Temporal compressive edge imaging enabled by a lensless diffuser camera.

Lensless imagers based on diffusers or encoding masks enable high-dimensional imaging from a single-shot measurement and have been applied in various applications. However, to further extract image information such as edge detection, conventional post-processing filtering operations are needed after the reconstruction of the original object images in the diffuser imaging systems. Here, we present the concept of a temporal compressive edge detection method based on a lensless diffuser camera, which can directly recover a time sequence of edge images of a moving object from a single-shot measurement, without further post-processing steps. Our approach provides higher image quality during edge detection, compared with the "conventional post-processing method." We demonstrate the effectiveness of this approach by both numerical simulation and experiments. The proof-of-concept approach can be further developed with other image post-processing operations or versatile computer vision assignments toward task-oriented intelligent lensless imaging systems.

Large-Area Near-Infrared Emission Enhancement on Single Upconversion Nanoparticles by Metal Nanohole Array.

Single lanthanide (Ln) ion doped upconversion nanoparticles (UCNPs) exhibit great potential for biomolecule sensing and counting. Plasmonic structures can improve the emission efficiency of single UCNPs by modulating the energy transferring process. Yet, achieving robust and large-area single UCNP emission modulation remains a challenge, which obstructs investigation and application of single UCNPs. Here, we present a strategy using metal nanohole arrays (NHAs) to achieve energy-transfer modulation on single UCNPs simultaneously within large-area plasmonic structures. By coupling surface plasmon polaritons (SPPs) with higher-intermediate state (1D2 → 3F3, 1D2 → 3H4) transitions, we achieved a remarkable up to 10-fold enhancement in 800 nm emission, surpassing the conventional approach of coupling SPPs with an intermediate ground state (3H4 → 3H6). We numerically simulate the electrical field distribution and reveal that luminescent enhancement is robust and insensitive to the exact location of particles. It is anticipated that the strategy provides a platform for widely exploring applications in single-particle quantitative biosensing.

Optical Nonlinearity Enabled Super-Resolved Multiplexing Microscopy.

Optical multiplexing for nanoscale object recognition is of great significance within the intricate domains of biology, medicine, anti-counterfeiting, and microscopic imaging. Traditionally, the multiplexing dimensions of nanoscopy are limited to emission intensity, color, lifetime, and polarization. Here, a novel dimension, optical nonlinearity, is proposed for super-resolved multiplexing microscopy. This optical nonlinearity is attributable to the energy transitions between multiple energy levels of the doped lanthanide ions in upconversion nanoparticles (UCNPs), resulting in unique optical fingerprints for UCNPs with different compositions. A vortex beam is applied to transport the optical nonlinearity onto the imaging point-spread function (PSF), creating a robust super-resolved multiplexing imaging strategy for differentiating UCNPs with distinctive optical nonlinearities. The composition information of the nanoparticles can be retrieved with variations of the corresponding PSF in the obtained image. Four channels multiplexing super-resolved imaging with a single scanning, applying emission color and nonlinearity of two orthogonal imaging dimensions with a spatial resolution higher than 150 nm (1/6.5λ), are demonstrated. This work provides a new and orthogonal dimension - optical nonlinearity - to existing multiplexing dimensions, which shows great potential in bioimaging, anti-counterfeiting, microarray assays, deep tissue multiplexing detection, and high-density data storage.

Multi-functional dual-path self-aligned polarization interference lithography.

