Abstract

Recent developments in the field of single molecule orientation imaging have led us to devise a simple framework for analyzing fluorescence intensity fluctuations in single molecule polarization sensitive experiments. Based on the new framework, rotational dynamics of individual molecules are quantified, in this paper, from the short time behavior of the time averaged fluorescence intensity fluctuation trajectories. The suggested model can be applied in single molecule fluorescence fluctuations experiments to extract accurate expectation values of photon counts during very short integration time in which rotational diffusion is likely not to be averaged out.

© 2012 OSA

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    [CrossRef]
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    [CrossRef] [PubMed]
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2011 (1)

G. Hinze, T. Basché, and R. A. L. Vallée, “Single molecule probing of dynamics in supercooled polymers,” Phys. Chem. Chem. Phys. 13(5), 1813–1818 (2011).
[CrossRef] [PubMed]

2010 (1)

G. Hinze and T. Basché, “Statistical analysis of time resolved single molecule fluorescence data without time binning,” J. Chem. Phys. 132(4), 044509 (2010).
[CrossRef] [PubMed]

2009 (1)

L. Turgeman, S. Carmi, and E. Barkai, “Fractional Feynman-Kac equation for non-brownian functionals,” Phys. Rev. Lett. 103(19), 190201 (2009).
[CrossRef] [PubMed]

2008 (1)

R. A. L. Vallée, T. Rohand, N. Boens, W. Dehaen, G. Hinze, and T. Basché, “Analysis of the exponential character of single molecule rotational correlation functions for large and small fluorescence collection angles,” J. Chem. Phys. 128(15), 154515 (2008).
[CrossRef] [PubMed]

2006 (1)

D. Fixler, Y. Namer, Y. Yishay, and M. Deutsch, “Influence of fluorescence anisotropy on fluorescence intensity and lifetime measurement: theory, simulations and experiments,” IEEE Trans. Biomed. Eng. 53(6), 1141–1152 (2006).
[CrossRef] [PubMed]

2005 (3)

C. Y. Wei, Y. H. Kim, R. K. Darst, P. J. Rossky, and D. A. Vanden Bout, “Origins of nonexponential decay in single molecule measurements of rotational dynamics,” Phys. Rev. Lett. 95(17), 173001 (2005).
[CrossRef] [PubMed]

R. A. L. Vallée, N. Tomczak, G. J. Vancso, L. Kuipers, and N. F. van Hulst, “Fluorescence lifetime fluctuations of single molecules probe local density fluctuations in disordered media: a bulk approach,” J. Chem. Phys. 122(11), 114704 (2005).
[CrossRef] [PubMed]

S. A. Rosenberg, M. E. Quinlan, J. N. Forkey, and Y. E. Goldman, “Rotational motions of macro-molecules by single-molecule fluorescence microscopy,” Acc. Chem. Res. 38(7), 583–593 (2005).
[CrossRef] [PubMed]

2004 (2)

X. Tan, D. Hu, T. C. Squier, and H. P. Lu, “Probing nanosecond protein motions of calmodulin by single-molecule fluorescence anisotropy,” Appl. Phys. Lett. 85(12), 2420–2422 (2004).
[CrossRef]

G. Hinze, G. Diezemann, and T. Basché, “Rotational correlation functions of single molecules,” Phys. Rev. Lett. 93(20), 203001 (2004).
[CrossRef] [PubMed]

2002 (5)

A. P. Bartko, K. Xu, and R. M. Dickson, “Three-dimensional single molecule rotational diffusion in glassy state polymer films,” Phys. Rev. Lett. 89(2), 026101 (2002).
[CrossRef] [PubMed]

H. Yang and S. Xie, “Probing single-molecule dynamics photon by photon,” J. Chem. Phys. 117(24), 10965–10979 (2002).
[CrossRef]

L. A. Deschenes and D. A. Vanden Bout, “Heterogeneous dynamics and domains in supercooled o-Terphenyl: a single molecule study,” J. Phys. Chem. B 106(44), 11438–11445 (2002).
[CrossRef]

R. Richert, “Heterogeneous dynamics in liquids: fluctuations in space and time,” J. Phys. Condens. Matter 14(23), R703–R738 (2002).
[CrossRef]

