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Aggregation-induced emission nanoparticles serve as promising fluorescence probes for multi-photon excitation microscopy due to the large absorption cross-section in the NIR-IIb region. Here we present organic AIE nanoparticles that feature a high absorption cross-section under three-photon excitation. We show that these enable ultra-deep NIR-IIa excited three-photon imaging in the in vivo mouse brain.

Photoluminescence (PL) of rare earth (RE) ions has been observed in RE ion-doped perovskite nanocrystals (PeNCs); however, the electroluminescence (EL) originating from the RE ions is still not ach...

Recently, various lanthanide ions (Ln3+) have been successfully doped into perovskite quantum dots (PQDs), and the quantum-cutting emission of 2F5/2-2F7/2 for Yb3+with a measurable inner efficiency of more than 100% has been discovered and applied as the luminescent converter of solar cells, which has opened a new branch for the application of PQDs. In this work, to further improve the quantum-cutting efficiency of Yb3+, the codoping and tridoping methods were used to improve the quantum-cutting emission of PQDs. The Yb3+-Ln3+ (Ln = Nd, Dy, Tb, Pr, Ce) pair-doped CsPbClxBryI3-x-y PQDs were fabricated, with all displaying excitonic emission, narrow-band emission of Ln3+ ions, and quantum-cutting emission of Yb3+ ions. It was interesting that Yb3+-Pr3+ as well as Yb3+-Ce3+ pairs could effectively sensitize the emission of Yb3+, owing to Pr3+ and Ce3+ ions offering intermediate energy states close to the exciton transition energy of the PQDs. After host composition optimization and tridoping investigation, overall emissions with a 173% photoluminescence quantum yield (PLQY) were obtained in the Yb3+-Pr3+-Ce3+-tridoped CsPbClBr2 PQDs. Then, the tridoped PQDs were designed as the down-converter for CuIn1-xGaxSe2 (CIGS) as well as the silicon solar cells, which leads to an enhancement of the power conversion efficiency (PCE) of as high as ∼20%. The modified CIGS was further employed to charge the smart mobile phone, which could largely shorten the charging time from 180 to 150 min. This finding is of great significant for expanding the application fields of the impurity-doped PQDs.

Employing lanthanide doped upconversion nanoparticles (UCNPs) as near-infrared absorbing photoactive materials is a feasible conception for constructing high efficient and stable narrowband wavelength-selective photodetectors, but limited by its upconversion luminescence efficiency. Herein, we experimentally and theoretically demonstrate upconversion luminescence (UCL) enhancement in monolayer UCNPs using plasmon semiconductor NPs (CsxWO3) and further explore its narrowband near-infrared photodetection application. The UCL improvement of 144 folds in CsxWO3/NaYF4/NaYF4:Yb3+, Er3+ hybrid was realized with the optimized spacer thickness (15 nm) and monolayer UCL. More than three orders enhancement was obtained via the semiconductor plasmon combined with core-shell UCNPs in both CsxWO3/NaYF4/monolayer-NaYF4:Yb3+, Er3+@NaYF4:Yb3+, Tm3+ and CsxWO3/NaYF4 /monolayer-NaYF4:Yb3+, Tm3+@NaYF4:Yb3+, Er3+. Interestingly, the higher enhancement of core's emissions was recorded in core-shell UCNPs by coupling with CsxWO3 NPs. The excitation field amplification dominates the high UCL enhancement, revealed by the UCL dynamics and the calculated electric field intensity. Finally, the high performance narrow photodetectors for 980 nm is constructed employing MAPbI3/CsxWO3/NaYF4/NaYF4:Yb3+, Er3+@NaYF4:Yb3+, Tm3+ hybrids, with narrow line width of 20 nm, high responsivity of 0.33 A/W, detectivity of 4.5 × 1010 Jones, and short response time of 180 ms, which is much better than the previous photodetectors. This finding provides keen approach for developing high efficient/performance UCNPs and narrowband photodetectors.

Due to the ultrathin structure, functional groups and excellent physical-chemical properties, Two-dimensional (2D) MXenes shows great potential for biomedical applications. Here, we prepared TiO2 inverse opal photonic crystals (IOPCs)/Ti3C2 quantum dots (QDs) composite film through the self-assembly method. Because of the widen absorption band of Ti3C2 QDs, TiO2 IOPCs/Ti3C2 composite film could have photocurrent effect from 280 to 900 nm, and the internal power conversion efficiency could reach to 26% at 350 nm. Owing to favourable energy levels, Ti3C2 QDs were formed the Type-II Heterojunction with TiO2, thus enabling directional transport charge for efficient charge separation. The Type-II Heterojunction photoelectrochemical (PEC) sensor consisting of TiO2/Ti3C2/Nafion electrode exhibited high stability, sensitivity, and selectivity for the detection of glutathione in buffered solution and cell extracts. Thus, the TiO2/Ti3C2/Nafion composite film provides a promising green electrode for sensitive PEC detection, which could realize some potential applications for disease early precaution and diagnose.

Pollution triggered by highly toxic heavy metal ions has become of worldwide critical concern; thus, it is urgent to develop an eco-friendly and nontoxic fluorescence probe for metal ions sensing. ...

This paper considers an affine maneuver tracking control problem for leader-follower type second-order multi-agent systems in the presence of time-varying delays, where the interaction topology is directed. Using the property of the affine transformation, this paper gives the sufficient and necessary conditions of achieving the affine localizability and extends it to the second-order condition. Under the (n + 1)-reachable condition of the given n-dimensional nominal formation with n + 1 leaders, a formation of agents can be reshaped in arbitrary dimension by only controlling these leaders. When the neighboring positions and velocities are available, a formation maneuver tracking control protocol with time-varying delays is constructed with the form of linear systems, where the tracking errors of the followers can be specified. Based on Lyapunov-Krasovskii stability theory, sufficient conditions to realize affine maneuvers are proposed and proved, and the unknown control gain matrix can be solved only by four linear matrix inequalities independent of the number of agents. Finally, corresponding simulations are carried out to verify the theoretical results, which show that these followers can track the time-varying references accurately and continuously.

