Laser spectroscopy imaging technique coupled withnanomaterials for cancer diagnosis: A review

Laser spectroscopic imaging techniques have received tremendous attention in the-eld of cancer diagnosis due to their high sensitivity,high temporal resolution,and short acquisition time.However,the limited tissue penetration of the laser is still a challenge for the in vivo diagnosis of deep-seated lesions.Nanomaterials have been universally integrated with spectroscopic imaging techniques for deeper cancer diagnosis in vivo.The components,morphology,and sizes of nanomaterials are delicately designed,which could realize cancer diagnosis in vivo or in situ.Considering the enhanced signal emitting from the nanomaterials,we emphasized their combination with spectroscopic imaging techniques for cancer diagnosis,like the surface-enhanced Raman scattering(SERS),photoacoustic,fluorescence,and laser-induced breakdown spectroscopy(LIBS).Applications ofthe above spectroscopic techniques offer new prospectsfor cancer diagnosis.

Two-photon live imaging of direct glia-to-neuron conversion in the mouse cortex

Over the past decade,a growing number of studies have reported transcription factor-based in situ reprogramming that can directly conve rt endogenous glial cells into functional neurons as an alternative approach for n euro regeneration in the adult mammalian central ne rvous system.Howeve r,many questions remain regarding how a terminally differentiated glial cell can transform into a delicate neuron that forms part of the intricate brain circuitry.In addition,concerns have recently been raised around the absence of astrocyte-to-neuron conversion in astrocytic lineage-tra cing mice.In this study,we employed repetitive two-photon imaging to continuously capture the in situ astrocyte-to-neuron conversion process following ecto pic expression of the neural transcription factor NeuroD1 in both prolife rating reactive astrocytes and lineage-tra ced astrocytes in the mouse cortex.Time-lapse imaging over several wee ks revealed the ste p-by-step transition from a typical astrocyte with numero us short,tapered branches to a typical neuro n with a few long neurites and dynamic growth cones that actively explored the local environment.In addition,these lineage-converting cells were able to migrate ra dially or to ngentially to relocate to suitable positions.Furthermore,two-photon Ca2+imaging and patch-clamp recordings confirmed that the newly generated neuro ns exhibited synchronous calcium signals,repetitive action potentials,and spontaneous synaptic responses,suggesting that they had made functional synaptic connections within local neural circuits.In conclusion,we directly visualized the step-by-step lineage conversion process from astrocytes to functional neurons in vivo and unambiguously demonstrated that adult mammalian brains are highly plastic with respect to their potential for neuro regeneration and neural circuit reconstruction.

Functional near-infrared spectroscopy in non-invasive neuromodulation

Non-invasive cerebral neuromodulation technologies are essential for the reorganization of cerebral neural networks,which have been widely applied in the field of central neurological diseases,such as stroke,Parkinson’s disease,and mental disorders.Although significant advances have been made in neuromodulation technologies,the identification of optimal neurostimulation paramete rs including the co rtical target,duration,and inhibition or excitation pattern is still limited due to the lack of guidance for neural circuits.Moreove r,the neural mechanism unde rlying neuromodulation for improved behavioral performance remains poorly understood.Recently,advancements in neuroimaging have provided insight into neuromodulation techniques.Functional near-infrared spectroscopy,as a novel non-invasive optical brain imaging method,can detect brain activity by measuring cerebral hemodynamics with the advantages of portability,high motion tole rance,and anti-electromagnetic interference.Coupling functional near-infra red spectroscopy with neuromodulation technologies offe rs an opportunity to monitor the cortical response,provide realtime feedbac k,and establish a closed-loop strategy integrating evaluation,feedbac k,and intervention for neurostimulation,which provides a theoretical basis for development of individualized precise neuro rehabilitation.We aimed to summarize the advantages of functional near-infra red spectroscopy and provide an ove rview of the current research on functional near-infrared spectroscopy in transcranial magnetic stimulation,transcranial electrical stimulation,neurofeedback,and braincomputer interfaces.Furthermore,the future perspectives and directions for the application of functional near-infrared spectroscopy in neuromodulation are summarized.In conclusion,functional near-infrared spectroscopy combined with neuromodulation may promote the optimization of central pellral reorganization to achieve better functional recovery form central nervous system diseases.