Manufacturing sharp features is one of the most desired requirements for lithography. Here, we demonstrate a dual-path self-aligned polarization interference lithography (Dp-SAP IL) for fabricating periodic nanostructures, featuring high-steepness and high-uniformization. Meanwhile, it can manufacture quasicrystals with adjustable rotation symmetry. We reveal the change of the non-orthogonality degree under different polarization states and incident angles. We find that incident light's transverse electric (TE) wave results in high interference contrast at arbitrary incident angles, with a minimum contrast of 0.9328, that is, realizing the self-alignment of the polarization state of incident light and reflected light. We experimentally demonstrate this approach by fabricating a series of diffraction gratings with periods ranging from 238.3 nm to 851.6 nm. The steepness of each grating is greater than 85 degrees. Different from the traditional interference lithography system, Dp-SAP IL realizes a structure color using two mutually perpendicular and non-interference paths. One path is for the photolithography of patterns onto the sample, and the other path is for generating nanostructures on the patterns. Our technique showcases the feasibility of obtaining high contrast interference fringes by simply tuning the polarization, with the potential for cost-effective manufacturing of nanostructures such as quasicrystals and structure color.

Dual-mode adaptive-SVD ghost imaging.

In this paper, we present a dual-mode adaptive singular value decomposition ghost imaging (A-SVD GI), which can be easily switched between the modes of imaging and edge detection. It can adaptively localize the foreground pixels via a threshold selection method. Then only the foreground region is illuminated by the singular value decomposition (SVD) - based patterns, consequently retrieving high-quality images with fewer sampling ratios. By changing the selecting range of foreground pixels, the A-SVD GI can be switched to the mode of edge detection to directly reveal the edge of objects, without needing the original image. We investigate the performance of these two modes through both numerical simulations and experiments. We also develop a single-round scheme to halve measurement numbers in experiments, instead of separately illuminating positive and negative patterns in traditional methods. The binarized SVD patterns, generated by the spatial dithering method, are modulated by a digital micromirror device (DMD) to speed up the data acquisition. This dual-mode A-SVD GI can be applied in various applications, such as remote sensing or target recognition, and could be further extended for multi-modality functional imaging/detection.

Controllable Preparation of Superparamagnetic Fe3O4@La(OH)3 Inorganic Polymer for Rapid Adsorption and Separation of Phosphate.

Superparamagnetic Fe3O4 particles have been synthesized by solvothermal method, and a layer of dense silica sol polymer is coated on the surface prepared by sol-gel technique; then La(OH)3 covered the surface of silica sol polymer in an irregular shape by controlled in situ growth technology. These magnetic materials are characterized by TEM, FT-IR, XRD, SEM, EDS and VSM; the results show that La(OH)3 nanoparticles have successfully modified on Fe3O4 surface. The prepared Fe3O4@La(OH)3 inorganic polymer has been used as adsorbent to remove phosphate efficiently. The effects of solution pH, adsorbent dosage and co-existing ions on phosphate removal are investigated. Moreover, the adsorption kinetic equation and isothermal model are used to describe the adsorption performance of Fe3O4@La(OH)3. It was observed that Fe3O4@La(OH)3 exhibits a fast equilibrium time of 20 min, high phosphate removal rate (>95.7%), high sorption capacity of 63.72 mgP/g, excellent selectivity for phosphate in the presence of competing ions, under the conditions of phosphate concentration 30 mgP/L, pH = 7, adsorbent dose 0.6 g/L and room temperature. The phosphate adsorption process by Fe3O4@La(OH)3 is best described by the pseudo-second-order equation and Langmuir isotherm model. Furthermore, the real samples and reusability experiment indicate that Fe3O4@La(OH)3 could be regenerated after desorption, and 92.78% phosphate removing remained after five cycles. Therefore, La(OH)3 nanoparticles deposited on the surface of monodisperse Fe3O4 microspheres have been synthesized for the first time by a controlled in-situ growth method. Experiments have proved that Fe3O4@La(OH)3 particles with fast separability, large adsorption capacity and easy reusability can be used as a promising material in the treatment of phosphate wastewater or organic pollutants containing phosphoric acid functional group.

Lanthanide Ion Resonance-Driven Rayleigh Scattering of Nanoparticles for Dual-Modality Interferometric Scattering Microscopy.

