Abstract

Droplet-based microfluidic systems enable miniaturization of chemical reactions in femtoliter to picoliter volume compartments. Quantifying mixing dynamics of the reagents in droplets is critical to determine the system performance. In this Letter, we developed a two-photon excitation fluorescence lifetime imaging technique to quantitatively image the mixing dynamics in microfluidic droplets. A cross/autocorrelation method was used to reconstruct a high-quality fluorescence lifetime image of the droplet. The fluorescence decay was analyzed for accurate determination of the mixing ratio at each pixel of the image.

© 2011 Optical Society of America

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References

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  2. S. Teh, R. Lin, L. Hung, and A. P. Lee, Lab Chip 8, 198 (2008).
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    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef]

2010 (1)

X. C. I. Solvas, M. Srisa-Art, A. J. de Mello, and J. B. Edel, Anal. Chem. 82, 3950 (2010).
[CrossRef]

2008 (4)

2006 (3)

J. T. Coleman, J. McKechnie, and D. Sinton, Lab Chip 6, 1033 (2006).
[CrossRef] [PubMed]

A. J. de Mello, Nature 442, 394 (2006).
[CrossRef]

W. Tanthapanichakoon, N. Aoki, K. Matsuyama, and K. Mae, Chem. Eng. Sci. 61, 4220 (2006).
[CrossRef]

2005 (2)

D. L. Chen, C. J. Gerdts, and R. F. Ismagilov, J. Am. Chem. Soc. 127, 9672 (2005).
[CrossRef] [PubMed]

B. K. H. Yen, A. Gunther, M. A. Schmidt, K. F. Jensen, and M. G. Bawendi, Angew. Chem. Int. Ed. 44, 5447 (2005).
[CrossRef]

2001 (1)

M. Maus, M. Cotlet, J. Hofkens, T. Gensch, F. C. De Schryver, J. Schaffer, and C. A. M. Seidel, Anal. Chem. 73, 2078 (2001).
[CrossRef] [PubMed]

Aoki, N.

W. Tanthapanichakoon, N. Aoki, K. Matsuyama, and K. Mae, Chem. Eng. Sci. 61, 4220 (2006).
[CrossRef]

Baldwin, G. S.

Bawendi, M. G.

B. K. H. Yen, A. Gunther, M. A. Schmidt, K. F. Jensen, and M. G. Bawendi, Angew. Chem. Int. Ed. 44, 5447 (2005).
[CrossRef]

Chen, D. L.

D. L. Chen, C. J. Gerdts, and R. F. Ismagilov, J. Am. Chem. Soc. 127, 9672 (2005).
[CrossRef] [PubMed]

Coleman, J. T.

J. T. Coleman, J. McKechnie, and D. Sinton, Lab Chip 6, 1033 (2006).
[CrossRef] [PubMed]

Cotlet, M.

M. Maus, M. Cotlet, J. Hofkens, T. Gensch, F. C. De Schryver, J. Schaffer, and C. A. M. Seidel, Anal. Chem. 73, 2078 (2001).
[CrossRef] [PubMed]

de Mello, A. J.

X. C. I. Solvas, M. Srisa-Art, A. J. de Mello, and J. B. Edel, Anal. Chem. 82, 3950 (2010).
[CrossRef]

M. Srisa-Art, A. J. de Mello, and J. B. Edel, Phys. Rev. Lett. 101, 014502 (2008).
[CrossRef] [PubMed]

T. Robinson, P. Valluri, H. B. Manning, D. M. Owen, I. Munro, C. B. Talbot, C. Dunsby, J. F. Eccleston, G. S. Baldwin, M. A. A. Neil, A. J. de Mello, and P. M. W. French, Opt. Lett. 33, 1887 (2008).
[CrossRef] [PubMed]

A. J. de Mello, Nature 442, 394 (2006).
[CrossRef]

De Schryver, F. C.

M. Maus, M. Cotlet, J. Hofkens, T. Gensch, F. C. De Schryver, J. Schaffer, and C. A. M. Seidel, Anal. Chem. 73, 2078 (2001).
[CrossRef] [PubMed]

Dunsby, C.

Eccleston, J. F.

Edel, J. B.

