Simultaneous measurements of global vibrational spectra and dephasing times of molecular vibrational modes by broadband time-resolved coherent anti-Stokes Raman scattering spectrography

In broadband coherent anti-Stokes Raman scattering （CARS） spectroscopy with supercontinuum （SC）, the simultaneously detectable spectral coverage is limited by the spectral continuity and the simultaneity of various spectral components of SC in an enough bandwidth. By numerical simulations, the optimal experimental conditions for improving the SC are obtained. The broadband time-resolved CARS spectrography based on the SC with required temporal and spectral distributions is realised. The global molecular vibrational spectrum with well suppressed nonresonant background noise can be obtained in a single measurement. At the same time, the measurements of dephasing times of various molecular vibrational modes can be conveniently achieved from intensities of a sequence of time-resolved CARS signals. It will be more helpful to provide a complete picture of molecular vibrations, and to exhibit a potential to understand not only both the solvent dynamics and the solute-solvent interactions, but also the mechanisms of chemical reactions in the fields of biology, chemistry and material science.

Selective excitation of molecular mode in a mixture by femtosecond resonance-enhanced coherent anti-Stokes Raman scattering spectroscopy

Femtosecond time-resolved coherent anti-Stokes Raman scattering （CARS） spectroscopy is used to investigate gaseous molecular dynamics. Due to the spectrally broad laser pulses, usually poorly resolved spectra result from this broad spectroscopy. However, it can be demonstrated that by the electronic resonance enhancement optimization control a selective excitation of specific vibrational mode is possible. Using an electronically resonance-enhanced effect, iodine molecule specific CARS spectroscopy can be obtained from a mixture of iodine-air at room temperature and a pressure of 1 atm （corresponding to a saturation iodine vapour as low as about 35 Pa）. The dynamics on either the electronically excited state or the ground state of iodine molecules obtained is consistent with previous studies （vacuum, heated and pure iodine） in the femtoseeond time resolved CARS spectroscopy, showing that an effective method of suppressing the non-resonant CARS background and other interferences is demonstrated.

Selective excitation and suppression of coherent anti-Stokes Raman scattering by shaping femtosecond pulses

Femtosecond coherent anti-Stokes Raman scattering （CARS） suffers from poor selectivity between neighbouring Raman levels due to the large bandwidth of the femtosecond pulses. This paper provides a new method to realize the selective excitation and suppression of femtosecond CARS by manipulating both the probe and pump （or Stokes） spectra. These theoretical results indicate that the CARS signals between neighbouring Raman levels are differentiated from their indistinguishable femtosecond CARS spectra by tailoring the probe spectrum, and then their selective excitation and suppression can be realized by supplementally manipulating the pump （or Stokes） spectrum with the π spectral phase step.

Coherent coupling between vibrational modes of C-H bonds at different positions studied by femtosecond time-resolved coherent anti-Stokes Raman scattering

We performed femtosecond time-resolved coherent anti-Stokes Raman scattering （fs-CARS） measurements on liquid toluene and PVK film. For both samples, we selectively excited the CH stretching vibrational modes and observed the expected quantum beat signals. The frequency of the well-defined beats is in good agreement with the energy difference between the two simultaneously excited modes, which demonstrates that a coherent coupling between the vibrational modes of the C H chemical bonds exists at the different positions of the molecules. The dephasing times of the excited modes are obtained simultaneously.

Supercontinuum fiber laser-based coherent anti-Stokes Raman scattering microscopy for label-free chemical imaging

Coherent anti-Stokes Raman scattering(CA RS)microscopy can resolve the chemical compo-nents and distribution of living biological systems in a label-firee manner and is favored in several disciplines.Current CA RS microscopes typically use bulky,high-performance solid-state lasers,which are expensive and sensitive to environmental changes.With their relatively low cost and environmental sensitivity,supercontinum fiber(SF)lasers with a small footprint have found increasing use in biomedical applications.Upon these features,in this paper,we homebuilt a low-cost CARS microscope based on a SF laser module(scCA RS microscope).This SF laser module is specially customized by adding a time synchronized seed source channel to the SF laser to form a dual-channel output laser.The performance of the scCARS microscope is evaluated with dimethyl sulfoxide,whose results confirm a spatial resolution of better than 500nm and a detection sensitivity of millimolar concentrations.The dual-color imaging capability is further demonstrated by imaging different species of mixed microspheres.We finally explore the potential of our scCARS microscope by mapping lipid droplets in different cancer cells and corneal stromal lenses.

