Search Results (41)

The development and characterization of a sustainable carboxymethylcellulose (CMC)-based material hosting Egyptian blue (EB) as a luminophore with emission in both the visible and NIR regions is herein presented and discussed, demonstrating its potential to be applied in a variety of applications, such as bioimaging, sensing, and security marking. Solution casting was used to synthesize the films, with citric acid (CA) as a crosslinking agent. Fully characterization was performed using attenuated total reflection (ATR) and coherent anti-Stokes Raman scattering (CARS) spectroscopy, zeta potential, UV–Vis, and photoluminescence (PL) spectroscopy, and thermal analysis techniques, such as thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). The results confirm the effective crosslinking of CMC with CA within CMC–EB–CA films with 1.5 and 3% of EB. The introduction of EB retained its usual NIR emission with λ_em max = ~950 nm reaching quantum yield values in the range of 11.2–12.8% while also enabling a stable dispersion within the CMC matrix, as confirmed using CARS imaging and zeta potential. Additionally, the CMC films exhibited the characteristic clustering-triggered emission (CTE) in the blue region at 430 nm with a slight increase in luminescence quantum yield (Φ) from 5.8 to 6.1% after crosslinking with citric acid. Full article

Coherent anti-Stokes Raman scattering (CARS) is a powerful nonlinear spectroscopic technique widely used in biological imaging, chemical analysis, and combustion and flame diagnostics. The adoption of pulse shapers in CARS has emerged as a useful approach, offering precise control of optical waveforms. By tailoring the phase, amplitude, and polarization of laser pulses, the pulse shaping approach enables selective excitation, spectral resolution improvement, and non-resonant background suppression in CARS. This paper presents a comprehensive review of applying pulse shaping techniques in CARS spectroscopy for biophotonics. There are two different pulse shaping strategies: passive pulse shaping and active pulse shaping. Two passive pulse shaping techniques, hybrid CARS and spectral focusing CARS, are reviewed. Active pulse shaping using a programmable pulse shaper such as spatial light modulator (SLM) is discussed for CARS spectroscopy. Combining active pulse shaping and passive shaping, optimizing CARS with acousto-optic programmable dispersive filters (AOPDFs) is discussed and illustrated with experimental examples conducted in the authors’ laboratory. These results underscore pulse shapers in advancing CARS technology, enabling improved sensitivity, specificity, and broader applications across diverse scientific fields. Full article

This paper presents an overview of the application of Raman spectroscopy (RS) in characterizing carotenoids, which have recently gained attention due to new findings on their health-promoting effects and rising demand in the food, pharmaceutical, and cosmetic industries. The backbone structure in the form of a polyene chain makes carotenoids sensitive to Raman spectroscopy, mainly due to the stretching vibrations of their conjugated double bonds. Raman spectroscopy is increasingly used in agricultural and food sciences and technologies as it is a non-preparative, environmentally friendly, fast and efficient method for characterizing target analytes. The application of RS in the qualitative and quantitative analysis of carotenoids requires the careful selection and adjustment of various instrument parameters (e.g., laser wavelength, laser power, spectral resolution, detector type, etc.) as well as performing complex chemometric modeling to interpret the Raman spectra. Most of the studies covered in this review focus more on qualitative than quantitative analysis. The most frequently used laser wavelengths are 1064, 785, and 532 nm, while 633 nm is the least used. Considering the sensitivity and complexity of RS, the present study focuses on the specific and critical points in the analysis of carotenoids by RS. The main methodological and experimental principles in the study of food carotenoids by RS are discussed and best practices recommended, while the future prospects and expectations for a wider application of RS, especially in food quality assessment, are emphasized. New Raman techniques such as Spatially Offset Raman Spectroscopy (SORS), Coherent Anti-Stokes Raman Spectroscopy (CARS) and Stimulated Raman Scattering Spectroscopy (SRS), as well as the application of artificial intelligence, are also described in the context of carotenoids analysis. Full article