Summary Advanced optical methods combined with various probes pave the way toward molecular imaging within living cells. However, major challenges are associated with the need to enhance the imaging resolution even further to the subcellular level for the imaging of larger tissues, as well as for in vivo studies. High scattering and absorption of opaque tissues limit the penetration of light into deep tissues and thus the optical imaging depth. Tissue optical clearing technique provides an innovative way to perform deep-tissue imaging. Recently, various optical clearing methods have been developed, which provide tissue clearing based on similar physical principles via different chemical approaches. Here, we introduce the mechanisms of the current clearing methods from fundamental physical and chemical perspectives, including the main physical principle, refractive index matching via various chemical approaches, such as dissociation of collagen, delipidation, decalcification, dehydration, and hyperhydration, to reduce scattering, as well as decolorization to reduce absorption., Graphical abstract, Subject areas: Optical Imaging; Biological Sciences; Research Methodologies; Biological Sciences Tools

The development of novel photosensitizers with aggregation-induced emission (AIE) characteristics has aroused tremendous interest, because it could combine efficient bioimaging with precise photodynamic therapy, which would thus dramatically promote applications in biomedical treatment. Among various AIE luminogens (AIEgens), heterocycle-containing molecules are highly promising for this usage because of their high photostability and tunable electronic properties. In this work, a pyrazine-containing AIEgen with a dicyanopyrazine moiety as an electron acceptor and a triphenylamine unit as an electron donor was chosen for study. The V-shaped donor-π-acceptor-π-donor structure of the AIEgen endowed its nanoparticles with excellent nonlinear optical properties for two-photon cell imaging under near-infrared laser excitation. Also, under the same excitation, the nanoparticles could produce reactive oxygen species and further kill the cells efficiently and accurately. The present work thus presents a pyrazine-containing AIEgen as a new photosensitizer for imaging-guided two-photon photodynamic therapy and gives more opportunities for deep-tissue treatment of cancer in future research.

A ratiometric near-infrared fluorescence probe based on IR-780 is developed and applied to fluoride anion (F-) detection in potable water and white flour as well as fluorescence imaging in living cells and mice. The proposed probe not only displays a linear ratiometric (F740/F690 nm) fluorescence response but also possesses near-infrared wavelengths to F- with a detection limit of 0.2 μM. Moreover, the designed probe displays high selectivity toward F-, which makes it feasible for F- detection in potable water and white flour. More importantly, applied to monitor F- in living HepG2 cells and male BALB/c mice, the probe indicates good biocompatibility and low cytotoxicity. However, no study for F- detection has been reported by a ratiometric NIR fluorescent probe so far. We expect that this probe with superior properties has great potential for use in F- detection in biological systems and in vivo studies.

NaLuF4: Yb3+/Er3+ phosphors are synthesized via a hydrothermal method. The photoluminescence properties of the phosphors are researched at a temperature range from 296 to 461 K under 1064 nm excitation. Fluorescence intensity ratio I/I0 shows a linear relationship with increasing the temperature from 296 to 420 K. The maximum sensitivity is obtained to be 0.0194 K-1 using non-contact ratiometric thermometer through multi-phonon assisted excitation.

We propose a broadband and high-efficiency four-wave-mixing wavelength converter based on parallel-cascaded micro-ring resonators (PCMRRs). By optimizing the distance between the mutually uncoupled ring resonators, we demonstrate that the PCMRR has a transmission spectrum with interleaved narrow and broad passbands. Broadband and high-efficiency wavelength conversion can be achieved by placing the pump and the signal in the narrow and broad passbands, respectively. We experimentally demonstrate a 25-GHz bandwidth wavelength converter based on optimally designed 3-ring PCMRR. Compared with the conventional single-ring-resonator-based wavelength converter with the same bandwidth, there is a 15-dB enhancement of conversion efficiency for the 3-ring PCMRR when the input pump power is 10 dBm.

Aggregation-induced emission luminogens (AIEgens) are fluorescent agents that are ideal for bioimaging and have been widely used for organelle targeting, cellular mapping, and tracing. Owing to their promising characteristics, AIEgen-based nanoparticles have recently been used for the stimulated emission depletion (STED) super-resolution imaging of fixed cells. In the present study, and for the first time, we used an AIEgen for dynamic STED nanoscopic imaging of a specific organelle in live cancer cells. TPA-T-CyP is a synthetic red&NIR-emitting luminogen with AIE features that can spontaneously and specifically aggregate on mitochondria without the need for encapsulation or surface modification. The STED efficiency of aggregated TPA-T-CyP can reach more than 80%, and super-resolution imaging of TPA-T-CyP-stained mitochondria in live HeLa cells is possible, with a lateral spatial resolution of 74 nm. We found that TPA-T-CyP enabled the dynamic visualization of mitochondria, and the motion, fusion, and fission of mitochondria were clearly observable on a super-resolution scale. AIEgen-based super-resolution organelle visualization has great potential for many basic biomedical studies.

The influence of nanocrystalline CoNiFeAl0.4Ti0.6Cr0.5 high-entropy alloy (HEA) particles addition on the microstructure and mechanical properties of SiCp/7075Al composites was investigated systematically. The CoNiFeAl0.4Ti0.6Cr0.5 high-entropy alloy was prepared by mechanical alloying, and the (5 vol% HEAp + 40 vol% SiCp)/7075Al (HEA-7075Al) and 45 vol% SiCp/7075Al (SiC-7075Al) composites were subsequently fabricated by squeeze casting. The HEA particles were well retained in the Al matrix and remained nanocrystalline following the squeeze casting and heat treatment process, which indicated that the CoNiFeAl0.4Ti0.6Cr0.5 high-entropy alloy has the advantage of sluggish diffusion behavior and thermal stability. The time for the HEA-7075Al composite reaching the aged-peak period (19.5 h) was slightly longer than that of the SiC-7075Al composite (15 h), indicating that the HEA particles addition has postponed the aging process, which can be ascribed to the decrease of dislocation density in the Al matrix, evaluated from XRD. Additionally, in contrast to the SiC-7075Al composite, the HEA-7075Al composite exhibits higher strength, better plasticity and higher modulus with the average values of 712 MPa, 0.82% and 171 GPa, respectively, which is the results of the good interface between HEA particles and Al matrix, high strength nanocrystalline HEA particles and proper dislocation density present in Al matrix.

