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result(s) for
"Sui, Laizhi"
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Engineering triangular carbon quantum dots with unprecedented narrow bandwidth emission for multicolored LEDs
2018
Carbon quantum dots (CQDs) have emerged as promising materials for optoelectronic applications on account of carbon’s intrinsic merits of high stability, low cost, and environment-friendliness. However, the CQDs usually give broad emission with full width at half maximum exceeding 80 nm, which fundamentally limit their display applications. Here we demonstrate multicolored narrow bandwidth emission (full width at half maximum of 30 nm) from triangular CQDs with a quantum yield up to 54–72%. Detailed structural and optical characterizations together with theoretical calculations reveal that the molecular purity and crystalline perfection of the triangular CQDs are key to the high color-purity. Moreover, multicolored light-emitting diodes based on these CQDs display good stability, high color-purity, and high-performance with maximum luminance of 1882–4762 cd m
−2
and current efficiency of 1.22–5.11 cd A
−1
. This work will set the stage for developing next-generation high-performance CQDs-based light-emitting diodes.
Carbon quantum dots have promising advantages such as high stability, low cost and environment-friendliness, but their broad emission band limits their application in displays. Here Yuan et al. synthesize these dots showing tunable emission color, high fluorescence and a narrow FWHM of only 30 nanometers.
Journal Article
Rational Design of Multi‐Color‐Emissive Carbon Dots in a Single Reaction System by Hydrothermal
2021
As an emerging building unit, carbon dots (CDs) have been igniting the revolutionaries in the fields of optoelectronics, biomedicine, and bioimaging. However, the difficulty of synthesizing CDs in aqueous solution with full‐spectrum emission severely hinders further investigation of their emission mechanism and their extensive applications in white light emitting diodes (LEDs). Here, the full‐color‐emission CDs with a unique structure consisting of sp3‐hybridized carbon cores with small domains of partially sp2‐hybridized carbon atoms are reported. First‐principle calculations are initially used to predict that the transformation from sp3 to sp2 hybridization redshifts the emission of CDs. Guided by the theoretical predictions, a simple, convenient, and controllable route to hydrothermally prepare CDs in a single reaction system is developed. The prepared CDs have full‐spectrum emission with an unprecedented two‐photon emission across the whole visible color range. These full‐color‐emission CDs can be further nurtured by slight modifications of the reaction conditions (e.g., temperature, pH) to generate the emission color from blue to red. Finally a flexible LEDs with full‐color emission by using epoxy CDs films is developed, indicating that the strategy affords an industry translational potential over traditional fluorophores. A novel multi‐color‐emissive carbon dots (CDs) with two‐photon fluorescence are developed in aqueous solution for the first time by slight modifications of the reaction conditions. Theoretical calculations combined with experiments show that the photoluminescence mechanism of the multi‐color‐emissive CDs is the size change and the conversion of sp3 to sp2 hybridization.
Journal Article
Electron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots
2022
Due to the complex core–shell structure and variety of surface functional groups, the photoluminescence (PL) mechanism of carbon dots (CDs) remain unclear. o-Phenylenediamine (oPD), as one of the most common precursors for preparing red emissive CDs, has been extensively studied. Interestingly, most of the red emission CDs based on oPD have similar PL emission characteristics. Herein, we prepared six different oPD-based CDs and found that they had almost the same PL emission and absorption spectra after purification. Structural and spectral characterization indicated that they had similar carbon core structures but different surface polymer shells. Furthermore, single-molecule PL spectroscopy confirmed that the multi-modal emission of those CDs originated from the transitions of different vibrational energy levels of the same PL center in the carbon core. In addition, the phenomenon of “spectral splitting” of single-particle CDs was observed at low temperature, which confirmed these oPD-based CDs were unique materials with properties of both organic molecules and quantum dots. Finally, theoretical calculations revealed their potential polymerization mode and carbon core structure. Moreover, we proposed the PL mechanism of red-emitting CDs based on oPD precursors; that is, the carbon core regulates the PL emission, and the polymer shell regulates the PL intensity. Our work resolves the controversy on the PL mechanism of oPD-based red CDs. These findings provide a general guide for the mechanism exploration and structural analysis of other types of CDs.
Journal Article
White Photoluminescent Ti 3 C 2 MXene Quantum Dots with Two‐Photon Fluorescence
2019
A recently created class of inorganic 2D materials, MXenes, has become a subject of intensive research. Reducing their dimensionality from 2D to 0D quantum dots (QDs) could result in extremely useful properties and functions. However, this type of research is scarce, and the reported Ti 3 C 2 MXene QDs (MQDs) have only shown blue fluorescence emission. This work demonstrates a facile, high‐output method for preparing bright white emitting Ti 3 C 2 MQDs. The resulting product is two layers thick with a lateral dimension of 13.1 nm. Importantly, the as prepared Ti 3 C 2 MQDs present strong two‐photon white fluorescence. Their fluorescence under high pressure is also investigated and it is found that the white emission is very stable and the pressure makes it possible to change from cool white emission to warm white emission. Hybrid nanocomposites are then fabricated by polymerizing Ti 3 C 2 MQDs in polydimethylsiloxane (PDMS) solution, and the bright white emitting hybrid materials in white light‐emitting diodes are used. This work provides a facile and general approach to modulate various nanoscale MXene materials, and could further aid the wide development of applications for MXene materials in various optical‐related fields.
