Abstract

We incorporate newly developed solid-state detector technology into time-resolved laser Raman spectroscopy, demonstrating the ability to distinguish spectra from Raman and fluorescence processes. As a proof of concept, we show fluorescence rejection on highly fluorescent mineral samples willemite and spodumene using a 128×128 single-photon avalanche diode (SPAD) array with a measured photon detection efficiency of 5%. The sensitivity achieved in this new instrument architecture is comparable to the sensitivity of a technically more complicated system using a traditional photocathode-based imager. By increasing the SPAD active area and improving coupling efficiency, we expect further improvements in sensitivity by over an order of magnitude. We discuss the relevance of these results to in situ planetary instruments, where size, weight, power, and radiation hardness are of prime concern. The potential large-scale manufacturability of silicon SPAD arrays makes them prime candidates for future portable and in situ Raman instruments spanning numerous applications where fluorescence interference is problematic.

© 2011 Optical Society of America

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  1. L. A. Nafie, J. Raman Spectrosc. 41, 1276 (2010).
    [CrossRef]
  2. R. Richards-Kortum and E. Sevick-Muraca, Annu. Rev. Phys. Chem. 47, 555 (1996).
    [CrossRef] [PubMed]
  3. K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, Chem. Rev. 99, 2957 (1999).
    [CrossRef]
  4. P. Vandenabeele, H. G. M. Edwards, and L. Moens, Chem. Rev. 107, 675 (2007).
    [CrossRef] [PubMed]
  5. N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
    [CrossRef]
  6. G. B. Courreges-Lacoste, B. Ahlers, and F. R. Perez, Spectrochim. Acta A 68, 1023 (2007).
    [CrossRef]
  7. A. Wang, B. L. Jolliff, and L. A. Haskin, “Investigating surface mineralogy, alteration processes, and biomarkers on Mars using laser Raman spectroscopy,” presented at the Sixth International Conference on Mars, Pasadena, Calif., July 20–25, 2003, abstract no. 3270.
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    [CrossRef] [PubMed]
  9. S. K. Sharma, A. K. Misra, S. M. Clegg, J. E. Barefield, R. C. Wiens, and T. Acosta, Phil. Trans. R. Soc. A 368, 3167 (2010), and references therein.
    [CrossRef] [PubMed]
  10. L. Carrara, C. Niclass, N. Scheidegger, H. Shea, and E. Charbon, in IEEE International Solid-State Circuits Conference (IEEE, 2009), p. 40.
  11. Y. Maruyama and E. Charbon, in Proceedings of the Transducers’11 Conference (IEEE, 2011), p. 1180.
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    [CrossRef]
  13. M. Gaft, R. Reisfeld, and G. Panczer, Modern Luminescence Spectroscopy of Minerals and Materials (Springer, 2005).

2010 (3)

L. A. Nafie, J. Raman Spectrosc. 41, 1276 (2010).
[CrossRef]

J. Blacksberg, G. Rossman, and A. Gleckler, Appl. Opt. 49, 4951 (2010).
[CrossRef] [PubMed]

S. K. Sharma, A. K. Misra, S. M. Clegg, J. E. Barefield, R. C. Wiens, and T. Acosta, Phil. Trans. R. Soc. A 368, 3167 (2010), and references therein.
[CrossRef] [PubMed]

2009 (1)

M. Gaft and L. Nagli, Eur. J. Mineral. 21, 33 (2009).
[CrossRef]

2008 (1)

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

2007 (2)

G. B. Courreges-Lacoste, B. Ahlers, and F. R. Perez, Spectrochim. Acta A 68, 1023 (2007).
[CrossRef]

P. Vandenabeele, H. G. M. Edwards, and L. Moens, Chem. Rev. 107, 675 (2007).
[CrossRef] [PubMed]

1999 (1)

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, Chem. Rev. 99, 2957 (1999).
[CrossRef]

1996 (1)

R. Richards-Kortum and E. Sevick-Muraca, Annu. Rev. Phys. Chem. 47, 555 (1996).
[CrossRef] [PubMed]

Acosta, T.

S. K. Sharma, A. K. Misra, S. M. Clegg, J. E. Barefield, R. C. Wiens, and T. Acosta, Phil. Trans. R. Soc. A 368, 3167 (2010), and references therein.
[CrossRef] [PubMed]

Ahlers, B.

G. B. Courreges-Lacoste, B. Ahlers, and F. R. Perez, Spectrochim. Acta A 68, 1023 (2007).
[CrossRef]

Barefield, J. E.

S. K. Sharma, A. K. Misra, S. M. Clegg, J. E. Barefield, R. C. Wiens, and T. Acosta, Phil. Trans. R. Soc. A 368, 3167 (2010), and references therein.
[CrossRef] [PubMed]

Blacksberg, J.

Carrara, L.