Monoclinic phase Gd2(MoO4)3: Yb3+/Er3+ phosphor is synthesized via a simple sol-gel method. The XRD result reveals that the phosphor possesses monoclinic structure with space group C2/c(15). Under the excitation of a 980 nm laser, its emission spectra shows remarkably intense green and negligible red emissions, which are all two-photon process. By investigating effect of temperature on green emission of the sample, the competition between the thermal agitation and non-radiative relaxation of 2H11/2 level can be found, which is verified by the measurement of lifetime. In addition, the sensitivity of optical thermometry is studied based on the fluorescence intensity ratio technique through infrared excited green upconversion. The maximum sensitivity is found to be about 0.02574 K−1 at 510.2 K, suggesting that the phosphor can be used as an excellent material for optical temperature sensing.

CsPbX3 (X = Cl, Br or I) perovskite quantum dots (PQDs) have attracted tremendous attention due to their extraordinarily excellent optical properties. However, there is still an obstacle for their bio-application, which is limited by their water-instability. In this work, we have designed a novel visible light triggered photoelectrochemical (PEC) sensor for dopamine (DA) based on CsPbBr1.5I1.5 PQD immobilized three-dimensional (3D) TiO2 inverse opal photonic crystals (IOPCs). Supported by the TiO2 IOPCs, the water-stability of the PQDs as well as that of the PEC sensor was considerably improved. Furthermore, employed as a photoactive material in PEC sensor, CsPbBr1.5I1.5 PQDs can expand the photocurrent response of the PEC sensor to the whole visible region. In addition, the modulation of the photonic stop band effect of TiO2 IOPCs on the incident light and the emission of PQDs could further enhance the photocurrent response. Such a PEC sensor demonstrates sensitive detection of DA in phosphate buffer saline solution and serum, with a good linear range from 0.1 μM to 250 μM and a low detection limit of approximately 0.012 μM. Our strategy opens an alternative horizon for PQD based PEC sensing, which could be more sensitive, convenient and inexpensive for clinical and biological analysis.

Luminescence concentration quenching, mainly due to a cross relaxation (CR) process between lanthanide ions (Ln3+), widely occurs in Ln3+ doped luminescent materials, setting a limit in the dopant content of Ln3+ emitters to withhold the brightness. Here, we introduced Na+ ions into the CaF2 host lattice codoped with Nd3+ emitters that alleviates concentration quenching greatly. And we show that the optimal dopant concentration of Nd3+ in colloidal CaF2:Nd nanoparticles increased from 10 to 30 mol%, resulting in an ∼32 times near-infrared (NIR) (1052 nm) brightness under 800 nm laser irradiation. Our mechanistic investigation suggests that the enhancement of NIR photo-luminescence (PL) could be attributed to not only the increasing crystallinity of nanoparticles but also the reducing concentration quenching of Nd3+ by improving the dopant distribution of Nd3+ ions in the CaF2 lattice, as evidenced by the high angle annular dark field images. These result in the optimal concentration increase to produce brightness enhancement greatly. This strategy can be utilized for other Ln3+ doped CaF2 based nanomaterials for bio-imaging.

Fluorescent carbon dots (FCDs) have attracted tremendous attention in biological applications. The short-wave infrared (SWIR, 900–1700 nm) spectral range is considered as a novel optical tissue window due to low photon scattering. In this work, we investigated the fluorescence characteristics of FCDs based on the SWIR spectral range. SWIR emissions were observed from FCDs for the first time, when long-wavelength excitation (e.g. longer than 731 nm) was adopted. Wavelength-tunable two-photon fluorescence could also be obtained from the FCDs, under 1000–1560 nm SWIR femtosecond (fs) excitation. Interestingly, when an fs excitation wavelength as long as 1560 nm was adopted, two typical nonlinear optical signals, namely two-photon fluorescence and third harmonic generation (THG), could be observed. Based on the one-photon SWIR fluorescence, FCDs were successfully utilized for in vivo sentinel node mapping and tumour imaging. Under SWIR fs excitation, FCD-assisted two-photon fluorescence microscopy realized deep-tissue imaging of zebrafish embryos and the brain neuron networks of mice. SWIR excited and emitting FCDs have potential as fluorescent probes for deep-tissue and high-contrast functional bioimaging and related applications in the future.

Herein, we propose a monolithic reflector-integrated waveguide photodetector with optical isolation between photosensitive mesa and N-contact mesa for achieving a high efficiency bandwidth product. In the proposed photodetector, the photosensitive mesa is optically isolated but electrically connected with the N-contact mesa; this is achieved by etching a portion of the core layer to form a groove on each side of the photosensitive mesa, enhancing the binding of the waveguide to optical power. Furthermore, a mesa is formed separate from the N-contact mesa at the end of the waveguide, and the metal film is deposited to act as a mirror, thereby increasing the effective absorption length of the device. Consequently, the mutual tradeoff between the bandwidth and quantum efficiency of the photodetector could be alleviated.

The ability to modulate the intensity of electromagnetic field by semiconductor plasmon nanoparticles is becoming attractive due to its unique doping-induced local surface plasmon resonance (LSPR) effect that is different from metals. Herein, we synthesized mCu2–xS@SiO2@Y2O3:Yb3+/Er3+ core–shell composites and experimentally and theoretically studied the semiconductor plasmon induced up-conversion enhancement and obtained 30-fold up-conversion enhancement compared with that of SiO2@Y2O3:Yb3+/Er3+ composites. The up-conversion enhancement was induced by the synthetic effect: the amplification of the excitation field and the increase of resonance energy transfer (ET) rate from Yb3+ ions to Er3+ ions. The experimental results were analyzed in the light of finite-difference time-domain (FDTD) calculations, confirming the effect of the amplification of the excitation field. In addition, up-conversion luminescence (UCL) spectra, up-conversion enhancement, and dynamics dependent on concentration (Yb3+ and Er3+ i...

Although lanthanide doped luminescent materials have been extensively investigated, a quantitative analysis of how temperature affects upconversion luminescence is still incomplete. The Gd2(MoO4)3:Er3+/Yb3+ phosphor is synthetized by sol-gel method. Based on the absorption spectra of Er3+ ions, J-O intensity parameters and radiative transition probabilities are computed to estimate the optical properties. In view of ion-phonon interaction, the phonon-assisted energy transfer and multiphonon relaxation are responsible for the temperature dependent luminescence. Additionally, cross relaxation probability for 4I11/2+4I11/2→4I15/2+4F7/2 is determined to be 240 s−1 through quantitative simulation of ion-ion interaction. These meaningful results are of vital values for the field of laser crystal and optical temperature sensing.

