A time gating system has been constructed that is capable of recording high quality Raman spectra of highly fluorescing biological samples while operating below the photodamage threshold. Using a collinear gating geometry and careful attention to power conservation, we have achieved all-optical switching with a one picosecond gating time and 5% peak gating efficiency. The energy per pulse in this instrument is more than 3 orders of magnitude weaker than previous reports. Using this system we have performed proof-of-concept experiments on a sample composed of perylene dissolved in toluene, and the stem of a Jasminum multiflorum plant, the latter case being particularly important for the study of plants used in production of cellulosic biofuels. In both cases, a high SNR spectrum of the high-wavenumber region of the spectrum was recorded in the presence of an overwhelming fluorescence background.

© 2010 Optical Society of America

1. M. Gniadecka, P. A. Philipsen, S. Sigurdsson, S. Wessel, O. F. Nielsen, D. H. Christensen, J. Hercogova, K. Rossen, H. K. Thomsen, R. Gniadecki, L. K. Hansen, and H. C. Wulf, "Melanoma diagnosis by Raman spectroscopy and neural networks: Structure alterations in proteins and lipids in intact cancer tissue," J. Invest. Dermatol. 122, 443-449 (2004). [CrossRef] [PubMed]
2. A. Nijssen, T. C. B. Schut, F. Heule, P. J. Caspers, D. P. Hayes, M. H. A. Neumann, and G. J. Puppels, "Discriminating basal cell carcinoma from its surrounding tissue by Raman spectroscopy," J. Invest. Dermatol. 119, 64-69 (2002). [CrossRef] [PubMed]
3. C. A. Lieber, S. K. Majumder, D. Billheimer, D. L. Ellis, and A. Mahadevan-Jansen, "Raman microspectroscopy for skin cancer detection in vitro," J. Biomed. Opt. 13, 024013 (2008). [CrossRef] [PubMed]
4. K. Chen, Y. Qin, F. Zheng, M. Sun, and D. Shi, "Diagnosis of colorectal cancer using Raman spectroscopy of laser-trapped single living epithelial cells," Opt. Lett. 31, 2015-2017 (2006). [CrossRef] [PubMed]
5. J. W. Chan, D. S. Taylor, S. M. Lane, T. Zwerdling, J. Tuscano, and T. Huser, "Nondestructive identification of individual leukemia cells by laser trapping Raman spectroscopy," Anal. Chem. 80, 2180-2187 (2008). [CrossRef] [PubMed]
6. Q. Y. Zhu, R. G. Quivey, and A. J. Berger, "Measurement of bacterial concentration fractions in polymicrobial mixtures by Raman microspectroscopy," J. Biomed. Opt. 9, 1182-1186 (2004). [CrossRef] [PubMed]
7. P. Rösch, M. Harz, M. Schmitt, K.-D. Peschke, O. Ronneberger, H. Burkhardt, H.-W. Motzkus, M. Lankers, S. Hofer, H. Thiele, and J. Pöpp, "Chemotaxonomic identification of single bacteria by micro-Raman spectroscopy: application to clean-room-relevant biological contaminations," Appl. Environ. Microbiol. 71, 1626-1637 (2005). [CrossRef]
8. T. J. Moritz, D. S. Taylor, C. R. Polage, D. Krol, S. M. Lane, and J. W. Chan, "Raman spectroscopic signatures of the metabolic states of escherichia coli cells and their dependence on antibiotics treatment," Biophys. J. 98, 742a (2010). [CrossRef]
9. K. A. Dehring, N. J. Crane, A. R. Smukler, J. B. McHugh, B. J. Roessler, and M. D. Morris, "Identifying chemical changes in subchondral bone taken from murine knee joints using Raman spectroscopy," Appl. Spectrosc. 60, 1134-1141 (2006). [CrossRef] [PubMed]
10. D. Qi, and A. J. Berger, "Chemical concentration measurement in blood serum and urine samples using liquidcore optical fiber Raman spectroscopy," Appl. Spectrosc. 46, 1726-1734 (2007).
11. A. P. Shreve, N. J. Cherepy, and R. A. Mathies, "Effective rejection of fluorescence interference in raman spectroscopy using a shifted excitation difference technique," Appl. Spectrosc. 46, 707-711 (1992). [CrossRef]
12. C. A. Lieber, and A. Mahadevan-Jansen, "Automated method for subtraction of fluorescence from biological Raman spectra," Appl. Spectrosc. 57, 1363-1367 (2003). [CrossRef] [PubMed]
13. B. D. Beier, and A. J. Berger, "Method for automated background subtraction from raman spectra containing known contaminants," Analyst (Lond.) 134, 1198-1202 (2009). [CrossRef] [PubMed]
