Oxide Derivatives of Nb2CTx MXene and Their Application as Electron Transport Layers in Perovskite Solar Cells: Unraveling the Oxidation Process and Functionalization.

In the realm of photovoltaic research, 2D transition metal carbides (MXenes) have gained significant interest due to their exceptional photoelectric capabilities. However, the instability of MXenes due to oxidation has a direct impact on their practical applications. In this work, the oxidation process of Nb2CTx MXene in aqueous systems is methodically simulated at the atomic level and nanosecond timescales, which elucidates the structural variations influenced by the synergistic effects of water and dissolved oxygen, predicting a transition from metal to semiconductor with 44% C atoms replaced by O atoms in Nb2CTx. Moreover, Nb2CTx with varying oxidation degrees is utilized as electron transport layers (ETLs) in perovskite solar cells (PSCs). Favorable energy level alignments with superior electron transfer capability are achieved by controlled oxidation. By further exploring the composites of Nb2CTx to its derivatives, the strong interaction of the nano-composites is demonstrated to be more effective for electron transport, thus the corresponding PSC achieves a better performance with long-term stability compared with the widely used ETLs like SnO2. This work unravels the oxidation dynamics of Nb2CTx and provides a promising approach to designing ETL by exploiting MXenes to their derivatives for photovoltaic technologies.

New insights into the alkoxy effects on auxiliary adsorption and inhibiting charge recombination in dye-sensitized solar cells with high open circuit voltage: a theoretical investigation.

Although introducing an alkoxy group is one of the most popular methods to suppress the interfacial charge recombination process of dye-sensitized solar cells, understanding of its effects is still limited and a microscopic picture of the alkoxy effects is lacking. Two ullazine dyes with distinct alkoxy chains at the donor part are used to investigate the effects of the alkoxy group on the adsorption, dye aggregation and charge recombination process in our study. Different from the usual assumption, we find that alkoxy chains can not only play a shielding role, but can also assist dye adsorption and inhibit the charge recombination process more effectively by covering the TiO2 surface. We also find that the existence of alkyl chains can well inhibit the aggregation of dyes and reduce intermolecular electron transfer. Furthermore, an important structural feature at the interface, the Ti-O interaction between the oxygen atom of the alkoxy group and the Ti atom of the surface is also found to contribute substantially to the interface stability. New insights into the effects of the alkoxy group on auxiliary adsorption and inhibiting charge recombination through reducing the recombination sites pave the way for rational design of sensitizers with high performance.

Afterglow-Suppressed Lu2O3:Eu3+ Nanoscintillators for High-Resolution and Dynamic Digital Radiographic Imaging.

Lu2(1-x)Eu2xO3 nanoscintillators (x = 0.005, 0.01, 0.03, 0.05, 0.07, and 0.10) with red emission were synthesized by a coprecipitation method. It is found that their photo- and radioluminescence intensities increase with increasing Eu3+ concentration until x = 0.05. According to their concentration-dependent luminescence intensity ratios (I610(C2)/I582(S6)), the existing energy transfer from Eu3+(S6) (occupying S6 sites) to Eu3+(C2) (occupying C2 sites) can be confirmed. Based on the spectral data and density functional theory (DFT) calculations, the origin of Lu2O3:Eu3+ persistent luminescence at low concentration might be related to the tunneling processes between Eu3+ (occupying C2 and S6 sites) and oxygen interstitials (Oi×). After dispersing afterglow-suppressed Lu2O3:Eu3+ nanoscintillators into polymethyl methacrylate (PMMA) polymer-acetone solution, flexible PMMA-Lu2O3:Eu3+ composite films with high thermal stability and radiation resistance were fabricated by a doctor blade method. As the flexible composite film was used as an imaging plate, static X-ray images with high spatial resolution (5.5 lp/mm) under an extremely low dose of ∼1.1 µGyair can be acquired. When a watch with a moving second hand was used as an object, the dynamic X-ray imaging can be realized under a dose rate of 55 µGyair·s-1. Our results demonstrate that Lu2O3:Eu3+ nanoscintillators can be regarded as candidate materials for dynamic digital radiographic imaging.

