Polaron engineering promotes NIR-II absorption of carbon quantum dots for bioimaging and cancer therapy.

Recent years have witnessed a surge of interest in tuning the optical properties of organic semiconductors for diverse applications. However, achieving control over the optical bandgap in the second near-infrared (NIR-II) window has remained a major challenge. To address this, here we report a polaron engineering strategy that introduces diverse defects into carbon quantum dots (CQDs). These defects induce lattice distortions resulting in the formation of polarons, which can absorb the near-field scattered light. Furthermore, the formed polarons in N-related vacancies can generate thermal energy through the coupling of lattice vibrations, while the portion associated with O-related defects can return to the ground state in the form of NIR-II fluorescence. On the basis of this optical absorption model, these CQDs have been successfully applied to NIR-II fluorescence imaging and photothermal therapy. This discovery could open a promising route for the polarons of organic semiconductor materials as NIR-II absorbers in nanomedical applications.

Polylysine-modified near-infrared-emitting carbon dots assemblies: Amplification of tumor accumulation for enhanced tumor photothermal therapy.

A key challenge to enhance the therapeutic outcome of photothermal therapy (PTT) is to improve the efficiency of passive targeted accumulation of photothermal agents at tumor sites. Carbon dots (CDs) are an ideal choice for application as photothermal agents because of their advantages such as adjustable fluorescence, high photothermal conversion efficiency, and excellent biocompatibility. Here, we synthesized polylysine-modified near-infrared (NIR)-emitting CDs assemblies (plys-CDs) through post-solvothermal reaction of NIR-emitting CDs with polylysine. The encapsulated structure of plys-CDs was confirmed by determining morphological, chemical, and luminescent properties. The particle size of CDs increased to approximately 40 ± 8 nm after polylysine modification and was within the size range appropriate for achieving superior enhanced permeability and retention effect. Plys-CDs maintained a high photothermal conversion efficiency of 54.9 %, coupled with increased tumor site accumulation, leading to a high efficacy in tumor PTT. Thus, plys-CDs have a great potential for application in photothermal ablation therapy of tumors.

Achieving Near-Unity Red Light Photoluminescence in Antimony Halide Crystals via Polyhedron Regulation.

Exploration of efficient red emitting antimony hybrid halide with large Stokes shift and zero self-absorption is highly desirable due to its enormous potential for applications in solid light emitting, and active optical waveguides. However, it is still challenging and rarely reported. Herein, a series of (TMS)2SbCl5 (TMS=triphenylsulfonium cation) crystals have been prepared with diverse [SbCl5]2- configurations and distinctive emission color. Among them, cubic-phase (TMS)2SbCl5 shows bright red emission with a large Stokes shift of 312 nm. In contrast, monoclinic and orthorhombic (TMS)2SbCl5 crystals deliver efficient yellow and orange emission, respectively. Comprehensive structural investigations reveal that larger Stokes shift and longer-wavelength emission of cubic (TMS)2SbCl5 can be attributed to the larger lattice volume and longer Sb⋅⋅⋅Sb distance, which favor sufficient structural aberration freedom at excited states. Together with robust stability, (TMS)2SbCl5 crystal family has been applied as optical waveguide with ultralow loss coefficient of 3.67 ⋅ 10-4 dB µm-1, and shows superior performance in white-light emission and anti-counterfeiting. In short, our study provides a novel and fundamental perspective to structure-property-application relationship of antimony hybrid halides, which will contribute to future rational design of high-performance emissive metal halides.

New insight into identifying sediment phosphorus sources in multi-source polluted urban river: Effect of environmental-induced microbial community succession on stability of microbial source tracking results.

Identifying sediment phosphorus sources, the key to control eutrophication, is hindered in multi-source polluted urban rivers by the lack of appropriate methods and data resolution. Community-based microbial source tracking (MST) offers new insight, but the bacterial communities could be affected by environmental fluctuations during the migration with sediments, which might induce instability of MST results. Therefore, the effects of environmental-induced community succession on the stability of MST were compared in this study. Liangxi River, a highly eutrophic urban river, was selected as the study area where sediment phosphorus sources are difficult to track because of multi-source pollution and complicated hydrodynamic conditions. Spearman correlation analysis (P < 0.05) was conducted to recognize a close relationship between sediment, bacterial communities and phosphorus, verifying the feasibility of MST for identify sediment phosphorus sources. Two distinct microbial community fingerprints were constructed based on whether excluded 113 vulnerable species, which were identified by analyzing the differences of microorganisms across a concentration gradient of exogenous phosphorus input in microbial environmental response experiment. Because of the lower unknown proportion and relative standard deviations, MST results were more stable and reliable when based on the fingerprints excluding species vulnerable to phosphorus. This study presents a novel insight on how to identify sediment phosphorus sources in multi-source polluted urban river, and would help to develop preferential control strategies for eutrophication management.