The World Health Organization (WHO) cancer agency predicts that more than 35 million cases of cancer will be experienced in 2050, a 77% increase over the 2022 estimate. Currently, the main cancers diagnosed are breast, lung, and colorectal. There is no standardized tool for cancer diagnoses; initially, clinical procedures are guided by the patient symptoms and usually involve biochemical blood tests, imaging, and biopsy. Label-free non-linear optical approaches are promising tools for tumor imaging, due to their inherent non-invasive biosafe contrast mechanisms and the ability to monitor collagen-related disorders, and biochemical and metabolic changes during cancer progression. In this review, the main non-linear microscopy techniques are discussed, according to three main contrast mechanisms: biochemical, metabolic, and structural imaging. Full article

Nonlinear optical microscopic imaging techniques have advanced for chemically sensitive imaging of solid and liquid samples but lack advancements for gaseous samples. In this work, wide-field three-color ultrafast coherent anti-Stokes Raman scattering microscopy is implemented for selectively imaging the ambient nitrogen gas. Our technique operates by capturing a series of spectrally selected images with a rate of 5–10 frames per second. The recorded data are analyzed both qualitatively and quantitatively. This technique has been demonstrated to be sensitive to a variation of approximately 10¹¹ nitrogen molecules in ambient air confined within a microscopic volume of 10 μm by 50 μm by 50 μm. We believe that our approach can potentially be extended toward real-time, in situ chemical imaging of the microscopic dynamics of gases, for example, in ammonia for nitrogen cycle, greenhouse gases for environmental pollution, plant fertilization regulation for precision agriculture, or byproducts produced from lower-temperature plasmas. Full article

Dupuytren’s disease (DD) is a prevalent fibroproliferative disorder of the hand, shaped by genetic, epigenetic, and environmental influences. The extracellular matrix (ECM) is a complex assembly of diverse macromolecules. Alterations in the ECM’s content, structure and organization can impact both normal physiological functions and pathological conditions. This study explored the content and organization of glycosaminoglycans, proteoglycans, and collagen in the ECM of patients at various stages of DD, assessing their potential as prognostic indicators. This research reveals, for the first time, relevant changes in the complexity of chondroitin/dermatan sulfate structures, specifically an increase of disaccharides containing iduronic acid residues covalently linked to either N-acetylgalactosamine 6-O-sulfated or N-acetylgalactosamine 4-O-sulfated, correlating with the disease’s severity. Additionally, we noted an increase in versican expression, a high molecular weight proteoglycan, across stages I to IV, while decorin, a small leucine-rich proteoglycan, significantly diminishes as DD progresses, both confirmed by mRNA analysis and protein detection via confocal microscopy. Coherent anti-Stokes Raman scattering (CARS) microscopy further demonstrated that collagen fibril architecture in DD varies importantly with disease stages. Moreover, the urinary excretion of both hyaluronic and sulfated glycosaminoglycans markedly decreased among DD patients.Our findings indicate that specific proteoglycans with galactosaminoglycan chains and collagen arrangements could serve as biomarkers for DD progression. The reduction in glycosaminoglycan excretion suggests a systemic manifestation of the disease. Full article

The combustion process is complex and harsh, and the supersonic combustion flow field is also characterized by short duration and supersonic speed, which makes the real-time diagnostic technology for the transient environment extremely demanding. It is of great significance to realize high time-resolved accurate measurement of temperature, component concentration, and other parametric information of the combustion field to study the transient chemical reaction dynamics of the combustion field. Femtosecond CARS spectroscopy can effectively avoid the collision effect between particles in the measurement process and reduce the influence of the non-resonant background to improve the measurement accuracy and realize the time-resolved measurement on a millisecond scale. This paper introduces the development history of femtosecond CARS spectroscopy, points out its advantages and disadvantages, and looks forward to the future development trend to carry out high time-resolved measurements, establish a database of temperature changes in various complex combustion fields, and provide support for the study of engine mechanisms. Full article