Y. Jung, E. Barkai, and R. J. Silbey, “A stochastic theory of single molecule spectroscopy,” Adv. Chem. Phys. 123, 199–266 (2002).
[CrossRef]

2001 (2)

J. T. Fourkas, “Rapid determination of the three-dimensional orientation of single molecules,” Opt. Lett. 26(4), 211–213 (2001).
[CrossRef] [PubMed]

D. Fixler, R. Tirosh, A. Shainberg, and M. Deutsch, “Cytoplasmic changes in cardiac cells during contraction cycle detected by fluorescence polarization,” J. Fluoresc. 11(2), 89–100 (2001).
[CrossRef]

1999 (1)

Y. Chen, J. D. Müller, P. T. C. So, and E. Gratton, “The photon counting histogram in fluorescence fluctuation spectroscopy,” Biophys. J. 77(1), 553–567 (1999).
[CrossRef] [PubMed]

1970 (1)

M. Zwanziger and M. Lax, “Exact photocount distributions for lasers near threshold,” Phys. Rev. Lett. 24(17), 937–940 (1970).
[CrossRef]

1958 (1)

L. Mandel, “Fluctuations of photon beams and their correlations,” Proc. Phys. Soc. 72(6), 1037–1048 (1958).
[CrossRef]

Barkai, E.

L. Turgeman, S. Carmi, and E. Barkai, “Fractional Feynman-Kac equation for non-brownian functionals,” Phys. Rev. Lett. 103(19), 190201 (2009).
[CrossRef] [PubMed]

Y. Jung, E. Barkai, and R. J. Silbey, “A stochastic theory of single molecule spectroscopy,” Adv. Chem. Phys. 123, 199–266 (2002).
[CrossRef]

Bartko, A. P.

A. P. Bartko, K. Xu, and R. M. Dickson, “Three-dimensional single molecule rotational diffusion in glassy state polymer films,” Phys. Rev. Lett. 89(2), 026101 (2002).
[CrossRef] [PubMed]

Basché, T.

G. Hinze, T. Basché, and R. A. L. Vallée, “Single molecule probing of dynamics in supercooled polymers,” Phys. Chem. Chem. Phys. 13(5), 1813–1818 (2011).
[CrossRef] [PubMed]

G. Hinze and T. Basché, “Statistical analysis of time resolved single molecule fluorescence data without time binning,” J. Chem. Phys. 132(4), 044509 (2010).
[CrossRef] [PubMed]

R. A. L. Vallée, T. Rohand, N. Boens, W. Dehaen, G. Hinze, and T. Basché, “Analysis of the exponential character of single molecule rotational correlation functions for large and small fluorescence collection angles,” J. Chem. Phys. 128(15), 154515 (2008).
[CrossRef] [PubMed]

G. Hinze, G. Diezemann, and T. Basché, “Rotational correlation functions of single molecules,” Phys. Rev. Lett. 93(20), 203001 (2004).
[CrossRef] [PubMed]

Boens, N.

R. A. L. Vallée, T. Rohand, N. Boens, W. Dehaen, G. Hinze, and T. Basché, “Analysis of the exponential character of single molecule rotational correlation functions for large and small fluorescence collection angles,” J. Chem. Phys. 128(15), 154515 (2008).
[CrossRef] [PubMed]

Carmi, S.

L. Turgeman, S. Carmi, and E. Barkai, “Fractional Feynman-Kac equation for non-brownian functionals,” Phys. Rev. Lett. 103(19), 190201 (2009).
[CrossRef] [PubMed]

Chen, Y.

Y. Chen, J. D. Müller, P. T. C. So, and E. Gratton, “The photon counting histogram in fluorescence fluctuation spectroscopy,” Biophys. J. 77(1), 553–567 (1999).
[CrossRef] [PubMed]

Darst, R. K.

C. Y. Wei, Y. H. Kim, R. K. Darst, P. J. Rossky, and D. A. Vanden Bout, “Origins of nonexponential decay in single molecule measurements of rotational dynamics,” Phys. Rev. Lett. 95(17), 173001 (2005).
[CrossRef] [PubMed]

Dehaen, W.

