New Insights into Photo-Fenton Chemistry: The Overlooked Role of Excited IronIII Species.

Direct photoreduction of FeIII is a widely recognized route for accelerating FeIII/FeII cycle in photo-Fenton chemistry. However, most of the wavelengths covering the full spectral range are insufficient to supply enough photon energy for the direct reduction process. Herein, the hitherto neglected mechanism of FeIII reduction that the FeIII indirect reduction pathway initiated by light energy-dependent reactivity variation and reactive excited state (ES) was explored. Evolution of excited-state FeIII species (*FeIII) resulting from metal-centered charge excitation (MCCE) of FeIII is experimentally verified using pulsed laser femtosecond transient absorption spectroscopy with UV-vis detection and theoretically verified by quantum chemical calculation. Intense photoinduced intravalence charge transition was observed at λ = 380 and 466 nm, revealing quartet 4MCCE and doublet 2MCCE and their exponential processes. Light energy-dependent variation of *FeIII reactivity was kinetically certified by fitting the apparent rate constant of the radical-chain sequence of photo-Fenton reactions. Covalency is found to compensate for the intravalence charge separation following photoexcitation of the metal center in the MCCE state of Fenton photosensitizer. The *FeIII is established as a model, demonstrating the intravalence hole delocalization in the ES can be leveraged for photo-Fenton reaction or other photocatalytic schemes based on electron transfer chemistry.

Origins of Selective Oxidation in Carbon-Based Nonradical Oxidation Processes toward Organic Pollutants: Quantitative Structure-Activity Relationships (QSARs).

Metal-free carbon material-mediated nonradical oxidation processes (C-NOPs) have emerged as a research hotspot due to their excellent performance in selectively eliminating organic pollutants in aqueous environments. However, the selective oxidation mechanisms of C-NOPs remain obscure due to the diversity of organic pollutants and nonradical active species. Herein, quantitative structure-activity relationship (QSAR) models were employed to unveil the origins of C-NOP selectivity toward organic pollutants in different oxidant systems. QSAR analysis based on adsorption and oxidation descriptors revealed that C-NOP selectivity depends on the oxidation potentials of organic pollutants rather than on adsorption interactions. However, the dominance of electronic effects in selective oxidation decreases with increasing structural complexity of organic pollutants. Moreover, the oxidation threshold solely depends on the inherent electronic nature of organic pollutants and not on the reactivity of nonradical active species. Notably, the accuracy of substituent descriptors (Hammett constants) and theoretical descriptors (e.g., highest occupied molecular orbital energy, ionization potential, and single-electron oxidation potential) is significantly influenced by the complexity and molecular state of organic pollutants. Overall, the study findings reveal the origins of organic pollutant-oriented selective oxidation and provide insight into the application of descriptors in QSAR analysis.

Effects of latroeggtoxin-VI on dopamine and α-synuclein in PC12 cells and the implications for Parkinson's disease.

BACKGROUND: Parkinson's disease (PD) is characterized by death of dopaminergic neurons leading to dopamine deficiency, excessive α-synuclein facilitating Lewy body formation, etc. Latroeggtoxin-VI (LETX-VI), a proteinaceous neurotoxin discovered from the eggs of spider L. tredecimguttatus, was previously found to promote the synthesis and release of PC12 cells, showing a great potential as a drug candidate for PD. However, the relevant mechanisms have not been understood completely. The present study explored the mechanism underlying the effects of LETX-VI on dopamine and α-synuclein of PC12 cells and the implications for PD. RESULTS: After PC12 cells were treated with LETX-VI, the level of dopamine was significantly increased in a dose-dependent way within a certain range of concentrations. Further mechanism analysis showed that LETX-VI upregulated the expression of tyrosine hydroxylase (TH) and L-dopa decarboxylase to enhance the biosynthesis of dopamine, and downregulated that of monoamine oxidase B to reduce the degradation of dopamine. At the same time, LETX-VI promoted the transport and release of dopamine through modulating the abundance and/or posttranslational modification of vesicular monoamine transporter 2 (VMAT2) and dopamine transporter (DAT). While the level of dopamine was increased by LETX-VI treatment, α-synuclein content was reduced by the spider toxin. α-Synuclein overexpression significantly decreased the dopamine level and LETX-VI efficiently alleviated the inhibitory action of excessive α-synuclein on dopamine. In the MPTP-induced mouse model of PD, application of LETX-VI ameliorated parkinsonian behaviors of the mice, and reduced the magnitude of MPTP-induced α-synuclein upregulation and TH downregulation. In addition, LETX-VI displayed neuroprotective effects by inhibiting MPTP-induced decrease in the numbers of TH-positive and Nissl-stained neurons in mouse brain tissues. CONCLUSIONS: All the results demonstrate that LETX-VI promotes the synthesis and release of dopamine in PC12 cells via multiple mechanisms including preventing abnormal α-synuclein accumulation, showing implications in the prevention and treatment of PD.

