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Author(s):  
Chao Guo ◽  
Jingying Zhai ◽  
Yifu Wang ◽  
Xinfeng Du ◽  
Zige Wang ◽  
...  

2021 ◽  
Author(s):  
Mengyao Liu ◽  
Yonghong Li ◽  
Wei Xing ◽  
Yuqin Zhang ◽  
Xi Xie ◽  
...  

Abstract BackgroundEffective and accurate screening of oncological biomarkers in peripheral blood circulation plays an increasingly vital role in diagnosis and prognosis. High-sensitivity assays can effectively aid clinical decision-making and intervene in cancer in a localized status before they metastasize and become unmanageable. Meanwhile, it is equally pivotal to prevent overdiagnosis of non-life-threatening cancer by eliminating unnecessary treatment and repeated blood draws. Unfortunately, current clinical screening methodologies can hardly simultaneously attain sufficient sensitivity and specificity, especially under resource-restrained circumstances. To circumvent such limitations, particularly for cancer biomarkers from early-onset and recurrence, we aim to develop a universal plasmonic platform for clinical applications, which macroscopically amplifies multiplexed fluorescence signals in a broad spectral window readily adapts to current assay setups without sophisticated accessories or expertise at low cost. MethodsThe plasmonic substrate was chemically synthesized in situ at the solid-liquid interface by rationally screening a panel of reducing monosaccharides and tuning the redox reactions at various catalyst densities and precursor concentrations. The redox properties were studied by Benedict’s assay and electrochemistry. We systemically characterized the morphologies and optical properties of the engineered plasmonic Ag structures by scanning electron microscopy (SEM) and spectroscopy. The structure-fluorescence enhancement correlation was explicitly explained by the finite-difference time-domain (FDTD) simulation and a computational model for gap distribution. Next, we established an enhanced fluoroimmunoassay (eFIA) using a model biomarker for prostate cancer (PCa) and validated it in healthy and PCa cohorts. Prognosis was explored in patients subject to surgical and hormonal interventions following recommended PCa guidelines. ResultsThe monosaccharide-mediated redox reaction yielded a broad category of Ag structures, including sparsely dispersed nanoparticles of various sizes, semi-continuous nanoislands, and crackless continuous films. Optimal broad-spectral fluorescence enhancement from green to far-red was observed for the inhomogeneous, irregularly-shaped semi-continuous Ag nanoisland substrate (AgNIS), synthesized from a well-balanced redox reaction at a stable rate mediated by mannose. In addition, different local electric field intensity distributions in response to various incident excitations were observed at the nanoscale, elucidating the need for irregular and inhomogeneous structures. AgNIS enabled a maximized 54.7-fold macroscopically amplified fluorescence and long-lasting photostability. Point-of-care availability was fulfilled using a customized smartphone prototype with well-paired optics. The eFIA effectively detected the PCa marker in cell lines, xenograft tumors, and patient sera. The plasmonic platform rendered a diagnostic sensitivity of 86.0% and a specificity of 94.7% and capably staged high-grade PCa that the clinical gold standard test failed to stratify. Patient prognosis of surgical and hormonal interventions was non-invasively monitored following efficient medical interventions. The assay time was significantly curtailed on the plasmonic platform upon microwave irradiation. ConclusionsBy investigating the effects of monosaccharides on the seed-mediated chemical synthesis of plasmonic Ag structures, we deduced that potent multiplexed fluorescence enhancement originated from both an adequate reducing power and a steady reduction rate. Furthermore, the inhomogeneous structure with adequate medium gap distances afforded optimal multiwavelength fluorescence enhancement, thus empowering an effective eFIA for PCa. The clinically validated diagnostic and prognostic features, along with the low sample volume, point-of-care feasibility with a smartphone, and microwave-shortened assay time, warrant its potential clinical translation for widespread cancer biomarker analysis.


