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Sample records for anti-stokes raman spectroscopy

  1. Coherent anti-Stokes Raman spectroscopy: Understanding the essentials

    NASA Astrophysics Data System (ADS)

    Ariunbold, Gombojav O.; Altangerel, Narangerel

    2016-12-01

    This paper is a brief overview to coherent anti- Stokes Raman spectroscopic technique and introduces the strengths and barriers to its use all based on the interpretation of simple theoretical formulae. The use of the Gaussian ultrashort pulses is highlighted as a practical elucidatory reconstruction tool of coherent Raman spectra. The paper presents the integral formulae for coherent anti-Stokes and Stokes Raman scattering, and discusses the closed-form solutions, its complex error function, and the delay time formula for enhancement of the inferred pure coherent Raman spectra. As an example, the timeresolved coherent Stokes Raman scattering experimental observations are quantitatively elucidated.Understanding the essentials of coherent Raman spectroscopy, therefore, promotes the importance of a number of experiments including the ones utilizing a broadband excitation with a narrowband delayed probing for successful background suppression.

  2. Combustion Diagnosis By Coherent Anti-Stokes Raman Spectroscopy (CARS)

    NASA Astrophysics Data System (ADS)

    Hall, Robert J.; Eckbreth, Alan C.

    1981-08-01

    Coherent anti-Stokes Raman spectroscopy (CARS) appears very promising for the remote, spatially and temporally precise probing of hostile combustion environments due to its large signal conversion efficiency and coherent signal nature. CARS is a wave mixing process in which incident laser beams at frequencies w1 and 0)2, with a frequency difference tuned to a Raman resonance in the molecular species being probed, interact to generate a coher-ent signal at frequency w3 = 2(.01 - w2. By analyzing the spectral distribution of the CARS signal, temperature measurements can be performed. Species concentration measurements derive from the intensity of the CARS radiation or, in certain cases, from its spectral shape. CARS spectra have been recorded in a variety of flames from the major flame constituents and generally show very good agreement with computer synthesized spectra. Significantly, CARS has been successfully demonstrated with both liquid and gaseous fuels in the primary zone and exhaust of practical combustors. Both thermometry and species concentration measurements have been performed. High pressure effects on CARS spectra have also been examined.

  3. Broadband coherent anti-Stokes Raman scattering spectroscopy in supercontinuum optical trap

    NASA Astrophysics Data System (ADS)

    Shi, Kebin; Li, Peng; Liu, Zhiwen

    2007-04-01

    The authors report on a supercontinuum tweezer which combines tweezing with broadband (˜3000cm-1) coherent anti-Stokes Raman scattering (CARS) spectroscopy by taking advantage of the high spatial coherence and broad bandwidth of pulsed supercontinuum generated in a nonlinear photonic crystal fiber. Polarization-discriminated and time-resolved CARS is investigated to suppress the nonresonant four-wave-mixing background.

  4. Single-pulse coherent anti-Stokes Raman spectroscopy via fiber Bragg grating

    NASA Astrophysics Data System (ADS)

    Oh, Seung Ryeol; Park, Joo Hyun; Kwon, Won Sik; Kim, Jin Hwan; Kim, Kyung-Soo; Lee, Jae Yong; Kim, Soohyun

    2016-03-01

    Fiber Bragg grating is used in a variety of applications. In this study, we suggest compact, cost-effective coherent anti- Stokes Raman spectroscopy which is based on the pulse shaping methods via commercialized fiber Bragg grating. The experiment is performed incorporating a commercialized femtosecond pulse laser system (MICRA, Coherent) with a 100 mm length of 780-HP fiber which is inscribed 50 mm of Bragg grating. The pump laser for coherent anti-Stokes Raman spectroscopy has a bandwidth of 90 nm and central wavelength of 815 nm with a notch shaped at 785 nm. The positive chirped pulse is compensated by chirped mirror set. We compensate almost 14000 fs2 of positive group delay dispersion for the transform-limited pulse at the sample position. The pulse duration was 15 fs with average power of 50 mW, and showed an adequate notch shape. Finally, coherent anti-Stokes Raman signals are observed using a spectrometer (Jobin Yvon Triax320 and TE-cooled Andor Newton EMCCD). We obtained coherent anti-Stokes Raman signal of acetone sample which have Raman peak at the spectral finger-print region. In conclusion, the proposed method is more simple and cost-effective than the methods of previous research which use grating pairs and resonant photonic crystal slab. Furthermore, the proposed method can be used as endoscope application.

  5. Vibrational energy dynamics of water studied with ultrafast Stokes and anti-Stokes Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Wang, Zhaohui; Pang, Yoonsoo; Dlott, Dana D.

    2004-10-01

    The transient Stokes Raman spectroscopy method is introduced to study the dynamics of OH-stretching vibrations in water excited by ultrashort infrared pulses. The combination of Stokes and anti-Stokes Raman probing allows the the absorption and emission contributions to be measured separately. Experiments with 3400 cm -1 pumping of OH-stretching of HOD solute in D 2O solvent are reported. The Stokes Raman method is used to study the delay between the excited-state decay and the ground-state recovery, the vibrational Stokes shift, and the generation of weakened hydrogen bonding due to heat released by vibrational relaxation.

  6. Simultaneous rotational coherent anti-Stokes Raman spectroscopy and coherent Stokes Raman spectroscopy with arbitrary pump-Stokes spectral separation.

    PubMed

    Eckbreth, A C; Anderson, T J

    1986-08-01

    A new approach to pure rotational coherent anti-Stokes Raman spectroscopy (CARS) and coherent Stokes Raman spectroscopy (CSRS) is demonstrated in which the pump and broadband Stokes lasers that are mixed have a large and arbitrary spectral separation. In this method, the rotational Raman coherences are established by different frequency components within the single, broadband Stokes source. The narrow band then scatters from the excited coherences, producing CARS and CSRS simultaneously. We discuss phase matching for this new technique and its inherent advantages relative to pure rotational CARS as normally implemented.

  7. Analysis for Coherent Anti-Stokes Raman Spectroscopy (CARS).

    DTIC Science & Technology

    1980-06-01

    Spectroscopy", in Chemical and Biochemical Applications of Lasers IV, C. Bradley Moore, ed; Academic Press, N.Y. (1979). 6. Gerhard Herzberg , "Infrared and...function as explained in Herzberg .4 Hence both processes will be stimulated by an incoming idler beam of even small bandwidth. For the equations to be...e-E V/kT (22) V where Ev = hc[we(v + 1/2) - weXe (v + 1/2) ) (23) The quantities we and weXe are available in Herzberg W for all diatomic molecules

  8. Femtosecond Coherent Anti-Stokes Raman Spectroscopy (CARS) As Next Generation Nonlinear LIDAR Spectroscopy and Microscopy

    SciTech Connect

    Ooi, C. H. Raymond

    2009-07-10

    Nonlinear spectroscopy using coherent anti-Stokes Raman scattering and femtosecond laser pulses has been successfully developed as powerful tools for chemical analysis and biological imaging. Recent developments show promising possibilities of incorporating CARS into LIDAR system for remote detection of molecular species in airborne particles. The corresponding theory is being developed to describe nonlinear scattering of a mesoscopic particle composed of complex molecules by laser pulses with arbitrary shape and spectral content. Microscopic many-body transform theory is used to compute the third order susceptibility for CARS in molecules with known absorption spectrum and vibrational modes. The theory is combined with an integral scattering formula and Mie-Lorentz formulae, giving a rigorous formalism which provides powerful numerical experimentation of CARS spectra, particularly on the variations with the laser parameters and the direction of detection.

  9. Combined coherent anti-Stokes Raman spectroscopy and linear Raman spectroscopy for simultaneous temperature and multiple species measurements.

    PubMed

    Weikl, Markus C; Beyrau, Frank; Kiefer, Johannes; Seeger, Thomas; Leipertz, Alfred

    2006-06-15

    The simultaneous application of pure rotational coherent anti-Stokes Raman spectroscopy (CARS) and vibrational linear Raman spectroscopy (LRS) for the measurement of temperature and species concentrations in combustion systems is demonstrated. In addition to the standard rotational CARS experimental setup, only one detection system (spectrometer and intensified CCD camera) for the collection of the LRS signals was applied. The emission of the broadband dye laser used for CARS was shifted to the deep red to avoid interferences with the LRS signals located in the visible region. First experimental results from a vaporizing propane spray using an engine injection system are shown.

  10. Width-Increased Dual-Pump Enhanced Coherent Anti-Stokes Raman Spectroscopy (WIDECARS)

    NASA Technical Reports Server (NTRS)

    Tedder, Sarah A.; Danehy, Paul M.; Cutler, Andrew D.

    2010-01-01

    WIDECARS is a dual-pump coherent anti-Stokes Raman Spectroscopy technique that is capable of simultaneously measuring temperature and species mole fractions of N2, O2, H2, C2H4, CO, and CO2. WIDECARS is designed for measurements of all the major species (except water) in supersonic combustion flows fueled with hydrogen and hydrogen/ethylene mixtures. The two lowest rotational energy levels of hydrogen detectable by WIDECARS are H2 S(3) and H2 S(4). The detection of these lines gives the system the capability to measure temperature and species concentrations in regions of the flow containing pure hydrogen fuel at room temperature.

  11. Single pulse phase-control interferometric coherent anti-StokesRaman scattering spectroscopy (CARS)

    SciTech Connect

    Lim, Sang-Hyun; Caster, Allison G.; Leone, Stephen R.

    2005-09-28

    In coherent anti-Stokes Raman scattering spectroscopy (CARS) experiments, usually the amplitude of the signal is measured and the phase information is lost. With a polarization- and phase-controlled pulse shaping technique, the relative phase between the resonant and non-resonant CARS signals is controlled, and spectral interferometry is performed without an interferometer. Both the real and imaginary parts of the background-free resonant CARS spectrum are measured via spectral interferometry between the resonant and non-resonant signals from the same sample. The resonant signal is amplified significantly by homodyne mixing with the non-resonant signal as a local oscillator, greatly improving the detection limit.

  12. Investigations of coherent anti-Stokes Raman spectroscopy /CARS/ for practical combustion diagnostics

    NASA Technical Reports Server (NTRS)

    Eckbreth, A. C.; Hall, R. J.; Shirley, J. A.; Verdieck, J. F.

    1981-01-01

    Coherent anti-Stokes Raman spectroscopy (CARS) is a coherent wave-mixing process in which the signal emerges as a laser-like beam in a precise direction. The spectroscopic technique is appropriate to spatially and temporally resolved measurements of temperature and major species concentrations in combustion. It has been generated from all of the dominant constituents in air-fed, hydrogen, and hydrocarbon fueled combustion, and found applicable to practical combustion systems. High pressure effects on CARS spectra have also been examined.

  13. Next generation hazard detection via ultrafast coherent anti-Stokes Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Brady, John J.; Pellegrino, Paul M.

    2013-05-01

    Multiplex coherent anti-Stokes Raman spectroscopy (MCARS) is used to detect an explosive precursor material and two chemical warfare simulants. The spectral bandwidth of the femtosecond laser pulse used in these studies is sufficient to coherently and simultaneously drive all the vibrational modes in the molecule of interest. The research performed here demonstrates that MCARS has the capability to detect an explosive precursor (e.g., acetone) and hazardous materials, such as dimethyl methylphosphonate and 2-chloroethyl methyl sulfide (a sarin and a mustard gas chemical warfare simulant, respectively), with high specificity. Evidence shows that MCARS is capable of overcoming common the sensitivity limitations of spontaneous Raman scattering, thus allowing for the detection of the target material in milliseconds with standard USB spectrometers as opposed to seconds with intensified spectrometers. The exponential increase in the number of scattered photons suggests that the MCARS technique may be capable of overcoming range detection challenges common to spontaneous Raman scattering.

  14. Raman optical activity spectroscopy by visible-excited coherent anti-Stokes Raman scattering.

    PubMed

    Hiramatsu, Kotaro; Leproux, Philippe; Couderc, Vincent; Nagata, Takashi; Kano, Hideaki

    2015-09-01

    We developed a Raman optical activity (ROA) spectroscopic system with visible-excited coherent anti-Stokes Raman scattering (CARS). A supercontinuum within the visible region was generated with a photonic crystal fiber pumped with both 532 and 1064 nm excitation, generating a multiplexed CARS-ROA spectrum covering the whole fingerprint region. In visible excitation, the CARS-ROA spectrum of (-)-β-pinene shows a higher contrast ratio of the chirality-induced signal to the achiral background than that of the previously reported near-infrared CARS-ROA spectrum.

  15. Low-concentration chemical sensing using surface-enhanced coherent anti-Stokes Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Hua, Xia; Sinyukov, Alexander; Traverso, Andrew; Veronine, Dmitri; Wang, Kai; Xia, Hui; Yang, Wenlong; Yuan, Luqi; Sokolov, Alexei; Scully, Marlan

    2010-10-01

    Measurements of surface enhanced coherent anti-Stokes Raman spectra (CARS) of cyclohexane are carried out. Random aggregates of gold nanoparticles for field enhancement were deposited on a glass substrate and were characterized using atomic force microscopy (AFM). Surface enhancement of the CARS signal by gold nanoparticles is observed. This technique can be used to detect low amounts of chemicals with a higher sensitivity compared to the conventional surface-enhanced Raman spectroscopy (SERS). The lowest detected concentration of cyclohexane in a thin film of methanol was 1%. However, it was not possible to detect any signal from the same sample of cyclohexane without gold nanoparticles using conventional CARS technique. Therefore, surface enhancement is necessary to achieve higher spectroscopy sensitivity. Further studies of nanostructure-enhanced electrical fields are required to quantitatively understand the observed effects and will be performed in the future.

  16. Analysis of organic pollutant degradation in pulsed plasma by coherent anti-Stokes Raman spectroscopy

    SciTech Connect

    Bratescu, Maria Antoneta; Hieda, Junko; Umemura, Tomonari; Saito, Nagahiro; Takai, Osamu

    2011-05-15

    The degradation of p-benzoquinone (p-BQ) in water was investigated by the coherent anti-Stokes Raman spectroscopy (CARS) method, in which the change of the anti-Stokes signal intensity corresponding to the vibrational transitions of the molecule is monitored during and after solution plasma processing (SPP). In the beginning of SPP treatment, the CARS signal intensity of the ring vibrational molecular transitions at 1233 and 1660 cm{sup -1} increases under the influence of the electric field of the plasma, depending on the delay time between the plasma pulse and the laser firing pulse. At the same time, the plasma contributes to the degradation of p-BQ molecules by generating hydrogen and hydroxyl radicals, which decompose p-BQ into different carboxylic acids. After SPP, the CARS signal intensity of the vibrational bands of p-BQ ceased and the degradation of p-BQ was confirmed by UV-visible absorption spectroscopy and liquid chromatography analysis.

  17. Molecular species-sensitive optical coherence tomography using coherent anti-stokes Raman scattering spectroscopy

    NASA Astrophysics Data System (ADS)

    Marks, Daniel L.; Bredfeldt, Jeremy; Hambir, Selezion; Dlott, Dana D.; Kitchell, Barbara; Gruebele, Martin; Boppart, Stephen A.

    2003-07-01

    We present our progress in developing a novel technique and instrument that images specific molecular species in biological tissues using Optical Coherence Tomography (OCT). Standard OCT instruments measure only the scattering from structural features, such as refractive index changes. We utilize Coherent Anti-Stokes Raman Scattering (CARS) Spectroscopy, a nonlinear optics technique that can selectively stimulate molecular groups, to gather compositional information from the sample. Being a coherent process, our instrument will produce interference between the nonlinear anti-Stokes signal produced in the sample and a reference molecular sample to both exclude background and nonresonant signals and range features in the tissue. Because of this, we will also gain the benefits of sensitivity that interferometry can provide. By utilizing the tunability of an optical parametric oscillator, we can address a range of molecular resonances from 1500 cm-1 to 3500 cm-1. This frequency range offers the possibility of measuring the distributions and densities of proteins, lipids, and nuclear material that we believe will be useful for determining the early presence of epithelial carcinomas. We demonstrate the principle of this imaging method by producing interference between two separately produced CARS signals from the same probe and Stokes beams.

  18. Real-time detection of bacterial spores using coherent anti-Stokes Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Dogariu, A.; Goltsov, A.; Pestov, D.; Sokolov, A. V.; Scully, M. O.

    2008-02-01

    We demonstrate a realistic method for detection of anthrax-type spores in real time based on their chemical fingerprints using coherent anti-Stokes Raman scattering. Specifically, we demonstrate that coherent Raman scattering can be used to successfully identify spores with high accuracy and high selectivity in less than 50ms.

  19. Coherent anti-Stokes Raman spectroscopy temperature measurements in a hydrogen-fueled supersonic combustor

    NASA Technical Reports Server (NTRS)

    Smith, Michael W.; Jarrett, Olin, Jr.; Antcliff, Richard R.; Northam, G. B.; Cutler, Andrew D.; Taylor, David J.

    1993-01-01

    Coherent anti-Stokes Raman spectroscopy (CARS) thermometry has been used to obtain static temperature cross sections in a three-dimensional supersonic combustor flowfield. Data were obtained in three spanwise planes downstream of a single normal fuel injector which was located downstream of a rearward-facing step. The freestream flow was nominally Mach 2 and was combustion heated to a total temperature of 1440 K (yielding a static temperature of about 800 K in the freestream) to simulate the inflow to a combustor operating at a flight Mach number of about 5.4. Since a broadband probe laser was used an instantaneous temperature sample was obtained with each laser shot at a repetition rate of 10 Hz. Thus root-mean-square (rms) temperatures and temperature probability density functions (pdf's) were obtained in addition to mean temperatures.

  20. Investigations of coherent anti-Stokes Raman spectroscopy /CARS/ for combustion diagnostics

    NASA Technical Reports Server (NTRS)

    Eckbreth, A. C.; Hall, R. J.; Shirley, J. A.

    1979-01-01

    Investigations of coherent anti-Stokes Raman spectroscopy (CARS) in a variety of flames are presented. Thermometry has received the primary emphasis in these studies, but species spectral and sensitivity studies will also be described. CARS is generated by mixing a 10 pps, frequency-doubled neodymium 'pump' laser with a spectrally broadband, laser-pumped, Stokes-shifted dye laser. This approach obviates the requirement to frequency scan the dye laser and generates the entire CARS spectrum with each pulse permitting, in principle, instantaneous measurements of medium properties. CARS spectra of N2, CO, O2, H2O, CO2 and CH4 in flames will be presented. In general these spectra exhibit very good agreement with computer synthesized spectra and permit measurements of temperature and species concentration. To illustrate the applicability of CARS to practical combustion diagnostics, CARS signatures from N2 have been employed to map the temperature field throughout a small, luminous, highly sooting propane diffusion flame

  1. Broadband coherent anti-Stokes Raman spectroscopy characterization of polymer thin films.

    PubMed

    Schultz, Zachary D; Gurau, Marc C; Richter, Lee J

    2006-10-01

    Broadband coherent anti-Stokes Raman spectroscopy (CARS) is demonstrated as an effective probe of polymer thin film materials. A simple modification to a 1 kHz broad bandwidth sum frequency generation (SFG) spectrometer permits acquisition of CARS spectra for polymer thin films less than 100 nm thick, a dimension relevant to organic electronic device applications. CARS spectra are compared to the conventional Raman spectra of polystyrene and the resonance-enhanced Raman spectra of poly(3-hexylthiophene). The CARS spectra obtained under these conditions consistently demonstrate enhanced signal-to-noise ratio compared to the spontaneous Raman scattering. The sensitivity of the CARS measurement is limited by the damage threshold of the samples. The dielectic properties of the substrate have a dramatic effect on the detected signal intensity. For ultrathin films, the strongest signals are obtained from fused silica surfaces. Similar to surface-enhanced Raman scattering (SERS), Au also gives a large signal, but contrary to SERS, no surface roughening is necessary.

  2. Theory of femtosecond coherent anti-Stokes Raman scattering spectroscopy of gas-phase transitions.

    PubMed

    Lucht, Robert P; Kinnius, Paul J; Roy, Sukesh; Gord, James R

    2007-07-28

    A theoretical analysis of coherent anti-Stokes Raman scattering (CARS) spectroscopy of gas-phase resonances using femtosecond lasers is performed. The time-dependent density matrix equations for the femtosecond CARS process are formulated and manipulated into a form suitable for solution by direct numerical integration (DNI). The temporal shapes of the pump, Stokes, and probe laser pulses are specified as an input to the DNI calculations. It is assumed that the laser pulse shapes are 70 fs Gaussians and that the pulses are Fourier-transform limited. A single excited electronic level is defined as an effective intermediate level in the Raman process, and transition strengths are adjusted to match the experimental Raman polarizability. The excitation of the Raman coherence is investigated for different Q-branch rotational transitions in the fundamental 2330 cm(-1) band of diatomic nitrogen, assuming that the pump and Stokes pulses are temporally overlapped. The excitation process is shown to be virtually identical for transitions ranging from Q2 to Q20. The excitation of the Raman coherences is also very efficient; for laser irradiances of 5x10(17) W/m2, corresponding approximately to a 100 microJ, 70 fs pulse focused to 50 microm, approximately 10% of the population of the ground Raman level is pumped to the excited Raman level during the impulsive pump-Stokes excitation, and the magnitude of the induced Raman coherence reaches 40% of its maximum possible value. The theoretical results are compared with the results of experiments where the femtosecond CARS signal is recorded as a function of probe delay with respect to the impulsive pump-Stokes excitation.

  3. Detection of Bacillus subtilis spores in water by means of broadband coherent anti-Stokes Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Petrov, Georgi I.; Yakovlev, Vladislav V.; Sokolov, Alexei V.; Scully, Marlan O.

    2005-11-01

    Broadband coherent anti-Stokes Raman scattering (CARS) spectroscopy is used for detection of bacterial spores in aqueous solution. Polarization CARS spectroscopy is employed to suppress the non-resonant background. CARS spectrum recorded in the spectral region from 700 to 1900 cm-1 exhibits all the characteristic features of spontaneous Raman spectrum taken for a solid powder and resembles that one of the dipicolinic acid, which is considered to be the major component of bacterial spores, including anthrax.

  4. Investigation of optical fibers for coherent anti-Stokes Raman scattering (CARS) spectroscopy in reacting flows

    NASA Astrophysics Data System (ADS)

    Hsu, Paul S.; Patnaik, Anil K.; Gord, James R.; Meyer, Terrence R.; Kulatilaka, Waruna D.; Roy, Sukesh

    2010-10-01

    The objective of this work is to investigate the feasibility of intense laser-beam propagation through optical fibers for temperature and species concentration measurements in gas-phase reacting flows using coherent anti-Stokes Raman scattering (CARS) spectroscopy. In particular, damage thresholds of fibers, nonlinear effects during beam propagation, and beam quality at the output of the fibers are studied for the propagation of nanosecond (ns) and picosecond (ps) laser beams. It is observed that ps pulses are better suited for fiber-based nonlinear optical spectroscopic techniques, which generally depend on laser irradiance rather than fluence. A ps fiber-coupled CARS system using multimode step-index fibers is developed. Temperature measurements using this system are demonstrated in an atmospheric pressure, near-adiabatic laboratory flame. Proof-of-concept measurements show significant promise for fiber-based CARS spectroscopy in harsh combustion environments. Furthermore, since ps-CARS spectroscopy allows the suppression of non-resonant background, this technique could be utilized for improving the sensitivity and accuracy of CARS thermometry in high-pressure hydrocarbon-fueled combustors.

  5. Improved scanning range for coherent anti-stokes Raman spectroscopy using a tunable optical parametric oscillator.

    PubMed

    Chen, P C

    1996-09-01

    Coherent anti-Stokes Raman spectroscopy (CARS) is a well-known form of nonlinear spectroscopy that has been used for a wide range of specialized quantitative applications. From an analytical chemist's point of view, however, conventional CARS is impractical as a tool for qualitative and quantitative analyses because the scan range is too short to produce complete vibrational spectra. This paper introduces a new technique, synchronously scanned optical parametric oscillator (OPO) CARS, that improves the potential for using nonlinear spectroscopy as an analytical technique in both gas- and condensed-phase samples. First, it uses a broadly tunable OPO to increase the scan range. Second, phase matching problems that limit scans in condensed-phase CARS are reduced by using both the signal and the idler beams in a synchronous scanning manner. Finally, this synchronous scanning method generates an output signal that remains fixed at a single wavelength (single-wavelength detection). Advantages of single-wavelength detection include reduction of stray light, simplicity, and elimination of the need for wavelength calibration of the detection optics. Results are presented on neat and mixed samples in gas and condensed phases.

  6. Raman spectroscopy and coherent anti-Stokes Raman scattering imaging: prospective tools for monitoring skeletal cells and skeletal regeneration

    PubMed Central

    Moura, Catarina Costa; Tare, Rahul S.; Oreffo, Richard O. C.; Mahajan, Sumeet

    2016-01-01

    The use of skeletal stem cells (SSCs) for cell-based therapies is currently one of the most promising areas for skeletal disease treatment and skeletal tissue repair. The ability for controlled modification of SSCs could provide significant therapeutic potential in regenerative medicine, with the prospect to permanently repopulate a host with stem cells and their progeny. Currently, SSC differentiation into the stromal lineages of bone, fat and cartilage is assessed using different approaches that typically require cell fixation or lysis, which are invasive or even destructive. Raman spectroscopy and coherent anti-Stokes Raman scattering (CARS) microscopy present an exciting alternative for studying biological systems in their natural state, without any perturbation. Here we review the applications of Raman spectroscopy and CARS imaging in stem-cell research, and discuss the potential of these two techniques for evaluating SSCs, skeletal tissues and skeletal regeneration as an exemplar. PMID:27170652

  7. Coherent anti-stokes Raman spectroscopy for detecting explosives in real time

    NASA Astrophysics Data System (ADS)

    Dogariu, Arthur; Pidwerbetsky, Alex

    2012-06-01

    We demonstrate real-time stand-off detection and imaging of trace explosives using collinear, backscattered Coherent Anti-Stokes Raman Spectroscopy (CARS). Using a hybrid time-resolved broad-band CARS we identify nanograms of explosives on the millisecond time scale. The broad-band excitation in the near-mid-infrared region excites the vibrational modes in the fingerprint region, and the time-delayed probe beam ensures the reduction of any non-resonant contributions to the CARS signal. The strong coherent enhancement allows for recording Raman spectra in real-time. We demonstrate stand-off detection by acquiring, analyzing, and identifying vibrational fingerprints in real-time with very high sensitivity and selectivity. By extending the focused region from a 100-micron sized spot to a 5mm long line we can obtain the spectral information from an extended region of the remote target with high spatial resolution. We demonstrate fast hyperspectral imaging by one-dimensional scanning of the Line-CARS. The three-dimensional data structure contains the vibrational spectra of the target at each sampled location, which allows for chemical mapping of the remote target.

  8. Combined spontaneous Stokes and coherent anti-Stokes Raman scattering spectroscopy

    NASA Astrophysics Data System (ADS)

    Becker, Karina; Kiefer, Johannes

    2016-05-01

    The simultaneous determination of multiple parameters is the key in the characterization of processes and materials that change with time. In combustion environments, the combined measurement of temperature and chemical composition is particularly desirable. In the present work, possible approaches for the simultaneous application of spontaneous Raman scattering (RS) and coherent anti-Stokes Raman scattering (CARS) spectroscopy are proposed and analyzed. While RS provides concentration information of all major species, vibrational CARS is a highly accurate thermometry tool at flame conditions. Five experimentally feasible CARS-RS schemes are identified and discussed with respect to signal intensity, measurement volume, and experimental complexity. From this analysis, one scheme was found to be the best option. It utilizes a broadband dye laser centered at 852 nm as a pump and the fundamental 1064-nm radiation of the Nd:YAG as Stokes laser. The third harmonic is used as CARS probe and RS laser. The experimentally most elegant scheme replaces the third harmonic in the above scheme by the second harmonic hence involving the smallest number of optical components in the setup.

  9. Temperature measurements in an industrial furnace by spontaneous anti-Stokes Raman spectroscopy

    SciTech Connect

    Zikratov, G.; Singh, J.P.; Yueh, F.Y.; Cook, R.L.

    1998-07-01

    Spontaneous anti-Stokes Raman scattering from N{sub 2} was employed to measure the temperature profiles inside an industrial furnace with a water-cooled probe. Prior to the field measurements, the system performance was evaluated and maximized in a laboratory furnace at several temperatures below 1,300 K. The temperatures of about 1,500 K have been measured in the industrial furnace, and they are in agreement with data recorded with a thermocouple probe. Spontaneous anti-Stokes Raman was found to be a reliable tool for non-intrusive absolute temperature measurements in industrial furnaces with relatively clean gas streams. Little dependence was found on the laser power and optics mis-alignment.

  10. Intracavity phase-matched coherent anti-Stokes Raman spectroscopy for trace gas detection.

    PubMed

    Zaitsu, Shin-ichi; Imasaka, Totaro

    2014-01-01

    We present a novel, cavity-enhanced spectroscopic technique based on a phase-matched Raman process to detect trace quantities of gas. The essence of this technique is the careful control of cavity dispersion to satisfy the phase-matching condition of coherent anti-Stokes Raman scattering (CARS) enhanced in a high-finesse optical cavity. A 6000-fold improvement of the CARS signal is observed under optimized conditions, indicating that this is a promising tool to quantify Raman-active molecules with an extremely low detection limit.

  11. Coherent Anti-Stokes Raman Spectroscopy (CARS) Measurements in Supersonic Combustors at NASA Langley Research Center

    NASA Technical Reports Server (NTRS)

    Danehy, Paul M.; OByrne, Sean B.; Tedder, Sarah A.; Cutler, Andrew D.

    2005-01-01

    This paper describes the recent use of coherent anti-Stokes Raman spectroscopy (CARS) to study supersonic combustion at NASA Langley Research Center. CARS is a nonlinear optical measurement technique used to measure temperature and species mole fractions remotely in harsh environments. A CARS system has been applied to two different combustor geometries at NASA Langley. Both experiments used the same vitiated wind-tunnel facility to create an air flow that simulates flight at Mach numbers of 6 and 7 for the combustor inlet and both experiments used hydrogen fuel. In the first experiment, the hydrogen was injected supersonically at a 30-degree angle with respect to the incoming flow. In the second experiment, the hydrogen was injected sonically at normal incidence. While these injection schemes produced significantly different flow features, the CARS method provided mean temperature, N2, O2 and H2 maps at multiple downstream locations for both. The primary aim of these measurements was to provide detailed flowfield information for computational fluid dynamics (CFD) code validation.

  12. Gas-phase diagnostic by time-resolved rotational coherent anti-Stokes Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Seeger, Thomas; Leipertz, A.

    2011-05-01

    Dual-broadband pure rotational CARS (RCARS) is nowadays a well-developed gas phase measurement technique. Nevertheless there are challenges for technical applications due to stray light interference, soot emission or droplets. Beside this for diffusion flames also a strong, unknown and varying non-resonant background signal is contributing to the CARS signal. Possible applications of time-resolved pure rotational coherent anti-Stokes Raman spectroscopy for different applications are demonstrated and its potential of for gas-phase thermometry is investigated. The field of application covers studies on flame research especially sooting flames as well as its use in technical combustion systems e.g., for the determination of the gas-phase temperature in the vaporizing spray of a GDI injector. A new advantageous approach by using picosecond (ps) laser sources as a diagnostic tool is also demonstrated. By time-delaying the ps probe laser beam problems due to stray light interference, soot emission or droplets can be reduced tremendously of even eliminated.

  13. Coherent anti-Stokes Raman scattering and spontaneous Raman spectroscopy and microscopy of microalgae with nitrogen depletion.

    PubMed

    He, X N; Allen, J; Black, P N; Baldacchini, T; Huang, X; Huang, H; Jiang, L; Lu, Y F

    2012-11-01

    Microalgae are extensively researched as potential feedstocks for biofuel production. Energy-rich compounds in microalgae, such as lipids, require efficient characterization techniques to investigate the metabolic pathways and the environmental factors influencing their accumulation. The model green alga Coccomyxa accumulates significant amounts of triacylglycerols (TAGs) under nitrogen depletion (N-depletion). To monitor the growth of TAGs (lipid) in microalgal cells, a study of microalgal cells (Coccomyxa sp. C169) using both spontaneous Raman and coherent anti-Stokes Raman scattering (CARS) spectroscopy and microscopy were carried out. Spontaneous Raman spectroscopy was conducted to analyze the components in the algal cells, while CARS was carried out to monitor the distribution of lipid droplets in the cells. Raman signals of carotenoid are greater in control microalgae compared to N-depleted cells. Raman signals of lipid droplets appear after N-depletion and its distribution can be clearly observed in the CARS microscopy. Both spontaneous Raman spectroscopy and CARS microscopy were found to be suitable analysis tools for microalgae.

  14. Ultrabroad femtosecond pulses for coherent anti-stokes Raman scattering spectroscopy

    NASA Astrophysics Data System (ADS)

    Wrzesinski, Paul J.

    This dissertation focus on the use of sub-ten femtosecond pulses applied to coherent anti-Stokes Raman scattering spectroscopy. The use of such a broadbandwidth pulse coupled with adaptive pulse shaping has provided a method to impulsively excite all vibrational modes within the bandwidth of the pulse. Furthermore, this method using only a single beam eliminates many of the experimental difficulties associated with the typical multi-beam CARS methods. The generation of supercontinuum has allowed for high energy, amplified pulses to reach the same time duration/bandwidth as lower energy femtosecond oscillators. This significant increase in pulse energy has allowed the single-beam CARS method to be extended beyond microspectrocopy, which requires the tight focusing conditions afforded by a microscope objective in order to reach the necessary pulse energy. This extension has opened single-beam CARS to fields such as remote sensing and combustion diagnostics. This dissertation presents the evolution of single-beam CARS in the context of these fields. Remote sensing is demonstrated at distances of 12 m for solids, liquids, and gases in a retro reflective set-up with signal to noise levels high enough for molecular identification. Single shot measurements are also made, along with direct backscatter measurements. CARS gas phase measurements are made on several atmospheric gases, as well as mixtures of gases. Mode-selective CARS excitation is used to excite a single Raman mode, creating a contrast mechanism that allows for direct visualization of a CO2 jet. Several gases were also measured in various pressure regimes to determine the number density relationship. Lastly, the group velocity dispersion of several combustion gases was measured to illustrate the temporal broadening that occurs when femtosecond pulses propagate in combustion environments. The ability to manipulate the axial resolution of a nonlinear optical process when using adaptive pulse shaping is also

  15. Coherent anti-Stokes Raman spectroscopy of shock-compressed liquid oxygen

    SciTech Connect

    Schmidt, S.C.; Moore, D.S.; Shaw, M.S.; Johnson, J.D.

    1989-01-01

    Vibrational spectra of liquid oxygen, shock compressed to several high-pressure/high-temperature states, were obtained using single- pulse multiplex coherent anti-Stokes Raman scattering (CARS). The experimental spectra were compared to synthetic spectra calculated using a semiclassical model for the CARS intensities and best fit vibrational frequencies, peak Raman susceptibilities, and Raman linewidths. Up to the maximum shock pressure of 9.6 GPa, the vibrational frequencies were found to increase monotonically with pressure. An empirical fit, which could be used as a pressure/temperature/frequency calibration standard, showed that the Raman frequency shifts could be accurately described by linear pressure and temperature dependences. Above /approx/9 GPa, the liquid oxygen opacity at 632.8 nm increased rapidly, presumably because of proximity (collision)-induced absorption. Calculations showed that the induced absorption did not resonantly enhance the CARS spectra, but did attenuate the laser beams and the CARS signals. 33 refs., 2 figs., 1 tab.

  16. Use of the Gerchberg-Saxton algorithm in optimal coherent anti-Stokes Raman spectroscopy.

    PubMed

    Moore, D S; McGrane, S D; Greenfield, M T; Scharff, R J; Chalmers, R E

    2012-01-01

    We are utilizing recent advances in ultrafast laser technology and recent discoveries in optimal shaping of laser pulses to significantly enhance the stand-off detection of explosives via control of molecular processes at the quantum level. Optimal dynamic detection of explosives is a method whereby the selectivity and sensitivity of any of a number of nonlinear spectroscopic methods are enhanced using optimal shaping of ultrafast laser pulses. We have recently investigated the Gerchberg-Saxton algorithm as a method to very quickly estimate the optimal spectral phase for a given analyte from its spontaneous Raman spectrum and the ultrafast laser pulse spectrum. Results for obtaining selective coherent anti-Stokes Raman spectra (CARS) for an analyte in a mixture, while suppressing the CARS signals from the other mixture components, are compared for the Gerchberg-Saxton method versus previously obtained results from closed-loop machine-learning optimization using evolutionary strategies.

  17. Polarization Sensitive Coherent Anti-Stokes Raman Spectroscopy of DCVJ in Doped Polymer

    NASA Astrophysics Data System (ADS)

    Ujj, Laszlo

    2014-05-01

    Coherent Raman Microscopy is an emerging technic and method to image biological samples such as living cells by recording vibrational fingerprints of molecules with high spatial resolution. The race is on to record the entire image during the shortest time possible in order to increase the time resolution of the recorded cellular events. The electronically enhanced polarization sensitive version of Coherent anti-Stokes Raman scattering is one of the method which can shorten the recording time and increase the sharpness of an image by enhancing the signal level of special molecular vibrational modes. In order to show the effectiveness of the method a model system, a highly fluorescence sample, DCVJ in a polymer matrix is investigated. Polarization sensitive resonance CARS spectra are recorded and analyzed. Vibrational signatures are extracted with model independent methods. Details of the measurements and data analysis will be presented. The author gratefully acknowledge the UWF for financial support.

  18. Coherent Anti-Stokes Raman Spectroscopy (cars) Gas Temperature Measurements in a Monodisperse Combusting Droplet Stream.

    NASA Astrophysics Data System (ADS)

    Zhu, Junyong

    1991-06-01

    This dissertation describes a coherent anti-Stokes Raman spectroscopy (CARS) instrument for spatially and temporally resolved non-intrusive temperature measurements in combustion environments. It presents a detailed description of the CARS system development and standard procedures to perform CARS gas temperature measurements,and procedures to analyze the CARS spectra for temperature determination. The dissertation also applies the CARS apparatus developed to a single monodisperse methanol droplet stream flame to demonstrate synchronous CARS temperature measurements. The measurements correlate the temperature field with the droplet position and give the local characteristics of the combusting droplet stream thermal field. These measurements are not possible with conventional thermal probes due to the perturbation caused by the probes and the poor temporal and spatial resolution. These CARS measurements are the first known non-intrusive characterization of the local temperature field near burning droplets. The experiments use a 50 μm diameter nozzle vibrated by a piezoelectric crystal to generate a monodisperse droplet stream with a droplet diameter of about 150 μm and droplet-to-droplet spacing of 10 droplet diameters. A frequency divider divides the crystal vibration frequency of 10 kHz 1000 times to synchronize the CARS laser firing (~ 10 Hz) with the droplet generation process. The results show that there is a small thermal wake behind each droplet in the stream. The temperature profile measured radially outward from the droplet has a local minimum near the droplet surface, rises to a maximum at about 7 droplet diameters away, and then falls to room temperature at a radial distance of 15 mm (100 droplet diameters). The temperature profile measured between two adjacent droplets on the stream axis is nearly flat, suggesting that individual flames do not surround each droplet. The local effects due to the presence of droplets completely disappear about 15 droplet

  19. Single-beam coherent anti-Stokes Raman scattering spectroscopy of N 2 using a shaped 7 fs laser pulse

    NASA Astrophysics Data System (ADS)

    Roy, Sukesh; Wrzesinski, Paul; Pestov, Dmitry; Gunaratne, Tissa; Dantus, Marcos; Gord, James R.

    2009-08-01

    The feasibility is explored by single-beam coherent anti-Stokes Raman scattering (CARS) spectroscopy of gas-phase diatomic molecules related to combusting flows, with implications for gas-phase thermometry. We demonstrate CARS of gas-phase N 2 using a shaped ˜ 7 fs laser pulse, investigate the dependence of the CARS signal on the total pressure of the probed environment, both in pure N 2 and in mixtures with Ar, discuss the observed signal-to-noise ratio, and suggest improvements to be considered for reliable single-shot measurements at flame temperatures.

  20. Investigation of fiber Bragg grating as a spectral notch shaper for single-pulse coherent anti-Stokes Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Oh, Seung Ryeol; Park, Joo Hyun; Kim, Kyung-Soo; Lee, Eun Seong; Lee, Jae Yong; Kim, Soohyun

    2017-01-01

    We experimentally demonstrate compact and efficient single-pulse coherent anti-Stokes Raman spectroscopy (CARS) via spectral notch shaping implemented with a fiber Bragg grating. We show that a fiber Bragg grating can serve as a narrowband notch filtering component on a 90 nm broadband femtosecond pulsed laser without spectral distortion. Finally, we obtain CARS spectra of various samples in the fingerprint region of molecular vibrations. This scheme has potential for compact implementations of all-fiber single-pulse multiplex CARS due to its compatibility with fiber optics.

  1. Quantitative, comparable coherent anti-Stokes Raman scattering (CARS) spectroscopy: correcting errors in phase retrieval

    NASA Astrophysics Data System (ADS)

    Camp, Charles H., Jr.; Lee, Young Jong; Cicerone, Marcus T.

    2016-04-01

    Coherent anti-Stokes Raman scattering (CARS) microspectroscopy has demonstrated significant potential for biological and materials imaging. To date, however, the primary mechanism of disseminating CARS spectroscopic information is through pseudocolor imagery, which explicitly neglects a vast majority of the hyperspectral data. Furthermore, current paradigms in CARS spectral processing do not lend themselves to quantitative sample-to-sample comparability. The primary limitation stems from the need to accurately measure the so-called nonresonant background (NRB) that is used to extract the chemically-sensitive Raman information from the raw spectra. Measurement of the NRB on a pixel-by-pixel basis is a nontrivial task; thus, reference NRB from glass or water are typically utilized, resulting in error between the actual and estimated amplitude and phase. In this manuscript, we present a new methodology for extracting the Raman spectral features that significantly suppresses these errors through phase detrending and scaling. Classic methods of error-correction, such as baseline detrending, are demonstrated to be inaccurate and to simply mask the underlying errors. The theoretical justification is presented by re-developing the theory of phase retrieval via the Kramers-Kronig relation, and we demonstrate that these results are also applicable to maximum entropy method-based phase retrieval. This new error-correction approach is experimentally applied to glycerol spectra and tissue images, demonstrating marked consistency between spectra obtained using different NRB estimates, and between spectra obtained on different instruments. Additionally, in order to facilitate implementation of these approaches, we have made many of the tools described herein available free for download.

  2. Two-beam ultrabroadband coherent anti-Stokes Raman spectroscopy for high resolution gas-phase multiplex imaging

    NASA Astrophysics Data System (ADS)

    Bohlin, Alexis; Kliewer, Christopher J.

    2014-01-01

    We propose and develop a method for wideband coherent anti-Stokes Raman spectroscopy (CARS) in the gas phase and demonstrate the single-shot measurement of N2, H2, CO2, O2, and CH4. Pure-rotational and vibrational O-, Q-, and S- branch spectra are collected simultaneously, with high spectral and spatial resolution, and within a single-laser-shot. The relative intensity of the rotational and vibrational signals can be tuned arbitrarily using polarization techniques. The ultrashort 7 fs pump and Stokes pulses are automatically overlapped temporally and spatially using a two-beam CARS technique, and the crossed probe beam allows for excellent spatial sectioning of the probed location.

  3. Two-beam ultrabroadband coherent anti-Stokes Raman spectroscopy for high resolution gas-phase multiplex imaging

    SciTech Connect

    Bohlin, Alexis; Kliewer, Christopher J.

    2014-01-20

    We propose and develop a method for wideband coherent anti-Stokes Raman spectroscopy (CARS) in the gas phase and demonstrate the single-shot measurement of N{sub 2}, H{sub 2}, CO{sub 2}, O{sub 2}, and CH{sub 4}. Pure-rotational and vibrational O-, Q-, and S- branch spectra are collected simultaneously, with high spectral and spatial resolution, and within a single-laser-shot. The relative intensity of the rotational and vibrational signals can be tuned arbitrarily using polarization techniques. The ultrashort 7 fs pump and Stokes pulses are automatically overlapped temporally and spatially using a two-beam CARS technique, and the crossed probe beam allows for excellent spatial sectioning of the probed location.

  4. Femtosecond coherent anti-Stokes Raman scattering spectroscopy of hydrogen bonded structure in water and aqueous solutions.

    PubMed

    Zhu, Huaning; Li, Yang; Vdović, Silvije; Long, Saran; He, Guiying; Guo, Qianjin

    2015-12-05

    Femtosecond coherent anti-Stokes Raman scattering (fsCARS) spectroscopy, together with perturbation theory based numerical calculation, is employed to study OH stretching (υOH) of pure water and aqueous lithium chloride solutions. Vibrational OH stretching (υOH) modes of aqueous solutions are Raman-excited by a pair of ultrashort, femtosecond laser pulses, and then probed through inelastic scattering of a third, time-delayed laser field. In order to overcome limited spectral resolution of fsCARS, numerical evaluation of the CARS signal through vibrational wave packet propagation was employed in order to confirm the position of distinctive OH stretching mode that is complicated by intramolecular and intermolecular vibrational coupling. Moreover, in order to come to a microscopic description of the observed CARS spectra for aqueous solutions, we have performed molecular dynamics simulations of aqueous lithium chloride solutions with varying concentrations at ambient conditions. To this end we have analyzed the equilibrium distributions of hydrogen bonds in the first solvation shells of the ions as well as in bulk water and also computed the average number of hydrogen bonds per water molecule. According to our experimental and theoretical results on time evolution of Raman OH stretching band of water, it can be inferred that the dissolved ions mainly influence hydrogen bond strength and structure of water molecules in the first hydration shell, the addition of lithium chloride primarily breaks the tetrahedral hydrogen bonding, promotes formation of the donor hydrogen bonding in water, and slightly increases the amount of free OH bonds.

  5. Rotational coherent anti-Stokes Raman spectroscopy (CARS) applied to thermometry in high-pressure hydrocarbon flames

    SciTech Connect

    Vestin, Fredrik; Sedarsky, David; Collin, Robert; Alden, Marcus; Linne, Mark; Bengtsson, Per-Erik

    2008-07-15

    Dual-broadband rotational coherent anti-Stokes Raman spectroscopy (DB-RCARS) has been investigated for thermometry under high-pressure and high-temperature conditions, in the product gas of fuel-lean hydrocarbon flames up to 1 MPa. Initial calibration measurements made in nitrogen, oxygen, and air, at pressures up to 1.55 MPa and temperatures up to 1800 K, showed good agreement between experimental and theoretical spectra. In the high-pressure flames, high-quality single-shot spectra were recorded in which nitrogen lines dominated, and peaks from CO{sub 2} and O{sub 2} were also visible. A spectral model including the species N{sub 2}, CO{sub 2}, and O{sub 2}, as well as the best available Raman linewidth models for flame thermometry, were used to evaluate the experimental spectra. Experimental problems as well as considerations related to the spectral evaluation are discussed. This work demonstrates the significant potential of DB-RCARS thermometry for applications in high-pressure and high-temperature environments. (author)

  6. Laser Heated High Density Fluids Probed by Coherent Anti-Stokes Raman Spectroscopy

    SciTech Connect

    Baer, B J; Yoo, C

    2004-05-19

    We describe an integrated experimental method of Coherent Antistoke Raman Spectroscopy (CARS), laser-heating and diamond-anvil cell (DAC) technologies probing molecular vibrations of transparent molecular fluids at the pressure-temperature conditions of energetic detonation and Giant planetary interiors. In this method, we use a microfabricated metal toroid to conductively heat a surrounding transparent sample in a DAC, using a CW Nd:YLF laser. The laser is operated at a TEM{sub 01*} mode to match the shape of the toroid and thus produces a uniform heating area. The CARS probe utilizes two pulsed lasers with similar cavity lengths: a commercial narrow-band mode-locked Q-switched Nd:YAG laser and a home-built broadband dye laser. A strong CARS signal is then produced from the sample in the central region of laser-heated metal toroid where the two laser pulses spatially and temporally coincide. In this paper, we will demonstrate that this technique is capable of producing high quality vibrational spectra from nitrogen fluid above 2000 K and 13 GPa, where the application of spontaneous Raman spectroscopy is limited because of intense thermal radiation.

  7. Coherent Anti-Stokes Raman Scattering Spectroscopy of Single Molecules in Solution

    SciTech Connect

    Sunney Xie, Wei Min, Chris Freudiger, Sijia Lu

    2012-01-18

    During this funding period, we have developed two breakthrough techniques. The first is stimulated Raman scattering microscopy, providing label-free chemical contrast for chemical and biomedical imaging based on vibrational spectroscopy. Spontaneous Raman microscopy provides specific vibrational signatures of chemical bonds, but is often hindered by low sensitivity. We developed a three-dimensional multiphoton vibrational imaging technique based on stimulated Raman scattering (SRS). The sensitivity of SRS imaging is significantly greater than that of spontaneous Raman microscopy, which is achieved by implementing high-frequency (megahertz) phase-sensitive detection. SRS microscopy has a major advantage over previous coherent Raman techniques in that it offers background-free and readily interpretable chemical contrast. We demonstrated a variety of biomedical applications, such as differentiating distributions of omega-3 fatty acids and saturated lipids in living cells, imaging of brain and skin tissues based on intrinsic lipid contrast, and monitoring drug delivery through the epidermis. This technology offers exciting prospect for medical imaging. The second technology we developed is stimulated emission microscopy. Many chromophores, such as haemoglobin and cytochromes, absorb but have undetectable fluorescence because the spontaneous emission is dominated by their fast non-radiative decay. Yet the detection of their absorption is difficult under a microscope. We use stimulated emission, which competes effectively with the nonradiative decay, to make the chromophores detectable, as a new contrast mechanism for optical microscopy. We demonstrate a variety of applications of stimulated emission microscopy, such as visualizing chromoproteins, non-fluorescent variants of the green fluorescent protein, monitoring lacZ gene expression with a chromogenic reporter, mapping transdermal drug distribu- tions without histological sectioning, and label-free microvascular

  8. Comparison of Gas Temperatures Measured by Coherent Anti-Stokes Raman Spectroscopy (CARS) of O(2) and N(2).

    PubMed

    Reichardt, T A; Schrader, P E; Farrow, R L

    2001-02-20

    We investigate the accuracy of temperature measurements by coherent anti-Stokes Raman spectroscopy (CARS) of O(2) and use measurements taken with N(2) CARS and a thermocouple for comparison. Scanning vibrational CARS spectra of O(2) and N(2) were recorded over a broad range of temperatures: between 294 K and 1900 K in air that was heated in a tube furnace and at approximately 2450 K in a fuel-lean CH(4)-O(2)-N(2) flame. Temperatures were derived from least-squares fits of simulated and experimental spectra. Both the fundamental vibrational band and the first hot vibrational band were included in fitting. In the case of the tube furnace, the N(2) and the O(2) CARS temperature measurements agreed to within 3%, and results were similar with the thermocouple; in the flame the agreement was to within 1%. We conclude that, for cases in which O(2) is present in sufficient concentrations ( approximately 10% or greater), the accuracy of O(2) thermometry is comparable with that of N(2).

  9. Time- and frequency-resolved coherent anti-Stokes Raman scattering spectroscopy with sub-25 fs laser pulses

    NASA Astrophysics Data System (ADS)

    Lausten, Rune; Smirnova, Olga; Sussman, Benjamin J.; Gräfe, Stefanie; Mouritzen, Anders S.; Stolow, Albert

    2008-06-01

    In general, many different diagrams can contribute to the signal measured in broadband four-wave mixing experiments. Care must therefore be taken when designing an experiment to be sensitive to only the desired diagram by taking advantage of phase matching, pulse timing, sequence, and the wavelengths employed. We use sub-25 fs pulses to create and monitor vibrational wavepackets in gaseous iodine, bromine, and iodine bromide through time- and frequency-resolved femtosecond coherent anti-Stokes Raman scattering (CARS) spectroscopy. We experimentally illustrate this using iodine, where the broad bandwidths of our pulses, and Boltzmann population in the lower three vibrational levels conspire to make a single diagram dominant in one spectral region of the signal spectrum. In another spectral region, however, the signal is the sum of two almost equally contributing diagrams, making it difficult to directly extract information about the molecular dynamics. We derive simple analytical expressions for the time- and frequency-resolved CARS signal to study the interplay of different diagrams. Expressions are given for all five diagrams which can contribute to the CARS signal in our case.

  10. Ultralow frequency Stokes and anti-Stokes Raman spectroscopy of single living cells and microparticles using a hot rubidium vapor filter.

    PubMed

    Lin, Jinda; Li, Yong-qing

    2014-01-01

    We report on ultralow frequency Stokes and anti-Stokes Raman spectroscopy of single living cells and microsized particles in an aqueous medium with a frequency shift down to 10 cm(-1) by the combination of a hot rubidium (Rb) vapor filter, a confocal pinhole, and optical trapping. A single frequency-stabilized diode laser beam at 780.2 nm is used to optically trap and excite a single living cell or microparticle, and the Rayleigh scattering light from the particle is effectively blocked with a Rb vapor cell and a confocal pinhole. Ultralow frequency Raman spectra of the trapped cells or microparticles in both Stokes and anti-Stokes regions are then measured with a single-stage CCD spectrograph.

  11. Analysis of slit function errors in single-shot coherent anti-Stokes Raman spectroscopy (CARS) in practical combustors

    SciTech Connect

    Heneghan, S.P.; Vangsness, M.D. )

    1991-09-01

    The temperature determined by a single-shot coherent anti-Stokes Raman spectroscopy (CARS) system is directly related to the half width at half maximum of the instrument slit function. Therefore, an accurate knowledge of the instrument slit function is necessary to determine temperature with CARS. However, in turbulent systems, the input slits of the spectrometer may be removed in order to guarantee signal throughput and establish the necessary dynamic range. In this case, the physical input slits of the spectrometer are replaced with apparent slits created by focussing the input beams near the entrance plane of the spectrometer. The slit function will then depend on the physical relationship among all of the optical components, the probe volume, and the dispersive performance of the spectrometer and detector, as well as the optical path through density and temperature gradients which may not be invariant in a turbulent system. The presence of high temperatures and turbulence levels can effect the size of the CARS signal origin and the optical path, and as a result, the slit function is not invariant. Ignoring these changes can result in large root mean square temperatures (decreased precision) as well as mean temperature errors. The variability of the slit width can be accounted for on a shot-to-shot basis by using a two parameter (HWHM of the slit function and temperature) fitting routine. For temperatures greater than 1200 K there is convergence on a best curve implying both a temperature and a slit width. This method can be used alone or in concert with various weighting schemes to improve the precision. There are two major advantages gained by allowing the slit function to vary in a CARS system: (a) it allows an increase in the precision; (b) it allows temperatures to be calculated without the assumption that the slit function does not change with temperature or turbulence or position within the flame.

  12. Application of a backside-illuminated charge-coupled-device camera for single-pulse coherent anti-Stokes Raman spectroscopy N(2) thermometry.

    PubMed

    Plath, I; Meier, W; Stricker, W

    1992-01-01

    The application of an unintensified backside-illuminated CCD for the acquisition of broadband single-pulse coherent anti-Stokes Raman spectroscopy (CARS) spectra is demonstrated. This CCD shows a quantum efficiency 5 times higher than a front-illuminated CCD and offers significant advantages compared with intensified linear photodiode array detectors generally used for single-pulse CARS thermometry. It overcomes the main drawbacks of the intensified linear photodiode array detector in single-pulse CARS N(2) spectroscopy: nonlinearity, limited dynamic range, and image persistence. A method for extending the dynamic range is demonstrated in a highly turbulent flame.

  13. Temperature Spatially Offset Raman Spectroscopy (T-SORS): Subsurface Chemically Specific Measurement of Temperature in Turbid Media Using Anti-Stokes Spatially Offset Raman Spectroscopy.

    PubMed

    Gardner, Benjamin; Matousek, Pavel; Stone, Nicholas

    2016-01-05

    Here we propose and demonstrate a new analytical method for the noninvasive measurement of subsurface temperatures within diffusely scattering (turbid) media in combination with high chemical selectivity. The method is based upon the first combination of Stokes/anti-Stokes light scattering measurements and the recently developed spatially offset Raman spectroscopy (SORS). This approach has been conceptually demonstrated by measuring material-specific temperatures within a turbid sublayer of poly(tetrafluoroethylene) (PTFE) through a highly diffusely scattering overlayer of poly(oxymethylene) POM (3 mm thick). Root-mean-square errors (RMSEs) of 0.16-0.71 °C were achieved when measuring temperatures over ranges between 24 and 45 °C. This unique capability complements the array of existing, predominantly surface-based, temperature measurement techniques. It paves the way for a wide range of topical applications including subsurface, chemically specific, noninvasive temperature measurements within translucent media including the human body, subsurface monitoring of chemical or catalytic processes in manufacture quality and process control, and research.

  14. Lorentzian amplitude and phase pulse shaping for nonresonant background suppression and enhanced spectral resolution in coherent anti-Stokes Raman scattering spectroscopy and microscopy.

    PubMed

    Konorov, Stanislav O; Blades, Michael W; Turner, Robin F B

    2010-07-01

    Femtosecond coherent anti-Stokes Raman scattering (CARS) spectroscopy offers several advantages over spontaneous Raman spectroscopy due to the inherently high sensitivity and low average power deposition in the sample. Femtosecond CARS can be implemented in a collinear pump/probe beam configuration for microspectroscopy applications and has emerged as a powerful technique for chemical imaging of biological specimens. However, one serious limitation of this approach is the presence of a high nonresonant background component that often obscures the resonant signals of interest. We report here an innovative pulse-shaping method based on Lorentzian amplitude and phase spectral modulation of a broadband femtosecond probe pulse that yields spectra with both high spectral resolution and no nonresonant background. No further mathematical analysis is needed to extract Raman spectra. The utility of the proposed method for CARS microscopy is demonstrated using a mixture of polystyrene and latex beads, as well as dry-fixed embryonic stem cells.

  15. Communication: two-dimensional gas-phase coherent anti-Stokes Raman spectroscopy (2D-CARS): simultaneous planar imaging and multiplex spectroscopy in a single laser shot.

    PubMed

    Bohlin, Alexis; Kliewer, Christopher J

    2013-06-14

    Coherent anti-Stokes Raman spectroscopy (CARS) has been widely used as a powerful tool for chemical sensing, molecular dynamics measurements, and rovibrational spectroscopy since its development over 30 years ago, finding use in fields of study as diverse as combustion diagnostics, cell biology, plasma physics, and the standoff detection of explosives. The capability for acquiring resolved CARS spectra in multiple spatial dimensions within a single laser shot has been a long-standing goal for the study of dynamical processes, but has proven elusive because of both phase-matching and detection considerations. Here, by combining new phase matching and detection schemes with the high efficiency of femtosecond excitation of Raman coherences, we introduce a technique for single-shot two-dimensional (2D) spatial measurements of gas phase CARS spectra. We demonstrate a spectrometer enabling both 2D plane imaging and spectroscopy simultaneously, and present the instantaneous measurement of 15,000 spatially correlated rotational CARS spectra in N2 and air over a 2D field of 40 mm(2).

  16. Communication: Two-dimensional gas-phase coherent anti-Stokes Raman spectroscopy (2D-CARS): Simultaneous planar imaging and multiplex spectroscopy in a single laser shot

    NASA Astrophysics Data System (ADS)

    Bohlin, Alexis; Kliewer, Christopher J.

    2013-06-01

    Coherent anti-Stokes Raman spectroscopy (CARS) has been widely used as a powerful tool for chemical sensing, molecular dynamics measurements, and rovibrational spectroscopy since its development over 30 years ago, finding use in fields of study as diverse as combustion diagnostics, cell biology, plasma physics, and the standoff detection of explosives. The capability for acquiring resolved CARS spectra in multiple spatial dimensions within a single laser shot has been a long-standing goal for the study of dynamical processes, but has proven elusive because of both phase-matching and detection considerations. Here, by combining new phase matching and detection schemes with the high efficiency of femtosecond excitation of Raman coherences, we introduce a technique for single-shot two-dimensional (2D) spatial measurements of gas phase CARS spectra. We demonstrate a spectrometer enabling both 2D plane imaging and spectroscopy simultaneously, and present the instantaneous measurement of 15 000 spatially correlated rotational CARS spectra in N2 and air over a 2D field of 40 mm2.

  17. Communication: Two-dimensional gas-phase coherent anti-Stokes Raman spectroscopy (2D-CARS): Simultaneous planar imaging and multiplex spectroscopy in a single laser shot

    SciTech Connect

    Bohlin, Alexis; Kliewer, Christopher J.

    2013-01-01

    Coherent anti-Stokes Raman spectroscopy (CARS) has been widely used as a powerful tool for chemical sensing, molecular dynamics measurements, and rovibrational spectroscopy since its development over 30 years ago, finding use in fields of study as diverse as combustion diagnostics, cell biology, plasma physics, and the standoff detection of explosives. The capability for acquiring resolved CARS spectra in multiple spatial dimensions within a single laser shot has been a long-standing goal for the study of dynamical processes, but has proven elusive because of both phase-matching and detection considerations. Here, by combining new phase matching and detection schemes with the high efficiency of femtosecond excitation of Raman coherences, we introduce a technique for single-shot two-dimensional (2D) spatial measurements of gas phase CARS spectra. We demonstrate a spectrometer enabling both 2D plane imaging and spectroscopy simultaneously, and present the instantaneous measurement of 15, 000 spatially correlated rotational CARS spectra in N2 and air over a 2D field of 40 mm2.

  18. Spontaneous and coherent anti-Stokes Raman spectroscopy of human gastrocnemius muscle biopsies in CH-stretching region for discrimination of peripheral artery disease.

    PubMed

    Huang, X; Irmak, S; Lu, Y F; Pipinos, I; Casale, G; Subbiah, J

    2015-08-01

    Peripheral Artery Disease (PAD) is a common manifestation of atherosclerosis, characterized by lower leg ischemia and myopathy in association with leg dysfunction. In the present study, Spontaneous and coherent anti-Stokes Raman scattering (CARS) spectroscopic techniques in CH-stretching spectral region were evaluated for discriminating healthy and diseased tissues of human gastrocnemius biopsies of control and PAD patients. Since Raman signatures of the tissues in the fingerprint region are highly complex and CH containing moieties are dense, CH-stretching limited spectral range was used to classify the diseased tissues. A total of 181 Raman spectra from 9 patients and 122 CARS spectra from 12 patients were acquired. Due to the high dimensionality of the data in Raman and CARS measurements, principal component analysis (PCA) was first performed to reduce the dimensionality of the data (6 and 9 principal scores for Raman and CARS, respectively) in the CH-stretching region, followed by a discriminant function analysis (DFA) to classify the samples into different categories based on disease severity. The CH2 and CH3 vibrational signatures were observed in the Raman and CARS spectroscopy. Raman and CARS data in conjunction with PCA-DFA analysis were capable of differentiating healthy and PAD gastrocnemius with an accuracy of 85.6% and 78.7%, respectively.

  19. Tracking Ultrafast Vibrational Cooling during Excited-State Proton Transfer Reaction with Anti-Stokes and Stokes Femtosecond Stimulated Raman Spectroscopy.

    PubMed

    Liu, Weimin; Tang, Longteng; Oscar, Breland G; Wang, Yanli; Chen, Cheng; Fang, Chong

    2017-03-02

    Energy dissipation following photoexcitation is foundational to photophysics and chemistry. Consequently, understanding such processes on molecular time scales holds paramount importance. Femtosecond stimulated Raman spectroscopy (FSRS) has been used to study the molecular structure-function relationships but usually on the Stokes side. Here, we perform both Stokes and anti-Stokes FSRS to track energy dissipation and excited-state proton transfer (ESPT) for the photoacid pyranine in aqueous solution. We reveal biphasic vibrational cooling on fs-ps time scales during ESPT. Characteristic low-frequency motions (<800 cm(-1)) exhibit initial energy dissipation (∼2 ps) that correlates with functional events of forming contact ion pairs via H-bonds between photoacid and water, which lengthens to ∼9 ps in methanol where ESPT is inhibited. The interplay between photoinduced dissipative and reactive channels is implied. Thermal cooling to bulk solvent occurs on the ∼50 ps time scale. These results demonstrate the combined Stokes and anti-Stokes FSRS as a powerful toolset to elucidate structural dynamics.

  20. Measurement of the Linewidths of Hydrogen Fluoride Q-Transitions Using Coherent Anti-Stokes Raman Spectroscopy.

    DTIC Science & Technology

    1983-12-01

    Editor). Topics in Current Physics: Raman Spectroscopy of Gases and Liquids. New York, Springer-Verlag, 1979. 6. Herzberg , Gerhard . Spectra of Diatomic...rotational levels. The state densities and transition frequencies for most diatomic molecules can be calculated from theory compiled by Herzberg (6). A...Molecules. .:ew York, Van Nostrand Reinhold, 1950. 7. Huber, K.P. and G. Herzberg . Molecular Spectra and Molecular Structure": IV. Constants of Piatomic

  1. Analysis of time resolved femtosecond and femtosecond/picosecond coherent anti-Stokes Raman spectroscopy: application to toluene and Rhodamine 6G.

    PubMed

    Niu, Kai; Lee, Soo-Y

    2012-02-14

    The third-order polarization for coherent anti-Stokes Raman scattering (CARS) from a pure state is described by 48 terms in perturbation theory, but only 4 terms satisfy the rotating wave approximation. They are represented by Feynman dual time-line diagrams and four-wave mixing energy level diagrams. In time-resolved (tr) fs and fs/ps CARS from the ground vibrational state, one resonant diagram, which is the typical CARS term, with three field interactions-pump, Stokes, followed by probe-on the ket is dominant. Using the separable, displaced harmonic oscillators approximation, an analytic result is obtained for the four-time correlation function in the CARS third-order polarization. Dlott's phenomenological expression for off-resonance CARS from the ground vibrational state is derived using a three-state model. We calculated the tr fs and fs/ps CARS for toluene and Rhodamine 6G (R6G), initially in the ground vibrational state, to compare with experimental results. The observed vibrational features and major peaks for both tr fs and fs/ps CARS, from off-resonance (for toluene) to resonance (for R6G) pump wavelengths, can be well reproduced by the calculations. The connections between fs/ps CARS, fs stimulated Raman spectroscopy, and impulsive stimulated scattering for toluene and R6G are discussed.

  2. What are the intensities and line-shapes of the twenty four polarization terms in coherent anti-Stokes Raman spectroscopy?

    NASA Astrophysics Data System (ADS)

    Niu, Kai; Lee, Soo-Y.

    2015-12-01

    Coherent anti-Stokes Raman spectroscopy (CARS) is conventionally described by just one diagram/term where the three electric field interactions act on the ket side in a Feynman dual time-line diagram in a specific time order of pump, Stokes and probe pulses. In theory, however, any third-order nonlinear spectroscopy with three different electric fields interacting with a molecule can be described by forty eight diagrams/terms. They reduce to just 24 diagrams/terms if we treat the time ordering of the electric field interactions on the ket independently of those on the bra, i.e. the ket and bra wave packets evolve independently. The twenty four polarization terms can be calculated in the multidimensional, separable harmonic oscillator model to obtain the intensities and line-shapes. It is shown that in fs/ps CARS, for the two cases of off-resonance CARS in toluene and resonance CARS in rhodamine 6G, where we use a fs pump pulse, a fs Stokes pulse and a ps probe pulse, we obtain sharp vibrational lines in four of the polarization terms where the pump and Stokes pulses can create a vibrational coherence on the ground electronic state, while the spectral line-shapes of the other twenty terms are broad and featureless. The conventional CARS term with sharp vibrational lines is the dominant term, with intensity at least one order of magnitude larger than the other terms.

  3. What are the intensities and line-shapes of the twenty four polarization terms in coherent anti-Stokes Raman spectroscopy?

    SciTech Connect

    Niu, Kai; Lee, Soo-Y.

    2015-12-15

    Coherent anti-Stokes Raman spectroscopy (CARS) is conventionally described by just one diagram/term where the three electric field interactions act on the ket side in a Feynman dual time-line diagram in a specific time order of pump, Stokes and probe pulses. In theory, however, any third-order nonlinear spectroscopy with three different electric fields interacting with a molecule can be described by forty eight diagrams/terms. They reduce to just 24 diagrams/terms if we treat the time ordering of the electric field interactions on the ket independently of those on the bra, i.e. the ket and bra wave packets evolve independently. The twenty four polarization terms can be calculated in the multidimensional, separable harmonic oscillator model to obtain the intensities and line-shapes. It is shown that in fs/ps CARS, for the two cases of off-resonance CARS in toluene and resonance CARS in rhodamine 6G, where we use a fs pump pulse, a fs Stokes pulse and a ps probe pulse, we obtain sharp vibrational lines in four of the polarization terms where the pump and Stokes pulses can create a vibrational coherence on the ground electronic state, while the spectral line-shapes of the other twenty terms are broad and featureless. The conventional CARS term with sharp vibrational lines is the dominant term, with intensity at least one order of magnitude larger than the other terms.