Analysis of differentially expressed genes discovers Latroeggtoxin VI-induced changes and SYNJ1 as a main target in PC12 cells.

BACKGROUND: Previous preliminary work found that Latroeggtoxin-VI (LETX-VI), a proteinaceous neurotoxin from the eggs of spider Latrodectus tredecimguttatus, could promote the synthesis and release of dopamine in PC12 cells. However, the underlying mechanisms have not been fully clear. Here, the effects of LETX-VI on the gene expression profile and dopamine in PC12 cells were analyzed with the differential transcriptome-based strategies. RESULTS: After treatment of PC12 cells with LETX-VI for 24 h, a total of 356 differentially expressed transcripts were identified. Of them 165 were up-regulated and 191 down-regulated. Relevant GO analysis indicated that LETX-VI modulated the expression of certain genes and thereby affected multiple biological processes in PC12 cells, including protein metabolism, nucleic acid metabolism, substance transport, signaling, neurotransmitter metabolism and release. When western blot analysis was employed to confirm the abundance levels of synaptojanin 1 and synuclein alpha interacting protein, the representatives of highly up- and down-regulated transcript-encoded proteins that are closely related with dopamine respectively, it was found that the level of synaptojanin 1 in the PC12 cells treated with LETX-VI was increased, whereas that of synuclein alpha interacting protein was not obviously altered, suggesting that synaptojanin 1 may be much more involved in the effects of LETX-VI on dopamine. After synaptojanin 1 level was knocked down using siRNA, the levels of both total and released dopamine were significantly decreased, indicating that synaptojanin 1 is a protein positively modulating the synthesis and secretion of dopamine. When the PC12 cells with knocked down synaptojanin 1 were treated by LETX-VI, the adverse effects of synaptojanin 1 knockdown on dopamine were attenuated, confirming that LETX-VI promotes the synthesis and secretion of dopamine at least partially by enhancing the expression of the gene SYNJ1 encoding synaptojanin 1. CONCLUSIONS: This work demonstrates that LETX-VI exerts multiple regulatory effects on the cellular processes in PC12 cells by altering the gene expression profile. LETX-VI modulates the expression of the genes closely related to the synthesis, transport and release of neurotransmitters especially dopamine in PC12 cells, with the gene SYNJ1 encoding synaptojanin 1 as a main target.

Removal of Phenols by Highly Active Periodate on Carbon Nanotubes: A Mechanistic Investigation.

Carbon nanotubes (CNTs) and their derivatives have been widely exploited to activate various oxidants for environmental remediation. However, the intrinsic mechanism of CNTs-driven periodate (PI) activation remains ambiguous, which significantly impedes their scientific progress toward practical application. Here, we found that CNTs can strongly boost PI activation for the oxidation of various phenols. Reactive oxygen species analysis, in situ Raman characterization, galvanic oxidation process experiments, and electrochemical tests revealed that CNTs could activate PI to form high-potential metastable intermediates (CNTs-PI*) rather than produce free radicals and 1O2, thereby facilitating direct electron transfer from the pollutants to PI. Additionally, we analyzed quantitative structure-activity relationships between rate constants of phenols oxidation and double descriptors (e.g., Hammett constants and logarithm of the octanol-water partition coefficient). The adsorption of phenols on CNT surfaces and their electronic properties are critical factors affecting the oxidation process. Besides, in the CNTs/PI system, phenol adsorbed the CNT surfaces was oxidized by the CNTs-PI* complexes, and products were mainly generated via the coupling reaction of phenoxyl radical. Most of the products adsorbed and accumulated on the CNT surfaces realized phenol removal from the bulk solution. Such a unique non-mineralization removal process achieved an extremely high apparent electron utilization efficiency of 378%. The activity evaluation and theoretical calculations of CNT derivatives confirmed that the carbonyl/ketonic functional groups and double-vacancy defects of the CNTs were the primary active sites, where high-oxidation-potential CNTs-PI* were formed. Further, the PI species could achieve a stoichiometric decomposition into iodate, a safe sink of iodine species, without the generation of typical iodinated byproducts. Our discovery provides new mechanistic insight into CNTs-driven PI activation for the green future of environmental remediation.