14. A. C. De Luca, M. Mazilu, A. Riches, C. S. Herrington, and K. Dholakia, "Online fluorescence suppression in modulated raman spectroscopy," Anal. Chem. 82, 738-745 (2010). [CrossRef]
15. P. Matousek, M. Towrie, A. Stanley, and A. W. Parker, "Efficient rejection of fluorescence from Raman spectra using picosecond Kerr gating," Appl. Spectrosc. 53, 1485-1489 (1999). [CrossRef]
16. P. Matousek, M. Towrie, C. Ma, W. M. Kwok, D. Phillips, W. T. Toner, and A. W. Parker, "Fluorescence suppression in resonance Raman spectroscopy using a high-performance picosecond Kerr gate," J. Raman Spectrosc. 32, 983-988 (2001). [CrossRef]
17. J. Dyer, W. J. Blau, C. G. Coates, C. M. Creely, J. D. Gavey, M. W. George, D. C. Grills, S. Hudson, J. M. Kelly, P. Matousek, J. J. McGarvey, J. McMaster, A. W. Parker, M. Towrie, and J. A. Weinstein, "The photophysics of fac-[Re(CO)3(dppz)(py)]+ in CH3CN: a comparative picosecond flash photolysis, transient infrared, transient resonance Raman and density functional theoretical study," Photochem. Photobiol. Sci. 2, 542-554 (2003). [CrossRef]
18. M. D. Morris, P. Matousek, M. Towrie, A. W. Parker, A. E. Goodship, and E. R. C. Draper, "Kerr-gated time resolved Raman spectroscopy of equine cortical bone tissue," J. Biomed. Opt. 10, 014014 (2005). [CrossRef]
19. R. Baker, P. Matousek, K. L. Ronayne, A. W. Parker, K. Rogers, and N. Stone, "Depth profiling of calcifications in breast tissue using picosecond Kerr-gated Raman spectroscopy," Analyst (Lond.) 132, 48-53 (2007). [CrossRef]
20. V. V. Yakovlev, "Time-gated confocal Raman microscopy," Spectroscopy 22, 41-45 (2007).
21. P. Matousek, "Deep non-invasive Raman spectroscopy of living tissue and powders," Chem. Soc. Rev. 36, ••• (2007). [CrossRef] [PubMed]
22. F. H. Loesel, J. P. Fischer, M. H. Götz, C. Horvath, T. Juhasz, F. Noack, N. Suhm, and J. F. Bille, "Non-thermal ablation of neural tissue with femtosecond laser pulses," Appl. Phys. B 66, 121-128 (1998). [CrossRef]
23. N. Gierlinger, and M. Schwanninger, "Chemical imaging of poplar wood cell walls by confocal Raman microscopy," Plant Physiol. 140, 1246-1254 (2006). [CrossRef] [PubMed]
24. M. Schmidt, A. M. Schwartzberg, A. Carroll, A. Chaibang, P. D. Adams, and P. J. Schuck, "Raman imaging of cell wall polymers in Aradopsis thaliana," Biochem. Biophys. Res. Commun. 395, 521-523 (2010). [CrossRef]
25. R. L. Sutherland, D. G. McLean, and S. Kirkpatrick, Handbook of Nonlinear Optics (Marcel Dekker, New York, NY, 2003). [CrossRef]
26. R. A. Ganeev, A. I. Ryasnyanskii, and H. Kuroda, "Nonlinear optical characteristics of carbon disulfide," Opt. Spectrosc. 100, 108-118 (2006). [CrossRef]
27. A. G. Vitukhnovsky, M. I. Sluch, J. G. Warren, and M. C. Petty, "The fluorescence of perylene-doped langmuir-blodgett films," Chem. Phys. Lett. 173, 425-429 (1990). [CrossRef]
28. J. K. Wilmshurst, and H. J. Bernstein, "The infrared and Raman spectra of toluene, toleuene-α-d3, m-xylene, and m-xylene- α α’-d 1/6," Can. J. Chem. 35, 911-925 (1957). [CrossRef]
29. E. M. Rubin, "Genomics of cellulosic biofuels," Nature 454, 841-845 (2008). [CrossRef] [PubMed]
30. Z. Li, L.-Q. Chu, J. V. Sweedler, and P. W. Bohn, "Spatial correlation of confocal Raman scattering and secondary ion mass spectrometric molecular images of lignocellulosic materials," Anal. Chem. 82, 2608-2611 (2010). [CrossRef] [PubMed]
31. J. M. Yarbrough, M. E. Himmel, and S.-Y. Ding, "Plant cell wall characterization using scanning probe microscopy techniques," Biotechnol. Biofuels 2, 17 (2009). [CrossRef] [PubMed]
32. A. Castellan, and R. S. Davidson, ""Steady-state and dynamic fluorescence emission from abies wood," J Photochem. Photobiol. A 78, 275-279 (1994). [CrossRef]
33. U. P. Agarwal, and S. A. Ralph, "FT-Raman spectroscopy of wood: identifying contributions of lignin and carbohydrate polymers in the spectrum of black spruce (Picea mariana)," Appl. Spectrosc. 51, 1648-1655 (1997). [CrossRef]