Photoluminescent and multi-phonon resonance Raman scattering dual-mode immunoassays based on CdS nanoparticles for HIgG detection.

A dual-mode immunoassay strategy based on CdS nanoparticles as signal probes with both of photoluminescent (PL) and multi-phonon resonance Raman scattering (MRRS) properties was developed. Simplified structural design and preparation were achieved due to the intrinsic integration of PL and MRRS dual signals in the single-unit CdS nanoprobes. Human immunoglobulin G (HIgG) was sensitively and specifically detected using the proposed PL-MRRS dual-mode strategy. The linear relationship between the HIgG concentration and the intensity of 707 nm PL peaks/300 cm-1 MRRS peaks under the excitation of 488 nm laser was established. The limit of detection was 0.93 fg mL-1 for PL and 1.10 fg mL-1 for MRRS. In comparison with previous IgG detection methods, the proposed method exhibited prominent advantages in detection sensitivity and working range with good stability and repeatability. An internal self-calibration was realized which ensured the accuracy and reliability of detection results. Both results of specificity experiments and serum sample analysis further confirmed the feasibility of the designed immunoassay strategy in practical serological detection.

A Pr3+ doping strategy for simultaneously optimizing the size and near infrared persistent luminescence of ZGGO:Cr3+ nanoparticles for potential bio-imaging.

Spinel-phase Zn2Ga2.98-xGe0.75O8:Cr0.020,Prx (ZGGO:Cr3+,Pr3+) near infrared (NIR) persistent luminescence nanoparticles (PLNPs) with different amounts of Pr3+ dopant were prepared by a hydrothermal method in combination with a subsequent annealing in a vacuum. For these nanoparticles, the averaged particle size decreases from 64 to 37 nm with increasing Pr3+ doping concentration from 0 to 0.025 and Cr3+ and Pr3+ ions are uniformly doped into the interior and surface of a single nanoparticle. It can be found that Pr3+ doping leads to the appearance of more anti-site pairs () around distorted octahedral Cr3+ ions and enhanced NIR emissions around 697 nm, which originate from the 2E(2G) → 4A2(4F) and 4T2(4F) → 4A2(4F) transitions of the interior and surface Cr3+ ions in the nanoparticles. In particular, for the interior Cr3+ ions in the Pr3+ doped nanoparticles, the enhanced NIR luminescence can be attributed to the suppressed energy transfer of the excited electrons from the 4T2(4F) level to the trap level related to anti-site pairs () around the distorted octahedral Cr3+ ions. Our results suggest that Pr3+ doped ZGGO:Cr3+ PLNPs have potential applications for bio-imaging.

Enhanced emission of encaged-OH--free Ca12(1-x)Sr12xAl14O33:0.1%Gd3+ conductive phosphors via tuning the encaged-electron concentration for low-voltage FEDs.

Encaged-OH--free Ca12(1-x)Sr12xAl14O33:0.1%Gd3+ conductive phosphors were prepared through a melt-solidification process in combination with a subsequent heat treatment. Absorption spectra showed that the maximum encaged-electron concentration was increased to 1.08 × 1021 cm-3 through optimizing the doping amount of Sr2+ (x = 0.005). Meanwhile, FTIR and Raman spectra indicated that pure Ca11.94Sr0.06Al14O33:0.1%Gd3+ conductive phosphor without encaged OH- and C22- anions was acquired. For the conductive powders heat-treated in air for different times, the encaged-electron concentrations were tuned from 1.02 × 1021 to 8.3 × 1020 cm-3. ESR, photoluminescence, and luminescence kinetics analyses indicated that the emission at 312 nm mainly originated from Gd3+ ions surrounded by encaged O2- anions, while Gd3+ ions surrounded by encaged electrons had a negative contribution to the UV emission due to the existence of an energy transfer process. Under low-voltage electron-beam excitation (3 kV), enhanced cathodoluminescence (CL) of the conductive phosphors could be achieved by tuning the encaged-electron concentrations. In particular, for the encaged-OH--free conductive phosphor, the emission intensity of the CL was about one order of magnitude higher than that of the conductive phosphor containing encaged OH- anions. Our results suggested that the encaged-OH--free conductive phosphors have potential application in low-voltage FEDs.