Metal Borides as Excellent Co-Catalysts for Boosted and Long-Lasting Fenton-like Reaction: Dual Co-Catalytic Centers of Metal and Boron.

The continuous electron supply for oxidant decomposition-induced reactive oxygen species (ROS) generation is the main contributor for the long-standing micropollutant oxidation in the iron-based advanced oxidation processes (AOPs). Herein, as a new class of co-catalysts, metal borides with dual active sites and preeminent conductive performance can effectively overcome the inherent drawback of Fenton-like reactions by steadily donating electrons to inactive Fe(III). Among the metal borides, tungsten boride (WB) exhibits a significant co-catalytic performance run ahead of common heterogeneous co-catalysts and exceptionally high stability. Based on qualitative and semi-quantitative tests, the hydroxyl radical, sulfate radical, and iron(IV)-oxo complex are all produced in the WB/Fe(III)/PDS system and Fe(IV)-induced methyl phenyl sulfoxide decomposition is up to 72%. Moreover, the production efficiency of ROS and relative proportions of radical and nonradical pathways change with various experimental conditions (dosages of PDS, WB, and solution pH) and water matrices. The rate-determining step of Fe(II) regeneration is greatly accelerated resulting from the synergetic effect between exposed metallic reactive sites and nonmetallic boron with reductive properties of WB. In addition, the self-dissolution of surface tungsten oxide and boron oxide leads to a renovated surface for sustainable Fe(III) reduction in long-term operations. Our discovery provides an efficient and sustainable strategy in the field of enhanced AOPs for water remediation.

The effect of awarding disability benefits on opioid consumption.

Strong empirical evidence points towards a significantly higher prevalence of opioid consumption among people receiving disability benefits (DB) than in the general population of the United States. However, no previous research established a causal relationship between the decision to award DB to applicants and their subsequent opioid use. We aim to contribute towards filling this gap. There are channels through which awarding DB may both increase and depress opioid consumption, and thus, ex ante, the sign of a potential causal relationship is ambiguous. To correct for the treatment endogeneity, since an individual's age at the time of the decision on an application impacts discontinuously at certain age cutoffs the award decision, we employ a fuzzy Regression Discontinuity model with three age cutoffs used for identification. We find that awarding DB increases the likelihood of using opioids by about 27-30 percentage points. This suggests that the positive association between DB receipt and opioid consumption is likely to be causal.

Neural network model combined with pupil recovery for Fourier ptychographic microscopy.

Fourier ptychographic microscopy (FPM) is a recently developed imaging approach aiming at circumventing the limitation of the space-bandwidth product (SBP) and acquiring a complex image with both wide field and high resolution. So far, in many algorithms that have been proposed to solve the FPM reconstruction problem, the pupil function is set to be a fixed value such as the coherent transfer function (CTF) of the system. However, the pupil aberration of the optical components in an FPM imaging system can significantly degrade the quality of the reconstruction results. In this paper, we build a trainable network (FINN-P) which combines the pupil recovery with the forward imaging process of FPM based on TensorFlow. Both the spectrum of the sample and pupil function are treated as the two-dimensional (2D) learnable weights of layers. Therefore, the complex object information and pupil function can be obtained simultaneously by minimizing the loss function in the training process. Simulated datasets are used to verify the effectiveness of pupil recovery, and experiments on the open source measured dataset demonstrate that our method can achieve better reconstruction results even in the presence of a large aberration. In addition, the recovered pupil function can be used as a good estimate before further analysis of the system optical transmission capability.

