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Sample records for raman scattering imaging

  1. Stimulated Raman scattering microscopy for biomedical imaging

    NASA Astrophysics Data System (ADS)

    Min, Wei; Freudiger, Christian W.; Lu, Sijia; He, Chengwei; Kang, Jing X.; Xie, X. Sunney

    2009-02-01

    Label-free chemical contrast is highly desirable in biomedical imaging. Spontaneous Raman microscopy provides specific vibrational signatures of chemical bonds, but is often hindered by low sensitivity. Here we report a 3D multi-photon vibrational imaging technique based on stimulated Raman scattering (SRS). The sensitivity of SRS is significantly greater than that of spontaneous Raman scattering, and is further enhanced by high-frequency (MHz) phase-sensitive detection. SRS microscopy has a major advantage over previous coherent Raman techniques in that it offers background-free and easily interpretable chemical contrast. We show 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.

  2. Image formation using stimulated raman scattering gain

    NASA Astrophysics Data System (ADS)

    Bespalov, V. G.; Makarov, E. A.; Stasel'ko, D. I.

    2016-07-01

    Theoretical analysis of the spatial, noise, and energy characteristics of an amplifier has been performed in the mode of spectral and time selection using subnanosecond stimulated Raman Scattering gain of weak echo signals in crystalline active media that are known for high (up to 10-1 cm/MW) gain coefficients. The possibility to reach high gain values has been demonstrated for weak signals from objects at acceptable angular sizes of the field of vision of an amplifier. To provide a signal-to-noise ratio that exceeds unity over the entire field of vision, the number of photons at the input to an amplifier that is required has to exceed the number of its resolution elements. Accurate determination of the possibilities of recording of weak echo signals and quality of images of targets that are obtained using amplifiers under stimulated Raman Scattering requires additional special experiments.

  3. Morphology-dependent stimulated Raman scattering imaging. I. Theoretical aspects

    SciTech Connect

    Aker, P.M.; Moortgat, P.A.; Zhang, J.

    1996-11-01

    Morphology-dependent stimulated Raman scattering is a nonlinear laser Raman spectroscopy that relies on using the cavity modes associated with micron-sized structures to enhance optical signal generation. Since different cavity modes occupy different regions in space, location-specific spectra can be generated. Here we outline the physics behind morphology-dependent stimulated Raman scattering imaging and model the signal generation process. The results show that a simple tailoring of the illumination conditions allows signal from single, but selectable, cavity modes to be generated. Thus, this nonlinear Raman technique can be used to image spatial variations in chemical composition and/or molecular structure within microstructures. {copyright} {ital 1996 American Institute of Physics.}

  4. Multimodality Raman and photoacoustic imaging of surface-enhanced-Raman-scattering-targeted tumor cells

    NASA Astrophysics Data System (ADS)

    Shi, Wei; Paproski, Robert J.; Shao, Peng; Forbrich, Alexander; Lewis, John D.; Zemp, Roger J.

    2016-02-01

    A multimodality Raman and photoacoustic imaging system is presented. This system has ultralow background and can detect tumor cells labeled with modified surface-enhanced-Raman-scattering (SERS) nanoparticles in vivo. Photoacoustic imaging provides microvascular context and can potentially be used to guide magnetic trapping of circulating tumor cells for SERS detection in animal models.

  5. Coherent Raman Scattering: Methods Towards Imaging with High Sensitivity

    NASA Astrophysics Data System (ADS)

    Bachler, Brandon Richard

    Coherent Raman spectroscopy is a powerful tool for molecular identification. For imaging applications, Raman spectroscopy techniques have offered a way of achieving endogenous chemical contrast without the need for fluorescent labeling. Increasing the sensitivity of Raman scattering microscopy is vital to performing high speed, chemically selective imaging. This thesis presents three experiments with the ultimate goal of increasing the sensitivity and quantifying limitations of different Raman techniques. The first experiment is a comparison of spontaneous and coherent Raman signal strengths under biological imaging conditions. While it is commonly stated in the literature that coherent Raman techniques provide orders of magnitude higher signal than spontaneous Raman, such a comparison has not been done under the low concentration, low excitation power conditions relevant for biological imaging. We determine a critical power above which coherent Raman methods provide higher signal and below which spontaneous Raman methods provide higher sensitivity. Contrary to what is commonly stated in the literature, spontaneous Raman can provide higher signal levels under common biological imaging conditions. The second experiment is a demonstration of the first multiplexed Raman-induced Kerr effect (BIKES) microscopy setup to date. We compare the signal-to-noise ratios between femtosecond stimulated Raman (FSRS) and RIKES for spectroscopy applications in solution and for microscopy applications with polystyrene beads. We find that for our samples, RIKES consistently provides a higher signal-to-noise ratio than FSRS for both applications. We also use RIKES microscopy to map out the distribution of cytoplasm in onion cells. Finally, a surface-enhanced Raman experiment is performed to observe and compare highly enhanced signals for spontaneous and coherent Raman spectroscopy. We use a commercial SERS substrate and observe significantly enhanced spontaneous Raman signals from

  6. Dental caries imaging using hyperspectral stimulated Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Wang, Zi; Zheng, Wei; Jian, Lin; Huang, Zhiwei

    2016-03-01

    We report the development of a polarization-resolved hyperspectral stimulated Raman scattering (SRS) imaging technique based on a picosecond (ps) laser-pumped optical parametric oscillator system for label-free imaging of dental caries. In our imaging system, hyperspectral SRS images (512×512 pixels) in both fingerprint region (800-1800 cm-1) and high-wavenumber region (2800-3600 cm-1) are acquired in minutes by scanning the wavelength of OPO output, which is a thousand times faster than conventional confocal micro Raman imaging. SRS spectra variations from normal enamel to caries obtained from the hyperspectral SRS images show the loss of phosphate and carbonate in the carious region. While polarization-resolved SRS images at 959 cm-1 demonstrate that the caries has higher depolarization ratio. Our results demonstrate that the polarization resolved-hyperspectral SRS imaging technique developed allows for rapid identification of the biochemical and structural changes of dental caries.

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

    PubMed

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

    2016-08-15

    We demonstrate an ambient light coherent anti-Stokes Raman scattering microscope that allows CARS imaging to be operated under environmental light for field use. The 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. The filters in both the spectral domain and the frequency domain effectively blocked the room light contamination of the CARS image. In situ hyperspectral CARS imaging of tumor tissue under ambient light is demonstrated. PMID:27519113

  8. Two-dimensional imaging of sprays with fluorescence, lasing, and stimulated Raman scattering

    SciTech Connect

    Acker, W.P. ); Serpenguezel, A.; Swindal, J.C.; Chang, R.K. )

    1992-06-20

    Two-dimensional fluorescence, lasing, and stimulated Raman scattering images of a hollow-cone nozzle spray are observed. The various constituents of the spray, such as vapor, liquid ligaments, small droplets, and large droplets, are distinguished by selectively imaging different colors associated with the inelastic light-scattering processes.

  9. Subcellular chemical and morphological analysis by stimulated Raman scattering microscopy and image analysis techniques.

    PubMed

    D'Arco, Annalisa; Brancati, Nadia; Ferrara, Maria Antonietta; Indolfi, Maurizio; Frucci, Maria; Sirleto, Luigi

    2016-05-01

    The visualization of heterogeneous morphology, segmentation and quantification of image features is a crucial point for nonlinear optics microscopy applications, spanning from imaging of living cells or tissues to biomedical diagnostic. In this paper, a methodology combining stimulated Raman scattering microscopy and image analysis technique is presented. The basic idea is to join the potential of vibrational contrast of stimulated Raman scattering and the strength of imaging analysis technique in order to delineate subcellular morphology with chemical specificity. Validation tests on label free imaging of polystyrene-beads and of adipocyte cells are reported and discussed. PMID:27231626

  10. Subcellular chemical and morphological analysis by stimulated Raman scattering microscopy and image analysis techniques

    PubMed Central

    D’Arco, Annalisa; Brancati, Nadia; Ferrara, Maria Antonietta; Indolfi, Maurizio; Frucci, Maria; Sirleto, Luigi

    2016-01-01

    The visualization of heterogeneous morphology, segmentation and quantification of image features is a crucial point for nonlinear optics microscopy applications, spanning from imaging of living cells or tissues to biomedical diagnostic. In this paper, a methodology combining stimulated Raman scattering microscopy and image analysis technique is presented. The basic idea is to join the potential of vibrational contrast of stimulated Raman scattering and the strength of imaging analysis technique in order to delineate subcellular morphology with chemical specificity. Validation tests on label free imaging of polystyrene-beads and of adipocyte cells are reported and discussed. PMID:27231626

  11. Subcellular chemical and morphological analysis by stimulated Raman scattering microscopy and image analysis techniques.

    PubMed

    D'Arco, Annalisa; Brancati, Nadia; Ferrara, Maria Antonietta; Indolfi, Maurizio; Frucci, Maria; Sirleto, Luigi

    2016-05-01

    The visualization of heterogeneous morphology, segmentation and quantification of image features is a crucial point for nonlinear optics microscopy applications, spanning from imaging of living cells or tissues to biomedical diagnostic. In this paper, a methodology combining stimulated Raman scattering microscopy and image analysis technique is presented. The basic idea is to join the potential of vibrational contrast of stimulated Raman scattering and the strength of imaging analysis technique in order to delineate subcellular morphology with chemical specificity. Validation tests on label free imaging of polystyrene-beads and of adipocyte cells are reported and discussed.

  12. 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

  13. Fast Vibrational Imaging of Single Cells and Tissues by Stimulated Raman Scattering Microscopy

    PubMed Central

    2015-01-01

    Conspectus Traditionally, molecules are analyzed in a test tube. Taking biochemistry as an example, the majority of our knowledge about cellular content comes from analysis of fixed cells or tissue homogenates using tools such as immunoblotting and liquid chromatography–mass spectrometry. These tools can indicate the presence of molecules but do not provide information on their location or interaction with each other in real time, restricting our understanding of the functions of the molecule under study. For real-time imaging of labeled molecules in live cells, fluorescence microscopy is the tool of choice. Fluorescent labels, however, are too bulky for small molecules such as fatty acids, amino acids, and cholesterol. These challenges highlight a critical need for development of chemical imaging platforms that allow in situ or in vivo analysis of molecules. Vibrational spectroscopy based on spontaneous Raman scattering is widely used for label-free analysis of chemical content in cells and tissues. However, the Raman process is a weak effect, limiting its application for fast chemical imaging of a living system. With high imaging speed and 3D spatial resolution, coherent Raman scattering microscopy is enabling a new approach for real-time vibrational imaging of single cells in a living system. In most experiments, coherent Raman processes involve two excitation fields denoted as pump at ωp and Stokes at ωs. When the beating frequency between the pump and Stokes fields (ωp – ωs) is resonant with a Raman-active molecular vibration, four major coherent Raman scattering processes occur simultaneously, namely, coherent anti-Stokes Raman scattering (CARS) at (ωp – ωs) + ωp, coherent Stokes Raman scattering (CSRS) at ωs – (ωp – ωs), stimulated Raman gain (SRG) at ωs, and stimulated Raman loss (SRL) at ωp. In SRG, the Stokes beam experiences a gain in intensity, whereas in SRL, the pump beam experiences a loss. Both SRG and SRL belong to

  14. Fast vibrational imaging of single cells and tissues by stimulated Raman scattering microscopy.

    PubMed

    Zhang, Delong; Wang, Ping; Slipchenko, Mikhail N; Cheng, Ji-Xin

    2014-08-19

    Traditionally, molecules are analyzed in a test tube. Taking biochemistry as an example, the majority of our knowledge about cellular content comes from analysis of fixed cells or tissue homogenates using tools such as immunoblotting and liquid chromatography-mass spectrometry. These tools can indicate the presence of molecules but do not provide information on their location or interaction with each other in real time, restricting our understanding of the functions of the molecule under study. For real-time imaging of labeled molecules in live cells, fluorescence microscopy is the tool of choice. Fluorescent labels, however, are too bulky for small molecules such as fatty acids, amino acids, and cholesterol. These challenges highlight a critical need for development of chemical imaging platforms that allow in situ or in vivo analysis of molecules. Vibrational spectroscopy based on spontaneous Raman scattering is widely used for label-free analysis of chemical content in cells and tissues. However, the Raman process is a weak effect, limiting its application for fast chemical imaging of a living system. With high imaging speed and 3D spatial resolution, coherent Raman scattering microscopy is enabling a new approach for real-time vibrational imaging of single cells in a living system. In most experiments, coherent Raman processes involve two excitation fields denoted as pump at ωp and Stokes at ωs. When the beating frequency between the pump and Stokes fields (ωp - ωs) is resonant with a Raman-active molecular vibration, four major coherent Raman scattering processes occur simultaneously, namely, coherent anti-Stokes Raman scattering (CARS) at (ωp - ωs) + ωp, coherent Stokes Raman scattering (CSRS) at ωs - (ωp - ωs), stimulated Raman gain (SRG) at ωs, and stimulated Raman loss (SRL) at ωp. In SRG, the Stokes beam experiences a gain in intensity, whereas in SRL, the pump beam experiences a loss. Both SRG and SRL belong to stimulated Raman scattering (SRS

  15. Spectrometer-free vibrational imaging by retrieving stimulated Raman signal from highly scattered photons

    PubMed Central

    Liao, Chien-Sheng; Wang, Pu; Wang, Ping; Li, Junjie; Lee, Hyeon Jeong; Eakins, Gregory; Cheng, Ji-Xin

    2015-01-01

    In vivo vibrational spectroscopic imaging is inhibited by relatively slow spectral acquisition on the second scale and low photon collection efficiency for a highly scattering system. Recently developed multiplex coherent anti-Stokes Raman scattering and stimulated Raman scattering techniques have improved the spectral acquisition time down to microsecond scale. These methods using a spectrometer setting are not suitable for turbid systems in which nearly all photons are scattered. We demonstrate vibrational imaging by spatial frequency multiplexing of incident photons and single photodiode detection of a stimulated Raman spectrum within 60 μs. Compared to the spectrometer setting, our method improved the photon collection efficiency by two orders of magnitude for highly scattering specimens. We demonstrated in vivo imaging of vitamin E distribution on mouse skin and in situ imaging of human breast cancerous tissues. The reported work opens new opportunities for spectroscopic imaging in a surgical room and for development of deep-tissue Raman spectroscopy toward molecular level diagnosis. PMID:26601311

  16. Chemical imaging with Fourier transform coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Cui, Meng; Skodack, Joshua; Ogilvie, Jennifer P

    2008-11-01

    We report chemical imaging using Fourier transform coherent anti-Stokes Raman scattering (FTCARS) microscopy. Adding a passively phase-stable local field to amplify the weak FTCARS signal, we also demonstrate interferometric FTCARS microscopy, permitting reduced incident power to be used for imaging. We discuss signal-to-noise considerations and the conditions necessary to effectively suppress background noise, allowing FTCARS microscopy that is limited by the shot noise of the detector. We also discuss differences between the signal-to-noise obtainable by time and frequency domain coherent anti-Stokes Raman scattering (CARS) methods. PMID:19122721

  17. Hyperspectral imaging with in-line interferometric femtosecond stimulated Raman scattering spectroscopy

    NASA Astrophysics Data System (ADS)

    Dobner, Sven; Fallnich, Carsten

    2014-02-01

    We present the hyperspectral imaging capabilities of in-line interferometric femtosecond stimulated Raman scattering. The beneficial features of this method, namely, the improved signal-to-background ratio compared to other applicable broadband stimulated Raman scattering methods and the simple experimental implementation, allow for a rather fast acquisition of three-dimensional raster-scanned hyperspectral data-sets, which is shown for PMMA beads and a lipid droplet in water as a demonstration. A subsequent application of a principle component analysis displays the chemical selectivity of the method.

  18. Hyperspectral imaging with in-line interferometric femtosecond stimulated Raman scattering spectroscopy.

    PubMed

    Dobner, Sven; Fallnich, Carsten

    2014-02-28

    We present the hyperspectral imaging capabilities of in-line interferometric femtosecond stimulated Raman scattering. The beneficial features of this method, namely, the improved signal-to-background ratio compared to other applicable broadband stimulated Raman scattering methods and the simple experimental implementation, allow for a rather fast acquisition of three-dimensional raster-scanned hyperspectral data-sets, which is shown for PMMA beads and a lipid droplet in water as a demonstration. A subsequent application of a principle component analysis displays the chemical selectivity of the method.

  19. Label-Free Cellular Imaging by Broadband Coherent Anti-Stokes Raman Scattering Microscopy

    PubMed Central

    Parekh, Sapun H.; Lee, Young Jong; Aamer, Khaled A.; Cicerone, Marcus T.

    2010-01-01

    Raman microspectroscopy can provide the chemical contrast needed to characterize the complex intracellular environment and macromolecular organization in cells without exogenous labels. It has shown a remarkable ability to detect chemical changes underlying cell differentiation and pathology-related chemical changes in tissues but has not been widely adopted for imaging, largely due to low signal levels. Broadband coherent anti-Stokes Raman scattering (B-CARS) offers the same inherent chemical contrast as spontaneous Raman but with increased acquisition rates. To date, however, only spectrally resolved signals from the strong CH-related vibrations have been used for CARS imaging. Here, we obtain Raman spectral images of single cells with a spectral range of 600–3200 cm−1, including signatures from weakly scattering modes as well as CH vibrations. We also show that B-CARS imaging can be used to measure spectral signatures of individual cells at least fivefold faster than spontaneous Raman microspectroscopy and can be used to generate maps of biochemical species in cells. This improved spectral range and signal intensity opens the door for more widespread use of vibrational spectroscopic imaging in biology and clinical diagnostics. PMID:20959111

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

    PubMed

    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

  1. 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

  2. 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

  3. Picosecond spectral coherent anti-Stokes Raman scattering imaging with principal component analysis of meibomian glands

    NASA Astrophysics Data System (ADS)

    Lin, Chia-Yu; Suhalim, Jeffrey L.; Nien, Chyong Ly; Miljković, Miloš D.; Diem, Max; Jester, James V.; Potma, Eric. O.

    2011-02-01

    The lipid distribution in the mouse meibomian gland was examined with picosecond spectral anti-Stokes Raman scattering (CARS) imaging. Spectral CARS data sets were generated by imaging specific localized regions of the gland within tissue sections at consecutive Raman shifts in the CH2 stretching vibrational range. Spectral differences between the location specific CARS spectra obtained in the lipid-rich regions of the acinus and the central duct were observed, which were confirmed with a Raman microspectroscopic analysis, and attributed to meibum lipid modifications within the gland. A principal component analysis of the spectral data set reveals changes in the CARS spectrum when transitioning from the acini to the central duct. These results demonstrate the utility of picosecond spectral CARS imaging combined with multivariate analysis for assessing differences in the distribution and composition of lipids in tissues.

  4. Label-Free Nanometer-Resolution Imaging of Biological Architectures through Surface Enhanced Raman Scattering

    PubMed Central

    Ayas, Sencer; Cinar, Goksu; Ozkan, Alper Devrim; Soran, Zeliha; Ekiz, Oner; Kocaay, Deniz; Tomak, Aysel; Toren, Pelin; Kaya, Yasin; Tunc, Ilknur; Zareie, Hadi; Tekinay, Turgay; Tekinay, Ayse Begum; Guler, Mustafa Ozgur; Dana, Aykutlu

    2013-01-01

    Label free imaging of the chemical environment of biological specimens would readily bridge the supramolecular and the cellular scales, if a chemical fingerprint technique such as Raman scattering can be coupled with super resolution imaging. We demonstrate the possibility of label-free super-resolution Raman imaging, by applying stochastic reconstruction to temporal fluctuations of the surface enhanced Raman scattering (SERS) signal which originate from biomolecular layers on large-area plasmonic surfaces with a high and uniform hot-spot density (>1011/cm2, 20 to 35 nm spacing). A resolution of 20 nm is demonstrated in reconstructed images of self-assembled peptide network and fibrilated lamellipodia of cardiomyocytes. Blink rate density is observed to be proportional to the excitation intensity and at high excitation densities (>10 kW/cm2) blinking is accompanied by molecular breakdown. However, at low powers, simultaneous Raman measurements show that SERS can provide sufficient blink rates required for image reconstruction without completely damaging the chemical structure. PMID:24022059

  5. Phase-shift effect of amplitude spread function on spectrum and image formation in coherent Raman scattering microspectroscopy.

    PubMed

    Fukutake, Naoki

    2016-03-01

    Coherent Raman scattering microspectroscopy, which includes coherent anti-Stokes Raman scattering (CARS) and stimulated Raman scattering (SRS) microspectroscopy, permits label-free hyperspectral imaging. We report the theoretical study of the phase-shift effect of the impulse response function on the spectral and image-forming properties of coherent Raman scattering microspectroscopy. We show that the spectrum and image are influenced by not only the NA of objective for excitation (NA(ex)) but also that for signal collection (NA(col)), in association with the phase-shift effect. We discuss that, under the condition NA(ex)≠NA(col), both the spectrum and the image become deformed by the phase-shift effect, which can be applied to the direct measurement of the imaginary part of the nonlinear susceptibility in CARS spectroscopy. We point out that, even in SRS microscopy, the nonresonant background can contribute to the image formation and cause the artifact in the image.

  6. Hyperspectral microscopic imaging by multiplex coherent anti-Stokes Raman scattering (CARS)

    NASA Astrophysics Data System (ADS)

    Khmaladze, Alexander; Jasensky, Joshua; Zhang, Chi; Han, Xiaofeng; Ding, Jun; Seeley, Emily; Liu, Xinran; Smith, Gary D.; Chen, Zhan

    2011-10-01

    Coherent anti-Stokes Raman scattering (CARS) microscopy is a powerful technique to image the chemical composition of complex samples in biophysics, biology and materials science. CARS is a four-wave mixing process. The application of a spectrally narrow pump beam and a spectrally wide Stokes beam excites multiple Raman transitions, which are probed by a probe beam. This generates a coherent directional CARS signal with several orders of magnitude higher intensity relative to spontaneous Raman scattering. Recent advances in the development of ultrafast lasers, as well as photonic crystal fibers (PCF), enable multiplex CARS. In this study, we employed two scanning imaging methods. In one, the detection is performed by a photo-multiplier tube (PMT) attached to the spectrometer. The acquisition of a series of images, while tuning the wavelengths between images, allows for subsequent reconstruction of spectra at each image point. The second method detects CARS spectrum in each point by a cooled coupled charged detector (CCD) camera. Coupled with point-by-point scanning, it allows for a hyperspectral microscopic imaging. We applied this CARS imaging system to study biological samples such as oocytes.

  7. Giant Raman scattering from J-aggregated dyes inside carbon nanotubes for multispectral imaging

    NASA Astrophysics Data System (ADS)

    Gaufrès, E.; Tang, N. Y.-Wa; Lapointe, F.; Cabana, J.; Nadon, M.-A.; Cottenye, N.; Raymond, F.; Szkopek, T.; Martel, R.

    2014-01-01

    Raman spectroscopy uses visible light to acquire vibrational fingerprints of molecules, thus making it a powerful tool for chemical analysis in a wide range of media. However, its potential for optical imaging at high resolution is severely limited by the fact that the Raman effect is weak. Here, we report the discovery of a giant Raman scattering effect from encapsulated and aggregated dye molecules inside single-walled carbon nanotubes. Measurements performed on rod-like dyes such as α-sexithiophene and β-carotene, assembled inside single-walled carbon nanotubes as highly polarizable J-aggregates, indicate a resonant Raman cross-section of (3 +/- 2) × 10-21 cm2 sr-1, which is well above the cross-section required for detecting individual aggregates at the highest optical resolution. Free from fluorescence background and photobleaching, this giant Raman effect allows the realization of a library of functionalized nanoprobe labels for Raman imaging with robust detection using multispectral analysis.

  8. Label-free DNA imaging in vivo with stimulated Raman scattering microscopy.

    PubMed

    Lu, Fa-Ke; Basu, Srinjan; Igras, Vivien; Hoang, Mai P; Ji, Minbiao; Fu, Dan; Holtom, Gary R; Neel, Victor A; Freudiger, Christian W; Fisher, David E; Xie, X Sunney

    2015-09-15

    Label-free DNA imaging is highly desirable in biology and medicine to perform live imaging without affecting cell function and to obtain instant histological tissue examination during surgical procedures. Here we show a label-free DNA imaging method with stimulated Raman scattering (SRS) microscopy for visualization of the cell nuclei in live animals and intact fresh human tissues with subcellular resolution. Relying on the distinct Raman spectral features of the carbon-hydrogen bonds in DNA, the distribution of DNA is retrieved from the strong background of proteins and lipids by linear decomposition of SRS images at three optimally selected Raman shifts. Based on changes on DNA condensation in the nucleus, we were able to capture chromosome dynamics during cell division both in vitro and in vivo. We tracked mouse skin cell proliferation, induced by drug treatment, through in vivo counting of the mitotic rate. Furthermore, we demonstrated a label-free histology method for human skin cancer diagnosis that provides comparable results to other conventional tissue staining methods such as H&E. Our approach exhibits higher sensitivity than SRS imaging of DNA in the fingerprint spectral region. Compared with spontaneous Raman imaging of DNA, our approach is three orders of magnitude faster, allowing both chromatin dynamic studies and label-free optical histology in real time.

  9. Label-free DNA imaging in vivo with stimulated Raman scattering microscopy

    PubMed Central

    Lu, Fa-Ke; Basu, Srinjan; Igras, Vivien; Hoang, Mai P.; Ji, Minbiao; Fu, Dan; Holtom, Gary R.; Neel, Victor A.; Freudiger, Christian W.; Fisher, David E.; Xie, X. Sunney

    2015-01-01

    Label-free DNA imaging is highly desirable in biology and medicine to perform live imaging without affecting cell function and to obtain instant histological tissue examination during surgical procedures. Here we show a label-free DNA imaging method with stimulated Raman scattering (SRS) microscopy for visualization of the cell nuclei in live animals and intact fresh human tissues with subcellular resolution. Relying on the distinct Raman spectral features of the carbon-hydrogen bonds in DNA, the distribution of DNA is retrieved from the strong background of proteins and lipids by linear decomposition of SRS images at three optimally selected Raman shifts. Based on changes on DNA condensation in the nucleus, we were able to capture chromosome dynamics during cell division both in vitro and in vivo. We tracked mouse skin cell proliferation, induced by drug treatment, through in vivo counting of the mitotic rate. Furthermore, we demonstrated a label-free histology method for human skin cancer diagnosis that provides comparable results to other conventional tissue staining methods such as H&E. Our approach exhibits higher sensitivity than SRS imaging of DNA in the fingerprint spectral region. Compared with spontaneous Raman imaging of DNA, our approach is three orders of magnitude faster, allowing both chromatin dynamic studies and label-free optical histology in real time. PMID:26324899

  10. Holographic coherent anti-Stokes Raman scattering bio-imaging

    PubMed Central

    Shi, Kebin; Edwards, Perry S.; Hu, Jing; Xu, Qian; Wang, Yanming; Psaltis, Demetri; Liu, Zhiwen

    2012-01-01

    CARS holography captures both the amplitude and the phase of a complex anti-Stokes field, and can perform three-dimensional imaging by digitally focusing onto different depths inside a specimen. The application of CARS holography for bio-imaging is demonstrated. It is shown that holographic CARS imaging of sub-cellular components in live HeLa cells can be achieved. PMID:22808443

  11. 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.

  12. Video-rate molecular imaging in vivo with stimulated Raman scattering.

    PubMed

    Saar, Brian G; Freudiger, Christian W; Reichman, Jay; Stanley, C Michael; Holtom, Gary R; Xie, X Sunney

    2010-12-01

    Optical imaging in vivo with molecular specificity is important in biomedicine because of its high spatial resolution and sensitivity compared with magnetic resonance imaging. Stimulated Raman scattering (SRS) microscopy allows highly sensitive optical imaging based on vibrational spectroscopy without adding toxic or perturbative labels. However, SRS imaging in living animals and humans has not been feasible because light cannot be collected through thick tissues, and motion-blur arises from slow imaging based on backscattered light. In this work, we enable in vivo SRS imaging by substantially enhancing the collection of the backscattered signal and increasing the imaging speed by three orders of magnitude to video rate. This approach allows label-free in vivo imaging of water, lipid, and protein in skin and mapping of penetration pathways of topically applied drugs in mice and humans.

  13. Spatial correlation of confocal Raman scattering and secondary ion mass spectrometric molecular images of lignocellulosic materials.

    PubMed

    Li, Zhen; Chu, Li-Qiang; Sweedler, Jonathan V; Bohn, Paul W

    2010-04-01

    A detailed chemical and structural understanding of pre-enzymatic processing of lignocellulosic materials (LCMs) is a key objective in the development of renewable energy. Efficient rendering of biomass components into fermentable substrates for conversion into biofuel feedstocks would benefit greatly from the development of new technologies to provide high-quality, spatially resolved chemical information about LCMs during the various processing states. In an effort to realize this important goal, spatially correlated confocal Raman and mass spectrometric images allow the extraction of three-dimensional information from the perennial grass, Miscanthus x giganteus. An optical microscopy-based landmark registry scheme was developed that allows samples to be transferred between laboratories at different institutions, while retaining the capability to access the same physical regions of the samples. Subsequent to higher resolution imaging via confocal Raman microscopy and secondary ion mass spectrometry (SIMS), laser desorption-ionization mass spectrometry was used to place these regions within the overall sample architecture. Excellent sample registry was evident in the highly correlated Raman and SIMS images. In addition, the correlation of vibrational Raman scattering with mass spectra from specific spatial locations allowed confirmation of the assignment of intracellular globular structures to hemicellulose-rich lignin complexes, an assignment which could only be made tentatively from either image alone. PMID:20205411

  14. Multicolor stimulated Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Lu, Fa-Ke; Ji, Minbiao; Fu, Dan; Ni, Xiaohui; Freudiger, Christian W.; Holtom, Gary; Xie, X. Sunney

    2012-08-01

    Stimulated Raman scattering (SRS) microscopy has opened up a wide range of biochemical imaging applications by probing a particular Raman-active molecule vibrational mode in the specimen. However, the original implementation with picosecond pulse excitation can only realize rapid chemical mapping with a single Raman band. Here we present a novel SRS microscopic technique using a grating-based pulse shaper for excitation and a grating-based spectrograph for detection to achieve simultaneous multicolor SRS imaging with high sensitivity and high acquisition speeds. In particular, we use a linear combination of the measured CH2 and CH3 stretching signals to map the distributions of protein and lipid contents simultaneously.

  15. Lock-in-detection-free line-scan stimulated Raman scattering microscopy for near video-rate Raman imaging.

    PubMed

    Wang, Zi; Zheng, Wei; Huang, Zhiwei

    2016-09-01

    We report on the development of a unique lock-in-detection-free line-scan stimulated Raman scattering microscopy technique based on a linear detector with a large full well capacity controlled by a field-programmable gate array (FPGA) for near video-rate Raman imaging. With the use of parallel excitation and detection scheme, the line-scan SRS imaging at 20 frames per second can be acquired with a ∼5-fold lower excitation power density, compared to conventional point-scan SRS imaging. The rapid data communication between the FPGA and the linear detector allows a high line-scanning rate to boost the SRS imaging speed without the need for lock-in detection. We demonstrate this lock-in-detection-free line-scan SRS imaging technique using the 0.5 μm polystyrene and 1.0 μm poly(methyl methacrylate) beads mixed in water, as well as living gastric cancer cells.

  16. Lock-in-detection-free line-scan stimulated Raman scattering microscopy for near video-rate Raman imaging.

    PubMed

    Wang, Zi; Zheng, Wei; Huang, Zhiwei

    2016-09-01

    We report on the development of a unique lock-in-detection-free line-scan stimulated Raman scattering microscopy technique based on a linear detector with a large full well capacity controlled by a field-programmable gate array (FPGA) for near video-rate Raman imaging. With the use of parallel excitation and detection scheme, the line-scan SRS imaging at 20 frames per second can be acquired with a ∼5-fold lower excitation power density, compared to conventional point-scan SRS imaging. The rapid data communication between the FPGA and the linear detector allows a high line-scanning rate to boost the SRS imaging speed without the need for lock-in detection. We demonstrate this lock-in-detection-free line-scan SRS imaging technique using the 0.5 μm polystyrene and 1.0 μm poly(methyl methacrylate) beads mixed in water, as well as living gastric cancer cells. PMID:27607947

  17. Imaging with Raman spectroscopy.

    PubMed

    Zhang, Yin; Hong, Hao; Cai, Weibo

    2010-09-01

    Raman spectroscopy, based on the inelastic scattering of a photon, has been widely used as an analytical tool in many research fields. Recently, Raman spectroscopy has also been explored for biomedical applications (e.g. cancer diagnosis) because it can provide detailed information on the chemical composition of cells and tissues. For imaging applications, several variations of Raman spectroscopy have been developed to enhance its sensitivity. This review article will provide a brief summary of Raman spectroscopy-based imaging, which includes the use of coherent anti-Stokes Raman spectroscopy (CARS, primarily used for imaging the C-H bond in lipids), surface-enhanced Raman spectroscopy (SERS, for which a variety of nanoparticles can be used as contrast agents), and single-walled carbon nanotubes (SWNTs, with its intrinsic Raman signal). The superb multiplexing capability of SERS-based Raman imaging can be extremely powerful in future research where different agents can be attached to different Raman tags to enable the interrogation of multiple biological events simultaneously in living subjects. The primary limitations of Raman imaging in humans are those also faced by other optical techniques, in particular limited tissue penetration. Over the last several years, Raman spectroscopy imaging has advanced significantly and many critical proof-of-principle experiments have been successfully carried out. It is expected that imaging with Raman Spectroscopy will continue to be a dynamic research field over the next decade.

  18. Advantages and Artifacts of Higher Order Modes in Nanoparticle Enhanced Back-Scattering Raman Imaging

    PubMed Central

    Schultz, Zachary D.; Stranick, Stephan J.

    2009-01-01

    In order to facilitate nanoparticle enhanced Raman imaging of complicated biological specimens, we have examined the use of higher order modes with radial and azimuthal polarizations focused onto a Au nanoparticle AFM tip utilizing a back-scattering reflection configuration. When comparing the Raman intensity profiles with the observed sample topography, the radial polarized configuration demonstrates enhanced spatial resolution. This enhanced resolution results from the direction of the induced electron oscillation in the metal nanoparticle oriented by the electromagnetic field at the laser focus. The electric field component along the direction of laser propagation, attendant to the radial polarization, creates an enhanced field along the z-axis and normal to the sample. Substantial enhancement is observed utilizing an intermediate numerical aperture objective (NA = 0.7), necessary for back-scattering measurements. The azimuthal polarization, similar to linear polarization, results in an enhanced field predominantly parallel to the sample, resulting in imaging artifacts. The Raman intensity profiles observed as the exciting laser polarization is switched between either a radially polarized or an azimuthally polarized state illustrate these imaging artifacts. Because azimuthal polarization arises readily from changes in the incident polarization onto the mode converter, the results presented here aid in identifying such artifacts when analyzing nanoparticle enhanced Raman spectroscopic images. Due to the power law decay of the enhanced field, an enhancement orientation normal to the sample enables contrast between structures smaller than the tip dimensions as the apex of the nanoparticle tip, where the enhancement is strongest, passes over the sample. These effects are demonstrated using both carbon nanotube and fixed biological samples. PMID:19947663

  19. Coherent Raman scattering microscopy for label-free imaging of live amphioxus

    NASA Astrophysics Data System (ADS)

    Yu, Zhilong; Chen, Tao; Zhang, Xiannian; Shen, Jie; Chen, Junyuan; Huang, Yanyi

    2012-03-01

    The existence of notochord distinguishes chordates from other phyla. Amphioxus is the only animal that keeps notochord during the whole life. Notochord is a unique organ for amphioxus, with its vertically arranged muscular notochordal plates, which is different from notochords in embryos of other chordates. We use stimulated Raman scattering (SRS) microscopy as a non-invasive technique to image the chemical components in amphioxus notochord. SRS provides chemical specificity as spontaneous Raman does and offers a higher sensitivity for fast acquisition. Unlike coherent anti- Stokes Raman scattering (CARS) microscopy, SRS microscopy doesn't have non-resonant background and can better differentiate different components in the specimen. We verify that the notochord is a protein-rich organ, which agrees well with the result of conventional staining methods. Detailed structures in notochordal plates and notochordal sheath are revealed by SRS microscopy with diffraction limited resolution. Our experiment shows that SRS microscopy is an excellent imaging tool for biochemical research with its intrinsic chemical selectivity, high spatiotemporal resolution and native 3D optical sectioning ability.

  20. Raman microspectrometer combined with scattering microscopy and lensless imaging for bacteria identification

    NASA Astrophysics Data System (ADS)

    Strola, S. A.; Schultz, E.; Allier, C. P.; DesRoches, B.; Lemmonier, J.; Dinten, J.-M.

    2013-03-01

    In this paper, we report on a compact prototype capable both of lensfree imaging, Raman spectrometry and scattering microscopy from bacteria samples. This instrument allows high-throughput real-time characterization without the need of markers, making it potentially suitable to field label-free biomedical and environmental applications. Samples are illuminated from above with a focused-collimated 532nm laser beam and can be x-y-z scanned. The bacteria detection is based on emerging lensfree imaging technology able to localize cells of interest over a large field-of-view of 24mm2. Raman signal and scattered light are then collected by separate measurement arms simultaneously. In the first arm the emission light is fed by a fiber into a prototype spectrometer, developed by Tornado Spectral System based on Tornado's High Throughput Virtual Slit (HTVS) novel technology. The enhanced light throughput in the spectral region of interest (500-1800 cm-1) reduces Raman acquisition time down to few seconds, thus facilitating experimental protocols and avoiding the bacteria deterioration induced by laser thermal heating. Scattered light impinging in the second arm is collected onto a charge-coupled-device. The reconstructed image allows studying the single bacteria diffraction pattern and their specific structural features. The characterization and identification of different bacteria have been performed to validate and optimize the acquisition system and the component setup. The results obtained demonstrate the benefits of these three techniques combination by providing the precise bacteria localization, their chemical composition and a morphology description. The procedure for a rapid identification of particular pathogen bacteria in a sample is illustrated.

  1. Surface-Enhanced Raman Scattering Nanoparticles as Optical Labels for Imaging Cell Surface Proteins

    NASA Astrophysics Data System (ADS)

    MacLaughlin, Christina M.

    Assaying the expression of cell surface proteins has widespread application for characterizing cell type, developmental stage, and monitoring disease transformation. Immunophenotyping is conducted by treating cells with labelled targeting moieties that have high affinity for relevant surface protein(s). The sensitivity and specificity of immunophenotyping is defined by the choice of contrast agent and therefore, the number of resolvable signals that can be used to simultaneously label cells. Narrow band width surface-enhanced Raman scattering (SERS) nanoparticles are proposed as optical labels for multiplexed immunophenotying. Two types of surface coatings were investigated to passivate the gold nanoparticles, incorporate SERS functionality, and to facilitate attachment of targeting antibodies. Thiolated poly(ethylene glycol) forms dative bonds with the gold surface and is compatible with multiple physisorbed Raman-active reporter molecules. Ternary lipid bilayers are used to encapsulate the gold nanoparticles particles, and incorporate three different classes of Raman reporters. TEM, UV-Visible absorbance spectroscopy, DLS, and electrophoretic light scattering were used characterize the particle coating. Colourimetric protein assay, and secondary antibody labelling were used to quantify the antibody conjugation. Three different in vitromodels were used to investigate the binding efficacy and specificity of SERS labels for their biomarker targets. Primary human CLL cells, LY10 B lymphoma, and A549 adenocarcinoma lines were targeted. Dark field imaging was used to visualize the colocalization of SERS labels with cells, and evidence of receptor clustering was obtained based on colour shifts of the particles' Rayleigh scattering. Widefield, and spatially-resolved Raman spectra were used to detect labels singly, and in combination from labelled cells. Fluorescence flow cytometry was used to test the particles' binding specificity, and SERS from labelled cells was also

  2. Raman scattering enhanced by plasmonic clusters and its application to single-molecule imaging

    SciTech Connect

    Yasuike, Tomokazu; Nobusada, Katsuyuki

    2015-12-31

    The optical response of the linear Au{sub 8} cluster is investigated by the linear response theory based on the density functional theory. It is revealed that the observed many peaks in the visible region originate from the interaction of the ideal plasmonic excitation along the molecular axis with the background d-electron excitations, i.e., the Landau damping. In spite of the existence of the damping, the Raman scattering is shown to be enhanced remarkably by the incident light resonant to the visible excitations. The novel imaging experiment with the atomic resolution is proposed by utilizing a plasmonic cluster as the probing tip.

  3. Microsecond Scale Vibrational Spectroscopic Imaging by Multiplex Stimulated Raman Scattering Microscopy

    PubMed Central

    Liao, Chien-Sheng; Slipchenko, Mikhail N.; Wang, Ping; Li, Junjie; Lee, Seung-Young; Oglesbee, Robert A.; Cheng, Ji-Xin

    2015-01-01

    Real-time vibrational spectroscopic imaging is desired for monitoring cellular states and cellular processes in a label-free manner. Raman spectroscopic imaging of highly dynamic systems is inhibited by relatively slow spectral acquisition on millisecond to second scale. Here, we report microsecond scale vibrational spectroscopic imaging by lock-in free parallel detection of spectrally dispersed stimulated Raman scattering signal. Using a homebuilt tuned amplifier array, our method enables Raman spectral acquisition, within the window defined by the broadband pulse, at the speed of 32 microseconds and with close to shot-noise limited detection sensitivity. Incorporated with multivariate curve resolution analysis, our platform allows compositional mapping of lipid droplets in single live cells, observation of intracellular retinoid metabolism, discrimination of fat droplets from protein-rich organelles in Caenorhabditis elegans, spectral detection of fast flowing tumor cells, and monitoring drug diffusion through skin tissue in vivo. The reported technique opens new opportunities for compositional analysis of cellular compartment in a microscope setting and high-throughput spectral profiling of single cells in a flow cytometer setting. PMID:26167336

  4. Raman Imaging

    NASA Astrophysics Data System (ADS)

    Stewart, Shona; Priore, Ryan J.; Nelson, Matthew P.; Treado, Patrick J.

    2012-07-01

    The past decade has seen an enormous increase in the number and breadth of imaging techniques developed for analysis in many industries, including pharmaceuticals, food, and especially biomedicine. Rather than accept single-dimensional forms of information, users now demand multidimensional assessment of samples. High specificity and the need for little or no sample preparation make Raman imaging a highly attractive analytical technique and provide motivation for continuing advances in its supporting technology and utilization. This review discusses the current tools employed in Raman imaging, the recent advances, and the major applications in this ever-growing analytical field.

  5. Raman scattering in crystals

    SciTech Connect

    Edwards, D.F.

    1988-09-30

    A tutorial presentation is given of Raman scattering in crystals. The physical concepts are emphasized rather than the detailed mathematical formalism. Starting with an introduction to the concepts of phonons and conservation laws, the effects of photon-phonon interactions are presented. This interaction concept is shown for a simple cubic crystal and is extended to a uniaxial crystal. The correlation table method is used for determining the number and symmetry of the Raman active modes. Finally, examples are given to illustrate the relative ease of using this group theoretical method and the predictions are compared with measured Raman spectra. 37 refs., 17 figs., 6 tabs.

  6. Live-Cell Bioorthogonal Chemical Imaging: Stimulated Raman Scattering Microscopy of Vibrational Probes.

    PubMed

    Wei, Lu; Hu, Fanghao; Chen, Zhixing; Shen, Yihui; Zhang, Luyuan; Min, Wei

    2016-08-16

    Innovations in light microscopy have tremendously revolutionized the way researchers study biological systems with subcellular resolution. In particular, fluorescence microscopy with the expanding choices of fluorescent probes has provided a comprehensive toolkit to tag and visualize various molecules of interest with exquisite specificity and high sensitivity. Although fluorescence microscopy is currently the method of choice for cellular imaging, it faces fundamental limitations for studying the vast number of small biomolecules. This is because common fluorescent labels, which are relatively bulky, could introduce considerable perturbation to or even completely alter the native functions of vital small biomolecules. Hence, despite their immense functional importance, these small biomolecules remain largely undetectable by fluorescence microscopy. To address this challenge, a bioorthogonal chemical imaging platform has recently been introduced. By coupling stimulated Raman scattering (SRS) microscopy, an emerging nonlinear Raman microscopy technique, with tiny and Raman-active vibrational probes (e.g., alkynes and stable isotopes), bioorthogonal chemical imaging exhibits superb sensitivity, specificity, and biocompatibility for imaging small biomolecules in live systems. In this Account, we review recent technical achievements for visualizing a broad spectrum of small biomolecules, including ribonucleosides and deoxyribonucleosides, amino acids, fatty acids, choline, glucose, cholesterol, and small-molecule drugs in live biological systems ranging from individual cells to animal tissues and model organisms. Importantly, this platform is compatible with live-cell biology, thus allowing real-time imaging of small-molecule dynamics. Moreover, we discuss further chemical and spectroscopic strategies for multicolor bioorthogonal chemical imaging, a valuable technique in the era of "omics". As a unique tool for biological discovery, this platform has been applied to

  7. Simultaneous stimulated Raman scattering and higher harmonic generation imaging for liver disease diagnosis without labeling

    NASA Astrophysics Data System (ADS)

    Lin, Jian; Wang, Zi; Zheng, Wei; Huang, Zhiwei

    2014-02-01

    Nonlinear optical microscopy (e.g., higher harmonic (second-/third- harmonic) generation (HHG), simulated Raman scattering (SRS)) has high diagnostic sensitivity and chemical specificity, making it a promising tool for label-free tissue and cell imaging. In this work, we report a development of a simultaneous SRS and HHG imaging technique for characterization of liver disease in a bile-duct-ligation rat-modal. HHG visualizes collagens formation and reveals the cell morphologic changes associated with liver fibrosis; whereas SRS identifies the distributions of hepatic fat cells formed in steatosis liver tissue. This work shows that the co-registration of SRS and HHG images can be an effective means for label-free diagnosis and characterization of liver steatosis/fibrosis at the cellular and molecular levels.

  8. Coherent anti-stokes Raman scattering microscopy for high speed non- staining biomolecular imaging.

    PubMed

    Hashimoto, Mamoru; Minamikawa, Takeo; Araki, Tsutomu

    2013-01-01

    Vibrational microscopy (Raman microscopy and infrared microscopy), which observes molecular vibrations, gives us the information of molecular species without staining because the observed signals are originated from intrinsic molecules of a cell. However, infrared radiation is absorbed with water, and the long wavelength (3-10 μm) limits the spatial resolution to several micrometers. Spontaneous emission of Raman scattering is quite feeble, and the Raman scattering often overlaps with one-photon fluorescence from a specimen. Coherent anti-Stokes Raman scattering (CARS) microscopy, which is one of the nonlinear Raman microscopy, is a method to overcome those problems. In this review, present system of CARS microscopy, the methods of background rejection, and applications are introduced.

  9. Stimulated Raman scattering detection for chemically specific time-resolved imaging of gases.

    PubMed

    Amer, Eynas; Gren, Per; Edenharder, Stefan; Sjödahl, Mikael

    2016-05-01

    A stimulated Raman scattering (SRS) imaging technique based on spatial modulation of the pump beam has been used to study gases. The SRS gain signal was separated from the Stokes beam background in the spatial frequency domain. The SRS signal shows linear behaviour with the gas pressure at a range from 1.0 to 8.0 bars. The signal is linearly proportional to the pump beam intensity while it is enhanced with increasing the Stokes beam intensity to a certain limit than it saturates. Further, the chemical specificity of the technique has been investigated. Two sharp peaks with line width at half maximum of about 0.30 nm have been obtained at Stokes beam wavelengths of 629.93 nm and 634.05 nm corresponding to the methane and ethylene gases, respectively. The results show that SRS imaging is a promising technique to provide chemical specificity as well as spatial and temporal information of gaseous species. PMID:27137608

  10. Imaging the Intact Mouse Cornea Using Coherent Anti-Stokes Raman scattering (CARS)

    PubMed Central

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

    2013-01-01

    Purpose. The aim of this study was to image the cellular and noncellular structures of the cornea and limbus in an intact mouse eye using the vibrational oscillation of the carbon–hydrogen bond in lipid membranes and autofluorescence as label-free contrast agents. Methods. Freshly enucleated mouse eyes were imaged using two nonlinear optical techniques: coherent anti-Stokes Raman scattering (CARS) and two-photon autofluorescence (TPAF). Sequential images were collected through the full thickness of the cornea and limbal regions. Line scans along the transverse/sagittal axes were also performed. Results. Analysis of multiple CARS/TPAF images revealed that corneal epithelial and endothelial cells could be identified by the lipid-rich plasma membrane CARS signal. The fluorescent signal from the collagen fibers of the corneal stroma was evident in the TPAF channel. The transition from the cornea to sclera at the limbus was marked by a change in collagen pattern (TPAF channel) and thickness of surface cells (CARS channel). Regions within the corneal stroma that lack collagen autofluorescence coincided with CARS signal, indicating the presence of stromal fibroblasts or nerve fibers. Conclusions. The CARS technique was successful in imaging cells in the intact mouse eye, both at the surface and within corneal tissue. Multiphoton images were comparable to histologic sections. The methods described here represent a new avenue for molecular specific imaging of the mouse eye. The lack of need for tissue fixation is unique compared with traditional histology imaging techniques. PMID:23821187

  11. Label-free chemically specific imaging in planta with stimulated Raman scattering microscopy.

    PubMed

    Mansfield, Jessica C; Littlejohn, George R; Seymour, Mark P; Lind, Rob J; Perfect, Sarah; Moger, Julian

    2013-05-21

    The growing world population puts ever-increasing demands on the agricultural and agrochemical industries to increase agricultural yields. This can only be achieved by investing in fundamental plant and agrochemical research and in the development of improved analytical tools to support research in these areas. There is currently a lack of analytical tools that provide noninvasive structural and chemical analysis of plant tissues at the cellular scale. Imaging techniques such as coherent anti-Stokes Raman scattering (CARS) and stimulated Raman scattering (SRS) microscopy provide label-free chemically specific image contrast based on vibrational spectroscopy. Over the past decade, these techniques have been shown to offer clear advantages for a vast range of biomedical research applications. The intrinsic vibrational contrast provides label-free quantitative functional analysis, it does not suffer from photobleaching, and it allows near real-time imaging in 3D with submicrometer spatial resolution. However, due to the susceptibility of current detection schemes to optical absorption and fluorescence from pigments (such as chlorophyll), the plant science and agrochemical research communities have not been able to benefit from these techniques and their application in plant research has remained virtually unexplored. In this paper, we explore the effect of chlorophyll fluorescence and absorption in CARS and SRS microscopy. We show that with the latter it is possible to use phase-sensitive detection to separate the vibrational signal from the (electronic) absorption processes. Finally, we demonstrate the potential of SRS for a range of in planta applications by presenting in situ chemical analysis of plant cell wall components, epicuticular waxes, and the deposition of agrochemical formulations onto the leaf surface.

  12. 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.

  13. Simultaneous Surface-Enhanced Raman Scattering Imaging and Spectroscopy in Confocal Mode.

    NASA Astrophysics Data System (ADS)

    Pristinski, Denis; Erol, Melek; Du, Henry; Sukhishvili, Svetlana

    2007-03-01

    Noble colloidal metal nanoparticles deposited on a planar substrate facilitate ultrasensitive measurements via surface-enhanced Raman scattering (SERS) spectroscopy. Due to the random nature of nanoparticle immobilization, the variation of interparticle distance and possible aggregate formation cause significant fluctuation in SERS signal intensity across the substrate. To study the nature of these intensity fluctuations we have built a microscope capable of simultaneous imaging in epi-fluorescent mode and spectroscopy of a point of interest in confocal mode. Two excitation beams from the same laser (DPSS 532 nm) are mixed to expose the imaged area and to focus on the point of interest through high N.A. objective. The scattered light collected by the same objective is filtered and split between a cooled CCD camera for imaging and a fiber-connected spectrometer for confocal mode spectroscopy. Positively charged Ag nanoparticles prepared by polyethyleneimine-assisted reduction were deposited on glass substrate and used for the assessment of uniformity of SERS signal from subsequently adsorbed anionic molecules and for the identification of proteins. ^1 Department of Chemical, BioMedical, and Materials Engineering ^2 Department of Chemistry and Chemical Biology

  14. Alkyne-Modulated Surface-Enhanced Raman Scattering-Palette for Optical Interference-Free and Multiplex Cellular Imaging.

    PubMed

    Chen, Yong; Ren, Jia-Qiang; Zhang, Xia-Guang; Wu, De-Yin; Shen, Ai-Guo; Hu, Ji-Ming

    2016-06-21

    The alkyne tags possess unique interference-free Raman emissions but are still hindered for further application in the field of biochemical labels due to its extremely weak spontaneous Raman scattering. With the aid of computational chemistry, herein, an alkyne-modulated surface-enhanced Raman scattering (SERS) palette is constructed based on rationally designed 4-ethynylbenzenethiol derivatives for spectroscopic signature, Au@Ag core for optical enhancement and an encapsulating polyallylamine shell for protection and conjugation. Even for the pigment rich plant cell (e.g., pollen), the alkyne-coded SERS tag can be highly discerned on two-dimension distribution impervious to strong organic interferences originating from resonance-enhanced Raman scattering or autofluorescence. In addition, the alkynyl-containing Raman reporters contribute especially narrow emission, band shift-tunable (2100-2300 cm(-1)) and tremendously enhanced Raman signals when the alkynyl group locates at para position of mercaptobenzene ring. Depending on only single Raman band, the suggested alkyne-modulated SERS-palette potentially provides a more effective solution for multiplex cellular imaging with vibrant colors, when the hyperspectral and fairly intense optical noises originating from lower wavenumber region (<1800 cm(-1)) are inevitable under complex ambient conditions. PMID:27223333

  15. 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

  16. Hyperspectral stimulated Raman scattering and multiphoton imaging for digital pathology of colonic disease

    NASA Astrophysics Data System (ADS)

    Wang, Zi; Zheng, Wei; Lin, Jian; Huang, Zhiwei

    2016-03-01

    Histopathology examinations of H&E stained biopsied tissues is the golden standard for colonic diseases (e.g., polyps, adenoma, and adenocarcinoma) diagnosis. However, staining effect of sample and doctor's expertise degree may greatly influence the diagnosis results. The information provided by the H&E stained sample is also limited to the morphological and PH information and no quantative information is available. In this paper, we report the development of a unique multimodal nonlinear optical microscopy (i.e., hyperspectral stimulated Raman scattering (hsSRS), second-harmonic generation (SHG), third-harmonic generation (THG), two-photon excitation fluorescence (TPEF)) platform for the diagnosis and characterization of colonic diseases. HsSRS in both fingerprint (800-1800 cm-1) and high-wavenumber (2800-3600 cm-1) regions allows us to discriminate different constituents with tiny difference in the Raman spectra. The increase of proteins and reduction of lipids could be observed with the progress of colonic cancer. SHG shows the distribution of collagen, which is found to aggregate for adenocarcinoma. TPEF provides the cell morphological and can reflect the damage inside glands caused by the diseases. THG shows the increase of optical heterogeneity related to cancer process. This work shows that the integrated hsSRS and TPEF/SHG/THG imaging technique can be an effective method for digital pathology of colonic diseases at the molecular and sub-cellular levels.

  17. Three-dimensional chemical imaging of skin using stimulated Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Drutis, Dane M.; Hancewicz, Thomas M.; Pashkovski, Eugene; Feng, Lin; Mihalov, Dawn; Holtom, Gary; Ananthapadmanabhan, Kavssery P.; Xie, X. Sunney; Misra, Manoj

    2014-11-01

    Stimulated Raman scattering (SRS) microscopy is used to generate structural and chemical three-dimensional images of native skin. We employed SRS microscopy to investigate the microanatomical features of skin and penetration of topically applied materials. Image depth stacks are collected at distinct wavelengths corresponding to vibrational modes of proteins, lipids, and water in the skin. We observed that corneocytes in stratum corneum are grouped together in clusters, 100 to 250 μm in diameter, separated by 10- to 25-μm-wide microanatomical skin-folds called canyons. These canyons occasionally extend down to depths comparable to that of the dermal-epidermal junction below the flat surface regions in porcine and human skin. SRS imaging shows the distribution of chemical species within cell clusters and canyons. Water is predominately located within the cell clusters, and its concentration rapidly increases at the transition from stratum corneum to viable epidermis. Canyons do not contain detectable levels of water and are rich in lipid material. Oleic acid-d34 applied to the skin surface lines the canyons down to a depth of 50 μm below the surface of the skin. This observation could have implications on the evaluation of penetration profiles of bioactive materials measured using traditional methods, such as tape-stripping.

  18. Three-dimensional chemical imaging of skin using stimulated Raman scattering microscopy.

    PubMed

    Drutis, Dane M; Hancewicz, Thomas M; Pashkovski, Eugene; Feng, Lin; Mihalov, Dawn; Holtom, Gary; Ananthapadmanabhan, Kavssery P; Xie, X Sunney; Misra, Manoj

    2014-01-01

    Stimulated Raman scattering (SRS) microscopy is used to generate structural and chemical three-dimensional images of native skin. We employed SRS microscopy to investigate the microanatomical features of skin and penetration of topically applied materials. Image depth stacks are collected at distinct wavelengths corresponding to vibrational modes of proteins, lipids, and water in the skin. We observed that corneocytes in stratum corneum are grouped together in clusters, 100 to 250 μm in diameter, separated by 10- to 25-μm-wide microanatomical skin-folds called canyons. These canyons occasionally extend down to depths comparable to that of the dermal-epidermal junction below the flat surface regions in porcine and human skin. SRS imaging shows the distribution of chemical species within cell clusters and canyons. Water is predominately located within the cell clusters, and its concentration rapidly increases at the transition from stratum corneum to viable epidermis. Canyons do not contain detectable levels of water and are rich in lipid material. Oleic acid-d34 applied to the skin surface lines the canyons down to a depth of 50 μm below the surface of the skin. This observation could have implications on the evaluation of penetration profiles of bioactive materials measured using traditional methods, such as tape-stripping.

  19. Vibrational Imaging with High Sensitivity via Epidetected Coherent Anti-Stokes Raman Scattering Microscopy

    SciTech Connect

    Volkmer, Andreas; Cheng, Ji-Xin; Sunney Xie, X.

    2001-07-09

    We demonstrate theoretically and experimentally a novel epidetection scheme for coherent anti-Stokes Raman scattering (CARS) microscopy that significantly improves the detection sensitivity. Calculations show that epidetected CARS (E-CARS) signals are present for scatterers smaller than the wavelength of light, whereas the large background signals from the surrounding bulk solvent are suppressed by destructive interference. E-CARS microscopy is capable of revealing small intracellular features that are otherwise buried by the strong water CARS signal.

  20. Quantitative vibrational imaging by hyperspectral stimulated Raman scattering microscopy and multivariate curve resolution analysis.

    PubMed

    Zhang, Delong; Wang, Ping; Slipchenko, Mikhail N; Ben-Amotz, Dor; Weiner, Andrew M; Cheng, Ji-Xin

    2013-01-01

    Spectroscopic imaging has been an increasingly critical approach for unveiling specific molecules in biological environments. Toward this goal, we demonstrate hyperspectral stimulated Raman loss (SRL) imaging by intrapulse spectral scanning through a femtosecond pulse shaper. The hyperspectral stack of SRL images is further analyzed by a multivariate curve resolution (MCR) method to reconstruct quantitative concentration images for each individual component and retrieve the corresponding vibrational Raman spectra. Using these methods, we demonstrate quantitative mapping of dimethyl sulfoxide concentration in aqueous solutions and in fat tissue. Moreover, MCR is performed on SRL images of breast cancer cells to generate maps of principal chemical components along with their respective vibrational spectra. These results show the great capability and potential of hyperspectral SRL microscopy for quantitative imaging of complicated biomolecule mixtures through resolving overlapped Raman bands.

  1. Comment on ``Morphology-dependent stimulated Raman scattering imaging'' [J. Chem. Phys. 105, 7276 (1996)

    NASA Astrophysics Data System (ADS)

    Campillo, A. J.; Eversole, J. D.; Lin, H.-B.

    1998-11-01

    We comment on a recent paper by J.-X. Zhang, P. A. Moortgat, and P. M. Aker [J. Chem. Phys. 105, 7276 (1996)]. We disagree with their interpretation of droplet stimulated Raman scattering spectral data as well as claims that surface electrical charge greatly affects hydrogen bonding at micrometer depths into water droplets.

  2. Molded plasmonic crystals for detecting and spatially imaging surface bound species by surface-enhanced Raman scattering.

    SciTech Connect

    Baca, A. J.; Truong, T. T.; Cambrea, L. R.; Montgomery, J. M.; Abdula, D.; Banks, T. R.; Yao, J.; Nuzzo, R. G.; Gray, S. K.; Rogers, J. A.

    2009-06-24

    This report introduces a type of plasmonic crystal that consists of metal coated nanostructures of relief molded on a polymer film as a substrate for surface-enhanced Raman scattering (SERS). Such crystals exhibit SERS enhancement factors of {approx} 10{sup 5}, over large areas and with sufficiently high levels of uniformity for precise two-dimensional Raman mapping of surface bound monolayers. The ease of fabrication together with the high sensitivities and spatial resolution that can be achieved suggests an attractive route to SERS substrates for portable chemical warfare agent detection, environmental monitors, noninvasive imaging of biomolecules, and other applications.