Despite their relatively low incidence globally, central nervous system (CNS) tumors remain amongst the most lethal cancers, with only a few other malignancies surpassing them in 5-year mortality rates. Treatment decisions for brain tumors heavily rely on histopathological analysis, particularly intraoperatively, to guide surgical interventions and optimize patient outcomes. Frozen sectioning has emerged as a vital intraoperative technique, allowing for highly accurate, rapid analysis of tissue samples, although it poses challenges regarding interpretive errors and tissue distortion. Raman histology, based on Raman spectroscopy, has shown great promise in providing label-free, molecular information for accurate intraoperative diagnosis, aiding in tumor resection and the identification of neurodegenerative disease. Techniques including Stimulated Raman Scattering (SRS), Coherent Anti-Stokes Raman Scattering (CARS), Surface-Enhanced Raman Scattering (SERS), and Tip-Enhanced Raman Scattering (TERS) have profoundly enhanced the speed and resolution of Raman imaging. Similarly, Confocal Laser Endomicroscopy (CLE) allows for real-time imaging and the rapid intraoperative histologic evaluation of specimens. While CLE is primarily utilized in gastrointestinal procedures, its application in neurosurgery is promising, particularly in the context of gliomas and meningiomas. This review focuses on discussing the immense progress in intraoperative histology within neurosurgery and provides insight into the impact of these advancements on enhancing patient outcomes. Full article

The influence of the interference between coherent processes in third-order nonlinear Raman scattering on the spectral shapes of Raman-scattered light waves is numerically modeled and discussed in the cases of commonly used coherent Raman spectroscopy techniques. The effects on the lineshapes depending on the laser intensity are analyzed for the coherent Raman spectroscopy performed via the excitation of molecular systems with focused laser pulses at high intensities. In this case, the interplay between the coherent processes in nonlinear Raman scattering, as well as laser power-induced resonance effects, may be significant and should be taken into account in the spectral lineshape analysis in coherent Raman spectroscopy and its related applications, since the coherent Raman spectra may be considerably modified. Full article

Simultaneous gas phase temperature and water vapor concentration measurement are important to understand reacting flows such as combustion or gas reforming processes. Here, coherent anti-Stokes Raman scattering (CARS) offers the possibility for non-intrusive measurements with a high temporal and spatial resolution. Therefore, this work demonstrates the simultaneous measurement of temperature and relative water vapor–nitrogen concentrations by using dual-pump vibrational coherent anti-Stokes Raman scattering (DPVCARS). A calibration procedure is developed for a temperature range of 473 K to 673 K and a water vapor concentration of 24% to 46% at ambient pressure. This setup is tested with 500 CARS single pulse spectra taken in a gas cell at a known temperature and concentration. Based on these results, information about precision and accuracy can be delivered. Full article

Information on the penetration depth, pathways, metabolization, storage of vehicles, active pharmaceutical ingredients (APIs), and functional cosmetic ingredients (FCIs) of topically applied formulations or contaminants (substances) in skin is of great importance for understanding their interaction with skin targets, treatment efficacy, and risk assessment—a challenging task in dermatology, cosmetology, and pharmacy. Non-invasive methods for the qualitative and quantitative visualization of substances in skin in vivo are favored and limited to optical imaging and spectroscopic methods such as fluorescence/reflectance confocal laser scanning microscopy (CLSM); two-photon tomography (2PT) combined with autofluorescence (2PT-AF), fluorescence lifetime imaging (2PT-FLIM), second-harmonic generation (SHG), coherent anti-Stokes Raman scattering (CARS), and reflectance confocal microscopy (2PT-RCM); three-photon tomography (3PT); confocal Raman micro-spectroscopy (CRM); surface-enhanced Raman scattering (SERS) micro-spectroscopy; stimulated Raman scattering (SRS) microscopy; and optical coherence tomography (OCT). This review summarizes the state of the art in the use of the CLSM, 2PT, 3PT, CRM, SERS, SRS, and OCT optical methods to study skin penetration in vivo non-invasively (302 references). The advantages, limitations, possibilities, and prospects of the reviewed optical methods are comprehensively discussed. The ex vivo studies discussed are potentially translatable into in vivo measurements. The requirements for the optical properties of substances to determine their penetration into skin by certain methods are highlighted. Full article