Enhancement of encaged electron concentration by Sr(2+) doping and improvement of Gd(3+) emission through controlling encaged anions in conductive C12A7 phosphors.

Conductive C12A7:0.1%Gd(3+),y%Sr(2+) powders with different Sr(2+) doping concentrations have been prepared in a H2 atmosphere by a solid state method in combination with subsequent UV-irradiation. The encaged electron concentration could be modulated through tuning Sr(2+) doping and its maximum value reaches 2.3 × 10(19) cm(-3). This is attributed to the competition between enhanced uptake and the release of the encaged anions during their formation and diffusion processes and the suppression of encaged electrons generation due to the increased encaged OH(-) anions and the decreased encaged O(2-) anions. Although there exists encaged electrons and different encaged anions (O(2-), H(-) and OH(-)) in C12A7 conductive powders prepared through the hydrogen route, a dominant local environment around Gd(3+) could be observed using electron spin resonance (ESR) detection. It can be ascribed to the stronger coupling of the encaged OH(-) to the framework of C12A7 than those of the encaged electrons, O(2-) and H(-) anions. In addition, emission of Gd(3+) ions is enhanced under UV or low voltage electron beam excitation and a new local environment around Gd(3+) ions appears through the thermal annealing in air because of the decrease of the encaged OH(-) anions and the increase of the encaged O(2-) anions. Our results suggested that Sr(2+) doping in combination with thermal annealing in air is an effective strategy for increasing the conductive performance and enhancing the emission of rare earth ions doped into C12A7 conductive phosphors for low-voltage field emission displays (FEDs).

Alkyl effects on charge recombination in copper electrolyte-based dye-sensitized solar cells: Insights for targeted molecular design towards high performance.

Two quinoxaline dyes utilized in copper-electrolyte-based dye-sensitized solar cells (Cu-DSSCs) are theoretically investigated to analyze the impact of alkyl chains on dye performance. The investigation shows that ZS4, known for its record efficiency of up to 13.2 %, exhibits higher electron coupling and fewer binding sites for dye-[Cu(tmby)2]2+ interaction compared to ZS5. Contrary to common belief, alkyl chains are found to not only provide shielding but also hinder the interaction between dye and [Cu(tmby)2]2+ by influencing the optimal conformation of dyes, thereby impeding the charge recombination process. It is crucial to consider the influence of alkyl chains on dye conformation when discussing the relationship between dye structure and performance, rather than oversimplifying it as often done traditionally. Building on these findings, eight dyes are strategically designed by adjusting the position of the alkyl chain to further decrease charge recombination compared to ZS4. Theoretical evaluation of these dyes reveals that changing the alkyl chain on the nitrogen atom from 2-ethylhexyl (ZS4) to 1-hexylheptyl (D3-2) not only reduces the charge recombination rate but also enhances light harvesting ability. Therefore, D3-2 shows potential as a candidate for experimental synthesis of high-performance Cu-DSSCs with improved efficiency.

Revealing oxygen effect on efficiency and stability of quantum dot photovoltaics.