High-resolution imaging of graphene by tip-enhanced coherent anti-Stokes Raman scattering

Coherent anti-Stokes Raman scattering(CARS)is able to enhance molecular signals by vibrational coherence compared to weak Raman signal.The surface or tip enhancement are successful technologies,which make it possible for Raman to detect single molecule with nanometer resolution.However,due to technical diffculties,tip-enhanced CARS(TECARS)is not as successful as expected.For single molecular detection,high sensitivity and resolution are two main challenges.Here,we reported the first single atom layer TECARS imaging on Graphene with the highest resolution about 20 nm,which has ever been reported.The highest EF_(TECARS/CARS) is about 10^(4),the similar order of magnitude with SECARS(EF of tip is usually smaller than that of substrates).Such resolution and sensitivity is promising for medical,biology and chemical applications in the future.

COHERENT ANTI-STOKES RAMAN SCATTERING MICROSCOPY TO MONITOR DRUG DISSOLUTION IN DIFFERENT ORAL PHARMACEUTICAL TABLETS

Coherent anti-Stokes Raman scattering(CARS)microscopy is used to visualize the release of a model drug(theophylline)from a lipid(tripalmitin)based tablet during dissolution.The effects of transformation and dissolution of the drug are imaged in real time.This study reveals that the manufacturing process causes significant differences in the release process:tablets prepared from powder show formation of theophylline monohydrate on the surface which prevents a controlled drug release,whereas solid lipid extrudates did not show formation of monohydrate.This visualization technique can aid future tablet design.

Wide-Field Vibrational Phase Contrast Imaging Based on Coherent Anti-Stokes Raman Scattering Holography

We propose and implement a wide-field vibrational phase contrast detection to obtain imaging of imaginary components of third-order nonlinear susceptibility in a coherent anti-Stokes Raman scattering （CARS） microscope with full suppression of the non-resonant background. This technique is based on the unique ability of recovering the phase of the generated CARS signal based on holographic recording. By capturing the phase distributions of the generated CARS field from the sample and from the environment under resonant illumination, we demonstrate the retrieval of imaginary components in the CARS microscope and achieve background free coherent Raman imaging.

Theoretical and experimental investigations of coherent phonon dynamics in sapphire crystal using femto-second time-resolved coherent anti-Stokes Raman scattering

We report on the theoretical and the experimental investigations of the coherent phonon dynamics in sapphire crystal using the femtosecond time-resolved coherent anti-Stokes Raman scattering （fs-CARS） technique. The temporal chirped white-light continuum （WLC） is used for the Stokes pulse, therefore we can perform the selective excitation of the phonon modes without using a complicated laser system. The expected quantum beat phenomenon is clearly observed. The theoretical formulas consist very well with the experimental results. The dephasing times of the excited phonon modes, the wavenumber difference, and the phase shift between the simultaneously excited modes are obtained and discussed. This work opens up a way to study directly high-frequency coherent phonon dynamics in bulk crystals on a femtosecond time scale and is especially helpful for understanding the nature of coherent phonons.

Analysis of detection limit to time-resolved coherent anti-Stokes Raman scattering nanoscopy

In the implementation of CARS nanoscopy, signal strength decreases with focal volume size decreasing. A crucial problem that remains to be solved is whether the reduced signal generated in the suppressed focal volume can be detected. Here reported is a theoretical analysis of detection limit （DL） to time-resolved CARS （T-CARS） nanoscopy based on our proposed additional probe-beam-induced phonon depletion （APIPD） method for the low concentration samples. In order to acquire a detailed shot-noise limited signal-to-noise （SNR） and the involved parameters to evaluate DL, the T-CARS process is described with full quantum theory to estimate the extreme power density levels of the pump and Stokes beams determined by saturation behavior of coherent phonons, which are both actually on the order of ~ 109 W/cm2. When the pump and Stokes intensities reach such values and the total intensity of the excitation beams arrives at a maximum tolerable by most biological samples in a certain suppressed focal volume （40-nm suppressed focal scale in APIPD method）, the DL correspondingly varies with exposure time, for example, DL values are 103 and 102 when exposure times are 20 ms and 200 ms respectively.