  4. Coherent anti-Stokes Raman scattering under electric field stimulation

    NASA Astrophysics Data System (ADS)

    Capitaine, Erwan; Ould Moussa, Nawel; Louot, Christophe; Lefort, Claire; Pagnoux, Dominique; Duclère, Jean-René; Kaneyasu, Junya F.; Kano, Hideaki; Duponchel, Ludovic; Couderc, Vincent; Leproux, Philippe

    2016-12-01

    We introduce an experiment using electro-CARS, an electro-optical method based on the combination of ultrabroadband multiplex coherent anti-Stokes Raman scattering (M-CARS) spectroscopy and electric field stimulation. We demonstrate that this method can effectively discriminate the resonant CARS signal from the nonresonant background owing to a phenomenon of molecular orientation in the sample medium. Such molecular orientation is intrinsically related to the induction of an electric dipole moment by the applied static electric field. Evidence of the electro-CARS effect is obtained with a solution of n -alkanes (CnH2 n +2 , 15 ≤n ≤40 ), for which an enhancement of the CARS signal-to-noise ratio is achieved in the case of CH2 and CH3 symmetric/asymmetric stretching vibrations. Additionally, an electric-field-induced second-harmonic generation experiment is performed in order to corroborate the orientational organization of molecules due to the electric field excitation. Finally, we use a simple mathematical approach to compare the vibrational information extracted from electro-CARS measurements with spontaneous Raman data and to highlight the impact of electric stimulation on the vibrational signal.

  5. Experimental demonstration of mode-selective phonon excitation of 6H-SiC by a mid-infrared laser with anti-Stokes Raman scattering spectroscopy

    SciTech Connect

    Yoshida, Kyohei; Hachiya, Kan; Okumura, Kensuke; Mishima, Kenta; Inukai, Motoharu; Torgasin, Konstantin; Omer, Mohamed; Sonobe, Taro; Zen, Heishun; Negm, Hani; Kii, Toshiteru; Masuda, Kai; Ohgaki, Hideaki

    2013-10-28

    Mode-selective phonon excitation by a mid-infrared laser (MIR-FEL) is demonstrated via anti-Stokes Raman scattering measurements of 6H-silicon carbide (SiC). Irradiation of SiC with MIR-FEL and a Nd-YAG laser at 14 K produced a peak where the Raman shift corresponds to a photon energy of 119 meV (10.4 μm). This phenomenon is induced by mode-selective phonon excitation through the irradiation of MIR-FEL, whose photon energy corresponds to the photon-absorption of a particular phonon mode.

  6. Collinear and noncollinear emission of anti-stokes and second order stokes Raman radiation

    NASA Astrophysics Data System (ADS)

    Aussenegg, F. R.; Lippitsch, M. E.; Brandmüller, J.; Nitsch, W.

    1981-04-01

    Generating higher order stimulated Raman scattering in benzene, apart from phase-matched anti-Stokes radiation a collinear anti-Stokes emission is observed, which is explained by parametric four-photon processes under mismatch condition.

  7. Time-resolved coherent anti-Stokes Raman spectroscopy (CARS) and the measurement of vibrational spectra in shock-compressed molecular materials

    SciTech Connect

    Moore, D.S.; Schmidt, S.C.

    1990-01-01

    We present the use of coherent anti-Stokes Raman scattering (CARS) in conjunction with a two-stage light-gas gun to obtain vibrational spectra of shock-compressed liquid N{sub 2}, O{sub 2}, CO, and their mixtures. The experimental spectra are compared to spectra calculated using a semiclassical model for CARS intensities to obtain vibrational frequencies, peak Raman susceptibilities, and linewidths. The derived spectroscopic parameters suggest thermal equilibrium of the vibrational populations is established in less than a few nanoseconds after shock passage. Vibrational temperatures obtained are compared to those derived from equation-of-state calculations. Shifts in the vibrational frequencies reflect the influence of increased density and temperature on the intramolecular motion. 11 refs., 5 figs.

  8. Coherent anti-Stokes Raman scattering imaging under ambient light

    PubMed Central

    Zhang, Yinxin; Liao, Chien-Sheng; Hong, Weili; Huang, Kai-Chih; Yang, Huaidong; Jin, Guofan; Cheng, Ji-Xin

    2017-01-01

    We demonstrate ambient light coherent anti-Stokes Raman scattering (AL-CARS) microscopy that allows CARS imaging to be operated under environment light for field use. CARS signal is modulated at megahertz frequency and detected by a photodiode equipped with a lab-built resonant amplifier, then extracted through a lock-in amplifier. Filters in both spectral domain and frequency domain effectively blocked room light contamination of the CARS image. In situ hyperspectral CARS imaging of tumor tissue under ambient light is demonstrated. PMID:27519113

  9. All-solid-state parametric Raman anti-Stokes laser at 508 nm.

    PubMed

    Mildren, R P; Coutts, D W; Spence, D J

    2009-01-19

    We report a parametric anti-Stokes Raman laser using potassium gadolinium tungstate, generating output chiefly at the first anti-Stokes at 508 nm. The compact 4.5 cm long device is pumped by a Q-switched 532 nm laser and uses an off-axis Stokes resonator to provide non-collinear phase matching between the pump and the generated Stokes and anti-Stokes fields. Anti-Stokes output energies up 0.27 mJ were obtained at a conversion efficiency from the pump of 0.46%. Second- and third-order anti-Stokes lines at 486 nm and 465 nm were also observed.

  10. High-spectral-resolution coherent anti-Stokes Raman scattering with interferometrically detected broadband chirped pulses.

    PubMed

    Jones, Gareth W; Marks, Daniel L; Vinegoni, Claudio; Boppart, Stephen A

    2006-05-15

    To achieve high-spectral-resolution multiplex coherent anti-Stokes Raman scattering (CARS), one typically uses a narrowband pump pulse and a broadband Stokes pulse. This is to ensure a correspondence between anti-Stokes and vibrational frequencies. We obtain high-resolution CARS spectra of isopropanol, using a broadband chirped pump pulse and a broadband Stokes pulse, by detecting the anti-Stokes pulse with spectral interferometry. With the temporally resolved anti-Stokes signal, we can remove the chirp of the anti-Stokes pulse and restore high spectral resolution while also rejecting nonresonant scattering.

  11. Polarized multiplex coherent anti-Stokes Raman scattering using a picosecond laser and a fiber supercontinuum.

    PubMed

    Michel, Sébastien; Courjaud, Antoine; Mottay, Eric; Finot, Christophe; Dudley, John; Rigneault, Hervé

    2011-02-01

    We perform multiplex coherent anti-Stokes Raman scattering (CARS) micro-spectroscopy with a picosecond pulsed laser and a broadband supercontinuum (SC) generated in photonic crystal fiber. CARS signal stability is achieved using an active fiber coupler that avoids thermal and mechanical drifts. We obtain multiplex CARS spectra for test liquids in the 600-2000 cm(-1) spectral range. In addition we investigate the polarization dependence of the CARS spectra when rotating the pump beam linear polarization state relative to the linearly polarized broad stokes SC. From these polarization measurements we deduce the Raman depolarization ratio, the resonant versus nonresonant contribution, the Raman resonance frequency, and the linewidth.

  12. Polarized multiplex coherent anti-Stokes Raman scattering using a picosecond laser and a fiber supercontinuum

    NASA Astrophysics Data System (ADS)

    Michel, Sébastien; Courjaud, Antoine; Mottay, Eric; Finot, Christophe; Dudley, John; Rigneault, Hervé

    2011-02-01

    We perform multiplex coherent anti-Stokes Raman scattering (CARS) micro-spectroscopy with a picosecond pulsed laser and a broadband supercontinuum (SC) generated in photonic crystal fiber. CARS signal stability is achieved using an active fiber coupler that avoids thermal and mechanical drifts. We obtain multiplex CARS spectra for test liquids in the 600-2000 cm-1 spectral range. In addition we investigate the polarization dependence of the CARS spectra when rotating the pump beam linear polarization state relative to the linearly polarized broad stokes SC. From these polarization measurements we deduce the Raman depolarization ratio, the resonant versus nonresonant contribution, the Raman resonance frequency, and the linewidth.

  13. Quantitative coherent anti-Stokes Raman scattering (CARS) microscopy.

    PubMed

    Day, James P R; Domke, Katrin F; Rago, Gianluca; Kano, Hideaki; Hamaguchi, Hiro-o; Vartiainen, Erik M; Bonn, Mischa

    2011-06-23

    The ability to observe samples qualitatively at the microscopic scale has greatly enhanced our understanding of the physical and biological world throughout the 400 year history of microscopic imaging, but there are relatively few techniques that can truly claim the ability to quantify the local concentration and composition of a sample. We review coherent anti-Stokes Raman scattering (CARS) as a quantitative, chemically specific, and label-free microscopy. We discuss the complicating influence of the nonresonant response on the CARS signal and the various experimental and mathematical approaches that can be adopted to extract quantitative information from CARS. We also review the uses to which CARS has been employed as a quantitative microscopy to solve challenges in material and biological science.

  14. Coherent anti-Stokes Raman scattering microscopy of single nanodiamonds

    PubMed Central

    Pope, Iestyn; Payne, Lukas; Zoriniants, George; Thomas, Evan; Williams, Oliver; Watson, Peter; Langbein, Wolfgang; Borri, Paola

    2016-01-01

    Nanoparticles have attracted enormous attention for biomedical applications as optical labels, drug delivery vehicles, and contrast agents in vivo. In the quest for superior photostability and bio-compatibility, nanodiamonds (NDs) are considered one of the best choices due to their unique structural, chemical, mechanical, and optical properties. So far, mainly fluorescent NDs have been utilized for cell imaging. However, their use is limited by the efficiency and costs in reliably producing fluorescent defect centers with stable optical properties. Here, we show that single non-fluorescing NDs exhibit strong coherent anti-Stokes Raman scattering (CARS) at the sp3 vibrational resonance of diamond. Using correlative light and electron microscopy, the relationship between CARS signal strength and ND size is quantified. The calibrated CARS signal in turn enables the analysis of the number and size of NDs internalized in living cells in situ, which opens the exciting prospect of following complex cellular trafficking pathways quantitatively. PMID:25305746

  15. Coherent anti-Stokes Raman scattering microscopy of single nanodiamonds

    NASA Astrophysics Data System (ADS)

    Pope, Iestyn; Payne, Lukas; Zoriniants, George; Thomas, Evan; Williams, Oliver; Watson, Peter; Langbein, Wolfgang; Borri, Paola

    2014-11-01

    Nanoparticles have attracted enormous attention for biomedical applications as optical labels, drug-delivery vehicles and contrast agents in vivo. In the quest for superior photostability and biocompatibility, nanodiamonds are considered one of the best choices due to their unique structural, chemical, mechanical and optical properties. So far, mainly fluorescent nanodiamonds have been utilized for cell imaging. However, their use is limited by the efficiency and costs in reliably producing fluorescent defect centres with stable optical properties. Here, we show that single non-fluorescing nanodiamonds exhibit strong coherent anti-Stokes Raman scattering (CARS) at the sp3 vibrational resonance of diamond. Using correlative light and electron microscopy, the relationship between CARS signal strength and nanodiamond size is quantified. The calibrated CARS signal in turn enables the analysis of the number and size of nanodiamonds internalized in living cells in situ, which opens the exciting prospect of following complex cellular trafficking pathways quantitatively.

  16. Coherent anti-Stokes Raman scattering microscopy of single nanodiamonds.

    PubMed

    Pope, Iestyn; Payne, Lukas; Zoriniants, George; Thomas, Evan; Williams, Oliver; Watson, Peter; Langbein, Wolfgang; Borri, Paola

    2014-11-01

    Nanoparticles have attracted enormous attention for biomedical applications as optical labels, drug-delivery vehicles and contrast agents in vivo. In the quest for superior photostability and biocompatibility, nanodiamonds are considered one of the best choices due to their unique structural, chemical, mechanical and optical properties. So far, mainly fluorescent nanodiamonds have been utilized for cell imaging. However, their use is limited by the efficiency and costs in reliably producing fluorescent defect centres with stable optical properties. Here, we show that single non-fluorescing nanodiamonds exhibit strong coherent anti-Stokes Raman scattering (CARS) at the sp(3) vibrational resonance of diamond. Using correlative light and electron microscopy, the relationship between CARS signal strength and nanodiamond size is quantified. The calibrated CARS signal in turn enables the analysis of the number and size of nanodiamonds internalized in living cells in situ, which opens the exciting prospect of following complex cellular trafficking pathways quantitatively.

  17. Coherent anti-Stokes Raman scattering and spontaneous Raman scattering diagnostics of nonequilibrium plasmas and flows

    NASA Astrophysics Data System (ADS)

    Lempert, Walter R.; Adamovich, Igor V.

    2014-10-01

    The paper provides an overview of the use of coherent anti-Stokes Raman scattering (CARS) and spontaneous Raman scattering for diagnostics of low-temperature nonequilibrium plasmas and nonequilibrium high-enthalpy flows. A brief review of the theoretical background of CARS, four-wave mixing and Raman scattering, as well as a discussion of experimental techniques and data reduction, are included. The experimental results reviewed include measurements of vibrational level populations, rotational/translational temperature, electric fields in a quasi-steady-state and transient molecular plasmas and afterglow, in nonequilibrium expansion flows, and behind strong shock waves. Insight into the kinetics of vibrational energy transfer, energy thermalization mechanisms and dynamics of the pulse discharge development, provided by these experiments, is discussed. Availability of short pulse duration, high peak power lasers, as well as broadband dye lasers, makes possible the use of these diagnostics at relatively low pressures, potentially with a sub-nanosecond time resolution, as well as obtaining single laser shot, high signal-to-noise spectra at higher pressures. Possibilities for the development of single-shot 2D CARS imaging and spectroscopy, using picosecond and femtosecond lasers, as well as novel phase matching and detection techniques, are discussed.

  18. Coherent anti-Stokes Raman scattering hyperspectral tissue imaging with a wavelength-swept system

    PubMed Central

    Bégin, Steve; Burgoyne, Bryan; Mercier, Vincent; Villeneuve, Alain; Vallée, Réal; Côté, Daniel

    2011-01-01

    We present a wavelength-swept coherent anti-Stokes Raman scattering (WS-CARS) spectroscopy system for hyperspectral imaging in thick tissue. We use a strategy where the Raman lines are excited sequentially, circumventing the need for a spectrometer. This fibre laser system, consisting of a pump laser synchronized with a rapidly tunable programmable laser (PL), can access Raman lines over a significant fraction of the high wavenumber region (2700–2950 cm−1) at rates of up to 10,000 spectral points per second. To demonstrate its capabilities, we have acquired WS-CARS spectra of several samples as well as images and hyperspectral images (HSI) of thick tissue both in forward and epi-detection. This instrument should be especially useful in providing local biochemical information with surrounding context supplied by imaging. PMID:21559141

  19. Coherent anti-Stokes Raman scattering microscopy: overcoming technical barriers for clinical translation.

    PubMed

    Tu, Haohua; Boppart, Stephen A

    2014-01-01

    Clinical translation of coherent anti-Stokes Raman scattering microscopy is of great interest because of the advantages of noninvasive label-free imaging, high sensitivity, and chemical specificity. For this to happen, we have identified and review the technical barriers that must be overcome. Prior investigations have developed advanced techniques (features), each of which can be used to effectively overcome one particular technical barrier. However, the implementation of one or a small number of these advanced features in previous attempts for clinical translation has often introduced more tradeoffs than benefits. In this review, we outline a strategy that would integrate multiple advanced features to overcome all the technical barriers simultaneously, effectively reduce tradeoffs, and synergistically optimize CARS microscopy for clinical translation. The operation of the envisioned system incorporates coherent Raman micro-spectroscopy for identifying vibrational biomolecular markers of disease and single-frequency (or hyperspectral) Raman imaging of these specific biomarkers for real-time in vivo diagnostics and monitoring.

  20. Nanosecond retinal structure changes in K-590 during the room-temperature bacteriorhodopsin photocycle: picosecond time-resolved coherent anti-stokes Raman spectroscopy.

    PubMed Central

    Weidlich, O; Ujj, L; Jäger, F; Atkinson, G H

    1997-01-01

    Time-resolved vibrational spectra are used to elucidate the structural changes in the retinal chromophore within the K-590 intermediate that precedes the formation of the L-550 intermediate in the room-temperature (RT) bacteriorhodopsin (BR) photocycle. Measured by picosecond time-resolved coherent anti-Stokes Raman scattering (PTR/CARS), these vibrational data are recorded within the 750 cm-1 to 1720 cm-1 spectral region and with time delays of 50-260 ns after the RT/BR photocycle is optically initiated by pulsed (< 3 ps, 1.75 nJ) excitation. Although K-590 remains structurally unchanged throughout the 50-ps to 1-ns time interval, distinct structural changes do appear over the 1-ns to 260-ns period. Specifically, comparisons of the 50-ps PTR/CARS spectra with those recorded with time delays of 1 ns to 260 ns reveal 1) three types of changes in the hydrogen-out-of-plane (HOOP) region: the appearance of a strong, new feature at 984 cm-1; intensity decreases for the bands at 957 cm-1, 952 cm-1, and 939 cm-1; and small changes intensity and/or frequency of bands at 855 cm-1 and 805 cm-1; and 2) two types of changes in the C-C stretching region: the intensity increase in the band at 1196 cm-1 and small intensity changes and/or frequency shifts for bands at 1300 cm-1 and 1362 cm-1. No changes are observed in the C = C stretching region, and no bands assignable to the Schiff base stretching mode (C = NH+) mode are found in any of the PTR/CARS spectra assignable to K-590. These PTR/CARS data are used, together with vibrational mode assignments derived from previous work, to characterize the retinal structural changes in K-590 as it evolves from its 3.5-ps formation (ps/K-590) through the nanosecond time regime (ns/K-590) that precedes the formation of L-550. The PTR/CARS data suggest that changes in the torsional modes near the C14-C15 = N bonds are directly associated with the appearance of ns/K-590, and perhaps with the KL intermediate proposed in earlier studies. These

  1. Transverse chemical interface detection with coherent anti-Stokes Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Brustlein, Sophie; Gachet, David; Billard, Franck; Rigneault, Hervé

    2011-08-01

    Transverse ``chemical'' interfaces are revealed with a conventional two beam narrowband coherent anti-Stokes Raman scattering microscopy setup in a collinear configuration. The exciting ``pump'' and ``Stokes'' beams are focused on the sample in two opposite directions. The subtraction of the two generated anti-Stokes signals gives rise to a signal that is directly proportional to the pure Raman spectrum of the resonant medium. This property is used to highlight an interface between glass and N,N-dimethylformamide (DMF) and recover the pure Raman spectrum of DMF around its 1408 cm-1 vibrational band.

  2. Phase-cycling coherent anti-Stokes Raman scattering using shaped femtosecond laser pulses.

    PubMed

    Li, Baolei; Warren, Warren S; Fischer, Martin C

    2010-12-06

    We demonstrate a homodyne coherent anti-Stokes Raman scattering (CARS) technique based on femtosecond laser pulse shaping. This technique utilizes fast phase cycling to extract nonlinear Raman signatures with a self-generated reference signal acting as a local oscillator. The local oscillator is generated at the focus and is intrinsically stable relative to the Raman signal even in highly scattering samples. We can therefore retrieve phase information from the Raman signal and can suppress the ubiquitous non-resonant background.

  3. Coherent Anti-Stokes Raman Spectroscopic Thermometry in a Supersonic Combustor

    NASA Technical Reports Server (NTRS)

    Cutler, A. D.; Danehy, P. M.; Springer, R. R.; OByrne, S.; Capriotti, D. P.; DeLoach, R.

    2003-01-01

    An experiment has been conducted to acquire data for the validation of computational fluid dynamics codes used in the design of supersonic combustors. The flow in a supersonic combustor, consisting of a diverging duct with a single downstream-angled wail injector, is studied. Combustor entrance Mach number is 2 and enthalpy nominally corresponds to Mach 7 flight. The primary measurement technique is coherent anti-Stokes Raman spectroscopy, but surface pressures and temperatures have also been acquired. Modern design of experiment techniques have been used to maximize the quality of the data set (for the given level of effort) and to minimize systematic errors. Temperature maps are obtained at several planes in the flow for a case in which the combustor is piloted by injecting fuel upstream of the main injector and one case in which it is not piloted. Boundary conditions and uncertainties are characterized.

  4. High enhancement factor of Au nano triangular prism structure for surface enhanced coherent anti-Stokes Raman scattering

    NASA Astrophysics Data System (ADS)

    Zhang, Zuyin; Song, Guofeng

    2017-02-01

    Coherent anti-Stokes Raman scattering spectroscopy (CARS) is a well-known detecting tool in biosensing and nonlinear spectroscopy. It can provide a non-invasive alternative without the need for exogenous labels, while the enhancement factor for surface plasmon resonances (SPR) are extensively used to increase the local field close to the oscillators and which can obtain high enhancement. In this work, we investigate the enhancement factor of our structure for surface-enhanced coherent anti-Stokes Raman scattering. The absorption spectrum of the structure has been studied, a wide range of absorption has been realized. The enhancement can be as high as 10{16} over standard CARS. Our design is very useful for improving the enhancement factor of surface-enhanced coherent anti-Stokes Raman scattering. Project supported by the National Key Research Program of China (No. 2011ZX01015-001) and the National Basic Research Program of China (Nos. 2011CBA00608, 2012CB619203, 2015CB351902, 2015CB932402).

  5. Broadband coherent anti-Stokes Raman scattering (CARS): a potential tool for atherosclerosis diagnostic imaging

    NASA Astrophysics Data System (ADS)

    Cormier, J.-F.; Ko, A.; Choo-Smith, L.-P.; Werner, J.; Kohlenberg, E.; Hewko, M.; Fréchette, J.; Fortin, M.; Noiseux, I.; Bouchard, J. P.; Gay, David; Desroches, P.; Roy-Moisan, Francois; Bourgault, Marie-Eve; Sowa, M. G.; Vernon, M. L.

    2007-02-01

    Nonlinear optical imaging technologies offer some intriguing medical diagnostic applications. Examples include fast imaging of elastin and collagen distributions in diseased tissues using two-photon fluorescence (TPF) and second harmonic generation (SHG), respectively. The 3D sectioning capabilities and biochemical specificity that enable fast imaging in highly scattering biological media lie at the heart of the appeal of these nonlinear approaches for medical applications. One of these promising nonlinear techniques relies on the resonance enhancement of the third order nonlinear susceptibility by a vibrational mode of a molecule. Coherent Anti-Stokes Raman Scattering (CARS) can provide similar vibrational information as a spontaneous Raman spectrum. The technique has been shown to be orders of magnitude more sensitive than spontaneous Raman, with video rate imaging demonstrated recently. In this work, we investigate the potential use of broadband CARS spectroscopy and CARS imaging for biochemical analysis of arterial tissue. Biochemical imaging data from broadband CARS is compared with spontaneous Raman microspectroscopy. The broadband CARS system comprised of a single femtosecond-laser is presented in detail. Issues related to data analysis, the advantages and current limitations of the CARS technique in biodiagnostics are discussed.

  6. Coherent anti-Stokes Raman scattering (CARS) microscopy visualizes pharmaceutical tablets during dissolution.

    PubMed

    Fussell, Andrew L; Kleinebudde, Peter; Herek, Jennifer; Strachan, Clare J; Offerhaus, Herman L

    2014-07-04

    Traditional pharmaceutical dissolution tests determine the amount of drug dissolved over time by measuring drug content in the dissolution medium. This method provides little direct information about what is happening on the surface of the dissolving tablet. As the tablet surface composition and structure can change during dissolution, it is essential to monitor it during dissolution testing. In this work coherent anti-Stokes Raman scattering microscopy is used to image the surface of tablets during dissolution while UV absorption spectroscopy is simultaneously providing inline analysis of dissolved drug concentration for tablets containing a 50% mixture of theophylline anhydrate and ethyl cellulose. The measurements showed that in situ CARS microscopy is capable of imaging selectively theophylline in the presence of ethyl cellulose. Additionally, the theophylline anhydrate converted to theophylline monohydrate during dissolution, with needle-shaped crystals growing on the tablet surface during dissolution. The conversion of theophylline anhydrate to monohydrate, combined with reduced exposure of the drug to the flowing dissolution medium resulted in decreased dissolution rates. Our results show that in situ CARS microscopy combined with inline UV absorption spectroscopy is capable of monitoring pharmaceutical tablet dissolution and correlating surface changes with changes in dissolution rate.

  7. Evaluation of turbulence induced noise in coherent anti-Stokes Raman scattering

    NASA Technical Reports Server (NTRS)

    Elliott, R. A.

    1982-01-01

    The effect of turbulence in a transonic wind tunnel on coherent anti-Stokes Raman scattering is considered. The driving pump and Stokes waves are taken to be coaxially propagating Gaussian beam waves which are focused on the Raman active medium through the turbulent boundary layer of the flow tube. The random index of refraction variations in the layer are modeled as phase perturbations of the driving waves which cause a reduction of the mean on-axis field and an increase in the mean diameter of the beams. Effective Gaussian beam parameters are developed and the radiated anti-Stokes power calculated as a function of the phase screen parameters. A significant reduction in signal strength occurs for realistic estimates of the phase screen parameter appropriate to a confined transonic flow. A method for estimating the signal degradation which could be applied to other experimental situations is presented.

  8. Combustion Diagnostics by Pure Rotational Coherent Anti-Stokes Raman Scattering

    NASA Astrophysics Data System (ADS)

    Leipertz, Alfred; Seeger, Thomas

    Since its first use in Richard Chang's laboratory in 1982 in a comparative study with vibrational coherent anti-Stokes Raman scattering (VCARS) in a flame, pure rotational coherent anti-Stokes Raman scattering (RCARS) has gained tremendous importance for gas temperature and relative species concentration measurements in combustion diagnostics. The field of application covers basic studies on diagnostics development and on flame research as well as its use in technical combustion systems, e.g., for the determination of the gas-phase temperature in the vaporizing spray of a gasoline direct injection (GDI) injector or for the simultaneous measurement of gas temperature and exhaust-gas-recirculation rate (EGR rate) in a homogeneous charge compression ignition (HCCI) engine. An overview is given on the fundamentals of the technique and on its most important technical applications.

  9. Single laser source for multimodal coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Pegoraro, Adrian F; Slepkov, Aaron D; Ridsdale, Andrew; Pezacki, John Paul; Stolow, Albert

    2010-09-01

    Short laser pulse technology has significantly contributed to biomedical research, especially via nonlinear optical microscopy. Coherent anti-Stokes Raman scattering (CARS) microscopy is a label-free, chemical-selective method that is growing in importance as improved methods and light sources develop. Here we discuss different approaches to laser source development for CARS microscopy and highlight the advantages of a multimodal CARS microscope, illustrated by selected applications in biomedical research.

  10. Macrophages interaction with pulmonary surfactant using coherent anti-Stokes Raman scattering (CARS) microscopy

    NASA Astrophysics Data System (ADS)

    Ocampo, Minette; Telesford, Dana Marie; Allen, Heather

    2012-04-01

    Alveolar pulmonary surfactant, composed mostly of phospholipids, is essential for maintenance of normal lung function. However, increased production of lung surfactant can lead to many pulmonary inflammatory disorders. Alveolar macrophages are responsible for the degradation of the surfactant and exhibit increased lipid uptake in inflamated lungs. Owing to their limited clearance capability, excessive accumulation of surfactant may impair their phagocytic function. In this study, the interaction of the macrophages with different lipid components was studied using coherent anti-Stokes Raman scattering (CARS) microscopy. CARS microscopy, a nonlinear vibrational technique which combines spectroscopy and microscopy, allows noninvasive characterization and imaging of chemical species without preparation or labeling. A monolayer of THP-1 macrophages and palmitic acid-d31 on phosphate buffer solution was transferred to a coverslip using the Langmuir-Blodgett method and then imaged using CARS by mapping the CH2 stretch signal of the lipid membrane of the macrophage and C-D stretch signal from palmitic acid-d31. Preliminary results showed CARS images of the macrophage on the solid substrate and thermal degradation of the sample due to long exposure to high laser power. A contrast image is expected to be observed by mapping the CH2 and C-D signals, which can show the lipid interaction and phagocytosis of the macrophage.

  11. Femtosecond Coherent Anti-Stokes Raman Scattering Gas Phase Thermometry at 5 kHz

    NASA Astrophysics Data System (ADS)

    Fineman, Claresta; Lucht, Robert

    2014-05-01

    Understanding the thermal instabilities occurring in turbulent combustion, such as in modern gas turbine combustors, is critical for more reliable and fuel-efficient operation. Non-intrusive laser based spectroscopy methods have been documented as the techniques of choice for turbulent combustion diagnostics. Specifically, femtosecond coherent anti-Stokes Raman scattering (fs-CARS) thermometry has been established for temporal resolution of turbulent fluctuations in flame structure and provides accurate measurements across a wide range of temperatures. Experiments performed to date include 5 kHz pure vibrational N2 chirped probe-pulse fs-CARS thermometry on non-premixed hydrogen jet diffusion flames, methane jet diffusion flames, and the DLR gas turbine model combustor (GTMC). The fs-CARS signal generation process requires precise spatial and temporal overlap of tightly focused pulsed laser beams of less than 100 fs pulse duration. Here, signal loss due to beam steering, pressure fluctuations, or shear layer density gradients can become a problem. The effect of such interferences has been investigated using high velocity flow of compressed nitrogen gas from a converging-diverging nozzle. Resulting changes in fs-CARS spectra have been studied. Funding for this work was provided by the U.S. Department of Energy, Division of Chemical Sciences, Geosciences and Biosciences.

  12. Chemical imaging by single pulse interferometric coherent anti-stokes Raman scattering microscopy.

    PubMed

    Lim, Sang-Hyun; Caster, Allison G; Nicolet, Olivier; Leone, Stephen R

    2006-03-23

    A single pulse interferometric coherent anti-Stokes Raman (CARS) spectroscopy method is used to obtain broadband CARS spectra and microscopy images of liquid and polymer samples. The pump, Stokes, and probe pulses are all selected inside a single broadband ultrafast pulse by a phase- and polarization-controlled pulse shaping technique and used to generate two spectral interference CARS signals simultaneously. The normalized difference of these two signals provides an amplified background-free broadband resonant CARS spectrum over the 400-1500 cm(-1) range with 35 cm(-1) spectral resolution. Chemically selective microscopy images of multicomponent polymer and liquid samples are investigated with this new CARS method. Multiplex CARS spectra at 10,000 spatial points are measured within a few minutes, and used to construct chemically selective microscopy images with a spatial resolution of 400 nm. The spectral bandwidth limits, sensitivity, homodyne amplification advantages, spatial resolution, depolarization, chromatic aberration, and chemical imaging aspects of this new technique are discussed in detail.

  13. Revealing silent vibration modes of nanomaterials by detecting anti-Stokes hyper-Raman scattering with femtosecond laser pulses.

    PubMed

    Zeng, Jianhua; Chen, Lei; Dai, Qiaofeng; Lan, Sheng; Tie, Shaolong

    2016-01-21

    We proposed a scheme in which normal Raman scattering is coupled with hyper-Raman scattering for generating a strong anti-Stokes hyper-Raman scattering in nanomaterials by using femtosecond laser pulses. The proposal was experimentally demonstrated by using a single-layer MoS2 on a SiO2/Si substrate, a 17 nm-thick MoS2 on an Au/SiO2 substrate and a 9 nm-thick MoS2 on a SiO2-SnO2/Ag/SiO2 substrate which were confirmed to be highly efficient for second harmonic generation. A strong anti-Stokes hyper-Raman scattering was also observed in other nanomaterials possessing large second-order susceptibilities, such as silicon quantum dots self-assembled into "coffee" rings and tubular Cu-doped ZnO nanorods. In all the cases, many Raman inactive vibration modes were clearly revealed in the anti-Stokes hyper-Raman scattering. Apart from the strong anti-Stokes hyper-Raman scattering, Stokes hyper-Raman scattering with small Raman shifts was detected during the ablation process of thick MoS2 layers. It was also observed by slightly defocusing the excitation light. The detection of anti-Stokes hyper-Raman scattering may serve as a new technique for studying the Raman inactive vibration modes in nanomaterials.

  14. Spectroscopie Raman Anti-Stokes Cohérente femtoseconde (DRASC fs) : expériences et modélisation dans le cas du mélange H{2} N{2} à basse pression

    NASA Astrophysics Data System (ADS)

    Chaussard, F.; Le Cong, N.; Lavorel, B.; Renard, V.; Faucher, O.; Tran, H.; Joubert, P.; Bonamy, L.

    2006-10-01

    Dans l'objectif du diagnostic de la température dans les milieux en combustion, la Diffusion Raman Anti-Stokes Cohérente résolue en temps (DRASC fs) est utilisée pour sonder H{2} dans les mélanges H{2}-N{2} à basse pression. Le dispositif DRASC mis en place est décrit en détail. Un nouveau modèle de la réponse DRASC temporelle, prenant en compte tous les effets collisionnels spécifiques à l'hydrogène (effets dits ”de vitesse") est présentée, ainsi que la comparaison avec l'expérience, l'accord se révélant très satisfaisant.

  15. Coherent anti-Stokes Raman microspectroscopy using spectral focusing with glass dispersion

    SciTech Connect

    Rocha-Mendoza, Israel; Langbein, Wolfgang; Borri, Paola

    2008-11-17

    We demonstrate experimentally that coherent anti-Stokes Raman microspectroscopy with high spectral resolution is achieved using femtosecond laser pulses chirped up to a few picoseconds by glass elements of known group-velocity dispersion without significant intensity losses. By simply choosing the length of the glass, the chirp of Stokes and pump pulses is tailored to obtain a spectral resolution given by the Fourier limit of the chirped pulse duration. We show that for chirped pulse durations shorter than or comparable to the Raman coherence time, maximum signal occurs for a pump arriving after the Stokes pulse, a time-ordering effect confirmed by numerical simulations.

  16. Broadly tunable dual-wavelength light source for coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Ganikhanov, Feruz; Carrasco, Silvia; Sunney Xie, X; Katz, Mordechai; Seitz, Wolfgang; Kopf, Daniel

    2006-05-01

    The signal and idler beams from a picosecond, synchronously pumped optical parametric oscillator (OPO) provide the two colors necessary for coherent anti-Stokes Raman scattering (CARS) microscopy. The OPO provides a continuously tunable frequency difference between the two beams over a broad range of Raman shifts (100-3700 cm(-1)) by varying the temperature of a single nonlinear crystal. The near-infrared output (900-1300 nm) allows for deep penetration into thick samples and reduced nonlinear photodamage. Applications of this light source to in vivo cell and ex vivo tissue imaging are demonstrated.

  17. Lipid-cell interactions in human monocytes investigated by doubly-resonant coherent anti-Stokes Raman scattering microscopy

    PubMed Central

    Weeks, Tyler; Schie, Iwan; den Hartigh, Laura J.; Rutledge, John C.; Huser, Thomas

    2011-01-01

    We demonstrate that doubly-resonant coherent anti-Stokes Raman scattering can provide enhanced and highly specific contrast for molecules containing unique Raman-active small molecular groups. This combination provides contrast for molecules that can otherwise be difficult to discriminate by Raman spectroscopy. Here, human monocytes were incubated with either deuterated oleic acid or 17-octadecynoic acid (a fatty acid with an end terminal acetylene group). The carbon-deuterium stretching vibration of the deuterated fatty acid, as well as the unique alkyne stretching vibration of the alkyne-containing fatty acid, were used to provide contrast for these exogenous free fatty acids. The combination of these unique modes with the common aliphatic carbon-hydrogen stretching vibration inherent to all fatty acid allowed for doubly-resonant detection of these unique molecules and enabled us to detect the presence of these lipids in areas within a cell where each molecular resonance by itself did not generate sufficient signal. PMID:21361680

  18. Direct imaging of molecular symmetry by coherent anti-stokes Raman scattering

    PubMed Central

    Cleff, Carsten; Gasecka, Alicja; Ferrand, Patrick; Rigneault, Hervé; Brasselet, Sophie; Duboisset, Julien

    2016-01-01

    Nonlinear optical methods, such as coherent anti-Stokes Raman scattering and stimulated Raman scattering, are able to perform label-free imaging, with chemical bonds specificity. Here we demonstrate that the use of circularly polarized light allows to retrieve not only the chemical nature but also the symmetry of the probed sample, in a single measurement. Our symmetry-resolved scheme offers simple access to the local organization of vibrational bonds and as a result provides enhanced image contrast for anisotropic samples, as well as an improved chemical selectivity. We quantify the local organization of vibrational bonds on crystalline and biological samples, thus providing information not accessible by spontaneous Raman and stimulated Raman scattering techniques. This work stands for a symmetry-resolved contrast in vibrational microscopy, with potential application in biological diagnostic. PMID:27189667

  19. Two-beam femtosecond coherent anti-Stokes Raman scattering for thermometry on CO2

    NASA Astrophysics Data System (ADS)

    Kerstan, M.; Makos, I.; Nolte, S.; Tünnermann, A.; Ackermann, R.

    2017-01-01

    We show that two-beam femtosecond coherent anti-Stokes Raman scattering can be effectively used for thermometry on CO2 for temperatures between ˜100 °C and ˜600 °C at a maximum pressure of 8.5 bar. The temperature measurement is based on probing the vibrationally excited states of CO2, using a ˜7 fs pump/Stokes pulse and a narrowband (˜0.3 nm) probe pulse. The temperatures can be derived from a single spectrum, obviating the need for a delay scan or a chirped probe pulse.

  20. Optimizing coherent anti-Stokes Raman scattering by genetic algorithm controlled pulse shaping

    NASA Astrophysics Data System (ADS)

    Yang, Wenlong; Sokolov, Alexei

    2010-10-01

    The hybrid coherent anti-Stokes Raman scattering (CARS) has been successful applied to fast chemical sensitive detections. As the development of femto-second pulse shaping techniques, it is of great interest to find the optimum pulse shapes for CARS. The optimum pulse shapes should minimize the non-resonant four wave mixing (NRFWM) background and maximize the CARS signal. A genetic algorithm (GA) is developed to make a heuristic searching for optimized pulse shapes, which give the best signal the background ratio. The GA is shown to be able to rediscover the hybrid CARS scheme and find optimized pulse shapes for customized applications by itself.

  1. A versatile setup using femtosecond adaptive spectroscopic techniques for coherent anti-Stokes Raman scattering

    SciTech Connect

    Shen, Yujie; Voronine, Dmitri V.; Sokolov, Alexei V.; Scully, Marlan O.

    2015-08-15

    We report a versatile setup based on the femtosecond adaptive spectroscopic techniques for coherent anti-Stokes Raman scattering. The setup uses a femtosecond Ti:Sapphire oscillator source and a folded 4f pulse shaper, in which the pulse shaping is carried out through conventional optical elements and does not require a spatial light modulator. Our setup is simple in alignment, and can be easily switched between the collinear single-beam and the noncollinear two-beam configurations. We demonstrate the capability for investigating both transparent and highly scattering samples by detecting transmitted and reflected signals, respectively.

  2. A versatile setup using femtosecond adaptive spectroscopic techniques for coherent anti-Stokes Raman scattering.

    PubMed

    Shen, Yujie; Voronine, Dmitri V; Sokolov, Alexei V; Scully, Marlan O

    2015-08-01

    We report a versatile setup based on the femtosecond adaptive spectroscopic techniques for coherent anti-Stokes Raman scattering. The setup uses a femtosecond Ti:Sapphire oscillator source and a folded 4f pulse shaper, in which the pulse shaping is carried out through conventional optical elements and does not require a spatial light modulator. Our setup is simple in alignment, and can be easily switched between the collinear single-beam and the noncollinear two-beam configurations. We demonstrate the capability for investigating both transparent and highly scattering samples by detecting transmitted and reflected signals, respectively.

  3. Spontaneous anti-Stokes Raman probe for gas temperature measurements in industrial furnaces.

    PubMed

    Zikratov, G; Yueh, F Y; Singh, J P; Norton, O P; Kumar, R A; Cook, R L

    1999-03-20

    A compact, pulsed Nd:YAG laser-based instrument has been built to measure in situ absolute gas temperatures in large industrial furnaces by use of spontaneous anti-Stokes Raman scattering. The backscattering configuration was used to simplify the optics alignment and increase signal-to-noise ratios. Gated signal detection significantly reduced the background emission that is found in combustion environments. The anti-Stokes instead of the Stokes component was used to eliminate contributions to spectra from cold atmospheric nitrogen. The system was evaluated in a methane/air flame and in a bench-top oven, and the technique was found to be a reliable tool for nonintrusive absolute temperature measurements with relatively clean gas streams. A water-cooled insertion probe was integrated with the Raman system for measurement of the temperature profiles inside an industrial furnace. Gas temperatures near 1500-1800 K at atmospheric pressure in an industrial furnace were inferred by fitting calculated profiles to experimental spectra with a standard deviation of less than 1% for averaging times of approximately 200 s. The temperatures inferred from Raman spectra are in good agreement with data recorded with a thermocouple probe.

  4. Excited-state wavepacket and potential reconstruction by coherent anti-Stokes Raman scattering.

    PubMed

    Avisar, David; Tannor, David J

    2015-01-28

    Among the major challenges in the chemical sciences is controlling chemical reactions and deciphering their mechanisms. Since much of chemistry occurs in excited electronic states, in the last three decades scientists have employed a wide variety of experimental techniques and theoretical methods to recover excited-state potential energy surfaces and the wavepackets that evolve on them. These methods have been partially successful but generally do not provide a complete reconstruction of either the excited state wavepacket or potential. We have recently proposed a methodology for reconstructing excited-state molecular wavepackets and the corresponding potential energy surface [Avisar and Tannor, Phys. Rev. Lett., 2011, 106, 170405]. In our approach, the wavepacket is represented as a superposition of the set of vibrational eigenfunctions of the molecular ground-state Hamiltonian. We assume that the multidimensional ground-state potential surface is known, and therefore these vibrational eigenfunctions are known as well. The time-dependent coefficients of the basis functions are obtained by experimental measurement of the resonant coherent anti-Stokes Raman scattering (CARS) signal. Our reconstruction strategy has several significant advantages: (1) the methodology requires no a priori knowledge of any excited-state potential. (2) It applies to dissociative as well as to bound excited-state potentials. (3) It is general for polyatomics. (4) The excited-state potential surface is reconstructed simultaneously with the wavepacket. Apart from making a general contribution to the field of excited-state spectroscopy, our method provides the information on the excited-state wavepacket and potential necessary to design laser pulse sequences to control photochemical reactions.

  5. Heterodyne coherent anti-Stokes Raman scattering by the phase control of its intrinsic background

    SciTech Connect

    Wang Xi; Wang Kai; Welch, George R.; Sokolov, Alexei V.

    2011-08-15

    We demonstrate the use of femtosecond laser pulse shaping for precise control of the interference between the coherent anti-Stokes Raman scattering (CARS) signal and the coherent nonresonant background generated within the same sample volume. Our technique is similar to heterodyne detection with the coherent background playing the role of the local oscillator field. In our experiment, we first apply two ultrashort (near-transform-limited) femtosecond pump and Stokes laser pulses to excite coherent molecular oscillations within a sample. After a short and controllable delay, we then apply a laser pulse that scatters off of these oscillations to produce the CARS signal. By making fine adjustments to the probe field spectral profile, we vary the relative phase between the Raman-resonant signal and the nonresonant background, and we observe a varying spectral interference pattern. These controlled variations of the measured pattern reveal the phase information within the Raman spectrum.

  6. Revealing silent vibration modes of nanomaterials by detecting anti-Stokes hyper-Raman scattering with femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Zeng, Jianhua; Chen, Lei; Dai, Qiaofeng; Lan, Sheng; Tie, Shaolong

    2016-01-01

    We proposed a scheme in which normal Raman scattering is coupled with hyper-Raman scattering for generating a strong anti-Stokes hyper-Raman scattering in nanomaterials by using femtosecond laser pulses. The proposal was experimentally demonstrated by using a single-layer MoS2 on a SiO2/Si substrate, a 17 nm-thick MoS2 on an Au/SiO2 substrate and a 9 nm-thick MoS2 on a SiO2-SnO2/Ag/SiO2 substrate which were confirmed to be highly efficient for second harmonic generation. A strong anti-Stokes hyper-Raman scattering was also observed in other nanomaterials possessing large second-order susceptibilities, such as silicon quantum dots self-assembled into ``coffee'' rings and tubular Cu-doped ZnO nanorods. In all the cases, many Raman inactive vibration modes were clearly revealed in the anti-Stokes hyper-Raman scattering. Apart from the strong anti-Stokes hyper-Raman scattering, Stokes hyper-Raman scattering with small Raman shifts was detected during the ablation process of thick MoS2 layers. It was also observed by slightly defocusing the excitation light. The detection of anti-Stokes hyper-Raman scattering may serve as a new technique for studying the Raman inactive vibration modes in nanomaterials.We proposed a scheme in which normal Raman scattering is coupled with hyper-Raman scattering for generating a strong anti-Stokes hyper-Raman scattering in nanomaterials by using femtosecond laser pulses. The proposal was experimentally demonstrated by using a single-layer MoS2 on a SiO2/Si substrate, a 17 nm-thick MoS2 on an Au/SiO2 substrate and a 9 nm-thick MoS2 on a SiO2-SnO2/Ag/SiO2 substrate which were confirmed to be highly efficient for second harmonic generation. A strong anti-Stokes hyper-Raman scattering was also observed in other nanomaterials possessing large second-order susceptibilities, such as silicon quantum dots self-assembled into ``coffee'' rings and tubular Cu-doped ZnO nanorods. In all the cases, many Raman inactive vibration modes were clearly

  7. Effects of tissue fixation on coherent anti-Stokes Raman scattering images of brain

    NASA Astrophysics Data System (ADS)

    Galli, Roberta; Uckermann, Ortrud; Koch, Edmund; Schackert, Gabriele; Kirsch, Matthias; Steiner, Gerald

    2014-07-01

    Coherent anti-Stokes Raman scattering (CARS) microscopy is an emerging multiphoton technique for the label-free histopathology of the central nervous system, by imaging the lipid content within the tissue. In order to apply the technique on standard histology sections, it is important to know the effects of tissue fixation on the CARS image. Here, we report the effects of two common fixation methods, namely with formalin and methanol-acetone, on mouse brain and human glioblastoma tissue. The variations induced by fixation on the CARS contrast and intensity were compared and interpreted using Raman microspectroscopy. The results show that, whenever unfixed cryosections cannot be used, fixation with formalin constitutes an alternative which does not deteriorate substantially the contrast generated by the different brain structures in the CARS image. Fixation with methanol-acetone strongly modifies the tissue lipid content and is therefore incompatible with the CARS imaging.

  8. Fiber optical parametric oscillator for coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Lamb, Erin S; Lefrancois, Simon; Ji, Minbiao; Wadsworth, William J; Xie, X Sunney; Wise, Frank W

    2013-10-15

    We present a synchronously pumped fiber optical parametric oscillator for coherent anti-Stokes Raman scattering microscopy. Pulses from a 1 μm Yb-doped fiber laser are amplified and frequency converted to 779-808 nm through normal dispersion four-wave mixing in a photonic crystal fiber. The idler frequency is resonant in the oscillator cavity, and we find that bandpass filtering the feedback is essential for stable, narrow-bandwidth output. Experimental results agree quite well with numerical simulations of the device. Transform-limited 2 ps pulses with energy up to 4 nJ can be generated at the signal wavelength. The average power is 180 mW, and the relative-intensity noise is much lower than that of a similar parametric amplifier. High-quality coherent Raman images of mouse tissues recorded with this source are presented.

  9. Glucose concentration measured by the hybrid coherent anti-Stokes Raman-scattering technique

    NASA Astrophysics Data System (ADS)

    Wang, Xi; Zhang, Aihua; Zhi, Miaochan; Sokolov, Alexei V.; Welch, George R.

    2010-01-01

    We investigate the possibility of using a hybrid coherent anti-Stokes Raman scattering technique for noninvasive monitoring of blood glucose levels. Our technique combines instantaneous coherent excitation of several characteristic molecular vibrations with subsequent probing of these vibrations by an optimally shaped, time-delayed, narrowband laser pulse. This pulse configuration mitigates the nonresonant four-wave mixing background while maximizing the Raman-resonant signal and allows rapid and highly specific detection even in the presence of multiple scattering. Under certain conditions we find that the measured signal is linearly proportional to the glucose concentration due to optical interference with the residual background light, which allows reliable detection of spectral signatures down to medically relevant glucose levels.

  10. Theory of femtosecond coherent anti-Stokes Raman backscattering enhanced by quantum coherence for standoff detection of bacterial spores

    NASA Astrophysics Data System (ADS)

    Ooi, C. H. Raymond; Beadie, Guy; Kattawar, George W.; Reintjes, John F.; Rostovtsev, Yuri; Zubairy, M. Suhail; Scully, Marlan O.

    2005-08-01

    Backscattered signal of coherent anti-Stokes Raman spectroscopy can be an extremely useful tool for remote identification of airborne particles, provided the signal is sufficiently large. We formulate a semiclassical theory of nonlinear scattering to estimate the number of detectable photons from a bacterial spore at a distance. For the first time, the theory incorporates enhanced quantum coherence via femtosecond pulses and a nonlinear process into the classical scattering problem. Our result shows a large backscattered signal in the far field, using typical parameters of an anthrax spore with maximally prepared vibrational coherence. Using train pulses of 1 kHz of repetition rate each with energy of 10 mJ, we estimate that about 107 photons can be detected by a 1 m diameter detector placed 1 km away from the spore in the backward scattering direction. The result shows the feasibility of developing a real time remote detection of hazardous microparticles in the atmosphere, particularly biopathogenic spores.

  11. Spectral features of anti-Stokes and Stokes modes generated by stimulated Raman scattering in liquid toluene

    NASA Astrophysics Data System (ADS)

    Yadav, Suchita; Kumar, Govind; Vijaya, R.

    2016-10-01

    Stimulated Raman scattering leading to the generation of four first-order Stokes modes at shifts of 862.9, 1035, 2967 and 3086 cm-1, one second-order Stokes mode at a shift of 2032.5 cm-1 and one first-order anti-Stokes mode at a shift of 946.3 cm-1 has been measured in an experiment using liquid toluene. The observed shifts are assigned to the earlier reported Raman shifts of toluene at 786, 1006, 2979, 3060 cm-1 due to ring-breathing mode, ring deformation mode, CH3 stretching mode and CH stretching mode, respectively. Simultaneous measurement of all the Raman modes, including the second-order Stokes and first-order anti-Stokes, and their correct assignment to the vibrational modes of toluene is not reported widely in earlier work. The Raman modes generated from toluene emerge as concentric rings of different diameters. The phase-matching angle for anti-Stokes generation is thus measured and compared with the expected value from calculation. The spectral broadening observed near two of the modes is explained with the help of Raman-active modes of toluene reported earlier by others. Raman shifts, threshold levels, gain and beam profile of all the modes, along with the phase matching of the anti-Stokes mode, are reported.

  12. Simultaneous observation of rotational coherent Stokes Raman scattering and coherent anti-Stokes Raman scattering in air and nitrogen

    NASA Technical Reports Server (NTRS)

    Snow, J. B.; Chang, R. K.; Zheng, J. B.; Leipertz, A.

    1983-01-01

    Rotational coherent Stokes Raman scattering (CSRS) and coherent anti-Stokes Raman scattering (CARS) in air and in nitrogen were observed simultaneously by using broadband generation and detection. In the broadband technique used, the entire CARS and CSRS spectrum was generated in a single laser pulse; the CSRS and CARS signals were dispersed by a spectrograph and detected simultaneously by an optical multichannel analyzer. A three-dimensional phase-matching geometry was used to achieve spatial resolution of the CSRS and CARS beams from the input beams. Under resonant conditions, similar experiments may provide a means of investigating the possible interaction between the CSRS and CARS processes in driving the rotational levels.

  13. Polarization properties, high-order Raman spectra, and frequency asymmetry between Stokes and anti-Stokes scattering of Raman modes in a graphite whisker

    NASA Astrophysics Data System (ADS)

    Tan, Pingheng; Hu, Chengyong; Dong, Jian; Shen, Wanci; Zhang, Baofa

    2001-12-01

    The Raman spectra of a new type of graphite whiskers have been measured in the range of 150-7800 cm-1. The intensity of the overtone (2D) located at ~2700 cm-1 is found to be about 10 times stronger than that of the C-C stretching mode (G) at 1582 cm-1. Because of the peculiar enhancement of the 2D mode, high-order Raman bands up to fifth order at ~7500 cm-1 have been observed. Polarized micro-Raman spectroscopy has been performed on an individual graphite whisker, and angular-dependent intensity measurements of all Raman modes in the VV and HV geometries are in agreement with the theoretical calculated results. Laser-energy-dependent dispersion effects and the frequency discrepancy of Raman modes between their Stokes and anti-Stokes lines in graphite whiskers are also carefully investigated. The energy dispersion of the D mode and G mode is very similar to that of highly oriented pyrolytic graphite (HOPG). In contrast to the Raman spectra of HOPG and other graphite materials, two laser-energy-dependent Raman lines are revealed in the low-frequency region of the Raman spectra of graphite whiskers, which are believed to be the resonantly enhanced phonons in the transverse-acoustic and longitudinal-acoustic phonon branches. Moreover, the obvious energy dispersion of the D' mode at ~1620 cm-1 is observed in graphite whiskers. The results clearly reveal how strongly the peak parameters of Raman modes of graphite materials are dependent on their structural geometry. The Stokes and anti-Stokes scattering experiments show that the frequency discrepancy between the Stokes and anti-Stokes sides of a Raman mode in graphite materials is equal to the frequency value covered by the one-phonon energy of this Raman mode in its frequency versus laser energy curve, which is the product of the one-phonon energy of this mode (Eωs) and the value of its laser-energy dispersions (∂Eωs/∂ɛL).

  14. Delivery of picosecond lasers in multimode fibers for coherent anti-Stokes Raman scattering imaging.

    PubMed

    Wang, Zhiyong; Yang, Yaliang; Luo, Pengfei; Gao, Liang; Wong, Kelvin K; Wong, Stephen T C

    2010-06-07

    We investigated the possibility of using standard commercial multimode fibers (MMF), Corning SMF28 fibers, to deliver picosecond excitation lasers for coherent anti-Stokes Raman scattering (CARS) imaging. We theoretically and/or experimentally analyzed issues associated with the fiber delivery, such as dispersion length, walk-off length, nonlinear length, average threshold power for self-phase modulations, and four-wave mixing (FWM). These analyses can also be applied to other types of fibers. We found that FWM signals are generated in MMF, but they can be filtered out using a long-pass filter for CARS imaging. Finally, we demonstrated that MMF can be used for delivery of picosecond excitation lasers in the CARS imaging system without any degradation of image quality.

  15. Coherent anti-Stokes Raman scattering for label-free biomedical imaging

    NASA Astrophysics Data System (ADS)

    Patel, Imran I.; Steuwe, Christian; Reichelt, Stefanie; Mahajan, Sumeet

    2013-09-01

    Coherent anti-Stokes Raman scattering (CARS) has established itself as an imaging technique capable of providing video-rate imaging of biological specimens through vibrational coherence of endogenous molecules. Current techniques predominantly involve the application of costly, invasive and potentially non-specific dyes or labels for imaging biomolecules. CARS microscopy can however provide a high-resolution and non-invasive alternative for imaging biomolecules of interest without the need for exogenous labels. Here we provide an overview of CARS including the technique and common instrumentation as well as its applications in biomedical imaging. We discuss the major biomedical areas where CARS has been applied such as in evaluating liver disease, progression of atherosclerosis, tumour classification and tracking drug delivery, whilst also assessing the future challenges for clinical translation.

  16. Shaping femtosecond coherent anti-Stokes Raman spectra using optimal control theory.

    PubMed

    Pezeshki, Soroosh; Schreiber, Michael; Kleinekathöfer, Ulrich

    2008-04-21

    Optimal control theory is used to tailor laser pulses which enhance a femtosecond time-resolved coherent anti-Stokes Raman scattering (fs-CARS) spectrum in a certain frequency range. For this aim the optimal control theory has to be applied to a target state distributed in time. Explicit control mechanisms are given for shaping either the Stokes or the probe pulse in the four-wave mixing process. A simple molecule for which highly accurate potential energy surfaces are available, namely molecular iodine, is used to test the procedure. This approach of controlling vibrational motion and delivering higher intensities to certain frequency ranges might also be important for the improvement of CARS microscopy.

  17. Automated identification of subcellular organelles by coherent anti-stokes Raman scattering.

    PubMed

    El-Mashtoly, Samir F; Niedieker, Daniel; Petersen, Dennis; Krauss, Sascha D; Freier, Erik; Maghnouj, Abdelouahid; Mosig, Axel; Hahn, Stephan; Kötting, Carsten; Gerwert, Klaus

    2014-05-06

    Coherent anti-Stokes Raman scattering (CARS) is an emerging tool for label-free characterization of living cells. Here, unsupervised multivariate analysis of CARS datasets was used to visualize the subcellular compartments. In addition, a supervised learning algorithm based on the "random forest" ensemble learning method as a classifier, was trained with CARS spectra using immunofluorescence images as a reference. The supervised classifier was then used, to our knowledge for the first time, to automatically identify lipid droplets, nucleus, nucleoli, and endoplasmic reticulum in datasets that are not used for training. These four subcellular components were simultaneously and label-free monitored instead of using several fluorescent labels. These results open new avenues for label-free time-resolved investigation of subcellular components in different cells, especially cancer cells.

  18. Chirped Probe Pulse Femtosecond Coherent Anti-Stokes Raman Scattering for Turbulent Combustion Diagnostics

    NASA Astrophysics Data System (ADS)

    Fineman, Claresta N.; Lucht, Robert P.

    2014-06-01

    Chirped probe pulse (CPP) femtosecond (fs) coherent anti-Stokes Raman scattering (CARS) thermometry at 5 kHz has been successfully applied for single-laser-shot flame temperature measurements in a mildly turbulent hydrogen-air jet diffusion flame, sooting methane-air jet diffusion flame, and most recently a turbulent combustor of practical interest. Measurements were performed at various heights and radial locations within each flame and resulted in temperatures ranging from 300 K to 2400 K. In the turbulent combustor every laser shot produced some resonant CARS signal; no loss of signal due to beam steering, pressure fluctuations, or shear layer density gradients was noticeable. Furthermore, the measurement volume spatial resolution is better than has previously been reported for other CARS experiments. Flame temperature measurements compare well with those previously reported in similar flames. These results indicate high repetition rate CPP fs-CARS is an excellent technique for the study of turbulent combustion.

  19. Investigation of microstructured chitosans by coherent anti-Stokes Raman microscopy.

    PubMed

    Dementjev, A; Mordas, G; Ulevičius, V; Gulbinas, V

    2015-03-01

    This work describes application of coherent anti-Stokes Raman scattering (CARS) microscopy technique for analytical characterization of microstructured materials based on chitosan. We demonstrate that nitrogen-hydrogen vibration band in the high wavenumber region of CARS spectrum prevails over response from oxygen-hydrogen vibrations and can be used as a spectral marker of chitosan. The chemically selective imaging is experimentally demonstrated by applying CARS microscopy to discriminate between chitosan and polystyrene microparticles. CARS microscopy was shown to be a valuable tool for characterization of polluted chitosan fibre from utilized engine filter material. A possibility to observe foreign material pieces on the surface of the polluted chitosan fibre is demonstrated and discussed.

  20. Visualizing resonances in the complex plane with vibrational phase contrast coherent anti-Stokes Raman scattering.

    PubMed

    Jurna, Martin; Garbacik, Erik T; Korterik, Jeroen P; Herek, Jennifer L; Otto, Cees; Offerhaus, Herman L

    2010-09-15

    In coherent anti-Stokes Raman scattering (CARS), the emitted signal carries both amplitude and phase information of the molecules in the focal volume. Most CARS experiments ignore the phase component, but its detection allows for two advantages over intensity-only CARS. First, the pure resonant response can be determined, and the nonresonant background rejected, by extracting the imaginary component of the complex response, enhancing the sensitivity of CARS measurements. Second, selectivity is increased via determination of the phase and amplitude, allowing separation of individual molecular components of a sample even when their vibrational bands overlap. Here, using vibrational phase contrast CARS (VPC-CARS), we demonstrate enhanced sensitivity in quantitative measurements of ethanol/methanol mixtures and increased selectivity in a heterogeneous mixture of plastics and water. This powerful technique opens a wide range of possibilities for studies of complicated systems where overlapping resonances limit standard methodologies.

  1. High-resolution extreme-ultraviolet spectroscopy of potassium using anti-Stokes radiation

    NASA Technical Reports Server (NTRS)

    Rothenberg, J. E.; Young, J. F.; Harris, S. E.

    1981-01-01

    The use of a new extreme-ultraviolet radiation source based on spontaneous anti-Stokes scattering for high-resolution absorption spectroscopy of transition originating from the 3p6 shell of potassium is reported. The region from 546.6 to 536.8 A is scanned at a resolution of about 1.2 Kayser. Within this region, four previously unreported lines are observed.

  2. Ex-CARS: exotic configuration for coherent anti-Stokes Raman scattering microspectroscopy utilizing two laser sources

    PubMed Central

    Yakovlev, Vladislav V.; Petrov, Georgi I.; Noojin, Gary D.; Harbert, Corey; Denton, Michael; Thomas, Robert

    2011-01-01

    We propose and experimentally demonstrate a new coherent anti-Stokes Raman scattering setting, which relies on a coherent excitation of Raman vibration using a broadband ultrashort laser pulse and signal read-out using a conventional continuous wave laser radiation. Such an exotic arrangement does not require any synchronization of two laser sources and can be used for direct comparison of amplitudes of nonlinear and spontaneous Raman signals. Ex-CARS in time- (top panel) and frequency- (bottom panel) domain. PMID:20635427

  3. Diffraction barrier breakthrough in coherent anti-Stokes Raman scattering microscopy by additional probe-beam-induced phonon depletion

    SciTech Connect

    Liu Wei; Niu Hanben

    2011-02-15

    We provide an approach to significantly break the diffraction limit in coherent anti-Stokes Raman scattering (CARS) microscopy via an additional probe-beam-induced photon depletion (APIPD). The additional probe beam, whose profile is doughnut shaped and whose wavelength is different from the Gaussian probe beam, depletes the phonons to yield an unwanted anti-Stokes signal within a certain bandwidth at the rim of the diffraction-limited spot. When the Gaussian probe beam that follows immediately arrives, no anti-Stokes signal is generated in this region, resembling stimulated emission depletion (STED) microscopy, and the spot-generating useful anti-Stokes signals by this beam are substantially suppressed to a much smaller dimension. Scanning the spot renders three-dimensional, label-free, and chemically selective CARS images with subdiffraction resolution. Also, resolution-enhanced images of the molecule, specified by its broadband even-total CARS spectral signals not only by one anti-Stokes signal for its special chemical bond, can be obtained by employing a supercontinuum source.

  4. Fast spectral coherent anti-Stokes Raman scattering microscopy with high-speed tunable picosecond laser.

    PubMed

    Cahyadi, Harsono; Iwatsuka, Junichi; Minamikawa, Takeo; Niioka, Hirohiko; Araki, Tsutomu; Hashimoto, Mamoru

    2013-09-01

    We develop a coherent anti-Stokes Raman scattering (CARS) microscopy system equipped with a tunable picosecond laser for high-speed wavelength scanning. An acousto-optic tunable filter (AOTF) is integrated in the laser cavity to enable wavelength scanning by varying the radio frequency waves applied to the AOTF crystal. An end mirror attached on a piezoelectric actuator and a pair of parallel plates driven by galvanometer motors are also introduced into the cavity to compensate for changes in the cavity length during wavelength scanning to allow synchronization with another picosecond laser. We demonstrate fast spectral imaging of 3T3-L1 adipocytes every 5  cm-1 in the Raman spectral region around 2850  cm-1 with an image acquisition time of 120 ms. We also demonstrate fast switching of Raman shifts between 2100 and 2850  cm-1, corresponding to CD2 symmetric stretching and CH2 symmetric stretching vibrations, respectively. The fast-switching CARS images reveal different locations of recrystallized deuterated and nondeuterated stearic acid.

  5. Coherent anti-Stokes Raman scattering enhancement of thymine adsorbed on graphene oxide

    PubMed Central

    2014-01-01

    Coherent anti-Stokes Raman scattering (CARS) of carbon nanostructures, namely, highly oriented pyrolytic graphite, graphene nanoplatelets, graphene oxide, and multiwall carbon nanotubes as well CARS spectra of thymine (Thy) molecules adsorbed on graphene oxide were studied. The spectra of the samples were compared with spontaneous Raman scattering (RS) spectra. The CARS spectra of Thy adsorbed on graphene oxide are characterized by shifts of the main bands in comparison with RS. The CARS spectra of the initial nanocarbons are definitely different: for all investigated materials, there is a redistribution of D- and G-mode intensities, significant shift of their frequencies (more than 20 cm-1), and appearance of new modes about 1,400 and 1,500 cm-1. The D band in CARS spectra is less changed than the G band; there is an absence of 2D-mode at 2,600 cm-1 for graphene and appearance of intensive modes of the second order between 2,400 and 3,000 cm-1. Multiphonon processes in graphene under many photon excitations seem to be responsible for the features of the CARS spectra. We found an enhancement of the CARS signal from thymine adsorbed on graphene oxide with maximum enhancement factor about 105. The probable mechanism of CARS enhancement is discussed. PMID:24948887

  6. Quantitative chemical imaging and unsupervised analysis using hyperspectral coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Masia, Francesco; Glen, Adam; Stephens, Phil; Borri, Paola; Langbein, Wolfgang

    2013-11-19

    In this work, we report a method to acquire and analyze hyperspectral coherent anti-Stokes Raman scattering (CARS) microscopy images of organic materials and biological samples resulting in an unbiased quantitative chemical analysis. The method employs singular value decomposition on the square root of the CARS intensity, providing an automatic determination of the components above noise, which are retained. Complex CARS susceptibility spectra, which are linear in the chemical composition, are retrieved from the CARS intensity spectra using the causality of the susceptibility by two methods, and their performance is evaluated by comparison with Raman spectra. We use non-negative matrix factorization applied to the imaginary part and the nonresonant real part of the susceptibility with an additional concentration constraint to obtain absolute susceptibility spectra of independently varying chemical components and their absolute concentration. We demonstrate the ability of the method to provide quantitative chemical analysis on known lipid mixtures. We then show the relevance of the method by imaging lipid-rich stem-cell-derived mouse adipocytes as well as differentiated embryonic stem cells with a low density of lipids. We retrieve and visualize the most significant chemical components with spectra given by water, lipid, and proteins segmenting the image into the cell surrounding, lipid droplets, cytosol, and the nucleus, and we reveal the chemical structure of the cells, with details visualized by the projection of the chemical contrast into a few relevant channels.

  7. Nanosecond coherent anti-Stokes Raman scattering for particle size characterization

    NASA Astrophysics Data System (ADS)

    El Bassri, Farid; Lefort, Claire; Capitaine, Erwan; Louot, Christophe; Pagnoux, Dominique; Couderc, Vincent; Leproux, Philippe

    2016-03-01

    Particle size analyzers based on laser scattering commonly make use of light diffraction and scattering around the particle considered in its medium. For particle size below 50 μm, Fraunhofer theory must be abandoned in favor of Mie model, which requires to know the complex refractive index of both the particle and the medium. In this paper, we demonstrate that particle size characterization can be realized by measuring the macroscopic Raman spectral response of the whole set of particles excited by a laser beam. We use a home-made setup based on coherent anti-Stokes Raman scattering (CARS) and having a 0.36 cm-1 spectral resolution, in which the laser source is a dual-output infrared nanosecond supercontinuum source (1064 nm monochromatic pump wave, 1100-1640 nm broadband Stokes wave). The samples are latex beads in water with different diameters (20 nm, 50 nm, 100 nm, 5 μm). The C-H stretching line around 3050 cm-1 is studied. For this vibration, we study the variation of both the CARS central frequency and linewidth as a function of the particles size. A quasi linear increase of the linewidth with the inverse of the diameter is measured. A difference of 15 cm-1 is obtained between beads with diameters of 5 μm and 20 nm respectively. The physical phenomena at the origin of this difference are discussed, especially considering the contributions of the center and of the boundaries of the object to the global Raman response.

  8. Dual-Pump Coherent Anti-Stokes Raman Scattering Temperature and CO2 Concentration Measurements

    NASA Technical Reports Server (NTRS)

    Lucht, Robert P.; Velur-Natarajan, Viswanathan; Carter, Campbell D.; Grinstead, Keith D., Jr.; Gord, James R.; Danehy, Paul M.; Fiechtner, G. J.; Farrow, Roger L.

    2003-01-01

    Measurements of temperature and CO2 concentration using dual-pump coherent anti-Stokes Raman scattering, (CARS) are described. The measurements were performed in laboratory flames,in a room-temperature gas cell, and on an engine test stand at the U.S. Air Force Research Laboratory, Wright-Patterson Air Force Base. A modeless dye laser, a single-mode Nd:YAG laser, and an unintensified back-illuminated charge-coupled device digital camera were used for these measurements. The CARS measurements were performed on a single-laser-shot basis. The standard deviations of the temperatures and CO2 mole fractions determined from single-shot dual-pump CARS spectra in steady laminar propane/air flames were approximately 2 and 10% of the mean values of approximately 2000 K and 0.10, respectively. The precision and accuracy of single-shot temperature measurements obtained from the nitrogen part of the dual-pump CARS system were investigated in detail in near-adiabatic hydrogen/air/CO2 flames. The precision of the CARS temperature measurements was found to be comparable to the best results reported in the literature for conventional two-laser, single-pump CARS. The application of dual-pump CARS for single-shot measurements in a swirl-stabilized combustor fueled with JP-8 was also demonstrated.

