Evolution of the Electronic Properties of Tellurium Crystals with Plasma Irradiation Treatment.

Tellurium exhibits exceptional intrinsic electronic properties. However, investigations into the modulation of tellurium's electronic properties through physical modification are notably scarce. Here, we present a comprehensive study focused on the evolution of the electronic properties of tellurium crystal flakes under plasma irradiation treatment by employing conductive atomic force microscopy and Raman spectroscopy. The plasma-treated tellurium experienced a process of defect generation through lattice breaking. Prior to the degradation of electronic transport performance due to plasma irradiation treatment, we made a remarkable observation: in the low-energy region of hydrogen plasma-treated tellurium, a notable enhancement in conductivity was unexpectedly detected. The mechanism underlying this enhancement in electronic transport performance was thoroughly elucidated by comparing it with the electronic structure induced by argon plasma irradiation. This study not only fundamentally uncovers the effects of plasma irradiation on tellurium crystal flakes but also unearths an unprecedented trend of enhanced electronic transport performance at low irradiation energies when utilizing hydrogen plasma. This abnormal trend bears significant implications for guiding the prospective application of tellurium-based 2D materials in the realm of electronic devices.

Efficient full-color emitting carbon-dot-based composite phosphors by chemical dispersion.

Realizing full-color emission plays a key role in exploring the luminescence mechanisms of carbon dots (CDots) and promoting the applications of CDots in light-emitting diodes (LEDs). Herein, a synthesis strategy for full-color emitting CDots was developed through the solvothermal reaction of citric acid and urea with a constant mass ratio but varying reactant concentrations in solvent. With the reactant concentrations increasing, a dual regulation mechanism including an enhanced nucleation growth process and subsequently increased C[double bond, length as m-dash]O/C[double bond, length as m-dash]N-related surface states should be responsible for the photoluminescence (PL) shift of CDots from blue to red. Relying on the hydrolyzation and condensation processes of 3-aminopropyltrimethoxysilane, a simple and universal method was developed by chemically dispersing the CDots into a cross-linked silica network on the surface of SiO2 nanoparticles to produce efficient full-color emitting SiO2/CDot composite phosphors with considerable PL quantum yields in the range of 30-60%. It was proved that the full-color emitting SiO2/CDot composite phosphors could be flexibly applied in packaging white LEDs, releasing pure white light at the Commission Internationale de L'Eclairage (CIE) coordinates of (0.33, 0.33) with a color rendering index (CRI) of 80.4 and a high color-rendering white light coming entirely from CDots with the CIE coordinates of (0.34, 0.36) and a CRI of 97.4, indicating promising application of the full-color emitting SiO2/CDot composite phosphors in the LED field.

Thermally Activated Upconversion Near-Infrared Photoluminescence from Carbon Dots Synthesized via Microwave Assisted Exfoliation.

Upconversion near-infrared (NIR) fluorescent carbon dots (CDs) are important for imaging applications. Herein, thermally activated upconversion photoluminescence (UCPL) in the NIR region, with an emission peak at 784 nm, which appears under 808 nm continuous-wave laser excitation, are realized in the NIR absorbing/emissive CDs (NIR-CDs). The NIR-CDs are synthesized by microwave-assisted exfoliation of red emissive CDs in dimethylformamide, and feature single or few-layered graphene-like cores. This structure provides an enhanced contact area of the graphene-like plates in the core with the electron-acceptor carbonyl groups in dimethylformamide, which contributes to the main NIR absorption band peaked at 724 nm and a tail band in 800-850 nm. Temperature-dependent photoluminescence spectra and transient absorption spectra confirm that the UCPL of NIR-CDs is due to the thermally activated electron transitions in the excited state, rather than the multiphoton absorption process. Temperature dependent upconversion NIR luminescence imaging is demonstrated for NIR-CDs embedded in a polyvinyl pyrrolidone film, and the NIR upconversion luminescence imaging in vivo using NIR-CDs in a mouse model is accomplished.

Efficient Red/Near-Infrared-Emissive Carbon Nanodots with Multiphoton Excited Upconversion Fluorescence.

