In-depth discussion on recent progress of fundamental understanding of AIE mechanisms, identifying the existing challenges and opportunities for future developments.
Nowadays, multivariate time series data are increasingly collected in various real world systems, e.g., power plants, wearable devices, etc. Anomaly detection and diagnosis in multivariate time series refer to identifying abnormal status in certain time steps and pinpointing the root causes. Building such a system, however, is challenging since it not only requires to capture the temporal dependency in each time series, but also need encode the inter-correlations between different pairs of time series. In addition, the system should be robust to noise and provide operators with different levels of anomaly scores based upon the severity of different incidents. Despite the fact that a number of unsupervised anomaly detection algorithms have been developed, few of them can jointly address these challenges. In this paper, we propose a Multi-Scale Convolutional Recurrent Encoder-Decoder (MSCRED), to perform anomaly detection and diagnosis in multivariate time series data. Specifically, MSCRED first constructs multi-scale (resolution) signature matrices to characterize multiple levels of the system statuses in different time steps. Subsequently, given the signature matrices, a convolutional encoder is employed to encode the inter-sensor (time series) correlations and an attention based Convolutional Long-Short Term Memory (ConvLSTM) network is developed to capture the temporal patterns. Finally, based upon the feature maps which encode the inter-sensor correlations and temporal information, a convolutional decoder is used to reconstruct the input signature matrices and the residual signature matrices are further utilized to detect and diagnose anomalies. Extensive empirical studies based on a synthetic dataset and a real power plant dataset demonstrate that MSCRED can outperform state-ofthe-art baseline methods.
Quick: An exogenously induced quick increase of the H2S concentration (80 s) in MCF‐7 cells can be visualized by ratiometric imaging using a new probe (CouMC) that can target mitochondria. CouMC was constructed by combining merocyanine and coumarin fluorophores. The selective nucleophilic addition of HS− to the merocyanine derivative at neutral pH is crucial for the rapid H2S detection.
Far-red and near-infrared (NIR) fluorescent materials possessing the characteristics of strong two-photon absorption and aggregation-induced emission (AIE) as well as specific targeting capability are much-sought-after for bioimaging and therapeutic applications due to their deep penetration depth and high resolution. Herein, a series of dipolar far-red and NIR AIE luminogens with a strong push-pull effect are designed and synthesized. The obtained fluorophores display bright far-red and NIR solid-state fluorescence with a high quantum yield of up to 30%, large Stokes shifts of up to 244 nm, and large two-photon absorption cross-sections of up to 887 GM. A total of three neutral AIEgens show specific lipid droplet (LD)-targeting capability, while the one with cationic and lipophilic characteristics tends to target the mitochondria specifically. All of the molecules demonstrate good biocompatibility, high brightness, and superior photostability. They also serve as efficient two-photon fluorescence-imaging agents for the clear visualization of LDs or mitochondria in living cells and tissues with deep tissue penetration (up to 150 μm) and high contrast. These AIEgens can efficiently generate singlet oxygen upon light irradiation for the photodynamic ablation of cancer cells. All of these intriguing results prove that these far-red and NIR AIEgens are excellent candidates for the two-photon fluorescence imaging of LDs or mitochondria and organelle-targeting photodynamic cancer therapy.
Seeking new methods to obtain elaborate artificial on-demand photoswitching with multiple functionalities remains challenging. Most of the systems reported so far possess only one specific function and their nonemissive nature in the aggregated state inevitably limit their applications. Herein, a tailored cyanostilbene-based molecule with aggregation-induced emission characteristic was synthesized and was found to exhibit efficient, multiple and controllable photoresponsive behaviors under different conditions. Specifically, three different reactions were involved: (i) reversible Z/E isomerization under room light and thermal treatment in CHCN, (ii) UV-induced photocyclization with a concomitant dramatic fluorescence enhancement, and (iii) regio- and stereoselective photodimerization in aqueous medium with microcrystal formation. Experimental and theoretical analyses gave visible insights and detailed mechanisms of the photoreaction processes. Fluorescent 2D photopattern with enhanced signal-to-background ratio was fabricated based on the controllable "turn-on" and "turn-off" photobehaviors in different states. The present study thus paves an easy yet efficient way to construct smart multiphotochromes for unique applications.
Pure organic materials with ultralong room-temperature phosphorescence (RTP) are attractive alternatives to inorganic phosphors. However, they generally show inefficient intersystem crossing (ISC) owing to weak spin-orbit coupling (SOC). A design principle based on the realization of small energy gap between the lowest singlet and triplet states (ΔE ) and pure ππ* configuration of the lowest triplet state (T ) via structural isomerism was used to obtain efficient and ultralong RTP materials. The meta isomer of carbazole-substituted methyl benzoate exhibits an ultralong lifetime of 795.0 ms with a quantum yield of 2.1 %. Study of the structure-property relationship shows that the varied steric and conjugation effects imposed by ester substituent at different positions are responsible for the small ΔE and pure ππ* configuration of T .
Limited therapeutic efficacy to hypoxic and refractory solid tumors has hindered the practical application of photodynamic therapy(PDT). Tw on ew benzothiophenylisoquinoline (btiq)-derived cyclometalated Ir III complexes, IrL1 and MitoIrL2,w ere constructed as potent photosensitizers, with the latter being designed for mitochondria accumulation. Both complexes demonstrated at ype IP DT process and caused photoinduced ferroptosis in tumor cells under hypoxia. This ferroptosis featured lipid peroxide accumulation, mitochondria shrinkage,d own-regulation of glutathione peroxidase 4(GPX4), and ferrostatin-1 (Fer-1)-inhibited cell death. Upon photoirradiation under hypoxia, mitochondria targeting MitoIrL2 caused mitochondria membrane potential (MMP) collapse,A TP production suppression, and induced cell apoptosis.T he synergetic effect of ferroptosis and apoptosis causes MitoIrL2 to outperform IrL1 in inhibiting the growth of MCF-7, PANC-1, MDA-MB-231 cells and multicellular spheroids.T his study demonstrates the first example of ferroptosis induced by photosensitizing Ir III complexes.Moreover,t he synergism of ferroptosis and apoptosis provides ap romising approach for combating hypoxics olid tumors through type IP DT processes.
The development of intelligent materials, in particular those showing the highly sensitive mechanoresponsive luminescence (MRL), is desirable but challenging. Here we report a design strategy for constructing high performance On–Off MRL materials by introducing nitrophenyl groups to molecules with aggregation-induced emission (AIE) characteristic. The on–off methodology employed is based on the control of the intersystem crossing (ISC) process. Experimental and theoretical investigations reveal that the nitrophenyl group effectively opens the nonradiative ISC channel to impart the high sensitivity and contrast On–Off behavior. On the other hand, the twisted AIE luminogen core endows enhanced reversibility and reduces the pressure required for the luminescence switching. Thin films can be readily fabricated from the designed materials to allow versatile applications in optical information recording and haptic sensing. The proposed design strategy thus provides a big step to expand the scope of the unique On–Off MRL family.
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