  9. Label-free imaging of human breast tissues using coherent anti-Stokes Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Yang, Yaliang; Gao, Liang; Wang, Zhiyong; Thrall, Michael J.; Luo, Pengfei; Wong, Kelvin K.; Wong, Stephen T.

    2011-03-01

    Breast cancer is a common disease in women. Current imaging and diagnostic methods for breast cancer confront several limitations, like time-consuming, invasive and with a high cost. Alternative strategies are in high demand to alleviate patients' trauma and lower medical expenses. Coherent anti-Stokes Raman scattering (CARS) imaging technique offers many advantages, including label-free, sub-wavelength spatial resolution and video-rate imaging speed. Therefore, it has been demonstrated as a powerful tool for various biomedical applications. In this study, we present a label-free fast imaging method to identify breast cancer and its subtypes using CARS microscopy. Human breast tissues, including normal, benign and invasive carcinomas, were imaged ex vivo using a custom-built CARS microscope. Compared with results from corresponding hematoxylin and eosin (H&E) stains, the CARS technique has demonstrated its capability in identifying morphological features in a similar way as in H&E stain. These features can be used to distinguish breast cancer from normal and benign tissues, and further separate cancer subtypes from each other. Our pilot study suggests that CARS microscopy could be used as a routine examination tool to characterize breast cancer ex vivo. Moreover, its label-free and fast imaging properties render this technique as a promising approach for in vivo and real-time imaging and diagnosis of breast cancer.

  10. Investigation of lipid homeostasis in living Drosophila by coherent anti-Stokes Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Chien, Cheng-Hao; Chen, Wei-Wen; Wu, June-Tai; Chang, Ta-Chau

    2012-12-01

    To improve our understanding of lipid metabolism, Drosophila is used as a model animal, and its lipid homeostasis is monitored by coherent anti-Stokes Raman scattering microscopy. We are able to achieve in vivo imaging of larval fat body (analogous to adipose tissue in mammals) and oenocytes (analogous to hepatocytes) in Drosophila larvae at subcellular level without any labeling. By overexpressing two lipid regulatory proteins-Brummer lipase (Bmm) and lipid storage droplet-2 (Lsd-2)-we found different phenotypes and responses under fed and starved conditions. Comparing with the control larva, we observed more lipid droplet accumulation by ˜twofold in oenocytes of fat-body-Bmm-overexpressing (FB-Bmm-overexpressing) mutant under fed condition, and less lipid by ˜fourfold in oenocytes of fat-body-Lsd-2-overexpressing (FB-Lsd-2-overexpressing) mutant under starved condition. Moreover, together with reduced size of lipid droplets, the lipid content in the fat body of FB-Bmm-overexpressing mutant decreases much faster than that of the control and FB-Lsd-2-overexpressing mutant during starvation. From long-term starvation assay, we found FB-Bmm-overexpressing mutant has a shorter lifespan, which can be attributed to faster consumption of lipid in its fat body. Our results demonstrate in vivo observations of direct influences of Bmm and Lsd-2 on lipid homeostasis in Drosophila larvae.

  11. Coherent anti-Stokes Raman scattering microscopy of human smooth muscle cells in bioengineered tissue scaffolds

    NASA Astrophysics Data System (ADS)

    Brackmann, Christian; Esguerra, Maricris; Olausson, Daniel; Delbro, Dick; Krettek, Alexandra; Gatenholm, Paul; Enejder, Annika

    2011-02-01

    The integration of living, human smooth muscle cells in biosynthesized cellulose scaffolds was monitored by nonlinear microscopy toward contractile artificial blood vessels. Combined coherent anti-Stokes Raman scattering (CARS) and second harmonic generation (SHG) microscopy was applied for studies of the cell interaction with the biopolymer network. CARS microscopy probing CH2-groups at 2845 cm-1 permitted three-dimensional imaging of the cells with high contrast for lipid-rich intracellular structures. SHG microscopy visualized the fibers of the cellulose scaffold, together with a small signal obtained from the cytoplasmic myosin of the muscle cells. From the overlay images we conclude a close interaction between cells and cellulose fibers. We followed the cell migration into the three-dimensional structure, illustrating that while the cells submerge into the scaffold they extrude filopodia on top of the surface. A comparison between compact and porous scaffolds reveals a migration depth of <10 μm for the former, whereas the porous type shows cells further submerged into the cellulose. Thus, the scaffold architecture determines the degree of cell integration. We conclude that the unique ability of nonlinear microscopy to visualize the three-dimensional composition of living, soft matter makes it an ideal instrument within tissue engineering.

  12. Multiplex coherent anti-Stokes Raman scattering microspectroscopy for monitoring molecular structural change in biological samples

    NASA Astrophysics Data System (ADS)

    Ohta, Takayuki; Hashizume, Hiroshi; Takeda, Keigo; Ishikawa, Kenji; Ito, Masafumi; Hori, Masaru

    2014-10-01

    Biological applications employing non-equilibrium plasma processing has been attracted much attention. It is essential to monitor the changes in an intracellular structure of the cell during the plasma exposure. In this study, we have analyzed the molecular structure of biological samples using multiplex coherent anti-Stokes Raman scattering (CARS) microspectroscopy. Two picosecond pulse lasers with fundamental (1064 nm) or the supercontinuum (460-2200 nm) were employed as a pump and Stokes beams of multiplex CARS microspectroscopy, respectively. The pump and the Stokes laser beams were collinearly overlapped and tightly focused into a sample using an objective lens of high numerical aperture. The CARS signal was collected by another microscope objective lens which is placed facing the first one. After passing through a short pass filter, the signal was dispersed by a polychromator, and was detected by a charge-coupled device camera. The sample was sandwiched by a coverslip and a glass bottom dish for the measurements and was placed on a piezo stage. The CARS signals of the quinhydrone crystal at 1655, 1584, 1237 and 1161 cm-1 were assigned to the C-C, C =O stretching, O-H and C-O stretching vibrational modes, respectively.

  13. Coherent anti-Stokes Raman scattering hyperspectral imaging of cartilage aiming for state discrimination of cell

    NASA Astrophysics Data System (ADS)

    Shiozawa, Manabu; Shirai, Masataka; Izumisawa, Junko; Tanabe, Maiko; Watanabe, Koich

    2016-07-01

    Noninvasive cell analyses are increasingly important in the medical field. A coherent anti-Stokes Raman scattering (CARS) microscope is the noninvasive imaging equipment and enables to obtain images indicating molecular distribution. However, due to low-signal intensity, it is still challenging to obtain images of the fingerprint region, in which many spectrum peaks correspond to compositions of a cell. Here, to identify cell differentiation by using multiplex CARS, we investigated hyperspectral imaging of the fingerprint region of living cells. To perform multiplex CARS, we used a prototype of a compact light source generating both pump light and broadband Stokes light. Assuming application to regenerative medicine, we chose a cartilage cell, whose differentiation is difficult to be identified by change of the cell morphology. Because one of the major components of cartilage is collagen, we focused on distribution of proline, which accounts for approximately 20% of collagen. The spectrum quality was improved by optical adjustments of the power branching ratio and divergence of Stokes light. Periphery of a cartilage cell was highlighted in a CARS image of proline, and this result suggests correspondence with collagen generated as an extracellular matrix. The possibility of noninvasive analyses by using CARS hyperspectral imaging was indicated.

  14. Coherent Anti-Stokes Raman Scattering (CARS) Microscopy: A Novel Technique for Imaging the Retina

    PubMed Central

    Masihzadeh, Omid; Ammar, David A.; Kahook, Malik Y.; Lei, Tim C.

    2013-01-01

    Purpose. To image the cellular and noncellular structures of the retina in an intact mouse eye without the application of exogenous fluorescent labels using noninvasive, nondestructive techniques. Methods. Freshly enucleated mouse eyes were imaged using two nonlinear optical techniques: coherent anti-Stokes Raman scattering (CARS) and two-photon autofluorescence (TPAF). Cross sectional transverse sections and sequential flat (en face) sagittal sections were collected from a region of sclera approximately midway between the limbus and optic nerve. Imaging proceeded from the surface of the sclera to a depth of ∼60 μm. Results. The fluorescent signal from collagen fibers within the sclera was evident in the TPAF channel; the scleral collagen fibers showed no organization and appeared randomly packed. The sclera contained regions lacking TPAF and CARS fluorescence of ∼3 to 15 μm in diameter that could represent small vessels or scleral fibroblasts. Intense punctate CARS signals from the retinal pigment epithelial layer were of a size and shape of retinyl storage esters. Rod outer segments could be identified by the CARS signal from their lipid-rich plasma membranes. Conclusions. CARS microscopy can be used to image the outer regions of the mammalian retina without the use of a fluorescent dye or exogenously expressed recombinant protein. With technical advancements, CARS/TPAF may represent a new avenue for noninvasively imaging the retina and might complement modalities currently used in clinical practice. PMID:23580484

  15. Coherent anti-Stokes Raman scattering microscopy driving the future of loaded mesoporous silica imaging.

    PubMed

    Fussell, Andrew L; Mah, Pei Ting; Offerhaus, Herman; Niemi, Sanna-Mari; Salonen, Jarno; Santos, Hélder A; Strachan, Clare

    2014-11-01

    This study reports the use of variants of coherent anti-Stokes Raman scattering (CARS) microscopy as a novel method for improved physicochemical characterization of drug-loaded silica particles. Ordered mesoporous silica is a biomaterial that can be loaded to carry a number of biochemicals, including poorly water-soluble drugs, by allowing the incorporation of drug into nanometer-sized pores. In this work, the loading of two poorly water-soluble model drugs, itraconazole and griseofulvin, in MCM-41 silica microparticles is characterized qualitatively, using the novel approach of CARS microscopy, which has advantages over other analytical approaches used to date and is non-destructive, rapid, label free, confocal and has chemical and physical specificity. The study investigated the effect of two solvent-based loading methods, namely immersion and rotary evaporation, and microparticle size on the three-dimensional (3-D) distribution of the two loaded drugs. Additionally, hyperspectral CARS microscopy was used to confirm the amorphous nature of the loaded drugs. Z-stacked CARS microscopy suggested that the drug, but not the loading method or particle size range, affected 3-D drug distribution. Hyperspectral CARS confirmed that the drug loaded in the MCM-41 silica microparticles was in an amorphous form. The results show that CARS microscopy and hyperspectral CARS microscopy can be used to provide further insights into the structural nature of loaded mesoporous silica microparticles as biomaterials.

  16. Clinical coherent anti-Stokes Raman scattering and multiphoton tomography of human skin with a femtosecond laser and photonic crystal fiber

    NASA Astrophysics Data System (ADS)

    Breunig, Hans Georg; Weinigel, Martin; Bückle, Rainer; Kellner-Höfer, Marcel; Lademann, Jürgen; Darvin, Maxim E.; Sterry, Wolfram; König, Karsten

    2013-02-01

    We report on in vivo coherent anti-Stokes Raman scattering spectroscopy (CARS), two-photon fluorescence and second-harmonic-generation imaging on human skin with a novel multimodal clinical CARS/multiphoton tomograph. CARS imaging is realized by a combination of femtosecond pulses with broadband continuum pulses generated by a photonic crystal fiber. The images reveal the microscopic distribution of (i) non-fluorescent lipids, (ii) endogenous fluorophores and (iii) the collagen network inside the human skin in vivo with subcellular resolution. Examples of healthy as well as cancer-affected skin are presented.

  17. Ab initio study of coherent anti-Stokes Raman scattering (CARS) of the 1,3,5-trinitro-1,3,5-triazacyclohexane (RDX) explosive

    NASA Astrophysics Data System (ADS)

    Mohammed, Abdelsalam; Ågren, Hans; Thorvaldsen, Andreas J.; Ruud, Kenneth

    2010-01-01

    Coherent anti-Stokes Raman scattering (CARS) of the 1,3,5-trinitro-1,3,5-triazacyclohexane (RDX) C 3H 6N 6O 6 molecule is studied by ab initio methods. The results are compared to available experimental observations and against calculations and experimental observations of the conventional non-resonant Raman spectrum for RDX. It is found that all intense bands in the observed CARS spectrum and all Raman differential cross sections are well reproduced by the calculations. The features of the resonant CARS signal vary strongly from the corresponding Raman signal, and are obtained with a considerably larger cross section, a fact that could further facilitate the use of CARS spectroscopy in applications of stand-off detection of gaseous samples at ultra-low concentrations.

  18. Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering for gas-phase temperature measurements

    NASA Astrophysics Data System (ADS)

    Miller, Joseph Daniel

    Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) is employed for quantitative gas-phase temperature measurements in combustion processes and heated flows. In this approach, ultrafast 100-fs laser pulses are used to induce vibrational and rotational transitions in N2 and O2, while a third spectrally narrowed picosecond pulse is used to probe the molecular response. Temporal suppression of the nonresonant contribution and elimination of collisional effects are achieved by delay of the probe pulse, while sufficient spectral resolution is maintained for frequency-domain detection and thermometry. A theoretical framework is developed to model experimental spectra by phenomenologically describing the temporal evolution of the vibrational and rotational wavepackets as a function of temperature and pressure. Interference-free, single-shot vibrational fs/ps CARS thermometry is demonstrated at 1-kHz from 1400-2400 K in a H2-air flame, with accuracy better than 3%. A time-asymmetric exponential pulse shape is introduced to optimize nonresonant suppression with a 103 reduction at a probe delay of 0.31 ps. Low-temperature single-shot thermometry (300-700 K) with better than 1.5% accuracy is demonstrated using a fully degenerate rotational fs/ps CARS scheme, and the influence of collision energy transfer on thermometry error is quantified at atmospheric pressure. Interference-free thermometry, without nonresonant contributions and collision-induced error, is demonstrated for the first time using rotational fs/ps CARS at room temperature and pressures from 1-15 atm. Finally, the temporal and spectral resolution of fs/ps CARS is exploited for transition-resolved time-domain measurements of N2 and O2 self-broadened S-branch Raman linewidths at pressures of 1-20 atm.

  19. Coherent Anti-Stokes Raman Scattering (CARS) as a Probe for Supersonic Hydrogen-Fuel/Air Mixing

    NASA Technical Reports Server (NTRS)

    Danehy, P. M.; O'Byrne, S.; Cutler, A. D.; Rodriguez, C. G.

    2003-01-01

    The dual-pump coherent anti-Stokes Raman spectroscopy (CARS) method was used to measure temperature and the absolute mole fractions of N2, O2 and H2 in a supersonic non-reacting fuel-air mixing experiment. Experiments were conducted in NASA Langley Research Center s Direct Connect Supersonic Combustion Test Facility. Under normal operation of this facility, hydrogen and air burn to increase the enthalpy of the test gas and O2 is added to simulate air. This gas is expanded through a Mach 2 nozzle and into a combustor model where fuel is then injected, mixes and burns. In the present experiment the O2 of the test gas is replaced by N2. The lack of oxidizer inhibited combustion of the injected H2 fuel jet allowing the fuel/air mixing process to be studied. CARS measurements were performed 427 mm downstream of the nozzle exit and 260 mm downstream of the fuel injector. Maps were obtained of the mean temperature, as well as the N2, O2 and H2 mean mole fraction fields. A map of mean H2O vapor mole fraction was also inferred from these measurements. Correlations between different measured parameters and their fluctuations are presented. The CARS measurements are compared with a preliminary computational prediction of the flow.

  20. Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Evans, Conor L.; Potma, Eric O.; Puoris'haag, Mehron; Côté, Daniel; Lin, Charles P.; Xie, X. Sunney

    2005-11-01

    Imaging living organisms with molecular selectivity typically requires the introduction of specific labels. Many applications in biology and medicine, however, would significantly benefit from a noninvasive imaging technique that circumvents such exogenous probes. In vivo microscopy based on vibrational spectroscopic contrast offers a unique approach for visualizing tissue architecture with molecular specificity. We have developed a sensitive technique for vibrational imaging of tissues by combining coherent anti-Stokes Raman scattering (CARS) with video-rate microscopy. Backscattering of the intense forward-propagating CARS radiation in tissue gives rise to a strong epi-CARS signal that makes in vivo imaging possible. This substantially large signal allows for real-time monitoring of dynamic processes, such as the diffusion of chemical compounds, in tissues. By tuning into the CH2 stretching vibrational band, we demonstrate CARS imaging and spectroscopy of lipid-rich tissue structures in the skin of a live mouse, including sebaceous glands, corneocytes, and adipocytes, with unprecedented contrast at subcellular resolution. nonlinear microscopy | vibrational imaging | back scattering

  1. Selective probing of vibrational hot states in bromine using time-resolved coherent anti-Stokes Raman scattering.

    PubMed

    Namboodiri, Mahesh; Liebers, Jörg; Kleinekathöfer, Ulrich; Materny, Arnulf

    2012-11-26

    In previous work (Scaria, A.; et al. Chem. Phys. Lett. 2009, 470, 39-43) it was shown that the excitation of the electronic B state in bromine can be characterized by transitions starting from vibrational hot states of the electronic ground X state. This contribution is strongly depending on the specific Franck-Condon factors for the chosen wavelength (in that work 540 nm) used for excitation. For the investigation of the resulting excited state dynamics, a pump-degenerate four-wave mixing (pump-DFWM) experiment was applied. To increase the vibrational selectivity, in the present work we have performed temperature-dependent time-resolved coherent anti-Stokes Raman scattering (CARS) spectroscopy to probe the B state dynamics of bromine. Also here, the wavelength of the excitation (in this case, the pump laser of the CARS process) was set to 540 nm for all measurements. The hot state contribution is small, even at high temperatures. It can be probed by tuning the Stokes wavelength to resonance. The time delay between the probe pulse and the time-coincident pump/Stokes pulse pair of the CARS process is scanned, giving access to the wave packet dynamics in the excited B state. The experimental observations are supported by quantum dynamical calculations.

  2. Hybrid single-source online Fourier transform coherent anti-Stokes Raman scattering/optical coherence tomography.

    PubMed

    Kamali, Tschackad; Považay, Boris; Kumar, Sunil; Silberberg, Yaron; Hermann, Boris; Werkmeister, René; Drexler, Wolfgang; Unterhuber, Angelika

    2014-10-01

    We demonstrate a multimodal optical coherence tomography (OCT) and online Fourier transform coherent anti-Stokes Raman scattering (FTCARS) platform using a single sub-12 femtosecond (fs) Ti:sapphire laser enabling simultaneous extraction of structural and chemical ("morphomolecular") information of biological samples. Spectral domain OCT prescreens the specimen providing a fast ultrahigh (4×12  μm axial and transverse) resolution wide field morphologic overview. Additional complementary intrinsic molecular information is obtained by zooming into regions of interest for fast label-free chemical mapping with online FTCARS spectroscopy. Background-free CARS is based on a Michelson interferometer in combination with a highly linear piezo stage, which allows for quick point-to-point extraction of CARS spectra in the fingerprint region in less than 125 ms with a resolution better than 4  cm(-1) without the need for averaging. OCT morphology and CARS spectral maps indicating phosphate and carbonate bond vibrations from human bone samples are extracted to demonstrate the performance of this hybrid imaging platform.

  3. Diagnosing lung cancer using coherent anti-Stokes Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Gao, Liang; Yang, Yaliang; Xing, Jiong; Thrall, Michael J.; Wang, Zhiyong; Li, Fuhai; Luo, Pengfei; Wong, Kelvin K.; Zhao, Hong; Wong, Stephen T. C.

    2011-03-01

    Lung carcinoma is the most prevalent type of cancer in the world, and it is responsible for more deaths than other types of cancer. During diagnosis, a pathologist primarily aims to differentiate small cell carcinoma from non-small cell carcinoma on biopsy and cytology specimens, which is time consuming due to the time required for tissue processing and staining. To speed up the diagnostic process, we investigated the feasibility of using coherent anti-Stokes Raman scattering (CARS) microscopy as a label-free strategy to image lung lesions and differentiate subtypes of lung cancers. Different mouse lung cancer models were developed by injecting human lung cancer cell lines, including adenocarcinoma, squamous cell carcinoma, and small cell carcinoma, into lungs of the nude mice. CARS images were acquired from normal lung tissues and different subtypes of cancer lesions ex vivo using intrinsic contrasts from symmetric CH2 bonds. These images showed good correlation with the hematoxylin and eosin (H&E) stained sections from the same tissue samples with regard to cell size, density, and cell-cell distance. These features are routinely used in diagnosing lung lesions. Our results showed that the CARS technique is capable of providing a visualizable platform to differentiate different kinds of lung cancers using the same pathological features without histological staining and thus has the potential to serve as a more efficient examination tool for diagnostic pathology. In addition, incorporating with suitable fiber-optic probes would render the CARS technique as a promising approach for in vivo diagnosis of lung cancer.

  4. Imaging of Lipids in Microalgae with Coherent Anti-Stokes Raman Scattering Microscopy1[OPEN

    PubMed Central

    Cavonius, Lillie; Fink, Helen; Kiskis, Juris; Albers, Eva; Undeland, Ingrid; Enejder, Annika

    2015-01-01

    Microalgae have great prospects as a sustainable resource of lipids for refinement into nutraceuticals and biodiesel, which increases the need for detailed insights into their intracellular lipid synthesis/storage mechanisms. As an alternative strategy to solvent- and label-based lipid quantification techniques, we introduce time-gated coherent anti-Stokes Raman scattering (CARS) microscopy for monitoring lipid contents in living algae, despite strong autofluorescence from the chloroplasts, at approximately picogram and subcellular levels by probing inherent molecular vibrations. Intracellular lipid droplet synthesis was followed in Phaeodactylum tricornutum algae grown under (1) light/nutrient-replete (control [Ctrl]), (2) light-limited (LL), and (3) nitrogen-starved (NS) conditions. Good correlation (r2 = 0.924) was found between lipid volume data yielded by CARS microscopy and total fatty acid content obtained from gas chromatography-mass spectrometry analysis. In Ctrl and LL cells, micron-sized lipid droplets were found to increase in number throughout the growth phases, particularly in the stationary phase. During more excessive lipid accumulation, as observed in NS cells, promising commercial harvest as biofuels and nutritional lipids, several micron-sized droplets were present already initially during cultivation, which then fused into a single giant droplet toward stationary phase alongside with new droplets emerging. CARS microspectroscopy further indicated lower lipid fluidity in NS cells than in Ctrl and LL cells, potentially due to higher fatty acid saturation. This agreed with the fatty acid profiles gathered by gas chromatography-mass spectrometry. CARS microscopy could thus provide quantitative and semiqualitative data at the single-cell level along with important insights into lipid-accumulating mechanisms, here revealing two different modes for normal and excessive lipid accumulation. PMID:25583924

  5. Standoff and arms-length detection of chemicals with single-beam coherent anti-Stokes Raman scattering.

    PubMed

    Li, Haowen; Harris, D Ahmasi; Xu, Bingwei; Wrzesinski, Paul J; Lozovoy, Vadim V; Dantus, Marcos

    2009-02-01

    The detection of chemicals from safe distances is vital in environments with potentially hazardous or explosive threats, where high sensitivity and fast detection speed are needed. Here we demonstrate standoff detection of several solids, liquids, and gases with single-beam coherent anti-Stokes Raman scattering. This approach utilizes a phase coherent ultrabroad-bandwidth femtosecond laser to probe the fundamental vibrations that constitute a molecule's fingerprint. Characteristic Raman lines for several chemicals are successfully obtained from arms-length and 12 m standoff distances. The sensitivity and speed of this approach are also demonstrated.

  6. Vibrationally resonant imaging of a single living cell by supercontinuum-based multiplex coherent anti-Stokes Raman scattering microspectroscopy

    NASA Astrophysics Data System (ADS)

    Kano, Hideaki; Hamaguchi, Hiro-O.

    2005-02-01

    Supercontinuum-based multiplex coherent anti-Stokes Raman scattering (CARS) microspectroscopy has been applied to vibrational imaging of a living fission yeast cell. We have successfully extracted only a vibrationally resonant CARS image from a characteristic spectral profile in the C-H stretching vibrational region. Using our simple but sensitive analysis, the vibrational contrast is significantly improved in comparison with a CARS imaging at a fixed Raman shift. The CARS image of a living yeast cell indicates several areas at which the signal is remarkably strong. They are considered to arise from mitochondria.

  7. Raman and coherent anti-Stokes Raman scattering microscopy studies of changes in lipid content and composition in hormone-treated breast and prostate cancer cells

    PubMed Central

    Potcoava, Mariana C.; Futia, Gregory L.; Aughenbaugh, Jessica; Schlaepfer, Isabel R.; Gibson, Emily A.

    2014-01-01

    Abstract. Increasing interest in the role of lipids in cancer cell proliferation and resistance to drug therapies has motivated the need to develop better tools for cellular lipid analysis. Quantification of lipids in cells is typically done by destructive chromatography protocols that do not provide spatial information on lipid distribution and prevent dynamic live cell studies. Methods that allow the analysis of lipid content in live cells are therefore of great importance. Using micro-Raman spectroscopy and coherent anti-Stokes Raman scattering (CARS) microscopy, we generated a lipid profile for breast (T47D, MDA-MB-231) and prostate (LNCaP, PC3) cancer cells upon exposure to medroxyprogesterone acetate (MPA) and synthetic androgen R1881. Combining Raman spectra with CARS imaging, we can study the process of hormone-mediated lipogenesis. Our results show that hormone-treated cancer cells T47D and LNCaP have an increased number and size of intracellular lipid droplets and higher degree of saturation than untreated cells. MDA-MB-231 and PC3 cancer cells showed no significant changes upon treatment. Principal component analysis with linear discriminant analysis of the Raman spectra was able to differentiate between cancer cells that were treated with MPA, R1881, and untreated. PMID:24933682

  8. Bandwidth optimization of femtosecond pure-rotational coherent anti-Stokes Raman scattering by pump/Stokes spectral focusing.

    DOE PAGES

    Kearney, Sean Patrick

    2014-07-01

    A simple spectral focusing scheme for bandwidth optimization of gas-phase rotational coherent anti-Stokes Raman scattering (CARS) spectra is presented. The method is useful when femtosecond pump/Stokes preparation of the Raman coherence is utilized. The approach is of practical utility when working with laser pulses that are not strictly transform limited, or when windows or other sources of pulse chirp may be present in the experiment. A delay between the femtosecond preparation pulses is introduced to shift the maximum Raman preparation away from zero frequency and toward the Stokes or anti-Stokes side of the spectrum with no loss in total preparationmore » bandwidth. Shifts of 100 cm-1 or more are attainable and allow for enhanced detection of high-energy (150-300 cm-1) rotational Raman transitions at near transform-limited optimum sensitivity. A simple theoretical treatment for the case of identical pump and Stokes pulses with linear frequency chirp is presented. The approach is then demonstrated experimentally for typical levels of transform-limited laser performance obtained our laboratory with nonresonant CARS in argon and Raman-resonant spectra from a lean H2/air flat flame.« less

  9. Bandwidth optimization of femtosecond pure-rotational coherent anti-Stokes Raman scattering by pump/Stokes spectral focusing.

    SciTech Connect

    Kearney, Sean Patrick

    2014-07-01

    A simple spectral focusing scheme for bandwidth optimization of gas-phase rotational coherent anti-Stokes Raman scattering (CARS) spectra is presented. The method is useful when femtosecond pump/Stokes preparation of the Raman coherence is utilized. The approach is of practical utility when working with laser pulses that are not strictly transform limited, or when windows or other sources of pulse chirp may be present in the experiment. A delay between the femtosecond preparation pulses is introduced to shift the maximum Raman preparation away from zero frequency and toward the Stokes or anti-Stokes side of the spectrum with no loss in total preparation bandwidth. Shifts of 100 cm-1 or more are attainable and allow for enhanced detection of high-energy (150-300 cm-1) rotational Raman transitions at near transform-limited optimum sensitivity. A simple theoretical treatment for the case of identical pump and Stokes pulses with linear frequency chirp is presented. The approach is then demonstrated experimentally for typical levels of transform-limited laser performance obtained our laboratory with nonresonant CARS in argon and Raman-resonant spectra from a lean H2/air flat flame.

  10. Bandwidth optimization of femtosecond pure-rotational coherent anti-Stokes Raman scattering by pump/Stokes spectral focusing.

    PubMed

    Kearney, Sean P

    2014-10-01

    A simple spectral focusing scheme for bandwidth optimization of gas-phase rotational coherent anti-Stokes Raman scattering (CARS) spectra is presented. The method is useful when femtosecond pump/Stokes preparation of the Raman coherence is utilized. The approach is of practical utility when working with laser pulses that are not strictly transform limited or when windows or other sources of pulse chirp may be present in the experiment. A delay between the femtosecond preparation pulses is introduced to shift the maximum Raman preparation away from zero frequency and toward the Stokes or anti-Stokes side of the spectrum with no loss in total preparation bandwidth. Shifts of 100 cm(-1) or more are attainable and allow for enhanced detection of high-energy (150-300 cm(-1)) rotational Raman transitions at near-transform-limited optimum sensitivity. A simple theoretical treatment for the case of identical pump and Stokes pulses with linear frequency chirp is presented. The approach is then demonstrated experimentally for typical levels of transform-limited laser performance obtained in our laboratory with nonresonant CARS in argon and Raman-resonant spectra from a lean H2 air flat flame.

  11. Dynamical rate theory of enzymatic reactions and triple-resonant coherent anti-Stokes Raman scattering microspectroscopy

    NASA Astrophysics Data System (ADS)

    Min, Wei

    Chapters 2-7 focus on physical enzymology. Despite its long history, recent single-molecule spectroscopy, among many others techniques, has generated new quantitative data that reveal unobserved features of protein dynamics and enzyme catalysis at unprecedented levels. Much of these are beyond the classic framework of transition state theory and Michalis-Menten (MM) enzyme kinetics. Due to the complexity of the problem, theoretical developments in this area have much lagged behind experiments. After an initial experimental characterization on single-molecule protein conformational fluctuations, we then develop a dynamical rate theory for enzyme catalyzed chemical reactions, from a statistical mechanics approach. Towards this goal, we formulate a two-dimensional (2D) multi-surface free energy description of the entire catalytic process that explicitly combines the concept of "fluctuating enzymes" with the MM enzyme kinetics. The outcome of this framework has two folds. On the rate theory side, going much beyond transition state theory, it connects conformational fluctuations to catalysis, allows for the interplay between energetics (e.g. Haldane's stain energy) and dynamics (e.g. Koshland's induced fit), and predicts the time dependence of single-enzyme catalysis. On the enzyme kinetics side, it gives mechanistic and unified understanding of MM and non-MM (both positive and negative cooperativity) kinetics of monomeric enzymes, in term of non-equilibrium steady state cycle on the 2D free energy surface. Chapters 8-11 present the principle and application of a new ultra-sensitive nonlinear optical microspectroscopy, femtosecond (fs) triple-resonant coherent anti-Stokes Raman scattering (CARS), in which the amplitude and phase of input fs laser pulses are optimally shaped to be in triple resonant with the molecular electronic and vibrational transitions to generate a coherent nonlinear signal beam at a new color with a highest possible efficiency. This technique

  12. Radially polarized tip-enhanced near-field coherent anti-Stokes Raman scattering microscopy for bioimaging

    NASA Astrophysics Data System (ADS)

    Lin, Jian; Er, Kenneth; Huang, Zhiwei

    2012-03-01

    CARS is meritorious in its ability to perform chemical selective imaging, but its spatial resolution is limited by the diffraction limit of light; however, this limit can be broken by combining CARS and near-field scanning microscope. In this work, we report a novel radially polarized near-field coherent anti-Stokes Raman scattering microscopy (RP-NF-CARS), which uses radially polarized light as excitation to enhance the electric field enhancement under a metallic tip, and improves the signal to background ratio compared with that using linearly polarized excitations. We applied RP-NF-CARS to image nano-scale polystyrene beads and biological system.

  13. Supercontinuum-based three-color three-pulse time-resolved coherent anti-Stokes Raman scattering.

    PubMed

    Zeytunyan, Aram; Crampton, Kevin T; Zadoyan, Ruben; Apkarian, Vartkess A

    2015-09-07

    We demonstrate the use of a photonic crystal fiber (PCF) as a compact three-color fs laser system operating at 76 MHz, limited only by the repetition rate of the pump laser. The system is suitable for background-free time-resolved four-wave mixing measurements, which arguably reach fundamental limits in signal detectivity. We give a detailed characterization of the near transform-limited multi-color pulses that are extracted from the PCF, and prove the system through time-resolved coherent anti-Stokes Raman scattering measurements in bipyridyl ethylene and styrene.

  14. Super-Spatial- and -Spectral-Resolution in Vibrational Imaging via Saturated Coherent Anti-Stokes Raman Scattering

    NASA Astrophysics Data System (ADS)

    Yonemaru, Yasuo; Palonpon, Almar F.; Kawano, Shogo; Smith, Nicholas I.; Kawata, Satoshi; Fujita, Katsumasa

    2015-07-01

    We demonstrate a vibrational microscopy technique with subdiffraction spatial resolution by the use of saturation of coherent anti-Stokes Raman scattering (CARS). The saturated CARS signals effectively produce a reduced point-spread function at harmonic frequencies, which is extracted by temporal modulation of the pump beam and demodulation of the CARS signal. An increase in spectral resolution and suppression of the nonresonant background signal accompany the spatial- resolution enhancement. Our simple, enhanced CARS technique promises to be useful in studying molecules in gas and liquid phases as well as soft condensed-matter systems.

  15. Gas-phase thermometry using delayed-probe-pulse picosecond coherent anti-Stokes Raman scattering spectra of H2.

    PubMed

    Stauffer, Hans U; Kulatilaka, Waruna D; Hsu, Paul S; Gord, James R; Roy, Sukesh

    2011-02-01

    We report the development and application of a simple theoretical model for extracting temperatures from picosecond-laser-based coherent anti-Stokes Raman scattering (CARS) spectra of H2 obtained using time-delayed probe pulses. This approach addresses the challenges associated with the effects of rotational-level-dependent decay lifetimes on time-delayed probing for CARS thermometry. A simple procedure is presented for accurate temperature determination based on a Boltzmann distribution using delayed-probe-pulse vibrational CARS spectra of H2; this procedure requires measurement at only a select handful of probe-pulse delays and requires no assumptions about sample environment.

  16. Coherent anti-Stokes Raman scattering imaging with a laser source delivered by a photonic crystal fiber.

    PubMed

    Wang, Haifeng; Huff, Terry B; Cheng, Ji-Xin

    2006-05-15

    We demonstrate laser-scanning coherent anti-Stokes Raman scattering (CARS) imaging with two excitation laser beams delivered by a large-mode-area photonic crystal fiber. The group-velocity dispersion and self-phase modulation effects are largely suppressed due to the large mode area of the fiber and the use of picosecond pulses. The fiber delivery preserves the signal level and image spatial resolution well. High-quality images of live spinal cord tissues are acquired using the fiber-delivered laser source. Our method provides a basic platform for developing a flexible and compact CARS imaging system.

  17. Comparative Study of Breast Normal and Cancer Cells Using Coherent Anti-Stokes Raman Scattering Microspectroscopy Imaging

    NASA Astrophysics Data System (ADS)

    Lee, Jang Hyuk; Cho, Eun Hee; Shin, Sang-Mo; Oh, Myoung-kyu; Ko, Do-Kyeong

    2012-08-01

    A coherent anti-Stokes Raman scattering (CARS) microspectroscopy imaging system was developed using a femtosecond laser and a photonic crystal fiber (PCF). We separated resonant and non-resonant CARS signals in the time domain by the chirp of the PCF, and applied this system to compare live human breast normal and cancer cells. The CARS image and spectrum at C-H stretch vibration in lipid droplets could subsequently be used to differentiate cancer cells from normal cells, thereby confirming the potential of the CARS microspectroscopy imaging system as a diagnostic tool that allows the high-sensitivity, high-resolution, and fast detection of breast cancer.

  18. Dual-pump vibrational/rotational femtosecond/picosecond coherent anti-Stokes Raman scattering temperature and species measurements.

    PubMed

    Dedic, Chloe E; Miller, Joseph D; Meyer, Terrence R

    2014-12-01

    A method for simultaneous ro-vibrational and pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) is presented for multi-species detection and improved temperature sensitivity from room temperature to flame conditions. N₂/CH₄ vibrational and N₂/O₂/H₂ rotational Raman coherences are excited simultaneously using fs pump pulses at 660 and 798 nm, respectively, and a common fs Stokes pulse at 798 nm. A fourth narrowband 798 nm ps pulse probes all coherence states at a time delay that minimizes nonresonant background and the effects of collisions. The transition strength is concentration dependent, while the distribution among observed transitions is related to temperature through the Boltzmann distribution. The broadband excitation pulses and multiplexed signal are demonstrated for accurate thermometry from 298 to 2400 K and concentration measurements of four key combustion species.

  19. Radially polarized tip-enhanced near-field coherent anti-Stokes Raman scattering microscopy for vibrational nano-imaging

    NASA Astrophysics Data System (ADS)

    Lin, Jian; Zi Jian Er, Kenneth; Zheng, Wei; Huang, Zhiwei

    2013-08-01

    We report a radially polarized tip-enhanced near-field coherent anti-Stokes Raman scattering (RP-TE-CARS) microscopy technique for high-contrast vibrational imaging of subcellular organelles at nano-scale resolutions. The radially polarized pump and Stokes laser beams are tightly focused onto the sample while a gold-coated metallic probe is placed at the upper surface of the sample to enhance the electric field and CARS signals. The back-scattered CARS signal is measured with the gold-coated nano-tip being stationary at the focal region of laser beams. The RP-TE-CARS signal is ˜6-fold higher than that using linearly polarized laser excitation. We demonstrate the good performance of the RP-TE-CARS technique developed by imaging sub-micron polystyrene beads and mitochondria at nano-scale resolutions.

  20. Spectrally-broad coherent anti-Stokes Raman scattering hyper-microscopy utilizing a Stokes supercontinuum pumped at 800 nm.

    PubMed

    Porquez, Jeremy G; Cole, Ryan A; Tabarangao, Joel T; Slepkov, Aaron D

    2016-10-01

    We demonstrate spectral-focusing based coherent anti-Stokes Raman scattering (SF-CARS) hyper-microscopy capable of probing vibrational frequencies from 630 cm(-1) to 3250 cm(-1) using a single Ti:Sapphire femtosecond laser operating at 800 nm, and a commercially-available supercontinuum-generating fibre module. A broad Stokes supercontinuum with significant spectral power at wavelengths between 800 nm and 940 nm is generated by power tuning the fibre module using atypically long and/or chirped ~200 fs pump pulses, allowing convenient access to lower vibrational frequencies in the fingerprint spectral region. This work significantly reduces the instrumental and technical requirements for multimodal CARS microscopy, while expanding the spectral capabilities of an established approach to SF-CARS.

  1. Spectrally-broad coherent anti-Stokes Raman scattering hyper-microscopy utilizing a Stokes supercontinuum pumped at 800 nm

    PubMed Central

    Porquez, Jeremy G.; Cole, Ryan A.; Tabarangao, Joel T.; Slepkov, Aaron D.

    2016-01-01

    We demonstrate spectral-focusing based coherent anti-Stokes Raman scattering (SF-CARS) hyper-microscopy capable of probing vibrational frequencies from 630 cm−1 to 3250 cm−1 using a single Ti:Sapphire femtosecond laser operating at 800 nm, and a commercially-available supercontinuum-generating fibre module. A broad Stokes supercontinuum with significant spectral power at wavelengths between 800 nm and 940 nm is generated by power tuning the fibre module using atypically long and/or chirped ~200 fs pump pulses, allowing convenient access to lower vibrational frequencies in the fingerprint spectral region. This work significantly reduces the instrumental and technical requirements for multimodal CARS microscopy, while expanding the spectral capabilities of an established approach to SF-CARS. PMID:27867735

  2. Effects of quenching on electronic-resonance-enhanced coherent anti-Stokes Raman scattering of nitric oxide

    NASA Astrophysics Data System (ADS)

    Roy, Sukesh; Kulatilaka, Waruna D.; Naik, Sameer V.; Laurendeau, Normand M.; Lucht, Robert P.; Gord, James R.

    2006-09-01

    We investigate the effects of gas-mixture composition on the electronic-resonance-enhanced coherent anti-Stokes Raman scattering (ERE-CARS) signals of nitric oxide (NO). From previous laser-induced fluorescence (LIF) studies, quenching rates are known to change drastically, by factors of 400-800, in mixtures of CO2/O2/N2. The observed ERE-CARS signal remains constant to within 30% whereas LIF signals from NO are predicted to decrease by more than two orders of magnitudes in the same environments. This is very significant for using NO ERE-CARS in high-pressure combustion environments where the electronic quenching rate can vary rapidly as a function of both space and time.

  3. Increasing the imaging depth of coherent anti-Stokes Raman scattering microscopy with a miniature microscope objective

    NASA Astrophysics Data System (ADS)

    Wang, Haifeng; Huff, Terry B.; Fu, Yan; Jia, Kevin Y.; Cheng, Ji-Xin

    2007-08-01

    A miniature objective lens with a tip diameter of 1.3 mm was used for extending the penetration depth of coherent anti-Stokes Raman scattering (CARS) microscopy. Its axial and lateral focal widths were determined to be 11.4 and 0.86 μm, respectively, by two-photon excitation fluorescence imaging of 200 nm beads at a 735 nm excitation wavelength. By inserting the lens tip into a soft gel sample, CARS images of 2 μm polystyrene beads 5 mm deep from the surface were acquired. The miniature objective was applied to CARS imaging of rat spinal cord white matter with a minimal requirement for surgery.

  4. In vivo histology: optical biopsies with chemical contrast using clinical multiphoton/coherent anti-Stokes Raman scattering tomography

    NASA Astrophysics Data System (ADS)

    Weinigel, M.; Breunig, H. G.; Kellner-Höfer, M.; Bückle, R.; Darvin, M. E.; Klemp, M.; Lademann, J.; König, K.

    2014-05-01

    The majority of existing coherent anti-Stokes Raman scattering (CARS) imaging systems are still huge and complicated laboratory systems and neither compact nor user-friendly nor mobile medically certified CARS systems. We have developed a new flexible multiphoton/CARS tomograph for imaging in a clinical environment. The system offers exceptional 360° flexibility with a very stable setup and enables label free ‘in vivo histology’ with chemical contrast within seconds. It can be completely operated by briefly trained non-laser experts. The imaging capability and flexibility of the novel in vivo tomograph are shown on optical biopsies with subcellular resolution and chemical contrast of patients suffering from psoriasis and squamous cell carcinoma.

  5. Multi-focus excitation coherent anti-Stokes Raman scattering (CARS) microscopy and its applications for real-time imaging.

    PubMed

    Minamikawa, Takeo; Hashimoto, Mamoru; Fujita, Katsumasa; Kawata, Satoshi; Araki, Tsutomu

    2009-06-08

    We developed a multi-focus excitation coherent anti-Stokes Raman scattering (CARS) microscope using a microlens array scanner for real-time molecular imaging. Parallel exposure of a specimen with light from two highly controlled picosecond mode-locked lasers (jitter of 30 fs through an electronic low-pass filter with 150 Hz bandwidth, point-by-point wavelength scan within 300 ms) and parallel detection with an image sensor enabled real-time imaging. We demonstrated real-time CARS imaging of polystyrene beads (frame rate of 30 fps), a giant multi-lamellar vesicle of dipalmitoylphosphatidylcholine (frame rate of 10 fps), and living HeLa cells (frame rate of 10 fps).

  6. Nonlinear optical interference of two successive coherent anti-Stokes Raman scattering signals for biological imaging applications.

    PubMed

    Lee, Eun Seong; Lee, Jae Yong; Yoo, Yong Shim

    2007-01-01

    The nonlinear optical interference of two successively generated coherent anti-Stokes Raman scattering (CARS) signals from two different samples placed in series is demonstrated for the imaging performance, in which a collinear phase matching geometry is used. The relative phase of two CARS signals is controlled by a phase-shifting unit made of dispersive glass materials of which the thickness can be precisely varied. The clear interference fringes are observed as the thickness of the phase-shifting unit changes. The interference effect is then utilized to achieve a better quality CARS image of a biological tissue taken from a mouse skin. Placing the tissue in the second sample position and performing raster scans of the laser beams on it, we can acquire a CARS image of higher contrast compared to the normal image obtained without interferometric implementation.

  7. Fiber-based optical parametric oscillator for high resolution coherent anti-Stokes Raman scattering (CARS) microscopy.

    PubMed

    Gottschall, Thomas; Meyer, Tobias; Baumgartl, Martin; Dietzek, Benjamin; Popp, Jürgen; Limpert, Jens; Tünnermann, Andreas

    2014-09-08

    Imaging based on coherent anti-Stokes Raman scattering (CARS) relies on the interaction of high peak-power, synchronized picosecond pulses with narrow bandwidths and a well-defined frequency difference. Recently a new type of fiber-based CARS laser source based on four-wave-mixing (FWM) has been developed. In order to enhance its spectral resolution and efficiency, a FWM based fiber optical parametric oscillator (FOPO) is proposed in this work. The source delivers 180 mW with 5.6 kW peak power for the CARS pump and 130 mW with 2.9 kW peak power for the Stokes signal. CARS resonances around 2850 and 2930 cm(-1) can be resolved with a resolution of 1 cm(-1) enabling high-contrast, spectrally resolved CARS imaging of biological tissue.

  8. Imaging receptor-mediated endocytosis with a polymeric nanoparticle-based coherent anti-stokes Raman scattering probe.

    PubMed

    Tong, Ling; Lu, Yanhui; Lee, Robert J; Cheng, Ji-Xin

    2007-08-23

    Coherent anti-Stokes Raman scattering (CARS) microscopy was used to visualize receptor-mediated endocytosis and intracellular trafficking with the aid of a CARS probe. The probe was made of 200-nm polystyrene particles encapsulated in folate-targeted liposomes. By tuning (omega(p) - omega(s)) to 3045 cm(-1), which corresponds to the aromatic C-H stretching vibration, the polystyrene nanoparticles with a high density of aromatic C-H bonds were detected with a high signal-to-noise ratio, while the epi-detected CARS signal from cellular organelles was cancelled by the destructive interference between the resonant contribution from the aliphatic C-H vibration and the nonresonant contribution. Without any photobleaching, the CARS probe allowed single-particle tracking analysis of intracellular endosome transport. No photodamage to cells was observed under the current experimental conditions. These results show the advantages and potential of using a CARS probe to study cellular processes.

  9. Longitudinal in vivo coherent anti-Stokes Raman scattering imaging of demyelination and remyelination in injured spinal cord

    NASA Astrophysics Data System (ADS)

    Shi, Yunzhou; Zhang, Delong; Huff, Terry B.; Wang, Xiaofei; Shi, Riyi; Xu, Xiao-Ming; Cheng, Ji-Xin

    2011-10-01

    In vivo imaging of white matter is important for the mechanistic understanding of demyelination and evaluation of remyelination therapies. Although white matter can be visualized by a strong coherent anti-Stokes Raman scattering (CARS) signal from axonal myelin, in vivo repetitive CARS imaging of the spinal cord remains a challenge due to complexities induced by the laminectomy surgery. We present a careful experimental design that enabled longitudinal CARS imaging of de- and remyelination at single axon level in live rats. In vivo CARS imaging of secretory phospholipase A2 induced myelin vesiculation, macrophage uptake of myelin debris, and spontaneous remyelination by Schwann cells are sequentially monitored over a 3 week period. Longitudinal visualization of de- and remyelination at a single axon level provides a novel platform for rational design of therapies aimed at promoting myelin plasticity and repair.

  10. Label-free imaging of lipid dynamics using Coherent Anti-stokes Raman Scattering (CARS) and Stimulated Raman Scattering (SRS) microscopy

    PubMed Central

    Folick, Andrew; Min, Wei; Wang, Meng C.

    2011-01-01

    The recently developed Coherent Anti-stokes Raman Scattering (CARS) microscopy and Stimulated Raman Scattering (SRS) microscopy have provided new methods to visualize the localization and regulation of biological molecules without the use of invasive and potentially perturbative labels. They allow rapid imaging of specific molecules with high resolution and sensitivity. These tools have been effectively applied to the study of lipid metabolism using Caenorhabditis elegans as a genetic model, unraveling new lipid storage phenotypes and their regulatory mechanisms. Here we review the underlying principle of CARS and SRS microscopy, as well as their recent applications in lipid biology research in C. elegans. PMID:21945002

  11. Multiparameter label-free flow cytometry using multiplex coherent anti-Stokes Raman scattering (MCARS) with biological applications

    NASA Astrophysics Data System (ADS)

    Camp, Charles H., Jr.; Yegnanarayanan, Siva; Eftekhar, Ali A.; Adibi, Ali

    2011-03-01

    Flow cytometry is an invaluable analytical tool that provides statistical information about sample populations. By optically probing samples at high-speed, flow cytometers retrieve information about basic morphology and composition. The optical elastic scatter is indicative of sample size and granularity while molecular information requires the addition of fluorescent labels, which have limitations such as spectral overlap, non-specific binding, and cellular toxicity. In this work, we present the first multiparameter label-free flow cytometer that observes the elastically forward-scattered light (FSC) and probes the intrinsic Raman vibrations of passing samples using multiplex coherent anti-Stokes Raman scattering (MCARS). MCARS, as a broadband technique, probes a large region of the Raman spectrum; thus, leading to rich molecularly-sensitive information. Additionally, we present the first experimental investigations of two biological systems using the multiparameter flow cytometer: Saccharomyces cerevisiae, a yeast often used as a model system for eukaryotic organisms, and Phaeodactylum tricornutum, a diatom under investigation for biofuel production.

  12. Method and system to measure temperature of gases using coherent anti-stokes doppler spectroscopy

    DOEpatents

    Rhodes, Mark

    2013-12-17

    A method of measuring a temperature of a noble gas in a chamber includes providing the noble gas in the chamber. The noble gas is characterized by a pressure and a temperature. The method also includes directing a first laser beam into the chamber and directing a second laser beam into the chamber. The first laser beam is characterized by a first frequency and the second laser beam is characterized by a second frequency. The method further includes converting at least a portion of the first laser beam and the second laser beam into a coherent anti-Stokes beam, measuring a Doppler broadening of the coherent anti-Stokes beam, and computing the temperature using the Doppler broadening.

  13. Picosecond coherent anti-Stokes Raman scattering (CARS) study of vibrational dephasing of carbon disulfide and benzene in solution

    NASA Technical Reports Server (NTRS)

    Perry, Joseph W.; Woodward, Anne M.; Stephenson, John C.

    1986-01-01

    The vibrational dephasing of the 656/cm mode (nu1, a1g) of CS2 and the 991/cm mode (nu2, a1g) of benzene have been studied as a function of concentration in mixtures with a number of solvents using a ps time-resolved CARS technique. This technique employs two tunable synchronously-pumped mode-locked dye lasers in a stimulated Raman pump, coherent anti-Stokes Raman probe time-resolved experiment. Results are obtained for CS2 in carbon tetrachloride, benzene, nitrobenzene, and ethanol and for benzene nu2 in CS2. The dephasing rates of CS2 nu1 increase on dilution with the polar solvents and decrease or remain constant on dilution with the nonpolar solvents. The CS2/benzene solutions show a contrasting behavior, with the CS2 nu1 dephasing rate being nearly independent of concentration whereas the benzene nu2 dephasing rate decreases on dilution. These results are compared to theoretical models for vibrational dephasing of polyatomic molecules in solution.

  14. Molecular orientation in dry and hydrated cellulose fibers: a coherent anti-Stokes Raman scattering microscopy study.

    PubMed

    Zimmerley, Maxwell; Younger, Rebecca; Valenton, Tiffany; Oertel, David C; Ward, Jimmie L; Potma, Eric O

    2010-08-12

    Coherent anti-Stokes Raman scattering (CARS) microscopy is combined with spontaneous Raman scattering microspectroscopy and second harmonic generation (SHG) microscopy to interrogate the molecular alignment in dry and hydrated cellulose fibers. Two types of cellulose were investigated: natural cellulose I in cotton fibers and regenerated cellulose II in rayon fibers. On the basis of the orientation of the methylene symmetric stretching vibration, the molecular alignment of cellulose microfibrils is found to be conserved on the micrometer scale. Whereas the molecular orientation in cotton shows modest variability along the fiber, the alignment of the cellulose units in rayon is highly consistent throughout the fiber. The ordered alignment is retained upon fiber hydration. Upon hydration of the cellulose fibers, an anisotropic electronic contribution is observed, which indicates an ordered incorporation of water molecules into the fiber structure. The third-order and second-order electronic polarizability of cellulose I are directed along the axis of the polyglucan chain. No second-order optical response is observed in cellulose II, supporting the antiparallel arrangement of the polyglucan chains in regenerated cellulose.

  15. Red-shifted solitons for coherent anti-Stokes Raman scattering microspectroscopy in a polarization-maintaining photonic crystal fiber

    NASA Astrophysics Data System (ADS)

    Yuan, Jinhui; Sang, Xinzhu; Wu, Qiang; Zhou, Guiyao; Li, Feng; Yu, Chongxiu; Wang, Kuiru; Yan, Binbin; Han, Ying; Tam, Hwa Yaw; Wai, Ping-kong Alexander

    2015-05-01

    An alternative light source for coherent anti-Stokes Raman scattering (CARS) microspectroscopy based on red-shifted solitons in a polarization-maintaining photonic crystal fiber (PM-PCF) is experimentally demonstrated. By coupling femtosecond pulses into the anomalous dispersion region of the fundamental mode of a PM-PCF along the slow and fast axes, the red-shifted solitons generated can be used as the Stokes beams when the pump pulses are chosen as the pump beams. Through the process of red-shift, the frequency differences of the pump-Stokes beams are tunable in the ranges of 0 to 4068 cm-1 and 0 to 4594 cm-1, respectively. Moreover, because of the well maintained polarization states of the pump and Stokes beams and the high output powers of the solitons, CARS microspectroscopy using the proposed source will have a high signal-to-noise ratio and short data acquisition time. CARS microspectroscopy based on the proposed all-fiber light source can be used for studying a wide range of vibrational Raman spectra.

  16. Hyperspectral coherent anti-Stokes Raman scattering microscopy for in situ analysis of solid-state crystal polymorphs

    NASA Astrophysics Data System (ADS)

    Garbacik, E. T.; Fussell, A. L.; Güres, S.; Korterik, J. P.; Otto, C.; Herek, J. L.; Offerhaus, H. L.

    2013-02-01

    Hyperspectral coherent anti-Stokes Raman scattering (CARS) microscopy is quickly becoming a prominent imaging modality because of its many advantages over the traditional paradigm of multispectral CARS. In particular, recording a significant portion of the vibrational spectrum at each spatial pixel allows image-wide spectral analysis at much higher rates than can be achieved with spontaneous Raman. We recently developed a hyperspectral CARS method, the driving principle behind which is the fast acquisition and display of a hyperspectral datacube as a set of intuitive images wherein each material in a sample appears with a unique trio of colors. Here we use this system to image and analyze two types of polymorphic samples: the pseudopolymorphic hydration of theophylline, and the packing polymorphs of the sugar alcohol mannitol. In addition to these solid-state form modifications we have observed spectral variations of crystalline mannitol and diprophylline as functions of their orientations relative to the optical fields. We use that information to visualize the distributions of these compounds in a pharmaceutical solid oral dosage form.

  17. Femtosecond pure-rotational coherent anti-stokes raman scattering gas phase diagnostics.

    SciTech Connect

    Kearney, Sean Patrick; Serrano, Justin Raymond

    2010-12-01

    We discuss recent experiments for the characterization of our femtosecond pure rotational CARS facility for observation of Raman transients in N{sub 2} and atmospheric air. The construction of a simplified femtosecond four-wave mixing system with only a single laser source is presented. Pure-rotational Raman transients reveal well-ordered time-domain recurrence peaks associated with the near-uniform spacing of rotational Raman peaks in the spectral domain. Long-time, 100-ps duration observations of the transient Raman polarization are presented, and the observed transients are compared to simulated results. Fourier transformation of the transients reveals two distinct sets of beat frequencies. Simulation results for temperatures from 300-700 K are used to illustrate the temperature sensitivity of the time-domain transients and their Fourier-transform counterparts. And strategies for diagnostics are briefly discussed. These results are being utilized to develop gas-phase measurement strategies for temperature and species concentration.

  18. Probe-pulse optimization for nonresonant suppression in hybrid fs/ps coherent anti-Stokes Raman scattering at high temperature.

    PubMed

    Miller, Joseph D; Slipchenko, Mikhail N; Meyer, Terrence R

    2011-07-04

    Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) offers accurate thermometry at kHz rates for combustion diagnostics. In high-temperature flames, selection of probe-pulse characteristics is key to simultaneously optimizing signal-to-nonresonant-background ratio, signal strength, and spectral resolution. We demonstrate a simple method for enhancing signal-to-nonresonant-background ratio by using a narrowband Lorentzian filter to generate a time-asymmetric probe pulse with full-width-half-maximum (FWHM) pulse width of only 240 fs. This allows detection within just 310 fs after the Raman excitation for eliminating nonresonant background while retaining 45% of the resonant signal at 2000 K. The narrow linewidth is comparable to that of a time-symmetric sinc2 probe pulse with a pulse width of ~2.4 ps generated with a conventional 4-f pulse shaper. This allows nonresonant-background-free, frequency-domain vibrational spectroscopy at high temperature, as verified using comparisons to a time-dependent theoretical fs/ps CARS model.

  19. Broadband hyperspectral coherent anti-Stokes Raman scattering microscopy for stain-free histological imaging with principal component analysis

    NASA Astrophysics Data System (ADS)

    Xu, Jingjiang; Guo, Baoshan; Wong, Kenneth K. Y.; Tsia, Kevin K.

    2014-02-01

    Routine procedures in standard histopathology involve laborious steps of tissue processing and staining for final examination. New techniques which can bypass these procedures and thus minimize the tissue handling error would be of great clinical value. Coherent anti-Stokes Raman scattering (CARS) microscopy is an attractive tool for label-free biochemical-specific characterization of biological specimen. However, a vast majority of prior works on CARS (or stimulated Raman scattering (SRS)) bioimaging restricted analyses on a narrowband or well-distinctive Raman spectral signatures. Although hyperspectral SRS/CARS imaging has recently emerged as a better solution to access wider-band spectral information in the image, studies mostly focused on a limited spectral range, e.g. CH-stretching vibration of lipids, or non-biological samples. Hyperspectral image information in the congested fingerprint spectrum generally remains untapped for biological samples. In this regard, we further explore ultrabroadband hyperspectral multiplex (HM-CARS) to perform chemoselective histological imaging with the goal of exploring its utility in stain-free clinical histopathology. Using the supercontinuum Stokes, our system can access the CARS spectral window as wide as >2000cm-1. In order to unravel the congested CARS spectra particularly in the fingerprint region, we first employ a spectral phase-retrieval algorithm based on Kramers-Kronig (KK) transform to minimize the non-resonant background in the CARS spectrum. We then apply principal component analysis (PCA) to identify and map the spatial distribution of different biochemical components in the tissues. We demonstrate chemoselective HM-CARS imaging of a colon tissue section which displays the key cellular structures that correspond well with standard stained-tissue observation.

  20. Effects of pressure variations on electronic-resonance-enhanced coherent anti-Stokes Raman scattering of nitric oxide

    NASA Astrophysics Data System (ADS)

    Kulatilaka, Waruna D.; Chai, Ning; Naik, Sameer V.; Roy, Sukesh; Laurendeau, Normand M.; Lucht, Robert P.; Kuehner, Joel P.; Gord, James R.

    2007-06-01

    The effects of pressure variations on the electronic-resonance-enhanced coherent anti-Stokes Raman scattering (ERE-CARS) signal of nitric oxide (NO) were studied at pressures ranging from 0.1 to 8 bar. ERE-CARS signals were recorded in a gas cell filled with a mixture of 300 ppm NO in N 2 buffer gas at room temperature. The ERE-CARS signal was found to increase with rising pressure up to 2 bar and to remain nearly constant thereafter. The spectra recorded at different cell pressures were modeled using a modified version of the Sandia CARSFT code. Laser-saturation effects were accounted for by systematically varying the theoretical ultraviolet probe-laser linewidth. Excellent agreement was obtained between theory and experiment for the pressure-scaling behavior of the ERE-CARS signal of NO. This finding, along with a negligible influence of electronic quenching on the ERE-CARS signal, provides strong incentive for the application of ERE-CARS to measurements of NO concentrations in high-pressure combustion environments.

  1. Nonperturbative Chemical Imaging of Organelle Transport in Living Cells with Coherent Anti-Stokes Raman Scattering Microscopy

    PubMed Central

    Nan, Xiaolin; Potma, Eric O.; Xie, X. Sunney

    2006-01-01

    Nonperturbative monitoring of intracellular organelle transport in unstained living cells was achieved with coherent anti-Stokes Raman scattering (CARS) microscopy. To avoid possible interference with the organelle transport introduced by laser radiation, we first examined different illumination conditions. Using a new photodamage criterion based on morphological changes of the cells, we determined the threshold values of both pulse energy and average power at relevant wavelengths. Under excitation conditions much milder than the threshold levels, we were able to monitor the motions of lipid droplet (LD) organelles in steroidogenic mouse adrenal cortical (Y-1) cells with CARS microscopy in real time without perturbations to the cells. Particle tracking analyses revealed subdiffusion as well as active transport of LDs along microtubules. Interestingly, LD active transport is only present in Y-1 cells that rounded up in culture, a morphological change associated with steroidogenesis, suggesting possible involvements of LD active transport in the latter. Simultaneous imaging of LDs and mitochondria with CARS and two-photon fluorescence microscopy clearly showed that interactions between the two organelles could be facilitated by high LD motility. These observations demonstrate CARS microscopy as a powerful noninvasive imaging tool for studying dynamic processes in living cells. PMID:16632501

  2. Paranodal myelin retraction in relapsing experimental autoimmune encephalomyelitis visualized by coherent anti-Stokes Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Fu, Yan; Frederick, Terra J.; Huff, Terry B.; Goings, Gwendolyn E.; Miller, Stephen D.; Cheng, Ji-Xin

    2011-10-01

    How demyelination is initiated is a standing question for pathology of multiple sclerosis. By label-free coherent anti-Stokes Raman scattering (CARS) imaging of myelin lipids, we investigate myelin integrity in the lumbar spinal cord tissue isolated from naïve SJL mice, and from mice at the onset, peak acute, and remission stages of relapsing experimental autoimmune encephalomyelitis (EAE). Progressive demyelinating disease is initially characterized by the retraction of paranodal myelin both at the onset of disease and at the borders of acute demyelinating lesions. Myelin retraction is confirmed by elongated distribution of neurofascin proteins visualized by immunofluorescence. The disruption of paranodal myelin subsequently exposes Kv1.2 channels at the juxtaparanodes and lead to the displacement of Kv1.2 channels to the paranodal and nodal domains. Paranodal myelin is partially restored during disease remission, indicating spontaneous myelin regeneration. These findings suggest that paranodal domain injury precedes formation of internodal demyelinating lesions in relapsing EAE. Our results also demonstrate that CARS microscopy is an effective readout of myelin disease burden.

  3. Assessment of liver steatosis and fibrosis in rats using integrated coherent anti-Stokes Raman scattering and multiphoton imaging technique

    NASA Astrophysics Data System (ADS)

    Lin, Jian; Lu, Fake; Zheng, Wei; Xu, Shuoyu; Tai, Dean; Yu, Hanry; Huang, Zhiwei

    2011-11-01

    We report the implementation of a unique integrated coherent anti-Stokes Raman scattering (CARS), second-harmonic generation (SHG), and two-photon excitation fluorescence (TPEF) microscopy imaging technique developed for label-free monitoring of the progression of liver steatosis and fibrosis generated in a bile duct ligation (BDL) rat model. Among the 21 adult rats used in this study, 18 rats were performed with BDL surgery and sacrificed each week from weeks 1 to 6 (n = 3 per week), respectively; whereas 3 rats as control were sacrificed at week 0. Colocalized imaging of the aggregated hepatic fats, collagen fibrils, and hepatocyte morphologies in liver tissue is realized by using the integrated CARS, SHG, and TPEF technique. The results show that there are significant accumulations of hepatic lipid droplets and collagen fibrils associated with severe hepatocyte necrosis in BDL rat liver as compared to a normal liver tissue. The volume of normal hepatocytes keeps decreasing and the fiber collagen content in BDL rat liver follows a growing trend until week 6; whereas the hepatic fat content reaches a maximum in week 4 and then appears to stop growing in week 6, indicating that liver steatosis and fibrosis induced in a BDL rat liver model may develop at different rates. This work demonstrates that the integrated CARS and multiphoton microscopy imaging technique has the potential to provide an effective means for early diagnosis and detection of liver steatosis and fibrosis without labeling.

  4. Dual/differential coherent anti-Stokes Raman scattering module for multiphoton microscopes with a femtosecond Ti:sapphire oscillator

    NASA Astrophysics Data System (ADS)

    Li, Bei; Borri, Paola; Langbein, Wolfgang

    2013-06-01

    In the last decade, coherent anti-Stokes Raman scattering (CARS) microscopy has emerged as a powerful multiphoton imaging technique offering label-free chemical sensitivity and high three-dimensional resolution. However, its widespread application in the life sciences has been hampered by the use of costly pulsed lasers, the existence of a nonresonant background requiring involved technical solutions for its efficient suppression, and the limited acquisition speed of multiplex techniques addressing several vibrational resonances, if improved chemical specificity is needed. We have recently reported a differential CARS technique (D-CARS), which simultaneously measures two vibrational frequencies, enhancing the chemical selectivity and sensitivity without introducing costly hardware, while maintaining fast acquisition. In this study, we demonstrate a compact, fully automated, cost-effective module, which integrates on hardware and software level with a commercial multiphoton microscope based on a single 100 fs Ti:Sapphire oscillator and enables D-CARS microscopy in a user-friendly format for applications in the life sciences.

  5. Dual/differential coherent anti-Stokes Raman scattering module for multiphoton microscopes with a femtosecond Ti:sapphire oscillator.

    PubMed

    Li, Bei; Borri, Paola; Langbein, Wolfgang

    2013-06-01

    In the last decade, coherent anti-Stokes Raman scattering (CARS) microscopy has emerged as a powerful multiphoton imaging technique offering label-free chemical sensitivity and high three-dimensional resolution. However, its widespread application in the life sciences has been hampered by the use of costly pulsed lasers, the existence of a nonresonant background requiring involved technical solutions for its efficient suppression, and the limited acquisition speed of multiplex techniques addressing several vibrational resonances, if improved chemical specificity is needed. We have recently reported a differential CARS technique (D-CARS), which simultaneously measures two vibrational frequencies, enhancing the chemical selectivity and sensitivity without introducing costly hardware, while maintaining fast acquisition. In this study, we demonstrate a compact, fully automated, cost-effective module, which integrates on hardware and software level with a commercial multiphoton microscope based on a single 100 fs Ti:Sapphire oscillator and enables D-CARS microscopy in a user-friendly format for applications in the life sciences.

  6. Detecting polymeric nanoparticles with coherent anti-stokes Raman scattering microscopy in tissues exhibiting fixative-induced autofluorescence

    NASA Astrophysics Data System (ADS)

    Garrett, N. L.; Godfrey, L.; Lalatsa, A.; Serrano, D. R.; Uchegbu, I. F.; Schatzlein, A.; Moger, J.

    2015-03-01

    Recent advances in pharmaceutical nanotechnology have enabled the development of nano-particulate medicines with enhanced drug performance. Although the fate of these nano-particles can be macroscopically tracked in the body (e.g. using radio-labeling techniques), there is little information about the sub-cellular scale mechanistic processes underlying the particle-tissue interactions, or how these interactions may correlate with pharmaceutical efficacy. To rationally engineer these nano-particles and thus optimize their performance, these mechanistic interactions must be fully understood. Coherent Anti-Stokes Raman scattering (CARS) microscopy provides a label-free means for visualizing biological samples, but can suffer from a strong non-resonant background in samples that are prepared using aldehyde-based fixatives. We demonstrate how formalin fixative affects the detection of polymeric nanoparticles within kidneys following oral administration using CARS microscopy, compared with samples that were snap-frozen. These findings have implications for clinical applications of CARS for probing nanoparticle distribution in tissue biopsies.