  3. Stimulated Raman scattering holography for time-resolved imaging of methane gas.

    PubMed

    Amer, Eynas; Gren, Per; Edenharder, Stefan; Sjödahl, Mikael

    2016-05-01

    In this paper, pulsed digital holographic detection is coupled to the stimulated Raman scattering (SRS) process for imaging gases. A Q-switched Nd-YAG laser (532 nm) has been used to pump methane gas (CH4) at pressures up to 12 bars. The frequency-tripled (355 nm) beam from the same laser was used to pump an optical parametric oscillator (OPO). The Stokes beam (from the OPO) has been tuned to 629.93 nm so that the frequency difference between the pump (532 nm) and the Stokes beams fits a Raman active vibrational mode of the methane molecule (2922  cm-1). The pump beam has been spatially modulated with fringes produced in a Michelson interferometer. The pump and the Stokes beams were overlapped in time, space, and polarization on the gas molecules, resulting in a stimulated Raman gain of the Stokes beam and a corresponding loss of the pump beam through the SRS process. The resulting gain of the Stokes beam has been detected using pulsed digital holography by blending it with a reference beam on the detector. Two holograms of the Stokes beam, without and with the pump beam fringes present, were recorded. Intensity maps calculated from the recorded digital holograms showed amplification of the Stokes beam at the position of overlap with the pump beam fringes and the gas molecules. The gain of the Stokes beam has been separated from the background in the Fourier domain. A gain of about 4.5% at a pump beam average intensity of 4  MW/cm2 and a Stokes beam intensity of 0.16  MW/cm2 have been recorded at a gas pressure of 12 bars. The gain decreased linearly with decreasing gas pressure. The results show that SRS holography is a promising technique to pinpoint a specific species and record its spatial and temporal distribution. PMID:27140351

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

    PubMed Central

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

    2009-01-01

    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 pico-second 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. PMID:16642124

  5. Stimulated rotational Raman scattering

    NASA Astrophysics Data System (ADS)

    Parazzoli, C. G.; Rafanelli, G. L.; Capps, D. M.; Drutman, C.

    1989-03-01

    The effect of Stimulated Rotational Raman Scattering (SRRS) processes on high energy laser directed energy weapon systems was studied. The program had 3 main objectives; achieving an accurate description of the physical processes involved in SRRS; developing a numerical algorithm to confidently evaluate SRRS-induced losses in the propagation of high energy laser beams in the uplink and downlink segments of the optical trains of various strategic defense system scenarios; and discovering possible methods to eliminate, or at least reduce, the deleterious effects of SRRS on the energy deposition on target. The following topics are discussed: the motivation for the accomplishments of the DOE program; the Semiclassical Theory of Non-Resonant SRRS for Diatomic Homonuclear Molecules; and then the following appendices; Calculation of the Dipole Transition Reduced Matrix Element, Guided Tour of Hughes SRRS Code, Running the Hughes SRRS Code, and Hughes SRRS Code Listing.

  6. Highly specific label-free molecular imaging with spectrally tailored excitation-stimulated Raman scattering (STE-SRS) microscopy

    NASA Astrophysics Data System (ADS)

    Freudiger, Christian W.; Min, Wei; Holtom, Gary R.; Xu, Bingwei; Dantus, Marcos; Sunney Xie, X.

    2011-02-01

    Label-free microscopy that has chemical contrast and high acquisition speeds up to video rates has recently been made possible using stimulated Raman scattering (SRS) microscopy. SRS imaging offers high sensitivity, but the spectral specificity of the original narrowband implementation is limited, making it difficult to distinguish chemical species with overlapping Raman bands. Here, we present a highly specific imaging method that allows mapping of a particular chemical species in the presence of interfering species, based on tailored multiplex excitation of its vibrational spectrum. This is implemented by spectral modulation of a broadband pump beam at a high frequency (>1 MHz), allowing detection of the SRS signal of the narrowband Stokes beam with high sensitivity. Using the scheme, we demonstrate quantification of cholesterol in the presence of lipids, and real-time three-dimensional spectral imaging of protein, stearic acid and oleic acid in live Caenorhabditis elegans.

  7. Surface-Enhanced Raman Scattering Active Plasmonic Nanoparticles with Ultrasmall Interior Nanogap for Multiplex Quantitative Detection and Cancer Cell Imaging.

    PubMed

    Li, Jiuxing; Zhu, Zhi; Zhu, Bingqing; Ma, Yanli; Lin, Bingqian; Liu, Rudi; Song, Yanling; Lin, Hui; Tu, Song; Yang, Chaoyong

    2016-08-01

    Due to its large enhancement effect, nanostructure-based surface-enhanced Raman scattering (SERS) technology had been widely applied for bioanalysis and cell imaging. However, most SERS nanostructures suffer from poor signal reproducibility, which hinders the application of SERS nanostructures in quantitative detection. We report an etching-assisted approach to synthesize SERS-active plasmonic nanoparticles with 1 nm interior nanogap for multiplex quantitative detection and cancer cell imaging. Raman dyes and methoxy poly(ethylene glycol) thiol (mPEG-SH) were attached to gold nanoparticles (AuNPs) to prepare gold cores. Next, Ag atoms were deposited on gold cores in the presence of Pluronic F127 to form a Ag shell. HAuCl4 was used to etch the Ag shell and form an interior nanogap in Au@AgAuNPs, leading to increased Raman intensity of dyes. SERS intensity distribution of Au@AgAuNPs was found to be more uniform than that of aggregated AuNPs. Finally, Au@AgAuNPs were used for multiplex quantitative detection and cancer cell imaging. With the advantages of simple and rapid preparation of Au@AgAuNPs with highly uniform, stable, and reproducible Raman intensity, the method reported here will widen the applications of SERS-active nanoparticles in diagnostics and imaging. PMID:27385563

  8. Polarization-resolved hyperspectral stimulated Raman scattering microscopy for label-free biomolecular imaging of the tooth

    NASA Astrophysics Data System (ADS)

    Wang, Zi; Zheng, Wei; Hsu, Chin-Ying Stephen; Huang, Zhiwei

    2016-01-01

    We report the development and implementation of a rapid polarization-resolved hyperspectral stimulated Raman scattering (SRS) microscopy technique for label-free biomolecular imaging of the tooth. The hyperspectral SRS imaging technique developed covers both fingerprint (800-1800 cm-1) and high-wavenumber (2800-3600 cm-1) regions for tooth Raman imaging without fluorescence background interference with an imaging speed of <0.3 s per frame of 512 × 512 pixels (˜1 μs per pixel), that is, >106 faster than confocal Raman imaging. Significant differences of hyperspectral SRS spectra among different tooth locations (e.g., dentin, enamel, and dentin-enamel junction) are observed, revealing the biochemical distribution differences across the tooth. Further polarization-resolved SRS imaging shows different polarization dependences related to the molecular orientation differences of various tooth locations. This work demonstrates the potential of polarization-resolved hyperspectral SRS imaging technique developed in rapidly characterizing biochemical structures and compositions as well as biomolecule organizations/orientations of the tooth without labeling.

  9. New imaging-based biomarkers for melanoma diagnosis using coherent Raman Scattering microscopy (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Wang, Hequn; Osseiran, Sam; Roider, Elisabeth; Fisher, David E.; Evans, Conor L.

    2016-02-01

    Recently, pheomelanin has been found to play a critical role in melanoma progression given its pro-oxidant chemical properties as well as its marked presence in pre-cancerous and malignant melanoma lesions, even in the absence of ultraviolet radiation. In addition, epidemiological evidence indicates a strong correlation between melanoma incidence and skin type, with the highest incidence occurring in individuals of the red-haired/fair-skinned phenotype. Interestingly, nevus count correlates well with melanoma incidence and skin type, except in the population most prone to developing melanoma, where nevus count strikingly drops. As such, a current hypothesis proposes that fair-skinned red-haired individuals, who are unable to stimulate production of eumelanin due to a mutation in MC1R in melanocytes, may actually harbor numerous "invisible", pheomelanin-rich nevi that evade clinical detection, supporting the high incidence of melanoma in that population. Here, we show for the very first time that melanocytes extracted from genetically modified MC1R-mutant, red-haired mice displayed bright perinuclear distributions of signal within the cells under coherent anti-Stokes Raman scattering (CARS) microscopy. Changes in pheomelanin production in siRNA knockdowns of cultured human melanoma cells were also sensed. We then successfully imaged pheomelanin distributions in both ex vivo and in vivo mouse ear skin. Finally, melanosomes within amelanotic melanoma patient tissue sections were found to show bright pheomelanin signals. This is the first time, to our knowledge, that pheomelanin has been found spatially localized in a human amelanotic melanoma sample. These pheomelanotic CARS features may be used as potential biomarkers for melanoma detection, especially for amelanotic melanomas.

  10. Stimulated Raman photoacoustic imaging

    PubMed Central

    Yakovlev, Vladislav V.; Zhang, Hao F.; Noojin, Gary D.; Denton, Michael L.; Thomas, Robert J.; Scully, Marlan O.

    2010-01-01

    Achieving label-free, molecular-specific imaging with high spatial resolution in deep tissue is often considered the grand challenge of optical imaging. To accomplish this goal, significant optical scattering in tissues has to be overcome while achieving molecular specificity without resorting to extrinsic labeling. We demonstrate the feasibility of developing such an optical imaging modality by combining the molecularly specific stimulated Raman excitation with the photoacoustic detection. By employing two ultrashort excitation laser pulses, separated in frequency by the vibrational frequency of a targeted molecule, only the specific vibrational level of the target molecules in the illuminated tissue volume is excited. This targeted optical absorption generates ultrasonic waves (referred to as stimulated Raman photoacoustic waves) which are detected using a traditional ultrasonic transducer to form an image following the design of the established photoacoustic microscopy. PMID:21059930

  11. Morphology-dependent stimulated Raman scattering imaging. II. Experimental studies of solvent structure in the diffuse electric double layer

    NASA Astrophysics Data System (ADS)

    Zhang, Jian-Xiang; Moortgat, Philip A.; Aker, Pamela M.

    1996-11-01

    Experimental confirmation that morphology-dependent stimulated Raman scattering can be used as an optical imaging technique is given. The water structure variations present at a charged water/air interface have been mapped. The measured structure variations track precisely that given by the Gouy-Chapman theory. We present, to our knowledge, the first experimental investigations of water solvent response in the diffuse part of the electric double layer. Imaging experiments on droplets charged to both positive and negative values have enabled us to determine the neutral water/air interface potential.

  12. Morphology-dependent stimulated Raman scattering imaging. II. Experimental studies of solvent structure in the diffuse electric double layer

    SciTech Connect

    Zhang, J.; Moortgat, P.A.; Aker, P.M.

    1996-11-01

    Experimental confirmation that morphology-dependent stimulated Raman scattering can be used as an optical imaging technique is given. The water structure variations present at a charged water/air interface have been mapped. The measured structure variations track precisely that given by the Gouy{endash}Chapman theory. We present, to our knowledge, the first experimental investigations of water solvent response in the diffuse part of the electric double layer. Imaging experiments on droplets charged to both positive and negative values have enabled us to determine the neutral water/air interface potential. {copyright} {ital 1996 American Institute of Physics.}

  13. Assessing Cholesterol Storage in Live Cells and C. elegans by Stimulated Raman Scattering Imaging of Phenyl-Diyne Cholesterol

    NASA Astrophysics Data System (ADS)

    Lee, Hyeon Jeong; Zhang, Wandi; Zhang, Delong; Yang, Yang; Liu, Bin; Barker, Eric L.; Buhman, Kimberly K.; Slipchenko, Lyudmila V.; Dai, Mingji; Cheng, Ji-Xin

    2015-01-01

    We report a cholesterol imaging method using rationally synthesized phenyl-diyne cholesterol (PhDY-Chol) and stimulated Raman scattering (SRS) microscope. The phenyl-diyne group is biologically inert and provides a Raman scattering cross section that is 88 times larger than the endogenous C = O stretching mode. SRS microscopy offers an imaging speed that is faster than spontaneous Raman microscopy by three orders of magnitude, and a detection sensitivity of 31 μM PhDY-Chol (~1,800 molecules in the excitation volume). Inside living CHO cells, PhDY-Chol mimics the behavior of cholesterol, including membrane incorporation and esterification. In a cellular model of Niemann-Pick type C disease, PhDY-Chol reflects the lysosomal accumulation of cholesterol, and shows relocation to lipid droplets after HPβCD treatment. In live C. elegans, PhDY-Chol mimics cholesterol uptake by intestinal cells and reflects cholesterol storage. Together, our work demonstrates an enabling platform for study of cholesterol storage and trafficking in living cells and vital organisms.

  14. Assessing Cholesterol Storage in Live Cells and C. elegans by Stimulated Raman Scattering Imaging of Phenyl-Diyne Cholesterol

    PubMed Central

    Lee, Hyeon Jeong; Zhang, Wandi; Zhang, Delong; Yang, Yang; Liu, Bin; Barker, Eric L.; Buhman, Kimberly K.; Slipchenko, Lyudmila V.; Dai, Mingji; Cheng, Ji-Xin

    2015-01-01

    We report a cholesterol imaging method using rationally synthesized phenyl-diyne cholesterol (PhDY-Chol) and stimulated Raman scattering (SRS) microscope. The phenyl-diyne group is biologically inert and provides a Raman scattering cross section that is 88 times larger than the endogenous C = O stretching mode. SRS microscopy offers an imaging speed that is faster than spontaneous Raman microscopy by three orders of magnitude, and a detection sensitivity of 31 μM PhDY-Chol (~1,800 molecules in the excitation volume). Inside living CHO cells, PhDY-Chol mimics the behavior of cholesterol, including membrane incorporation and esterification. In a cellular model of Niemann-Pick type C disease, PhDY-Chol reflects the lysosomal accumulation of cholesterol, and shows relocation to lipid droplets after HPβCD treatment. In live C. elegans, PhDY-Chol mimics cholesterol uptake by intestinal cells and reflects cholesterol storage. Together, our work demonstrates an enabling platform for study of cholesterol storage and trafficking in living cells and vital organisms. PMID:25608867

  15. Integrated coherent anti-Stokes Raman scattering and multiphoton microscopy for biomolecular imaging using spectral filtering of a femtosecond laser

    NASA Astrophysics Data System (ADS)

    Lu, Fake; Zheng, Wei; Lin, Jian; Huang, Zhiwei

    2010-03-01

    We report on a unique implementation of a dual 4-f paired-gratings spectral filtering of a femtosecond (fs) laser to realize high contrast coherent anti-Stokes Raman scattering (CARS) microscopy and high quality multiphoton microscopy on the same platform for label-free biomolecular imaging. The 4-f gratings filtering enables readily conversion of the 100 fs laser pulse trains into transform-limited 1 picosecond (ps) pulses in the spectral range of 700-1600 nm for CARS imaging. Compared with fs-CARS microscopy, our ps-CARS imaging yields an approximately tenfold improvement in spectral resolution, while a twofold improvement in nonresonant background suppression. High quality second-harmonic generation and two-photon excitation fluorescence imaging can also be acquired in tandem when swapping the 4-f grating filtering from the ps mode to fs mode. We demonstrate this multimodal nonlinear optical microscopy technique by imaging 465 nm polystyrene beads in water and animal liver tissue.

  16. Texture analysis and classification in coherent anti-Stokes Raman scattering (CARS) microscopy images for automated detection of skin cancer.

    PubMed

    Legesse, Fisseha Bekele; Medyukhina, Anna; Heuke, Sandro; Popp, Jürgen

    2015-07-01

    Coherent anti-Stokes Raman scattering (CARS) microscopy is a powerful tool for fast label-free tissue imaging, which is promising for early medical diagnostics. To facilitate the diagnostic process, automatic image analysis algorithms, which are capable of extracting relevant features from the image content, are needed. In this contribution we perform an automated classification of healthy and tumor areas in CARS images of basal cell carcinoma (BCC) skin samples. The classification is based on extraction of texture features from image regions and subsequent classification of these regions into healthy and cancerous with a perceptron algorithm. The developed approach is capable of an accurate classification of texture types with high sensitivity and specificity, which is an important step towards an automated tumor detection procedure. PMID:25797604

  17. 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.

  18. High-sensitivity, real-time, ratiometric imaging of surface-enhanced Raman scattering nanoparticles with a clinically translatable Raman endoscope device

    PubMed Central

    Garai, Ellis; Sensarn, Steven; Zavaleta, Cristina L.; Van de Sompel, Dominique; Loewke, Nathan O.; Mandella, Michael J.

    2013-01-01

    Abstract. Topical application and quantification of targeted, surface-enhanced Raman scattering (SERS) nanoparticles offer a new technique that has the potential for early detection of epithelial cancers of hollow organs. Although less toxic than intravenous delivery, the additional washing required to remove unbound nanoparticles cannot necessarily eliminate nonspecific pooling. Therefore, we developed a real-time, ratiometric imaging technique to determine the relative concentrations of at least two spectrally unique nanoparticle types, where one serves as a nontargeted control. This approach improves the specific detection of bound, targeted nanoparticles by adjusting for working distance and for any nonspecific accumulation following washing. We engineered hardware and software to acquire SERS signals and ratios in real time and display them via a graphical user interface. We report quantitative, ratiometric imaging with nanoparticles at pM and sub-pM concentrations and at varying working distances, up to 50 mm. Additionally, we discuss optimization of a Raman endoscope by evaluating the effects of lens material and fiber coating on background noise, and theoretically modeling and simulating collection efficiency at various working distances. This work will enable the development of a clinically translatable, noncontact Raman endoscope capable of rapidly scanning large, topographically complex tissue surfaces for small and otherwise hard to detect lesions. PMID:24008818

  19. An optimized electroporation method for delivering nanoparticles into living cells for surface-enhanced Raman scattering imaging

    NASA Astrophysics Data System (ADS)

    Yu, Yun; Wang, Jing; Lin, Juqiang; Lin, Duo; Chen, Weiwei; Feng, Shangyuan; Huang, Zufang; Li, Yongzeng; Huang, Hao; Shi, Hong; Chen, Rong

    2016-04-01

    The existing electroporation method can rapidly deliver nanoparticles (NPs) into living cells for intracellular surface-enhanced Raman scattering (SERS) imaging. Unfortunately, the cellular SERS signals are major from molecules located near the two poles of the cell facing toward to the electrodes because most NPs enter cells through these two poles and easily happen to aggregate there. Here, we present an optimized electroporation method for transferring NPs into living cells to obtain a uniform NPs distribution. The distribution of intracellular NPs was monitored by the SERS signal of 4-mercaptobenzoic acid, which is sandwiched between the Au-Ag core-shell and validated by TEM images. In addition, based on this uniform distribution of NPs, we then detected the distribution of cellular molecules like phenylalanine and lipid via SERS imaging. Results demonstrate the great potential for the optimized electroporation-based SERS imaging in cellular study.

  20. 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.

  1. A Real-Time Clinical Endoscopic System for Intraluminal, Multiplexed Imaging of Surface-Enhanced Raman Scattering Nanoparticles

    PubMed Central

    Garai, Ellis; Loewke, Nathan O.; Rogalla, Stephan; Mandella, Michael J.; Felt, Stephen A.; Friedland, Shai; Liu, Jonathan T. C.; Gambhir, Sanjiv S.; Contag, Christopher H.

    2015-01-01

    The detection of biomarker-targeting surface-enhanced Raman scattering (SERS) nanoparticles (NPs) in the human gastrointestinal tract has the potential to improve early cancer detection; however, a clinically relevant device with rapid Raman-imaging capability has not been described. Here we report the design and in vivo demonstration of a miniature, non-contact, opto-electro-mechanical Raman device as an accessory to clinical endoscopes that can provide multiplexed molecular data via a panel of SERS NPs. This device enables rapid circumferential scanning of topologically complex luminal surfaces of hollow organs (e.g., colon and esophagus) and produces quantitative images of the relative concentrations of SERS NPs that are present. Human and swine studies have demonstrated the speed and simplicity of this technique. This approach also offers unparalleled multiplexing capabilities by simultaneously detecting the unique spectral fingerprints of multiple SERS NPs. Therefore, this new screening strategy has the potential to improve diagnosis and to guide therapy by enabling sensitive quantitative molecular detection of small and otherwise hard-to-detect lesions in the context of white-light endoscopy. PMID:25923788

  2. Live-cell vibrational imaging of choline metabolites by stimulated Raman scattering coupled with isotope-based metabolic labeling

    PubMed Central

    Hu, Fanghao; Wei, Lu; Zheng, Chaogu; Shen, Yihui

    2014-01-01

    Choline is a small molecule that occupies a key position in the biochemistry of all living organisms. Recent studies have strongly implicated choline metabolites in cancer, atherosclerosis and nervous system development. To detect choline and its metabolites, existing physical methods such as magnetic resonance spectroscopy and positron emission tomography, are often limited by the poor spatial resolution and substantial radiation dose. Fluorescence imaging, although with submicrometer resolution, requires introduction of bulky fluorophores and thus is difficult in labeling the small choline molecule. By combining the emerging bond-selective stimulated Raman scattering microscopy with metabolic incorporation of deuterated choline, herein we have achieved high resolution imaging of choline-containing metabolites in living mammalian cell lines, primary hippocampal neurons and multicellular organism C. elegans. Different subcellular distributions of choline metabolites are observed between cancer cells and non-cancer cells, which may reveal functional difference in the choline metabolism and lipid-mediated signaling events. In neurons, choline incorporation is visualized within both soma and neurites, where choline metabolites are more evenly distributed compared to the protein. Furthermore, choline localization is also observed in the pharynx region of C. elegans larvae, consistent with its organogenesis mechanism. These applications demonstrate the potential of isotope-based stimulated Raman scattering microscopy for future choline-related disease detection and development monitoring in vivo. PMID:24555181

  3. Characterization of conductive nanobiomaterials derived from viral assemblies by low-voltage STEM imaging and Raman scattering

    NASA Astrophysics Data System (ADS)

    Plascencia-Villa, Germán; Carreño-Fuentes, Liliana; Bahena, Daniel; José-Yacamán, Miguel; Palomares, Laura A.; Ramírez, Octavio T.

    2014-09-01

    New technologies require the development of novel nanomaterials that need to be fully characterized to achieve their potential. High-resolution low-voltage scanning transmission electron microscopy (STEM) has proven to be a very powerful technique in nanotechnology, but its use for the characterization of nanobiomaterials has been limited. Rotavirus VP6 self-assembles into nanotubular assemblies that possess an intrinsic affinity for Au ions. This property was exploited to produce hybrid nanobiomaterials by the in situ functionalization of recombinant VP6 nanotubes with gold nanoparticles. In this work, Raman spectroscopy and advanced analytical electron microscopy imaging with spherical aberration-corrected (Cs) STEM and nanodiffraction at low-voltage doses were employed to characterize nanobiomaterials. STEM imaging revealed the precise structure and arrangement of the protein templates, as well as the nanostructure and atomic arrangement of gold nanoparticles with high spatial sub-Angstrom resolution and avoided radiation damage. The imaging was coupled with backscattered electron imaging, ultra-high resolution scanning electron microscopy and x-ray spectroscopy. The hybrid nanobiomaterials that were obtained showed unique properties as bioelectronic conductive devices and showed enhanced Raman scattering by their precise arrangement into superlattices, displaying the utility of viral assemblies as functional integrative self-assembled nanomaterials for novel applications.

  4. Plasmon Mapping in Metallic Nanostructures and its Application to Single Molecule Surface Enhanced Raman Scattering: Imaging Electromagnetic Hot-Spots and Analyte Location

    SciTech Connect

    Camden, Jon P

    2013-07-16

    A major component of this proposal is to elucidate the connection between optical and electron excitation of plasmon modes in metallic nanostructures. These accomplishments are reported: developed a routine protocol for obtaining spatially resolved, low energy EELS spectra, and resonance Rayleigh scattering spectra from the same nanostructures.; correlated optical scattering spectra and plasmon maps obtained using STEM/EELS.; and imaged electromagnetic hot spots responsible for single-molecule surface-enhanced Raman scattering (SMSERS).

  5. Penetration of silver nanoparticles into porcine skin ex vivo using fluorescence lifetime imaging microscopy, Raman microscopy, and surface-enhanced Raman scattering microscopy.

    PubMed

    Zhu, Yongjian; Choe, Chun-Sik; Ahlberg, Sebastian; Meinke, Martina C; Alexiev, Ulrike; Lademann, Juergen; Darvin, Maxim E

    2015-05-01

    In order to investigate the penetration depth of silver nanoparticles (Ag NPs) inside the skin, porcine ears treated with Ag NPs are measured by two-photon tomography with a fluorescence lifetime imaging microscopy (TPT-FLIM) technique, confocal Raman microscopy (CRM), and surface-enhanced Raman scattering (SERS) microscopy. Ag NPs are coated with poly-N-vinylpyrrolidone and dispersed in pure water solutions. After the application of Ag NPs, porcine ears are stored in the incubator for 24 h at a temperature of 37°C. The TPT-FLIM measurement results show a dramatic decrease of the Ag NPs' signal intensity from the skin surface to a depth of 4 μm. Below 4 μm, the Ag NPs' signal continues to decline, having completely disappeared at 12 to 14 μm depth. CRM shows that the penetration depth of Ag NPs is 11.1 ± 2.1 μm. The penetration depth measured with a highly sensitive SERS microscopy reaches 15.6 ± 8.3 μm. Several results obtained with SERS show that the penetration depth of Ag NPs can exceed the stratum corneum (SC) thickness, which can be explained by both penetration of trace amounts of Ag NPs through the SC barrier and by the measurements inside the hair follicle, which cannot be excluded in the experiment. PMID:25394476

  6. Penetration of silver nanoparticles into porcine skin ex vivo using fluorescence lifetime imaging microscopy, Raman microscopy, and surface-enhanced Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Zhu, Yongjian; Choe, Chun-Sik; Ahlberg, Sebastian; Meinke, Martina C.; Alexiev, Ulrike; Lademann, Juergen; Darvin, Maxim E.

    2015-05-01

    In order to investigate the penetration depth of silver nanoparticles (Ag NPs) inside the skin, porcine ears treated with Ag NPs are measured by two-photon tomography with a fluorescence lifetime imaging microscopy (TPT-FLIM) technique, confocal Raman microscopy (CRM), and surface-enhanced Raman scattering (SERS) microscopy. Ag NPs are coated with poly-N-vinylpyrrolidone and dispersed in pure water solutions. After the application of Ag NPs, porcine ears are stored in the incubator for 24 h at a temperature of 37°C. The TPT-FLIM measurement results show a dramatic decrease of the Ag NPs' signal intensity from the skin surface to a depth of 4 μm. Below 4 μm, the Ag NPs' signal continues to decline, having completely disappeared at 12 to 14 μm depth. CRM shows that the penetration depth of Ag NPs is 11.1±2.1 μm. The penetration depth measured with a highly sensitive SERS microscopy reaches 15.6±8.3 μm. Several results obtained with SERS show that the penetration depth of Ag NPs can exceed the stratum corneum (SC) thickness, which can be explained by both penetration of trace amounts of Ag NPs through the SC barrier and by the measurements inside the hair follicle, which cannot be excluded in the experiment.

  7. Penetration of silver nanoparticles into porcine skin ex vivo using fluorescence lifetime imaging microscopy, Raman microscopy, and surface-enhanced Raman scattering microscopy.

    PubMed

    Zhu, Yongjian; Choe, Chun-Sik; Ahlberg, Sebastian; Meinke, Martina C; Alexiev, Ulrike; Lademann, Juergen; Darvin, Maxim E

    2015-05-01

    In order to investigate the penetration depth of silver nanoparticles (Ag NPs) inside the skin, porcine ears treated with Ag NPs are measured by two-photon tomography with a fluorescence lifetime imaging microscopy (TPT-FLIM) technique, confocal Raman microscopy (CRM), and surface-enhanced Raman scattering (SERS) microscopy. Ag NPs are coated with poly-N-vinylpyrrolidone and dispersed in pure water solutions. After the application of Ag NPs, porcine ears are stored in the incubator for 24 h at a temperature of 37°C. The TPT-FLIM measurement results show a dramatic decrease of the Ag NPs' signal intensity from the skin surface to a depth of 4 μm. Below 4 μm, the Ag NPs' signal continues to decline, having completely disappeared at 12 to 14 μm depth. CRM shows that the penetration depth of Ag NPs is 11.1 ± 2.1 μm. The penetration depth measured with a highly sensitive SERS microscopy reaches 15.6 ± 8.3 μm. Several results obtained with SERS show that the penetration depth of Ag NPs can exceed the stratum corneum (SC) thickness, which can be explained by both penetration of trace amounts of Ag NPs through the SC barrier and by the measurements inside the hair follicle, which cannot be excluded in the experiment.

  8. 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

  9. Integrated femtosecond stimulated Raman scattering and two-photon fluorescence imaging of subcellular lipid and vesicular structures.

    PubMed

    Li, Xuesong; Lam, Wen Jiun; Cao, Zhe; Hao, Yan; Sun, Qiqi; He, Sicong; Mak, Ho Yi; Qu, Jianan Y

    2015-11-01

    The primary goal of this study is to demonstrate that stimulated Raman scattering (SRS) as a new imaging modality can be integrated into a femtosecond (fs) nonlinear optical (NLO) microscope system. The fs sources of high pulse peak power are routinely used in multimodal nonlinear microscopy to enable efficient excitation of multiple NLO signals. However, with fs excitations, the SRS imaging of subcellular lipid and vesicular structures encounters significant interference from proteins due to poor spectral resolution and a lack of chemical specificity, respectively. We developed a unique NLO microscope of fs excitation that enables rapid acquisition of SRS and multiple two-photon excited fluorescence (TPEF) signals. In the in vivo imaging of transgenic C. elegans animals, we discovered that by cross-filtering false positive lipid signals based on the TPEF signals from tryptophan-bearing endogenous proteins and lysosome-related organelles, the imaging system produced highly accurate assignment of SRS signals to lipid. Furthermore, we demonstrated that the multimodal NLO microscope system could sequentially image lipid structure/content and organelles, such as mitochondria, lysosomes, and the endoplasmic reticulum, which are intricately linked to lipid metabolism.

  10. Integrated femtosecond stimulated Raman scattering and two-photon fluorescence imaging of subcellular lipid and vesicular structures

    NASA Astrophysics Data System (ADS)

    Li, Xuesong; Lam, Wen Jiun; Cao, Zhe; Hao, Yan; Sun, Qiqi; He, Sicong; Mak, Ho Yi; Qu, Jianan Y.

    2015-11-01

    The primary goal of this study is to demonstrate that stimulated Raman scattering (SRS) as a new imaging modality can be integrated into a femtosecond (fs) nonlinear optical (NLO) microscope system. The fs sources of high pulse peak power are routinely used in multimodal nonlinear microscopy to enable efficient excitation of multiple NLO signals. However, with fs excitations, the SRS imaging of subcellular lipid and vesicular structures encounters significant interference from proteins due to poor spectral resolution and a lack of chemical specificity, respectively. We developed a unique NLO microscope of fs excitation that enables rapid acquisition of SRS and multiple two-photon excited fluorescence (TPEF) signals. In the in vivo imaging of transgenic C. elegans animals, we discovered that by cross-filtering false positive lipid signals based on the TPEF signals from tryptophan-bearing endogenous proteins and lysosome-related organelles, the imaging system produced highly accurate assignment of SRS signals to lipid. Furthermore, we demonstrated that the multimodal NLO microscope system could sequentially image lipid structure/content and organelles, such as mitochondria, lysosomes, and the endoplasmic reticulum, which are intricately linked to lipid metabolism.

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

    PubMed Central

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

    2005-01-01

    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. PMID:16263923

  12. Integrated femtosecond stimulated Raman scattering and two-photon fluorescence imaging of subcellular lipid and vesicular structures.

    PubMed

    Li, Xuesong; Lam, Wen Jiun; Cao, Zhe; Hao, Yan; Sun, Qiqi; He, Sicong; Mak, Ho Yi; Qu, Jianan Y

    2015-11-01

    The primary goal of this study is to demonstrate that stimulated Raman scattering (SRS) as a new imaging modality can be integrated into a femtosecond (fs) nonlinear optical (NLO) microscope system. The fs sources of high pulse peak power are routinely used in multimodal nonlinear microscopy to enable efficient excitation of multiple NLO signals. However, with fs excitations, the SRS imaging of subcellular lipid and vesicular structures encounters significant interference from proteins due to poor spectral resolution and a lack of chemical specificity, respectively. We developed a unique NLO microscope of fs excitation that enables rapid acquisition of SRS and multiple two-photon excited fluorescence (TPEF) signals. In the in vivo imaging of transgenic C. elegans animals, we discovered that by cross-filtering false positive lipid signals based on the TPEF signals from tryptophan-bearing endogenous proteins and lysosome-related organelles, the imaging system produced highly accurate assignment of SRS signals to lipid. Furthermore, we demonstrated that the multimodal NLO microscope system could sequentially image lipid structure/content and organelles, such as mitochondria, lysosomes, and the endoplasmic reticulum, which are intricately linked to lipid metabolism. PMID:26580697

  13. 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.

  14. Multifunctional superparamagnetic nanoshells: combining two-photon luminescence imaging, surface-enhanced Raman scattering and magnetic separation.

    PubMed

    Jin, Xiulong; Li, Haiyan; Wang, Shanshan; Kong, Ni; Xu, Hong; Fu, Qihua; Gu, Hongchen; Ye, Jian

    2014-11-01

    With the increasing need for multi-purpose analysis in the biomedical field, traditional single diagnosis methods cannot meet the requirements. Therefore new multifunctional technologies and materials for the integration of sample collection, sensing and imaging are in great demand. Core-shell nanoparticles offer a unique platform to combine multifunctions in a single particle. In this work, we have constructed a novel type of core-shell superparamagnetic nanoshell (Fe₃O₄@SiO₂@Au), composed of a Fe₃O₄ cluster core, a thin Au shell and a SiO₂ layer in between. The obtained multifunctional nanoparticles combine the magnetic properties and plasmonic optical properties effectively, which were well investigated by a number of experimental characterization methods and theoretical simulations. We have demonstrated that Fe₃O₄@SiO₂@Au nanoparticles can be utilized for two-photon luminescence (TPL) imaging, near-infrared surface-enhanced Raman scattering (NIR SERS) and cell collection by magnetic separation. The TPL intensity could be further greatly enhanced through the plasmon coupling effect in the self-assembled nanoparticle chains, which were triggered by an external magnetic field. In addition, Fe₃O₄@SiO₂@Au nanoparticles may have great potential applications such as enhanced magnetic resonance imaging (MRI) and photo-thermotherapy. Successful combination of multifunctions including magnetic response, biosensing and bioimaging in single nanoparticles allows further manipulation, real-time tracking, and intracellular molecule analysis of live cells at a single-cell level. PMID:25329447

  15. Vibrational imaging of glucose uptake activity in live cells and tissues by stimulated Raman scattering microscopy (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Hu, Fanghao; Chen, Zhixing; Zhang, Luyuan; Shen, Yihui; Wei, Lu; Min, Wei

    2016-03-01

    Glucose is consumed as an energy source by virtually all living organisms, from bacteria to humans. Its uptake activity closely reflects the cellular metabolic status in various pathophysiological transformations, such as diabetes and cancer. Extensive efforts such as positron emission tomography, magnetic resonance imaging and fluorescence microscopy have been made to specifically image glucose uptake activity but all with technical limitations. Here, we report a new platform to visualize glucose uptake activity in live cells and tissues with subcellular resolution and minimal perturbation. A novel glucose analogue with a small alkyne tag (carbon-carbon triple bond) is developed to mimic natural glucose for cellular uptake, which can be imaged with high sensitivity and specificity by targeting the strong and characteristic alkyne vibration on stimulated Raman scattering (SRS) microscope to generate a quantitative three dimensional concentration map. Cancer cells with differing metabolic characteristics can be distinguished. Heterogeneous uptake patterns are observed in tumor xenograft tissues, neuronal culture and mouse brain tissues with clear cell-cell variations. Therefore, by offering the distinct advantage of optical resolution but without the undesirable influence of bulky fluorophores, our method of coupling SRS with alkyne labeled glucose will be an attractive tool to study energy demands of living systems at the single cell level.

  16. 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

  17. Stimulated Raman Scattering Microscopy with a Robust Fibre Laser Source

    PubMed Central

    Freudiger, Christian W.; Yang, Wenlong; Holtom, Gary R.; Peyghambarian, Nasser; Xie, X. Sunney; Kieu, Khanh Q.

    2014-01-01

    Stimulated Raman Scattering microscopy allows label-free chemical imaging and has enabled exciting applications in biology, material science, and medicine. It provides a major advantage in imaging speed over spontaneous Raman scattering and has improved image contrast and spectral fidelity compared to coherent anti-Stokes Raman. Wider adoption of the technique has, however, been hindered by the need for a costly and environmentally sensitive tunable ultra-fast dual-wavelength source. We present the development of an optimized all-fibre laser system based on the optical synchronization of two picosecond power amplifiers. To circumvent the high-frequency laser noise intrinsic to amplified fibre lasers, we have further developed a high-speed noise cancellation system based on voltage-subtraction autobalanced detection. We demonstrate uncompromised imaging performance of our fibre-laser based stimulated Raman scattering microscope with shot-noise limited sensitivity and an imaging speed up to 1 frame/s. PMID:25313312

  18. Raman and coherent anti-Stokes Raman scattering microspectroscopy for biomedical applications.

    PubMed

    Krafft, Christoph; Dietzek, Benjamin; Schmitt, Michael; Popp, Jürgen

    2012-04-01

    A tutorial article is presented for the use of linear and nonlinear Raman microspectroscopies in biomedical diagnostics. Coherent anti-Stokes Raman scattering (CARS) is the most frequently applied nonlinear variant of Raman spectroscopy. The basic concepts of Raman and CARS are introduced first, and subsequent biomedical applications of Raman and CARS are described. Raman microspectroscopy is applied to both in-vivo and in-vitro tissue diagnostics, and the characterization and identification of individual mammalian cells. These applications benefit from the fact that Raman spectra provide specific information on the chemical composition and molecular structure in a label-free and nondestructive manner. Combining the chemical specificity of Raman spectroscopy with the spatial resolution of an optical microscope allows recording hyperspectral images with molecular contrast. We also elaborate on interfacing Raman spectroscopic tools with other technologies such as optical tweezing, microfluidics and fiber optic probes. Thereby, we aim at presenting a guide into one exciting branch of modern biophotonics research.

  19. Raman and coherent anti-Stokes Raman scattering microspectroscopy for biomedical applications

    NASA Astrophysics Data System (ADS)

    Krafft, Christoph; Dietzek, Benjamin; Schmitt, Michael; Popp, Jürgen

    2012-04-01

    A tutorial article is presented for the use of linear and nonlinear Raman microspectroscopies in biomedical diagnostics. Coherent anti-Stokes Raman scattering (CARS) is the most frequently applied nonlinear variant of Raman spectroscopy. The basic concepts of Raman and CARS are introduced first, and subsequent biomedical applications of Raman and CARS are described. Raman microspectroscopy is applied to both in-vivo and in-vitro tissue diagnostics, and the characterization and identification of individual mammalian cells. These applications benefit from the fact that Raman spectra provide specific information on the chemical composition and molecular structure in a label-free and nondestructive manner. Combining the chemical specificity of Raman spectroscopy with the spatial resolution of an optical microscope allows recording hyperspectral images with molecular contrast. We also elaborate on interfacing Raman spectroscopic tools with other technologies such as optical tweezing, microfluidics and fiber optic probes. Thereby, we aim at presenting a guide into one exciting branch of modern biophotonics research.

  20. Surface enhanced Raman scattering on Tardigrada--towards monitoring and imaging molecular structures in live cryptobiotic organisms.

    PubMed

    Kneipp, Harald; Møbjerg, Nadja; Jørgensen, Aslak; Bohr, Henrik G; Hélix-Nielsen, Claus; Kneipp, Janina; Kneipp, Katrin

    2013-10-01

    Tardigrades are microscopic metazoans which are able to survive extreme physical and chemical conditions by entering a stress tolerant state called cryptobiosis. At present, the molecular mechanisms behind cryptobiosis are still poorly understood. We show that surface enhanced Raman scattering supported by plasmonic gold nanoparticles can measure molecular constituents and their local distribution in live tardigrades. Surface enhanced Raman signatures allow to differentiate between two species and indicate molecular structural differences between tardigrades in water and in a dry state. This opens new avenues for exploring cryptobiosis by studying molecular changes in live cryptobiotic organisms.

  1. Surface enhanced Raman scattering on Tardigrada--towards monitoring and imaging molecular structures in live cryptobiotic organisms.

    PubMed

    Kneipp, Harald; Møbjerg, Nadja; Jørgensen, Aslak; Bohr, Henrik G; Hélix-Nielsen, Claus; Kneipp, Janina; Kneipp, Katrin

    2013-10-01

    Tardigrades are microscopic metazoans which are able to survive extreme physical and chemical conditions by entering a stress tolerant state called cryptobiosis. At present, the molecular mechanisms behind cryptobiosis are still poorly understood. We show that surface enhanced Raman scattering supported by plasmonic gold nanoparticles can measure molecular constituents and their local distribution in live tardigrades. Surface enhanced Raman signatures allow to differentiate between two species and indicate molecular structural differences between tardigrades in water and in a dry state. This opens new avenues for exploring cryptobiosis by studying molecular changes in live cryptobiotic organisms. PMID:23225705

  2. 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. PMID:18026271

  3. Imaging the intracellular distribution of tyrosine kinase inhibitors in living cells with quantitative hyperspectral stimulated Raman scattering

    NASA Astrophysics Data System (ADS)

    Fu, Dan; Zhou, Jing; Zhu, Wenjing Suzanne; Manley, Paul W.; Wang, Y. Karen; Hood, Tami; Wylie, Andrew; Xie, X. Sunney

    2014-07-01

    ABL1 tyrosine-kinase inhibitors (TKI) are front-line therapy for chronic myelogenous leukaemia and are among the best-known examples of targeted cancer therapeutics. However, the dynamic uptake into cells of TKIs of low molecular weight and their intracellular behaviour is unknown because of the difficulty of observing non-fluorescent small molecules at subcellular resolution. Here we report the direct label-free visualization and quantification of two TKI drugs (imatinib and nilotinib) inside living cells using hyperspectral stimulated Raman scattering imaging. Concentrations of both drugs were enriched over 1,000-fold in lysosomes as a result of their lysosomotropic properties. In addition, low solubility appeared to contribute significantly to the surprisingly large accumulation of nilotinib. We further show that the lysosomal trapping of imatinib was reduced more than tenfold when chloroquine is used simultaneously, which suggests that chloroquine may increase the efficacy of TKIs through lysosome-mediated drug-drug interaction in addition to the commonly proposed autophagy-inhibition mechanism.

  4. Understanding Polymer-Fullerene Morphology in Organic Solar Cells via Photoluminescence, Raman Scattering, and Spectroscopic Imaging

    NASA Astrophysics Data System (ADS)

    Carach, Christopher Andrew

    Understanding and controlling carrier transport in conjugated polymer films and composites is critical to the development and application of plastic solar cells. Recent efforts have focused on "bulk heterojunction" structures where a conjugated polymer donor is mixed at the nanoscale with a fullerene acceptor to achieve large interfacial areas for exciton splitting. In these systems, fabrication protocols dramatically affect device efficiency and charge transport is intimately tied to film morphology through local order, domain formation, and compositional heterogeneity. We employ both far-field and confocal/near-field optical spectroscopy (absorbance, low-temperature photoluminescence, Raman) to study chain order (aggregation, pi-stacking), photo-oxidation, and local morphology in conjugated polymer (PPV and polythiophene) -- fullerene (PCBM) blends. Through quantitative analysis of exciton bandwidths, emission intensity, and vibronic lineshapes, we demonstrate that competition exists between the chemical "disordering" effect of photo-degradation and the physical "ordering" effect of aggregation, each of which dominate under different processing conditions. Large changes in photoluminescence and Raman show that PCBM begins to significantly hinder intra-chain planarization and inter-chain pi-overlap at a critical PCBM weight fraction. Furthermore, the critical weight fraction is a function of the polymer regiochemistry, occurring at lower PCBM weight fractions for a more regio-random polymer. Mild thermal annealing of blended films was seen to restore order, which results from PCBM phase segregation (lower dispersion) and growth of polymer aggregates. Spatially resolved spectral analysis of photoluminescence was also used to map fullerene diffusion and agglomeration as well as detect local changes in interfacial contact between donor and acceptor domains due to thermal annealing.

  5. Imaging growth of neurites in conditioned hydrogel by coherent anti-stokes raman scattering microscopy.

    PubMed

    Conovaloff, Aaron; Wang, Han-Wei; Cheng, Ji-Xin; Panitch, Alyssa

    2009-10-01

    Cultured DRGs in different gel scaffolds were analyzed using CA RS microscopy to determine its possible use as a label-free imaging option for tracking cellular growth in a gel scaffold. This study demonstrates for the first time the applicability of CA RS microscopy to the imaging of live neuronal cells in GAG hydrogels. By tuning the laser beating frequency, omega(p)-omega(s), to match the vibration of C-H bonds in the cell membrane, the CA RS signal yields detailed, high-quality images of neurites with single membrane detection sensitivity. The results demonstrate that CA RS imaging allows monitoring of cellular growth in a tissue scaffold over time, with a contrast that shows comparable cellular structures to those obtained using standard fluorescent staining techniques. These findings show the potential of CARS microscopy to assist in the understanding of organogenesis processes in a tissue scaffold. PMID:20539743

  6. Excitation of coherent terahertz radiation by stimulated Raman scatterings

    SciTech Connect

    Liu, Z. J.; He, X. T.; Zheng, C. Y.; Zhu Shaoping; Cao, L. H.; Wang Yugang

    2010-02-15

    The excitation of terahertz radiation by stimulated Raman scattering is considered. Vlasov-Maxwell numerical simulations show that powerful terahertz radiation can be produced by cascade Raman scatterings.

  7. An integrated coherent anti-Stokes Raman scattering and multiphoton imaging technique for liver disease diagnosis

    NASA Astrophysics Data System (ADS)

    Lin, Jian; Lu, Fake; Zheng, Wei; Yu, Hanry; Sheppard, Colin; Huang, Zhiwei

    2012-03-01

    Liver steatosis and fibrosis are two prevalence liver diseases and may eventually develop into hepatocellular carcinoma (HCC) Due to their prevalence and severity, much work has been done to develop efficient diagnostic methods and therapies. Nonlinear optical microscopy has high sensitivity and chemical specificity for major biochemical compounds, making it a powerful tool for tissue imaging without staining. In this study, three nonlinear microscopy imaging modalities are applied to the study of liver diseases in a bile duct ligation rat modal. CARS shows the distributions of fats or lipids quantitatively across the tissue; SHG visualizes the collagens; and TPEF reveals the morphology of hepatic cells. The results clearly show the development of liver steatosis and fibrosis with time, and the hepatic fat and collagen fibrils are quantified. This study demonstrates the ability of multimodal nonlinear optical microscopy for liver disease diagnosis, and may provide new insights into the understanding of the mechanisms of steatosis/fibrosis transformations at the cellular and molecular levels.

  8. Label-free real-time imaging of myelination in the Xenopus laevis tadpole by in vivo stimulated Raman scattering microscopy

    PubMed Central

    Hu, Chun-Rui; Zhang, Delong; Slipchenko, Mikhail N.; Cheng, Ji-Xin; Hu, Bing

    2014-01-01

    Abstract. The myelin sheath plays an important role as the axon in the functioning of the neural system, and myelin degradation is a hallmark pathology of multiple sclerosis and spinal cord injury. Electron microscopy, fluorescent microscopy, and magnetic resonance imaging are three major techniques used for myelin visualization. However, microscopic observation of myelin in living organisms remains a challenge. Using a newly developed stimulated Raman scattering microscopy approach, we report noninvasive, label-free, real-time in vivo imaging of myelination by a single-Schwann cell, maturation of a single node of Ranvier, and myelin degradation in the transparent body of the Xenopus laevis tadpole. PMID:25104411

  9. Label-free real-time imaging of myelination in the Xenopus laevis tadpole by in vivo stimulated Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Hu, Chun-Rui; Zhang, Delong; Slipchenko, Mikhail N.; Cheng, Ji-Xin; Hu, Bing

    2014-08-01

    The myelin sheath plays an important role as the axon in the functioning of the neural system, and myelin degradation is a hallmark pathology of multiple sclerosis and spinal cord injury. Electron microscopy, fluorescent microscopy, and magnetic resonance imaging are three major techniques used for myelin visualization. However, microscopic observation of myelin in living organisms remains a challenge. Using a newly developed stimulated Raman scattering microscopy approach, we report noninvasive, label-free, real-time in vivo imaging of myelination by a single-Schwann cell, maturation of a single node of Ranvier, and myelin degradation in the transparent body of the Xenopus laevis tadpole.

  10. 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.

  11. 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.

  12. Electride Mediated Surface Enhanced Raman Scattering (SERS)

    NASA Technical Reports Server (NTRS)

    Anderson, Mark S. (Inventor)

    2016-01-01

    An electride may provide surface enhanced Raman scattering (SERS). The electride, a compound where the electrons serve as anions, may be a ceramic electride, such as a conductive ceramic derived from mayenite, or an organic electride, for example. The textured electride surface or electride particles may strongly enhance the Raman scattering of organic or other Raman active analytes. This may also provide a sensitive method for monitoring the chemistry and electronic environment at the electride surface. The results are evidence of a new class of polariton (i.e., a surface electride-polariton resonance mechanism) that is analogous to the surface plasmon-polariton resonance that mediates conventional SERS.

  13. Aggregation induced Raman scattering of squaraine dye: Implementation in diagnosis of cervical cancer dysplasia by SERS imaging.

    PubMed

    Narayanan, Nisha; Karunakaran, Varsha; Paul, Willi; Venugopal, Karunakaran; Sujathan, K; Kumar Maiti, Kaustabh

    2015-08-15

    The extent of squaraine dye aggregation that reflects on surface enhanced Raman signal scattering (SERS) intensity upon adsorption on nano-roughened gold surface has been investigated. Here we have synthesized a serious of six squaraine dyes consisting of two different electron donor moiety i.e. 1,1,2-trimethyl-1H-benzo[e]indole and 2-methylbenzo[d]thiazole which modulates the chemisorptions and hydrophobicity being designated as SQ1, SQ2, SQ3, SQ4, SQ5 and SQ6. Interestingly, SQ2 (mono lipoic acid appended), SQ5 and SQ6 (conjugated with hexyl and dodecyl side chain) squaraine derivatives having more tendency of aggregation in DMSO-water mixed solvent showed significant increase of Raman scattering in the fingerprint region when chemisorbed on spherical gold nanoparticles. Two sets of SERS nanotags were prepared with colloidal gold nanoparticle (Au-NPs size: 40 nm) by incorporating Raman reporters SQ2 and SQ5 followed by thiolated PEG encapsulation (SH-PEG, SH-PEG-COOH) denoted as AuNPs-SQ2-PEG and AuNPs-SQ5-PEG. Further conjugation of these nanotag with monoclonal antibodies specific to over expressed receptors, EGFR and p16/Ki-67 in cervical cancer cell, HeLa showed prominent SERS mapping intensity and selectivity towards cell surface and nucleus. The fast and accurate recognition obtained by antibody triggered SERS-nanotag has been compared with conventional time consuming immunocytochemistry technique which prompted us to extend further investigation using real patient cervical smear sample for a non-invasive, ultrafast and accurate diagnosis. PMID:25801955

  14. Aggregation induced Raman scattering of squaraine dye: Implementation in diagnosis of cervical cancer dysplasia by SERS imaging.

    PubMed

    Narayanan, Nisha; Karunakaran, Varsha; Paul, Willi; Venugopal, Karunakaran; Sujathan, K; Kumar Maiti, Kaustabh

    2015-08-15

    The extent of squaraine dye aggregation that reflects on surface enhanced Raman signal scattering (SERS) intensity upon adsorption on nano-roughened gold surface has been investigated. Here we have synthesized a serious of six squaraine dyes consisting of two different electron donor moiety i.e. 1,1,2-trimethyl-1H-benzo[e]indole and 2-methylbenzo[d]thiazole which modulates the chemisorptions and hydrophobicity being designated as SQ1, SQ2, SQ3, SQ4, SQ5 and SQ6. Interestingly, SQ2 (mono lipoic acid appended), SQ5 and SQ6 (conjugated with hexyl and dodecyl side chain) squaraine derivatives having more tendency of aggregation in DMSO-water mixed solvent showed significant increase of Raman scattering in the fingerprint region when chemisorbed on spherical gold nanoparticles. Two sets of SERS nanotags were prepared with colloidal gold nanoparticle (Au-NPs size: 40 nm) by incorporating Raman reporters SQ2 and SQ5 followed by thiolated PEG encapsulation (SH-PEG, SH-PEG-COOH) denoted as AuNPs-SQ2-PEG and AuNPs-SQ5-PEG. Further conjugation of these nanotag with monoclonal antibodies specific to over expressed receptors, EGFR and p16/Ki-67 in cervical cancer cell, HeLa showed prominent SERS mapping intensity and selectivity towards cell surface and nucleus. The fast and accurate recognition obtained by antibody triggered SERS-nanotag has been compared with conventional time consuming immunocytochemistry technique which prompted us to extend further investigation using real patient cervical smear sample for a non-invasive, ultrafast and accurate diagnosis.

  15. Aerosol particle analysis by Raman scattering technique

    SciTech Connect

    Fung, K.H.; Tang, I.N.

    1992-10-01

    Laser Raman spectroscopy is a very versatile tool for chemical characterization of micron-sized particles. Such particles are abundant in nature, and in numerous energy-related processes. In order to elucidate the formation mechanisms and understand the subsequent chemical transformation under a variety of reaction conditions, it is imperative to develop analytical measurement techniques for in situ monitoring of these suspended particles. In this report, we outline our recent work on spontaneous Raman, resonance Raman and non-linear Raman scattering as a novel technique for chemical analysis of aerosol particles as well as supersaturated solution droplets.

  16. Backward stimulated Raman scattering in water

    NASA Astrophysics Data System (ADS)

    Tcherniega, N.; Sokolovskaia, A.; Kudriavtseva, A. D.; Barille, R.; Rivoire, G.

    2000-07-01

    The backward Stimulated Raman scattering (BSRS) is studied in liquid water. We show that BSRS can be produced by small volumes of active materials. Our experimental results and calculations with different geometries and intensities of excitation allow us to choose the best experimental set-up for BSRS efficiencies. The competition with librational scattering is also observed.

  17. 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. PMID:25198903

  18. Surface-Enhanced Raman Scattering and Biophysics

    NASA Astrophysics Data System (ADS)

    Kneipp, Katrin

    2001-03-01

    Surface-enhanced Raman scattering (SERS) is a phenomenon resulting in strongly increased Raman signals from molecules which have been attached to metallic nanostructures such as colloidal silver or gold particles. The effect combines the structural information content of a vibrational spectroscopy with extremely high sensitivity and in some cases, it showes promise in overcoming the low-sensitivity problems inherent in Raman spectroscopy. Cross sections effective in SERS can reach 10 16 to 10 15 cm2 per molecule corresponding to enhancement factors of about fourteen orders of magnitude compared with “normal” non-resonant Raman scattering. Such extremely large cross sections are sufficient for single molecule Raman spectroscopy. The high sensitivity and particularly the single molecule capabilities open up exciting perspectives for SERS as tool for basic research in biophysics, biochemistry and in laboratory medicine, where it allows to study extremely small amounts of biolomedically relevant molecules in order to understand development of diseases, treatment and therapy control based on molecular structural information at the single molecule level. The most spectacular applications might appear in rapidly spectroscopic characterization of specific DNA fragments down to structurally sensitive detection of single bases in order to elucidate the human genome sequence without any labeling technology. I will briefly introduce the SERS effect and report experiments with Raman scattering of single molecules. Potential and limitations of surface-enhanced Raman techniques as a tool in biophysics and biomedical spectroscopy will be considered.

  19. 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. PMID:17663581

  20. Signal contrast in coherent Raman scattering: Optical phonons versus biomolecules

    NASA Astrophysics Data System (ADS)

    Voronin, A. A.; Zheltikov, A. M.

    2012-09-01

    We show that the limiting contrast of the coherent anti-Stokes Raman scattering (CARS) signal with respect to the coherent background due to nonresonant four-wave mixing is controlled by the Q factor of the Raman mode and is independent of the parameters of laser pulses. High-Q phonon modes of semiconductor nanoparticles, such as diamond nanoprobes, can therefore substantially enhance the contrast of CARS images, as well as the sensitivity of CARS spectroscopy and microscopy compared to typical Raman-active vibrations of organic molecules in biotissues.

  1. Influence of Raman scattering on ocean color inversion models.

    PubMed

    Westberry, Toby K; Boss, Emmanuel; Lee, Zhongping

    2013-08-01

    Raman scattering can be a significant contributor to the emergent radiance spectrum from the surface ocean. Here, we present an analytical approach to directly estimate the Raman contribution to remote sensing reflectance, and evaluate its effects on optical properties estimated from two common semianalytical inversion models. For application of the method to ocean color remote sensing, spectral irradiance products in the ultraviolet from the OMI instrument are merged with MODerate-resolution Imaging Spectroradiometer (MODIS) data in the visible. The resulting global fields of Raman-corrected optical properties show significant differences from standard retrievals, particularly for the particulate backscattering coefficient, b(bp), where average errors in clear ocean waters are ~50%. Given the interest in transforming b(bp) into biogeochemical quantities, Raman scattering must be accounted for in semianalytical inversion schemes. PMID:23913078

  2. Temperature dependence of sapphire fiber Raman scattering

    DOE PAGES

    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.

  3. Theoretical investigation on the pumping effect of stimulated Brillouin scattering on stimulated Raman scattering in water

    NASA Astrophysics Data System (ADS)

    Shi, J.; Chen, X.; Ouyang, M.; Gong, W.; Su, Y.; Liu, D.

    2012-02-01

    The pumping effect of stimulated Brillouin scattering on stimulated Raman scattering is investigated theoretically through the coupled wave equations of stimulated Brillouin scattering and stimulated Raman scattering. The numerical simulations are in agreement with the experimental results. They indicate that the backward stimulated Raman scattering is excited and amplified collectively by both pump laser and stimulated Brillouin scattering.

  4. Raman scattering studies of pollutant systems.

    NASA Technical Reports Server (NTRS)

    Schwiesow, R. L.

    1971-01-01

    Results and techniques for laboratory measurements of Raman scattering cross sections and depolarization ratios of atmospheric gases as a function of the incident photon energy are discussed. Referred to N2, the cross section of H2O changes by a factor of 2 as the incident photon energy is changed by 5%. Less striking results are obtained for SO2, NO and other atmospheric gases. Tentative results are given for spectral features of scattering from polluted air-water interfaces. Raman lidar is assessed as a potentially useful aid in remote sensing of atmospheric and water-borne pollution distributions at least in near-source concentrations.

  5. Integrated Raman and angular scattering of single biological cells

    NASA Astrophysics Data System (ADS)

    Smith, Zachary J.

    2009-12-01

    Raman, or inelastic, scattering and angle-resolved elastic scattering are two optical processes that have found wide use in the study of biological systems. Raman scattering quantitatively reports on the chemical composition of a sample by probing molecular vibrations, while elastic scattering reports on the morphology of a sample by detecting structure-induced coherent interference between incident and scattered light. We present the construction of a multimodal microscope platform capable of gathering both elastically and inelastically scattered light from a 38 mum2 region in both epi- and trans-illumination geometries. Simultaneous monitoring of elastic and inelastic scattering from a microscopic region allows noninvasive characterization of a living sample without the need for exogenous dyes or labels. A sample is illuminated either from above or below with a focused 785 nm TEM00 mode laser beam, with elastic and inelastic scattering collected by two separate measurement arms. The measurements may be made either simultaneously, if identical illumination geometries are used, or sequentially, if the two modalities utilize opposing illumination paths. In the inelastic arm, Stokes-shifted light is dispersed by a spectrograph onto a CCD array. In the elastic scattering collection arm, a relay system images the microscope's back aperture onto a CCD detector array to yield an angle-resolved elastic scattering pattern. Post-processing of the inelastic scattering to remove fluorescence signals yields high quality Raman spectra that report on the sample's chemical makeup. Comparison of the elastically scattered pupil images to generalized Lorenz-Mie theory yields estimated size distributions of scatterers within the sample. In this thesis we will present validations of the IRAM instrument through measurements performed on single beads of a few microns in size, as well as on ensembles of sub-micron particles of known size distributions. The benefits and drawbacks of the

  6. 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.

  7. 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.

