reabsorption losses. Compared with GSH-AuNCs in solution, the photoluminescence quantum yields (PL-QYs) of the LSCs can be enhanced, accompanied with a lengthened PL lifetime owing to the suppression of non-radiative recombination rates. In addition, the LSCs do not suffer from severe concentration-induced PL quenching, which is a common weakness for conventional luminophores. As a result, a common trade-off between light-harvesting efficiency and solid-state PL-QYs can be bypassed due to nearly-zero spectral overlap integral between the optical absorption and PL emission. We expect that GSH-AuNCs hold great promise for serving as luminophores for 'green' LSCs by further enhancing solid-state PL-QYs.

Synthesis of N-doped graphene quantum dots by pulsed laser ablation with diethylenetriamine (DETA) and their photoluminescence.

We report a facile, fast, and one-step approach to prepare N-doped graphene quantum dots (GQDs) using pulsed laser ablation with diethylenetriamine (DETA). The synthesized N-doped GQDs with an average size of about 3.4 nm and an N/C atomic ratio of 26% have been demonstrated. Compared to pristine GQDs, the N-doped GQDs emit enhanced photoluminescence (PL) with a factor as high as 66, originated from the enhanced densities of pyridinic and graphitic N. The temperature-dependent PL of the N-doped GQDs was studied from cryogenic to room temperature. An anomalous temperature dependence of PL intensity was observed for the N-doped GQDs, which was ascribed to a carrier transfer mechanism from a dopant-induced state to the quantum-dot emitting state.

Solid-state, ambient-operation thermally activated delayed fluorescence from flexible, non-toxic gold-nanocluster thin films: towards the development of biocompatible light-emitting devices.

Luminescent gold nanoclusters (AuNCs) with good biocompatibility have gained much attention in bio-photonics. In addition, they also exhibit a unique photo-physical property, namely thermally activated delayed fluorescence (TADF), by which both singlet and triplet excitons can be harvested. The combination of their non-toxic material property and unique TADF behavior makes AuNCs biocompatible nano-emitters for bio-related light-emitting devices. Unfortunately, the TADF emission is quenched when colloidal AuNCs are transferred to solid states under ambient environment. Here, a facile, low-cost and effective method was used to generate efficient and stable TADF emissions from solid AuNCs under ambient environment using polyvinyl alcohol as a solid matrix. To unravel the underlying mechanism, temperature-dependent static and transient photoluminescence measurements were performed and we found that two factors are crucial for solid TADF emission: small energy splitting between singlet and triplet states and the stabilization of the triplet states. Solid TADF films were also deposited on the flexible plastic substrate with patterned structures, thus mitigating the waveguide-mode losses. In addition, we also demonstrated that warm white light can be generated based on a co-doped single emissive layer, consisting of non-toxic, solution-processed TADF AuNCs and fluorescent carbon dots under UV excitation.

Origin of tunable photoluminescence from graphene quantum dots synthesized via pulsed laser ablation.

A one-step synthesis of graphene quantum dots (GQDs) has been implemented using pulsed laser ablation (PLA) with carboxyl-functionalized multiwalled carbon nanotubes (MWCNTs). The synthesized GQDs with an average size smaller than 3 nm were obtained by the fragmentation of MWCNTs via oxidative cutting. The GQDs can generate tunable photoluminescence (PL) ranging from green to blue by controlling the PLA time. The PL spectrum (decay time) of the green GQDs remains unchanged under different excitation energies (emission energies), while that of the blue GQDs correlates with the excitation energy (emission energy). On the basis of the pH and temperature dependence of PL, we suggest that the localized intrinsic states associated with the sp(2) nanodomains and delocalized extrinsic states embedded on the GQD surface are responsible for blue and green emission in GQDs, respectively.

Distance dependence of energy transfer from InGaN quantum wells to graphene oxide.

We report the distance-dependent energy transfer from an InGaN quantum well to graphene oxide (GO) by time-resolved photoluminescence (PL). A pronounced shortening of the PL decay time in the InGaN quantum well was observed when interacting with GO. The nature of the energy-transfer process has been analyzed, and we find the energy-transfer efficiency depends on the 1/d² separation distance, which is dominated by the layer-to-layer dipole coupling.