Apodized coherent transfer function constraint for partially coherent Fourier ptychographic microscopy.

Fourier ptychographic microscopy (FPM) is a recently developed computational microscopy approach that produces both wide field-of-view (FOV) and high resolution (HR) intensity and a phase image of the sample. Inspired by the ideas of synthetic aperture and phase retrieval, FPM iteratively stitches multiple low-resolution (LR) images with variable illumination angles in Fourier space to reconstruct an HR complex image. Typically, FPM illuminating the sample with an LED array is approximated as a coherent imaging process, and the coherent transfer function (CTF) is imposed as a support constraint in Fourier space. However, a millimeter-scale LED is inapposite to be treated as a coherent light source. As a result, the quality of reconstructed image is degraded by the inappropriate approximation. In this paper, we analyze the coherence of an FPM system and propose a novel constraint approach termed Apodized CTF (AC) constraint in Fourier space. Results on both simulated data and actual captured data show that this new constraint is more stable and robust than CTF. This approach can also relax the coherence requirement of illumination. In addition, it is simple, does not require additional computations, and is easy to be embedded in almost all the reconstruction algorithms proposed so far.

Spatial confinement Fenton oxidation realized via tunable nanopore structure of porous carbon.

Spatially confined structure exhibits surprising physics and chemistry properties that significantly impact the thermodynamics and kinetics of oxidation reactions. Herein, porous carbons are rationally designed for tunable nanopore structures (micropores, 4.12 % ∼ 91.64 %) and diverse spatial confinement ability, as indicated by their differential enhancement performances in the Fenton oxidation. Porous carbons can alter the characteristics of the charge transport process for accelerating sustainable electron shuttle between hydrogen peroxide and iron species, and thus exhibit long-term performance (17 cycling tests). The positive spatial confinement for boosting Fenton oxidation (charge transport, mass transfer) occurs in nanochannels < 1 nm, while the diminished effect ranges of 1-1.5 nm, and the adverse effect ranges greater than 1.5 nm. The density functional theory calculation provides further support for certifying the promoted charge transport process and spatial confinement for hydroxyl radical inside the confined nanochannel structure (below 1 nm, especially) by the comparatively large electron cloud and the relatively negative adsorption energy, respectively. Coupling nanochannels with the Fenton oxidation greatly utilize hydrogen peroxide, due to spatial nanoconfinement and selective adsorption towards target contaminants. This strategy of deploying nanochannels in catalyst design can be applied for the elaborate construction of efficient nanostructured catalysts for environmental remediation.

pH-modulated oxidation of organic pollutants for water decontamination: A deep insight into reactivity and oxidation pathway.

Solution pH is one of the primary factors affecting the efficiency of water decontamination. Although the influence of pH on oxidants activation, catalyst activity, and reactive oxygen species have been widely explored, there is still a scarcity of systemic studies on the changes in the oxidation behavior of organic pollutants at different pH levels. Herein, we report the influence laws of pH on the forms, reactivities, active sites, degradation pathways, and products toxicities of organic pollutants. Changes in pH cause the protonation or deprotonation of organic pollutants and further affect their forms and chemistry (e.g., electrostatic force, hydrophobicity, and oxidation potential). The oxidation potential of organic pollutants follows the order: protonated form > pristine form > deprotonated form. Moreover, protonation or deprotonation can modify the active sites and degradation pathways of organic pollutants, wherein deprotonation renders them more susceptible to electrophilic attack, while protonation reduces their activity against electrophilic and nucleophilic attacks. Additionally, pH adjustments can modify the degradation pathway and the toxicity of transformation products. Overall, pH changes can affect the oxidation fate of organic pollutants by altering their structure, which distinguishes it from the effect of pH on oxidants or oxidant activation processes.

Latroeggtoxin-VI protects nerve cells and prevents depression by inhibiting NF-κB signaling pathway activation and excessive inflammation.