We developed a wideband transverse magnetic (TM) −reflected polarizer composed of BK7 prism and Ag/Cr/TiO2 film. Based on the polarization-dependent loss of coupled plasmon-waveguide resonance (CPWR), BK7 prism/Ag/Cr/TiO2/air layered structure can reflect the TM-components of lightwave and severely attenuate the transverse electric (TE) −components in a wavelength range from 600 nm to 900 nm at incident angles greater than the critical angle of total reflection. In terms of its practical application, a compact, low cost surface plasmon resonance (SPR) configuration with an integrated polarizer for wavelength modulation is presented and experimentally demonstrated.

The authors describe a new phosphor of the composition Gd2(WO4)3:0.3%Ho/0.5%Tm/15%Yb that displays distinctly improved sensitivity to temperature (T) due to non-thermally coupled energy levels of Ho(III) and Tm(III) ions. Under 980 nm excitation, the upconverted blue (peaking at 473 nm), green (540 nm) and red (655 and 700 nm) fluorescences exhibit T-dependent luminescence in the 295 to 595 K range. The T sensing capability was investigated by using a ratiometric (2-wavelength) technique. The maximum sensitivity to T is found to be 26.14 × 10−3 K−1 at 595 K based on the red [Tm(III)] and green [Ho(III)] emissions. The colors of the phosphor are located in the white region of the CIE diagram in the whole T-range which also makes it suitable for use in white displays.

Photon upconversion (UC) is an attractive strategy to substantially enhance the power conversion efficiency (PCE) of solar cells via upconverting unavailable near-infrared sunlight to available visible light. However, to date, it is almost infeasible to achieve effective PCE improvement of solar cells with the assistance of UC materials, limited by their poor UC efficiency and extremely weak and narrowband near-infrared absorption. Here, we demonstrate the efficient photon energy UC in semiconductor plasmon mCu2−xS@SiO2@Er2O3 (mCSE) nanocomposites, where the broadband semiconductor plasmon (800–1600 nm) of mCu2−xS serves as an antenna to sensitize UC of Er2O3 nanoparticles. The overall upconversion luminescence (UCL) of the composites was dramatically enhanced by a factor of ∼1000, with a maximal inner quantum efficiency of 14.3%. The excitation range was expanded, ranging from 800 to 1600 nm. As a proof-of-concept, the highly efficient mCSE nanocomposites were utilized to improve the PCE of perovskite solar cells (PSCs). The expansion of the near-infrared response (800–1000 nm) and considerable improvement of the PCE were obtained, with an optimum PCE of 17.8%. The mCSE composites in PSCs enhanced the photocurrent via electron transfer from oxygen defects to the conduction band of TiO2 under irradiation of one sunlight. Under irradiation of 15 suns, the electron transfer and reabsorption of UCL both contributed to the enhancement of PCE. Our work can provide an insightful thought on boosting UC efficiency as well as broadening the PCE of PSCs.

In this paper, we have synthesized erbium and ytterbium codoped sodium gadolinium fluoride (NaGdF4:Yb/Er) nanophosphors (NPs), aiming to extend the solar light harvest of PTB7 from visible into near-infrared. Evidence shows that Yb concentration plays an important role in upconversion, because it can inhibit the back energy transfer process and absorb considerable low-energy photons. Subsequently, NaGdF4:Yb/Er NPs have been incorporated into the photocatalytic titania (TiO $_2$ ) nanoparticle layer to probe into electron transfer dynamics, and the photovoltaic performance of the assembled solar cells has been explored. The results show that NaGdF4:Yb/Er NPs excited at 976 nm present green and red emissions. After interfacing with bare or NP-doped electron donor TiO $_2$ , the lifetime of the emerged electron transfer has been shortened from 840 to 466 ps, and correspondingly, the electron transfer rate outstrips that of the bare TiO $_2$ by a factor of 2.6. Consequently, an efficiency enhancement has been obtained with power conversion efficiency increasing to 3.61% from 2.81% of pure TiO $_2$ /PTB7. This work provides an efficient and facile approach to enhance the device performance by the codoping of robust rare-earth ions to widen the harvesting range of solar spectrum, boost electron transfer rate, and eventually strengthen the device performance.

A series of LiLa 9− x (SiO 4 ) 6 O 2 : x Ce 3+ phosphors were prepared by a conventional high temperature solid state reaction method, and their spectroscopic characteristic were systematically investigated. Two types of Ce 3+ -emitting centers with emission at about 380 and 430 nm can be found in the phosphors LiLa 9 (SiO 4 ) 6 O 2 :Ce 3+ . The Stokes shift and crystal field depression of Ce(1) and Ce(2) are investigated. The decay characteristics of Ce(1) and Ce(2) are discussed.

Two-photon excited fluorescence microscopy and nanoparticle-assisted photodynamic therapy (PDT) are two important areas in biomedical research, and their combination can be more beneficial. A type of red emissive photosensitizer (PS) with aggregation-induced emission (AIE) features, which is called tetraphenylethylene (TPE-red), was synthesized and further encapsulated with poly(styrene-co-maleic anhydride) (PSMA) to form nanoparticles. Two-photon fluorescence, as well as two-photon excited reactive oxygen species (ROS) generation by TPE-red–PSMA nanoparticles, was characterized. A large two-photon absorption cross-section was observed at 1040 nm with a femtosecond (fs) laser. PDT via two-photon excitation was well realized on tumor cells, using TPE-red–PSMA nanoparticles as PSs under 1040 nm fs laser excitation. Based on our study, we believe that two-photon excited PDT with AIE-active PSs has great potential applications in deep tissue imaging-guided therapy.

