Abstract

We have used resonance Raman scattering as a novel noninvasive optical technology to measure carotenoid antioxidants in living human tissues of healthy volunteers. By use of blue-green laser excitation, clearly distinguishable carotenoid Raman spectra superimposed on a fluorescence background are obtained. The Raman spectra are obtained within less than a minute, and the required laser light exposure levels are well within safety standards. Our technique can be used for rapid screening of carotenoid levels in large populations and may have applications for assessing antioxidant status and the risk for diseases related to oxidative stress.

© 2001 Optical Society of America

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  1. T. W. M. Boileau, A. C. Moore, and J. W. Erdman, in Antioxidant Status, Diet, Nutrition, and Health, A. M. Papas, ed. (CRC Press, Boca Raton, Fla., 1999), p. 144.
  2. T. R. Hata, T. A. Scholz, I. V. Ermakov, R. W. McClane, F. Khachik, W. Gellermann, and L. K. Pershing, J. Invest. Dermat. 115, 441 (2000).
    [CrossRef]
  3. F. Böhm, J. H. Tinkler, and T. G. Truscott, Nature Med. 1, 98 (1995).
    [CrossRef]
  4. C. S. Foote and R. W. Denny, J. Am. Chem. Soc. 90, 6233 (1968).
    [CrossRef]
  5. A. Farmillo and F. Wilkinson, Photochem. Photobiol. 18, 447 (1973).
    [CrossRef]
  6. P. F. Conn, W. Schalch, and T. G. Truscott, J. Photochem. Photobiol. B 11, 41 (1991).
    [CrossRef] [PubMed]
  7. L. C. Chen, L. Sly, C. S. Jones, R. De Tarone, and L. M. Luca, Carcinogenesis 14, 713 (1993).
    [CrossRef] [PubMed]
  8. H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
    [CrossRef] [PubMed]
  9. I. V. Ermakov, R. W. McClane, W. Gellermann, and P. S. Bernstein, Opt. Lett. 26, 202 (2001).
    [CrossRef]
  10. A. P. Shreve, J. K. Trautman, T. G. Owens, and A. C. Albrecht, Chem. Phys. Lett. 178, 89 (1991).
  11. Y. Koyama, I. Takatsuka, M. Nakata, and M. Tasumi, J. Raman Spectrosc. 19, 37 (1988).
    [CrossRef]
  12. F. Inagaki, M. Tasumi, and T. Miyazawa, J. Mol. Spectrosc. 50, 286 (1974).
    [CrossRef]
  13. American National Standards Institute, “American national standard for safe use of lasers,” (Laser Institute of America, Orlando, Fla., 2000).
  14. D. J. Leffell, M. L. Stetz, L. M. Milstone, and L. I. Deckelbaum, Arch. Dermatol. 124, 1514 (1988).
    [CrossRef] [PubMed]

2001

2000

T. R. Hata, T. A. Scholz, I. V. Ermakov, R. W. McClane, F. Khachik, W. Gellermann, and L. K. Pershing, J. Invest. Dermat. 115, 441 (2000).
[CrossRef]

1999

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

1995

F. Böhm, J. H. Tinkler, and T. G. Truscott, Nature Med. 1, 98 (1995).
[CrossRef]

1993

L. C. Chen, L. Sly, C. S. Jones, R. De Tarone, and L. M. Luca, Carcinogenesis 14, 713 (1993).
[CrossRef] [PubMed]

1991

P. F. Conn, W. Schalch, and T. G. Truscott, J. Photochem. Photobiol. B 11, 41 (1991).
[CrossRef] [PubMed]

A. P. Shreve, J. K. Trautman, T. G. Owens, and A. C. Albrecht, Chem. Phys. Lett. 178, 89 (1991).

1988

Y. Koyama, I. Takatsuka, M. Nakata, and M. Tasumi, J. Raman Spectrosc. 19, 37 (1988).
[CrossRef]

D. J. Leffell, M. L. Stetz, L. M. Milstone, and L. I. Deckelbaum, Arch. Dermatol. 124, 1514 (1988).
[CrossRef] [PubMed]

1974

F. Inagaki, M. Tasumi, and T. Miyazawa, J. Mol. Spectrosc. 50, 286 (1974).
[CrossRef]

1973

A. Farmillo and F. Wilkinson, Photochem. Photobiol. 18, 447 (1973).
[CrossRef]

1968

C. S. Foote and R. W. Denny, J. Am. Chem. Soc. 90, 6233 (1968).
[CrossRef]

Alberts, D.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Albrecht, A. C.