Journal Article
Multiphoton excited singlet/triplet mixed self-trapped exciton emission
2023
Multiphoton excited luminescence is of paramount importance in the field of optical detection and biological photonics. Self-trapped exciton (STE) emission with self-absorption-free advantages provide a choice for multiphoton excited luminescence. Herein, multiphoton excited singlet/triplet mixed STE emission with a large full width at half-maximum (617 meV) and Stokes shift (1.29 eV) has been demonstrated in single-crystalline ZnO nanocrystals. Temperature dependent steady state, transient state and time-resolved electron spin resonance spectra demonstrate a mixture of singlet (63%) and triplet (37%) mixed STE emission, which contributes to a high photoluminescence quantum yield (60.5%). First-principles calculations suggest 48.34 meV energy per exciton stored by phonons in the distorted lattice of excited states, and 58 meV singlet-triplet splitting energy for the nanocrystals being consistent with the experimental measurements. The model clarifies long and controversial debates on ZnO emission in visible region, and the multiphoton excited singlet/triplet mixed STE emission is also observed.
Here the author study Self-trapped exciton emission for multiphoton excited luminescence in ZnO nanoparticle which until now have not been explored. They provide a reason for the emission enhancement and apply these materials in optical imaging for a proof of concept.
Journal Article
Graphitic Nitrogen and High‐Crystalline Triggered Strong Photoluminescence and Room‐Temperature Ferromagnetism in Carbonized Polymer Dots
by
Wu, Min
,
Zhu, Shoujun
,
Yong, Xue
in
Atoms & subatomic particles
,
Carbon
,
carbonized polymer dots
2019
Carbonized polymer dots (CPDs) have great potential for bioimaging and biosensing owing to their low toxicity, low cost, resistance to photobleaching, and low environmental impact. Here, the hydrothermal condensation of biomolecules (l‐serine and l‐tryptophan) is used to vary the CPDs' inner structure from amorphous to lattice. A new type of carbon lattice CPD is thus demonstrated that is bright (the photoluminescence quantum yield (PLQY) is as high as 89.57%) and shows room‐temperature ferromagnetism (RTFM), with the magnetic moment increasing from 0.0025 emu g−1 in crosslinked polymer clusters to 0.021 emu g−1 in the latticed sample. Hydrothermal synthesis at 300 °C leads to a distinct type of CPD with an obvious carbon lattice, which shows the highest PLQY and the greatest ferromagnetism. Then, the origin of the RTFM is examined in the CPDs via first‐principles calculation, revealing that graphitic nitrogen triggers RTFM in CPDs. Moreover, a possible growth mechanism is suggested that includes kinetics as an important factor in the formation of the CPD crystallites. Overall, these findings identify graphitic nitrogen and high crystallinity as crucial to the enhancement of the CPDs' photoluminescence and room‐temperature ferromagnetism which suggests that they deserve more research attention to develop practical applications. A new type of carbon lattice carbonized polymer dots (CPD) is demonstrated that is bright, with a photoluminescence quantum yield as high as 89.57%. It also shows room temperature ferromagnetism (RTFM), with the magnetic moment increasing from 0.0025 emu g−1 in crosslinked polymer clusters to 0.021 emu g−1 in the lattice sample.
Journal Article
Brightening self-trapped exciton emission in 2D metal-organic chalcogenolates via argentophilicity-mediated anisotropic compression
2025
An emerging class of two-dimensional semiconductor materials, metal-organic chalcogenolates (MOCs), have garnered significant attention due to the strong excitonic effects arising from their intrinsic soft, hybrid multiquantum-well structures. However, modifying excitonic transitions that strongly couple to the argentophilic networks and constructing their structure-property relationships in MOCs remain daunting challenges. Here, we use silver phenylselenolate (AgSePh) as a model system to manipulate excitonic behavior and uncover the fundamental photophysical mechanisms through pressure engineering. A bright broadband Stokes-shifted emission is observed in AgSePh crystals along with the disappearance of blue narrow emission upon compression, which is attributed to the pressure-induced carrier transformation from free exciton to self-trapping exciton states. The considerable compressibility of the Ag-Se inorganic monolayer, driven by weakly bound argentophilic interactions, generates pronounced argentophilic intralayer distortion while simultaneously enhancing exciton-phonon coupling and excitonic oscillator strength. This work demonstrates the remarkable tunability of excitonic properties in layered MOCs.