Compared with visible light, near-infrared (NIR) light has deeper penetration in biological tissues. Three-photon fluorescence microscopy (3PFM) can effectively utilize the NIR excitation to obtain high-contrast images in the deep tissue. However, the weak three-photon fluorescence signals may be not well presented in the traditional fluorescence intensity imaging mode. Fluorescence lifetime of certain probes is insensitive to the intensity of the excitation laser. Moreover, fluorescence lifetime imaging microscopy (FLIM) can detect weak signals by utilizing time-correlated single photon counting (TCSPC) technique. Thus, it would be an improved strategy to combine the 3PFM imaging with the FLIM together. Herein, DCDPP-2TPA, a novel aggregation-induced emission luminogen (AIEgen), was adopted as the fluorescent probes. The three-photon absorption cross-section of the AIEgen, which has a deep-red fluorescence emission, was proved to be large. DCDPP-2TPA nanoparticles were synthesized, and the three-photon fluorescence lifetime of which was measured in water. Moreover, in vivo three-photon fluorescence lifetime microscopic imaging of a craniotomy mouse was conducted via a home-made optical system. High contrast cerebrovascular images of different vertical depths were obtained and the maximum depth was about 600 [Formula: see text]m. Even reaching the depth of 600 [Formula: see text]m, tiny capillary vessels as small as 1.9 [Formula: see text]m could still be distinguished. The three-photon fluorescence lifetimes of the capillaries in some representative images were in accord with that of DCDPP-2TPA nanoparticles in water. A vivid 3D reconstruction was further organized to present a wealth of lifetime information. In the future, the combination strategy of 3PFM and FLIM could be further applied in the brain functional imaging.

Nonlinear optical microscopy has become a powerful tool in bioimaging research due to its unique capabilities of deep optical sectioning, high-spatial-resolution imaging, and 3D reconstruction of biological specimens. Developing organic fluorescent probes with strong nonlinear optical effects, in particular third-harmonic generation (THG), is promising for exploiting nonlinear microscopic imaging for biomedical applications. Herein, a simple method for preparing organic nanocrystals based on an aggregation-induced emission (AIE) luminogen (DCCN) with bright near-infrared emission is successfully demonstrated. Aggregation-induced nonlinear optical effects, including two-photon fluorescence (2PF), three-photon fluorescence (3PF), and THG, of DCCN are observed in nanoparticles, especially for crystalline nanoparticles. The nanocrystals of DCCN are successfully applied for 2PF microscopy at 1040 nm NIR-II excitation and THG microscopy at 1560 nm NIR-II excitation, respectively, to reconstruct the 3D vasculature of the mouse cerebral vasculature. Impressively, the THG microscopy provides much higher spatial resolution and brightness than the 2PF microscopy and can visualize small vessels with diameters of ≈2.7 µm at the deepest depth of 800 µm in a mouse brain. Thus, this is expected to inspire new insights into the development of advanced AIE materials with multiple nonlinearity, in particular THG, for multimodal nonlinear optical microscopy.

Using fluorescent probes to detect endogenous hydrogen peroxide, which is associated with many diseases in the human body, remains an essential technique. Cyanine fluorochromes are a class of dyes that have attracted much attention and are widely used in the synthesis of fluorescent probes. In this article, a novel near-infrared (NIR) fluorescence probe for the detection of hydrogen peroxide was constructed and successfully applied to imaging endogenous hydrogen peroxide in vivo. Notably, probe 1 was designed by connecting 4-(bromomethyl)benzeneboronic acid pinacol ester as the sensing unit to the IR-780 hemicyanine skeleton, which exhibits excellent properties like NIR fluorescence emission over 700 nm. Probe 1 has satisfactory sensitivity to hydrogen peroxide with a low detection limit of 0.14 μM (S/N = 3), attributed to a responding mechanism that leads to the oxidation of phenylboronic acid pinacol ester and thereby releases fluorophore 2. Moreover, probe 1 displays excellent selectivity towards hydrogen peroxide over other substances. Taking advantage of these properties, the probe proved to be cell-permeable. Based on the results of N-acetylcysteine and rotenone together, probe 1 is capable of clearly visualizing endogenously produced hydrogen peroxide in living HepG2 cells and mice. The superior performance of the probe, as a reliable chemical tool, makes it of great potential application for exploring the role played by hydrogen peroxide in biological systems.

Quantum dots (QDs) have become promising light sources for next-generation lightings and displays. Realizing their applications in optoelectronic devices requires that QDs should retain their superior optical performances in condense QD films. However, most QD systems suffer intense photoluminescence (PL) quenching after film formation. Here, we report device-grade thick-shell CdZnSe/ZnSe/ZnS QDs with near-unity PL quantum yield (QY) in QD solution and 82% PL QY in QD film. We demonstrate that the thick shell functions well in restraining undesired inter-dot energy transfer by separating the emitting cores in condense QD film, and therefore preserving their superior emission properties. White light-emitting diodes (WLEDs) integrated with 5 different CdZnSe/ZnSe/ZnS QDs cover the visible spectrum, delivering a color rendering index (CRI) Ra as high as 91.4, a luminous efficiency (LE) of 68.5 lm/W and a warm bright sun light with correlated color temperature (CCT) of 4138 K. In particular, the champion CdZnSe/ZnSe/ZnS based WLED exhibits a special color index R9 as high as 93.1.

Aromatic polyamide fiber becomes the most important material for ballistic protection purposes because of the high modulus and strength from the 1960s. To obtain an insightful understanding of the mechanical deformation of Kevlar, a detailed multiscale model is developed in this paper based on the structures of Kevlar from molecular scale to macroscopic scale. By analyzing the molecular structures of Kevlar, the high modulus of Kevlar fibers can be attributed to the high stiffness of aromatic polyamide chains and the massively distributed hydrogen bonds in the material. The damage initiation and evolution in Kevlar fiber can be captured at the microfibril scale. It can be found that the material strength in the grain boundary regions is only 1.9 GPa, resulting in much lower strength of the whole Kevlar fiber (2.5–3.3 GPa), compared to the theoretical strength of the aromatic polyamide crystals (>30 GPa). The structural parameters of Kevlar fiber (pleated width, misorientation angle and skin thickness) are also studied to understand the contribution of these parameters to the stretching behavior of a Kevlar Bundle, which is significant to the future improvement of aromatic polyamide fibers for reinforcement purposes in advanced equipment.