  8. Nanorough gold for enhanced Raman scattering

    PubMed Central

    Kim, Jeonghwan; Kang, Kyung-Nam; Sarkar, Anirban; Malempati, Pallavi; Hah, Dooyoung; Daniels-Race, Theda; Feldman, Martin

    2013-01-01

    Conventional Raman scattering is a workhorse technique for detecting and identifying complex molecular samples. In surface enhanced Raman scattering, a nanorough metallic surface close to the sample enhances the Raman signal enormously. In this work, the surface is on a clear epoxy substrate. The epoxy is cast on a silicon wafer, using 20 nm of gold as a mold release. This single step process already produces useful enhanced Raman signals. However, the Raman signal is further enhanced by (1) depositing additional gold on the epoxy substrate and (2) by using a combination of wet and dry etches to roughen the silicon substrate before casting the epoxy. The advantage of a clear substrate is that the Raman signal may be obtained by passing light through the substrate, with opaque samples simply placed against the surface. Results were obtained with solutions of Rhodamine 6G in deionized water over a range of concentrations from 1 nM to 1 mM. In all cases, the signal to noise ratio was greater than 10:1. PMID:24353928

  9. Nonlinear kinetic modeling of stimulated Raman scattering

    NASA Astrophysics Data System (ADS)

    Benisti, Didier

    2011-10-01

    Despite its importance for many applications, such as or Raman amplification or inertial confinement fusion, deriving a nonlinear estimate of Raman reflectivity in a plasma has remained quite a challenge for decades. This is mainly due to the nonlinear modification of the electron distribution function induced by the plasma wave (EPW), which, in turn, modifies the propagation of this wave. In this paper is derived an envelope equation for the EPW valid in 3D and which accounts for the nonlinear change of its collisionless (Landau-like) damping rate, group velocity, coupling to the electromagnetic drive, frequency and wave number. Our theoretical predictions for each of these terms are carefully compared against results from Vlasov simulations of stimulated Raman scattering (SRS), as well as with other theories. Moreover, our envelope model shows to be as accurate as a Vlasov code in predicting Raman threshold in 1D. Making comparisons with experimental results nevertheless requires including transverse dimensions and letting Raman start from noise. To this end, we performed a completely new derivation of the electrostatic fluctuations in a plasma, which accounts nonlinear effects. Moreover, based on our Multi-D simulations of Raman scattering with our envelope code BRAMA, we discuss the effect on SRS of wave front bowing, transverse detrapping and of a completely new defocussing effect due to the local change in the direction of the EPW group velocity induced by the nonlinear decrease of Landau damping.

  10. Transparent material thickness measurements by Raman scattering.

    PubMed

    Pershin, Sergey M; Lednev, Vasily N; Yulmetov, Renat N; Klinkov, Vladimir K; Bunkin, Alexey F

    2015-07-01

    An efficient and simple and convenient technique for transparent samples thickness measurements by Raman spectroscopy is suggested. The elastic scattering can be effectively used for sample border indication if the refractive index changes more than 3%, while it fails to detect an ice-to-water border of floating ice. The alternative is to use Raman spectroscopy to detect the interface between different layers of transparent materials. The difference between the Raman spectra of poly methyl methacrylate (PMMA) and water, and between ice and liquid water were employed to locate the PMMA-water and ice-water interfaces, while elastic scattering was used for air-solid surface detection. This approach yields an error of 2%-5% indicating that it is promising to express a remote and noninvasive thickness measurement technique in field experiments. PMID:26193136

  11. Observation of Raman scattering by cloud droplets in the atmosphere.

    PubMed

    Melfi, S H; Evans, K D; Li, J; Whiteman, D; Ferrare, R; Schwemmer, G

    1997-05-20

    In a recent field campaign, the NASA Goddard Space Flight Center scanning Raman lidar measured, in the water vapor channel, Raman scattering from low-level clouds well in excess of 100% relative humidity. The excess scattering has been interpreted to be spontaneous Raman scattering by liquid water in the cloud droplets. A review of research on Raman scattering by microspheres indicates that the technique may provide a remote method to observe cloud liquid water. The clouds studied appear, from Mie scattering, to have two distinct layers with only the upper layer showing significant Raman scattering from liquid water in the droplets. PMID:18253375

  12. Observation of Raman scattering by cloud droplets in the atmosphere.

    PubMed

    Melfi, S H; Evans, K D; Li, J; Whiteman, D; Ferrare, R; Schwemmer, G

    1997-05-20

    In a recent field campaign, the NASA Goddard Space Flight Center scanning Raman lidar measured, in the water vapor channel, Raman scattering from low-level clouds well in excess of 100% relative humidity. The excess scattering has been interpreted to be spontaneous Raman scattering by liquid water in the cloud droplets. A review of research on Raman scattering by microspheres indicates that the technique may provide a remote method to observe cloud liquid water. The clouds studied appear, from Mie scattering, to have two distinct layers with only the upper layer showing significant Raman scattering from liquid water in the droplets.

  13. Raman scattering in the atmospheres of the major planets

    NASA Technical Reports Server (NTRS)

    Cochran, W. D.; Trafton, L. M.

    1978-01-01

    A technique is developed to calculate the detailed effects of Raman scattering in an inhomogeneous anisotropically scattering atmosphere. The technique is applied to evaluations of Raman scattering by H2 in the atmosphere of the major planets. It is noted that Raman scattering produces an insufficient decrease in the blue and ultraviolet regions to explain the albedos of all planets investigated. For all major planets, the filling-in of solar line cores and the generation of the Raman-shifted ghosts of the Fraunhofer spectrum are observed. With regard to Uranus and Neptune, Raman scattering is seen to exert a major influence on the formation and profile of strong red and near infrared CH4 bands, and Raman scattering by H2 explains the residual intensity in the cores of these bands. Raman scattering by H2 must also be taken into account in the scattering of photons into the cores of saturated absorption bands.

  14. 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.

  15. 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.

  16. Raman Reporter-Coupled Ag(core)@Au(shell) Nanostars for in Vivo Improved Surface Enhanced Raman Scattering Imaging and Near-infrared-Triggered Photothermal Therapy in Breast Cancers.

    PubMed

    Zeng, Leyong; Pan, Yuanwei; Wang, Shouju; Wang, Xin; Zhao, Xinmei; Ren, Wenzhi; Lu, Guangming; Wu, Aiguo

    2015-08-01

    Noble-metal nanomaterials were widely investigated as theranostic systems for surface enhanced Raman scattering (SERS) imaging, and also for photothermal therapy (PTT) of cancers. However, it was still a major challenge to explore multifunctional nanoprobes with high performance, high stability, and low toxicity. In this work, Raman reporter (DTTC)-coupled Agcore@Aushell nanostars (Ag@Au-DTTC) were synthesized and investigated for in vivo improved SERS imaging and near-infrared (NIR)-triggered PTT of breast cancers. By the two-step coupling of DTTC, the SERS signal was improved obviously, and the cytotoxicity of nanoparticles was also decreased by coating Au nanostars onto Ag nanoparticles. The as-prepared Ag@Au-DTTC nanostars showed high photostability and excellent photothermal performance, in which the photothermal conversion efficiency was up to 79.01% under the irradiation of an 808 nm laser. The in vitro and in vivo SERS measurements of Ag@Au-DTTC nanostars showed that the many sharp and narrow Raman peaks located at 508, 782, 844, 1135, 1242, 1331, 1464, 1510, and 1580 cm(-1) could be obviously observed in MCF-7 cells and in MCF-7 tumor-bearing nude mice, compared with that in pure DTTC. In 14-day treatments, the tumor volume of MCF-7 tumor-bearing nude mice injected with Ag@Au-DTTC nanostars and irradiated by an 808 nm laser almost disappeared. This study demonstrated that the as-prepared Ag@Au-DTTC nanostars could be excellent multifunctional agents for improved SERS imaging and NIR-triggered PTT of breast cancers with low risk. PMID:26204589

  17. Coherent Raman Scattering Microscopy in Biology and Medicine.

    PubMed

    Zhang, Chi; Zhang, Delong; Cheng, Ji-Xin

    2015-01-01

    Advancements in coherent Raman scattering (CRS) microscopy have enabled label-free visualization and analysis of functional, endogenous biomolecules in living systems. When compared with spontaneous Raman microscopy, a key advantage of CRS microscopy is the dramatic improvement in imaging speed, which gives rise to real-time vibrational imaging of live biological samples. Using molecular vibrational signatures, recently developed hyperspectral CRS microscopy has improved the readout of chemical information available from CRS images. In this article, we review recent achievements in CRS microscopy, focusing on the theory of the CRS signal-to-noise ratio, imaging speed, technical developments, and applications of CRS imaging in bioscience and clinical settings. In addition, we present possible future directions that the use of this technology may take. PMID:26514285

  18. Coherent Raman Scattering Microscopy in Biology and Medicine

    PubMed Central

    Zhang, Chi; Zhang, Delong; Cheng, Ji-Xin

    2016-01-01

    Advancements in coherent Raman scattering (CRS) microscopy have enabled label-free visualization and analysis of functional, endogenous biomolecules in living systems. When compared with spontaneous Raman microscopy, a key advantage of CRS microscopy is the dramatic improvement in imaging speed, which gives rise to real-time vibrational imaging of live biological samples. Using molecular vibrational signatures, recently developed hyperspectral CRS microscopy has improved the readout of chemical information available from CRS images. In this article, we review recent achievements in CRS microscopy, focusing on the theory of the CRS signal-to-noise ratio, imaging speed, technical developments, and applications of CRS imaging in bioscience and clinical settings. In addition, we present possible future directions that the use of this technology may take. PMID:26514285

  19. Cobalt Nanopartciles for Enhanced Raman Scattering

    NASA Astrophysics Data System (ADS)

    Dunmire, David; Romero, Danilo; Hight Walker, Angela

    2003-03-01

    Low-frequency Raman spectra of cobalt nanoparticles ( 10 nm) have been obtained. This optical characterization is supported by other methods such as TEM, AFM and SQUID magnetometry. A cryo-magnet coupled to a triple grating spectrometer enables the scattering measurements at a range of sample temperatures (4K to 300K) and magnetic field strengths (0T to 8T). Cobalt nanoparticles have a complicated phase diagram which reveals three unique crystal structures resulting in distinctive and tunable magnetic properties and a self-assembly capability well suited for building SERS-active substrates. Coating of the cobalt particles with a monolayer of gold is also being pursued to further enhance the Raman scattering signal while maintaining the unique magnetic properties of the particles.

  20. Measurement of spin coherence using Raman scattering

    NASA Astrophysics Data System (ADS)

    Sun, Z.; Delteil, A.; Faelt, S.; Imamoǧlu, A.

    2016-06-01

    Ramsey interferometry provides a natural way to determine the coherence time of most qubit systems. Recent experiments on quantum dots, however, demonstrated that dynamical nuclear spin polarization can strongly influence the measurement process, making it difficult to extract the T2* coherence time using standard optical Ramsey pulses. Here, we demonstrate an alternative method for spin coherence measurement that is based on first-order coherence of photons generated in spin-flip Raman scattering. We show that if a quantum emitter is driven by a weak monochromatic laser, Raman coherence is determined exclusively by spin coherence, allowing for a direct determination of spin T2* time. When combined with coherence measurements on Rayleigh scattered photons, our technique enables us to identify coherent and incoherent contributions to resonance fluorescence, and to minimize the latter. We verify the validity of our technique by comparing our results to those determined from Ramsey interferometry for electron and heavy-hole spins.

  1. 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.

  2. 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.

  3. Multimodal imaging of living cells with multiplex coherent anti-stokes raman scattering (CARS), third-order sum frequency generation (TSFG) and two-photon excitation fluorescence (TPEF) using a nanosecond white-light laser source.

    PubMed

    Segawa, Hiroki; Okuno, Masanari; Leproux, Philippe; Couderc, Vincent; Ozawa, Takeaki; Kano, Hideaki

    2015-01-01

    The subnanosecond "white-light laser" source has been applied to multimodal, multiphoton, and multiplex spectroscopic imaging (M(3) spectroscopic imaging) with coherent anti-Stokes Raman scattering (CARS), third-order sum frequency generation (TSFG), and two-photon excitation fluorescence (TPEF). As the proof-of-principle experiment, we performed simultaneous imaging of polystyrene beads with TSFG and TPEF. This technique is then applied to live cell imaging. Mouse L929 fibroblastic cells are clearly visualized by CARS, TSFG, and TPEF processes. M(3) spectroscopic imaging provides various and unique cellular information with different image contrast based on each multiphoton process.

  4. Multimodal imaging of living cells with multiplex coherent anti-stokes raman scattering (CARS), third-order sum frequency generation (TSFG) and two-photon excitation fluorescence (TPEF) using a nanosecond white-light laser source.

    PubMed

    Segawa, Hiroki; Okuno, Masanari; Leproux, Philippe; Couderc, Vincent; Ozawa, Takeaki; Kano, Hideaki

    2015-01-01

    The subnanosecond "white-light laser" source has been applied to multimodal, multiphoton, and multiplex spectroscopic imaging (M(3) spectroscopic imaging) with coherent anti-Stokes Raman scattering (CARS), third-order sum frequency generation (TSFG), and two-photon excitation fluorescence (TPEF). As the proof-of-principle experiment, we performed simultaneous imaging of polystyrene beads with TSFG and TPEF. This technique is then applied to live cell imaging. Mouse L929 fibroblastic cells are clearly visualized by CARS, TSFG, and TPEF processes. M(3) spectroscopic imaging provides various and unique cellular information with different image contrast based on each multiphoton process. PMID:25864673

  5. Raman imaging of extraterrestrial materials

    NASA Astrophysics Data System (ADS)

    Wang, Alian; Korotev, Randy L.; Jolliff, Bradley L.; Ling, Zongcheng

    2015-07-01

    Laser Raman Spectroscopy has been proposed and is under extensive development for surface exploration missions to planetary bodies of our Solar System. It reveals information on molecular structure and chemistry. The spatial distribution of molecular species in natural geological samples and planetary materials has significance for the geological processes by which they formed. Raman imaging is the best way to combine the molecular identification and characterization of geologic materials with their spatial distribution. This paper reports Raman imaging studies of five types of extraterrestrial materials and three terrestrial samples using a state-of-the-art Raman imaging system. The Raman spectral features of major, minor, and trace species in these samples, together with their spatial correlations revealed by these Raman imaging studies indicate the genetic relationships and the geological processes that these materials have been experienced. For robotic planetary surface exploration mission, a simple yet very useful molecular map of a sample can be generated by using line-scan or grid-scan of an in situ Raman system with tightly focused laser beam.

  6. Circularly polarized coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Upputuri, Paul Kumar; Lin, Jian; Gong, Li; Liu, Xiang-Yang; Wang, Haifeng; Huang, Zhiwei

    2013-04-15

    We demonstrate circularly polarized coherent anti-Stokes Raman scattering (CP-CARS) microscopy that significantly suppresses the nonresonant background for high-contrast vibrational imaging. Circularly polarized pump and Stokes fields with opposite handedness are used to excite CARS signal. In this case, theoretically the nonresonant CARS signal and resonant CARS signal from isotropic media will completely vanish, while the resonant CARS signal from anisotropic structures can still exist. This allows CARS imaging of anisotropic samples with enhanced resonant contrast. Furthermore, we performed CP-CARS imaging on fibroin fibers from silkworm silk, and the results confirmed its effectiveness in background suppression. PMID:23595452

  7. Raman scattering in a whispering mode optical waveguide

    DOEpatents

    Kurnit, Norman A.

    1982-01-01

    A device and method for Raman scattering in a whispering mode optical waveguide. Both a helical ribbon and cylinder are disclosed which incorporate an additional curvature .rho. p for confining the beam to increase intensity. A Raman scattering medium is disposed in the optical path of the beam as it propagates along the waveguide. Raman scattering is enhanced by the high intensities of the beam and long interaction path lengths which are achieved in a small volume.

  8. Phononic Molecules Studied by Raman Scattering

    SciTech Connect

    Lanzillotti-Kimura, N. D.; Fainstein, A.; Jusserand, B.; Lemaitre, A.

    2010-01-04

    An acoustic nanocavity can confine phonons in such a way that they act like electrons in an atom. By combining two of these phononic-atoms, it is possible to form a phononic 'molecule', with acoustic modes that are similar to the electronic states in a hydrogen molecule. We report Raman scattering experiments performed in a monolithic structure formed by a phononic molecule embedded in an optical cavity. The acoustic mode splitting becomes evident through both the amplification and change of selection rules induced by the optical cavity confinement. The results are in perfect agreement with photoelastic model simulations.

  9. Stimulated Raman scattering microscopy: an emerging tool for drug discovery.

    PubMed

    Tipping, W J; Lee, M; Serrels, A; Brunton, V G; Hulme, A N

    2016-04-21

    Optical microscopy techniques have emerged as a cornerstone of biomedical research, capable of probing the cellular functions of a vast range of substrates, whilst being minimally invasive to the cells or tissues of interest. Incorporating biological imaging into the early stages of the drug discovery process can provide invaluable information about drug activity within complex disease models. Spontaneous Raman spectroscopy has been widely used as a platform for the study of cells and their components based on chemical composition; but slow acquisition rates, poor resolution and a lack of sensitivity have hampered further development. A new generation of stimulated Raman techniques is emerging which allows the imaging of cells, tissues and organisms at faster acquisition speeds, and with greater resolution and sensitivity than previously possible. This review focuses on the development of stimulated Raman scattering (SRS), and covers the use of bioorthogonal tags to enhance sample detection, and recent applications of both spontaneous Raman and SRS as novel imaging platforms to facilitate the drug discovery process. PMID:26839248

  10. Stimulated Raman scattering microscopy: an emerging tool for drug discovery

    PubMed Central

    Tipping, W. J.; Lee, M.; Serrels, A.; Brunton, V. G.

    2016-01-01

    Optical microscopy techniques have emerged as a cornerstone of biomedical research, capable of probing the cellular functions of a vast range of substrates, whilst being minimally invasive to the cells or tissues of interest. Incorporating biological imaging into the early stages of the drug discovery process can provide invaluable information about drug activity within complex disease models. Spontaneous Raman spectroscopy has been widely used as a platform for the study of cells and their components based on chemical composition; but slow acquisition rates, poor resolution and a lack of sensitivity have hampered further development. A new generation of stimulated Raman techniques is emerging which allows the imaging of cells, tissues and organisms at faster acquisition speeds, and with greater resolution and sensitivity than previously possible. This review focuses on the development of stimulated Raman scattering (SRS), and covers the use of bioorthogonal tags to enhance sample detection, and recent applications of both spontaneous Raman and SRS as novel imaging platforms to facilitate the drug discovery process. PMID:26839248

  11. Construction of an integrated Raman- and angular-scattering microscope.

    PubMed

    Smith, Zachary J; Berger, Andrew J

    2009-04-01

    We report on the construction of a multimodal microscope platform capable of gathering both elastically and inelastically scattered light from a 38 mum(2) region in both epi- and transillumination geometries. Simultaneous monitoring of elastic and inelastic scattering from a microscopic region allows noninvasive characterization of the chemistry and morphology of a living sample without the need for exogenous dyes or labels, thus allowing measurements to be made longitudinally in time on the same sample as it evolves naturally. A sample is illuminated either from above or below with a focused 785 nm TEM(00) mode laser beam, with elastic and inelastic scattering collected by two separate measurement arms. The measurements may be made either simultaneously, if identical illumination geometries are used, or sequentially, if the two modalities utilize opposing illumination paths. In the inelastic arm, Stokes-shifted light is dispersed by a spectrograph onto a charge-coupled device (CCD) array. In the elastic scattering collection arm, a relay system images the microscope's back aperture onto a CCD array. Postprocessing of the inelastic scattering to remove fluorescence signals yields high quality Raman spectra that report on the sample's chemical makeup. Comparison of the elastically scattered pupil images to generalized Lorenz-Mie theory yields estimated size distributions of scatterers within the sample. PMID:19405678

  12. Measurement of Concentration Distribution of Hydrogen Gas Flow by Measuring the Intensity of Raman Scattering Light

    NASA Astrophysics Data System (ADS)

    Asahi, Ippei; Ninomiya, Hideki

    An experimental study to visualize and measure the concentration distribution of hydrogen gas flow using the Raman scattering was performed. A Nd:YAG laser of wavelength at 355 nm was used, and the beam pattern was transformed into a rectangle and a sheet beam was formed. The Raman scattered light was observed at a right angle with respect to the laser beam axis using a gated ICCD camera and an interference filter. Shadowgraph images were obtained at the same condition. The Raman scattering light image from atmospheric nitrogen was first acquired and the function of Raman scattering light acquisition and the background light suppression was confirmed. Next, images of the Raman scattering light image and shadowgraph of hydrogen gas discharged from a nozzle into the atmosphere were acquired. The two obtained Raman images were compared and the spatial concentration distribution of the flow of the hydrogen gas at different flow rates was calculated. This method is effective for visualizing the gas flow and measuring the concentration distribution of the Raman active molecules, such as hydrogen gas.

  13. Surface Raman scattering from effervescent magnetic peroxyborates

    NASA Astrophysics Data System (ADS)

    Walrafen, G. E.; Krishnan, P. N.; Griscom, D. L.; Munro, R.

    1982-06-01

    Surface Raman scattering using a spinning technique was investigated for solid NaBO3.4H2O and NaBO3.H2O as well as for electron bombarded peroxyborates heated for various times and at temperatures form 110-180 deg C, and for solid Na2O2 and BaO2. The Raman spectra indicate that the breakdown of peroxy groups is accompanied by the formation of trapped molecular O2. Quantitative Raman intensity data were also obtained as functions of heating time at 115 deg C for the 1556 cm-1 line from O2 and for the 890 and 705 cm-1 lines whose intensities scale with the peroxy concentration. These intensity data were treated by logistics theory, and they were found to be consistent with a second-order auto-catalyzed forward reaction dependent on the product of the peroxy and O2 concentrations, plus a first-order reverse reaction dependent only on the O2 concentration.

  14. Surface Raman scattering from effervescent magnetic peroxyborates

    NASA Astrophysics Data System (ADS)

    Walrafen, G. E.; Krishnan, P. N.; Hokmabadi, M.; Griscom, D. L.; Munro, R. G.

    1982-10-01

    Surface Raman scattering using a spinning technique was investigated for solid NaBO3ṡ4H2O and NaBO3ṡH2O, as well as for electron bombarded peroxyborates, for peroxyborates heated for various times and at temperatures for 110-180 °C, and for solid Na2O2 and BaO2. The Raman spectra indicate that the breakdown of peroxy groups is accompanied by the formation of trapped molecular O2. Quantitative Raman intensity data were also obtained as functions of heating time at 115 °C for the 1556 cm-1 line from O2 and for the 890 and 705 cm-1 lines whose intensities scale with the peroxy concentration. These intensity data were treated by logistics theory, and they were found to be consistent with a second-order autocatalyzed forward reaction dependent on the product of the peroxy and O2 concentrations, plus a first-order reverse reaction dependent only on the O2 concentration.

  15. Enhanced Raman scattering of biological molecules

    NASA Astrophysics Data System (ADS)

    Montoya, Joseph R.

    The results presented in this thesis, originate from the aspiration to develop an identification algorithm for Salmonella enterica Serovar Enteritidis (S. enterica), Escherichia coli (E. coli), Bacillus globigii ( B. globigii), and Bacillus megaterium ( B. megaterium) using "enhanced" Raman scattering. We realized our goal, with a method utilizing an immunoassay process in a spectroscopic technique, and the direct use of the enhanced spectral response due to bacterial surface elements. The enhanced Raman signal originates from Surface Enhanced Raman Scattering (SERS) and/or Morphological Dependent Resonances (MDR's). We utilized a modified Lee-Meisel colloidal production method to produce a SERS active substrate, which was applied to a SERS application for the amino acid Glycine. The comparison indicates that the SERS/FRACTAL/MDR process can produce an increase of 107 times more signal than the bulk Raman signal from Glycine. In the extension of the Glycine results, we studied the use of SERS related to S. enterica, where we have shown that the aromatic amino acid contribution from Phenylalanine, Tyrosine, and Tryptophan produces a SERS response that can be used to identify the associated SERS vibrational modes of a S. enterica one or two antibody complexes. The "fingerprint" associated with the spectral signature in conjunction with an enhanced Raman signal allows conclusions to be made: (1) about the orientation of the secondary structure on the metal; (2) whether bound/unbound antibody can be neglected; (3) whether we can lower the detection limit. We have lowered the detection limit of S. enterica to 106 bacteria/ml. We also show a profound difference between S. enterica and E. coli SERS spectra even when there exists non-specific binding on E. coli indicating a protein conformation change induced by the addition of the antigen S. enterica. We confirm TEM imagery data, indicating that the source of the aromatic amino acid SERS response is originating from

  16. 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

  17. Pumping effect of stimulated Brillouin scattering on stimulated Raman scattering in water

    NASA Astrophysics Data System (ADS)

    Liu, Dahe; Shi, Jinwei; Ouyang, Min; Chen, Xudong; Liu, Juan; He, Xingdao

    2009-09-01

    It is investigated experimentally that stimulated Raman scattering (SRS) can be enhanced by stimulated Brillouin scattering (SBS). Two physical mechanisms of these phenomena were analyzed. These phenomena show that not only the competition between SBS and SRS exists, the pumping effect of stimulated Brillouin scattering on back-stimulated Raman scattering is also a commonly existing rule regardless of the experimental conditions.

  18. Label-Free Chemical Imaging of Catalytic Solids by Coherent Anti-Stokes Raman Scattering and Synchrotron-Based Infrared Microscopy

    SciTech Connect

    Kox, M.; Domke, K; Day, J; Rago, G; Stavitski, E; Bonn, M; Weckhuysen, B

    2009-01-01

    Take a look inside: The combination of coherent anti-Stokes Raman scattering and synchrotron-based IR microscopy during the catalytic conversion of thiophene derivatives on zeolite crystals yields space- and time-resolved chemically specific information without the need for labeling (see picture). The thiophene reactant is mostly present in the center of the crystal, and the product is aligned within the straight pores of the zeolites.

  19. Sensitive Trimodal Magnetic Resonance Imaging-Surface-Enhanced Resonance Raman Scattering-Fluorescence Detection of Cancer Cells with Stable Magneto-Plasmonic Nanoprobes.

    PubMed

    Carrouée, Ambre; Allard-Vannier, Emilie; Même, Sandra; Szeremeta, Frederic; Beloeil, Jean-Claude; Chourpa, Igor

    2015-11-17

    Novel magneto-plasmonic nanoprobes were designed for multimodal diagnosis of cancer by combination of magnetic resonance imaging (MRI), surface-enhanced resonance Raman scattering (SERRS), and fluorescence emission in the very near infrared (VNIR). A controlled electrostatic assembly of silver nanoparticles (AgNPs), superparamagnetic iron oxide nanoparticles (SPIONs), VNIR dye Nile Blue (NB), and biopolymer chitosan (Chi) was used to formulate the AgIONs-Chi nanoprobes. The formulation protocol did not involve organic solvents and was rapid and efficient as confirmed by magnetic sorting. The SERRS response of the nanoprobes was very intense and constant for days. It decreased linearly upon 1000-fold dilution and was still recognizable at 0.1 nM NB concentration. After 30 days of storage, the SERRS loss was less than 30% and the hydrodynamic size of the AgIONs-Chi in PBS remained below 200 nm. The gradual decrease of the ratio SERRS/fluorescence allowed one to monitor the release of the fluorescent molecule upon long-term nanoprobe dissociation. The AgIONs-Chi exhibited 2-fold higher MRI contrast than that of commercially available SPION suspensions. Finally, the nanoprobes were actively uptaken by HeLa cancer cells and ensured trimodal MRI-SERRS-fluorescence detection of 10 μL cell inclusions in cm-sized agarose gels used here as phantom models of microtumors. The above results show that the magneto-plasmonic AgIONs-Chi are promising substrates for SERRS analysis in solution and for multimodal imaging of cancer cells. PMID:26488315

  20. Suppression of lasing by stimulated Raman scattering in microdroplets

    NASA Astrophysics Data System (ADS)

    Kwok, Alfred S.; Chang, Richard K.

    1993-10-01

    At high input-laser intensity, partial suppression of lasing by intense stimulated Raman scattering of ethanol in a 10(exp - 4) M Rhodamine 6G-doped ethanol droplet can be observed when the Raman signal overlaps with the lasing spectrum. Extra stimulated emission of the Rhodamine 6G can saturate the Rhodamine 6G lasing gain to below threshold, caused by stimulated Raman scattering of ethanol.

  1. Lidar measurements of rotational Raman and double scattering.

    PubMed

    Cohen, A; Kleiman, M; Cooney, J

    1978-06-15

    The analysis of unusually strong Raman backscattering signals from clouds shows that such signals cannot be merely related to filter on-line leakage. Theoretical calculations of Raman double scattering in an atmosphere with high optical depth values are presented, and it is shown that the Raman multiple scattering effect is not negligible. The results of the calculations are in good agreement with the experimental data.

  2. Detection of latent prints by Raman imaging

    DOEpatents

    Lewis, Linda Anne; Connatser, Raynella Magdalene; Lewis, Sr., Samuel Arthur

    2011-01-11

    The present invention relates to a method for detecting a print on a surface, the method comprising: (a) contacting the print with a Raman surface-enhancing agent to produce a Raman-enhanced print; and (b) detecting the Raman-enhanced print using a Raman spectroscopic method. The invention is particularly directed to the imaging of latent fingerprints.

  3. Raman scattering mediated by neighboring molecules

    NASA Astrophysics Data System (ADS)

    Williams, Mathew D.; Bradshaw, David S.; Andrews, David L.

    2016-05-01

    Raman scattering is most commonly associated with a change in vibrational state within individual molecules, the corresponding frequency shift in the scattered light affording a key way of identifying material structures. In theories where both matter and light are treated quantum mechanically, the fundamental scattering process is represented as the concurrent annihilation of a photon from one radiation mode and creation of another in a different mode. Developing this quantum electrodynamical formulation, the focus of the present work is on the spectroscopic consequences of electrodynamic coupling between neighboring molecules or other kinds of optical center. To encompass these nanoscale interactions, through which the molecular states evolve under the dual influence of the input light and local fields, this work identifies and determines two major mechanisms for each of which different selection rules apply. The constituent optical centers are considered to be chemically different and held in a fixed orientation with respect to each other, either as two components of a larger molecule or a molecular assembly that can undergo free rotation in a fluid medium or as parts of a larger, solid material. The two centers are considered to be separated beyond wavefunction overlap but close enough together to fall within an optical near-field limit, which leads to high inverse power dependences on their local separation. In this investigation, individual centers undergo a Stokes transition, whilst each neighbor of a different species remains in its original electronic and vibrational state. Analogous principles are applicable for the anti-Stokes case. The analysis concludes by considering the experimental consequences of applying this spectroscopic interpretation to fluid media; explicitly, the selection rules and the impact of pressure on the radiant intensity of this process.

  4. Raman scattering mediated by neighboring molecules.

    PubMed

    Williams, Mathew D; Bradshaw, David S; Andrews, David L

    2016-05-01

    Raman scattering is most commonly associated with a change in vibrational state within individual molecules, the corresponding frequency shift in the scattered light affording a key way of identifying material structures. In theories where both matter and light are treated quantum mechanically, the fundamental scattering process is represented as the concurrent annihilation of a photon from one radiation mode and creation of another in a different mode. Developing this quantum electrodynamical formulation, the focus of the present work is on the spectroscopic consequences of electrodynamic coupling between neighboring molecules or other kinds of optical center. To encompass these nanoscale interactions, through which the molecular states evolve under the dual influence of the input light and local fields, this work identifies and determines two major mechanisms for each of which different selection rules apply. The constituent optical centers are considered to be chemically different and held in a fixed orientation with respect to each other, either as two components of a larger molecule or a molecular assembly that can undergo free rotation in a fluid medium or as parts of a larger, solid material. The two centers are considered to be separated beyond wavefunction overlap but close enough together to fall within an optical near-field limit, which leads to high inverse power dependences on their local separation. In this investigation, individual centers undergo a Stokes transition, whilst each neighbor of a different species remains in its original electronic and vibrational state. Analogous principles are applicable for the anti-Stokes case. The analysis concludes by considering the experimental consequences of applying this spectroscopic interpretation to fluid media; explicitly, the selection rules and the impact of pressure on the radiant intensity of this process.

  5. Raman scattering mediated by neighboring molecules.

    PubMed

    Williams, Mathew D; Bradshaw, David S; Andrews, David L

    2016-05-01

    Raman scattering is most commonly associated with a change in vibrational state within individual molecules, the corresponding frequency shift in the scattered light affording a key way of identifying material structures. In theories where both matter and light are treated quantum mechanically, the fundamental scattering process is represented as the concurrent annihilation of a photon from one radiation mode and creation of another in a different mode. Developing this quantum electrodynamical formulation, the focus of the present work is on the spectroscopic consequences of electrodynamic coupling between neighboring molecules or other kinds of optical center. To encompass these nanoscale interactions, through which the molecular states evolve under the dual influence of the input light and local fields, this work identifies and determines two major mechanisms for each of which different selection rules apply. The constituent optical centers are considered to be chemically different and held in a fixed orientation with respect to each other, either as two components of a larger molecule or a molecular assembly that can undergo free rotation in a fluid medium or as parts of a larger, solid material. The two centers are considered to be separated beyond wavefunction overlap but close enough together to fall within an optical near-field limit, which leads to high inverse power dependences on their local separation. In this investigation, individual centers undergo a Stokes transition, whilst each neighbor of a different species remains in its original electronic and vibrational state. Analogous principles are applicable for the anti-Stokes case. The analysis concludes by considering the experimental consequences of applying this spectroscopic interpretation to fluid media; explicitly, the selection rules and the impact of pressure on the radiant intensity of this process. PMID:27155637

  6. Ultraviolet Raman scattering from persistent chemical warfare agents

    NASA Astrophysics Data System (ADS)

    Kullander, Fredrik; Wästerby, Pär.; Landström, Lars

    2016-05-01

    Laser induced Raman scattering at excitation wavelengths in the middle ultraviolet was examined using a pulsed tunable laser based spectrometer system. Droplets of chemical warfare agents, with a volume of 2 μl, were placed on a silicon surface and irradiated with sequences of laser pulses. The Raman scattering from V-series nerve agents, Tabun (GA) and Mustard gas (HD) was studied with the aim of finding the optimum parameters and the requirements for a detection system. A particular emphasis was put on V-agents that have been previously shown to yield relatively weak Raman scattering in this excitation band.

  7. Rotational Raman scattering (Ring effect) in satellite backscatter ultraviolet measurements

    NASA Astrophysics Data System (ADS)

    Cebula, Richard P.; Joiner, Joanna; Bhartia, Pawan K.; Hilsenrath, Ernest; McPeters, Richard D.; Park, Hongwoo

    1995-07-01

    A detailed radiative transfer calculation has been carried out to estimate the effects of rotational Raman scattering (RRS) on satellite measurements of backscattered ultraviolet radiation. Raman-scattered light is shifted in frequency from the incident light, which causes filling in of solar Fraunhofer lines in the observed backscattered spectrum (also known as the Ring effect). The magnitude of the rotational Raman scattering filling in is a function of wavelength, solar zenith angle, surface reflectance, surface pressure, and instrument spectral resolution. The filling in predicted by our model is found to be in agreement with observations from the Shuttle Solar Backscatter Ultraviolet Radiometer and the Nimbus-7 Solar Backscatter Ultraviolet Radiometer.

  8. Solid-state Raman image amplification

    NASA Astrophysics Data System (ADS)

    Calmes, Lonnie Kirkland

    Amplification of low-light-level optical images is important for extending the range of lidar systems that image and detect objects in the atmosphere and underwater. The use of range-gating to produce images of particular range bins is also important in minimizing the image degradation due to light that is scattered backward from aerosols, smoke, or water along the imaging path. For practical lidar systems that must be operated within sight of unprotected observers, eye safety is of the utmost importance. This dissertation describes a new type of eye-safe, range-gated lidar sensing element based on Solid-state Raman Image Amplification (SSRIA) in a solid- state optical crystal. SSRIA can amplify low-level images in the eye-safe infrared at 1.556 μm with gains up to 106 with the addition of only quantum- limited noise. The high gains from SSRIA can compensate for low quantum efficiency detectors and can reduce the need for detector cooling. The range-gate of SSRIA is controlled by the pulsewidth of the pump laser and can be as short as 30-100 cm, using pump pulses of 2-6.7 nsec FWHM. A rate equation theoretical model is derived to help in the design of short pulsed Raman lasers. A theoretical model for the quantum noise properties of SSRIA is presented. SSRIA results in higher SNR images throughout a broad range of incident light levels, in contrast to the increasing noise factor with reduced gain in image intensified CCD's. A theoretical framework for the optical resolution of SSRIA is presented and it is shown that SSRIA can produce higher resolution than ICCD's. SSRIA is also superior in rejecting unwanted sunlight background, further increasing image SNR. Lastly, SSRIA can be combined with optical pre-filtering to perform optical image processing functions such as high-pass filtering and automatic target detection/recognition. The application of this technology to underwater imaging, called Marine Raman Image Amplification (MARIA) is also discussed. MARIA

  9. Nanopillars array for surface enhanced Raman scattering

    SciTech Connect

    S.P. Chang, A; Bora, M; Nguyen, H T; Behymer, E M; Larson, C C; Britten, J A; Carter, J C; Bond, T C

    2011-04-14

    The authors present a new class of surface-enhanced Raman scattering (SERS) substrates based on lithographically-defined two-dimensional rectangular array of nanopillars. Two types of nanopillars within this class are discussed: vertical pillars and tapered pillars. For the vertical pillars, the gap between each pair of nanopillars is small enough (< 50 nm) such that highly confined plasmonic cavity resonances are supported between the pillars when light is incident upon them, and the anti-nodes of these resonances act as three-dimensional hotspots for SERS. For the tapered pillars, SERS enhancement arises from the nanofocusing effect due to the sharp tip on top. SERS experiments were carried out on these substrates using various concentrations of 1,2 bis-(4-pyridyl)-ethylene (BPE), benzenethiol (BT) monolayer and toluene vapor. The results show that SERS enhancement factor of over 0.5 x 10{sup 9} can be achieved, and BPE can be detected down to femto-molar concentration level. The results also show promising potential for the use of these substrates in environmental monitoring of gases and vapors such as volatile organic compounds.

  10. Tip-enhanced Raman scattering of bacillus subtilis spores

    NASA Astrophysics Data System (ADS)

    Rusciano, G.; Zito, G.; Pesce, G.; Sasso, A.; Isticato, R.; Ricca, E.

    2015-07-01

    Understanding of the complex interactions of molecules at biological interfaces is a fundamental issue in biochemistry, biotechnology as well as biomedicine. A plethora of biological processes are ruled by the molecular texture of cellular membrane: cellular communications, drug transportations and cellular recognition are just a few examples of such chemically-mediated processes. Tip-Enhanced Raman Scattering (TERS) is a novel, Raman-based technique which is ideally suited for this purpose. TERS relies on the combination of scanning probe microscopy and Raman spectroscopy. The basic idea is the use of a metalled tip as a sort of optical nano-antenna, which gives place to SERS effect close to the tip end. Herein, we present the application of TERS to analyze the surface of Bacillus subtilis spores. The choice of this biological systems is related to the fact that a number of reasons support the use of spores as a mucosal delivery system. The remarkable and well-documented resistance of spores to various environmental and toxic effects make them clear potentials as a novel, surface-display system. Our experimental outcomes demonstrate that TERS is able to provide a nano-scale chemical imaging of spore surface. Moreover, we demonstrate that TERS allows differentiation between wilde-type spore and genetically modified strains. These results hold promise for the characterization and optimization of spore surface for drug-delivery applications.

  11. Stimulated Raman scattering of water maser lines in astrophysical plasmas

    NASA Astrophysics Data System (ADS)

    Gangadhara, R. T.; Deguchi, Shuji; Lesch, H.

    1999-10-01

    Radiative transfer equations are derived and solved for the stimulated Raman scattering of water maser lines in the astrophysical plasmas with electrons density of about 106-107 cm-3. In stimulated Raman scattering, the energy of the water maser line is transferred to the side band modes: Stokes mode and anti-Stokes mode. The Stokes mode is easily produced by backward Raman scattering while the anti-Stokes mode is created by the interacting intersecting masers in the plasma. The intensity of the Stokes mode is higher than that of the anti-Stokes mode. These side band modes are proposed as explanation for the extreme velocity features observed in the galaxy NGC 4258. The threshold value of the brightness temperature for the Raman scattering is about 1016-1019 K, and it is satisfied in the case of NGC 4258.

  12. Raman scattering from rapid thermally annealed tungsten silicide

    NASA Technical Reports Server (NTRS)

    Kumar, Sandeep; Dasgupta, Samhita; Jackson, Howard E.; Boyd, Joseph T.

    1987-01-01

    Raman scattering as a technique for studying the formation of tungsten silicide is presented. The tungsten silicide films have been formed by rapid thermal annealing of thin tungsten films sputter deposited on silicon substrates. The Raman data are interpreted by using data from resistivity measurements, Auger and Rutherford backscattering measurements, and scanning electron microscopy.

  13. Light source for narrow and broadband coherent Raman scattering microspectroscopy.

    PubMed

    Brinkmann, Maximilian; Dobner, Sven; Fallnich, Carsten

    2015-12-01

    We present a light source that is well adapted to both narrow- and broadband coherent Raman scattering (CRS) methods. Based on a single oscillator, the light source delivers synchronized broadband pulses via supercontinuum generation and narrowband, frequency-tunable pulses via four-wave mixing in a photonic crystal fiber. Seeding the four-wave mixing with a spectrally filtered part of the supercontinuum yields high-pulse energies up to 8 nJ and the possibility of scanning a bandwidth of 2000  cm(-1) in 25 ms. All pulses are emitted with a repetition frequency of 1 MHz, which ensures efficient generation of CRS signals while avoiding significant damage of the samples. Consequently, the light source combines the performance of individual narrow- and broadband CRS light sources in one setup, thus enabling hyperspectral imaging and rapid single-resonance imaging in parallel. PMID:26625022

  14. Ponderomotive potential and backward Raman scattering in dense quantum plasmas

    SciTech Connect

    Son, S.

    2014-03-15

    The backward Raman scattering is studied in dense quantum plasmas. The coefficients in the backward Raman scattering is found to be underestimated (overestimated) in the classical theory if the excited Langmuir wave has low-wave vector (high-wave vector). The second-order quantum perturbation theory shows that the second harmonic of the ponderomotive potential arises naturally even in a single particle motion contrary to the classical prediction.

  15. Stimulated anti-Stokes Raman scattering in microdroplets.

    PubMed

    Leach, D H; Chang, R K; Acker, W P

    1992-03-15

    Stimulated anti-Stokes Raman scattering (SARS) generated by one input beam is observed from CCI(4), ethanol, and water droplets. The first-order SARS intensity is approximately 10(4) times lower than the first-order stimulated-Raman-scattering (SRS) intensity for ethanol droplets. Simultaneous detection of SARS and SRS for water droplets shows an occasional lack of correlation between the SARS and SRS spectra.

  16. Chemical monitors based on Surface-Enhanced Raman Scattering (SERS)

    SciTech Connect

    Vo-Dinh, T.; Alarie, J.P.; Sutherland, W.S.; Stokes, D.L.; Miller, G.H.

    1992-12-31

    This paper presents an overview of the development of chemical monitors using the Surface-Enhanced Raman Scattering (SERS) technique. The SERS effect is based on recent experimental observations, which have indicated enhancement of the Raman scattering efficiency by factors up to 10{sup 8} when a compound is adsorbed on rough metallic surfaces having submicron protrusions. The focus of our research efforts is on the development of SERS-active sensors and instrumentation capable of field analysis and remote sensing.

  17. Dynamic Volume Holography and Optical Information Processing by Raman Scattering

    SciTech Connect

    Dodin,I.Y.; Fisch, N.J.

    2002-09-05

    A method of producing holograms of three-dimensional optical pulses is proposed. It is shown that both the amplitude and the phase profile of three-dimensional optical pulse can be stored in dynamic perturbations of a Raman medium, such as plasma. By employing Raman scattering in a nonlinear medium, information carried by a laser pulse can be captured in the form of a slowly propagating low-frequency wave that persists for a time large compared with the pulse duration. If such a hologram is then probed with a short laser pulse, the information stored in the medium can be retrieved in a second scattered electromagnetic wave. The recording and retrieving processes can conserve robustly the pulse shape, thus enabling the recording and retrieving with fidelity of information stored in optical signals. While storing or reading the pulse structure, the optical information can be processed as an analogue or digital signal, which allows simultaneous transformation of three-dimensional continuous images or computing discrete arrays of binary data. By adjusting the phase fronts of the reference pulses, one can also perform focusing, redirecting, and other types of transformation of the output pulses.

  18. Raman Scattering of Azafullerene C48N12

    SciTech Connect

    Manaa, M R

    2004-09-22

    Raman scattering activities and Raman-active frequencies are reported for the minimum energy structure of azafullerene C{sub 48}N{sub 12} at the B3LYP/6-31G* level of theory. Analysis of the vibrational spectrum shows that the most intense IR and Raman bands are those associated with C-C vibrations, and that strong IR and Raman C-N vibrations occur below 1400 cm{sup -1}. Together with the recently reported infrared, optical absorption and x-ray spectroscopies, a complete identification of this cluster should now be feasible.

  19. Raman and surface-enhanced Raman scattering (SERS) studies of the thrombin-binding aptamer.

    PubMed

    Wu, Tsai-Chin; Vasudev, Milana; Dutta, Mitra; Stroscio, Michael A

    2013-06-01

    Surface-enhanced Raman scattering is used to study the Raman spectra and peak shifts the thrombin-binding aptamer (TBA) on substrates having two different geometries; one with a single stranded sequence and one with double stranded sequence. The Raman signals of the deoxyribonucleic acids on both substrates are enhanced and specific peaks of bases are identified. These results are highly reproducible and have promising applications in low cost nucleic acid detection.

  20. The Use of Spontaneous Raman Scattering for Hydrogen Leak Detection

    NASA Technical Reports Server (NTRS)

    Degroot, Wim A.

    1994-01-01

    A fiber optic probe has been built and demonstrated that utilizes back scattered spontaneous Raman spectroscopy to detect and identify gaseous species. The small probe, coupled to the laser and data acquisition equipment with optical fibers, has applications in gaseous leak detection and process monitoring. The probe design and data acquisition system are described. Raman scattering theory has been reviewed and the results of intensity calculations of hydrogen and nitrogen Raman scattering are given. Because the device is in its developmental stage, only preliminary experimental results are presented here. Intensity scans across the rotational-vibrational Raman lines of nitrogen and hydrogen are presented. Nitrogen at a partial pressure of 0.077 MPa was detected. Hydrogen at a partial pressure of 2 kPa approached the lower limit of detectability with the present apparatus. Potential instrument improvements that would allow more sensitive and rapid hydrogen detection are identified.

  1. On surface Raman scattering and luminescence radiation in boron carbide.

    PubMed

    Werheit, H; Filipov, V; Schwarz, U; Armbrüster, M; Leithe-Jasper, A; Tanaka, T; Shalamberidze, S O

    2010-02-01

    The discrepancy between Raman spectra of boron carbide obtained by Fourier transform Raman and conventional Raman spectrometry is systematically investigated. While at photon energies below the exciton energy (1.560 eV), Raman scattering of bulk phonons of boron carbide occurs, photon energies exceeding the fundamental absorption edge (2.09 eV) evoke additional patterns, which may essentially be attributed to luminescence or to the excitation of Raman-active processes in the surface region. The reason for this is the very high fundamental absorption in boron carbide inducing a very small penetration depth of the exciting laser radiation. Raman excitations essentially restricted to the boron carbide surface region yield spectra which considerably differ from bulk phonon ones, thus indicating structural modifications.

  2. 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

  3. Broadband stimulated Raman scattering spectroscopy by a photonic time stretcher.

    PubMed

    Saltarelli, Francesco; Kumar, Vikas; Viola, Daniele; Crisafi, Francesco; Preda, Fabrizio; Cerullo, Giulio; Polli, Dario

    2016-09-19

    Stimulated Raman scattering spectroscopy is a powerful technique for label-free molecular identification, but its broadband implementation is technically challenging. We introduce and experimentally demonstrate a novel approach based on photonic time stretch. The broadband femtosecond Stokes pulse, after interacting with the sample, is stretched by a telecom fiber to ≈15ns, mapping its spectrum in time. The signal is sampled through a fast analog-to-digital converter, providing single-shot spectra at 80-kHz rate. We demonstrate ≈10-5 sensitivity over ≈500cm-1 in the C-H region. Our results pave the way to high-speed broadband vibrational imaging for materials science and biophotonics. PMID:27661870

  4. Ocean Raman Scattering in Satellite Backscatter UV Measurements

    NASA Technical Reports Server (NTRS)

    Vasilkov, Alexander P.; Joiner, Joanna; Gleason, James; Bhartia, Pawan; Bhartia, P. K. (Technical Monitor)

    2002-01-01

    Ocean Raman scattering significantly contributes to the filling-in of solar Fraunhofer lines measured by satellite backscatter ultraviolet (buy) instruments in the cloudless atmosphere over clear ocean waters. A model accounting for this effect in buy measurements is developed and compared with observations from the Global Ozone Monitoring Experiment (GONE). The model extends existing models for ocean Raman scattering to the UV spectral range. Ocean Raman scattering radiance is propagated through the atmosphere using a concept of the Lambert equivalent reflectively and an accurate radiative transfer model for Rayleigh scattering. The model and observations can be used to evaluate laboratory measurements of pure water absorption in the UV. The good agreement between model and observations suggests that buy instruments may be useful for estimating chlorophyll content.

  5. Development and integration of Raman imaging capabilities to Sandia National Laboratories hyperspectral fluorescence imaging instrument.

    SciTech Connect

    Timlin, Jerilyn Ann; Nieman, Linda T.

    2005-11-01

    Raman spectroscopic imaging is a powerful technique for visualizing chemical differences within a variety of samples based on the interaction of a substance's molecular vibrations with laser light. While Raman imaging can provide a unique view of samples such as residual stress within silicon devices, chemical degradation, material aging, and sample heterogeneity, the Raman scattering process is often weak and thus requires very sensitive collection optics and detectors. Many commercial instruments (including ones owned here at Sandia National Laboratories) generate Raman images by raster scanning a point focused laser beam across a sample--a process which can expose a sample to extreme levels of laser light and requires lengthy acquisition times. Our previous research efforts have led to the development of a state-of-the-art two-dimensional hyperspectral imager for fluorescence imaging applications such as microarray scanning. This report details the design, integration, and characterization of a line-scan Raman imaging module added to this efficient hyperspectral fluorescence microscope. The original hyperspectral fluorescence instrument serves as the framework for excitation and sample manipulation for the Raman imaging system, while a more appropriate axial transmissive Raman imaging spectrometer and detector are utilized for collection of the Raman scatter. The result is a unique and flexible dual-modality fluorescence and Raman imaging system capable of high-speed imaging at high spatial and spectral resolutions. Care was taken throughout the design and integration process not to hinder any of the fluorescence imaging capabilities. For example, an operator can switch between the fluorescence and Raman modalities without need for extensive optical realignment. The instrument performance has been characterized and sample data is presented.

  6. Suppression of resonance Raman scattering via ground state depletion towards sub-diffraction-limited label-free microscopy.

    PubMed

    Rieger, Steffen; Fischedick, Markus; Boller, Klaus-Jochen; Fallnich, Carsten

    2016-09-01

    We report on the first experimental demonstration of the suppression of spontaneous Raman scattering via ground state depletion. The concept of Raman suppression can be used to achieve sub-diffraction-limited resolution in label-free microscopy by exploiting spatially selective signal suppression when imaging a sample with a combination of Gaussian- and donut-shaped beams and reconstructing a resolution-enhanced image from this data. Using a nanosecond pulsed laser source with an emission wavelength of 355 nm, the ground state of tris(bipyridine)ruthenium(II) molecules solved in acetonitrile was depleted and the spontaneous Raman scattering at 355 nm suppressed by nearly 50 %. Based on spectroscopic data retrieved from our experiment, we modeled the Raman image of a scattering center in order to demonstrate the applicability of this effect for superresolution Raman microscopy. PMID:27607677

  7. Suppression of resonance Raman scattering via ground state depletion towards sub-diffraction-limited label-free microscopy.

    PubMed

    Rieger, Steffen; Fischedick, Markus; Boller, Klaus-Jochen; Fallnich, Carsten

    2016-09-01

    We report on the first experimental demonstration of the suppression of spontaneous Raman scattering via ground state depletion. The concept of Raman suppression can be used to achieve sub-diffraction-limited resolution in label-free microscopy by exploiting spatially selective signal suppression when imaging a sample with a combination of Gaussian- and donut-shaped beams and reconstructing a resolution-enhanced image from this data. Using a nanosecond pulsed laser source with an emission wavelength of 355 nm, the ground state of tris(bipyridine)ruthenium(II) molecules solved in acetonitrile was depleted and the spontaneous Raman scattering at 355 nm suppressed by nearly 50 %. Based on spectroscopic data retrieved from our experiment, we modeled the Raman image of a scattering center in order to demonstrate the applicability of this effect for superresolution Raman microscopy.

  8. Spectral signatures of Raman scattering as probes of exoplanetary atmospheres

    NASA Astrophysics Data System (ADS)

    Oklopcic, Antonija; Hirata, Christopher M.; Heng, Kevin

    2016-10-01

    Raman scattering by molecules in a planetary atmosphere leaves specific spectral signatures imprinted in the reflected light and the geometric albedo spectrum of the planet. Raman-scattered light causes filling-in of absorption lines in the incident spectrum, thus producing sharp peaks in the geometric albedo. It also shifts the wavelengths of spectral features in the reflected light causing the so-called Raman ghost lines. Signatures of Raman scattering have been observed and studied in the atmospheres of planets in the Solar System. We investigate whether they could be detected in nearby exoplanets using the next-generation observational facilities. We explore which stellar types are the most promising candidates for hosting exoplanets with strong Raman features in their albedo spectra. If observed, Raman albedo peaks could be used to distinguish between clear and cloudy atmospheres -- even for atmospheres composed of heavy molecular species. Raman ghost lines, although typically much fainter than the albedo peaks, could give valuable information on the composition and the temperature of the atmosphere.

  9. Coherent Scatter Imaging Measurements

    NASA Astrophysics Data System (ADS)

    Ur Rehman, Mahboob

    In conventional radiography, anatomical information of the patients can be obtained, distinguishing different tissue types, e.g. bone and soft tissue. However, it is difficult to obtain appreciable contrast between two different types of soft tissues. Instead, coherent x-ray scattering can be utilized to obtain images which can differentiate between normal and cancerous cells of breast. An x-ray system using a conventional source and simple slot apertures was tested. Materials with scatter signatures that mimic breast cancer were buried in layers of fat of increasing thickness and imaged. The result showed that the contrast and signal to noise ratio (SNR) remained high even with added fat layers and short scan times.

  10. High-Speed Coherent Raman Fingerprint Imaging of Biological Tissues

    PubMed Central

    Camp, Charles H.; Lee, Young Jong; Heddleston, John M.; Hartshorn, Christopher M.; Hight Walker, Angela R.; Rich, Jeremy N.; Lathia, Justin D.; Cicerone, Marcus T.

    2014-01-01

    An imaging platform based on broadband coherent anti-Stokes Raman scattering (BCARS) has been developed which provides an advantageous combination of speed, sensitivity and spectral breadth. The system utilizes a configuration of laser sources that probes the entire biologically-relevant Raman window (500 cm−1 to 3500 cm−1) with high resolution (< 10 cm−1). It strongly and efficiently stimulates Raman transitions within the typically weak “fingerprint” region using intrapulse 3-colour excitation, and utilizes the nonresonant background (NRB) to heterodyne amplify weak Raman signals. We demonstrate high-speed chemical imaging in two- and three-dimensional views of healthy murine liver and pancreas tissues and interfaces between xenograft brain tumours and the surrounding healthy brain matter. PMID:25621002

  11. High-speed coherent Raman fingerprint imaging of biological tissues

    NASA Astrophysics Data System (ADS)

    Camp, Charles H., Jr.; Lee, Young Jong; Heddleston, John M.; Hartshorn, Christopher M.; Walker, Angela R. Hight; Rich, Jeremy N.; Lathia, Justin D.; Cicerone, Marcus T.

    2014-08-01

    An imaging platform based on broadband coherent anti-Stokes Raman scattering has been developed that provides an advantageous combination of speed, sensitivity and spectral breadth. The system utilizes a configuration of laser sources that probes the entire biologically relevant Raman window (500-3,500 cm-1) with high resolution (<10 cm-1). It strongly and efficiently stimulates Raman transitions within the typically weak ‘fingerprint’ region using intrapulse three-colour excitation, and utilizes the non-resonant background to heterodyne-amplify weak Raman signals. We demonstrate high-speed chemical imaging in two- and three-dimensional views of healthy murine liver and pancreas tissues as well as interfaces between xenograft brain tumours and the surrounding healthy brain matter.

  12. Raman Imaging with a Fiber-Coupled Multichannel Spectrograph

    PubMed Central

    Schmälzlin, Elmar; Moralejo, Benito; Rutowska, Monika; Monreal-Ibero, Ana; Sandin, Christer; Tarcea, Nicolae; Popp, Jürgen; Roth, Martin M.

    2014-01-01

    Until now, spatially resolved Raman Spectroscopy has required to scan a sample under investigation in a time-consuming step-by-step procedure. Here, we present a technique that allows the capture of an entire Raman image with only one single exposure. The Raman scattering arising from the sample was collected with a fiber-coupled high-performance astronomy spectrograph. The probe head consisting of an array of 20 × 20 multimode fibers was linked to the camera port of a microscope. To demonstrate the high potential of this new concept, Raman images of reference samples were recorded. Entire chemical maps were received without the need for a scanning procedure. PMID:25420149

  13. Ring-shaped backward stimulated Raman scattering driven by stimulated Brillouin scattering.

    PubMed

    Feng, Chengyong; Diels, Jean-Claude; Xu, Xiaozhen; Arissian, Ladan

    2015-06-29

    Backward stimulated Raman scattering is generated in water, pumped by pre-compressed pulses from a single-cell stimulated Brillouin scattering pulse compressor. The maximum energy efficiency of 9% is achieved by employing a circularly-polarized pump pulse at its energy of 50 mJ, around which point the backward stimulated Raman scattering also exhibits a ring-shaped profile. The correlations between spatial and temporal profiles as well as the intensities of the backward stimulated Raman and the stimulated Brillouin scattering generated from Raman cell indicate that the ring-shaped backward stimulated Raman is driven by intense stimulated Brillouin scattering. We demonstrate the latter process to be much more efficient for the backward Raman generation than the conventional process in which the laser itself pumps a backward stimulated Raman beam. It is shown that a further increase in pump energy leads to a drop in efficiency, combined with a break-up of the ring pattern of backward stimulated Raman. These effects are associated with filament generation above a certain threshold.

  14. Fiber optic direct Raman imaging system based on a hollow-core fiber bundle

    NASA Astrophysics Data System (ADS)

    Inoue, S.; Katagiri, T.; Matsuura, Y.

    2015-03-01

    A Raman imaging system which combined a hollow fiber bundle and a direct imaging technique was constructed for high-speed endoscopic Raman imaging. The hollow fiber bundle is fabricated by depositing a silver thin film on the inner surface of pre-drawn glass capillary bundle. It performs as a fiber optic probe which transmits a Raman image with high signal-to-noise ratio because the propagating light is confined into the air core inducing little light scattering. The field of view on the sample is uniformly irradiated by the excitation laser light via the probe. The back-scattered image is collected by the probe and captured directly by an image sensor. A pair of thin film tunable filters is used to select target Raman band. This imaging system enables flexible and high-speed Raman imaging of biological tissues.

  15. Raman Scattering at Plasmonic Junctions Shorted by Conductive Molecular Bridges

    SciTech Connect

    El-Khoury, Patrick Z.; Hu, Dehong; Apkarian, V. Ara; Hess, Wayne P.

    2013-04-10

    Intensity spikes in Raman scattering, accompanied by switching between line spectra and band spectra, can be assigned to shorting the junction plasmon through molecular conductive bridges. This is demonstrated through Raman trajectories recorded at a plasmonic junction formed by a gold AFM tip in contact with a silver surface coated either with biphenyl-4,4’-dithiol or biphenyl-4-thiol. The fluctuations are absent in the monothiol. In effect, the making and breaking of chemical bonds is tracked.

  16. Surface-enhanced Raman scattering (SERS) dosimeter and probe

    DOEpatents

    Vo-Dinh, Tuan

    1995-01-01

    A dosimeter and probe for measuring exposure to chemical and biological compounds is disclosed. The dosimeter or probe includes a collector which may be analyzed by surface-enhanced Raman spectroscopy. The collector comprises a surface-enhanced Raman scattering-active material having a coating applied thereto to improve the adsorption properties of the collector. The collector may also be used in automated sequential devises, in probe array devices.

  17. Remote sensing of subsurface water temperature by Raman scattering

    NASA Technical Reports Server (NTRS)

    Leonard, D. A.; Caputo, B.; Hoge, F. E.

    1979-01-01

    The application of Raman scattering to remote sensing of subsurface water temperature and salinity is considered, and both theoretical and experimental aspects of the technique are discussed. Recent experimental field measurements obtained in coastal waters and on a trans-Atlantic/Mediterranean research cruise are correlated with theoretical expectations. It is concluded that the Raman technique for remote sensing of subsurface water temperature has been brought from theoretical and laboratory stages to the point where practical utilization can now be developed.

