Journal of Raman Spectroscopy

Cover image for Vol. 43 Issue 5

Special Issue: Development and applications of nonlinear optical spectroscopy - 10th ECONOS / 30th ECW meeting in Enschede, The Netherlands

May 2012

Volume 43, Issue 5

Pages 593–688

Issue edited by: Herman Offerhaus, Peter Radi, Cees Otto

  1. Editorials

    1. Top of page
    2. Editorials
    3. Research Articles
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  2. Research Articles

    1. Top of page
    2. Editorials
    3. Research Articles
    1. Herman–Wallis corrections in dual-pump CARS intensities for combustion temperature and species (pages 595–598)

      Michele Marrocco, Gaetano Magnotti and Andrew D. Cutler

      Version of Record online: 20 MAR 2012 | DOI: 10.1002/jrs.3131

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      Dual-pump CARS spectra of nitrogen and oxygen are used to verify the effect of vibration-rotation coupling (quantified through the Herman–Wallis factor) on diagnostic predictions of temperature and mole fractions in flames. Beyond the known thermometric correction of about 0.5%, mole fractions are subject to variations of about 1% for nitrogen at stoichiometric conditions, whereas the sensitivity of oxygen to vibration-rotation coupling can reach 2.5%.

    2. On the sensitivity of rotational O2 CARS thermometry to the Herman–Wallis factor (pages 599–603)

      Alexis Bohlin, Emil Nordström, Per-Erik Bengtsson and Michele Marrocco

      Version of Record online: 17 APR 2012 | DOI: 10.1002/jrs.3147

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      Various literature values for the Herman–Wallis factor have been used as input data to the calculation of rotational O2 coherent anti-Stokes Raman scattering spectra. The sensitivity of evaluated temperatures to these Herman–Wallis factors has been examined and leads to differences not greater than 1% in the range from 300 to 2100 K. However, when neglecting this parameter, rotational N2 and O2 CARS thermometry could overestimate the temperature by about 1.5-2.0% at flame conditions.

    3. Validation of a rotational coherent anti-Stokes Raman scattering model for N2O at temperatures from 295 K to 796 K (pages 604–610)

      Alexis Bohlin, Alem Kindeya, Emil Nordström and Per-Erik Bengtsson

      Version of Record online: 12 APR 2012 | DOI: 10.1002/jrs.3148

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      Pure rotational coherent anti-Stokes Raman scattering spectra of N2O have been recorded in a series of temperature calibrated cell measurements in the region 295–796 K. A theoretical rotational coherent anti-Stokes Raman scattering code for N2O was implemented and temperature analysis was performed by fitting the modeled theoretical spectra to the experimental spectra. Excellent agreement between experimental and modeled spectra was obtained and the thermometric accuracy for the measurements was evaluated to better than 1%.

    4. Saturation and Stark broadening effects in dual-pump CARS of N2, O2, and H2 (pages 611–620)

      Gaetano Magnotti, Andrew D. Cutler, G. C. Herring, Sarah A. Tedder and Paul M. Danehy

      Version of Record online: 4 MAY 2012 | DOI: 10.1002/jrs.3133

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      We have investigated the effects of Stark broadening and stimulated Raman pumping on dual-pump coherent anti-Stokes Raman spectroscopy measurements of temperature, O2, N2, and H2 absolute mole fraction. Laser irradiance thresholds above which these effects become significant have been determined experimentally and compared with theoretical predictions.

    5. Vibration–rotation interaction in time-resolved coherent anti-Stokes Raman scattering for gas-phase thermometry (pages 621–626)

      Michele Marrocco

      Version of Record online: 2 MAR 2012 | DOI: 10.1002/jrs.3135

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      Femtosecond coherent anti-Stokes Raman scattering (CARS) excitation is here tested to understand the theoretical sensitivity of light homonuclear diatomics (namely H2, N2 and O2) to the vibration–rotation interaction measured by means of the Herman–Wallis (HW) factor. The results suggest the strong sensitivity of time-resolved H2 CARS (Figure). Heavier diatomics are less sensitive, but the choice of an appropriate HW factor can contribute to improve the confidence in CARS thermometry with ultrashort laser pulses.