Light scattering from nanoparticles is significant in nanoscale imaging, photon confinement. and biosensing. However, engineering the scattering spectrum, traditionally by modifying the geometric feature of particles, requires synthesis and fabrication with nanometre accuracy. Here it is reported that doping lanthanide ions can engineer the scattering properties of low-refractive-index nanoparticles. When the excitation wavelength matches the ion resonance frequency of lanthanide ions, the polarizability and the resulted scattering cross-section of nanoparticles are dramatically enhanced. It is demonstrated that these purposely engineered nanoparticles can be used for interferometric scattering (iSCAT) microscopy. Conceptually, a dual-modality iSCAT microscopy is further developed to identify different nanoparticle types in living HeLa cells. The work provides insight into engineering the scattering features by doping elements in nanomaterials, further inspiring exploration of the geometry-independent scattering modulation strategy.

Exploiting Dynamic Nonlinearity in Upconversion Nanoparticles for Super-Resolution Imaging.

Single-beam super-resolution microscopy, also known as superlinear microscopy, exploits the nonlinear response of fluorescent probes in confocal microscopy. The technique requires no complex purpose-built system, light field modulation, or beam shaping. Here, we present a strategy to enhance this technique's spatial resolution by modulating excitation intensity during image acquisition. This modulation induces dynamic optical nonlinearity in upconversion nanoparticles (UCNPs), resulting in variations of nonlinear fluorescence response in the obtained images. The higher orders of fluorescence response can be extracted with a proposed weighted finite difference imaging algorithm from raw fluorescence images to generate an image with higher resolution than superlinear microscopy images. We apply this approach to resolve single nanoparticles in a large area, improving the resolution to 132 nm. This work suggests a new scope for the development of dynamic nonlinear fluorescent probes in super-resolution nanoscopy.

Experimental Study on Microbial Induced Calcium Carbonate Precipitation to Enhance Reservoir Recovery.

Background: Bacillus subtilis can produce urease in the presence of urea as the main carbon source and induce mineralization in the presence of precipitable cations. Objectives: The objective of our study was to demonstrate that Bacillus subtilis catabolizes glucose first in the presence of both glucose and urea carbon sources. Using its feature of catabolizing glucose first to delay the mineralization time, it proved its potential application in enhancing the recovery of heterogeneous reservoirs. Material and Methods: The metabolic process of Bacillus subtilis was monitored by changing the glucose content in the bacterial medium by UV spectrophotometer and pH meter. Using a non-homogeneous physical model, experiments were conducted to improve reservoir recovery by microbial mineralization after polymer oil drive. Results: The higher the glucose content in the medium, the longer the time for the pH of the bacterial solution to reach 7 and the longer the end of the logarithmic phase of growth. the glucose content of the 48 h medium was significantly correlated with the consumption of the bacteria and the quality of the precipitation. In the oil drive experiment the permeability of the high permeability model was reduced from 1200 md to 136 md with a reduction rate of 88.6 %, and the permeability of the low permeability model was reduced by 22 md, and the crude oil recovery was increased by 7.9 %. Conclusions: It was demonstrated that the addition of glucose to the culture medium retarded the mineralization of bacteria. Only 0.2 times the pore volume of the bacterial solution and the cementing solution is required to form an effective seal, thus improving the recovery of crude oil.

Research status and development of microbial induced calcium carbonate mineralization technology.

In nature, biomineralization is a common phenomenon, which can be further divided into authigenic and artificially induced mineralization. In recent years, artificially induced mineralization technology has been gradually extended to major engineering fields. Therefore, by elaborating the reaction mechanism and bacteria of mineralization process, and summarized various molecular dynamics equations involved in the mineralization process, including microbial and nutrient transport equations, microbial adsorption equations, growth equations, urea hydrolysis equations, and precipitation equations. Because of the environmental adaptation stage of microorganisms in sandy soil, their reaction rate in sandy soil environment is slower than that in solution environment, the influencing factors are more different, in general, including substrate concentration, temperature, pH, particle size and grouting method. Based on the characteristics of microbial mineralization such as strong cementation ability, fast, efficient, and easy to control, there are good prospects for application in sandy soil curing, building improvement, heavy metal fixation, oil reservoir dissection, and CO2 capture. Finally, it is discussed and summarized the problems and future development directions on the road of commercialization of microbial induced calcium carbonate precipitation technology from laboratory to field application.