  18. Surface-enhanced Raman scattering (SERS) dosimeter and probe

    DOEpatents

    Vo-Dinh, T.

    1995-03-21

    A dosimeter and probe for measuring exposure to chemical and biological compounds is disclosed. The dosimeter or probe includes a collector which may be analyzed by surface-enhanced Raman spectroscopy. The collector comprises a surface-enhanced Raman scattering-active material having a coating applied thereto to improve the adsorption properties of the collector. The collector may also be used in automated sequential devices, in probe array devices. 10 figures.

  19. Confocal Raman imaging of crystalline an glassy materials

    SciTech Connect

    Bradley, N.L.; Morris, M.D.

    1995-12-31

    Spatial distribution of materials components can be measured by confocal Raman imaging. We describe a confocal line-imaging system in which the spectrograph entrance slit functions as a spatial filter. The instrument uses a scanning galvanometer mirror to generate uniform intensity line illumination. A flexure mount with better than 0.1 micrometer positioning accuracy moves the sample under the fixed optical system. The Raman scatter is collected and projected along the entrance slit of an axial transmissive spectrograph. A CCD collects spatially resolved spectra.

  20. Microwave-assisted synthesis of surface-enhanced Raman scattering nanoprobes for cellular sensing.

    PubMed

    Bowey, Kristen; Tanguay, Jean-François; Sandros, Marinella G; Tabrizian, Maryam

    2014-10-01

    The fabrication of 4-mercaptobenzoic acid (4-MBA) antibody-functionalized gold nanoparticles via microwave technology for surface-enhanced Raman scattering (SERS)-based cellular nanosensing is reported. Nanoprobes were characterized by UV-vis absorbance, Raman scattering properties, and observed by TEM imaging. Results showed that microwave irradiation rapidly yielded nanoprobes with significant Raman scattering intensity and suitable stability to support antibody conjugation in under 10min. Functionalized nanoprobes demonstrated the ability to map the expression of vascular adhesion molecule-1 (VCAM-1) in human coronary artery endothelial (HCAE) cells, indicating that microwave fabrication presents a viable and rapid approach to SERS nanoprobe construction. The successful application of SERS nanoprobes to localize biomarker expression in vitro may ultimately be used for early diagnostic and preventative functions in medicine.

  1. Chemical Contribution to Surface-Enahanced Raman Scattering

    SciTech Connect

    Persson, Bo Nils J; Zhao, Ke; Zhang, Zhenyu

    2006-01-01

    We present a new mechanism for the chemical contribution to surface-enhanced Raman scattering (SERS). The theory considers the modulation of the polarizability of a metal nanocluster or a flat metal surface by the vibrational motion of an adsorbed molecule. The modulated polarization of the substrate coupled with the incident light will contribute to the Raman scattering enhancement. We show that for a metal cluster and for a flat metal surface this new chemical contribution may enhance the Raman scattering intensity by a factor of {approx} 10{sup 2} and {approx}10{sup 4}, respectively. The new SERS process is determined by the electric field parallel to the surface of the metal substrate at the molecular binding site.

  2. Spontaneous Raman Scattering Diagnostics for High-pressure Gaseous Flames

    NASA Technical Reports Server (NTRS)

    Kojima, Jun; Nguyen, Quang-Viet; Reddy, D. R. (Technical Monitor)

    2002-01-01

    A high-pressure (up to 60 atm) gaseous burner facility with optical access that provides steady, reproducible flames with high precision, and the ability to use multiple fuel/oxidizer combinations has been developed. In addition, a high-performance spontaneous Raman scattering system for use in the above facility has also been developed. Together, the two systems will be used to acquire and establish a comprehensive Raman scattering spectral database for use as a quantitative high-pressure calibration of single-shot Raman scattering measurements in high-pressure combustion systems. Using these facilities, the Raman spectra of H2-Air flames were successfully measured at pressures up to 20 atm. The spectra demonstrated clear rotational and ro-vibrational Raman features of H2, N2, and H2O. theoretical Raman spectra of pure rotational H2, vibrational H2, and vibrational N2 were calculated using a classical harmonic-oscillator model with pressure broadening effects and fitted to the data. At a gas temperature of 1889 K for a phi = 1.34 H2-Air flame, the model and the data showed good agreement, confirming a ro-vibrational equilibrium temperature.

  3. Research on chirped pulse stimulated Raman scattering in ethanol

    NASA Astrophysics Data System (ADS)

    Guo, Xiao-Yang; Zou, Xiao; Xu, Yi; Lu, Xiao-Ming; Wang, Cheng; Liu, Yan-Qi; Li, Yan-Yan; Leng, Yu-Xin; Li, Ru-Xin

    2014-11-01

    We report a generation of 10.6% conversion efficiency near 1053 nm first order Stokes pulse in stimulated Raman scattering pumped using 800 nm Ti:sapphire based femtosecond pulses that are stretched to 460 ps, obtained by use of a single pass ethonal Raman shifter. The Stokes pulse almost maintains the bandwidth of the pump and is compressed to ~10 ps using a mismatched grating-pair. The spectral characteristic of the Raman pulse is calculated and the results explain the observed transient features.

  4. Remote measurements of the atmosphere using Raman scattering.

    NASA Technical Reports Server (NTRS)

    Melfi, S. H.

    1972-01-01

    Raman optical radar measurements of the atmosphere demonstrate that the technique may be used to obtain quantitative measurements of the spatial distribution of individual atmospheric molecular trace constituents (in particular water vapor) and of the major constituents. It is shown that monitoring Raman signals from atmospheric nitrogen aids in interpreting elastic scattering measurements by eliminating attenuation effects. In general, the experimental results show good agreement with independent meteorological measurements. Finally, experimental data are utilized to estimate the Raman backscatter cross section for water vapor excited at 3471.5 A.

  5. Remote measurements of the atmosphere using Raman scattering.

    PubMed

    Melfi, S H

    1972-07-01

    The Raman optical radar measurements of the atmosphere presented demonstrate that the technique may be used to obtain quantitative measurements of the spatial distribution of individual atmospheric molecular trace constituents, in particular water vapor, as well as those of the major constituents. In addition, it is shown that monitoring Raman signals from atmospheric nitrogen aids in interpreting elastic scattering measurements by eliminating attenuation effects. In general, the experimental results show good agreement with independent meteorological measurements. Finally, experimental data are utilized to estimate the Raman backscatter cross section for water vapor excited at 3471.5 A as sigmaH(2)O/sigmaN(2) = 3.8 +/- 25%.

  6. Optically seeded stimulated Raman scattering of aqueous sulfate microdroplets

    NASA Astrophysics Data System (ADS)

    Pasternack, Louise; Fleming, James W.; Owrutsky, Jeffrey C.

    1996-07-01

    Optically seeded, stimulated Raman scattering is demonstrated for 25- mu m -radius water droplets containing sulfate. Frequency-doubled Nd:YAG laser-excited Stokes radiation from the 3450- cm -1 O-H-stretching vibration of water provides the seed for morphology-dependent stimulated Raman scattering from the nu 1 vibration of sulfate that is excited by a dye laser. Seeding enhances the otherwise weaker signal for low concentrations of the anion, thereby reducing the solute detection limit, by a method that does not require changing of the droplet composition.

  7. Oblique Raman and polariton scattering in lithium iodate

    SciTech Connect

    Falk, J.; Moshrefzadeh, R.

    1985-02-01

    The authors have predicted and measured tuning of the LO and TO oblique Raman and the oblique polariton frequencies in the 769-848 cm/sup -1/ spectral region in lithium iodate. Oblique scattering in LilO/sub 3/ is produced by coupling of A and E symmetry crystal modes. The resulting LO and TO frequencies lie between the frequencies of the contributing modes. The intensity of the scattered light observed indicates that construction of CW or quasi-CW stimulated oblique Raman and polariton oscillators are possible.

  8. Resonance electronic Raman scattering in rare earth crystals

    SciTech Connect

    Williams, G.M.

    1988-11-10

    The intensities of Raman scattering transitions between electronic energy levels of trivalent rare earth ions doped into transparent crystals were measured and compared to theory. A particle emphasis was placed on the examination of the effect of intermediate state resonances on the Raman scattering intensities. Two specific systems were studied: Ce/sup 3 +/(4f/sup 1/) in single crystals of LuPO/sub 4/ and Er/sup 3 +/(4f/sup 11/) in single crystals of ErPO/sub 4/. 134 refs., 92 figs., 33 tabs.

  9. Molecular alignment and orientation with a hybrid Raman scattering technique

    NASA Astrophysics Data System (ADS)

    Bustard, Philip J.; Lausten, R.; Sussman, Benjamin J.

    2012-11-01

    We demonstrate a scheme for the preparation of molecular alignment and angular momentum orientation using a hybrid combination of two limits of Raman scattering. First a weak, impulsive pump pulse initializes the system via the nonresonant dynamic Stark effect. Then, having overcome the influence of the vacuum fluctuations, an amplification pulse selectively enhances the initial coherences by transient stimulated Raman scattering, generating alignment and angular momentum orientation of molecular hydrogen. The amplitude and phase of the resulting coherent dynamics are experimentally probed, indicating an amplification factor of 4.5. An analytic theory is developed to model the dynamics.

  10. Theory of resonant multiphonon Raman scattering in graphene monolayers

    NASA Astrophysics Data System (ADS)

    Basko, Denis; Aleiner, Igor

    2007-03-01

    The Raman spectrum of graphene consists of distinct narrow peaks corresponding to different optical phonon branches as well as their overtones [1]. We show how the relative intensities of the overtone peaks encode information about relative strengths of different inelastic scattering processes electrons are subject to. In particular, assuming that the most important processes are electron-phonon and electron-electron scattering, it is shown that one can deduce their relative interaction strengths from the Raman spectra. [1] A. C. Ferrari et al., Phys. Rev. Lett. 97, 187401 (2006); A. Gupta et al., cond-mat/0606593; D. Graf et al., cond-mat/0607562.

  11. A fiber-laser-based stimulated Raman scattering spectral microscope

    NASA Astrophysics Data System (ADS)

    Nose, Keisuke; Ozeki, Yasuyuki; Kishi, Tatsuya; Sumimura, Kazuhiko; Kanematsu, Yasuo; Itoh, Kazuyoshi

    2013-02-01

    Stimulated Raman scattering (SRS) spectral microscopy is a powerful technique for label-free biological imaging because it allows us to distinguish chemical species with overlapping Raman bands. Here we present an SRS spectral microscope based only on fiber lasers (FL's), which offer the possibilities of downsizing and simplification of the system. A femtosecond figure-8 Er-FL at a repetition rate of 54.4 MHz is used to generate pump pulses. After amplified by an Er doped fiber amplifier, Er-FL pulses are spectrally compressed to 2-ps second harmonic pulses. For generating Stokes pulses, a femtosecond Yb-FL pulses at a repetition rate of 27.2 MHz is used. Then these lasers are synchronized by a phase locked loop, which consists of a two-photon absorption photodetector, a loop filter, a phase modulator in the Er- FL cavity, and a piezo electric transducer in the Yb-FL cavity. The intensity noise of pump pulses is reduced by the collinear balanced detection (CBD) technique based on delay-and-add fiber lines. Experimentally, we confirmed that the intensity noise level of probe pulses was close to the shot noise limit. The Stokes pulses are introduced to a wavelength tunable band pass filter (BPF), which consists of a galvanomirror scanner, a 4-f optical system, a reflection grating, and a collimator. This system is able to scan the wavenumber from 2850 cm-1 to 3100 cm-1 by tuning the BPF. We succeeded in the spectral imaging of a mixture of polystyrene beads and poly(methyl methacrylate) beads.

  12. Raman scattering and in-water ocean optical properties

    NASA Technical Reports Server (NTRS)

    Marshall, Bruce R.; Smith, Raymond C.

    1990-01-01

    Inelastic (transpectral) scattering may contribute significantly to the in-water light field. Major mechanisms for inelastic scattering include Raman scattering, which is important in clear ocean waters, and fluorescence from a variety of sources, which may be important in more turbid waters. The Raman cross section for liquid water is found to be 8.2 x 10 to the -30th sq cm/sr molecule, which is in agreement with the lower range of published values. Inelastic scattering has important ramifications for several aspects of marine biooptics, including the determination of in-water spectral absorption, the estimation of clear-water ocean optical properties, and possibly various aspects of algal photobiology.

  13. Surface-enhanced Raman scattering from AgNP-graphene-AgNP sandwiched nanostructures

    NASA Astrophysics Data System (ADS)

    Wu, Jian; Xu, Yijun; Xu, Pengyu; Pan, Zhenghui; Chen, Sheng; Shen, Qishen; Zhan, Li; Zhang, Yuegang; Ni, Weihai

    2015-10-01

    We developed a facile approach toward hybrid AgNP-graphene-AgNP sandwiched structures using self-organized monolayered AgNPs from wet chemical synthesis for the optimized enhancement of the Raman response of monolayer graphene. We demonstrate that the Raman scattering of graphene can be enhanced 530 fold in the hybrid structure. The Raman enhancement is sensitively dependent on the hybrid structure, incident angle, and excitation wavelength. A systematic simulation is performed, which well explains the enhancement mechanism. Our study indicates that the enhancement resulted from the plasmonic coupling between the AgNPs on the opposite sides of graphene. Our approach towards ideal substrates offers great potential to produce a ``hot surface'' for enhancing the Raman response of two-dimensional materials.We developed a facile approach toward hybrid AgNP-graphene-AgNP sandwiched structures using self-organized monolayered AgNPs from wet chemical synthesis for the optimized enhancement of the Raman response of monolayer graphene. We demonstrate that the Raman scattering of graphene can be enhanced 530 fold in the hybrid structure. The Raman enhancement is sensitively dependent on the hybrid structure, incident angle, and excitation wavelength. A systematic simulation is performed, which well explains the enhancement mechanism. Our study indicates that the enhancement resulted from the plasmonic coupling between the AgNPs on the opposite sides of graphene. Our approach towards ideal substrates offers great potential to produce a ``hot surface'' for enhancing the Raman response of two-dimensional materials. Electronic supplementary information (ESI) available: Additional SEM images, electric field enhancement profiles, Raman scattering spectra, and structure-dependent peak ratios. See DOI: 10.1039/c5nr04500b

  14. Raman scattering of IrTe2

    NASA Astrophysics Data System (ADS)

    Lee, Alexander; Thorsmolle, Verner; Artyukhin, Sergey; Yang, Jun; Cheong, Sang-Wook; Blumberg, Girsh

    2014-03-01

    IrTe2 presents a layered compound with a triangular lattice. It is known to exhibit a first order structural phase transition at approximately 260 K which is of a first order, corresponding to a formation of a superstructure with a period of five unit cells. Using polarized Raman spectroscopy we have studied the temperature dependence of 14 observed Raman allowed phononic modes. These phonons couple strongly to this transition and one additional first order transition at approximately 170 K. In the high-temperature phase only 3 modes are observed, while below approximately 280 K all 14 modes become visible. Below approximately 170 K only 11 modes are observed. Our results shed light on the possible mechanism driving the transitions. ACL, VKT and GB acknowledge support by NSF DMR-1104884.

  15. 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.

  16. Surface-enhanced Raman scattering (SERS) and surface-enhanced resonance Raman scattering (SERRS): a review of applications.

    PubMed

    McNay, Graeme; Eustace, David; Smith, W Ewen; Faulds, Karen; Graham, Duncan

    2011-08-01

    Surface-enhanced Raman scattering (SERS) and surface-enhanced resonance Raman scattering (SERRS) can provide positive identification of an analyte or an analyte mixture with high sensitivity and selectivity. Better understanding of the theory and advances in the understanding of the practice have led to the development of practical applications in which the unique advantages of SERS/SERRS have been used to provide effective solutions to difficult analytical problems. This review presents a basic theory and illustrates the way in which SERS/SERRS has been developed for practical use.

  17. Using Raman scattering for water areas monitoring

    NASA Astrophysics Data System (ADS)

    Timchenko, E. V.; Timchenko, P. E.; Platonov, I. A.; Tregub, N. V.; Asadova, A. A.; Mukhanova, I. M.

    2016-04-01

    The results of studies on the effects of heavy metals on aquatic plants using the method of Raman spectroscopy (RS). Introduced optical coefficient, reflecting changes in chlorophyll and carotinoids in relation to the hemicellulose under the influence of heavy metals, defined as the ratio of the intensities of the RS on the wavenumbers 1547 cm-1, 1522 cm-1 to the intensity of the line 1734 cm-1. Was monitored waters of the Samara region on the basis of this coefficient.

  18. Resonant Raman scattering background in XRF spectra of binary samples

    NASA Astrophysics Data System (ADS)

    Sánchez, Héctor Jorge; Leani, Juan José

    2015-02-01

    In x-ray fluorescence analysis, spectra present singular characteristics produced by the different scattering processes. When atoms are irradiated with incident energy lower and close to an absorption edge, scattering peaks appear due to an inelastic process known as resonant Raman scattering. In this work we present theoretical calculations of the resonant Raman scattering contributions to the background of x-ray fluorescence spectra of binary samples of current technological or biological interest. On one hand, a binary alloy of Fe with traces of Mn (Mn: 0.01%, Fe: 99.99%) was studied because of its importance in the stainless steels industries. On the second hand a pure sample of Ti with V traces (Ti: 99%, V: 1%) was analyzed due to the current relevance in medical applications. In order to perform the calculations the Shiraiwa and Fujino's model was used to calculate characteristic intensities and scattering interactions. This model makes certain assumptions and approximations to achieve the calculations, especially in the case of the geometrical conditions and the incident and take-off beams. For the binary sample studied in this work and the considered experimental conditions, the calculations show that the resonant Raman scattering background is significant under the fluorescent peak, affects the symmetry of the peaks and, depending on the concentrations, overcomes the enhancements contributions (secondary fluorescence).

  19. Nanoscale array structures suitable for surface enhanced raman scattering and methods related thereto

    DOEpatents

    Bond, Tiziana C.; Miles, Robin; Davidson, James C.; Liu, Gang Logan

    2015-07-14

    Methods for fabricating nanoscale array structures suitable for surface enhanced Raman scattering, structures thus obtained, and methods to characterize the nanoscale array structures suitable for surface enhanced Raman scattering. Nanoscale array structures may comprise nanotrees, nanorecesses and tapered nanopillars.

  20. Nanoscale array structures suitable for surface enhanced raman scattering and methods related thereto

    DOEpatents

    Bond, Tiziana C.; Miles, Robin; Davidson, James C.; Liu, Gang Logan

    2014-07-22

    Methods for fabricating nanoscale array structures suitable for surface enhanced Raman scattering, structures thus obtained, and methods to characterize the nanoscale array structures suitable for surface enhanced Raman scattering. Nanoscale array structures may comprise nanotrees, nanorecesses and tapered nanopillars.

  1. Nanoscale array structures suitable for surface enhanced raman scattering and methods related thereto

    SciTech Connect

    Bond, Tiziana C; Miles, Robin; Davidson, James; Liu, Gang Logan

    2015-11-03

    Methods for fabricating nanoscale array structures suitable for surface enhanced Raman scattering, structures thus obtained, and methods to characterize the nanoscale array structures suitable for surface enhanced Raman scattering. Nanoscale array structures may comprise nanotrees, nanorecesses and tapered nanopillars.

  2. Standoff ultraviolet raman scattering detection of trace levels of explosives.

    SciTech Connect

    Kulp, Thomas J.; Bisson, Scott E.; Reichardt, Thomas A.

    2011-10-01

    Ultraviolet (UV) Raman scattering with a 244-nm laser is evaluated for standoff detection of explosive compounds. The measured Raman scattering albedo is incorporated into a performance model that focused on standoff detection of trace levels of explosives. This model shows that detection at {approx}100 m would likely require tens of seconds, discouraging application at such ranges, and prohibiting search-mode detection, while leaving open the possibility of short-range point-and-stare detection. UV Raman spectra are also acquired for a number of anticipated background surfaces: tile, concrete, aluminum, cloth, and two different car paints (black and silver). While these spectra contained features in the same spectral range as those for TNT, we do not observe any spectra similar to that of TNT.

  3. Stimulated Raman scattering seeded by a fibre continuum

    NASA Technical Reports Server (NTRS)

    Selker, M. D.; Lawandy, N. M.

    1990-01-01

    A broadband continuum generated in a germanosilicate optical fiber has been used as a coherent seed to initiate stimulated Raman scattering in gases. The technique used is described. The results show a fivefold increase in conversion efficiency and a similar reduction in the requisite pump power.

  4. Laser scattering on an atmospheric pressure plasma jet: disentangling Rayleigh, Raman and Thomson scattering

    NASA Astrophysics Data System (ADS)

    van Gessel, A. F. H.; Carbone, E. A. D.; Bruggeman, P. J.; van der Mullen, J. J. A. M.

    2012-02-01

    Laser scattering provides a very direct method for measuring the local densities and temperatures inside a plasma. We present new experimental results of laser scattering on an argon atmospheric pressure microwave plasma jet operating in an air environment. The plasma is very small so a high spatial resolution is required to study the effect of the penetration of air molecules into the plasma. The scattering signal has three overlapping contributions: Rayleigh scattering from heavy particles, Thomson scattering from free electrons and Raman scattering from molecules. The Rayleigh scattering signal is filtered out optically with a triple grating spectrometer. The disentanglement of the Thomson and Raman signals is done with a newly designed fitting method. With a single measurement we determine profiles of the electron temperature, electron density, gas temperature, partial air pressure and the N2/O2 ratio, with a spatial resolution of 50 µm, and including absolute calibration.

  5. Coherent Raman scattering microscopy: an emerging platform for biology and medicine (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Xie, Sunney S.

    2016-03-01

    Stimulated Raman scattering (SRS) microscopy is a label-free and noninvasive imaging technique using vibration spectroscopy as the contrast mechanism. Recent advances have allowed significant improvements in sensitivity, selectivity, robustness, and cost reduction, opening a wide range of biomedical applications. In particular, it provides instant tissue examination without the need of previous histological staining, and is best suited for imaging small metabolite molecules. An overview will be given to a variety of biomedical applications of SRS microscopy.

  6. Improving sensitivity in nonlinear Raman microspectroscopy imaging and sensing

    PubMed Central

    Arora, Rajan; Petrov, Georgi I.; Liu, Jian; Yakovlev, Vladislav V.

    2011-01-01

    Nonlinear Raman microspectroscopy based on a broadband coherent anti-Stokes Raman scattering is an emerging technique for noninvasive, chemically specific, microscopic analysis of tissues and large population of cells and particles. The sensitivity of this imaging is a critical aspect of a number of the proposed biomedical application. It is shown that the incident laser power is the major parameter controlling this sensitivity. By careful optimizing the laser system, the high-quality vibrational spectra acquisition at the multi-kHz rate becomes feasible. PMID:21361677

  7. Detection of melamine on fractals of unmodified gold nanoparticles by surface-enhanced Raman scattering.

    PubMed

    Roy, Pradip Kumar; Huang, Yi-Fan; Chattopadhyay, Surojit

    2014-01-01

    A simple way of detecting melamine in raw milk is demonstrated via surface-enhanced Raman spectroscopy (SERS) using fractals of bare and nonfunctionalized ~30 nm gold nanoparticles (AuNP) distributed on a solid support. The technique demonstrates the formation of AuNP fractals, from a random distribution, upon exposure to melamine, that enhance the Raman scattering cross-section to enable detection by SERS. The agglomeration, which is pronounced at higher melamine concentrations, is demonstrated directly through imaging, and the red-shift of the plasmon absorption peak of the AuNP fractal away from 530 nm by finite difference time domain (FDTD) calculations. The agglomeration results in a strong plasmon field, shown by FDTD, over the interparticle sites that enhances the Raman scattering cross-section of melamine and ensures unambiguous detection. Limit of detection of 100 ppb could be achieved reproducibly.

  8. Laser sheet dropsizing based on two-dimensional Raman and Mie scattering

    SciTech Connect

    Malarski, Anna; Schuerer, Benedikt; Schmitz, Ingo; Zigan, Lars; Fluegel, Alexandre; Leipertz, Alfred

    2009-04-01

    The imaging and quantification of droplet sizes in sprays is a challenging task for optical scientists and engineers. Laser sheet dropsizing (LSDS) combines the two-dimensional information of two different optical processes, one that is proportional to the droplet volume and one that depends on the droplet surface, e.g., Mie scattering. Besides Mie scattering, here we use two-dimensional Raman scattering as the volume-dependent measurement technique. Two different calibration strategies are presented and discussed. Two-dimensional droplet size distributions in a spray have been validated in comparison with the results of point-resolved phase Doppler anemometry (PDA) measurements.

  9. Ring effect studies: Rayleigh scattering, including molecular parameters for rotational Raman scattering, and the Fraunhofer spectrum.

    PubMed

    Chance, K V; Spurr, R J

    1997-07-20

    Improved parameters for the description of Rayleigh scattering in air and for the detailed rotational Raman scattering component for scattering by O(2) and N(2) are presented for the wavelength range 200-1000 nm. These parameters enable more accurate calculations to be made of bulk molecular scattering and of the Ring effect for a variety of atmospheric radiative transfer and constituent retrieval applications. A solar reference spectrum with accurate absolute vacuum wavelength calibration, suitable for convolution with the rotational Raman spectrum for Ring effect calculations, has been produced at 0.01-nm resolution from several sources. It is convolved with the rotational Raman spectra of O(2) and N(2) to produce an atmospheric Ring effect source spectrum.

  10. AROTEL Temperature Retrievals Within PSC's Using Raman Scattering

    NASA Technical Reports Server (NTRS)

    Burris, John; McGee, Thomas; Hoegy, Walt; Heaps, William; Twigg, Larry; Sumnicht, Grant; Hostetler, Chris; Einaudi, Franco (Technical Monitor)

    2000-01-01

    NASA Goddard Space Flight Center's Airborne Raman Ozone Temperature Lidar (AROTEL) made temperature retrievals within Polar Stratospheric Clouds (PSCs) on several flights during the SAGE III Ozone Loss and Validation Experiment (SOLVE) campaign. The location of the PSCs was confirmed using simultaneously acquired data from the NASA Langley Aerosol lidar. Retrievals were made on flight dates 991207, 991210 and 000127 from just above the aircraft to 25 kilometers geometric altitude. Raman temperature retrievals are, to first order, insensitive to Mie interference because the Raman signals are red shifted by 2331 cm(exp -1) from the initial laser wavelength. Backscattering from clouds and aerosols is consequently not observed by the detector; however, extinction does impact the measurement and limits retrievals to optically thin clouds. Comparisons between retrievals employing Rayleigh and Raman scattering show the Raman temperatures to be significantly warmer than those employing Rayleigh scattering. Uncertainties are a function of altitude: at 25 km they were approximately 3 K. Temperature profiles could not be retrieved for optically thick clouds.

  11. Surface enhanced Raman scattering spectroscopic waveguide

    DOEpatents

    Lascola, Robert J; McWhorter, Christopher S; Murph, Simona H

    2015-04-14

    A waveguide for use with surface-enhanced Raman spectroscopy is provided that includes a base structure with an inner surface that defines a cavity and that has an axis. Multiple molecules of an analyte are capable of being located within the cavity at the same time. A base layer is located on the inner surface of the base structure. The base layer extends in an axial direction along an axial length of an excitation section. Nanoparticles are carried by the base layer and may be uniformly distributed along the entire axial length of the excitation section. A flow cell for introducing analyte and excitation light into the waveguide and a method of applying nanoparticles may also be provided.

  12. Raman Scattering in a New Carbon Material

    NASA Technical Reports Server (NTRS)

    Voronov, O. A.; Street, K. W., Jr.

    2010-01-01

    Samples of a new carbon material, Diamonite-B, were fabricated under high pressure from a commercial carbon black--identified as mixed fullerenes. The new material is neither graphite-like nor diamond-like, but exhibits electrical properties close to graphite and mechanical properties close to diamond. The use of Raman spectroscopy to investigate the vibrational dynamics of this new carbon material and to provide structural characterization of its short-, medium- and long-range order is reported. We also provide the results of investigations of these samples by high-resolution electron microscopy and X-ray diffraction. Hardness, electrical conductivity, thermal conductivity and other properties of this new material are compared with synthetic graphite-like and diamond-like materials, two other phases of synthetic bulk carbon.

  13. Stimulated Raman scattering in micrometer-sized droplets: measurements of angular scattering characteristics.

    PubMed

    Pinnick, R G; Biswas, A; Armstrong, R L; Latifi, H; Creegan, E; Srivastava, V; Fernandez, G

    1988-12-01

    Measurements of the angular scattering characteristics of elastic and stimulated Raman scattering (SRS) in single (nominal 20-microm-radius) water, ethanol, and CC1(4) droplets irradiated with 0.532-microm-wavelength radiation from a pulsed laser demonstrate that SRS is more isotropic than elastic scattering yet qualitatively mimics angularly smoothed elastic scattering patterns. The angular fine structure characteristic of the coherent elastic scattering process is lacking in SRS, regardless of whether the SRS derives from multiple orders of Stokes shifts, multiple resonances within a single Stokes shift, or single resonances within a single Stokes shift.

  14. Coherent anti-Stokes Raman scattering microscopy in a microcavity

    NASA Astrophysics Data System (ADS)

    Marrocco, Michele

    2007-06-01

    The combination of nonlinear spectroscopy and cavity QED is a stimulating field of research [see, for example, S. M. Spillane et al., Nature 415, 621 (2002)]. In this work, coherent anti-Stokes Raman scattering (CARS) taking place within a microcavity with parallel mirrors, is studied. The interest stems from the fact that CARS is a powerful nonlinear spectroscopic technique, particularly useful in imaging of microscopic samples [A. Zumbusch et al., Phys. Rev. Lett. 82, 4142 (1999)]. The theory of CARS microscopy applied to a sample placed within the microcavity is developed and the calculated CARS power in comparison with its free-space value shows the characteristic oscillation between inhibition and enhancement. If d and lambda indicate the cavity spacing and the anti-Stokes wavelength, inhibition is then found for d smaller than lambda and becomes complete only for microscope objectives operated in dry conditions. It is also found that the first enhancement at d=lambda is more relevant for microscopes with smaller numerical apertures. Higher numerical apertures, instead, reveal weaker cavity effects as a consequence of the larger collection efficiency.

  15. Achieving molecular selectivity in imaging using multiphoton Raman spectroscopy techniques

    SciTech Connect

    Holtom, Gary R. ); Thrall, Brian D. ); Chin, Beek Yoke ); Wiley, H Steven ); Colson, Steven D. )

    2000-12-01

    In the case of most imaging methods, contrast is generated either by physical properties of the sample (Differential Image Contrast, Phase Contrast), or by fluorescent labels that are localized to a particular protein or organelle. Standard Raman and infrared methods for obtaining images are based upon the intrinsic vibrational properties of molecules, and thus obviate the need for attached flurophores. Unfortunately, they have significant limitations for live-cell imaging. However, an active Raman method, called Coherent Anti-Stokes Raman Scattering (CARS), is well suited for microscopy, and provides a new means for imaging specific molecules. Vibrational imaging techniques, such as CARS, avoid problems associated with photobleaching and photo-induced toxicity often associated with the use of fluorescent labels with live cells. Because the laser configuration needed to implement CARS technology is similar to that used in other multiphoton microscopy methods, such as two -photon fluorescence and harmonic generation, it is possible to combine imaging modalities, thus generating simultaneous CARS and fluorescence images. A particularly powerful aspect of CARS microscopy is its ability to selectively image deuterated compounds, thus allowing the visualization of molecules, such as lipids, that are chemically indistinguishable from the native species.

  16. Fiber four-wave mixing source for coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Lefrancois, Simon; Fu, Dan; Holtom, Gary R; Kong, Lingjie; Wadsworth, William J; Schneider, Patrick; Herda, Robert; Zach, Armin; Sunney Xie, X; Wise, Frank W

    2012-05-15

    We present a fiber-format picosecond light source for coherent anti-Stokes Raman scattering microscopy. Pulses from a Yb-doped fiber amplifier are frequency converted by four-wave mixing (FWM) in normal-dispersion photonic crystal fiber to produce a synchronized two-color picosecond pulse train. We show that seeding the FWM process overcomes the deleterious effects of group-velocity mismatch and allows efficient conversion into narrow frequency bands. The source generates more than 160 mW of nearly transform-limited pulses tunable from 775 to 815 nm. High-quality coherent Raman images of animal tissues and cells acquired with this source are presented.

  17. Raman scattering in molecular junctions: a pseudoparticle formulation.

    PubMed

    White, Alexander J; Tretiak, Sergei; Galperin, Michael

    2014-02-12

    We present a formulation of Raman spectroscopy in molecular junctions based on a many-body state representation of the molecule. The approach goes beyond the previous effective single orbital formalism and provides a convenient way to incorporate computational methods and tools proven for equilibrium molecular spectroscopy into the realm of current carrying junctions. The presented framework is illustrated by first principle simulations of Raman response in a three-ring oligophenylene vinylene terminating in amine functional groups (OPV3) junction. The calculated shift in Stokes lines and estimate of vibrational heating by electric current agree with available experimental data. In particular, our results suggest that participation of the OPV3 cation in Raman scattering under bias may be responsible for the observed shift, and that the direction of the shift depends on renormalization of normal modes. This work is a step toward atomistic quantum ab initio modeling of the optical response of nonequilibrium electronic dynamics in molecular junctions. PMID:24447295

  18. 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.

  19. Internal multiple-scattering hole-enhanced Raman spectroscopy: improved backscattering Fourier transform Raman sampling in pharmaceutical tablets utilizing cylindrical-conical holes.

    PubMed

    Larkin, Peter J; Santangelo, Matthew; Šašiċ, Slobodan

    2012-08-01

    The benefits of Raman signal enhancement and improved measurement precision are demonstrated using 180° backscattering Fourier transform Raman (FT-Raman) spectroscopy from drilled cylindrical-conical holes within pharmaceutical tablet cores. Multiple scattering of the incident laser light within the holes results in an increased Raman signal due to the larger Raman sampling volume. This is important for overcoming typical sub-sampling issues encountered when employing FT-Raman backscattering of heterogeneous pharmaceutical tablets. Hole depth and diameter were found to be important experimental parameters and were optimized to yield the greatest signal enhancement. The FT-Raman spectra collected using backscattering from cylindrical-conical holes is compared to typical 180° backscattering from flat surfaces using tablet cores of Excedrin® and Vivarin®. Raman chemical images are used to establish a representative sampling area. We observe a three- to five-fold increase in the Raman intensity and a two-fold improvement in the measurement precision when sampling from cylindrical-conical holes rather than classic backscattering from flat tablet cores. Self-absorption effects on analyte band ratios are negligible in the fingerprint region but are more significant at the higher near-infrared (NIR) absorbances found in the C-H/O-H/-N-H stretching region. The sampling technique will facilitate developing quantitative FT-Raman methods for application to pharmaceutical tablets using the fingerprint spectral region.

  20. Raman Hyperspectral Imaging of Microfossils: Potential Pitfalls

    PubMed Central

    Olcott Marshall, Alison

    2013-01-01

    Abstract Initially, Raman spectroscopy was a specialized technique used by vibrational spectroscopists; however, due to rapid advancements in instrumentation and imaging techniques over the last few decades, Raman spectrometers are widely available at many institutions, allowing Raman spectroscopy to become a widespread analytical tool in mineralogy and other geological sciences. Hyperspectral imaging, in particular, has become popular due to the fact that Raman spectroscopy can quickly delineate crystallographic and compositional differences in 2-D and 3-D at the micron scale. Although this rapid growth of applications to the Earth sciences has provided great insight across the geological sciences, the ease of application as the instruments become increasingly automated combined with nonspecialists using this techique has resulted in the propagation of errors and misunderstandings throughout the field. For example, the literature now includes misassigned vibration modes, inappropriate spectral processing techniques, confocal depth of laser penetration incorrectly estimated into opaque crystalline solids, and a misconstrued understanding of the anisotropic nature of sp2 carbons. Key Words: Raman spectroscopy—Raman imaging—Confocal Raman spectroscopy—Disordered sp2 carbons—Hematite—Microfossils. Astrobiology 13, 920–931. PMID:24088070

  1. Time-encoded Raman scattering (TICO-Raman) with Fourier domain mode locked (FDML) lasers

    NASA Astrophysics Data System (ADS)

    Karpf, Sebastian; Eibl, Matthias; Wieser, Wolfgang; Klein, Thomas; Huber, Robert

    2015-07-01

    We present a new concept for performing stimulated Raman spectroscopy and microscopy by employing rapidly wavelength swept Fourier Domain Mode locked (FDML) lasers [1]. FDML lasers are known for fastest imaging in swept-source optical coherence tomography [2, 3]. We employ this continuous and repetitive wavelength sweep to generate broadband, high resolution stimulated Raman spectra with a new, time-encoded (TICO) concept [4]. This allows for encoding and detecting the stimulated Raman gain on the FDML laser intensity directly in time. Therefore we use actively modulated pump lasers, which are electronically synchronized to the FDML laser, in combination with a fast analog-to-digital converter (ADC) at 1.8 GSamples/s. We present hyperspectral Raman images with color-coded, molecular contrast.

  2. Hyperspectral image analysis for CARS, SRS, and Raman data

    PubMed Central

    Karuna, Arnica; Borri, Paola; Langbein, Wolfgang

    2015-01-01

    In this work, we have significantly enhanced the capabilities of the hyperspectral image analysis (HIA) first developed by Masia et al. 1 The HIA introduced a method to factorize the hyperspectral data into the product of component concentrations and spectra for quantitative analysis of the chemical composition of the sample. The enhancements shown here comprise (1) a spatial weighting to reduce the spatial variation of the spectral error, which improves the retrieval of the chemical components with significant local but small global concentrations; (2) a new selection criterion for the spectra used when applying sparse sampling2 to speed up sequential hyperspectral imaging; and (3) a filter for outliers in the data using singular value decomposition, suited e.g. to suppress motion artifacts. We demonstrate the enhancements on coherent anti‐Stokes Raman scattering, stimulated Raman scattering, and spontaneous Raman data. We provide the HIA software as executable for public use. © 2015 The Authors. Journal of Raman Spectroscopy published by John Wiley & Sons, Ltd. PMID:27478301

  3. Raman scattering with strongly coupled vibron-polaritons

    NASA Astrophysics Data System (ADS)

    Strashko, Artem; Keeling, Jonathan

    2016-08-01

    Strong coupling between cavity photons and molecular vibrations can lead to the formation of vibron-polaritons. In a recent experiment with PVAc molecules in a metal-metal microcavity [Shalabney et al., Angew. Chem., Int. Ed. 54, 7971 (2015), 10.1002/anie.201502979], such a coupling was observed to enhance the Raman scattering probability by several orders of magnitude. Inspired by this, we theoretically analyze the effect of strong photon-vibron coupling on the Raman scattering amplitude of organic molecules. This problem has recently been addressed by del Pino, Feist, and Garcia-Vidal [J. Phys. Chem. C 119, 29132 (2015), 10.1021/acs.jpcc.5b11654] using exact numerics for a small number of molecules. In this paper we derive compact analytic results for any number of molecules, also including the ultrastrong-coupling regime. Our calculations predict a division of the Raman signal into upper and lower polariton modes, with some enhancement to the lower polariton Raman amplitude due to the mode softening under strong coupling.

  4. Effect of isotopic disorder on Raman scattering spectra of crystals

    SciTech Connect

    Plekhanov, V.G.

    1995-03-01

    The first results of a quantitative study into the effect of isotopic disorder on optical phonon states, revealed as a broadening and shift of LO({Gamma}) phonon lines in second-order Raman scattering spectra of LiH{sub x}D{sub 1-x} crystals, are presented. The presence in the spectra of a local vibration at small values of x and the two-mode character of the LO{Gamma} phonons for x {le} 0.45, together with the substantial broadening of the LO({Gamma}) phonon scattering lines, suggest the presence of a considerable isotopic disorder effect, which implies unambiguously strong LO({Gamma}) phonon scattering. Additional supporting evidence comes from the disagreement of the above experimental finding with the coherent-potential-model predictions for the case of weak phonon scattering. 21 refs., 3 figs.

  5. Founding fathers of light scattering and surface-enhanced Raman scattering.

    PubMed

    Kerker, M

    1991-11-20

    One can view our comprehension of surface-enhanced Raman scattering, particularly that by colloidal dispersions of metal sols, as the merging of two traditions in light-scattering theory and practice. One of these originated with Michael Faraday's work on brilliantly colored metal sols, which was taken up by Richard Zsigmondy and then by Gustav Mie, who accounted for the colors by electromagnetic-scattering theory. The other tradition starts with John Tyndall's work with aerosols, which stimulated Lord Rayleigh's entry into the field. Lord Rayleigh was perplexed by observations made with sulfur hydrosols, which in turn were explored by C. V. Raman. Raman's extensive work in light scattering led to his subsequent discovery of the Raman effect. These two traditions were then intertwined when it was shown that the same physical effect that caused Faraday's sols to exhibit their brilliant colors was also the origin of the enhancement of Raman signals from molecules adsorbed on the metal particles that compose these sols.

  6. The Discovery of Raman Scattering in H II Regions

    NASA Astrophysics Data System (ADS)

    Dopita, Michael A.; Nicholls, David C.; Sutherland, Ralph S.; Kewley, Lisa J.; Groves, Brent A.

    2016-06-01

    We report here on the discovery of faint extended wings of Hα observed out to an apparent velocity of ˜7600 km s-1 in the Orion Nebula (M42) and in five H ii regions in the Large and the Small Magellanic Clouds. We show that these wings are caused by Raman scattering of both the O i and Si ii resonance lines and stellar continuum UV photons with H i followed by radiative decay to the H i n = 2 level. The broad wings also seen in Hβ and in Hγ result from Raman scattering of the UV continuum in the H i n = 4 and n = 5 levels, respectively. The Raman scattering fluorescence is correlated with the intensity of the narrow permitted lines of O i and Si ii. In the case of Si ii, this is explained by radiative pumping of the same 1023.7 Å resonance line involved in the Raman scattering by the Lyβ radiation field. The subsequent radiative cascade produces enhanced Si ii λλ5978.9, 6347.1, and 6371.4 Å permitted transitions. Finally, we show that in O i, radiative pumping of the 1025.76 Å resonance line by the Lyman series radiation field is also the cause of the enhancement in the permitted lines of this species lying near Hα in wavelength, but here the process is a little more complex. We argue that all these processes are active in the zone of the H ii region near the ionization front.

  7. Enhanced stimulated Raman scattering in temperature controlled liquid water

    NASA Astrophysics Data System (ADS)

    Ganot, Yuval; Shrenkel, Shmuel; Barmashenko, Boris D.; Bar, Ilana

    2014-08-01

    The dependence of single pass stimulated Raman scattering (SRS) in liquid water on temperature was investigated. Thermal self-defocusing and competition with backward stimulated Brillouin scattering were found to be the major limiting factors for forward SRS (FSRS) generation. Experiments were performed to show that water cooling reduces these factors, resulting in significant enhancement of the FSRS and leading to a maximum conversion efficiency of 35% for pump energy of 120 mJ/pulse and for water at a temperature of 4 °C. Computer simulations of the involved waves resulted in FSRS efficiencies agreeing well with the experimental ones.

  8. Enhanced Raman Scattering on In-Plane Anisotropic Layered Materials.

    PubMed

    Lin, Jingjing; Liang, Liangbo; Ling, Xi; Zhang, Shuqing; Mao, Nannan; Zhang, Na; Sumpter, Bobby G; Meunier, Vincent; Tong, Lianming; Zhang, Jin

    2015-12-16

    Surface-enhanced Raman scattering (SERS) on two-dimensional (2D) layered materials has provided a unique platform to study the chemical mechanism (CM) of the enhancement due to its natural separation from electromagnetic enhancement. The CM stems from the charge interactions between the substrate and molecules. Despite the extensive studies of the energy alignment between 2D materials and molecules, an understanding of how the electronic properties of the substrate are explicitly involved in the charge interaction is still unclear. Lately, a new group of 2D layered materials with anisotropic structures, including orthorhombic black phosphorus (BP) and triclinic rhenium disulfide (ReS2), has attracted great interest due to their unique anisotropic electrical and optical properties. Herein, we report a unique anisotropic Raman enhancement on few-layered BP and ReS2 using copper phthalocyanine (CuPc) molecules as a Raman probe, which is absent on isotropic graphene and h-BN. According to detailed Raman tensor analysis and density functional theory calculations, anisotropic charge interactions between the 2D materials and molecules are responsible for the angular dependence of the Raman enhancement. Our findings not only provide new insights into the CM process in SERS, but also open up new avenues for the exploration and application of the electronic properties of anisotropic 2D layered materials. PMID:26583533

  9. Designer Plasmonics Nanostructures Approaching Single Molecule Raman Scattering

    NASA Astrophysics Data System (ADS)

    Gordon, Reuven; Min, Qiao; Andrade, Gustavo F. S.; Brolo, Alexandre G.

    2010-03-01

    Since the early reports of single molecule Raman scattering detection using randomly roughened metal substrates [Phys. Rev. Lett. 78, 1667 - 1670 (1997), Science 21, 275(5303), 1102 - 1106 (1997)], there has been considerable interest in achieving single molecule Raman spectroscopy from fabricated nanostructures that are not random. Such designer plasmonic nanostructures have the advantages of improved control over the near-field enhancement magnitude, deterministic placement of the local-field hot-spots, optimized collection efficiency and greater reproducibility. Previously, we have created a metal nanostructures with measured 20 molecule Raman signal limit of detection [J. Phys. Chem. C 112 (39), 15098-15101, (2008)]. To achieve the desired near-field electric field enhancements, those nanostructures contained familiar elements to the plasmonic community: concentric focusing rings and subwavelength focusing tapers. Here, we will describe improved designs that have enabled us to improve those results by a factor of 6. We will also show polarization dependent studies that clearly demonstrate the plasmonic nature of the subwavelength focusing structures, including experimental polarization-resolved Raman spectroscopy maps. We are beginning statistical analysis experiments to determine if single molecule Raman is present in these nanostructures.

  10. Enhanced Raman Scattering on In-Plane Anisotropic Layered Materials.

    PubMed

    Lin, Jingjing; Liang, Liangbo; Ling, Xi; Zhang, Shuqing; Mao, Nannan; Zhang, Na; Sumpter, Bobby G; Meunier, Vincent; Tong, Lianming; Zhang, Jin

    2015-12-16

    Surface-enhanced Raman scattering (SERS) on two-dimensional (2D) layered materials has provided a unique platform to study the chemical mechanism (CM) of the enhancement due to its natural separation from electromagnetic enhancement. The CM stems from the charge interactions between the substrate and molecules. Despite the extensive studies of the energy alignment between 2D materials and molecules, an understanding of how the electronic properties of the substrate are explicitly involved in the charge interaction is still unclear. Lately, a new group of 2D layered materials with anisotropic structures, including orthorhombic black phosphorus (BP) and triclinic rhenium disulfide (ReS2), has attracted great interest due to their unique anisotropic electrical and optical properties. Herein, we report a unique anisotropic Raman enhancement on few-layered BP and ReS2 using copper phthalocyanine (CuPc) molecules as a Raman probe, which is absent on isotropic graphene and h-BN. According to detailed Raman tensor analysis and density functional theory calculations, anisotropic charge interactions between the 2D materials and molecules are responsible for the angular dependence of the Raman enhancement. Our findings not only provide new insights into the CM process in SERS, but also open up new avenues for the exploration and application of the electronic properties of anisotropic 2D layered materials.

  11. Enhanced Raman Scattering on In-plane Anisotropic Layered Materials

    DOE PAGES

    Liang, Liangbo; Meunier, Vincent; Sumpter, Bobby G.; Ling, Xi; Lin, Jingjing; Zhang, Shuqing; Mao, Nannan; Zhang, Na; Tong, Lianming; Zhang, Jin

    2015-11-19

    Surface-enhanced Raman scattering (SERS) on two-dimensional (2D) layered materials has provided a unique platform to study the chemical mechanism (CM) of the enhancement due to its natural separation from electromagnetic enhancement. The CM stems from the basic charge interactions between the substrate and molecules. Despite the extensive studies of the energy alignment between 2D materials and molecules, an understanding of how the electronic properties of the substrate are explicitly involved in the charge interaction is still unclear. Lately, a new group of 2D layered materials with anisotropic structure, including orthorhombic black phosphorus (BP) and triclinic rhenium disulphide (ReS2), has attractedmore » great interest due to their unique anisotropic electrical and optical properties. Herein, we report a unique anisotropic Raman enhancement on few-layered BP and ReS2 using copper phthalocyanine (CuPc) molecules as a Raman probe, which is absent on isotropic graphene and h-BN. According to detailed Raman tensor analysis and density functional theory calculations, anisotropic charge interactions due to the anisotropic carrier mobilities of the 2D materials are responsible for the angular dependence of the Raman enhancement. Our findings not only provide new insights into the CM process in SERS, but also open up new avenues for the exploration and application of the electronic properties of anisotropic 2D layered materials.« less

  12. Enhanced Raman Scattering on In-plane Anisotropic Layered Materials

    SciTech Connect

    Liang, Liangbo; Meunier, Vincent; Sumpter, Bobby G.; Ling, Xi; Lin, Jingjing; Zhang, Shuqing; Mao, Nannan; Zhang, Na; Tong, Lianming; Zhang, Jin

    2015-11-19

    Surface-enhanced Raman scattering (SERS) on two-dimensional (2D) layered materials has provided a unique platform to study the chemical mechanism (CM) of the enhancement due to its natural separation from electromagnetic enhancement. The CM stems from the basic charge interactions between the substrate and molecules. Despite the extensive studies of the energy alignment between 2D materials and molecules, an understanding of how the electronic properties of the substrate are explicitly involved in the charge interaction is still unclear. Lately, a new group of 2D layered materials with anisotropic structure, including orthorhombic black phosphorus (BP) and triclinic rhenium disulphide (ReS2), has attracted great interest due to their unique anisotropic electrical and optical properties. Herein, we report a unique anisotropic Raman enhancement on few-layered BP and ReS2 using copper phthalocyanine (CuPc) molecules as a Raman probe, which is absent on isotropic graphene and h-BN. According to detailed Raman tensor analysis and density functional theory calculations, anisotropic charge interactions due to the anisotropic carrier mobilities of the 2D materials are responsible for the angular dependence of the Raman enhancement. Our findings not only provide new insights into the CM process in SERS, but also open up new avenues for the exploration and application of the electronic properties of anisotropic 2D layered materials.

  13. Liquid core capillary-based Raman probe for surface-enhanced Raman scattering detection

    NASA Astrophysics Data System (ADS)

    Zhang, Zhuo; Xiao, Rui; Yang, Tianxin; Bo, Xiaochen; Wang, Shengqi

    2014-03-01

    High-sensitivity surface-enhanced Raman scattering (SERS) signal detection was achieved using a novel optical probe based on a processed capillary tube. The probe was produced by immobilizing silver nanoparticles (SNPs) in alkanethiol self-assembled monolayers on a capillary tube wall surface through a chemical coating technique. The developed probe could detect Rhodamine 6G with good sensitivity (10-9) due to enhanced interaction volume, high excitation and collection efficiency, and additional enhancement of hot nanojunctions. The proposed Raman probe provides a simple, cheap, fast, compact, and high-sensitivity SERS signal detection method for many potential applications, including chemical, biological, medical, and environmental fields.

  14. Raman scattering of few-layers MoTe2

    NASA Astrophysics Data System (ADS)

    Grzeszczyk, M.; Gołasa, K.; Zinkiewicz, M.; Nogajewski, K.; Molas, M. R.; Potemski, M.; Wysmołek, A.; Babiński, A.

    2016-06-01

    We report on room-temperature Raman scattering measurements in few-layer crystals of exfoliated molybdenum ditelluride (MoTe2) performed with the use of 632.8 nm (1.96 eV) laser light excitation. In agreement with a recent study reported by Froehlicher et al (2015 Nano Lett. 15 6481) we observe a complex structure of the out-of-plane vibrational modes ({{{A}}}1{{g}}{/{{A}}}1\\prime ), which can be explained in terms of interlayer interactions between single atomic planes of MoTe2. In the case of low-energy shear and breathing modes of rigid interlayer vibrations, it is shown that their energy evolution with the number of layers can be well reproduced within a linear chain model with only the nearest neighbor interaction taken into account. Based on this model the corresponding in-plane and out-of-plane force constants are determined. We also show that the Raman scattering in MoTe2 measured using 514.5 nm (2.41 eV) laser light excitation results in much simpler spectra. We argue that the rich structure of the out-of-plane vibrational modes observed in Raman scattering spectra excited with the use of 632.8 nm laser light results from its resonance with the electronic transition at the M point of the MoTe2 first Brillouin zone.

  15. Line-scan Raman spectroscopy for detection and imaging of explosives traces by a compact Raman spectrometer

    NASA Astrophysics Data System (ADS)

    Malka, Itamar; Bar, Ilana

    2016-02-01

    Measurements of Raman scattering spectra and of Raman maps of particles of explosives and related compounds [potassium nitrate, 2,4-dinitrotoluene (DNT), 2,4,6-trinitrotoluene (TNT) and 1,3,5-trinitro-1,3,5-triazacyclohexane (RDX)] were performed by a homebuilt compact Raman system, functioning with a 532-nm laser beam, focused as a point or line, along with full vertical binning or image readout of an intensified charge-coupled device camera. High specificity and sensitivity were obtained by line-excitation, which allowed fast detection and mapping of explosive particles with a relatively simple system.

  16. Denoising Stimulated Raman Spectroscopic Images by Total Variation Minimization

    PubMed Central

    Liao, Chien-Sheng; Choi, Joon Hee; Zhang, Delong; Chan, Stanley H.; Cheng, Ji-Xin

    2016-01-01

    High-speed coherent Raman scattering imaging is opening a new avenue to unveiling the cellular machinery by visualizing the spatio-temporal dynamics of target molecules or intracellular organelles. By extracting signals from the laser at MHz modulation frequency, current stimulated Raman scattering (SRS) microscopy has reached shot noise limited detection sensitivity. The laser-based local oscillator in SRS microscopy not only generates high levels of signal, but also delivers a large shot noise which degrades image quality and spectral fidelity. Here, we demonstrate a denoising algorithm that removes the noise in both spatial and spectral domains by total variation minimization. The signal-to-noise ratio of SRS spectroscopic images was improved by up to 57 times for diluted dimethyl sulfoxide solutions and by 15 times for biological tissues. Weak Raman peaks of target molecules originally buried in the noise were unraveled. Coupling the denoising algorithm with multivariate curve resolution allowed discrimination of fat stores from protein-rich organelles in C. elegans. Together, our method significantly improved detection sensitivity without frame averaging, which can be useful for in vivo spectroscopic imaging. PMID:26955400

  17. Enhanced Raman Microprobe Imaging of Single-Wall Carbon Nanotubes

    NASA Technical Reports Server (NTRS)

    Hadjiev, V. G.; Arepalli, S.; Nikolaev, P.; Jandl, S.; Yowell, L.

    2003-01-01

    We explore Raman microprobe capabilities to visualize single wall carbon nanotubes (SWCNTs). Although this technique is limited to a micron scale, we demonstrate that images of individual SWCNTs, bundles or their agglomerates can be generated by mapping Raman active elementary excitations. We measured the Raman response from carbon vibrations in SWCNTs excited by confocal scanning of a focused laser beam. Carbon vibrations reveal key characteristics of SWCNTs as nanotube diameter distribution (radial breathing modes, RBM, 100-300 cm(exp -1)), presence of defects and functional groups (D-mode, 1300-1350 cm(exp -1)), strain and oxidation states of SWCNTs, as well as metallic or semiconducting character of the tubes encoded in the lineshape of the G-modes at 1520-1600 cm(exp - 1). In addition, SWCNTs are highly anisotropic scatterers. The Raman response from a SWCNT is maximal for incident light polarization parallel to the tube axis and vanishing for perpendicular directions. We show that the SWCNT bundle shape or direction can be determined, with some limitations, from a set of Raman images taken at two orthogonal directions of the incident light polarization.

  18. A novel non-imaging optics based Raman spectroscopy device for transdermal blood analyte measurement

    PubMed Central

    Kong, Chae-Ryon; Barman, Ishan; Dingari, Narahara Chari; Kang, Jeon Woong; Galindo, Luis; Dasari, Ramachandra R.; Feld, Michael S.

    2011-01-01

    Due to its high chemical specificity, Raman spectroscopy has been considered to be a promising technique for non-invasive disease diagnosis. However, during Raman excitation, less than one out of a million photons undergo spontaneous Raman scattering and such weakness in Raman scattered light often require highly efficient collection of Raman scattered light for the analysis of biological tissues. We present a novel non-imaging optics based portable Raman spectroscopy instrument designed for enhanced light collection. While the instrument was demonstrated on transdermal blood glucose measurement, it can also be used for detection of other clinically relevant blood analytes such as creatinine, urea and cholesterol, as well as other tissue diagnosis applications. For enhanced light collection, a non-imaging optical element called compound hyperbolic concentrator (CHC) converts the wide angular range of scattered photons (numerical aperture (NA) of 1.0) from the tissue into a limited range of angles accommodated by the acceptance angles of the collection system (e.g., an optical fiber with NA of 0.22). A CHC enables collimation of scattered light directions to within extremely narrow range of angles while also maintaining practical physical dimensions. Such a design allows for the development of a very efficient and compact spectroscopy system for analyzing highly scattering biological tissues. Using the CHC-based portable Raman instrument in a clinical research setting, we demonstrate successful transdermal blood glucose predictions in human subjects undergoing oral glucose tolerance tests. PMID:22125761

  19. [High definition Raman microscopic imaging]. Progress report, May 1, 1992--June 30, 1993

    SciTech Connect

    Morris, M.D.

    1993-11-01

    Confocal Raman microscopy was developed and used to study molecular sulfur inclusions in glass pellets. The Raman spectrum of water was used as a noninvasive temperature probe in operating electrophoresis capillaries. A macro-scale imager was used to image water Raman scattering using 30 mW 532 nm; it can be used to map boundaries, impurity distributions, and morphological changes in polymers and ceramics. A holographic beam splitter was obtained. Surface-enhanced Raman spectra was obtained from inside zebra fish embryos as a model system. Future research plans are given.

  20. Measurements of Raman scattering in the middle ultraviolet band from persistent chemical warfare agents

    NASA Astrophysics Data System (ADS)

    Kullander, Fredrik; Landström, Lars; Lundén, Hampus; Mohammed, Abdesalam; Olofsson, Göran; Wästerby, Pär.

    2014-05-01

    The very low Raman scattering cross section and the fluorescence background limit the measuring range of Raman based instruments operating in the visible or infrared band. We are exploring if laser excitation in the middle ultraviolet (UV) band between 200 and 300 nm is useful and advantageous for detection of persistent chemical warfare agents (CWA) on various kinds of surfaces. The UV Raman scattering from tabun, mustard gas, VX and relevant simulants in the form of liquid surface contaminations has been measured using a laboratory experimental setup with a short standoff distance around 1 meter. Droplets having a volume of 1 μl were irradiated with a tunable pulsed laser swept within the middle UV band. A general trend is that the signal strength moves through an optimum when the laser excitation wavelength is swept between 240 and 300 nm. The signal from tabun reaches a maximum around 265 nm, the signal from mustard gas around 275 nm. The Raman signal from VX is comparably weak. Raman imaging by the use of a narrow bandpass UV filter is also demonstrated.

  1. Geometric effect on surface enhanced Raman scattering of nanoporous gold: Improving Raman scattering by tailoring ligament and nanopore ratios

    SciTech Connect

    Lang, X. Y.; Chen, L. Y.; Guan, P. F.; Fujita, T.; Chen, M. W.

    2009-05-25

    We have synthesized nanoporous gold (NPG) films with a nanostructure consisting of small nanopores and large gold ligaments by the combination of chemical dealloying and electroless plating. The NPG films exhibit dramatic improvement in surface enhanced Raman scattering (SERS) in comparison with the conventional NPG. The superior SERS effect of the NPG films results from the confluence effect of enhanced local surface plasmon fields and electromagnetic coupling between ligaments, as well as the weak plasmon damping with increasing gold ligament sizes.

  2. Unconventional physical mechanisms between stimulated Brillouin scattering and backward stimulated Raman scattering in liquid water

    NASA Astrophysics Data System (ADS)

    Shi, Jiulin; Liu, Juan; Li, Shujing; Xia, Jian; Liu, Jian'an; Fang, Wei; Yang, Kecheng; He, Xingdao

    2011-07-01

    In this paper, the stimulated Brillouin scattering (SBS) and the backward stimulated Raman scattering (BSRS) excited by a focused Gaussian laser in liquid water with different attenuation coefficients are investigated experimentally. Experimental results indicate that the relationships between SBS and BSRS are not merely competitive; the former has an obvious amplifying effect on the latter. Also, two different physical mechanisms were discussed in order to explain these phenomena.