A rened analytical model for reconstruction problems in diuse reectance spectroscopy

A rened analytical model of spatially resolved diffuse reectance with small source-detector separations(SDSs)for the in vivo skin studies is proposed.Compared to the conventional model developed by Farrell et al.,it accounts for the limited acceptance angle of the detectorber.The rened model is validated in the wide range of optical parameters by Monte Carlo simulations of skin diffuse reectance at SDSs of units of mm.Cases of uniform dermis and two-layered epidermis-dermis structures are studied.Higher accuracy of the rened model compared to the conventional one is demonstrated in the separate,constraint-free reconstruction of absorption and reduced scattering spectra of uniform dermis from the Monte Carlo simulated data.In the case of epidermis-dermis geometry,the recovered values of reduced scattering in dermis are overestimated and the recovered values of absorption are underestimated for both analytical models.Presumably,in the presence of a thin mismatched topical layer,only the effective attenuation coe±cient of the bottom layer can be accurately recovered using a diffusion theorybased analytical model while separate reconstruction of absorption and reduced scattering fails due to the inapplicability of the method of images.These-ndings require implementation of more sophisticated models of light transfer in inhomogeneous media in the recovery algorithms.

In situ infrared, Raman and X-ray spectroscopy for the mechanistic understanding of hydrogen evolution reaction

Hydrogen production by water reduction reactions has received considerable attention because hydrogen is considered a clean-energy carrier,key for a sustainable energy future.Computational methods have been widely used to study the reaction mechanism of the hydrogen evolution reaction(HER),but the calculation results need to be supported by experimental results and direct evidence to confirm the mechanistic insights.In this review,we discuss the fundamental principles of the in situ spectroscopic strategy and a theoretical model for a mechanistic understanding of the HER.In addition,we investigate recent studies by in situ Fourier transform infrared(FTIR),Raman spectroscopy,and X-ray absorption spectroscopy(XAS) and cover new findings that occur at the catalyst-electrolyte interface during HER.These spectroscopic strategies provide practical ways to elucidate catalyst phase,reaction intermediate,catalyst-electrolyte interface,intermediate binding energy,metal valency state,and coordination environment during HER.

Temperature-feedback two-photon-responsive metal-organic frameworks for efficient photothermal therapy

The realization of real-time thermal feedback for monitoring photothermal therapy(PTT)under near-infrared(NIR)light irradiation is of great interest and challenge for antitumor therapy.Herein,by assembling highly efficient photothermal conversion gold nanorods and a temperature-responsive probe((E)-4-(4-(diethylamino)styryl)-1-methylpyridin-1-ium,PyS)within MOF-199,an intelligent nanoplatform(AMPP)was fabricated for simultaneous chemodynamic therapy and NIR light-induced temperature-feedback PTT.The fluorescence intensity and temperature of the PyS probe are linearly related due to the restriction of the rotation of the characteristic monomethine bridge.Moreover,the copper ions resulting from the degradation of MOF-199 in an acidic microenvironment can convert H_(2)O_(2)into•OH,resulting in tumor ablation through a Fenton-like reaction,and this process can be accelerated by increasing the temperature.This study establishes a feasible platform for fabricating highly sensitive temperature sensors for efficient temperature-feedback PTT.