Anal. Chem.

• J. W. Chan, D. S. Taylor, S. M. Lane, T. Zwerdling, J. Tuscano, and T. Huser, "Nondestructive identification of individual leukemia cells by laser trapping Raman spectroscopy," Anal. Chem. 80, 2180-2187 (2008). [CrossRef] [PubMed]
• A. C. De Luca, M. Mazilu, A. Riches, C. S. Herrington, and K. Dholakia, "Online fluorescence suppression in modulated raman spectroscopy," Anal. Chem. 82, 738-745 (2010). [CrossRef]
• Z. Li, L.-Q. Chu, J. V. Sweedler, and P. W. Bohn, "Spatial correlation of confocal Raman scattering and secondary ion mass spectrometric molecular images of lignocellulosic materials," Anal. Chem. 82, 2608-2611 (2010). [CrossRef] [PubMed]

Analyst (Lond.)

• B. D. Beier, and A. J. Berger, "Method for automated background subtraction from raman spectra containing known contaminants," Analyst (Lond.) 134, 1198-1202 (2009). [CrossRef] [PubMed]
• R. Baker, P. Matousek, K. L. Ronayne, A. W. Parker, K. Rogers, and N. Stone, "Depth profiling of calcifications in breast tissue using picosecond Kerr-gated Raman spectroscopy," Analyst (Lond.) 132, 48-53 (2007). [CrossRef]

Appl. Environ. Microbiol.

• P. Rösch, M. Harz, M. Schmitt, K.-D. Peschke, O. Ronneberger, H. Burkhardt, H.-W. Motzkus, M. Lankers, S. Hofer, H. Thiele, and J. Pöpp, "Chemotaxonomic identification of single bacteria by micro-Raman spectroscopy: application to clean-room-relevant biological contaminations," Appl. Environ. Microbiol. 71, 1626-1637 (2005). [CrossRef]

Appl. Phys. B

• F. H. Loesel, J. P. Fischer, M. H. Götz, C. Horvath, T. Juhasz, F. Noack, N. Suhm, and J. F. Bille, "Non-thermal ablation of neural tissue with femtosecond laser pulses," Appl. Phys. B 66, 121-128 (1998). [CrossRef]

Appl. Spectrosc.

