Subdiffusive molecular motion in nanochannels observed by fluorescence correlation spectroscopy.
The influence of confinement on biomolecule motion in glass channels of nanometric height has been investigated with fluorescence correlation spectroscopy (FCS). We measured intrachannel molecule diffusion time and concentration based on a single-component diffusion model as a function of molecule size to channel height (r(g)/h). Poly(ethylene glycol) (PEG) of 20 kDa and dextran of 40 kDa showed a reduction of their diffusion coefficients of almost 1 order of magnitude when nanochannel height approached probe diameter, whereas rhodamine 6G (Rh6G) was shown to be almost unaffected from confinement. Subdiffusive motion has been proven for flexible molecules in nanochannels, and deviations toward a square root dependence of mobility with time for confinement up to molecule size r(g)/h approximately 0.5 were registered. Diffusion coefficient time dependence has been evaluated and described with a model that accounts for diffusion time increase due to molecule rearrangements related to molecule flexibility and surface interactions dynamics. The evaluation of the subdiffusive mode and the key parameters extracted at the single-molecule level of partitioning, intrachannel diffusion time, desorption time, and binding probability at surfaces can be exploited for the engineering of bioanalytic nanodevices.
De Santo
Ilaria
I
Interdisciplinary Research Centre on Biomaterials (CRIB), University Federico II, Piazzale Tecchio 80, 80125, Naples, Italy.
Causa
Filippo
F
Netti
Paolo A
PA
D000327:Adsorption; D003911:Dextrans / Q000737:chemistry; D004058:Diffusion; D005456:Fluorescent Dyes / Q000737:chemistry; D007700:Kinetics; D053761:Nanocomposites / Q000737:chemistry*; D010316:Particle Size; D011092:Polyethylene Glycols / Q000737:chemistry; D012235:Rhodamines / Q000737:chemistry; D013050:Spectrometry, Fluorescence / Q000379:methods*
D003911:Dextrans; D005456:Fluorescent Dyes; D012235:Rhodamines; C026188:rhodamine 6G; D011092:Polyethylene Glycols