Aggregation-induced emission (AIE) luminogen displays bright fluorescence and has photobleaching resistance in its aggregation state. It is an ideal fluorescent contrast agent for bioimaging. Multiphoton microscopy is an important tool for bioimaging since it possesses the ability to penetrate deep into biological tissues. Herein, we used AIE luminogen together with multiphoton microscopy for long-term imaging of zebrafish. A typical AIE luminogen, 2,3-bis(4-(phenyl(4- (1,2,2-triphenylvinyl) phenyl)amino)phenyl) fumaronitrile (TPE-TPA-FN or TTF), was encapsulated with 1,2-distearoyl-sn-glycero-3-phosphoethanola-mine-N-[methoxy(polyethylene glycol)-2000] (DSPE-mPEG2000) to form nanodots that exhibited bright three-photon fluorescence under 1,560 nm-femtosecond (fs) laser excitation. The TTF-nanodots were chemically stable in a wide range of pH values and showed no in vivo toxicity in zebrafish according to a series of biological tests. The TTF-nanodots were microinjected into zebrafish embryos, and the different growth stages of the labeled embryos were monitored with a three-photon fluorescence microscope. TTF-nanodots could be traced inside the zebrafish body for as long as 120 hours. In addition, the TTF-nanodots were utilized to target the blood vessel of zebrafish, and three-photon fluorescence angiogram was performed. More importantly, these nanodots were highly resistant to photobleaching under 1,560 nm-fs excitation, allowing long-term imaging of zebrafish.

Hexagonal phase NaLuF4:Yb3+/Er3+ nanorods were synthesized hydrothermally. An analysis of the intense green upconversion emissions at 525 nm and 550 nm in hexagonal phase NaLuF4:Yb3/+Er3+ nanorods under excitation power density of 4.2 W/cm2 available from a diode laser emitting at 976 nm, have been undertaken. Fluorescence intensity ratio (FIR) variation of temperature-sensitive green upconversion emissions at 525 nm and 550 nm in this material was recorded in the physiological range from 295 to 343 K. The maximum sensitivity derived from the FIR technique of the green upconversion emissions is approximately 0.0044 K−1. Experimental results implied that hexagonal phase NaLuF4:Yb3/+Er3+ nanorods was a potential candidate for optical temperature sensor.

Pure zero-valent iron (ZVI) has poor catalytic capacity due to its agglomeration and slow corrosion rate in neutral solution and hence requires acid condition for heterogeneous Fenton reaction. In this study, we develop an activated carbon (AC)-supported ZVI catalyst (AC-Fe0) that was prepared with a one-step reductive roasting method by employing AC as a reductant and supporting matrix. The constructed AC-Fe0 was then used for Fenton degradation of an azo dye reactive brilliant orange (X-GN). Analyses from multiple characterization techniques (e.g., scanning electron microscopy, X-ray diffraction, and Brunnaer-Emmett-Teller) show that ZVI particles with a diameter of about 5 μm were dispersed on the surface and pores of the AC. We show that the AC-Fe0 could be used as a highly effective catalyst for Fenton degradation of X-GN. A nearly unity efficiency of X-GN decoloration was achieved within 80 min reaction time under neutral solution condition that was attributed to the well-dispersion of ZVI particles on the AC and the formation of numerous galvanic cells between the ZVI and the AC. The decoloration of X-GN was found to follow the pseudo-first order kinetics and the apparent rate constant was measured to be 6.5 × 10−2 min−1 at 30°C. We conclude that this newly-developed AC-Fe0 technique greatly reduces the generation of massive iron-containing sludge as the remaining ferric ion in the solution was minimized (

Novel phosphors Ca6La2Na2(PO4)6F2:0.10Eu2+/Eu3+, xTb3+ (x = 0, 0.05, 0.10, 0.20, 0.30, 0.40, 0.50) were prepared by a solid state reaction in a CO-reducing atmosphere. The fluorescence spectra of samples Ca6La2Na2(PO4)6F2:xEu2+ reveal that still a small number of Eu3+ ions are detected in the host. The Eu2+ → Tb3+ → Eu3+ energy transfer process in Ca6La2Na2(PO4)6F2:0.10Eu2+/Eu3+, xTb3+ phosphors was discussed in detail through the excitation, emission spectra and the fluorescence decay. As a result of Eu2+ sensitization, the relative emission intensity of Ca6La2Na2(PO4)6F2:0.10Eu2+/Eu3+, xTb3+ is enhanced under near-ultraviolet light excitation. Furthermore, tunable emission with a large color gamut can be obtained by changing the Tb3+ doping concentration. These results indicate that the Ca6La2Na2(PO4)6F2:Eu2+/Eu3+, Tb3+ phosphors will have potential use in n-UV chip pumped white LED devices.

In this work, thulium and ytterbium codoped gadolinium molybdate (Gd2(MoO4)3:Yb/Tm) nanophosphors (NPs) have been synthesized, followed by being incorporated into a photo-catalytic titania (TiO2) nanoparticle layer. In detail, morphology and phase identification of the prepared NPs are first characterized and then the up-conversion of the Gd2(MoO4)3:Yb/Tm NPs is studied. Electron transfer dynamics after interfacing with bare or NP-doped electron donor TiO2 and the corresponding photovoltaic performance of solar cells are explored. The results show that Gd2(MoO4)3:Yb/Tm NPs excited at 976 nm exhibit intense blue (460–498 nm) and weak red (627–669 nm) emissions. The lifetime of electron transfer is shortened from 817 to 316 ps after incorporating NPs and correspondingly the electron transfer rate outstrips by 3 times that of the bare TiO2. Consequently, a notable power conversion efficiency of 4.15% is achieved as compared to 3.17% of pure TiO2/PTB7. This work demonstrates that the co-doping of robust rare earth ions with different unique functions can widen the harvesting range of the solar spectrum, boost electron transfer rate and eventually strengthen device performance, without complicated interfacial and structural engineering.