Red/near-infrared (NIR) emissive carbon nanodots (CNDs) with photoluminescence (PL) quantum yield (QY) of 57% are prepared via an in situ solvent-free carbonization strategy for the first time. 1-Photon and 2-photon cellular imaging is demonstrated by using the CNDs as red/NIR fluorescence agent due to the high PL QY and low biotoxicity. Further study shows that the red/NIR CNDs exhibit multiphoton excited (MPE) upconversion fluorescence under excitation of 800-2000 nm, which involves three NIR windows (NIR-I, 650-950 nm; NIR-II, 1100-1350; NIR-III, 1600-1870 nm). 2-Photon, 3-photon, and 4-photon excited fluorescence of the CNDs under excitation of different wavelengths is achieved. This study develops an in situ solvent-free carbonization method for efficient red/NIR emissive CNDs with MPE upconversion fluorescence, which may push forward the application of the CNDs in bioimaging.

Synthesis of green emissive carbon dots@montmorillonite composites and their application for fabrication of light-emitting diodes and latent fingerprints markers.

Multifunctional solid-state luminescent materials are strongly desired in a wide variety of applications. In this work, green emissive carbon dots@montmorillonite (g-CDs@MMT) composites were synthesized based on green emissive carbon dots and MMT clays in a convenient method by embedding g-CDs into the MMT clays. Due to the confinement of g-CDs in the layered structure of the MMT clay matrix, g-CDs are uniformly dispersed in the resulting g-CDs@MMT solid-state composites. This efficiently prevents the aggregation-induced solid-state luminescence quenching of g-CDs, and a photoluminescence quantum yield of 11% could be achieved by the g-CDs@MMT composites under a 405 nm light. Additionally, the g-CDs@MMT composites exhibit low-toxicity, excellent thermal stability, photostability, resistance to organic solvents, and a small particle size. All of these advantages enable applications in fabricating white light-emitting diodes with different color temperatures, where the g-CDs@MMT composites are applied as the color conversion layer. Furthermore, by using the g-CDs@MMT composites as a fluorescence labeling marker, the latent fingerprint detection on a variety of object surfaces could be realized.

Carbon dots produced via space-confined vacuum heating: maintaining efficient luminescence in both dispersed and aggregated states.

Aggregation-induced quenching (AIQ) of emission is an obstacle for the development of carbon dots (CDots) for solid-state luminescent devices. In this work, we introduce a method to avoid AIQ and to produce highly luminescent CDots through a space-confined vacuum heating synthesis. In the presence of CaCl2, a mixture of citric acid and urea forms an inflated foam under vacuum heating at 120 °C. Upon gradually increasing the heating temperature to 250 °C, blue emissive molecular species are first formed, and are then transformed into uniform-sized green emissive CDots through dehydration and carbonization processes taking place in the confined ultrathin spaces of the foam walls. The green luminescence of these CDots originates from conjugated sp2 domains, and these CDots exhibit a high photoluminescence quantum yield (PLQY) of 72% in ethanol solution. Remarkably, due to the existence of only one type of recombination center in these nanoparticles, AIQ does not take place in CDot-based close-packed films, which show strong emission with a PLQY of 65%. Utilizing the differences in the emission properties of vacuum heating produced CDots, CDots synthesized through microwave-assisted heating, and commercial green fluorescent organic ink (namely, excitation-dependent vs. excitation-independent emission, and different stability against photobleaching), multilevel data encryption has been demonstrated.

Surface related intrinsic luminescence from carbon nanodots: solvent dependent piezochromism.

There has been a long standing debate on the luminescence origination from carbon nanodots (CDs). Herein, we report the solvent dependent piezochromism of CDs by diamond anvil cells experiment. Red- and blue-shift piezochromism were observed in CDs with N,N-dimethylformamide and water as pressure transmitting medium (PTM) with increasing pressure from atmospheric pressure to 25 GPa, which were related to increased π-π stacking and protic-solvent-induced surface chemical structural changes, respectively. Based on theoretical modeling and structural analysis of hydrothermally treated CDs (h-CDs), the reversible and irreversible piezochromism from green emission to blue emission with water as PTM was attributed to pressure induced enhanced intermolecular hydrogen bonding and addition reaction between water molecules and surface electron withdrawing groups on the CDs, respectively. The decreased electron withdrawing ability of the surface chemical structures of CDs further affects their intrinsic luminescence. This work provides a new understanding of the piezochromic luminescence origination from CDs, which is related to the surface related intrinsic luminescence.