Colloidal quantum dot solar cells (CQDSCs) have received great attention in the development of scalable and stable photovoltaic devices. Despite the high power-conversion-efficiency (PCE) reported, stability investigations are still limited and the exact degradation mechanisms of CQDSCs remain unclear under different atmosphere conditions. In this study, the atmospheric influence on the ZnO electron transport layer material (ETL), halide-passivated lead sulfide CQDs (PbS-PbI2) photoactive layer material and 1,2-ethanedithiol-PbS CQDs (PbS-EDT) hole transport material on device stability in PbS CQDSCs is investigated. It was found that O2 had negligible influence on PbS-PbI2, but it did induce the increase in work function of ZnO ETL and PbS-EDT layers. Notably, the increase of the ZnO work function (WFZnO) induces the formation of interface barrier between ZnO and PbS-PbI2, leading to a deterioration in device efficiency. By further replacing ZnO ETL with SnO2, a multi-interface collaborative CQDSC was constructed to realize the PCE with high stability. This study identifies the efficiency evolution that is inherent in CQDSCs under different atmospheric conditions.

Facial Action Unit Detection via Adaptive Attention and Relation.

Facial action unit (AU) detection is challenging due to the difficulty in capturing correlated information from subtle and dynamic AUs. Existing methods often resort to the localization of correlated regions of AUs, in which predefining local AU attentions by correlated facial landmarks often discards essential parts, or learning global attention maps often contains irrelevant areas. Furthermore, existing relational reasoning methods often employ common patterns for all AUs while ignoring the specific way of each AU. To tackle these limitations, we propose a novel adaptive attention and relation (AAR) framework for facial AU detection. Specifically, we propose an adaptive attention regression network to regress the global attention map of each AU under the constraint of attention predefinition and the guidance of AU detection, which is beneficial for capturing both specified dependencies by landmarks in strongly correlated regions and facial globally distributed dependencies in weakly correlated regions. Moreover, considering the diversity and dynamics of AUs, we propose an adaptive spatio-temporal graph convolutional network to simultaneously reason the independent pattern of each AU, the inter-dependencies among AUs, as well as the temporal dependencies. Extensive experiments show that our approach (i) achieves competitive performance on challenging benchmarks including BP4D, DISFA, and GFT in constrained scenarios and Aff-Wild2 in unconstrained scenarios, and (ii) can precisely learn the regional correlation distribution of each AU.

A dual-mode method for detection of miRNA based on the photoluminescence and resonance light scattering.

MicroRNAs (miRNAs) hold potential as useful biomarkers for early diagnosis and evaluation of diverse cancers, but their low abundance and short length make the detection of miRNAs face low sensitivity and accuracy. Herein, a photoluminescence (PL)-resonance light scattering (RLS) dual-mode method was developed for the sensitive and accurate detection of miRNA-141 using CdTe quantum dots (QDs) and Au nanoparticles. The presence of miRNA-141 induced PL quenching and RLS increasing. The limit of detection (LOD) was as low as 3.7 fM, and the miRNA-141 was detected linearly in a range from 10 fM to 10 nM. The dual signals generated no mutual interference and were detected using the same spectrophotometer, allowing for mutual validation to ensure the accuracy and reliability of the detection results. This study proposes valuable references for constructing dual-mode detection methods.

Ethanol Solution Plasma Loads Carbon Dots onto 2D HNb3O8 for Enhanced Photocatalysis.

Layered metal oxoacids hold potential as photocatalysts due to their facile exfoliation to two-dimensional (2D) nanosheets with a large surface area and a short migration distance for photoexcited charge carriers. However, the utilization of electrons in photocatalytic processes is restricted by the competitive trapping of electrons by metal ions. In this work, we attempt to improve the utilization of photogenerated electrons over exfoliated HNb3O8 nanosheets by solution plasma activation. On dispersing exfoliated HNb3O8 nanosheets in ethanol solution plasma, the defects in HNb3O8 can be engineered, and carbon dots (CDs) can be anchored on the surface of HNb3O8 nanosheets in situ. In comparison with pristine HNb3O8 nanosheets, the rate of photocatalytic hydrogen evolution can be increased by 317.7 times over the HNb3O8/C heterojunction, and the apparent quantum efficiency of hydrogen production can be as high as 5.05%. The reason for the high photocatalytic performance is explored by the comparison of activation between plasma-in-ethanol and plasma-in-water, which reveals that CD anchoring and defect engineering indeed promote charge separation and hence lead to enhanced photocatalytic activity. This work provides an alternative approach to synthesize CDs and activate 2D-layered compounds with MO6 (M = Nb, Ti, and W) octahedral building blocks in the host layer for enhanced photocatalytic evolution of hydrogen.