• U. P. Agarwal, and S. A. Ralph, "FT-Raman spectroscopy of wood: identifying contributions of lignin and carbohydrate polymers in the spectrum of black spruce (Picea mariana)," Appl. Spectrosc. 51, 1648-1655 (1997). [CrossRef]
• P. Matousek, M. Towrie, A. Stanley, and A. W. Parker, "Efficient rejection of fluorescence from Raman spectra using picosecond Kerr gating," Appl. Spectrosc. 53, 1485-1489 (1999). [CrossRef]
• K. A. Dehring, N. J. Crane, A. R. Smukler, J. B. McHugh, B. J. Roessler, and M. D. Morris, "Identifying chemical changes in subchondral bone taken from murine knee joints using Raman spectroscopy," Appl. Spectrosc. 60, 1134-1141 (2006). [CrossRef] [PubMed]
• D. Qi, and A. J. Berger, "Chemical concentration measurement in blood serum and urine samples using liquidcore optical fiber Raman spectroscopy," Appl. Spectrosc. 46, 1726-1734 (2007).
• A. P. Shreve, N. J. Cherepy, and R. A. Mathies, "Effective rejection of fluorescence interference in raman spectroscopy using a shifted excitation difference technique," Appl. Spectrosc. 46, 707-711 (1992). [CrossRef]
• C. A. Lieber, and A. Mahadevan-Jansen, "Automated method for subtraction of fluorescence from biological Raman spectra," Appl. Spectrosc. 57, 1363-1367 (2003). [CrossRef] [PubMed]

Biochem. Biophys. Res. Commun.

• M. Schmidt, A. M. Schwartzberg, A. Carroll, A. Chaibang, P. D. Adams, and P. J. Schuck, "Raman imaging of cell wall polymers in Aradopsis thaliana," Biochem. Biophys. Res. Commun. 395, 521-523 (2010). [CrossRef]

Biophys. J.

• T. J. Moritz, D. S. Taylor, C. R. Polage, D. Krol, S. M. Lane, and J. W. Chan, "Raman spectroscopic signatures of the metabolic states of escherichia coli cells and their dependence on antibiotics treatment," Biophys. J. 98, 742a (2010). [CrossRef]

Biotechnol. Biofuels

• J. M. Yarbrough, M. E. Himmel, and S.-Y. Ding, "Plant cell wall characterization using scanning probe microscopy techniques," Biotechnol. Biofuels 2, 17 (2009). [CrossRef] [PubMed]

Can. J. Chem.

• J. K. Wilmshurst, and H. J. Bernstein, "The infrared and Raman spectra of toluene, toleuene-α-d3, m-xylene, and m-xylene- α α’-d 1/6," Can. J. Chem. 35, 911-925 (1957). [CrossRef]

Chem. Phys. Lett.

• A. G. Vitukhnovsky, M. I. Sluch, J. G. Warren, and M. C. Petty, "The fluorescence of perylene-doped langmuir-blodgett films," Chem. Phys. Lett. 173, 425-429 (1990). [CrossRef]

Chem. Soc. Rev.

