Abstract

We investigate how light samples disordered porous materials such as ceramics and pharmaceutical materials. By combining photon time-of-flight spectroscopy and sensitive laser-based gas sensing, we obtain information on the extent to which light interacts with solid and pore volumes, respectively. Comparison with mercury intrusion porosimetry shows that light predominantly interacts with the solid. Analysis based on a two-state model does not fully explain observations, revealing a need for refined modeling. Nonetheless, excellent correlation between actual porosity and the porosity experienced by photons demonstrates the potential of nondestructive optical porosimetry based on gas absorption.

© 2010 Optical Society of America

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  1. D. S. Wiersma, P. Bartolini, A. Lagendijk, and R. Righini, Nature 390, 671 (1997).
    [CrossRef]
  2. P. M. Johnson, A. Imhof, B. P. J. Bret, J. G. Rivas, and A. Lagendijk, Phys. Rev. E 68, 016604 (2003).
    [CrossRef]
  3. P. Matousek, Chem. Soc. Rev. 36, 1292 (2007).
    [CrossRef] [PubMed]
  4. L. A. Averett and P. R. Griffiths, Appl. Spectrosc. 62, 377 (2008).
    [CrossRef] [PubMed]
  5. Z. Q. Shi and C. A. Anderson, Anal. Chem. 81, 1389 (2009).
    [CrossRef] [PubMed]
  6. J. G. J. Peelen and R. Metselaa, J. Appl. Phys. 45, 216 (1974).
    [CrossRef]
  7. J. Manara, R. Caps, F. Raether, and J. Fricke, Opt. Commun. 168, 237 (1999).
    [CrossRef]
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    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef] [PubMed]
  19. F. J. P. Schuurmans, D. Vanmaekelbergh, J. van de Lagemaat, and A. Lagendijk, Science 284, 141 (1999).
    [CrossRef] [PubMed]

2010 (1)

T. Svensson and Z. Shen, Appl. Phys. Lett. 96, 021107(2010).
[CrossRef]

2009 (2)

Z. Q. Shi and C. A. Anderson, Anal. Chem. 81, 1389 (2009).
[CrossRef] [PubMed]

T. Svensson, E. Alerstam, D. Khoptyar, J. Johansson, S. Folestad, and S. Andersson-Engels, Rev. Sci. Instrum. 80, 063105 (2009).
[CrossRef] [PubMed]

2008 (6)

C. Toninelli, E. Vekris, G. A. Ozin, S. John, and D. S. Wiersma, Phys. Rev. Lett. 101, 123901 (2008).
[CrossRef] [PubMed]

A. Wolf, B. Terheiden, and R. Brendel, J. Appl. Phys. 104, (2008).
[CrossRef]

T. Svensson, M. Andersson, L. Rippe, S. Svanberg, S. Andersson-Engels, J. Johansson, and S. Folestad, Appl. Phys. B 90, 345 (2008).
[CrossRef]

T. Svensson, M. Andersson, L. Rippe, J. Johansson, S. Folestad, and S. Andersson-Engels, Opt. Lett. 33, 80 (2008).
[CrossRef]

L. A. Averett and P. R. Griffiths, Appl. Spectrosc. 62, 377 (2008).
[CrossRef] [PubMed]

E. Alerstam, S. Andersson-Engels, and T. Svensson, Opt. Express 16, 10440 (2008).
[CrossRef] [PubMed]

2007 (1)

P. Matousek, Chem. Soc. Rev. 36, 1292 (2007).
[CrossRef] [PubMed]

2005 (1)

M. Schmiedeberg, M. F. Miri, and H. Stark, Eur. Phys. J. E 18, 123 (2005).
[CrossRef] [PubMed]

2004 (1)

A. S. Gittings, R. Bandyopadhyay, and D. J. Durian, Europhys. Lett. 65, 414 (2004).
[CrossRef]

2003 (1)

P. M. Johnson, A. Imhof, B. P. J. Bret, J. G. Rivas, and A. Lagendijk, Phys. Rev. E 68, 016604 (2003).
[CrossRef]

2002 (1)

2001 (1)

1999 (2)

F. J. P. Schuurmans, D. Vanmaekelbergh, J. van de Lagemaat, and A. Lagendijk, Science 284, 141 (1999).
[CrossRef] [PubMed]

J. Manara, R. Caps, F. Raether, and J. Fricke, Opt. Commun. 168, 237 (1999).
[CrossRef]

1997 (1)

D. S. Wiersma, P. Bartolini, A. Lagendijk, and R. Righini, Nature 390, 671 (1997).
[CrossRef]

1974 (1)

J. G. J. Peelen and R. Metselaa, J. Appl. Phys. 45, 216 (1974).
[CrossRef]

af Klinteberg, C.

Alerstam, E.

