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Virtual Journal for Biomedical Optics

Virtual Journal for Biomedical Optics


  • Editor: Gregory W. Faris
  • Vol. 1, Iss. 5 — May. 5, 2006

Direct extraction of Raman line-shapes from congested CARS spectra

Erik M. Vartiainen, Hilde A. Rinia, Michiel Müller, and Mischa Bonn  »View Author Affiliations

Optics Express, Vol. 14, Issue 8, pp. 3622-3630 (2006)

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We show that Raman line-shapes can be extracted directly from congested coherent anti-Stokes Raman scattering (CARS) spectra, by using a numerical method to retrieve the phase-information hidden in measured CARS spectra. The proposed method utilizes the maximum entropy (ME) model to fit the CARS spectra and to further extract the imaginary part of the Raman susceptibility providing the Raman line-shape similar to the spontaneous Raman scattering spectrum. It circumvents the challenges arising with experimentally determining the real and imaginary parts of the susceptibility independently. Another important advantage of this method is that no a priori information regarding the vibrational resonances is required in the analysis. This permits, for the first time, the quantitative analysis of CARS spectra and microscopy images without any knowledge of e.g. sample composition or Raman response.

© 2006 Optical Society of America

OCIS Codes
(000.3860) General : Mathematical methods in physics
(300.6230) Spectroscopy : Spectroscopy, coherent anti-Stokes Raman scattering

ToC Category:

Original Manuscript: March 3, 2006
Revised Manuscript: March 30, 2006
Manuscript Accepted: April 1, 2006
Published: April 17, 2006

Virtual Issues
Vol. 1, Iss. 5 Virtual Journal for Biomedical Optics

Erik M. Vartiainen, Hilde A. Rinia, Michiel Müller, and Mischa Bonn, "Direct extraction of Raman line-shapes from congested CARS spectra," Opt. Express 14, 3622-3630 (2006)