Personalized Image Aesthetics Assessment via Meta-Learning With Bilevel Gradient Optimization.

Typical image aesthetics assessment (IAA) is modeled for the generic aesthetics perceived by an "average" user. However, such generic aesthetics models neglect the fact that users' aesthetic preferences vary significantly depending on their unique preferences. Therefore, it is essential to tackle the issue for personalized IAA (PIAA). Since PIAA is a typical small sample learning (SSL) problem, existing PIAA models are usually built by fine-tuning the well-established generic IAA (GIAA) models, which are regarded as prior knowledge. Nevertheless, this kind of prior knowledge based on "average aesthetics" fails to incarnate the aesthetic diversity of different people. In order to learn the shared prior knowledge when different people judge aesthetics, that is, learn how people judge image aesthetics, we propose a PIAA method based on meta-learning with bilevel gradient optimization (BLG-PIAA), which is trained using individual aesthetic data directly and generalizes to unknown users quickly. The proposed approach consists of two phases: 1) meta-training and 2) meta-testing. In meta-training, the aesthetics assessment of each user is regarded as a task, and the training set of each task is divided into two sets: 1) support set and 2) query set. Unlike traditional methods that train a GIAA model based on average aesthetics, we train an aesthetic meta-learner model by bilevel gradient updating from the support set to the query set using many users' PIAA tasks. In meta-testing, the aesthetic meta-learner model is fine-tuned using a small amount of aesthetic data of a target user to obtain the PIAA model. The experimental results show that the proposed method outperforms the state-of-the-art PIAA metrics, and the learned prior model of BLG-PIAA can be quickly adapted to unseen PIAA tasks.

Photothermal conversion performance and acid-induced aggregation of PLNP-Bi2S3 composite nanoplatforms.

Poly(sodium 4-styrenesulfonate) (PSS) molecule modified PLNP-Bi2S3 composite nanoplatforms were constructed by using polyvinylpyrrolidone (PVP) modified Bi2S3 nanoparticles (∼4.6 nm) as a photothermal agent and hexadecyl trimethyl ammonium bromide (CTAB) coated Zn2Ga2.98Ge0.75O8:Cr0.023+ (ZGGO:Cr3+@CTAB) persistent luminescence nanoparticles (PLNPs) through electrostatic adsorption. It is found that the above composite nanoplatforms have excellent laser-irradiation thermal stability and good photothermal conversion performance. The measured photothermal conversion efficiency is ∼44%, which is higher than that (∼37%) of the PLNP-GNR (gold nanorod) composite nanoplatforms. Meanwhile, PSS modified PLNP-Bi2S3 composite nanoplatforms exhibited good solution dispersibility in blood and normal tissue environments. While reaching tumor sites, the above composite nanoplatforms can be rapidly accumulated in cancer cells with acidic environments. This pH-responsive acid-induced aggregation can be ascribed to the chemical reaction induced by the protonation of PSS modified PLNP-Bi2S3 composite nanoplatforms with a negatively charged surface in the acidic environments. Our results suggest that PSS modified PLNP-Bi2S3 composite nanoplatforms might be applied to precision diagnosis and therapy of deep-tissue tumors.

White luminescence of Dy3+ ions doped 12CaO 7Al2O3 nanopowders under UV light excitation.