Unveiling novel perspectives on niche differentiation and plasticity in rhizosphere phosphorus forms of submerged macrophytes with different stoichiometric homeostasis.

Stoichiometric homeostasis is the ability of organisms to maintain their element composition through various physiological mechanisms, regardless of changes in nutrient availability. Phosphorus (P) is a critical limiting element for eutrophication. Submerged macrophytes with different stoichiometric homeostasis regulated sediment P pollution by nutrient resorption, but whether and how P homeostasis and resorption in submerged macrophytes changed under variable plant community structure was unclear. Increasing evidence suggests that rhizosphere microbes drive niche overlap and differentiation for different P forms to constitute submerged macrophyte community structure. However, a greater understanding of how this occurs is required. This study examined the process underlying the metabolism of different rhizosphere P forms of submerged macrophytes under different cultivation patterns by analyzing physicochemical data, basic plant traits, microbial communities, and transcriptomics. The results indicate that alkaline phosphatase serves as a key factor in revealing the existence of a link between plant traits (path coefficient = 0.335, p < 0.05) and interactions with rhizosphere microbial communities (average path coefficient = 0.362, p < 0.05). Moreover, this study demonstrates that microbial communities further influence the niche plasticity of P by mediating plant root P metabolism genes (path coefficient = 0.354, p < 0.05) and rhizosphere microbial phosphorus storage (average path coefficient = 0.605, p < 0.01). This research not only contributes to a deeper comprehension of stoichiometric homeostasis and nutrient dynamics but also provides valuable insights into potential strategies for managing and restoring submerged macrophyte-dominated ecosystems in the face of changing nutrient conditions.

Coupling of static ultramicromagnetic field with elastic micropillar-structured substrate for cell response.

Micropillars have emerged as promising tools for a wide range of biological applications, while the influence of magnetic fields on cell behavior regulation has been increasingly recognized. However, the combined effect of micropillars and magnetic fields on cell behaviors remains poorly understood. In this study, we investigated the responses of H9c2 cells to ultramicromagnetic micropillar arrays using NdFeB as the tuned magnetic particles. We conducted a comparative analysis between PDMS micropillars and NdFeB/PDMS micropillars to assess their impact on cell function. Our results revealed that H9c2 cells exhibited significantly enhanced proliferation and notable cytoskeletal rearrangements on the ultramicromagnetic micropillars, surpassing the effects observed with pure PDMS micropillars. Immunostaining further indicated that cells cultured on ultramicromagnetic micropillars displayed heightened contractility compared to those on PDMS micropillars. Remarkably, the ultramicromagnetic micropillars also demonstrated the ability to decrease reactive oxygen species (ROS) levels, thereby preventing F-actin degeneration. Consequently, this study introduces ultramicromagnetic micropillars as a novel tool for the regulation and detection of cell behaviors, thus paving the way for advanced investigations in tissue engineering, single-cell analysis, and the development of flexible sensors for cellular-level studies.

Applications of flexible electronics related to cardiocerebral vascular system.

Ensuring accessible and high-quality healthcare worldwide requires field-deployable and affordable clinical diagnostic tools with high performance. In recent years, flexible electronics with wearable and implantable capabilities have garnered significant attention from researchers, which functioned as vital clinical diagnostic-assisted tools by real-time signal transmission from interested targets in vivo. As the most crucial and complex system of human body, cardiocerebral vascular system together with heart-brain network attracts researchers inputting profuse and indefatigable efforts on proper flexible electronics design and materials selection, trying to overcome the impassable gulf between vivid organisms and rigid inorganic units. This article reviews recent breakthroughs in flexible electronics specifically applied to cardiocerebral vascular system and heart-brain network. Relevant sensor types and working principles, electronics materials selection and treatment methods are expounded. Applications of flexible electronics related to these interested organs and systems are specially highlighted. Through precedent great working studies, we conclude their merits and point out some limitations in this emerging field, thus will help to pave the way for revolutionary flexible electronics and diagnosis assisted tools development.

Flexible, Transparent, and Wafer-Scale Artificial Synapse Array Based on TiOx /Ti3 C2 Tx Film for Neuromorphic Computing.