T. Svensson, E. Alerstam, D. Khoptyar, J. Johansson, S. Folestad, and S. Andersson-Engels, Rev. Sci. Instrum. 80, 063105 (2009).
[CrossRef] [PubMed]

E. Alerstam, S. Andersson-Engels, and T. Svensson, Opt. Express 16, 10440 (2008).
[CrossRef] [PubMed]

Alnis, J.

Anderson, C. A.

Z. Q. Shi and C. A. Anderson, Anal. Chem. 81, 1389 (2009).
[CrossRef] [PubMed]

Andersson, M.

T. Svensson, M. Andersson, L. Rippe, S. Svanberg, S. Andersson-Engels, J. Johansson, and S. Folestad, Appl. Phys. B 90, 345 (2008).
[CrossRef]

T. Svensson, M. Andersson, L. Rippe, J. Johansson, S. Folestad, and S. Andersson-Engels, Opt. Lett. 33, 80 (2008).
[CrossRef]

Andersson-Engels, S.

Averett, L. A.

Bandyopadhyay, R.

A. S. Gittings, R. Bandyopadhyay, and D. J. Durian, Europhys. Lett. 65, 414 (2004).
[CrossRef]

Bartolini, P.

D. S. Wiersma, P. Bartolini, A. Lagendijk, and R. Righini, Nature 390, 671 (1997).
[CrossRef]

Brendel, R.

A. Wolf, B. Terheiden, and R. Brendel, J. Appl. Phys. 104, (2008).
[CrossRef]

Bret, B. P. J.

P. M. Johnson, A. Imhof, B. P. J. Bret, J. G. Rivas, and A. Lagendijk, Phys. Rev. E 68, 016604 (2003).
[CrossRef]

Caps, R.

J. Manara, R. Caps, F. Raether, and J. Fricke, Opt. Commun. 168, 237 (1999).
[CrossRef]

Durian, D. J.

A. S. Gittings, R. Bandyopadhyay, and D. J. Durian, Europhys. Lett. 65, 414 (2004).
[CrossRef]

Folestad, S.

T. Svensson, E. Alerstam, D. Khoptyar, J. Johansson, S. Folestad, and S. Andersson-Engels, Rev. Sci. Instrum. 80, 063105 (2009).
[CrossRef] [PubMed]

T. Svensson, M. Andersson, L. Rippe, J. Johansson, S. Folestad, and S. Andersson-Engels, Opt. Lett. 33, 80 (2008).
[CrossRef]

T. Svensson, M. Andersson, L. Rippe, S. Svanberg, S. Andersson-Engels, J. Johansson, and S. Folestad, Appl. Phys. B 90, 345 (2008).
[CrossRef]

Fricke, J.

J. Manara, R. Caps, F. Raether, and J. Fricke, Opt. Commun. 168, 237 (1999).
[CrossRef]

Gittings, A. S.

A. S. Gittings, R. Bandyopadhyay, and D. J. Durian, Europhys. Lett. 65, 414 (2004).
[CrossRef]

Griffiths, P. R.

Imhof, A.

P. M. Johnson, A. Imhof, B. P. J. Bret, J. G. Rivas, and A. Lagendijk, Phys. Rev. E 68, 016604 (2003).
[CrossRef]

Johansson, J.

T. Svensson, E. Alerstam, D. Khoptyar, J. Johansson, S. Folestad, and S. Andersson-Engels, Rev. Sci. Instrum. 80, 063105 (2009).
[CrossRef] [PubMed]

T. Svensson, M. Andersson, L. Rippe, J. Johansson, S. Folestad, and S. Andersson-Engels, Opt. Lett. 33, 80 (2008).
[CrossRef]

T. Svensson, M. Andersson, L. Rippe, S. Svanberg, S. Andersson-Engels, J. Johansson, and S. Folestad, Appl. Phys. B 90, 345 (2008).
[CrossRef]

John, S.

C. Toninelli, E. Vekris, G. A. Ozin, S. John, and D. S. Wiersma, Phys. Rev. Lett. 101, 123901 (2008).
[CrossRef] [PubMed]

Johnson, P. M.

P. M. Johnson, A. Imhof, B. P. J. Bret, J. G. Rivas, and A. Lagendijk, Phys. Rev. E 68, 016604 (2003).
[CrossRef]

Khoptyar, D.

T. Svensson, E. Alerstam, D. Khoptyar, J. Johansson, S. Folestad, and S. Andersson-Engels, Rev. Sci. Instrum. 80, 063105 (2009).
[CrossRef] [PubMed]

Lagendijk, A.

P. M. Johnson, A. Imhof, B. P. J. Bret, J. G. Rivas, and A. Lagendijk, Phys. Rev. E 68, 016604 (2003).
[CrossRef]

F. J. P. Schuurmans, D. Vanmaekelbergh, J. van de Lagemaat, and A. Lagendijk, Science 284, 141 (1999).
[CrossRef] [PubMed]

D. S. Wiersma, P. Bartolini, A. Lagendijk, and R. Righini, Nature 390, 671 (1997).
[CrossRef]

Manara, J.