Novel phosphors Ca2NaSiO4F:Eu were synthesized successfully by the conventional solid-state method in CO atmosphere, and their spectroscopic properties in UV−vis region were investigated. The photoluminescence properties show that Eu3+ ions were partially reduced to Eu2+ in Ca2NaSiO4F. As a result of radiation and re-absorption energy transfer from Eu2+ to Eu3+, both Eu2+ bluish-green emission at around 520 nm and Eu3+ red emission are observed in the emission spectra under the n-UV light excitation. Furthermore, the ratio between Eu2+ and Eu3+ emissions varies with increasing content of overall Eu. Because relative intensity of the red component from Eu3+ became systematically stronger, white light emission can be realized by combining the emission of Eu2+ and Eu3+ in a single host lattice under n-UV light excitation. These results indicate that the Ca2NaSiO4F:Eu phosphors have potential applications as a n-UV convertible phosphor for light-emitting diodes. Keywords: Phosphors, Luminescence, White LED, Optical materials

In this work, ytterbium–erbium co-doped strontium molybdate (SrMoO4, SMO) nanophosphors (NPs), denoted as SMO:Yb/Er, have been successfully prepared. These NPs were then incorporated into TiO2 acceptor films in hybrid solar cells to enhance light harvesting by virtue of an up-conversion process where low energy photons can be converted into high energy photons through multi-photon processes. The results showed that the SMO:Yb/Er single crystal NPs are capable of turning near infrared photons into visible ones that can be easily captured by poly(thieno[3,4-b]-thiophene/benzodithiophene) (PTB7). The results indicate that the electron transfer rate at the PTB7/TiO2 donor/acceptor interface has been boosted sharply from 0.59 to 1.35 × 109 s−1. Consequently, a hybrid solar cell based on SMO:Yb/Er NP-doped TiO2/PTB7 delivers a high power conversion efficiency of up to 3.61%, thus leading to an efficiency enhancement of around 28% as compared to that of the neat PTB7/TiO2 counterpart (2.81%). This work demonstrates a promising approach to engineering efficient photovoltaic devices by taking advantage of the versatility of rare-earth ion doped oxides that function by modifying light in the solar spectrum.

In this work, three new diketopyrrolopyrrole (DPP)-based multi-branched derivatives (YJ-1, YJ-2 and YJ-3) with triphenylamine, 2,4,6-tri([1,1′-biphenyl]-4-yl)-1,3,5-triazine and 2,2′,2′′-(nitrilotr-is([1,1′-biphenyl]-4′,4-diyl))tris(3-phenylacrylonitrile) cores have been designed and synthesized. Their one- and two-photon absorption properties have been investigated. The two-photon absorption cross sections (σ) measured by the open aperture Z-scan technique are determined to be 2912, 2016 and 2800 GM for YJ-(1–3), respectively. This result indicates that donor–acceptor–donor (D–A–D)-type molecules are benefit to improve σ and their σ data increase with the better intramolecular charge transfer (ICT). Also, all of the three DPP derivatives exhibit good aggregation-induced emission (AIE) properties which are very weakly fluorescent in DMF, but a strong red fluorescent emission in solid state and in the aggregate state. More importantly, diketopyrrolopyrrole with tri-phenylamine (YJ-1) was applied for cell imaging and two-photon excited fluorescence in vivo imaging of mouse ear.

Organic fluorescent dyes with high quantum yield are widely applied in bioimaging and biosensing. However, most of them suffer from a severe effect called aggregation-caused quenching (ACQ), which means that their fluorescence is quenched at high molecular concentrations or in the aggregation state. Aggregation-induced emission (AIE) is a diametrically opposite phenomenon to ACQ, and luminogens with this feature can effectively solve this problem. Graphene oxide has been utilized as a quencher for many fluorescent dyes, based on which biosensing can be achieved. However, using graphene oxide as a surface modification agent of fluorescent nanoparticles is seldom reported. In this article, we used nanographene oxide (NGO) to encapsulate fluorescent nanoparticles, which consisted of a type of AIE dye named TPE-TPA-FN (TTF). NGO significantly improved the stability of nanoparticles in aqueous dispersion. In addition, this method could control the size of nanoparticles' flexibly as well as increase their emission efficiency. We then used the NGO-modified TTF nanoparticles to achieve three-photon fluorescence bioimaging. The architecture of ear blood vessels in mice and the distribution of nanoparticles in zebrafish could be observed clearly. Furthermore, we extended this method to other AIE luminogens and showed it was widely feasible.

Filterless narrowband near-infrared photodetectors (NIRPDs) offer significantly reducing cost and the system volume for various applications, but limited by the poor photosensitivity. Herein, we theoretically and experimentally demonstrate a novel class of sensitive filterless NIRPDs in CsPbF3: Zn2+-Yb3+- Tm3+ (or Er3+) perovskite nanocrystals (PeNCs)/Au nanorods (NRs) array hybrid via direct photon-electric upconverion (UC) from ground state of Yb3+- Tm3+ (or Er3+) to conduction band of PeNCs. It shows the selectively spectral photodetection at 980-nm NIR region with all full-width at half-maximum of 20 nm, high responsivity of 106 A/W, detectivity of 1.52 × 1012 Jones, and external quantum efficiency of 135%. The excellent performance can be mainly ascribed to (1) direct photon-electric UC mechanism; (2) the reduced trapping-center density, high carrier mobility, and increased extraction and separation efficient of election-hole pairs of PeNCs; (3) localized surface plasmon enhancement. Our findings open the exciting potential for developing the next-generation narrow NIRPDs.

Poly-p-phenylene terephthalamide (PPTA) fibers, such as DuPont's Kevlar fiber, are widely used in various fiber-reinforced composites due to their outstanding tensile stiffness, strength, and energy absorption capacity. To further improve the strength of PPTA-based fibers, it is necessary to investigate the molecular deformation mechanisms of these fibers while being coupled with nanoreinforcements. In this work, molecular dynamics method is used to predict the mechanical performance of carbon nanotubes (CNTs) reinforced Kevlar fibers, based on the molecular modeling of crystal interfaces in the microstructure of Kevlar fiber with the help of surface-modified CNTs, the tensile strength of Kevlar fibers can be increased by 27.8–39.7%. Furthermore, the mechanism of binding stability of CNTs is investigated by modifying the functional groups of CNTs, in which the hydrogen bonds (H-bonds) interaction plays an important role.