A high-density neuromorphic computing memristor array based on 2D materials paves the way for next-generation information-processing components and in-memory computing systems. However, the traditional 2D-materials-based memristor devices suffer from poor flexibility and opacity, which hinders the application of memristors in flexible electronics. Here, a flexible artificial synapse array based on TiOx /Ti3 C2 Tx film is fabricated by a convenient and energy-efficient solution-processing technique, which realizes high transmittance (≈90%) and oxidation resistance (>30 days). The TiOx /Ti3 C2 Tx memristor shows low device-to-device variability, long memory retention and endurance, a high ON/OFF ratio, and fundamental synaptic behavior. Furthermore, satisfactory flexibility (R = 1.0 mm) and mechanical endurance (104 bending cycles) of the TiOx /Ti3 C2 Tx memristor are achieved, which is superior to other film memristors prepared by chemical vapor deposition. In addition, high-precision (>96.44%) MNIST handwritten digits recognition classification simulation indicates that the TiOx /Ti3 C2 Tx artificial synapse array holds promise for future neuromorphic computing applications, and provides excellent high-density neuron circuits for new flexible intelligent electronic equipment.

Constructing Oxygen-Related Defects in Carbon Nanodots with Janus Optical Properties: Noninvasive NIR Fluorescent Imaging and Effective Photocatalytic Therapy.

Noninvasive fluorescence (FL) imaging and high-performance photocatalytic therapy (PCT) are opposing optical properties that are difficult to combine in a single material system. Herein, a facile approach to introducing oxygen-related defects in carbon dots (CDs) via post-oxidation with 2-iodoxybenzoic acid is reported, in which some nitrogen atoms are substituted by oxygen atoms. Unpaired electrons in these oxygen-related defects rearrange the electronic structure of the oxidized CDs (ox-CDs), resulting in an emerging near-infrared (NIR) absorption band. These defects not only contribute to enhanced NIR bandgap emission but also act as trappers for photoexcited electrons to promote efficient charge separation on the surface, leading to abundant photo-generated holes on the ox-CDs surface under visible-light irradiation. Under white LED torch irradiation, the photo-generated holes oxidize hydroxide to hydroxyl radicals in the acidification of the aqueous solution. In contrast, no hydroxyl radicals are detected in the ox-CDs aqueous solution under 730 nm laser irradiation, indicating noninvasive NIR FL imaging potential. Utilizing the Janus optical properties of the ox-CDs, the in vivo NIR FL imaging of sentinel lymph nodes around tumors and efficient photothermal enhanced tumor PCT are demonstrated.

Feature ghost imaging for color identification.

On the basis of computational ghost imaging (CGI), we present a new imaging technique, feature ghost imaging (FGI), which can convert the color information into distinguishable edge features in retrieved grayscale images. With the edge features extracted by different order operators, FGI can obtain the shape and the color information of objects simultaneously in a single-round detection using one single-pixel detector. The feature distinction of rainbow colors is presented in numerical simulations and the verification of FGI's practical performance is conducted in experiments. Furnishing a new perspective to the imaging of colored objects, our FGI extends the function and the application fields of traditional CGI while sustaining the simplicity of the experimental setup.

Visible-light-induced strong oxidation capacity of metal-free carbon nanodots through photo-induced surface reduction for photocatalytic antibacterial and tumor therapy.

Biocompatible metal-free carbon dots (CDs) with good photo-induced strong oxidation capacity in aqueous solutions are scarce for high-performance photocatalytic antibacterial and tumor therapy. In this work, we achieved effective visible light-induced cell death and antibacterial performance based on biocompatible metal-free CDs. The visible-light-induced reducing ability of the surface electron-withdrawing structure of the CDs allowed for the remaining photo-induced holes with high oxidation capacity to oxidize water molecules and generate hydroxyl radicals. Antibiotic-resistant bacteria were effectively inhibited by the CDs under xenon lamp irradiation with 450 nm long pass filter. Moreover, CD-based tumor photocatalytic therapy in mice was achieved using a xenon lamp with 450 nm long pass filter (0.3 W cm-2).

L-Arginine-Functionalized Carbon Dots with Enhanced Red Emission and Upregulated Intracellular L-Arginine Intake for Obesity Inhibition.

Obesity is a major global health problem that significantly increases the risk of many other diseases. Herein, a facile method of suppressing lipogenesis and obesity using L-arginine-functionalized carbon dots (L-Arg@CDots) is reported. The prepared CDots with a negative surface charge form stronger bonds than D-arginine and lysine with L-Arg in water. The L-Arg@CDots in the aqueous solution offer a high photoluminescence quantum yield of 23.6% in the red wavelength region. The proposed L-Arg functionalization strategy not only protects the red emission of the CDots from quenching by water molecules but also enhances the intracellular uptake of L-Arg to reduce lipogenesis. Injection of L-Arg@CDots can reduce the body weight increase in ob/ob mice by suppressing their food intake and shrinking the white adipose tissue cells, thereby significantly inhibiting obesity.

