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The residence probability: single molecule fluorescence correlation spectroscopy and reversible geminate
1The Fritz Haber Research Center, Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel. agmon@fh.huji.ac.il
Physical Chemistry Chemical Physics : PCCP
|August 24, 2011
Summary
This study calculates particle residence probability in a sphere, crucial for fluorescence correlation spectroscopy (FCS) analysis. New approximations for near-field scanning optical microscopy (NSOM)-FCS autocorrelation functions (ACF) are presented.
Area of Science:
- Physical Chemistry
- Chemical Physics
- Biophysics
Background:
- Freely diffusing particles in confined spaces are fundamental in various scientific fields.
- Fluorescence Correlation Spectroscopy (FCS) is a powerful technique for studying molecular dynamics.
- Near-field Scanning Optical Microscopy (NSOM) probes offer high spatial resolution for FCS measurements.
Purpose of the Study:
- To calculate the residence probability of a diffusing particle within a d-dimensional ball.
- To develop and validate analytical expressions for autocorrelation functions (ACF) in NSOM-FCS.
- To explore potential applications in two-photon FCS and extract more information from FCS experiments.
Main Methods:
- Laplace transform of residence probability was calculated in Laplace space for general dimensionality.
- Inversion into the time domain was performed for one- and three-dimensional cases.
- Asymptotic behaviors (short- and long-time) were derived and compared with exact results.
Main Results:
- Exact solutions for residence probability in 1D and 3D were obtained.
- New approximations for the two-dimensional ACF in NSOM-FCS were derived.
- An analytic expression for a three-dimensional ACF was provided, relevant for two-photon FCS.
Conclusions:
- The derived approximations enhance the analysis of NSOM-FCS data.
- The findings offer a more detailed understanding of particle diffusion in confined geometries.
- Long-time tails in FCS experiments may contain significant information, analogous to binding probabilities in chemical reactions.
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