In vivo theranostics with near-infrared-emitting carbon dots-highly efficient photothermal therapy based on passive targeting after intravenous administration.

Carbon dots that exhibit near-infrared fluorescence (NIR CDs) are considered emerging nanomaterials for advanced biomedical applications with low toxicity and superior photostability and targeting compared to currently used photoluminescence agents. Despite progress in the synthesis of NIR CDs, there remains a key obstacle to using them as an in vivo theranostic agent. This work demonstrates that the newly developed sulfur and nitrogen codoped NIR CDs are highly efficient in photothermal therapy (PTT) in mouse models (conversion efficiency of 59%) and can be readily visualized by photoluminescence and photoacoustic imaging. The real theranostic potential of NIR CDs is enhanced by their unique biodistribution and targeting. Contrary to all other nanomaterials that have been tested in biomedicine, they are excreted through the body's renal filtration system. Moreover, after intravenous injection, NIR CDs are accumulated in tumor tissue via passive targeting, without any active species such as antibodies. Due to their accumulation in tumor tissue without the need for intratumor injection, high photothermal conversion, excellent optical and photoacoustic imaging performance, and renal excretion, the developed CDs are suitable for transfer to clinical biomedical practice.

Investigation of Interface Effect on the Performance of CH3NH3PbCl3/ZnO UV Photodetectors.

Recent investigations indicate that the performance of organic-inorganic perovskite optoelectronic devices can be improved by combining the perovskites and the inorganic materials. However, very few studies have focused on the investigation of perovskites/inorganic semiconductor hybrid UV photodetectors and their detailed performance-enhancement mechanism is still not very clear. In this work, a CH3NH3PbCl3/ZnO UV photodetector has been first demonstrated and investigated. Both the photoresponsivity and response speed of the hybrid device are higher than those of pure CH3NH3PbCl3 and ZnO devices. The photoluminescence and transient absorption spectra indicate that the photoinduced electron transfer between CH3NH3PbCl3 and ZnO should be responsible for the performance enhancement of the hybrid device. In addition, the high crystal quality of CH3NH3PbCl3 on ZnO film is another important reason for the excellent UV detection performance. Our findings in this work provide new insights into the intrinsic photophysics essential for perovskite optoelectronic devices.

Multilevel Data Encryption Using Thermal-Treatment Controlled Room Temperature Phosphorescence of Carbon Dot/Polyvinylalcohol Composites.

Thermal-treatment controlled room temperature phosphorescence is realized by embedding either originally synthesized carbon dots (CDs) or 200 °C thermal-treated CDs into a polyvinylalcohol (PVA) matrix through post-synthetic thermal annealing at 200 or 150 °C. The thermal-treatment controlled phosphorescence is attributed to the transfer of photoexcitation from the excited singlet state to the triplet state through intersystem crossing, followed by radiative transition to the ground state, which is due to decrease of quenchers (oxygen) in the CDs and suppression of the vibrational dissipations through the chemical bonding of CDs in the PVA matrix. Multilevel fluorescence/phosphorescence data encryption is demonstrated based on the thermal-treatment controlled phosphorescence from CD@PVA composites.

Hydrogen Peroxide-Treated Carbon Dot Phosphor with a Bathochromic-Shifted, Aggregation-Enhanced Emission for Light-Emitting Devices and Visible Light Communication.

It is demonstrated that treatment of blue-emissive carbon dots (CDs) with aqueous hydrogen peroxide (H2O2) results in the green emissive solid state CD phosphor with photoluminescence quantum yield of 25% and short luminescence lifetime of 6 ns. The bathochromic-shifted, enhanced green emission of H2O2-treated CDs in the powder is ascribed to surface state changes occurring in the aggregated material. Using the green emissive H2O2-treated CD phosphor, down-conversion white-light-emitting devices with cool, pure, and warm white light are fabricated. Moreover, using the green emissive CD phosphor as a color converter, a laser-based white-light source is realized, and visible light communication with a high modulation bandwidth of up to 285 MHz and data transmission rate of ≈435 Mbps is demonstrated.

