ANALYSIS OF SIMULATED DIFFUSION AND ADSORPTION WITH AN ANALYTICAL MODEL FOR FLUORESCENCE CORRELATION SPECTROSCOPY
Keywords:
confocal microscopy;, computer simulation;, Monte Carlo simulation;, FCS;
Abstract
Fluorescence correlation spectroscopy (FCS) is a powerful tool to predict molecular diffusivity in femtoliter observation volume. The applicable analytical model in 3-D for porous chromatographic environment has been introduced to evaluate in this contribution. Regarding chromatographic environment, it is important to understand and characterize both diffusion and adsorption-desorption kinetics at interfacial area between mobile and stationary phases. In this contribution, a demonstration of a newly designed analytical model for FCS was presented that can predict simulated diffusion and adsorption-desorption kinetics in 3-D matrix. This work was motivated by a previous 2-D analytical solution study. The range of desorption rate (800–1000 1/s) was found to be where the analytical model can predict the molecular dynamics most accurately and precisely.
References
1. Magde, D., E. Elson, and W.W. Webb, Thermodynamic Fluctuations in a Reacting System---Measurement by Fluorescence Correlation Spectroscopy. Physical Review Letters, 1972. 29(11): p. 705-708.
2. Magde, D., E.L. Elson, and W.W. Webb, Fluorescence correlation spectroscopy. II. An experimental realization. Biopolymers, 1974. 13(1): p. 29-61.
3. Elson, E.L. and D. Magde, Fluorescence correlation spectroscopy. I. Conceptual basis and theory. Biopolymers, 1974. 13(1): p. 1-27.
4. Hansen, R.L. and J.M. Harris, Measuring Reversible Adsorption Kinetics of Small Molecules at Solid/Liquid Interfaces by Total Internal Reflection Fluorescence Correlation Spectroscopy. Analytical Chemistry, 1998. 70(20): p. 4247-4256.
5. Elson, E.L., Fluorescence correlation spectroscopy: past, present, future. Biophys J, 2011. 101(12): p. 2855-70.
6. Haustein, E. and P. Schwille, Fluorescence correlation spectroscopy: novel variations of an established technique. Annu Rev Biophys Biomol Struct, 2007. 36: p. 151-69.
7. Yu, L., et al., A Comprehensive Review of Fluorescence Correlation Spectroscopy. Frontiers in Physics, 2021. 9.
8. Banks, D.S., et al., Characterizing anomalous diffusion in crowded polymer solutions and gels over five decades in time with variable-lengthscale fluorescence correlation spectroscopy. Soft Matter, 2016. 12(18): p. 4190-203.
9. Jazani, S., et al., An alternative framework for fluorescence correlation spectroscopy. Nat Commun, 2019. 10(1): p. 3662.
10. Neuweiler, H., et al., Dynamics of unfolded polypeptide chains in crowded environment studied by fluorescence correlation spectroscopy. J Mol Biol, 2007. 365(3): p. 856-69.
11. Lee, H.B., et al., Rotational and translational diffusion of size-dependent fluorescent probes in homogeneous and heterogeneous environments. Phys Chem Chem Phys, 2018. 20(37): p. 24045-24057.
12. National Academies of Sciences, E. and Medicine, A Research Agenda for Transforming Separation Science. 2019, Washington, DC: The National Academies Press. 114.
13. Wirth, M.J. and M.A. Legg, Single-molecule probing of adsorption and diffusion on silica surfaces. Annu Rev Phys Chem, 2007. 58: p. 489-510.
14. Wirth, M.J., M.D. Ludes, and D.J. Swinton, Spectroscopic Observation of Adsorption to Active Silanols. Analytical Chemistry, 1999. 71(18): p. 3911-3917.
15. Gritti, F. and G. Guiochon, Mass transfer kinetics, band broadening and column efficiency. J Chromatogr A, 2012. 1221: p. 2-40.
16. Gritti, F. and G. Guiochon, Influence of the degree of coverage of C18-bonded stationary phases on the mass transfer mechanism and its kinetics. J Chromatogr A, 2006. 1128(1-2): p. 45-60.
17. Ries, J. and P. Schwille, Fluorescence correlation spectroscopy. Bioessays, 2012. 34(5): p. 361-8.
18. Ries, J., E.P. Petrov, and P. Schwille, Total internal reflection fluorescence correlation spectroscopy: effects of lateral diffusion and surface-generated fluorescence. Biophys J, 2008. 95(1): p. 390-9.
19. Petrasek, Z. and P. Schwille, Precise measurement of diffusion coefficients using scanning fluorescence correlation spectroscopy. Biophys J, 2008. 94(4): p. 1437-48.
20. Zhong, Z., et al., Probing strong adsorption of solute onto C18-silica gel by fluorescence correlation imaging and single-molecule spectroscopy under RPLC conditions. Anal Chem, 2005. 77(8): p. 2303-10.
21. Lee, H., ; Geng, M. L., Imaging diffusion and adsorption in chromatographic nanoporous silica particles with fluorescence correlation spectroscopy. Submitted to ACS Measurement Science Au, 2023.
22. Wirth, M.J., M.D. Ludes, and D.J. Swinton, Analytic Solution to the Autocorrelation Function for Lateral Diffusion and Rare Strong Adsorption. Applied Spectroscopy, 2001. 55(6): p. 663-669.