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  1. G. R. Holtom, B. D. Thrall, B. Chin, and D. Colson, "Achieving molecular selectivity in imaging using multiphoton Raman spectroscopy techniques," Traffic 2, 781-788 (2001). [CrossRef] [PubMed]
  2. J. X. Cheng and X. S. Xie, "Coherent Anti-Stokes Raman Scattering Microscopy: Instrumentation, Theory, and Applications," J. Phys. Chem. B 108, 827-840 (2004). [CrossRef]
  3. A. Volkmer, "Vibrational imaging and microspectroscopies based on coherent anti-Stokes Raman scattering microscopy," J. Phys. D: Appl. Phys. 38, R59-R81 (2005). [CrossRef]
  4. G. J. Puppels, F. F. M. de Mul, C. Otto, J. Greve, M. Robert-Nicoud, D. J. Arndt-Jovin, and T. M. Jovin, "Studying single living cells and chromosomes by confocal Raman microspectroscopy," Nature 347, 301-303 (1990). [CrossRef] [PubMed]
  5. H. van Manen, Y. M. Kraan, D. Roos, and C. Otto, "Single-cell Raman and fluorescence microscopy reveal the association of lipid bodies with phagosomes in leukocytes," Proc. Natl. Acad. Sci. USA 102, 10159-10164 (2005). [CrossRef] [PubMed]
  6. M. Müller and J. M. Schins, "Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy," J. Phys. Chem. B 106, 3715-3723 (2002). [CrossRef]
  7. G. W. H. Wurpel, J. M. Schins, and M. Müller, "Chemical specificity in 3D imaging with multiplex CARS microscopy," Opt. Lett. 27, 1093-1095 (2002). [CrossRef]
  8. J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "Multiplex coherent anti-Stokes Raman scattering microspectroscopy and study of lipid vesicles," J. Phys. Chem. B 106, 8493-8498 (2002). [CrossRef]
  9. M. Müller, J. M. Schins, and G. W. H. Wurpel, "Shot-noise limited detection sensitivity in multiplex CARS microscopy," SPIE 5323, 195-204 (2004). [CrossRef]
  10. G. W. H. Wurpel, J. M. Schins, and M. Müller, "Direct measurement of chain order in single lipid mono- and bilayers with multiplex CARS," J. Phys. Chem. B 108, 3400-3403 (2004). [CrossRef]
  11. S. A. Akhmanov, A. F. Bunkin, S. G. Ivanov, and N. I. Koroteev, "Polarization active Raman spectroscopy and coherent Raman elipsometry," Sov. Phys. JETP 47, 667-678 (1978).
  12. J. Cheng, L. D. Book, and X. S. Xie, "Polarization coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 26, 1341-1343 (2001). [CrossRef]
  13. A. Volkmer, L. D. Book, and X. S. Xie, "Time-resolved coherent anti-Stokes Raman scattering microscopy: imaging based on Raman free induction decay," Appl. Phys. Lett. 80, 1505-1507 (2002). [CrossRef]
  14. D. Oron, N. Dudovich, D. Yelihn, and Y. Silberberg, "Quantum control of coherent anti-Stokes Raman processes," Phys. Rev. A 65, 4340814 (2002). [CrossRef]
  15. D. Oron, N. Dudovich, and Y. Silberberg, "Femtosecond Phase-and-Polarization Control for Background-Free Coherent Anti-Stokes Raman Spectroscopy," Phys. Rev. Lett. 90, 213902 (2003). [CrossRef] [PubMed]
  16. A. Volkmer, J. Cheng, and X. S. Xie, "Vibrational imaging with high sensitivity via epidetected coherent anti-Stokes Raman scattering microscopy," Phys. Rev. Lett. 87, 23901 (2001). [CrossRef]
  17. J. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "An epi-detected coherent anti-Stokes Raman scattering (E-CARS) microscope with high spectral resolution and high sensitivity," J. Phys. Chem. B 105, 1277-1280 (2001). [CrossRef]
  18. H. A. Rinia, M. Bonn, and M. Müller, "Quantitative multiplex CARS spectroscopy in congested spectral regions," J. Phys. Chem. B 110, 4472-4479 (2006). [CrossRef] [PubMed]
  19. F. Y. Yueh and E. J. Beiting, "Simultaneous N2, CO, and H2 multiplex CARS measurements in combustion environments using a single dye laser," Appl. Opt. 27, 3233-3243 (1988). [CrossRef] [PubMed]
  20. C. F. Kaminski and P. Ewart, "Multiplex H2 coherent anti-Stokes Raman scattering thermometry with a modeless laser," Appl. Opt. 36, 731-734 (1997). [CrossRef] [PubMed]
  21. C. Otto, A. Voroshilov, S. G. Kruglik, and J. Greve, "Vibrational bands of luminescent zinc(II)-octaethyl-porphyrin using a polarization-sensitive 'microscopic' multiplex CARS technique," J. Raman Spectrosc. 32, 495-501 (2001). [CrossRef]
  22. D. Oron, N. Dudovich, and Y. Silberberg, "Single-pulse phase-contrast nonlinear Raman spectroscopy," Phys. Rev. Lett. 89, 27300 (2002). [CrossRef]
  23. S. Lim, A. G. Caster, and S. R. Leone, "Single-pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy," Phys. Rev. A 72, 41803 (2005). [CrossRef]
  24. E. O. Potma, C. L. Evans and X. S. Xie, "Heterodyne coherent anti-Stokes Raman scattering (CARS) imaging," Opt. Lett. 31, 241-243 (2006). [CrossRef] [PubMed]
  25. D.L. Marks, C. Vinegoni, J.S. Bredfeldt and S.A. Boppart, "Interferometric differentiation between resonant coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85, 5787-5789 (2004). [CrossRef]
  26. E. M. Vartiainen, "Phase retrieval approach for coherent anti-Stokes Raman scattering spectrum analysis," J. Opt. Soc. Am. B 9, 1209-1214 (1992). [CrossRef]
  27. E. M. Vartiainen, K.-E. Peiponen, and T. Asakura, "Phase retrieval in optical spectroscopy: resolving optical constants from power spectra," Appl. Spectrosc. 50, 1283-1289 (1996). [CrossRef]
  28. R. A. MacPhail, H. L. Strauss, R. G. Snyder, and C. A. Elliger, "Carbon-hydrogen stretching modes and the structure of n-alkyl chains. 2. Long, all-trans chains," J. Phys. Chem. 88, 334-341 (1984). [CrossRef]
  29. R. Mendelsohn and D. J. Moore, "Vibrational spectroscopic studies of lipid domains in biomembranes and model systems," Chem. Phys. Lipids 96, 141-157 (1998). [CrossRef]
  30. K. T. Yue, C. L. Martin, D. Chen, P. Nelson, D. L. Sloan, and R. Callender, "Raman spectroscopy of oxidized and reduced nicotinamide adenine dinucleotides," Biochem 25, 4941-4947 (1986). [CrossRef]
  31. L. Rimai, T. Cole, J. L. Parsons, J. T. Hickmott, Jr., and E. B. Carew, "Studies of Raman spectra of water solutions of Adenosine tri-, di-, and monophosphate and some related compounds," Biophys. J. 9, 320-329 (1969). [CrossRef] [PubMed]
  32. R. H. Jenkins, R. Tuma, J. T. Juuti, D. H. Bamford and J. J. Thomas, "A novel Raman spectrophotometric method for quantitative measurement of nucleoside triphosphate hydrolysis," Biospectroscopy 5, 3-8 (1999). [CrossRef] [PubMed]

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