    6. New structural and vibrational opportunities combining Hyper-Rayleigh/hyper-Raman and Raman scattering in isotropic materials (pages 627–636)

      Vincent Rodriguez

      Version of Record online: 12 APR 2012 | DOI: 10.1002/jrs.3132

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      Illustrations in the field of ionic liquids and oxide glasses of combined spontaneous hyper-Raman and Raman scattering studies are given, also taking advantage of hyper-Rayleigh scattering, which specifically provides a unique structural and quantitative classification of the scatterers in terms of their dipolar/octupolar character. In addition, new transverse optical–longitudinal optical features in hyper-Raman in the 90° scattering geometry are evidenced that selectively enlighten or cancel longitudinal optical modes.

    7. Maximum entropy and time-domain Kramers–Kronig phase retrieval approaches are functionally equivalent for CARS microspectroscopy (pages 637–643)

      Marcus T. Cicerone, Khaled A. Aamer, Young Jong Lee and Erik Vartiainen

      Version of Record online: 26 APR 2012 | DOI: 10.1002/jrs.3169

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      Two methods, time-domain Kramers Kronig (TDKK) and maximum entropy (MEM), are commonly used for recovering Raman spectra from spectrally broad coherent anti-Stokes Raman scattering (CARS) signals. Here we compare these methods with respect to their ability to faithfully and robustly recover Raman spectra from CARS spectra simulated to reproduce a range of scenarios expected for experimental data and their efficiency. We find that the TDKK and MEM approaches perform in functionally equivalent ways, having only minor differences between them.

    8. A wide-field arrangement for single-shot CARS imaging of living cells (pages 644–650)

      A. Silve, N. Dorval, T. Schmid, L.M. Mir and B. Attal-Tretout

      Version of Record online: 27 APR 2012 | DOI: 10.1002/jrs.4051

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      A new arrangement for wide-field CARS imaging using nanosecond dye lasers in a non-phase- matching illumination is presented. The chemical selectivity of the signal is demonstrated on polystyrene beads. The experimental arrangement has enabled the acquisition of images of living cells in suspension with a satisfactory signal-to-background ratio by using only a single pair of laser shots. Lack of damage on cells has been demonstrated in conditions leading to strong CARS signal generation.

    9. Rapid identification of heterogeneous mixture components with hyperspectral coherent anti-Stokes Raman scattering imaging (pages 651–655)

      Erik T. Garbacik, Jennifer L. Herek, Cees Otto and Herman L. Offerhaus

      Version of Record online: 3 MAY 2012 | DOI: 10.1002/jrs.4064

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      For the rapid analysis of complicated heterogeneous mixtures, we have developed a method to acquire and intuitively display hyperspectral coherent anti-Stokes Raman scattering images. Color-coding each frame of the hyperspectral data cube according to vibrational frequency results in a two-dimensional projection wherein each compound appears with a unique hue. We demonstrate the capabilities of this system by identifying seven crystalline amino acids in a mixture by direct visual analysis of the colored projection.

    10. Tip-enhanced broadband CARS spectroscopy and imaging using a photonic crystal fiber based broadband light source (pages 656–661)

      Kentaro Furusawa, Norihiko Hayazawa, Francesca Celine Catalan, Takayuki Okamoto and Satoshi Kawata

      Version of Record online: 4 APR 2012 | DOI: 10.1002/jrs.3151

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      We report tip-enhanced broadband coherent anti-Stokes Raman scattering spectroscopy and imaging based on a broadband light source using a photonic crystal fiber. Multiplexing from 900 cm–1 to 2200 cm–1 is achieved by optimizing the supercontinuum generation. By combining this system with a shear-force microscope, semiconducting carbon nanotubes are imaged with a spatial resolution of 60 nm. Our results show that tip-enhanced broadband coherent anti-Stokes Raman scattering image exhibits a positive contrast even though the enhancement effect has not been fully optimized.