Selective Excitation of Two-pulse Femtosecond Coherent Anti-Stokes Raman Scattering in a Mixture

In this paper, we experimentally study the selective excitation of two-pulse femtosecond coherent anti-Stokes Raman scattering (CARS) in a mixture of dibromomethane (CH2Br2) and chloroform (CHCl3) by adaptive pulse shaping based on genetic algorithm. Second harmonic generation frequency-resolved optical gating (SHG-FROG) traces indicate that the spectral amplitude and phase of the optimal pulse are both modulated. Finally, we discuss the physical mechanism for the selective excitation of femtosecond CARS based on the retrieved information from SHG-FROG traces.

Comparison between Microwave Coherent and Incoherent Scattering Models in Corn Field

[Objective] The aim was to compare and analyze microwave coherent and incoherent scattering models in a corn field. [Method] In the research, based on a coherent scattering model （Stile）, we proposed a coherent scattering model exclusive for corn, in which, physical optics （PO） and infinite-length dielectric cylinder were used to calculate single-scattering matrices of corn leaves and stalks. In addition, coherent components produced from interaction among the scattering mechanisms were also considered and this coherent model was compared with the Michigan Mi- crowave Canopy Scattering （MIMICS） model. The measured data in a corn filed in Gongzhuling in Jilin Province were used as the input parameters of the coherent and incoherent models. We simulated backscattering coefficients of VV and HH po- larization at L and C bands and made a comparison between the simulation results. [Result] The simulation results at L-band were poor, which indicated that we could not find regularity at early growth stage of vegetation. In addition, comparisons be- tween coherent and incoherent scattering models proved that the coherence triggered by the scattering mechanism was small. [Conclusion] In the research, we analyzed differences between coherent and incoherent scattering models with change of incident angle, and further analysis on the differences with change of vegetation and soil needed to be made in future.

Imaging through scattering layers using a near-infrared low-spatial-coherence fiber random laser

Optical memory effect-based speckle-correlated technology has been developed for reconstructing hidden objectsfrom disordered speckle patterns,achieving imaging through scattering layers.However,the lighting efficiency and fieldof view of existing speckle-correlated imaging systems are limited.Here,a near-infrared low spatial coherence fiberrandom laser illumination method is proposed to address the above limitations.Through the utilization of random Rayleighscattering within dispersion-shifted fibers to provide feedback,coupled with stimulated Raman scattering for amplification,a near-infrared fiber random laser exhibiting a high spectral density and extremely low spatial coherence is generated.Based on the designed fiber random laser,speckle-correlated imaging through scattering layers is achieved,with highlighting efficiency and a large imaging field of view.This work improves the performance of speckle-correlated imagingand enriches the research on imaging through scattering medium.

Effect of CC Coherent Vibration on Relative Raman Scattering Cross Sections of All-trans β-Carotene

We have determined the Raman scattering cross sections（RSCSs） of fl-carotene for C=C and C-C stretching modes, with the 1444 cm^-1 Raman band of cyclohexane as internal standard, in different solvents at low concentrations by measuring Raman intensity. The results show that RSCSs of β-carotene were 10^6-10^7 times larger than the general RSCSs, we analyzed that this enhancement was caused not only by the resonance Raman effect but also by nonlinear coherent CC vibration in aqueous β-carotene. Moreover, overtone and combinations of it were also observed and their intensities were 10%-20% of those of their fundamentals when β-carotene was dissolved in non-polar solvents, respectively.

Incoherent and coherent beam combination for master oscillator/power amplifier system with stimulated Brillouin scattering mirror

In this paper, we studied incoherent and coherent beam combining for the master oscillator/power amplifier （MOPA） system with stimulated Brillouin scattering （SBS） mirror. Optic field intensity distributions in the near and far field are numerically calculated for the two kinds of system. The results show that good beam quality in the far field could be obtained. It provides a theoretical basis for experimental research in the future.

