Comparison of the Smoluchowski approach with modern alternative approaches to diffusion-influenced fluorescence quenching: The effect of intense excitation pulses

Naumann, W.; Szabó, Attila

doi:10.1063/1.474401

Cited by 40 publications

(22 citation statements)

References 16 publications

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“…Within these activities, the effect of the excitation pulse shape and intensity on the fluorescence yield has also been investigated. 17,18 To understand the effect of a unimolecular back reaction on the quenching yield, in a recent paper 10 we investigated the kinetics of fluorescence quenching by reversible excimer formation on the basis of non-Markovian rate equations obtained in a many-particle approach. Under the assumption that excimer formation and dissociation occurs via contact events, or by longer-range reactions which obey the principle of detailed balance, exact analytic expressions could be derived for the rate kernels in the low-density limit.…”

Section: Introductionmentioning

confidence: 99%

Fluorescence quenching by reversible excimer formation: Kinetics and yield predictions for a classical potential association–dissociation model

Naumann

2004

The Journal of Chemical Physics

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Fluorescence quenching by reversible excimer formation is studied on the assumption that excimer formation and dissociation can be modelled as entering and leaving the attractive region of an monomer excited-monomer interaction potential by diffusion. To get some general insight in the kinetic consequences of such a type of modelling, the simple case of an attractive square-well potential is investigated. It is shown that three different kinetic regimes have to be distinguished: Two "reversible" ones in case of slow excimer radiative decay, in which the quenching kinetics can be formulated by Markovian or non-Markovian rate equations with both excimer formation and excimer dissociation terms, and an effectively "irreversible" regime if the excimer radiative decay is too rapid to allow the excimer equilibration. In the latter case a dissociation coefficient can no longer be defined and the quenching kinetics can only be predicted on the basis of generalized rate equations of a net-excimer-formation type. It is shown how the quenching constant formula must be generalized to be applicable in all kinetic situations.

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Section: Introductionmentioning

confidence: 99%

Fluorescence quenching by reversible excimer formation: Kinetics and yield predictions for a classical potential association–dissociation model

Naumann

2004

The Journal of Chemical Physics

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“…However, close similarity of channel extraction and superposition decoupling takes place only for the simplest reaction A + B → C + B in spatially homogeneous reacting systems. Any complication of the system makes the superposition approximation unsuitable [57,58] and essentially different from EPA. For the reaction under study the above channel extraction gives the equation for two-particle correlation pattern π 1,1,0 (A 1 , B 1 , t) …”

Section: Equations For Two-particle Cp In Epamentioning

confidence: 99%

Influence of the force interaction on accumulation of macroscopic correlations in elementary reaction A + B → C

2012

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The applicability of the Encounter Theory (ET) (the prototype of the Collision Theory) concepts for widely occurring diffusion assisted irreversible bulk reaction A + B → C (for example, radical reaction) in dilute solutions taking account of initial microscopic correlations and force interactions between reactants has been treated theoretically with modern many-particle method for the derivation of nonMarkovian binary kinetic equations. The method shows that taking into consideration initial correlations and force interactions leads to the redefinition of the Markovian rate constant only in the expressions derived earlier. Thus, just as in the reaction A + A → C and the reaction A + B → C neglecting force and initial correlations, the Modified Encounter Theory (MET), when reduced to equations of a Regular Form, both extends the time applicability range of ET homogeneous rate equation, and yields the inhomogeneous equation of the Generalized Encounter Theory (GET). It reveals macroscopic correlations induced by the encounters in the reservoir of free walks in full agreement with physical considerations. Time accumulation of macroscopic correlations obeys the same time law as in the previously considered case neglecting force interactions. Just the rate of the process will change, according to traditional redefinition of the steady-state constant of the reaction.

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“…This is emphasized because the SA is widely considered, regardless of the reaction scheme, to describe the dynamics of a static reactant and independently diffusing B's based on the result of irreversible reaction kinetics. 42 In contrast with the SA, the present theory implements the molecular history effects properly as discussed in Sec. II.…”

Section: ͑414͒mentioning

confidence: 99%

Kinetic theory of bimolecular reactions in liquid. III. Reversible association–dissociation: A+B⇄C

Yang

Lee

Shin

1998

The Journal of Chemical Physics

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Articles you may be interested inWater-gas-shift reaction on metal nanoparticles and surfacesThe integral encounter theory of multistage reactions containing association-dissociation reaction stages. III. Taking account of quantum states of reactants A theoretical formalism based on the fully renormalized kinetic theory is applied to a diffusion-influenced pseudo-first order reaction kinetics of reversible association-dissociation A ϩB C including unimolecular decay processes. Linear response of the system, initially at equilibrium, to a thermal perturbation is examined and a rate kernel equation for the reactant concentrations is derived. The rate kernel has a hierarchical structure and the propagator appeared in the kernel expression is truncated by a disconnected approximation. When the unimolecular reactions are turned off, the response of the system not only shows the long-time power law of t Ϫ3/2 but also displays the proper behavior over the whole time region in accordance with previous computer simulation results. Moreover, it is shown that the amplitude of the long-time behavior predicted by previous workers is modified by a certain correction factor P which contains dynamical correlation effects. In this way, many-body complication inherent to the history of reactive pair creation is properly implemented in the description of the reversible kinetics. We compare the present theory with the other existing theories such as the rate equation, the superposition approximation, and the convolution approaches. In some limiting cases, results obtained from the present theory can be reduced to those from the existing theories.

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Comparison of the Smoluchowski approach with modern alternative approaches to diffusion-influenced fluorescence quenching: The effect of intense excitation pulses

Cited by 40 publications

References 16 publications

Fluorescence quenching by reversible excimer formation: Kinetics and yield predictions for a classical potential association–dissociation model

Fluorescence quenching by reversible excimer formation: Kinetics and yield predictions for a classical potential association–dissociation model

Influence of the force interaction on accumulation of macroscopic correlations in elementary reaction A + B → C

Kinetic theory of bimolecular reactions in liquid. III. Reversible association–dissociation: A+B⇄C

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