Two-photon polymerization lithography for imaging optics

Optical imaging systems have greatly extended human visual capabilities,enabling the observation and understanding of diverse phenomena.Imaging technologies span a broad spectrum of wavelengths from x-ray to radio frequencies and impact research activities and our daily lives.Traditional glass lenses are fabricated through a series of complex processes,while polymers offer versatility and ease of production.However,modern applications often require complex lens assemblies,driving the need for miniaturization and advanced designs with micro-and nanoscale features to surpass the capabilities of traditional fabrication methods.Three-dimensional(3D)printing,or additive manufacturing,presents a solution to these challenges with benefits of rapid prototyping,customized geometries,and efficient production,particularly suited for miniaturized optical imaging devices.Various 3D printing methods have demonstrated advantages over traditional counterparts,yet challenges remain in achieving nanoscale resolutions.Two-photon polymerization lithography(TPL),a nanoscale 3D printing technique,enables the fabrication of intricate structures beyond the optical diffraction limit via the nonlinear process of two-photon absorption within liquid resin.It offers unprecedented abilities,e.g.alignment-free fabrication,micro-and nanoscale capabilities,and rapid prototyping of almost arbitrary complex 3D nanostructures.In this review,we emphasize the importance of the criteria for optical performance evaluation of imaging devices,discuss material properties relevant to TPL,fabrication techniques,and highlight the application of TPL in optical imaging.As the first panoramic review on this topic,it will equip researchers with foundational knowledge and recent advancements of TPL for imaging optics,promoting a deeper understanding of the field.By leveraging on its high-resolution capability,extensive material range,and true 3D processing,alongside advances in materials,fabrication,and design,we envisage disruptive solutions to current challenges and a promising incorporation of TPL in future optical imaging applications.

Near Infrared Spectroscopy (NIRS) Model-Based Prediction for Protein Content in Cowpea

Cowpea (Vigna unguiculata L. Walp) is a multi-purpose legume with high quality protein for human consumption and livestock. The objective of this work was to develop near-infrared spectroscopy (NIRS) prediction models to estimate protein content in cowpea. A total of 116 cowpea breeding lines with a wide range of protein contents (19.28 % to 32.04%) were selected to build the model using whole seed and ground seed samples. Partial least-squares discriminant analysis (PLS-DA) regression technique with different pre-treatments (derivatives, standard normal variate, and multiplicative scatter correction) were carried out to develop the protein prediction model. Results showed: 1) spectral plots of both the whole seed and ground seed showed higher spectral scatter at higher wavelengths (>1450 nm), 2) data pre-processing affects prediction accuracy for bot whole seed and ground seed samples, 3) prediction using ground seed samples (0.64 R2 0.85) is better than the whole seed (0.33 R2 0.78), and 4) the data pre-processing second derivative with standard normal variate has the best prediction (R2_whole seed = 0.78, R2_ground seed = 0.85). The results will be of interest in cowpea breeding programs aimed at improving total seed protein content.

Investigation on Binding between Cations and Amides using UV Raman Spectroscopy

The interaction of proteins with salt ions plays an important role in life activities.We used butyramide as a model molecule to investigate the interaction of protein backbones with cations.The experiment was performed in an aqueous solution of metal chloride using UV Raman spectroscopy.It was found that well-hydrated metal cations(Ca^(2+),Mg^(2+))tend to bind to C=O in the amide bond,resulting in redistribution of the amide I band peaks.Specifically,the peak intensity ratio of 1655 cm^(-1)to 1610 cm^(-1)increases significantly with increasing concentrations.However,this phenomenon is not obviously observed in NaCl solution.Furthermore,we studied the effect of salt ions on the water structures.The addition of Ca^(2+)and Mg^(2+)is beneficial to the enhancement of the water signal at the 3400 cm^(-1)position,while the Na^(+)at the same concentration is not obvious.The results have shown that the interaction between cations and amides satisfies the following order:Ca^(2+)>Mg^(2+)>Na^(+),which conforms to the Hofmeister series.

A dual-route optical emission spectroscopy diagnostic with wide spectral range and high wavelength resolution on HL-2A tokamak