Coherent Raman scattering imaging of lipid metabolism in cancer

Cancer cells dysregulate lipid metabolism to accelerate energy production and biomolecule synthesis for rapid growth.Lipid metabolism is highly dynamic and intrinsically heterogeneous at the single cell level.Although°uorescence microscopy has been commonly used for cancer research,bulky°uorescent probes can hardly label small lipid molecules without perturbing their biological activities.Such a challenge can be overcome by coherent Raman scattering(CRS)microscopy,which is capable of chemically selective,highly sensitive,submicron resolution and high-speed imaging of lipid molecules in single live cells without any labeling.Recently developed hyperspectral and multiplex CRS microscopy enables quantitative mapping of various lipid metabolites in situ.Further incorporation of CRS microscopy with Raman tags greatly increases molecular selectivity based on the distinct Raman peaks well separated from the endogenous cellular background.Owing to these unique advantages,CRS microscopy sheds new insights into the role of lipid metabolism in cancer development and progression.This review focuses on the latest applications of CRS microscopy in the study of lipid metabolism in cancer.

Self-trapping Characteristics of Partially Coherent Optical Beam in Photonic Crystal Fiber under Compton Scattering

Using the mutually coherent function, the self-trapping of the circle partially coherent optical beam in the total internal reflective photonic crystal fiber(TIRPCF) under Compton scattering is studied. The study shows that the composition of the non-coherent optical beam in the optical spectrum and the diffraction effect are decreased by Compton scattering, and the probability of forming the soliton is greatly increased. The vibration peak value in the propagation, compressed degree, changed cycle, and radius of the soliton are all smaller than those before the scattering, but its coherent radius is larger than that before the scattering. In this propagation, the self-focusing plays a key role.

Far-zone behaviors of scattering-induced statistical properties of partially polarized spatially and spectrally partially coherent electromagnetic pulsed beam

In this study, we explore the far-zero behaviors of a scattered partially polarized spatially and spectrally partially coherent electromagnetic pulsed beam irradiating on a deterministic medium. The analytical formula for the cross-spectral density matrix elements of this beam in the spherical coordinate system is derived. Within the framework of the first-order Born approximation, the effects of the scattering angle θ, the source parameters (i.e., the pulse duration T0 and the temporal coherence length Tcxx), and the scatterer parameter (i.e., the effective width of the medium σR) on the spectral density, the spectral shift, the spectral degree of polarization, and the degree of spectral coherence of the scattered source in the far-zero field are studied numerically and comparatively. Our work improves the scattering theory of stochastic electromagnetic beams and it may be useful for the applications involving the interaction between incident light waves and scattering media.

Collective coherent emission of electrons in strong laser fields and perspective for hard x-ray lasers

Coherent motion of particles in a plasma can imprint itself on radiation.The recent advent of high-power lasers—allowing the nonlinear inverse Compton-scattering regime to be reached—has opened the possibility of looking at collective effects in laser–plasma interactions.Under certain conditions,the collective interaction of many electrons with a laser pulse can generate coherent radiation in the hard x-ray regime.This perspective paper explains the limitations under which such a regime might be attained.

Detecting spatio-temporal urban surface changes using identified temporary coherent scatterers

Synthetic aperture radar(SAR) is able to detect surface changes in urban areas with a short revisit time, showing its capability in disaster assessment and urbanization monitoring.Most presented change detection methods are conducted using couples of SAR amplitude images. However, a prior date of surface change is required to select a feasible image pair. We propose an automatic spatio-temporal change detection method by identifying the temporary coherent scatterers. Based on amplitude time series, χ^(2)-test and iterative single pixel change detection are proposed to identify all step-times: the moments of the surface change. Then the parameters, e.g., deformation velocity and relative height, are estimated and corresponding coherent periods are identified by using interferometric phase time series. With identified temporary coherent scatterers, different types of temporal surface changes can be classified using the location of the coherent periods and spatial significant changes are identified combining point density and F values. The main advantage of our method is automatically detecting spatio-temporal surface changes without prior information. Experimental results by the proposed method show that both appearing and disappearing buildings with their step-times are successfully identified and results by ascending and descending SAR images show a good agreement.