J. Manara, R. Caps, F. Raether, and J. Fricke, Opt. Commun. 168, 237 (1999).
[CrossRef]

Matousek, P.

P. Matousek, Chem. Soc. Rev. 36, 1292 (2007).
[CrossRef] [PubMed]

Metselaa, R.

J. G. J. Peelen and R. Metselaa, J. Appl. Phys. 45, 216 (1974).
[CrossRef]

Miri, M. F.

M. Schmiedeberg, M. F. Miri, and H. Stark, Eur. Phys. J. E 18, 123 (2005).
[CrossRef] [PubMed]

Ozin, G. A.

C. Toninelli, E. Vekris, G. A. Ozin, S. John, and D. S. Wiersma, Phys. Rev. Lett. 101, 123901 (2008).
[CrossRef] [PubMed]

Peelen, J. G. J.

J. G. J. Peelen and R. Metselaa, J. Appl. Phys. 45, 216 (1974).
[CrossRef]

Raether, F.

J. Manara, R. Caps, F. Raether, and J. Fricke, Opt. Commun. 168, 237 (1999).
[CrossRef]

Righini, R.

D. S. Wiersma, P. Bartolini, A. Lagendijk, and R. Righini, Nature 390, 671 (1997).
[CrossRef]

Rippe, L.

T. Svensson, M. Andersson, L. Rippe, S. Svanberg, S. Andersson-Engels, J. Johansson, and S. Folestad, Appl. Phys. B 90, 345 (2008).
[CrossRef]

T. Svensson, M. Andersson, L. Rippe, J. Johansson, S. Folestad, and S. Andersson-Engels, Opt. Lett. 33, 80 (2008).
[CrossRef]

Rivas, J. G.

P. M. Johnson, A. Imhof, B. P. J. Bret, J. G. Rivas, and A. Lagendijk, Phys. Rev. E 68, 016604 (2003).
[CrossRef]

Schmiedeberg, M.

M. Schmiedeberg, M. F. Miri, and H. Stark, Eur. Phys. J. E 18, 123 (2005).
[CrossRef] [PubMed]

Schuurmans, F. J. P.

F. J. P. Schuurmans, D. Vanmaekelbergh, J. van de Lagemaat, and A. Lagendijk, Science 284, 141 (1999).
[CrossRef] [PubMed]

Shen, Z.

T. Svensson and Z. Shen, Appl. Phys. Lett. 96, 021107(2010).
[CrossRef]

Shi, Z. Q.

Z. Q. Shi and C. A. Anderson, Anal. Chem. 81, 1389 (2009).
[CrossRef] [PubMed]

Sjöholm, M.

Somesfalean, G.

Stark, H.

M. Schmiedeberg, M. F. Miri, and H. Stark, Eur. Phys. J. E 18, 123 (2005).
[CrossRef] [PubMed]

Svanberg, S.

Svensson, T.

T. Svensson and Z. Shen, Appl. Phys. Lett. 96, 021107(2010).
[CrossRef]

T. Svensson, E. Alerstam, D. Khoptyar, J. Johansson, S. Folestad, and S. Andersson-Engels, Rev. Sci. Instrum. 80, 063105 (2009).
[CrossRef] [PubMed]

E. Alerstam, S. Andersson-Engels, and T. Svensson, Opt. Express 16, 10440 (2008).
[CrossRef] [PubMed]

T. Svensson, M. Andersson, L. Rippe, J. Johansson, S. Folestad, and S. Andersson-Engels, Opt. Lett. 33, 80 (2008).
[CrossRef]

T. Svensson, M. Andersson, L. Rippe, S. Svanberg, S. Andersson-Engels, J. Johansson, and S. Folestad, Appl. Phys. B 90, 345 (2008).
[CrossRef]

Terheiden, B.

A. Wolf, B. Terheiden, and R. Brendel, J. Appl. Phys. 104, (2008).
[CrossRef]

Toninelli, C.

C. Toninelli, E. Vekris, G. A. Ozin, S. John, and D. S. Wiersma, Phys. Rev. Lett. 101, 123901 (2008).
[CrossRef] [PubMed]

van de Lagemaat, J.

F. J. P. Schuurmans, D. Vanmaekelbergh, J. van de Lagemaat, and A. Lagendijk, Science 284, 141 (1999).
[CrossRef] [PubMed]

Vanmaekelbergh, D.

F. J. P. Schuurmans, D. Vanmaekelbergh, J. van de Lagemaat, and A. Lagendijk, Science 284, 141 (1999).
[CrossRef] [PubMed]

Vekris, E.