  3. Multicolor stimulated Raman scattering microscopy with a rapidly tunable optical parametric oscillator.

    PubMed

    Kong, Lingjie; Ji, Minbiao; Holtom, Gary R; Fu, Dan; Freudiger, Christian W; Xie, X Sunney

    2013-01-15

    Stimulated Raman scattering (SRS) microscopy allows label-free chemical imaging based on vibrational spectroscopy. Narrowband excitation with picosecond lasers creates the highest signal levels and enables imaging speeds up to video-rate, but it sacrifices chemical specificity in samples with overlapping bands compared to broadband (multiplex) excitation. We develop a rapidly tunable picosecond optical parametric oscillator with an electro-optical tunable Lyot filter, and demonstrate multicolor SRS microscopy with synchronized line-by-line wavelength tuning to avoid spectral artifacts due to sample movement. We show sensitive imaging of three different kinds of polymer beads and live HeLa cells with moving intracellular lipid droplets.

  4. Backward stimulated Raman scattering in water and water solutions

    NASA Astrophysics Data System (ADS)

    Kudryavtseva, Anna D.; Baranov, Anatolii N.; Sokolovskaya, Albina I.; Tcherniega, Nicolaii V.; Barille, Regis; Rivoire, Genevieve

    2001-02-01

    12 Energetical and spectral characteristics of backward stimulated Raman scattering (BSRS) in water and water solutions of organic liquids (acetone, benzene, ethanol, cyclohexane) at different excitation conditions have been experimentally investigated. Maximum conversion efficiency of laser light into BSRS wave was about 40%. For picosecond range experimental results and calculations are presented showing the BSRS intensity as a function of the main experimental parameters concerning the geometry of excitation and the exciting intensity. Thus it's possible to forecast the best experimental set-up in term of BSRS efficiencies and to estimate the minimum length of water necessary to detect BSRS. Competition with other scatterings is observed. In nanosecond range simultaneously with BSRS stimulated Brillouin scattering has been excited. Possible applications are discussed.

  5. Raman scattering or fluorescence emission? Raman spectroscopy study on lime-based building and conservation materials.

    PubMed

    Kaszowska, Zofia; Malek, Kamilla; Staniszewska-Slezak, Emilia; Niedzielska, Karina

    2016-12-01

    This work presents an in-depth study on Raman spectra excited with 1064 and 532nm lasers of lime binders employed in the past as building materials and revealed today as valuable conservation materials. We focus our interest on the bands of strong intensity, which are present in the spectra of all binders acquired with laser excitation at 1064nm, but absent in the corresponding spectra acquired with laser excitation at 532nm. We suggest, that the first group of spectra represents fluorescence phenomena of unknown origin and the second true Raman scattering. In our studies, we also include two other phases of lime cycle, i.e. calcium carbonate (a few samples of calcite of various origins) and calcium oxide (quicklime) to assess how structural and chemical transformations of lime phases affect the NIR-Raman spectral profile. Furthermore, we analyse a set of carbonated limewashes and lime binders derived from old plasters to give an insight into their spectral characteristics after excitation with the 1064nm laser line. NIR-Raman micro-mapping results are also presented to reveal the spatial distribution of building materials and fluorescent species in the cross-section of plaster samples taken from a 15th century chapel. Our study shows that the Raman analysis can help identify lime-based building and conservation materials, however, a caution is advised in the interpretation of the spectra acquired using 1064nm excitation. PMID:27314909

  6. Raman scattering or fluorescence emission? Raman spectroscopy study on lime-based building and conservation materials.

    PubMed

    Kaszowska, Zofia; Malek, Kamilla; Staniszewska-Slezak, Emilia; Niedzielska, Karina

    2016-12-01

    This work presents an in-depth study on Raman spectra excited with 1064 and 532nm lasers of lime binders employed in the past as building materials and revealed today as valuable conservation materials. We focus our interest on the bands of strong intensity, which are present in the spectra of all binders acquired with laser excitation at 1064nm, but absent in the corresponding spectra acquired with laser excitation at 532nm. We suggest, that the first group of spectra represents fluorescence phenomena of unknown origin and the second true Raman scattering. In our studies, we also include two other phases of lime cycle, i.e. calcium carbonate (a few samples of calcite of various origins) and calcium oxide (quicklime) to assess how structural and chemical transformations of lime phases affect the NIR-Raman spectral profile. Furthermore, we analyse a set of carbonated limewashes and lime binders derived from old plasters to give an insight into their spectral characteristics after excitation with the 1064nm laser line. NIR-Raman micro-mapping results are also presented to reveal the spatial distribution of building materials and fluorescent species in the cross-section of plaster samples taken from a 15th century chapel. Our study shows that the Raman analysis can help identify lime-based building and conservation materials, however, a caution is advised in the interpretation of the spectra acquired using 1064nm excitation.

  7. In Situ and In Vivo Molecular Analysis by Coherent Raman Scattering Microscopy

    NASA Astrophysics Data System (ADS)

    Liao, Chien-Sheng; Cheng, Ji-Xin

    2016-06-01

    Coherent Raman scattering (CRS) microscopy is a high-speed vibrational imaging platform with the ability to visualize the chemical content of a living specimen by using molecular vibrational fingerprints. We review technical advances and biological applications of CRS microscopy. The basic theory of CRS and the state-of-the-art instrumentation of a CRS microscope are presented. We further summarize and compare the algorithms that are used to separate the Raman signal from the nonresonant background, to denoise a CRS image, and to decompose a hyperspectral CRS image into concentration maps of principal components. Important applications of single-frequency and hyperspectral CRS microscopy are highlighted. Potential directions of CRS microscopy are discussed.

  8. Supercontinuum generation for coherent anti-Stokes Raman scattering microscopy with photonic crystal fibers.

    PubMed

    Klarskov, Pernille; Isomäki, Antti; Hansen, Kim P; Andersen, Peter E

    2011-12-19

    Photonic crystal fiber (PCF) designs with two zero-dispersion wavelengths (ZDWs) are experimentally investigated in order to suggest a novel PCF for coherent anti-Stokes Raman scattering (CARS) microscopy. From our investigation, we select the optimum PCF design and demonstrate a tailored spectrum with power concentrated around the relevant wavelengths for lipid imaging (648 nm and 1027 nm). This new PCF is characterized by varying the fiber length, the average power, and the pulse width of the fs pump pulses. It was found that the selected PCF design gave a significantly improved spectral distribution compared to an existing PCF for CARS microscopy. Furthermore, the PCF is designed in a twofold symmetric structure allowing for polarization maintaining propagation. Finally, the pulse propagation is investigated numerically showing good agreement with the measured spectrum. From the numerical analysis, the nonlinear effects responsible for the spectral broadening are explained to be soliton fission processes, dispersive waves, and stimulated Raman scattering. PMID:22274252

  9. Advantages of coherent antistokes Raman scattering (CARS) in environmental monitoring

    NASA Astrophysics Data System (ADS)

    Paetzold, Ralf; Voss, Eberhard; de Vries, Thorsten; Darpel, H.; Anders, Angelika

    1999-09-01

    The objective of this investigation was to develop a fast method for the in-situ characterization of chemicals solved in water based on Coherent Antistokes Raman Scattering (CARS). In order to test the potential of CARS as a tool for the in-situ spectroscopy scanning and multiplex CARS techniques were investigated. Polarization CARS (PCARS) was used to reduce the nonvibrational resonant signal generated by the electron cloud of the solvent molecules. The spectra of some alcohols and pollutants such as pyridine, nitrate and sulfate were investigated. Computer simulations were applied for the evaluation of the CARS spectra. The most evident advantage of CARS in comparison with other Raman methods is the very short time to achieve a spectrum. The shortest time to get a spectrum is limited by the length of the laser pulse (e.g. 5 ns). In addition no sample preparation is necessary.

  10. Vibronic Raman Scattering at the Quantum Limit of Plasmons

    SciTech Connect

    El-Khoury, Patrick Z.; Hess, Wayne P.

    2014-07-09

    We record sequences of Raman spectra at a plasmonic junction formed by a gold AFM tip in contact with a silver surface coated with 4,4’-dimercaptostilbene (DMS). A 2D correlation analysis of the recorded trajectories reveals that the observable vibrational states can be divided into sub-sets. The first set comprises the totally symmetric vibrations of DMS (ag) that are neither correlated with each other nor to the fluctuating background, which is assigned to the signature of charge transfer plasmons tunneling through DMS. The second set consists of bu vibrations, which are correlated both with each other and with the continuum. Our findings are rationalized on the basis of the charge-transfer theory of Raman scattering, and illustrate how the tunneling plasmons modulate the vibronic coupling term from which the intensities of the bu states are derived.

  11. Complete analytic anharmonic hyper-Raman scattering spectra.

    PubMed

    Cornaton, Yann; Ringholm, Magnus; Ruud, Kenneth

    2016-08-10

    We present the first computational treatment of the complete second-order vibrational perturbation theory applied to hyper-Raman scattering spectroscopy. The required molecular properties are calculated in a fully analytic manner using a recently developed program [Ringholm, Jonsson and Ruud, J. Comp. Chem., 2014, 35, 622] that utilizes recursive routines. For some of the properties, these calculations are the first analytic calculations of their kind at their respective levels of theory. We apply this approach to the calculation of the hyper-Raman spectra of methane, ethane and ethylene and compare these to available experimental data. We show that the anharmonic corrections have a larger effect on the vibrational frequencies than on the spectral intensities, but that the inclusion of combination and overtone bands in the anharmonic treatment can improve the agreement with the experimental data, although the quality of available experimental data limits a detailed comparison. PMID:27459194

  12. Determination of nicotine by surface-enhanced Raman scattering (SERS)

    SciTech Connect

    Barber, T.E.; List, M.S.; Haas, J.W. III; Wachter, E.A. )

    1994-11-01

    The analytical application of surface-enhanced Raman spectroscopy (SERS) to the determination of nicotine is demonstrated. A simple spectroelectrochemical method using a copper or silver electrode as the SERS substrate has been developed, consisting of three steps: polishing a working electrode to a mirror finish; roughening the electrode in an electrolyte solution; and, finally, depositing the nicotine analyte onto the roughened electrode after immersion in a sample solution. During the reduction cycle, a large enhancement in nicotine Raman scattering is observed at the electrode surface. The intensity of the SERS signal on a silver electrode is linear with concentration from 10 to 900 ppb, with an estimated detection limit of 7 ppb. The total analysis time per sample is approximately five minutes. This procedure has been used to analyze the extract from a cigarette side-stream smoke sample (environmental tobacco smoke); the SERS results agree well with those of conventional gas chromatographic analysis.

  13. Raman scattering characterization of space solar cell structures

    NASA Technical Reports Server (NTRS)

    Mintairov, Alexander M.; Khvostikov, V. P.; Paleeva, E. V.; Sorokina, S. V.

    1995-01-01

    A contactless method for the determination of the free-carrier density and the composition distribution across the thickness of 3-5 multi-layer solar cell structures, using the Raman scattering method, is developed. The method includes a step analysis of Raman spectra from optical phonons and phonon-plasmon modes of different layers. The method provides simultaneous measurements of the element composition and the thickness of the structure's layers together with the free-carrier density. The results of measurements of the free-carrier density composition distributions of the liquid phase epitaxy grown AlGaAs/GaAs and GaSb solar cell structures are presented and discussed.

  14. Resonant electronic Raman scattering: A BCS-like system

    NASA Astrophysics Data System (ADS)

    Rodrigues, Leonarde N.; Arantes, A.; Schüller, C.; Bell, M. J. V.; Anjos, V.

    2016-05-01

    In this paper we investigate the resonant intersubband Raman scattering of two-dimensional electron systems in GaAs-AlGaAs single quantum wells. Self-consistent calculations of the polarized and depolarized Raman cross sections show that the appearance of excitations at the unrenormalized single-particle energy are related to three factors: the extreme resonance regime, the existence of degeneracy in intersubband excitations of the electron gas, and, finally, degeneracy in the interactions between pairs of excitations. It is demonstrated that the physics that governs the problem is similar to the one that gives rise to the formation of the superconducting state in the BCS theory of normal metals. Comparison between experiment and theory shows an excellent agreement.

  15. Smart surface-enhanced Raman scattering traceable drug delivery systems.

    PubMed

    Liu, Lei; Tang, Yonghong; Dai, Sheng; Kleitz, Freddy; Qiao, Shi Zhang

    2016-07-01

    A novel smart nanoparticle-based system has been developed for tracking intracellular drug delivery through surface-enhanced Raman scattering (SERS). This new drug delivery system (DDS) shows targeted cytotoxicity towards cancer cells via pH-cleavable covalent carboxylic hydrazone links and the SERS tracing capability based on gold@silica nanocarriers. Doxorubicin, as a model anticancer drug, was employed to compare SERS with conventional fluorescence tracing approaches. It is evident that SERS demonstrates higher sensitivity and resolution, revealing intracellular details, as the strengths of the original Raman signals can be amplified by SERS. Importantly, non-destructive SERS will provide the designed DDS with great autonomy and potential to study the dynamic procedures of non-fluorescent drug delivery into living cells. PMID:27297745

  16. Smart surface-enhanced Raman scattering traceable drug delivery systems

    NASA Astrophysics Data System (ADS)

    Liu, Lei; Tang, Yonghong; Dai, Sheng; Kleitz, Freddy; Qiao, Shi Zhang

    2016-06-01

    A novel smart nanoparticle-based system has been developed for tracking intracellular drug delivery through surface-enhanced Raman scattering (SERS). This new drug delivery system (DDS) shows targeted cytotoxicity towards cancer cells via pH-cleavable covalent carboxylic hydrazone links and the SERS tracing capability based on gold@silica nanocarriers. Doxorubicin, as a model anticancer drug, was employed to compare SERS with conventional fluorescence tracing approaches. It is evident that SERS demonstrates higher sensitivity and resolution, revealing intracellular details, as the strengths of the original Raman signals can be amplified by SERS. Importantly, non-destructive SERS will provide the designed DDS with great autonomy and potential to study the dynamic procedures of non-fluorescent drug delivery into living cells.A novel smart nanoparticle-based system has been developed for tracking intracellular drug delivery through surface-enhanced Raman scattering (SERS). This new drug delivery system (DDS) shows targeted cytotoxicity towards cancer cells via pH-cleavable covalent carboxylic hydrazone links and the SERS tracing capability based on gold@silica nanocarriers. Doxorubicin, as a model anticancer drug, was employed to compare SERS with conventional fluorescence tracing approaches. It is evident that SERS demonstrates higher sensitivity and resolution, revealing intracellular details, as the strengths of the original Raman signals can be amplified by SERS. Importantly, non-destructive SERS will provide the designed DDS with great autonomy and potential to study the dynamic procedures of non-fluorescent drug delivery into living cells. Electronic supplementary information (ESI) available. See DOI: 10.1039/c6nr03869g

  17. Stimulated Raman scattering of laser dye mixtures dissolved in multiple scattering media

    SciTech Connect

    Yashchuk, V P; Komyshan, A O; Tikhonov, E A; Olkhovyk, L A

    2014-10-31

    Stimulated Raman scattering (SRS) of a mixture of rhodamine 6G and pyrromethene 605 laser dyes in vesicular films is studied. It is shown that a peculiar interaction of dyes occurs under conditions of multiple scattering of light from vesicles. This interaction manifests itself as SRS excitation of one of the dyes by random lasing of the other dye, provided that the random lasing spectrum overlaps the Stokes lines of the first dye. In addition, there is energy transfer between molecules of these dyes if their luminescence and absorption spectra overlap. The results obtained confirm that the mechanism of SRS from laser dyes in multiple scattering media is similar to that in coherent-active Raman spectroscopy. These results extend the possibility of determining the vibrational spectrum of dye molecules from their secondary radiation in these media. (nonlinear optical phenomena)

  18. Simultaneous stimulated Raman, Brillouin, and electron-acoustic scattering reveals a potential saturation mechanism in Raman plasma amplifiers

    SciTech Connect

    Turnbull, D.; Li, S.; Morozov, A.; Suckewer, S.

    2012-08-15

    In a Raman plasma amplifier, the aim is to create plasma conditions in which Raman backscattering is the fastest growing instability, outrunning all competing effects so that it is possible to amplify and compress a laser beam to unprecedented unfocused intensities by utilizing that instability. However, achieving high efficiencies via this scheme has proven very difficult experimentally. Recent data show the simultaneous occurrence of stimulated Raman scattering (SRS), stimulated Brillouin scattering (SBS), and stimulated electron-acoustic scattering (SEAS). The appearance of SEAS is indicative of strong particle trapping, the existence of which is hard to justify without highlighting the interplay between SRS and SBS.

  19. Kinetic Enhancement of Raman Backscatter, and Electron Acoustic Thomson Scatter

    SciTech Connect

    Strozzi, D J; Williams, E A; Langdon, A B; Bers, A

    2006-09-01

    1-D Eulerian Vlasov-Maxwell simulations are presented which show kinetic enhancement of stimulated Raman backscatter (SRBS) due to electron trapping in regimes of heavy linear Landau damping. The conventional Raman Langmuir wave is transformed into a set of beam acoustic modes [L. Yin et al., Phys. Rev. E 73, 025401 (2006)]. For the first time, a low phase velocity electron acoustic wave (EAW) is seen developing from the self-consistent Raman physics. Backscatter of the pump laser off the EAW fluctuations is reported and referred to as electron acoustic Thomson scatter. This light is similar in wavelength to, although much lower in amplitude than, the reflected light between the pump and SRBS wavelengths observed in single hot spot experiments, and previously interpreted as stimulated electron acoustic scatter [D. S. Montgomery et al., Phys. Rev. Lett. 87, 155001 (2001)]. The EAW observed in our simulations is strongest well below the phase-matched frequency for electron acoustic scatter, and therefore the EAW is not produced by it. The beating of different beam acoustic modes is proposed as the EAW excitation mechanism, and is called beam acoustic decay. Supporting evidence for this process, including bispectral analysis, is presented. The linear electrostatic modes, found by projecting the numerical distribution function onto a Gauss-Hermite basis, include beam acoustic modes (some of which are unstable even without parametric coupling to light waves) and a strongly-damped EAW similar to the observed one. This linear EAW results from non-Maxwellian features in the electron distribution, rather than nonlinearity due to electron trapping.

  20. Return Current Electron Beams and Their Generation of "Raman" Scattering

    NASA Astrophysics Data System (ADS)

    Simon, A.

    1998-11-01

    For some years, we(A. Simon and R. W. Short, Phys. Rev. Lett. 53), 1912 (1984). have proposed that the only reasonable explanation for many of the observations of "Raman" scattering is the presence of an electron beam in the plasma. (The beam creates a bump-on-tail instability.) Two major objections to this picture have been observation of Raman when no n_c/4 surface was present, with no likely source for the electron beam, and the necessity for the initially outward directed beam to bounce once to create the proper waves. Now new observations on LLE's OMEGA(R. Petrasso et al), this conference. and at LULI(C. Labaune et al)., Phys. Plasma 5, 234 (1998). have suggested a new origin for the electron beam. This new scenario answers the previous objections, maintains electron beams as the explanation of the older experiments, and may clear up puzzling observations that have remained unexplained. The new scenario is based on two assumptions: (1) High positive potentials develop in target plasmas during their creation. (2) A high-intensity laser beam initiates spark discharges from nearby surfaces to the target plasma. The resulting return current of electrons should be much more delta-like, is initially inwardly directed, and no longer requires the continued presence of a n_c/4 surface. Scattering of the interaction beam from the BOT waves yields the observed Raman signal. Experimental observations that support this picture will be cited. ``Pulsation'' of the scattering and broadband ``flashes'' are a natural part of this scenario. This work was supported by the U.S. Department of Energy Office of Inertial Confinement Fusion under Cooperative Agreement No. DE-FC03-92SF19460.

  1. Plasmon enhanced Raman scattering effect for an atom near a carbon nanotube.

    PubMed

    Bondarev, I V

    2015-02-23

    Quantum electrodynamics theory of the resonance Raman scattering is developed for an atom in a close proximity to a carbon nanotube. The theory predicts a dramatic enhancement of the Raman intensity in the strong atomic coupling regime to nanotube plasmon near-fields. This resonance scattering is a manifestation of the general electromagnetic surface enhanced Raman scattering effect, and can be used in designing efficient nanotube based optical sensing substrates for single atom detection, precision spontaneous emission control, and manipulation. PMID:25836436

  2. Surface-enhanced Raman scattering on diatom biosilica photonic crystals

    NASA Astrophysics Data System (ADS)

    Ren, Fanghui; Campbell, Jeremy; Hasan, Dihan; Wang, Xiangyu; Rorrer, Gregory L.; Wang, Alan X.

    Diatoms are a group of single-celled photosynthetic algae that make skeletal shells of hydrated amorphous silica, called frustules, which possess hierarchical nanoscale photonic crystal features made by a bottom-up approach at ambient temperature and pressure. In this paper, we theoretically investigate electric field enhancements of plasmonic nanoparticles coated on the surface of diatom skeletal shells. Surface-Enhanced Raman Scattering substrates are prepared by evaporating 10 nm thick silver film and self-assembling silver nanoparticles on diatom surfaces, which show significantly better SERS signals than silver nanoparticles on flat glass substrates.

  3. α-Glycine under high pressures: a Raman scattering study

    NASA Astrophysics Data System (ADS)

    Murli, Chitra; Sharma, Surinder M.; Karmakar, S.; Sikka, S. K.

    2003-11-01

    High-pressure behaviour of α-glycine has been investigated up to ∼23 GPa using Raman scattering technique. The experimental results show slope change in the CO 2 bending, NH 3 torsional and NH 3 rocking modes around 3 GPa and are interpreted in terms of change in the nature of an N-H⋯O-C intra-layer hydrogen bond at this pressure. Several other spectral features seem to arise from pressure-induced variations in the inter-molecular coupling.

  4. Resonant impulsive-stimulated Raman scattering on malachite green

    SciTech Connect

    Chesnoy, J.; Mokhtari, A.

    1988-10-01

    We have studied in the femtosecond regime the transient dynamics of dichroism (anisotropic absorption), birefringence, and frequency shift induced by an intense femtosecond pump beam in the dye malachite green in solution. Vibrational quantum beats were observed superimposed on the saturated absorption and dispersion signals and quantitatively explained in terms of impulsive-stimulated Raman scattering close to an electronic resonance. The selectivity for observation of the vibrations in the two electronic states is described for the different experimental schemes. We discuss the access to vibrational and electronic dynamics in both ground and excited electronic states and compare the possibilities to those of previous techniques.

  5. Surface-enhanced Raman scattering from silver-coated opals.

    PubMed

    Mu, Weiqiang; Hwang, Dae-Kue; Chang, Robert P H; Sukharev, Maxim; Tice, Daniel B; Ketterson, John B

    2011-03-28

    We describe surface-enhanced Raman scattering measurements from a benzenethiol monolayer adsorbed on a silver-coated film that is, in turn, deposited on an artificial opal, where the latter is a close-packed three-dimensional dielectric lattice formed from polystyrene spheres. Data for a range of sphere sizes, silver film thicknesses, and laser excitation wavelengths are obtained. Enhancement factors can be in the range of 10(7). To partially explain these large enhancements, we have performed model finite-difference time domain simulations of the position-dependent electric fields generated at the opal surfaces for several experimentally studied laser wavelengths and sphere diameters.

  6. Stimulated Raman scattering of laser from periodically spaced nanoparticles

    SciTech Connect

    Parashar, J.

    2009-09-15

    A periodic lattice of nanoparticles supports an electrostatic mode of space charge oscillations with frequency lying in a narrow band and varying periodically around {omega}{sub pe}/{radical}(3) with the wave number, where {omega}{sub pe} is the plasma frequency of electrons inside a nanoparticle. A laser impinged on such a lattice undergoes stimulated Raman scattering producing backward sideband electromagnetic radiation. The growth rate is maximum around the pump frequency {omega}{sub 0}=0.75{omega}{sub pe}, and then decreases gradually.

  7. Laser-scanning coherent anti-Stokes Raman scattering microscopy and applications to cell biology.

    PubMed Central

    Cheng, Ji-Xin; Jia, Y Kevin; Zheng, Gengfeng; Xie, X Sunney

    2002-01-01

    Laser-scanning coherent anti-Stokes Raman scattering (CARS) microscopy with fast data acquisition and high sensitivity has been developed for vibrational imaging of live cells. High three-dimensional (3D) resolution is achieved with two collinearly overlapped near infrared picosecond beams and a water objective with a high numerical aperture. Forward-detected CARS (F-CARS) and epi-detected CARS (E-CARS) images are recorded simultaneously. F-CARS is used for visualizing features comparable to or larger than the excitation wavelength, while E-CARS allows detection of smaller features with a high contrast. F-CARS and E-CARS images of live and unstained cells reveal details invisible in differential interference-contrast images. High-speed vibrational imaging of unstained cells undergoing mitosis and apoptosis has been carried out. For live NIH 3T3 cells in metaphase, 3D distribution of chromosomes is mapped at the frequency of the DNA backbone Raman band, while the vesicles surrounding the nucleus is imaged by E-CARS at the frequency of the C-H stretching Raman band. Apoptosis in NIH 3T3 cells is monitored using the CARS signal from aliphatic C-H stretching vibration. PMID:12080137

  8. Experimental evaluation of the twofold electromagnetic enhancement theory of surface-enhanced resonance Raman scattering

    SciTech Connect

    Yoshida, Ken-ichi; Itoh, Tamitake; Biju, Vasudevanpillai; Ishikawa, Mitsuru; Ozaki, Yukihiro

    2009-02-15

    We examined an electromagnetic (EM) theory of surface-enhanced resonance Raman scattering (SERRS) using single Ag nanoaggregates. The SERRS-EM theory is characterized by twofold EM enhancement induced by the coupling of plasmon resonance with both excitation and emission of Raman scattering plus fluorescence. The total emission cross-section spectra of enhanced Raman scattering and enhanced fluorescence were calculated using the following parameters: the spectrum of enhancement factor induced by plasmon resonance, resonance Raman scattering overlapped with fluorescence, and excitation wavelengths. The calculations well agreed with experimental total emission cross-section spectra, thus providing strong indications that the SERRS-EM theory is quantitatively correct.

  9. Probing Nanoscale Surface Enhanced Raman Scattering Fluctuation Dynamics using Correlated AFM and Confocal Ultramicroscopy

    SciTech Connect

    Suh, Yung D.; Schenter, Gregory K.; Zhu, Leyun; Lu, H PETER.

    2003-10-01

    We have studied the laser-excitation-intensity-dependent and Ag-nanocluster interstitial-site-dependent SERS intensity fluctuations under low molecule surface coverage of rhodamine 6G and cytochrome c. a new two-channel photon time-stamping system coupled with atomic force microscopic (AFM), Raman spectroscopic, and imaging microscopy was developed and applied to record Raman intensity fluctuation trajectories at sub-microsecond resolution correlated with in-situ characterization of the nanoparticle clusters. Our experimental results suggest that the nanoconfinement of the local electromagnetic-field enhancement and the interaction of the local field with the molecules, presumably under rotational motions, result in nano-Raman fluctuations. The SERS spectral fluctuation was pertinent to the nanoscale local enhancement and local interaction of the molecules with the surface when the number of molecules to contribute the microscopic Raman signal collected from a diffraction-limited focus spot. The SERS fluctuation dynamics were both photo-induced and spontaneous for rhodamine 6G, but only the photo-induced interstitial sites with heterogeneous geometries. To interpret the observed nano-SERS fluctuation dynamics, we used computer simulation of optical multiple scattering, based on multi-sphere scattering Mie theory, and rotational diffusion of molecules at an interstitial site, based on a random walk in orientation space.

  10. Monitoring lipid accumulation in the green microalga Botryococcus braunii with frequency-modulated stimulated Raman scattering

    NASA Astrophysics Data System (ADS)

    Wang, Chun-Chin; Chandrappa, Dayananda; Smirnoff, Nicholas; Moger, Julian

    2015-03-01

    The potential of microalgae as a source of renewable energy has received considerable interest because they can produce lipids (fatty acids and isoprenoids) that can be readily converted into biofuels. However, significant research in this area is required to increase yields to make this a viable renewable source of energy. An analytical tool that could provide quantitative in situ spectroscopic analysis of lipids synthesis in individual microalgae would significantly enhance our capability to understand the synthesis process at the cellular level and lead to the development of strategies for increasing yield. Stimulated Raman scattering (SRS) microscopy has great potential in this area however, the pump-probe signal from two-color two-photon absorption of pigments (chlorophyll and carotenoids) overwhelm the SRS signal and prevent its application. Clearly, the development of a background suppression technique is of significant value for this important research area. To overcome the limitation of SRS in pigmented specimens, we establish a frequency-modulated stimulated Raman scattering (FM-SRS) microscopy that eliminates the non-Raman background by rapidly toggling on-and-off the targeted Raman resonance. Moreover, we perform the background-free imaging and analysis of intracellular lipid droplets and extracellular hydrocarbons in a green microalga with FM-SRS microscopy. We believe that FM-SRS microscopy demonstrates the potential for many applications in pigmented cells and provides the opportunity for improved selective visualization of the chemical composition of algae and plants

  11. Theoretical calculation (DFT), Raman and surface-enhanced Raman scattering (SERS) study of ponceau 4R

    NASA Astrophysics Data System (ADS)

    Xie, Yunfei; Li, Yan; Sun, Yingying; Wang, Heya; Qian, He; Yao, Weirong

    2012-10-01

    Ponceau 4R is used as a coloring agent in many different products, such as food, drinks, medicines, cosmetics and tobacco. However, ponceau 4R also shows carcinogenic, teratogenic and mutagenic behavior in high doses. In this work, standard Raman, theoretical Raman and surface-enhanced Raman scattering (SERS) spectra have been used to investigate ponceau 4R. More specifically, density functional theory (DFT) calculations have been used to calculate the optimized Raman spectrum of ponceau 4R at the B3LYP/6-31G(d) level. This has provided a better understanding of the optimized geometry and vibrational frequencies of this dye. In addition, the experimental spectrum of ponceau 4R has been compared with the theoretical spectrum; good agreement was obtained. Finally, it has shown that using SERS the detection limit of the ponceau 4R solution can be as low as 5 μg/mL. This has been achieved by SERS measurements of ponceau 4R on a substrate of gold nanoparticles. The SERS peaks at 1030, 1236, 1356 and 1502 cm-1 were chosen as index for semi-quantitative analysis, showing that the SERS technique provided a useful ultrasensitive method for the detection of ponceau 4R.

  12. Surface-enhanced Raman scattering as a higher-order Raman process

    NASA Astrophysics Data System (ADS)

    Mueller, Niclas S.; Heeg, Sebastian; Reich, Stephanie

    2016-08-01

    We propose to understand surface-enhanced Raman scattering (SERS) as a higher-order Raman process that contains the plasmonic excitation. The SERS amplitudes are calculated with third- and fourth-order perturbation theory. Treating the plasmonic excitation as a quasiparticle, we derive analytic expressions for all coupling matrix elements. This leads to a general theory of plasmonic enhancement in SERS that can be applied to arbitrary plasmonic nanostructures. We obtain the plasmon eigenvectors of a gold nanosphere and a nanosphere dimer. They are used to calculate the enhancement of the Raman cross section of a molecule coupled to the dipole plasmon mode. The enhancement of the cross section is up to three orders of magnitude stronger than predicted by the theory of electromagnetic enhancement. The difference is most pronounced in vacuum and decreases with increasing dielectric constant of the embedding medium. The predictions from understanding SERS as a higher-order Raman process agree well with recent experiments; they highlight the dominance of plasmonic enhancement in SERS.

  13. The Inclusion of Raman Scattering Effects in the Combined Ocean-Atmosphere Radiative Transfer Model MOMO to Estimate the Influence of Raman Scattering in Case 1 Waters on Satellite Ocean Remote Sensing Applications

    NASA Astrophysics Data System (ADS)

    von Bismarck, J.; Fischer, J.

    2011-12-01

    source, the MOMO program structure allows the inclusion of other elastic and inelastic sources, e.g. fluorescence effects. To estimate the influence of Raman scattered light from case 1 waters on satellite remote sensing applications, tables with Raman fractions where computed for water-leaving and top-of-atmosphere radiances for the spectral channels of the OLCI imaging spectrometer on the upcoming ESA remote sensing satellite SENTINEL-3. The tables where generated for different chlorophyll concentrations, incorporating a bio optical model, and accounting for possible variations of salinity (0 - 40 PSU) and temperature (5° - 30° C) of the water. These results, also pointing out the importance of the inclusion of clear Water Raman scattering contributions in ocean and atmosphere remote sensing applications, are presented.

  14. Thomson Scattering Density Calibration by Rayleigh and Rotational Raman Scattering on NSTX

    SciTech Connect

    B.P. LeBlanc

    2008-07-16

    The multi-point Thomson scattering (MPTS) diagnostic measures the profiles of the electron temperature Te(R) and density ne(R) on the horizontal midplane of NSTX. Normal operation makes use of Rayleigh scattering in nitrogen or argon to derive the density profile. While the Rayleigh scattering ne(R) calibration has been validated by comparison with other density measurements and through its correlation with plasma phenomena, it does require dedicated detectors at the laser wavelength in this filter polychromator based diagnostic. The presence of dust and/or stray laser light precludes routine use of these dedicated spectral channels for Thomson scattering measurement. Hence it is of interest to investigate the use of Raman scattering in nitrogen for the purpose of density calibration, since it could free up detection equipment, which could then be used for the instrumentation of additional radial channels. In this paper the viewing optics "geometrical factor" profiles obtained from Rayleigh and Raman scattering are compared. While both techniques agree nominally, residual effects on the order of 10% remain and will be discussed.

  15. Magnetic-Polaron-Induced Enhancement of Surface Raman Scattering

    PubMed Central

    Shao, Qi; Liao, Fan; Ruotolo, Antonio

    2016-01-01

    The studies of the effects of magnetic field on surface enhanced Raman scattering (SERS) have been so far limited to the case of ferromagnetic/noble-metal, core/shell nano-particles, where the influence was always found to be negative. In this work, we investigate the influence of magnetic field on a diluted magnetic semiconductor/metal SERS system. Guided by three dimensional finite-difference time-domain simulations, a high efficient SERS substrate was obtained by diluting Mn into Au-capped ZnO, which results in an increase of the dielectric constant and, therefore, an enhancement of Raman signals. More remarkably, an increase of intensities as well as a reduction of the relative standard deviation (RSD) of Raman signals have been observed as a function of the external magnetic strength. We ascribe these positive influences to magnetic-field induced nucleation of bound magnetic polarons in the Mn doped ZnO. The combination of diluted magnetic semiconductors and SERS may open a new avenue for future magneto-optical applications. PMID:26754049

  16. Rapid surface enhanced Raman scattering detection method for chloramphenicol residues.

    PubMed

    Ji, Wei; Yao, Weirong

    2015-06-01

    Chloramphenicol (CAP) is a widely used amide alcohol antibiotics, which has been banned from using in food producing animals in many countries. In this study, surface enhanced Raman scattering (SERS) coupled with gold colloidal nanoparticles was used for the rapid analysis of CAP. Density functional theory (DFT) calculations were conducted with Gaussian 03 at the B3LYP level using the 3-21G(d) and 6-31G(d) basis sets to analyze the assignment of vibrations. Affirmatively, the theoretical Raman spectrum of CAP was in complete agreement with the experimental spectrum. They both exhibited three strong peaks characteristic of CAP at 1104 cm(-1), 1344 cm(-1), 1596 cm(-1), which were used for rapid qualitative analysis of CAP residues in food samples. The use of SERS as a method for the measurements of CAP was explored by comparing use of different solvents, gold colloidal nanoparticles concentration and absorption time. The method of the detection limit was determined as 0.1 μg/mL using optimum conditions. The Raman peak at 1344 cm(-1) was used as the index for quantitative analysis of CAP in food samples, with a linear correlation of R(2)=0.9802. Quantitative analysis of CAP residues in foods revealed that the SERS technique with gold colloidal nanoparticles was sensitive and of a good stability and linear correlation, and suited for rapid analysis of CAP residue in a variety of food samples. PMID:25754387

  17. Probing ultrafast processes by fifth order Stimulated Raman Scattering

    NASA Astrophysics Data System (ADS)

    Fumero, G.; Batignani, G.; Dorfman, K. E.; Mukamel, S.; Scopigno, T.

    2016-02-01

    We present the full diagrammatic description of non-resonant impulsive femtosecond stimulated Raman spectroscopy in a multimode model system. In this technique the pump-probe scheme is exploited to study the vibrational structure of the sample via stimulated Raman scattering. We apply closed-time-path-loop diagrams to calculate the complete response of the system at the relevant perturbation order. We show that, in presence of low-frequency modes, coherences created by the impulsive pump modify the resulting Raman signal, which oscillates from gain to loss features, depending on the time delay between the pump and probe pulses. This leads to a redistribution of photons among the fields involved in the process and, consequently, the energy flows between fields and matter. Moreover, through this formalism, we address the case of extremely short delays in which the pump and probe fields overlap in time. We find that, even in absence of photo-induced dynamics due to absorption of the pump pulse, the overlap condition can generate time dependent features, arising from additional diagrams, which offer no contribution for well separated pulses.

  18. Rapid surface enhanced Raman scattering detection method for chloramphenicol residues

    NASA Astrophysics Data System (ADS)

    Ji, Wei; Yao, Weirong

    2015-06-01

    Chloramphenicol (CAP) is a widely used amide alcohol antibiotics, which has been banned from using in food producing animals in many countries. In this study, surface enhanced Raman scattering (SERS) coupled with gold colloidal nanoparticles was used for the rapid analysis of CAP. Density functional theory (DFT) calculations were conducted with Gaussian 03 at the B3LYP level using the 3-21G(d) and 6-31G(d) basis sets to analyze the assignment of vibrations. Affirmatively, the theoretical Raman spectrum of CAP was in complete agreement with the experimental spectrum. They both exhibited three strong peaks characteristic of CAP at 1104 cm-1, 1344 cm-1, 1596 cm-1, which were used for rapid qualitative analysis of CAP residues in food samples. The use of SERS as a method for the measurements of CAP was explored by comparing use of different solvents, gold colloidal nanoparticles concentration and absorption time. The method of the detection limit was determined as 0.1 μg/mL using optimum conditions. The Raman peak at 1344 cm-1 was used as the index for quantitative analysis of CAP in food samples, with a linear correlation of R2 = 0.9802. Quantitative analysis of CAP residues in foods revealed that the SERS technique with gold colloidal nanoparticles was sensitive and of a good stability and linear correlation, and suited for rapid analysis of CAP residue in a variety of food samples.

  19. Coherent anti-Stokes Raman scattering microscopy of samples probed with Gaussian volumes.

    PubMed

    Marrocco, Michele

    2008-12-25

    Coherent anti-Stokes Raman scattering (CARS) microscopy is becoming increasingly popular to characterize biochemical samples. Within this context, we show that theoretical analysis can still be accomplished under the simple assumption of Gaussian volumes instead of spatial shapes obtainable from diffraction necessary to describe the tight-focusing condition realized within the focus of microscopes with high numerical apertures. The assumption, common in other physical and chemical spectroscopic techniques based on microscopy (e.g., fluorescence correlation spectroscopy, photon counting histogram) and never applied to CARS, is here used to determine the expression of the anti-Stokes electric field. Contrary to the standard approach resorting to numerical methods, we find that either the field is analytical for certain shapes of the Raman scatterer or the numerical reconstruction is strongly limited. In addition, we examine tests against two typical problems found in the literature, namely, a description of CARS radiation patterns and CARS imaging. With regard to the latter, we remark that the loss of spatial symmetry, the treatment of which is onerous in standard CARS microscopy because of possible separations between the microscope focus and the Raman scatterer, can be handled with ease in the limit of Gaussian volumes. An example is considered for polystyrene beads that are usually employed as test model of a CARS response of relevant biochemical samples. PMID:19093820

  20. Applications of Raman and Surface-Enhanced Raman Scattering to the Analysis of Eukaryotic Samples

    NASA Astrophysics Data System (ADS)

    Schulte, Franziska; Joseph, Virginia; Panne, Ulrich; Kneipp, Janina

    In this chapter, we discuss Raman scattering and surface-enhanced Raman scattering (SERS) for the analysis of cellular samples of plant and animal origin which are several tens to hundreds of microns in size. As was shown in the past several years, the favorable properties of noble metal nanostructures can be used to generate SERS signals in very complex biological samples such as cells, and result in an improved sensitivity and spatial resolution. Pollen grains, the physiological containers that produce the male gametes of seed plants, consist of a few vegetative cells and one generative cell, surrounded by a biopolymer shell. Their chemical composition has been a subject of research of plant physiologists, biochemists [1, 2], and lately even materials scientists [3, 4] for various reasons. In spite of a multitude of applied analytical approaches it could not be elucidated in its entirety yet. Animal cells from cell cultures have been a subject of intense studies due to their application in virtually all fields of biomedical research, ranging from studies of basic biological mechanisms to models for pharmaceutical and diagnostic research. Many aspects of all kinds of cellular processes including signalling, transport, and gene regulation have been elucidated, but many more facts about cell biology will need to be understood in order to efficiently address issues such as cancer, viral infection or genetic disorder. Using the information from spectroscopic methods, in particular combining normal Raman spectroscopy and SERS may open up new perspectives on cellular biochemistry. New sensitive Raman-based tools are being developed for the biochemical analysis of cellular processes [5-8].

  1. Romantic Story or Raman Scattering? Rose Petals as Ecofriendly, Low-Cost Substrates for Ultrasensitive Surface-Enhanced Raman Scattering.

    PubMed

    Chou, Sin-Yi; Yu, Chen-Chieh; Yen, Yu-Ting; Lin, Keng-Te; Chen, Hsuen-Li; Su, Wei-Fang

    2015-06-16

    In this Article, we present a facile approach for the preparation of ecofriendly substrates, based on common rose petals, for ultrasensitive surface-enhanced Raman scattering (SERS). The hydrophobic concentrating effect of the rose petals allows us to concentrate metal nanoparticle (NP) aggregates and analytes onto their surfaces. From a systematic investigation of the SERS performance when using upper and lower epidermises as substrates, we find that the lower epidermis, with its quasi-three-dimensional (quasi-3D) nanofold structure, is the superior biotemplate for SERS applications. The metal NPs and analytes are both closely packed in the quasi-3D structure of the lower epidermis, thereby enhancing the Raman signals dramatically within the depth of focus (DOF) of the Raman optical system. We have also found the effect of the pigment of the petals on the SERS performance. With the novel petal-based substrate, the SERS measurements reveal a detection limit for rhodamine 6G below the femtomolar regime (10(-15) M), with high reproducibility. Moreover, when we employ an upside-down drying process, the unique effect of the Wenzal state of the hydrophobic petal surface further concentrate the analytes and enhanced the SERS signals. Rose petals are green, natural materials that appear to have great potential for use in biosensors and biophotonics.

  2. A small animal Raman instrument for rapid, wide-area, spectroscopic imaging

    PubMed Central

    Bohndiek, Sarah E.; Wagadarikar, Ashwin; Zavaleta, Cristina L.; Van de Sompel, Dominique; Garai, Ellis; Jokerst, Jesse V.; Yazdanfar, Siavash; Gambhir, Sanjiv S.

    2013-01-01

    Raman spectroscopy, amplified by surface enhanced Raman scattering (SERS) nanoparticles, is a molecular imaging modality with ultra-high sensitivity and the unique ability to multiplex readouts from different molecular targets using a single wavelength of excitation. This approach holds exciting prospects for a range of applications in medicine, including identification and characterization of malignancy during endoscopy and intraoperative image guidance of surgical resection. The development of Raman molecular imaging with SERS nanoparticles is presently limited by long acquisition times, poor spatial resolution, small field of view, and difficulty in animal handling with existing Raman spectroscopy instruments. Our goal is to overcome these limitations by designing a bespoke instrument for Raman molecular imaging in small animals. Here, we present a unique and dedicated small-animal Raman imaging instrument that enables rapid, high-spatial resolution, spectroscopic imaging over a wide field of view (> 6 cm2), with simplified animal handling. Imaging of SERS nanoparticles in small animals demonstrated that this small animal Raman imaging system can detect multiplexed SERS signals in both superficial and deep tissue locations at least an order of magnitude faster than existing systems without compromising sensitivity. PMID:23821752

  3. Improved contrast radially polarized coherent anti-Stokes Raman scattering microscopy using annular aperture detection

    NASA Astrophysics Data System (ADS)

    Lin, Jian; Lu, Fake; Wang, Haifeng; Zheng, Wei; Sheppard, Colin, Jr.; Huang, Zhiwei

    2009-09-01

    We propose a unique annular aperture detection scheme in radially polarized coherent anti-Stokes Raman scattering (RP-CARS) microscopy for significantly removing nonresonant background for high contrast vibrational imaging. Our finite-difference time-domain calculations show that the maximum radiation patterns of RP-CARS signals from the scatterers vary with the scatterer's sizes, which are different from nonresonant CARS radiation from surrounding water. By applying appropriate sizes of annular stop apertures in the detection path, the nonresonant background from water can be effectively suppressed, yielding over 110-fold improvements in signal-to-background ratio for the forward-detected RP-CARS, while over 50-fold improvements for the backward RP-CARS detection.

  4. Surface plasmon enhanced Raman scattering frequency and angular resonance of Raman scattered light from pyridine on Au, Ag and Cu electrodes

    NASA Astrophysics Data System (ADS)

    Pettinger, B.; Wenning, U.; Wetzel, H.

    1980-12-01

    The strong dependence of the surface Raman intensity on the exciting frequency and on the angle of incidence for pyridine molecules adsorbed on Au, Ag and Cu electrodes after a weak oxidation/reduction cycle is evidence for a surface plasmon enhanced Raman scattering (SPERS).

  5. In vivo chemical and structural analysis of plant cuticular waxes using stimulated Raman scattering microscopy.

    PubMed

    Littlejohn, George R; Mansfield, Jessica C; Parker, David; Lind, Rob; Perfect, Sarah; Seymour, Mark; Smirnoff, Nicholas; Love, John; Moger, Julian

    2015-05-01

    The cuticle is a ubiquitous, predominantly waxy layer on the aerial parts of higher plants that fulfils a number of essential physiological roles, including regulating evapotranspiration, light reflection, and heat tolerance, control of development, and providing an essential barrier between the organism and environmental agents such as chemicals or some pathogens. The structure and composition of the cuticle are closely associated but are typically investigated separately using a combination of structural imaging and biochemical analysis of extracted waxes. Recently, techniques that combine stain-free imaging and biochemical analysis, including Fourier transform infrared spectroscopy microscopy and coherent anti-Stokes Raman spectroscopy microscopy, have been used to investigate the cuticle, but the detection sensitivity is severely limited by the background signals from plant pigments. We present a new method for label-free, in vivo structural and biochemical analysis of plant cuticles based on stimulated Raman scattering (SRS) microscopy. As a proof of principle, we used SRS microscopy to analyze the cuticles from a variety of plants at different times in development. We demonstrate that the SRS virtually eliminates the background interference compared with coherent anti-Stokes Raman spectroscopy imaging and results in label-free, chemically specific confocal images of cuticle architecture with simultaneous characterization of cuticle composition. This innovative use of the SRS spectroscopy may find applications in agrochemical research and development or in studies of wax deposition during leaf development and, as such, represents an important step in the study of higher plant cuticles.

  6. 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

  7. Subnanogram detection of dyes on filter paper by surface-enhanced Raman scattering spectrometry

    SciTech Connect

    Tran, C.D.

    1984-04-01

    A technique is demonstrated for the detection of subnanogram quantities of dyes adsorbed on filter paper. The introduction of silver colloidal hydrosols stabilized on the filter paper provides the necessary conditions for surface-enhanced Raman scattering. The Raman scattering was performed using a 3 mW He-Ne laser.

  8. Raman scattering method and apparatus for measuring isotope ratios and isotopic abundances

    DOEpatents

    Harney, Robert C.; Bloom, Stewart D.

    1978-01-01

    Raman scattering is used to measure isotope ratios and/or isotopic abundances. A beam of quasi-monochromatic photons is directed onto the sample to be analyzed, and the resulting Raman-scattered photons are detected and counted for each isotopic species of interest. These photon counts are treated mathematically to yield the desired isotope ratios or isotopic abundances.

  9. A deformable nanoplasmonic membrane reveals universal correlations between plasmon resonance and surface enhanced Raman scattering.

    PubMed

    Kang, Minhee; Kim, Jae-Jun; Oh, Young-Jae; Park, Sang-Gil; Jeong, Ki-Hun

    2014-07-01

    A quantitative correlation between plasmon resonance and surface enhanced Raman scattering (SERS) signals is revealed by using a novel active plasmonic method, that is, a deformable nanoplasmonic membrane. A single SERS peak has the maximum gain at the corresponding plasmon resonance wavelength, which has the maximum extinction product of an excitation and the corresponding Raman scattering wavelengths.

  10. Enhanced Raman Scattering from Aromatic Dithiols Electrosprayed into Plasmonic Nanojunctions

    SciTech Connect

    El-Khoury, Patrick Z.; Johnson, Grant E.; Novikova, Irina V.; Gong, Yu; Joly, Alan G.; Evans, James E.; Zamkov, Mikhail; Laskin, Julia; Hess, Wayne P.

    2015-12-01

    We describe surface enhanced Raman spectroscopy (SERS) experiments in which molecular coverage is systematically varied from 3.8 x 105 to 3.8 x 102 to 0.38 molecules/μm2 using electrospray deposition of ethanolic 4,4’-dimercaptostilbene (DMS) solutions. The plasmonic SERS substrate used herein consists of a well-characterized 2-dimensional (2D) array of silver nanospheres [see El-Khoury et al., J. Chem. Phys., 2014, 141, 214308], previously shown to feature uniform topography and plasmonic response, as well as intense SERS activity. When compared to their ensemble averaged analogues, the spatially and temporally averaged spectra of a single molecule exhibit several unique features including: (i) distinct relative intensities of the observable Raman-active vibrational states, (ii) more pronounced SERS backgrounds, and (iii) broader Raman lines indicative of faster vibrational dephasing. The first observation may be understood on the basis of an intuitive physical picture in which removal of averaging over multiple molecules exposes the tensorial nature of Raman scattering. When an oriented single molecule gives rise to the recorded SERS spectra, the relative orientation of the molecule with respect to vector components of the local electric field determines the relative intensities of the observable vibrational states. Using a single molecule SERS framework described herein, we derive a unique molecular orientation in which a single DMS molecule is isolated at a nanojunction formed between two silver nanospheres in the 2D array. The DMS molecule is found lying nearly flat with respect to the metal surface. The derived orientation of a single molecule at a plasmonic nanojunction is consistent with observations (ii) and (iii). In particular, a careful inspection of the temporal spectral variations along the recorded single molecule SERS time sequences reveals that the time-averaged SERS backgrounds arise from individual molecular events, marked by broadened SERS

  11. Raman Spectroscopic Imaging of the Whole Ciona intestinalis Embryo during Development

    PubMed Central

    Nakamura, Mitsuru J.; Hotta, Kohji; Oka, Kotaro

    2013-01-01

    Intracellular composition and the distribution of bio-molecules play central roles in the specification of cell fates and morphogenesis during embryogenesis. Consequently, investigation of changes in the expression and distribution of bio-molecules, especially mRNAs and proteins, is an important challenge in developmental biology. Raman spectroscopic imaging, a non-invasive and label-free technique, allows simultaneous imaging of the intracellular composition and distribution of multiple bio-molecules. In this study, we explored the application of Raman spectroscopic imaging in the whole Ciona intestinalis embryo during development. Analysis of Raman spectra scattered from C. intestinalis embryos revealed a number of localized patterns of high Raman intensity within the embryo. Based on the observed distribution of bio-molecules, we succeeded in identifying the location and structure of differentiated muscle and endoderm within the whole embryo, up to the tailbud stage, in a label-free manner. Furthermore, during cell differentiation, we detected significant differences in cell state between muscle/endoderm daughter cells and daughter cells with other fates that had divided from the same mother cells; this was achieved by focusing on the Raman intensity of single Raman bands at 1002 or 1526 cm−1, respectively. This study reports the first application of Raman spectroscopic imaging to the study of identifying and characterizing differentiating tissues in a whole chordate embryo. Our results suggest that Raman spectroscopic imaging is a feasible label-free technique for investigating the developmental process of the whole embryo of C. intestinalis. PMID:23977129

  12. Angle-resolved surface-enhanced Raman scattering on metallic nanostructured plasmonic crystals.

    PubMed

    Baumberg, Jeremy J; Kelf, Timothy A; Sugawara, Yoshihiro; Cintra, Suzanne; Abdelsalam, Mamdouh E; Bartlett, Phillip N; Russell, Andrea E

    2005-11-01

    Surface-enhanced Raman scattering is an ideal tool for identifying molecules from the "fingerprint" of their molecular bonds; unfortunately, this process lacks a full microscopic understanding and, practically, is plagued with irreproducibility. Using nanostructured metal surfaces, we demonstrate strong correlations between plasmon resonances and Raman enhancements. Evidence for simultaneous ingoing and outgoing resonances in wavelength and angle sheds new light on the Raman enhancement process, allowing optimization of a new generation of reproducible Raman substrates.

  13. Simultaneous laser-induced fluorescence and Raman imaging inside a hydrogen engine.

    PubMed

    Engel, Sascha Ronald; Koch, Peter; Braeuer, Andreas; Leipertz, Alfred

    2009-12-10

    We report on the simultaneous and two-dimensional measurement of laser-induced fluorescence (LIF) and Raman scattering (Ramanography) applied inside a hydrogen internal combustion (IC) engine. Two different LIF tracer molecules, triethylamine (TEA) and trimethylamine (TMA), were used for the LIF experiments. The LIF and Raman results were found to be in very good agreement. The simultaneous application of Ramanography and LIF imaging indicated that TMA is the more suitable LIF tracer molecule, compared to TEA. PMID:20011004

  14. Simultaneous laser-induced fluorescence and Raman imaging inside a hydrogen engine.

    PubMed

    Engel, Sascha Ronald; Koch, Peter; Braeuer, Andreas; Leipertz, Alfred

    2009-12-10

    We report on the simultaneous and two-dimensional measurement of laser-induced fluorescence (LIF) and Raman scattering (Ramanography) applied inside a hydrogen internal combustion (IC) engine. Two different LIF tracer molecules, triethylamine (TEA) and trimethylamine (TMA), were used for the LIF experiments. The LIF and Raman results were found to be in very good agreement. The simultaneous application of Ramanography and LIF imaging indicated that TMA is the more suitable LIF tracer molecule, compared to TEA.

  15. Structural analysis of molybdo-zinc-phosphate glasses: Neutron scattering, FTIR, Raman scattering, MAS NMR studies

    NASA Astrophysics Data System (ADS)

    Renuka, C.; Shinde, A. B.; Krishna, P. S. R.; Reddy, C. Narayana

    2016-08-01

    Vitreous samples were prepared in the xMoO3-17ZnO-(83-x) NaPO3 with 35 ≥ x ≥ 55 glass forming system by energy efficient microwave heating method. Structural evolution of the vitreous network was monitored as a function of composition by differential scanning calorimetry (DSC), Fourier transform infrared spectroscopy (FTIR), Raman scattering, Magic Angle Spin Nuclear magnetic resonance (MAS NMR) and Neutron scattering. Addition of MoO3 to the ZnO-NaPO3 glass leads to a pronounced increase in glass transition temperature (Tg) suggesting a significant increase in network connectivity and strength. In order to analyze FTIR and Raman scattering, a simple structural model is presented to rationalize the experimental observations. A number of structural units are formed due to network modification, and the resulting glass may be characterized by a network polyhedral with different numbers of unshared corners. 31P MAS NMR confirms a clear distinction between structural species having 3, 2, 1, 0 bridging oxygens (BOs). Further, Neutron scattering studies were used to probe the structure of these glasses. The result suggests that all the investigated glasses have structures based on chains of four coordinated phosphate and six coordinated molybdate units, besides, two different lengths of P-O bonds in tetrahedral phosphate units that are assigned to bonds of the P-atom with terminal and bridging oxygen atoms.

  16. Fiber four-wave mixing source for coherent anti-Stokes Raman scattering microscopy.

    PubMed

    Lefrancois, Simon; Fu, Dan; Holtom, Gary R; Kong, Lingjie; Wadsworth, William J; Schneider, Patrick; Herda, Robert; Zach, Armin; Sunney Xie, X; Wise, Frank W

    2012-05-15

    We present a fiber-format picosecond light source for coherent anti-Stokes Raman scattering microscopy. Pulses from a Yb-doped fiber amplifier are frequency converted by four-wave mixing (FWM) in normal-dispersion photonic crystal fiber to produce a synchronized two-color picosecond pulse train. We show that seeding the FWM process overcomes the deleterious effects of group-velocity mismatch and allows efficient conversion into narrow frequency bands. The source generates more than 160 mW of nearly transform-limited pulses tunable from 775 to 815 nm. High-quality coherent Raman images of animal tissues and cells acquired with this source are presented. PMID:22627526

  17. Quantitative detection of chemical compounds in human hair with coherent anti-Stokes Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Zimmerley, Maxwell; Lin, Chia-Yu; Oertel, David C.; Marsh, Jennifer M.; Ward, Jimmie L.; Potma, Eric Olaf

    2009-07-01

    Coherent anti-Stokes Raman scattering (CARS) microscopy is used to determine the distribution and concentration of selected compounds in intact human hair. By generating images based on ratiometric CARS contrast, quantitative concentration maps of both water and externally applied d-glycine are produced in the cortex of human hair fibers. Both water and d-glycine are found to homogeneously distribute throughout the cortical regions of the hair. The ability to selectively detect molecular agents in hair fibers is of direct relevance to understanding the chemical and physical mechanisms that underlie the performance of hair-care products.

  18. Compact, low-noise, all-solid-state laser system for stimulated Raman scattering microscopy.

    PubMed

    Steinle, Tobias; Kumar, Vikas; Steinmann, Andy; Marangoni, Marco; Cerullo, Giulio; Giessen, Harald

    2015-02-15

    We present a highly stable and compact laser source for stimulated Raman scattering (SRS) microscopy. cw-seeding of an optical parametric amplifier pumped by a bulk femtosecond Yb-oscillator and self-phase modulation in a tapered fiber allow for broad tunability without any optical or electronic synchronization. The source features noise levels of the Stokes beam close to the shot-noise limit at MHz modulation frequencies. We demonstrate the superior performance of our system by SRS imaging of micrometer-sized polymer beads. PMID:25680158

  19. Surface-enhanced Raman scattering in art and archaeology

    NASA Astrophysics Data System (ADS)

    Leona, Marco

    2005-11-01

    The identification of natural dyes found in archaeological objects and in works of art as textile dyes and lake pigments is a demanding analytical task. To address the problems raised by the very low dye content of dyed fibers and lake pigments, and by the requirement to remove only microscopic samples, surface enhanced Raman scattering techniques were investigated for application to museum objects. SERS gives excellent results with the majority of natural dyes, including: alizarin, purpurin, laccaic acid, carminic acid, kermesic acid, shikonin, juglone, lawsone, brazilin and brazilein, haematoxylin and haematein, fisetin, quercitrin, quercetin, rutin, and morin. In this study, limits of detection were determined for representative dyes and different SERS supports such as citrate reduced Ag colloid and silver nanoisland films. SERS was successfully used to identify natural madder in a microscopic fragment from a severely degraded 11th Century Byzantine textile recently excavated in Amorium, Turkey.

  20. Q-branch Raman scattering and modern kinetic thoery

    SciTech Connect

    Monchick, L.

    1993-12-01

    The program is an extension of previous APL work whose general aim was to calculate line shapes of nearly resonant isolated line transitions with solutions of a popular quantum kinetic equation-the Waldmann-Snider equation-using well known advanced solution techniques developed for the classical Boltzmann equation. The advanced techniques explored have been a BGK type approximation, which is termed the Generalized Hess Method (GHM), and conversion of the collision operator to a block diagonal matrix of symmetric collision kernels which then can be approximated by discrete ordinate methods. The latter method, which is termed the Collision Kernel method (CC), is capable of the highest accuracy and has been used quite successfully for Q-branch Raman scattering. The GHM method, not quite as accurate, is applicable over a wider range of pressures and has proven quite useful.

  1. Quantum random bit generation using stimulated Raman scattering.

    PubMed

    Bustard, Philip J; Moffatt, Doug; Lausten, Rune; Wu, Guorong; Walmsley, Ian A; Sussman, Benjamin J

    2011-12-01

    Random number sequences are a critical resource in a wide variety of information systems, including applications in cryptography, simulation, and data sampling. We introduce a quantum random number generator based on the phase measurement of Stokes light generated by amplification of zero-point vacuum fluctuations using stimulated Raman scattering. This is an example of quantum noise amplification using the most noise-free process possible: near unitary quantum evolution. The use of phase offers robustness to classical pump noise and the ability to generate multiple bits per measurement. The Stokes light is generated with high intensity and as a result, fast detectors with high signal-to-noise ratios can be used for measurement, eliminating the need for single-photon sensitive devices. The demonstrated implementation uses optical phonons in bulk diamond. PMID:22273908

  2. Quantum random bit generation using stimulated Raman scattering.

    PubMed

    Bustard, Philip J; Moffatt, Doug; Lausten, Rune; Wu, Guorong; Walmsley, Ian A; Sussman, Benjamin J

    2011-12-01

    Random number sequences are a critical resource in a wide variety of information systems, including applications in cryptography, simulation, and data sampling. We introduce a quantum random number generator based on the phase measurement of Stokes light generated by amplification of zero-point vacuum fluctuations using stimulated Raman scattering. This is an example of quantum noise amplification using the most noise-free process possible: near unitary quantum evolution. The use of phase offers robustness to classical pump noise and the ability to generate multiple bits per measurement. The Stokes light is generated with high intensity and as a result, fast detectors with high signal-to-noise ratios can be used for measurement, eliminating the need for single-photon sensitive devices. The demonstrated implementation uses optical phonons in bulk diamond.