23. Aragón, S.R. and R. Pecora, Fluorescence correlation spectroscopy as a probe of molecular dynamics. The Journal of Chemical Physics, 1976. 64(4): p. 1791-1803.
24. Eigen, M. and R. Rigler, Sorting single molecules: application to diagnostics and evolutionary biotechnology. Proc Natl Acad Sci U S A, 1994. 91(13): p. 5740-7.
25. Ries, J., et al., A comprehensive framework for fluorescence cross-correlation spectroscopy. New Journal of Physics, 2010. 12(11): p. 113009.
2. Magde, D., E.L. Elson, and W.W. Webb, Fluorescence correlation spectroscopy. II. An experimental realization. Biopolymers, 1974. 13(1): p. 29-61.
3. Elson, E.L. and D. Magde, Fluorescence correlation spectroscopy. I. Conceptual basis and theory. Biopolymers, 1974. 13(1): p. 1-27.
4. Hansen, R.L. and J.M. Harris, Measuring Reversible Adsorption Kinetics of Small Molecules at Solid/Liquid Interfaces by Total Internal Reflection Fluorescence Correlation Spectroscopy. Analytical Chemistry, 1998. 70(20): p. 4247-4256.
5. Elson, E.L., Fluorescence correlation spectroscopy: past, present, future. Biophys J, 2011. 101(12): p. 2855-70.
6. Haustein, E. and P. Schwille, Fluorescence correlation spectroscopy: novel variations of an established technique. Annu Rev Biophys Biomol Struct, 2007. 36: p. 151-69.
7. Yu, L., et al., A Comprehensive Review of Fluorescence Correlation Spectroscopy. Frontiers in Physics, 2021. 9.
8. Banks, D.S., et al., Characterizing anomalous diffusion in crowded polymer solutions and gels over five decades in time with variable-lengthscale fluorescence correlation spectroscopy. Soft Matter, 2016. 12(18): p. 4190-203.
9. Jazani, S., et al., An alternative framework for fluorescence correlation spectroscopy. Nat Commun, 2019. 10(1): p. 3662.
10. Neuweiler, H., et al., Dynamics of unfolded polypeptide chains in crowded environment studied by fluorescence correlation spectroscopy. J Mol Biol, 2007. 365(3): p. 856-69.
11. Lee, H.B., et al., Rotational and translational diffusion of size-dependent fluorescent probes in homogeneous and heterogeneous environments. Phys Chem Chem Phys, 2018. 20(37): p. 24045-24057.
12. National Academies of Sciences, E. and Medicine, A Research Agenda for Transforming Separation Science. 2019, Washington, DC: The National Academies Press. 114.
13. Wirth, M.J. and M.A. Legg, Single-molecule probing of adsorption and diffusion on silica surfaces. Annu Rev Phys Chem, 2007. 58: p. 489-510.
14. Wirth, M.J., M.D. Ludes, and D.J. Swinton, Spectroscopic Observation of Adsorption to Active Silanols. Analytical Chemistry, 1999. 71(18): p. 3911-3917.
15. Gritti, F. and G. Guiochon, Mass transfer kinetics, band broadening and column efficiency. J Chromatogr A, 2012. 1221: p. 2-40.
16. Gritti, F. and G. Guiochon, Influence of the degree of coverage of C18-bonded stationary phases on the mass transfer mechanism and its kinetics. J Chromatogr A, 2006. 1128(1-2): p. 45-60.
17. Ries, J. and P. Schwille, Fluorescence correlation spectroscopy. Bioessays, 2012. 34(5): p. 361-8.
18. Ries, J., E.P. Petrov, and P. Schwille, Total internal reflection fluorescence correlation spectroscopy: effects of lateral diffusion and surface-generated fluorescence. Biophys J, 2008. 95(1): p. 390-9.
19. Petrasek, Z. and P. Schwille, Precise measurement of diffusion coefficients using scanning fluorescence correlation spectroscopy. Biophys J, 2008. 94(4): p. 1437-48.
20. Zhong, Z., et al., Probing strong adsorption of solute onto C18-silica gel by fluorescence correlation imaging and single-molecule spectroscopy under RPLC conditions. Anal Chem, 2005. 77(8): p. 2303-10.
21. Lee, H., ; Geng, M. L., Imaging diffusion and adsorption in chromatographic nanoporous silica particles with fluorescence correlation spectroscopy. Submitted to ACS Measurement Science Au, 2023.
22. Wirth, M.J., M.D. Ludes, and D.J. Swinton, Analytic Solution to the Autocorrelation Function for Lateral Diffusion and Rare Strong Adsorption. Applied Spectroscopy, 2001. 55(6): p. 663-669.
23. Aragón, S.R. and R. Pecora, Fluorescence correlation spectroscopy as a probe of molecular dynamics. The Journal of Chemical Physics, 1976. 64(4): p. 1791-1803.
24. Eigen, M. and R. Rigler, Sorting single molecules: application to diagnostics and evolutionary biotechnology. Proc Natl Acad Sci U S A, 1994. 91(13): p. 5740-7.
25. Ries, J., et al., A comprehensive framework for fluorescence cross-correlation spectroscopy. New Journal of Physics, 2010. 12(11): p. 113009.