L. Carrara, C. Niclass, N. Scheidegger, H. Shea, and E. Charbon, in IEEE International Solid-State Circuits Conference (IEEE, 2009), p. 40.

Charbon, E.

L. Carrara, C. Niclass, N. Scheidegger, H. Shea, and E. Charbon, in IEEE International Solid-State Circuits Conference (IEEE, 2009), p. 40.

Y. Maruyama and E. Charbon, in Proceedings of the Transducers’11 Conference (IEEE, 2011), p. 1180.

Clegg, S. M.

S. K. Sharma, A. K. Misra, S. M. Clegg, J. E. Barefield, R. C. Wiens, and T. Acosta, Phil. Trans. R. Soc. A 368, 3167 (2010), and references therein.
[CrossRef] [PubMed]

Courreges-Lacoste, G. B.

G. B. Courreges-Lacoste, B. Ahlers, and F. R. Perez, Spectrochim. Acta A 68, 1023 (2007).
[CrossRef]

Dasari, R. R.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, Chem. Rev. 99, 2957 (1999).
[CrossRef]

Edwards, H. G. M.

P. Vandenabeele, H. G. M. Edwards, and L. Moens, Chem. Rev. 107, 675 (2007).
[CrossRef] [PubMed]

Feld, M. S.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, Chem. Rev. 99, 2957 (1999).
[CrossRef]

Frosch, T.

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

Gaft, M.

M. Gaft and L. Nagli, Eur. J. Mineral. 21, 33 (2009).
[CrossRef]

M. Gaft, R. Reisfeld, and G. Panczer, Modern Luminescence Spectroscopy of Minerals and Materials (Springer, 2005).

Gleckler, A.

Haskin, L. A.

A. Wang, B. L. Jolliff, and L. A. Haskin, “Investigating surface mineralogy, alteration processes, and biomarkers on Mars using laser Raman spectroscopy,” presented at the Sixth International Conference on Mars, Pasadena, Calif., July 20–25, 2003, abstract no. 3270.

Hilchenbach, M.

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

Hochleitner, R.

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

Hofer, S.

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

Itzkan, I.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, Chem. Rev. 99, 2957 (1999).
[CrossRef]

Jolliff, B. L.

A. Wang, B. L. Jolliff, and L. A. Haskin, “Investigating surface mineralogy, alteration processes, and biomarkers on Mars using laser Raman spectroscopy,” presented at the Sixth International Conference on Mars, Pasadena, Calif., July 20–25, 2003, abstract no. 3270.

Kneipp, H.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, Chem. Rev. 99, 2957 (1999).
[CrossRef]

Kneipp, K.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, Chem. Rev. 99, 2957 (1999).
[CrossRef]

Maruyama, Y.

Y. Maruyama and E. Charbon, in Proceedings of the Transducers’11 Conference (IEEE, 2011), p. 1180.

Misra, A. K.

S. K. Sharma, A. K. Misra, S. M. Clegg, J. E. Barefield, R. C. Wiens, and T. Acosta, Phil. Trans. R. Soc. A 368, 3167 (2010), and references therein.
[CrossRef] [PubMed]

Moens, L.

P. Vandenabeele, H. G. M. Edwards, and L. Moens, Chem. Rev. 107, 675 (2007).
[CrossRef] [PubMed]

Nafie, L. A.

L. A. Nafie, J. Raman Spectrosc. 41, 1276 (2010).
[CrossRef]

Nagli, L.

M. Gaft and L. Nagli, Eur. J. Mineral. 21, 33 (2009).
[CrossRef]

Niclass, C.

L. Carrara, C. Niclass, N. Scheidegger, H. Shea, and E. Charbon, in IEEE International Solid-State Circuits Conference (IEEE, 2009), p. 40.

Panczer, G.

M. Gaft, R. Reisfeld, and G. Panczer, Modern Luminescence Spectroscopy of Minerals and Materials (Springer, 2005).

Perez, F. R.

G. B. Courreges-Lacoste, B. Ahlers, and F. R. Perez, Spectrochim. Acta A 68, 1023 (2007).
[CrossRef]

Popp, J.

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

Reisfeld, R.

M. Gaft, R. Reisfeld, and G. Panczer, Modern Luminescence Spectroscopy of Minerals and Materials (Springer, 2005).

Richards-Kortum, R.

R. Richards-Kortum and E. Sevick-Muraca, Annu. Rev. Phys. Chem. 47, 555 (1996).
[CrossRef] [PubMed]

Rösch, P.

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

Rossman, G.

Scheidegger, N.

L. Carrara, C. Niclass, N. Scheidegger, H. Shea, and E. Charbon, in IEEE International Solid-State Circuits Conference (IEEE, 2009), p. 40.

Sevick-Muraca, E.