R. A. L. Vallée, T. Rohand, N. Boens, W. Dehaen, G. Hinze, and T. Basché, “Analysis of the exponential character of single molecule rotational correlation functions for large and small fluorescence collection angles,” J. Chem. Phys. 128(15), 154515 (2008).
[CrossRef] [PubMed]

Deschenes, L. A.

L. A. Deschenes and D. A. Vanden Bout, “Heterogeneous dynamics and domains in supercooled o-Terphenyl: a single molecule study,” J. Phys. Chem. B 106(44), 11438–11445 (2002).
[CrossRef]

Deutsch, M.

D. Fixler, Y. Namer, Y. Yishay, and M. Deutsch, “Influence of fluorescence anisotropy on fluorescence intensity and lifetime measurement: theory, simulations and experiments,” IEEE Trans. Biomed. Eng. 53(6), 1141–1152 (2006).
[CrossRef] [PubMed]

D. Fixler, R. Tirosh, A. Shainberg, and M. Deutsch, “Cytoplasmic changes in cardiac cells during contraction cycle detected by fluorescence polarization,” J. Fluoresc. 11(2), 89–100 (2001).
[CrossRef]

Dickson, R. M.

A. P. Bartko, K. Xu, and R. M. Dickson, “Three-dimensional single molecule rotational diffusion in glassy state polymer films,” Phys. Rev. Lett. 89(2), 026101 (2002).
[CrossRef] [PubMed]

Diezemann, G.

G. Hinze, G. Diezemann, and T. Basché, “Rotational correlation functions of single molecules,” Phys. Rev. Lett. 93(20), 203001 (2004).
[CrossRef] [PubMed]

Fixler, D.

D. Fixler, Y. Namer, Y. Yishay, and M. Deutsch, “Influence of fluorescence anisotropy on fluorescence intensity and lifetime measurement: theory, simulations and experiments,” IEEE Trans. Biomed. Eng. 53(6), 1141–1152 (2006).
[CrossRef] [PubMed]

D. Fixler, R. Tirosh, A. Shainberg, and M. Deutsch, “Cytoplasmic changes in cardiac cells during contraction cycle detected by fluorescence polarization,” J. Fluoresc. 11(2), 89–100 (2001).
[CrossRef]

Forkey, J. N.

S. A. Rosenberg, M. E. Quinlan, J. N. Forkey, and Y. E. Goldman, “Rotational motions of macro-molecules by single-molecule fluorescence microscopy,” Acc. Chem. Res. 38(7), 583–593 (2005).
[CrossRef] [PubMed]

Fourkas, J. T.

Goldman, Y. E.

S. A. Rosenberg, M. E. Quinlan, J. N. Forkey, and Y. E. Goldman, “Rotational motions of macro-molecules by single-molecule fluorescence microscopy,” Acc. Chem. Res. 38(7), 583–593 (2005).
[CrossRef] [PubMed]

Gratton, E.

Y. Chen, J. D. Müller, P. T. C. So, and E. Gratton, “The photon counting histogram in fluorescence fluctuation spectroscopy,” Biophys. J. 77(1), 553–567 (1999).
[CrossRef] [PubMed]

Hinze, G.

G. Hinze, T. Basché, and R. A. L. Vallée, “Single molecule probing of dynamics in supercooled polymers,” Phys. Chem. Chem. Phys. 13(5), 1813–1818 (2011).
[CrossRef] [PubMed]

G. Hinze and T. Basché, “Statistical analysis of time resolved single molecule fluorescence data without time binning,” J. Chem. Phys. 132(4), 044509 (2010).
[CrossRef] [PubMed]

R. A. L. Vallée, T. Rohand, N. Boens, W. Dehaen, G. Hinze, and T. Basché, “Analysis of the exponential character of single molecule rotational correlation functions for large and small fluorescence collection angles,” J. Chem. Phys. 128(15), 154515 (2008).
[CrossRef] [PubMed]

G. Hinze, G. Diezemann, and T. Basché, “Rotational correlation functions of single molecules,” Phys. Rev. Lett. 93(20), 203001 (2004).
[CrossRef] [PubMed]

Hu, D.