A dual-route optical emission spectroscopy(D-OES)diagnostic is newly developed to monitor the optical emission from the X-point plasma region on the HL-2 A tokamak.This diagnostic is composed of an imaging system,a beam-splitting system for dual-route measurements,fiber bundles,a spectrometer system,and a control and acquisition system.One route is used to obtain wide-spectral-range spectra,and the other route is used to acquire high-wavelengthresolution line shapes.The spectral resolution of the wide-range spectrometers is 0.8 nm with a coverage of 800 nm(@200-1000 nm).The spectral resolution of the high-resolution spectrometer is 0.01 nm with a coverage of 6 nm(@200-660 nm).The spatial resolution of each route of D-OES is about 4 cm with 11 channels.The temporal resolution is 16 ms at maximum in the single-channel mode.Wide-range spectra(containing Balmer series and a Fulcher band)and highly resolved Ha line shapes are obtained by D-OES in the hydrogen glow discharge in the lab.D-OES measurements are carried out in the high-density deuterium experiments of HL-2A.The electron density n_(e)and deuterium temperature T_(D) in the X-point multifaceted asymmetric radiation from the edge(MARFE)region are derived simultaneously by fitting the measured D_(a) shape.The density n_(e)is observed to increase from~8.7×10^(18)m^(-3)to~7.8×10^(19)m^(-3),and the temperature T_(D)drops from~14.4 eV to~2.3 eV after the onset of MARFE in the discharge#38260.

Core-level spectroscopy of the photodissociation process of BrCN molecule

Fewest-switches surfacing hopping(FSSH) simulations have been performed with the high-level multi-reference electronic structure method to explore the coupled electronic and nuclear dynamics upon photoexcitation of cyanogen bromide(BrCN). The potential energy surfaces(PES) of BrCN are charted as functions of the Jacobi coordinates(R, θ). An indepth examination of the FSSH trajectories reveals the temporal dynamics of the molecule and the population changes of the lowest twelve states during BrCN's photodissociation process, which presents a rich tapestry of dynamical information.Furthermore, the carbon K-edge x-ray absorption spectroscopy(XAS) is calculated with multi-reference inner-shell spectral simulations. The rotation of the CN fragment and the elongation of the C–Br bond are found to be the reason for the peak shifting in the XAS. Our findings offer a nuanced interpretation for inner-shell probe investigations of BrCN, setting the stage for a deeper understanding of the photodissociation process of cyanogen halides molecules.

Negligible normal fluid in superconducting state of heavily overdoped Bi_(2)Sr_(2)CaCu_(2)O_(8+δ) detected by ultra-low temperature angle-resolved photoemission spectroscopy

In high temperature cuprate superconductors,it was found that the superfluid density decreases with the increase of hole doping.One natural question is whether there exists normal fluid in the superconducting state in the overdoped region.In this paper,we have carried out high-resolution ultra-low temperature laser-based angle-resolved photoemission measurements on a heavily overdoped Bi2212 sample with a T_(c) of 48 K.We find that this heavily overdoped Bi2212 remains in the strong coupling regime with 2Δ_(0)/(k_(B)T_(c))=5.8.The single-particle scattering rate is very small along the nodal direction(~5 meV) and increases as the momentum moves from the nodal to the antinodal regions.A hard superconducting gap opening is observed near the antinodal region with the spectral weight at the Fermi level fully suppressed to zero.The normal fluid is found to be negligibly small in the superconducting state of this heavily overdoped Bi2212.These results provide key information to understand the high T_(c) mechanism in the cuprate superconductors.

Estimating the yield stress of soft materials via laser-induced breakdown spectroscopy

Taking three typical soft samples prepared respectively by loose packings of 77-,95-,and 109-μm copper grains as examples,we perform an experiment to investigate the energy-dependent laser-induced breakdown spectroscopy(LIBS)of soft materials.We discovered a reversal phenomenon in the trend of energy dependence of plasma emission intensity:increasing initially and then decreasing separated by a well-defined critical energy.The trend reversal is attributed to the laser-induced recoil pressure at the critical energy just matching the sample's yield strength.As a result,a one-to-one correspondence can be well established between the samples'yield stress and the critical energy that is easily obtainable from LIBS measurements.This allows us to propose an innovative method for estimating the yield stress of soft materials via LIBS with attractive advantages including in-situ remote detection,real-time data collection,and minimal destructive to sample.