X. C. I. Solvas, M. Srisa-Art, A. J. de Mello, and J. B. Edel, Anal. Chem. 82, 3950 (2010).
[CrossRef]

M. Srisa-Art, A. J. de Mello, and J. B. Edel, Phys. Rev. Lett. 101, 014502 (2008).
[CrossRef] [PubMed]

French, P. M. W.

Gensch, T.

M. Maus, M. Cotlet, J. Hofkens, T. Gensch, F. C. De Schryver, J. Schaffer, and C. A. M. Seidel, Anal. Chem. 73, 2078 (2001).
[CrossRef] [PubMed]

Gerdts, C. J.

D. L. Chen, C. J. Gerdts, and R. F. Ismagilov, J. Am. Chem. Soc. 127, 9672 (2005).
[CrossRef] [PubMed]

Gunther, A.

B. K. H. Yen, A. Gunther, M. A. Schmidt, K. F. Jensen, and M. G. Bawendi, Angew. Chem. Int. Ed. 44, 5447 (2005).
[CrossRef]

Hofkens, J.

M. Maus, M. Cotlet, J. Hofkens, T. Gensch, F. C. De Schryver, J. Schaffer, and C. A. M. Seidel, Anal. Chem. 73, 2078 (2001).
[CrossRef] [PubMed]

Hung, L.

S. Teh, R. Lin, L. Hung, and A. P. Lee, Lab Chip 8, 198 (2008).
[CrossRef] [PubMed]

Ismagilov, R. F.

D. L. Chen, C. J. Gerdts, and R. F. Ismagilov, J. Am. Chem. Soc. 127, 9672 (2005).
[CrossRef] [PubMed]

Jensen, K. F.

B. K. H. Yen, A. Gunther, M. A. Schmidt, K. F. Jensen, and M. G. Bawendi, Angew. Chem. Int. Ed. 44, 5447 (2005).
[CrossRef]

Lee, A. P.

S. Teh, R. Lin, L. Hung, and A. P. Lee, Lab Chip 8, 198 (2008).
[CrossRef] [PubMed]

Li, D.

Lin, R.

S. Teh, R. Lin, L. Hung, and A. P. Lee, Lab Chip 8, 198 (2008).
[CrossRef] [PubMed]

Mae, K.

W. Tanthapanichakoon, N. Aoki, K. Matsuyama, and K. Mae, Chem. Eng. Sci. 61, 4220 (2006).
[CrossRef]

Manning, H. B.

Matsuyama, K.

W. Tanthapanichakoon, N. Aoki, K. Matsuyama, and K. Mae, Chem. Eng. Sci. 61, 4220 (2006).
[CrossRef]

Maus, M.

M. Maus, M. Cotlet, J. Hofkens, T. Gensch, F. C. De Schryver, J. Schaffer, and C. A. M. Seidel, Anal. Chem. 73, 2078 (2001).
[CrossRef] [PubMed]

McKechnie, J.

J. T. Coleman, J. McKechnie, and D. Sinton, Lab Chip 6, 1033 (2006).
[CrossRef] [PubMed]

Munro, I.

Neil, M. A. A.

Owen, D. M.

Qu, J. Y.

Robinson, T.

Schaffer, J.

M. Maus, M. Cotlet, J. Hofkens, T. Gensch, F. C. De Schryver, J. Schaffer, and C. A. M. Seidel, Anal. Chem. 73, 2078 (2001).
[CrossRef] [PubMed]

Schmidt, M. A.

B. K. H. Yen, A. Gunther, M. A. Schmidt, K. F. Jensen, and M. G. Bawendi, Angew. Chem. Int. Ed. 44, 5447 (2005).
[CrossRef]

Seidel, C. A. M.

M. Maus, M. Cotlet, J. Hofkens, T. Gensch, F. C. De Schryver, J. Schaffer, and C. A. M. Seidel, Anal. Chem. 73, 2078 (2001).
[CrossRef] [PubMed]

Sinton, D.

J. T. Coleman, J. McKechnie, and D. Sinton, Lab Chip 6, 1033 (2006).
[CrossRef] [PubMed]

Solvas, X. C. I.

X. C. I. Solvas, M. Srisa-Art, A. J. de Mello, and J. B. Edel, Anal. Chem. 82, 3950 (2010).
[CrossRef]

Srisa-Art, M.