Local photothermal/photodynamic synergistic antibacterial therapy based on two-dimensional BP@CQDs triggered by single NIR light source.

Pathogenic bacteria-infected wound healing faces challenges even though many advanced antibiotics and antibacterial nanoagents have been developed. Herein, we established a two-dimensional antibacterial nanoplatform with synergistic photothermal therapy (PTT) and photodynamic therapy (PDT) antibacterial capabilities mediated by a single 808 nm laser irradiation. The nanoplatform is constructed by combining black phosphorus (BP) obtained by liquid phase exfoliation and hydrothermally prepared tellurium-doped carbon quantum dots (CQDs) prepared by electrostatic interaction. As a result, the photothermal conversion of BP and hydroxyl radical (‧OH) production of CQDs under NIR laser makes the nanoplatform (BP@CQDs) possess an outstanding antibacterial performance against S. aureus and E. coli (as high as 92.7% and 98.4%, respectively), resulting in a faster wound closure ratio than another infected wound. Moreover, in vitro and in vivo researches showed that BP@CQDs have good hemocompatibility, cytocompatibility, and biocompatibility during the therapeutic process. This work demonstrates the broad application prospect of BP nanosheets in infectious microenvironments and develops a potential strategy for S. aureus-infected wound repair.

Dual enzyme-mimic nanozyme based on single-atom construction strategy for photothermal-augmented nanocatalytic therapy in the second near-infrared biowindow.

Nanozyme-based catalytic therapy, an emerging therapeutic pattern, has significantly incorporated in the advancement of tumor therapy by generating lethal reactive oxygen species. Nevertheless, most of the nanozymes have mono catalytic performances with H2O2 in the tumor microenvironment (TME), which lowers their therapeutic efficiency. Herein, we design a newly-developed single-atom Fe dispersed N-doped mesoporous carbon nanospheres (SAFe-NMCNs) nanozyme with high H2O2 affinity for photothermal-augmented nanocatalytic therapy. The SAFe-NMCNs nanozyme possesses dual enzyme-mimic catalytic activity which not only acts as a catalase-mimic role to achieve ultrasonic imaging in tumor site by O2 generation, but also exhibits the superior peroxidase-mimic catalytic performance to generate •OH for nanocatalytic therapy. Besides, the SAFe-NMCNs nanozyme with strong optical absorption in the second near-infrared (NIR-II) region shows excellent photothermal conversion performance. The peroxidase-mimic catalytic process of SAFe-NMCNs nanozyme is realized using density functional theory (DFT). Both in vitro and in vivo results indicate that the SAFe-NMCNs nanozyme can efficiently suppress tumor cells growth by a synergistic therapy effect with photothermal-augmented nanocatalytic therapy. The work developed a single-atom-coordinated nanozyme with dual-enzyme catalytic performance and achieve hyperthermia-augmented nanocatalytic therapy effect, can open a window for potential biological applications.

Optical Fingerprint Classification of Single Upconversion Nanoparticles by Deep Learning.

Highly controlled synthesis of upconversion nanoparticles (UCNPs) can be achieved in the heterogeneous design, so that a library of optical properties can be arbitrarily produced by depositing multiple lanthanide ions. Such a control offers the potential in creating nanoscale barcodes carrying high-capacity information. With the increasing creation of optical information, it poses more challenges in decoding them in an accurate, high-throughput, and speedy fashion. Here, we reported that the deep-learning approach can recognize the complexity of the optical fingerprints from different UCNPs. Under a wide-field microscope, the lifetime profiles of hundreds of single nanoparticles can be collected at once, which offers a sufficient amount of data to develop deep-learning algorithms. We demonstrated that high accuracies of over 90% can be achieved in classifying 14 kinds of UCNPs. This work suggests new opportunities in handling the diverse properties of nanoscale optical barcodes toward the establishment of vast luminescent information carriers.