  7. Label-free Evaluation of Hepatic Microvesicular Steatosis with Multimodal Coherent Anti-Stokes Raman Scattering Microscopy

    PubMed Central

    Le, Thuc T.; Ziemba, Amy; Urasaki, Yasuyo; Brotman, Steven; Pizzorno, Giuseppe

    2012-01-01

    Hepatic microvesicular steatosis is a hallmark of drug-induced hepatotoxicity and early-stage fatty liver disease. Current histopathology techniques are inadequate for the clinical evaluation of hepatic microvesicular steatosis. In this paper, we explore the use of multimodal coherent anti-Stokes Raman scattering (CARS) microscopy for the detection and characterization of hepatic microvesicular steatosis. We show that CARS microscopy is more sensitive than Oil Red O histology for the detection of microvesicular steatosis. Computer-assisted analysis of liver lipid level based on CARS signal intensity is consistent with triglyceride measurement using a standard biochemical assay. Most importantly, in a single measurement procedure on unprocessed and unstained liver tissues, multimodal CARS imaging provides a wealth of critical information including the detection of microvesicular steatosis and quantitation of liver lipid content, number and size of lipid droplets, and lipid unsaturation and packing order of lipid droplets. Such information can only be assessed by multiple different methods on processed and stained liver tissues or tissue extracts using current standard analytical techniques. Multimodal CARS microscopy also permits label-free identification of lipid-rich non-parenchymal cells. In addition, label-free and non-perturbative CARS imaging allow rapid screening of mitochondrial toxins-induced microvesicular steatosis in primary hepatocyte cultures. With its sensitivity and versatility, multimodal CARS microscopy should be a powerful tool for the clinical evaluation of hepatic microvesicular steatosis. PMID:23226469

  8. Quantitative chemical imaging with background-free multiplex coherent anti-Stokes Raman scattering by dual-soliton Stokes pulses

    PubMed Central

    Chen, Kun; Wu, Tao; Wei, Haoyun; Zhou, Tian; Li, Yan

    2016-01-01

    Coherent anti-Stokes Raman microscopy (CARS) is a quantitative, chemically specific, and label-free optical imaging technique for studying inhomogeneous systems. However, the complicating influence of the nonresonant response on the CARS signal severely limits its sensitivity and specificity and especially limits the extent to which CARS microscopy has been used as a fully quantitative imaging technique. On the basis of spectral focusing mechanism, we establish a dual-soliton Stokes based CARS microspectroscopy and microscopy scheme capable of quantifying the spatial information of densities and chemical composition within inhomogeneous samples, using a single fiber laser. Dual-soliton Stokes scheme not only removes the nonresonant background but also allows robust acquisition of multiple characteristic vibrational frequencies. This all-fiber based laser source can cover the entire fingerprint (800-2200 cm−1) region with a spectral resolution of 15 cm−1. We demonstrate that quantitative degree determination of lipid-chain unsaturation in the fatty acids mixture can be achieved by the characterization of C = C stretching and CH2 deformation vibrations. For microscopy purposes, we show that the spatially inhomogeneous distribution of lipid droplets can be further quantitatively visualized using this quantified degree of lipid unsaturation in the acyl chain for contrast in the hyperspectral CARS images. The combination of compact excitation source and background-free capability to facilitate extraction of quantitative composition information with multiplex spectral peaks will enable wider applications of quantitative chemical imaging in studying biological and material systems. PMID:27867704

  9. Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics

    DOE PAGES

    Kunnus, Kristjan; Josefsson, Ida; Rajkovic, Ivan; ...

    2016-10-07

    Here, ultrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbitalmore » and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO)5 in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-ray pulses is given—which will be covered experimentally by upcoming transform-limited x-ray sources.« less

  10. Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics

    SciTech Connect

    Kunnus, Kristjan; Josefsson, Ida; Rajkovic, Ivan; Schreck, Simon; Quevedo, Wilson; Beye, Martin; Grübel, Sebastian; Scholz, Mirko; Nordlund, Dennis; Zhang, Wenkai; Hartsock, Robert W.; Gaffney, Kelly J.; Schlotter, William F.; Turner, Joshua J.; Kennedy, Brian; Hennies, Franz; Techert, Simone; Wernet, Philippe; Odelius, Michael; Föhlisch, Alexander

    2016-10-07

    Here, ultrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbital and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO)5 in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-ray pulses is given—which will be covered experimentally by upcoming transform-limited x-ray sources.

  11. Development of Combined Dual-Pump Vibrational and Pure-Rotational Coherent Anti-Stokes Raman Scattering Technique.

    NASA Astrophysics Data System (ADS)

    Satija, Aman; Lucht, Robert P.

    2015-06-01

    Coherent anti-Stokes Raman scattering is a parametric, four-wave mixing process. CARS, as a diagnostic technique, has been used extensively for obtaining accurate temperature and species concentration information in non-reacting and reacting flows. Dual-pump vibrational CARS (DPVCARS) can provide quantitative temperature and concentration information on multiple species in the probe volume. Mole-fraction information on molecules such as N2, O2, H2 and CO2 have been obtained in flames with peak temperature in excess of 2000 K. Although DPVCARS provides high accuracy at higher temperatures it has low sensitivity at lower temperatures (below 800 K). Typically, pure-rotational CARS (PRCARS) provides excellent sensitivity and precision at lower temperatures. We have combined DPVCARS and two-beam PRCARS into a single system which employs three laser beams at different wavelengths. The accuracy and precision of the new combined CARS system has been characterized in laminar flames. The system's single-shot precision is better than 5.5 % between 295-2200 K, indicating its suitability for diagnostics in turbulent flames. The new system has been applied towards understanding flame structure of CH4/H2/air laminar flames, stabilized in a counter-flow burner. Here, we present results detailing the development and application of the new combined CARS technique.

  12. Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics

    NASA Astrophysics Data System (ADS)

    Kunnus, Kristjan; Josefsson, Ida; Rajkovic, Ivan; Schreck, Simon; Quevedo, Wilson; Beye, Martin; Grübel, Sebastian; Scholz, Mirko; Nordlund, Dennis; Zhang, Wenkai; Hartsock, Robert W.; Gaffney, Kelly J.; Schlotter, William F.; Turner, Joshua J.; Kennedy, Brian; Hennies, Franz; Techert, Simone; Wernet, Philippe; Odelius, Michael; Föhlisch, Alexander

    2016-10-01

    Ultrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbital and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO)5 in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-ray pulses is given—which will be covered experimentally by upcoming transform-limited x-ray sources.

  13. Tracing engineered nanomaterials in biological tissues using coherent anti-Stokes Raman scattering (CARS) microscopy - A critical review.

    PubMed

    Goodhead, Rhys M; Moger, Julian; Galloway, Tamara S; Tyler, Charles R

    2015-01-01

    Nanomaterials (NMs) are used in an extremely diverse range of products and are increasingly entering the environment, driving a need to better understand their potential health effects in both humans and wildlife. A major challenge in nanoparticle (eco)toxicology is the ability to localise NMs post exposure, to enable more targeted biological effects analyses. A range of imaging techniques have been applied to do so, but they are limited, requiring either extensive processing of the material, staining or use of high intensity illumination that can lead to photo damage and/or have limited tissue penetration. Coherent anti-Stokes Raman scattering (CARS) microscopy is a label-free imaging technique, providing contrast based on the intrinsic molecular vibrations of a specimen, circumventing the need for chemical perturbation by exogenous labels. CARS uses near infra-red excitation wavelengths which allow microscopy at depths of several hundred microns in intact tissues and minimises photo-damage to live and delicate samples. Here we provide an overview of the CARS process and present a series of illustrative examples demonstrating its application for detecting NMs within biological tissues, ranging from isolated cells to whole organisms and including materials spanning metals to polymers. We highlight the advantages of this technique which include chemically selective live imaging and substantial depth penetration, but we also discuss its limitations when applied to nanotoxicology, which most notably include the lack of resolution for studies on single nanoparticles.

  14. Effects of phase and coupling between the vibrational modes on selective excitation in coherent anti-Stokes Raman scattering microscopy

    SciTech Connect

    Patel, Vishesha; Malinovsky, Vladimir S.; Malinovskaya, Svetlana

    2010-06-15

    Coherent anti-Stokes Raman scattering (CARS) microscopy has been a major tool of investigation of biological structures as it contains the vibrational signature of molecules. A quantum control method based on chirped pulse adiabatic passage was recently proposed for selective excitation of a predetermined vibrational mode in CARS microscopy [Malinovskaya and Malinovsky, Opt. Lett. 32, 707 (2007)]. The method utilizes the chirp sign variation at the peak pulse amplitude and gives a robust adiabatic excitation of the desired vibrational mode. Using this method, we investigate the impact of coupling between vibrational modes in molecules on controllability of excitation of the CARS signal. We analyze two models of two coupled two-level systems (TLSs) having slightly different transitional frequencies. The first model, featuring degenerate ground states of the TLSs, gives robust adiabatic excitation and maximum coherence in the resonant TLS for positive value of the chirp. In the second model, implying nondegenerate ground states in the TLSs, a population distribution is observed in both TLSs, resulting in a lack of selectivity of excitation and low coherence. It is shown that the relative phase and coupling between the TLSs play an important role in optimizing coherence in the desired vibrational mode and suppressing unwanted transitions in CARS microscopy.

  15. Ratio of the surface-enhanced anti-Stokes scattering to the surface-enhanced Stokes-Raman scattering for molecules adsorbed on a silver electrode

    NASA Astrophysics Data System (ADS)

    Brolo, A. G.; Sanderson, A. C.; Smith, A. P.

    2004-01-01

    Surface-enhanced Raman scattering (SERS) from oxazine 720 (oxa), rhodamine 6G (R6G), and pyridine (py) adsorbed on a rough silver surface was observed. The silver electrode was immersed in aqueous solutions permitting control of the potential bias applied to the surface. SERS spectra in the Stokes and anti-Stokes regions were obtained for several applied potentials and two laser excitation energies. Normalized ratios between the anti-Stokes and the Stokes intensities K were calculated from the SERS spectra. The K ratios differed from unity for all the systems investigated. A preferential enhancement of the (surface-enhanced) Stokes scattering was observed for oxa and py. In contrast, the K ratios were higher than unity for R6G, indicating an increase in the anti-Stokes signal. The K ratios measured in this work decreased with the excitation energy and showed a dependence on the energy of the vibrational modes. These results were satisfactorily explained using resonance models, based on the charge-transfer and electromagnetic theories for SERS. No evidence for a SERS-induced nonthermal population distribution among the vibrational states of the adsorbed molecules (vibrational optical pumping) was found. Therefore, we conclude that the main features of the preferential enhancement of the anti-Stokes scattering for an adsorbed molecule on rough silver can be fully understood in the context of current SERS theories.

  16. Pressure measurements using hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering.

    PubMed

    Kearney, Sean P; Danehy, Paul M

    2015-09-01

    We investigate the feasibility of gas-phase pressure measurements using fs/ps rotational CARS. Femtosecond pump and Stokes pulses impulsively prepare a rotational Raman coherence, which is probed by a high-energy 5-ps pulse introduced at a time delay from the Raman preparation. These ultrafast laser pulses are shorter than collisional-dephasing time scales, enabling a new hybrid time- and frequency-domain detection scheme for pressure. Single-laser-shot rotational CARS spectra were recorded from N2 contained in a room-temperature gas cell for pressures from 0.4 to 3 atm and probe delays ranging from 16 to 298 ps. Sensitivity of the accuracy and precision of the pressure data to probe delay was investigated. The technique exhibits superior precision and comparable accuracy to previous laser-diagnostic pressure measurements.

  17. In vivo lipid saturation study of C. elegans using quantitative broadband coherent anti-Stokes Raman imaging (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Littleton, Bradley; Kavanagh, Thomas; Nie, Yu; Abbate, Vincenzo; Hylands, Peter; Sturzenbaum, Stephen; Richards, David

    2016-03-01

    In vivo lipid saturation maps of microscopic nematodes (Caenorhabditis elegans) have been produced using our novel Spectral Interferometric Polarisation Coherent anti-Stokes Raman Scattering (SIP-CARS) imaging technique. This technique employs simple passive polarisation optics and a balanced homodyne detection scheme to exploit symmetries in the CARS polarisation response resulting in the complete cancellation of the non-resonant background (NRB) and real component of the CARS signal (with no prior or post assumptions as regards to their form). The remaining imaginary component of the CARS response is linear with analyte concentration and directly relatable to the spontaneous Raman spectrum [1]. Furthermore, the resonant CARS signal is interferometrically amplified by the non-resonant response, a necessity for rapid imaging at biologically relevant powers [2]. This technique permits acquisition of a broad NRB-free spectrum, in excess of 1800cm-1, in a single exposure at each pixel. This allows simultaneous determination of lipid droplet saturation, from the fingerprint region, and lipid order, from the C-H stretch region from which maps can be readily constructed. Additionally exploiting the dispersive nature of our signal collection two-photon autofluorescence can be isolated and images subsequently produced. We have successfully applied this technique to identify differences in lipid saturation distributions in selective C. elegans mutants and demonstrated that the technique is sufficiently sensitive to detect the effects of lipid metabolism altering drugs on wild type C. elegans. [1] Littleton et al, Phys Rev Lett, 111, 103902 (2013) [2] Parekh et al, Biophys J, 99, 2695-2704 (2010)

  18. Temperature measurements in metalized propellant combustion using hybrid fs/ps coherent anti-Stokes Raman scattering

    DOE PAGES

    Kearney, Sean P.; Guildenbecher, Daniel R.

    2016-06-20

    We apply ultrafast pure-rotational coherent anti-Stokes Raman scattering (CARS) for temperature and relative oxygen concentration measurements in the plume emanating from a burning, aluminized ammonium-perchlorate propellant strand. Combustion of these metal-based propellants is a particularly hostile environment for laser-based diagnostics, with intense background luminosity and scattering from hot metal particles as large as several hundred micrometers in diameter. CARS spectra that were previously obtained using nanosecond pulsed lasers in an aluminum-particle-seeded flame are examined and are determined to be severely impacted by nonresonant background, presumably as a result of the plasma formed by particulate-enhanced laser-induced breakdown. Introduction of femtosecond/picosecond (fs/ps)more » laser pulses improves CARS detection by providing time-gated elimination of strong nonresonant background interference. Single-laser-shot fs/ps CARS spectra were acquired from the burning propellant plume, with picosecond probe-pulse delays of 0 and 16 ps from the femtosecond pump and Stokes pulses. At zero delay, nonresonant background overwhelms the Raman-resonant spectroscopic features. Time-delayed probing results in the acquisition of background-free spectra that were successfully fit for temperature and relative oxygen content. Temperature probability densities and temperature/oxygen correlations were constructed from ensembles of several thousand single-laser-shot measurements with the CARS measurement volume positioned within 3 mm or less of the burning propellant surface. Lastly, the results show that ultrafast CARS is a potentially enabling technology for probing harsh, particle-laden flame environments.« less

  19. Temperature measurements in metalized propellant combustion using hybrid fs/ps coherent anti-Stokes Raman scattering.

    PubMed

    Kearney, Sean P; Guildenbecher, Daniel R

    2016-06-20

    We apply ultrafast pure-rotational coherent anti-Stokes Raman scattering (CARS) for temperature and relative oxygen concentration measurements in the plume emanating from a burning, aluminized ammonium-perchlorate propellant strand. Combustion of these metal-based propellants is a particularly hostile environment for laser-based diagnostics, with intense background luminosity and scattering from hot metal particles as large as several hundred micrometers in diameter. CARS spectra that were previously obtained using nanosecond pulsed lasers in an aluminum-particle-seeded flame are examined and are determined to be severely impacted by nonresonant background, presumably as a result of the plasma formed by particulate-enhanced laser-induced breakdown. Introduction of femtosecond/picosecond (fs/ps) laser pulses improves CARS detection by providing time-gated elimination of strong nonresonant background interference. Single-laser-shot fs/ps CARS spectra were acquired from the burning propellant plume, with picosecond probe-pulse delays of 0 and 16 ps from the femtosecond pump and Stokes pulses. At zero delay, nonresonant background overwhelms the Raman-resonant spectroscopic features. Time-delayed probing results in the acquisition of background-free spectra that were successfully fit for temperature and relative oxygen content. Temperature probability densities and temperature/oxygen correlations were constructed from ensembles of several thousand single-laser-shot measurements with the CARS measurement volume positioned within 3 mm or less of the burning propellant surface. The results show that ultrafast CARS is a potentially enabling technology for probing harsh, particle-laden flame environments.

  20. Temperature measurements in metalized propellant combustion using hybrid fs/ps coherent anti-Stokes Raman scattering

    SciTech Connect

    Kearney, Sean P.; Guildenbecher, Daniel R.

    2016-06-20

    We apply ultrafast pure-rotational coherent anti-Stokes Raman scattering (CARS) for temperature and relative oxygen concentration measurements in the plume emanating from a burning, aluminized ammonium-perchlorate propellant strand. Combustion of these metal-based propellants is a particularly hostile environment for laser-based diagnostics, with intense background luminosity and scattering from hot metal particles as large as several hundred micrometers in diameter. CARS spectra that were previously obtained using nanosecond pulsed lasers in an aluminum-particle-seeded flame are examined and are determined to be severely impacted by nonresonant background, presumably as a result of the plasma formed by particulate-enhanced laser-induced breakdown. Introduction of femtosecond/picosecond (fs/ps) laser pulses improves CARS detection by providing time-gated elimination of strong nonresonant background interference. Single-laser-shot fs/ps CARS spectra were acquired from the burning propellant plume, with picosecond probe-pulse delays of 0 and 16 ps from the femtosecond pump and Stokes pulses. At zero delay, nonresonant background overwhelms the Raman-resonant spectroscopic features. Time-delayed probing results in the acquisition of background-free spectra that were successfully fit for temperature and relative oxygen content. Temperature probability densities and temperature/oxygen correlations were constructed from ensembles of several thousand single-laser-shot measurements with the CARS measurement volume positioned within 3 mm or less of the burning propellant surface. Lastly, the results show that ultrafast CARS is a potentially enabling technology for probing harsh, particle-laden flame environments.

  1. Exploring the interactions between peptides and lipid bilayers using coherent anti-Stokes Raman scattering and two-photon fluorescence

    NASA Astrophysics Data System (ADS)

    Mari, M.; Mouras, R.; Downes, A.; Elfick, A.

    2011-06-01

    We have used a versatile and powerful microscope[1] for multi-modal biomedical imaging on which we combine Coherent Anti-Stokes Raman Scattering (CARS) with Two Photon Excitation Fluorescence (TPEF) using a Nd: YVO4 pump laser. We acquired 2PEF, CARS, and phase contrast images of Multilamellar Vesicles (MLVs) and Giant Unilamellar Vesicles (GUVs), as well as Raman spectra of the constituent lipids. A wide range of peptides are harmful to cells by altering the structure of the biological membranes. This effect depends on the composition of the membrane and the chemical structure of the peptide. The peptide we studied is the beta amyloid Aβ which is a major component of the amyloid plaques deposited on neuronal membranes of Alzheimer's disease (AD) patients. AD is neurodegenerative disorder in which the hallmark symptoms include cognitive decline and dementia[2] and is characterized by the formation of extracellular amyloid fibrils on the neuronal membranes of the brain. Many questions still remain unanswered concerning the destabilization of cellular ionic homeostasis due to pores formed during the interactions of lipid membranes with peptides. In this project, biomimics of cell membranes are used. The structures that best mimic the plasma membranes are MLVs or GUVs. These vesicles are formed using the gentle hydration technique[3] or the electroformation technique[4] respectively and are composed of phospholipids such as DOPC, DPPC, D62PPC and their binary mixtures. The MLVs and GUVs imaging by CARS and TPEF microscopy not only permits the direct imaging of the leakage phenomenon caused by the toxic peptide (Aβ) on the lipid bilayer, but also records simultaneously the lateral structure of the bilayer and peptide distribution in the plane across the membrane.

  2. Ultrafast saturation of electronic-resonance-enhanced coherent anti-Stokes Raman scattering and comparison for pulse durations in the nanosecond to femtosecond regime

    NASA Astrophysics Data System (ADS)

    Patnaik, Anil K.; Roy, Sukesh; Gord, James R.

    2016-02-01

    The saturation threshold of a probe pulse in an ultrafast electronic-resonance-enhanced (ERE) coherent anti-Stokes Raman spectroscopy (CARS) configuration is calculated. We demonstrate that while the underdamping condition is a sufficient condition for saturation of ERE-CARS with the long-pulse excitations, a transient gain must be achieved to saturate the ERE-CARS signal for the ultrafast probe regime. We identify that the area under the probe pulse can be used as a definitive parameter to determine the criterion for a saturation threshold for ultrafast ERE-CARS. From a simplified analytical solution and a detailed numerical calculation based on density-matrix equations, the saturation threshold of ERE-CARS is compared for a wide range of probe-pulse durations from the 10-ns to the 10-fs regime. The theory explains both qualitatively and quantitatively the saturation thresholds of resonant transitions and also gives a predictive capability for other pulse duration regimes. The presented criterion for the saturation threshold will be useful in establishing the design parameters for ultrafast ERE-CARS.

  3. Label-free imaging of trabecular meshwork cells using Coherent Anti-Stokes Raman Scattering (CARS) microscopy

    PubMed Central

    Lei, Tim C.; Ammar, David A.; Masihzadeh, Omid; Gibson, Emily A.

    2011-01-01

    Purpose To image the human trabecular meshwork (TM) using a non-invasive, non-destructive technique without the application of exogenous label. Methods Flat-mounted TM samples from a human cadaver eye were imaged using two nonlinear optical techniques: coherent anti-Stokes Raman scattering (CARS) and two-photon autofluorescence (TPAF). In TPAF, two optical photons are simultaneously absorbed and excite molecules in the sample that then emit a higher energy photon. The signal is predominately from collagen and elastin. The CARS technique uses two laser frequencies to specifically excite carbon-hydrogen bonds, allowing the visualization of lipid-rich cell membranes. Multiple images were taken along an axis perpendicular to the surface of the TM for subsequent analysis. Results Analysis of multiple TPAF images of the TM reveals the characteristic overlapping bundles of collagen of various sizes. Simultaneous CARS imaging revealed elliptical structures of ~7×10 µm in diameter populating the meshwork which were consistent with TM cells. Irregularly shaped objects of ~4 µm diameter appeared in both the TPAF and CARS channels, and are consistent with melanin granules. Conclusions CARS techniques were successful in imaging live TM cells in freshly isolated human TM samples. Similar images have been obtained with standard histological techniques, however the method described here has the advantage of being performed on unprocessed, unfixed tissue free from the potential distortions of the fine tissue morphology that can occur due to infusion of fixatives and treatment with alcohols. CARS imaging of the TM represents a new avenue for exploring details of aqueous outflow and TM cell physiology. PMID:22025898

  4. Imaging the Effects of Prostaglandin Analogues on Cultured Trabecular Meshwork Cells by Coherent Anti-Stokes Raman Scattering

    PubMed Central

    Lei, Tim C.; Masihzadeh, Omid; Kahook, Malik Y.; Ammar, David A.

    2013-01-01

    Purpose. The aim of this study was to nondestructively monitor morphological changes to the lipid membranes of primary cultures of living human trabecular meshwork cells (hTMC) without the application of exogenous label. Methods. Live hTMC were imaged using two nonlinear optical techniques: coherent anti-Stokes Raman scattering (CARS) and two-photon autofluorescence (TPAF). The hTMC were treated with a commercial formulation of latanoprost (0.5 μg/mL) for 24 hours before imaging. Untreated cells and cells treated with vehicle containing the preservative benzalkonium chloride (BAK; 2 μg/mL) were imaged as controls. After CARS/TPAF imaging, hTMC were fixed, stained with the fluorescent lipid dye Nile Red, and imaged by conventional confocal microscopy to verify lipid membrane structures. Results. Analysis of CARS/TPAF images of hTMC treated with latanoprost revealed multiple intracellular lipid membranes absent from untreated or BAK-treated hTMC. Treatment of hTMC with sodium fluoride or ouabain, agents shown to cause morphological changes to hTMC, also did not induce formation of intracellular lipid membranes. Conclusions. CARS microscopy detected changes in living hTMC morphology that were validated by subsequent histological stain. Prostaglandin-induced changes to hTMC involved rearrangement of lipid membranes within these cells. These in vitro results identify a novel biological response to a class of antiglaucoma drugs, and further experiments are needed to establish how this effect is involved in the hypotensive action of prostaglandin analogues in vivo. PMID:23900606

  5. Coherent anti-Stokes Raman scattering in isolated air-guided modes of a hollow-core photonic-crystal fiber

    SciTech Connect

    Fedotov, A.B.; Zheltikov, A.M.; Konorov, S.O.; Mitrokhin, V.P.; Serebryannikov, E.E

    2004-10-01

    Hollow-core photonic-crystal fibers are shown to offer the unique possibility of coherent excitation and probing of Raman-active vibrations in molecules by isolated air-guided modes of electromagnetic radiation. A 3-cm section of a hollow photonic-crystal fiber is used to prepare isolated air-guided modes of pump and probe fields for a coherent excitation of 2331-cm{sup -1} Q-branch vibrations of molecular nitrogen in the gas filling the fiber core, enhancing coherent anti-Stokes Raman scattering through these vibrations by a factor of 15 relative to the regime of tight focusing.

  6. Dynamical study of the water penetration process into a cellulose acetate film studied by coherent anti-Stokes Raman scattering (CARS) microspectroscopy

    NASA Astrophysics Data System (ADS)

    Fujisawa, Rie; Ohno, Tomoya; Kaneyasu, Junya F.; Leproux, Philippe; Couderc, Vincent; Kita, Hiroshi; Kano, Hideaki

    2016-07-01

    The penetration process of water into a cellulose acetate film was traced in real time by coherent anti-Stokes Raman scattering (CARS) microspectroscopy. The Cdbnd O stretch mode was red-shifted due to hydrogen-bond formation. We also found that two Raman bands at 1605 cm-1 and 1665 cm-1 emerged only in the early stage of the water penetration process. Based on the combined analysis of the experimental and computational studies, these bands at 1605 cm-1 and 1665 cm-1 were assigned as the OH bend mode due to hydrogen-bonded penetrated water and hydrogen-bonded OH groups in pyranose rings, respectively.

  7. Differential two-signal picosecond-pulse coherent anti-Stokes Raman scattering imaging microscopy by using a dual-mode optical parametric oscillator.

    PubMed

    Yoo, Yong Shim; Lee, Dong-Hoon; Cho, Hyuck

    2007-11-15

    We propose and demonstrate a novel differential two-signal technique of coherent anti-Stokes Raman scattering (CARS) imaging microscopy using a picosecond (ps) optical parametric oscillator (OPO). By adjusting a Lyot filter inside the cavity, we operated the OPO oscillating in two stable modes separated by a few nanometers. The CARS images generated by the two modes are separated by a spectrograph behind the microscope setup, and their differential image is directly obtained by balanced lock-in detection. The feasibility of the technique is experimentally verified by imaging micrometer-sized polystyrene beads immersed in water.

  8. Raman Spectroscopy.

    ERIC Educational Resources Information Center

    Gerrard, Donald L.

    1984-01-01

    Reviews literature on Raman spectroscopy from late 1981 to late 1983. Topic areas include: instrumentation and sampling; liquids and solutions; gases and matrix isolation; biological molecules; polymers; high-temperature and high-pressure studies; Raman microscopy; thin films and surfaces; resonance-enhanced and surface-enhanced spectroscopy; and…

  9. Quantitative, Label-Free Characterization of Stem Cell Differentiation at the Single-Cell Level by Broadband Coherent Anti-Stokes Raman Scattering Microscopy

    PubMed Central

    Lee, Young Jong; Vega, Sebastián L.; Patel, Parth J.; Aamer, Khaled A.; Moghe, Prabhas V.

    2014-01-01

    We use broadband coherent anti-Stokes Raman scattering (BCARS) microscopy to characterize lineage commitment of individual human mesenchymal stem cells cultured in adipogenic, osteogenic, and basal culture media. We treat hyperspectral images obtained by BCARS in two independent ways, obtaining robust metrics for differentiation. In one approach, pixel counts corresponding to functional markers, lipids, and minerals, are used to classify individual cells as belonging to one of the three lineage groups: adipocytes, osteoblasts, and undifferentiated stem cells. In the second approach, we use multivariate analysis of Raman spectra averaged exclusively over cytosol regions of individual cells to classify the cells into the same three groups, with consistent results. The exceptionally high speed of spectral imaging with BCARS allows us to chemically map a large number of cells with high spatial resolution, revealing not only the phenotype of individual cells, but also population heterogeneity in the degree of phenotype commitment. PMID:24224876

  10. Interference-free gas-phase thermometry at elevated pressure using hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering.

    PubMed

    Miller, Joseph D; Dedic, Chloe E; Roy, Sukesh; Gord, James R; Meyer, Terrence R

    2012-02-27

    Rotational-level-dependent dephasing rates and nonresonant background can lead to significant uncertainties in coherent anti-Stokes Raman scattering (CARS) thermometry under high-pressure, low-temperature conditions if the gas composition is unknown. Hybrid femtosecond/picosecond rotational CARS is employed to minimize or eliminate the influence of collisions and nonresonant background for accurate, frequency-domain thermometry at elevated pressure. The ability to ignore these interferences and achieve thermometric errors of <5% is demonstrated for N2 and O2 at pressures up to 15 atm. Beyond 15 atm, the effects of collisions cannot be ignored but can be minimized using a short probe delay (~6.5 ps) after Raman excitation, thereby improving thermometric accuracy with a time- and frequency-resolved theoretical model.

  11. Polarization suppression of the nonresonant background in femtosecond coherent anti-Stokes Raman scattering for flame thermometry at 5 kHz.

    PubMed

    Richardson, Daniel R; Bangar, Devashish; Lucht, Robert P

    2012-09-10

    Coherent anti-Stokes Raman scattering (CARS) spectra are acquired at 5 kHz in steady and unsteady flames while suppressing the nonresonant background by polarization techniques. Broadband femtosecond (fs) pump and Stokes pulses efficiently excite many Raman transitions in diatomic nitrogen which subsequently interfere and decay. Single-laser-shot measurements are performed as the decay of the Raman coherence is mapped to the frequency of the CARS signal by a chirped-probe pulse (CPP). As temperature increases, more Raman transitions contribute to the Raman coherence which leads to faster decay of the Raman coherence. Experimental fs CARS spectra are compared to a theoretical model to extract temperature measurements. The effects of probe time delay and temperature on nonresonant background suppressed CPP fs CARS spectra are examined. By suppressing the nonresonant background the evolution of the Raman coherence near zero probe time delay is more clearly revealed. The structure of the CPP fs CARS spectra with and without nonresonant background suppression is compared. The utility of polarization suppression of the nonresonant background for CPP fs CARS measurements is discussed.

  12. Emerging technology: applications of Raman spectroscopy for prostate cancer.

    PubMed

    Kast, Rachel E; Tucker, Stephanie C; Killian, Kevin; Trexler, Micaela; Honn, Kenneth V; Auner, Gregory W

    2014-09-01

    There is a need in prostate cancer diagnostics and research for a label-free imaging methodology that is nondestructive, rapid, objective, and uninfluenced by water. Raman spectroscopy provides a molecular signature, which can be scaled from micron-level regions of interest in cells to macroscopic areas of tissue. It can be used for applications ranging from in vivo or in vitro diagnostics to basic science laboratory testing. This work describes the fundamentals of Raman spectroscopy and complementary techniques including surface enhanced Raman scattering, resonance Raman spectroscopy, coherent anti-Stokes Raman spectroscopy, confocal Raman spectroscopy, stimulated Raman scattering, and spatially offset Raman spectroscopy. Clinical applications of Raman spectroscopy to prostate cancer will be discussed, including screening, biopsy, margin assessment, and monitoring of treatment efficacy. Laboratory applications including cell identification, culture monitoring, therapeutics development, and live imaging of cellular processes are discussed. Potential future avenues of research are described, with emphasis on multiplexing Raman spectroscopy with other modalities.

  13. In planta imaging of Δ9-tetrahydrocannabinolic acid in Cannabis sativa L. with hyperspectral coherent anti-Stokes Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Garbacik, Erik T.; Korai, Roza P.; Frater, Eric H.; Korterik, Jeroen P.; Otto, Cees; Offerhaus, Herman L.

    2013-04-01

    Nature has developed many pathways to produce medicinal products of extraordinary potency and specificity with significantly higher efficiencies than current synthetic methods can achieve. Identification of these mechanisms and their precise locations within plants could substantially increase the yield of a number of natural pharmaceutics. We report label-free imaging of Δ9-tetrahydrocannabinolic acid (THCa) in Cannabis sativa L. using coherent anti-Stokes Raman scattering microscopy. In line with previous observations we find high concentrations of THCa in pistillate flowering bodies and relatively low amounts within flowering bracts. Surprisingly, we find differences in the local morphologies of the THCa-containing bodies: organelles within bracts are large, diffuse, and spheroidal, whereas in pistillate flowers they are generally compact, dense, and have heterogeneous structures. We have also identified two distinct vibrational signatures associated with THCa, both in pure crystalline form and within Cannabis plants; at present the exact natures of these spectra remain an open question.

  14. In planta imaging of Δ⁹-tetrahydrocannabinolic acid in Cannabis sativa L. with hyperspectral coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Garbacik, Erik T; Korai, Roza P; Frater, Eric H; Korterik, Jeroen P; Otto, Cees; Offerhaus, Herman L

    2013-04-01

    Nature has developed many pathways to produce medicinal products of extraordinary potency and specificity with significantly higher efficiencies than current synthetic methods can achieve. Identification of these mechanisms and their precise locations within plants could substantially increase the yield of a number of natural pharmaceutics. We report label-free imaging of Δ⁹-tetrahydrocannabinolic acid (THCa) in Cannabis sativa L. using coherent anti-Stokes Raman scattering microscopy. In line with previous observations we find high concentrations of THCa in pistillate flowering bodies and relatively low amounts within flowering bracts. Surprisingly, we find differences in the local morphologies of the THCa-containing bodies: organelles within bracts are large, diffuse, and spheroidal, whereas in pistillate flowers they are generally compact, dense, and have heterogeneous structures. We have also identified two distinct vibrational signatures associated with THCa, both in pure crystalline form and within Cannabis plants; at present the exact natures of these spectra remain an open question.

  15. Hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering at flame temperatures using a second-harmonic bandwidth-compressed probe.

    PubMed

    Kearney, Sean P; Scoglietti, Daniel J

    2013-03-15

    We demonstrate an approach for picosecond probe-beam generation that enables hybrid femtosecond/picosecond pure-rotational coherent anti-Stokes Raman scattering (CARS) measurements in flames. Sum-frequency generation of bandwidth-compressed picosecond radiation from femtosecond pumps with phase-conjugate chirps provides probe pulses with energies in excess of 1 mJ that are temporally locked to the femtosecond pump/Stokes preparation. This method overcomes previous limitations on hybrid femtosecond/picosecond rotational CARS techniques, which have relied upon less efficient bandwidth-reduction processes that have generally resulted in prohibitively low probe energy for flame measurements. We provide the details of the second-harmonic approach and demonstrate the technique in near-adiabatic hydrogen/air flames.

  16. Hyperspectral imaging and characterization of live cells by broadband coherent anti-Stokes Raman scattering (CARS) microscopy with singular value decomposition (SVD) analysis.

    PubMed

    Khmaladze, Alexander; Jasensky, Joshua; Price, Erika; Zhang, Chi; Boughton, Andrew; Han, Xiaofeng; Seeley, Emily; Liu, Xinran; Banaszak Holl, Mark M; Chen, Zhan

    2014-01-01

    Coherent anti-Stokes Raman scattering (CARS) microscopy can be used as a powerful imaging technique to identify chemical compositions of complex samples in biology, biophysics, medicine, and materials science. In this work we developed a CARS microscopic system capable of hyperspectral imaging. By employing an ultrafast laser source, a photonic crystal fiber, and a scanning laser microscope together with spectral detection by a highly sensitive back-illuminated cooled charge-coupled device (CCD) camera, we were able to rapidly acquire and process hyperspectral images of live cells with chemical selectivity. We discuss various aspects of hyperspectral CARS image analysis and demonstrate the use of singular value decomposition methods to characterize the cellular lipid content.

  17. Experimental comparison of single-shot broadband vibrational and dual-broadband pure rotational coherent anti-Stokes Raman scattering in hot air.

    PubMed

    Seeger, T; Leipertz, A

    1996-05-20

    Broadband vibrational and dual-broadband pure rotational coherent anti-Stokes Raman scattering (CARS) have been compared in a high-temperature oven, in which the accuracy and single-shot precision of gas temperature and relative O(2)- and N(2)-concentration measurements in hot air were probed over a temperature range that is typical for many combustion processes. To ensure a realistic comparison, we used nearly the same experimental setup for both CARS techniques. Besides temperature information, dual-broadband pure rotational CARS offers the possibility of achieving simultaneous single-shot concentration measurements. The comparison shows that this technique also has significant advantages in temperature evaluation over a large temperature range in comparison with vibrational CARS.

  18. Laser sources for Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Kilmer, J.; Iadevaia, A.; Yin, Y.

    2011-06-01

    While conventional Raman Spectroscopy (RS) has predominately used fixed wavelength cw lasers, advanced Raman spectroscopic techniques such as Stimulated Raman and some types of Raman Imaging typically need pulsed lasers with sufficient energy to induce the Raman process. In addition, pulsed lasers are beneficial for the following Raman techniques: Time Resolved Raman (TRR), Resonance Raman (RR), or non linear Raman techniques, such as Coherent anti-Stokes Raman spectroscopy (CARS). Here the naturally narrower linewidth of a ns pulse width laser is advantageous to a broader linewidth ultrafast pulsed laser. In this paper, we report on the development of a compact, highly efficient, high power solid-state Ti: Sapphire laser ideally suited for many Raman spectroscopic techniques. This laser produces nanosecond pulses at kHz repetition rates with a tunable output wavelength from ~1 micron to ~200 nm and pulse energies up to 1 mJ. The narrow bandwidth of this laser (<0.1cm-1) is ideally suited for applications such as Laser-induced fluorescence (LIF) measurement of OH free-radicals concentrations, atmospheric LIDAR and Raman spectroscopy. New KBBF and RBBF deep ultraviolet (DUV) and vacuum ultraviolet (VUV) crystals are now available that enable direct doubling of the SHG output of these tunable Ti: Sapphire lasers to directly achieve wavelengths as short as 175 nm without the need to generate the 3rd harmonic and utilize frequency mixing. This results in a highly efficient output in the DUV/VUV, enabling improved signal to noise ratios (S/N) in these previously difficult wavelength regions. Photonics Industries has recently achieved a few mW of power at 193nm with such direct doubling crystals.

  19. Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Gleeson, Helen F.

    Raman spectroscopy has been used as a tool to study liquid crystals for several decades. There are several features that make Raman spectroscopy an important characterisation method. It is bond-specific, so can provide information about the interaction of liquid crystals with colloidal systems and can offer an insight into phase transitions. The polarization dependence of the scattering can be used to determine order parameters in liquid crystal systems. Finally, the relatively high spatial resolution of the technique (∽1 μm) can be used to explore spatiallydependent order in soft matter systems. This chapter describes the most important ways in which Raman spectroscopy can be used to reveal information about liquid crystal systems, illustrated by examples. Both the theoretical background and experimental considerations are described, providing a comprehensive introduction to anybody interested in using the technique to understand liquid crystal systems.

  20. New topics in coherent anti-stokes raman scattering gas-phase diagnostics : femtosecond rotational CARS and electric-field measurements.

    SciTech Connect

    Lempert, Walter R.; Barnat, Edward V.; Kearney, Sean Patrick; Serrano, Justin Raymond

    2010-07-01

    We discuss two recent diagnostic-development efforts in our laboratory: femtosecond pure-rotational Coherent anti-Stokes Raman scattering (CARS) for thermometry and species detection in nitrogen and air, and nanosecond vibrational CARS measurements of electric fields in air. Transient pure-rotational fs-CARS data show the evolution of the rotational Raman polarization in nitrogen and air over the first 20 ps after impulsive pump/Stokes excitation. The Raman-resonant signal strength at long time delays is large, and we additionally observe large time separation between the fs-CARS signatures of nitrogen and oxygen, so that the pure-rotational approach to fs-CARS has promise for simultaneous species and temperature measurements with suppressed nonresonant background. Nanosecond vibrational CARS of nitrogen for electric-field measurements is also demonstrated. In the presence of an electric field, a dipole is induced in the otherwise nonpolar nitrogen molecule, which can be probed with the introduction of strong collinear pump and Stokes fields, resulting in CARS signal radiation in the infrared. The electric-field diagnostic is demonstrated in air, where the strength of the coherent infrared emission and sensitivity our field measurements is quantified, and the scaling of the infrared signal with field strength is verified.

  1. Scanning near-field optical coherent anti-Stokes Raman microscopy (SNOM-CARS) with femtosecond laser pulses in vibrational and electronic resonance.

    PubMed

    Namboodiri, Mahesh; Khan, Tahir Zeb; Bom, Sidhant; Flachenecker, Günter; Materny, Arnulf

    2013-01-14

    Accessing ultrafast photoinduced molecular dynamics on a femtosecond time-scale with vibrational selectivity and at the same time sub-diffraction limited spatial resolution would help to gain important information about ultrafast processes in nanostructures. While nonlinear Raman techniques have been used to obtain highly resolved images in combination with near-field microscopy, the use of femtosecond laser pulses in electronic resonance still constitutes a big challenge. Here, we present our first results on coherent anti-Stokes Raman scattering (fs-CARS) with femtosecond laser pulses detected in the near-field using scanning near-field optical microscopy (SNOM). We demonstrate that highly spatially resolved images can be obtained from poly(3-hexylthiophene) (P3HT) nano-structures where the fs-CARS process was in resonance with the P3HT absorption and with characteristic P3HT vibrational modes without destruction of the samples. Sub-diffraction limited lateral resolution is achieved. Especially the height resolution clearly surpasses that obtained with standard microCARS. These results will be the basis for future investigations of mode-selective dynamics in the near field.

  2. Protein expression guided chemical profiling of living cells by the simultaneous observation of Raman scattering and anti-Stokes fluorescence emission

    PubMed Central

    Chiu, Liang-da; Ichimura, Taro; Sekiya, Takumasa; Machiyama, Hiroaki; Watanabe, Tomonobu; Fujita, Hideaki; Ozawa, Takeaki; Fujita, Katsumasa

    2017-01-01

    Our current understanding of molecular biology provides a clear picture of how the genome, transcriptome and proteome regulate each other, but how the chemical environment of the cell plays a role in cellular regulation remains much to be studied. Here we show an imaging method using hybrid fluorescence-Raman microscopy that measures the chemical micro-environment associated with protein expression patterns in a living cell. Simultaneous detection of fluorescence and Raman signals, realised by spectrally separating the two modes through the single photon anti-Stokes fluorescence emission of fluorescent proteins, enables the accurate correlation of the chemical fingerprint of a specimen to its physiological state. Subsequent experiments revealed the slight chemical differences that enabled the chemical profiling of mouse embryonic stem cells with and without Oct4 expression. Furthermore, using the fluorescent probe as localisation guide, we successfully analysed the detailed chemical content of cell nucleus and Golgi body. The technique can be further applied to a wide range of biomedical studies for the better understanding of chemical events during biological processes. PMID:28272392

  3. Real-time imaging of laser-induced membrane disruption of a living cell observed with multifocus coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Minamikawa, Takeo; Niioka, Hirohiko; Araki, Tsutomu; Hashimoto, Mamoru

    2011-02-01

    We demonstrate the real-time imaging of laser-induced disruption of the cellular membrane in a living HeLa cell and its cellular response with a multifocus coherent anti-Stokes Raman scattering (CARS) microscope. A near-infrared pulsed laser beam tightly focused on the cellular membrane of a living cell induces ablation at the focal point causing a local disruption of the cellular membrane. After the membrane disruption a dark spot decreasing CARS intensity of 2840 cm(-1) Raman shift at the disrupted site appears. This dark spot immediately disappears and a strong CARS signal is observed around the disrupted site. This increase of the CARS signal might be caused by resealing of the disrupted site via aggregation of the patch lipid vesicles in the cytoplasm. The accumulation of lipids around the disrupted site is also confirmed with three-dimensional CARS images of a cell before and after membrane disruption. The temporal behavior of the CARS signal at the disrupted site is observed to detect the fusion dynamics of patch vesicles.

  4. Implementation of a Coherent Anti-Stokes Raman Scattering (CARS) System on a Ti:Sapphire and OPO Laser Based Standard Laser Scanning Microscope.

    PubMed

    Mytskaniuk, Vasyl; Bardin, Fabrice; Boukhaddaoui, Hassan; Rigneault, Herve; Tricaud, Nicolas

    2016-07-17

    Laser scanning microscopes combining a femtosecond Ti:sapphire laser and an optical parametric oscillator (OPO) to duplicate the laser line have become available for biologists. These systems are primarily designed for multi-channel two-photon fluorescence microscopy. However, without any modification, complementary non-linear optical microscopy such as second-harmonic generation (SHG) or third harmonic generation (THG) can also be performed with this set-up, allowing label-free imaging of structured molecules or aqueous medium-lipid interfaces. These techniques are well suited for in-vivo observation, but are limited in chemical specificity. Chemically selective imaging can be obtained from inherent vibration signals based on Raman scattering. Confocal Raman microscopy provides 3D spatial resolution, but it requires high average power and long acquisition time. To overcome these difficulties, recent advances in laser technology have permitted the development of nonlinear optical vibrational microscopy, in particular coherent anti-Stokes Raman scattering (CARS). CARS microscopy has therefore emerged as a powerful tool for biological and live cell imaging, by chemically mapping lipids (via C-H stretch vibration), water (via O-H stretch vibrations), proteins or DNA. In this work, we describe the implementation of the CARS technique on a standard OPO-coupled multiphoton laser scanning microscope. It is based on the in-time synchronization of the two laser lines by adjusting the length of one of the laser beam path. We present a step-by-step implementation of this technique on an existing multiphoton system. A basic background in experimental optics is helpful and the presented system does not require expensive supplementary equipment. We also illustrate CARS imaging obtained on myelin sheaths of sciatic nerve of rodent, and we show that this imaging can be performed simultaneously with other nonlinear optical imaging, such as standard two-photon fluorescence technique

  5. Dispersion of the resonant nonlinear optical susceptibility obtained with femtosecond time-domain coherent anti-Stokes Raman scattering.

    PubMed

    Yang, Shan; Ganikhanov, Feruz

    2013-11-15

    We propose and experimentally demonstrate a method that is capable of resolving both real and imaginary parts of third-order nonlinearity (χ(3)) in the vicinity of Raman resonances. Dispersion of χ(3) can be obtained from a medium probed within microscopic volumes with a spectral resolution of better than 0.10 cm(-1).

  6. Engineering of phase matching for mid-infrared coherent anti-Stokes Raman wavelength conversion with orthogonally polarized pump and Stokes waves in silicon-on-sapphire waveguides.

    PubMed

    Wang, Zhaolu; Liu, Hongjun; Huang, Nan; Sun, Qibing; Li, Xuefeng

    2013-11-20

    The conversion efficiency of mid-infrared wavelength conversion based on coherent anti-Stokes Raman scattering with TE-polarized pump and TM-polarized Stokes waves is theoretically investigated in silicon-on-sapphire (SOS) waveguides. The peak conversion efficiency of -10  dB is obtained when the linear propagation loss is 1  dB/cm at Δk=0; however, it is reduced to -13.6  dB when the linear propagation loss is 2  dB/cm. The phase matching for wavelength conversion with orthogonally polarized pump and Stokes waves can be realized by engineering the birefringence in SOS waveguides, because proper phase mismatch induced by birefringence together with material dispersion-induced phase mismatch can counteract the large phase mismatch induced by waveguide dispersion. Moreover, compared with the phase matching for identically polarized pump and Stokes waves, the phase matching for orthogonally polarized pump and Stokes waves can be realized in a SOS waveguide with much smaller cross section, which reduces the power requirement for optical systems.

  7. Label-free imaging of Drosophila in vivo by coherent anti-Stokes Raman scattering and two-photon excitation autofluorescence microscopy

    NASA Astrophysics Data System (ADS)

    Chien, Cheng-Hao; Chen, Wei-Wen; Wu, June-Tai; Chang, Ta-Chau

    2011-01-01

    Drosophila is one of the most valuable model organisms for studying genetics and developmental biology. The fat body in Drosophila, which is analogous to the liver and adipose tissue in human, stores lipids that act as an energy source during its development. At the early stages of metamorphosis, the fat body remodeling occurs involving the dissociation of the fat body into individual fat cells. Here we introduce a combination of coherent anti-Stokes Raman scattering (CARS) and two-photon excitation autofluorescence (TPE-F) microscopy to achieve label-free imaging of Drosophila in vivo at larval and pupal stages. The strong CARS signal from lipids allows direct imaging of the larval fat body and pupal fat cells. In addition, the use of TPE-F microscopy allows the observation of other internal organs in the larva and autofluorescent globules in fat cells. During the dissociation of the fat body, the findings of the degradation of lipid droplets and an increase in autofluorescent globules indicate the consumption of lipids and the recruitment of proteins in fat cells. Through in vivo imaging and direct monitoring, CARS microscopy may help elucidate how metamorphosis is regulated and study the lipid metabolism in Drosophila.

  8. Longitudinal, 3D in vivo imaging of sebaceous glands by coherent anti-Stokes Raman scattering microscopy –normal function and response to cryotherapy

    PubMed Central

    Jung, Yookyung; Tam, Joshua; Jalian, H. Ray; Anderson, R. Rox; Evans, Conor L.

    2014-01-01

    Sebaceous glands perform complex functions, and are centrally involved in the pathogenesis of acne vulgaris. Current techniques for studying sebaceous glands are mostly static in nature, whereas the gland’s main function – excretion of sebum via the holocrine mechanism – can only be evaluated over time. We present a longitudinal, real-time alternative – the in vivo, label-free imaging of sebaceous glands using Coherent Anti-Stokes Raman Scattering (CARS) microscopy, which is used to selectively visualize lipids. In mouse ears, CARS microscopy revealed dynamic changes in sebaceous glands during the holocrine secretion process, as well as in response to damage to the glands caused by cooling. Detailed gland structure, plus the active migration of individual sebocytes and cohorts of sebocytes were measured. Cooling produced characteristic changes in sebocyte structure and migration. This study demonstrates that CARS microscopy is a promising tool for studying the sebaceous gland and its associated disorders in three-dimensions in vivo. PMID:25026458

  9. 1-kHz two-dimensional coherent anti-Stokes Raman scattering (2D-CARS) for gas-phase thermometry.

    PubMed

    Miller, Joseph D; Slipchenko, Mikhail N; Mance, Jason G; Roy, Sukesh; Gord, James R

    2016-10-31

    Two-dimensional gas-phase coherent anti-Stokes Raman scattering (2D-CARS) thermometry is demonstrated at 1 kHz in a heated jet. A hybrid femtosecond/picosecond CARS configuration is used in a two-beam phase-matching arrangement with a 100-femtosecond pump/Stokes pulse and a 107-picosecond probe pulse. The femtosecond pulse is generated using a mode-locked oscillator and regenerative amplifier that is synchronized to a separate picosecond oscillator and burst-mode amplifier. The CARS signal is spectrally dispersed in a custom imaging spectrometer and detected using a high-speed camera with image intensifier. 1-kHz, single-shot planar measurements at room temperature exhibit error of 2.6% and shot-to-shot variations of 2.6%. The spatial variation in measured temperature is 9.4%. 2D-CARS temperature measurements are demonstrated in a heated O2 jet to capture the spatiotemporal evolution of the temperature field.

  10. Multimodal coherent anti-Stokes Raman scattering microscopy reveals microglia-associated myelin and axonal dysfunction in multiple sclerosis-like lesions in mice

    NASA Astrophysics Data System (ADS)

    Imitola, Jaime; Côté, Daniel; Rasmussen, Stine; Xie, X. Sunney; Liu, Yingru; Chitnis, Tanuja; Sidman, Richard L.; Lin, Charles. P.; Khoury, Samia J.

    2011-02-01

    Myelin loss and axonal degeneration predominate in many neurological disorders; however, methods to visualize them simultaneously in live tissue are unavailable. We describe a new imaging strategy combining video rate reflectance and fluorescence confocal imaging with coherent anti-Stokes Raman scattering (CARS) microscopy tuned to CH2 vibration of myelin lipids, applied in live tissue of animals with chronic experimental autoimmune encephalomyelitis (EAE). Our method allows monitoring over time of demyelination and neurodegeneration in brain slices with high spatial resolution and signal-to-noise ratio. Local areas of severe loss of lipid signal indicative of demyelination and loss of the reflectance signal from axons were seen in the corpus callosum and spinal cord of EAE animals. Even in myelinated areas of EAE mice, the intensity of myelin lipid signals is significantly reduced. Using heterozygous knock-in mice in which green fluorescent protein replaces the CX3CR1 coding sequence that labels central nervous system microglia, we find areas of activated microglia colocalized with areas of altered reflectance and CARS signals reflecting axonal injury and demyelination. Our data demonstrate the use of multimodal CARS microscopy for characterization of demyelinating and neurodegenerative pathology in a mouse model of multiple sclerosis, and further confirm the critical role of microglia in chronic inflammatory neurodegeneration.

  11. Impact of refractive index mismatches on coherent anti-Stokes Raman scattering and multiphoton autofluorescence tomography of human skin in vivo.

    PubMed

    Weinigel, M; Breunig, H G; Darvin, M E; Klemp, M; Röwert-Huber, J; Lademann, J; König, K

    2015-09-07

    Optical non-linear multimodal tomography is a powerful diagnostic imaging tool to analyse human skin based on its autofluorescence and second-harmonic generation signals. Recently, the field of clinical non-linear imaging has been extended by adding coherent anti-Stokes Raman scattering (CARS)-a further optical sectioning method for the detection of non-fluorescent molecules. However, the heterogeneity of refractive indices of different substances in complex tissues like human skin can have a strong influence on CARS image formation and requires careful clinical interpretation of the detected signals. Interestingly, very regular patterns are present in the CARS images, which have no correspondence to the morphology revealed by autofluorescence at the same depth. The purpose of this paper is to clarify this phenomenon and to sensitize users for possible artefacts. A further part of this paper is the detailed comparison of CARS and autofluorescence images of healthy human skin in vivo covering the complete epidermis and part of the upper dermis by employing the flexible medical non-linear tomograph MPTflex CARS.

  12. A dynamic, cytoplasmic triacylglycerol pool in enterocytes revealed by ex vivo and in vivo coherent anti-Stokes Raman scattering imagings⃞

    PubMed Central

    Zhu, Jiabin; Lee, Bonggi; Buhman, Kimberly K.; Cheng, Ji-Xin

    2009-01-01

    The absorptive cells of the small intestine, enterocytes, are not generally thought of as a cell type that stores triacylglycerols (TGs) in cytoplasmic lipid droplets (LDs). We revisit TG metabolism in enterocytes by ex vivo and in vivo coherent anti-Stokes Raman scattering (CARS) imaging of small intestine of mice during dietary fat absorption (DFA). We directly visualized the presence of LDs in enterocytes. We determined lipid amount and quantified LD number and size as a function of intestinal location and time post-lipid challenge via gavage feeding. The LDs were confirmed to be primarily TG by biochemical analysis. Combined CARS and fluorescence imaging indicated that the large LDs were located in the cytoplasm, associated with the tail-interacting protein of 47 kDa. Furthermore, in vivo CARS imaging showed real-time variation in the amount of TG stored in LDs through the process of DFA. Our results highlight a dynamic, cytoplasmic TG pool in enterocytes that may play previously unexpected roles in processes, such as regulating postprandial blood TG concentrations. PMID:19218555

  13. Multimodal coherent anti-Stokes Raman scattering microscopy reveals microglia-associated myelin and axonal dysfunction in multiple sclerosis-like lesions in mice

    PubMed Central

    Imitola, Jaime; Côté, Daniel; Rasmussen, Stine; Xie, X. Sunney; Liu, Yingru; Chitnis, Tanuja; Sidman, Richard L.; Lin, Charles. P.; Khoury, Samia J.

    2011-01-01

    Myelin loss and axonal degeneration predominate in many neurological disorders; however, methods to visualize them simultaneously in live tissue are unavailable. We describe a new imaging strategy combining video rate reflectance and fluorescence confocal imaging with coherent anti-Stokes Raman scattering (CARS) microscopy tuned to CH2 vibration of myelin lipids, applied in live tissue of animals with chronic experimental autoimmune encephalomyelitis (EAE). Our method allows monitoring over time of demyelination and neurodegeneration in brain slices with high spatial resolution and signal-to-noise ratio. Local areas of severe loss of lipid signal indicative of demyelination and loss of the reflectance signal from axons were seen in the corpus callosum and spinal cord of EAE animals. Even in myelinated areas of EAE mice, the intensity of myelin lipid signals is significantly reduced. Using heterozygous knock-in mice in which green fluorescent protein replaces the CX3CR1 coding sequence that labels central nervous system microglia, we find areas of activated microglia colocalized with areas of altered reflectance and CARS signals reflecting axonal injury and demyelination. Our data demonstrate the use of multimodal CARS microscopy for characterization of demyelinating and neurodegenerative pathology in a mouse model of multiple sclerosis, and further confirm the critical role of microglia in chronic inflammatory neurodegeneration. PMID:21361672

  14. Single-shot gas-phase thermometry using pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering.

    PubMed

    Miller, Joseph D; Roy, Sukesh; Slipchenko, Mikhail N; Gord, James R; Meyer, Terrence R

    2011-08-01

    High-repetition-rate, single-laser-shot measurements are important for the investigation of unsteady flows where temperature and species concentrations can vary significantly. Here, we demonstrate single-shot, pure-rotational, hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps RCARS) thermometry based on a kHz-rate fs laser source. Interferences that can affect nanosecond (ns) and ps CARS, such as nonresonant background and collisional dephasing, are eliminated by selecting an appropriate time delay between the 100-fs pump/Stokes pulses and the pulse-shaped 8.4-ps probe. A time- and frequency-domain theoretical model is introduced to account for rotational-level dependent collisional dephasing and indicates that the optimal probe-pulse time delay is 13.5 ps to 30 ps. This time delay allows for uncorrected best-fit N2-RCARS temperature measurements with ~1% accuracy. Hence, the hybrid fs/ps RCARS approach can be performed with kHz-rate laser sources while avoiding corrections that can be difficult to predict in unsteady flows.

  15. Single-shot gas-phase thermometry using pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering

    NASA Astrophysics Data System (ADS)

    Miller, Joseph D.; Roy, Sukesh; Slipchenko, Mikhail N.; Gord, James R.; Meyer, Terrence R.

    2011-08-01

    High-repetition-rate, single-laser-shot measurements are important for the investigation of unsteady flows where temperature and species concentrations can vary significantly. Here, we demonstrate single-shot, pure-rotational, hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps RCARS) thermometry based on a kHz-rate fs laser source. Interferences that can affect nanosecond (ns) and ps CARS, such as nonresonant background and collisional dephasing, are eliminated by selecting an appropriate time delay between the 100-fs pump/Stokes pulses and the pulse-shaped 8.4-ps probe. A time- and frequency-domain theoretical model is introduced to account for rotational-level dependent collisional dephasing and indicates that the optimal probe-pulse time delay is 13.5 ps to 30 ps. This time delay allows for uncorrected best-fit N2-RCARS temperature measurements with ~1% accuracy. Hence, the hybrid fs/ps RCARS approach can be performed with kHz-rate laser sources while avoiding corrections that can be difficult to predict in unsteady flows.

  16. Coherent anti-Stokes Raman scattering microscope with a high-signal-to-noise ratio, high stability, and high-speed imaging for live cell observation

    NASA Astrophysics Data System (ADS)

    Hayashi, Shinichi; Takimoto, Shinichi; Hashimoto, Takeshi

    2007-02-01

    Coherent anti-Stokes Raman scattering (CARS) microscopy, which can produce images of specific molecules without staining, has attracted the attention of researchers, as it matches the need for molecular imaging and pathway analysis of live cells. In particular, there have been an increasing number of CARS experimental results regarding lipids in live cells, which cannot be fluorescently tagged while keeping the cells alive. One of the important applications of lipid research is for the metabolic syndrome. Since the metabolic syndrome is said to be related to the lipids in lipocytes, blood, arterial vessels, and so on, the CARS technique is expected to find application in this field. However, CARS microscopy requires a pair of picosecond laser pulses, which overlap both temporally and spatially. This makes the optical adjustments of a CARS microscope challenging. The authors developed a CARS unit that includes optics for easy and stable adjustment of the overlap of these laser pulses. Adding the CARS unit to a laser scanning microscope provides CARS images of a high signal-to-noise ratio, with an acquisition rate as high as 2 microseconds per pixel. Thus, images of fast-moving lipid droplets in Hela cells were obtained.

  17. Lipid droplet pattern and nondroplet-like structure in two fat mutants of Caenorhabditis elegans revealed by coherent anti-Stokes Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Yi, Yung-Hsiang; Chien, Cheng-Hao; Chen, Wei-Wen; Ma, Tian-Hsiang; Liu, Kuan-Yu; Chang, Yu-Sun; Chang, Ta-Chau; Lo, Szecheng J.

    2014-01-01

    Lipid is an important energy source and essential component for plasma and organelle membranes in all kinds of cells. Coherent anti-Stokes Raman scattering (CARS) microscopy is a label-free and nonlinear optical technique that can be used to monitor the lipid distribution in live organisms. Here, we utilize CARS microscopy to investigate the pattern of lipid droplets in two live Caenorhabditis elegans mutants (fat-2 and fat-3). The CARS images showed a striking decrease in the size, number, and content of lipid droplets in the fat-2 mutant but a slight difference in the fat-3 mutant as compared with the wild-type worm. Moreover, a nondroplet-like structure with enhanced CARS signal was detected for the first time in the uterus of fat-2 and fat-3 mutants. In addition, transgenic fat-2 mutant expressing a GFP fusion protein of vitellogenin-2 (a yolk lipoprotein) revealed that the enhanced CARS signal colocalized with the GFP signal, which suggests that the nondroplet-like structure is primarily due to the accumulation of yolk lipoproteins. Together, this study implies that CARS microscopy is a potential tool to study the distribution of yolk lipoproteins, in addition to lipid droplets, in live animals.

  18. Raman spectroscopy

    SciTech Connect

    Gerrard, D.L.; Bowley, H.J.

    1988-06-15

    The period of this review is from late 1985 to late 1987. During this time over 6000 papers have been published in the scientific literature dealing with many applications of Raman spectroscopy and extending its use to new areas of study. This article covers only those papers that are relevant to the analytical chemist and this necessitates a highly selective approach. There are some areas that have been the subject of many papers with relatively few being of analytical interest. In such cases the reader is referred to appropriate reviews which are detailed in this section.

  19. Near-resonance enhanced O2 detection for dual-broadband pure rotational coherent anti-Stokes Raman scattering with an ultraviolet-visible setup at 266 nm

    SciTech Connect

    Schenk, Martin; Seeger, Thomas; Leipertz, Alfred

    2005-07-01

    Broadband and dual-broadband coherent anti-Stokes Raman scattering (CARS) are widely established tools for nonintrusive gas diagnostics. Up to now the investigations have been mainly performed for electronic nonresonant conditions of the gas species of interest. We report on the enhancement of the O2-N2 detection limit of dual-broadband pure rotational CARS by shifting the wavelength of the narrowband pump laser from the commonly used 532-266 nm. This enhancement is caused when the Schumann-Runge absorption band is approached near 176 nm. The principal concept of this experiment, i.e., covering the Raman resonance with a single- or dual-broadband combination of lasers in the visible range and moving only the narrowband probe laser near or directly into electronic resonant conditions in the UV range, should also be applicable to broadband CARS experiments to directly exploit electronic resonance effects for the purpose of single-shot concentration measurements of minority species. To quantify the enhancement in O2 sensitivity, comparative measurements at both a 266 and a 532 nm narrowband pump laser wavelength are presented, employing a 4-dicyanomethylene-2-methyl-6-(p-dimethylaminostyryl)-4H-pyram (DCM) dye laser as a broadband laser source at 635 nm. An increase of approximately 13% in the ratio of the rotational CARS cross sections of O2 and N2 was obtained. The broad spectral width of the CARS excitation profile was approximately equal for both setups. Further enhancement should be achievable by shifting the narrowband pump laser closer toward 176 nm, for example, with a frequency-doubled optical parametric oscillator or an excimer laser. The principal concept of this experiment should also be applicable to broadband CARS experiments to directly exploit electronic resonance effects of the narrowband pump laser with electronic transitions of minority species for the purpose of single-shot concentration measurements of those species.

  20. Raman Spectroscopy Of Glass-Crystalline Transformations

    NASA Astrophysics Data System (ADS)

    Haro, E.; Balkanski, M.

    1988-01-01

    Glass-crystalline transition is induced by laser irradiation on a GeSe bulk glass sample. The structural changes are detected by Raman spectroscopy. The speed of the crystallization process depends on the laser irradiation intensity. We have studied this crystallization process for three different powers of irradiation. It is found that the speed of crystallization increases with power. Stokes and anti-Stokes spectra were recorded during the transformation. From this data temperature was inferred at different stages of crystallization. The significance of this temperature is discussed.

  1. Application of a high power Yb fiber-based laser compatible with commercial optical parametric oscillator for coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Hage, Charles-Henri; Boisset, Simon; Ibrahim, Ali; Morin, Franck; Hoenninger, Clemens; Grunske, Tobias; Souissi, Sami; Heliot, Laurent; Leray, Aymeric

    2014-06-01

    Coherent anti-Stokes Raman scattering (CARS) microscopy is a powerful tool for chemical analysis at a subcellular level, frequently used for imaging lipid dynamics in living cells. We report a high-power picosecond fiber-based laser and its application for optical parametric oscillator (OPO) pumping and CARS microscopy. This fiber-based laser has been carefully characterized. It produces 5 ps pulses with 0.8 nm spectral width at a 1,030 nm wavelength with more than 10 W of average power at 80 MHz repetition rate; these spectral and temporal properties can be slightly modified. We then study the influence of these modifications on the spectral and temporal properties of the OPO. We find that the OPO system generates a weakly spectrally chirped signal beam constituted of 3 ps pulses with 0.4 nm spectral width tunable from 790 to 930 nm optimal for CARS imaging. The frequency doubling unconverted part is composed of 7-8 ps pulses with 0.75 nm spectral width compatible with CARS imaging. We also study the influence of the fiber laser properties on the CARS signal generated by distilled water. In agreement with theory, we find that shorter temporal pulses allow higher peak powers and thus higher CARS signal, if the spectral widths are less than 10 cm(-1) . We demonstrate that this source is suitable for performing CARS imaging of living cells during several hours without photodamages. We finally demonstrate CARS imaging on more complex aquatic organisms called copepods (micro-crustaceans), on which we distinguish morphological details and lipid reserves.

  2. Time- and frequency-dependent model of time-resolved coherent anti-Stokes Raman scattering (CARS) with a picosecond-duration probe pulse.

    PubMed

    Stauffer, Hans U; Miller, Joseph D; Slipchenko, Mikhail N; Meyer, Terrence R; Prince, Benjamin D; Roy, Sukesh; Gord, James R

    2014-01-14

    The hybrid femtosecond∕picosecond coherent anti-Stokes Raman scattering (fs∕ps CARS) technique presents a promising alternative to either fs time-resolved or ps frequency-resolved CARS in both gas-phase thermometry and condensed-phase excited-state dynamics applications. A theoretical description of time-dependent CARS is used to examine this recently developed probe technique, and quantitative comparisons of the full time-frequency evolution show excellent accuracy in predicting the experimental vibrational CARS spectra obtained for two model systems. The interrelated time- and frequency-domain spectral signatures of gas-phase species produced by hybrid fs∕ps CARS are explored with a focus on gas-phase N2 vibrational CARS, which is commonly used as a thermometric diagnostic of combusting flows. In particular, we discuss the merits of the simple top-hat spectral filter typically used to generate the ps-duration hybrid fs∕ps CARS probe pulse, including strong discrimination against non-resonant background that often contaminates CARS signal. It is further demonstrated, via comparison with vibrational CARS results on a time-evolving solvated organic chromophore, that this top-hat probe-pulse configuration can provide improved spectral resolution, although the degree of improvement depends on the dephasing timescales of the observed molecular modes and the duration and timing of the narrowband final pulse. Additionally, we discuss the virtues of a frequency-domain Lorentzian probe-pulse lineshape and its potential for improving the hybrid fs∕ps CARS technique as a diagnostic in high-pressure gas-phase thermometry applications.

  3. Gas phase temperature measurements in the liquid and particle regime of a flame spray pyrolysis process using O2-based pure rotational coherent anti-Stokes Raman scattering.

    PubMed

    Engel, Sascha R; Koegler, Andreas F; Gao, Yi; Kilian, Daniel; Voigt, Michael; Seeger, Thomas; Peukert, Wolfgang; Leipertz, Alfred

    2012-09-01

    For the production of oxide nanoparticles at a commercial scale, flame spray processes are frequently used where mostly oxygen is fed to the flame if high combustion temperatures and thus small primary particle sizes are desired. To improve the understanding of these complex processes in situ, noninvasive optical measurement techniques were applied to characterize the extremely turbulent and unsteady combustion field at those positions where the particles are formed from precursor containing organic solvent droplets. This particle-forming regime was identified by laser-induced breakdown detection. The gas phase temperatures in the surrounding of droplets and particles were measured with O(2)-based pure rotational coherent anti-Stokes Raman scattering (CARS). Pure rotational CARS measurements benefit from a polarization filtering technique that is essential in particle and droplet environments for acquiring CARS spectra suitable for temperature fitting. Due to different signal disturbing processes only the minority of the collected signals could be used for temperature evaluation. The selection of these suitable signals is one of the major problems to be solved for a reliable evaluation process. Applying these filtering and signal selection steps temperature measurements have successfully been conducted. Time-resolved, single-pulse measurements exhibit temperatures between near-room and combustion temperatures due to the strongly fluctuating and flickering behavior of the particle-generating flame. The mean flame temperatures determined from the single-pulse data are decreasing with increasing particle concentrations. They indicate the dissipation of large amounts of energy from the surrounding gas phase in the presence of particles.

  4. Time- and frequency-dependent model of time-resolved coherent anti-Stokes Raman scattering (CARS) with a picosecond-duration probe pulse

    NASA Astrophysics Data System (ADS)

    Stauffer, Hans U.; Miller, Joseph D.; Slipchenko, Mikhail N.; Meyer, Terrence R.; Prince, Benjamin D.; Roy, Sukesh; Gord, James R.