12CaO 7Al2O3:Dy3+ nanopowders were successfully synthesized by the chemical co-precipitation method. X-ray diffraction result shows that the single 12CaO 7Al2O3 phase is formed with Dy3+ ions to replace the Ca2+ ions in the host of 12CaO 7Al2O3. The yellow and blue emissions, attributed to the forced electric dipole transition of 4F(9/2) --> 6H(13/2) centered at 571 nm and the magnetic dipole transition of 4F(9/2) --> 6H(15/2) centered at 480 nm, respectively, were observed. The integrated intensity ratios of yellow to blue increase from 1.63 to 1.70 with Dy3+ concentration increasing from 0.8 to 2.0% for the as-prepared 12CaO 7Al2O3:xDy3+ phosphor. The significantly enhanced emission intensities of 12CaO 7Al2O3:1.0% Dy3+ phosphor annealed at 900 degrees C for 2 hours in vacuum ambient could be ascribed to the decrease of OH(-) groups and the change of the surface topography. The thermal stability and the Commission International de l'Eclairage coordinates were also investigated. All the photoluminescence characteristics indicate that Dy3+ ions doped 12CaO 7Al2O3 may be a good candidate for the solid state lighting phosphor as well as white light-emitting diodes.

IE-IQA: Intelligibility Enriched Generalizable No-Reference Image Quality Assessment.

Image quality assessment (IQA) for authentic distortions in the wild is challenging. Though current IQA metrics have achieved decent performance for synthetic distortions, they still cannot be satisfactorily applied to realistic distortions because of the generalization problem. Improving generalization ability is an urgent task to make IQA algorithms serviceable in real-world applications, while relevant research is still rare. Fundamentally, image quality is determined by both distortion degree and intelligibility. However, current IQA metrics mostly focus on the distortion aspect and do not fully investigate the intelligibility, which is crucial for achieving robust quality estimation. Motivated by this, this paper presents a new framework for building highly generalizable image quality model by integrating the intelligibility. We first analyze the relation between intelligibility and image quality. Then we propose a bilateral network to integrate the above two aspects of image quality. During the fusion process, feature selection strategy is further devised to avoid negative transfer. The framework not only catches the conventional distortion features but also integrates intelligibility features properly, based on which a highly generalizable no-reference image quality model is achieved. Extensive experiments are conducted based on five intelligibility tasks, and the results demonstrate that the proposed approach outperforms the state-of-the-art metrics, and the intelligibility task consistently improves metric performance and generalization ability.

Personality-assisted Multi-task Learning for Generic and Personalized Image Aesthetics Assessment.

Traditional image aesthetics assessment (IAA) approaches mainly predict the average aesthetic score of an image. However, people tend to have different tastes on image aesthetics, which is mainly determined by their subjective preferences. As an important subjective trait, personality is believed to be a key factor in modeling individual's subjective preference. In this paper, we present a personality-assisted multi-task deep learning framework for both generic and personalized image aesthetics assessment. The proposed framework comprises two stages. In the first stage, a multi-task learning network with shared weights is proposed to predict the aesthetics distribution of an image and Big-Five (BF) personality traits of people who like the image. The generic aesthetics score of the image can be generated based on the predicted aesthetics distribution. In order to capture the common representation of generic image aesthetics and people's personality traits, a Siamese network is trained using aesthetics data and personality data jointly. In the second stage, based on the predicted personality traits and generic aesthetics of an image, an inter-task fusion is introduced to generate individual's personalized aesthetic scores on the image. The performance of the proposed method is evaluated using two public image aesthetics databases. The experimental results demonstrate that the proposed method outperforms the state-of-the-arts in both generic and personalized IAA tasks.

Theoretical insights on the comparison of champion dyes SM315 and C275 used for DSSCs reaching over 12% efficiency and the further optimization of C275.