Pressure brightens the self-trapped exciton emission in 2D semiconducting metalorganic chalcogenolates by manipulating exciton-phonon coupling and argentophilicity-driven lattice distortion.
Journal Article
White Photoluminescent Ti3C2 MXene Quantum Dots with Two‐Photon Fluorescence
2019
A recently created class of inorganic 2D materials, MXenes, has become a subject of intensive research. Reducing their dimensionality from 2D to 0D quantum dots (QDs) could result in extremely useful properties and functions. However, this type of research is scarce, and the reported Ti3C2 MXene QDs (MQDs) have only shown blue fluorescence emission. This work demonstrates a facile, high‐output method for preparing bright white emitting Ti3C2 MQDs. The resulting product is two layers thick with a lateral dimension of 13.1 nm. Importantly, the as prepared Ti3C2 MQDs present strong two‐photon white fluorescence. Their fluorescence under high pressure is also investigated and it is found that the white emission is very stable and the pressure makes it possible to change from cool white emission to warm white emission. Hybrid nanocomposites are then fabricated by polymerizing Ti3C2 MQDs in polydimethylsiloxane (PDMS) solution, and the bright white emitting hybrid materials in white light‐emitting diodes are used. This work provides a facile and general approach to modulate various nanoscale MXene materials, and could further aid the wide development of applications for MXene materials in various optical‐related fields. A facile, high‐output method for the fabrication of Ti3C2 MXene quantum dots (MQDs) with direct white photoluminescence and two‐photon fluorescence is unprecedentedly designed. High‐pressure studies of Ti3C2 MQDs are also performed, demonstrating a stable white emission that changes from cool white emission to warm white emission. The work paves a general way to achieve nanoscale MXene materials with enhanced applications in various optical‐related fields.
Journal Article
Deviatoric stress-induced transition of self-trapped exciton emissions
by
Yang, Dongwen
,
Liu, Hang
,
Qin, Jinxu
in
639/624/1107/527/1819
,
639/925/930/527/1819
,
Clean energy
2025
Self-trapped exciton (STE) emissions, featured by broad spectral band and minimal self-absorption, have garnered considerable attention for advanced lighting and imaging applications. However, developing strategies to facilitate multiple STE states, modulate the emission energy and extend the emission range remains a great challenge. Here, we introduce deviatoric stress to induce another intrinsic STE state (STE-2) and enable transitions between the intrinsic STE state (STE-1) and STE-2 in pyramidal ZnO nanocrystals. This approach results in a remarkable shift in emission energy, from yellow-green (2.34 eV) to deep-blue (2.88 eV). Combined in-situ stress monitoring and optical experiments show that the STE-2 state originates from a potential well generated by the deviatoric yield deformation of the pyramidal crystals under deviatoric stress. Spectroscopic and dynamical characterizations of the two STE emissions reveal a transition process in the carrier’s relaxation pathway from STE-2 to STE-1, and conversely at much higher pressures. These findings demonstrate that deviatoric stress serves as a robust tool for modulating STE emissions and provide new insights into the evolution of carrier dynamics of STE emissions.
Deviatoric stress induces an intrinsic self-trapped exciton state (STE-2) and enables transitions between two intrinsic STE states in pyramidal ZnO nanocrystals. This approach results in a remarkable shift in emission energy, from 2.34 eV to 2.88 eV.
Journal Article
Highly Efficient Photosensitizers with Molecular Vibrational Torsion for Cancer Photodynamic Therapy
2023
The development of highly effective photosensitizers (PSs) for photodynamic therapy remains a great challenge at present. Most PSs rely on the heavy-atom effect or the spin–orbit charge-transfer intersystem crossing (SOCT-ISC) effect to promote ISC, which brings about additional cytotoxicity, and the latter is susceptible to the interference of solvent environment. Herein, an immanent universal property named photoinduced molecular vibrational torsion (PVT)-enhanced spin–orbit coupling (PVT-SOC) in PSs has been first revealed. PVT is verified to be a widespread intrinsic property of quinoid cyanine (QCy) dyes that occurs on an extremely short time scale (10–10 s) and can be captured by transient spectra. The PVT property can provide reinforced SOC as the occurrence of ISC predicted by the El Sayed rules (1ππ*–3nπ*), which ensures efficient photosensitization ability for QCy dyes. Hence, QTCy7-Ac exhibited the highest singlet oxygen yield (13-fold higher than that of TCy7) and lossless fluorescence quantum yield (ΦF) under near-infrared (NIR) irradiation. The preeminent photochemical properties accompanied by high biosecurity enable it to effectively perform photoablation in solid tumors. The revelation of this property supplies a new route for constructing high-performance PSs for achieving enhanced cancer phototherapy.
Journal Article