    2014-01-01

    The hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) technique presents a promising alternative to either fs time-resolved or ps frequency-resolved CARS in both gas-phase thermometry and condensed-phase excited-state dynamics applications. A theoretical description of time-dependent CARS is used to examine this recently developed probe technique, and quantitative comparisons of the full time-frequency evolution show excellent accuracy in predicting the experimental vibrational CARS spectra obtained for two model systems. The interrelated time- and frequency-domain spectral signatures of gas-phase species produced by hybrid fs/ps CARS are explored with a focus on gas-phase N2 vibrational CARS, which is commonly used as a thermometric diagnostic of combusting flows. In particular, we discuss the merits of the simple top-hat spectral filter typically used to generate the ps-duration hybrid fs/ps CARS probe pulse, including strong discrimination against non-resonant background that often contaminates CARS signal. It is further demonstrated, via comparison with vibrational CARS results on a time-evolving solvated organic chromophore, that this top-hat probe-pulse configuration can provide improved spectral resolution, although the degree of improvement depends on the dephasing timescales of the observed molecular modes and the duration and timing of the narrowband final pulse. Additionally, we discuss the virtues of a frequency-domain Lorentzian probe-pulse lineshape and its potential for improving the hybrid fs/ps CARS technique as a diagnostic in high-pressure gas-phase thermometry applications.

  5. Fiber bundle based endomicroscopy prototype with two collection channels for simultaneous coherent anti-Stokes Raman scattering and second harmonic generation imaging

    NASA Astrophysics Data System (ADS)

    Liu, Zhengfan; Satira, Zachary A.; Wang, Xi; Xu, Xiaoyun; Chen, Xu; Wong, Kelvin; Chen, Shufen; Xin, Jianguo; Wong, Stephen T. C.

    2014-02-01

    Label-free multiphoton imaging is promising for replacing biopsy and could offer new strategies for intraoperative or surgical applications. Coherent anti-Stokes Raman scattering (CARS) imaging could provide lipid-band contrast, and second harmonic generation (SHG) imaging is useful for imaging collagen, tendon and muscle fibers. A combination of these two imaging modalities could provide rich information and this combination has been studied by researchers to investigate diseases through microscopy imaging. The combination of these two imaging modalities in endomicroscopy imaging has been rarely investigated. In this research, a fiber bundle consisted of one excitation fiber and 18 collection fibers was developed in our endomicroscopy prototype. The 18 collection fibers were divided into two collection channels with 9 fibers in each channel. These two channels could be used together as one channel for effective signal collection or used separately for simplifying detection part of the system. Differences of collection pattern of these two channels were investigated. Collection difference of central excitation fiber and surrounding 18 fibers was also investigated, which reveals the potential ability of this system to measure forward to backward (F/B) ratio in SHG imaging. CARS imaging of mouse adipocyte and SHG imaging of mouse tail tendon were performed to demonstrate the CARS and SHG tissue imaging performance of this system. Simultaneous CARS and SHG imaging ability of this system was demonstrated by mouse tail imaging. This fiber bundle based endomicroscopy imaging prototype, offers a promising platform for constructing efficient fiber-based CARS and SHG multimodal endomicroscopes for label free intraoperative imaging applications.

  6. Picosecond anti-Stokes generation in a photonic-crystal fiber for interferometric CARS microscopy.

    PubMed

    Andresen, Esben Ravn; Keiding, Søren Rud; Potma, Eric Olaf

    2006-08-07

    We generate tunable picosecond anti-Stokes pulses by four-wave mixing of two picosecond pump and Stokes pulse trains in a photonic-crystal fiber. The visible, spectrally narrow anti-Stokes pulses with shifts over 150 nm are generated without generating other spectral features. As a demonstration, we employ the generated anti-Stokes pulses as reference pulses in an interferometric coherent anti-Stokes Raman scattering imaging experiment showing that interpulse coherence among the pump, Stokes and anti-Stokes beams is retained.

  7. Coherent anti-Stokes Raman scattering for quantitative temperature and concentration measurements in a high-pressure gas turbine combustor rig

    NASA Astrophysics Data System (ADS)

    Thariyan, Mathew Paul

    Dual-pump coherent anti-Stokes Raman scattering (DP-CARS) temperature and major species (CO2/N2) concentration measurements have been performed in an optically-accessible high-pressure gas turbine combustor facility (GTCF) and for partially-premixed and non-premixed flames in a laminar counter-flow burner. A window assembly incorporating pairs of thin and thick fused silica windows on three sides was designed, fabricated, and assembled in the GTCF for advanced laser diagnostic studies. An injection-seeded optical parametric oscillator (OPO) was used as a narrowband pump laser source in the dual-pump CARS system. Large prisms on computer-controlled translation stages were used to direct the CARS beams either into the main optics leg for measurements in the GTCF or to a reference optics leg for measurements of the nonresonant CARS spectrum and for aligning the CARS system. Combusting flows were stabilized with liquid fuel injection only for the central injector of a 9-element lean direct injection (LDI) device developed at NASA Glenn Research Center. The combustor was operated using Jet A fuel at inlet air temperatures up to 725 K and combustor pressures up to 1.03 MPa. Single-shot DP-CARS spectra were analyzed using the Sandia CARSFT code in the batch operation mode to yield instantaneous temperature and CO2/N2 concentration ratio values. Spatial maps of mean and standard deviations of temperature and CO2/N2 concentrations were obtained in the high-pressure LDI flames by translating the CARS probe volume in axial and vertical directions inside the combustor rig. The mean temperature fields demonstrate the effect of the combustor conditions on the overall flame length and the average flame structure. The temperature relative standard deviation values indicate thermal fluctuations due to the presence of recirculation zones and/or flame brush fluctuations. The correlation between the temperature and relative CO 2 concentration data has been studied at various combustor

  8. Spontaneous transient ultrafast coherent raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Meiselman, Seth

    I explore the application of Transient Coherent Ultrafast Phonon Spectroscopy (TCUPS) to the measurement of vibrational coherence dynamics of liquid alcohols. The demonstrated technique is complementary to and, in some cases, simpler than traditional stimulated spectroscopy techniques in that it does not require more than one laser and is free of non-resonant background. I demonstrate coherence measurements of single-photon-level collective excitations: a single vibrational state at 1033 (1/cm) in; a pair of simultaneous excited vibrational states at 2834 and 2944 (1/cm) in methanol; and three simultaneous excited states at 2885, ˜2930, and 2976 (1/cm) in isopropanol. I develop a Fourier-transform-based analysis of the TCUPS data that overcomes poor signal-to-noise ratio and signal degradation due to etaloning and fluorescence. The coherence lifetimes and oscillation frequencies agree with frequency-domain line-shape measurements and femtosecond Coherent anti-Stokes Raman Scattering (CARS) measurements.

  9. Measurement of the surface-enhanced coherent anti-Stokes Raman scattering (SECARS) due to the 1574 cm(-1) surface-enhanced Raman scattering (SERS) mode of benzenethiol using low-power (<20 mW) CW diode lasers.

    PubMed

    Aggarwal, Roshan L; Farrar, Lewis W; Greeneltch, Nathan G; Van Duyne, Richard P; Polla, Dennis L

    2013-02-01

    The surface-enhanced coherent anti-Stokes Raman scattering (SECARS) from a self-assembled monolayer (SAM) of benzenethiol on a silver-coated surface-enhanced Raman scattering (SERS) substrate has been measured for the 1574 cm(-1) SERS mode. A value of 9.6 ± 1.7×10(-14) W was determined for the resonant component of the SECARS signal using 17.8 mW of 784.9 nm pump laser power and 7.1 mW of 895.5 nm Stokes laser power; the pump and Stokes lasers were polarized parallel to each other but perpendicular to the grooves of the diffraction grating in the spectrometer. The measured value of resonant component of the SECARS signal is in agreement with the calculated value of 9.3×10(-14) W using the measured value of 8.7 ± 0.5 cm(-1) for the SERS linewidth Γ (full width at half-maximum) and the value of 5.7 ± 1.4×10(-7) for the product of the Raman cross section σSERS and the surface concentration Ns of the benzenethiol SAM. The xxxx component of the resonant part of the third-order nonlinear optical susceptibility |3 χxxxx((3)R)| for the 1574 cm(-1) SERS mode has been determined to be 4.3 ± 1.1×10(-5) cm·g(-1)·s(2). The SERS enhancement factor for the 1574 cm(-1) mode was determined to be 3.6 ± 0.9×10(7) using the value of 1.8×10(15) molecules/cm(2) for Ns.

  10. Electric Field in a Plasma Channel in a High-Pressure Nanosecond Discharge in Hydrogen: A Coherent Anti-Stokes Raman Scattering Study

    NASA Astrophysics Data System (ADS)

    Yatom, S.; Tskhai, S.; Krasik, Ya. E.

    2013-12-01

    Experimental results of a study of the electric field in a plasma channel produced during nanosecond discharge at a H2 gas pressure of (2-3)×105 Pa by the coherent anti-Stokes scattering method are reported. The discharge was ignited by applying a voltage pulse with an amplitude of ˜100 kV and a duration of ˜5 ns to a blade cathode placed at a distance of 10 and 20 mm from the anode. It was shown that this type of gas discharge is characterized by the presence of an electric field in the plasma channel with root-mean-square intensities of up to 30 kV/cm. Using polarization measurements, it was found that the direction of the electric field is along the cathode-anode axis.

  11. The many facets of Raman spectroscopy for biomedical analysis.

    PubMed

    Krafft, Christoph; Popp, Jürgen

    2015-01-01

    A critical review is presented on the use of linear and nonlinear Raman microspectroscopy in biomedical diagnostics of bacteria, cells, and tissues. This contribution is combined with an overview of the achievements of our research group. Linear Raman spectroscopy offers a wealth of chemical and molecular information. Its routine clinical application poses a challenge due to relatively weak signal intensities and confounding overlapping effects. Nonlinear variants of Raman spectroscopy such as coherent anti-Stokes Raman scattering (CARS) and stimulated Raman scattering (SRS) have been recognized as tools for rapid image acquisition. Imaging applications benefit from the fact that contrast is based on the chemical composition and molecular structures in a label-free and nondestructive manner. Although not label-free, surface enhanced Raman scattering (SERS) has also been recognized as a complementary biomedical tool to increase sensitivity. The current state of the art is evaluated, illustrative examples are given, future developments are pointed out, and important reviews and references from the current literature are selected. The topics are identification of bacteria and single cells, imaging of single cells, Raman activated cell sorting, diagnosis of tissue sections, fiber optic Raman spectroscopy, and progress in coherent Raman scattering in tissue diagnosis. The roles of networks-such as Raman4clinics and CLIRSPEC on a European level-and early adopters in the translation, dissemination, and validation of new methods are discussed.

  12. THz-Raman: accessing molecular structure with Raman spectroscopy for enhanced chemical identification, analysis, and monitoring

    NASA Astrophysics Data System (ADS)

    Heyler, Randy A.; Carriere, James T. A.; Havermeyer, Frank

    2013-05-01

    Structural analysis via spectroscopic measurement of rotational and vibrational modes is of increasing interest for many applications, since these spectra can reveal unique and important structural and behavioral information about a wide range of materials. However these modes correspond to very low frequency (~5cm-1 - 200cm-1, or 150 GHz-6 THz) emissions, which have been traditionally difficult and/or expensive to access through conventional Raman and Terahertz spectroscopy techniques. We report on a new, inexpensive, and highly efficient approach to gathering ultra-low-frequency Stokes and anti-Stokes Raman spectra (referred to as "THz-Raman") on a broad range of materials, opening potential new applications and analytical tools for chemical and trace detection, identification, and forensics analysis. Results are presented on explosives, pharmaceuticals, and common elements that show strong THz-Raman spectra, leading to clear discrimination of polymorphs, and improved sensitivity and reliability for chemical identification.

  13. Noise autocorrelation spectroscopy with coherent Raman scattering

    NASA Astrophysics Data System (ADS)

    Xu, Xiaoji G.; Konorov, Stanislav O.; Hepburn, John W.; Milner, Valery

    2008-02-01

    Coherent anti-Stokes Raman scattering (CARS) with femtosecond laser pulses has become a widespread method in nonlinear optical spectroscopy and microscopy. As a third-order nonlinear process, femtosecond CARS exhibits high efficiency at low average laser power. High sensitivity to molecular structure enables detection of small quantities of complex molecules and non-invasive biological imaging. Temporal and spectral resolution of CARS is typically limited by the duration of the excitation pulses and their frequency bandwidth, respectively. Broadband femtosecond pulses are advantageous for time-resolved CARS spectroscopy, but offer poor spectral resolution. The latter can be improved by invoking optical or quantum interference at the expense of increasing complexity of instrumentation and susceptibility to noise. Here, we present a new approach to coherent Raman spectroscopy in which high resolution is achieved by means of deliberately introduced noise. The proposed method combines the efficiency of a coherent process with the robustness of incoherent light. It does require averaging over different noise realizations, but no temporal scanning or spectral pulse shaping as commonly used by frequency-resolved spectroscopic methods with ultrashort pulses.

  14. High-resolution inverse Raman and resonant-wave-mixing spectroscopy

    SciTech Connect

    Rahn, L.A.

    1993-12-01

    These research activities consist of high-resolution inverse Raman spectroscopy (IRS) and resonant wave-mixing spectroscopy to support the development of nonlinear-optical techniques for temperature and concentration measurements in combustion research. Objectives of this work include development of spectral models of important molecular species needed to perform coherent anti-Stokes Raman spectroscopy (CARS) measurements and the investigation of new nonlinear-optical processes as potential diagnostic techniques. Some of the techniques being investigated include frequency-degenerate and nearly frequency-degenerate resonant four-wave-mixing (DFWM and NDFWM), and resonant multi-wave mixing (RMWM).

  15. Comparison of Raman Scattering Methods for Combustion Dynamics Measurements.

    DTIC Science & Technology

    1982-10-01

    CM PENNEY, and S WARSHAW F49620-77-C-0094 S. PERFORMING ORGANIZATION NAME AND ADDRESS 10. PROGRAM ELEMENT. PROJECT, TASK GENERAL ELECTRIC CO. AREA...OPTICAL DIAGNOSTICS RAMAN SCATTERING LUMINOSITY TEMPERATURE CARS (CO!ERENT ANTI-STOKES SOOT DENSITY RAMAN SPECTROSCOPY) 20. ABSTRACT (Continue an...OF THIS PA*E (SMn .. L.. # SMCUWITY CLASIFICATION OF THIS PAOC(3Wsm Datae. CARS (coherent anti-Stokes Raman spect~9sopy!) to Aiimp),q, f.0U*5. l and

  16. Optimizing the Laser-Pulse Configuration for Coherent Raman Spectroscopy

    NASA Astrophysics Data System (ADS)

    Pestov, Dmitry; Murawski, Robert K.; Ariunbold, Gombojav O.; Wang, Xi; Zhi, Miaochan; Sokolov, Alexei V.; Sautenkov, Vladimir A.; Rostovtsev, Yuri V.; Dogariu, Arthur; Huang, Yu; Scully, Marlan O.

    2007-04-01

    We introduce a hybrid technique that combines the robustness of frequency-resolved coherent anti-Stokes Raman scattering (CARS) with the advantages of time-resolved CARS spectroscopy. Instantaneous coherent broadband excitation of several characteristic molecular vibrations and the subsequent probing of these vibrations by an optimally shaped time-delayed narrowband laser pulse help to suppress the nonresonant background and to retrieve the species-specific signal. We used this technique for coherent Raman spectroscopy of sodium dipicolinate powder, which is similar to calcium dipicolinate (a marker molecule for bacterial endospores, such as Bacillus subtilis and Bacillus anthracis), and we demonstrated a rapid and highly specific detection scheme that works even in the presence of multiple scattering.

  17. Optimizing the laser-pulse configuration for coherent Raman spectroscopy.

    PubMed

    Pestov, Dmitry; Murawski, Robert K; Ariunbold, Gombojav O; Wang, Xi; Zhi, Miaochan; Sokolov, Alexei V; Sautenkov, Vladimir A; Rostovtsev, Yuri V; Dogariu, Arthur; Huang, Yu; Scully, Marlan O

    2007-04-13

    We introduce a hybrid technique that combines the robustness of frequency-resolved coherent anti-Stokes Raman scattering (CARS) with the advantages of time-resolved CARS spectroscopy. Instantaneous coherent broadband excitation of several characteristic molecular vibrations and the subsequent probing of these vibrations by an optimally shaped time-delayed narrowband laser pulse help to suppress the nonresonant background and to retrieve the species-specific signal. We used this technique for coherent Raman spectroscopy of sodium dipicolinate powder, which is similar to calcium dipicolinate (a marker molecule for bacterial endospores, such as Bacillus subtilis and Bacillus anthracis), and we demonstrated a rapid and highly specific detection scheme that works even in the presence of multiple scattering.

  18. In vivo second-harmonic generation and ex vivo coherent anti-stokes raman scattering microscopy to study the effect of obesity to fibroblast cell function using an Yb-fiber laser-based CARS extension unit.

    PubMed

    Haluszka, Dóra; Lőrincz, Kende; Molnár, Gábor; Tamás, Gábor; Kolonics, Attila; Szipőcs, Róbert; Kárpáti, Sarolta; Wikonkál, Norbert M

    2015-09-01

    Nonlinear microscopy techniques are being increasingly used to perform in vivo studies in dermatology. These methods enable us to investigate the morphology and monitor the physiological process in the skin by the use of femtosecond lasers operating in the red, near-infrared spectral range (680-1,300 nm). In this work we used two different techniques that require no labeling: second harmonic generation (SHG) for collagen detection and coherent anti-Stokes Raman scattering (CARS) to assess lipid distribution in genetically obese murine skin. Obesity is one of the most serious public health problems due to its high and increasing prevalence and the associated risk of type 2 diabetes and cardiovascular diseases. Other than these diseases, nearly half of patients with diabetes mellitus suffer from dermatological complications such as delayed wound healing, foot ulcers and several other skin changes. In our experiment we investigated and followed the effects of obesity on dermal collagen alterations and adipocyte enlargement using a technique not reported in the literature so far. Our results indicate that the in vivo SHG and ex vivo CARS imaging technique might be an important tool for diagnosis of diabetes-related skin disorders in the near future.

  19. Raman spectroscopy in astrobiology.

    PubMed

    Jorge Villar, Susana E; Edwards, Howell G M

    2006-01-01

    Raman spectroscopy is proposed as a valuable analytical technique for planetary exploration because it is sensitive to organic and inorganic compounds and able to unambiguously identify key spectral markers in a mixture of biological and geological components; furthermore, sample manipulation is not required and any size of sample can be studied without chemical or mechanical pretreatment. NASA and ESA are considering the adoption of miniaturised Raman spectrometers for inclusion in suites of analytical instrumentation to be placed on robotic landers on Mars in the near future to search for extinct or extant life signals. In this paper we review the advantages and limitations of Raman spectroscopy for the analysis of complex specimens with relevance to the detection of bio- and geomarkers in extremophilic organisms which are considered to be terrestrial analogues of possible extraterrestial life that could have developed on planetary surfaces.

  20. Hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering temperature and concentration measurements using two different picosecond-duration probes.

    PubMed

    Kearney, Sean P; Scoglietti, Daniel J; Kliewer, Christopher J

    2013-05-20

    A hybrid fs/ps pure-rotational CARS scheme is characterized in furnace-heated air at temperatures from 290 to 800 K. Impulsive femtosecond excitation is used to prepare a rotational Raman coherence that is probed with a ps-duration beam generated from an initially broadband fs pulse that is bandwidth limited using air-spaced Fabry-Perot etalons. CARS spectra are generated using 1.5- and 7.0-ps duration probe beams with corresponding coarse and narrow spectral widths. The spectra are fitted using a simple phenomenological model for both shot-averaged and single-shot measurements of temperature and oxygen mole fraction. Our single-shot temperature measurements exhibit high levels of precision and accuracy when the spectrally coarse 1.5-ps probe beam is used, demonstrating that high spectral resolution is not required for thermometry. An initial assessment of concentration measurements in air is also provided, with best results obtained using the higher resolution 7.0-ps probe. This systematic assessment of the hybrid CARS technique demonstrates its utility for practical application in low-temperature gas-phase systems.

  1. Collisional excitation of CO by H2O - An astrophysicist's guide to obtaining rate constants from coherent anti-Stokes Raman line shape data

    NASA Technical Reports Server (NTRS)

    Green, Sheldon

    1993-01-01

    Rate constants for excitation of CO by collisions with H2O are needed to understand recent observations of comet spectra. These collision rates are closely related to spectral line shape parameters, especially those for Raman Q-branch spectra. Because such spectra have become quite important for thermometry applications, much effort has been invested in understanding this process. Although it is not generally possible to extract state-to-state rate constants directly from the data as there are too many unknowns, if the matrix of state-to-state rates can be expressed in terms of a rate-law model which depends only on rotational quantum numbers plus a few parameters, the parameters can be determined from the data; this has been done with some success for many systems, especially those relevant to combustion processes. Although such an analysis has not yet been done for CO-H2O, this system is expected to behave similarly to N2-H2O which has been well studies; modifications of parameters for the latter system are suggested which should provide a reasonable description of rate constants for the former.

  2. Low wavenumber Raman spectroscopy using atomic filters (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Xue, Xiaobo; Janisch, Corey; Chen, Yizhu; Liu, Zhiwen; Chen, Jingbiao

    2016-10-01

    Low-wavenumber Raman spectroscopy has long been demonstrated as a method of optical characterization in a variety of applications, such as thermal detection and semiconductor analysis. However, accessing low-wavenumber Raman shifts remains a challenge, usually requiring an expensive and complex multi-stage spectrographic system to measure several cm-1 Raman shifts. In this work, we demonstrate a method to measure low-wavenumber Raman shifts down to 1 cm-1 using atomic filters. By using a narrow-band Faraday anomalous dispersion optical filter to remove spontaneous emission noise from the laser cavity and a heated atomic cell as a notch filter to remove the excitation laser, the system is able to measure low Raman shifts (down to 1 cm-1). To demonstrate the capabilities, we measure the broadband Raman spectrum from a silica optical fiber with approximately 0.3 cm-1 resolution, detecting both Stokes and Anti-Stokes Raman shift as low as 0.7 cm-1.

  3. Molecule-surface interactions probed by optimized surface-enhanced coherent Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Voronine, Dmitri; Sinyukov, Alexander; Hua, Xia; Zhang, Guowan; Yang, Wenlong; Wang, Kai; Jha, Pankaj; Welch, George; Sokolov, Alexei; Scully, Marlan

    2012-06-01

    Nanoscale molecular sensing is carried out using a time-resolved coherent anti-Stokes Raman scattering (CARS) spectroscopy with optimized laser pulse configurations. This novel technique combines the advantages of an improved spectral resolution, suppressed non-resonant background and near-field surface enhancement of the Raman signal. We detect two species of pyridine in a vicinity of aggregated gold nanoparticles and measure their vibrational dephasing times which reveal the effects of surface environment and molecule-surface interactions on the ultrafast molecular dynamics. This technique may be applied to a variety of artificial and biological systems and complex molecular mixtures and has a potential for nanophotonic sensing applications.

  4. Pure electrical, highly-efficient and sidelobe free coherent Raman spectroscopy using acousto-optics tunable filter (AOTF)

    NASA Astrophysics Data System (ADS)

    Meng, Zhaokai; Petrov, Georgi I.; Yakovlev, Vladislav V.

    2016-02-01

    Fast and sensitive Raman spectroscopy measurements are imperative for a large number of applications in biomedical imaging, remote sensing and material characterization. Stimulated Raman spectroscopy offers a substantial improvement in the signal-to-noise ratio but is often limited to a discrete number of wavelengths. In this report, by introducing an electronically-tunable acousto-optical filter as a wavelength selector, a novel approach to a broadband stimulated Raman spectroscopy is demonstrated. The corresponding Raman shift covers the spectral range from 600 cm‑1 to 4500 cm‑1, sufficient for probing most vibrational Raman transitions. We validated the use of the new instrumentation to both coherent anti-Stokes scattering (CARS) and stimulated Raman scattering (SRS) spectroscopies.

  5. Pure electrical, highly-efficient and sidelobe free coherent Raman spectroscopy using acousto-optics tunable filter (AOTF).

    PubMed

    Meng, Zhaokai; Petrov, Georgi I; Yakovlev, Vladislav V

    2016-02-01

    Fast and sensitive Raman spectroscopy measurements are imperative for a large number of applications in biomedical imaging, remote sensing and material characterization. Stimulated Raman spectroscopy offers a substantial improvement in the signal-to-noise ratio but is often limited to a discrete number of wavelengths. In this report, by introducing an electronically-tunable acousto-optical filter as a wavelength selector, a novel approach to a broadband stimulated Raman spectroscopy is demonstrated. The corresponding Raman shift covers the spectral range from 600 cm(-1) to 4500 cm(-1), sufficient for probing most vibrational Raman transitions. We validated the use of the new instrumentation to both coherent anti-Stokes scattering (CARS) and stimulated Raman scattering (SRS) spectroscopies.

  6. Resonance Raman spectroscopy.

    PubMed

    Robert, Bruno

    2009-01-01

    Resonance Raman spectroscopy may yield precise information on the conformation of, and on the interactions assumed by, the chromophores involved in the first steps of the photosynthetic process, whether isolated in solvents, embedded in soluble or membrane proteins, or, as shown recently, in vivo. By making use of this technique, it is possible, for instance, to relate the electronic properties of these molecules to their structure and/or the physical properties of their environment, or to determine subtle changes of their conformation associated with regulatory processes. After a short introduction to the physical principles that govern resonance Raman spectroscopy, the information content of resonance Raman spectra of chlorophyll and carotenoid molecules is described in this review, together with the experiments which helped in determining which structural parameter each Raman band is sensitive to. A selection of applications of this technique is then presented, in order to give a fair and precise idea of which type of information can be obtained from its use in the field of photosynthesis.

  7. Picosecond Pump-Probe Raman Spectroscopy of Excited States and Relaxation Phenomena in the Condensed Phase.

    NASA Astrophysics Data System (ADS)

    Lingle, Robert, Jr.

    This dissertation describes the development and application of pump-probe Raman spectroscopy using 8 ps laser pulses as a technique for the study of relaxation phenomena in the condensed phase. I show three examples of systems studied by this technique. First, the dissipation of the heat deposited in the cage of solvent molecules surrounding a photodissociated diatomic solute is directly measured in the solvent Raman spectrum. Second, we provide a full characterization of the excited A^ ' state of iodine which is formed in solution following photodissociation. This work discusses the solvent dependence of the iodine atom recombination process and points toward (iodine atom-solvent molecule) complexes as an intermediate species leading to recombination on the A^' state. We measure and rationalize the rates for both vibrational relaxation within and electronic relaxation out of the A^ ' state. Turning to a laser system, we measure the chromophore-to-protein vibrational relaxation time in deoxyhemoglobin. We learn that mechanical energy finds its way out of the heme and into the protein matrix with 2 to 5 ps exponential time constant. Both the study of iodine and deoxyhemoglobin emphasize that measuring the dynamics of the Stokes and anti-Stokes transient Raman signals provides a direct and powerful method to study vibrational population relaxation. Raman spectra are directly sensitive to vibrational level spacings and populations. As a result, Raman bands dynamics can be affected by electronic, vibrational, and conformational processes. Most previous Raman picosecond experiments have lacked the sensitivity necessary to probe the weak, transient anti-Stokes spectrum, which provides invaluable information on vibrational population dynamics. We also use a subtraction procedure to isolate the transient features in the spectrum, making our spectra taken at kiloHertz repetition rates very sensitive to small changes in the spectrum. This enables us to compare directly the

  8. Investigation of Optical Fibers for Coherent Anti-Stokes Raman Scattering (CARS) Spectroscopy in Reacting Flows (Postprint)

    DTIC Science & Technology

    2012-03-01

    hydrocar- bon-fueled combustors . 1 Introduction Various nonlinear spectroscopic techniques exist for measuring temperature, velocity, and chemical...CARS signal. Hence, performing state-of-the-art CARS measurements based on free-stand- ing optics in harsh environments such as combustors and gas...practical combustor , with a focal spot diameter of *100 lm and an interaction length of *1.5 mm, it was observed that the optimal energy for a 8- to 10-ns

  9. Gas Diagnostic Measurements by Coherent Anti-Stokes Raman Spectroscopy: Feasibility Calculations for Water Vapor in Combustion Systems.

    DTIC Science & Technology

    1980-06-01

    L. St. Peters and M. Lapp, J. of the Optical Society of America, 64, 712 (1974) along with the theory of Ref. 25. 24. Gerhard Herzberg , Molecular...Research Center, (United Technologies Research Center report R79-954390-8, East Hartford, CT, 1979). 37. Gerhard Herzberg , Molecular Spectra and

  10. THz-Raman spectroscopy for explosives, chemical, and biological detection

    NASA Astrophysics Data System (ADS)

    Carriere, James T. A.; Havermeyer, Frank; Heyler, Randy A.

    2013-05-01

    Raman and Terahertz spectroscopy are both widely used for their ability to safely and remotely identify unknown materials. Each approach has its advantages and disadvantages. Traditional Raman spectroscopy typically measures molecular energy transitions in the 200-5000cm-1 region corresponding to sub-molecular stretching or bending transitions, while Terahertz spectroscopy measures molecular energy transitions in the 1-200cm-1 region (30GHz - 6THz) that correspond to low energy rotational modes or vibrational modes of the entire molecule. Many difficult to detect explosives and other hazardous chemicals are known to have multiple relatively strong transitions in this "Terahertz" (<200cm-1, <6THz) regime, suggesting this method as a powerful complementary approach for identification. However, THz signal generation is often expensive, many THz spectroscopy systems are limited to just a few THz range, and strong water absorption bands in this region can act to mask certain transitions if great care isn't taken during sample preparation. Alternatively, low-frequency or "THz-Raman" spectroscopy, which covers the ~5cm-1 to 200cm-1 (150GHz - 6 THz) regions and beyond, offers a powerful, compact and economical alternative to probe these low energy transitions. We present results from a new approach for extending the range of Raman spectroscopy into the Terahertz regime using an ultra-narrow-band volume holographic grating (VHG) based notch filter system. An integrated, compact Raman system is demonstrated utilizing a single stage spectrometer to show both Stokes and anti-Stokes measurements down to <10cm-1 on traditionally difficult to detect explosives, as well as other chemical and biological samples.

  11. Tip-enhanced THz Raman spectroscopy for local temperature determination at the nanoscale.

    PubMed

    Balois, Maria Vanessa; Hayazawa, Norihiko; Catalan, Francesca Celine; Kawata, Satoshi; Yano, Taka-Aki; Hayashi, Tomohiro

    2015-11-01

    Local temperature of a nanoscale volume is precisely determined by tip-enhanced terahertz Raman spectroscopy in the low temperature range of several tens of degrees. Heat generated by the tip-enhanced electric field is directly transferred to single-walled carbon nanotubes by heat conduction and radiation at the nanoscale. This heating modulates the intensity ratio of anti-Stokes/Stokes Raman scattering of the radial breathing mode of the carbon nanotube based on the Boltzmann distribution at elevated temperatures. Owing to the low-energy feature of the radial breathing mode, the local temperature of the probing volume has been successfully extracted with high sensitivity. The dependence of the temperature rise underneath the tip apex on the incident power coincides with the analytical results calculated by finite element method based on the tip enhancement effect and the consequent steady-state temperature via Joule heat generation. The results show that the local temperature at the nanoscale can be controlled in the low temperature range simply by the incident laser power while exhibiting a sufficiently high tip enhancement effect as an analytical tool for thermally sensitive materials (e.g., proteins, DNA). Graphical Abstract Tip-enhanced THz Raman spectroscopy detects the low frequency Raman mode both in Stokes and anti-Stokes shifts, which precisely reflects the local temperature of the sample volume.

  12. Raman spectroscopy of oral bacteria

    NASA Astrophysics Data System (ADS)

    Berger, Andrew J.; Zhu, Qingyuan; Quivey, Robert G.

    2003-10-01

    Raman spectroscopy has been employed to measure the varying concentrations of two oral bacteria in simple mixtures. Evaporated droplets of centrifuged mixtures of Streptococcus sanguis and Streptococcus mutans were analyzed via Raman microspectroscopy. The concentration of s. sanguis was determined based upon the measured Raman spectrum, using partial least squares cross-validation, with an r2 value of 0.98.

  13. [Improvement of anti-stokes energy transfer between rare earth ions--2. Numerical calculation and analysis].

    PubMed

    Chen, Xiao-bo; Wang, Ce; Kang, Dong-guo; Sawanobori, Naruhito; Wang, Shui-feng; Li, Yong-liang; Wang, Ping

    2010-08-01

    The dynamics of all levels were calculated numerically in the present article for Er(0.5)Yb(3):FOV oxyfluoride nanophase vitroceramics. The population dynamical processes were analyzed carefully. It was found for the first time that traditional phonon-assisted energy transfer theory of rare earth ion energy transfer can not well explain the observed experimental calibrated results, as it does not take into account the difference between Stokes and anti-Stokes process. A coefficient, the improved factor of the intensity ratio of Stokes to anti-Stokes process in quantum Raman theory compared to classical Raman theory, was introduced for the first time to successfully describe the anti-Stokes energy transfer. The theoretical improvement results are coincident with experiments very well. This improvement is very significant and indispensable when the photonics of nanomaterials is probed.

  14. Time-resolved Raman spectroscopy of shock compressed single crystal HMX

    NASA Astrophysics Data System (ADS)

    Scharff, R. J.; Whitley, V. H.; Stahl, D. B.; Dattelbaum, D. M.

    2009-06-01

    Shock initiation of an energetic organic solid is generally considered to proceed via a mechanism through which low frequency acoustic phonons are upconverted to higher frequency bond stretching vibrations in the crystal. To elucidate changes in molecular structure under shock loading, a series of well defined gas gun driven plate impact experiments coupled to time-resolved Raman spectroscopy were performed on single crystal β-HMX. We will also present progress in obtaining temperature measurements in the shocked material using a Stokes/anti-Stokes intensity ratio method.

  15. Nonlinear Raman Techniques in Femtosecond Time Resolved Spectroscopy for the Analysis and Control of Molecular Dynamics

    NASA Astrophysics Data System (ADS)

    Materny, Arnulf; Konradi, Jakow; Namboodiri, Vinu; Namboodiri, Mahesh; Scaria, Abraham

    2008-11-01

    The use of four-wave mixing techniques in femtosecond time-resolved spectroscopy has considerable advantages. Due to the many degrees of freedom offered e.g. by coherent anti-Stokes Raman scattering (CARS), the dynamics even of complex systems can be analyzed in detail. Using pulse shaping techniques in combination with a self-learning loop approach, molecular mode excitation can be controlled very efficiently in a multi-photon excitation process. Results obtained from the optimal control of CARS on β-carotene are discussed.

  16. Nonlinear Raman Techniques in Femtosecond Time Resolved Spectroscopy for the Analysis and Control of Molecular Dynamics

    SciTech Connect

    Materny, Arnulf; Konradi, Jakow; Namboodiri, Vinu; Namboodiri, Mahesh; Scaria, Abraham

    2008-11-14

    The use of four-wave mixing techniques in femtosecond time-resolved spectroscopy has considerable advantages. Due to the many degrees of freedom offered e.g. by coherent anti-Stokes Raman scattering (CARS), the dynamics even of complex systems can be analyzed in detail. Using pulse shaping techniques in combination with a self-learning loop approach, molecular mode excitation can be controlled very efficiently in a multi-photon excitation process. Results obtained from the optimal control of CARS on {beta}-carotene are discussed.

  17. Industrial applications of Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Grasselli, J. G.; Walder, F.; Petty, C.; Kemeny, G.

    1993-03-01

    In the last two decades, Raman spectroscopy has matured as an important method for the study of molecules and complex molecular systems. This is evident from the number of fine texts and the many review articles which have been published describing theory and applications of Raman spectroscopy over a very broad range of subjects (1-10). Raman spectroscopy is the essential partner to infrared spectroscopy for a complete vibrational analysis of a molecule in structure determinations. From the understanding developed on small molecules, theory was extended to interpret the spectra of larger systems such as polymers, biological molecules, and ordered condensed phases. The contribution of Raman spectroscopy to these areas has been significant. It was the development of commercial lasers in the 1960s which spurred the renewed interest in the Raman technique. But applications were still limited for highly fluorescing or intensely colored systems. In 1986, a breakthrough paper by Hirschfeld and Chase (11) described the use of near-infrared laser excitation and a commercial interferometer-based FT-IR spectrometer to record FT-Raman spectra. Significant advantages included the inherent multiplex, throughput and data processing features of the FT interferometers and the use of a ND:YAG laser (1.064 μm) which dramatically decreased problems with sample fluorescence and decomposition. A deluge of papers describing applications of FT-Raman spectroscopy can be found in the Journal of Raman Spectroscopy, Spectrochimica Acta (special issues 40A ad 47A), and Applied Spectroscopy since then.

  18. Femtosecond Stimulated Raman Spectroscopy.

    PubMed

    Dietze, Daniel R; Mathies, Richard A

    2016-05-04

    Femtosecond stimulated Raman spectroscopy (FSRS) is an ultrafast nonlinear optical technique that provides vibrational structural information with high temporal (sub-50 fs) precision and high spectral (10 cm(-1) ) resolution. Since the first full demonstration of its capabilities ≈15 years ago, FSRS has evolved into a mature technique, giving deep insights into chemical and biochemical reaction dynamics that would be inaccessible with any other technique. It is now being routinely applied to virtually all possible photochemical reactions and systems spanning from single molecules in solution to thin films, bulk crystals and macromolecular proteins. This review starts with an historic overview and discusses the theoretical and experimental concepts behind this technology. Emphasis is put on the current state-of-the-art experimental realization and several variations of FSRS that have been developed. The unique capabilities of FSRS are illustrated through a comprehensive presentation of experiments to date followed by prospects.

  19. Broadband coherent Raman spectroscopy running at 24,000 spectra per second

    PubMed Central

    Hashimoto, Kazuki; Takahashi, Megumi; Ideguchi, Takuro; Goda, Keisuke

    2016-01-01

    We present a Fourier-transform coherent anti-Stokes Raman scattering (FT-CARS) spectroscopy technique that achieves broadband CARS measurements at an ultrahigh scan rate of more than 20,000 spectra/s – more than 20 times higher than that of previous broadband coherent Raman scattering spectroscopy techniques. This is made possible by an integration of a FT-CARS system and a rapid-scanning retro-reflective optical path length scanner. To demonstrate the technique’s strength, we use it to perform broadband CARS spectroscopy of the transient mixing dynamics of toluene and benzene in the fingerprint region (200–1500 cm−1) with spectral resolution of 10 cm−1 at a record high scan rate of 24,000 spectra/s. Our rapid-scanning FT-CARS technique holds great promise for studying chemical dynamics and wide-field label-free biomedical imaging. PMID:26875786

  20. Broadband coherent Raman spectroscopy running at 24,000 spectra per second.

    PubMed

    Hashimoto, Kazuki; Takahashi, Megumi; Ideguchi, Takuro; Goda, Keisuke

    2016-02-15

    We present a Fourier-transform coherent anti-Stokes Raman scattering (FT-CARS) spectroscopy technique that achieves broadband CARS measurements at an ultrahigh scan rate of more than 20,000 spectra/s - more than 20 times higher than that of previous broadband coherent Raman scattering spectroscopy techniques. This is made possible by an integration of a FT-CARS system and a rapid-scanning retro-reflective optical path length scanner. To demonstrate the technique's strength, we use it to perform broadband CARS spectroscopy of the transient mixing dynamics of toluene and benzene in the fingerprint region (200-1500 cm(-1)) with spectral resolution of 10 cm(-1) at a record high scan rate of 24,000 spectra/s. Our rapid-scanning FT-CARS technique holds great promise for studying chemical dynamics and wide-field label-free biomedical imaging.

  1. Broadband coherent Raman spectroscopy running at 24,000 spectra per second

    NASA Astrophysics Data System (ADS)

    Hashimoto, Kazuki; Takahashi, Megumi; Ideguchi, Takuro; Goda, Keisuke

    2016-02-01

    We present a Fourier-transform coherent anti-Stokes Raman scattering (FT-CARS) spectroscopy technique that achieves broadband CARS measurements at an ultrahigh scan rate of more than 20,000 spectra/s – more than 20 times higher than that of previous broadband coherent Raman scattering spectroscopy techniques. This is made possible by an integration of a FT-CARS system and a rapid-scanning retro-reflective optical path length scanner. To demonstrate the technique’s strength, we use it to perform broadband CARS spectroscopy of the transient mixing dynamics of toluene and benzene in the fingerprint region (200–1500 cm‑1) with spectral resolution of 10 cm‑1 at a record high scan rate of 24,000 spectra/s. Our rapid-scanning FT-CARS technique holds great promise for studying chemical dynamics and wide-field label-free biomedical imaging.

  2. Tackling field-portable Raman spectroscopy of real world samples

    NASA Astrophysics Data System (ADS)

    Shand, Neil C.

    2008-10-01

    A major challenge confronting first responders, customs authorities and other security-related organisations is the accurate, rapid, and safe identification of potentially hazardous chemicals outside a laboratory environment. Currently, a range of hand portable Raman equipment is commercially available that is low cost and increasingly more sophisticated. These systems are generally based on the 785nm Stokes shifted Raman technique with many using dispersive grating spectrometers. This technique offers a broad range of capabilities including the ability to analyse illicit drugs, explosives, chemical weapons and pre-cursors but still has some fundamental constraints. 'Real world' samples, such as those found at a crime scene, will often not be presented in the most accessible manner. Simple issues such as glass fluorescence can make an otherwise tractable sample impossible to analyse in-situ. A new generation of portable Raman equipment is currently being developed to address these issues. Consideration is given to the use of longer wavelength for fluorescence reduction. Alternative optical designs are being tested to compensate for the signal reduction incurred by moving to longer wavelengths. Furthermore, the use of anti-Stokes spectroscopy is being considered as well as investigating the robustness and portability of traditional Fourier Transform interferometer designs along with future advances in detector technology and ultra small spectrometers.

  3. Probing non-adiabatic conical intersections using absorption, spontaneous Raman, and femtosecond stimulated Raman spectroscopy

    SciTech Connect

    Patuwo, Michael Y.; Lee, Soo-Y.

    2013-12-21

    We present the time-frame calculated photoabsorption spectrum (ABS), spontaneous Raman excitation profile (REP), femtosecond stimulated Raman spectroscopy (FSRS) spectrum, and femtosecond stimulated Raman excitation profile (FSREP) results of a two-mode and three-mode, three-electronic-states model Hamiltonians containing conical intersections (CIs) along its two upper diabatic electronic states, e{sub 1} (dark) and e{sub 2} (bright), with and without coupling (nonadiabatic dynamics) along an asymmetric mode. For every electronic state in each model, there is one coupling mode and the rest of the modes are symmetric tuning modes. The CI appears in the Hamiltonian as off-diagonal entries to the potential term that couple the two upper states, in the form of a linear function of the coupling mode. We show that: (a) the ABS, REP, and FSREP for Stokes and anti-Stokes lines contain similar information about the e{sub 1} and e{sub 2} vibrational bands, (b) the FSRS spectra feature narrow stationary peaks and broader moving peaks contributed by the different resonant components of the third-order polarization terms from perturbation theory, and (c) a relatively strong and narrow stationary band of the allowed first overtone of the asymmetric coupling mode is observed in the Stokes FSREP in the e{sub 1} energy region with coupling to e{sub 2}.

  4. Probing non-adiabatic conical intersections using absorption, spontaneous Raman, and femtosecond stimulated Raman spectroscopy.

    PubMed

    Patuwo, Michael Y; Lee, Soo-Y

    2013-12-21

    We present the time-frame calculated photoabsorption spectrum (ABS), spontaneous Raman excitation profile (REP), femtosecond stimulated Raman spectroscopy (FSRS) spectrum, and femtosecond stimulated Raman excitation profile (FSREP) results of a two-mode and three-mode, three-electronic-states model Hamiltonians containing conical intersections (CIs) along its two upper diabatic electronic states, e1 (dark) and e2 (bright), with and without coupling (nonadiabatic dynamics) along an asymmetric mode. For every electronic state in each model, there is one coupling mode and the rest of the modes are symmetric tuning modes. The CI appears in the Hamiltonian as off-diagonal entries to the potential term that couple the two upper states, in the form of a linear function of the coupling mode. We show that: (a) the ABS, REP, and FSREP for Stokes and anti-Stokes lines contain similar information about the e1 and e2 vibrational bands, (b) the FSRS spectra feature narrow stationary peaks and broader moving peaks contributed by the different resonant components of the third-order polarization terms from perturbation theory, and (c) a relatively strong and narrow stationary band of the allowed first overtone of the asymmetric coupling mode is observed in the Stokes FSREP in the e1 energy region with coupling to e2.

  5. Observation of anomalous Stokes versus anti-Stokes ratio in MoTe2 atomic layers

    NASA Astrophysics Data System (ADS)

    Goldstein, Thomas; Chen, Shao-Yu; Xiao, Di; Ramasubramaniam, Ashwin; Yan, Jun

    We grow hexagonal molybdenum ditelluride (MoTe2), a prototypical transition metal dichalcogenide (TMDC) semiconductor, with chemical vapor transport methods and investigate its atomic layers with Stokes and anti-Stokes Raman scattering. We report observation of all six types of zone center optical phonons. Quite remarkably, the anti-Stokes Raman intensity of the low energy layer-breathing mode becomes more intense than the Stokes peak under certain experimental conditions, creating an illusion of 'negative temperature'. This effect is tunable, and can be switched from anti-Stokes enhancement to suppression by varying the excitation wavelength. We interpret this observation to be a result of resonance effects arising from the C excitons in the vicinity of the Brillouin zone center, which are robust even for multiple layers of MoTe2. The intense anti-Stokes Raman scattering provides a cooling channel for the crystal and opens up opportunities for laser cooling of atomically thin TMDC semiconductor devices. Supported by the University of Massachusetts Amherst, the National Science Foundation Center for Hierarchical Manufacturing (CMMI-1025020) and Office of Emerging Frontiers in Research and Innovation (EFRI-1433496).

  6. Theoretical analysis of anharmonic coupling and cascading Raman signals observed with femtosecond stimulated Raman spectroscopy.

    PubMed

    Mehlenbacher, Randy D; Lyons, Brendon; Wilson, Kristina C; Du, Yong; McCamant, David W

    2009-12-28

    We present a classical theoretical treatment of a two-dimensional Raman spectroscopy based on the initiation of vibrational coherence with an impulsive Raman pump and subsequent probing by two-pulse femtosecond stimulated Raman spectroscopy (FSRS). The classical model offers an intuitive picture of the molecular dynamics initiated by each laser pulse and the generation of the signal field traveling along the probe wave vector. Previous reports have assigned the observed FSRS signals to anharmonic coupling between the impulsively driven vibration and the higher-frequency vibration observed with FSRS. However, we show that the observed signals are not due to anharmonic coupling, which is shown to be a fifth-order coherent Raman process, but instead due to cascades of coherent Raman signals. Specifically, the observed vibrational sidebands are generated by parallel cascades in which a coherent anti-Stokes or Stokes Raman spectroscopy (i.e., CARS or CSRS) field generated by the coherent coupling of the impulsive pump and the Raman pump pulses participates in a third-order FSRS transition. Additional sequential cascades are discussed that will give rise to cascade artifacts at the fundamental FSRS frequencies. It is shown that the intended fifth-order FSRS signals, generated by an anharmonic coupling mechanism, will produce signals of approximately 10(-4) DeltaOD (change in the optical density). The cascading signals, however, will produce stimulated Raman signal of approximately 10(-2) DeltaOD, as has been observed experimentally. Experiments probing deuterochloroform find significant sidebands of the CCl(3) bend, which has an E type symmetry, shifted from the A(1) type C-D and C-Cl stretching modes, despite the fact that third-order anharmonic coupling between these modes is forbidden by symmetry. Experiments probing a 50:50 mixture of chloroform and d-chloroform find equivalent intensity signals of low-frequency CDCl(3) modes as sidebands shifted from both the C

  7. Raman spectroscopy in halophile research

    PubMed Central

    Jehlička, Jan; Oren, Aharon

    2013-01-01

    Raman spectroscopy plays a major role in robust detection of biomolecules and mineral signatures in halophile research. An overview of Raman spectroscopic investigations in halophile research of the last decade is given here to show advantages of the approach, progress made as well as limits of the technique. Raman spectroscopy is an excellent tool to monitor and identify microbial pigments and other biomolecules in extant and extinct halophile biomass. Studies of bottom gypsum crusts from salterns, native evaporitic sediments, halite inclusions, and endoliths as well as cultures of halophilic microorganisms permitted to understand the content, distribution, and behavior of important molecular species. The first papers describing Raman spectroscopic detection of microbiological and geochemical key markers using portable instruments are highlighted as well. PMID:24339823

  8. Raman Spectroscopy and Microscopy of Individual Cells andCellular Components

    SciTech Connect

    Chan, J; Fore, S; Wachsmann-Hogiu, S; Huser, T

    2008-05-15

    Raman spectroscopy provides the unique opportunity to non-destructively analyze chemical concentrations on the submicron length scale in individual cells without the need for optical labels. This enables the rapid assessment of cellular biochemistry inside living cells, and it allows for their continuous analysis to determine cellular response to external events. Here, we review recent developments in the analysis of single cells, subcellular compartments, and chemical imaging based on Raman spectroscopic techniques. Spontaneous Raman spectroscopy provides for the full spectral assessment of cellular biochemistry, while coherent Raman techniques, such as coherent anti-Stokes Raman scattering is primarily used as an imaging tool comparable to confocal fluorescence microscopy. These techniques are complemented by surface-enhanced Raman spectroscopy, which provides higher sensitivity and local specificity, and also extends the techniques to chemical indicators, i.e. pH sensing. We review the strengths and weaknesses of each technique, demonstrate some of their applications and discuss their potential for future research in cell biology and biomedicine.

  9. Laser crater enhanced Raman spectroscopy.

    PubMed

    Lednev, Vasily N; Sdvizhenskii, Pavel A; Grishin, Mikhail Ya; Filippov, Mikhail N; Shchegolikhin, Alexander N; Pershin, Sergey M

    2017-02-01

    Raman signal enhancement by multiple scattering inside laser crater cones was observed for the first time, to the best of our knowledge. Laser crater enhanced Raman spectroscopy (LCERS) yielded a 14-fold increase in the Raman spectra bands due to efficient multiple scattering of laser irradiation within the laser crater walls. The same pulsed Nd:YAG laser (532 nm, 10 ns) was used for both laser crater formation and Raman scattering experiments by varying the output pulse energy. First, powerful pulses are used to produce the laser crater; then low-energy pulses are used to perform Raman scattering measurements. The laser crater profile and its alignment with the laser beam waist were found to be the key parameters for the optimization of the Raman spectrum intensity enhancement. Raman intensity enhancement resulted from increased surface scattering area at the crater walls, rather than spatially offset Raman scattering. The increased signal-to-noise ratio resulted in limits of detection improvement for quantitative analysis using LCERS.

  10. Raman Spectroscopy of Microbial Pigments

    PubMed Central

    Edwards, Howell G. M.; Oren, Aharon

    2014-01-01

    Raman spectroscopy is a rapid nondestructive technique providing spectroscopic and structural information on both organic and inorganic molecular compounds. Extensive applications for the method in the characterization of pigments have been found. Due to the high sensitivity of Raman spectroscopy for the detection of chlorophylls, carotenoids, scytonemin, and a range of other pigments found in the microbial world, it is an excellent technique to monitor the presence of such pigments, both in pure cultures and in environmental samples. Miniaturized portable handheld instruments are available; these instruments can be used to detect pigments in microbiological samples of different types and origins under field conditions. PMID:24682303

  11. Raman spectroscopy of advanced materials.

    PubMed

    Huong, P V

    1996-06-01

    Many micro-structural aspects of advanced materials and the incidence on the physical properties have been elucidated by Raman micro-spectroscopy. The potential of this technique is demonstrated with new materials interesting in both academic and industrial developments: new carbons and diamonds, superconductors, semiconductors, superhards.

  12. Surface-Enhanced Raman Spectroscopy.

    ERIC Educational Resources Information Center

    Garrell, Robin L.

    1989-01-01

    Reviews the basis for the technique and its experimental requirements. Describes a few examples of the analytical problems to which surface-enhanced Raman spectroscopy (SERS) has been and can be applied. Provides a perspective on the current limitations and frontiers in developing SERS as an analytical technique. (MVL)

  13. Method And System For Examining Biological Materials Using Low Power Cw Excitation Raman Spectroscopy.

    DOEpatents

    Alfano, Robert R.; Wang, Wubao

    2003-05-06

    A method and system for examining biological materials using low-power cw excitation Raman spectroscopy. A low-power continuous wave (cw) pump laser beam and a low-power cw Stokes (or anti-Stokes) probe laser beam simultaneously illuminate a biological material and traverse the biological material in collinearity. The pump beam, whose frequency is varied, is used to induce Raman emission from the biological material. The intensity of the probe beam, whose frequency is kept constant, is monitored as it leaves the biological material. When the difference between the pump and probe excitation frequencies is equal to a Raman vibrational mode frequency of the biological material, the weak probe signal becomes amplified by one or more orders of magnitude (typically up to about 10.sup.4 -10.sup.6) due to the Raman emission from the pump beam. In this manner, by monitoring the intensity of the probe beam emitted from the biological material as the pump beam is varied in frequency, one can obtain an excitation Raman spectrum for the biological material tested. The present invention may be applied to in the in vivo and/or in vitro diagnosis of diabetes, heart disease, hepatitis, cancers and other diseases by measuring the characteristic excitation Raman lines of blood glucose, cholesterol, serum glutamic oxalacetic transaminase (SGOT)/serum glutamic pyruvic transaminase (SGPT), tissues and other corresponding Raman-active body constituents, respectively.

  14. Diagnostic Imaging in Flames with Instantaneous Planar Coherent Raman Spectroscopy.

    PubMed

    Bohlin, A; Kliewer, C J

    2014-04-03

    Spatial mapping of temperature and molecular species concentrations is vitally important in studies of gaseous chemically reacting flows. Temperature marks the evolution of heat release and energy transfer, while species concentration gradients provide critical information on mixing and chemical reaction. Coherent anti-Stokes Raman spectroscopy (CARS) was pioneered in measurements of such processes almost 40 years ago and is authoritative in terms of the accuracy and precision it may provide. While a reacting flow is fully characterized in three-dimensional space, a limitation of CARS has been its applicability as a point-wise measurement technique, motivating advancement toward CARS imaging, and attempts have been made considering one-dimensional probing. Here, we report development of two-dimensional CARS, with the first diagnostics of a planar field in a combusting flow within a single laser pulse, resulting in measured isotherms ranging from 450 K up to typical hydrocarbon flame temperatures of about 2000 K with chemical mapping of O2 and N2.

  15. Quantitative fiber-optic Raman spectroscopy for tissue Raman measurements

    NASA Astrophysics Data System (ADS)

    Duraipandian, Shiyamala; Bergholt, Mads; Zheng, Wei; Huang, Zhiwei

    2014-03-01

    Molecular profiling of tissue using near-infrared (NIR) Raman spectroscopy has shown great promise for in vivo detection and prognostication of cancer. The Raman spectra measured from the tissue generally contain fundamental information about the absolute biomolecular concentrations in tissue and its changes associated with disease transformation. However, producing analogues tissue Raman spectra present a great technical challenge. In this preliminary study, we propose a method to ensure the reproducible tissue Raman measurements and validated with the in vivo Raman spectra (n=150) of inner lip acquired using different laser powers (i.e., 30 and 60 mW). A rapid Raman spectroscopy system coupled with a ball-lens fiber-optic Raman probe was utilized for tissue Raman measurements. The investigational results showed that the variations between the spectra measured with different laser powers are almost negligible, facilitating the quantitative analysis of tissue Raman measurements in vivo.

  16. Raman spectroscopy of bone metastasis

    NASA Astrophysics Data System (ADS)

    Esmonde-White, Karen A.; Sottnik, Joseph; Morris, Michael; Keller, Evan

    2012-02-01

    Raman spectroscopy of bone has been used to characterize chemical changes occurring in diseases such as osteoporosis, osteoarthritis and osteomyelitis. Metastasis of cancer into bone causes changes to bone quality that are similar to those observed in osteoporosis, such as decreased bone strength, but with an accelerated timeframe. In particular, osteolytic (bone degrading) lesions in bone metastasis have a marked effect on patient quality of life because of increased risk of fractures, pain, and hypercalcemia. We use Raman spectroscopy to examine bone from two different mouse models of osteolytic bone metastasis. Raman spectroscopy measures physicochemical information which cannot be obtained through standard biochemical and histological measurements. This study was reviewed and approved by the University of Michigan University Committee on the Care and Use of Animals. Two mouse models of prostate cancer bone metastasis, RM1 (n=3) and PC3-luc (n=4) were examined. Tibiae were injected with RM1 or PC3-luc cancer cells, while the contralateral tibiae received a placebo injection for use as controls. After 2 weeks of incubation, the mice were sacrificed and the tibiae were examined by Raman microspectroscopy (λ=785 nm). Spectroscopic markers corresponding to mineral stoichiometry, bone mineralization, and mineral crystallinity were compared in spectra from the cancerous and control tibiae. X-ray imaging of the tibia confirmed extensive osteolysis in the RM1 mice, with tumor invasion into adjoining soft tissue and moderate osteolysis in the PC3-luc mice. Raman spectroscopic markers indicate that osteolytic lesions are less mineralized than normal bone tissue, with an altered mineral stoichiometry and crystallinity.

  17. Plasmon-assisted chemical reactions revealed by high-vacuum tip-enhanced Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Lu, Shuaicheng; Sheng, Shaoxiang; Zhang, Zhenglong; Xu, Hongxing; Zheng, Hairong

    2014-08-01

    Tip-enhanced Raman spectroscopy (TERS) is the technique that combines the nanoscale spatial resolution of a scanning probe microscope and the highly sensitive Raman spectroscopy enhanced by the surface plasmons. It is suitable for chemical analysis at nanometer scale. Recently, TERS exhibited powerful potential in analyzing the chemical reactions at nanoscale. The high sensitivity and spatial resolution of TERS enable us to learn the reaction processes more clearly. More importantly, the chemical reaction in TERS is assisted by surface plasmons, which provides us an optical method to manipulate the chemical reactions at nanoscale. Here using our home-built high-vacuum tip-enhanced Raman spectroscopy (HV-TERS) setup, we successfully observed the plasmon-assisted molecule dimerization and dissociation reactions. In HV-TERS system, under laser illumination, 4-nitrobenzenethiol (4NBT) molecules can be dimerized to p,p'-dimercaptoazobenzene (DMAB), and dissociation reaction occurs for malachite green (MG) molecules. Using our HV-TERS setup, the dynamic processes of the reactions are clearly revealed. The chemical reactions can be manipulated by controlling the plasmon intensity through changing the power of the incident laser, the tunneling current and the bias voltage. We also investigated the role of plasmonic thermal effect in the reactions by measuring both the Stokes and anti- Stokes Raman peaks. Our findings extend the applications of TERS, which can help to study the chemical reactions and understand the dynamic processes at single molecular level, and even design molecules by the plasmon-assisted chemical reactions.

  18. FT-Raman Spectroscopy: A Catalyst for the Raman Explosion?

    ERIC Educational Resources Information Center

    Chase, Bruce

    2007-01-01

    The limitations of Fourier transform (FT) Raman spectroscopy, which is used to detect and analyze the scattered radiation, are discussed. FT-Raman has served to revitalize a field that was lagging and the presence of Raman instrumentation as a routine analytical tool is established for the foreseeable future.

  19. Raman spectroscopy of biomedical polyethylenes.

    PubMed

    Pezzotti, Giuseppe

    2017-03-27

    With the development of three-dimensional Raman algorithms for local mapping of oxidation and plastic strain, and the ability to resolve molecular orientation patterns with microscopic spatial resolution, there is an opportunity to re-examine many of the foundations on which our understanding of biomedical grade ultra-high molecular weight polyethylenes (UHMWPEs) are based. By implementing polarized Raman spectroscopy into an automatized tool with an improved precision in non-destructively resolving Euler angles, oxidation levels, and microscopic strain, we become capable to make accurate and traceable measurements of the in vitro and in vivo tribological responses of a variety of commercially available UHMWPE bearings for artificial hip and knee joints. In this paper, we first review the foundations and the main algorithms for Raman analyses of oxidation and strain of biomedical polyethylene. Then, we critically re-examine a large body of Raman data previously collected on different polyethylene joint components after in vitro testing or in vivo service, in order to shed new light on an area of particular importance to joint orthopedics: the microscopic nature of UHMWPE surface degradation in the human body. A complex scenario of physical chemistry appears from the Raman analyses, which highlights the importance of molecular-scale phenomena besides mere microstructural changes. The availability of the Raman microscopic probe for visualizing oxidation patterns unveiled striking findings related to the chemical contribution to wear degradation: chain-breaking and subsequent formation of carboxylic acid sites preferentially occur in correspondence of third-phase regions, and they are triggered by emission of dehydroxylated oxygen from ceramic oxide counterparts. These findings profoundly differ from more popular (and simplistic) notions of mechanistic tribology adopted in analyzing joint simulator data.

  20. Transcutaneous Raman Spectroscopy of Bone

    NASA Astrophysics Data System (ADS)

    Maher, Jason R.

    Clinical diagnoses of bone health and fracture risk typically rely upon measurements of bone density or structure, but the strength of a bone is also dependent upon its chemical composition. One technology that has been used extensively in ex vivo, exposed-bone studies to measure the chemical composition of bone is Raman spectroscopy. This spectroscopic technique provides chemical information about a sample by probing its molecular vibrations. In the case of bone tissue, Raman spectra provide chemical information about both the inorganic mineral and organic matrix components, which each contribute to bone strength. To explore the relationship between bone strength and chemical composition, our laboratory has contributed to ex vivo, exposed-bone animal studies of rheumatoid arthritis, glucocorticoid-induced osteoporosis, and prolonged lead exposure. All of these studies suggest that Raman-based predictions of biomechanical strength may be more accurate than those produced by the clinically-used parameter of bone mineral density. The utility of Raman spectroscopy in ex vivo, exposed-bone studies has inspired attempts to perform bone spectroscopy transcutaneously. Although the results are promising, further advancements are necessary to make non-invasive, in vivo measurements of bone that are of sufficient quality to generate accurate predictions of fracture risk. In order to separate the signals from bone and soft tissue that contribute to a transcutaneous measurement, we developed an overconstrained extraction algorithm that is based upon fitting with spectral libraries derived from separately-acquired measurements of the underlying tissue components. This approach allows for accurate spectral unmixing despite the fact that similar chemical components (e.g., type I collagen) are present in both soft tissue and bone and was applied to experimental data in order to transcutaneously detect, to our knowledge for the first time, age- and disease-related spectral

  1. Raman and Photoluminescence Spectroscopy in Mineral Identification

    NASA Astrophysics Data System (ADS)

    Kuehn, J. W.

    2014-06-01

    Raman spectroscopy is particularly useful for rapid identification of minerals and gemstones. Raman spectrometers also allow PL studies for authentication of samples and geological provenance, diamond type screening and detection of HPHT treatments.

  2. Raman Spectroscopy of Ocular Tissue

    NASA Astrophysics Data System (ADS)

    Ermakov, Igor V.; Sharifzadeh, Mohsen; Gellermann, Warner

    The optically transparent nature of the human eye has motivated numerous Raman studies aimed at the non-invasive optical probing of ocular tissue components critical to healthy vision. Investigations include the qualitative and quantitative detection of tissue-specific molecular constituents, compositional changes occurring with development of ocular pathology, and the detection and tracking of ocular drugs and nutritional supplements. Motivated by a better understanding of the molecular mechanisms leading to cataract formation in the aging human lens, a great deal of work has centered on the Raman detection of proteins and water content in the lens. Several protein groups and the hydroxyl response are readily detectable. Changes of protein compositions can be studied in excised noncataractous tissue versus aged tissue preparations as well as in tissue samples with artificially induced cataracts. Most of these studies are carried out in vitro using suitable animal models and conventional Raman techniques. Tissue water content plays an important role in optimum light transmission of the outermost transparent ocular structure, the cornea. Using confocal Raman spectroscopy techniques, it has been possible to non-invasively measure the water to protein ratio as a measure of hydration status and to track drug-induced changes of the hydration levels in the rabbit cornea at various depths. The aqueous humor, normally supplying nutrients to cornea and lens, has an advantageous anterior location for Raman studies. Increasing efforts are pursued to non-invasively detect the presence of glucose and therapeutic concentrations of antibiotic drugs in this medium. In retinal tissue, Raman spectroscopy proves to be an important tool for research into the causes of macular degeneration, the leading cause of irreversible vision disorders and blindness in the elderly. It has been possible to detect the spectral features of advanced glycation and advanced lipooxydation end products in

  3. Inflammation-related alterations of lipids after spinal cord injury revealed by Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Tamosaityte, Sandra; Galli, Roberta; Uckermann, Ortrud; Sitoci-Ficici, Kerim H.; Koch, Maria; Later, Robert; Schackert, Gabriele; Koch, Edmund; Steiner, Gerald; Kirsch, Matthias

    2016-06-01

    Spinal cord injury (SCI) triggers several lipid alterations in nervous tissue. It is characterized by extensive demyelination and the inflammatory response leads to accumulation of activated microglia/macrophages, which often transform into foam cells by accumulation of lipid droplets after engulfment of the damaged myelin sheaths. Using an experimental rat model, Raman microspectroscopy was applied to retrieve the modifications of the lipid distribution following SCI. Coherent anti-Stokes Raman scattering (CARS) and endogenous two-photon fluorescence (TPEF) microscopies were used for the detection of lipid-laden inflammatory cells. The Raman mapping of CH2 deformation mode intensity at 1440 cm-1 retrieved the lipid-depleted injury core. Preserved white matter and inflammatory regions with myelin fragmentation and foam cells were localized by specifically addressing the distribution of esterified lipids, i.e., by mapping the intensity of the carbonyl Raman band at 1743 cm-1, and were in agreement with CARS/TPEF microscopy. Principal component analysis revealed that the inflammatory regions are notably rich in saturated fatty acids. Therefore, Raman spectroscopy enabled to specifically detect inflammation after SCI and myelin degradation products.

  4. Raman spectroscopy peer review report

    SciTech Connect

    Winkelman, W.D.; Eberlein, S.J.

    1994-09-01

    The Hanford Site in eastern Washington includes 177 underground storage tanks (UST), which contain waste materials produced during the production of nuclear fuels. The materials in the tanks must be characterized to support the retrieval, processing, and final disposition of the waste. Characterization is currently performed by removing waste samples for analyses in a hot cell or laboratory. A review of the Hanford Raman Spectroscopy Program was held in Richland on March 23 and 24, 1994. A team of principal investigators and researchers made presentations that covered both technical and programmatic aspects of the Hanford Site Raman work. After these presentations and discussions, the review panel met in a closed session to formalize a list of findings. The reviewers agreed that Raman spectroscopy is an excellent method to attack the tank waste characterization and screening problems that were presented. They agreed that there was a good chance that the method would be successful as presently envisioned. The reviewers provided the following primary recommendations: evaluation a laser with wavelength in the near infrared; provide optical filters at or near the sampling end of the fiber-optic probe; develop and implement a strategy for frequent calibration of the system; do not try to further increase Raman resolution at the expense of wavelength range; clearly identify and differentiate between requirements for providing a short-term operational system and requirements for optimizing a system for long-term field use; and determine the best optical configuration, which may include reduced fiber-optic diameter and/or short focal length and low F-number spectrographs.

  5. Induced Stokes or anti-Stokes nuclear transitions

    SciTech Connect

    Eliezer, S. |; Martinez-Val, J.M.; Velarde, G.

    1995-11-01

    It is suggested that laser-generated soft x rays can be used to induce Stokes or anti-Stokes nuclear transitions. Isomeric transitions in {sup 99}Tc and {sup 179}Hf are considered as Stokes and anti-Stokes transitions, respectively. It is shown that success of the proposed scheme may open the way for a gamma-ray laser. 18 refs., 2 figs.

  6. Development of coherent Raman measurements of temperature in condensed phases

    SciTech Connect

    Mcgrane, Shawn D; Dang, Nhan C; Bolme, Cindy A; Moore, David S

    2010-12-08

    We report theoretical considerations and preliminary data on various forms of coherent Raman spectroscopy that have been considered as candidates for measurement of temperature in condensed phase experiments with picosecond time resolution. Due to the inherent broadness and congestion of vibrational features in condensed phase solids, particularly at high temperatures and pressures, only approaches that rely on the ratio of anti-Stokes to Stokes spectral features are considered. Methods that rely on resolution of vibrational progressions, calibration of frequency shifts with temperature and pressure in reference experiments, or detailed comparison to calculation are inappropriate or impossible for our applications. In particular, we consider femtosecond stimulated Raman spectroscopy (FSRS), femtosecond/picosecond hybrid coherent Raman spectroscopy (multiplex CARS), and optical heterodyne detected femtosecond Raman induced Kerr Effect spectroscopy (OHD-FRIKES). We show that only FSRS has the ability to measure temperature via an anti-Stokes to Stokes ratio of peaks.