X. Tan, D. Hu, T. C. Squier, and H. P. Lu, “Probing nanosecond protein motions of calmodulin by single-molecule fluorescence anisotropy,” Appl. Phys. Lett. 85(12), 2420–2422 (2004).
[CrossRef]

Jung, Y.

Y. Jung, E. Barkai, and R. J. Silbey, “A stochastic theory of single molecule spectroscopy,” Adv. Chem. Phys. 123, 199–266 (2002).
[CrossRef]

Kim, Y. H.

C. Y. Wei, Y. H. Kim, R. K. Darst, P. J. Rossky, and D. A. Vanden Bout, “Origins of nonexponential decay in single molecule measurements of rotational dynamics,” Phys. Rev. Lett. 95(17), 173001 (2005).
[CrossRef] [PubMed]

Kuipers, L.

R. A. L. Vallée, N. Tomczak, G. J. Vancso, L. Kuipers, and N. F. van Hulst, “Fluorescence lifetime fluctuations of single molecules probe local density fluctuations in disordered media: a bulk approach,” J. Chem. Phys. 122(11), 114704 (2005).
[CrossRef] [PubMed]

Lax, M.

M. Zwanziger and M. Lax, “Exact photocount distributions for lasers near threshold,” Phys. Rev. Lett. 24(17), 937–940 (1970).
[CrossRef]

Lu, H. P.

X. Tan, D. Hu, T. C. Squier, and H. P. Lu, “Probing nanosecond protein motions of calmodulin by single-molecule fluorescence anisotropy,” Appl. Phys. Lett. 85(12), 2420–2422 (2004).
[CrossRef]

Mandel, L.

L. Mandel, “Fluctuations of photon beams and their correlations,” Proc. Phys. Soc. 72(6), 1037–1048 (1958).
[CrossRef]

Müller, J. D.

Y. Chen, J. D. Müller, P. T. C. So, and E. Gratton, “The photon counting histogram in fluorescence fluctuation spectroscopy,” Biophys. J. 77(1), 553–567 (1999).
[CrossRef] [PubMed]

Namer, Y.

D. Fixler, Y. Namer, Y. Yishay, and M. Deutsch, “Influence of fluorescence anisotropy on fluorescence intensity and lifetime measurement: theory, simulations and experiments,” IEEE Trans. Biomed. Eng. 53(6), 1141–1152 (2006).
[CrossRef] [PubMed]

Quinlan, M. E.

S. A. Rosenberg, M. E. Quinlan, J. N. Forkey, and Y. E. Goldman, “Rotational motions of macro-molecules by single-molecule fluorescence microscopy,” Acc. Chem. Res. 38(7), 583–593 (2005).
[CrossRef] [PubMed]

Richert, R.

R. Richert, “Heterogeneous dynamics in liquids: fluctuations in space and time,” J. Phys. Condens. Matter 14(23), R703–R738 (2002).
[CrossRef]

Rohand, T.

R. A. L. Vallée, T. Rohand, N. Boens, W. Dehaen, G. Hinze, and T. Basché, “Analysis of the exponential character of single molecule rotational correlation functions for large and small fluorescence collection angles,” J. Chem. Phys. 128(15), 154515 (2008).
[CrossRef] [PubMed]

Rosenberg, S. A.

S. A. Rosenberg, M. E. Quinlan, J. N. Forkey, and Y. E. Goldman, “Rotational motions of macro-molecules by single-molecule fluorescence microscopy,” Acc. Chem. Res. 38(7), 583–593 (2005).
[CrossRef] [PubMed]

Rossky, P. J.

C. Y. Wei, Y. H. Kim, R. K. Darst, P. J. Rossky, and D. A. Vanden Bout, “Origins of nonexponential decay in single molecule measurements of rotational dynamics,” Phys. Rev. Lett. 95(17), 173001 (2005).
[CrossRef] [PubMed]

Shainberg, A.

D. Fixler, R. Tirosh, A. Shainberg, and M. Deutsch, “Cytoplasmic changes in cardiac cells during contraction cycle detected by fluorescence polarization,” J. Fluoresc. 11(2), 89–100 (2001).
[CrossRef]

Silbey, R. J.