Research on batch multielement rapid quantitative analysis based on the standard curve-assisted calibration-free laserinduced breakdown spectroscopy method

This study proposes a batch rapid quantitative analysis method for multiple elements by combining the advantages of standard curve(SC)and calibration-free laser-induced breakdown spectroscopy(CF-LIBS)technology to achieve synchronous,rapid,and accurate measurement of elements in a large number of samples,namely,SC-assisted CF-LIBS.Al alloy standard samples,divided into calibration and test samples,were applied to validate the proposed method.SC was built based on the characteristic line of Pb and Cr in the calibration sample,and the contents of Pb and Cr in the test sample were calculated with relative errors of 6%and 4%,respectively.SC built using Cr with multiple characteristic lines yielded better calculation results.The relative contents of ten elements in the test sample were calculated using CF-LIBS.Subsequently,the SC-assisted CF-LIBS was executed,with the majority of the calculation relative errors falling within the range of 2%-5%.Finally,the Al and Na contents of the Al alloy were predicted.The results demonstrate that it effectively enables the rapid and accurate quantitative analysis of multiple elements after a single-element SC analysis of the tested samples.Furthermore,this quantitative analysis method was successfully applied to soil and Astragalus samples,realizing an accurate calculation of the contents of multiple elements.Thus,it is important to advance the LIBS quantitative analysis and its related applications.

Wavelength calibration and spectral analysis of vacuum ultraviolet spectroscopy in EAST

A vacuum ultraviolet(VUV)spectroscopy with a focal length of 1 m has been engineered specifically for observing edge impurity emissions in Experimental Advanced Superconducting Tokamak(EAST).In this study,wavelength calibration for the VUV spectroscopy is achieved utilizing a zinc lamp.The grating angle and charge-coupled device(CCD)position are carefully calibrated for different wavelength positions.The wavelength calibration of the VUV spectroscopy is crucial for improving the accuracy of impurity spectral data,and is required to identify more impurity spectral lines for impurity transport research.Impurity spectra of EAST plasmas have also been obtained in the wavelength range of 50–300 nm with relatively high spectral resolution.It is found that the impurity emissions in the edge region are still dominated by low-Z impurities,such as carbon,oxygen,and nitrogen,albeit with the application of fulltungsten divertors on the EAST tokamak.

Laser-induced breakdown spectroscopy as a method for millimeter-scale inspection of surface flatness

A non-contact method for millimeter-scale inspection of material surface flatness via Laser-Induced Breakdown Spectroscopy(LIBS)is investigated experimentally.The experiment is performed using a planished surface of an alloy steel sample to simulate its various flatness,ranging from 0 to 4.4 mm,by adjusting the laser focal plane to the surface distance with a step length of 0.2 mm.It is found that LIBS measurements are successful in inspecting the flatness differences among these simulated cases,implying that the method investigated here is feasible.It is also found that,for achieving the inspection of surface flatness within such a wide range,when univariate analysis is applied,a piecewise calibration model must be constructed.This is due to the complex dependence of plasma formation conditions on the surface flatness,which inevitably complicates the inspection procedure.To solve the problem,a multivariate analysis with the help of Back-Propagation Neural Network(BPNN)algorithms is applied to further construct the calibration model.By detailed analysis of the model performance,we demonstrate that a unified calibration model can be well established based on BPNN algorithms for unambiguous millimeter-scale range inspection of surface flatness with a resolution of about 0.2 mm.

Quantifying the chemical composition of weathering products of Hainan basalts with reflectance spectroscopy and its implications for Mars