Molecules ◽  
2021 ◽  
Vol 26 (23) ◽  
pp. 7281
Author(s):  
William E. Gilbraith ◽  
J. Chance Carter ◽  
Kristl L. Adams ◽  
Karl S. Booksh ◽  
Joshua M. Ottaway

We present four unique prediction techniques, combined with multiple data pre-processing methods, utilizing a wide range of both oil types and oil peroxide values (PV) as well as incorporating natural aging for peroxide creation. Samples were PV assayed using a standard starch titration method, AOCS Method Cd 8-53, and used as a verified reference method for PV determination. Near-infrared (NIR) spectra were collected from each sample in two unique optical pathlengths (OPLs), 2 and 24 mm, then fused into a third distinct set. All three sets were used in partial least squares (PLS) regression, ridge regression, LASSO regression, and elastic net regression model calculation. While no individual regression model was established as the best, global models for each regression type and pre-processing method show good agreement between all regression types when performed in their optimal scenarios. Furthermore, small spectral window size boxcar averaging shows prediction accuracy improvements for edible oil PVs. Best-performing models for each regression type are: PLS regression, 25 point boxcar window fused OPL spectral information RMSEP = 2.50; ridge regression, 5 point boxcar window, 24 mm OPL, RMSEP = 2.20; LASSO raw spectral information, 24 mm OPL, RMSEP = 1.80; and elastic net, 10 point boxcar window, 24 mm OPL, RMSEP = 1.91. The results show promising advancements in the development of a full global model for PV determination of edible oils.


2021 ◽  
Author(s):  
Humberto Antunes de Almeida Filho ◽  
Fabio C. L. Almeida

Thioredoxins are ubiquous proteins with 2 cysteines at the active site. The isoform 1 of Thioredoxin from Saccharomyces cerevisae (Trx1) has six sulphur aminoacids, two cysteines and four methionines. In this work we performed the replacement of cysteines by selenocysteines by growth of a transformed celular expression vector E. coli BL21-DE3 in selenocysteine containing culture medium. The Maldi-TOF spectra of Seleno/Sulphur substituted Trx1 revealed six component peaks with 46-48 Da range between them, that is the isotopic Seleno-Sulfur difference, showing the replacement of the Cysteines and Methionines to Selenocysteines and Selenomethionines. The Maldi-TOF spectra of the peptides derived from Trypsin digestion of the purified Thioredoxin (peptide mass fingerprint) show Selenocysteine and Selenomethionine containing peptides. Therefore we are demonstrating that cystein can be replaced by selenocystein and be metabolically converted to selenomethionine during Trx1 heterologous translation. Furthermore, the Maldi-TOF spectra are showing the presence of the most abundant isotopes of selenium inserted in the peptides containing cysteine and methionine, derived from the Trx1 digestion. The one dimensional 77 Se − 1 H heteronuclear multiple quantum coherence NMR spectroscopy (1D-HMQC) for reduced Seleno substituted Trx1 (Se-Trx1), revealed three ressonance lines for 1 H β 1 from Selenocysteines 30 and 33, between 1.6 and 2,0 ppm. The bidimensional HMQC spectra (2D-HMQC) of the reduced Se Trx1 show the 77 Se ressonance signal in 178 ppm, coupled with 1 H β 1 and 1 H β 2 lines between 2.1 and 1.8 ppm. The 1D-HMQC for oxidized Trx1 revealed the only one broad resonance in 2.6 ppm probably relative to the 1 H β 1 protons. The 2D-HMQC spectrum of oxidized protein shows a higher chemical shift of selenocysteine 77 Se (832 ppm) if compared to reduced state (178 ppm). Together these data are showing that the protocol of Se − S substitution developed here is a efficient method to label the active site of Thioredoxin 1 with a broad band chemical shift atom 77 Se. Furthermore the large spectral window of the 77 Se NMR detected between reduced and oxidized states of the Thioredoxin 1 shows that this atom is an excellent probe for accessing oxidative states and probably the conformational dynamics of the active site of the Se-Trx1.