Preselectable Optical Fingerprints of Heterogeneous Upconversion Nanoparticles.

The control in optical uniformity of single nanoparticles and tuning their diversity in multiple dimensions, dot to dot, holds the key to unlocking nanoscale applications. Here we report that the entire lifetime profile of the single upconversion nanoparticle (τ2 profile) can be resolved by confocal, wide-field, and super-resolution microscopy techniques. The advances in both spatial and temporal resolutions push the limit of optical multiplexing from microscale to nanoscale. We further demonstrate that the time-domain optical fingerprints can be created by utilizing nanophotonic upconversion schemes, including interfacial energy migration, concentration dependency, energy transfer, and isolation of surface quenchers. We exemplify that three multiple dimensions, including the excitation wavelength, emission color, and τ2 profile, can be built into the nanoscale derivative τ2-dots. Creating a vast library of individually preselectable nanotags opens up a new horizon for diverse applications, spanning from sub-diffraction-limit data storage to high-throughput single-molecule digital assays and super-resolution imaging.

Heterochromatic Nonlinear Optical Responses in Upconversion Nanoparticles for Super-Resolution Nanoscopy.

Point spread function (PSF) engineering by an emitter's response can code higher-spatial-frequency information of an image for microscopy to achieve super-resolution. However, complexed excitation optics or repetitive scans are needed, which explains the issues of low speed, poor stability, and operational complexity associated with the current laser scanning microscopy approaches. Here, the diverse emission responses of upconversion nanoparticles (UCNPs) are reported for super-resolution nanoscopy to improve the imaging quality and speed. The method only needs a doughnut-shaped scanning excitation beam at an appropriate power density. By collecting the four-photon emission of single UCNPs, the high-frequency information of a super-resolution image can be resolved through the doughnut-emission PSF. Meanwhile, the two-photon state of the same nanoparticle is oversaturated, so that the complementary lower-frequency information of the super-resolution image can be simultaneously collected by the Gaussian-like emission PSF. This leads to a method of Fourier-domain heterochromatic fusion, which allows the extended capability of the engineered PSFs to cover both low- and high-frequency information to yield optimized image quality. This approach achieves a spatial resolution of 40 nm, 1/24th of the excitation wavelength. This work suggests a new scope for developing nonlinear multi-color emitting probes in super-resolution nanoscopy.

Tumor Microenvironment-Activatable Cyclic Cascade Reaction to Reinforce Multimodal Combination Therapy by Destroying the Extracellular Matrix.

The optimal therapy effect of tumors is frequently restricted by the dense extracellular matrix (ECM) and anoxia. Herein, an intelligent BPNs-Arg-GOx@MnO2 (BAGM) nanozyme is innovatively designed as a multimodal synergistic therapeutic paradigm that possesses both nitric oxide (NO) self-supplying and ECM degradation properties to reinforce the therapy effect by a tumor microenvironment (TME)-activatable cyclic cascade catalytic reaction. This theranostic nanoplatform is constructed by using polyethyleneimine-modified black phosphorus nanosheets as a "fishnet" to attach l-Arginine (l-Arg) and glucose oxidase (GOx) and then depositing mini-sized MnO2 nanosheets (MNs) on the surface by a facile situ biomineralization method. As an intelligent "switch", the MNs can effectively trigger the cascade reaction by disintegrating intracellular H2O2 to release O2. Then, the conjugated GOx can utilize O2 production to catalyze intracellular glucose to generate H2O2, which not only starves the tumor cells but also promotes oxidation of l-Arg to NO. Thereafter, matrix metalloproteinases will be activated by NO production to degrade the dense ECM and transform matrix collagen into a loose state. In turn, a loose ECM can enhance the accumulation of the BAGM nanozyme and thereby reinforce synergistic photothermal therapy/starvation therapy/NO gas therapy. Both in vitro and in vivo results indicate that the TME-tunable BAGM therapeutic nanoplatform with cascade anticancer property and satisfactory biosecurity shows potential in nanomedicine.