C. Toninelli, E. Vekris, G. A. Ozin, S. John, and D. S. Wiersma, Phys. Rev. Lett. 101, 123901 (2008).
[CrossRef] [PubMed]

Wiersma, D. S.

C. Toninelli, E. Vekris, G. A. Ozin, S. John, and D. S. Wiersma, Phys. Rev. Lett. 101, 123901 (2008).
[CrossRef] [PubMed]

D. S. Wiersma, P. Bartolini, A. Lagendijk, and R. Righini, Nature 390, 671 (1997).
[CrossRef]

Wolf, A.

A. Wolf, B. Terheiden, and R. Brendel, J. Appl. Phys. 104, (2008).
[CrossRef]

Anal. Chem. (1)

Z. Q. Shi and C. A. Anderson, Anal. Chem. 81, 1389 (2009).
[CrossRef] [PubMed]

Appl. Opt. (1)

Appl. Phys. B (1)

T. Svensson, M. Andersson, L. Rippe, S. Svanberg, S. Andersson-Engels, J. Johansson, and S. Folestad, Appl. Phys. B 90, 345 (2008).
[CrossRef]

Appl. Phys. Lett. (1)

T. Svensson and Z. Shen, Appl. Phys. Lett. 96, 021107(2010).
[CrossRef]

Appl. Spectrosc. (1)

Chem. Soc. Rev. (1)

P. Matousek, Chem. Soc. Rev. 36, 1292 (2007).
[CrossRef] [PubMed]

Eur. Phys. J. E (1)

M. Schmiedeberg, M. F. Miri, and H. Stark, Eur. Phys. J. E 18, 123 (2005).
[CrossRef] [PubMed]

Europhys. Lett. (1)

A. S. Gittings, R. Bandyopadhyay, and D. J. Durian, Europhys. Lett. 65, 414 (2004).
[CrossRef]

J. Appl. Phys. (2)

A. Wolf, B. Terheiden, and R. Brendel, J. Appl. Phys. 104, (2008).
[CrossRef]

J. G. J. Peelen and R. Metselaa, J. Appl. Phys. 45, 216 (1974).
[CrossRef]

Nature (1)

D. S. Wiersma, P. Bartolini, A. Lagendijk, and R. Righini, Nature 390, 671 (1997).
[CrossRef]

Opt. Commun. (1)

J. Manara, R. Caps, F. Raether, and J. Fricke, Opt. Commun. 168, 237 (1999).
[CrossRef]

Opt. Express (1)

Opt. Lett. (2)

Phys. Rev. E (1)

P. M. Johnson, A. Imhof, B. P. J. Bret, J. G. Rivas, and A. Lagendijk, Phys. Rev. E 68, 016604 (2003).
[CrossRef]

Phys. Rev. Lett. (1)

C. Toninelli, E. Vekris, G. A. Ozin, S. John, and D. S. Wiersma, Phys. Rev. Lett. 101, 123901 (2008).
[CrossRef] [PubMed]

Rev. Sci. Instrum. (1)

T. Svensson, E. Alerstam, D. Khoptyar, J. Johansson, S. Folestad, and S. Andersson-Engels, Rev. Sci. Instrum. 80, 063105 (2009).
[CrossRef] [PubMed]

Science (1)

F. J. P. Schuurmans, D. Vanmaekelbergh, J. van de Lagemaat, and A. Lagendijk, Science 284, 141 (1999).
[CrossRef] [PubMed]

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Figures (4)

Fig. 1
Fig. 1

(a) PTOFS and (b) GASMAS data from the macroporous alumina. Diffusion modeling [12] yields a reduced scattering of 1300 cm 1 and negligible absorption. The gas absorption signal is a 2 f WMS signal. Evaluation using an air spectrum [12] yields a pathlength of 66.0 mm (including a 7.2 mm offset).

Fig. 2
Fig. 2

Cumulative mercury intrusion for tablets. 1 6 μm pores dominate the pore volume. Compression removes large pores, shifting large-pore cutoff from 5 to 2 μm .

Fig. 3
Fig. 3

Comparison of optical porosity, ϕ opt , and porosity given by mercury intrusion, ϕ Hg , for 12 pharmaceutical samples. The solid line shows porosity expected from assuming an MCC density of 1.46 g / cm 3 . To avoid artifacts due to deformation at high mercury pressures, ϕ Hg is based on the cumulative intrusion at 0.1 μm and may thus be a slight underestimation of the true porosity.

Fig. 4
Fig. 4

Correlation between optical and actual porosity (correlation coefficient 0.98, ϕ opt 0.48 ϕ × Hg ).

Equations (2)

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L = L s + L p = c 0 n s 1 t s + c 0 t p ,
ϕ opt = π p ϕ π p ϕ + π s ( 1 ϕ ) .

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