  3. Detection of volatile organic compounds using surface enhanced Raman scattering

    SciTech Connect

    Chang, A S; Maiti, A; Ileri, N; Bora, M; Larson, C C; Britten, J A; Bond, T C

    2012-03-22

    The authors present the detection of volatile organic compounds directly in their vapor phase by surface-enhanced Raman scattering (SERS) substrates based on lithographically-defined two-dimensional rectangular array of nanopillars. The type of nanopillars is known as the tapered pillars. For the tapered pillars, SERS enhancement arises from the nanofocusing effect due to the sharp tip on top. SERS experiments were carried out on these substrates using various concentrations of toluene vapor. The results show that SERS signal from a toluene vapor concentration of ppm level can be achieved, and the toluene vapor can be detected within minutes of exposing the SERS substrate to the vapor. A simple adsorption model is developed which gives results matching the experimental data. The results also show promising potential for the use of these substrates in environmental monitoring of gases and vapors.

  4. Three-dimensional theory of stimulated Raman scattering

    NASA Astrophysics Data System (ADS)

    Sørensen, Martin W.; Sørensen, Anders S.

    2009-09-01

    We present a three-dimensional theory of stimulated Raman scattering (SRS) or super-radiance. In particular we address how the spatial and temporal properties of the generated SRS beam or Stokes beam of radiation depends on the spatial properties of the gain medium. Maxwell equations for the Stokes field operators and of the atomic operators are solved analytically and a correlation function for the Stokes field is derived. In the analysis we identify a super-radiating part of the Stokes radiation that exhibit beam characteristics. We show how the intensity in this beam builds up in time and at some point largely dominates the total Stokes radiation of the gain medium. We show how the SRS depends on the Fresnel number and the optical depth and that in fact these two factors are the only factors describing the coherent radiation.

  5. Isotopic gas analysis through Purcell cavity enhanced Raman scattering

    NASA Astrophysics Data System (ADS)

    Petrak, B.; Cooper, J.; Konthasinghe, K.; Peiris, M.; Djeu, N.; Hopkins, A. J.; Muller, A.

    2016-02-01

    Purcell enhanced Raman scattering (PERS) by means of a doubly resonant Fabry-Perot microcavity (mode volume ≈ 100 μm3 and finesse ≈ 30 000) has been investigated as a technique for isotopic ratio gas analysis. At the pump frequency, the resonant cavity supports a buildup of circulating power while simultaneously enabling Purcell spontaneous emission rate enhancement at the resonant Stokes frequency. The three most common isotopologues of CO2 gas were quantified, and a signal was obtained from 13C16O2 down to a partial pressure of 2 Torr. Due to its small size and low pump power needed (˜10 mW) PERS lends itself to miniaturization. Furthermore, since the cavity is resonant with the emission frequency, future improvements could allow it to serve as its own spectral analyzer and no separate spectroscopic device would be needed.

  6. Femtoliter silver cups as surface enhanced Raman scattering active containers.

    PubMed

    Bhuvana, T; Kulkarni, G U

    2009-01-28

    Femtoliter capacity Ag cups formed by the pulsed laser ablation of an Ag foil have been tried out as substrates for surface enhanced Raman scattering (SERS) measurements. The cups are formed as the impinging droplets from the laser plume undergo a flow pattern before freezing into cup-like structures, resulting in a surface roughness (approximately 35 nm) that makes them ideal for SERS studies. The internal volume of the cups is in the femtoliter (10(-15) l) range, well suited for small-scale reactions, particularly in biological studies. The cups exhibit enhancement factors of the order of 10(6) with the analyte molecule thiophenol. Individual cups have been dosed attoliter quantities (10(-18) l) of the analyte and detected. PMID:19417320

  7. Surface-enhanced Raman scattering of rat tissues.

    PubMed

    Aydin, Omer; Kahraman, Mehmet; Kiliç, Ertuğul; Culha, Mustafa

    2009-06-01

    Surface-enhanced Raman scattering (SERS) is proven to be a powerful tool for investigation of biological structures. In this study, tissues obtained from different rat organs are examined using SERS. The tissue samples are crushed with a pestle after sudden freezing in liquid nitrogen and mixed with a concentrated colloidal silver nanoparticle suspension. The reproducibility of SERS spectra acquired from several tissue samples from different organs is demonstrated. The collected spectra are comparatively evaluated based on the physiological function of the organ from which the tissue is obtained. The spectra from the tissues show significant differences and indicate that they can be used for tissue characterization and differentiation. The identification of the origins of the bands on the spectra is also attempted. This study suggests that SERS can be used to monitor the changes at the molecular level during metabolic changes in an organ or tissue as a result of a disease or another cause. PMID:19531293

  8. Semiclassical model of stimulated Raman scattering in photonic crystals.

    PubMed

    Florescu, Lucia; Zhang, Xiang

    2005-07-01

    We study the stimulated Raman scattering (SRS) of light from an atomic system embedded in a photonic crystal and coherently pumped by a laser field. In our study, the electromagnetic field is treated classically and the atomic system is described quantum mechanically. Considering a decomposition of the pump and Stokes fields into the Bloch modes of the photonic crystals and using a multiscale analysis, we derive the Maxwell-Bloch equations for SRS in photonic crystals. These equations contain effective parameters that characterize the SRS gain, the nonlinear atomic response to the electromagnetic field, and the group velocity and that can be calculated in terms of the Bloch modes of the unperturbed photonic crystal. We show that if the pump laser frequency is tuned near a photonic band edge and the atomic system is carefully chosen such that the Stokes mode matches another photonic band edge, low-threshold, enhanced Raman amplification is possible. Possible physical realizations of SRS in photonic crystals are also discussed.

  9. Assessing Telomere Length Using Surface Enhanced Raman Scattering

    NASA Astrophysics Data System (ADS)

    Zong, Shenfei; Wang, Zhuyuan; Chen, Hui; Cui, Yiping

    2014-11-01

    Telomere length can provide valuable insight into telomeres and telomerase related diseases, including cancer. Here, we present a brand-new optical telomere length measurement protocol using surface enhanced Raman scattering (SERS). In this protocol, two single strand DNA are used as SERS probes. They are labeled with two different Raman molecules and can specifically hybridize with telomeres and centromere, respectively. First, genome DNA is extracted from cells. Then the telomere and centromere SERS probes are added into the genome DNA. After hybridization with genome DNA, excess SERS probes are removed by magnetic capturing nanoparticles. Finally, the genome DNA with SERS probes attached is dropped onto a SERS substrate and subjected to SERS measurement. Longer telomeres result in more attached telomere probes, thus a stronger SERS signal. Consequently, SERS signal can be used as an indicator of telomere length. Centromere is used as the inner control. By calibrating the SERS intensity of telomere probe with that of the centromere probe, SERS based telomere measurement is realized. This protocol does not require polymerase chain reaction (PCR) or electrophoresis procedures, which greatly simplifies the detection process. We anticipate that this easy-operation and cost-effective protocol is a fine alternative for the assessment of telomere length.

  10. Fingerprinting CBRNE materials using surface-enhanced Raman scattering

    NASA Astrophysics Data System (ADS)

    Bertone, Jane F.; Spencer, Kevin M.; Sylvia, James M.

    2008-04-01

    One approach to CBRNE detection is analytical monitoring with portable spectroscopy systems. Such a technique needs to work in adverse environments, be amenable to use by field operators, and, given the sensitive nature of the target materials, should have an extremely rapid response time with no false negatives. This research demonstrates that surface-enhanced Raman scattering (SERS) is capable of detecting ppb levels of CBRNE materials with high sensitivity and no false positives. We present reproducible and selective detection using novel SERS structures that exhibit an inherently uniform surface morphology, leading to rapid, reproducible manufacturing. Our work includes receiver-operator characteristic (ROC) curves for the detection of both conventional and improvised nitro explosives at low signal-to-noise ratios. We also present the detection of added CBRNE materials including chemical and biological agents as well as nuclear enriching materials. Our expertise extends to instrumentation of portable, robust Raman spectrographs that can be packaged with our sensors for a versatile security tool with applications extending from points of entry to points of production, from people to objects and freight.

  11. 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.

  12. 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. PMID:24013358

  13. Ultrasensitive surface-enhanced Raman scattering detection in common fluids

    PubMed Central

    Yang, Shikuan; Dai, Xianming; Stogin, Birgitt Boschitsch; Wong, Tak-Sing

    2016-01-01

    Detecting target analytes with high specificity and sensitivity in any fluid is of fundamental importance to analytical science and technology. Surface-enhanced Raman scattering (SERS) has proven to be capable of detecting single molecules with high specificity, but achieving single-molecule sensitivity in any highly diluted solutions remains a challenge. Here we demonstrate a universal platform that allows for the enrichment and delivery of analytes into the SERS-sensitive sites in both aqueous and nonaqueous fluids, and its subsequent quantitative detection of Rhodamine 6G (R6G) down to ∼75 fM level (10−15 mol⋅L−1). Our platform, termed slippery liquid-infused porous surface-enhanced Raman scattering (SLIPSERS), is based on a slippery, omniphobic substrate that enables the complete concentration of analytes and SERS substrates (e.g., Au nanoparticles) within an evaporating liquid droplet. Combining our SLIPSERS platform with a SERS mapping technique, we have systematically quantified the probability, p(c), of detecting R6G molecules at concentrations c ranging from 750 fM (p > 90%) down to 75 aM (10−18 mol⋅L−1) levels (p ≤ 1.4%). The ability to detect analytes down to attomolar level is the lowest limit of detection for any SERS-based detection reported thus far. We have shown that analytes present in liquid, solid, or air phases can be extracted using a suitable liquid solvent and subsequently detected through SLIPSERS. Based on this platform, we have further demonstrated ultrasensitive detection of chemical and biological molecules as well as environmental contaminants within a broad range of common fluids for potential applications related to analytical chemistry, molecular diagnostics, environmental monitoring, and national security. PMID:26719413

  14. Ultrasensitive surface-enhanced Raman scattering detection in common fluids.

    PubMed

    Yang, Shikuan; Dai, Xianming; Stogin, Birgitt Boschitsch; Wong, Tak-Sing

    2016-01-12

    Detecting target analytes with high specificity and sensitivity in any fluid is of fundamental importance to analytical science and technology. Surface-enhanced Raman scattering (SERS) has proven to be capable of detecting single molecules with high specificity, but achieving single-molecule sensitivity in any highly diluted solutions remains a challenge. Here we demonstrate a universal platform that allows for the enrichment and delivery of analytes into the SERS-sensitive sites in both aqueous and nonaqueous fluids, and its subsequent quantitative detection of Rhodamine 6G (R6G) down to ∼75 fM level (10(-15) mol⋅L(-1)). Our platform, termed slippery liquid-infused porous surface-enhanced Raman scattering (SLIPSERS), is based on a slippery, omniphobic substrate that enables the complete concentration of analytes and SERS substrates (e.g., Au nanoparticles) within an evaporating liquid droplet. Combining our SLIPSERS platform with a SERS mapping technique, we have systematically quantified the probability, p(c), of detecting R6G molecules at concentrations c ranging from 750 fM (p > 90%) down to 75 aM (10(-18) mol⋅L(-1)) levels (p ≤ 1.4%). The ability to detect analytes down to attomolar level is the lowest limit of detection for any SERS-based detection reported thus far. We have shown that analytes present in liquid, solid, or air phases can be extracted using a suitable liquid solvent and subsequently detected through SLIPSERS. Based on this platform, we have further demonstrated ultrasensitive detection of chemical and biological molecules as well as environmental contaminants within a broad range of common fluids for potential applications related to analytical chemistry, molecular diagnostics, environmental monitoring, and national security. PMID:26719413

  15. Raman Scattering from few-layer Graphene Films

    NASA Astrophysics Data System (ADS)

    Gupta, A.; Joshi, P.; Srinivas, T.; Eklund, Peter

    2006-03-01

    Few layer-graphene sheet (nGL's) films, where n is the number of graphene layers, are new two-dimensional sp^2 carbon systems that have been shown to produce exciting Fractional Quantum Hall phenomena. We report here on the first Raman scattering (RS) results of nGLs. nGLs with lateral dimensions of ˜1-3 μm were prepared by chemical delamination of graphite flake or HOPG and then transferred from solution onto substrates (mica, pyrex,In/pyrex and Au/pyrex). RS spectra have been collected on nGL's with n=1, 2, 3 and compared with the graphite. Graphite exhibits two E2g interlayer modes at 42 cm-1 and 1582 cm-1. The Raman spectra of (n=1-3) nGLs were found to exhibit peaks at 1350 cm-1 and 1620 cm-1, i.e., near frequencies associated with high phonon density of states. The high frequency E2g band is found to split into two bands when the nGL is supported on metallic substrates (In,Au). In both these cases, we observe bands at 1583 cm-1, ˜1592 cm-1 rather than one band at 1581 cm-1 when the nGL is on insulating pyrex. The splitting of the interlayer band when on metallic substrates is identified with charge transfer between the nGL and the substrate. The phonon density of states scattering observed does not appear to be due to disorder in the basal plane.

  16. Stimulated Brillouin Scattering Microscopic Imaging

    PubMed Central

    Ballmann, Charles W.; Thompson, Jonathan V.; Traverso, Andrew J.; Meng, Zhaokai; Scully, Marlan O.; Yakovlev, Vladislav V.

    2015-01-01

    Two-dimensional stimulated Brillouin scattering microscopy is demonstrated for the first time using low power continuous-wave lasers tunable around 780 nm. Spontaneous Brillouin spectroscopy has much potential for probing viscoelastic properties remotely and non-invasively on a microscopic scale. Nonlinear Brillouin scattering spectroscopy and microscopy may provide a way to tremendously accelerate the data aquisition and improve spatial resolution. This general imaging setup can be easily adapted for specific applications in biology and material science. The low power and optical wavelengths in the water transparency window used in this setup provide a powerful bioimaging technique for probing the mechanical properties of hard and soft tissue. PMID:26691398

  17. Stimulated Brillouin Scattering Microscopic Imaging.

    PubMed

    Ballmann, Charles W; Thompson, Jonathan V; Traverso, Andrew J; Meng, Zhaokai; Scully, Marlan O; Yakovlev, Vladislav V

    2015-01-01

    Two-dimensional stimulated Brillouin scattering microscopy is demonstrated for the first time using low power continuous-wave lasers tunable around 780 nm. Spontaneous Brillouin spectroscopy has much potential for probing viscoelastic properties remotely and non-invasively on a microscopic scale. Nonlinear Brillouin scattering spectroscopy and microscopy may provide a way to tremendously accelerate the data aquisition and improve spatial resolution. This general imaging setup can be easily adapted for specific applications in biology and material science. The low power and optical wavelengths in the water transparency window used in this setup provide a powerful bioimaging technique for probing the mechanical properties of hard and soft tissue.

  18. Stimulated Brillouin Scattering Microscopic Imaging

    NASA Astrophysics Data System (ADS)

    Ballmann, Charles W.; Thompson, Jonathan V.; Traverso, Andrew J.; Meng, Zhaokai; Scully, Marlan O.; Yakovlev, Vladislav V.

    2015-12-01

    Two-dimensional stimulated Brillouin scattering microscopy is demonstrated for the first time using low power continuous-wave lasers tunable around 780 nm. Spontaneous Brillouin spectroscopy has much potential for probing viscoelastic properties remotely and non-invasively on a microscopic scale. Nonlinear Brillouin scattering spectroscopy and microscopy may provide a way to tremendously accelerate the data aquisition and improve spatial resolution. This general imaging setup can be easily adapted for specific applications in biology and material science. The low power and optical wavelengths in the water transparency window used in this setup provide a powerful bioimaging technique for probing the mechanical properties of hard and soft tissue.

  19. Polarization modulated background-free hyperspectral stimulated Raman scattering microscopy (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Houle, Marie-Andrée.; Andreana, Marco; Ridsdale, Andrew; Moffatt, Doug; Lausten, Rune; Légaré, François; Stolow, Albert

    2016-03-01

    Stimulated Raman Scattering (SRS) microscopy is a nonlinear microscopy technique based on Raman vibrational resonances determined by the frequency difference between Pump and Stokes laser pulses. Modulation of one laser beam transfers the modulation to the other, as either a gain in Stokes (SRG) or a loss in Pump power (SRL). SRS microscopy does not exhibit the four-wave mixing nonresonant background characteristic of CARS microscopy. However, other background signals due to two-photon absorption, thermal lensing or cross-phase modulation (XPM) do reduce the detection sensitivity and can distort the hyperspectral scans. Phase sensitive lock-in detection can reduce contributions from two-photon absorption, which is out-of-phase for the SRG case. However, the background signal due to XPM, which can be in-phase with SRS, can reduce the detection sensitivity. We present a novel polarization modulation (PM) scheme in SRS microscopy which greatly reduces the nonresonant XPM background, demonstrated here for the SRL case. Since many Raman vibrational transitions are parallel polarized, the SRS signal is maximum (minimum) when the polarizations of the pump and the Stokes beams are parallel (perpendicular). However, in both parallel and perpendicular Pump-Stokes geometries, XPM is non-zero in many media. Therefore, PM can remove the XPM background without significantly reducing the SRS signal. Our results show that the PM-SRS successfully removes the nonresonant signal due to XPM. High imaging contrast is observed, concomitant with high sensitivity at very low analyte concentrations and undistorted Raman spectra.

  20. In vivo Coherent Raman Imaging for Neuroscience Applications

    NASA Astrophysics Data System (ADS)

    Cote, Daniel

    2010-08-01

    The use of coherent Raman imaging is described for applications in neuroscience. Myelin imaging of the spinal cord can be performed with Raman imaging through the use of the vibration in carbon-hydrogen bonds, dominant in lipids. First, we demonstrate in vivo histomorphometry in live animal for characterization of myelin-related nervous system pathologies. This is used to characterize spinal cord health during multiple sclerosis. Second, Raman spectroscopy of tissue is discussed. We discuss the challenges that live animal imaging brings, together with important aspects of coherent Raman imaging in tissue.

  1. Spontaneous and stimulated Raman scattering in silica-cladded silicon photonic crystal waveguides

    NASA Astrophysics Data System (ADS)

    Hsiao, Yi-Hua; Iwamoto, Satoshi; Arakawa, Yasuhiko

    2015-04-01

    We report the observation of spontaneous and stimulated Raman scattering in a silica-cladded silicon photonic crystal (PhC) waveguide (WG) with modified holes. Spontaneous Raman scattering in the WG was enhanced when the Stokes wavelength was approached to the bandedge of a WG mode. A maximum enhancement up to ˜5 times was obtained in the present work. At a Stokes wavelength in the lower group velocity region, nonlinear increase of the Stokes power as the pump power, a clear indication of the onset of stimulated Raman scattering, was observed. Moreover, Raman amplification with an external signal beam was also demonstrated. On-off gain becomes small as the Stokes wavelength gets away from the bandedge of the WG mode. These are the first observations of Raman scattering effects in silica-cladded silicon PhC structures.

  2. A Raman-based endoscopic strategy for multiplexed molecular imaging.

    PubMed

    Zavaleta, Cristina L; Garai, Ellis; Liu, Jonathan T C; Sensarn, Steven; Mandella, Michael J; Van de Sompel, Dominique; Friedland, Shai; Van Dam, Jacques; Contag, Christopher H; Gambhir, Sanjiv S

    2013-06-18

    Endoscopic imaging is an invaluable diagnostic tool allowing minimally invasive access to tissues deep within the body. It has played a key role in screening colon cancer and is credited with preventing deaths through the detection and removal of precancerous polyps. However, conventional white-light endoscopy offers physicians structural information without the biochemical information that would be advantageous for early detection and is essential for molecular typing. To address this unmet need, we have developed a unique accessory, noncontact, fiber optic-based Raman spectroscopy device that has the potential to provide real-time, multiplexed functional information during routine endoscopy. This device is ideally suited for detection of functionalized surface-enhanced Raman scattering (SERS) nanoparticles as molecular imaging contrast agents. This device was designed for insertion through a clinical endoscope and has the potential to detect and quantify the presence of a multiplexed panel of tumor-targeting SERS nanoparticles. Characterization of the Raman instrument was performed with SERS particles on excised human tissue samples, and it has shown unsurpassed sensitivity and multiplexing capabilities, detecting 326-fM concentrations of SERS nanoparticles and unmixing 10 variations of colocalized SERS nanoparticles. Another unique feature of our noncontact Raman endoscope is that it has been designed for efficient use over a wide range of working distances from 1 to 10 mm. This is necessary to accommodate for imperfect centering during endoscopy and the nonuniform surface topology of human tissue. Using this endoscope as a key part of a multiplexed detection approach could allow endoscopists to distinguish between normal and precancerous tissues rapidly and to identify flat lesions that are otherwise missed.

  3. In vitro colocalization of plasmonic nano-biolabels and biomolecules using plasmonic and Raman scattering microspectroscopy

    NASA Astrophysics Data System (ADS)

    Chaudhari, Kamalesh; Pradeep, Thalappil

    2015-04-01

    An insight into the intracellular fate of theranostics is important for improving their potential in biological applications. In vivo efficacy of plasmonic theranostics depends on our ability to monitor temporal changes in their size, shape, and state of aggregation, and the identification of molecules adsorbed on their surfaces. We develop a technique which combines plasmonic and Raman scattering microspectroscopy to colocalize plasmonic scattering from metallic nanoparticles with the Raman signatures of biomolecules adsorbed on the surface of the former. Using this technique, we have colocalized biomolecules with the plasmonic scattering from silver nanoparticles in the vicinity of Escherichia coli bacteria. To prove the applicability of this setup for the measurements on mammalian cells, imaging of HEK293 cells treated with gold nanoparticles was performed. We discuss the importance of such correlated measurements over individual techniques, although the latter may lead to misinterpretation of results. Finally, with the above-mentioned examples, we have given criteria to improve the specificity of theranostics. We believe that this methodology will be considered as a prime development in the assessment of theranostics.

  4. Raman microscopy of silicon for electronic displays and solar cells: Enhanced Raman scattering observed for microstructured surface

    NASA Astrophysics Data System (ADS)

    Kitahara, K.; Ishizaki, A.

    2012-12-01

    This paper describes Raman spectroscopy of microstructured silicon (Si), which is used for electronic displays, solar cells, and other applications. Enhanced Raman scattering was found for excimer laser crystallized polycrystalline Si (ELC poly-Si) thin films, texture-structured Si, black Si, and porous Si. Raman scattering of those materials reflects mainly the conditions at projections on their surfaces. Atomic force microscopy and Raman spectroscopy for ELC poly-Si indicated that hillocks and ridges are located at grain boundaries where the defect density is relatively large and the thermal stress in the films is somewhat relaxed. The enhancement effect was shown to be useful for detecting a local vibration mode that could not be easily detected for mirror-finished Si. The variation in the enhancement ratio with the incident light wavelength was examined for comparison with the electromagnetic model.

  5. Raman scattering study of rare-earth hexaboride

    NASA Astrophysics Data System (ADS)

    Ogita, N.; Nagai, S.; Udagawa, M.; Iga, F.; Sera, M.; Oguchi, T.; Akimitsu, J.; Kunii, S.

    2005-04-01

    The excitation-energy, polarization, pressure, and temperature dependences of Raman scattering spectra have been measured for the RB6 crystals ( R=Ca, La, Ce, Pr, Sm, Gd, Dy, and Yb). In the Raman spectra, the extra peaks have been clearly observed at around 200 cm-1, except for the Raman-active phonons and CEF excitations. The extra peaks show anomalous behavior in the temperature, polarization, and lattice parameter dependences. These anomalous behaviors originate from the vibration of the rare-earth ions in octahedral B 6 cage, and the extra peaks can be assigned as the second-order Raman excitations of T 1u[3]. To check the validity of our assignment, we have measured the pressure dependence. In this paper, the results of the “ extra peaks” at about 200 cm -1, and pressure dependence of SmB 6 are presented. The sample preparation and experimental details are explained in our previous report [3]. The Pm3m symmetry of RB 6 gives us the phonon numbers at Brilloiun zone center; Γ=A1g+Eg+T1g+T2g+3T1u+T2u. The Raman-active phonons are A1g, Eg, and T2g, which are the vibration of boron octahedra. In cubic symmetry, all Raman-active phonons appear in the (x+y,x+y) polarization geometry. In the notation of (x,y), x and y denote the polarization directions of incident and scattered light, respectively. x and y correspond to the crystal axes of [1 0 0] and [0 1 0], respectively. Fig. 1 shows the Raman spectra of trivalent RB6 at room temperature in the energy region below T2g phonons ( ≃700 cm-1). Each spectrum is depicted in the order of the decreasing lattice parameters from top to bottom. As shown in Fig. 1, the energy of T2g phonon decreases with increasing lattice parameter, and this is normal dependence. However, the extra peaks (arrows) show an anti-trend for T2g phonon's. Focusing on the size of cage space consisting of surrounding borons for rare earth ion a-rR( a and rR are lattice parameter and ionic radius, respectively), the energy of the peaks is

  6. Ultrasensitive protein detection in terms of multiphonon resonance Raman scattering in ZnS nanocrystals

    NASA Astrophysics Data System (ADS)

    Chu, Xueying; Hong, Xia; Zou, Peng; Men, Jing; Liu, Yichun

    2011-06-01

    Ultrasensitive protein detection was realized using multiphonon Resonance Raman scattering in ZnS nanocrystals. The longitudinal optical phonon line of ZnS and its overtones, which are called multiphonon Raman lines (MRLs), were used as the Raman probe signals. MRLs have a narrow bandwidth, high stability in aqueous solution, and strong resistance to interference from surface variations. Our results show that these features allow for reliable biodetection with good selectivity and high specificity. The detection limit is about 5 fM. This Raman scattering-based methodology will greatly extend the potential applications for ZnS in the biomedical sciences.

  7. Inverse scattering transform analysis of Stokes-anti-Stokes stimulated Raman scattering

    NASA Astrophysics Data System (ADS)

    Gerdjikov, V. S.; Kostov, N. A.

    1996-11-01

    A system of Maxwell-Bloch type equations (MBE's), describing stimulated Raman scattering with both Stokes and anti-Stokes waves taken into account, is investigated. We introduce variables S3 and S+/-, which are bilinear in the electromagnetic fields, and prove that the corresponding equations possess Lax representation. This fact is used to obtain additional solutions for S3, S+/- and for the MBE's which include solitons, periodical waves, and self-similarity solutions. The transient and bright threshold solitons are also analyzed.

  8. Enhanced Raman scattering from aromatic dithiols electrosprayed into plasmonic nanojunctions.

    PubMed

    El-Khoury, Patrick Z; Johnson, Grant E; Novikova, Irina V; Gong, Yu; Joly, Alan G; Evans, James E; Zamkov, Mikhail; Laskin, Julia; Hess, Wayne P

    2015-01-01

    We describe surface enhanced Raman spectroscopy (SERS) experiments in which molecular coverage is systematically varied from 3.8 × 10(5) to 3.8 × 10(2) to 0.38 molecules per μm(2) using electrospray deposition of ethanolic 4,4'-dimercaptostilbene (DMS) solutions. The plasmonic SERS substrate used herein consists of a well-characterized 2-dimensional (2D) array of silver nanospheres (see El-Khoury et al., J. Chem. Phys., 2014, 141, 214308), previously shown to feature uniform topography and plasmonic response, as well as intense SERS activity. When compared to their ensemble averaged analogues, the spatially and temporally averaged spectra of a single molecule exhibit several unique features including: (i) distinct relative intensities of the observable Raman-active vibrational states, (ii) more pronounced SERS backgrounds, and (iii) broader Raman lines indicative of faster vibrational dephasing. The first observation may be understood on the basis of an intuitive physical picture in which the removal of averaging over multiple molecules exposes the tensorial nature of Raman scattering. When an oriented single molecule gives rise to the recorded SERS spectra, the relative orientation of the molecule with respect to vector components of the local electric field determines the relative intensities of the observable vibrational states. Using a single molecule SERS framework, described herein, we derive a unique molecular orientation in which a single DMS molecule is isolated at a nanojunction formed between two silver nanospheres in the 2D array. The DMS molecule is found lying nearly flat with respect to the metal. The derived orientation of a single molecule at a plasmonic nanojunction is consistent with observations (ii) and (iii). In particular, a careful inspection of the temporal spectral variations along the recorded single molecule SERS time sequences reveals that the time-averaged SERS backgrounds arise from individual molecular events, marked by broadened

  9. Enhanced Raman scattering from aromatic dithiols electrosprayed into plasmonic nanojunctions.

    PubMed

    El-Khoury, Patrick Z; Johnson, Grant E; Novikova, Irina V; Gong, Yu; Joly, Alan G; Evans, James E; Zamkov, Mikhail; Laskin, Julia; Hess, Wayne P

    2015-01-01

    We describe surface enhanced Raman spectroscopy (SERS) experiments in which molecular coverage is systematically varied from 3.8 × 10(5) to 3.8 × 10(2) to 0.38 molecules per μm(2) using electrospray deposition of ethanolic 4,4'-dimercaptostilbene (DMS) solutions. The plasmonic SERS substrate used herein consists of a well-characterized 2-dimensional (2D) array of silver nanospheres (see El-Khoury et al., J. Chem. Phys., 2014, 141, 214308), previously shown to feature uniform topography and plasmonic response, as well as intense SERS activity. When compared to their ensemble averaged analogues, the spatially and temporally averaged spectra of a single molecule exhibit several unique features including: (i) distinct relative intensities of the observable Raman-active vibrational states, (ii) more pronounced SERS backgrounds, and (iii) broader Raman lines indicative of faster vibrational dephasing. The first observation may be understood on the basis of an intuitive physical picture in which the removal of averaging over multiple molecules exposes the tensorial nature of Raman scattering. When an oriented single molecule gives rise to the recorded SERS spectra, the relative orientation of the molecule with respect to vector components of the local electric field determines the relative intensities of the observable vibrational states. Using a single molecule SERS framework, described herein, we derive a unique molecular orientation in which a single DMS molecule is isolated at a nanojunction formed between two silver nanospheres in the 2D array. The DMS molecule is found lying nearly flat with respect to the metal. The derived orientation of a single molecule at a plasmonic nanojunction is consistent with observations (ii) and (iii). In particular, a careful inspection of the temporal spectral variations along the recorded single molecule SERS time sequences reveals that the time-averaged SERS backgrounds arise from individual molecular events, marked by broadened

  10. Raman scattering by H2 and N2 in the atmospheres of exoplanets

    NASA Astrophysics Data System (ADS)

    Oklopcic, Antonija; Hirata, Christopher M.; Heng, Kevin

    2016-06-01

    Rayleigh scattering is an important source of opacity in the atmospheres of exoplanets at short optical and near-UV wavelengths. Raman scattering is an inelastic process related to Rayleigh scattering, but with a weaker cross section. We analyze the signatures of Raman scattering imprinted in the reflected light and the geometric albedo of exoplanets. Raman scattering causes filling-in of absorption lines in the incident spectrum, thus producing sharp enhancements in the geometric albedo. It also shifts the wavelengths of spectral features in the reflected light causing the Raman ghost lines. Observing the albedo enhancements could be used to measure the column density of the scattering molecule and provide constrains on the presence of clouds and hazes in the atmosphere. Observing the Raman ghost lines could be used to spectroscopically identify the main scatterer in the atmosphere -- molecules like H2 or N2 which do not show prominent spectral signatures in the optical wavelength range. If detected, ghost lines could also provide information about the temperature of the atmosphere. Here we present how these signatures of Raman scattering in hydrogen- and nitrogen-dominated atmospheres can be used as probes of atmospheric pressure, temperature and composition. We analyze the feasibility of detecting these features in the albedo spectra of nearby exoplanets with the existing and future observational facilities.

  11. Chip-Scale Bioassays Based on Surface-Enhanced Raman Scattering: Fundamentals and Applications

    SciTech Connect

    Park, Hye-Young

    2005-01-01

    This work explores the development and application of chip-scale bioassays based on surface-enhanced Raman scattering (SERS) for high throughput and high sensitivity analysis of biomolecules. The size effect of gold nanoparticles on the intensity of SERS is first presented. A sandwich immunoassay was performed using Raman-labeled immunogold nanoparticles with various sizes. The SERS responses were correlated to particle densities, which were obtained by atomic force microscopy (AFM). The response of individual particles was also investigated using Raman-microscope and an array of gold islands on a silicon substrate. The location and the size of individual particles were mapped using AFM. The next study describes a low-level detection of Escherichia coli 0157:H7 and simulants of biological warfare agents in a sandwich immunoassay format using SERS labels, which have been termed Extrinsic Raman labels (ERLs). A new ERL scheme based on a mixed monolayer is also introduced. The mixed monolayer ERLs were created by covering the gold nanoparticles with a mixture of two thiolates, one thiolate for covalently binding antibody to the particle and the other thiolate for producing a strong Raman signal. An assay platform based on mixed self-assembled monolayers (SAMs) on gold is then presented. The mixed SAMs were prepared from dithiobis(succinimidyl undecanoate) (DSU) to covalently bind antibodies on gold substrate and oligo(ethylene glycol)-terminated thiol to prevent nonspecific adsorption of antibodies. After the mixed SAMs surfaces, formed from various mole fraction of DSU were incubated with antibodies, AFM was used to image individual antibodies on the surface. The final study presents a collaborative work on the single molecule adsorption of YOYO-I labeled {lambda}-DNA at compositionally patterned SAMs using total internal reflection fluorescence microscopy. The role of solution pH, {lambda}-DNA concentration, and domain size was investigated. This work also revealed

  12. Enhancing stimulated Raman scattering of weaker gain Raman modes in microdroplets by seeding and efficient pumping

    NASA Astrophysics Data System (ADS)

    Mazumder, Md. Mohiuddin; Fields, Mitchell H.; Hartings, Justin M.; Pu, Xiaoyun; Kwok, Alfred S.; Schaschek, Karl; Chang, Richard K.

    1996-05-01

    High-Q morphology-dependent resonances (MDR's) in microdroplets provide optical feedback for nonlinear processes such as stimulated Raman scattering (SRS). The SRS signal from weaker gain modes or from the minority species in a binary mixture droplet is small, because of depletion of the pump beam by the strongest-gain Raman mode. We present an effective- average Raman gain formula and discuss the factors that contribute to the enhancement of SRS intensity. Spatial overlap between pump wave and SRS wave is an important factor in determining the SRS intensity. We have observed that in a binary mixture microdroplet, the SRS of the majority species is more efficient (because of good spatial overlap) in pumping the minority species than the input laser itself. Laser-induced distortion can couple light efficiently into a droplet. We have used a variable number (3 - 6) of mode-locked 100-psec laser pulses focused on the droplet rim. The SRS emission from a minority species increases as the number of input pulses is increased, because cumulative laser-induced surface distortion couples more energy into the droplet. SRS signal at the Stokes shift of a weaker gain mode or of the mode of a minority species can be enhanced by seeding light at the SRS wavelengths. The seed signal is obtained from the fluorescence of a dye added to the microdroplet or from external coupling of light into the droplet. A lasing dye (Rhodamine 6G) is added to pure ethanol droplet. By using an excimer-pumped tunable dye laser as the excitation source, the weaker gain C-C-O mode (882 cm-1 Stokes shift) of ethanol is overlapped spectrally with the fluorescence and lasing of R6G. The SRS signal of the C-C-O mode is enhanced, because (1) the fluorescence of R6G at the SRS wavelength adds to the spontaneous SRS emission and (2) the gain from population inversion adds to the Raman gain. We have also observed enhanced SRS emission from a minority species (benzene) in dodecane by using internal dye seeding

  13. In-Vivo functional optical-resolution photoacoustic microscopy with stimulated Raman scattering fiber-laser source.

    PubMed

    Hajireza, Parsin; Forbrich, Alexander; Zemp, Roger

    2014-02-01

    In this paper a multi-wavelength optical-resolution photoacoustic microscopy (OR-PAM) system using stimulated Raman scattering is demonstrated for both phantom and in vivo imaging. A 1-ns pulse width ytterbium-doped fiber laser is coupled into a single-mode polarization maintaining fiber. Discrete Raman-shifted wavelength peaks extending to nearly 800 nm are generated with pulse energies sufficient for OR-PAM imaging. Bandpass filters are used to select imaging wavelengths. A dual-mirror galvanometer system was used to scan the focused outputs across samples of carbon fiber networks, 200μm dye-filled tubes, and Swiss Webster mouse ears. Photoacoustic signals were collected in transmission mode and used to create maximum amplitude projection C-scan images. Double dye experiments and in vivo oxygen saturation estimation confirmed functional imaging potential.

  14. In-Vivo functional optical-resolution photoacoustic microscopy with stimulated Raman scattering fiber-laser source.

    PubMed

    Hajireza, Parsin; Forbrich, Alexander; Zemp, Roger

    2014-02-01

    In this paper a multi-wavelength optical-resolution photoacoustic microscopy (OR-PAM) system using stimulated Raman scattering is demonstrated for both phantom and in vivo imaging. A 1-ns pulse width ytterbium-doped fiber laser is coupled into a single-mode polarization maintaining fiber. Discrete Raman-shifted wavelength peaks extending to nearly 800 nm are generated with pulse energies sufficient for OR-PAM imaging. Bandpass filters are used to select imaging wavelengths. A dual-mirror galvanometer system was used to scan the focused outputs across samples of carbon fiber networks, 200μm dye-filled tubes, and Swiss Webster mouse ears. Photoacoustic signals were collected in transmission mode and used to create maximum amplitude projection C-scan images. Double dye experiments and in vivo oxygen saturation estimation confirmed functional imaging potential. PMID:24575346

  15. In-Vivo functional optical-resolution photoacoustic microscopy with stimulated Raman scattering fiber-laser source

    PubMed Central

    Hajireza, Parsin; Forbrich, Alexander; Zemp, Roger

    2014-01-01

    In this paper a multi-wavelength optical-resolution photoacoustic microscopy (OR-PAM) system using stimulated Raman scattering is demonstrated for both phantom and in vivo imaging. A 1-ns pulse width ytterbium-doped fiber laser is coupled into a single-mode polarization maintaining fiber. Discrete Raman-shifted wavelength peaks extending to nearly 800 nm are generated with pulse energies sufficient for OR-PAM imaging. Bandpass filters are used to select imaging wavelengths. A dual-mirror galvanometer system was used to scan the focused outputs across samples of carbon fiber networks, 200μm dye-filled tubes, and Swiss Webster mouse ears. Photoacoustic signals were collected in transmission mode and used to create maximum amplitude projection C-scan images. Double dye experiments and in vivo oxygen saturation estimation confirmed functional imaging potential. PMID:24575346

  16. Dispersion-based stimulated Raman scattering spectroscopy, holography, and optical coherence tomography (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Robles, Francisco E.; Fischer, Martin C.; Warren, Warren S.

    2016-03-01

    Stimulated Raman scattering (SRS) enables fast, high resolution imaging of chemical constituents important to biological structures and functional processes. While this technology has shown remarkable potential, it is currently limited to point scanning and can only probe a few Raman bands at a time. In this work we take a fundamentally different approach to detecting the small nonlinear signals based on dispersion effects that accompany the loss/gain processes in SRS. We use a modified pump-probe system (pulses with duration of ~0.5 ps and 75 fs, respectively) with interferometric detection in the Fourier-domain to demonstrate that the dispersive measurements are more robust to noise (e.g., laser noise) compared to conventional amplitude measurements, which in turn permits facile spectral and spatial multiplexing. Results show that it is possible to assess a broadband dispersion spectrum (currently limited to ~400 cm-1) with a single laser shot or spectrometer acquisition (20-50 µs). For molecular imaging with broadband spectral information, we achieve spatial pixel rates of 2.5 kHz, and will discuss how this can be further improved to 20-50 kHz. We also combine SRS with optical coherence tomography (OCT) (molecular and structural information are rendered from the same data), which enables axial multiplexing by coherence gating and paves the way for volumetric biochemical imaging. The approach is tested on a thin water-and-oil phantom, a thick scattering polystyrene bead phantom, and thick freshly excised human adipose tissue. Finally, we will outline other opportunities for spatial multiplexing using wide-field holography and spectroscopic-OCT, which would massively parallelize the spatial and spectral information. The combination of dispersion-based SRS and phase imaging has the potential to enable faster wide-area and volumetric molecular imaging. Such methods would be valuable in a clinical setting for many applications.

  17. Direct Observation of Single DNA Structural Alterations at Low Forces with Surface-Enhanced Raman Scattering

    PubMed Central

    Rao, Satish; Raj, Saurabh; Cossins, Benjamin; Marro, Monica; Guallar, Victor; Petrov, Dmitri

    2013-01-01

    DNA experiences numerous mechanical events, necessitating single-molecule force spectroscopy techniques to provide insight into DNA mechanics as a whole system. Inherent Brownian motion limits current force spectroscopy methods from observing possible bond level structural changes. We combine optical trapping and surface-enhanced Raman scattering to establish a direct relationship between DNA’s extension and structure in the low force, entropic regime. A DNA molecule is trapped close to a surface-enhanced Raman scattering substrate to facilitate a detectable Raman signal. DNA Raman modes shift in response to applied force, indicating phosphodiester mechanical alterations. Molecular dynamic simulations confirm the local structural alterations and the Raman sensitive band identified experimentally. The combined Raman and force spectroscopy technique, to our knowledge, is a novel methodology that can be generalized to all single-molecule studies. PMID:23332068

  18. Silicon nanohybrid-based surface-enhanced Raman scattering sensors.

    PubMed

    Wang, Houyu; Jiang, Xiangxu; Lee, Shuit-Tong; He, Yao

    2014-11-01

    Nanomaterial-based surface-enhanced Raman scattering (SERS) sensors are highly promising analytical tools, capable of ultrasensitive, multiplex, and nondestructive detection of chemical and biological species. Extensive efforts have been made to design various silicon nanohybrid-based SERS substrates such as gold/silver nanoparticle (NP)-decorated silicon nanowires, Au/Ag NP-decorated silicon wafers (AuNP@Si), and so forth. In comparison to free AuNP- and AgNP-based SERS sensors, the silicon nanohybrid-based SERS sensors feature higher enhancement factors (EFs) and excellent reproducibility, since SERS hot spots are efficiently coupled and stabilized through interconnection to the semiconducting silicon substrates. Consequently, in the past decade, giant advancements in the development of silicon nanohybrid-based SERS sensors have been witnessed for myriad sensing applications. In this review, the representative achievements related to the design of high-performance silicon nanohybrid-based SERS sensors and their use for chemical and biological analysis are reviewed in a detailed way. Furthermore, the major opportunities and challenges in this field are discussed from a broad perspective and possible future directions.

  19. Raman Scattering from Atmospheric Nitrogen in the Stratosphere

    NASA Technical Reports Server (NTRS)

    Garvey, M. J.; Kent, G. S.

    1973-01-01

    The Mark II laser radar system at Kingston, Jamaica, has been used to make observations on the Raman shifted line from atmospheric nitrogen at 828.5 nm. The size of the system makes it possible to detect signals from heights of up to 40 kilometres. The effects of aerosol scattering observed using a single wavelength are almost eliminated, and a profile of nitrogen density may be obtained. Assuming a constant mixing ratio, this may be interpreted as a profile of atmospheric density whose accuracy is comparable to that obtained from routine meteorological soundings. In order to obtain an accurate profile several interfering effects have had to be examined and, where necessary, eliminated. These include: 1) Fluorescence in optical components 2) Leakage of signal at 694.3 nm. 3) Overload effects and non-linearities in the receiving and counting electronics. Most of these effects have been carefully examined and comparisons are being made between the observed atmospheric density profiles and local meteorological radio-sonde measurements. Good agreement has been obtained over the region of overlap (15 - 30 KID), discrepancies being of the same order as the experimental accuracy (1-10%), depending on height and length of period of observation.

  20. Graphene thickness-controlled photocatalysis and surface enhanced Raman scattering.

    PubMed

    Kuo, Cheng-Chi; Chen, Chun-Hu

    2014-11-01

    Exceptional photocatalytic enhancement of graphene-semiconductor composites has been widely reported, but our understanding of the role that graphene plays in this enhancement remains limited, which arises from the difficulty of precisely controlling graphene hybridization. Here we present a general platform of a graphene-semiconductor hybrid panel (GHP) system wherein a precise number of layers of graphene are hybridized with photoactive semiconductors (e.g. TiO2, ZnO) to study systematically how graphene affects the photocatalysis. The results show that the graphene enhancement of the photocatalysis depends on the number of graphene layers, with the maximum performance observed at 3 layers. Photodeposited indicators of gold particles further reveal that graphene thickness governs the density of photocatalytic sites and charge transfer efficiency at the graphene-semiconductor interfaces. We suggest that quantized energy levels caused by different numbers of stacked graphene sheets along the vector normal to the graphene basal plane affect the charge transfer routes and lead to the graphene thickness-controlled photocatalysis. GHP substrates deposited with gold particles are promising, uniform substrates for surface enhanced Raman scattering (SERS) applications with the enhancement factor as high as ∼10(8) on 3-layer graphene.

  1. Hierarchical electrohydrodynamic structures for surface-enhanced Raman scattering.

    PubMed

    Goldberg-Oppenheimer, Pola; Mahajan, Sumeet; Steiner, Ullrich

    2012-06-19

    Surface enhanced Raman scattering (SERS) is a well-established spectroscopic technique that requires nanoscale metal structures to achieve high signal sensitivity. While most SERS substrates are manufactured by conventional lithographic methods, the development of a cost-effective approach to create nanostructured surfaces is a much sought-after goal in the SERS community. Here, a method is established to create controlled, self-organized, hierarchical nanostructures using electrohydrodynamic (HEHD) instabilities. The created structures are readily fine-tuned, which is an important requirement for optimizing SERS to obtain the highest enhancements. HEHD pattern formation enables the fabrication of multiscale 3D structured arrays as SERS-active platforms. Importantly, each of the HEHD-patterned individual structural units yield a considerable SERS enhancement. This enables each single unit to function as an isolated sensor. Each of the formed structures can be effectively tuned and tailored to provide high SERS enhancement, while arising from different HEHD morphologies. The HEHD fabrication of sub-micrometer architectures is straightforward and robust, providing an elegant route for high-throughput biological and chemical sensing. PMID:22488810

  2. Sputtered gold films for surface-enhanced Raman scattering

    SciTech Connect

    Maya, L.; Vallet, C.E.; Lee, Y.H.

    1997-03-01

    Sputtered gold films in a pure form or as nanocomposites in silica or silicon nitride were screened for surface-enhanced Raman scattering (SERS) activity using Rhodamine 6G as a probe. The films were prepared by sputtering pure gold or solidified Au{endash}Si alloys in plasmas generated in a dc glow discharge apparatus. The plasmas were produced with argon, nitrogen, or argon{endash}oxygen as the sputtering gas to directly deposit gold films or in the latter case a gold oxide intermediate. The alloys produce nanocomposite films in a silicon nitride or silica matrix depending on the plasma gas. SERS activity was detected in some of the films thus leading to a search for the critical parameters that controlled this phenomenon. The films were characterized by profilometry, x-ray diffraction, and atomic force microscopy. SERS activity was found to be correlated to crystallite size in the 10{endash}25 nm range and to roughness larger than 15 nm, and it was independent of film thickness. Sputtered gold films, particularly those containing the gold as a nanocomposite in silica are attractive media for SERS because of excellent adherence, ruggedness, and simplicity in preparation. {copyright} {ital 1997 American Vacuum Society.}

  3. Tip-enhanced Raman spectroscopic imaging of patterned thiol monolayers

    PubMed Central

    Stadler, Johannes; Schmid, Thomas; Opilik, Lothar; Kuhn, Phillip; Dittrich, Petra S

    2011-01-01

    Summary Full spectroscopic imaging by means of tip-enhanced Raman spectroscopy (TERS) was used to measure the distribution of two isomeric thiols (2-mercaptopyridine (2-PySH) and 4-mercaptopyridine (4-PySH)) in a self-assembled monolayer (SAM) on a gold surface. From a patterned sample created by microcontact printing, an image with full spectral information in every pixel was acquired. The spectroscopic data is in good agreement with the expected molecular distribution on the sample surface due to the microcontact printing process. Using specific marker bands at 1000 cm−1 for 2-PySH and 1100 cm−1 for 4-PySH, both isomers could be localized on the surface and semi-quantitative information was deduced from the band intensities. Even though nanometer size resolution information was not required, the large signal enhancement of TERS was employed here to detect a monolayer coverage of weakly scattering analytes that were not detectable with normal Raman spectroscopy, emphasizing the usefulness of TERS. PMID:22003457

  4. Computer simulation of surface-enhanced Raman scattering in nanostructured metamaterials

    SciTech Connect

    Boyarintsev, S. O.; Sarychev, A. K.

    2011-12-15

    The simulation of local field fluctuations and surface-enhanced Raman scattering in percolation systems at the percolation threshold is described. An approximate real-space renormalization group method was used in the simulation. It allows one to radically reduce the computation time compared to an exact calculation and to obtain detailed information about the electromagnetic field. The local fields in real macroscopic systems can be calculated by using this approximation. A computer simulation of the local fields in metal island (percolation) films has been performed by the developed method. The calculation has confirmed the existence of giant local field fluctuations. In turn, the local electric field excites Raman scattering. The local fields of surface-enhanced Raman scattering have been calculated for the first time. The dependence of the Raman scattering enhancement factor on the reference frequency and Stokes shift has been derived. An experimental observation of this dependence could be considered as a confirmation of the electromagnetic nature of the enhancement.

  5. Laboratory Studies of Perchlorate Deliquescence and Water Adsorption at the Surface of Mars with Raman Scattering

    NASA Astrophysics Data System (ADS)

    Nikolakakos, G.; Whiteway, J. A.

    2016-09-01

    Laser Raman scattering has been applied in order to experimentally study the exchange of water between the surface and atmosphere on Mars. Results show that both deliquescence of salts and adsorption by minerals are likely currently active processes.

  6. Influence of stimulated Raman scattering on the conversion efficiency in four wave mixing

    SciTech Connect

    Wunderlich, R.; Moore, M.A.; Garrett, W.R.; Payne, M.G.

    1988-01-01

    Secondary nonlinear optical effects following parametric four wave mixing in sodium vapor are investigated. The generated ultraviolet radiation induces stimulated Raman scattering and other four wave mixing process. Population transfer due to Raman transitions strongly influences the phase matching conditions for the primary mixing process. Pulse shortening and a reduction in conversion efficiency are observed. 8 refs., 3 figs.

  7. A note on two-phonon coherent anti-stokes Raman scattering

    SciTech Connect

    Shen, Y. R.

    1981-01-01

    Difference-frequency mixing of two pump waves can in principle excite two coherent phonon waves via the parametric process. Finally, only when the phonon excitation is small can the nonlinear susceptibility of two-phonon coherent anti-Stokes Raman scattering be described as proportional to the product of two Raman tensors.

  8. Accounting for Transverse Inhomogeneity of Radiation Beams in Laser Raman Scattering

    NASA Astrophysics Data System (ADS)

    Apanasevich, P. A.; Dashkevich, V. I.; Timofeeva, G. I.

    2016-05-01

    A simple method of accounting for transverse inhomogeneity of the pump and Stokes radiation beams in the description of stimulated Raman scattering (SRS) using intensity-transfer equations for interacting beams is proposed. Features of the method are illustrated using the calculated dependences of the Raman laser efficiency on the output mirror reflectivity and the pump pulse energy as examples.

  9. Facile Synthesis of Uniform Raspberry-Like Gold Nanoparticles for High Performance Surface Enhanced Raman Scattering.

    PubMed

    Rong, Yun; Zhang, Lei; Liu, Zhenzhong; Dai, Liwei; Huang, Youju; Chen, Tao

    2016-06-01

    Hierarchical Au nanostructures have attracted considerable attention owing to their rich hot-spots in inherent structures that have found various applications in surface-enhanced Raman scattering (SERS) based sensing and imaging. Herein we facilely synthesized uniform hierarchical raspberry-like Au nanostructures with tunable size via a seed-mediated growth approach employing a binary mixture of quaternized chitosan (QCS) and 5-bromosalicylic acid (5-BrSA). 5-BrSA plays an important role in tuning shapes and improving uniformity of resultant gold nanoparticles (AuNPs). The obtained raspberry-like Au nanostructures have a spherical profile and randomly arranged protrusions on the outsides, and their size can be finely tuned in a range from 50 to 120 nm. The rough surfaces of the special raspberry-like Au nanostructures endow them higher SERS performance than spherical Au spheres with smooth surfaces, which is promising for the application of SERS based sensors and optical imaging. PMID:27427615

  10. Interferometric polarization coherent anti-Stokes Raman scattering (IP-CARS) microscopy.

    PubMed

    Lu, Fake; Zheng, Wei; Sheppard, Colin; Huang, Zhiwei

    2008-03-15

    We report a novel interferometry-based polarization coherent anti-Stokes Raman scattering (IP-CARS) implementation for effectively suppressing the nonresonant background while significantly amplifying the resonant signal for vibrational imaging. By modulating the phase difference between the two interference CARS signals generated from the same sample and measuring the peak-to-peak intensity of the periodically modulated interference CARS signal, the IP-CARS technique yields a sixfold improvement in the signal-to-background ratio compared with conventional CARS while providing an approximately 20-fold amplification of the resonant CARS signal compared with conventional polarization CARS. We demonstrate this method by imaging 4.69 microm polystyrene beads and unstained human epithelial cells immersed in water. PMID:18347723

  11. Finding electromagnetic and chemical enhancement factors of surface-enhanced Raman scattering.

    PubMed

    Dvoynenko, Mykhaylo M; Wang, Juen-Kai

    2007-12-15

    The authors report two methods to determine electromagnetic and chemical enhancement factors in surface-enhanced Raman scattering (SERS), which are based on saturation property and decay dynamics of photoluminescence and concurrent measurements of photoluminescence and resonance Raman scattering intensities. Considerations for experimental implementation are discussed. This study is expected to facilitate the understanding of SERS mechanisms and the advancement of the usage of SERS in chemical and biological sensor applications.

  12. A new class of nontoxic nanoparticle tags based on surface enhanced Raman scattering

    NASA Astrophysics Data System (ADS)

    Qian, X.-M.; Ansari, D.; Nie, Shuming

    2007-02-01

    The advance of nanotechnology has boosted the development of ultra-sensitive biosensors for biomedical applications. Most recently, optical detection based biosensors have been demonstrated in medical imaging and diagnosis employing nanocrystals such as fluorescent quantum dots (QDs) and plasmon resonant metal nanoparticles to achieve femto-molar detection. An intriguing but far less explored approach for biological diagnostics relies on an emerging ultrasensitive technology -- surface enhanced Raman scattering (SERS) spectroscopy. We have developed a stable SERS nano-tag by grafting hydrophilic polymer to gold nanoparticle-dye molecule complexes to preserve the spectral signature and fully control the aggregation states. The light-emitting power and scattered light of both QDs and SERS nano-tags have been recorded under the same experimental conditions using dark field microscope, fluorometer, and Raman instrument. A comparison in brightness, sensitivity level, and quantum efficiency between SERS nano-tags and near infrared (NIR) QDs has been assessed on both bulk colloidal solution and single particle measurements. Well-designed SERS nano-tags exhibit excellent advantages over NIR QDs.

  13. Multiplex coherent anti-Stokes Raman scattering microscopy on lipid droplets in HeLa cells

    NASA Astrophysics Data System (ADS)

    Rinia, Hilde A.; Burger, Koert N. J.; Bonn, Mischa; Müller, Michiel

    2007-07-01

    Lipid droplets have become a major research topic recently, as they are found to be involved in obesity related diseases. Most of this research has been focused on the localization of the proteins playing a role in lipid droplet formation or breakdown. The role of different lipid species however remains unclear because it is difficult to distinguish different fatty acids with the present microscopy techniques. Coherent Anti-Stokes Raman scattering (CARS) is the non-linear analogue of spontaneous Raman scattering. Multiplex CARS microscopy can provide quantitative, chemical and physical information, making it an excellent tool to study the composition and thermodynamic phase of lipid droplets. To investigate the potential of CARS in this field, we have incubated HeLa cells with four different fatty acids, varying in saturation. The fatty acids were internalized by the cells and stored as lipid droplets, which we imaged with multiplex CARS microscopy. We were able to distinguish either of the fatty acids as such in lipid droplets inside the cells. Furthermore, we found that solid phase fatty acids were fluidized when present in lipid droplets. This illustrates the potential of CARS microscopy to elucidate the possible role of the chemistry of fatty acids in lipid droplet regulation.

  14. Kinetically driven Raman scattering in short, bi-speckle laser-plasma interaction experiments

    NASA Astrophysics Data System (ADS)

    Glize, Kevin; Rousseaux, Christophe; Baton, Sophie; Dervieux, Vincent; Lancia, Livia

    2015-11-01

    In order to investigate collective speckles behavior in laser-plasma interaction, bi-speckle experiments have been performed using the ELFIE facility (LULI). Two independent laser pulses (1.06 nm, 1.5 ps FWHM) interact with preformed He plasma (0.06 nc, 300 eV). The first beam drives stimulated Raman scattering, while the second, which its intensity is set near SRS threshold, is focused near the first one (typically 90 μm). The interaction, with crossed and parallel polarization, was studied for both variation of the time delay and the lateral distance between the two pulses, featuring a highly resolved Thomson-scattering diagnostic and backward Raman imaging. It is shown that the kinetic perturbations are of primary importance on triggering SRS in the weak speckle, which exhibits SRS instability up to an expectedly long time delay after the interaction of the strong one. The experimental results will be discussed with the help of 2D PIC simulations (CALDER code).

  15. Optical diagnosis and characterization of dental caries with polarization-resolved hyperspectral stimulated Raman scattering microscopy.

    PubMed

    Wang, Zi; Zheng, Wei; Hsu, Stephen Chin-Ying; Huang, Zhiwei

    2016-04-01

    We report the utility of a rapid polarization-resolved hyperspectral stimulated Raman scattering (SRS) imaging technique developed for optical diagnosis and characterization of dental caries in the tooth. Hyperspectral SRS images (512 × 512 pixels) of the tooth covering both the fingerprint (800-1800 cm(-1)) and high-wavenumber (2800-3600 cm(-1)) regions can be acquired within 15 minutes, which is at least 10(3) faster in imaging speed than confocal Raman mapping. Hyperspectral SRS imaging uncovers the biochemical distributions and variations across the carious enamel in the tooth. SRS imaging shows that compared to the sound enamel, the mineral content in the body of lesion decreases by 55%; while increasing up to 110% in the surface zone, indicating the formation of a hyper-mineralized layer due to the remineralization process. Further polarized SRS imaging shows that the depolarization ratios of hydroxyapatite crystals (ν 1-PO4 (3-) of SRS at 959 cm(-1)) of the tooth in the sound enamel, translucent zone, body of lesion and the surface zone are 0.035 ± 0.01, 0.052 ± 0.02, 0.314 ± 0.1, 0.038 ± 0.02, respectively, providing a new diagnostic criterion for discriminating carious lesions from sound enamel in the teeth. This work demonstrates for the first time that the polarization-resolved hyperspectral SRS imaging technique can be used for quantitatively determining tooth mineralization levels and discriminating carious lesions from sound enamel in a rapid fashion, proving its promising potential of early detection and diagnosis of dental caries without labeling. PMID:27446654

  16. Optical diagnosis and characterization of dental caries with polarization-resolved hyperspectral stimulated Raman scattering microscopy

    PubMed Central

    Wang, Zi; Zheng, Wei; Hsu, Stephen Chin-Ying; Huang, Zhiwei

    2016-01-01

    We report the utility of a rapid polarization-resolved hyperspectral stimulated Raman scattering (SRS) imaging technique developed for optical diagnosis and characterization of dental caries in the tooth. Hyperspectral SRS images (512 × 512 pixels) of the tooth covering both the fingerprint (800-1800 cm−1) and high-wavenumber (2800-3600 cm−1) regions can be acquired within 15 minutes, which is at least 103 faster in imaging speed than confocal Raman mapping. Hyperspectral SRS imaging uncovers the biochemical distributions and variations across the carious enamel in the tooth. SRS imaging shows that compared to the sound enamel, the mineral content in the body of lesion decreases by 55%; while increasing up to 110% in the surface zone, indicating the formation of a hyper-mineralized layer due to the remineralization process. Further polarized SRS imaging shows that the depolarization ratios of hydroxyapatite crystals (ν1-PO43- of SRS at 959 cm−1) of the tooth in the sound enamel, translucent zone, body of lesion and the surface zone are 0.035 ± 0.01, 0.052 ± 0.02, 0.314 ± 0.1, 0.038 ± 0.02, respectively, providing a new diagnostic criterion for discriminating carious lesions from sound enamel in the teeth. This work demonstrates for the first time that the polarization-resolved hyperspectral SRS imaging technique can be used for quantitatively determining tooth mineralization levels and discriminating carious lesions from sound enamel in a rapid fashion, proving its promising potential of early detection and diagnosis of dental caries without labeling. PMID:27446654

  17. Detecting mineral content in turbid medium using nonlinear Raman imaging: feasibility study

    PubMed Central

    Arora, Rajan; Petrov, Georgi I.; Noojin, Gary D.; Thomas, Patrick A.; Denton, Michael L.; Rockwell, Benjamin A.; Thomas, Robert J.; Yakovlev, Vladislav V.