    11. Coherent Raman spectroscopy with a fiber-format femtosecond oscillator (pages 662–667)

      Vikas Kumar, Michele Casella, Egle Molotokaite, Dario Polli, Giulio Cerullo and Marco Marangoni

      Version of Record online: 26 APR 2012 | DOI: 10.1002/jrs.3160

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      We report on the recent development of a new technological approach for coherent Raman spectroscopy/microscopy based on spectral compression of femtosecond pulses emitted by an amplified multiple-branch Er:fiber oscillator. Spectral compression is achieved by group-velocity mismatched second-harmonic generation in periodically poled nonlinear crystals, and it allows efficient synthesis of multiple synchronized narrow-bandwidth picosecond pulses with frequency difference continuously tunable from 1000 to 3500 cm−1. The system offers performances close to the current state of the art both for coherent anti-Stokes Raman scattering (CARS) and for stimulated Raman scattering (SRS), but with significant advantages in terms of compactness and versatility. In fact, several configurations can be easily implemented, including multiplex CARS, two-color imaging and nonresonant background suppression in CARS.

    12. Imaging cortical vasculature with stimulated Raman scattering and two-photon photothermal lensing microscopy (pages 668–674)

      Julian Moger, Natalie. L. Garrett, David Begley, Larisa Mihoreanu, Aikaterini Lalatsa, Maria Victoria Lozano, Mariarosa Mazza, Andreas Schatzlein and Ijeoma Uchegbu

      Version of Record online: 26 APR 2012 | DOI: 10.1002/jrs.3156

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      The ability to map microvascular morphology and hemodynamic parameters, such as blood volume, is desirable for many biomedical studies and will lead to a deeper understanding of the mechanisms of angiogenesis and vascular disease. We present a novel approach that combines stimulated Raman scattering and two-photon photothermal lensing to provide simultaneous visualisation of cortical microvasular morphology and surrounding cellular structures. Volumetric analysis allows a direct quantification of local haematocrit volume rather than relying upon average plasma volume-to-haematocrit ratios.

    13. CARS and SHG microscopy to follow collagen production in living human corneal fibroblasts and mesenchymal stem cells in fibrin hydrogel 3D cultures (pages 675–680)

      L. Mortati, C. Divieto and M. P. Sassi

      Version of Record online: 27 APR 2012 | DOI: 10.1002/jrs.3171

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      Coherent anti-Stokes Raman scattering microscopy is used in conjunction with second harmonic generation technique to follow collagen production by living cells in three-dimensional cultures. An account is given of the application of noninvasive, label-free multimodal coherent anti-Stokes Raman scattering and second harmonic generation microscopy in the monitoring of the early stages of stem cell differentiation within a three-dimensional scaffold in short-term and long-term experiments. The results provide further evidence of the efficacy of fibrin hydrogel as a scaffold autoinducing the differentiation stimulus.

    14. Label-free imaging of polymeric nanomedicines using coherent anti-stokes Raman scattering microscopy (pages 681–688)

      N. L. Garrett, A. Lalatsa, D. Begley, L. Mihoreanu, I. F. Uchegbu, A. G. Schätzlein and J. Moger

      Version of Record online: 26 APR 2012 | DOI: 10.1002/jrs.3170

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      Nanoparticulate drug delivery can greatly improve the efficacy of pharmaceuticals; however the mechanisms by which these nanoparticles interact with tissues are still unclear. Our ability to understand these mechanisms is hindered by the lack of traditional imaging modalities for directly visualising such small particles without external contrast agents or deleteriously invasive procedures. We present CARS microscopy as a novel tool for label-free detection of nanoparticulate drug carriers against a background of biological tissue and cells.