Theoretical insights on the comparison between the champion dyes SM315 and C275 used for high-performance dye-sensitized solar cells (DSSCs) reaching over 12% efficiency with different electron donors only (porphyrin for SM315 and indenoperylene for C275) were explored for the first time. The intrinsic reasons for the significantly improved monochromatic photon-to-electric current conversion efficiency (IPCE) and open circuit voltage (Voc) of C275-based DSSCs over those of SM315 were revealed. According to our results, we find that the larger IPCE of C275 is attributed to its larger electronic coupling, smaller reorganization energy, reduced exciton binding energy and enhanced charge transfer character, all of which when combined lead to a larger electron injection efficiency. In addition, the larger Voc of C275 is due to a greater number of injected electrons, a smaller molecular volume and a smaller projected area, which lead to a more compact adsorption layer with a hindered charge recombination process. Thus, C275 is expected to have more potential to further optimize high-performance DSSCs. In view of the primary shortcoming of C275, which is its relatively narrow absorption spectrum, further optimization was made through structural modification using a series of heterocyclic anchoring groups. Using the same evaluation criteria, the theoretical screening of these dyes based on C275 is carried out. We find that indenoperylene dye with a barbituric acid (BA) anchoring group is a promising candidate for the experimental synthesis of high-performance DSSCs with improved Jsc, Voc and adsorption stability.

Enhanced near infrared persistent luminescence of Zn2Ga2.98Ge0.75O8:Cr0.02 3+ nanoparticles by partial substitution of Ge4+ by Sn4.

Spinel-phase Zn2Ga2.98Ge0.75-x Sn x O8:Cr0.02 3+ (ZGGSO:Cr3+) nanoparticles with various Sn4+ concentrations were prepared by a hydrothermal method in combination with a post-annealing in vacuum at high temperature. For these nanoparticles, the observed near infrared (NIR) persistent luminescence peaked at ∼697 nm and originates from the 2E, 4T2 (4F) → 4A2 transitions of Cr3+ and the afterglow time exceeds 800 min. For both the interior and surface Cr3+ ions in the ZGGSO host, it can be found that the increased energy transfer from Cr3+ to the deep trap (anti-site defects, ) after the substitution of Ge4+ by Sn4+ plays a key role in enhancing the persistent luminescence of the ZGGSO:Cr3+ nanoparticles. Strikingly, this energy transfer process can be controlled through the variations in the crystal field strength and the trap depths. Our results suggest that not only Sn4+ substitution can improve in vivo bioimaging but also the existence of deep traps in ZGGSO:Cr3+ nanoparticles is helpful for retracing in vivo bioimaging at any time.

A vacuum-annealing strategy for improving near-infrared super long persistent luminescence in Cr(3+) doped zinc gallogermanate nanoparticles for bio-imaging.

Novel Cr(3+) doped zinc gallogermanate (ZGGO) nanoparticles with 697 nm near-infrared (NIR) super long afterglow were prepared via a hydrothermal method. Subsequently, a vacuum-annealing strategy was adopted to improve NIR afterglow in ZGGO:Cr(3+) nanoparticles. For the sample annealed at 800 °C, no variation in the particle size is observed, the persistent luminescence increases by an order of magnitude (∼14 times) and the NIR afterglow time reaches more than 15 hours relative to the as-prepared sample. After annealing at temperatures higher than 880 °C, the persistent luminescence of the nanoparticles is enhanced, but they show aggregated-surface behavior. Meanwhile, shallow and deep traps are generated, related to the antisite defects and VGe-Cr(3+)-VO defect clusters, respectively. Finally, we apply ZGGO:Cr(3+) persistent luminescence nanoparticles (PLNPs) to a human serum albumin (HSA) colloid solution, and more than 1 h of NIR persistent luminescence is detected under 320 nm excitation. The quenching effect of NIR luminescence by OH(-) in the HSA solution is observed based on the reduced contribution of surface Cr(3+) in PLNPs to NIR luminescence. Our results suggest that ZGGO:Cr(3+) PLNPs have potential applications for in vivo bio-imaging.