2021 ◽  
Author(s):  
Leon Kuhn ◽  
Jonas Kuhn ◽  
Thomas Wagner ◽  
Ulrich Platt

Abstract. Monitoring of NO2 is in the interest of public health, because NO2 contributes to the decline of air quality in many urban regions. Its abundance can be a direct cause of asthmatic and cardiovascular diseases and plays a significant part in forming other pollutants such as ozone or particulate matter. Spectroscopic methods have proven to be reliable and of high selectivity by utilizing the characteristic spectral absorption signature of trace gasses such as NO2. However, they typically lack the spatio-temporal resolution required for real-time imaging measurements of NO2 emissions. We propose imaging measurements of NO2 in the visible spectral range using a novel instrument, an NO2 camera based on the principle of Gas Correlation Spectroscopy (GCS). For this purpose two gas cells (cuvettes) are placed in front of two camera modules. One gas cell is empty, while the other is filled with a high concentration of the target gas. The filled gas cell operates as a non-dispersive spectral filter to the incoming light, maintaining the two-dimensional imaging capability of the sensor arrays. NO2 images are generated on the basis of the signal ratio between the two images in the spectral window between 430 and 445 nm, where the NO2 absorption cross section is strongly structured. The capabilities and limits of the instrument are investigated in a numerical forward model. The predictions of this model are verified in a proof-of-concept measurement, in which the column densities in specially prepared reference cells were measured with the NO2 camera and a conventional DOAS instrument. Finally, results from measurements at a large power plant, the Großkraftwerk Mannheim (GKM), are presented. NO2 column densities of the plume emitted from a GKM chimney are quantified at a spatio-temporal resolution of 1/6 frames per second (FPS) and 0.92 m × 0.92 m. A detection limit of 1.89 · 1016 molec cm−2 was reached. An NO2 mass flux of Fm = (7.41 ± 4.23) kg h−1 was estimated on the basis of momentary wind speeds obtained from consecutive images. The camera results are verified by comparison to NO2 slant column densities obtained from elevation scans with a MAX-DOAS instrument. The instrument prototype is highly portable and cost-efficient at building costs of below 2,000 Euro.


Cancers ◽  
2021 ◽  
Vol 13 (20) ◽  
pp. 5109
Author(s):  
Patutong Chatchawal ◽  
Molin Wongwattanakul ◽  
Patcharaporn Tippayawat ◽  
Kamilla Kochan ◽  
Nichada Jearanaikoon ◽  
...  

Cholangiocarcinoma (CCA) is a malignancy of the bile duct epithelium. Opisthorchis viverrini infection is a known high-risk factor for CCA and in found, predominantly, in Northeast Thailand. The silent disease development and ineffective diagnosis have led to late-stage detection and reduction in the survival rate. Attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR) is currently being explored as a diagnostic tool in medicine. In this study, we apply ATR-FTIR to discriminate CCA sera from hepatocellular carcinoma (HCC), biliary disease (BD) and healthy donors using a multivariate analysis. Spectral markers differing from healthy ones are observed in the collagen band at 1284, 1339 and 1035 cm−1, the phosphate band () at 1073 cm−1, the polysaccharides band at 1152 cm−1 and 1747 cm−1 of lipid ester carbonyl. A Principal Component Analysis (PCA) shows discrimination between CCA and healthy sera using the 1400–1000 cm−1 region and the combined 1800—1700 + 1400–1000 cm−1 region. Partial Least Square-Discriminant Analysis (PLS-DA) scores plots in four of five regions investigated, namely, the 1400–1000 cm−1, 1800–1000 cm−1, 3000–2800 + 1800–1000 cm−1 and 1800–1700 + 1400–1000 cm−1 regions, show discrimination between sera from CCA and healthy volunteers. It was not possible to separate CCA from HCC and BD by PCA and PLS-DA. CCA spectral modelling is established using the PLS-DA, Support Vector Machine (SVM), Random Forest (RF) and Neural Network (NN). The best model is the NN, which achieved a sensitivity of 80–100% and a specificity between 83 and 100% for CCA, depending on the spectral window used to model the spectra. This study demonstrates the potential of ATR-FTIR spectroscopy and spectral modelling as an additional tool to discriminate CCA from other conditions.


Author(s):  
Fabio de Moliner ◽  
Ina Biazruchka ◽  
Karolina Konsewicz ◽  
Sam Benson ◽  
Suraj Singh ◽  
...  