    2012-01-01

    Osteoporosis is a bone disease characterized by reduced mineral content with resulting changes in bone architecture, which in turn increases the risk of bone fracture. Raman spectroscopy has an intrinsic sensitivity to the chemical content of the bone, but its application to study bones in vivo is limited due to strong optical scattering in tissue. It has been proposed that Raman excitation with photoacoustic detection can successfully address the problem of chemically specific imaging in deep tissue. In this report, the principal possibility of photoacoustic imaging for detecting mineral content is evaluated. PMID:22337734

  18. Models for coherent anti-Stokes Raman scattering in Raman devices and in spectroscopy

    NASA Astrophysics Data System (ADS)

    Vermeulen, Nathalie; Debaes, Christof; Thienpont, Hugo

    2010-06-01

    We present our latest findings on the nature and behavior of CARS in active Raman devices, such as Raman converters and Raman lasers, which operate at exact Raman resonance. We demonstrate that the CARS mechanism in these devices actually comprises two opposite and competing interactions, which respectively create and annihilate phonons in the Raman-active medium. Furthermore, we show that both the phase mismatch of the CARS process and the level of pump depletion determine which of these two interactions takes place along the fields' propagation path in the Raman devices. Finally, we compare this CARS model with the model used by the CARS spectroscopy community, and explain that the difference between both models is mainly due to the fact that "CARS" in the context of Raman devices refers to Ramanresonant four-wave mixing, whereas "CARS" in the context of spectroscopy often denotes a two-step Raman interaction.

  19. Image-guided Raman spectroscopic recovery of canine cortical bone contrast in situ

    PubMed Central

    Srinivasan, Subhadra; Schulmerich, Matthew; Cole, Jacqueline H.; Dooley, Kathryn A.; Kreider, Jaclynn M.; Pogue, Brian W.; Morris, Michael D.; Goldstein, Steven A.

    2009-01-01

    Raman scattering provides valuable biochemical and molecular markers for studying bone tissue composition with use in predicting fracture risk in osteoporosis. Raman tomography can image through a few centimeters of tissue but is limited by low spatial resolution. X-ray computed tomography (CT) imaging can provide high-resolution image-guidance of the Raman spectroscopic characterization, which enhances the quantitative recovery of the Raman signals, and this technique provides additional information to standard imaging methods. This hypothesis was tested in data measured from Teflon® tissue phantoms and from a canine limb. Image-guided Raman spectroscopy (IG-RS) of the canine limb using CT images of the tissue to guide the recovery recovered a contrast of 145:1 between the cortical bone and background. Considerably less contrast was found without the CT image to guide recovery. This study presents the first known IG-RS results from tissue and indicates that intrinsically high contrasts (on the order of a hundred fold) are available. PMID:18679495

  20. In Vivo Metabolic Fingerprinting of Neutral Lipids with Hyperspectral Stimulated Raman Scattering Microscopy

    PubMed Central

    2015-01-01

    Metabolic fingerprinting provides valuable information on the physiopathological states of cells and tissues. Traditional imaging mass spectrometry and magnetic resonance imaging are unable to probe the spatial-temporal dynamics of metabolites at the subcellular level due to either lack of spatial resolution or inability to perform live cell imaging. Here we report a complementary metabolic imaging technique that is based on hyperspectral stimulated Raman scattering (hsSRS). We demonstrated the use of hsSRS imaging in quantifying two major neutral lipids: cholesteryl ester and triacylglycerol in cells and tissues. Our imaging results revealed previously unknown changes of lipid composition associated with obesity and steatohepatitis. We further used stable-isotope labeling to trace the metabolic dynamics of fatty acids in live cells and live Caenorhabditis elegans with hsSRS imaging. We found that unsaturated fatty acid has preferential uptake into lipid storage while saturated fatty acid exhibits toxicity in hepatic cells. Simultaneous metabolic fingerprinting of deuterium-labeled saturated and unsaturated fatty acids in living C. elegans revealed that there is a lack of interaction between the two, unlike previously hypothesized. Our findings provide new approaches for metabolic tracing of neutral lipids and their precursors in living cells and organisms, and could potentially serve as a general approach for metabolic fingerprinting of other metabolites. PMID:24869754

  1. Influence of reabsorption and reemission on stimulated Raman scattering of polymethine dyes in multiple scattering media

    SciTech Connect

    Yashchuk, V P; Komyshan, A O; Smaliuk, A P; Prygodiuk, O A; Ishchenko, A A; Olkhovyk, L A

    2013-12-31

    It is shown that reabsorption of the luminescence radiation in the range of its overlapping with the absorption spectrum and the following reemission to a long-wavelength range may noticeably affect the process of stimulated Raman scattering (SRS) in polymethine dyes in multiple scattering media (MSM). This is related to the fact that SRS in such media occurs jointly with the random lasing (RL), which favors SRS and makes up with it a united nonlinear process. Reemission into the long-wavelength spectrum range amplified in MSM causes the RL spectrum to shift to longer wavelengths and initiates the long-wavelength band of RL, in which a main part of the lasing energy is concentrated. This weakens or completely stops the SRS if the band is beyond the range of possible spectral localisation of Stokes lines. This process depends on the efficiency of light scattering, dye concentration, temperature and pump intensity; hence, there exist optimal values of these parameters for obtaining SRS in MSM. (nonlinear optical phenomena)

  2. Molecular diffusion in the human nail measured by stimulated Raman scattering microscopy

    PubMed Central

    Chiu, Wing Sin; Belsey, Natalie A.; Garrett, Natalie L.; Moger, Julian; Delgado-Charro, M. Begoña; Guy, Richard H.

    2015-01-01

    The effective treatment of diseases of the nail remains an important unmet medical need, primarily because of poor drug delivery. To address this challenge, the diffusion, in real time, of topically applied chemicals into the human nail has been visualized and characterized using stimulated Raman scattering (SRS) microscopy. Deuterated water (D2O), propylene glycol (PG-d8), and dimethyl sulphoxide (DMSO-d6) were separately applied to the dorsal surface of human nail samples. SRS microscopy was used to image D2O, PG-d8/DMSO-d6, and the nail through the O-D, -CD2, and -CH2 bond stretching Raman signals, respectively. Signal intensities obtained were measured as functions of time and of depth into the nail. It was observed that the diffusion of D2O was more than an order of magnitude faster than that of PG-d8 and DMSO-d6. Normalization of the Raman signals, to correct in part for scattering and absorption, permitted semiquantitative analysis of the permeation profiles and strongly suggested that solvent diffusion diverged from classical behavior and that derived diffusivities may be concentration dependent. It appeared that the uptake of solvent progressively undermined the integrity of the nail. This previously unreported application of SRS has permitted, therefore, direct visualization and semiquantitation of solvent penetration into the human nail. The kinetics of uptake of the three chemicals studied demonstrated that each altered its own diffusion in the nail in an apparently concentration-dependent fashion. The scale of the unexpected behavior observed may prove beneficial in the design and optimization of drug formulations to treat recalcitrant nail disease. PMID:26056283

  3. Molecular diffusion in the human nail measured by stimulated Raman scattering microscopy.

    PubMed

    Chiu, Wing Sin; Belsey, Natalie A; Garrett, Natalie L; Moger, Julian; Delgado-Charro, M Begoña; Guy, Richard H

    2015-06-23

    The effective treatment of diseases of the nail remains an important unmet medical need, primarily because of poor drug delivery. To address this challenge, the diffusion, in real time, of topically applied chemicals into the human nail has been visualized and characterized using stimulated Raman scattering (SRS) microscopy. Deuterated water (D2O), propylene glycol (PG-d8), and dimethyl sulphoxide (DMSO-d6) were separately applied to the dorsal surface of human nail samples. SRS microscopy was used to image D2O, PG-d8/DMSO-d6, and the nail through the O-D, -CD2, and -CH2 bond stretching Raman signals, respectively. Signal intensities obtained were measured as functions of time and of depth into the nail. It was observed that the diffusion of D2O was more than an order of magnitude faster than that of PG-d8 and DMSO-d6. Normalization of the Raman signals, to correct in part for scattering and absorption, permitted semiquantitative analysis of the permeation profiles and strongly suggested that solvent diffusion diverged from classical behavior and that derived diffusivities may be concentration dependent. It appeared that the uptake of solvent progressively undermined the integrity of the nail. This previously unreported application of SRS has permitted, therefore, direct visualization and semiquantitation of solvent penetration into the human nail. The kinetics of uptake of the three chemicals studied demonstrated that each altered its own diffusion in the nail in an apparently concentration-dependent fashion. The scale of the unexpected behavior observed may prove beneficial in the design and optimization of drug formulations to treat recalcitrant nail disease.

  4. Spontaneous and stimulated Raman scattering in ZnWO{sub 4} crystals

    SciTech Connect

    Basiev, Tasoltan T; Karasik, Aleksandr Ya; Sobol, A A; Chunaev, D S; Shukshin, V E

    2011-04-30

    Spontaneous and stimulated Raman scattering (SRS) are studied in ZnWO{sub 4} crystals with a wolframite structure. The polarised Raman scattering spectra corresponding to all the six independent Raman tensor components are measured. The frequencies of the complete set of vibrational modes are identified. The threshold pump energies for SRS in ZnWO{sub 4} and KGd(WO{sub 4}){sub 2} crystals are measured upon excitation by picosecond 1047-nm pulses of a Nd:YLF laser. The SRS gains for ZnWO{sub 4} crystals are determined based on the measured thresholds and spectroscopic parameters of the crystals. (nonlinear optics phenomena)

  5. Impulsive rotational Raman scattering of N2 by a remote "air laser" in femtosecond laser filament.

    PubMed

    Ni, Jielei; Chu, Wei; Zhang, Haisu; Zeng, Bin; Yao, Jinping; Qiao, Lingling; Li, Guihua; Jing, Chenrui; Xie, Hongqiang; Xu, Huailiang; Cheng, Ya; Xu, Zhizhan

    2014-04-15

    We report on experimental realization of impulsive rotational Raman scattering from neutral nitrogen molecules in a femtosecond laser filament using an intense self-induced white-light seeding "air laser" generated during the filamentation of an 800 nm Ti:sapphire laser in nitrogen gas. The impulsive rotational Raman fingerprint signals are observed with a maximum conversion efficiency of ∼0.8%. Our observation provides a promising way of remote identification and location of chemical species in the atmosphere by a rotational Raman scattering of molecules. PMID:24978965

  6. Preclinical evaluation of Raman nanoparticle biodistribution for their potential use in clinical endoscopy imaging.

    PubMed

    Zavaleta, Cristina L; Hartman, Keith B; Miao, Zheng; James, Michelle L; Kempen, Paul; Thakor, Avnesh S; Nielsen, Carsten H; Sinclair, Robert; Cheng, Zhen; Gambhir, Sanjiv S

    2011-08-01

    Raman imaging offers unsurpassed sensitivity and multiplexing capabilities. However, its limited depth of light penetration makes direct clinical translation challenging. Therefore, a more suitable way to harness its attributes in a clinical setting would be to couple Raman spectroscopy with endoscopy. The use of an accessory Raman endoscope in conjunction with topically administered tumor-targeting Raman nanoparticles during a routine colonoscopy could offer a new way to sensitively detect dysplastic lesions while circumventing Raman's limited depth of penetration and avoiding systemic toxicity. In this study, the natural biodistribution of gold surface-enhanced Raman scattering (SERS) nanoparticles is evaluated by radiolabeling them with (64) Cu and imaging their localization over time using micropositron emission tomography (PET). Mice are injected either intravenously (IV) or intrarectally (IR) with approximately 100 microcuries (μCi) (3.7 megabecquerel (MBq)) of (64) Cu-SERS nanoparticles and imaged with microPET at various time points post injection. Quantitative biodistribution data are obtained as % injected dose per gram (%ID g(-1)) from each organ, and the results correlate well with the corresponding microPET images, revealing that IV-injected mice have significantly higher uptake (p < 0.05) in the liver (5 h = 8.96% ID g(-1); 24 h = 8.27% ID g(-1)) than IR-injected mice (5 h = 0.09% ID g(-1); 24 h = 0.08% ID g(-1)). IR-injected mice show localized uptake in the large intestine (5 h = 10.37% ID g(-1); 24 h = 0.42% ID g(-1)) with minimal uptake in other organs. Raman imaging of excised tissues correlate well with biodistribution data. These results suggest that the topical application of SERS nanoparticles in the mouse colon appears to minimize their systemic distribution, thus avoiding potential toxicity and supporting the clinical translation of Raman spectroscopy as an endoscopic imaging tool.

  7. Surface Enhanced Raman Scattering studies of L-amino acids adsorbed on silver nanoclusters

    NASA Astrophysics Data System (ADS)

    Botta, Raju; Rajanikanth, A.; Bansal, C.

    2015-01-01

    Silver nanocluster films were prepared using plasma inert gas phase condensation technique. These were used as Raman active substrates for Surface Enhanced Raman Scattering (SERS) studies of 19 standard L-amino acids adsorbed on the surface of Ag nanoclusters via Agsbnd N bonds. A detailed study of two essential aromatic amino acids viz. L-Phenylalanine and L-Tryptophan showed a correlation between the Raman intensity of the characteristic lines of phenol and indole side chains and their molar concentrations in the range 1 μM-1 mM. This indicates that Raman studies can be used for quantitative determination of the amino acids in proteins.

  8. Label-free imaging of biomolecules in food products using stimulated Raman microscopy

    NASA Astrophysics Data System (ADS)

    Roeffaers, Maarten B. J.; Zhang, Xu; Freudiger, Christian W.; Saar, Brian G.; van Ruijven, Marjolein; van Dalen, Gerard; Xiao, Chunhong; Xie, X. Sunney

    2010-11-01

    The development of methods that allow microscale studies of complex biomaterials based on their molecular composition is of great interest to a wide range of research fields. We show that stimulated Raman scattering (SRS) microscopy is an excellent analytical tool to study distributions of different biomolecules in multiphasic systems. SRS combines the label-free molecular specificity of vibrational spectroscopy with an enhanced sensitivity due to coherent excitation of molecular vibrations. Compared to previous imaging studies using coherent anti-Stokes Raman scattering microscopy, the main advantage of SRS microscopy is the absence of the unwanted nonresonant background, which translates into a superior sensitivity and undistorted vibrational spectra. We compare spectra of complex materials obtained with stimulated Raman scattering and spontaneous Raman scattering in the crowded fingerprint region. We find that, as expected, there is excellent correspondence and that the SRS spectra are free from interference from background fluorescence. In addition, we show high-resolution imaging of the distributions of selected biomolecules, such as lipids and proteins, in food products with SRS microscopy.

  9. Label-free imaging of biomolecules in food products using stimulated Raman microscopy

    NASA Astrophysics Data System (ADS)

    Roeffaers, Maarten B. J.; Zhang, Xu; Freudiger, Christian W.; Saar, Brian G.; Ruijven, Marjolein Van; Dalen, Gerard Van; Xiao, Chunhong; Xie, X. Sunney

    2011-02-01

    The development of methods that allow microscale studies of complex biomaterials based on their molecular composition is of great interest to a wide range of research fields. We show that stimulated Raman scattering (SRS) microscopy is an excellent analytical tool to study distributions of different biomolecules in multiphasic systems. SRS combines the label-free molecular specificity of vibrational spectroscopy with an enhanced sensitivity due to coherent excitation of molecular vibrations. Compared to previous imaging studies using coherent anti-Stokes Raman scattering microscopy, the main advantage of SRS microscopy is the absence of the unwanted nonresonant background, which translates into a superior sensitivity and undistorted vibrational spectra. We compare spectra of complex materials obtained with stimulated Raman scattering and spontaneous Raman scattering in the crowded fingerprint region. We find that, as expected, there is excellent correspondence and that the SRS spectra are free from interference from background fluorescence. In addition, we show high-resolution imaging of the distributions of selected biomolecules, such as lipids and proteins, in food products with SRS microscopy.

  10. Coupled wave equations theory of surface-enhanced femtosecond stimulated Raman scattering.

    PubMed

    McAnally, Michael O; McMahon, Jeffrey M; Van Duyne, Richard P; Schatz, George C

    2016-09-01

    We present a coupled wave semiclassical theory to describe plasmonic enhancement effects in surface-enhanced femtosecond stimulated Raman scattering (SE-FSRS). A key result is that the plasmon enhanced fields which drive the vibrational equation of motion for each normal mode results in dispersive lineshapes in the SE-FSRS spectrum. This result, which reproduces experimental lineshapes, demonstrates that plasmon-enhanced stimulated Raman methods provide unique sensitivity to a plasmonic response. Our derived SE-FSRS theory shows a plasmonic enhancement of |gpu|(2)ImχR(ω)gst (2)/ImχR(ω), where |gpu|(2) is the absolute square of the plasmonic enhancement from the Raman pump, χR(ω) is the Raman susceptibility, and gst is the plasmonic enhancement of the Stokes field in SE-FSRS. We conclude with a discussion on potential future experimental and theoretical directions for the field of plasmonically enhanced coherent Raman scattering. PMID:27608988

  11. Surface-enhanced Raman scattering (SERS) spectroscopic analysis of herba houttuyniae decoction (HHD)

    NASA Astrophysics Data System (ADS)

    Chen, Weiwei; Lin, Jia; Feng, Shangyuan; Huang, Hao; Yu, Yun; Lin, Duo; Chen, Rong

    2014-11-01

    The normal Raman spectrum and surface-enhanced Raman scattering (SERS) spectrum of herba houttuyniae decoction (HHD) were tested and analyzed. The characteristic SERS bands of HHD were tentatively assigned. There was no Raman signal in normal Raman spectrum of HHD. However, as a result of the silver colloid enhanced effects on the Raman scattering of HHD, we observed that the SERS spectrum of HHD had primary thirteen SERS peaks such as 538, 620, 686, 730, 955, 1030, 1231, 1240, 1325, 1400, 1472, 1564 and 1651 cm-1, and there were six strong signals at 538, 620, 730, 955, 1325 and 1400 cm-1 bands. The results showed that the SERS spectroscopy might provide a new kind of high-sensitive, accurate, easy, and rapid detecting method for traditional Chinese medicine (TCM).

  12. Coupled wave equations theory of surface-enhanced femtosecond stimulated Raman scattering

    NASA Astrophysics Data System (ADS)

    McAnally, Michael O.; McMahon, Jeffrey M.; Van Duyne, Richard P.; Schatz, George C.

    2016-09-01

    We present a coupled wave semiclassical theory to describe plasmonic enhancement effects in surface-enhanced femtosecond stimulated Raman scattering (SE-FSRS). A key result is that the plasmon enhanced fields which drive the vibrational equation of motion for each normal mode results in dispersive lineshapes in the SE-FSRS spectrum. This result, which reproduces experimental lineshapes, demonstrates that plasmon-enhanced stimulated Raman methods provide unique sensitivity to a plasmonic response. Our derived SE-FSRS theory shows a plasmonic enhancement of |gp u|2I m {" separators="χR(ω ) gst 2 }/I m {" separators="χR(ω ) }, where |gpu|2 is the absolute square of the plasmonic enhancement from the Raman pump, χR(ω) is the Raman susceptibility, and gst is the plasmonic enhancement of the Stokes field in SE-FSRS. We conclude with a discussion on potential future experimental and theoretical directions for the field of plasmonically enhanced coherent Raman scattering.

  13. Raman Scattered He II 4332 and Photoionization Model in the Symbiotic Star V1016 Cygni

    NASA Astrophysics Data System (ADS)

    Lee, H.-W.; Heo, J.-E.; Lee, B.-C.

    2014-08-01

    Symbiotic stars are wide binary systems of a white dwarf and a mass losing giant. They exhibit unique Raman scattered features as a result of inelastic scattering of far UV line photons by atomic hydrogen. Co-existence of a far UV He II emission region and a thick H I region in symbiotic stars is necessary for the formation of Raman-scattered features blueward of hydrogen Balmer emission lines. Being a single electron atom, He II has the same atomic structure as the hydrogen atom and hence emits far UV emission lines that are slightly blueward of hydrogen Lyman lines. These far UV He II emission lines can be Raman scattered to appear blueward of hydrogen Balmer lines. In particular, the symbiotic star V1016 Cyg is found to exhibit Raman scattered He II 4332 feature in the BOES high resolution spectrum. Our profile fitting of Raman scattered He II 4332 is consistent with the mass loss geometry proposed by Jung & Lee (2004). We use the photoionization code ‘ CLOUDY' to estimate the far UV He II emission lines and make comparisons with the observed Raman scattered He II 4332 blueward of Hγ in the high resolution echelle V1016 Cyg. The emission nebula is assumed to be of uniform density of 108 cm-3 that is illuminated by a black body characterized by its temperature and total luminosity. With our comparisons we conclude that the Raman scattered He II features are consistent with the existence of a photoionized nebula by a hot black body source with temperature 7-8× 104 K with a luminosity 1038erg s-1.

  14. Probing the evaporation of ternary ethanol-methanol-water droplets by cavity enhanced Raman scattering.

    PubMed

    Howle, Chris R; Homer, Chris J; Hopkins, Rebecca J; Reid, Jonathan P

    2007-10-21

    Cavity enhanced Raman scattering is used to characterise the evolving composition of ternary aerosol droplets containing methanol, ethanol and water during evaporation into a dry nitrogen atmosphere. Measurements made using non-linear stimulated Raman scattering from these ternary alcohol-water droplets allow the in situ determination of the concentration of the two alcohol components with high accuracy. The overlapping spontaneous Raman bands of the two alcohol components, arising from C-H stretching vibrational modes, are spectrally-resolved in stimulated Raman scattering measurements. We also demonstrate that the evaporation measurements are consistent with a quasi-steady state evaporation model, which can be used to interpret the evaporation dynamics occurring at a range of pressures at a particular evaporation time.

  15. 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.

  16. A New Way to Measure Cirrus Ice Water Content by Using Ice Raman Scatter with Raman Lidar

    NASA Technical Reports Server (NTRS)

    Wang, Zhien; Whiteman, David N.; Demoz, Belay; Veselovskii, Igor

    2004-01-01

    High and cold cirrus clouds mainly contain irregular ice crystals, such as, columns, hexagonal plates, bullet rosettes, and dendrites, and have different impacts on the climate system than low-level clouds, such as stratus, stratocumulus, and cumulus. The radiative effects of cirrus clouds on the current and future climate depend strongly on cirrus cloud microphysical properties including ice water content (IWC) and ice crystal sizes, which are mostly an unknown aspect of cinus clouds. Because of the natural complexity of cirrus clouds and their high locations, it is a challenging task to get them accurately by both remote sensing and in situ sampling. This study presents a new method to remotely sense cirrus microphysical properties by using ice Raman scatter with a Raman lidar. The intensity of Raman scattering is fundamentally proportional to the number of molecules involved. Therefore, ice Raman scattering signal provides a more direct way to measure IWC than other remote sensing methods. Case studies show that this method has the potential to provide essential information of cirrus microphysical properties to study cloud physical processes in cirrus clouds.

  17. Raman calibration of the HT-7 yttrium aluminum garnet Thomson scattering for electron density measurements

    SciTech Connect

    Zang Qing; Zhao Junyu; Gao Xiang; Shi Lingwei; Zhang Tao; Xi Xiaoqi; Yang Li; Hu Qingsheng; Sajjad, S.

    2007-11-15

    A multipulse neodym doped yttrium aluminum garnet laser Thomson scattering system calibrated by the anti-Stokes rotational Raman scattering from nitrogen gas had been developed in the HT-7 superconducting Tokmak. By virtue of this system, measured electron density results of the plasma were obtained. The results showed good repeatability and its total uncertainty was estimated to be {+-}18%.

  18. Dual Raman-Brillouin Microscope for Chemical and Mechanical Characterization and Imaging.

    PubMed

    Traverso, Andrew J; Thompson, Jonathan V; Steelman, Zachary A; Meng, Zhaokai; Scully, Marlan O; Yakovlev, Vladislav V

    2015-08-01

    We present a unique confocal microscope capable of measuring the Raman and Brillouin spectra simultaneously from a single spatial location. Raman and Brillouin scattering offer complementary information about a material's chemical and mechanical structure, respectively, and concurrent monitoring of both of these spectra would set a new standard for material characterization. We achieve this by applying recent innovations in Brillouin spectroscopy that reduce the necessary acquisition times to durations comparable to conventional Raman spectroscopy while attaining a high level of spectral accuracy. To demonstrate the potential of the system, we map the Raman and Brillouin spectra of a molded poly(ethylene glycol) diacrylate (PEGDA) hydrogel sample in cyclohexane to create two-dimensional images with high contrast at microscale resolutions. This powerful tool has the potential for very diverse analytical applications in basic science, industry, and medicine.

  19. 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.

  20. Air stable colloidal copper nanoparticles: Synthesis, characterization and their surface-enhanced Raman scattering properties

    NASA Astrophysics Data System (ADS)

    Ramani, Thekkathu; Leon Prasanth, K.; Sreedhar, Bojja

    2016-03-01

    Air stable colloidal copper nanoparticles are synthesized by a simple chemical reduction method using octadecylsilane as a reducing agent and octadecylamine as a stabilizing agent in toluene without any inert gas. The formation of nanosized copper was confirmed by its characteristic surface plasmon absorption peaks in UV-visible spectra. The transmission electron microscopic (TEM) images show that the resulting copper nanoparticles are distributed uniformly with a narrow size distribution. The X-ray diffraction (XRD) demonstrated that the obtained copper nanoparticles are single crystalline nanoparticles. Fourier transform infra-red (FT-IR) spectroscopic data suggested that the silane Si-H is responsible for the reduction of copper ions. And also the resulting colloidal copper nanoparticles exhibit large surface-enhanced Raman scattering (SERS) signals.

  1. Simulation of stimulated Brillouin scattering and stimulated Raman scattering in shock ignition

    NASA Astrophysics Data System (ADS)

    Hao, L.; Li, J.; Liu, W. D.; Yan, R.; Ren, C.

    2016-04-01

    We study stimulated Brillouin scattering (SBS) and stimulated Raman scattering (SRS) in shock ignition by comparing fluid and particle-in-cell (PIC) simulations. Under typical parameters for the OMEGA experiments [Theobald et al., Phys. Plasmas 19, 102706 (2012)], a series of 1D fluid simulations with laser intensities ranging between 2 × 1015 and 2 × 1016 W/cm2 finds that SBS is the dominant instability, which increases significantly with the incident intensity. Strong pump depletion caused by SBS and SRS limits the transmitted intensity at the 0.17nc to be less than 3.5 × 1015 W/cm2. The PIC simulations show similar physics but with higher saturation levels for SBS and SRS convective modes and stronger pump depletion due to higher seed levels for the electromagnetic fields in PIC codes. Plasma flow profiles are found to be important in proper modeling of SBS and limiting its reflectivity in both the fluid and PIC simulations.

  2. Detection of S02 and N02 in Stack Plume by Raman Scattering and Fluorescence

    NASA Technical Reports Server (NTRS)

    Nakahara, S.; Ito, K.; Ito, S.

    1973-01-01

    We have been studying laser-Raman radar which can be used as the remote detector of sulfur dioxide concentration in the stack plume of boiler exhaust gas, and some results have been published. In this paper, we report the interference of nitrogen dioxide fluorescence against sulfur dioxide Raman scattering and the measuring method of sulfur dioxide and nitrogen dioxide concentration. In a stack plume, high density dust and high concentration carbon dioxide are included, therefore very strong Mie back-scattering and carbon dioxide Raman scattering are observed. The separation of these scattering signals from sulfur dioxide Raman signal was the first problem for the laser-Raman radar. But, this problem was solved by using the filter which have high resolving power. It is well known that nitrogen dioxide can be excited to emit fluorescence of broad spectrum by blue-green light. The light source of the laser-Raman radar is SH of Nd:YAG laser, and boiler exhaust gas includes several tens ppm of nitrogen dioxide, then the interference of nitrogen dioxide fluorescence brings the error to sulfur dioxide measurement. 'rhe rejection of the interference can be achieved by the subtraction of the nitrogen dioxide fluorescence contribution from detected signal at sulfur dioxide Raman scattering wavelength. The nitrogen dioxide fluorescence contribution can be measured by two methods. The first is to convert the nitrogen dioxide fluorescence intensity which is measured at a different wavelength from sulfur dioxide Raman line into the one at sulfur dioxide Raman line. The second is to convert the detected signal intensity, which is obtained when the range gate is set just behind the plume, into the one obtained at the range of the plume using the difference of the time dependence between sulfur dioxide Raman scattering and nitrogen dioxide fluorescence. Nitrogen dioxide fluorescence has lifetime of about 300nS, while Raman scattering has none. By either of the two methods, the

  3. Toward digital staining using stimulated Raman scattering and statistical machine learning

    NASA Astrophysics Data System (ADS)

    Tanji, K.; Otsuka, Y.; Satoh, S.; Hashimoto, H.; Ozeki, Y.; Itoh, Kazuyoshi

    2014-03-01

    Stimulated Raman scattering (SRS) spectral microscopy is a promising imaging method, based on vibrational spectroscopy, which can visualize biological tissues with chemical specificity. SRS spectral microscopy has been used to obtain two-dimensional spectral images of rat liver tissue, three-dimensional images of a vessel in rat liver, and in vivo spectral images of mouse ear skin. Various multivariate analysis techniques, such as principal component analysis and independent component analysis, have been used to obtain spectral images. In this study, we propose a digital staining method. This method uses SRS spectra and statistical machine learning that makes use of prior knowledge of spectral peaks and their two-dimensional distributional patterns corresponding to the composition of tissue samples. The method selects spectral peaks on the basis of Mahalanobis distance, which is defined as the ratio of inter-group variation to intragroup variation. We also make use of higher-order local autocorrelations as feature values for two-dimensional distributional patterns. This combination of techniques allows groups corresponding to different intracellular structures to be clearly discriminated in the multidimensional feature space. We investigate the performance of our method on mouse liver tissue samples and show that the proposed method can digitally stain each intracellular structure such as cell nuclei, cytoplasm, and erythrocytes separately and clearly without time-consuming chemical staining processes. We anticipate that our method could be applied to computer-aided pathological diagnosis.

  4. RAMAN SCATTERED He II {lambda}4332 IN THE SYMBIOTIC STAR V1016 CYGNI

    SciTech Connect

    Lee, Hee-Won

    2012-05-10

    Raman scattering of He II line photons with atomic hydrogen is important in studying the mass loss processes in many symbiotic stars and a number of young planetary nebulae. We calculate the scattering cross sections and branching ratios associated with the Raman scattered He II {lambda}4332 feature formed through inelastic scattering of He II {lambda}949 with a hydrogen atom. At the line center of He II {lambda}949, the total scattering cross section is computed to be {sigma}{sub tot} = 2.5 Multiplication-Sign 10{sup -22} cm{sup 2}, and the branching ratio into the level 2s is 0.12. We also present a high-resolution spectrum of the symbiotic star V1016 Cygni obtained with the 1.8 m telescope at Mt. Bohyun to investigate the Raman scattering origin of the broad feature blueward of He II {lambda}4338. Based on the atomic calculation, we perform Monte Carlo calculations for the line formation. The scattering region is assumed to be a part of a uniform spherical shell that subtends a solid angle {Delta}{Omega} = {pi} steradian with a neutral column density N{sub HI} = 1.0 x 10{sup 21} cm{sup -2}. By adding a far-UV continuum around He II {lambda}949 normalized by the equivalent width of He II {lambda}949 to be 2.3 Angstrom-Sign , we obtain a good fit for both the Raman scattered He II {lambda}4332 and the broad wings around H{gamma}. Our analysis of the Raman feature blueward of H{gamma} in V1016 Cyg is consistent with the previous study of the Raman features blueward of H{alpha} and H{beta} by Jung and Lee.

  5. Coherent scatter imaging Monte Carlo simulation.

    PubMed

    Hassan, Laila; MacDonald, Carolyn A

    2016-07-01

    Conventional mammography can suffer from poor contrast between healthy and cancerous tissues due to the small difference in attenuation properties. Coherent scatter slot scan imaging is an imaging technique which provides additional information and is compatible with conventional mammography. A Monte Carlo simulation of coherent scatter slot scan imaging was performed to assess its performance and provide system optimization. Coherent scatter could be exploited using a system similar to conventional slot scan mammography system with antiscatter grids tilted at the characteristic angle of cancerous tissues. System optimization was performed across several parameters, including source voltage, tilt angle, grid distances, grid ratio, and shielding geometry. The simulated carcinomas were detectable for tumors as small as 5 mm in diameter, so coherent scatter analysis using a wide-slot setup could be promising as an enhancement for screening mammography. Employing coherent scatter information simultaneously with conventional mammography could yield a conventional high spatial resolution image with additional coherent scatter information. PMID:27610397

  6. Microscopic Imaging and Spectroscopy with Scattered Light

    PubMed Central

    Boustany, Nada N.; Boppart, Stephen A.; Backman, Vadim

    2012-01-01

    Optical contrast based on elastic scattering interactions between light and matter can be used to probe cellular structure and dynamics, and image tissue architecture. The quantitative nature and high sensitivity of light scattering signals to subtle alterations in tissue morphology, as well as the ability to visualize unstained tissue in vivo, has recently generated significant interest in optical scatter based biosensing and imaging. Here we review the fundamental methodologies used to acquire and interpret optical scatter data. We report on recent findings in this field and present current advances in optical scatter techniques and computational methods. Cellular and tissue data enabled by current advances in optical scatter spectroscopy and imaging stand to impact a variety of biomedical applications including clinical tissue diagnosis, in vivo imaging, drug discovery and basic cell biology. PMID:20617940

  7. Experimental investigation on the competition between wideband stimulated Brillouin scattering and forward stimulated Raman scattering in water.

    PubMed

    Shi, Jiulin; Chen, Wei; Mo, Xiaofeng; Liu, Juan; He, Xingdao; Yang, Kecheng

    2012-07-15

    The utilization of a simple focused optical cell to bring to light the competition between wideband stimulated Brillouin scattering (WSBS) and forward stimulated Raman scattering (FSRS) is investigated experimentally. A pulsed, wide bandwidth second-harmonic Nd:YAG laser is used as the pump source. We found that, the competition between WSBS and FSRS is an alternate process, which one dominated depends on the linewidth and energy of the pump laser, focal length, and optical breakdown.

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

    NASA Astrophysics Data System (ADS)

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

    2014-11-01

    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.

  9. Saturation of vibrational coherent anti-Stokes Raman scattering mediated by saturation of the rotational Raman transition

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

    Saturation of vibrational Raman coherence and coherent anti-Stokes Raman scattering (CARS) using femtosecond (fs) excitation pulses is investigated theoretically. The pump in a typical fs-CARS configuration has a bandwidth of a few hundred cm-1 that can couple tens of rotational states of room-air nitrogen molecules simultaneously, unlike in CARS with longer pulse durations. It is demonstrated that the vibrational coherence and also the vibrational CARS with fs excitation display saturationlike behavior once the rotational coherence is saturated. The Raman saturation threshold for the fs pump is numerically estimated to be at a peak intensity of ˜1022 W/m2, which is six to seven orders of magnitude higher than that in the nanosecond regime. The results are compared with the known saturation thresholds in different pulse-duration regimes and placed in perspective with other nonlinear thresholds reported in fs excitation regimes.

  10. Interaction of anthranilic acid with silver nanoparticles: A Raman, surface-enhanced Raman scattering and density functional theoretical study

    NASA Astrophysics Data System (ADS)

    Chadha, Ridhima; Maiti, Nandita; Kapoor, Sudhir

    2014-11-01

    Raman and surface-enhanced Raman scattering (SERS) studies of anthranilic acid have been investigated in solid, aqueous solution and on silver colloid. Anthranilic acid plays a key role in the brain in the production of quinolinic acid which is a powerful excitant and convulsant substance. Due to its medicinal importance, the surface adsorption properties of anthranilic acid have been studied. The experimental Raman and SERS data is supported with DFT calculations using B3LYP functional with aug-cc-pvdz and LANL2DZ basis sets. The comparison of experimental and theoretical results infers that anthranilate is chemisorbed to the silver surface directly through the carboxylate group with a perpendicular orientation. The time-dependent SERS spectrum of anthranilate showed no observable change indicating no structural transformation with time. The SERS spectrum recorded at different excitation wavelengths helped in understanding the origin of the SERS mechanism.

  11. Enhancement of stimulated Raman scattering of weak-gain Raman modes in a pendant drop by dye-lasing gain

    NASA Astrophysics Data System (ADS)

    Pu, Xiao-Yun; Yang, Zheng; Lee, Wing-Kee

    2004-02-01

    The enhancement of stimulated Raman scattering (SRS) of weak-gain Raman modes in pendant drops is accomplished by overlapping Stokes wavelengths of the Raman modes with the Rhodamine 640 dye-lasing gain region (called the gain-overlap method). The dye concentration and the pumping intensity of frequency-doubled Nd:YAG lasers determine the efficiency of the enhancement. We apply the gain-overlap technique at optimal dye concentration and pump intensity to probe minority species in pendant drops formed by binary mixtures. The limits of detectable concentrations of the minority species, methanol in methanol-ethanol and ethanol in ethanol-water (dye-doped) mixtures, are much less than those in undoped mixtures. The smooth fluorescence-lasing spectral curves emitted from dye-doped pendant drops reduce complications in distinguishing SRS signals from quasi-periodic fluorescence-lasing spectra in microdroplets.

  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. The design and implementation of a high-fidelity Raman imaging microscope.

    PubMed

    Goldstein, S R; Kidder, L H; Herne, T M; Levin, I W; Lewis, E N

    1996-10-01

    We describe a Raman imaging microscope that produces high-fidelity, large format Raman images and Raman spectra from samples as small as 1 micron in size. Laser illumination is delivered to the object by means of an infinity corrected microscope objective, either by a galvanometer scanning system or a widefield fibre optic. Wavelength selection of Raman scattered emission is achieved by an acousto-optic tunable filter (AOTF), which maintains image fidelity and provides either continuous or random wavelength selection. The collimated AOTF output is imaged first by a tube lens and then by a projection lens onto a cooled silicon CCD array. Instrument features, including factors that determine the system's spatial and spectral resolution, and design considerations are discussed in detail. Images and spectra of test objects and samples that demonstrate the capability of this imaging spectrometer are presented. The potential of intrinsic chemical imaging is discussed in terms of its use in the analyses of a variety of chemical and biological samples. PMID:8923757

  14. Surface enhanced Raman scattering for detection of Pseudomonas aeruginosa quorum sensing compounds

    NASA Astrophysics Data System (ADS)

    Thrift, Will; Bhattacharjee, Arunima; Darvishzadeh-Varcheie, Mahsa; Lu, Ying; Hochbaum, Allon; Capolino, Filippo; Whiteson, Katrine; Ragan, Regina

    2015-08-01

    Pseudomonas aeruginosa (PA), a biofilm forming bacterium, commonly affects cystic fibrosis, burn victims, and immunocompromised patients. PA produces pyocyanin, an aromatic, redox active, secondary metabolite as part of its quorum sensing signaling system activated during biofilm formation. Surface enhanced Raman scattering (SERS) sensors composed of Au nanospheres chemically assembled into clusters on diblock copolymer templates were fabricated and the ability to detect pyocyanin to monitor biofilm formation was investigated. Electromagnetic full wave simulations of clusters observed in scanning electron microcopy images show that the localized surface plasmon resonance wavelength is 696 nm for a dimer with a gap spacing of 1 nm in an average dielectric environment of the polymer and analyte; the local electric field enhancement is on the order of 400 at resonance, relative to free space. SERS data acquired at 785 nm excitation from a monolayer of benzenethiol on fabricated samples was compared with Raman data of pure benzenethiol and enhancement factors as large as 8×109 were calculated that are consistent with simulated field enhancements. Using this system, the limit of detection of pyocyanin in pure gradients was determined to be 10 parts per billion. In SERS data of the supernatant from the time dependent growth of PA shaking cultures, pyocyanin vibrational modes were clearly observable during the logarithmic growth phase corresponding to activation of genes related to biofilm formation. These results pave the way for the use of SERS sensors for the early detection of biofilm formation, leading to reduced healthcare costs and better patient outcomes.

  15. Surface-enhanced Raman scattering activities of carbon nanotubes decorated with silver nanoparticles.

    PubMed

    Zhang, Xiaolei; Zhang, Jie; Quan, Jiamin; Wang, Ning; Zhu, Yong

    2016-10-01

    We synthesized a carbon nanotube (CNT) loaded with silver nanoparticles (AgNPs) composite as an effective surface enhanced Raman scattering (SERS) substrate via a low-cost, simple citrate reduction method. The hybrid materials were confirmed by scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD), ultraviolet-visible (UV-vis) spectrophotometer and Raman spectroscopy. Rhodamine 6G (R6G) was used as the probe analyte. The experimental results indicated that the detection concentration level was down to 10(-14) M. Additionally, we discussed the uniformity by conducting SERS position mapping within an area of 5 μm × 5 μm; meanwhile, we performed time-course SERS mapping experiments to study the evaporation process of probe molecules of the prepared samples. Finally, we simulated the electromagnetic field distribution based on SEM images (obtained the ratio of surface area to the area of silver particles) by the finite difference time domain (FDTD) method.

  16. Dual Raman-Brillouin microscope for chemical and mechanical characterization and imaging (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Yakovlev, Vladislav V.

    2016-03-01

    We present a unique confocal microscope capable of measuring the Raman and Brillouin spectra simultaneously from a single spatial location. Raman and Brillouin scattering offer complementary information about a material's chemical and mechanical structure, respectively, and concurrent monitoring of both of these spectra would set a new standard for material characterization. We achieve this by applying recent innovations in Brillouin spectroscopy that reduce the necessary acquisition times to durations comparable to conventional Raman spectroscopy while attaining a high level of spectral accuracy. To demonstrate the potential of the system, we apply this system for imaging melanoma, arteriosclerotic plaque, embryonic development, bones and biomaterials. The developed instrument has the potential for very diverse analytical applications in basic biomedical science and biomedical diagnostics and imaging.

  17. Resonant stimulation of Raman scattering from single-crystal thiophene/phenylene co-oligomers

    SciTech Connect

    Yanagi, Hisao Marutani, Yusuke; Matsuoka, Naoki; Hiramatsu, Toru; Ishizumi, Atsushi; Sasaki, Fumio; Hotta, Shu

    2013-12-09

    Amplified Raman scattering was observed from single crystals of thiophene/phenylene co-oligomers (TPCOs). Under ns-pulsed excitation, the TPCO crystals exhibited amplified spontaneous emission (ASE) at resonant absorption wavelengths. With increasing excitation wavelength to the 0-0 absorption edge, the stimulated resonant Raman peaks appeared both in the 0-1 and 0-2 ASE band regions. When the excitation wavelength coincided with the 0-1 ASE band energy, the Raman peaks selectively appeared in the 0-2 ASE band. Such unusual enhancement of the 0-2 Raman scattering was ascribed to resonant stimulation via vibronic coupling with electronic transitions in the uniaxially oriented TPCO molecules.

  18. 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.

  19. Adaptive optics applied to coherent anti-Stokes Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Girkin, John M.; Poland, Simon P.; Wright, Amanda J.; Freudiger, Christian; Evans, Conor L.; Xie, X. Sunney

    2008-02-01

    We report on the use of adaptive optics in coherent anti-Stokes Raman scattering microscopy (CARS) to improve the image brightness and quality at increased optical penetration depths in biological material. The principle of the technique is to shape the incoming wavefront in such a way that it counteracts the aberrations introduced by imperfect optics and the varying refractive index of the sample. In recent years adaptive optics have been implemented in multiphoton and confocal microscopy. CARS microscopy is proving to be a powerful tool for non-invasive and label-free biomedical imaging with vibrational contrast. As the contrast mechanism is based on a 3 rd order non-linear optical process, it is highly susceptible to aberrations, thus CARS signals are commonly lost beyond the depth of ~100 μm in tissue. We demonstrate the combination of adaptive optics and CARS microscopy for deep-tissue imaging using a deformable membrane mirror. A random search optimization algorithm using the CARS intensity as the figure of merit determined the correct mirror-shape in order to correct for the aberrations. We highlight two different methods of implementation, using a look up table technique and by performing the optimizing in situ. We demonstrate a significant increase in brightness and image quality in an agarose/polystyrene-bead sample and white chicken muscle, pushing the penetration depth beyond 200 μm.

  20. Electroless Gold-Modified Diatoms as Surface-Enhanced Raman Scattering Supports.

    PubMed

    Pannico, Marianna; Rea, Ilaria; Chandrasekaran, Soundarrajan; Musto, Pellegrino; Voelcker, Nicolas H; De Stefano, Luca

    2016-12-01

    Porous biosilica from diatom frustules is well known for its peculiar optical and mechanical properties. In this work, gold-coated diatom frustules are used as low-cost, ready available, functional support for surface-enhanced Raman scattering. Due to the morphology of the nanostructured surface and the smoothness of gold deposition via an electroless process, an enhancement factor for the p-mercaptoaniline Raman signal of the order of 10(5) is obtained. PMID:27356562

  1. Coherent anti-Stokes Raman scattering in benzene and nitromethane shock-compressed to 10 GPa

    SciTech Connect

    Schmidt, S.C.; Moore, D.S.; Shaner, J.W.; Shampine, D.L.; Holt, W.T.

    1985-01-01

    The frequency shifts of the ring-stretching mode of shock-compressed liquid benzene and the CN stretching mode of nitromethane have been measured using coherent anti-Stokes Raman scattering. Shock pressures up to 11 GPa were achieved using a two-stage light gas gun. The frequency shifted Raman signal was generated using single pulse Nd:YAG and broadband-type lasers. 16 refs., 3 figs.

  2. Electroless Gold-Modified Diatoms as Surface-Enhanced Raman Scattering Supports

    NASA Astrophysics Data System (ADS)

    Pannico, Marianna; Rea, Ilaria; Chandrasekaran, Soundarrajan; Musto, Pellegrino; Voelcker, Nicolas H.; De Stefano, Luca

    2016-06-01

    Porous biosilica from diatom frustules is well known for its peculiar optical and mechanical properties. In this work, gold-coated diatom frustules are used as low-cost, ready available, functional support for surface-enhanced Raman scattering. Due to the morphology of the nanostructured surface and the smoothness of gold deposition via an electroless process, an enhancement factor for the p-mercaptoaniline Raman signal of the order of 105 is obtained.

  3. Electroless Gold-Modified Diatoms as Surface-Enhanced Raman Scattering Supports.

    PubMed

    Pannico, Marianna; Rea, Ilaria; Chandrasekaran, Soundarrajan; Musto, Pellegrino; Voelcker, Nicolas H; De Stefano, Luca

    2016-12-01

    Porous biosilica from diatom frustules is well known for its peculiar optical and mechanical properties. In this work, gold-coated diatom frustules are used as low-cost, ready available, functional support for surface-enhanced Raman scattering. Due to the morphology of the nanostructured surface and the smoothness of gold deposition via an electroless process, an enhancement factor for the p-mercaptoaniline Raman signal of the order of 10(5) is obtained.

  4. A study of surface enhanced Raman scattering for furfural adsorbed on silver surface

    NASA Astrophysics Data System (ADS)

    Jia, Ting-jian; Li, Peng-wei; Shang, Zhi-guo; Zhang, Ling; He, Ting-chao; Mo, Yu-jun

    2008-02-01

    The normal Raman spectrum (NRS) and the surface enhanced Raman scattering (SERS) spectrum of furfural in silver colloid were recorded and analyzed in this paper. The assignment of these bands to furfural molecules was performed by density functional theory (DFT) calculation. The data of the SERS by comparing with the one of NRS show that furfural molecules are adsorbed on the silver surface via the nonbonding electrons of the carbonyl oxygen.

  5. Raman scattering from a superconductivity-induced bound state in MgB2.

    PubMed

    Zeyher, R

    2003-03-14

    It is shown that the sharp peak in the E(2g) Raman spectrum of superconducting MgB2 is due to a bound state caused by the electron-phonon coupling. Our theory explains why this peak appears only in the spectra with E(2g) symmetry and only in the sigma but not the pi bands. The properties of the bound state and the Raman spectrum are investigated, also in the presence of impurity scattering.

  6. Optical wavefront shaping for the enhancement of Raman signal in scattering media

    NASA Astrophysics Data System (ADS)

    Thompson, Jonathan V.; Throckmorton, Graham A.; Hokr, Brett H.; Yakovlev, Vladislav V.

    2016-03-01

    The ability to non-invasively focus light through scattering media has significant applications in many fields ranging from nanotechnology to deep tissue sensing. Until recently, the multiple light scattering events that occur in complex media such as biological tissue have inhibited the focusing ability and penetration depth of optical tools. Through the use of optical wavefront shaping, the spatial distortions due to these scattering events can be corrected, and the incident light can be focused through the scattering medium. Here, we demonstrate that wavefront shaping can be used to non-invasively enhance the Raman signal of a material through a scattering medium. Raman signal enhancement was achieved using backscattered light and a continuous sequential algorithm. Our results show the potential of wavefront shaping as an important addition to non-invasive detection techniques.

  7. Multi-wavelength Raman scattering of nanostructured Al-doped zinc oxide

    SciTech Connect

    Russo, V.; Ghidelli, M.; Gondoni, P.

    2014-02-21

    In this work we present a detailed Raman scattering investigation of zinc oxide and aluminum-doped zinc oxide (AZO) films characterized by a variety of nanoscale structures and morphologies and synthesized by pulsed laser deposition under different oxygen pressure conditions. The comparison of Raman spectra for pure ZnO and AZO films with similar morphology at the nano/mesoscale allows to investigate the relation between Raman features (peak or band positions, width, relative intensity) and material properties such as local structural order, stoichiometry, and doping. Moreover Raman measurements with three different excitation lines (532, 457, and 325 nm) point out a strong correlation between vibrational and electronic properties. This observation confirms the relevance of a multi-wavelength Raman investigation to obtain a complete structural characterization of advanced doped oxide materials.

  8. Biophotonics of skin: method for correction of deep Raman spectra distorted by elastic scattering

    NASA Astrophysics Data System (ADS)

    Roig, Blandine; Koenig, Anne; Perraut, François; Piot, Olivier; Gobinet, Cyril; Manfait, Michel; Dinten, Jean-Marc

    2015-03-01

    Confocal Raman microspectroscopy allows in-depth molecular and conformational characterization of biological tissues non-invasively. Unfortunately, spectral distortions occur due to elastic scattering. Our objective is to correct the attenuation of in-depth Raman peaks intensity by considering this phenomenon, enabling thus quantitative diagnosis. In this purpose, we developed PDMS phantoms mimicking skin optical properties used as tools for instrument calibration and data processing method validation. An optical system based on a fibers bundle has been previously developed for in vivo skin characterization with Diffuse Reflectance Spectroscopy (DRS). Used on our phantoms, this technique allows checking their optical properties: the targeted ones were retrieved. Raman microspectroscopy was performed using a commercial confocal microscope. Depth profiles were constructed from integrated intensity of some specific PDMS Raman vibrations. Acquired on monolayer phantoms, they display a decline which is increasing with the scattering coefficient. Furthermore, when acquiring Raman spectra on multilayered phantoms, the signal attenuation through each single layer is directly dependent on its own scattering property. Therefore, determining the optical properties of any biological sample, obtained with DRS for example, is crucial to correct properly Raman depth profiles. A model, inspired from S.L. Jacques's expression for Confocal Reflectance Microscopy and modified at some points, is proposed and tested to fit the depth profiles obtained on the phantoms as function of the reduced scattering coefficient. Consequently, once the optical properties of a biological sample are known, the intensity of deep Raman spectra distorted by elastic scattering can be corrected with our reliable model, permitting thus to consider quantitative studies for purposes of characterization or diagnosis.

  9. Directional Raman scattering from single molecules in the feed gaps of optical antennas.

    PubMed

    Wang, Dongxing; Zhu, Wenqi; Best, Michael D; Camden, Jon P; Crozier, Kenneth B

    2013-05-01

    Controlling light from single emitters is an overarching theme of nano-optics. Antennas are routinely used to modify the angular emission patterns of radio wave sources. "Optical antennas" translate these principles to visible and infrared wavelengths and have been recently used to modify fluorescence from single quantum dots and single molecules. Understanding the properties of single molecules, however, would be advanced were one able to observe their vibrational spectra through Raman scattering in a very reproducible manner but it is a hugely challenging task, as Raman scattering cross sections are very weak. Here we measure for the first time the highly directional emission patterns of Raman scattering from single molecules in the feed gaps of optical antennas fabricated on a chip. More than a thousand single molecule events are observed, revealing that an unprecedented near-unity fraction of optical antennas have single molecule sensitivity.

  10. The effects of Raman scattering accompanied by the soliton excitation occurring in molecular crystals

    NASA Astrophysics Data System (ADS)

    Pang, X. F.

    2001-06-01

    A theoretical research is made for the effects of Raman scattering caused by the soliton excitation occurring in the organic molecular crystals, e.g., acetanilide, on the basis of vibration model of amide-I. The energy gap between the soliton state and the vibron state have been found by partial diagonalized method in second quantized representation, which is 18.1-33 cm -1. This result is approximately consistent with the red shift value obtained from the experiments, 16 cm -1. The differential cross-section of the Raman scattering, arising from the soliton excitation, has also been obtained. Finally, we derive some properties of the Raman scattering in such a case. This result establishes spectral signatures of the soliton in the molecular crystals, which may be observed in the experiment.

  11. Surface-enhanced Raman scattering from finite arrays of gold nano-patches

    SciTech Connect

    Vincenti, M. A.; Ceglia, D. de; Grande, M.; Petruzzelli, V.; D'Orazio, A.; Bianco, G. V.; Bruno, G.; Stomeo, T.; De Vittorio, M.; Scalora, M.

    2013-01-07

    We experimentally investigate the surface-enhanced Raman scattering (SERS) response of a 2D-periodic array of square gold nano-patches, functionalized by means of a conjugated, rigid thiol. We measure a Raman signal enhancement up to 200 times more intense compared to other plasmon-based nanostructures functionalized with the same molecule, and show that the enhancement is not strictly correlated to the presence of plasmonic resonances. The agreement between experimental and theoretical results reveals the importance of a full-wave analysis based on the inclusion of the actual scattering cross section of the molecule. The proposed numerical approach may serve not only as a tool to predict the enhancement of Raman signal scattered from strongly resonant nanostructure but also as an effective instrument to engineer SERS platforms that target specific molecules.

  12. Application and Miniaturization of Linear and Nonlinear Raman Microscopy for Biomedical Imaging

    NASA Astrophysics Data System (ADS)

    Mittal, Richa

    Current diagnostics for several disorders rely on surgical biopsy or evaluation of ex vivo bodily fluids, which have numerous drawbacks. We evaluated the potential for vibrational techniques (both linear and nonlinear Raman) as a reliable and noninvasive diagnostic tool. Raman spectroscopy is an optical technique for molecular analysis that has been used extensively in various biomedical applications. Based on demonstrated capabilities of Raman spectroscopy we evaluated the potential of the technique for providing a noninvasive diagnosis of mucopolysaccharidosis (MPS). These studies show that Raman spectroscopy can detect subtle changes in tissue biochemistry. In applications where sub-micrometer visualization of tissue compositional change is required, a transition from spectroscopy to high quality imaging is necessary. Nonlinear vibrational microscopy is sensitive to the same molecular vibrations as linear Raman, but features fast imaging capabilities. Coherent Raman scattering when combined with other nonlinear optical (NLO) techniques (like two-photon excited fluorescence and second harmonic generation) forms a collection of advanced optical techniques that provide noninvasive chemical contrast at submicron resolution. This capability to examine tissues without external molecular agents is driving the NLO approach towards clinical applications. However, the unique imaging capabilities of NLO microscopy are accompanied by complex instrument requirements. Clinical examination requires portable imaging systems for rapid inspection of tissues. Optical components utilized in NLO microscopy would then need substantial miniaturization and optimization to enable in vivo use. The challenges in designing compact microscope objective lenses and laser beam scanning mechanisms are discussed. The development of multimodal NLO probes for imaging oral cavity tissue is presented. Our prototype has been examined for ex vivo tissue imaging based on intrinsic fluorescence and SHG

  13. Note: A portable Raman analyzer for microfluidic chips based on a dichroic beam splitter for integration of imaging and signal collection light paths

    SciTech Connect

    Geng, Yijia; Xu, Shuping; Xu, Weiqing; Chen, Lei; Chen, Gang; Bi, Wenbin; Cui, Haining

    2015-05-15

    An integrated and portable Raman analyzer featuring an inverted probe fixed on a motor-driving adjustable optical module was designed for the combination of a microfluidic system. It possesses a micro-imaging function. The inverted configuration is advantageous to locate and focus microfluidic channels. Different from commercial micro-imaging Raman spectrometers using manual switchable light path, this analyzer adopts a dichroic beam splitter for both imaging and signal collection light paths, which avoids movable parts and improves the integration and stability of optics. Combined with surface-enhanced Raman scattering technique, this portable Raman micro-analyzer is promising as a powerful tool for microfluidic analytics.

  14. On the critical role of Rayleigh scattering in single-molecule surface-enhanced Raman scattering via a plasmonic nanogap.

    PubMed

    Chen, Bao-Qin; Zhang, Chao; Li, Jiafang; Li, Zhi-Yuan; Xia, Younan

    2016-08-25

    Electromagnetic and chemical enhancement mechanisms are commonly used to account for single-molecule surface-enhanced Raman scattering (SM-SERS). Due to many practical limitations, however, the overall enhancement factor summed up from these two mechanisms is typically 5-6 orders of magnitude below the level of 10(14)-10(15) required for SM-SERS. Here, we demonstrate that the multiple elastic Rayleigh scattering of a molecule could play a critical role in further enhancing the Raman signal, when the molecule is trapped in a 2 nm gap between two Ag nanoparticles, pushing the overall enhancement factor close to the level needed for SM-SERS. As a universal physical process for all molecules interacting with light, we believe that Rayleigh scattering plays a pivotal and as yet unrecognized role in SERS, in particular, for enabling single-molecule sensitivity. PMID:27526632

  15. High-sensitivity pesticide detection using particle-enhanced resonant Raman scattering

    NASA Astrophysics Data System (ADS)

    Ranjan, Bikas; Saito, Yuika; Verma, Prabhat

    2016-03-01

    The use of pesticides in agriculture has raised concerns, as even a small residual of pesticide on food can be harmful. It is therefore of great importance to develop a robust technique to detect tiny amounts of pesticides. Although Raman spectroscopy is frequently used for chemical identification, it is not suitable for extremely low molecular concentrations. We propose a technique called particle-enhanced resonant Raman spectroscopy to detect extremely low concentrations of pesticides, where gold nanoparticles of desired plasmonic resonance are synthesized to match the resonance in Raman scattering. We successfully demonstrated the detection of extremely low amounts of pesticides on oranges.

  16. Characterization of semiconductor core shell nanoparticles by resonant Raman scattering and photoluminescence spectroscopy

    NASA Astrophysics Data System (ADS)

    Dzhagan, V. M.; Valakh, M. Ya.; Raevskaya, A. E.; Stroyuk, A. L.; Kuchmiy, S. Ya.; Zahn, D. R. T.

    2008-11-01

    Colloidal CdSe nanoparticles (NPs), passivated with CdS and ZnS, were characterized by resonant Raman scattering and photoluminescence (PL). The effect of the passivating shell, its volume and formation procedure on optical and vibrational spectra is discussed. Analyzing the Raman peaks due to optical phonons inside the core and those related to the core-shell interface allows some understanding of the relation between the core-shell structure and its PL properties to be achieved. In particular, a compositional intermixing at the core/shell interface of the NPs was deduced from the Raman spectra, which can noticeably affect their PL intensity.

  17. [Enhancing stimulated Raman scattering of water and heavy water lattice vibration by laser induced plasma].

    PubMed

    Shan, Xiao-Ning; Men, Zhi-Wei; Zhou, Mi; Sun, Cheng-Lin; Li, Zuo-Wei; Wang, Yi-Ding; Li, Zhan-Long

    2013-08-01

    Stimulated Raman scattering was studied in water and heavy water using pulse laser at the wavelength of 532nm, not only obtaining the stimulated Raman of O-H and O-D stretching vibration, but also obtaining the stimulated Raman lattice vibration. When the laser energy was 130 mJ, the low frequency Stokes and anti-Stokes 313 cm(-1) line of water could be observed; When the laser energy was 160 mJ, the low frequnecy Stokes and anti-Stokes 280 cm(-1) line of heavy water could be observed. The results were explained by physics mechanism of laser induced plasma.

