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.
27 July 2022 in ACS Applied Materials & Interfaces
Carbon dots (CDs) are a family of fluorescent nanoparticles displaying a wide range of interesting properties, which make them attractive for potential applications in different fields like bioimaging, photocatalysis, and many others. However, despite many years of dedicated studies, wide variations exist in the literature concerning the reported photostability of CDs, and even the photoluminescence mechanism is still unclear. Furthermore, an increasing number of recent studies have highlighted the photobleaching (PB) of CDs under intense UV or visible light beams. PB phenomena need to be fully addressed to optimize practical uses of CDs and can also provide information on the fundamental mechanism underlying their fluorescence. Moreover, the lack of systematic studies comparing several types of CDs displaying different fluorescence properties represents another gap in the literature. In this study, we explored the optical properties of a full palette of CDs displaying a range from blue to red emissions, synthesized using different routes and varying precursors. We investigated the photostability of different CDs by observing in situ their time-resolved fluorescence degradation or optical absorption changes under equivalent experimental conditions and laser irradiation. The results about different PB kinetics clearly indicate that even CDs showing comparable emission properties may exhibit radically different resistances to PB, suggesting systematic connections between the resistance to PB, the characteristic spectral range of emission, and CD quantum yields. To exploit the PB dynamics as a powerful tool to investigate CD photophysics, we also carried out dedicated experiments in a partial illumination geometry, allowing us to analyze the recovery of the fluorescence due to diffusion. Based on the experimental results, we conclude that the nature of the CD fluorescence cannot be solely ascribable to small optically active molecules free diffusing in solution, contributing to shed light on one of the most debated issues in the photophysics of CDs.
In recent years, the progress toward lighting miniaturization is focused on luminescent nanomaterials. Among them, fluorescent carbon dots (CDs) are receiving increasing attention thanks to their astonishing optical properties complemented by their intrinsic biocompatibility and low toxicity. The CDs can be easily dispersed in water, organic solvents or incorporated in polymeric matrices, preserving their emission properties. However, the relationship between their structural and optical properties is still not fully elucidated, motivating a consistent research effort for the comprehension of their features. Nevertheless, CDs demonstrate to be efficient gain materials for lasing, thanks to their high quantum yield (QY), emission tunability in the visible and near infrared (NIR) range, short lifetimes, and high absorption cross section, even if the synthetic reproducibility, the low reaction yield and the spectral width of the emission may limit their effective exploitation. This review summarizes the latest advancements in the investigation of the characteristic properties of CDs that make laser action possible, illustrating optical geometries for lasing and random lasing, both in solution and solid state, and the few currently demonstrated breakthroughs. While the journey toward their effective application is still long, the potential of CD‐based laser sources is promising in various technological fields and futuristic perspectives will be discussed.
Strain‐dependent electronic and optical properties are one of the most appealing features of 2D semiconductors, like monolayer (1L) MoS 2 . However, measuring and controlling the homogeneity of strain within the channel is crucial for next‐generation MoS 2 field‐effect transistors (FETs). This article reports a multiscale investigation of backgated FETs fabricated using large‐area 1L MoS 2 flakes grown by liquid‐precursor‐intermediated chemical vapor deposition on SiO 2 /Si substrates. The devices exhibit very attractive properties for ultra‐low power applications, such as an Ion / Ioff > 10 6 and a normally off electrical behavior. The combination of temperature‐dependent analyses of the FET transfer characteristics and nanoscale resolution potential mapping by Kelvin probe force microscopy shows a fully depleted MoS 2 channel at VG = 0 and an effective Schottky barrier Φ B,FB = 0.21 eV at flatband voltage VFB = 17.9 V. An inhomogeneous tensile strain ( ε ) distribution along the channel length is revealed by micro‐Raman and photoluminescence (PL) mapping, with a reduced ε and blue‐shifted PL energy close to the Ni/Au source/drain contacts, suggesting a biaxial compression of 1L MoS 2 induced by metal deposition. The implications of these observations on the effective mass m eff variation along the channel and the current injection from source/drain contacts have been discussed in the perspective of future ultra‐scaled‐devices applications.
Carbon Dots (CDs) are fluorescent carbon-based nanoparticles that have attracted increasing attention in recent years as environment-friendly and cost-effective fluorophores. An application that can benefit from CDs in a relatively short-term perspective is the fabrication of color-converting materials in phosphor-converted white LEDs (WLEDs). In this work we present a one-pot solvothermal synthesis of polymer-passivated CDs that show a dual emission band (in the green and in the red regions) upon blue light excitation. A purposely designed numerical approach enables evaluating how the spectroscopic properties of such CDs can be profitable for application in WLEDs emulating daylight characteristics. Subsequently, we fabricate nanocomposite coatings based on the dual color-emitting CDs via solution-based strategies, and we compare their color-converting properties with those of the simulated ones to finally accomplish white light emission. The combined numerical and experimental approach can find a general use to reduce the number of experimental trial-and-error steps required for optimization of CD optical properties for lighting application.