R. Richards-Kortum and E. Sevick-Muraca, Annu. Rev. Phys. Chem. 47, 555 (1996).
[CrossRef] [PubMed]

Sharma, S. K.

S. K. Sharma, A. K. Misra, S. M. Clegg, J. E. Barefield, R. C. Wiens, and T. Acosta, Phil. Trans. R. Soc. A 368, 3167 (2010), and references therein.
[CrossRef] [PubMed]

Shea, H.

L. Carrara, C. Niclass, N. Scheidegger, H. Shea, and E. Charbon, in IEEE International Solid-State Circuits Conference (IEEE, 2009), p. 40.

Stuffler, T.

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

Tarcea, N.

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

Thiele, H.

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

Vandenabeele, P.

P. Vandenabeele, H. G. M. Edwards, and L. Moens, Chem. Rev. 107, 675 (2007).
[CrossRef] [PubMed]

Wang, A.

A. Wang, B. L. Jolliff, and L. A. Haskin, “Investigating surface mineralogy, alteration processes, and biomarkers on Mars using laser Raman spectroscopy,” presented at the Sixth International Conference on Mars, Pasadena, Calif., July 20–25, 2003, abstract no. 3270.

Wiens, R. C.

S. K. Sharma, A. K. Misra, S. M. Clegg, J. E. Barefield, R. C. Wiens, and T. Acosta, Phil. Trans. R. Soc. A 368, 3167 (2010), and references therein.
[CrossRef] [PubMed]

Annu. Rev. Phys. Chem. (1)

R. Richards-Kortum and E. Sevick-Muraca, Annu. Rev. Phys. Chem. 47, 555 (1996).
[CrossRef] [PubMed]

Appl. Opt. (1)

Chem. Rev. (2)

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, Chem. Rev. 99, 2957 (1999).
[CrossRef]

P. Vandenabeele, H. G. M. Edwards, and L. Moens, Chem. Rev. 107, 675 (2007).
[CrossRef] [PubMed]

Eur. J. Mineral. (1)

M. Gaft and L. Nagli, Eur. J. Mineral. 21, 33 (2009).
[CrossRef]

J. Raman Spectrosc. (1)

L. A. Nafie, J. Raman Spectrosc. 41, 1276 (2010).
[CrossRef]

Phil. Trans. R. Soc. A (1)

S. K. Sharma, A. K. Misra, S. M. Clegg, J. E. Barefield, R. C. Wiens, and T. Acosta, Phil. Trans. R. Soc. A 368, 3167 (2010), and references therein.
[CrossRef] [PubMed]

Space Sci. Rev. (1)

N. Tarcea, T. Frosch, P. Rösch, M. Hilchenbach, T. Stuffler, S. Hofer, H. Thiele, R. Hochleitner, and J. Popp, Space Sci. Rev. 135, 281 (2008)
[CrossRef]

Spectrochim. Acta A (1)

G. B. Courreges-Lacoste, B. Ahlers, and F. R. Perez, Spectrochim. Acta A 68, 1023 (2007).
[CrossRef]

Other (4)

A. Wang, B. L. Jolliff, and L. A. Haskin, “Investigating surface mineralogy, alteration processes, and biomarkers on Mars using laser Raman spectroscopy,” presented at the Sixth International Conference on Mars, Pasadena, Calif., July 20–25, 2003, abstract no. 3270.

L. Carrara, C. Niclass, N. Scheidegger, H. Shea, and E. Charbon, in IEEE International Solid-State Circuits Conference (IEEE, 2009), p. 40.

Y. Maruyama and E. Charbon, in Proceedings of the Transducers’11 Conference (IEEE, 2011), p. 1180.

M. Gaft, R. Reisfeld, and G. Panczer, Modern Luminescence Spectroscopy of Minerals and Materials (Springer, 2005).

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Figures (4)

Fig. 1
Fig. 1

Time-resolved spectra of the highly fluorescent mineral willemite using the 128 × 128 SPAD array. The top image uses a shorter gate time, eliminating the large fluorescence background. The spectra on the right are generated by summing 30 columns in the image.

Fig. 2
Fig. 2

Counts per frame as a function of the number of photons incident on the SPAD. The PDE obtained from the curve fit is 5%.

Fig. 3
Fig. 3

Comparison of willemite Raman spectra using a CCD, streak camera, and 128 × 128 SPAD. The gate time is the time after the start of the laser pulse over which the return signal is averaged. The spectrum obtained with the CCD (CW Raman) is overwhelmed by fluorescence, and the streak camera and SPAD yield similar results with clear Raman spectra.

Fig. 4
Fig. 4

Comparison of spodumene Raman spectra with gate time 32 ns and > 5 μs . A spectrum from the RRUFF database (taken at 785 nm to avoid fluorescence) is shown for reference. The spectra are offset for clarity.

Tables (1)

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Table 1 Experimental Parameters

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