Ultrastrong Absorption Meets Ultraweak Absorption: Unraveling the Energy-Dissipative Routes for Dye-Sensitized Upconversion Luminescence.

Dye sensitization is becoming a new dimension to highly improve the upconversion luminescence (UCL) of lanthanide-doped upconversion nanoparticles (UCNPs). However, there is still a lack of general understanding of the dye-UCNPs interactions, especially the confused large mismatch between the inputs and outputs. By taking dye-sensitized NaYF4:Yb/Er@NaYF4:Nd UCNPs as a model system, we not only revealed the in-depth energy-dissipative process for dye-sensitized UCL but also confirmed the first ever experimental observation of the energy back transfer (EBT) in the dye-sensitized UCL. Furthermore, this energy-dissipative EBT restricted the optimal ratio of dyes to UCNP. By unearthing all of the energy loss behind the EBT, energy transfer, and energy migration processes, this paper sheds light on the further design of effective dye-sensitized nanosystems for UCL or even downconversion luminescence.

Microwave-Assisted Heating Method toward Multicolor Quantum Dot-Based Phosphors with Much Improved Luminescence.

Solid-state highly photoluminescent quantum dot (QD)-based phosphors attract great scientific interests as color converters because of an increasing demand for white-light-emitting devices. Herein, a microwave-assisted heating method is presented to fabricate multicolor QD-based phosphors within 30 s through microwave-assisted heating of the mixture of QDs and sodium silicate aqueous solution. In the composites, the formed cross-linked networks not only play as a matrix to prevent QD aggregation in solid state but also cause the variation of the refractive index around QDs and the QD surface optimization, which contributes to good stabilities and twice enhancement in photoluminescence quantum yields (69%) compared with the initial QD aqueous solution (33%). Using the QD-based phosphors as color conversion layers, white-light-emitting diodes were realized with controllable color temperature, high color purity, and high color-rendering index (90.3), which show a great potential in display and illumination. Furthermore, the luminescence lifetime of the QD-based phosphors is less than 25 ns. The potential application of the QD-based phosphors in visible light communication was also demonstrated, with the modulation bandwidth achieving 42 MHz.

Red carbon dots-based phosphors for white light-emitting diodes with color rendering index of 92.

Exploration of solid-state efficient red emissive carbon dots (CDs) phosphors is strongly desired for the development of high performance CDs-based white light-emitting diodes (WLEDs). In this work, enhanced red emissive CDs-based phosphors with photoluminescence quantum yields (PLQYs) of 25% were prepared by embedding red emissive CDs (PLQYs of 23%) into polyvinyl pyrrolidone (PVP). Because of the protection of PVP, the phosphors could preserve strong luminescence under long-term UV excitation or being mixed with conventional packaging materials. By applying the red emissive phosphors as the color conversion layer, WLEDs with high color rendering index of 92 and color coordinate of (0.33, 0.33) are fabricated.

Near-Infrared Excitation/Emission and Multiphoton-Induced Fluorescence of Carbon Dots.

Carbon dots (CDs) have significant potential for use in various fields including biomedicine, bioimaging, and optoelectronics. However, inefficient excitation and emission of CDs in both near-infrared (NIR-I and NIR-II) windows remains an issue. Solving this problem would yield significant improvement in the tissue-penetration depth for in vivo bioimaging with CDs. Here, an NIR absorption band and enhanced NIR fluorescence are both realized through the surface engineering of CDs, exploiting electron-acceptor groups, namely molecules or polymers rich in sulfoxide/carbonyl groups. These groups, which are bound to the outer layers and the edges of the CDs, influence the optical bandgap and promote electron transitions under NIR excitation. NIR-imaging information encryption and in vivo NIR fluorescence imaging of the stomach of a living mouse using CDs modified with poly(vinylpyrrolidone) in aqueous solution are demonstrated. In addition, excitation by a 1400 nm femtosecond laser yields simultaneous two-photon-induced NIR emission and three-photon-induced red emission of CDs in dimethyl sulfoxide. This study represents the realization of both NIR-I excitation and emission as well as two-photon- and three-photon-induced fluorescence of CDs excited in an NIR-II window, and provides a rational design approach for construction and clinical applications of CD-based NIR imaging agents.

White light emission in Bi3+/Mn2+ ion co-doped CsPbCl3 perovskite nanocrystals.