  7. Method And System For Examining Biological Materials Using Low Power Cw Excitation Raman Spectroscopy.

    DOEpatents

    Alfano, Robert R.; Wang, Wubao

    2000-11-21

    A method and system for examining biological materials using low-power cw excitation Raman spectroscopy. In accordance with the teachings of the invention, a low-power continuous wave (cw) pump laser beam and a low-power cw Stokes (or anti-Stokes) probe laser beam simultaneously illuminate a biological material and traverse the biological material in collinearity. The pump beam, whose frequency is varied, is used to induce Raman emission from the biological material. The intensity of the probe beam, whose frequency is kept constant, is monitored as it leaves the biological material. When the difference between the pump and probe excitation frequencies is equal to a Raman vibrational mode frequency of the biological material, the weak probe signal becomes amplified by one or more orders of magnitude (typically up to about 10.sup.4 -10.sup.6) due to the Raman emission from the pump beam. In this manner, by monitoring the intensity of the probe beam emitted from the biological material as the pump beam is varied in frequency, one can obtain an excitation Raman spectrum for the biological material tested. The present invention may be applied to in the in vivo and/or in vitro diagnosis of diabetes, heart disease, hepatitis, cancers and other diseases by measuring the characteristic excitation Raman lines of blood glucose, cholesterol, serum glutamic oxalacetic transaminase (SGOT)/serum glutamic pyruvic tansaminase (SGPT), tissues and other corresponding Raman-active body constituents, respectively. For example, it may also be used to diagnose diseases associated with the concentration of Raman-active constituents in urine, lymph and saliva It may be used to identify cancer in the breast, cervix, uterus, ovaries and the like by measuring the fingerprint excitation Raman spectra of these tissues. It may also be used to reveal the growing of tumors or cancers by measuring the levels of nitric oxide in tissue.

  8. Drug analysis by Raman and micro-Raman spectroscopy.

    PubMed

    Huong, P V

    1986-01-01

    The technique of Raman spectroscopy, resonance Raman spectroscopy and micro-Raman spectroscopy is described for application to drug analysis and investigation. Possibilities and limits are mentioned for qualitative and quantitative analyses as well as for studies of structure and interactions. Some principal interaction modes, such as hydrogen bonding, proton transfer, charge transfer and ion-molecule attraction, are shown to explain drug reactivity. Illustrations are given based on several drug families, in particular vitamins, anti-depressants, cardio-active and anticancer drugs.

  9. Surface-Enhanced Raman Spectroscopy

    NASA Astrophysics Data System (ADS)

    Stiles, Paul L.; Dieringer, Jon A.; Shah, Nilam C.; van Duyne, Richard P.

    2008-07-01

    The ability to control the size, shape, and material of a surface has reinvigorated the field of surface-enhanced Raman spectroscopy (SERS). Because excitation of the localized surface plasmon resonance of a nanostructured surface or nanoparticle lies at the heart of SERS, the ability to reliably control the surface characteristics has taken SERS from an interesting surface phenomenon to a rapidly developing analytical tool. This article first explains many fundamental features of SERS and then describes the use of nanosphere lithography for the fabrication of highly reproducible and robust SERS substrates. In particular, we review metal film over nanosphere surfaces as excellent candidates for several experiments that were once impossible with more primitive SERS substrates (e.g., metal island films). The article also describes progress in applying SERS to the detection of chemical warfare agents and several biological molecules.

  10. Raman spectroscopy of transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Saito, R.; Tatsumi, Y.; Huang, S.; Ling, X.; Dresselhaus, M. S.

    2016-09-01

    Raman spectroscopy of transition metal dichalcogenides (TMDs) is reviewed based on our recent theoretical and experimental works. First, we discuss the semi-classical and quantum mechanical description for the polarization dependence of Raman spectra of TMDs in which the optical dipole transition matrix elements as a function of laser excitation energy are important for understanding the polarization dependence of the Raman intensity and Raman tensor. Overviewing the symmetry of TMDs, we discuss the dependence of the Raman spectra of TMDs on layer thickness, polarization, laser energy and the structural phase. Furthermore, we discuss the Raman spectra of twisted bilayer and heterostructures of TMDs. Finally, we give our perspectives on the Raman spectroscopy of TMDs.

  11. Raman spectroscopy of transition metal dichalcogenides.

    PubMed

    Saito, R; Tatsumi, Y; Huang, S; Ling, X; Dresselhaus, M S

    2016-09-07

    Raman spectroscopy of transition metal dichalcogenides (TMDs) is reviewed based on our recent theoretical and experimental works. First, we discuss the semi-classical and quantum mechanical description for the polarization dependence of Raman spectra of TMDs in which the optical dipole transition matrix elements as a function of laser excitation energy are important for understanding the polarization dependence of the Raman intensity and Raman tensor. Overviewing the symmetry of TMDs, we discuss the dependence of the Raman spectra of TMDs on layer thickness, polarization, laser energy and the structural phase. Furthermore, we discuss the Raman spectra of twisted bilayer and heterostructures of TMDs. Finally, we give our perspectives on the Raman spectroscopy of TMDs.

  12. Applications of Raman spectroscopy in life science

    NASA Astrophysics Data System (ADS)

    Martin, Airton A.; T. Soto, Cláudio A.; Ali, Syed M.; Neto, Lázaro P. M.; Canevari, Renata A.; Pereira, Liliane; Fávero, Priscila P.

    2015-06-01

    Raman spectroscopy has been applied to the analysis of biological samples for the last 12 years providing detection of changes occurring at the molecular level during the pathological transformation of the tissue. The potential use of this technology in cancer diagnosis has shown encouraging results for the in vivo, real-time and minimally invasive diagnosis. Confocal Raman technics has also been successfully applied in the analysis of skin aging process providing new insights in this field. In this paper it is presented the latest biomedical applications of Raman spectroscopy in our laboratory. It is shown that Raman spectroscopy (RS) has been used for biochemical and molecular characterization of thyroid tissue by micro-Raman spectroscopy and gene expression analysis. This study aimed to improve the discrimination between different thyroid pathologies by Raman analysis. A total of 35 thyroid tissues samples including normal tissue (n=10), goiter (n=10), papillary (n=10) and follicular carcinomas (n=5) were analyzed. The confocal Raman spectroscopy allowed a maximum discrimination of 91.1% between normal and tumor tissues, 84.8% between benign and malignant pathologies and 84.6% among carcinomas analyzed. It will be also report the application of in vivo confocal Raman spectroscopy as an important sensor for detecting advanced glycation products (AGEs) on human skin.

  13. Anti-Stokes shift luminescent materials for bio-applications.

    PubMed

    Zhu, Xingjun; Su, Qianqian; Feng, Wei; Li, Fuyou

    2017-02-20

    Anti-Stokes shift luminescence is a special optical process, which converts long-wavelength excitation to short-wavelength emission. This unique ability is especially helpful for bio-applications, because the longer-wavelength light source, usually referring to near infrared light, has a larger penetration depth offering a longer working distance for in vivo applications. The anti-Stokes shift luminescence signal can also be distinguished from the auto-fluorescence of biological tissues, thus reducing background interference during bioimaging. Herein, we summarize recent advances in anti-Stokes shift luminescent materials, including lanthanide and triplet-triplet-annihilation-based upconversion nanomaterials, and newly improved hot-band absorption-based luminescent materials. We focus on the synthetic strategies, optical optimization and biological applications as well as present comparative discussions on the luminescence mechanisms and characteristics of these three types of luminescent materials.

  14. CARS (Coherent Anti-Stokes Raman Scattering) Spectroscopy of the Reaction Zone of Methane-Nitrous Oxide and RDX Propellant Flames.

    DTIC Science & Technology

    1986-01-01

    et al. (ref 14) ex- plicitly included reactions of HCN and NO in the BDP aodel. Miller and Coffee (refs 15 and 16) gave detailed comparisons of the...37), respec- tively. These and previous studies have shown that the conversion of fuel nitro - gen to HCN is almost quantitative and independent of the...Combustion and Flame, vol 46, 1982, p 51. 16. M. S. Miller and T. P. Coffee , Combustion and Flame, vol 50, 1983, pp b5 and 75. 17. Sylvia A. J. Druet and

  15. Raman spectroscopy: the gateway into tomorrow's virology

    PubMed Central

    Lambert, Phelps J; Whitman, Audy G; Dyson, Ossie F; Akula, Shaw M

    2006-01-01

    In the molecular world, researchers act as detectives working hard to unravel the mysteries surrounding cells. One of the researchers' greatest tools in this endeavor has been Raman spectroscopy. Raman spectroscopy is a spectroscopic technique that measures the unique Raman spectra for every type of biological molecule. As such, Raman spectroscopy has the potential to provide scientists with a library of spectra that can be used to unravel the makeup of an unknown molecule. However, this technique is limited in that it is not able to manipulate particular structures without disturbing their unique environment. Recently, a novel technology that combines Raman spectroscopy with optical tweezers, termed Raman tweezers, evades this problem due to its ability to manipulate a sample without physical contact. As such, Raman tweezers has the potential to become an incredibly effective diagnostic tool for differentially distinguishing tissue, and therefore holds great promise in the field of virology for distinguishing between various virally infected cells. This review provides an introduction for a virologist into the world of spectroscopy and explores many of the potential applications of Raman tweezers in virology. PMID:16805914

  16. Raman spectroscopy: the gateway into tomorrow's virology.

    PubMed

    Lambert, Phelps J; Whitman, Audy G; Dyson, Ossie F; Akula, Shaw M

    2006-06-28

    In the molecular world, researchers act as detectives working hard to unravel the mysteries surrounding cells. One of the researchers' greatest tools in this endeavor has been Raman spectroscopy. Raman spectroscopy is a spectroscopic technique that measures the unique Raman spectra for every type of biological molecule. As such, Raman spectroscopy has the potential to provide scientists with a library of spectra that can be used to unravel the makeup of an unknown molecule. However, this technique is limited in that it is not able to manipulate particular structures without disturbing their unique environment. Recently, a novel technology that combines Raman spectroscopy with optical tweezers, termed Raman tweezers, evades this problem due to its ability to manipulate a sample without physical contact. As such, Raman tweezers has the potential to become an incredibly effective diagnostic tool for differentially distinguishing tissue, and therefore holds great promise in the field of virology for distinguishing between various virally infected cells. This review provides an introduction for a virologist into the world of spectroscopy and explores many of the potential applications of Raman tweezers in virology.

  17. Stress measurement in MEMS using Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Animoto, Sherwin T.; Chang, Dick J.; Birkitt, Andra D.

    1998-09-01

    Raman spectroscopy is used as a non-contact method in measuring stresses at the surface of a crystalline structure or the crystalline-coated surface of an amorphous structure. The stress measurement capability is based on the relative frequency shift of Raman spectra when the crystal lattice is strained. The Raman spectroscopy has a resolution on the order of a few micrometer (micrometers ) which may be used to probe the local non-uniform stress distribution and thus address the material nonhomogeneity. This paper presents the Raman secular equation for general and cubic crystal systems and discusses the stress field effects to Raman frequency shifts and polarization. Experimental testing will include the calibration of the Raman signal versus mechanically applied stresses using single crystal strips, poly-silicon coatings deposited on different specimen configurations, and the stress measurements on a frequently used MEMS structure, cantilever beam, subject to electrostatic forces. Correlation of the experimental results with the analytical prediction will be addressed.

  18. Study of virus by Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Moor, K.; Kitamura, H.; Hashimoto, K.; Sawa, M.; Andriana, B. B.; Ohtani, K.; Yagura, T.; Sato, H.

    2013-02-01

    Problem of viruses is very actual for nowadays. Some viruses, which are responsible for human of all tumors, are about 15 %. Main purposes this study, early detection virus in live cell without labeling and in the real time by Raman spectroscopy. Micro Raman spectroscopy (mRs) is a technique that uses a Raman spectrometer to measure the spectra of microscopic samples. According to the Raman spectroscopy, it becomes possible to study the metabolites of a live cultured cell without labeling. We used mRs to detect the virus via HEK 293 cell line-infected adenovirus. We obtained raman specters of lives cells with viruses in 24 hours and 7 days after the infection. As the result, there is some biochemical changing after the treatment of cell with virus. One of biochemical alteration is at 1081 cm-1. For the clarification result, we use confocal fluorescent microscopy and transmission electron microscopy (TEM).

  19. Occlusal caries detection using polarized Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Ionita, I.; Bulou, A.

    2008-02-01

    The tooth enamel, because of its hydroxyapatite composition, must present a Raman spectrum with strong polarization anisotropy. Carious lesions of the enamel will produce an alteration of local symmetry and will increase much more scattering of light. This will reduce the anisotropy of the Raman spectra. Because of the difference between high sensitivity to polarization of the 959 cm -1 Raman peak in sound enamel and low sensitivity in carried enamel, Raman polarized spectroscopy could be a useful method to early detect teeth caries.

  20. Applications of Raman spectroscopy to gemology.

    PubMed

    Bersani, Danilo; Lottici, Pier Paolo

    2010-08-01

    Being nondestructive and requiring short measurement times, a low amount of material, and no sample preparation, Raman spectroscopy is used for routine investigation in the study of gemstone inclusions and treatments and for the characterization of mounted gems. In this work, a review of the use of laboratory Raman and micro-Raman spectrometers and of portable Raman systems in the gemology field is given, focusing on gem identification and on the evaluation of the composition, provenance, and genesis of gems. Many examples are shown of the use of Raman spectroscopy as a tool for the identification of imitations, synthetic gems, and enhancement treatments in natural gemstones. Some recent developments are described, with particular attention being given to the semiprecious stone jade and to two important organic materials used in jewelry, i.e., pearls and corals.

  1. Raman spectroscopy in pharmaceutical product design.

    PubMed

    Paudel, Amrit; Raijada, Dhara; Rantanen, Jukka

    2015-07-15

    Almost 100 years after the discovery of the Raman scattering phenomenon, related analytical techniques have emerged as important tools in biomedical sciences. Raman spectroscopy and microscopy are frontier, non-invasive analytical techniques amenable for diverse biomedical areas, ranging from molecular-based drug discovery, design of innovative drug delivery systems and quality control of finished products. This review presents concise accounts of various conventional and emerging Raman instrumentations including associated hyphenated tools of pharmaceutical interest. Moreover, relevant application cases of Raman spectroscopy in early and late phase pharmaceutical development, process analysis and micro-structural analysis of drug delivery systems are introduced. Finally, potential areas of future advancement and application of Raman spectroscopic techniques are discussed.

  2. Scanning angle Raman spectroscopy: Investigation of Raman scatter enhancement techniques for chemical analysis

    SciTech Connect

    Meyer, Matthew W.

    2013-01-01

    This thesis outlines advancements in Raman scatter enhancement techniques by applying evanescent fields, standing-waves (waveguides) and surface enhancements to increase the generated mean square electric field, which is directly related to the intensity of Raman scattering. These techniques are accomplished by employing scanning angle Raman spectroscopy and surface enhanced Raman spectroscopy. A 1064 nm multichannel Raman spectrometer is discussed for chemical analysis of lignin. Extending dispersive multichannel Raman spectroscopy to 1064 nm reduces the fluorescence interference that can mask the weaker Raman scattering. Overall, these techniques help address the major obstacles in Raman spectroscopy for chemical analysis, which include the inherently weak Raman cross section and susceptibility to fluorescence interference.

  3. Online fluorescence suppression in modulated Raman spectroscopy.

    PubMed

    De Luca, Anna Chiara; Mazilu, Michael; Riches, Andrew; Herrington, C Simon; Dholakia, Kishan

    2010-01-15

    Label-free chemical characterization of single cells is an important aim for biomedical research. Standard Raman spectroscopy provides intrinsic biochemical markers for noninvasive analysis of biological samples but is often hindered by the presence of fluorescence background. In this paper, we present an innovative modulated Raman spectroscopy technique to filter out the Raman spectra from the fluorescence background. The method is based on the principle that the fluorescence background does not change whereas the Raman scattering is shifted by the periodical modulation of the laser wavelength. Exploiting this physical property and importantly the multichannel lock-in detection of the Raman signal, the modulation technique fulfills the requirements of an effective fluorescence subtraction method. Indeed, once the synchronization and calibration procedure is performed, minimal user intervention is required, making the method online and less time-consuming than the other fluorescent suppression methods. We analyze the modulated Raman signal and shifted excitation Raman difference spectroscopy (SERDS) signal of 2 mum-sized polystyrene beads suspended in a solution of fluorescent dye as a function of modulation rate. We show that the signal-to-noise ratio of the modulated Raman spectra at the highest modulation rate is 3 times higher than the SERDS one. To finally evaluate the real benefits of the modulated Raman spectroscopy, we apply our technique to Chinese hamster ovary cells (CHO). Specifically, by analyzing separate spectra from the membrane, cytoplasm, and nucleus of CHO cells, we demonstrate the ability of this method to obtain localized sensitive chemical information from cells, away from the interfering fluorescence background. In particular, statistical analysis of the Raman data and classification using PCA (principal component analysis) indicate that our method allows us to distinguish between different cell locations with higher sensitivity and

  4. CONDENSED MATTER: ELECTRONIC STRUCTURE, ELECTRICAL, MAGNETIC, AND OPTICAL PROPERTIES: Improved anti-Stokes energy transfer between rare earth ions in Er(0.5)Yb(9.5): FOV oxyfluoride vitroceramics explains the strong color reversal

    NASA Astrophysics Data System (ADS)

    Chen, Xiao-Bo; Wang, Ce; Gregory, Salamo J.; Naruhito, Sawanobori; Kang, Dong-Guo; Masaaki, Ohtsuka; Yang, Guo-Jian; Peng, Fang-Lin

    2009-12-01

    The widely used energy transfer theory is a foundation of luminescence, in which the rates of Stokes and anti-Stokes processes have the same calculation formula. An improvement on the anti-Stokes energy transfer to explain the fluorescence intensity reversal between the red and green fluorescence of Er(0.5)Yb(9.5):FOV is reported in the present article. The range of the intensity reversal σ was measured to be 877. Dynamic processes for 16 levels were simulated. A coefficient, the improvement factor of the intensity ratio of Stokes to anti-Stokes processes in quantum Raman theory compared to classical Raman theory, is introduced to successfully describe the anti-Stokes energy transfer. A new method to calculate the distance between the rare earth ions, which is critical for the energy transfer calculation, is proposed. The validity of these important improvements is also proved by experiment.

  5. Raman spectroscopy at the tritium laboratory Karlsruhe

    SciTech Connect

    Schloesser, M.; Bornschein, B.; Fischer, S.; Kassel, F.; Rupp, S.; Sturm, M.; James, T.M.; Telle, H.H.

    2015-03-15

    Raman spectroscopy is employed successfully for analysis of hydrogen isotopologues at the Tritium Laboratory Karlsruhe (TLK). Raman spectroscopy is based on the inelastic scattering of photons off molecules. Energy is transferred to the molecules as rotational/vibrational excitation being characteristic for each type of molecule. Thus, qualitative analysis is possible from the Raman shifted light, while quantitative information can be obtained from the signal intensities. After years of research and development, the technique is now well-advanced providing fast (< 10 s), precise (< 0.1%) and true (< 3%) compositional analysis of gas mixtures of hydrogen isotopologues. In this paper, we summarize the recent achievements in the further development on this technique, and the various applications for which it is used at TLK. Raman spectroscopy has evolved as a versatile, highly accurate key method for quantitative analysis complementing the port-folio of analytic techniques at the TLK.

  6. Coherent Anti-Stokes Raman Scattering of Molecular Gases

    DTIC Science & Technology

    1977-08-01

    2 at vqm q where w and m are .., natural vibration frequency and tie reduced mass of the molecules, respecItiveiy, and ’ Is the damping con;tant of...5976 No. 17 CO 2143 8157 6044 No. 17 CO2 1388 7683 6333 No. 16 (1000) 1286 7624 6374 No. 16 (0200) H20 3654 9304 5538 No. 10 H2 4160 9764 5387 No

  7. Manifestations of nonlinear optical effects in a novel SRS-active crystal—natural topaz, Al2(F1-x(OH)x)2SiO4: many-phonon χ(3)-lasing, more than sesqui-octave Stokes and anti-Stokes multi-wavelength comb lasing, cascaded and cross-cascaded χ(3)↔χ(3) Raman-induced interactions under single- and dual-wavelength picosecond collinear coherent pumping, THG and combined SRS-promoting phonon modes

    NASA Astrophysics Data System (ADS)

    Kaminskii, A. A.; Lux, O.; Rhee, H.; Eichler, H. J.; Yoneda, H.; Shirakawa, A.; Ueda, K.; Rückamp, R.; Bohatý, L.; Becker, P.

    2013-07-01

    Natural crystals of topaz, Al2(F1-x(OH)x)2SiO4 were found to be an attractive Raman gain material and a subject for the investigation of different χ(3)-nonlinear optical effects. We present several manifestations of photon-phonon interactions related to SRS and RFWM processes initiated by picosecond excitations at room and cryogenic (≈9 K) temperature. Among them are octave-spanning Stokes and anti-Stokes generation in the visible and near-IR spectral range, combined SRS-active phonon modes, cross-cascaded up-conversion, χ(3)↔χ(3) lasing, as well as THG via self-sum frequency parametric generation. All recorded Raman-induced lasing lines are identified and attributed to the promoting χ(3)-vibration transitions. Based on the experimental data, theoretical simulations employing Fourier analysis are performed to demonstrate the potential of wide SRS frequency combs in terms of ultra-short pulse generation. On the 50th anniversary of the discovery of stimulated Raman scattering.

  8. Anti-Stokes Laser Cooling in Bulk Erbium-Doped Materials

    SciTech Connect

    Fernandez, Joaquin; Balda, Rolindes

    2006-07-21

    We report the first observation of anti-Stokes laser-induced cooling in the Er{sup 3+} ratio KPb{sub 2}Cl{sub 5} crystal and in the Er{sup 3+} ratio CNBZn (CdF{sub 2}-CdCl{sub 2}-NaF-BaF{sub 2}-BaCl{sub 2}-ZnF{sub 2}) glass. The internal cooling efficiencies have been calculated by using photothermal deflection spectroscopy. Thermal scans acquired with an infrared thermal camera proved the bulk cooling capability of the studied samples. The implications of these results are discussed.

  9. Using Raman spectroscopy to characterize biological materials.

    PubMed

    Butler, Holly J; Ashton, Lorna; Bird, Benjamin; Cinque, Gianfelice; Curtis, Kelly; Dorney, Jennifer; Esmonde-White, Karen; Fullwood, Nigel J; Gardner, Benjamin; Martin-Hirsch, Pierre L; Walsh, Michael J; McAinsh, Martin R; Stone, Nicholas; Martin, Francis L

    2016-04-01

    Raman spectroscopy can be used to measure the chemical composition of a sample, which can in turn be used to extract biological information. Many materials have characteristic Raman spectra, which means that Raman spectroscopy has proven to be an effective analytical approach in geology, semiconductor, materials and polymer science fields. The application of Raman spectroscopy and microscopy within biology is rapidly increasing because it can provide chemical and compositional information, but it does not typically suffer from interference from water molecules. Analysis does not conventionally require extensive sample preparation; biochemical and structural information can usually be obtained without labeling. In this protocol, we aim to standardize and bring together multiple experimental approaches from key leaders in the field for obtaining Raman spectra using a microspectrometer. As examples of the range of biological samples that can be analyzed, we provide instructions for acquiring Raman spectra, maps and images for fresh plant tissue, formalin-fixed and fresh frozen mammalian tissue, fixed cells and biofluids. We explore a robust approach for sample preparation, instrumentation, acquisition parameters and data processing. By using this approach, we expect that a typical Raman experiment can be performed by a nonspecialist user to generate high-quality data for biological materials analysis.

  10. High pressure-temperature Raman spectroscopy of H2-H2O clathrate.

    NASA Astrophysics Data System (ADS)

    Somayazulu, Maddury; Levedahl, Alexander; Goncharov, Alexander; Mao, Ho-Kwang; Hemley, Russell

    2007-03-01

    The melting curve of the C2 clathrate H2-H2O has been determined by in-situ Raman spectroscopy measurements in an externally heated diamond anvil cell. We have determined the melting curve to a maximum pressure of 27 GPa. These are the first measurements on the melting line in this clathrate. Depending on the stoichiometry of the starting mixture of H2 and H2O, we are able to study either a mixture of C2 and H2O or C2 and H2. In either case, we were able to pinpoint the melting of the clathrate from the measurements of the molecular stretching mode (vibron) in the clathrate. In the case of C2 + Ice VII, we observe the vibron in the clathrate at a frequency higher than in pure H2 at the same pressure. We have cross-calibrated the melting temperatures using the Stokes-anti Stokes ratio of the diamond first order and Raman active TO phonon of cubic Boron Nitride. We find that the clathrate melts well above the H2 melting at all pressures studied indicating that the stabilization of this clathrate at high pressures is indeed due to interactions between the host and guest molecules.

  11. Towards Single-Shot Detection of Bacterial Endospores via Coherent Raman Spectroscopy

    NASA Astrophysics Data System (ADS)

    Pestov, Dmitry; Wang, Xi; Ariunbold, Gombojav; Murawski, Robert; Sautenkov, Vladimir; Sokolov, Alexei; Scully, Marlan

    2007-10-01

    Recent advances in coherent anti-Stokes Raman scattering (CARS) spectroscopy hold exciting promise to make the most out of now readily available ultrafast laser sources. Techniques have been devised to mitigate the nonresonant four-wave-mixing in favor of informative Raman-resonant signal. In particular, a hybrid technique for CARS (see Science 316, 265 (2007)) brings together the advantages of coherent broadband pump-Stokes excitation of molecular vibrations and their time-delayed but frequency-resolved probing via a spectrally narrowed and shaped laser pulse. We apply this technique to the problem of real-time detection of warfare bioagents and report single-shot acquisition of a distinct CARS spectrum from a small volume of B. subtilis endospores (˜10^4 spores), a harmless surrogate for B. anthracis. We study the dependence of the CARS signal on the energy of the ultrashort preparation pulses and find the limit on the pulse energy fluence (˜0.2 J/cm^2), imposed by the laser-induced damage of the spores.

  12. Surface-Enhanced Femtosecond Stimulated Raman Spectroscopy.

    PubMed

    Frontiera, Renee R; Henry, Anne-Isabelle; Gruenke, Natalie L; Van Duyne, Richard P

    2011-05-19

    Surface-enhanced Raman spectroscopy (SERS) and femtosecond stimulated Raman spectroscopy (FSRS) have revolutionized the Raman spectroscopy field. SERS provides spectroscopic detection of single molecules, and FSRS enables the acquisition of Raman spectra on the ultrafast time scale of molecular motion. Here, we present the first successful combination of these two techniques, demonstrating surface-enhanced femtosecond stimulated Raman spectroscopy (SE-FSRS) using gold nanoantennas with embedded reporter molecules. Using a picosecond Raman and femtosecond probe pulse, the time- and ensemble-averaged enhancement factor is estimated to be in the range of 10(4)-10(6). We report the line shapes, power dependence, and magnitude of the SE-FSRS signal and discuss contributions to sample degradation on the minute time scale. With these first successful proof-of-principle experiments, time-resolved SE-FSRS techniques can now be rationally attempted with the goals of investigating the dynamics of plasmonic materials as well as examining the contributions of environmental heterogeneities by probing more homogeneous molecular subsets.

  13. Raman spectroscopy of white wines.

    PubMed

    Martin, Coralie; Bruneel, Jean-Luc; Guyon, François; Médina, Bernard; Jourdes, Michael; Teissedre, Pierre-Louis; Guillaume, François

    2015-08-15

    The feasibility of exploiting Raman scattering to analyze white wines has been investigated using 3 different wavelengths of the incoming laser radiation in the near-UV (325 nm), visible (532 nm) and near infrared (785 nm). To help in the interpretation of the Raman spectra, the absorption properties in the UV-visible range of two wine samples as well as their laser induced fluorescence have also been investigated. Thanks to the strong intensity enhancement of the Raman scattered light due to electronic resonance with 325 nm laser excitation, hydroxycinnamic acids may be detected and analyzed selectively. Fructose and glucose may also be easily detected below ca. 1000 cm(-1). This feasibility study demonstrates the potential of the Raman spectroscopic technique for the analysis of white wines.

  14. Polymorph Discrimination using Low Wavenumber Raman Spectroscopy

    PubMed Central

    Roy, Saikat; Chamberlin, Brianna; Matzger, Adam J.

    2016-01-01

    Characterization of crystalline polymorphs and their quantitation has become an integral part of the pre-clinical drug development process. Raman spectroscopy is a powerful technique for the rapid identification of phases of pharmaceuticals. In the present work we demonstrate the use of low wavenumber Raman vibrational spectroscopy (including phonon measurement) for discrimination among polymorphs. A total of 10 polymorphic pharmaceuticals were employed to conduct a critical assessment. Raman scattering in the low frequency region (10–400 cm−1), which includes crystal lattice vibrations, has been analyzed and the results indicate lattice phonon Raman scattering can be used for rapid discrimination of polymorphic phases with additional discriminating power compared to conventional collection strategies. Moreover structural insight and conformational changes can be detected with this approach. PMID:27642248

  15. Multiplex coherent raman spectroscopy detector and method

    DOEpatents

    Chen, Peter; Joyner, Candace C.; Patrick, Sheena T.; Guyer, Dean R.

    2004-06-08

    A multiplex coherent Raman spectrometer (10) and spectroscopy method rapidly detects and identifies individual components of a chemical mixture separated by a separation technique, such as gas chromatography. The spectrometer (10) and method accurately identify a variety of compounds because they produce the entire gas phase vibrational Raman spectrum of the unknown gas. This is accomplished by tilting a Raman cell (20) to produce a high-intensity, backward-stimulated, coherent Raman beam of 683 nm, which drives a degenerate optical parametric oscillator (28) to produce a broadband beam of 1100-1700 nm covering a range of more than 3000 wavenumber. This broadband beam is combined with a narrowband beam of 532 nm having a bandwidth of 0.003 wavenumbers and focused into a heated windowless cell (38) that receives gases separated by a gas chromatograph (40). The Raman radiation scattered from these gases is filtered and sent to a monochromator (50) with multichannel detection.

  16. Multiplex coherent raman spectroscopy detector and method

    NASA Technical Reports Server (NTRS)

    Chen, Peter (Inventor); Joyner, Candace C. (Inventor); Patrick, Sheena T. (Inventor); Guyer, Dean R. (Inventor)

    2004-01-01

    A multiplex coherent Raman spectrometer (10) and spectroscopy method rapidly detects and identifies individual components of a chemical mixture separated by a separation technique, such as gas chromatography. The spectrometer (10) and method accurately identify a variety of compounds because they produce the entire gas phase vibrational Raman spectrum of the unknown gas. This is accomplished by tilting a Raman cell (20) to produce a high-intensity, backward-stimulated, coherent Raman beam of 683 nm, which drives a degenerate optical parametric oscillator (28) to produce a broadband beam of 1100-1700 nm covering a range of more than 3000 wavenumber. This broadband beam is combined with a narrowband beam of 532 nm having a bandwidth of 0.003 wavenumbers and focused into a heated windowless cell (38) that receives gases separated by a gas chromatograph (40). The Raman radiation scattered from these gases is filtered and sent to a monochromator (50) with multichannel detection.

  17. Raman spectroscopy under extreme conditions

    SciTech Connect

    Goncharov, A F; Crowhurst, J C

    2004-11-05

    We report the results of Raman measurements of various materials under simultaneous conditions of high temperature and high pressure in the diamond anvil cell (DAC). High temperatures are generated by laser heating or internal resistive (ohmic) heating or a combination of both. We present Raman spectra of cubic boron nitride (cBN) to 40 GPa and up to 2300 K that show a continuous pressure and temperature shift of the frequency of the transverse optical mode. We have also obtained high-pressure Raman spectra from a new noble metal nitride, which we synthesized at approximately 50 GPa and 2000 K. We have obtained high-temperature spectra from pure nitrogen to 39 GPa and up to 2000 K, which show the presence of a hot band that has previously been observed in CARS measurements. These measurements have also allowed us to constrain the melting curve and to examine changes in the intramolecular potential with pressure.

  18. Coherent Raman spectroscopy for supersonic flow measurments

    NASA Technical Reports Server (NTRS)

    She, C. Y.

    1986-01-01

    In collaboration with NASA/Langley Research Center, a truly nonintrusive and nonseeding method for measuring supersonic molecular flow parameters was proposed and developed at Colorado State University. The feasibility of this Raman Doppler Velocimetry (RDV), currently operated in a scanning mode, was demonstrated not only in a laboratory environment at Colorado State University, but also in a major wind tunnel at NASA/Langley Research Center. The research progress of the RDV development is summarized. In addition, methods of coherent Rayleigh-Brillouin spectroscopy and single-pulse coherent Raman spectroscopy are investigated, respectively, for measurements of high-pressure and turbulent flows.

  19. Process analytical applications of Raman spectroscopy.

    PubMed

    Rantanen, Jukka

    2007-02-01

    There is an increasing demand for new approaches to understand the chemical and physical phenomena that occur during pharmaceutical unit operations. Obtaining real-time information from processes opens new perspectives for safer and more efficient manufacture of pharmaceuticals. Raman spectroscopy provides a molecular level insight into processing, and therefore it is a future process analytical tool. In this review, different applications of Raman spectroscopy in the field of process analysis of pharmaceutical solid dosage forms are summarized. In addition, pitfalls associated with interfacing to the process environment and challenges within data management are discussed.

  20. Determination of 3D molecular orientation by concurrent polarization analysis of multiple Raman modes in broadband CARS spectroscopy

    PubMed Central

    2016-01-01

    A theoretical description is presented about a new analysis method to determine three-dimensional (3D) molecular orientation by concurrently analyzing multiple Raman polarization profiles. Conventional approaches to polarization Raman spectroscopy are based on single peaks, and their 2D-projected polarization profiles are limited in providing 3D orientational information. Our new method analyzes multiple Raman profiles acquired by a single polarization scanning measurement of broadband coherent anti-Stokes Raman scattering (BCARS). Because the analysis uses only dimensionless quantities, such as intensity ratios and phase difference between multiple profiles, the results are not affected by sample concentration and the system response function. We describe how to determine the 3D molecular orientation with the dimensionless observables by using two simplified model cases. In addition, we discuss the effect of orientational broadening on the polarization profiles in the two model cases. We find that in the presence of broadening we can still determine the mean 3D orientation angles and, furthermore, the degree of orientational broadening. PMID:26561197

  1. Raman Studies of Carbon Nanostructures

    NASA Astrophysics Data System (ADS)

    Jorio, Ado; Souza Filho, Antonio G.

    2016-07-01

    This article reviews recent advances on the use of Raman spectroscopy to study and characterize carbon nanostructures. It starts with a brief survey of Raman spectroscopy of graphene and carbon nanotubes, followed by recent developments in the field. Various novel topics, including Stokes-anti-Stokes correlation, tip-enhanced Raman spectroscopy in two dimensions, phonon coherence, and high-pressure and shielding effects, are presented. Some consequences for other fields—quantum optics, near-field electromagnetism, archeology, materials and soil sciences—are discussed. The review ends with a discussion of new perspectives on Raman spectroscopy of carbon nanostructures, including how this technique can contribute to the development of biotechnological applications and nanotoxicology.

  2. Revisiting the Young's double slit experiment for background-free nonlinear Raman spectroscopy and microscopy.

    PubMed

    Gachet, David; Brustlein, Sophie; Rigneault, Hervé

    2010-05-28

    In the Young's double slit experiment, the spatial shift of the interference pattern projected onto a screen is directly related to the phase difference between the fields diffracted by the two slits. We apply this property to fields emitted by nonlinear processes and thus demonstrate background-free coherent anti-Stokes Raman scattering microscopy near an axial interface between a resonant and a nonresonant medium. This method is relevant to remove the nonresonant background in other coherent resonant processes.

  3. Temperature dependence of sapphire fiber Raman scattering

    SciTech Connect

    Liu, Bo; Yu, Zhihao; Tian, Zhipeng; Homa, Daniel; Hill, Cary; Wang, Anbo; Pickrell, Gary

    2015-04-27

    Anti-Stokes Raman scattering in sapphire fiber has been observed for the first time. Temperature dependence of Raman peaks’ intensity, frequency shift, and linewidth were also measured. Three anti-Stokes Raman peaks were observed at temperatures higher than 300°C in a 0.72-m-long sapphire fiber excited by a second-harmonic Nd YAG laser. The intensity of anti-Stokes peaks are comparable to that of Stokes peaks when the temperature increases to 1033°C. We foresee the combination of sapphire fiber Stokes and anti-Stokes measurement in use as a mechanism for ultrahigh temperature sensing.

  4. Raman spectroscopy of newberyite, hannayite and struvite

    NASA Astrophysics Data System (ADS)

    Frost, Ray L.; Weier, Matt L.; Martens, Wayde N.; Henry, Dermot A.; Mills, Stuart J.

    2005-11-01

    The phosphate minerals hannayite, newberyite and struvite have been studied by Raman spectroscopy using a thermal stage. Hannayite and newberyite are characterised by an intense band at around 980 cm -1 assigned to the v symmetric stretching vibration of the HPO 4 units. In contrast the symmetric stretching mode is observed at 942 cm -1 for struvite. The Raman spectra are characterised by multiple v anti-symmetric stretching bands and v and v bending modes indicating strong distortion of the HPO 4 and PO 4 units. Hannayite and newberyite are defined by bands at 3382 and 3350 cm -1 attributed to HOPO 3 vibrations and hannayite and struvite by bands at 2990, 2973 and 2874 assigned to NH 4+ bands. Raman spectroscopy has proven most useful for the analysis of these 'cave' minerals where complex paragenetic relationships exist between the minerals.

  5. Raman Spectroscopy Cell-based Biosensors

    PubMed Central

    Notingher, Ioan

    2007-01-01

    One of the main challenges faced by biodetection systems is the ability to detect and identify a large range of toxins at low concentrations and in short times. Cell-based biosensors rely on detecting changes in cell behaviour, metabolism, or induction of cell death following exposure of live cells to toxic agents. Raman spectroscopy is a powerful technique for studying cellular biochemistry. Different toxic chemicals have different effects on living cells and induce different time-dependent biochemical changes related to cell death mechanisms. Cellular changes start with membrane receptor signalling leading to cytoplasmic shrinkage and nuclear fragmentation. The potential advantage of Raman spectroscopy cell-based systems is that they are not engineered to respond specifically to a single toxic agent but are free to react to many biologically active compounds. Raman spectroscopy biosensors can also provide additional information from the time-dependent changes of cellular biochemistry. Since no cell labelling or staining is required, the specific time dependent biochemical changes in the living cells can be used for the identification and quantification of the toxic agents. Thus, detection of biochemical changes of cells by Raman spectroscopy could overcome the limitations of other biosensor techniques, with respect to detection and discrimination of a large range of toxic agents. Further developments of this technique may also include integration of cellular microarrays for high throughput in vitro toxicological testing of pharmaceuticals and in situ monitoring of the growth of engineered tissues.

  6. Raman spectroscopy of saliva as a perspective method for periodontitis diagnostics Raman spectroscopy of saliva

    NASA Astrophysics Data System (ADS)

    Gonchukov, S.; Sukhinina, A.; Bakhmutov, D.; Minaeva, S.

    2012-01-01

    In view of its potential for biological tissues analyses at a molecular level, Raman spectroscopy in optical range has been the object of biomedical research for the last years. The main aim of this work is the development of Raman spectroscopy for organic content identifying and determination of biomarkers of saliva at a molecular level for periodontitis diagnostics. Four spectral regions were determined: 1155 and 1525 cm-1, 1033 and 1611 cm-1, which can be used as biomarkers of this widespread disease.

  7. Raman spectroscopy of Alzheimer's diseased tissue

    NASA Astrophysics Data System (ADS)

    Sudworth, Caroline D.; Krasner, Neville

    2004-07-01

    Alzheimer's disease is one of the most common forms of dementia, and causes steady memory loss and mental regression. It is also accompanied by severe atrophy of the brain. However, the pathological biomarkers of the disease can only be confirmed and examined upon the death of the patient. A commercial (Renishaw PLC, UK) Raman system with an 830 nm NIR diode laser was used to analyse brain samples, which were flash frozen at post-mortem. Ethical approval was sought for these samples. The Alzheimer's diseased samples contained a number of biomarkers, including neuritic plaques and tangles. The Raman spectra were examined by order to differentiate between normal and Alzheimer's diseased brain tissues. Preliminary results indicate that Alzheimer's diseased tissues can be differentiated from control tissues using Raman spectroscopy. The Raman spectra differ in terms of peak intensity, and the presence of a stronger amide I band in the 1667 cm-1 region which occurs more prominently in the Alzheimer's diseased tissue. These preliminary results indicate that the beta-amyloid protein originating from neuritic plaques can be identified with Raman spectroscopy.

  8. Detection Of Biochips By Raman And Surface Enhanced Raman Spectroscopies

    NASA Astrophysics Data System (ADS)

    Kantarovich, Keren; Tsarfati, Inbal; Gheber, Levi A.; Haupt, Karsten; Bar, Ilana

    2010-08-01

    Biochips constitute a rapidly increasing research field driven by the versatility of sensing devices and the importance of their applications in the bioanalytical field, drug development, environmental monitoring, food analysis, etc. Common strategies used for creating biochips and for reading them have extensive limitations, motivating development of miniature biochips and label-free formats. To achieve these goals we combined the nano fountain pen method, for printing microscale features with Raman spectroscopy or surface enhanced Raman spectroscopy (SERS) for reading droplets of synthetic receptors. These receptors include molecularly imprinted polymers (MIPs), which are obtained by polymerization of suitable functional and cross-linking monomers around molecular templates. MIPs are characterized by higher physical and chemical stability than biomacromolecules, and therefore are potentially very suitable as recognition elements for biosensors, or biochips. The monitored bands in the Raman and SERS spectra could be related to the taken up compound, allowing direct detection of the template, i.e., the β-blocking drug propranolol in the imprinted droplets, as well as imaging of individual and multiple dots in an array. This study shows that the combination of nanolithography techniques with SERS might open the possibility of miniaturized arrayed MIP sensors with label-free, specific and quantitative detection.

  9. Candida parapsilosis Biofilm Identification by Raman Spectroscopy

    PubMed Central

    Samek, Ota; Mlynariková, Katarina; Bernatová, Silvie; Ježek, Jan; Krzyžánek, Vladislav; Šiler, Martin; Zemánek, Pavel; Růžička, Filip; Holá, Veronika; Mahelová, Martina

    2014-01-01

    Colonies of Candida parapsilosis on culture plates were probed directly in situ using Raman spectroscopy for rapid identification of specific strains separated by a given time intervals (up to months apart). To classify the Raman spectra, data analysis was performed using the approach of principal component analysis (PCA). The analysis of the data sets generated during the scans of individual colonies reveals that despite the inhomogeneity of the biological samples unambiguous associations to individual strains (two biofilm-positive and two biofilm-negative) could be made. PMID:25535081

  10. Candida parapsilosis biofilm identification by Raman spectroscopy.

    PubMed

    Samek, Ota; Mlynariková, Katarina; Bernatová, Silvie; Ježek, Jan; Krzyžánek, Vladislav; Šiler, Martin; Zemánek, Pavel; Růžička, Filip; Holá, Veronika; Mahelová, Martina

    2014-12-22

    Colonies of Candida parapsilosis on culture plates were probed directly in situ using Raman spectroscopy for rapid identification of specific strains separated by a given time intervals (up to months apart). To classify the Raman spectra, data analysis was performed using the approach of principal component analysis (PCA). The analysis of the data sets generated during the scans of individual colonies reveals that despite the inhomogeneity of the biological samples unambiguous associations to individual strains (two biofilm-positive and two biofilm-negative) could be made.

  11. Blood proteins analysis by Raman spectroscopy method

    NASA Astrophysics Data System (ADS)

    Artemyev, D. N.; Bratchenko, I. A.; Khristoforova, Yu. A.; Lykina, A. A.; Myakinin, O. O.; Kuzmina, T. P.; Davydkin, I. L.; Zakharov, V. P.

    2016-04-01

    This work is devoted to study the possibility of plasma proteins (albumin, globulins) concentration measurement using Raman spectroscopy setup. The blood plasma and whole blood were studied in this research. The obtained Raman spectra showed significant variation of intensities of certain spectral bands 940, 1005, 1330, 1450 and 1650 cm-1 for different protein fractions. Partial least squares regression analysis was used for determination of correlation coefficients. We have shown that the proposed method represents the structure and biochemical composition of major blood proteins.

  12. Raman Spectroscopy of Soft Musculoskeletal Tissues

    PubMed Central

    Esmonde-White, Karen

    2015-01-01

    Tendon, ligament, and joint tissues are important in maintaining daily function. They can be affected by disease, age, and injury. Slow tissue turnover, hierarchical structure and function, and nonlinear mechanical properties present challenges to diagnosing and treating soft musculoskeletal tissues. Understanding these tissues in health, disease, and injury is important to improving pharmacologic and surgical repair outcomes. Raman spectroscopy is an important tool in the examination of soft musculoskeletal tissues. This article highlights exciting basic science and clinical/translational Raman studies of cartilage, tendon, and ligament. PMID:25286106

  13. Raman spectroscopy of triolein under high pressures

    NASA Astrophysics Data System (ADS)

    Tefelski, D. B.; Jastrzębski, C.; Wierzbicki, M.; Siegoczyński, R. M.; Rostocki, A. J.; Wieja, K.; Kościesza, R.

    2010-03-01

    This article presents results of the high pressure Raman spectroscopy of triolein. Triolein, a triacylglyceride (TAG) of oleic acid, is an unsaturated fat, present in natural oils such as olive oil. As a basic food component and an energy storage molecule, it has considerable importance for food and fuel industries. To generate pressure in the experiment, we used a high-pressure cylindrical chamber with sapphire windows, presented in (R.M. Siegoczyński, R. Kościesza, D.B. Tefelski, and A. Kos, Molecular collapse - modification of the liquid structure induced by pressure in oleic acid, High Press. Res. 29 (2009), pp. 61-66). Pressure up to 750 MPa was applied. A Raman spectrometer in "macro"-configuration was employed. Raman spectroscopy provides information on changes of vibrational modes related to structural changes of triolein under pressure. Interesting changes in the triglyceride C‒H stretching region at 2650-3100 cm-1 were observed under high-pressures. Changes were also observed in the ester carbonyl (C˭ O) stretching region 1700-1780 cm-1 and the C‒C stretching region at 1050-1150 cm-1. The overall luminescence of the sample decreased under pressure, making it possible to set longer spectrum acquisition time and obtain more details of the spectrum. The registered changes suggest that the high-pressure solid phase of triolein is organized as β-polymorphic, as was reported in (C. Akita, T. Kawaguchi, and F. Kaneko, Structural study on polymorphism of cis-unsaturated triacylglycerol: Triolein, J. Phys. Chem. B 110 (2006), pp. 4346-4353; E. Da Silva and D. Rousseau, Molecular order and thermodynamics of the solid-liquid transition in triglycerides via Raman spectroscopy, Phys. Chem. Chem. Phys. 10 (2008), pp. 4606-4613) (with temperature-induced phase transitions). The research has shown that Raman spectroscopy in TAGs under pressure reveals useful information about its structural changes.

  14. The effect of aqueous solution in Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Kang, Jian; Yuan, Xiaojuan; Dong, Xiao; Gu, Huaimin

    2009-08-01

    In Raman detection, the most popular solution for the samples is tri-distilled water. But the effect of aqueous solution is barely studied in Raman spectroscopy. In fact Raman spectroscopy of solid-state and liquid-state are obvious different. In addition, FWHM of Raman spectral peaks also change evidently. In this paper, several samples were selected for the experiment; including sodium nitrate, sodium nitrite, glucose and caffeine. By comparing the Raman spectroscopy of samples at different concentrations, it is found that the concentration of the sample can affect the strength of Raman spectroscopy, but it can hardly impact FWHM of Raman spectral peaks. By comparing the Raman spectroscopy of liquid-state with the Raman spectroscopy of solid-state, it is observed that the FWHM of some Raman spectral peaks varied obviously; that may be because when the sample was dissolved into the water, the crystal lattice structure was broken, and for some samples atom form became ion form in aqueous solution. Those structural variations caused the variation of the FWHM. The Raman spectroscopy of caffeine aqueous solution at very low concentration was also detected and analyzed. Compared with the Raman spectra of solid-state samples, it is found that some Raman spectral peaks disappeared when the sample was dissolved in water. It is possible that the low concentration of the sample result in the weakening of Raman signals and the disappearing of some weak Raman spectral peaks. Then Ag nanoparticles were added into the caffeine aqueous solution, the results suggest that surface enhanced Raman spectroscopy (SERS) not only can enhance the Raman spectral signal, but also can reduce the effect of aqueous solution. It is concluded that the concentration of sample only affects the strength of Raman spectroscopy; the aqueous solution can affect the FWHM of Raman spectral peaks; and SERS can reduce the effect of aqueous solution.

  15. Drug Stability Analysis by Raman Spectroscopy

    PubMed Central

    Shende, Chetan; Smith, Wayne; Brouillette, Carl; Farquharson, Stuart

    2014-01-01

    Pharmaceutical drugs are available to astronauts to help them overcome the deleterious effects of weightlessness, sickness and injuries. Unfortunately, recent studies have shown that some of the drugs currently used may degrade more rapidly in space, losing their potency before their expiration dates. To complicate matters, the degradation products of some drugs can be toxic. Here, we present a preliminary investigation of the ability of Raman spectroscopy to quantify mixtures of four drugs; acetaminophen, azithromycin, epinephrine, and lidocaine, with their primary degradation products. The Raman spectra for the mixtures were replicated by adding the pure spectra of the drug and its degradant to determine the relative percent contributions using classical least squares. This multivariate approach allowed determining concentrations in ~10 min with a limit of detection of ~4% of the degradant. These results suggest that a Raman analyzer could be used to assess drug potency, nondestructively, at the time of use to ensure crewmember safety. PMID:25533308

  16. Drug stability analysis by Raman spectroscopy.

    PubMed

    Shende, Chetan; Smith, Wayne; Brouillette, Carl; Farquharson, Stuart

    2014-12-22

    Pharmaceutical drugs are available to astronauts to help them overcome the deleterious effects of weightlessness, sickness and injuries. Unfortunately, recent studies have shown that some of the drugs currently used may degrade more rapidly in space, losing their potency before their expiration dates. To complicate matters, the degradation products of some drugs can be toxic. Here, we present a preliminary investigation of the ability of Raman spectroscopy to quantify mixtures of four drugs; acetaminophen, azithromycin, epinephrine, and lidocaine, with their primary degradation products. The Raman spectra for the mixtures were replicated by adding the pure spectra of the drug and its degradant to determine the relative percent contributions using classical least squares. This multivariate approach allowed determining concentrations in ~10 min with a limit of detection of ~4% of the degradant. These results suggest that a Raman analyzer could be used to assess drug potency, nondestructively, at the time of use to ensure crewmember safety.

  17. Remote adjustable focus Raman spectroscopy probe

    DOEpatents

    Schmucker, John E.; Blasi, Raymond J.; Archer, William B.

    1999-01-01

    A remote adjustable focus Raman spectroscopy probe allows for analyzing Raman scattered light from a point of interest external probe. An environmental barrier including at least one window separates the probe from the point of interest. An optical tube is disposed adjacent to the environmental barrier and includes a long working length compound lens objective next to the window. A beam splitter and a mirror are at the other end. A mechanical means is used to translated the prove body in the X, Y, and Z directions resulting in a variable focus optical apparatus. Laser light is reflected by the beam splitter and directed toward the compound lens objective, then through the window and focused on the point of interest. Raman scattered light is then collected by the compound lens objective and directed through the beam splitter to a mirror. A device for analyzing the light, such as a monochrometer, is coupled to the mirror.

  18. Characterization of Kevlar Using Raman Spectroscopy

    NASA Technical Reports Server (NTRS)

    Washer, Glenn; Brooks, Thomas; Saulsberry, Regor

    2007-01-01

    This paper explores the characterization of Kevlar composite materials using Raman spectroscopy. The goal of the research is to develop and understand the Raman spectrum of Kevlar materials to provide a foundation for the development of nondestructive evaluation (NDE) technologies based on the interaction of laser light with the polymer Kevlar. The paper discusses the fundamental aspects of experimental characterization of the spectrum of Kevlar, including the effects of incident wavelength, polarization and laser power. The effects of environmental exposure of Kevlar materials on certain characteristics of its Raman spectrum are explored, as well as the effects of applied stress. This data may provide a foundation for the development of NDE technologies intended to detect the in-situ deterioration of Kevlar materials used for engineering applications that can later be extended to other materials such as carbon fiber composites.

  19. Remote Adjustable focus Raman Spectroscopy Probe

    SciTech Connect

    Schmucker, John E.; Blasi, Raymond J.; Archer, William B.

    1998-07-28

    A remote adjustable focus Raman spectroscopy probe allows for analyzing Raman scattered light from a point of interest external to the probe. An environmental barrier including at least one window separates the probe from the point of interest. An optical tube is disposed adjacent to the environmental barrier and includes along working length compound lens objective next to the window. A beam splitter and a mirror are at the other end. A mechanical means is used to translate the probe body in the X, Y, and Z directions resulting in a variable focus optical apparatus. Laser light is reflected by the beam splitter and directed toward the compound lens objective, then through the window and focused on the point of interest. Raman scattered light is then collected by the compound lens objective and directed through the beam splitter to a mirror. A device for analyzing the light, such as a monochrometer, is coupled to the mirror.

  20. Raman spectroscopy system with hollow fiber probes

    NASA Astrophysics Data System (ADS)

    Liu, Bing-hong; Shi, Yi-Wei

    2012-11-01

    A Raman remote spectroscopy system was realized using flexible hollow optical fiber as laser emittion and signal collection probes. A silver-coated hollow fiber has low-loss property and flat transmission characteristics in the visible wavelength regions. Compared with conventional silica optical fiber, little background fluorescence noise was observed with optical fiber as the probe, which would be of great advantages to the detection in low frequency Raman shift region. The complex filtering and focusing system was thus unnecessary. The Raman spectra of CaCO3 and PE were obtained by using the system and a reasonable signal to noise ratio was attained without any lens. Experiments with probes made of conventional silica optical fibers were also conducted for comparisons. Furthermore, a silver-coated hollow glass waveguide was used as sample cell to detect liquid phase sample. We used a 6 cm-long hollow fiber as the liquid cell and Butt-couplings with emitting and collecting fibers. Experiment results show that the system obtained high signal to noise ratio because of the longer optical length between sample and laser light. We also give the elementary theoretical analysis for the hollow fiber sample cell. The parameters of the fiber which would affect the system were discussed. Hollow fiber has shown to be a potential fiber probe or sample cell for Raman spectroscopy.

  1. Detecting changes during pregnancy with Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Vargis, Elizabeth; Robertson, Kesha; Al-Hendy, Ayman; Reese, Jeff; Mahadevan-Jansen, Anita

    2010-02-01

    Preterm labor is the second leading cause of neonatal mortality and leads to a myriad of complications like delayed development and cerebral palsy. Currently, there is no way to accurately predict preterm labor, making its prevention and treatment virtually impossible. While there are some at-risk patients, over half of all preterm births do not fall into any high-risk category. This study seeks to predict and prevent preterm labor by using Raman spectroscopy to detect changes in the cervix during pregnancy. Since Raman spectroscopy has been used to detect cancers in vivo in organs like the cervix and skin, it follows that spectra will change over the course of pregnancy. Previous studies have shown that fluorescence decreased during pregnancy and increased during post-partum exams to pre-pregnancy levels. We believe significant changes will occur in the Raman spectra obtained during the course of pregnancy. In this study, Raman spectra from the cervix of pregnant mice and women will be acquired. Specific changes that occur due to cervical softening or changes in hormonal levels will be observed to understand the likelihood that a female mouse or a woman will enter labor.

  2. Raman Spectroscopy for Analysis of Thorium Compounds

    SciTech Connect

    Su, Yin-Fong; Johnson, Timothy J.; Olsen, Khris B.

    2016-05-12

    The thorium fuel cycle is an alternative to the uranium fuel cycle in that when 232Th is irradiated with neutrons it is converted to 233U, another fissile isotope. There are several chemical forms of thorium which are used in the Th fuel cycle. Recently, Raman spectroscopy has become a very portable and facile analytical technique useful for many applications, including e.g. determining the chemical composition of different materials such as for thorium compounds. The technique continues to improve with the development of ever-more sensitive instrumentation and better software. Using a laboratory Fourier-transform (FT)-Raman spectrometer with a 785 nm wavelength laser, we were able to obtain Raman spectra from a series of thorium-bearing compounds of unknown origin. These spectra were compared to the spectra of in-stock-laboratory thorium compounds including ThO2, ThF4, Th(CO3)2 and Th(C2O4)2. The unknown spectra showed very good agreement to the known standards, demonstrating the applicability of Raman spectroscopy for detection and identification of these nuclear materials.

  3. Non-invasive chemically specific measurement of subsurface temperature in biological tissues using surface-enhanced spatially offset Raman spectroscopy.

    PubMed

    Gardner, Benjamin; Stone, Nicholas; Matousek, Pavel

    2016-06-23

    Here we demonstrate for the first time the viability of characterising non-invasively the subsurface temperature of SERS nanoparticles embedded within biological tissues using spatially offset Raman spectroscopy (SORS). The proposed analytical method (T-SESORS) is applicable in general to diffusely scattering (turbid) media and features high sensitivity and high chemical selectivity. The method relies on monitoring the Stokes and anti-Stokes bands of SERS nanoparticles in depth using SORS. The approach has been conceptually demonstrated using a SORS variant, transmission Raman spectroscopy (TRS), by measuring subsurface temperatures within a slab of porcine tissue (5 mm thick). Root-mean-square errors (RMSEs) of 0.20 °C were achieved when measuring temperatures over ranges between 25 and 44 °C. This unique capability complements the array of existing, predominantly surface-based, temperature monitoring techniques. It expands on a previously demonstrated SORS temperature monitoring capability by adding extra sensitivity stemming from SERS to low concentration analytes. The technique paves the way for a wide range of applications including subsurface, chemical-specific, non-invasive temperature analysis within turbid translucent media including: the human body, subsurface monitoring of chemical (e.g. catalytic) processes in manufacture quality and process control and research. Additionally, the method opens prospects for control of thermal treatment of cancer in vivo with direct non-invasive feedback on the temperature of mediating plasmonic nanoparticles.

  4. Perspective: Two-dimensional resonance Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Molesky, Brian P.; Guo, Zhenkun; Cheshire, Thomas P.; Moran, Andrew M.

    2016-11-01

    Two-dimensional resonance Raman (2DRR) spectroscopy has been developed for studies of photochemical reaction mechanisms and structural heterogeneity in complex systems. The 2DRR method can leverage electronic resonance enhancement to selectively probe chromophores embedded in complex environments (e.g., a cofactor in a protein). In addition, correlations between the two dimensions of the 2DRR spectrum reveal information that is not available in traditional Raman techniques. For example, distributions of reactant and product geometries can be correlated in systems that undergo chemical reactions on the femtosecond time scale. Structural heterogeneity in an ensemble may also be reflected in the 2D spectroscopic line shapes of both reactive and non-reactive systems. In this perspective article, these capabilities of 2DRR spectroscopy are discussed in the context of recent applications to the photodissociation reactions of triiodide and myoglobin. We also address key differences between the signal generation mechanisms for 2DRR and off-resonant 2D Raman spectroscopies. Most notably, it has been shown that these two techniques are subject to a tradeoff between sensitivity to anharmonicity and susceptibility to artifacts. Overall, recent experimental developments and applications of the 2DRR method suggest great potential for the future of the technique.

  5. The Impact of Array Detectors on Raman Spectroscopy

    ERIC Educational Resources Information Center

    Denson, Stephen C.; Pommier, Carolyn J. S.; Denton, M. Bonner

    2007-01-01

    The impact of array detectors in the field of Raman spectroscopy and all low-light-level spectroscopic techniques is examined. The high sensitivity of array detectors has allowed Raman spectroscopy to be used to detect compounds at part per million concentrations and to perform Raman analyses at advantageous wavelengths.

  6. Quantum theory of time-resolved femtosecond stimulated Raman spectroscopy: direct versus cascade processes and application to CDCl3.

    PubMed

    Zhao, Bin; Sun, Zhigang; Lee, Soo-Y

    2011-01-14

    We present a quantum mechanical wave packet treatment of time-resolved femtosecond stimulated Raman spectroscopy (FSRS), or two-dimensional (2D) FSRS, where a vibrational coherence is initiated with an impulsive Raman pump which is subsequently probed by FSRS. It complements the recent classical treatment by Mehlenbacher et al. [J. Chem. Phys. 131, 244512 (2009)]. In this 2D-FSRS, two processes can occur concurrently but with different intensities: a direct fifth-order process taking place on one molecule, and a cascade process comprising two third-order processes on two different molecules. The cascade process comprises a parallel and a sequential cascade. The theory is applied to the 2D-FSRS of CDCl(3) where calculations showed that: (a) the cascade process is stronger than the direct fifth-order process by one order of magnitude, (b) the sidebands assigned to C-Cl E and A(1) bends, observed on both sides of the Stokes C-D stretch frequency, are not due to anharmonic coupling between the C-D stretch and the C-Cl bends, but are instead due to the coherent anti-Stokes Raman spectroscopy (CARS) and coherent Stokes Raman spectroscopy (CSRS) fields produced in the first step of the cascade process, (c) for each delay time between the femtosecond impulsive pump and FSRS probe pulses, the line shape of the sidebands shows an inversion symmetry about the C-D stretch frequency, and this is due to the 180(∘) phase difference between the CARS and CSRS fields that produced the left and right sidebands, and (d) for each sideband, the line shape changes from positive Lorentzian to dispersive to negative Lorentzian, then to negative dispersive and back to positive Lorentzian with the period of the bending vibration, and it is correlated with the momentum of the wave packet prepared on the ground-state surface by the impulsive pump along the sideband normal coordinate.

  7. Raman Spectroscopy: Incorporating the Chemical Dimension into Dermatological Diagnosis

    PubMed Central

    Sharma, Amit; Sharma, Shruti; Zarrow, Anna; Schwartz, Robert A; Lambert, W Clark

    2016-01-01

    Raman spectroscopy provides chemical analysis of tissue in vivo. By measuring the inelastic interactions of light with matter, Raman spectroscopy can determine the chemical composition of a sample. Diseases that are visually difficult to visually distinguish can be delineated based on differences in chemical composition of the affected tissue. Raman spectroscopy has successfully found spectroscopic signatures for skin cancers and differentiated those of benign skin growths. With current and on-going advances in optics and computing, inexpensive and effective Raman systems may soon be available for clinical use. Raman spectroscopy provides direct analyses of skin lesions, thereby improving both disease diagnosis and management. PMID:26955087

  8. Raman and infrared spectroscopy of selected vanadates.

    PubMed

    Frost, Ray L; Erickson, Kristy L; Weier, Matt L; Carmody, Onuma

    2005-03-01

    Raman and infrared spectroscopy has been used to study the structure of selected vanadates including pascoite, huemulite, barnesite, hewettite, metahewettite, hummerite. Pascoite, rauvite and huemulite are examples of simple salts involving the decavanadates anion (V10O28)6-. Decavanadate consists of four distinct VO6 units which are reflected in Raman bands at the higher wavenumbers. The Raman spectra of these minerals are characterised by two intense bands at 991 and 965 cm(-1). Four pascoite Raman bands are observed at 991, 965, 958 and 905 cm(-1) and originate from four distinct VO6 sites. The other minerals namely barnesite, hewettite, metahewettite and hummerite have similar layered structures to the decavanadates but are based upon (V5O14)3- units. Barnesite is characterised by a single Raman band at 1010 cm(-1), whilst hummerite has Raman bands at 999 and 962 cm(-1). The absence of four distinct bands indicates the overlap of the vibrational modes from two of the VO6 sites. Metarossite is characterised by a strong band at 953 cm(-1). These bands are assigned to nu1 symmetric stretching modes of (V6O16)2- units and terminal VO3 units. In the infrared spectra of these minerals, bands are observed in the 837-860 cm(-1) and in the 803-833 cm(-1) region. In some of the Raman spectra bands are observed for pascoite, hummerite and metahewettite in similar positions. These bands are assigned to nu3 antisymmetric stretching of (V10O28)6- units or (V5O14)3- units. Because of the complexity of the spectra in the low wavenumber region assignment of bands is difficult. Bands are observed in the 404-458 cm(-1) region and are assigned to the nu2 bending modes of (V10O28)6- units or (V5O14)3- units. Raman bands are observed in the 530-620 cm(-1) region and are assigned to the nu4 bending modes of (V10O28)6- units or (V5O14)3- units. The Raman spectra of the vanadates in the low wavenumber region are complex with multiple overlapping bands which are probably due to VO

  9. Raman and infrared spectroscopy of selected vanadates

    NASA Astrophysics Data System (ADS)

    Frost, Ray L.; Erickson, Kristy L.; Weier, Matt L.; Carmody, Onuma

    2005-03-01

    Raman and infrared spectroscopy has been used to study the structure of selected vanadates including pascoite, huemulite, barnesite, hewettite, metahewettite, hummerite. Pascoite, rauvite and huemulite are examples of simple salts involving the decavanadates anion (V 10O 28) 6-. Decavanadate consists of four distinct VO 6 units which are reflected in Raman bands at the higher wavenumbers. The Raman spectra of these minerals are characterised by two intense bands at 991 and 965 cm -1. Four pascoite Raman bands are observed at 991, 965, 958 and 905 cm -1 and originate from four distinct VO 6 sites. The other minerals namely barnesite, hewettite, metahewettite and hummerite have similar layered structures to the decavanadates but are based upon (V 5O 14) 3- units. Barnesite is characterised by a single Raman band at 1010 cm -1, whilst hummerite has Raman bands at 999 and 962 cm -1. The absence of four distinct bands indicates the overlap of the vibrational modes from two of the VO 6 sites. Metarossite is characterised by a strong band at 953 cm -1. These bands are assigned to ν1 symmetric stretching modes of (V 6O 16) 2- units and terminal VO 3 units. In the infrared spectra of these minerals, bands are observed in the 837-860 cm -1 and in the 803-833 cm -1 region. In some of the Raman spectra bands are observed for pascoite, hummerite and metahewettite in similar positions. These bands are assigned to ν 3 antisymmetric stretching of (V 10O 28) 6- units or (V 5O 14) 3- units. Because of the complexity of the spectra in the low wavenumber region assignment of bands is difficult. Bands are observed in the 404-458 cm -1 region and are assigned to the ν2 bending modes of (V 10O 28) 6- units or (V 5O 14) 3- units. Raman bands are observed in the 530-620 cm -1 region and are assigned to the ν4 bending modes of (V 10O 28) 6- units or (V 5O 14) 3- units. The Raman spectra of the vanadates in the low wavenumber region are complex with multiple overlapping bands which are

  10. Applications of Raman Spectroscopy to Virology and Microbial Analysis

    NASA Astrophysics Data System (ADS)

    Harz, Michaela; Stöckel, Stephan; Ciobotă, Valerian; Cialla, Dana; Rösch, Petra; Popp, Jürgen

    This chapter reports from the utilization of Raman spectroscopic techniques like Raman microscopy, Raman optical activity (ROA), UV-resonance Raman (UVRR)-spectroscopy, surface enhanced Raman spectroscopy (SERS), and tip-enhanced Raman spectroscopy (TERS) for the investigation of viruses and microorganisms, especially bacteria and yeasts for medical and pharmaceutical applications. The application of these Raman techniques allows for the analysis of chemical components of cells and subcellular regions, as well as the monitoring of chemical differences occurring as a result of the growth of microorganisms. In addition, the interaction of microorganisms with active pharmaceutical agents can be investigated. In combination with chemometric methods Raman spectroscopy can also be applied to identify microorganisms both in micro colonies and even on single cells.

  11. Micro-Raman Spectroscopy for the Determination of Local Temperature Increases in TiO2 Thin Films due to the Effect of Radiation.

    PubMed

    Gallardo, Juan Jesús; Navas, Javier; Zorrilla, David; Alcántara, Rodrigo; Valor, Diego; Fernández-Lorenzo, Concha; Martín-Calleja, Joaquín

    2016-07-01

    This study applied a classic method involving Raman spectroscopy and the use of Stokes and anti-Stokes peaks to measure the temperature of TiO2 thin films found in dye-sensitized solar cells (DSSCs). In addition, three mathematical formulae were used and analyzed to estimate the increase in temperature generated solely by the effect of the radiation. The tests and calculations performed showed an increase in the temperature of the TiO2 film. That is, the films were heated by the radiation they were exposed to. A temperature increase of up to 30 K was detected for the sample with a single layer of TiO2, and over 40 K for the sample with three layers for the highest radiation powers used, and greater increases in temperature were observed in the thicker films.

  12. Electronic resonances in broadband stimulated Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Batignani, G.; Pontecorvo, E.; Giovannetti, G.; Ferrante, C.; Fumero, G.; Scopigno, T.

    2016-01-01

    Spontaneous Raman spectroscopy is a formidable tool to probe molecular vibrations. Under electronic resonance conditions, the cross section can be selectively enhanced enabling structural sensitivity to specific chromophores and reaction centers. The addition of an ultrashort, broadband femtosecond pulse to the excitation field allows for coherent stimulation of diverse molecular vibrations. Within such a scheme, vibrational spectra are engraved onto a highly directional field, and can be heterodyne detected overwhelming fluorescence and other incoherent signals. At variance with spontaneous resonance Raman, however, interpreting the spectral information is not straightforward, due to the manifold of field interactions concurring to the third order nonlinear response. Taking as an example vibrational spectra of heme proteins excited in the Soret band, we introduce a general approach to extract the stimulated Raman excitation profiles from complex spectral lineshapes. Specifically, by a quantum treatment of the matter through density matrix description of the third order nonlinear polarization, we identify the contributions which generate the Raman bands, by taking into account for the cross section of each process.

  13. Noninvasive glucose sensing by transcutaneous Raman spectroscopy

    PubMed Central

    Shih, Wei-Chuan; Bechtel, Kate L.; Rebec, Mihailo V.