X. C. I. Solvas, M. Srisa-Art, A. J. de Mello, and J. B. Edel, Anal. Chem. 82, 3950 (2010).
[CrossRef]

M. Srisa-Art, A. J. de Mello, and J. B. Edel, Phys. Rev. Lett. 101, 014502 (2008).
[CrossRef] [PubMed]

Talbot, C. B.

Tanthapanichakoon, W.

W. Tanthapanichakoon, N. Aoki, K. Matsuyama, and K. Mae, Chem. Eng. Sci. 61, 4220 (2006).
[CrossRef]

Teh, S.

S. Teh, R. Lin, L. Hung, and A. P. Lee, Lab Chip 8, 198 (2008).
[CrossRef] [PubMed]

Valluri, P.

Yen, B. K. H.

B. K. H. Yen, A. Gunther, M. A. Schmidt, K. F. Jensen, and M. G. Bawendi, Angew. Chem. Int. Ed. 44, 5447 (2005).
[CrossRef]

Zheng, W.

Anal. Chem. (2)

M. Maus, M. Cotlet, J. Hofkens, T. Gensch, F. C. De Schryver, J. Schaffer, and C. A. M. Seidel, Anal. Chem. 73, 2078 (2001).
[CrossRef] [PubMed]

X. C. I. Solvas, M. Srisa-Art, A. J. de Mello, and J. B. Edel, Anal. Chem. 82, 3950 (2010).
[CrossRef]

Angew. Chem. Int. Ed. (1)

B. K. H. Yen, A. Gunther, M. A. Schmidt, K. F. Jensen, and M. G. Bawendi, Angew. Chem. Int. Ed. 44, 5447 (2005).
[CrossRef]

Chem. Eng. Sci. (1)

W. Tanthapanichakoon, N. Aoki, K. Matsuyama, and K. Mae, Chem. Eng. Sci. 61, 4220 (2006).
[CrossRef]

J. Am. Chem. Soc. (1)

D. L. Chen, C. J. Gerdts, and R. F. Ismagilov, J. Am. Chem. Soc. 127, 9672 (2005).
[CrossRef] [PubMed]

Lab Chip (2)

J. T. Coleman, J. McKechnie, and D. Sinton, Lab Chip 6, 1033 (2006).
[CrossRef] [PubMed]

S. Teh, R. Lin, L. Hung, and A. P. Lee, Lab Chip 8, 198 (2008).
[CrossRef] [PubMed]

Nature (1)

A. J. de Mello, Nature 442, 394 (2006).
[CrossRef]

Opt. Lett. (2)

Phys. Rev. Lett. (1)

M. Srisa-Art, A. J. de Mello, and J. B. Edel, Phys. Rev. Lett. 101, 014502 (2008).
[CrossRef] [PubMed]

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Figures (3)

Fig. 1
Fig. 1

Image of droplet generation captured by a CCD camera. The scale bar is 50 μm .

Fig. 2
Fig. 2

Fluorescence characteristics of two mixing solutions. (a) Fluorescence decays for Lucifer ( lifetime 5.0 ns ) and Alexa 430 ( lifetime 3.1 ns ). (b) Calculated mixing ratio as a function of photon counts using the LS approach. (c) Measured and calculated mixing ratios from 11 bulk solutions using the division ratio method. (d) Calculated mixing ratio as a function of photon counts using the division ratio method.

Fig. 3
Fig. 3

Methods and results of quantitative mapping of two fluid mixing in droplets. (a) Representative line scanning signal of five droplets. (b) Autocorrelation function of corresponding line-scanning signal. (c) Images of droplets taken by a CCD at the locations of 100, 300, and 500 μm from the cross junction. (d) Reconstructed fluorescence intensity images of droplets at corresponding locations. (e) Mixing ratio images of droplets. (f), (g) Fluorescence intensity images for Alexa 430 and Lucifer Yellow dyes.

Equations (2)

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D Ratio = I Peak I Tail = M Alexa × I P - Alexa + ( 1 - M Alexa ) × I P - Lucifer M Alexa × I T - Alexa + ( 1 - M Alexa ) × I T - Lucifer ,
I Alexa = I Total × M Alexa × F M Alexa × F + ( 1 M Alexa ) ,

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