2014
DOI: 10.1063/1.4870937
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Effects of excluded volume and correlated molecular orientations on Förster resonance energy transfer in liquid water

Abstract: Förster theory for the survival probability of excited chromophores is generalized to include the effects of excluded volume and orientation correlation in the molecular distribution. An analytical expression for survival probability was derived and written in terms of a few simple elementary functions. Because of the excluded volume, the survival probability exhibits exponential decay at early times and stretched exponential decay at later times. Experimental schemes to determine the size of the molecular exc… Show more

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Cited by 2 publications
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“…For longer times when ( r 0 / a ) 6 τ ≫ 1, eq reduces to I HS (τ; a ) → I F (τ) – ρ n ( a / r 0 ) n /λ, which corresponds to the Förster theory description with an additional pre-exponential factor, e ρ n ( a / r 0 ) n /λ . The kinetic transition from an exponential to a stretched exponential behavior has been discussed by Tcherkasskaya et al and also recently by us Figure compares the survival probabilities as they decay due to the vibrational FRET; the kinetic transition behavior is clearly seen.…”
Section: Excluded Volume Effectmentioning
confidence: 63%
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“…For longer times when ( r 0 / a ) 6 τ ≫ 1, eq reduces to I HS (τ; a ) → I F (τ) – ρ n ( a / r 0 ) n /λ, which corresponds to the Förster theory description with an additional pre-exponential factor, e ρ n ( a / r 0 ) n /λ . The kinetic transition from an exponential to a stretched exponential behavior has been discussed by Tcherkasskaya et al and also recently by us Figure compares the survival probabilities as they decay due to the vibrational FRET; the kinetic transition behavior is clearly seen.…”
Section: Excluded Volume Effectmentioning
confidence: 63%
“…Within the dipole–dipole coupling mechanism, the intermolecular VET rate constant averaged over the pairs of two randomly oriented bonds separated by a distance r is given by the Förster formula where τ 0 is the intrinsic vibrational lifetime of excited OH bonds and r 0 is so-called Förster radius. In the bulk phase of liquid water, the values of the two parameters were, respectively, experimentally measured to be τ 0 = 250 fs and theoretically calculated , to be r 0 = 1.73 Å. The lifetime and Förster radius are the parameters specifically depending on the conditions under which water molecules are placed.…”
Section: Förster Theorymentioning
confidence: 99%
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