AbstractThe development of fluorophores emitting in the near-infrared spectral window has gained increased attention given their suitable features for biological imaging. In this work, we have optimised a general and straightforward synthetic approach to prepare a small library of near-infrared-emitting C-bridged nitrobenzodiazoles using commercial precursors. C-bridged benzodiazoles have low molecular weight and neutral character as important features that are not common in most near-infrared dyes. We have investigated their fluorescence response in the presence of a wide array of 60 different biomolecules and identified compound 3i as a potential chemosensor to discriminate between Fe2+ and Fe3+ ions in aqueous media.


Sensors ◽  
2021 ◽  
Vol 21 (16) ◽  
pp. 5600 ◽  
Author(s):  
Octavian Dănilă ◽  
Doina Mănăilă-Maximean ◽  
Ana Bărar ◽  
Valery A. Loiko

We report simulations on the spectral behavior of non-layered gold-silicon and all-silicon frequency-selective metasurfaces in an asymmetric element configuration in the mid-infrared spectral window of 5–5.8 μm. The non-layered layout is experimentally feasible due to recent technological advances such as nano-imprint and nano-stencil lithography, and the spectral window was chosen due to the multitude of applications in sensing and imaging. The architecture exhibits significant resonance in the window of interest as well as extended tunability by means of variation of cell element sizes and relative coordinates. The results indicate that the proposed metasurface architecture is a viable candidate for mid-infrared absorbers, sensors and imaging systems.


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
L. Lackner ◽  
M. Dusel ◽  
O. A. Egorov ◽  
B. Han ◽  
H. Knopf ◽  
...  

AbstractEngineering non-linear hybrid light-matter states in tailored lattices is a central research strategy for the simulation of complex Hamiltonians. Excitons in atomically thin crystals are an ideal active medium for such purposes, since they couple strongly with light and bear the potential to harness giant non-linearities and interactions while presenting a simple sample-processing and room temperature operability. We demonstrate lattice polaritons, based on an open, high-quality optical cavity, with an imprinted photonic lattice strongly coupled to excitons in a WS2 monolayer. We experimentally observe the emergence of the canonical band-structure of particles in a one-dimensional lattice at room temperature, and demonstrate frequency reconfigurability over a spectral window exceeding 85 meV, as well as the systematic variation of the nearest-neighbour coupling, reflected by a tunability in the bandwidth of the p-band polaritons by 7 meV. The technology presented in this work is a critical demonstration towards reconfigurable photonic emulators operated with non-linear photonic fluids, offering a simple experimental implementation and working at ambient conditions.


Sensors ◽  
2021 ◽  
Vol 21 (14) ◽  
pp. 4886
Author(s):  
Shilei Li ◽  
Maofang Gao ◽  
Zhao-Liang Li

A series of algorithms for satellite retrievals of sun-induced chlorophyll fluorescence (SIF) have been developed and applied to different sensors. However, research on SIF retrieval using hyperspectral data is performed in narrow spectral windows, assuming that SIF remains constant. In this paper, based on the singular vector decomposition (SVD) technique, we present an approach for retrieving SIF, which can be applied to remotely sensed data with ultra-high spectral resolution and in a broad spectral window without assuming that the SIF remains constant. The idea is to combine the first singular vector, the pivotal information of the non-fluorescence spectrum, with the low-frequency contribution of the atmosphere, plus a linear combination of the remaining singular vectors to express the non-fluorescence spectrum. Subject to instrument settings, the retrieval was performed within a spectral window of approximately 7 nm that contained only Fraunhofer lines. In our retrieval, hyperspectral data of the O2-A band from the first Chinese carbon dioxide observation satellite (TanSat) was used. The Bayesian Information Criterion (BIC) was introduced to self-adaptively determine the number of free parameters and reduce retrieval noise. SIF retrievals were compared with TanSat SIF and OCO-2 SIF. The results showed good consistency and rationality. A sensitivity analysis was also conducted to verify the performance of this approach. To summarize, the approach would provide more possibilities for retrieving SIF from hyperspectral data.


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