Colloidal perovskite nanocrystals (NCs), especially the fully inorganic cesium lead halide (CsPbX3, X = Cl, Br, I) NCs, have been considered as promising candidates for lighting and display applications due to their narrow band emission, tunable band gap and high photoluminescence quantum yields (QYs). However, owing to the anion exchange in the CsPbX3 NCs, stable multi-color and white light emissions are difficult to achieve, thus limiting their practical optoelectronic applications. In this work, dual ion Bi3+/Mn2+ codoped CsPbCl3 perovskite NCs were prepared through the hot injection method for the first time to the best of our knowledge. Through simply adjusting the doping ion concentrations, the codoped NCs exhibited tunable emissions spanning the wide range of correlated color temperature (CCT) from 19 000 K to 4250 K under UV excitation. This interesting spectroscopic behaviour benefits from efficient energy transfer from the perovskite NC host to the intrinsic energy levels of Bi3+ or Mn2+ doping ions. Finally, taking advantage of the cooperation between the excitonic transition of the CsPbCl3 perovskite NC host and the intrinsic emissions from Bi3+ and Mn2+ ions, white light emission with the Commission Internationale de l'Eclairage (CIE) color coordinates of (0.33, 0.29) was developed in the codoped CsPbCl3 NCs.

Doping Lanthanide into Perovskite Nanocrystals: Highly Improved and Expanded Optical Properties.

Cesium lead halide (CsPbX3) perovskite nanocrystals (NCs) have demonstrated extremely excellent optical properties and great application potentials in various optoelectronic devices. However, because of the anion exchange, it is difficult to achieve white-light and multicolor emission for practical applications. Herein, we present the successful doping of various lanthanide ions (Ce3+, Sm3+, Eu3+, Tb3+, Dy3+, Er3+, and Yb3+) into the lattices of CsPbCl3 perovskite NCs through a modified hot-injection method. For the lanthanide ions doped perovskite NCs, high photoluminescence quantum yield (QY) and stable and widely tunable multicolor emissions spanning from visible to near-infrared (NIR) regions are successfully obtained. This work indicates that the doped perovskite NCs will inherit most of the unique optical properties of lanthanide ions and deliver them to the perovskite NC host, thus endowing the family of perovskite materials with excellent optical, electric, or magnetic properties.

Dual-mode humidity detection using a lanthanide-based metal-organic framework: towards multifunctional humidity sensors.

Combined photoluminescence and impedance spectroscopy studies show that a europium-based metal-organic framework behaves as a highly effective and reliable humidity sensor, enabling dual-mode humidity detection.

Preparation and application of carbon-nanodot@NaCl composite phosphors with strong green emission.

Luminescent carbon nanodots (CDots) have attracted much attention, but their luminescence is usually quenched in solid state. Efficient green or yellow emissive CDot-based phosphors are scarce. In this work, green emissive CDot@NaCl composite phosphors were fabricated through a convenient, low cost and eco-friendly way by embedding green emissive CDots (g-CDot) in NaCl crystals. With the protection of NaCl host, the g-CDot@NaCl composite phosphors exhibit good photostability, significant resistance to organic solvents, and improved photoluminescence quantum yields up to 25%. White light-emitting diodes with tunable color temperatures (3944-5478K) and CIE coordinates have been realized based on the g-CDot@NaCl composite phosphors.

Electrostatic Assembly Guided Synthesis of Highly Luminescent Carbon-Nanodots@BaSO4 Hybrid Phosphors with Improved Stability.

Carbon nanodots (CNDs)@BaSO4 hybrid phosphors are fabricated in an easy and low-cost process by sequentially assembling Ba2+ and SO42- ions onto the surface of carbon nanodots through electrostatic attraction. CNDs act as the nucleus to attract these reactive ions and provide the luminescent centers in the hybrid phosphors. This strategy is versatile for a variety of negatively charged CNDs with different emission colors. The advantage of the resultant hybrid phosphors is that their luminescence exhibits excellent thermal and photostability, as well as remarkable resistance to strong acid/alkali and common organic solvents. These merits allow for the fabrication of CNDs-based light-emitting diodes using the CNDs@BaSO4 hybrid phosphors as a color conversion layer.