A. P. Shreve, J. K. Trautman, T. G. Owens, and A. C. Albrecht, Chem. Phys. Lett. 178, 89 (1991).

Bernstein, P. S.

Böhm, F.

F. Böhm, J. H. Tinkler, and T. G. Truscott, Nature Med. 1, 98 (1995).
[CrossRef]

Boileau, T. W. M.

T. W. M. Boileau, A. C. Moore, and J. W. Erdman, in Antioxidant Status, Diet, Nutrition, and Health, A. M. Papas, ed. (CRC Press, Boca Raton, Fla., 1999), p. 144.

Chen, L. C.

L. C. Chen, L. Sly, C. S. Jones, R. De Tarone, and L. M. Luca, Carcinogenesis 14, 713 (1993).
[CrossRef] [PubMed]

Conn, P. F.

P. F. Conn, W. Schalch, and T. G. Truscott, J. Photochem. Photobiol. B 11, 41 (1991).
[CrossRef] [PubMed]

De Tarone, R.

L. C. Chen, L. Sly, C. S. Jones, R. De Tarone, and L. M. Luca, Carcinogenesis 14, 713 (1993).
[CrossRef] [PubMed]

Deckelbaum, L. I.

D. J. Leffell, M. L. Stetz, L. M. Milstone, and L. I. Deckelbaum, Arch. Dermatol. 124, 1514 (1988).
[CrossRef] [PubMed]

Denny, R. W.

C. S. Foote and R. W. Denny, J. Am. Chem. Soc. 90, 6233 (1968).
[CrossRef]

Erdman, J. W.

T. W. M. Boileau, A. C. Moore, and J. W. Erdman, in Antioxidant Status, Diet, Nutrition, and Health, A. M. Papas, ed. (CRC Press, Boca Raton, Fla., 1999), p. 144.

Ermakov, I. V.

I. V. Ermakov, R. W. McClane, W. Gellermann, and P. S. Bernstein, Opt. Lett. 26, 202 (2001).
[CrossRef]

T. R. Hata, T. A. Scholz, I. V. Ermakov, R. W. McClane, F. Khachik, W. Gellermann, and L. K. Pershing, J. Invest. Dermat. 115, 441 (2000).
[CrossRef]

Farmillo, A.

A. Farmillo and F. Wilkinson, Photochem. Photobiol. 18, 447 (1973).
[CrossRef]

Foote, C. S.

C. S. Foote and R. W. Denny, J. Am. Chem. Soc. 90, 6233 (1968).
[CrossRef]

Friedman, S.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Garewal, H. S.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Gellermann, W.

I. V. Ermakov, R. W. McClane, W. Gellermann, and P. S. Bernstein, Opt. Lett. 26, 202 (2001).
[CrossRef]

T. R. Hata, T. A. Scholz, I. V. Ermakov, R. W. McClane, F. Khachik, W. Gellermann, and L. K. Pershing, J. Invest. Dermat. 115, 441 (2000).
[CrossRef]

Graver, E.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Hata, T. R.

T. R. Hata, T. A. Scholz, I. V. Ermakov, R. W. McClane, F. Khachik, W. Gellermann, and L. K. Pershing, J. Invest. Dermat. 115, 441 (2000).
[CrossRef]

Inagaki, F.

F. Inagaki, M. Tasumi, and T. Miyazawa, J. Mol. Spectrosc. 50, 286 (1974).
[CrossRef]

Jones, C. S.

L. C. Chen, L. Sly, C. S. Jones, R. De Tarone, and L. M. Luca, Carcinogenesis 14, 713 (1993).
[CrossRef] [PubMed]

Katz, R.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Khachik, F.

T. R. Hata, T. A. Scholz, I. V. Ermakov, R. W. McClane, F. Khachik, W. Gellermann, and L. K. Pershing, J. Invest. Dermat. 115, 441 (2000).
[CrossRef]

Kiersch, T.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Koyama, Y.