    2015-01-01

    Abstract. We present the development of a transcutaneous Raman spectroscopy system and analysis algorithm for noninvasive glucose sensing. The instrument and algorithm were tested in a preclinical study in which a dog model was used. To achieve a robust glucose test system, the blood levels were clamped for periods of up to 45 min. Glucose clamping and rise/fall patterns have been achieved by injecting glucose and insulin into the ear veins of the dog. Venous blood samples were drawn every 5 min and a plasma glucose concentration was obtained and used to maintain the clamps, to build the calibration model, and to evaluate the performance of the system. We evaluated the utility of the simultaneously acquired Raman spectra to be used to determine the plasma glucose values during the 8-h experiment. We obtained prediction errors in the range of ∼1.5−2  mM. These were in-line with a best-case theoretical estimate considering the limitations of the signal-to-noise ratio estimates. As expected, the transition regions of the clamp study produced larger predictive errors than the stable regions. This is related to the divergence of the interstitial fluid (ISF) and plasma glucose values during those periods. Two key contributors to error beside the ISF/plasma difference were photobleaching and detector drift. The study demonstrated the potential of Raman spectroscopy in noninvasive applications and provides areas where the technology can be improved in future studies. PMID:25688542

  14. Diagnosing breast cancer by using Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Haka, Abigail S.; Shafer-Peltier, Karen E.; Fitzmaurice, Maryann; Crowe, Joseph; Dasari, Ramachandra R.; Feld, Michael S.

    2005-08-01

    We employ Raman spectroscopy to diagnose benign and malignant lesions in human breast tissue based on chemical composition. In this study, 130 Raman spectra are acquired from ex vivo samples of human breast tissue (normal, fibrocystic change, fibroadenoma, and infiltrating carcinoma) from 58 patients. Data are fit by using a linear combination model in which nine basis spectra represent the morphologic and chemical features of breast tissue. The resulting fit coefficients provide insight into the chemical/morphological makeup of the tissue and are used to develop diagnostic algorithms. The fit coefficients for fat and collagen are the key parameters in the resulting diagnostic algorithm, which classifies samples according to their specific pathological diagnoses, attaining 94% sensitivity and 96% specificity for distinguishing cancerous tissues from normal and benign tissues. The excellent results demonstrate that Raman spectroscopy has the potential to be applied in vivo to accurately classify breast lesions, thereby reducing the number of excisional breast biopsies that are performed. Author contributions: M.F., J.C., R.R.D., and M.S.F. designed research; A.S.H. and K.E.S.-P. performed research; A.S.H. and M.F. analyzed data; and A.S.H. wrote the paper.This paper was submitted directly (Track II) to the PNAS office.Abbreviations: DEH, ductal epithelial hyperplasia; ROC, receiver operating characteristic; N/C, nuclear-to-cytoplasm.

  15. Noninvasive glucose sensing by transcutaneous Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Shih, Wei-Chuan; Bechtel, Kate L.; Rebec, Mihailo V.

    2015-05-01

    We present the development of a transcutaneous Raman spectroscopy system and analysis algorithm for noninvasive glucose sensing. The instrument and algorithm were tested in a preclinical study in which a dog model was used. To achieve a robust glucose test system, the blood levels were clamped for periods of up to 45 min. Glucose clamping and rise/fall patterns have been achieved by injecting glucose and insulin into the ear veins of the dog. Venous blood samples were drawn every 5 min and a plasma glucose concentration was obtained and used to maintain the clamps, to build the calibration model, and to evaluate the performance of the system. We evaluated the utility of the simultaneously acquired Raman spectra to be used to determine the plasma glucose values during the 8-h experiment. We obtained prediction errors in the range of ˜1.5-2 mM. These were in-line with a best-case theoretical estimate considering the limitations of the signal-to-noise ratio estimates. As expected, the transition regions of the clamp study produced larger predictive errors than the stable regions. This is related to the divergence of the interstitial fluid (ISF) and plasma glucose values during those periods. Two key contributors to error beside the ISF/plasma difference were photobleaching and detector drift. The study demonstrated the potential of Raman spectroscopy in noninvasive applications and provides areas where the technology can be improved in future studies.

  16. Laser tweezers Raman spectroscopy of single cells

    NASA Astrophysics Data System (ADS)

    Chen, De

    Raman scattering is an inelastic collision between the vibrating molecules inside the sample and the incident photons. During this process, energy exchange takes place between the photon and the scattering molecule. By measuring the energy change of the photon, the molecular vibration mode can be probed. The vibrational spectrum contains valuable information about the disposition of atomic nuclei and chemical bonds within a molecule, the chemical compositions and the interactions between the molecule and its surroundings. In this dissertation, laser tweezers Raman spectroscopy (LTRS) technique is applied for the analysis of biological cells and human cells at single cell level. In LTRS, an individual cell is trapped in aqueous medium with laser tweezers, and Raman scattering spectra from the trapped cell are recorded in real-time. The Raman spectra of these cells can be used to reveal the dynamical processes of cell growth, cell response to environment changes, and can be used as the finger print for the identification of a bacterial cell species. Several biophysical experiments were carried out using LTRS: (1) the dynamic germination process of individual spores of Bacillus thuringiensis was detected via Ca-DPA, a spore-specific biomarker molecule; (2) inactivation and killing of Bacillus subtilis spores by microwave irradiation and wet heat were studied at single cell level; (3) the heat shock activation process of single B. subtilis spores were analyzed, in which the reversible transition from glass-like state at low temperature to liquid-like state at high temperature in spore was revealed at the molecular level; (4) the kinetic processes of bacterial cell lysis of E. coli by lysozyme and by temperature induction of lambda phage were detected real-time; (5) the fixation and rehydration of human platelets were quantitatively evaluated and characterized with Raman spectroscopy method, which provided a rapid way to quantify the quality of freeze-dried therapeutic

  17. Detection of bacterial endospores by means of ultrafast coherent Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Pestov, Dmitry Sergeyevich

    This work is devoted to formulation and development of a laser spectroscopic technique for rapid detection of biohazards, such as Bacillus anthracis spores. Coherent anti-Stokes Raman scattering (CARS) is used as an underlying process for active retrieval of species-specific characteristics of an analyte. Vibrational modes of constituent molecules are Raman-excited by a pair of ultrashort, femtosecond laser pulses, and then probed through inelastic scattering of a third, time-delayed laser field. We first employ the already known time-resolved CARS technique. We apply it to the spectroscopy of easy-to-handle methanol-water mixtures, and then continue building our expertise on solutions of dipicolinic acid (DPA) and its salts, which happen to be marker molecules for bacterial spores. Various acquisition schemes are evaluated, and the preference is given to multi-channel frequency-resolved detection, when the whole CARS spectrum is recorded as a function of the probe pulse delay. We demonstrate a simple detection algorithm that manages to differentiate DPA solution from common interferents. We investigate experimentally the advantages and disadvantages of near-resonant probing of the excited molecular coherence, and finally observe the indicative backscattered CARS signal from DPA and NaDPA powders. The possibility of selective Raman excitation via pulse shaping of the preparation pulses is also demonstrated. The analysis of time-resolved CARS experiments on powders and B. subtilis spores, a harmless surrogate for B. anthracis, facilitates the formulation of a new approach, where we take full advantage of the multi-channel frequency-resolved acquisition and spectrally discriminate the Raman-resonant CARS signal from the background due to other instantaneous four-wave mixing (FWM) processes. Using narrowband probing, we decrease the magnitude of the nonresonant FWM, which is further suppressed by the timing of the laser pulses. The devised technique, referred to as

  18. A Study of Overheating of Thermostatically Controlled TiO2 Thin Films by Using Raman Spectroscopy.

    PubMed

    Gallardo, Juan Jesús; Navas, Javier; Zorrilla, David; Alcántara, Rodrigo; Valor, Diego; Sánchez-Coronilla, Antonio; Hernández, Norge Cruz; Fernández-Lorenzo, Concha; Martín-Calleja, Joaquín

    2015-12-21

    In this study a classic Raman spectroscopy method is applied and the intensity ratio of Stokes and anti-Stokes peaks is used to measure the temperature of thermostatically controlled TiO2 thin films. In addition, three mathematical formulae are used and analyzed to estimate the temperature of the TiO2 thin films. Overheating of the samples above the thermostatically controlled temperature was observed while recording the Raman spectra, with a temperature increase of up to 30 K being detected. DFT-periodic calculations showed that the anatase (101) surface had a smaller band gap than bulk anatase. Thus, it can absorb the laser radiation with a wavelength of 532 nm that is used in the experimental setup. Part of the absorbed photon energy transfers into phonon energy, heating up the anatase phase, thus leading to the heating of the samples. Moreover, overheating of the samples indicates that the experimental method used in this study can lead to deviations in their real absolute temperature values.

  19. Simultaneous Conoscopic Holography and Raman Spectroscopy

    NASA Technical Reports Server (NTRS)

    Schramm, Harry F.; Kaiser, Bruce

    2005-01-01

    A new instrument was developed for chemical characterization of surfaces that combines the analytical power of Raman spectroscopy with the three-dimensional topographic information provided by conoscopic holography. The figure schematically depicts the proposed hybrid instrument. The output of the conoscopic holographic portion of the instrument is a topographical map of the surface; the output of the Raman portion of the instrument is hyperspectral Raman data, from which the chemical and/or biological composition of the surface would be deduced. By virtue of the basic principles of design and operation of the instrument, the hyperspectral image data would be inherently spatially registered with the topographical data. In conoscopic holography, the object and reference beams of classical holography are replaced by the ordinary and extraordinary components generated by a single beam traveling through a birefringent, uniaxial crystal. In the basic conoscopic configuration, a laser light is projected onto a specimen and the resulting illuminated spot becomes a point source of diffuse light that propagates in every direction. The laser beam is rasterscanned in two dimensions (x and y) perpendicular to the beam axis (z), and at each x,y location, the pattern of interference between the ordinary and extraordinary rays is recorded. The recorded interferogram constitutes the conoscopic hologram. Of particular significance for the proposed instrument is that the conoscopic hologram contains information on the z coordinate (height) of the illuminated surface spot. Hence, a topographical map of the specimen is constructed point-by-point by rastering the laser beam in the x and y directions and correlating the x and y coordinates with the z information obtained from the interferograms. Conoscopic imaging is an established method, and conoscopic laboratory instruments for surface metrology are commercially available. In Raman spectroscopy of a surface, one measures the spectrum

  20. Exploring many body interactions with Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Tian, Yao

    Many-body interactions are cornerstones of contemporary solid state physics research. Especially, phonon related interactions such as phonon-phonon coupling, spin-phonon coupling and electron-phonon coupling constantly present new challenges. To study phonon related many-body interactions, temperature dependent Raman spectroscopy is employed. Firstly, a new design and construction of a Raman microscope aimed at high collection eciency, positional and thermal stability is discussed. The application of the home-built Raman microscope is shown in the context of two types of novel materials; Cr2Ge2Te6 (spin-phonon coupling) and Bi2Te3-xSex (phonon-phonon coupling). Cr2Ge2Te6 is one of the rare class of ferromagnetic semiconductors and recent thermal transport studies suggest the spin and lattice are strongly coupled in its cousin compound Cr2Si2Te6. In this work, the spin-phonon coupling in Cr2Ge2Te6 has been revealed in multiple ways: we observed a split of two phonon modes due to the breaking of time reversal symmetry; the anomalous hardening of an additional three modes; and a dramatic enhancement of the phonon lifetimes. It is well-known that the phonon-phonon interaction plays a signicant role in determining the thermal transport properties of thermoelectrics. A comprehensive study of the phonon dynamics of Bi2Te3-xSex has been performed. We found that the unusual temperature dependence of dierent phonon modes originates from both cubic and quartic anharmonicity. These results are consistent with the resonance bonding mechanism, suggesting that the resonance bonding may be a common feature for conventional thermoelectrics. In the Raman spectra of Bi2Te2Se, the origin of the extra Raman feature has been debated for decades. Through a temperature dependent Raman study, we were able to prove the feature is generated by a Te-Se antisite induced local mode. The anomalous linewidth of the local mode as well as the anharmonic behavior were explained through a statistical

  1. Measuring Rocket Engine Temperatures with Hydrogen Raman Spectroscopy

    NASA Technical Reports Server (NTRS)

    Wehrmeyer, Joseph A.

    2002-01-01

    Laser-based combustion diagnostics, such as single-pulse UV Raman spectroscopy and visible Raman spectroscopy, have been successfully applied to optically-accessible rocket-like test articles. If an independent pressure measurement is available, Raman major species concentration measurements can also provide a temperature measurement. However it is desirable to obtain a Raman-derived temperature measurement without the need for simultaneous pressure measurement, especially when chamber pressure may vary spatially. This report describes Raman temperature measurements obtained by exploiting the variation in shape of the H2 Raman spectrum. Hydrogen is advantageous since it is ubiquitous in H2-O2 systems and its Raman spectrum is simpler than for other diatomics. However the influence of high pressure on the H2 Raman spectrum must be investigated. At moderate pressures, well below those of rocket engines, the Raman spectra of O2 and N2 are known to become featureless due to collisional broadening.

  2. Characterization of amino acids using Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Jenkins, Amanda L.; Larsen, Richard A.; Williams, Timothy B.

    2005-05-01

    A key process in the development of new drugs is elucidation of the interaction between the drug molecule and the target protein. Such knowledge then makes it possible to make systematic structural modifications of the drug molecule to optimize the interaction. Many analytical techniques can be applied to proteins in solution such as circular dichroism, ultraviolet, and fluorescence spectroscopy but these all have limitations. In this paper, we investigate the feasibility of using relatively simple, visible light Raman spectroscopic methods to investigate amino acids and related biopolymers.

  3. Characterization of Thalidomide using Raman Spectroscopy

    NASA Astrophysics Data System (ADS)

    Cipriani, Penelope; Smith, Candace Y.

    2008-02-01

    Thalidomide is a potent anticancer therapeutic drug whose mechanism of action has not yet been elucidated. In this report, experimental Raman spectroscopy is used to determine and characterize the vibrational frequencies of the drug. These normal modes are then compared to their quantum mechanical counterparts, which have been computed using density functional theory. Upon analysis of the spectra, we found that there was a high level of agreement between the wavenumbers. As such, this spectroscopic technique may be a viable tool for examining the way in which this drug interacts with its target molecules.

  4. Role of Raman spectroscopy and surface enhanced Raman spectroscopy in colorectal cancer

    PubMed Central

    Jenkins, Cerys A; Lewis, Paul D; Dunstan, Peter R; Harris, Dean A

    2016-01-01

    Colorectal cancer (CRC) is the fourth most common cancer in the United Kingdom and is the second largest cause of cancer related death in the United Kingdom after lung cancer. Currently in the United Kingdom there is not a diagnostic test that has sufficient differentiation between patients with cancer and those without cancer so the current referral system relies on symptomatic presentation in a primary care setting. Raman spectroscopy and surface enhanced Raman spectroscopy (SERS) are forms of vibrational spectroscopy that offer a non-destructive method to gain molecular information about biological samples. The techniques offer a wide range of applications from in vivo or in vitro diagnostics using endoscopic probes, to the use of micro-spectrometers for analysis of biofluids. The techniques have the potential to detect molecular changes prior to any morphological changes occurring in the tissue and therefore could offer many possibilities to aid the detection of CRC. The purpose of this review is to look at the current state of diagnostic technology in the United Kingdom. The development of Raman spectroscopy and SERS in clinical applications relation for CRC will then be discussed. Finally, future areas of research of Raman/SERS as a clinical tool for the diagnosis of CRC are also discussed. PMID:27190582

  5. UTI diagnosis and antibiogram using Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Kastanos, Evdokia; Kyriakides, Alexandros; Hadjigeorgiou, Katerina; Pitris, Constantinos

    2009-07-01

    Urinary tract infection diagnosis and antibiogram require a 48 hour waiting period using conventional methods. This results in ineffective treatments, increased costs and most importantly in increased resistance to antibiotics. In this work, a novel method for classifying bacteria and determining their sensitivity to an antibiotic using Raman spectroscopy is described. Raman spectra of three species of gram negative Enterobacteria, most commonly responsible for urinary tract infections, were collected. The study included 25 samples each of E.coli, Klebsiella p. and Proteus spp. A novel algorithm based on spectral ratios followed by discriminant analysis resulted in classification with over 94% accuracy. Sensitivity and specificity for the three types of bacteria ranged from 88-100%. For the development of an antibiogram, bacterial samples were treated with the antibiotic ciprofloxacin to which they were all sensitive. Sensitivity to the antibiotic was evident after analysis of the Raman signatures of bacteria treated or not treated with this antibiotic as early as two hours after exposure. This technique can lead to the development of new technology for urinary tract infection diagnosis and antibiogram with same day results, bypassing urine cultures and avoiding all undesirable consequences of current practice.

  6. Coronagraphic Notch Filter for Raman Spectroscopy

    NASA Technical Reports Server (NTRS)

    Cohen, David; Stirbl, Robert

    2004-01-01

    A modified coronagraph has been proposed as a prototype of improved notch filters in Raman spectrometers. Coronagraphic notch filters could offer alternatives to both (1) the large and expensive double or triple monochromators in older Raman spectrometers and (2) holographic notch filters, which are less expensive but are subject to environmental degradation as well as to limitations of geometry and spectral range. Measurement of a Raman spectrum is an exercise in measuring and resolving faint spectral lines close to a bright peak: In Raman spectroscopy, a monochromatic beam of light (the pump beam) excites a sample of material that one seeks to analyze. The pump beam generates a small flux of scattered light at wavelengths slightly greater than that of the pump beam. The shift in wavelength of the scattered light from the pump wavelength is known in the art as the Stokes shift. Typically, the flux of scattered light is of the order of 10 7 that of the pump beam and the Stokes shift lies in the wave-number range of 100 to 3,000 cm 1. A notch filter can be used to suppress the pump-beam spectral peak while passing the nearby faint Raman spectral lines. The basic principles of design and operation of a coronagraph offer an opportunity for engineering the spectral transmittance of the optics in a Raman spectrometer. A classical coronagraph may be understood as two imaging systems placed end to end, such that the first system forms an intermediate real image of a nominally infinitely distant object and the second system forms a final real image of the intermediate real image. If the light incident on the first telescope is collimated, then the intermediate image is a point-spread function (PSF). If an appropriately tailored occulting spot (e.g., a Gaussian-apodized spot with maximum absorption on axis) is placed on the intermediate image plane, then the instrument inhibits transmission of light from an on-axis source. However, the PSFs of off-axis light sources are

  7. In vivo Raman spectroscopy of cervix cancers

    NASA Astrophysics Data System (ADS)

    Rubina, S.; Sathe, Priyanka; Dora, Tapas Kumar; Chopra, Supriya; Maheshwari, Amita; Krishna, C. Murali

    2014-03-01

    Cervix-cancer is the third most common female cancer worldwide. It is the leading cancer among Indian females with more than million new diagnosed cases and 50% mortality, annually. The high mortality rates can be attributed to late diagnosis. Efficacy of Raman spectroscopy in classification of normal and pathological conditions in cervix cancers on diverse populations has already been demonstrated. Our earlier ex vivo studies have shown the feasibility of classifying normal and cancer cervix tissues as well as responders/non-responders to Concurrent chemoradiotherapy (CCRT). The present study was carried out to explore feasibility of in vivo Raman spectroscopic methods in classifying normal and cancerous conditions in Indian population. A total of 182 normal and 132 tumor in vivo Raman spectra, from 63 subjects, were recorded using a fiberoptic probe coupled HE-785 spectrometer, under clinical supervision. Spectra were acquired for 5 s and averaged over 3 times at 80 mW laser power. Spectra of normal conditions suggest strong collagenous features and abundance of non-collagenous proteins and DNA in case of tumors. Preprocessed spectra were subjected to Principal Component-Linear Discrimination Analysis (PCLDA) followed by leave-one-out-cross-validation. Classification efficiency of ~96.7% and 100% for normal and cancerous conditions respectively, were observed. Findings of the study corroborates earlier studies and suggest applicability of Raman spectroscopic methods in combination with appropriate multivariate tool for objective, noninvasive and rapid diagnosis of cervical cancers in Indian population. In view of encouraging results, extensive validation studies will be undertaken to confirm the findings.

  8. Characterization and identification of contraband using UV resonant Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Lacey, Richard J.; Hayward, Ian P.; Sands, H. S.; Batchelder, David N.

    1997-02-01

    A range of explosives and narcotics have been examined using Raman spectroscopy with 244 nm excitation. This wavelength of excitation eliminates the fluorescence problems associated with excitation at visible wavelengths. Comparison with spectra obtained using visible excitation reveals that resonance Raman scattering is occurring. This results in simplified spectra, and enhanced Raman scattering efficiencies.

  9. Resonant Raman spectroscopy of twisted multilayer graphene

    NASA Astrophysics Data System (ADS)

    Wu, Jiang-Bin; Zhang, Xin; Ijäs, Mari; Han, Wen-Peng; Qiao, Xiao-Fen; Li, Xiao-Li; Jiang, De-Sheng; Ferrari, Andrea C.; Tan, Ping-Heng

    2014-11-01

    Graphene and other two-dimensional crystals can be combined to form various hybrids and heterostructures, creating materials on demand with properties determined by the interlayer interaction. This is the case even for a single material, where multilayer stacks with different relative orientation have different optical and electronic properties. Probing and understanding the interface coupling is thus of primary importance for fundamental science and applications. Here we study twisted multilayer graphene flakes with multi-wavelength Raman spectroscopy. We find a significant intensity enhancement of the interlayer coupling modes (C peaks) due to resonance with new optically allowed electronic transitions, determined by the relative orientation of the layers. The interlayer coupling results in a Davydov splitting of the C peak in systems consisting of two equivalent graphene multilayers. This allows us to directly quantify the interlayer interaction, which is much smaller compared with Bernal-stacked interfaces. This paves the way to the use of Raman spectroscopy to uncover the interface coupling of two-dimensional hybrids and heterostructures.

  10. Combined fiber probe for fluorescence lifetime and Raman spectroscopy

    PubMed Central

    Dochow, Sebastian; Ma, Dinglong; Latka, Ines; Bocklitz, Thomas; Hartl, Brad; Bec, Julien; Fatakdawala, Hussain; Marple, Eric; Urmey, Kirk; Wachsmann-Hogiu, Sebastian; Schmitt, Michael; Marcu, Laura; Popp, Jürgen

    2016-01-01

    In this contribution we present a dual modality fiber optic probe combining fluorescence lifetime imaging (FLIm) and Raman spectroscopy for in vivo endoscopic applications. The presented multi-spectroscopy probe enables efficient excitation and collection of fluorescence lifetime signals for FLIm in the UV/visible wavelength region, as well as of Raman spectra in the near-IR for simultaneous Raman/FLIm imaging. The probe was characterized in terms of its lateral resolution and distance dependency of the Raman and FLIm signals. In addition, the feasibility of the probe for in vivo FLIm and Raman spectral characterization of tissue was demonstrated. PMID:26093843

  11. Determining the Authenticity of Gemstones Using Raman Spectroscopy

    NASA Astrophysics Data System (ADS)

    Aponick, Aaron; Marchozzi, Emedio; Johnston, Cynthia R.; Wigal, Carl T.

    1998-04-01

    The benefits of laser spectroscopy in the undergraduate curriculum have been the focus of several recent articles in this journal. Raman spectroscopy has been of particular interest since the similarities of Raman to conventional infrared spectroscopy make the interpretation of spectral data well within undergraduate comprehension. In addition, the accessibility to this technology is now within the reach of most undergraduate institutions. This paper reports the development of an experiment using Raman spectroscopy which determines the authenticity of both diamonds and pearls. The resulting spectra provide an introduction to vibrational spectroscopy and can be used in a variety of laboratory courses ranging from introductory chemistry to instrumental analysis.

  12. Ultra high resolution molecular beam cars spectroscopy with application to planetary atmospheric molecules

    NASA Technical Reports Server (NTRS)

    Byer, R. L.

    1982-01-01

    The measurement of high resolution pulsed and continuous wave (CW) coherent anti-Stokes Raman spectroscopy (CARS) measurements in pulsed and steady state supersonic expansions were demonstrated. Pulsed molecular beam sources were characterized, and saturation of a Raman transition and, for the first time, the Raman spectrum of a complex molecular cluster were observed. The observation of CW CARS spectra in a molecular expansion and the effects of transit time broadening is described. Supersonic expansion is established as a viable technique for high resolution Raman spectroscopy of cold molecules with resolutions of 100 MH2.

  13. In-line interferometric femtosecond stimulated Raman scattering spectroscopy.

    PubMed

    Dobner, Sven; Groß, Petra; Fallnich, Carsten

    2013-06-28

    We present in-line interferometric femtosecond stimulated Raman scattering (II-FSRS), a new method to measure the spectral Raman intensity and phase over a broad spectral range, potentially in a single shot. An analytic model is developed, that excellently reproduces the measured spectra. Additionally, the performance of II-FSRS is directly compared in experiments to two established techniques, namely femtosecond stimulated Raman scattering and femtosecond Raman induced Kerr-effect spectroscopy.

  14. Coherent Raman Studies of Shocked Liquids

    NASA Astrophysics Data System (ADS)

    McGrane, Shawn; Brown, Kathryn; Dang, Nhan; Bolme, Cynthia; Moore, David

    2013-06-01

    Transient vibrational spectroscopies offer the potential to directly observe time dependent shock induced chemical reaction kinetics. We report recent experiments that couple a hybrid picosecond/femtosecond coherent anti-Stokes Raman spectroscopy (CARS) diagnostic with our tabletop ultrafast laser driven shock platform. Initial results on liquids shocked to 20 GPa suggest that sub-picosecond dephasing at high pressure and temperature may limit the application of this nonresonant background free version of CARS. Initial results using interferometric CARS to increase sensitivity and overcome these limitations will be presented.

  15. Evaluating internal maturity of tomatoes using spatially offset Raman spectroscopy

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Spatially offset Raman spectroscopy technique was investigated for evaluating internal maturity of intact tomatoes. A Raman spectroscopy system was assembled to acquire spatially offset spectra in the wavenumber range of 200–2500 cm–1. A 785-nm laser was used as the excitation source and the measure...

  16. The hallmarks of breast cancer by Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Abramczyk, H.; Surmacki, J.; Brożek-Płuska, B.; Morawiec, Z.; Tazbir, M.

    2009-04-01

    This paper presents new biological results on ex vivo breast tissue based on Raman spectroscopy and demonstrates its power as diagnostic tool with the key advantage in breast cancer research. The results presented here demonstrate the ability of Raman spectroscopy to accurately characterize cancer tissue and distinguish between normal, malignant and benign types. The goal of the paper is to develop the diagnostic ability of Raman spectroscopy in order to find an optical marker of cancer in the breast tissue. Applications of Raman spectroscopy in breast cancer research are in the early stages of development in the world. To the best of our knowledge, this paper is one of the most statistically reliable reports (1100 spectra, 99 patients) on Raman spectroscopy-based diagnosis of breast cancers among the world women population.

  17. Raman Spectrometric Detection Methods for Early and Non-Invasive Diagnosis of Alzheimer's Disease.

    PubMed

    Huang, Chia-Chi; Isidoro, Ciro

    2017-03-18

    The continuous increasing rate of patients suffering of Alzheimer's disease (AD) worldwide requires the adoption of novel techniques for non-invasive early diagnosis and monitoring of the disease. Here we review the various Raman spectroscopic techniques, including Fourier Transform-Raman spectroscopy, surface-enhanced Raman scattering spectroscopy, coherent anti-Stokes Raman scattering spectroscopy, and confocal Raman microspectroscopy, that could be used for the diagnosis of AD. These techniques have shown the potential to detect AD biomarkers, such as the amyloid-β peptide and the tau protein, or the neurotransmitters involved in the disease (e.g., Glutamate and γ-Aminobutyric acid), or the typical structural alterations in specific brain areas. The possibility to detect the specific biomarkers in liquid biopsies and to obtain high resolution 3D microscope images of the affected area make the Raman spectroscopy a valuable ally in the early diagnosis and monitoring of AD.

  18. Raman spectroscopy explores molecular structural signatures of hidden materials in depth: Universal Multiple Angle Raman Spectroscopy

    PubMed Central

    Sil, Sanchita; Umapathy, Siva

    2014-01-01

    Non-invasive 3D imaging in materials and medical research involves methodologies such as X-ray imaging, MRI, fluorescence and optical coherence tomography, NIR absorption imaging, etc., providing global morphological/density/absorption changes of the hidden components. However, molecular information of such buried materials has been elusive. In this article we demonstrate observation of molecular structural information of materials hidden/buried in depth using Raman scattering. Typically, Raman spectroscopic observations are made at fixed collection angles, such as, 90°, 135°, and 180°, except in spatially offset Raman scattering (SORS) (only back scattering based collection of photons) and transmission techniques. Such specific collection angles restrict the observations of Raman signals either from or near the surface of the materials. Universal Multiple Angle Raman Spectroscopy (UMARS) presented here employs the principle of (a) penetration depth of photons and then diffuse propagation through non-absorbing media by multiple scattering and (b) detection of signals from all the observable angles. PMID:24930768

  19. Measurement of clathrate hydrates via Raman spectroscopy

    USGS Publications Warehouse

    Sum, A.K.; Burruss, R.C.; Sloan, E.D.

    1997-01-01

    Raman spectra of clathrate hydrate guest molecules are presented for three known structures (I (sI), II (sII), and H (sH)) in the following systems: CH4 (sI), CO2 (sI), C3H8 (sII), CH4 + CO2 (sI), CD4 + C3H8 (sII), CH4 + N2 (sI), CH4 + THF-d8 (sII), and CH4 + C7D14 (sH). Relative occupancy of CH4 in the large and small cavities of sI were determined by deconvoluting the ??1 symmetric bands, resulting in hydration numbers of 6.04 ?? 0.03. The frequency of the ??1 bands for CH4 in structures I, II, and H differ statistically, so that Raman spectroscopy is a potential tool to identify hydrate crystal structure. Hydrate guest compositions were also measured for two vapor compositions of the CH4 + CO2 system, and they compared favorably with predictions. The large cavities were measured to be almost fully occupied by CH4 and CO2, whereas only a small fraction of the small cavities are occupied by CH4. No CO2 was found in the small cavities. Hydration numbers from 7.27 to 7.45 were calculated for the mixed hydrate.

  20. Raman spectroscopy of ion irradiated diamond

    NASA Astrophysics Data System (ADS)

    Brunetto, R.; Baratta, G. A.; Strazzulla, G.

    2004-07-01

    Ion irradiation experiments of diamond samples at room temperature have been performed by using in situ Raman spectroscopy as diagnostic technique. Different ions are used with energies of 200 or 400 keV. The area of virgin diamond Raman band (at 1332 cm-1) decreases exponentially as the ion fluence increases. This is due to changes in the optical properties of the damaged samples in the visible spectral range. Results from different ions demonstrate that this effect is correlated with the number of displacements/cm2, i.e., with the energy lost by ions through elastic collisions with target nuclei. Amorphous carbon (sp2) is formed after a threshold of about 2×1022 vacancies/cm3, or about 16 eV/C-atom deposited by elastic collisions. The peak position and full width at half maximum of the D line and G line of the synthesized amorphous carbon are studied. In particular, the G-line peak position shifts from the initial 1545 cm-1 to about 1515 cm-1 at the higher doses. The results are also discussed in view of their relevance in astrophysical environments.

  1. Combined fiber probe for fluorescence lifetime and Raman spectroscopy.

    PubMed

    Dochow, Sebastian; Ma, Dinglong; Latka, Ines; Bocklitz, Thomas; Hartl, Brad; Bec, Julien; Fatakdawala, Hussain; Marple, Eric; Urmey, Kirk; Wachsmann-Hogiu, Sebastian; Schmitt, Michael; Marcu, Laura; Popp, Jürgen

    2015-11-01

    In this contribution we present a dual modality fiber optic probe combining fluorescence lifetime imaging (FLIm) and Raman spectroscopy for in vivo endoscopic applications. The presented multi-spectroscopy probe enables efficient excitation and collection of fluorescence lifetime signals for FLIm in the UV/visible wavelength region, as well as of Raman spectra in the near-IR for simultaneous Raman/FLIm imaging. The probe was characterized in terms of its lateral resolution and distance dependency of the Raman and FLIm signals. In addition, the feasibility of the probe for in vivo FLIm and Raman spectral characterization of tissue was demonstrated. Graphical Abstract An image comparison between FLIm and Raman spectroscopy acquired with the bimodal probe onseveral tissue samples.

  2. Raman Spectroscopy of Optically Trapped Single Biological Micro-Particles.

    PubMed

    Redding, Brandon; Schwab, Mark; Pan, Yong-le

    2015-08-04

    The combination of optical trapping with Raman spectroscopy provides a powerful method for the study, characterization, and identification of biological micro-particles. In essence, optical trapping helps to overcome the limitation imposed by the relative inefficiency of the Raman scattering process. This allows Raman spectroscopy to be applied to individual biological particles in air and in liquid, providing the potential for particle identification with high specificity, longitudinal studies of changes in particle composition, and characterization of the heterogeneity of individual particles in a population. In this review, we introduce the techniques used to integrate Raman spectroscopy with optical trapping in order to study individual biological particles in liquid and air. We then provide an overview of some of the most promising applications of this technique, highlighting the unique types of measurements enabled by the combination of Raman spectroscopy with optical trapping. Finally, we present a brief discussion of future research directions in the field.

  3. Raman Spectroscopy of Optically Trapped Single Biological Micro-Particles

    PubMed Central

    Redding, Brandon; Schwab, Mark J.; Pan, Yong-le

    2015-01-01

    The combination of optical trapping with Raman spectroscopy provides a powerful method for the study, characterization, and identification of biological micro-particles. In essence, optical trapping helps to overcome the limitation imposed by the relative inefficiency of the Raman scattering process. This allows Raman spectroscopy to be applied to individual biological particles in air and in liquid, providing the potential for particle identification with high specificity, longitudinal studies of changes in particle composition, and characterization of the heterogeneity of individual particles in a population. In this review, we introduce the techniques used to integrate Raman spectroscopy with optical trapping in order to study individual biological particles in liquid and air. We then provide an overview of some of the most promising applications of this technique, highlighting the unique types of measurements enabled by the combination of Raman spectroscopy with optical trapping. Finally, we present a brief discussion of future research directions in the field. PMID:26247952

  4. Raman spectroscopy of human saliva for acute myocardial infarction detection

    NASA Astrophysics Data System (ADS)

    Chen, Maowen; Chen, Yuanxiang; Wu, Shanshan; Huang, Wei; Lin, Jinyong; Weng, Guo-Xing; Chen, Rong

    2014-09-01

    Raman spectroscopy is a rapidly non-invasive technique with great potential for biomedical research. The aim of this study was to evaluate the feasibility of using Raman spectroscopy of human saliva for acute myocardial infarction (AMI) detection. Raman spectroscopy measurements were performed on two groups of saliva samples: one group from patients (n=30) with confirmed AMI and the other group from healthy controls (n=31). The diagnostic performance for differentiating AMI saliva from normal saliva was evaluated by multivariate statistical analysis. The combination of principal component analysis (PCA) and linear discriminate analysis (LDA) of the measured Raman spectra separated the spectral features of the two groups into two distinct clusters with little overlaps, rendering the sensitivity of 80.0% and specificity of 80.6%. The results from this exploratory study demonstrated that Raman spectroscopy of human saliva can serve as a potentially clinical tool for rapid AMI detection and screening.

  5. In situ cellular level Raman spectroscopy of the thyroid.

    PubMed

    Law, Alan Wing Lun; Ahmed, Rafay; Cheung, Tsz Wing; Mak, Chun Yu; Lau, Condon

    2017-02-01

    We report a novel Raman spectroscopy method for in situ cellular level analysis of the thyroid. Thyroids are harvested from control and lithium treated mice. Lithium is used to treat bipolar disorder, but affects thyroid function. Raman spectra are acquired with a confocal setup (514 nm laser, 20 µm spot) focused on a follicular lumen. Raman peaks are observed at 1440, 1656, and 1746 cm(-1), corresponding to tyrosine, an important amino acid for protein synthesis. Peaks are also observed at 563, 1087, 1265 and 1301 cm(-1). With lithium, the tyrosine peaks increase, indicating tyrosine buildup. Raman spectroscopy can study the impact of many exogenous treatments on thyroid biochemistry.

  6. Raman spectroscopy for optical diagnosis of laryngeal cancer

    NASA Astrophysics Data System (ADS)

    Teh, Seng Khoon; Zheng, Wei; Lau, David P.; Huang, Zhiwei

    2008-02-01

    In this report, the diagnostic ability of near-infrared (NIR) Raman spectroscopy for identifying the malignant tumors from normal tissues in the larynx was studied. A rapid NIR Raman system was utilized. Multivariate statistical techniques were employed to develop effective diagnostic algorithms. Raman spectra in the range of 800-1,800 cm-1 differed significantly between normal and malignant tumor tissues. The diagnostic algorithms can yielded a diagnostic sensitivity of 92.9% and specificity 83.3% for separating malignant tumors from normal laryngeal tissues. NIR Raman spectroscopy with multivariate statistical techniques has a potential for the non-invasive detection of malignant tumors in the larynx.

  7. In situ cellular level Raman spectroscopy of the thyroid

    PubMed Central

    Law, Alan Wing Lun; Ahmed, Rafay; Cheung, Tsz Wing; Mak, Chun Yu; Lau, Condon

    2017-01-01

    We report a novel Raman spectroscopy method for in situ cellular level analysis of the thyroid. Thyroids are harvested from control and lithium treated mice. Lithium is used to treat bipolar disorder, but affects thyroid function. Raman spectra are acquired with a confocal setup (514 nm laser, 20 µm spot) focused on a follicular lumen. Raman peaks are observed at 1440, 1656, and 1746 cm−1, corresponding to tyrosine, an important amino acid for protein synthesis. Peaks are also observed at 563, 1087, 1265 and 1301 cm−1. With lithium, the tyrosine peaks increase, indicating tyrosine buildup. Raman spectroscopy can study the impact of many exogenous treatments on thyroid biochemistry. PMID:28270975

  8. NONLINEAR OPTICS: Coherent laser spectroscopy of matter utilizing waveguide structures

    NASA Astrophysics Data System (ADS)

    Chaus, A. I.; Yashkir, Yu N.

    1990-07-01

    Some features of CARS spectroscopy in waveguide structures are investigated theoretically taking into account stimulated Raman amplification of a weak pump wave in the field of a strong wave and allowing for the phase matching. A four-photon intermode coupling which occurs under amplification conditions results in energy diffusion between different modes. General expressions for the intensities of the pump waves undergoing stimulated amplification and for the anti-Stokes signal are derived and analyzed.

  9. From Femtosecond Dynamics to Breast Cancer Diagnosis by Raman Spectroscopy

    NASA Astrophysics Data System (ADS)

    Abramczyk, H.; Placek, I.; BroŻek-Płuska, B.; Kurczewski, K.; Morawiec, Z.; Tazbir, M.

    2007-12-01

    This paper presents new results based on Raman spectroscopy and demonstrates its utilisation as a diagnostic and development tool with the key advantage in breast cancer research. Applications of Raman spectroscopy in cancer research are in the early stages of development. However, research presented here as well as performed in a few other laboratories demonstrate the ability of Raman spectroscopy to accurately characterize cancer tissue and distinguish between normal, malignant and benign types. The main goals of bio-Raman spectroscopy at this stage are threefold. Firstly, the aim is to develop the diagnostic ability of Raman spectroscopy so it can be implemented in a clinical environment, producing accurate and rapid diagnoses. Secondly, the aim is to optimize the technique as a diagnostic tool for the non-invasive real time medical applications. Thirdly, the aim is to formulate some hypothesis based on Raman spectroscopy on the molecular mechanism which drives the transformation of normal human cells into highly malignant derivatives. To the best of our knowledge, this is the most statistically reliable report on Raman spectroscopy-based diagnosis of breast cancers among the world women population.

  10. From Femtosecond Dynamics to Breast Cancer Diagnosis by Raman Spectroscopy

    SciTech Connect

    Abramczyk, H.; Placek, I.; Brozek-Pluska, B.; Kurczewski, K.; Morawiec, Z.; Tazbir, M.

    2007-12-26

    This paper presents new results based on Raman spectroscopy and demonstrates its utilisation as a diagnostic and development tool with the key advantage in breast cancer research. Applications of Raman spectroscopy in cancer research are in the early stages of development. However, research presented here as well as performed in a few other laboratories demonstrate the ability of Raman spectroscopy to accurately characterize cancer tissue and distinguish between normal, malignant and benign types. The main goals of bio-Raman spectroscopy at this stage are threefold. Firstly, the aim is to develop the diagnostic ability of Raman spectroscopy so it can be implemented in a clinical environment, producing accurate and rapid diagnoses. Secondly, the aim is to optimize the technique as a diagnostic tool for the non-invasive real time medical applications. Thirdly, the aim is to formulate some hypothesis based on Raman spectroscopy on the molecular mechanism which drives the transformation of normal human cells into highly malignant derivatives. To the best of our knowledge, this is the most statistically reliable report on Raman spectroscopy-based diagnosis of breast cancers among the world women population.

  11. Optimizing coherent Raman scattering with plasmonic nanoparticles

    NASA Astrophysics Data System (ADS)

    Voronine, Dmitri; Hua, Xia; Sinyukov, Alexander; Ballmann, Charles; Sokolov, Alexei; Scully, Marlan

    2013-03-01

    Two commonly used techniques that provide species-specific spectroscopic signals in the form of vibrational fingerprints are surface-enhanced Raman scattering (SERS) and coherent anti-Stokes Raman scattering (CARS) spectroscopies. In order to enhance the signal, SERS takes advantage of the electromagnetic near-field enhancement while CARS employs molecular coherence. We have combined these two techniques to achieve best-of-both-worlds maximum signal enhancement by using optimized laser pulse shaping and time-resolved detection. We applied this new time-resolved surface-enhanced coherent anti-Stokes Raman scattering (tr-SECARS) technique to investigate various molecular complexes in a vicinity of gold nanoparticles. While large signal enhancement has previously been achieved in SERS, surfaced-enhanced coherent signals have shown lower values. We investigate the mechanisms of these effects by analyzing the spatial dependence of the coherent Raman spectra for different hot spots in aggregated plasmonic nanoparticles. Understanding coherence effects in surface-enhanced Raman scattering may lead to improved nanoscale sensors.

  12. Raman versus CARS microscopy: when one is better than the other

    NASA Astrophysics Data System (ADS)

    Petrov, G. I.; Arora, R.; Saha, A.; Heathcote, R. D.; Ravula, S.; Brener, I.; Yakovlev, V. V.

    2007-02-01

    Since the first introduction of Raman microscope in 1973, optical and laser technology has made a tremendous step forward. However, despite of the obvious advantages of being a very informative and nondestructive method of studying biological samples, spontaneous Raman scattering suffers from a series of limitations such as a fluorescent background and a low signal level. Nonlinear Raman spectroscopy and, in particular, spectroscopy of coherent anti-Stokes Raman scattering (CARS) can resolve most of the problems associated with conventional Raman spectroscopy. In this report, the most critical issues of the CARS microspectroscopy setup design are reviewed and several exciting potential applications of the broadband CARS microspectroscopy, where the CARS microscopy has an advantage with respect to Raman microscopy, are outlined.

  13. Raman spectroscopy of gliomas: an exploratory study

    NASA Astrophysics Data System (ADS)

    Shenoy, Mahesh; Hole, Arti R.; Shridhar, E.; Moiyadi, Aliasgar V.; Krishna, C. Murali

    2014-03-01

    Gliomas are extremely infiltrative type of brain cancers, the borders of which are difficult to locate. Gliomas largely consist of tumors of astrocytic or oligodendroglial lineage. Usually stereotactic surgery is performed to obtain tumor tissue sample. Complete excision of these tumors with preservation of uninvolved normal areas is important during brain tumor surgeries. The present study was undertaken to explore feasibility of classifying abnormal and normal glioma tissues with Raman spectroscopy (RS). RS is a nondestructive vibrational spectroscopic technique, which provides information about molecular composition, molecular structures and molecular interactions in tissue. Postoperated 33 (20-abnormal and 13-normal) gliomas tissue samples of different grades were collected under clinical supervision. Five micron section from tissue sample was used for confirmatory histopathological diagnosis while the remaining tissue was placed on CaF2 window and spectra were acquired using a fiberoptic-probe-coupled HE-785 Raman-spectrometer. Spectral acquisition parameters were laser power-80mW, integration-20s and averaged over 3 accumulations. Spectra were pre-processed and subjected to unsupervised Principal-Component Analysis (PCA) to identify trends of classification. Supervised PC-LDA (Principal-Component-Linear-Discriminant Analysis) was used to develop standard-models using spectra of 12 normal and abnormal specimens each. Leave-one-out crossvalidation yielded classification-efficiency of 90% and 80% for normal and abnormal conditions, respectively. Evaluation with an independent-test data-set comprising of 135 spectra of 9 samples provided sensitivity of 100% and specificity of 70%. Findings of this preliminary study may pave way for objective tumor margin assessment during brain surgery.

  14. Forensic and homeland security applications of modern portable Raman spectroscopy.

    PubMed

    Izake, Emad L

    2010-10-10

    Modern detection and identification of chemical and biological hazards within the forensic and homeland security contexts may well require conducting the analysis in field while adapting a non-contact approach to the hazard. Technological achievements on both surface and resonance enhancement Raman scattering re-developed Raman spectroscopy to become the most adaptable spectroscopy technique for stand-off and non-contact analysis of hazards. On the other hand, spatially offset Raman spectroscopy proved to be very valuable for non-invasive chemical analysis of hazards concealed within non-transparent containers and packaging.

  15. Periodontitis diagnostics using resonance Raman spectroscopy on saliva

    NASA Astrophysics Data System (ADS)

    Gonchukov, S.; Sukhinina, A.; Bakhmutov, D.; Biryukova, T.; Tsvetkov, M.; Bagratashvily, V.

    2013-07-01

    In view of its wealth of molecular information, Raman spectroscopy has been the subject of active biomedical research. The aim of this work is Raman spectroscopy (RS) application for the determination of molecular biomarkers in saliva with the objective of early periodontitis detection. As was shown in our previous study, carotenoids contained in saliva can be molecular fingerprint information for the periodontitis level. It is shown here that the carotenoid RS lines at wavenumbers of 1156 and 1524 cm-1 can be easily detected and serve as reliable biomarkers of periodontitis using resonance Raman spectroscopy of dry saliva.

  16. Nanoparticle Based Surface-Enhanced Raman Spectroscopy

    SciTech Connect

    Talley, C E; Huser, T R; Hollars, C W; Jusinski, L; Laurence, T; Lane, S M

    2005-01-03

    Surface-enhanced Raman scattering is a powerful tool for the investigation of biological samples. Following a brief introduction to Raman and surface-enhanced Raman scattering, several examples of biophotonic applications of SERS are discussed. The concept of nanoparticle based sensors using SERS is introduced and the development of these sensors is discussed.

  17. Investigation of biomineralization by Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Fatscher, Robert William

    Biomineralization is a process in which living organism grow composite materials consisting of inorganic and organic materials. This produces a composite material consisting of both inorganic and organic components, with superior mechanical properties. In the human body bone and dentin are both examples of biominerals. In this research Raman spectroscopy was used to characterize dentin from mice and human teeth, to determine composition. In the mouse tooth samples areas of irregular dentin were found, along the inside of the tooth, to be in the process of mineralization. By analyzing the samples along these areas we were able to determine the composition of dentin and track how it changed in these area. By analysis of the mineral to matrix ratio the areas of irregular dentin were determined to have less mineral present. Observations of other organic components and collagen in increased concentrations in this area suggested these area were in the process of biomineralization. The understanding of the structure of dentin and its biomineralization process is of crucial importance when trying reproduce dentin. Scientists and engineers are able to produce dentin minerals in vitro by culturing various dental stem cells. The ability to create dentin mineral from cells could lead to methods of repairing dentin in patients, or even lead to the creation of a completely engineered tooth. While dentin-like materials can be produced in a laboratory environment, analysis and comparison of the composition of these materials must be performed to ensure the mineral produced is consistent with dentin. Mineralized nodules from six different dental stem cell lines were cultured to produce a mineralized deposit. Utilizing Raman spectroscopy, we were able to determine cell source dependent differences in a variety of dental stem cells, and compare the mineral produced to native dentin. Orthopedic implants are implants used to replace damaged bone, examples include knee, hip and dental

  18. Sensitivity of Raman spectroscopy to normal patient variability

    PubMed Central

    Vargis, Elizabeth; Byrd, Teresa; Logan, Quinisha; Khabele, Dineo; Mahadevan-Jansen, Anita

    2011-01-01

    Many groups have used Raman spectroscopy for diagnosing cervical dysplasia; however, there have been few studies looking at the effect of normal physiological variations on Raman spectra. We assess four patient variables that may affect normal Raman spectra: Race/ethnicity, body mass index (BMI), parity, and socioeconomic status. Raman spectra were acquired from a diverse population of 75 patients undergoing routine screening for cervical dysplasia. Classification of Raman spectra from patients with a normal cervix is performed using sparse multinomial logistic regression (SMLR) to determine if any of these variables has a significant effect. Results suggest that BMI and parity have the greatest impact, whereas race/ethnicity and socioeconomic status have a limited effect. Incorporating BMI and obstetric history into classification algorithms may increase sensitivity and specificity rates of disease classification using Raman spectroscopy. Studies are underway to assess the effect of these variables on disease. PMID:22112136

  19. Sensitivity of Raman spectroscopy to normal patient variability

    NASA Astrophysics Data System (ADS)

    Vargis, Elizabeth; Byrd, Teresa; Logan, Quinisha; Khabele, Dineo; Mahadevan-Jansen, Anita

    2011-11-01

    Many groups have used Raman spectroscopy for diagnosing cervical dysplasia; however, there have been few studies looking at the effect of normal physiological variations on Raman spectra. We assess four patient variables that may affect normal Raman spectra: Race/ethnicity, body mass index (BMI), parity, and socioeconomic status. Raman spectra were acquired from a diverse population of 75 patients undergoing routine screening for cervical dysplasia. Classification of Raman spectra from patients with a normal cervix is performed using sparse multinomial logistic regression (SMLR) to determine if any of these variables has a significant effect. Results suggest that BMI and parity have the greatest impact, whereas race/ethnicity and socioeconomic status have a limited effect. Incorporating BMI and obstetric history into classification algorithms may increase sensitivity and specificity rates of disease classification using Raman spectroscopy. Studies are underway to assess the effect of these variables on disease.

  20. Real-time in vivo cancer diagnosis using Raman spectroscopy.

    PubMed

    Wang, Wenbo; Zhao, Jianhua; Short, Michael; Zeng, Haishan

    2015-07-01

    Raman spectroscopy has becoming a practical tool for rapid in vivo tissue diagnosis. This paper provides an overview on the latest development of real-time in vivo Raman systems for cancer detection. Instrumentation, data handling, as well as oncology applications of Raman techniques were covered. Optic fiber probes designs for Raman spectroscopy were discussed. Spectral data pre-processing, feature extraction, and classification between normal/benign and malignant tissues were surveyed. Applications of Raman techniques for clinical diagnosis for different types of cancers, including skin cancer, lung cancer, stomach cancer, oesophageal cancer, colorectal cancer, cervical cancer, and breast cancer, were summarized. Schematic of a real-time Raman spectrometer for skin cancer detection. Without correction, the image captured on CCD camera for a straight entrance slit has a curvature. By arranging the optic fiber array in reverse orientation, the curvature could be effectively corrected.

  1. Application of Raman Spectroscopy for Nondestructive Evaluation of Composite Materials

    NASA Technical Reports Server (NTRS)

    Washer, Glenn A.; Brooks, Thomas M. B.; Saulsberry, Regor

    2007-01-01

    This paper will present an overview of efforts to investigate the application of Raman spectroscopy for the characterization of Kevlar materials. Raman spectroscopy is a laser technique that is sensitive to molecular interactions in materials such as Kevlar, graphite and carbon used in composite materials. The overall goal of this research reported here is to evaluate Raman spectroscopy as a potential nondestructive evaluation (NDE) tool for the detection of stress rupture in Kevlar composite over-wrapped pressure vessels (COPVs). Characterization of the Raman spectra of Kevlar yarn and strands will be presented and compared with analytical models provided in the literature. Results of testing to investigate the effects of creep and high-temperature aging on the Raman spectra will be presented.

  2. Application of Raman spectroscopy to forensic fibre cases.

    PubMed

    Lepot, L; De Wael, K; Gason, F; Gilbert, B

    2008-09-01

    Five forensic fibre cases in which Raman spectroscopy proved to be a good complementary method for microspectrophotometry (MSP) are described. Absorption spectra in the visible range are indeed sometimes characteristic ofa certain dye but this one can be subsequently identified unambiguously by Raman spectroscopy using a spectral library. In other cases the comparison of Raman spectra of reference fibres and suspect fibres led to an improvement of the discrimination power. The Raman measurements have been performed directly on mounted fibres and the spectra showed only little interference from the mounting resin and glass. Raman spectroscopy is therefore a powerful method that can be applied in routine fibre analysis following optical microscopy and MSP measurements.

  3. Clinical instrumentation and applications of Raman spectroscopy

    PubMed Central

    Pence, Isaac

    2016-01-01

    Clinical diagnostic devices provide new sources of information that give insight about the state of health which can then be used to manage patient care. These tools can be as simple as an otoscope to better visualize the ear canal or as complex as a wireless capsule endoscope to monitor the gastrointestinal tract. It is with tools such as these that medical practitioners can determine when a patient is healthy and to make an appropriate diagnosis when he/she is not. The goal of diagnostic medicine then is to efficiently determine the presence and cause of disease in order to provide the most appropriate intervention. The earliest form of medical diagnostics relied on the eye – direct visual observation of the interaction of light with the sample. This technique was espoused by Hippocrates in his 5th century BCE work Epidemics, in which the pallor of a patient’s skin and the coloring of the bodily fluids could be indicative of health. In the last hundred years, medical diagnosis has moved from relying on visual inspection to relying on numerous technological tools that are based on various types of interaction of the sample with different types of energy – light, ultrasound, radio waves, X-rays etc. Modern advances in science and technology have depended on enhancing technologies for the detection of these interactions for improved visualization of human health. Optical methods have been focused on providing this information in the micron to millimeter scale while ultrasound, X-ray, and radio waves have been key in aiding in the millimeter to centimeter scale. While a few optical technologies have achieved the status of medical instruments, many remain in the research and development phase despite persistent efforts by many researchers in the translation of these methods for clinical care. Of these, Raman spectroscopy has been described as a sensitive method that can provide biochemical information about tissue state while maintaining the capability of

  4. Clinical instrumentation and applications of Raman spectroscopy.

    PubMed

    Pence, Isaac; Mahadevan-Jansen, Anita

    2016-04-07

    Clinical diagnostic devices provide new sources of information that give insight about the state of health which can then be used to manage patient care. These tools can be as simple as an otoscope to better visualize the ear canal or as complex as a wireless capsule endoscope to monitor the gastrointestinal tract. It is with tools such as these that medical practitioners can determine when a patient is healthy and to make an appropriate diagnosis when he/she is not. The goal of diagnostic medicine then is to efficiently determine the presence and cause of disease in order to provide the most appropriate intervention. The earliest form of medical diagnostics relied on the eye - direct visual observation of the interaction of light with the sample. This technique was espoused by Hippocrates in his 5th century BCE work Epidemics, in which the pallor of a patient's skin and the coloring of the bodily fluids could be indicative of health. In the last hundred years, medical diagnosis has moved from relying on visual inspection to relying on numerous technological tools that are based on various types of interaction of the sample with different types of energy - light, ultrasound, radio waves, X-rays etc. Modern advances in science and technology have depended on enhancing technologies for the detection of these interactions for improved visualization of human health. Optical methods have been focused on providing this information in the micron to millimeter scale while ultrasound, X-ray, and radio waves have been key in aiding in the millimeter to centimeter scale. While a few optical technologies have achieved the status of medical instruments, many remain in the research and development phase despite persistent efforts by many researchers in the translation of these methods for clinical care. Of these, Raman spectroscopy has been described as a sensitive method that can provide biochemical information about tissue state while maintaining the capability of delivering

  5. Optical parametric oscillator-based light source for coherent Raman scattering microscopy: practical overview

    NASA Astrophysics Data System (ADS)

    Brustlein, Sophie; Ferrand, Patrick; Walther, Nico; Brasselet, Sophie; Billaudeau, Cyrille; Marguet, Didier; Rigneault, Hervé

    2011-02-01

    We present the assets and constraints of using optical parametric oscillators (OPOs) to perform point scanning nonlinear microscopy and spectroscopy with special emphasis on coherent Raman spectroscopy. The difterent possible configurations starting with one OPO and two OPOs are described in detail and with comments that are intended to be practically useful for the user. Explicit examples on test samples such as nonlinear organic crystal, polystyrene beads, and fresh mouse tissues are given. Special emphasis is given to background-free coherent Raman anti-Stokes scattering (CARS) imaging, including CARS hyperspectral imaging in a fully automated mode with commercial OPOs.

  6. Applications of spatially offset Raman spectroscopy to defense and security

    NASA Astrophysics Data System (ADS)

    Guicheteau, Jason; Hopkins, Rebecca

    2016-05-01

    Spatially offset Raman spectroscopy (SORS) allows for sub-surface and through barrier detection and has applications in drug analysis, cancer detection, forensic science, as well as defense and security. This paper reviews previous efforts in SORS and other through barrier Raman techniques and presents a discussion on current research in defense and security applications.

  7. [Identification of B jade by Raman spectroscopy].

    PubMed

    Zu, En-dong; Chen, Da-peng; Zhang, Peng-xiang

    2003-02-01

    Raman spectroscopy has been found to be a useful tool for identification of bleached and polymer-impregnated jadeites (so-called B jade). The major advantage of this system over classical methods of gem testing is the non-destructive identification of inclusions in gemstones and the determination of organic fracture filling in jade. Fissures in jadeites have been filled with oils and various resins to enhance their clarity, such as paraffin wax, paraffin oil, AB glue and epoxy resins. They show different peaks depending on their chemical composition. The characteristic spectrum ranges from 1,200-1,700 cm-1 to 2,800-3,100 cm-1. The spectra of resins show that they all have four strongest peaks related with phenyl: two C-C stretching modes at 1,116 and 1,609 cm-1, respectively, one C-H stretching mode at 3,069 cm-1, and a in-plane C-H bending mode at 1,189 cm-1. In addition, other two -CH2, -CH3 stretching modes at 2,906 and 2,869 cm-1, respectively, are very similar to paraffin. Therefore, the peaks at 1,116, 1,609, 1,189 and 3,069 cm-1 are important in distinguishing resin from paraffin, and we can identify B jade depending on them.

  8. Wavelength dependent resonance Raman band intensity of broadband stimulated Raman spectroscopy of malachite green in ethanol

    NASA Astrophysics Data System (ADS)

    Cen, Qiongyan; He, Yuhan; Xu, Mei; Wang, Jingjing; Wang, Zhaohui

    2015-03-01

    Resonance broadband stimulated Raman spectroscopy of malachite green in ethanol has been performed. With a tuning picosecond visible laser source and a broadband Raman probe, the Raman gain and loss spectra have been measured simultaneously. By scanning the Raman pump across the first absorption band of the molecule, we found that the resonant Raman bands could be only seen when the pump laser tuned in the range of the red edge of the S1←S0 transition. Dispersive lineshapes of resonant Raman bands have been observed in the Raman loss spectra, while the line shape is normal (same as spontaneous Raman) in the Raman gain spectra. Although, the resonant bands in the loss spectrum are usually stronger than that in the gain spectrum, the band intensities of both loss and gain linearly increase with the pump energy. The relative magnitude of each corresponding resonant band in the Raman loss and gain varies with the pump wavelength. Mode specified Raman excitation profiles have been obtained through broadband stimulated Raman measurement.

  9. Comparison of Fresh and Aged TNT with Multiwavelength Raman Spectroscopy

    DTIC Science & Technology

    2014-12-04

    Naval Research Laboratory Washington, DC 20375-5320 NRL/MR/6730--14-9572 Comparison of Fresh and Aged TNT with Multiwavelength Raman Spectroscopy...NUMBER OF PAGES 17. LIMITATION OF ABSTRACT Comparison of Fresh and Aged TNT with Multiwavelength Raman Spectroscopy Robert Lunsford, Jacob Grun, and...fresh and aged variants. This is particularly true of UV aging which had the greater effect on the sample of the two aging processes tested

  10. Spatially offset Raman spectroscopy based on a line-scan hyperspectral Raman system

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Spatially offset Raman spectroscopy (SORS) is a technique that can obtain subsurface layered information by collecting Raman spectra from a series of surface positions laterally offset from the excitation laser. The current methods of SORS measurement are typically either slow due to mechanical move...

  11. Cutaneous porphyrins exhibit anti-stokes fluorescence that is detectable in sebum (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Tian, Giselle; Zeng, Haishan; Zhao, Jianhua; Wu, Zhenguo; Al Jasser, Mohammed; Lui, Harvey; Mclean, David I.

    2016-02-01

    Porphyrins produced by Propionibacterium acnes represent the principal fluorophore associated with acne, and appear as orange-red luminescence under the Wood's lamp. Assessment of acne based on Wood's lamp (UV) or visible light illumination is limited by photon penetration depth and has limited sensitivity for earlier stage lesions. Inducing fluorescence with near infrared (NIR) excitation may provide an alternative way to assess porphyrin-related skin disorders. We discovered that under 785 nm CW laser excitation PpIX powder exhibits fluorescence emission in the shorter wavelength range of 600-715 nm with an intensity that is linearly dependent on the excitation power. We attribute this shorter wavelength emission to anti-Stokes fluorescence. Similar anti-Stokes fluorescence was also detected focally in all skin-derived samples containing porphyrins. Regular (Stokes) fluorescence was present under UV and visible light excitation on ex vivo nasal skin and sebum from uninflamed acne, but not on nose surface smears or sebum from inflamed acne. Co-registered CW laser-excited anti-Stokes fluorescence and fs laser-excited multi-photon fluorescence images of PpIX powder showed similar features. In the skin samples because of the anti-Stokes effect, the NIR-induced fluorescence was presumably specific for porphyrins since there appeared to be no anti-Stokes emission signals from other typical skin fluorophores such as lipids, keratins and collagen. Anti-Stokes fluorescence under NIR CW excitation is more sensitive and specific for porphyrin detection than UV- or visible light-excited regular fluorescence and fs laser-excited multi-photon fluorescence. This approach also has higher image contrast compared to NIR fs laser-based multi-photon fluorescence imaging. The anti-Stokes fluorescence of porphyrins within sebum could potentially be applied to detecting and targeting acne lesions for treatment via fluorescence image guidance.

  12. Approximate chemical analysis of volcanic glasses using Raman spectroscopy

    PubMed Central

    Morgavi, Daniele; Hess, Kai‐Uwe; Neuville, Daniel R.; Borovkov, Nikita; Perugini, Diego; Dingwell, Donald B.

    2015-01-01

    The effect of chemical composition on the Raman spectra of a series of natural calcalkaline silicate glasses has been quantified by performing electron microprobe analyses and obtaining Raman spectra on glassy filaments (~450 µm) derived from a magma mingling experiment. The results provide a robust compositionally‐dependent database for the Raman spectra of natural silicate glasses along the calcalkaline series. An empirical model based on both the acquired Raman spectra and an ideal mixing equation between calcalkaline basaltic and rhyolitic end‐members is constructed enabling the estimation of the chemical composition and degree of polymerization of silicate glasses using Raman spectra. The model is relatively insensitive to acquisition conditions and has been validated using the MPI‐DING geochemical standard glasses1 as well as further samples. The methods and model developed here offer several advantages compared with other analytical and spectroscopic methods such as infrared spectroscopy, X‐ray fluorescence spectroscopy, electron and ion microprobe analyses, inasmuch as Raman spectroscopy can be performed with a high spatial resolution (1 µm2) without the need for any sample preparation as a nondestructive technique. This study represents an advance in efforts to provide the first database of Raman spectra for natural silicate glasses and yields a new approach for the treatment of Raman spectra, which allows us to extract approximate information about the chemical composition of natural silicate glasses using Raman spectroscopy. We anticipate its application in handheld in situ terrestrial field studies of silicate glasses under extreme conditions (e.g. extraterrestrial and submarine environments). © 2015 The Authors Journal of Raman Spectroscopy Published by John Wiley & Sons Ltd PMID:27656038

  13. [Surface-enhanced Raman spectroscopy analysis of thiabendazole pesticide].

    PubMed

    Lin, Lei; Wu, Rui-mei; Liu, Mu-hua; Wang, Xiao-bin; Yan, Lin-yuan

    2015-02-01

    Surface-enhanced Raman spectroscopy (SERS) technique was used to analyze the Raman peaks of thiabendazole pesticides in the present paper. Surface enhanced substrates of silver nanoparticle were made based on microwave technology. Raman signals of thiabendazole were collected by laser Micro-Raman spectrometer with 514. 5 and 785 nm excitation wavelengths, respectively. The Raman peaks at different excitation wavelengths were analyzed and compared. The Raman peaks 782 and 1 012 at 785 nm excitation wavelength were stronger, which were C--H out-of-plane vibrations. While 1284, 1450 and 1592 cm(-1) at 514.5 nm excitation wavelength were stronger, which were vng and C==N stretching. The study results showed that the intensity of Raman peak and Raman shift at different excitation wavelengths were different And strong Raman signals were observed at 782, 1012, 1284, 1450 and 1592 cm(-1) at 514.5 and 785 nm excitation wavelengths. These characteristic vibrational modes are characteristic Raman peaks of carbendazim pesticide. The results can provide basis for the rapid screening of pesticide residue in agricultural products and food based on Raman spectrum.

  14. Rapid monitoring of benzylpenicillin sodium using Raman and surface enhanced Raman spectroscopy.

    PubMed

    Jiang, Xin; Qin, Xiaoyu; Yin, Di; Gong, Mengdi; Yang, Libin; Zhao, Bing; Ruan, Weidong

    2015-04-05

    At present, fluorescence spectroscopy, ultraviolet spectroscopy and infrared spectroscopy are usually used to detect drug molecules, however the information about using Raman spectroscopy to detect drug molecules is very few. In this work normal Raman spectroscopy and surface-enhanced Raman spectroscopy were utilized to study benzylpenicillin sodium (NaBP). The results show that NaBP is close to the surface of silver substrate through the carboxyl group, and the detection limit of NaBP is reduced to 1×10(-7) mol/L. Accordingly, the quantitative analysis of NaBP can be carried out in the range of 1×10(-4)-1×10(-7) mol/L concentration. And it is proved that NaBP is not stable in acid and alkali conditions and the decomposition reaction is very complex.

  15. Generation of a vacuum ultraviolet to visible Raman frequency comb in H_2-filled kagomé photonic crystal fiber

    NASA Astrophysics Data System (ADS)

    Mridha, M. K.; Novoa, D.; Bauerschmidt, S. T.; Abdolvand, A.; St. J. Russell, P.

    2016-06-01

    We report the generation of a purely vibrational Raman comb, extending from the vacuum ultraviolet (184 nm) to the visible (478 nm), in hydrogen-filled kagom\\'e-style photonic crystal fiber pumped at 266 nm. Stimulated Raman scattering and molecular modulation processes are enhanced by higher Raman gain in the ultraviolet. Owing to the pressure-tunable normal dispersion landscape of the fiber-gas system in the ultraviolet, higher-order anti-Stokes bands are generated preferentially in higher-order fiber modes. The results pave the way towards tunable fiber-based sources of deep- and vacuum ultraviolet light for applications in, e.g., spectroscopy and biomedicine.

  16. Micro-Raman spectroscopy for meat type detection

    NASA Astrophysics Data System (ADS)

    De Biasio, M.; Stampfer, P.; Leitner, R.; Huck, C. W.; Wiedemair, V.; Balthasar, D.

    2015-06-01

    The recent horse meat scandal in Europe increased the demand for optical sensors that can identify meat type. Micro-Raman spectroscopy is a promising technique for the discrimination of meat types. Here, we present micro-Raman measurements of chicken, pork, turkey, mutton, beef and horse meat test samples. The data was analyzed with different combinations of data normalization and classification approaches. Our results show that Raman spectroscopy can discriminate between different meat types. Red and white meat are easily discriminated, however a sophisticated chemometric model is required to discriminate species within these groups.

  17. Gaseous trace analysis using pulsed photoacoustic Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Siebert, D. R.; West, G. A.; Barrett, J. J.

    1980-01-01

    The paper describes a method for the trace analysis of gases, based on the pulsed photoacoustic Raman spectroscopy (PARS) technique. It is reported that the method has been applied to the analysis of mixtures of CH4 in N2, CO2 in N2, and N2O in N2 at concentrations near 1 ppm. Attention is given to the apparatus used and means of improving the method's sensitivity as well as sensitivity-limiting processes are evaluated. Finally, the analytical capabilities of this technique are compared with both direct (IR) absorption and other Raman techniques such as CARS and stimulated Raman gain spectroscopy (SRGS).