• P. Matousek, "Deep non-invasive Raman spectroscopy of living tissue and powders," Chem. Soc. Rev. 36, ••• (2007). [CrossRef] [PubMed]

J Photochem. Photobiol. A

• A. Castellan, and R. S. Davidson, ""Steady-state and dynamic fluorescence emission from abies wood," J Photochem. Photobiol. A 78, 275-279 (1994). [CrossRef]

J. Biomed. Opt.

• M. D. Morris, P. Matousek, M. Towrie, A. W. Parker, A. E. Goodship, and E. R. C. Draper, "Kerr-gated time resolved Raman spectroscopy of equine cortical bone tissue," J. Biomed. Opt. 10, 014014 (2005). [CrossRef]
• Q. Y. Zhu, R. G. Quivey, and A. J. Berger, "Measurement of bacterial concentration fractions in polymicrobial mixtures by Raman microspectroscopy," J. Biomed. Opt. 9, 1182-1186 (2004). [CrossRef] [PubMed]
• C. A. Lieber, S. K. Majumder, D. Billheimer, D. L. Ellis, and A. Mahadevan-Jansen, "Raman microspectroscopy for skin cancer detection in vitro," J. Biomed. Opt. 13, 024013 (2008). [CrossRef] [PubMed]

J. Invest. Dermatol.

• M. Gniadecka, P. A. Philipsen, S. Sigurdsson, S. Wessel, O. F. Nielsen, D. H. Christensen, J. Hercogova, K. Rossen, H. K. Thomsen, R. Gniadecki, L. K. Hansen, and H. C. Wulf, "Melanoma diagnosis by Raman spectroscopy and neural networks: Structure alterations in proteins and lipids in intact cancer tissue," J. Invest. Dermatol. 122, 443-449 (2004). [CrossRef] [PubMed]
• A. Nijssen, T. C. B. Schut, F. Heule, P. J. Caspers, D. P. Hayes, M. H. A. Neumann, and G. J. Puppels, "Discriminating basal cell carcinoma from its surrounding tissue by Raman spectroscopy," J. Invest. Dermatol. 119, 64-69 (2002). [CrossRef] [PubMed]

J. Raman Spectrosc.

• P. Matousek, M. Towrie, C. Ma, W. M. Kwok, D. Phillips, W. T. Toner, and A. W. Parker, "Fluorescence suppression in resonance Raman spectroscopy using a high-performance picosecond Kerr gate," J. Raman Spectrosc. 32, 983-988 (2001). [CrossRef]

Nature

• E. M. Rubin, "Genomics of cellulosic biofuels," Nature 454, 841-845 (2008). [CrossRef] [PubMed]

Opt. Lett.

• K. Chen, Y. Qin, F. Zheng, M. Sun, and D. Shi, "Diagnosis of colorectal cancer using Raman spectroscopy of laser-trapped single living epithelial cells," Opt. Lett. 31, 2015-2017 (2006). [CrossRef] [PubMed]

Opt. Spectrosc.

• R. A. Ganeev, A. I. Ryasnyanskii, and H. Kuroda, "Nonlinear optical characteristics of carbon disulfide," Opt. Spectrosc. 100, 108-118 (2006). [CrossRef]

Photochem. Photobiol. Sci.

• J. Dyer, W. J. Blau, C. G. Coates, C. M. Creely, J. D. Gavey, M. W. George, D. C. Grills, S. Hudson, J. M. Kelly, P. Matousek, J. J. McGarvey, J. McMaster, A. W. Parker, M. Towrie, and J. A. Weinstein, "The photophysics of fac-[Re(CO)3(dppz)(py)]+ in CH3CN: a comparative picosecond flash photolysis, transient infrared, transient resonance Raman and density functional theoretical study," Photochem. Photobiol. Sci. 2, 542-554 (2003). [CrossRef]

Plant Physiol.

• N. Gierlinger, and M. Schwanninger, "Chemical imaging of poplar wood cell walls by confocal Raman microscopy," Plant Physiol. 140, 1246-1254 (2006). [CrossRef] [PubMed]

Spectroscopy

• V. V. Yakovlev, "Time-gated confocal Raman microscopy," Spectroscopy 22, 41-45 (2007).

Other

• R. L. Sutherland, D. G. McLean, and S. Kirkpatrick, Handbook of Nonlinear Optics (Marcel Dekker, New York, NY, 2003). [CrossRef]

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