Y. Koyama, I. Takatsuka, M. Nakata, and M. Tasumi, J. Raman Spectrosc. 19, 37 (1988).
[CrossRef]

Leffell, D. J.

D. J. Leffell, M. L. Stetz, L. M. Milstone, and L. I. Deckelbaum, Arch. Dermatol. 124, 1514 (1988).
[CrossRef] [PubMed]

Luca, L. M.

L. C. Chen, L. Sly, C. S. Jones, R. De Tarone, and L. M. Luca, Carcinogenesis 14, 713 (1993).
[CrossRef] [PubMed]

Mayne, S.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

McClane, R. W.

I. V. Ermakov, R. W. McClane, W. Gellermann, and P. S. Bernstein, Opt. Lett. 26, 202 (2001).
[CrossRef]

T. R. Hata, T. A. Scholz, I. V. Ermakov, R. W. McClane, F. Khachik, W. Gellermann, and L. K. Pershing, J. Invest. Dermat. 115, 441 (2000).
[CrossRef]

Meyskens, F.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Milstone, L. M.

D. J. Leffell, M. L. Stetz, L. M. Milstone, and L. I. Deckelbaum, Arch. Dermatol. 124, 1514 (1988).
[CrossRef] [PubMed]

Miyazawa, T.

F. Inagaki, M. Tasumi, and T. Miyazawa, J. Mol. Spectrosc. 50, 286 (1974).
[CrossRef]

Moore, A. C.

T. W. M. Boileau, A. C. Moore, and J. W. Erdman, in Antioxidant Status, Diet, Nutrition, and Health, A. M. Papas, ed. (CRC Press, Boca Raton, Fla., 1999), p. 144.

Morse, D.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Nakata, M.

Y. Koyama, I. Takatsuka, M. Nakata, and M. Tasumi, J. Raman Spectrosc. 19, 37 (1988).
[CrossRef]

Owens, T. G.

A. P. Shreve, J. K. Trautman, T. G. Owens, and A. C. Albrecht, Chem. Phys. Lett. 178, 89 (1991).

Pendrys, D.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Peng, Y.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Pershing, L. K.

T. R. Hata, T. A. Scholz, I. V. Ermakov, R. W. McClane, F. Khachik, W. Gellermann, and L. K. Pershing, J. Invest. Dermat. 115, 441 (2000).
[CrossRef]

Pitcock, J.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Schalch, W.

P. F. Conn, W. Schalch, and T. G. Truscott, J. Photochem. Photobiol. B 11, 41 (1991).
[CrossRef] [PubMed]

Scholz, T. A.

T. R. Hata, T. A. Scholz, I. V. Ermakov, R. W. McClane, F. Khachik, W. Gellermann, and L. K. Pershing, J. Invest. Dermat. 115, 441 (2000).
[CrossRef]

Shreve, A. P.

A. P. Shreve, J. K. Trautman, T. G. Owens, and A. C. Albrecht, Chem. Phys. Lett. 178, 89 (1991).

Sly, L.

L. C. Chen, L. Sly, C. S. Jones, R. De Tarone, and L. M. Luca, Carcinogenesis 14, 713 (1993).
[CrossRef] [PubMed]

Stetz, M. L.

D. J. Leffell, M. L. Stetz, L. M. Milstone, and L. I. Deckelbaum, Arch. Dermatol. 124, 1514 (1988).
[CrossRef] [PubMed]

Takatsuka, I.

Y. Koyama, I. Takatsuka, M. Nakata, and M. Tasumi, J. Raman Spectrosc. 19, 37 (1988).
[CrossRef]

Tasumi, M.

Y. Koyama, I. Takatsuka, M. Nakata, and M. Tasumi, J. Raman Spectrosc. 19, 37 (1988).
[CrossRef]

F. Inagaki, M. Tasumi, and T. Miyazawa, J. Mol. Spectrosc. 50, 286 (1974).
[CrossRef]

Tinkler, J. H.

F. Böhm, J. H. Tinkler, and T. G. Truscott, Nature Med. 1, 98 (1995).
[CrossRef]

Trautman, J. K.