  18. Raman Spectroscopy as an Accurate Probe of Defects in Graphene

    NASA Astrophysics Data System (ADS)

    Rodriguez-Nieva, Joaquin; Barros, Eduardo; Saito, Riichiro; Dresselhaus, Mildred

    2014-03-01

    Raman Spectroscopy has proved to be an invaluable non-destructive technique that allows us to obtain intrinsic information about graphene. Furthermore, defect-induced Raman features, namely the D and D' bands, have previously been used to assess the purity of graphitic samples. However, quantitative studies of the signatures of the different types of defects on the Raman spectra is still an open problem. Experimental results already suggest that the Raman intensity ratio ID /ID' may allow us to identify the nature of the defects. We study from a theoretical point of view the power and limitations of Raman spectroscopy in the study of defects in graphene. We derive an analytic model that describes the Double Resonance Raman process of disordered graphene samples, and which explicitly shows the role played by both the defect-dependent parameters as well as the experimentally-controlled variables. We compare our model with previous Raman experiments, and use it to guide new ways in which defects in graphene can be accurately probed with Raman spectroscopy. We acknowledge support from NSF grant DMR1004147.

  19. Raman spectroscopy in the analysis of food and pharmaceutical nanomaterials.

    PubMed

    Li, Ying-Sing; Church, Jeffrey S

    2014-03-01

    Raman scattering is an inelastic phenomenon. Although its cross section is very small, recent advances in electronics, lasers, optics, and nanotechnology have made Raman spectroscopy suitable in many areas of application. The present article reviews the applications of Raman spectroscopy in food and drug analysis and inspection, including those associated with nanomaterials. Brief overviews of basic Raman scattering theory, instrumentation, and statistical data analysis are also given. With the advent of Raman enhancement mechanisms and the progress being made in metal nanomaterials and nanoscale metal surfaces fabrications, surface enhanced Raman scattering spectroscopy has become an extra sensitive method, which is applicable not only for analysis of foods and drugs, but also for intracellular and intercellular imaging. A Raman spectrometer coupled with a fiber optics probe has great potential in applications such as monitoring and quality control in industrial food processing, food safety in agricultural plant production, and convenient inspection of pharmaceutical products, even through different types of packing. A challenge for the routine application of surface enhanced Raman scattering for quantitative analysis is reproducibility. Success in this area can be approached with each or a combination of the following methods: (1) fabrication of nanostructurally regular and uniform substrates; (2) application of statistic data analysis; and (3) isotopic dilution.

  20. Snapshot depth sensitive Raman spectroscopy in layered tissues.

    PubMed

    Liu, Wei; Ong, Yi Hong; Yu, Xiao Jun; Ju, Jian; Perlaki, Clint Michael; Liu, Lin Bo; Liu, Quan

    2016-12-12

    Depth sensitive Raman spectroscopy has been shown effective in the detection of depth dependent Raman spectra in layered tissues. However, the current techniques for depth sensitive Raman measurements based on fiber-optic probes suffer from poor depth resolution and significant variation in probe-sample contact. In contrast, those lens based techniques either require the change in objective-sample distance or suffer from slow spectral acquisition. We report a snapshot depth-sensitive Raman technique based on an axicon lens and a ring-to-line fiber assembly to simultaneously acquire Raman signals emitted from five different depths in the non-contact manner without moving any component. A numerical tool was developed to simulate ray tracing and optimize the snapshot depth sensitive setup to achieve the tradeoff between signal collection efficiency and depth resolution for Raman measurements in the skin. Moreover, the snapshot system was demonstrated to be able to acquire depth sensitive Raman spectra from not only transparent and turbid skin phantoms but also from ex vivo pork tissues and in vivo human thumbnails when the excitation laser power was limited to the maximum permissible exposure for human skin. The results suggest the great potential of snapshot depth sensitive Raman spectroscopy in the characterization of the skin and other layered tissues in the clinical setting or other similar applications such as quality monitoring of tablets and capsules in pharmaceutical industry requiring the rapid measurement of depth dependent Raman spectra.

  1. Clinical cancer diagnosis using optical fiber-delivered coherent anti-stokes ramon scattering microscopy

    NASA Astrophysics Data System (ADS)

    Gao, Liang

    This thesis describes the development of a combined label-free imaging and analytical strategy for intraoperative characterization of cancer lesions using the coherent anti-Stokes Raman scattering imaging (CARS) technique. A cell morphology-based analytical platform is developed to characterize CARS images and, hence, provide diagnostic information using disease-related pathology features. This strategy is validated for three different applications, including margin detection for radical prostatectomy, differential diagnosis of lung cancer, as well as detection and differentiation of breast cancer subtypes for in situ analysis of margin status during lumpectomy. As the major contribution of this thesis, the developed analytical strategy shows high accuracy and specificity for all three diseases and thus has introduced the CARS imaging technique into the field of human cancer diagnosis, which holds substantial potential for clinical translations. In addition, I have contributed a project aimed at miniaturizing the CARS imaging device into a microendoscope setup through a fiber-delivery strategy. A four-wave-mixing (FWM) background signal, which is caused by simultaneous delivery of the two CARS-generating excitation laser beams, is initially identified. A polarization-based strategy is then introduced and tested for suppression of this FWM noise. The approach shows effective suppression of the FWM signal, both on microscopic and prototype endoscopic setups, indicating the potential of developing a novel microendoscope with a compatible size for clinical use. These positive results show promise for the development of an all-fiber-based, label-free imaging and analytical platform for minimally invasive detection and diagnosis of cancers during surgery or surgical-biopsy, thus improving surgical outcomes and reducing patients' suffering.

  2. Micro-Raman spectroscopy on oral tissues

    NASA Astrophysics Data System (ADS)

    Zenone, F.; Lepore, M.; Perna, G.; Carmone, P.; Riccio, R.; Gaeta, G. M.; Capozzi, V.

    2006-02-01

    Micro-Raman Spectroscopy (μ-RS) provides a unique tool in medicine for a not invasive and real time analysis of biological tissue for biopsy and "in vivo" investigation. Based on the evaluation of molecular vibration frequencies, the μ-RS is able to detect the main molecular bonds of protein constituents, as the C-H and C-C ones. Changes in frequency or in the relative intensity of the vibration modes revealed by μ-RS can be related to changes of chemical bond and of protein structure induced by pathology. The μ-RS has been performed on samples of oral tissue from informed patients, affected by pemphigus vulgaris (an oral pathology) in an advanced regression state. The biopsies were thin slices (about 1mm thick) with 6mm diameter. The sample was measured through a 170 μm thick cover-glass. The experimental set-up was mainly composed by a He-Ne laser and a monochromator equipped with a Peltier cell and with a grating of 1800 grooves/mm. The laser light was focused on the sample surface by means of a long focal length 50X optical objective. The main protein bonds are clearly detectable in the considered samples and this give important information on the integrity and on the state of tissue components (lipids and proteins), and consequently on the occurrence of pathology. The potential application of this method for in vivo analysis is an invaluable alternative to biopsy and pathological examinations for many medical application as screening diagnostic, therapy progress examination, and surgical support.

  3. Raman and surface-enhanced Raman spectroscopy for renal condition monitoring

    NASA Astrophysics Data System (ADS)

    Li, Jingting; Li, Ming; Du, Yong; Santos, Greggy M.; Mohan, Chandra; Shih, Wei-Chuan

    2016-03-01

    Non- and minimally-invasive techniques can provide advantages in the monitoring and clinical diagnostics in renal diseases. Although renal biopsy may be useful in establishing diagnosis in several diseases, it is an invasive approach and impractical for longitudinal disease monitoring. To address this unmet need, we have developed two techniques based on Raman spectroscopy. First, we have investigated the potential of diagnosing and staging nephritis by analyzing kidney tissue Raman spectra using multivariate techniques. Secondly, we have developed a urine creatinine sensor based on surface-enhanced Raman spectroscopy with performance near commercial assays which require relatively laborious sample preparation and longer time.

  4. Gas-phase single-shot thermometry at 1 kHz using fs-CARS spectroscopy.

    PubMed

    Roy, Sukesh; Kulatilaka, Waruna D; Richardson, Daniel R; Lucht, Robert P; Gord, James R

    2009-12-15

    Single-laser-shot temperature measurements at a data rate of 1 kHz employing femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy of N(2) are demonstrated. The measurements are performed using a chirped-probe pulse to map the time-dependent frequency-spread dephasing of the Raman coherence, which is created by approximately 80-fs pump and Stokes beams, into the spectrum of the coherent anti-Stokes Raman scattering signal pulse. Temperature is determined from the spectral shape of the fs-CARS signal for probe delays of approximately 2 ps with respect to the pump-Stokes excitation. The accuracy and precision of the measurements for the 300-2400 K range are found to be approximately 1%-6% and approximately 1.5%-3%, respectively.

  5. Mode-dependent dispersion in Raman line shapes: Observation and implications from ultrafast Raman loss spectroscopy

    SciTech Connect

    Umapathy, S.; Mallick, B.; Lakshmanna, A.

    2010-07-14

    Ultrafast Raman loss spectroscopy (URLS) enables one to obtain the vibrational structural information of molecular systems including fluorescent materials. URLS, a nonlinear process analog to stimulated Raman gain, involves a narrow bandwidth picosecond Raman pump pulse and a femtosecond broadband white light continuum. Under nonresonant condition, the Raman response appears as a negative (loss) signal, whereas, on resonance with the electronic transition the line shape changes from a negative to a positive through a dispersive form. The intensities observed and thus, the Franck-Condon activity (coordinate dependent), are sensitive to the wavelength of the white light corresponding to a particular Raman frequency with respect to the Raman pump pulse wavelength, i.e., there is a mode-dependent response in URLS.

  6. Raman spectroscopy for planetary exploration and characterization of extraterrestrial materials

    NASA Astrophysics Data System (ADS)

    Acosta-Maeda, Tayro E.

    The sharp spectral features of Raman spectra are widely recognized to provide unequivocal and accurate chemical characterization of organic and inorganic compounds. Therefore Raman spectroscopy can be used to detect minerals, water bearing minerals, organic and biological materials and biomarkers in the context of planetary science. This dissertation extends the applicability of the Raman technique both laboratory based micro-Raman and remote Raman sensing ahead of planetary exploration missions to Mars employing Raman spectrometers. The interpretation of Raman imaging from a meteorite taken with a micro-Raman system revealed a close correlation between the blue color in natural ringwoodite and a new observed Raman peak that shows strong resonance Raman enhancement. The data suggest that ringwoodite exists both in the spinel structure and in the partially inverse spinel structure. In the field of remote Raman, this dissertation provides carefully derived Raman cross-section values for various organic liquids and inorganic polyatomic ions in aqueous solutions that will be useful for estimating detection capabilities of 532 nm excitation remote Raman systems for planetary exploration. Suitability of remote 532 nm Raman systems for future applications is explored. A portable, compact time-resolved instrument using a 3-inch diameter telescope is used it to demonstrate daytime detection of amino acids and nucleobases from a distance of 8 m. The measurements with a larger 8-inch Raman system demonstrate that it is possible to acquire good quality Raman spectra of various materials from a 430 meter remote distance during daylight with detection times of 10 seconds, and in some cases as short as 1 second, during daylight and in a realistic outdoor context. To my knowledge, these are the only remote Raman spectra at this distance that provide unambiguous detection of compounds important for planetary science, such as water and water ice, dry ice, sulfur, sulfates, various

  7. Resonance Raman spectroscopy study of protonated porphyrin

    NASA Astrophysics Data System (ADS)

    Gorski, A.; Starukhin, A.; Stavrov, S.; Gawinkowski, S.; Waluk, J.

    2017-02-01

    Resonance Raman microscopy was used to study the resonance Raman scattering of the diacid (diprotonated form) of free-base porphyrin (21H,23H-porphine) in a crystal powder and KBr pellets. Intensive lines in the spectral range between 100 ÷ 1000 cm- 1 have been detected and assigned as spectral manifestation of out-of-plane modes. The Raman spectra were simulated by means of DFT methods and compared with the experimental data. It is evident from experimental and theoretical results that the activation of out-of-plane modes arises from saddle distortion of the porphyrin macrocycle upon formation of its diprotonated form.

  8. Shining light on neurosurgery diagnostics using Raman spectroscopy.

    PubMed

    Broadbent, Brandy; Tseng, James; Kast, Rachel; Noh, Thomas; Brusatori, Michelle; Kalkanis, Steven N; Auner, Gregory W

    2016-10-01

    Surgical excision of brain tumors provides a means of cytoreduction and diagnosis while minimizing neurologic deficit and improving overall survival. Despite advances in functional and three-dimensional stereotactic navigation and intraoperative magnetic resonance imaging, delineating tissue in real time with physiological confirmation is challenging. Raman spectroscopy is a promising investigative and diagnostic tool for neurosurgery, which provides rapid, non-destructive molecular characterization in vivo or in vitro for biopsy, margin assessment, or laboratory uses. The Raman Effect occurs when light temporarily changes a bond's polarizability, causing change in the vibrational frequency, with a corresponding change in energy/wavelength of the scattered photon. The recorded inelastic scattering results in a "fingerprint" or Raman spectrum of the constituent under investigation. The amount, location, and intensity of peaks in the fingerprint vary based on the amount of vibrational bonds in a molecule and their ensemble interactions with each other. Distinct differences between various pathologic conditions are shown as different intensities of the same peak, or shifting of a peak based on the binding conformation. Raman spectroscopy has potential for integration into clinical practice, particularly in distinguishing normal and diseased tissue as an adjunct to standard pathologic diagnosis. Further, development of fiber-optic Raman probes that fit through the instrument port of a standard endoscope now allows researchers and clinicians to utilize spectroscopic information for evaluation of in vivo tissue. This review highlights the need for such an instrument, summarizes neurosurgical Raman work performed to date, and discusses the future applications of neurosurgical Raman spectroscopy.

  9. [Current views on surface enhanced Raman spectroscopy in microbiology].

    PubMed

    Jia, Xiaoxiao; Li, Jing; Qin, Tian; Deng, Aihua; Liu, Wenjun

    2015-05-01

    Raman spectroscopy has generated many branches during the development for more than 90 years. Surface enhanced Raman spectroscopy (SERS) improves SNR by using the interaction between tested materials and the surface of rough metal, as to quickly get higher sensitivity and precision spectroscopy without sample pretreatment. This article describes the characteristic and classification of SERS, and updates the theory and clinical application of SERS. It also summarizes the present status and progress of SERS in various disciplines and illustrates the necessity and urgency of its research, which provides rationale for the application for SERS in microbiology.

  10. Approximate chemical analysis of volcanic glasses using Raman spectroscopy.

    PubMed

    Di Genova, Danilo; Morgavi, Daniele; Hess, Kai-Uwe; Neuville, Daniel R; Borovkov, Nikita; Perugini, Diego; Dingwell, Donald B

    2015-12-01

    The effect of chemical composition on the Raman spectra of a series of natural calcalkaline silicate glasses has been quantified by performing electron microprobe analyses and obtaining Raman spectra on glassy filaments (~450 µm) derived from a magma mingling experiment. The results provide a robust compositionally-dependent database for the Raman spectra of natural silicate glasses along the calcalkaline series. An empirical model based on both the acquired Raman spectra and an ideal mixing equation between calcalkaline basaltic and rhyolitic end-members is constructed enabling the estimation of the chemical composition and degree of polymerization of silicate glasses using Raman spectra. The model is relatively insensitive to acquisition conditions and has been validated using the MPI-DING geochemical standard glasses1 as well as further samples. The methods and model developed here offer several advantages compared with other analytical and spectroscopic methods such as infrared spectroscopy, X-ray fluorescence spectroscopy, electron and ion microprobe analyses, inasmuch as Raman spectroscopy can be performed with a high spatial resolution (1 µm(2)) without the need for any sample preparation as a nondestructive technique. This study represents an advance in efforts to provide the first database of Raman spectra for natural silicate glasses and yields a new approach for the treatment of Raman spectra, which allows us to extract approximate information about the chemical composition of natural silicate glasses using Raman spectroscopy. We anticipate its application in handheld in situ terrestrial field studies of silicate glasses under extreme conditions (e.g. extraterrestrial and submarine environments).

  11. Femtosecond stimulated Raman scattering picosecond molecular thermometry in condensed phases.

    PubMed

    Dang, N C; Bolme, C A; Moore, D S; McGrane, S D

    2011-07-22

    We demonstrate the capability of femtosecond stimulated Raman scattering (FSRS) data to measure the temperature of condensed matter at the molecular vibrational level. We report the temperature dependence of Raman loss to Raman gain ratios for low frequency modes (<300  cm(-1)) in a CaCO3 single crystal from cryogenic to room temperature, which is shown to be in agreement with theoretical predictions. We also report the measurements of nonequilibrium time evolution of mode specific vibrational temperatures in the CaCO3 single crystal to demonstrate that FSRS can measure temperature on picosecond time scales. Finally, we point out the unique origin of this temperature dependent anti-Stokes to Stokes ratio in stimulated Raman, which is not present in other coherent Raman spectroscopies. These measurements require no material dependent parameters or prior calibration.

  12. Anti-Stokes luminescence in the light of second order perturbation theory

    SciTech Connect

    Bhattacharya, Rupak Pal, Bipul Bansal, Bhavtosh

    2014-11-10

    Anti-Stokes photoluminescence is measured in high-quality GaAs quantum wells. The primary pathway for interband optical absorption and hence emission under subbandgap photoexcitation is the optical phonon-mediated second-order electric dipole transition. This conclusion is drawn from the remarkable agreement between predictions of second-order perturbation calculation and the measured intensity of anti-Stokes photoluminescence, both as function of the detuning wavelength and temperature. The results are of direct relevance to laser cooling of solids where phonon-assisted upconversion is a necessary condition.

  13. Evaluation of thyroid tissue by Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Teixeira, C. S. B.; Bitar, R. A.; Santos, A. B. O.; Kulcsar, M. A. V.; Friguglietti, C. U. M.; Martinho, H. S.; da Costa, R. B.; Martin, A. A.

    2010-02-01

    Thyroid gland is a small gland in the neck consisting of two lobes connected by an isthmus. Thyroid's main function is to produce the hormones thyroxine (T4), triiodothyronine (T3) and calcitonin. Thyroid disorders can disturb the production of these hormones, which will affect numerous processes within the body such as: regulating metabolism and increasing utilization of cholesterol, fats, proteins, and carbohydrates. The gland itself can also be injured; for example, neoplasias, which have been considered the most important, causing damage of to the gland and are difficult to diagnose. There are several types of thyroid cancer: Papillary, Follicular, Medullary, and Anaplastic. The occurrence rate, in general is between 4 and 7%; which is on the increase (30%), probably due to new technology that is able to find small thyroid cancers that may not have been found previously. The most common method used for thyroid diagnoses are: anamnesis, ultrasonography, and laboratory exams (Fine Needle Aspiration Biopsy- FNAB). However, the sensitivity of those test are rather poor, with a high rate of false-negative results, therefore there is an urgent need to develop new diagnostic techniques. Raman spectroscopy has been presented as a valuable tool for cancer diagnosis in many different tissues. In this work, 27 fragments of the thyroid were collected from 18 patients, comprising the following histologic groups: goitre adjacent tissue, goitre nodular tissue, follicular adenoma, follicular carcinoma, and papillary carcinoma. Spectral collection was done with a commercial FTRaman Spectrometer (Bruker RFS100/S) using a 1064 nm laser excitation and Ge detector. Principal Component Analysis, Cluster Analysis, and Linear Discriminant Analysis with cross-validation were applied as spectral classification algorithm. Comparing the goitre adjacent tissue with the goitre nodular region, an index of 58.3% of correct classification was obtained. Between goitre (nodular region and

  14. Surface Raman spectroscopy as a probe of surface chemistry

    NASA Astrophysics Data System (ADS)

    Child, Craig M.; Foster, Michelle; Ivanecky, J. E., III; Perry, Scott S.; Campion, Alan

    1995-09-01

    Unenhanced surface Raman spectroscopy has been used to study the chemistry of polymers adsorbed on solid surfaces and the chemical enhancement mechanism of surface-enhanced Raman scattering. The adsorption and reactions of the polyimide monomers pyromellitic dianhydride (PMDA) and oxydianiline on silver, copper and silicon surfaces under ultrahigh vacuum have been investigated. These include both nondissociative physisorption and dissociative chemisorption of the monomers, and the condensation polymerization to form adsorbed polyimide. The intermediate polyamic acid is detected for the first time in a surface experiment. PMDA adsorbed on Cu(111) shows chemical enhancement in the absence of electromagnetic enhancement. High resolution electron energy loss spectroscopy has revealed a strong charge transfer absorption near the Raman excitation frequency. This observation provides strong support for a proposed resonance Raman chemical enhancement mechanism.

  15. Histochemical analysis of biological tissues using Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Manoharan, Ramasamy; Wang, Yang; Feld, Michael S.

    1996-02-01

    This paper reviews the application of the Raman spectroscopic technique for analysis of biological tissue. The advantages and disadvantages of visible, near-IR and UV excitations are described, and the problems and prospects of using these methodologies for disease diagnosis are addressed. In situ analysis of tissue proteins, lens, cornea, blood constituents, biological stones and several hard tissues is reviewed, and the potentials for diagnosing arterial disease, and cancer in gynecological tissues, soft tissues, breast, colon, bladder and brain are also presented. Recent technological advances in instrumentation allow the use of Raman spectroscopy for real time histochemical analysis of tissues. The capability of Raman microspectroscopy for providing spatial information about the distribution of biochemical constituents in tissues has been demonstrated. The work reviewed indicates the promise of Raman spectroscopy for endoscopic imaging and real-time quantitation of biochemical constituents in clinical situations.

  16. Developing fibre optic Raman probes for applications in clinical spectroscopy.

    PubMed

    Stevens, Oliver; Iping Petterson, Ingeborg E; Day, John C C; Stone, Nick

    2016-04-07

    Raman spectroscopy has been shown by various groups over the last two decades to have significant capability in discriminating disease states in bodily fluids, cells and tissues. Recent development in instrumentation, optics and manufacturing approaches has facilitated the design and demonstration of various novel in vivo probes, which have applicability for myriad of applications. This review focusses on key considerations and recommendations for application specific clinical Raman probe design and construction. Raman probes can be utilised as clinical tools able to provide rapid, non-invasive, real-time molecular analysis of disease specific changes in tissues. Clearly the target tissue location, the significance of spectral changes with disease and the possible access routes to the region of interest will vary for each clinical application considered. This review provides insight into design and construction considerations, including suitable probe designs and manufacturing materials compatible with Raman spectroscopy.

  17. Remote cure monitoring of polymeric resins by laser Raman spectroscopy

    SciTech Connect

    Hong, K.C.; Vess, T.M.; Lyon, R.E.; Myrick, M.L.

    1993-05-01

    The validity of using Raman spectroscopy to monitor the cure chemistries of amine-cured epoxy is demonstrated by correlating NIR absorbance measurements with Raman measurements for a concentration series of bisphenol-A diglycidylether in its own reaction product with diethylamine. The intensity of a normalized Raman peak at 1240 cm{sup {minus}l}, assigned to the epoxide functionality, was found to be linearly related to the concentration of epoxide groups in the resin mixtures. Also, it is shown that the Ciba-Geigy Matrimid 5292 system can be monitored by ex-situ FT-Raman spectroscopy by observing changes in the carbonyl stretching (1773 cm{sup {minus}1}) or the C=C stretching of maleimide (1587 cm{sup {minus}1}) during the cure reaction.

  18. Proximal and point detection of contaminated surfaces using Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Guicheteau, Jason A.; Christesen, Steven D.; Tripathi, Ashish; Emmons, Erik D.; Wilcox, Phillip G.; Emge, Darren K.; Pardoe, Ian J.; Fountain, Augustus W., III

    2011-11-01

    We are actively investigating the use of Raman spectroscopy for proximal standoff detection of chemicals and explosive materials on surfaces. These studies include Raman Chemical Imaging of contaminated fingerprints for forensic attribution and the assessments of commercial handheld or portable Raman instruments operating with near-infrared (IR) as well as ultraviolet (UV) laser excitation specifically developed for on-the-move reconnaissance of chemical contamination. As part of these efforts, we have measured the Raman cross sections of chemical agents, toxic industrial chemicals, and explosives from the UV to NIR. We have also measured and modeled the effect interrogation angle has on the Raman return from droplets on man-made surfaces. Realistic droplet distributions have been modeled and tested against variations in surface scan patterns and laser spot size for determining the optimum scan characteristics for detection of relevant surface contamination.

  19. Monitoring the influence of antibiotic exposure using Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Samek, Ota; Zemanek, Pavel; Bernatova, Silvie; Jezek, Jan; Sery, Mojmir; Jakl, Petr; Siler, Martin; Ruzicka, Filip

    2014-03-01

    Here we report on combination of the data obtained from MICs (minimum inhibitory concentrations) with infor- mation of microoragnisms fingerprint provided by Raman spectroscopy. In our feasibility study we could follow mechanisms of the bacteriostatic versus bactericidal action on biofilm-positive Staphylococcus epidermidis simply by monitoring Raman bands corresponding to DNA translating the changes introduced by selected antibiotics. The Raman spectra of Staphylococcus epidermidis treated with a bacteriostatic agent show little effect on DNA which is in contrast with the action of a bactericidal agent where decreased in dedicated Raman spectra signal strength suggests DNA fragmentation. Moreover, we demonstrate that Raman tweezers are indeed able to distinguish strains of biofilm-forming (biofilm-positive) and biofilm-negative Staphylococcus epidermidis strains using principal component analysis (PCA).

  20. Remote Raman spectroscopy for planetary exploration: a review.

    PubMed

    Angel, S Michael; Gomer, Nathaniel R; Sharma, Shiv K; McKay, Chris

    2012-02-01

    In this review, we discuss the current state of standoff Raman spectroscopy as it applies to remote planetary applications, including standoff instrumentation, the technique's ability to identify biologically and geologically important analytes, and the feasibility to make standoff Raman measurements under various planetary conditions. This is not intended to be an exhaustive review of standoff Raman and many excellent papers are not mentioned. Rather it is intended to give the reader a quick review of the types of standoff Raman systems that are being developed and that might be suitable for astrospectroscopy, a look at specific analytes that are of interest for planetary applications, planetary measurement opportunities and challenges that need to be solved, and a brief discussion of the feasibility of making surface and plume planetary Raman measurements from an orbiting spacecraft.

  1. Generation of a vacuum ultraviolet to visible Raman frequency comb in H2-filled kagomé photonic crystal fiber.

    PubMed

    Mridha, M K; Novoa, D; Bauerschmidt, S T; Abdolvand, A; St J Russell, P

    2016-06-15

    We report on the generation of a purely vibrational Raman comb, extending from the vacuum ultraviolet (184 nm) to the visible (478 nm), in hydrogen-filled kagomé-style photonic crystal fiber pumped at 266 nm. Stimulated Raman scattering and molecular modulation processes are enhanced by higher Raman gain in the ultraviolet. Owing to the pressure-tunable normal dispersion landscape of the "fiber + gas" system in the ultraviolet, higher-order anti-Stokes bands are generated preferentially in higher-order fiber modes. The results pave the way toward tunable fiber-based sources of deep and vacuum ultraviolet light for applications in, e.g., spectroscopy and biomedicine.

  2. Single Molecule Raman Spectroscopy Under High Pressure

    NASA Astrophysics Data System (ADS)

    Fu, Yuanxi; Dlott, Dana

    2014-06-01

    Pressure effects on surface-enhanced Raman scattering spectra of Rhdoamine 6G adsorbed on silver nanoparticle surfaces was studied using a confocal Raman microscope. Colloidal silver nanoparticles were treated with Rhodamine 6G (R6G) and its isotopically substituted partner, R6G-d4. Mixed isotopomers let us identify single-molecule spectra, since multiple-molecule spectra would show vibrational transitions from both species. The nanoparticles were embedded into a poly vinyl alcohol film, and loaded into a diamond anvil cell for the high-pressure Raman scattering measurement. Argon was the pressure medium. Ambient pressure Raman scattering spectra showed few single-molecule spectra. At moderately high pressure ( 1GPa), a surprising effect was observed. The number of sites with observable spectra decreased dramatically, and most of the spectra that could be observed were due to single molecules. The effects of high pressure suppressed the multiple-molecule Raman sites, leaving only the single-molecule sites to be observed.

  3. Single bacteria identification by Raman spectroscopy.

    PubMed

    Strola, Samy Andrea; Baritaux, Jean-Charles; Schultz, Emmanuelle; Simon, Anne Catherine; Allier, Cédric; Espagnon, Isabelle; Jary, Dorothée; Dinten, Jean-Marc

    2014-01-01

    We report on rapid identification of single bacteria using a low-cost, compact, Raman spectroscope. We demonstrate that a 60-s procedure is sufficient to acquire a comprehensive Raman spectrum in the range of 600 to 3300 cm⁻¹. This time includes localization of small bacteria aggregates, alignment on a single individual, and spontaneous Raman scattering signal collection. Fast localization of small bacteria aggregates, typically composed of less than a dozen individuals, is achieved by lensfree imaging over a large field of view of 24 mm². The lensfree image also allows precise alignment of a single bacteria with the probing beam without the need for a standard microscope. Raman scattered light from a 34-mW continuous laser at 532 nm was fed to a customized spectrometer (prototype Tornado Spectral Systems). Owing to the high light throughput of this spectrometer, integration times as low as 10 s were found acceptable. We have recorded a total of 1200 spectra over seven bacterial species. Using this database and an optimized preprocessing, classification rates of ~90% were obtained. The speed and sensitivity of our Raman spectrometer pave the way for high-throughput and nondestructive real-time bacteria identification assays. This compact and low-cost technology can benefit biomedical, clinical diagnostic, and environmental applications.

  4. Single bacteria identification by Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Strola, Samy Andrea; Baritaux, Jean-Charles; Schultz, Emmanuelle; Simon, Anne Catherine; Allier, Cédric; Espagnon, Isabelle; Jary, Dorothée; Dinten, Jean-Marc

    2014-11-01

    We report on rapid identification of single bacteria using a low-cost, compact, Raman spectroscope. We demonstrate that a 60-s procedure is sufficient to acquire a comprehensive Raman spectrum in the range of 600 to 3300. This time includes localization of small bacteria aggregates, alignment on a single individual, and spontaneous Raman scattering signal collection. Fast localization of small bacteria aggregates, typically composed of less than a dozen individuals, is achieved by lensfree imaging over a large field of view of 24. The lensfree image also allows precise alignment of a single bacteria with the probing beam without the need for a standard microscope. Raman scattered light from a 34-mW continuous laser at 532 nm was fed to a customized spectrometer (prototype Tornado Spectral Systems). Owing to the high light throughput of this spectrometer, integration times as low as 10 s were found acceptable. We have recorded a total of 1200 spectra over seven bacterial species. Using this database and an optimized preprocessing, classification rates of ˜90% were obtained. The speed and sensitivity of our Raman spectrometer pave the way for high-throughput and nondestructive real-time bacteria identification assays. This compact and low-cost technology can benefit biomedical, clinical diagnostic, and environmental applications.

  5. Raman and CARS microspectroscopy of cells and tissues.

    PubMed

    Krafft, Christoph; Dietzek, Benjamin; Popp, Jürgen

    2009-06-01

    Raman spectroscopy has been recognized to be a powerful tool to study cells and tissues because the method provides molecular information without external markers such as stains or radioactive labels. To overcome the disadvantage of low signal intensities from most biomolecules, enhancement effects are utilized. A non-linear variant of Raman spectroscopy called coherent anti-Stokes Raman spectroscopy (CARS) belongs to the most promising techniques because it combines signal enhancement due to the coherent nature of the process with further advantages such as directional emission, narrow spectral bandwidth and no disturbing interference with autofluorescence. This review describes briefly the principles of the methods and summarizes applications to cells and tissues that are expected to gain significance in the future such as the combination with imaging approaches, microscopy, optical traps and fiber-optic probes.

  6. Quantum Mechanical Description of Raman Scattering from Molecules in Plasmonic Cavities.

    PubMed

    Schmidt, Mikolaj K; Esteban, Ruben; González-Tudela, Alejandro; Giedke, Geza; Aizpurua, Javier

    2016-06-28

    Plasmon-enhanced Raman scattering can push single-molecule vibrational spectroscopy beyond a regime addressable by classical electrodynamics. We employ a quantum electrodynamics (QED) description of the coherent interaction of plasmons and molecular vibrations that reveal the emergence of nonlinearities in the inelastic response of the system. For realistic situations, we predict the onset of phonon-stimulated Raman scattering and a counterintuitive dependence of the anti-Stokes emission on the frequency of excitation. We further show that this QED framework opens a venue to analyze the correlations of photons emitted from a plasmonic cavity.

  7. Identification and discrimination of polycyclic aromatic hydrocarbons using Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Cloutis, Edward; Szymanski, Paul; Applin, Daniel; Goltz, Douglas

    2016-08-01

    Polycyclic aromatic hydrocarbons (PAHs) are widely present throughout the Solar System and beyond. They have been implicated as a contributor to unidentified infrared emission bands in the interstellar medium, comprise a substantial portion of the insoluble organic matter in carbonaceous chondrites, are expected stable components of organic matter on Mars, and are present in a wide range of terrestrial hydrocarbons and as components of biomolecules. However, PAH structures can be very complicated, making their identification challenging. Raman spectroscopy is known to be especially sensitive to the highly polarizable C-C and C=C bonds found in PAHs, and therefore, can be a powerful tool for PAH structural and compositional elucidation. This study examined Raman spectra of 48 different PAHs to determine the degree to which Raman spectroscopy could be used to uniquely identify different species, factors that control the positions of major Raman peaks, the degree to which induced fluorescence affects the intensity of Raman peaks, its usefulness for PAH discrimination, and the effects of varying excitation wavelength on some PAH Raman spectra. It was found that the arrangement and composition of phenyl (benzene) rings, and the type and position of functional groups can greatly affect fluorescence, positions and intensities of Raman peaks associated with the PAH backbone, and the introduction of new Raman peaks. Among the functional groups found on many of the PAHs that were analyzed, only a few Raman peaks corresponding to the molecular vibrations of these groups could be clearly distinguished. Comparison of the PAH Raman spectra that were acquired with both 532 and 785 nm excitation found that the longer wavelength resulted in reduced fluorescence, consistent with previous studies.

  8. Raman spectroscopy of polyhedral carbon nano-onions

    NASA Astrophysics Data System (ADS)

    Codorniu Pujals, Daniel; Arias de Fuentes, Olimpia; Desdín García, Luis F.; Cazzanelli, Enzo; Caputi, Lorenzo S.

    2015-09-01

    The Raman spectra of polyhedral carbon nano-onions (PCO), obtained by underwater arc discharge of graphite electrodes, are studied. While the general Raman spectrum of PCO is very similar to those of other carbon nanostructures, including spherical nano-onions, the fine structure of the G and 2D bands gives valuable information that allows using Raman spectroscopy for differentiating the PCO from other carbon structures. The interpretation of the features of the fine structure of the spectra is supported by evidences obtained by TEM.

  9. Time-resolved Raman spectroscopy for in situ planetary mineralogy.

    PubMed

    Blacksberg, Jordana; Rossman, George R; Gleckler, Anthony

    2010-09-10

    Planetary mineralogy can be revealed through a variety of remote sensing and in situ investigations that precede any plans for eventual sample return. We briefly review those techniques and focus on the capabilities for on-surface in situ examination of Mars, Venus, the Moon, asteroids, and other bodies. Over the past decade, Raman spectroscopy has continued to develop as a prime candidate for the next generation of in situ planetary instruments, as it provides definitive structural and compositional information of minerals in their natural geological context. Traditional continuous-wave Raman spectroscopy using a green laser suffers from fluorescence interference, which can be large (sometimes saturating the detector), particularly in altered minerals, which are of the greatest geophysical interest. Taking advantage of the fact that fluorescence occurs at a later time than the instantaneous Raman signal, we have developed a time-resolved Raman spectrometer that uses a streak camera and pulsed miniature microchip laser to provide picosecond time resolution. Our ability to observe the complete time evolution of Raman and fluorescence spectra in minerals makes this technique ideal for exploration of diverse planetary environments, some of which are expected to contain strong, if not overwhelming, fluorescence signatures. We discuss performance capability and present time-resolved pulsed Raman spectra collected from several highly fluorescent and Mars-relevant minerals. In particular, we have found that conventional Raman spectra from fine grained clays, sulfates, and phosphates exhibited large fluorescent signatures, but high quality spectra could be obtained using our time-resolved approach.

  10. Power Budget Analysis for Waveguide-Enhanced Raman Spectroscopy.

    PubMed

    Wang, Zilong; Pearce, Stuart J; Lin, Yung-Chun; Zervas, Michalis N; Bartlett, Philip N; Wilkinson, James S

    2016-08-01

    Waveguide-enhanced Raman spectroscopy (WERS) is emerging as an attractive alternative to plasmonic surface-enhanced Raman spectroscopy approaches as it can provide more reproducible quantitative spectra on a robust chip without the need for nanostructured plasmonic materials. Realizing portable WERS systems with high sensitivity using low-cost laser diodes and compact spectrometers requires a detailed analysis of the power budget from laser to spectrometer chip. In this paper, we describe theoretical optimization of planar waveguides for maximum Raman excitation efficiency, demonstrate WERS for toluene on a silicon process compatible high index contrast tantalum pentoxide waveguide, measure the absolute conversion efficiency from pump power to received power in an individual Raman line, and compare this with a power budget analysis of the complete system including collection with an optical fiber and interfacing to a compact spectrometer. Optimized 110 nm thick Ta2O5 waveguides on silica substrates excited at a wavelength of 637 nm are shown experimentally to yield overall system power conversion efficiency of ∼0.5 × 10(-12) from the pump power in the waveguide to the collected Raman power in the 1002 cm(-1) Raman line of toluene, in comparison with a calculated efficiency of 3.9 × 10(-12) Collection efficiency is dictated by the numerical and physical apertures of the spectral detection system but may be improved by further engineering the spatial and angular Raman scattering distributions.

  11. Fiber-optic Raman Spectroscopy of Joint Tissues

    PubMed Central

    Esmonde-White, Karen A.; Esmonde-White, Francis W.L.; Morris, Michael D.

    2011-01-01

    In this study, we report adaptation of Raman spectroscopy for arthroscopy of joint tissues using a custom-built fiber optic probe. Differentiation of healthy and damaged tissue or examination of subsurface tissue, such as subchondral bone, is a challenge in arthroscopy because visual inspection may not provide sufficient contrast. Discrimination of healthy versus damaged tissue may be improved by incorporating point spectroscopy or hyperspectral imaging into arthroscopy where contrast is based on molecular structure or chemical composition. Articular joint surfaces of knee cadaveric human tissue and tissue phantoms were examined using a custom-designed Raman fiber optic probe. Fiber-optic Raman spectra were compared against reference spectra of cartilage, subchondral bone and cancellous bone collected using Raman microspectroscopy. In fiber-optic Raman spectra of the articular surface, there was an effect of cartilage thickness on recovery of signal from subchondral bone. At sites with intact cartilage, the bone mineralization ratio decreased but there was a minimal effect in the bone mineral chemistry ratios. Tissue phantoms were prepared as experimental models of the osteochondral interface. Raman spectra of tissue phantoms suggested that optical scattering of cartilage has a large effect on the relative cartilage and bone signal. Finite element analysis modeling of light fluence in the osteochondral interface confirmed experimental findings in human cadaveric tissue and tissue phantoms. These first studies demonstrate proof of principle for Raman arthroscopic measurement of joint tissues and provide a basis for future clinical or animal model studies. PMID:21359366

  12. The substrate matters in the Raman spectroscopy analysis of cells.

    PubMed

    Mikoliunaite, Lina; Rodriguez, Raul D; Sheremet, Evgeniya; Kolchuzhin, Vladimir; Mehner, Jan; Ramanavicius, Arunas; Zahn, Dietrich R T

    2015-08-27

    Raman spectroscopy is a powerful analytical method that allows deposited and/or immobilized cells to be evaluated without complex sample preparation or labeling. However, a main limitation of Raman spectroscopy in cell analysis is the extremely weak Raman intensity that results in low signal to noise ratios. Therefore, it is important to seize any opportunity that increases the intensity of the Raman signal and to understand whether and how the signal enhancement changes with respect to the substrate used. Our experimental results show clear differences in the spectroscopic response from cells on different surfaces. This result is partly due to the difference in spatial distribution of electric field at the substrate/cell interface as shown by numerical simulations. We found that the substrate also changes the spatial location of maximum field enhancement around the cells. Moreover, beyond conventional flat surfaces, we introduce an efficient nanostructured silver substrate that largely enhances the Raman signal intensity from a single yeast cell. This work contributes to the field of vibrational spectroscopy analysis by providing a fresh look at the significance of the substrate for Raman investigations in cell research.

  13. The substrate matters in the Raman spectroscopy analysis of cells

    PubMed Central

    Mikoliunaite, Lina; Rodriguez, Raul D.; Sheremet, Evgeniya; Kolchuzhin, Vladimir; Mehner, Jan; Ramanavicius, Arunas; Zahn, Dietrich R.T.

    2015-01-01

    Raman spectroscopy is a powerful analytical method that allows deposited and/or immobilized cells to be evaluated without complex sample preparation or labeling. However, a main limitation of Raman spectroscopy in cell analysis is the extremely weak Raman intensity that results in low signal to noise ratios. Therefore, it is important to seize any opportunity that increases the intensity of the Raman signal and to understand whether and how the signal enhancement changes with respect to the substrate used. Our experimental results show clear differences in the spectroscopic response from cells on different surfaces. This result is partly due to the difference in spatial distribution of electric field at the substrate/cell interface as shown by numerical simulations. We found that the substrate also changes the spatial location of maximum field enhancement around the cells. Moreover, beyond conventional flat surfaces, we introduce an efficient nanostructured silver substrate that largely enhances the Raman signal intensity from a single yeast cell. This work contributes to the field of vibrational spectroscopy analysis by providing a fresh look at the significance of the substrate for Raman investigations in cell research. PMID:26310910

  14. Potential of Raman and Infrared Spectroscopy for Plant Analysis

    NASA Astrophysics Data System (ADS)

    Schulz, H.

    2008-11-01

    Various mid-infrared (MIR) and Raman spectroscopic methods applied to the analysis of valuable plant substances or quality parameters in selected horticultural and agricultural crops are presented. Generally, both spectroscopy techniques allow to identify simultaneously characteristic key bands of individual plant components (e.g. carotenoids, alkaloids, polyacetylenes, fatty acids, amino acids, terpenoids). In contrast to MIR methods Raman spectroscopy mostly does not need any sample pre-treatment; even fresh plant material can be analysed without difficulty because water shows only weak Raman scattering properties. In some cases a significant sensivity enhancement of Raman signals can be achieved if the exciting laser wavelength is adjusted to the absorption range of particular plant chromophores such as carotenoids (Resonance Raman effect). Applying FT-IR or FT Raman micro-spectroscopy the distribution of certain plant constituents in the cell wall can be identified without the need for any physical separation. Furthermore it is also possible to analyse secondary metabolites occurring in the cell vacuoles if significant key bands do not coincide with the spectral background of the plant matrix.

  15. Raman spectroscopy of blood in-vitro

    NASA Astrophysics Data System (ADS)

    Villanueva-Luna, A. E.; Castro-Ramos, J.; Vazquez-Montiel, S.; Flores-Gil, A.; Ortiz-Lima, C. M.; Delgado-Atencio, J. A.

    2012-03-01

    We present Raman spectra from a sample of 8 volunteers that have different type of blood. The experimental data were carried out using a 785 nm excitation laser and an ocean optics spectrometer of 6 cm-1 resolution, with a used spectral region from 1000 to 1800 cm-1. We find Raman features at 1000 and 1542 cm-1 regarded with hemoglobin and its derivatives. Also we find Raman features at 1248 and 1342 cm-1 that are now regarded with pure fibrin. In this work, we use Principal Component analysis (PCA) to determine all variations of our samples, which allows us to define a classification of the influence of the blood type. Finally, we found vibrational lines of cholesterol, glucose and triglycerides that are reported in literature.

  16. Characterization of oil-producing microalgae using Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Samek, O.; Zemánek, P.; Jonáš, A.; Telle, H. H.

    2011-10-01

    Raman spectroscopy offers a powerful alternative analytical method for the detection and identification of lipids/oil in biological samples, such as algae and fish. Recent research in the authors' groups, and experimental data only very recently published by us and a few other groups suggest that Raman spectroscopy can be exploited in instances where fast and accurate determination of the iodine value (associated with the degree of lipid unsaturation) is required. Here the current status of Raman spectroscopy applications on algae is reviewed, and particular attention is given to the efforts of identifying and selecting oil-rich algal strains for the potential mass production of commercial biofuels and for utilization in the food industry.

  17. Two-dimensional Raman-terahertz spectroscopy of water

    PubMed Central

    Savolainen, Janne; Ahmed, Saima; Hamm, Peter

    2013-01-01

    Two-dimensional Raman-terahertz (THz) spectroscopy is presented as a multidimensional spectroscopy directly in the far-IR regime. The method is used to explore the dynamics of the collective intermolecular modes of liquid water at ambient temperatures that emerge from the hydrogen-bond networks water forming. Two-dimensional Raman-THz spectroscopy interrogates these modes twice and as such can elucidate couplings and inhomogeneities of the various degrees of freedoms. An echo in the 2D Raman-THz response is indeed identified, indicating that a heterogeneous distribution of hydrogen-bond networks exists, albeit only on a very short 100-fs timescale. This timescale appears to be too short to be compatible with more extended, persistent structures assumed within a two-state model of water. PMID:24297930

  18. Dengue blood analysis by Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Rehman, A.; Anwar, S.; Firdous, S.; Ahmed, M.; Rasheed, R.; Nawaz, M.

    2012-06-01

    In this work Raman spectra of normal and dengue infected serum and whole blood were analyzed. In normal whole blood and serum characteristic peaks were observed when excited at 442 and 532 nm. In dengue whole blood and serum all peaks found to be blue shifted with reduced Raman intensity. Dengue whole blood and serum shows two peaks at 1614 and 1750 cm-1 which are due to presence of Immunoglobulin antibodies IgG and IgM. Whole study provides a route of information for diagnosis of dengue viral infection.

  19. Metallized Capillaries as Probes for Raman Spectroscopy

    NASA Technical Reports Server (NTRS)

    Pelletier, Michael

    2003-01-01

    A class of miniature probes has been proposed to supplant the fiber-optic probes used heretofore in some Raman and fluorescence spectroscopic systems. A probe according to the proposal would include a capillary tube coated with metal on its inside to make it reflective. A microlens would be hermetically sealed onto one end of the tube. A spectroscopic probe head would contain a single such probe, which would both deliver laser light to a sample and collect Raman or fluorescent light emitted by the sample.

  20. Characterization of propellants under thermal stress by Raman Spectroscopy

    SciTech Connect

    Fell, N.F. Jr.; McNesby, K.L.

    1995-12-31

    Raman spectroscopy is used in the characterization of propellant temperatures. Both FT-Raman grains during exposure to elevate with NIR (1064 nm, Nd:YAG) excitation and a dispersive system with visible (514.5 nm, Ar+ laser) excitation are used and compared. Raman spectroscopy permits the in situ examination of propellants during the heating process. By looking at the Raman spectra of the various propellants as a function of temperature, it is possible to evaluate effects of binders and plasticizers on the thermal behavior of the propellants. Such information may be useful for estimating the effective shelf lives of propellants. The scattering intensity decreases as a function of temperature as a result of the loss in crystallinity of the principal component of the formulation as it is heated above its melting point. Since the gas-phase decomposition products are not observed and therefore do not interfere with the collection of the scattered emission from the condensed-phase products, Raman spectroscopy also allows the examination of only the condensed-phase decomposition products. This is a significant advantage over absorption spectroscopies, such as FTIR and UV-VIS absorption, which are sensitive to all of the components in the beam path. The use of visible wavelength excitation should prevent thermal damage to the sample observed with the NIR laser. A slight red shift of the features below 500 cm-1, especially in the feature at 150 cm-1, is observed. The peaks also broaden with increasing temperature, as would be expected.

  1. Characterization of uranium tetrafluoride (UF4) with Raman spectroscopy

    DOE PAGES

    Villa-Aleman, Eliel; Wellons, Matthew S.

    2016-03-22

    The Raman spectrum of uranium tetrafluoride (UF4) is unambiguously characterized with multiple Raman excitation laser sources for the first time. Across different laser excitation wavelengths, UF4 demonstrates 16 distinct Raman bands within the 50-400 cm-1 region. The observed Raman bands are representative of various F-F vibrational modes. UF4 also shows intense fluorescent bands in the 325 – 750 nm spectral region. Comparison of the UF4 spectrum with the ZrF4 spectrum, its crystalline analog, demonstrates a similar Raman band structure consistent with group theory predictions for expected Raman bands. Additionally, a demonstration of combined scanning electron microscopy (SEM) and in situmore » Raman spectroscopy microanalytical measurements of UF4 particulates shows that despite the inherent weak intensity of Raman bands, identification and characterization are possible for micron-sized particulates with modern instrumentation. The published well characterized UF4 spectrum is extremely relevant to nuclear materials and nuclear safeguard applications.« less

  2. Spectro-temporal shaping of supercontinuum for subnanosecond time-coded M-CARS spectroscopy.

    PubMed

    Shalaby, Badr M; Louot, Christophe; Capitaine, Erwan; Krupa, Katarzyna; Labruyère, Alexis; Tonello, Alessandro; Pagnoux, Dominique; Leproux, Philippe; Couderc, Vincent

    2016-11-01

    A supercontinuum laser source was designed for multiplex-coherent anti-Stokes Raman scattering spectroscopy. This source was based on the use of a germanium-doped standard optical fiber with a zero dispersion wavelength at 1600 nm and pumped at 1064 nm. We analyzed the nonlinear spectro-temporal interrelations of a subnanosecond pulse propagating in a normal dispersion regime in the presence of a multiple Raman cascading process and strong conversion. The multiple Raman orders permitted the generation of a high-power flat spectrum with a specific nonlinear dynamics that can open the way to subnanosecond time-coded multiplex CARS systems.

  3. FIFTH SEMINAR IN MEMORY OF D.N. KLYSHKO: Anti-Stokes femtosecond photon echo in a polymer film

    NASA Astrophysics Data System (ADS)

    Petrushkin, S. V.; Samartsev, V. V.

    2007-12-01

    An anti-Stokes model is proposed which explains the room-temperature blue shift of the echo-signal spectrum compared to the spectrum of exciting femtosecond pulses in a polymer film doped with dye molecules. The possibility of realising the anti-Stokes regime of coherent laser cooling of such films is analysed.

  4. Raman spectroscopy of garnet-group minerals

    USGS Publications Warehouse

    Mingsheng, P.; Mao, Ho-kwang; Dien, L.; Chao, E.C.T.

    1994-01-01

    The Raman spectra of the natural end members of the garnet-group minerals, which include pyrope, almandine and spessarite of Fe-Al garnet series and grossularite, andradite and uvarovite of Ca-Fe garnet series, have been studied. Measured Raman spectra of these minerals are reasonably and qualitatively assigned to the internal modes, translational and rotatory modes of SiO4 tetrahedra, as well as the translational motion of bivalent cations in the X site. The stretch and rotatory Alg modes for the Fe-Al garnet series show obvious Raman shifts as compared with those for the Ca-Fe garnet series, owing to the cations residing in the X site connected with SiO4 tetrahedra by sharing the two edges. The Raman shifts of all members within either of the series are attributed mainly to the properties of cations in the X site for the Fe-Al garnet series and in the Y site for the Ca-Fe garnet series. ?? 1994 Institute of Geochemistry, Chinese Academy of Sciences.

  5. Interferometric background reduction for femtosecond stimulated Raman scattering loss spectroscopy.

    PubMed

    Dobner, Sven; Cleff, Carsten; Fallnich, Carsten; Groß, Petra

    2012-11-07

    We present a purely optical method for background suppression in nonlinear spectroscopy based on linear interferometry. Employing an unbalanced Sagnac interferometer, an unprecedented background reduction of 17  dB over a broad bandwidth of 60  THz (2000  cm(-1)) is achieved and its application to femtosecond stimulated Raman scattering loss spectroscopy is demonstrated. Apart from raising the signal-to-background ratio in the measurement of the Raman intensity spectrum, this interferometric method grants access to the spectral phase of the resonant χ(3) contribution. The spectral phase becomes apparent as a dispersive lineshape and is reproduced numerically with a simple oscillator model.

  6. In vivo molecular labeling of halogenated volatile anesthetics via intrinsic molecular vibrations using nonlinear Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Nagashima, Yu; Suzuki, Takayuki; Terada, Sumio; Tsuji, Shoji; Misawa, Kazuhiko

    2011-01-01

    Halogenated volatile anesthetics are frequently used for inhaled anesthesia in clinical practice. No appropriate biological method has been available for visualizing their localization in action. Therefore, despite their frequent use, the mechanism of action of these drugs has not been fully investigated. We measured coherent anti-Stokes Raman scattering (CARS) spectra of sevoflurane and isoflurane, two of the most representative volatile anesthetics, and determined the low-frequency vibrational modes without nonresonant background disturbance. Molecular dynamics calculations predict that these modes are associated with multiple halogen atoms. Because halogen atoms rarely appear in biological compounds, the entire spectral landscape of these modes is expected to be a good marker for investigating the spatial localization of these drugs within the intracellular environment. Using live squid giant axons, we could detect the unique CARS spectra of sevoflurane for the first time in a biological setting.

  7. Development and biological applications of optical tweezers and Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Xie, Chang'an

    Optical tweezers is a three-dimensional manipulation tool that employs a gradient force that originates from the single highly focused laser beam. Raman spectroscopy is a molecular analytical tool that can give a highly unique "fingerprint" for each substance by measuring the unique vibrations of its molecules. The combination of these two optical techniques offers a new tool for the manipulation and identification of single biological cells and microscopic particles. In this thesis, we designed and implemented a Laser-Tweezers-Raman-Spectroscopy (LTRS) system, also called the Raman-tweezers, for the simultaneous capture and analysis of both biological particles and non-biological particles. We show that microparticles can be conveniently captured at the focus of a laser beam and the Raman spectra of trapped particles can be acquired with high quality. The LTRS system overcomes the intrinsic Brownian motion and cell motility of microparticles in solution and provides a promising tool for in situ identifying suspicious agents. In order to increase the signal to noise ratio, several schemes were employed in LTRS system to reduce the blank noise and the fluorescence signal coming from analytes and the surrounding background. These techniques include near-infrared excitation, optical levitation, confocal microscopy, and frequency-shifted Raman difference. The LTRS system has been applied for the study in cell biology at the single cell level. With the built Raman-tweezers system, we studied the dynamic physiological processes of single living cells, including cell cycle, the transcription and translation of recombinant protein in transgenic yeast cells and the T cell activation. We also studied cell damage and associated biochemical processes in optical traps, UV radiations, and evaluated heating by near-infrared Raman spectroscopy. These studies show that the Raman-tweezers system is feasible to provide rapid and reliable diagnosis of cellular disorders and can be

  8. Condition Assessment of Kevlar Composite Materials Using Raman Spectroscopy

    NASA Technical Reports Server (NTRS)

    Washer, Glenn; Brooks, Thomas; Saulsberry, Regor

    2007-01-01

    This viewgraph presentation includes the following main concepts. Goal: To evaluate Raman spectroscopy as a potential NDE tool for the detection of stress rupture in Kevlar. Objective: Test a series of strand samples that have been aged under various conditions and evaluate differences and trends in the Raman response. Hypothesis: Reduction in strength associated with stress rupture may manifest from changes in the polymer at a molecular level. If so, than these changes may effect the vibrational characteristics of the material, and consequently the Raman spectra produced from the material. Problem Statement: Kevlar composite over-wrapped pressure vessels (COPVs) on the space shuttles are greater than 25 years old. Stress rupture phenomena is not well understood for COPVs. Other COPVs are planned for hydrogen-fueled vehicles using Carbon composite material. Raman spectroscopy is being explored as an non-destructive evaluation (NDE) technique to predict the onset of stress rupture in Kevlar composite materials. Test aged Kevlar strands to discover trends in the Raman response. Strength reduction in Kevlar polymer will manifest itself on the Raman spectra. Conclusions: Raman spectroscopy has shown relative changes in the intensity and FWHM of the 1613 cm(exp -1) peak. Reduction in relative intensity for creep, fleet leader, and SIM specimens compared to the virgin strands. Increase in FWHM has been observed for the creep and fleet leader specimens compared to the virgin strands. Changes in the Raman spectra may result from redistributing loads within the material due to the disruption of hydrogen bonding between crystallites or defects in the crystallites from aging the Kevlar strands. Peak shifting has not been observed to date. Analysis is ongoing. Stress measurements may provide a tool in the short term.

  9. Stokes and anti-stokes stimulated Mie scattering on nanoparticle suspensions of latex

    NASA Astrophysics Data System (ADS)

    Burkhanov, I. S.; Krivokhizha, S. V.; Chaikov, L. L.

    2016-12-01

    Stokes and anti-Stokes shifts of stimulated concentration light scattering (SCLS, stimulated Mie scattering) in suspensions of various-sized latex nanoparticles in water were measured by the light guide scheme, under conditions of backscattering in the presence of convection.

  10. Kerr-gated picosecond Raman spectroscopy and Raman photon migration of equine bone tissue with 400-nm excitation

    NASA Astrophysics Data System (ADS)

    Morris, Michael D.; Goodship, Allen E.; Draper, Edward R. C.; Matousek, Pavel; Towrie, Michael; Parker, Anthony W.

    2004-07-01

    We show that Raman spectroscopy with visible lasers, even in the deep blue is possible with time-gated Raman spectroscopy. A 4 picosec time gate allows efficient fluorescence rejection, up to 1000X, and provides almost background-free Raman spectra with low incident laser power. The technology enables spectroscopy with better than 10X higher scattering efficiency than is possible with the NIR (785 nm and 830 nm) lasers that are conventionally used. Raman photon migration is shown to allow depth penetration. We show for the first time that Kerr-gated Raman spectra of bone tissue with blue laser excitation enables both fluorescence rejection and depth penetration.

  11. Application of the Raman Spectroscopy to Identification of Titanomagnetites

    NASA Astrophysics Data System (ADS)

    Tatsumi-Petrochilos, L.; Gilder, S. A.; Zinin, P.; Hammer, J. E.; Fuller, M. D.

    2008-12-01

    The titanomagnetite-magnetite series serves as important magnetic carriers in paleomagnetic studies. Commonly Curie points are used to determine the composition of these magnetic phases. However, Curie points generally reflect bulk rock properties and do not provide insight for individual grains. Determination of individual Fe-Ti oxide grains can be done by petrography or with electron microprobe techniques. In contrast to these methods, which require special sample preparation, Raman spectroscopy can be done with minimal preparation. We have therefore investigated the Raman spectra for magnetite, TM20, TM40, and TM60, so that we can identify titanomagnetites with different Ti content in rocks. The samples were prepared following methods of Wanamaker and Moskovitz (1994). The Ti concentrations were verified by thermomagnetic analysis (Gilder and LeGoff, 2005). The Raman spectra were obtained with WITec Raman Confocal Microscope 200 using a green laser. Slight shifts and changes in relative intensities of the peaks at the characteristic wavelengths of the Raman spectra that correspond to different molecular vibrations were observed. These changes can serve to identify the composition of individual titanomagnetite grains. It also enables mapping of the variation of the composition within grains and the distribution of compositions of grains within a rock. We have applied the technique to synthetic Martian samples and found relatively uniform compositions between different grains. In contrast, variable oxide compositions are discerned using the Raman spectroscopy in natural basalts erupted from East Maui volcano.

  12. Vibrational characterization of pheomelanin and trichochrome F by Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Galván, Ismael; Jorge, Alberto; Solano, Francisco; Wakamatsu, Kazumasa

    2013-06-01

    We characterize for the first time the vibrational state of natural pheomelanin using Raman spectroscopy and model pigment synthesized from 5-S-cysteinyldopa. The shape of the Raman spectrum was very different from that of eumelanin. Four Raman bands were visible in the 500-2000 cm-1 wavenumber region about 500, 1150, 1490 and 2000 cm-1, which we assigned to the out-of-plane deformation and the stretching vibration of the phenyl rings, to the stretching vibration of C-N bonds or the stretching and wagging vibration of CH2, and to overtone or combination bands. Interestingly, we also show that the Raman spectrum of synthetic trichochrome F, a pigment that may be produced along with pheomelanin during pheomelanogenesis, is different from that of pheomelanin and similar to the spectrum of eumelanin. We could detect Raman signal of both eumelanin and pheomelanin in feathers and hairs where both pigments simultaneously occur without the need of isolating the pigment. This indicates that Raman spectroscopy represents a non-invasive method to detect pheomelanin and distinguish it from other pigments. This may be especially relevant to detect pheomelanin in animal skin including humans, where it has been associated with animal appearance and classification, human phototypes, prevention of skin diseases and cancer risk.

  13. [Study on the treatment turquoise using Raman spectroscopy].

    PubMed

    Chen, Quan-li; Yuan, Xin-qiang; Chen, Jing-zhong; Qi, Li-jian

    2010-07-01

    Due to a variety of the enhancement and treatment turquoises discovered in gem markets, the identification of turquoise is becoming more and more difficult. By using laser Raman spectroscopy analysis, the characteristics of Raman spectra of the pressed and filled turquoises were studied. The results show that laser Raman spectroscopy is an effective technique to identify the enhancement and treatment turquoises and the natural ones, moreover, it's a non-destructive testing method. The Raman spectra of the enhancement and treatment turquoises are resulted mainly from the vibrational mode and frequency of water, hydroxyl units, PO4 tetrahedron and CH2 units. Besides, they have the characteristic Raman spectra peaks at 2,937, 2,883 and 1,451 cm(-1) which are attributed to the stretching vibration and the bending vibration of CH2, respectively. These characteristic Raman vibration bands, it will help to distinguish the natural turquoises and the treatment ones. The study provides a new train of thought on the rapid, accurate, and non-destructive identification of turquoise.

  14. Raman Spectroscopy Study of Prostatic Adenocarcinoma Bulk Tissues

    NASA Astrophysics Data System (ADS)

    Devpura, S.; Dai, H.; Thakur, J. S.; Naik, R.; Cao, A.; Pandya, A.; Auner, G. W.; Sarkar, F.; Sakr, W.; Naik, V.

    2009-03-01

    Prostate cancer is one of the most common types of cancer among men. The mortality rate for this disease can be dramatically reduced if it can be diagnosed in its early stages. Raman spectroscopy is one of the optical techniques which can provide fingerprints of a disease in terms of its molecular composition which changes due to the onset of disease. The aim of this project is to investigate the differences in the Raman spectra to identify benign epithelium (BE), prostatic intraepithelial neoplasia (PIN) and adenocarcinoma of various Gleason grades in archived bulk tissues embedded in paraffin wax. For each tissue, two adjacent tissue sections were cut and dewaxed, where one of the sections was stained using haematoxylin and eosin for histological examination and the other unstained adjacent section was used for Raman spectroscopic studies. We have collected Raman spectra from 10 prostatic adenocarcinoma dewaxed tissue sections using Raman microscope (785 nm excitation laser). The data were analyzed using statistical methods of principal component analysis and discriminant function analysis to classify the tissue regions. The results indicate that Raman Spectroscopy can differentiate between BE, PIN and Cancer regions.

  15. Resonance Raman spectroscopy in twisted bilayer graphene

    NASA Astrophysics Data System (ADS)

    Righi, A.; Venezuela, P.; Chacham, H.; Costa, S. D.; Fantini, C.; Ruoff, R. S.; Colombo, L.; Bacsa, W. S.; Pimenta, M. A.

    2013-12-01

    In this work we study the Raman spectra of twisted bilayer graphene samples, with different twisting angles, by changing the incident laser energy between 2.54 and 4.14 eV. The spectra exhibit a number of extra peaks, classified in different families, each one associated with bilayer graphenes with different twisting rotational angles. We theoretically analyze the laser energy dependence of these extra peaks considering a set of discrete wavevectors within the interior of the Brillouin zone of graphene, which activate special double-resonance Raman processes. Our result show a nice qualitative agreement between the experimental and simulated spectra, demonstrating that these extra peaks are indeed ascribed to an umklapp double-resonance process in graphene systems.

  16. Raman spectroscopy for bacterial identification and characterization

    NASA Astrophysics Data System (ADS)

    Bernatová, Silvie; Samek, Ota; Pilát, Zdeněk.; Šerý, Mojmír.; Ježek, Jan; Krzyžánek, Vladislav; Zemánek, Pavel; Ružička, Filip

    2012-01-01

    The main goal of our investigation is to use Raman tweezers technique so that the responce of Raman scattering on microorganisms suspended in liquid media (bacteria, algae and yeast cells in microfluidic chips) can be used to identify different species. The investigations presented here include identification of different bacteria strains (biofilm-positive and biofilm-negative) and yeast cells by using principal component analysis (PCA). The main driving force behind our investigation was a common problem in the clinical microbiology laboratory - how to distinguish between contaminant and invasive isolates. Invasive bacterial/yeast isolates can be assumed to form a biofilm, while isolates which do not form a biofilm can be treated as contaminant. Thus, the latter do not represent an important virulence factor.

  17. Raman spectroscopy: Caution when interpreting organic carbon from oxidising environments

    NASA Astrophysics Data System (ADS)

    Brolly, Connor; Parnell, John; Bowden, Stephen

    2016-02-01

    Oxidation on Mars is primarily caused by the high influx of cosmic and solar radiation which interacts with the Martian surface. The evidence of this can be seen in the ubiquitous red colouration of the Martian sediment. This radiation will destroy most signals of life in the top few metres of the Martian surface. If organic carbon (one of the building blocks of life) is present within the accessible Martian sediments, it is very likely that it will have experienced some oxidation. ESA's ExoMars mission set to fly in 2018, has on board a miniaturised Raman spectrometer. As Raman spectroscopy is sensitive to carbonaceous material and will be primarily used to characterise organics, it is essential that the effect oxidation has on the Raman carbon signal is assessed. Oxidised carbonaceous shales were analysed using Raman spectroscopy to assess this issue. Results show that haematite has a band which occurs in the same frequency as the carbon D band, which cannot be distinguished from each other. This can lead to a misidentification of the carbon D band and a misinterpretation of the carbon order. Consequently, caution must be taken when applying Raman spectroscopy for organic carbon analysis in oxidised terrestrial and extraterrestrial environments, including on Mars.

  18. Remote temperature monitoring in ocular tissue using confocal Raman spectroscopy.

    PubMed

    Bauer, Noel J C; Motamedi, Massoud; Hendrikse, Fred; Wicksted, James P

    2005-01-01

    We demonstrated the feasibility of Raman spectroscopy for remote temperature monitoring within the aqueous humor of the rabbit eye in vivo. Using a confocal Raman spectroscopy system, Raman spectra from 2580 to 3800 cm(-1) were recorded in HPLC-grade water and in the aqueous humor of the rabbit eye under in vivo and ex vivo conditions within a temperature range of 14-34 degrees C. The ratio between the integrated Raman intensities of two temperature dependent OH-vibrational regions (OH2/OH1) in the spectra of water showed high linear dependence on temperature both in pure water [0.0049(+/-1.2%)T+0.4522(+/-0.5%), R2=0.99, n=50, p<0.05], as well as in the rabbit aqueous humor [0.0036(+/-2.8%)T+0.4966(+/-0.6%), R2=0.98, n=162, p<0.05] with a high degree of reproducibility and sensitivity ( approximately 0.2-0.7 degrees C). Raman spectroscopy can be used for high resolution and remote monitoring of temperature in the aqueous humor under in vivo conditions.

  19. Probing Nanoscale Ferroelectricity by Ultraviolet Raman Spectroscopy

    DTIC Science & Technology

    2006-09-15

    gap materials because the visible photon energy is much smaller than the band gap (10). Consequently, the absorption is extremely weak and the...UV ex- citation, the photon energy is above the band gaps of ferroelectrics, leading to a much stronger absorption and a shorter penetration depth...preventing light from entering the substrate. UV excitation near the band gap also leads to strong resonance enhancement of Raman sig- nals. This is

  20. Raman spectroscopy and oral exfoliative cytology

    NASA Astrophysics Data System (ADS)

    Sahu, Aditi; Shah, Nupur; Mahimkar, Manoj; Garud, Mandavi; Pagare, Sandeep; Nair, Sudhir; Krishna, C. Murali

    2014-03-01

    Early detection of oral cancers can substantially improve disease-free survival rates. Ex vivo and in vivo Raman spectroscopic (RS) studies on oral cancer have demonstrated the applicability of RS in identifying not only malignant and premalignant conditions but also cancer-field-effects: the earliest events in oral carcinogenesis. RS has also been explored for cervical exfoliated cells analysis. Exfoliated cells are associated with several advantages like non-invasive sampling, higher patient compliance, transportation and analysis at a central facility: obviating need for on-site instrumentation. Thus, oral exfoliative cytology coupled with RS may serve as a useful adjunct for oral cancer screening. In this study, exfoliated cells from healthy controls with and without tobacco habits, premalignant lesions (leukoplakia and tobacco-pouch-keratosis) and their contralateral mucosa were collected using a Cytobrush. Cells were harvested by vortexing and centrifugation at 6000 rpm. The cellular yield was ascertained using Neubauer's chamber. Cell pellets were placed on a CaF2 window and Raman spectra were acquired using a Raman microprobe (40X objective) coupled HE-785 Raman spectrometer. Approximately 7 spectra were recorded from each pellet, following which pellet was smeared onto a glass slide, fixed in 95% ethanol and subjected to Pap staining for cytological diagnosis (gold standard). Preliminary PC-LDA followed by leave-one-out cross validation indicate delineation of cells from healthy and all pathological conditions. A tendency of classification was also seen between cells from contralateral, healthy tobacco and site of premalignant lesions. These results will be validated by cytological findings, which will serve as the basis for building standard models of each condition.