Efficient energy transfer from InGaN quantum wells to Ag nanoparticles.

Nonradiative energy transfer from an InGaN quantum well to Ag nanoparticles is unambiguously demonstrated by the time-resolved photoluminescence. The distance dependence of the energy transfer rate is found to be proportional to 1/d(3), in good agreement with the prediction of the dipole interaction calculated from the Joule losses in acceptors. The maximum energy-transfer efficiency of this energy transfer system can be as high as 83%.

Probing the photoluminescence properties of gold nanoclusters by fluorescence lifetime correlation spectroscopy.

Gold nanoclusters (Au NCs) have attracted much attention for promising applications in biological imaging owing to their tiny sizes and biocompatibility. So far, most efforts have been focused on the strategies for fabricating high-quality Au NCs and then characterized by conventional ensemble measurement. Here, a fusion single-molecule technique combining fluorescence correlation spectroscopy and time-correlated single-photon counting can be successfully applied to probe the photoluminescence (PL) properties for sparse Au NCs. In this case, the triplet-state dynamics and diffusion process can be observed simultaneously and the relevant time constants can be derived. This work provides a complementary insight into the PL mechanism at the molecular levels for Au NCs in solution.

Single fluorescent gold nanoclusters.

Both ensemble and single-molecule measurements were performed to explore the fluorescence properties of Au nanoclusters (NCs). Photoinduced fluorescence enhancement was observed for ensemble NCs in solution, but photobleaching was found at ambient environments. At the single-molecule level, fluorescence blinking and single-step photobleaching were observed. Furthermore, their time-resolved fluorescence shows a single exponential decay with a lifetime of approximately 7 ns and is insensitive to changes in fluorescence intensity. The lifetime distribution is more homogeneous within ensemble Au NCs as compared to CdSe QDs. Therefore, Au NCs have potential applications as nontoxic fluorescent labels for lifetime-based imaging microscopy. However, their low quantum yields and poor photostability are disadvantageous factors, which require further improvement.

Perceptions of hand hygiene practices in China.

Hand hygiene is considered one of the most important infection control measures for preventing healthcare-associated infections. However, compliance rates with recommended hand hygiene practices in hospitals remain low. Previous literature on ways to improve hand hygiene practices has focused on the USA and Europe, whereas studies from developing countries are less common. In this study, we sought to identify common issues and potential strategies for improving hand hygiene practices in hospitals in China. We used a qualitative survey design based on in-depth interviews with 25 key hospital and public health staff in eight hospitals selected by the Chinese Ministry of Health. We found that hospital workers viewed hand hygiene as paramount to effective infection control and had adequate knowledge about proper hand hygiene practices. Despite these positive attitudes and adequate knowledge, critical challenges to improving rates of proper hand hygiene practices were identified. These included lack of needed resources, limited organisational authority of hospital infection control departments, and ineffective use of data monitoring and feedback to motivate improvements. Our study suggests that a pivotal issue for improving hand hygiene practice in China is providing infection control departments adequate attention, priority, and influence within the hospital, with a clear line of authority to senior management. Elevating the place of infection control on the hospital organisational chart and changing the paradigm of surveillance to continuous monitoring and effective data feedback are central to achieving improved hand hygiene practices and quality of care.

Fluorescence signals of quantum dots influenced by spatially controlled array structures.

Fluorescence signals of quantum dots (QDs) influenced by different array structures of gold-coated silicon nanorods (SiNRs) were investigated via experimental observations and two-dimensional (2D) finite element method (FEM) simulations. On the densest gold-coated SiNRs array structure, the highest QD fluorescence quenching rates were observed and on the sparsest array structure, the highest QD fluorescence enhancement rates were observed. By developing a new technique which obtains the optical image of the array structures without losing information about the QD locations, we were able to further investigate how the QD fluorescence is influenced by spatially controlled array structures.

A facile method to prepare "green" nano-phosphors with a large Stokes-shift and solid-state enhanced photophysical properties based on surface-modified gold nanoclusters.