Depression has a high incidence and seriously endangers human health. Accumulated evidence indicates that targeting neuroinflammation is a potential avenue for neuroprotection and thus depression prevention. Herein, the effects of latroeggtoxin-VI (LETX-VI), a bioactive protein from the eggs of spider Latrodectus tredecimguttatus, on lipopolysaccharide (LPS)-induced inflammation and depression were systematically investigated using RAW264.7 macrophages and depression mouse model. Pretreatment with LETX-VI suppressed LPS-evoked NF-κB signaling pathway activation, inhibited LPS-induced over-production of NO, iNOS, IL-6 and TNF-α; at the same time LETX-VI mitigated the inhibitory effect of LPS on the expression of anti-inflammatory factors such as Arg-1, thereby suppressing oxidative stress and excessive inflammation. Culture of PC12 cells with the conditioned medium of RAW264.7 cells pretreated with LETX-VI demonstrated the neuroprotective effect of LETX-VI due to its anti-inflammation effect. In the LPS-induced depression mouse model, pretreatment with LETX-VI improved the LPS-induced depression-like behaviors, inhibited the activation of microglia and astrocytes, prevented the down-regulation of Nurr1 expression and alleviated the LPS-caused adverse changes in the brain tissues. Taken together, these in vitro and in vivo findings provide powerful insights into the anti-inflammation-based neuroprotective and antidepressant mechanisms of LETX-VI, which is helpful to deeply reveal the biological effects and potential applications of LETX-VI.

Insights into the mediation of Ca2+ signaling in the promoting effects of LETX-VI on the synthesis and release of dopamine.

Latroeggtoxin-VI (LETX-VI) is an active protein and was previously demonstrated to have effects on the synthesis and release of dopamine. Hererin, the involvement of Ca2+ signaling in the effects of LETX-VI on dopamine was systematically investigated, using PC12 cells as a neuron model. LETX-VI was shown to promote dopamine release from PC12 cells both in the presence and absence of extracellular Ca2+; however the presence of extracellular Ca2+ was favorable for enhancing the promoting effects of LETX-VI on dopamine, because LETX-VI facilitated the influx of extracellular Ca2+ through the L-type calcium channels in plasma membrane (PM) to increase cytosolic Ca2+ concentration. LETX-VI was able to penetrate the PM of PC12 cells to act on the Ca2+ channel proteins IP3Rs and RyRs in the endoplasm reticulum (ER) membrane, opening the Ca2+ channels and promoting the release of ER Ca2+ to elevate cytosolic Ca2+ level. With the help of intracellular Ca2+ chelator BAPTA, the elevated cytosolic Ca2+ level was proven to play crucial role for the enhanced promoting effects of LETX-VI on dopamine. Taken together, LETX-VI is able to open the Ca2+ channels in both PM and ER membrane simultaneously to facilitate extracellular Ca2+ influx and ER Ca2+ release, and thus increases the cytosolic Ca2+ concentration to enhance the promoting effects on the synthesis and release of dopamine.

Experimental study of viscosity modification coupled with phase transfer catalysis for enhanced remediation of non-aqueous phase trichloroethene polluted heterogeneous aquifer.

The degradation of dense non-aqueous phase liquid trichloroethene in low permeability zone is a challenging issue due to limited mass transfer between water-soluble oxidants (i.e., MnO4-) and residual phase trichloroethene and the bypassing of amendments in low permeability zone. This work accomplished trichloroethene oxidation enhancement through coupling viscosity modification by using xanthan with phase transfer of MnO4- by using phase transfer catalyst (PTC). Experiments were conducted by sand columns and 2D-tanks, and results revealed that after ~11.7 g of trichloroethene was injected in each tank, the mass of trichloroethene degradation was 1.3, 5.9, 6.9 and 8.5 g in MnO4-, MnO4- + xanthan, MnO4- + PTC and MnO4- + PTC + xanthan reaction systems, respectively. Combining PTC and xanthan with MnO4- increased the rate of continuous formation of Cl-, reflected in the acceleration of heterogeneous reactions and MnO4- transport enhancement in low permeability zone by PTC and xanthan. Moreover, PTC promoted dissolved Mn (Ⅱ) and Mn (Ⅲ) formation in the process of MnO4- reduction, and thus effectively inhibited MnO2 generation. In conclusion, the results revealed that PTC and xanthan could perform their respective contributions to mass transfer and amendment transport for jointly enhanced the remediation of trichloroethene polluted heterogeneous aquifer.