Assignment of Core and Surface States in Multicolor-Emissive Carbon Dots.

It is important to reveal the luminescence mechanisms of carbon dots (CDs). Herein, CDs with two types of optical centers are synthesized from citric acid in formamide by a solvothermal method, and show high photoluminescence quantum yield reaching 42%. Their green/yellow emission exhibits pronounced vibrational structure and high resistance toward photobleaching, while broad red photoluminescence is sensitive to solvents, temperature, and UV-IR. Under UV-IR, the red emission is gradually bleached due to the photoinduced dehydration of the deprotonated surface of CDs in dimethyl sulfoxide, while this process is hindered in water. From the analysis of steady-state and time-resolved photoluminescence and transient absorption data together with density functional theory calculations, the green/ yellow emission is assigned to conjugated sp2 -domains (core state) similar to organic dye derivatives stacked within disk-shaped CDs; and the broad red emission-to oxygen-containing groups bound to sp2 -domains (surface state), whereas energy transfer from the core to the surface state can happen.

Computing Shor's algorithmic steps with interference patterns of classical light.

When considered as orthogonal bases in distinct vector spaces, the unit vectors of polarization directions and the Laguerre-Gaussian modes of polarization amplitude are inseparable, constituting a so-called classical entangled light beam. Equating this classical entanglement to quantum entanglement necessary for computing purpose, we show that the parallelism featured in Shor's factoring algorithm is equivalent to the concurrent light-path propagation of an entangled beam or pulse train. A gedanken experiment is proposed for executing the key algorithmic steps of modular exponentiation and Fourier transform on a target integer N using only classical manipulations on the amplitudes and polarization directions. The multiplicative order associated with the sought-after integer factors is identified through a four-hole diffraction interference from sources obtained from the entangled beam profile. The unique mapping from the fringe patterns to the computed order is demonstrated through simulations for the case [Formula: see text].

Photocatalytic Pt(IV)-Coordinated Carbon Dots for Precision Tumor Therapy.

Rapid, efficient, and precise cancer therapy is highly desired. Here, this work reports solvothermally synthesized photoactivatable Pt(IV)-coordinated carbon dots (Pt-CDs) and their bovine serum albumin (BSA) complex (Pt-CDs@BSA) as a novel orange light-triggered anti-tumor therapeutic agent. The homogeneously distributed Pt(IV) in the Pt-CDs (Pt: 17.2 wt%) and their carbon cores with significant visible absorption exhibit excellent photocatalytic properties, which not only efficiently releases cytotoxic Pt(II) species but also promotes hydroxy radical generation from water under orange light. When triggered with a 589 nm laser, Pt-CDs@BSA possesses the ultrastrong cancer cell killing capacities of intracellular Pt(II) species release, hydroxyl radical generation, and acidification, which induce powerful immunogenic cell death. Activation of Pt-CDs@BSA by a single treatment with a 589 nm laser effectively eliminated the primary tumor and inhibited distant tumor growth and lung metastasis. This study thus presents a new concept for building photoactivatable Pt(IV)-enriched nanodrug-based CDs for precision cancer therapy.

Single-pixel imaging with Gao-Boole patterns.

Single-pixel imaging (SPI) can perceive the world using only a single-pixel detector, but long sampling times with a series of patterns are inevitable for SPI, which is the bottleneck for its practical application. Developing new patterns to reduce the sampling times might provide opportunities to address this challenge. Based on the Kronecker product of Hadamard matrix, we here design a complete set of new patterns, called Gao-Boole patterns, for SPI. Compared to orthogonal Hadamard basis patterns with elements valued as +1 or -1, our Gao-Boole patterns are non-orthogonal ones and the element values are designed as +1 or 0. Using our Gao-Boole patterns, the reconstructed quality of a target image (N × N pixels) is as high as the Hadamard one but only with half pattern numbers of the Hadamard ones, for both full sampling (N2 for Gao-Boole patterns, 2N2 for Hadamard basis patterns) and undersampling cases in experiment. Effectively reducing the patterns numbers and sampling times without sacrificing imaging quality, our designed Gao-Boole patterns provide a superior option for structural patterns in SPI and help to steer SPI toward practical imaging application.

Extraordinarily Stable Aqueous Electrochromic Battery Based on Li4Ti5O12 and Hybrid Al3+/Zn2+ Electrolyte.