Multiplexed structured illumination super-resolution imaging with lifetime-engineered upconversion nanoparticles.

The emerging optical multiplexing within nanoscale shows super-capacity in encoding information by using lifetime fingerprints from luminescent nanoparticles. However, the optical diffraction limit compromises the decoding accuracy and throughput of the nanoparticles during conventional widefield imaging. This, in turn, challenges the quality of nanoparticles to afford the modulated excitation condition and further retain the multiplexed optical fingerprints for super-resolution multiplexing. Here we report a tailor-made multiplexed super-resolution imaging method using the lifetime-engineered upconversion nanoparticles. We demonstrate that the nanoparticles are bright, uniform, and stable under structured illumination, which supports a lateral resolution of 185 nm, less than 1/4th of the excitation wavelength. We further develop a deep learning algorithm to coordinate with super-resolution images for more accurate decoding compared to a numeric algorithm. We demonstrate a three-channel super-resolution imaging based optical multiplexing with decoding accuracies above 93% for each channel and larger than 60% accuracy for potential seven-channel multiplexing. The improved resolution provides high throughput by resolving the particles within the diffraction-limited spots, which enables higher multiplexing capacity in space. This lifetime multiplexing super-resolution method opens a new horizon for handling the growing amount of information content, disease source, and security risk in modern society.

Influence of Non-Structural Parameters on Dual Parallel Jet Characteristics of Porous Nozzles.

As an important actuator of the dual parallel jet, the porous nozzle has some non-structural parameters (such as inlet pressure, nozzle spacing ratio, etc.) which have a significant influence on energy transport, chemical combustion and pollutant generation. The research on the microfluidic state of the porous nozzle dual parallel jet, however, remains insufficient because of its microjet pattern and complex intersection process. In this paper, the authors used numerical simulation and an experimental method to clarify the influence of porous nozzles' non-structural parameters on dual parallel jet characteristics. The results show that the inlet pressure only changes the pressure peak value on the parallel jet axis; the starting point (SP) and peak point (PP) on the parallel jet axis, which are located at Xsp = 22 mm and Xpp = 75 mm, respectively, are not changed; and with the increase in the nozzle spacing ratio, the merging points (MPs) on the parallel jet axis are Xmp = 25 mm, 32 mm and 59 mm, respectively. The merging point and the combined point move to a farther distance and the inner deflection angle of the jet is weakened.

Correction: Video-rate upconversion display from optimized lanthanide ion doped upconversion nanoparticles.

Correction for 'Video-rate upconversion display from optimized lanthanide ion doped upconversion nanoparticles' by Laixu Gao et al., Nanoscale, 2020, DOI: .

Video-rate upconversion display from optimized lanthanide ion doped upconversion nanoparticles.

Volumetric displays that create bright image points within a transparent bulk are one of the most attractive technologies in everyday life. Lanthanide ion doped upconversion nanoparticles (UCNPs) are promising luminescent nanomaterials for background free, full-colour volumetric displays of transparent bulk materials. However, video-rate display using UCNPs has been limited by their low emission intensity. Herein, we developed a video-rate upconversion display system with much enhanced brightness. The integral emission intensity of the single UCNPs was fully employed for video-rate display. It was maximized by optimizing the emitter concentration and, more importantly, by temporally synchronizing the scanning time of the excitation light to the the raised emission time of the single UCNPs. The excitation power dependent emission response and emission time decay curves were systematically characterized for the single UCNPs with various emitter concentrations from 0.5% to 6%. 1%Tm3+ doped UCNPs presented the highest integral emission intensity. By embedding this UCNPs into a polyvinyl acetate (PVA) film, we achieved a two-dimensional (2D) upconversion display with a frame rate of 29 Hz for 35 by 50 pixels. This work demonstrates that the temporal response as well as the integral emission intensity enable video-rate upconversion display.