Colloidal nano-materials, such as quantum dots (QDs) have been applied to light-conversion nano-phosphors due to their unique tunable emission. However, most of the QDs involve toxic elements and are synthesized in a hazardous solvent. In addition, conventional QD nano-phosphors with a small Stokes shift suffered from reabsorption losses and aggregation-induced quenching in the solid state. Here, we demonstrate a facile, matrix-free method to prepare eco-friendly nano-phosphors with a large Stokes shift based on aqueous thiolate-stabilized gold nanoclusters (GSH-AuNCs) with simple surface modifications. Our method is just to drop GSH-AuNCs solution on the aluminum foil and then surface-modified AuNCs (Al-GSH-AuNCs) can be spontaneously precipitated out of the aqueous solution. Compared with pristine GSH-AuNCs in solution, the Al-GSH-AuNCs exhibit enhanced solid-state PL quantum yields, lengthened PL lifetime, and spectral blue shift, which can be attributed to the aggregation-induced emission enhancement facilitated by surface modifications. Such surface-treatment induced aggregation of AuNCs can restrict the surface-ligand motion, leading to the enhancement of PL properties in the solid state. In addition, the Al-GSH-AuNCs nano-phosphors with a large Stokes shift can mitigate the aggregation-induced PL quenching and reabsorption losses, which would be potential candidates for "green" nano-phosphors.

Photo-induced Doping in GaN Epilayers with Graphene Quantum Dots.

We demonstrate a new doping scheme where photo-induced carriers from graphene quantum dots (GQDs) can be injected into GaN and greatly enhance photoluminescence (PL) in GaN epilayers. An 8.3-fold enhancement of PL in GaN is observed after the doping. On the basis of time-resolved PL studies, the PL enhancement is attributed to the carrier transfer from GQDs to GaN. Such a carrier transfer process is caused by the work function difference between GQDs and GaN, which is verified by Kelvin probe measurements. We have also observed that photocurrent in GaN can be enhanced by 23-fold due to photo-induced doping with GQDs. The improved optical and transport properties from photo-induced doping are promising for applications in GaN-based optoelectronic devices.

A Facile and Low-Cost Method to Enhance the Internal Quantum Yield and External Light-Extraction Efficiency for Flexible Light-Emitting Carbon-Dot Films.

Solution-processed, non-toxic carbon dots (CDs) have attracted much attention due to their unique photoluminescence (PL) properties. They are promising emissive layers for flexible light-emitting devices. To this end, the CDs in pristine aqueous solutions need to be transferred to form solid-state thin films without sacrificing their original PL characteristics. Unfortunately, solid-state PL quenching induced by extra non-radiative (NR) energy transfer among CDs would significantly hinder their practical applications in optoelectronics. Here, a facile, low-cost and effective method has been utilized to fabricate high-performance CD/polymer light-emitting flexible films with submicron-structured patterns. The patterned polymers can serve as a solid matrix to disperse and passivate CDs, thus achieving high internal quantum yields of 61%. In addition, they can act as an out-coupler to mitigate the waveguide-mode losses, approximately doubling the external light-extraction efficiency. Such CD/polymer composites also exhibit good photo-stability, and thus can be used as eco-friendly, low-cost phosphors for solid-state lighting.

Laser-ablation production of graphene oxide nanostructures: from ribbons to quantum dots.

A new one-step method for the preparation of graphene oxide (GO) nanostructures has been developed by pulsed laser ablation in GO solution. The formation of different shapes of GO nanostructures, such as ribbons, nanoflakes (including nano-squares, nano-rectangles, nano-triangles, nano-hexagons, and nano-disks) and quantum dots, has been demonstrated by scanning electron microscopy and transmission electron microscopy. Photoreduction for the GO occurred during irradiation by the pulsed laser. The GO quantum dots exhibit a blue photoluminescence, originating from recombination of the localized carriers in the zigzag-edge states.

Antibunching single-photon emission and blinking suppression of CdSe/ZnS quantum dots.

We demonstrated that by properly coupling to silver nanoprisms, single CdSe/ZnS semiconductor quantum dots (QDs) exhibited suppressed blinking behavior, an enhanced fluorescence intensity ( approximately 2.5 fold), increased radiative decay rates ( approximately 12.5 fold), and antibunching single-photon emission. All these modifications significantly promote the overall performance of the proposed single-photon sources based on colloidal semiconductor QDs.