  18. Wrinkled nanoporous gold films with ultrahigh surface-enhanced Raman scattering enhancement.

    PubMed

    Zhang, Ling; Lang, Xingyou; Hirata, Akihiko; Chen, Mingwei

    2011-06-28

    Amplified by plasomonic nanostructured metals, Raman intensity of organic molecules and biomolecules can be dramatically improved, particularly at "hot spots" where intense electromagnetic fields are produced in the vicinity of narrow nanogaps between metallic nanostructures. Therefore, developing new substrates with a high density of "hot spots" has been the recent topic of intense study. Here we report wrinkled nanoporous gold films that contain abundant Raman-active nanogaps produced by deformation and fracture of nanowire-like gold ligaments. This novel nanostructure yields ultrahigh surface enhanced Raman scattering for molecule detection.

  19. Lowering of stimulated Raman scattering threshold as a result of light capture

    NASA Astrophysics Data System (ADS)

    Gorelik, V. S.; Negriyko, A. M.; Orlovich, V. A.; Sverbil, P. P.; Tcherniega, N. V.; Vodchits, A. I.; Voinov, Y. P.; Zlobina, L. I.

    2015-01-01

    Stimulated Raman Scattering in globular photonic crystals and globular photonic glasses at different diameters of globules (250 - 400 nm) with embedded molecular liquids is studied under excitation by nanosecond or picoseconds laser pulses. Substantial decrease of Stimulated Raman Scattering threshold was observed. Such phenomenon was explained as the result of laser radiation field increase in globular photonic structures due to photonic density of states enhancement near the edges of photonic stop bands of photonic crystals and due to Mie resonance or whispering gallery modes effect revealing in photonic glasses. Stimulated Raman Scattering threshold lowering as a result of light capture in globular photonic crystals and photonic glasses opens the way to new efficient laser sources created on the base of composite globular photonic structures. Experimental data on spectra of Stimulated Raman Scattering in light and heavy waters are presented. As sources of exciting light the powerful ultra short solid state laser pulses with 532.0 nm wavelength and giant pulses of Ruby laser (694.3 nm) have been used. Several Stokes and anti-Stokes satellites were observed. Libration modes have been excited and resulted in some additional Raman bands at low frequency region and also as combining tones.

  20. Raman scattering spectra of insect virus PrGV-VP and their surface-enhanced Raman scattering spectra adsorbed on silver

    NASA Astrophysics Data System (ADS)

    Bao, PeiDi; Huang, TianQuan; Liu, XinMing; Wu, Tieqiao

    1998-04-01

    The ordinary Raman scattering (ORS) spectra of virion protein of Granulosis Virus of Cabbage Butterfly Preris rapae (PrGV-VP) and their surface-enhanced Raman scattering (SERS) spectra adsorbed on the surface of silver colloid particles have been found that the Raman signal in the SERS spectra was enhanced by a factor of about 8 X 102. In ORS spectra of PrGV-VP, it indicates that PrGV-VP has a predominantly random-coil secondary structures. All tyrosine residues are exposed. And the PrGV-VP has a gauche-gauche- gauche configuration of the C-C-S-S-C-C linkage. In SERS spectra of PrGV-VP, the intensities of bands related to COO group and NH2 group vibrations are relatively strong. We interpret that the PrGV-VP are adsorbed on the Ag surface through both the carboxylate groups and the amino groups. The efficient enhancement of amide I and amide II vibrations are impeded, because the peptide groups of PrGV-VP are screened by the side-chains amino acid residues. The Raman enhancement of PrGV-VP has a short-range mechanism. The chemisorption is a main mechanism on Ag hydrosols of PrGV- VP.

  1. Time-lapse Raman imaging of osteoblast differentiation

    NASA Astrophysics Data System (ADS)

    Hashimoto, Aya; Yamaguchi, Yoshinori; Chiu, Liang-Da; Morimoto, Chiaki; Fujita, Katsumasa; Takedachi, Masahide; Kawata, Satoshi; Murakami, Shinya; Tamiya, Eiichi

    2015-07-01

    Osteoblastic mineralization occurs during the early stages of bone formation. During this mineralization, hydroxyapatite (HA), a major component of bone, is synthesized, generating hard tissue. Many of the mechanisms driving biomineralization remain unclear because the traditional biochemical assays used to investigate them are destructive techniques incompatible with viable cells. To determine the temporal changes in mineralization-related biomolecules at mineralization spots, we performed time-lapse Raman imaging of mouse osteoblasts at a subcellular resolution throughout the mineralization process. Raman imaging enabled us to analyze the dynamics of the related biomolecules at mineralization spots throughout the entire process of mineralization. Here, we stimulated KUSA-A1 cells to differentiate into osteoblasts and conducted time-lapse Raman imaging on them every 4 hours for 24 hours, beginning 5 days after the stimulation. The HA and cytochrome c Raman bands were used as markers for osteoblastic mineralization and apoptosis. From the Raman images successfully acquired throughout the mineralization process, we found that β-carotene acts as a biomarker that indicates the initiation of osteoblastic mineralization. A fluctuation of cytochrome c concentration, which indicates cell apoptosis, was also observed during mineralization. We expect time-lapse Raman imaging to help us to further elucidate osteoblastic mineralization mechanisms that have previously been unobservable.

  2. Time-lapse Raman imaging of osteoblast differentiation

    PubMed Central

    Hashimoto, Aya; Yamaguchi, Yoshinori; Chiu, Liang-da; Morimoto, Chiaki; Fujita, Katsumasa; Takedachi, Masahide; Kawata, Satoshi; Murakami, Shinya; Tamiya, Eiichi

    2015-01-01

    Osteoblastic mineralization occurs during the early stages of bone formation. During this mineralization, hydroxyapatite (HA), a major component of bone, is synthesized, generating hard tissue. Many of the mechanisms driving biomineralization remain unclear because the traditional biochemical assays used to investigate them are destructive techniques incompatible with viable cells. To determine the temporal changes in mineralization-related biomolecules at mineralization spots, we performed time-lapse Raman imaging of mouse osteoblasts at a subcellular resolution throughout the mineralization process. Raman imaging enabled us to analyze the dynamics of the related biomolecules at mineralization spots throughout the entire process of mineralization. Here, we stimulated KUSA-A1 cells to differentiate into osteoblasts and conducted time-lapse Raman imaging on them every 4 hours for 24 hours, beginning 5 days after the stimulation. The HA and cytochrome c Raman bands were used as markers for osteoblastic mineralization and apoptosis. From the Raman images successfully acquired throughout the mineralization process, we found that β-carotene acts as a biomarker that indicates the initiation of osteoblastic mineralization. A fluctuation of cytochrome c concentration, which indicates cell apoptosis, was also observed during mineralization. We expect time-lapse Raman imaging to help us to further elucidate osteoblastic mineralization mechanisms that have previously been unobservable. PMID:26211729

  3. Highly sensitive single-beam heterodyne coherent anti-Stokes Raman scattering

    NASA Astrophysics Data System (ADS)

    von Vacano, Bernhard; Buckup, Tiago; Motzkus, Marcus

    2006-08-01

    Single-beam coherent anti-Stokes Raman-scattering (CARS) microspectroscopy achieves a complete CARS scheme with a femtosecond laser. Here, we introduce heterodyne detection in a simple experimental extension: the optical fields driving the CARS process and the local oscillator used for heterodyning are derived from a single beam of ultrashort laser pulses by pulse shaping. The heterodyne signal is amplified by more than 3 orders of magnitude and is linearly dependent on the concentration of Raman scatterers. This dramatically increases the sensitivity of chemically selective detection at microscopic resolution while maintaining the simplicity of the single-beam setup.

  4. Filling in of Fraunhofer lines in the ocean by Raman scattering.

    PubMed

    Kattawar, G W; Xu, X

    1992-10-20

    We have developed a Monte Carlo program that can account for Raman scattering in the ocean when polarization effects are not considered. The program is capable of coupling an inhomogeneous atmosphere to an inhomogeneous ocean through a dielectric interface. We have studied the filling in of both the 486-nm H(beta) and the 518-nm Mg Fraunhofer lines caused by Raman scattering in the ocean. The amount of fill varies with solar zenith angle, angle of view, depth in the ocean, and magnitude of the cross sections. By monitoring the shapes of Fraunhofer lines we can learn a great deal about the relative importance of this inelastic process in oceanic optics.

  5. Infrared reflection and Raman scattering on Ba 1-xRb xBiO 3

    NASA Astrophysics Data System (ADS)

    Inoue, A.; Iyo, A.; Oiji, Y.; Tanaka, Y.; Tokumoto, M.; Uwe, H.; Sakudo, T.

    1991-12-01

    Measurements of infrared (IR) reflectivity and Raman scattering have been performed on Ba 1-xRb xBiO 3. The oscillator strength of the Bi-Bi stretching mode decreases with increasing Rb concentration, while the frequency change is small. The phonons detected by the Raman scattering experiment have the same frequencies as the LO phonons, although the system has the center of symmetry in the average structure. It is suggested that the coherence length of the charge density wave shorter than the incident laser wavelength 5145Å gets shorter with increasing the Rb concentration.

  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. PMID:27203727

  7. Theory of Two-Magnon Raman Scattering in Iron Pnictides and Chalcogenides

    SciTech Connect

    Chen, C. C.

    2011-08-15

    Although the parent iron-based pnictides and chalcogenides are itinerant antiferromagnets, the use of local moment picture to understand their magnetic properties is still widespread. We study magnetic Raman scattering from a local moment perspective for various quantum spin models proposed for this new class of superconductors. These models vary greatly in the level of magnetic frustration and show a vastly different two-magnon Raman response. Light scattering by two-magnon excitations thus provides a robust and independent measure of the underlying spin interactions. In accord with other recent experiments, our results indicate that the amount of magnetic frustration in these systems may be small.

  8. 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.

  9. The controlled pulsed laser deposition of Ag nanoparticle arrays for surface enhanced Raman scattering.

    PubMed

    D'Andrea, C; Neri, F; Ossi, P M; Santo, N; Trusso, S

    2009-06-17

    An effective method for the production of surface enhanced Raman scattering (SERS) active substrates is presented. Nanostructured silver thin films are pulsed laser deposited in an argon atmosphere. The films consist of arrays of nanoparticles whose size is controlled by the Ar pressure. The surface morphology of the films can be tuned by the laser pulse number. Nanoparticle size is calculated by a phenomenological model taking into account the dynamics of the laser generated silver plasma. The SERS activity of the films is investigated by Raman scattering of adsorbed rhodamine 6G at different concentrations.

  10. Surface-enhanced resonance Raman scattering from methylviologen at a silver electrode: Evidence for two distinct adsorption interactions

    SciTech Connect

    Feng, Qiao; Yue, W.; Cotton, T.M. )

    1990-03-08

    The electronic absorption and resonance Raman spectra of methylviologen radical cation (MV{sup {sm bullet}+}) and fully reduced methylviologen (MV{sup 0}) have been characterized. The enhancement of Raman and resonance Raman (RR) scattering from the dication and its reduction products at polished and roughened silver electrodes was also investigated.

  11. Contributed Review: A new synchronized source solution for coherent Raman scattering microscopy.

    PubMed

    Wang, Ke; Wang, Yuxin; Liang, Runfu; Wang, Jiaqi; Qiu, Ping

    2016-07-01

    Based on vibrational spectroscopy, coherent Raman Scattering (CRS) microscopy allows label-free imaging of biological and chemical samples with endogenous image contrast. Two-color, synchronized picosecond pulses are typically used for high spectral resolution imaging, which in turn constitutes a dramatic laser source challenge for CRS microscopy. Recently, synchronized time-lens source, inspired from ultrafast optical signal processing, has emerged as a promising laser source solution and has found application in various modalities of CRS microscopy. Time-lens is based on space-time analogy, which uses a "lens" in the time domain to compress long optical pulses or even continuous waves to ultrashort pulses, mimicking a lens in the space domain. Phase and intensity modulators driven with electrical signals are used in the time-lens source for picosecond pulse generation. As a result, the time-lens source is highly versatile and naturally compatible with modulation capabilities. More importantly, if the electrical signals used to drive the time-lens source are derived from other laser sources, such as mode-locked lasers, then synchronization between them can be realized, underlying the physics of a synchronized time-lens source. In this paper, we review recent progress on the basic principle, design of the synchronized time-lens source, and its applications to CRS microscopy of both biological and chemical samples. PMID:27475540

  12. Contributed Review: A new synchronized source solution for coherent Raman scattering microscopy

    NASA Astrophysics Data System (ADS)

    Wang, Ke; Wang, Yuxin; Liang, Runfu; Wang, Jiaqi; Qiu, Ping

    2016-07-01

    Based on vibrational spectroscopy, coherent Raman Scattering (CRS) microscopy allows label-free imaging of biological and chemical samples with endogenous image contrast. Two-color, synchronized picosecond pulses are typically used for high spectral resolution imaging, which in turn constitutes a dramatic laser source challenge for CRS microscopy. Recently, synchronized time-lens source, inspired from ultrafast optical signal processing, has emerged as a promising laser source solution and has found application in various modalities of CRS microscopy. Time-lens is based on space-time analogy, which uses a "lens" in the time domain to compress long optical pulses or even continuous waves to ultrashort pulses, mimicking a lens in the space domain. Phase and intensity modulators driven with electrical signals are used in the time-lens source for picosecond pulse generation. As a result, the time-lens source is highly versatile and naturally compatible with modulation capabilities. More importantly, if the electrical signals used to drive the time-lens source are derived from other laser sources, such as mode-locked lasers, then synchronization between them can be realized, underlying the physics of a synchronized time-lens source. In this paper, we review recent progress on the basic principle, design of the synchronized time-lens source, and its applications to CRS microscopy of both biological and chemical samples.

  13. In Vivo Chemical and Structural Analysis of Plant Cuticular Waxes Using Stimulated Raman Scattering Microscopy1[OPEN

    PubMed Central

    Mansfield, Jessica C.; Perfect, Sarah; Seymour, Mark; Smirnoff, Nicholas; Love, John; Moger, Julian

    2015-01-01

    The cuticle is a ubiquitous, predominantly waxy layer on the aerial parts of higher plants that fulfils a number of essential physiological roles, including regulating evapotranspiration, light reflection, and heat tolerance, control of development, and providing an essential barrier between the organism and environmental agents such as chemicals or some pathogens. The structure and composition of the cuticle are closely associated but are typically investigated separately using a combination of structural imaging and biochemical analysis of extracted waxes. Recently, techniques that combine stain-free imaging and biochemical analysis, including Fourier transform infrared spectroscopy microscopy and coherent anti-Stokes Raman spectroscopy microscopy, have been used to investigate the cuticle, but the detection sensitivity is severely limited by the background signals from plant pigments. We present a new method for label-free, in vivo structural and biochemical analysis of plant cuticles based on stimulated Raman scattering (SRS) microscopy. As a proof of principle, we used SRS microscopy to analyze the cuticles from a variety of plants at different times in development. We demonstrate that the SRS virtually eliminates the background interference compared with coherent anti-Stokes Raman spectroscopy imaging and results in label-free, chemically specific confocal images of cuticle architecture with simultaneous characterization of cuticle composition. This innovative use of the SRS spectroscopy may find applications in agrochemical research and development or in studies of wax deposition during leaf development and, as such, represents an important step in the study of higher plant cuticles. PMID:25783412

  14. Multiband electron resonant Raman scattering in quantum wells in a magnetic field

    NASA Astrophysics Data System (ADS)

    López-Richard, V.; Hai, G.-Q.; Trallero-Giner, C.; Marques, G. E.

    2003-04-01

    A theoretical model has been developed for the electronic resonant Raman scattering processes in direct band zinc blende type semiconductor quantum wells in a magnetic field. In order to take into account the spin-flip transitions, anomalous behavior of the Landau levels and the Landè g factor, an 8×8 Kane-Weiler Hamiltonian model has been considered for the evaluation of the Raman scattering amplitude. Elements concerning the selection rules of resonant inelastic light scattering in quantum well systems are reported. The multiband model predicts conditions for resonant spin-flip Raman processes in several light scattering configurations for crossed and parallel polarization. Special emphasis is given to the effects of the interlevel coupling and mixing within the conduction subband and their relation to spin-flip and inter-Landau level transitions. Symmetry and electronic properties of the level structure in the first conduction subband as well as anomalous Landè factors are discussed in terms of complementary Raman scattering configurations, Fermi energy, and multiband parameters.

  15. Learning-based imaging through scattering media.

    PubMed

    Horisaki, Ryoichi; Takagi, Ryosuke; Tanida, Jun

    2016-06-27

    We present a machine-learning-based method for single-shot imaging through scattering media. The inverse scattering process was calculated based on a nonlinear regression algorithm by learning a number of training object-speckle pairs. In the experimental demonstration, multilayer phase objects between scattering plates were reconstructed from intensity measurements. Our approach enables model-free sensing, where it is not necessary to know the sensing processes/models. PMID:27410537

  16. Accurate and approximate calculations of Raman scattering in the atmosphere of Neptune

    NASA Astrophysics Data System (ADS)

    Sromovsky, L. A.

    2005-01-01

    Raman scattering by H 2 in Neptune's atmosphere has significant effects on its reflectivity for λ<0.5 μm, producing baseline decreases of ˜20% in a clear atmosphere and ˜10% in a hazy atmosphere. However, few accurate Raman calculations are carried out because of their complexity and computational costs. Here we present the first radiation transfer algorithm that includes both polarization and Raman scattering and facilitates computation of spatially resolved spectra. New calculations show that Cochran and Trafton's (1978, Astrophys. J. 219, 756-762) suggestion that light reflected in the deep CH 4 bands is mainly Raman scattered is not valid for current estimates of the CH 4 vertical distribution, which implies only a 4% Raman contribution. Comparisons with IUE, HST, and groundbased observations confirm that high altitude haze absorption is reducing Neptune's geometric albedo by ˜6% in the 0.22-0.26 μm range and by ˜13% in the 0.35-0.45 μm range. A sample haze model with 0.2 optical depths of 0.2-μm radius particles between 0.1 and 0.8 bars fits reasonably well, but is not a unique solution. We used accurate calculations to evaluate several approximations of Raman scattering. The Karkoschka (1994, Icarus 111, 174-192) method of applying Raman corrections to calculated spectra and removing Raman effects from observed spectra is shown to have limited applicability and to undercorrect the depths of weak CH 4 absorption bands. The relatively large Q-branch contribution observed by Karkoschka is shown to be consistent with current estimates of Raman cross-sections. The Wallace (1972, Astrophys. J. 176, 249-257) approximation, produces geometric albedo ˜5% low as originally proposed, but can be made much more accurate by including a scattering contribution from the vibrational transition. The original Pollack et al. (1986, Icarus 65, 442-466) approximation is inaccurate and unstable, but can be greatly improved by several simple modifications. A new

  17. MicroRaman Spectroscopy and Raman Imaging of Basal Cell Carcinoma

    NASA Astrophysics Data System (ADS)

    Short, M. A.; Zeng, H.; Lui, H.

    2005-03-01

    We have measured the Raman spectra of normal and cancerous skin tissues using a confocal microRaman spectrograph with a sub-micron spatial resolution. We found that the Raman spectrum of a cell nucleolus is different from the spectra measured outside the nucleolus and considerably different from those measured outside the nucleus. In addition, we found significant spectroscopic differences between normal and cancer-bearing sites in the dermis region. In order to utilize these differences for non-invasive skin cancer diagnosis, we have developed a Raman imaging system that clearly demonstrates the structure, location and distribution of cells in unstained skin biopsy samples. Our method is expected to be useful for the detection and characterization of skin cancer based on the known distinct cellular differences between normal and malignant skin.

  18. Resonant Raman scattering theory for Kitaev models and their Majorana fermion boundary modes

    NASA Astrophysics Data System (ADS)

    Perreault, Brent; Knolle, Johannes; Perkins, Natalia B.; Burnell, F. J.

    2016-09-01

    We study the inelastic light scattering response in two- (2D) and three-dimensional (3D) Kitaev spin-liquid models with Majorana spinon band structures in the symmetry classes BDI and D leading to protected gapless surface modes. We present a detailed calculation of the resonant Raman/Brillouin scattering vertex relevant to iridate and ruthenate compounds whose low-energy physics is believed to be proximate to these spin-liquid phases. In the symmetry class BDI, we find that while the resonant scattering on thin films can detect the gapless boundary modes of spin liquids, the nonresonant processes do not couple to them. For the symmetry class D, however, we find that the coupling between both types of light-scattering processes and the low-energy surface states is strongly suppressed. Additionally, we describe the effect of weak time-reversal symmetry breaking perturbations on the bulk Raman response of these systems.

  19. Effect of photodynamic therapy on single cancer cells studied by integrated Raman and angular scattering microscopy

    NASA Astrophysics Data System (ADS)

    Shipp, Dustin W.; Mitra, Soumya; Foster, Thomas H.; Berger, Andrew J.

    2012-01-01

    Using integrated Raman and angular scattering microscopy (IRAM), we follow the response of EMT6 cancer cells to photodynamic therapy (PDT) treatment. The study combines two non-labelling light scattering techniques to extract chemical information and organelle sizes from single cells. Each cell is measured repeatedly over several hours to follow changes in these parameters as the cell responds to the PDT treatment. An automated algorithm identifies which parameters are changing in time. Size parameters extracted from angular scattering measurements show a decrease in the size of 1-micron-diameter scatterers in treated cells. Treated cells also exhibit trends in several Raman peaks, denoting changes in chemical concentrations of proteins, nucleic acids, and lipids. Each of these parameters - acquired from both measurement modalities - can be monitored on a cell-by-cell basis. The ability to track these chemical and structural changes over time allows access to greater knowledge of biological processes.

  20. RAMAN spectroscopy imaging improves the diagnosis of papillary thyroid carcinoma

    PubMed Central

    Rau, Julietta V.; Graziani, Valerio; Fosca, Marco; Taffon, Chiara; Rocchia, Massimiliano; Crucitti, Pierfilippo; Pozzilli, Paolo; Onetti Muda, Andrea; Caricato, Marco; Crescenzi, Anna

    2016-01-01

    Recent investigations strongly suggest that Raman spectroscopy (RS) can be used as a clinical tool in cancer diagnosis to improve diagnostic accuracy. In this study, we evaluated the efficiency of Raman imaging microscopy to discriminate between healthy and neoplastic thyroid tissue, by analyzing main variants of Papillary Thyroid Carcinoma (PTC), the most common type of thyroid cancer. We performed Raman imaging of large tissue areas (from 100 × 100 μm2 up to 1 × 1 mm2), collecting 38 maps containing about 9000 Raman spectra. Multivariate statistical methods, including Linear Discriminant Analysis (LDA), were applied to translate Raman spectra differences between healthy and PTC tissues into diagnostically useful information for a reliable tissue classification. Our study is the first demonstration of specific biochemical features of the PTC profile, characterized by significant presence of carotenoids with respect to the healthy tissue. Moreover, this is the first evidence of Raman spectra differentiation between classical and follicular variant of PTC, discriminated by LDA with high efficiency. The combined histological and Raman microscopy analyses allow clear-cut integration of morphological and biochemical observations, with dramatic improvement of efficiency and reliability in the differential diagnosis of neoplastic thyroid nodules, paving the way to integrative findings for tumorigenesis and novel therapeutic strategies. PMID:27725756

  1. RAMAN spectroscopy imaging improves the diagnosis of papillary thyroid carcinoma

    NASA Astrophysics Data System (ADS)

    Rau, Julietta V.; Graziani, Valerio; Fosca, Marco; Taffon, Chiara; Rocchia, Massimiliano; Crucitti, Pierfilippo; Pozzilli, Paolo; Onetti Muda, Andrea; Caricato, Marco; Crescenzi, Anna

    2016-10-01

    Recent investigations strongly suggest that Raman spectroscopy (RS) can be used as a clinical tool in cancer diagnosis to improve diagnostic accuracy. In this study, we evaluated the efficiency of Raman imaging microscopy to discriminate between healthy and neoplastic thyroid tissue, by analyzing main variants of Papillary Thyroid Carcinoma (PTC), the most common type of thyroid cancer. We performed Raman imaging of large tissue areas (from 100 × 100 μm2 up to 1 × 1 mm2), collecting 38 maps containing about 9000 Raman spectra. Multivariate statistical methods, including Linear Discriminant Analysis (LDA), were applied to translate Raman spectra differences between healthy and PTC tissues into diagnostically useful information for a reliable tissue classification. Our study is the first demonstration of specific biochemical features of the PTC profile, characterized by significant presence of carotenoids with respect to the healthy tissue. Moreover, this is the first evidence of Raman spectra differentiation between classical and follicular variant of PTC, discriminated by LDA with high efficiency. The combined histological and Raman microscopy analyses allow clear-cut integration of morphological and biochemical observations, with dramatic improvement of efficiency and reliability in the differential diagnosis of neoplastic thyroid nodules, paving the way to integrative findings for tumorigenesis and novel therapeutic strategies.

  2. Improved Intrapulse Raman Scattering Control via Asymmetric Airy Pulses

    NASA Astrophysics Data System (ADS)

    Hu, Yi; Tehranchi, Amirhossein; Wabnitz, Stefan; Kashyap, Raman; Chen, Zhigang; Morandotti, Roberto

    2015-02-01

    We experimentally demonstrate the possibility of tuning the frequency of a laser pulse via the use of an Airy pulse-seeded soliton self-frequency shift. The intrinsically asymmetric nature of Airy pulses, typically featured by either leading or trailing oscillatory tails (relatively to the main lobe), is revealed through the nonlinear generation of both a primary and a secondary Raman soliton self-frequency shift, a phenomenon which is driven by the soliton fission processes. The resulting frequency shift can be carefully controlled by using time-reversed Airy pulses or, alternatively, by applying an offset to the cubic phase modulation used to generate the pulses. When compared with the use of conventional chirped Gaussian pulses, our technique brings about unique advantages in terms of both efficient frequency tuning and feasibility, along with the generation and control of multicolor Raman solitons with enhanced tunability. Our theoretical analysis agrees well with our experimental observations.

  3. Raman-based imaging uncovers the effects of alginate hydrogel implants in spinal cord injury

    NASA Astrophysics Data System (ADS)

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

    2015-07-01

    The treatment of spinal cord injury by using implants that provide a permissive environment for axonal growth is in the focus of the research for regenerative therapies. Here, Raman-based label-free techniques were applied for the characterization of morphochemical properties of surgically induced spinal cord injury in the rat that received an implant of soft unfunctionalized alginate hydrogel. Raman microspectroscopy followed by chemometrics allowed mapping the different degenerative areas, while multimodal multiphoton microscopy (e.g. the combination of coherent anti-Stokes Raman scattering (CARS), endogenous two-photon fluorescence and second harmonic generation on the same platform) enabled to address the morphochemistry of the tissue at cellular level. The regions of injury, characterized by demyelination and scarring, were retrieved and the distribution of key tissue components was evaluated by Raman mapping. The alginate hydrogel was detected in the lesion up to six months after implantation and had positive effects on the nervous tissue. For instance, multimodal multiphoton microscopy complemented the results of Raman mapping, providing the micromorphology of lipid-rich tissue structures by CARS and enabling to discern lipid-rich regions that contained myelinated axons from degenerative regions characterized by myelin fragmentation and presence of foam cells. These findings demonstrate that Raman-based imaging methods provide useful information for the evaluation of alginate implant effects and have therefore the potential to contribute to new strategies for monitoring degenerative and regenerative processes induced in SCI, thereby improving the effectiveness of therapies.

  4. Cavity coherent-state cloning via Raman scattering

    SciTech Connect

    Alexanian, Moorad

    2003-03-01

    The Raman interaction of atoms singly traversing a two-mode cavity constitutes a quantum-cloning machine for coherent states. The quality of the two identical output coherent states is independent of the initial, albeit different, coherent state, initially present inside the cavity. The cloning of nonorthogonal states indicates that the entanglement of the output states for an arbitrary initial state is the essence of the no-cloning theorem.

  5. Quantitative Raman imaging investigations of mixing phenomena in high-pressure cryogenic jets.

    PubMed

    Decker, M; Schik, A; Meier, U E; Stricker, W

    1998-08-20

    A two-dimensional Raman technique was used to investigate mixing phenomena of cryogenic jets under both supercritical and transcritical conditions. The aim of this study was to enlarge the experimental data basis for modeling purposes and to provide quantitative information to help to improve the design of injectors for high-pressure rocket engine combustion chambers. Cryogenic nitrogen, which served as substitute for liquid O(2), was injected into N(2) at room temperature at pressures up to 6.0 MPa. The liquid N(2) jet could be atomized by a coaxial H(2) flow. Raman scattering was generated with a XeF excimer laser. The resulting signal images were discriminated against background by spectral filtering and preferential detection of light with a polarization corresponding to the polarization of the laser, thus making use of the conserved polarization of the Raman-scattered light. The Raman images were converted into density distributions of N(2) and H(2), respectively, as well as into temperature distributions for a variety of experimental conditions.

  6. Raman scattering in sodium nitrite crystals near the phase transition

    NASA Astrophysics Data System (ADS)

    Gorelik, V. S.; Pyatyshev, A. Yu.; Krylov, A. S.

    2016-01-01

    Optical Raman spectra of a ferroelectric sodium nitrite crystal have been detected in a wide spectrum range at various temperatures, including the region of the ferroelectric phase transition. A manifestation of a transverse soft polar mode of the A 1( z) type responsible for the ferroelectric phase transition has been discovered in the spectrum at room temperature. This mode has been found to become overdamped even far from the ferroelectric phase transition temperature. This mode also appears as a central peak under heating. It has been found that the pseudoscalar mode of the A 2 type has the highest intensity in the Raman spectrum of sodium nitrite. The frequency corresponding to the maximum intensity of this mode in the Raman spectrum varies from 130 cm-1 at 123 K to 106 cm-1 at T = 513 K. A fair agreement of the experimental data for the A 1( z) mode with the Lyddane-Sachs-Teller relation has been established. The polariton curves for the A 1( z) polar mode and the dispersion curves for axinons has been plotted.

  7. Onset of stimulated Raman scattering of a laser in a plasma in the presence of hot drifting electrons

    SciTech Connect

    Gupta, D. N. Yadav, Pinki; Avinash, K.; Jang, D. G.; Suk, H.; Hur, M. S.

    2015-05-15

    Stimulated Raman scattering of a laser in plasmas with energetic drifting electrons was investigated by analyzing the growth of interacting waves during the Raman scattering process. The Langmuir wave and scattered electromagnetic sideband wave grow initially and are dampened after attaining a maximum level that indicates a periodic exchange of energy between the pump wave and the daughter waves. The presence of energetic drifting electrons in the laser-produced plasma influences the stimulated Raman scattering process. The plasma wave generated by Raman scattering may be influenced by the energetic electrons, which enhance the growth rate of the instability. Our results show that the presence of energetic (hot) drifting electrons in a plasma has an important effect on the evolution of the interacting waves. This phenomenon is modeled via two-dimensional particle-in-cell simulations of the propagation and interaction of the laser under Raman instability.

  8. Surface-enhanced Raman scattering on optical material fabricated by femtosecond laser

    NASA Astrophysics Data System (ADS)

    Wang, Wenhui; Huo, Haibin; Wu, Nan; Shen, Mengyan; Guthy, Charles; Wang, Xingwei

    2010-04-01

    Raman spectroscopy is a technology that can detect and distinguish materials based on the materials' Raman scattering. However, the signal produced using this technology is usually too small to be useful. The Raman spectrum signal can be enhanced by creating rough patches on the surface of the material. In this paper, a novel method to produce nanometer-sized features on optical materials such as glass, fused silica, and quartz substrate is presented. Using a femtosecond laser, the transparent materials are sputtered and deposited. When the materials cool down, they produce structures with nano-features. These nano-features on optical materials can make designing optical sensing systems much easier. Scanning electron microscope photos of nano-structures on quartz substrate and optical fiber show that features less than 100 nm in size have been successfully fabricated. The 3D micro- and nano-structures of the sensor were studied using a confocal Raman spectrum microscope and focused ion-beam milling. Raman spectrum signals show that the strength of the signal generated by Raman scattering was greatly enhanced compared to substrates without nano-features.

  9. The use of surface-enhanced Raman scattering for detecting molecular evidence of life in rocks, sediments, and sedimentary deposits.

    PubMed

    Bowden, Stephen A; Wilson, Rab; Cooper, Jonathan M; Parnell, John

    2010-01-01

    Raman spectroscopy is a versatile analytical technique capable of characterizing the composition of both inorganic and organic materials. Consequently, it is frequently suggested as a payload on many planetary landers. Only approximately 1 in every 10(6) photons are Raman scattered; therefore, the detection of trace quantities of an analyte dispersed in a sample matrix can be much harder to achieve. To overcome this, surface-enhanced Raman scattering (SERS) and surface-enhanced resonance Raman scattering (SERRS) both provide greatly enhanced signals (enhancements between 10(5) and 10(9)) through the analyte's interaction with the locally generated surface plasmons, which occur at a "roughened" or nanostructured metallic surface (e.g., Cu, Au, and Ag). Both SERS and SERRS may therefore provide a viable technique for trace analysis of samples. In this paper, we describe the development of SERS assays for analyzing trace amounts of compounds present in the solvent extracts of sedimentary deposits. These assays were used to detect biological pigments present in an Arctic microoasis (a small locale of elevated biological productivity) and its detrital regolith, characterize the pigmentation of microbial mats around hydrothermal springs, and detect fossil organic matter in hydrothermal deposits. These field study examples demonstrate that SERS technology is sufficiently mature to be applied to many astrobiological analog studies on Earth. Many current and proposed imaging systems intended for remote deployment already posses the instrumental components needed for SERS. The addition of wet chemistry sample processing facilities to these instruments could yield field-deployable analytical instruments with a broadened analytical window for detecting organic compounds with a biological or geological origin.

  10. The use of surface-enhanced Raman scattering for detecting molecular evidence of life in rocks, sediments, and sedimentary deposits.

    PubMed

    Bowden, Stephen A; Wilson, Rab; Cooper, Jonathan M; Parnell, John

    2010-01-01

    Raman spectroscopy is a versatile analytical technique capable of characterizing the composition of both inorganic and organic materials. Consequently, it is frequently suggested as a payload on many planetary landers. Only approximately 1 in every 10(6) photons are Raman scattered; therefore, the detection of trace quantities of an analyte dispersed in a sample matrix can be much harder to achieve. To overcome this, surface-enhanced Raman scattering (SERS) and surface-enhanced resonance Raman scattering (SERRS) both provide greatly enhanced signals (enhancements between 10(5) and 10(9)) through the analyte's interaction with the locally generated surface plasmons, which occur at a "roughened" or nanostructured metallic surface (e.g., Cu, Au, and Ag). Both SERS and SERRS may therefore provide a viable technique for trace analysis of samples. In this paper, we describe the development of SERS assays for analyzing trace amounts of compounds present in the solvent extracts of sedimentary deposits. These assays were used to detect biological pigments present in an Arctic microoasis (a small locale of elevated biological productivity) and its detrital regolith, characterize the pigmentation of microbial mats around hydrothermal springs, and detect fossil organic matter in hydrothermal deposits. These field study examples demonstrate that SERS technology is sufficiently mature to be applied to many astrobiological analog studies on Earth. Many current and proposed imaging systems intended for remote deployment already posses the instrumental components needed for SERS. The addition of wet chemistry sample processing facilities to these instruments could yield field-deployable analytical instruments with a broadened analytical window for detecting organic compounds with a biological or geological origin. PMID:20735253

  11. Using Raman Spectroscopy and Surface-Enhanced Raman Scattering to Identify Colorants in Art: An Experiment for an Upper-Division Chemistry Laboratory

    ERIC Educational Resources Information Center

    Mayhew, Hannah E.; Frano, Kristen A.; Svoboda, Shelley A.; Wustholz, Kristin L.

    2015-01-01

    Surface-enhanced Raman scattering (SERS) studies of art represent an attractive way to introduce undergraduate students to concepts in nanoscience, vibrational spectroscopy, and instrumental analysis. Here, we present an undergraduate analytical or physical chemistry laboratory wherein a combination of normal Raman and SERS spectroscopy is used to…

  12. Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy: Expanding the Versatility of Surface-Enhanced Raman Scattering

    NASA Astrophysics Data System (ADS)

    Anema, Jason R.; Li, Jian-Feng; Yang, Zhi-Lin; Ren, Bin; Tian, Zhong-Qun

    2011-07-01

    Surface-enhanced Raman scattering (SERS) is a powerful technique for detection and characterization because of its extremely high sensitivity and the rich structural information that it can offer. However, most SERS substrates are composed of Au, Ag, or Cu, and a lack of substrate generality has greatly limited the breadth of the use of SERS. Recently, we have devised a method by which SERS can be obtained from virtually any surface. Au nanoparticles are coated with ultrathin silica shells. The Au core provides Raman signal enhancement; the silica shell prevents the core from coming into direct contact with probe/analyte molecules or the surface over which these particles are spread (i.e., prevents the contamination of the chemical system under study). In the present review, we expand upon previous discussion of the enhancement mechanism; procedures for the synthesis and characterization of our nanoparticles; and applications in surface chemistry, electrochemistry, and inspection.

  13. Plasmonics for surface-enhanced Raman scattering: from classical to quantum

    NASA Astrophysics Data System (ADS)

    Zhu, Wenqi

    Metallic nanostructures that employ localized surface plasmon resonances to capture or radiate electromagnetic waves at optical frequencies are termed "plasmonic optical antennas". These structures enhance light-matter interactions in an efficient manner, enabling unique linear and nonlinear optical applications. One such application is surface-enhanced Raman scattering (SERS), which employs plasmonic antennas to enhance Raman cross-section of molecules by orders of magnitude. SERS has attracted a significant amount of research attention since it enables molecules to be identified through their characteristic vibrational spectra, even at the single molecule level. In this thesis, we investigate the mechanisms underlying electromagnetic enhancement in SERS, and optimize plasmonic optical antenna designs to allow efficient SERS detection. We first demonstrate a top-down fabrication procedure to reproducibly fabricate plasmonic dimers with controllable gap widths that can be as small as 3 nm. We experimentally demonstrate that SERS enhancements increase as the gap size is reduced. The method we introduce is capable of routinely delivering reproducible SERS substrates with high enhancement factors. We then investigate a technique termed "energy-momentum spectroscopy" to measure Raman emission patterns, i.e. the angular distribution of Raman scattering. In particular, we demonstrate how they are modified by plasmonic optical antennas. It is found that the Raman scattering from molecules on plasmonic dimers (pairs of gold rods) forms two beams into the substrate which supports the dimers. This would normally necessitate the use of an objective lens with a large numerical aperture for efficient collection. We investigate the abilities of two alternative optical antenna designs to modify the angular distribution of Raman scattering. We term this effect "beamed Raman scattering". The first antenna design is that of Yagi-Uda antennas. The second design consists of plasmonic

  14. Rapid detection of benzoyl peroxide in wheat flour by using Raman scattering spectroscopy

    NASA Astrophysics Data System (ADS)

    Zhao, Juan; Peng, Yankun; Chao, Kuanglin; Qin, Jianwei; Dhakal, Sagar; Xu, Tianfeng

    2015-05-01

    Benzoyl peroxide is a common flour additive that improves the whiteness of flour and the storage properties of flour products. However, benzoyl peroxide adversely affects the nutritional content of flour, and excess consumption causes nausea, dizziness, other poisoning, and serious liver damage. This study was focus on detection of the benzoyl peroxide added in wheat flour. A Raman scattering spectroscopy system was used to acquire spectral signal from sample data and identify benzoyl peroxide based on Raman spectral peak position. The optical devices consisted of Raman spectrometer and CCD camera, 785 nm laser module, optical fiber, prober, and a translation stage to develop a real-time, nondestructive detection system. Pure flour, pure benzoyl peroxide and different concentrations of benzoyl peroxide mixed with flour were prepared as three sets samples to measure the Raman spectrum. These samples were placed in the same type of petri dish to maintain a fixed distance between the Raman CCD and petri dish during spectral collection. The mixed samples were worked by pretreatment of homogenization and collected multiple sets of data of each mixture. The exposure time of this experiment was set at 0.5s. The Savitzky Golay (S-G) algorithm and polynomial curve-fitting method was applied to remove the fluorescence background from the Raman spectrum. The Raman spectral peaks at 619 cm-1, 848 cm-1, 890 cm-1, 1001 cm-1, 1234 cm-1, 1603cm-1, 1777cm-1 were identified as the Raman fingerprint of benzoyl peroxide. Based on the relationship between the Raman intensity of the most prominent peak at around 1001 cm-1 and log values of benzoyl peroxide concentrations, the chemical concentration prediction model was developed. This research demonstrated that Raman detection system could effectively and rapidly identify benzoyl peroxide adulteration in wheat flour. The experimental result is promising and the system with further modification can be applicable for more products in near

  15. Cars (coherent anti-Stokes Raman scattering) diagnostics in reacting mixtures

    SciTech Connect

    Valentini, J.J. )

    1989-01-01

    Coherent anti-Stokes Raman scattering (CARS) is a coherent optical variant of the inelastic light scattering process known as the Raman effect. CARS spectroscopy possesses the universality of Raman spectroscopy but with greatly enhanced sensitivity. It is insensitive to background luminescence, can be configured to allow remote measurements, has excellent temporal and spatial resolution, and can provide detailed information on both the chemical composition and physical state of gas, liquid, and solid samples. Because of these desirable attributes CARS has become an important optical diagnostic method, in particular for characterizing combustion media, plasmas, and chemically reacting mixtures. This article provides a brief introduction and overview of such applications of CARS, with a particular emphasis on the last of these.

  16. Enhanced Raman scattering assisted by ultrahigh order modes of the double metal cladding waveguide

    SciTech Connect

    Xu, Tian; Huang, Liming; Jin, Yonglong; Fang, Jinghuai E-mail: fjhuai@ntu.edu.cn; Yin, Cheng E-mail: fjhuai@ntu.edu.cn; Huang, Meizhen

    2014-10-20

    Distinguished from the usual strategy to enhance the Raman scattering such as creating hot spots in the surface-enhanced Raman scattering, this paper takes a quite different approach based on the double metal cladding waveguide. The target analyte is located in the guiding layer of sub-millimeter scale, where several ultrahigh order modes with high intensity are simultaneously excited via a focused laser beam. The experimental setup is simple, and both simulation and experimental results confirm the enhancement mechanism of these oscillating modes. Other appealing features include the large detection area and the ability to excite guided modes via both polarizations. This scheme can be applied to large molecules detection and readily integrated with other Raman enhancement techniques.

  17. Measurement of the Raman scattering cross section of the breathing mode in KDP and DKDP crystals.

    PubMed

    Demos, Stavros G; Raman, Rajesh N; Yang, Steven T; Negres, Raluca A; Schaffers, Kathleen I; Henesian, Mark A

    2011-10-10

    The spontaneous Raman scattering cross sections of the main peaks (related to the A1 vibrational mode) in rapid and conventional grown potassium dihydrogen phosphate and deuterated crystals are measured at 532 nm, 355 nm, and 266 nm. The measurement involves the use of the Raman line of water centered at 3400 cm-1 as a reference to obtain relative values of the cross sections which are subsequently normalized against the known absolute value for water as a function of excitation wavelength. This measurement enables the estimation of the transverse stimulated Raman scattering gain of these nonlinear optical materials in various configurations suitable for frequency conversion and beam control in high-power, large-aperture laser systems.

  18. Raman scattering of rare earth sesquioxide Ho₂O₃: A pressure and temperature dependent study

    SciTech Connect

    Pandey, Sugandha Dogra; Samanta, K.; Singh, Jasveer; Sharma, Nita Dilawar; Bandyopadhyay, A. K.

    2014-10-07

    Pressure and temperature dependent Raman scattering studies on Ho₂O₃ have been carried out to investigate the structural transition and the anharmonic behavior of the phonons. Ho₂O₃ undergoes a transition from cubic to monoclinic phase above 15.5 GPa, which is partially reversible on decompression. The anharmonic behavior of the phonon modes of Ho₂O₃ from 80 K to 440 K has been investigated. We find an anomalous line-width change with temperature. The mode Grüneisen parameter of bulk Ho₂O₃ was estimated from high pressure Raman investigation up to 29 GPa. Furthermore, the anharmonic components were calculated from the temperature dependent Raman scattering.

  19. 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.

  20. [Obtaining aerosol backscattering coefficient using pure rotational Raman-Mie scattering spectrum].

    PubMed

    Rong, Wei; Chen, Si-Ying; Zhang, Yin-Chao; Chen, He; Guo, Pan

    2012-11-01

    Both the traditional Klett and Fernald methods used to obtain atmospheric aerosol backscattering coefficient require the hypothesis of relationship between the extinction coefficient and backscattering coefficient, and this will bring error. According to the theory that the pure rotational Raman backscattering coefficient is only related to atmospheric temperature and pressure, a new method is presented for inverting aerosol backscattering coefficient, which needed the intensity of elastic scattering and rotational Raman combined with atmospheric temperature and pressure obtained with the sounding balloons in this article. This method can not only eliminate the errors of the traditional Klett and Fernald methods caused by the hypothesis, but also avoid the error caused by the correction of the overlap. Finally, the aerosol backscattering coefficient was acquired by using this method and the data obtained via the Raman-Mie scattering Lidar of our lab. And the result was compared with that of Klett and Fernald. PMID:23387171

  1. Deep-UV surface-enhanced resonance Raman scattering of adenine on aluminum nanoparticle arrays.

    PubMed

    Jha, Shankar K; Ahmed, Zeeshan; Agio, Mario; Ekinci, Yasin; Löffler, Jörg F

    2012-02-01

    We report the ultrasensitive detection of adenine using deep-UV surface-enhanced resonance Raman scattering on aluminum nanostructures. Well-defined Al nanoparticle arrays fabricated over large areas using extreme-UV interference lithography exhibited sharp and tunable plasmon resonances in the UV and deep-UV wavelength ranges. Theoretical modeling based on the finite-difference time-domain method was used to understand the near-field and far-field optical properties of the nanoparticle arrays. Raman measurements were performed on adenine molecules coated uniformly on the Al nanoparticle arrays at a laser excitation wavelength of 257.2 nm. With this technique, less than 10 amol of label-free adenine molecules could be detected reproducibly in real time. Zeptomole (~30,000 molecules) detection sensitivity was readily achieved proving that deep-UV surface-enhanced resonance Raman scattering is an extremely sensitive tool for the detection of biomolecules.

  2. Fiber-optic apparatus and method for measurement of luminescence and raman scattering

    DOEpatents

    Myrick, Michael L.; Angel, Stanley M.

    1993-01-01

    A dual fiber forward scattering optrode for Raman spectroscopy with the remote ends of the fibers in opposed, spaced relationship to each other to form a analyte sampling space therebetween and the method of measuring Raman spectra utilizing same. One optical fiber is for sending an exciting signal to the remote sampling space and, at its remote end, has a collimating microlens and an optical filter for filtering out background emissions generated in the fiber. The other optical fiber is for collecting the Raman scattering signal at the remote sampling space and, at its remote end, has a collimating microlens and an optical filter to prevent the exciting signal from the exciting fiber from entering the collection fiber and to thereby prevent the generation of background emissions in the collecting fiber.

  3. Fiber-optic apparatus and method for measurement of luminescence and Raman scattering

    DOEpatents

    Myrick, M.L.; Angel, S.M.

    1993-03-16

    A dual fiber forward scattering optrode for Raman spectroscopy with the remote ends of the fibers in opposed, spaced relationship to each other to form a analyte sampling space therebetween and the method of measuring Raman spectra utilizing same are described. One optical fiber is for sending an exciting signal to the remote sampling space and, at its remote end, has a collimating microlens and an optical filter for filtering out background emissions generated in the fiber. The other optical fiber is for collecting the Raman scattering signal at the remote sampling space and, at its remote end, has a collimating microlens and an optical filter to prevent the exciting signal from the exciting fiber from entering the collection fiber and to thereby prevent the generation of background emissions in the collecting fiber.

  4. Raman scattering of linear chains of strongly coupled Ag nanoparticles on SWCNTs

    PubMed Central

    Valmalette, Jean-Christophe; Tan, Zhenquan; Abe, Hiroya; Ohara, Satoshi

    2014-01-01

    We compare the Raman scattering properties of hybrid nanostructures consisting of Ag nanoparticles (NPs) in disordered and aligned arrangements on single-walled carbon nanotubes (SWCNTs) as a result of chemical and photoreduction methods. In the latter case, the unique structure of the very small Ag NP (from 4 to 7 nm) chains generated an extremely large mode at 969 cm−1 that was assigned to the sulphate-silver interaction at the NP surface. Another strong mode was present at 1201 cm−1 and was assigned to an IR-active mode of sodium dodecyl sulphate (SDS); this mode was observed because the symmetry changes altered the selection rules. We demonstrate that both the UV photoreduction of silver and the presence of SWCNTs are necessary to produce this very strong Raman scattering. The Raman modes of the SWCNTs are also significantly modified by the presence of Ag NP chains along the nanotubes. PMID:24912409

  5. Stimulated resonance Raman scattering from single crystals of a thiophene/phenylene co-oligomer

    NASA Astrophysics Data System (ADS)

    Yanagi, Hisao; Yoshiki, Atsutoshi; Hotta, Shu; Kobayashi, Shunsuke

    2003-09-01

    We have investigated the stimulated resonance Raman scattering from single crystals of a thiophene/phenylene co-oligomer. The very narrow lines [full width at half maximum (FWHM)=11-20 cm-1] are observed in the same spectral regions where the spectrally narrowed emissions (FWHM≈300 cm-1) occur upon excitation with intense laser pulse. We related these modes to the stimulated resonance Raman scattering. Two lines of Raman shifts of 1466 and 1605 cm-1 are of molecular origin. Another line with an energy shift of ˜1260 cm-1 from excitation energy, on the other hand, implies the presence of the coherence of crystal origin. The associated split lines accompanying this mode are thought to constitute the longitudinal modes in the Fabry-Pérot cavity naturally formed in the crystals.

  6. Gold Nanoparticle Coated Carbon Nanotube Ring with Enhanced Raman Scattering and Photothermal Conversion Property for Theranostic Applications.

    PubMed

    Song, Jibin; Wang, Feng; Yang, Xiangyu; Ning, Bo; Harp, Mary G; Culp, Stephen H; Hu, Song; Huang, Peng; Nie, Liming; Chen, Jingyi; Chen, Xiaoyuan

    2016-06-01

    We report a new type of carbon nanotube ring (CNTR) coated with gold nanoparticles (CNTR@AuNPs) using CNTR as a template and surface attached redox-active polymer as a reducing agent. This nanostructure of CNTR bundle embedded in the gap of closely attached AuNPs can play multiple roles as a Raman probe to detect cancer cells and a photoacoustic (PA) contrast agent for imaging-guided cancer therapy. The CNTR@AuNP exhibits substantially higher Raman and optical signals than CNTR coated with a complete Au shell (CNTR@AuNS) and straight CNT@AuNP. The extinction intensity of CNTR@AuNP is about 120-fold higher than that of CNTR at 808 nm, and the surface enhanced Raman scattering (SERS) signal of CNTR@AuNP is about 110 times stronger than that of CNTR, presumably due to the combined effects of enhanced coupling between the embedded CNTR and the plasmon mode of the closely attached AuNPs, and the strong electromagnetic field in the cavity of the AuNP shell originated from the intercoupling of AuNPs. The greatly enhanced PA signal and photothermal conversion property of CNTR@AuNP were successfully employed for imaging and imaging-guided cancer therapy in two tumor xenograft models. Experimental observations were further supported by numerical simulations and perturbation theory analysis. PMID:27193381

  7. Excitons in one-phonon resonant Raman scattering: Fröhlich and interference effects

    NASA Astrophysics Data System (ADS)

    Cantarero, A.; Trallero-Giner, C.; Cardona, M.

    1989-12-01

    A theoretical model of resonant Raman scattering including excitons as intermediate states in the process is compared with recent experimental results in some III-V compound semiconductors where the Raman polarizability was obtained in absolute value for several scattering configurations. In particular, Fröhlich (F) interaction and its interference with the deformation potential (DP) one is analyzed in the E0+Δ0 critical point (CP) of GaAs at three different temperatures. Also the E0 and E0+Δ0 CP of GaP and E0+Δ0 of GaSb are analyzed. We show that the inclusion of impurity-induced forbidden LO-phonon Raman scattering is not necessary when excitonic effects are considered. The experimental data of GaAs corresponding to F interaction can be fitted by assuming a Fröhlich constant cF=0.14 eV Aṥ/2. Lifetime broadenings of 12 meV (10 K), 14 meV (100 K), and 28 meV (300 K) are deduced. The lifetime broadening of GaAs and GaSb at 100 K are taken from two-phonon Raman scattering spectra where the incoming and outgoing resonances are well defined. The general features in the comparison with the experiment is that the measured spectra corresponding to F interaction are well fitted; however, the theoretical interference is stronger than the measured one.

  8. BRIEF COMMUNICATIONS: Coherent anti-Stokes Raman scattering by excited ions in a laser plasma

    NASA Astrophysics Data System (ADS)

    Gladkov, S. M.; Zheltikov, Aleksei M.; Koroteev, Nikolai I.; Rychev, M. V.; Fedotov, Andrei B.

    1989-07-01

    The coherent anti-Stokes Raman scattering (CARS) method was used in observation of excited Al II, Al III, In II and N II in an optical breakdown plasma. The feasibility of CARS spectroscopy of multiply charged ions in a laser plasma was established.

  9. Enhanced Raman scattering from cesium suboxides on silver particles and the structure of S-1 photocathodes

    NASA Technical Reports Server (NTRS)

    Bates, C. W., Jr.

    1984-01-01

    An explanation is given for the results of recent enhanced Raman scattering studies of photomultiplier tubes with S-1 photocathode surfaces which indicated the presence of Cs11O3 but not Cs2O. The reason for the discrepancy between the currently accepted model of the S-1 and this recent result is discussed.

  10. System and method for linearly amplifying optical analog signals by backward Raman scattering

    DOEpatents

    Lin, Cheng-Heui

    1988-07-05

    A system for linearly amplifying an optical analog signal by backward stimulated Raman scattering comprises a laser source for generating a pump pulse; and an optic fiber having two opposed apertures, a first aperture for receiving the pump pulse and a second aperture for receiving the optical analog signal, wherein the optical analog signal is linearly amplified to an amplified optical analog signal.

  11. Semiconductor-enhanced Raman scattering for highly robust SERS sensing: the case of phosphate analysis.

    PubMed

    Ji, Wei; Song, Wei; Tanabe, Ichiro; Wang, Yue; Zhao, Bing; Ozaki, Yukihiro

    2015-05-01

    Quantitative analysis of phosphate anions was achieved by measurement of "turn-off" SERS based on the first-layer effect of a chemical mechanism. More importantly, our results demonstrate that it is possible, by means of semiconductor-enhanced Raman scattering, to enhance the SERS sensing performance including stability and reproducibility.

  12. Detection and differentiation of Salmonella serotypes using Surface Enhanced Raman Scattering (SERS) technique.

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Surface Enhanced Raman Scattering (SERS) can detect pathogens rapidly and accurately. The metal surface for the SERS spectroscopy was a silver nano-particle encapsulated biopolymer polyvinyl alcohol nano-colloid deposited on a stainless steel plate. Salmonella Typhimurium and Salmonella Enteritidis...

  13. Stable silver/biopolymer hybrid plasmonic nanostructures for high performance surface enhanced raman scattering (SERS)

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Silver/biopolymer nanoparticles were prepared by adding 100 mg silver nitrate to 2% polyvinyl alcohol solution and reduced the silver nitrate into silver ion using 2 % trisodium citrate for high performance Surface Enhanced Raman Scattering (SERS) substrates. Optical properties of nanoparticle were ...

  14. Intermolecular and low-frequency intramolecular Raman scattering study of racemic ibuprofen

    NASA Astrophysics Data System (ADS)

    Lazarević, J. J.; Uskoković-Marković, S.; Jelikić-Stankov, M.; Radonjić, M.; Tanasković, D.; Lazarević, N.; Popović, Z. V.

    We report the low-temperature Raman scattering study of racemic ibuprofen. Detailed analysis of the racemic ibuprofen crystal symmetry, related to the vibrational properties of the system, has been presented. The first principle calculations of a single ibuprofen molecule dynamical properties are compered with experimental data. Nineteen, out of 26 modes expected for the spectral region below 200 cm-1, have been observed.

  15. 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

  16. Development and applications of tunable, narrow band lasers and stimulated Raman scattering devices for atmospheric lidar

    NASA Technical Reports Server (NTRS)

    Wilkerson, Thomas D.

    1993-01-01

    The main thrust of the program was the study of stimulated Raman processes for application to atmospheric lidar measurements. This has involved the development of tunable lasers, the detailed study of stimulated Raman scattering, and the use of the Raman-shifted light for new measurements of molecular line strengths and line widths. The principal spectral region explored in this work was the visible and near-IR wavelengths between 500 nm and 1.5 microns. Recent alexandrite ring laser experiments are reported. The experiments involved diode injection-locking, Raman shifting, and frequency-doubling. The experiments succeeded in producing tunable light at 577 and 937 nm with line widths in the range 80-160 MHz.

  17. Influence of strong and weak hydrogen bonds in ices on stimulated Raman scattering.

    PubMed

    Li, Tianyu; Li, Fangfang; Li, Zhanlong; Sun, Chenglin; Tong, Junhong; Fang, Wenhui; Men, Zhiwei

    2016-03-15

    Stimulated Raman scattering (SRS) in liquid water and ice Ih using Nd:YAG laser is investigated. The spectrum of backward SRS (BSRS) in water is acquired. The spectrum shows an unexpected SRS peak at around 3453  cm(-1) besides the normal peak, which is similar to the spontaneous Raman spectrum of ice VII. The ice VII phase will be formed by laser-induced shock compression in liquid water. Simultaneously, unlike the spontaneous Raman spectrum, the pre-resonance SRS of ice Ih at around 3110 and 3210  cm(-1) is observed. The Raman peaks appeared in liquid water and ice Ih are attributed to the effect of strong and weak hydrogen bonds (H bonds), which should be ubiquitous in other ice phases.

  18. Tip-enhanced Raman scattering (TERS) from hemozoin crystals within a sectioned erythrocyte.

    PubMed

    Wood, Bayden R; Bailo, Elena; Khiavi, Mehdi Asghari; Tilley, Leann; Deed, Samantha; Deckert-Gaudig, Tanja; McNaughton, Don; Deckert, Volker

    2011-05-11

    Tip-enhanced Raman scattering (TERS) is a powerful technique to obtain molecular information on a nanometer scale, however, the technique has been limited to cell surfaces, viruses, and isolated molecules. Here we show that TERS can be used to probe hemozoin crystals at less than 20 nm spatial resolution in the digestive vacuole of a sectioned malaria parasite-infected cell. The TERS spectra clearly show characteristic bands of hemozoin that can be correlated to a precise position on the crystal by comparison with the corresponding atomic force microscopy (AFM) image. These are the first recorded AFM images of hemozoin crystals inside malaria-infected cells and clearly show the hemozoin crystals protruding from the embedding medium. TERS spectra recorded of these crystals show spectral features consistent with a five-coordinate high-spin ferric heme complex, which include the electron density marker band ν(4) at 1373 cm(-1) and other porphyrin skeletal and ring breathing modes at approximately 1636, 1557, 1412, 1314, 1123, and 1066 cm(-1). These results demonstrate the potential of the AFM/TERS technique to obtain nanoscale molecular information within a sectioned single cell. We foresee this approach paving the way to a new independent drug screening modality for detection of drugs binding to the hemozoin surface within the digestive vacuole of the malaria trophozoite.

  19. Detection of human brain tumor infiltration with quantitative stimulated Raman scattering microscopy.

    PubMed

    Ji, Minbiao; Lewis, Spencer; Camelo-Piragua, Sandra; Ramkissoon, Shakti H; Snuderl, Matija; Venneti, Sriram; Fisher-Hubbard, Amanda; Garrard, Mia; Fu, Dan; Wang, Anthony C; Heth, Jason A; Maher, Cormac O; Sanai, Nader; Johnson, Timothy D; Freudiger, Christian W; Sagher, Oren; Xie, Xiaoliang Sunney; Orringer, Daniel A

    2015-10-14

    Differentiating tumor from normal brain is a major barrier to achieving optimal outcome in brain tumor surgery. New imaging techniques for visualizing tumor margins during surgery are needed to improve surgical results. We recently demonstrated the ability of stimulated Raman scattering (SRS) microscopy, a nondestructive, label-free optical method, to reveal glioma infiltration in animal models. We show that SRS reveals human brain tumor infiltration in fresh, unprocessed surgical specimens from 22 neurosurgical patients. SRS detects tumor infiltration in near-perfect agreement with standard hematoxylin and eosin light microscopy (κ = 0.86). The unique chemical contrast specific to SRS microscopy enables tumor detection by revealing quantifiable alterations in tissue cellularity, axonal density, and protein/lipid ratio in tumor-infiltrated tissues. To ensure that SRS microscopic data can be easily used in brain tumor surgery, without the need for expert interpretation, we created a classifier based on cellularity, axonal density, and protein/lipid ratio in SRS images capable of detecting tumor infiltration with 97.5% sensitivity and 98.5% specificity. Quantitative SRS microscopy detects the spread of tumor cells, even in brain tissue surrounding a tumor that appears grossly normal. By accurately revealing tumor infiltration, quantitative SRS microscopy holds potential for improving the accuracy of brain tumor surgery.

  20. 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

    2014-01-01

    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. PMID:25045833