With the development of the hyperspectral remote sensing technique,extensive chemical weathering profiles have been identified on Mars.These weathering sequences,formed through precipitation-driven leaching processes,can reflect the paleoenvironments and paleoclimates during pedogenic processes.The specific composition and stratigraphic profiles mirror the mineralogical and chemical trends observed in weathered basalts on Hainan Island in south China.In this study,we investigated the laboratory reflectance spectra of a 53-m-long drilling core of a thick basaltic weathering profile collected from Hainan Island.We established a quantitative spectral model by combining the genetic algorithm and partial least squares regression(GA-PLSR)to predict the chemical properties(SiO2,Al2O3,Fe2O3)and index of laterization(IOL).The entire sample set was divided into a calibration set of 25 samples and a validation set of 12 samples.Specifically,the GA was used to select the spectral subsets for each composition,which were then input into the PLSR model to derive the chemical concentration.The coefficient of determination(R2)values on the validation set for SiO2,Al2O3,Fe2O3,and the IOL were greater than 0.9.In addition,the effects of various spectral preprocessing techniques on the model accuracy were evaluated.We found that the spectral derivative treatment boosted the prediction accuracy of the GA-PLSR model.The improvement achieved with the second derivative was more pronounced than when using the first derivative.The quantitative model developed in this work has the potential to estimate the contents of similar weathering basalt products,and thus infer the degree of alteration and provide insights into paleoclimatic conditions.Moreover,the informative bands selected by the GA can serve as a guideline for designing spectral channels for the next generation of spectrometers.

Initial measurement of ultrafast charge exchange recombination spectroscopy on the EAST tokamak

Ultrafast charge exchange recombination spectroscopy(UF-CXRS)has been developed on the EAST tokamak(Yingying Li et al 2019 Fusion Eng.Des.146522)to measure fast evolutions of ion temperature and toroidal velocity.Here,we report the preliminary diagnostic measurements after relative sensitivity calibration.The measurement results show a much higher temporal resolution compared with conventional CXRS,benefiting from the usage of a prismcoupled,high-dispersion volume-phase holographic transmission grating and a high quantum efficiency,high-gain detector array.Utilizing the UF-CXRS diagnostic,the fast evolutions of the ion temperature and rotation velocity during a set of high-frequency small-amplitude edgelocalized modes(ELMs)are obtained on the EAST tokamak,which are then compared with the case of large-amplitude ELMs.

Ultrafast carrier dynamics in GeSn thin film based on time-resolved terahertz spectroscopy

We measure the time-resolved terahertz spectroscopy of GeSn thin film and studied the ultrafast dynamics of its photo-generated carriers.The experimental results show that there are photo-generated carriers in GeSn under femtosecond laser excitation at 2500 nm,and its pump-induced photoconductivity can be explained by the Drude–Smith model.The carrier recombination process is mainly dominated by defect-assisted Auger processes and defect capture.The firstand second-order recombination rates are obtained by the rate equation fitting,which are(2.6±1.1)×10^(-2)ps^(-1)and(6.6±1.8)×10^(-19)cm^(3)·ps^(-1),respectively.Meanwhile,we also obtain the diffusion length of photo-generated carriers in GeSn,which is about 0.4μm,and it changes with the pump delay time.These results are important for the GeSn-based infrared optoelectronic devices,and demonstrate that Ge Sn materials can be applied to high-speed optoelectronic detectors and other applications.

Application of a neural network model with multimodal fusion for fluorescence spectroscopy

In energy-dispersive X-ray fluorescence spectroscopy,the estimation of the pulse amplitude determines the accuracy of the spectrum measurement.The error generated by the amplitude estimation of the pulse output distorted by the measurement system leads to false peaks in the measured spectrum.To eliminate these false peaks and achieve an accurate estimation of the distorted pulse amplitude,a composite neural network model is proposed,which embeds long and short-term memory(LSTM)into the UNet structure.The UNet network realizes the fusion of pulse sequence features and the LSTM model realizes pulse amplitude estimation.The model is trained using simulated pulse datasets with different amplitudes and distortion times.For the pulse height estimation,the average relative error of the trained model on the test set was approximately 0.64%,which is 27.37% lower than that of the traditional trapezoidal shaping algorithm.Offline processing of a standard iron source further validated the pulse height estimation performance of the UNet-LSTM model.After estimating the amplitude of the distorted pulses using the model,the false peak area was reduced by approximately 91% over the full spectrum and was corrected to the characteristic peak region of interest(ROI).The corrected peak area accounted for approximately 1.32%of the characteristic peak ROI area.The results indicate that the model can accurately estimate the height of distorted pulses and has substantial corrective effects on false peaks.