Aqueous electrochromic battery (ECB) is a multifunctional technology that shows great potential in various applications including energy-saving buildings and wearable batteries with visible energy levels. However, owing to the mismatch between traditional electrochromic materials and the electrolyte, aqueous ECBs generally exhibit poor cycling stability which bottlenecks their practical commercialization. Herein, we present an ultrastable electrochromic system composed of lithium titanate (Li4Ti5O12, LTO) electrode and Al3+/Zn2+ hybrid electrolyte. The fully compatible system exhibits excellent redox reaction reversibility, thus leading to extremely high cycling stabilities in optical contrast (12 500 cycles with unnoticeable degradation) and energy storage (4000 cycles with 82.6% retention of capacity), superior electrochromic performances including high optical contrast (∼74.73%) and fast responses (4.35 s/7.65 s for bleaching/coloring), as well as excellent discharge areal capacity of 151.94 mAh m-2. The extraordinary cycling stability can be attributed to the robust [TiO6] octahedral frameworks which remain chemically active even upon the gradual substitution of Li+ with Al3+ in LTO over multiple operation cycles. The high-performance electrochromic system demonstrated here not only makes the commercialization of low-cost, high-safety aqueous-based electrochromic devices possible but also provides potential design guidance for LTO-related materials used in aqueous-based energy storage devices.

Tuning colour centres at a twisted hexagonal boron nitride interface.

The colour centre platform holds promise for quantum technologies, and hexagonal boron nitride has attracted attention due to the high brightness and stability, optically addressable spin states and wide wavelength coverage discovered in its emitters. However, its application is hindered by the typically random defect distribution and complex mesoscopic environment. Here, employing cathodoluminescence, we demonstrate on-demand activation and control of colour centre emission at the twisted interface of two hexagonal boron nitride flakes. Further, we show that colour centre emission brightness can be enhanced by two orders of magnitude by tuning the twist angle. Additionally, by applying an external voltage, nearly 100% brightness modulation is achieved. Our ab initio GW and GW plus Bethe-Salpeter equation calculations suggest that the emission is correlated to nitrogen vacancies and that a twist-induced moiré potential facilitates electron-hole recombination. This mechanism is further exploited to draw nanoscale colour centre patterns using electron beams.

Toward Strong Near-Infrared Absorption/Emission from Carbon Dots in Aqueous Media through Solvothermal Fusion of Large Conjugated Perylene Derivatives with Post-Surface Engineering.

Carbon dots (CDs) have attracted significant interest as one of the most emerging photoluminescence (PL) nanomaterials. However, the realization of CDs with dominant near-infrared (NIR) absorption/emission peaks in aqueous solution remains a great challenge. Herein, CDs with both main NIR absorption bands at 720 nm and NIR emission bands at 745 nm in an aqueous solution are fabricated for the first time by fusing large conjugated perylene derivatives under solvothermal treatment. With post-surface engineering, the polyethyleneimine modified CDs (PEI-CDs) exhibit enhanced PL quantum yields (PLQY) up to 8.3% and 18.8% in bovine serum albumin aqueous and DMF solutions, which is the highest PLQY of CDs in NIR region under NIR excitation. Density functional theory calculations support the strategy of fusing large conjugated perylene derivatives to achieve NIR emissions from CDs. Compared to the commercial NIR dye Indocyanine green, PEI-CDs exhibit excellent photostability and much lower cost. Furthermore, the obtained PEI-CDs illustrate the advantages of remarkable two-photon NIR angiography and in vivo NIR fluorescence bioimaging. This work demonstrates a promising strategy of fusing large conjugated molecules for preparing CDs with strong NIR absorption/emission to promote their bioimaging applications.

Bridging the Interfacial Contact for Improved Stability and Efficiency of Inverted Perovskite Solar Cells.

Inverted perovskite solar cells (PSCs) have received widespread attention due to their facile fabrication and wide applications. However, their power conversion efficiency (PCE) is reported lower than that of regular PSCs because of the undesirable interfacial contact between perovskite and the hydrophobic hole transport layer (HTL). Here, an interface regulation strategy is proposed to overcome this limitation. A small molecule ([2-(9H-carbazol-9-yl) ethyl] phosphonic acid, abbreviated as 2P), composed of carbazole and phosphonic acid groups, is inserted between perovskite and HTL. Morphological characterization and theoretical calculation reveal that perovskite bonds stronger on 2P-modified HTL than on pristine HTL. The improved interfacial contact facilitates hole extraction and retards degradation. Upon the incorporation of 2P, inverted PSCs deliver a high PCE of over 22% with superior stability, keeping 84.6% of initial efficiency after 7200 h storage under an ambient atmosphere with a relative humidity of ≈30-40%. This strategy provides a simple and efficient way to boost the performance of inverted PSCs.