Y. Jung, E. Barkai, and R. J. Silbey, “A stochastic theory of single molecule spectroscopy,” Adv. Chem. Phys. 123, 199–266 (2002).
[CrossRef]

So, P. T. C.

Y. Chen, J. D. Müller, P. T. C. So, and E. Gratton, “The photon counting histogram in fluorescence fluctuation spectroscopy,” Biophys. J. 77(1), 553–567 (1999).
[CrossRef] [PubMed]

Squier, T. C.

X. Tan, D. Hu, T. C. Squier, and H. P. Lu, “Probing nanosecond protein motions of calmodulin by single-molecule fluorescence anisotropy,” Appl. Phys. Lett. 85(12), 2420–2422 (2004).
[CrossRef]

Tan, X.

X. Tan, D. Hu, T. C. Squier, and H. P. Lu, “Probing nanosecond protein motions of calmodulin by single-molecule fluorescence anisotropy,” Appl. Phys. Lett. 85(12), 2420–2422 (2004).
[CrossRef]

Tirosh, R.

D. Fixler, R. Tirosh, A. Shainberg, and M. Deutsch, “Cytoplasmic changes in cardiac cells during contraction cycle detected by fluorescence polarization,” J. Fluoresc. 11(2), 89–100 (2001).
[CrossRef]

Tomczak, N.

R. A. L. Vallée, N. Tomczak, G. J. Vancso, L. Kuipers, and N. F. van Hulst, “Fluorescence lifetime fluctuations of single molecules probe local density fluctuations in disordered media: a bulk approach,” J. Chem. Phys. 122(11), 114704 (2005).
[CrossRef] [PubMed]

Turgeman, L.

L. Turgeman, S. Carmi, and E. Barkai, “Fractional Feynman-Kac equation for non-brownian functionals,” Phys. Rev. Lett. 103(19), 190201 (2009).
[CrossRef] [PubMed]

Vallée, R. A. L.

G. Hinze, T. Basché, and R. A. L. Vallée, “Single molecule probing of dynamics in supercooled polymers,” Phys. Chem. Chem. Phys. 13(5), 1813–1818 (2011).
[CrossRef] [PubMed]

R. A. L. Vallée, T. Rohand, N. Boens, W. Dehaen, G. Hinze, and T. Basché, “Analysis of the exponential character of single molecule rotational correlation functions for large and small fluorescence collection angles,” J. Chem. Phys. 128(15), 154515 (2008).
[CrossRef] [PubMed]

R. A. L. Vallée, N. Tomczak, G. J. Vancso, L. Kuipers, and N. F. van Hulst, “Fluorescence lifetime fluctuations of single molecules probe local density fluctuations in disordered media: a bulk approach,” J. Chem. Phys. 122(11), 114704 (2005).
[CrossRef] [PubMed]

van Hulst, N. F.

R. A. L. Vallée, N. Tomczak, G. J. Vancso, L. Kuipers, and N. F. van Hulst, “Fluorescence lifetime fluctuations of single molecules probe local density fluctuations in disordered media: a bulk approach,” J. Chem. Phys. 122(11), 114704 (2005).
[CrossRef] [PubMed]

Vancso, G. J.

R. A. L. Vallée, N. Tomczak, G. J. Vancso, L. Kuipers, and N. F. van Hulst, “Fluorescence lifetime fluctuations of single molecules probe local density fluctuations in disordered media: a bulk approach,” J. Chem. Phys. 122(11), 114704 (2005).
[CrossRef] [PubMed]

Vanden Bout, D. A.

C. Y. Wei, Y. H. Kim, R. K. Darst, P. J. Rossky, and D. A. Vanden Bout, “Origins of nonexponential decay in single molecule measurements of rotational dynamics,” Phys. Rev. Lett. 95(17), 173001 (2005).
[CrossRef] [PubMed]

L. A. Deschenes and D. A. Vanden Bout, “Heterogeneous dynamics and domains in supercooled o-Terphenyl: a single molecule study,” J. Phys. Chem. B 106(44), 11438–11445 (2002).
[CrossRef]

Wei, C. Y.