Interfacial compositions of fat globules modulate the digestion behaviour of milk triglycerides in the gastrointestinal tract, thereby affecting lipid metabolism and delivery of nutrients. In this study, we aim to understand the impact of emulsifiers on lipid digestibility and the self-assembled liquid crystal structures formed by anhydrous milk fat (AMF) during digestion. AMF was emulsified with casein and milk phospholipids, and digestion was performed in both gastric and small intestinal conditions to account for changes at the oil/water interface following enzymatic digestion in the gastric phase. Small angle X-ray scattering was used to characterise the self-assembled structures of the digestion products, while coherent anti-Stokes Raman scattering microscopy was utilised to probe changes in lipid distribution at the single droplet level during digestion. Our findings confirmed that emulsifiers play a key role in the digestion of AMF. Milk phospholipids exhibited a protective effect on milk triglycerides against pancreatic lipase digestion by slowing digestion, but this effect was slightly negated in emulsions pre-digested under gastric conditions. The overall types of liquid crystal structures formed after digestion of casein- and milk phospholipids-emulsified AMF were comparable to commercial bovine milk irrespective of gastric pre-treatment. However, emulsification of AMF with milk phospholipids resulted in changes in the microstructures of the liquid crystal phases, suggesting potential interactions between the digested products of the fat globules and milk phospholipids. This study highlights the importance of emulsifiers in regulating lipid digestion behaviour and lipid self-assembly during digestion. Full article

Cryopreservation has emerged as a low-maintenance, cost-effective solution for the long-term preservation of vegetatively propagated crops. Shoot tip cryopreservation often makes use of vitrification methods that employ highly concentrated mixtures of cryoprotecting agents; however, little is understood as to how these cryoprotecting agents protect cells and tissues from freezing. In this study, we use coherent anti-Stokes Raman scattering microscopy to directly visualize where dimethyl sulfoxide (DMSO) localizes within Mentha × piperita shoot tips. We find that DMSO fully penetrates the shoot tip tissue within 10 min of exposure. Variations in signal intensities across images suggest that DMSO may interact with cellular components, leading to its accumulation in specific regions. Full article

In view of the uncertainty in the calibration process of two-color plane laser-induced fluorescence (PLIF) temperature measurement, a new calibration method is proposed, in which the influence of fluorescence yield is considered. The calibration process was carried out at high and low temperature region, respectively. Then, the bias of thermometry results origin from quenching is restrained. This new calibration method is validated in a jet flame with temperature range of 1300–1800 K. Here, the temperature results from Coherent Anti-Stokes Raman scattering (CARS), single-point calibrated PLIF, and two-point calibrated PLIF are all acquired with the maximum standard errors of 13 K, 36 K, and 37 K, respectively. The temperature deviation between the average results from PLIF and Coherent Anti-Stokes Raman scattering (CARS) is 120 K and 10 K, when the two-point and one-point calibration methods are used. Therefore, the two-point calibrated PLIF is preferred in the combustion field, especially with a large temperature range and strong quenching coefficient. Full article

Long-term, repeatable monitoring of the appearance and progress of Alzheimer’s disease (AD) in real time can be extremely beneficial to acquire highly reliable diagnostic insights, which is crucial for devising apt strategies towards effective AD treatment. Herein, we present an optimized innovative cranial window imaging method for the long-term repeatable imaging of amyloid-β (Aβ) plaques and vessels in an AD mouse model. Basically, two-photon excitation fluorescence (TPEF) microscopy was used to monitor the fluorescently labeled Aβ plaques, whereas the label-free blood vessels were studied using coherent anti-Stokes Raman scattering (CARS) microscopy in the live in vivo AD mouse model. It was possible to clearly observe the Aβ deposition and vascular structure in the target cortex localization for 31 weeks in the AD mouse model using this method. The combined TPEF/CARS imaging studies were also instrumental in realizing the relationship between the tendency of Aβ deposition and ageing. Essentially, the progression of cerebral amyloid angiopathy (CAA) in the AD mouse model was quantitatively characterized, which revealed that the proportion Aβ deposition in the unit vessel can increase from 13.63% to 28.80% upon increasing the age of mice from 8 months old to 14 months old. The proposed imaging method provided an efficient, safe, repeatable platform with simple target localization aptitude towards monitoring the brain tissues, which is an integral part of studying any brain-related physiological or disease conditions to extract crucial structural and functional information. Full article