InP quantum dots (QDs) are typical III-V group semiconductor nanocrystals that feature large excitonic Bohr radius and high carrier mobility. The merits of InP QDs include large absorption coefficient, broad color tunability, and low toxicity, which render them promising alternatives to classic Cd/Pb-based QDs for applications in practical settings. Over the past two decades, the advances in wet-chemistry methods have enabled the synthesis of small-sized colloidal InP QDs with the assistance of organic ligands. By proper selection of synthetic protocols and precursor materials coupled with surface passivation, the QYs of InP QDs are pushed to near unity with modest color purity. The state-of-the-art InP QDs with appealing optical and electronic properties have excelled in many applications with the potential for commercialization. This work focuses on the recent development of wet-chemistry protocols and various precursor materials for the synthesis and surface modification of InP QDs. Current methods for constructing light-emitting diodes using novel InP-based QDs are also summarized.

High quality blue emitting quantum dots (QDs) are regarded as promising nanomaterials for lasers, photovoltaic cells and displays. However, few reports realize high photoluminescence quantum yield (PL QY), narrow emission band width and pure blue emitting (450∼460 nm) simultaneously. Herein we propose a facile one-step synthesis of thick shell blue emitting CdZnS/ZnS QDs. ZnS shell was overcoated on the prepared cores by directly introducing zinc oleate/S TBP solution (zinc oleate powder and S dissolved in TBP) into mixture without any purification steps and the thickness of ZnS shell was controlled by adjusting the adding amount of zinc oleate/S TBP solution. The optimal QDs with ten monolayers of ZnS shell exhibit pure blue light (∼455 nm) with narrow line width (full width half maximum, FWHM 17.2 nm) and high photoluminescent quantum yield (QY) (92%). Due to the thick ZnS shell, nonradiative recombination of the QD solids is suppressed efficiently.

Lead ion is one of the most toxic metallic pollutants, lacking of photoluminescence probe in organic products. In this work, the lead free perovskite CsSnX3 (X = Cl, Cl/Br, or Br) quantum dots (QDs) were employed as a novel fluorescent probe for the detection of lead ion in the oily products, with high sensitivity and high selectivity. The highly enhanced photoluminescence, the red shift and the reduction of the full wavelength at half maximum (FWHM) of emission spectra of CsSnX3 QDs were observed after adding Pb2+ ions, originating from the substitution of Sn2+ by Pb2+ ions in situ. A wide dynamic range from 1 × 10−8 M to 1 × 10−2 M and a low limit of detection (3.5 × 10−9 M) were obtained. Finally, the CsSnBr3 QDs was successfully employed to probe Pb2+ ions in mask, hair dye, nail polish and oil paint. Our probe provides a promising device to detect Pb2+ ions in organic solution system.

The development of fluorogens with deep-red emission is one of the hottest topics of investigation in the field of bio/chemosensors and bioimaging. Herein, the tunable fluorescence of perylene diimide (PDI) derivatives was achieved by the incorporation of varied isolation groups linked on the PDI core. With the enlarged sizes of isolation groups, the conversion from aggregation caused quenching to aggregation-induced emission was obtained in their fluorescence variations from solutions to nanoparticles, as the result of the efficient inhibition of π-π stacking by the larger isolation groups. Accordingly, DCzPDI bearing 1,3-di(9H-carbazol-9-yl)benzene as the biggest isolation group exhibited the bright deep-red emission in the aggregated state with a quantum yield of 12.3%. Combined with the three-photon excited fluorescence microscopy (3PFM) technology, through-skull 3PFM imaging of mouse cerebral vasculature can be realized by DCzPDI nanoparticles with good biocompatibility, and the penetration depth can be as deep as 450 μm.

Currently, a serious problem obstructing the large-scale clinical applications of fluorescence technique is the shallow penetration depth. Two-photon fluorescence microscopic imaging with excitation in the longer-wavelength near-infrared (NIR) region (>1100 nm) and emission in the NIR-I region (650-950 nm) is a good choice to realize deep-tissue and high-resolution imaging. Here, we report ultradeep two-photon fluorescence bioimaging with 1300 nm NIR-II excitation and NIR-I emission (peak ∼810 nm) based on a NIR aggregation-induced emission luminogen (AIEgen). The crab-shaped AIEgen possesses a planar core structure and several twisting phenyl/naphthyl rotators, affording both high fluorescence quantum yield and efficient two-photon activity. The organic AIE dots show high stability, good biocompatibility, and a large two-photon absorption cross section of 1.22 × 103 GM. Under 1300 nm NIR-II excitation, in vivo two-photon fluorescence microscopic imaging helps to reconstruct the 3D vasculature with a high spatial resolution of sub-3.5 μm beyond the white matter (>840 μm) and even to the hippocampus (>960 μm) and visualize small vessels of ∼5 μm as deep as 1065 μm in mouse brain, which is among the largest penetration depths and best spatial resolution of in vivo two-photon imaging. Rational comparison with the AIE dots manifests that two-photon imaging outperforms the one-photon mode for high-resolution deep imaging. This work will inspire more sight and insight into the development of efficient NIR fluorophores for deep-tissue biomedical imaging.

Fabrication of near-infrared light-triggered photoelectrochemical (PEC) sensors based on the upconversion nanophosphors (UCNPs) is a novel approach, which exhibits the advantages of low background signal and non-damage to the biological substance as well as high sensitivity and improved electric detection in PEC sensors. Herein we demonstrate the preparation of novel and high-quality ZnO inverse opal photonic crystals (IOPCs)/Ag/NaYF4:Yb,Tm hybrid films by different advanced film techniques, including colloidal self-assembling, vapor phase deposition and pulsed laser deposition and its application to sensitive detection of alpha-fetoprotein (AFP). In the complex device, ZnO IOPCs and surface plasmon resonance (SPR) of silver had ability to largely enhance local excitation electromagnetic field of NaYF4:Yb,Tm, resulting in efficient near-infrared to visible/ultraviolet upconversion luminescence (UCL). The ultraviolet light emitted by NaYF4:Yb,Tm could b further reabsorbed by ZnO, generating PEC responses. Furthermore, because of the high specific surface area of ZnO IOPCs and the conductivity of Ag films, ZnO IOPCs/Ag/NaYF4:Yb,Tm hybrid films based near-infrared light-triggered PEC sensors showed ultrasensitive detection of AFP with a linear range from 0.05 ng mL−1 to 100 ng mL−1 and a low detection limit of ∼0.04 ng mL−1 (40 pg mL−1). Such an advanced device also shows promise in detection of other cancer markers in clinical and biological analysis.