A. P. Shreve, J. K. Trautman, T. G. Owens, and A. C. Albrecht, Chem. Phys. Lett. 178, 89 (1991).

Truscott, T. G.

F. Böhm, J. H. Tinkler, and T. G. Truscott, Nature Med. 1, 98 (1995).
[CrossRef]

P. F. Conn, W. Schalch, and T. G. Truscott, J. Photochem. Photobiol. B 11, 41 (1991).
[CrossRef] [PubMed]

Wilkinson, F.

A. Farmillo and F. Wilkinson, Photochem. Photobiol. 18, 447 (1973).
[CrossRef]

Arch Otolaryngol. Head Neck Surg.

H. S. Garewal, R. Katz, F. Meyskens, J. Pitcock, D. Morse, S. Friedman, Y. Peng, D. Pendrys, S. Mayne, D. Alberts, T. Kiersch, and E. Graver, Arch Otolaryngol. Head Neck Surg. 125, 1305 (1999).
[CrossRef] [PubMed]

Arch. Dermatol.

D. J. Leffell, M. L. Stetz, L. M. Milstone, and L. I. Deckelbaum, Arch. Dermatol. 124, 1514 (1988).
[CrossRef] [PubMed]

Carcinogenesis

L. C. Chen, L. Sly, C. S. Jones, R. De Tarone, and L. M. Luca, Carcinogenesis 14, 713 (1993).
[CrossRef] [PubMed]

Chem. Phys. Lett.

A. P. Shreve, J. K. Trautman, T. G. Owens, and A. C. Albrecht, Chem. Phys. Lett. 178, 89 (1991).

J. Am. Chem. Soc.

C. S. Foote and R. W. Denny, J. Am. Chem. Soc. 90, 6233 (1968).
[CrossRef]

J. Invest. Dermat.

T. R. Hata, T. A. Scholz, I. V. Ermakov, R. W. McClane, F. Khachik, W. Gellermann, and L. K. Pershing, J. Invest. Dermat. 115, 441 (2000).
[CrossRef]

J. Mol. Spectrosc.

F. Inagaki, M. Tasumi, and T. Miyazawa, J. Mol. Spectrosc. 50, 286 (1974).
[CrossRef]

J. Photochem. Photobiol. B

P. F. Conn, W. Schalch, and T. G. Truscott, J. Photochem. Photobiol. B 11, 41 (1991).
[CrossRef] [PubMed]

J. Raman Spectrosc.

Y. Koyama, I. Takatsuka, M. Nakata, and M. Tasumi, J. Raman Spectrosc. 19, 37 (1988).
[CrossRef]

Nature Med.

F. Böhm, J. H. Tinkler, and T. G. Truscott, Nature Med. 1, 98 (1995).
[CrossRef]

Opt. Lett.

Photochem. Photobiol.

A. Farmillo and F. Wilkinson, Photochem. Photobiol. 18, 447 (1973).
[CrossRef]

Other

T. W. M. Boileau, A. C. Moore, and J. W. Erdman, in Antioxidant Status, Diet, Nutrition, and Health, A. M. Papas, ed. (CRC Press, Boca Raton, Fla., 1999), p. 144.

American National Standards Institute, “American national standard for safe use of lasers,” (Laser Institute of America, Orlando, Fla., 2000).

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Figures (4)

Fig. 1
Fig. 1

Resonance Raman spectrum of a dried β-carotene–methanol solution spotted on a thin Teflon substrate.

Fig. 2
Fig. 2

Typical Raman spectra for (a) human forearm skin and (b) oral cavity tissue, measured in vivo. Top traces, spectra obtained before subtraction of native fluorescence background; bottom traces, after subtraction.

Fig. 3
Fig. 3

Bleaching behavior of human skin fluorescence. (a) Fluorescence spectra before and after 7-min illumination at 200mW/cm2 intensity. (b) Fluorescence intensities (at 530  nm) and Raman response versus time during irradiation with 488-nm light at 20 and 200mW/cm2. Note that the Raman response stays constant, whereas the fluorescence bleaches with time.

Fig. 4
Fig. 4

Histogram of Raman measurements for a group of 57 healthy subjects, showing a wide distribution of carotenoid levels among them.

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