C. Y. Wei, Y. H. Kim, R. K. Darst, P. J. Rossky, and D. A. Vanden Bout, “Origins of nonexponential decay in single molecule measurements of rotational dynamics,” Phys. Rev. Lett. 95(17), 173001 (2005).
[CrossRef] [PubMed]

Xie, S.

H. Yang and S. Xie, “Probing single-molecule dynamics photon by photon,” J. Chem. Phys. 117(24), 10965–10979 (2002).
[CrossRef]

Xu, K.

A. P. Bartko, K. Xu, and R. M. Dickson, “Three-dimensional single molecule rotational diffusion in glassy state polymer films,” Phys. Rev. Lett. 89(2), 026101 (2002).
[CrossRef] [PubMed]

Yang, H.

H. Yang and S. Xie, “Probing single-molecule dynamics photon by photon,” J. Chem. Phys. 117(24), 10965–10979 (2002).
[CrossRef]

Yishay, Y.

D. Fixler, Y. Namer, Y. Yishay, and M. Deutsch, “Influence of fluorescence anisotropy on fluorescence intensity and lifetime measurement: theory, simulations and experiments,” IEEE Trans. Biomed. Eng. 53(6), 1141–1152 (2006).
[CrossRef] [PubMed]

Zwanziger, M.

M. Zwanziger and M. Lax, “Exact photocount distributions for lasers near threshold,” Phys. Rev. Lett. 24(17), 937–940 (1970).
[CrossRef]

Acc. Chem. Res. (1)

S. A. Rosenberg, M. E. Quinlan, J. N. Forkey, and Y. E. Goldman, “Rotational motions of macro-molecules by single-molecule fluorescence microscopy,” Acc. Chem. Res. 38(7), 583–593 (2005).
[CrossRef] [PubMed]

Adv. Chem. Phys. (1)

Y. Jung, E. Barkai, and R. J. Silbey, “A stochastic theory of single molecule spectroscopy,” Adv. Chem. Phys. 123, 199–266 (2002).
[CrossRef]

Appl. Phys. Lett. (1)

X. Tan, D. Hu, T. C. Squier, and H. P. Lu, “Probing nanosecond protein motions of calmodulin by single-molecule fluorescence anisotropy,” Appl. Phys. Lett. 85(12), 2420–2422 (2004).
[CrossRef]

Biophys. J. (1)

Y. Chen, J. D. Müller, P. T. C. So, and E. Gratton, “The photon counting histogram in fluorescence fluctuation spectroscopy,” Biophys. J. 77(1), 553–567 (1999).
[CrossRef] [PubMed]

IEEE Trans. Biomed. Eng. (1)

D. Fixler, Y. Namer, Y. Yishay, and M. Deutsch, “Influence of fluorescence anisotropy on fluorescence intensity and lifetime measurement: theory, simulations and experiments,” IEEE Trans. Biomed. Eng. 53(6), 1141–1152 (2006).
[CrossRef] [PubMed]

J. Chem. Phys. (4)

R. A. L. Vallée, T. Rohand, N. Boens, W. Dehaen, G. Hinze, and T. Basché, “Analysis of the exponential character of single molecule rotational correlation functions for large and small fluorescence collection angles,” J. Chem. Phys. 128(15), 154515 (2008).
[CrossRef] [PubMed]

H. Yang and S. Xie, “Probing single-molecule dynamics photon by photon,” J. Chem. Phys. 117(24), 10965–10979 (2002).
[CrossRef]

R. A. L. Vallée, N. Tomczak, G. J. Vancso, L. Kuipers, and N. F. van Hulst, “Fluorescence lifetime fluctuations of single molecules probe local density fluctuations in disordered media: a bulk approach,” J. Chem. Phys. 122(11), 114704 (2005).
[CrossRef] [PubMed]

G. Hinze and T. Basché, “Statistical analysis of time resolved single molecule fluorescence data without time binning,” J. Chem. Phys. 132(4), 044509 (2010).
[CrossRef] [PubMed]

J. Fluoresc. (1)

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