High-resolution 3D Fourier ptychographic reconstruction using a hemispherical illumination source with multiplexed-coded strategy.

Fourier ptychography is a promising and flexible imaging technique that can achieve 2D quantitative reconstruction with higher resolution beyond the limitation of the system. Meanwhile, by using different imaging models, the same platform can be applied to achieve 3D refractive index reconstruction. To improve the illumination NA as much as possible while reducing the intensity attenuation problem caused by the LED board used in the traditional FP platform, we apply a hemispherical lighting structure and design a new LED arrangement according to 3D Fourier diffraction theory. Therefore, we could obtain the illumination of 0.98NA using 187 LEDs and achieve imaging half-pitch resolutions of ∼174 nm and ∼524 nm for the lateral and axial directions respectively, using a 40×/0.6NA objective lens. Furthermore, to reduce the number of captured images required and realize real-time data collection, we apply the multiplexed-coded illumination strategy and compare several coded patterns through simulation and experiment. Through comparison, we determined a radial-coded illumination pattern that could achieve more similar results as sequential scanning and increase the acquisition speed to above 1 Hz. Therefore, this paper provides the possibility of this technique in real-time 3D observation of in vitro live samples.

Nitrogen-doped carbon nanotubes enhanced Fenton chemistry: Role of near-free iron(III) for sustainable iron(III)/iron(II) cycles.

The sluggish kinetics of Fe(II) recovery strongly impedes the scientific progress of Fenton reaction (Fe(II)/H2O2) towards practical application. Here, we propose a novel mechanism that metal-free nitrogen-doped carbon nanotubes (NCNT) can enhance Fenton chemistry with H2O2 as electron donors by elevating the oxidation potential of Fe(III). NCNT remarkably promotes the circulation of Fe(III)/Fe(II) to produce hydroxyl radical (•OH) with excellent stability for multiple usages (more than 10 cycles) in the NCNT/Fe(III)/H2O2 system. Although carbonyl on NCNT can act as the electron supplier for Fe(III) reduction, the behavior of NCNT is distinct from common reductants such as hydroxylamine and boron. Electrochemical analysis and density functional theory calculation unveil that nitrogen sites of NCNT can weakly bind with Fe(III) to elevate the oxidation potential of Fe(III) (named near-free Fe(III), primarily FeOH2+) at pH ranging from 2.0 to 4.0. Without inputs of external stimulations or electron sacrificers, near-free Fe(III) can promote H2O2 induced reduction of Fe(III) to initiate Fenton chain reactions for long-lasting generation of •OH. To our delight, it is a common property of N-doped carbon materials (e.g., graphene, carbon nanofibers, and acetylene black), our research thus provides a novel, sustainable, and green strategy for promoting Fenton chemistry.

Synaptotagmin 1-mediated cell membrane penetration and dopamine release enhancement by latroeggtoxin-VI.

Latroeggtoxin-VI (LETX-VI), a proteinaceous neurotoxin mined from the egg transcriptome of spider L. tredecimguttatus, was previously found to promote the release of dopamine from PC12 cells. However, the relevant molecular mechanism has not been fully clear. Here LETX-VI was demonstrated to rapidly penetrate the plasma membrane of PC12 cells via the vesicle exocytosis/endocytosis cycle, during which vesicular transmembrane protein synaptotagmin 1 (Syt1) functions as a receptor, with its vesicle luminal domain interacting with the C-terminal region of LETX-VI. The C-terminal sequence of LETX-VI is the functional region for both entering cells and promoting dopamine release. After gaining entry into the PC12 cells, LETX-VI down-regulated the phosphorylation levels of Syt1 at T201 and T195, thereby facilitating vesicle fusion with plasma membrane and thus promoting dopamine release. The relevant mechanism analysis indicated that LETX-VI has a protein phosphatase 2A (PP2A) activator activity. The present work has not only probed into the Syt1-mediated action mechanism of LETX-VI, but also revealed the structure-function relationship of the toxin, thus suggesting its potential applications in the drug transmembrane delivery and treatment of the diseases related to dopamine release and PP2A activity deficiency.

Double-flow convolutional neural network for rapid large field of view Fourier ptychographic reconstruction.

Fourier ptychographic microscopy is a promising imaging technique which can circumvent the space-bandwidth product of the system and achieve a reconstruction result with wide field-of-view (FOV), high-resolution and quantitative phase information. However, traditional iterative-based methods typically require multiple times to get convergence, and due to the wave vector deviation in different areas, the millimeter-level full-FOV cannot be well reconstructed once and typically required to be separated into several portions with sufficient overlaps and reconstructed separately, which makes traditional methods suffer from long reconstruction time for a large-FOV (of the order of minutes) and limits the application in real-time large-FOV monitoring of live sample in vitro. Here we propose a novel deep-learning based method called DFNN which can be used in place of traditional iterative-based methods to increase the quality of single large-FOV reconstruction and reducing the processing time from 167.5 to 0.1125 second. In addition, we demonstrate that by training based on the simulation dataset with high-entropy property (Opt. Express 28, 24 152 [2020]), DFNN could has fine generalizability and little dependence on the morphological features of samples. The superior robustness of DFNN against noise is also demonstrated in both simulation and experiment. Furthermore, our model shows more robustness against the wave vector deviation. Therefore, we could achieve better results at the edge areas of a single large-FOV reconstruction. Our method demonstrates a promising way to perform real-time single large-FOV reconstructions and provides further possibilities for real-time large-FOV monitoring of live samples with sub-cellular resolution.

Single full-FOV reconstruction Fourier ptychographic microscopy.

Fourier ptychographic microscopy (FPM) is a recently developed computational imaging technique that has high-resolution and wide field-of-view (FOV). FPM bypasses the NA limit of the system by stitching a number of variable-illuminated measured images in Fourier space. On the basis of the wide FOV of the low NA objective, the high-resolution image with a wide FOV can be reconstructed through the phase recovery algorithm. However, the high-resolution reconstruction images are affected by the LED array point light source. The results are: (1) the intensities collected by the sample are severely declined when edge LEDs illuminate the sample; (2) the multiple reconstructions are caused by wavevectors inconsistency for the full FOV images. Here, we propose a new lighting scheme termed full FOV Fourier ptychographic microscopy (F3PM). By combining the LED array and telecentric lens, the method can provide plane waves with different angles while maintaining uniform intensity. Benefiting from the telecentric performance and f‒θ property of the telecentric lens, the system stability is improved and the relationship between the position of LED and its illumination angle is simplified. The excellent plane wave provided by the telecentric lens guarantees the same wavevector in the full FOV, and we use this wavevector to reconstruct the full FOV during one time. The area and diameter of the single reconstruction FOV reached 14.6mm 2 and 5.4 mm, respectively, and the diameter is very close to the field number (5.5 mm) of the 4× objective. Compared with the traditional FPM, we have increased the diameter of FOV in a single reconstruction by ∼ 10 times, eliminating the complicated steps of computational redundancy and image stitching.

Graphene oxide mediated co-generation of C-doping and oxygen defects in Bi2WO6 nanosheets: a combined DRIFTS and DFT investigation.

In order to efficiently control air pollutants using photocatalytic technology, the co-generation of C-doping and oxygen vacancies (OVs) in Bi2WO6 (BWO) nanosheets was achieved by a graphene oxide (GO)-mediated hydrothermal method. The photocatalytic performance was highly improved with the synergistic effects of C-doping and OVs. The experimental characterization and DFT calculations were closely combined to reveal that the C element could serve as both an electron acceptor and channel for charge transfer to promote charge separation. Meanwhile, the OVs could induce the formation of a defect level in the band gap which increases the production of ˙OH as the primary reactive species by introducing more light-generated holes into the valence band. Meanwhile, the OVs could enhance the generation of ˙O2- species via the promotion of O2 adsorption and activation on the catalyst surface. Moreover, the reaction intermediates were monitored and the mechanism of photocatalytic NO oxidation was proposed based on in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The design concept of photocatalyst modification with C-doping and OVs could offer a novel strategy to enhance the performance for environmental applications.