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The Journal of Chemical Physics

Influence of Resonance Transfer on Luminescence Decay

Kenneth B. Eisenthal, Seymour Siegel

Published Aug 1, 1964• 206 citations
Publisher

Abstract

The effects of dipole—dipole resonance transfer on the population and decay of excited donor molecules are discussed. The limitation of the previous treatments of this problem to flash excitation is demonstrated. The present treatment is applicable to systems which have achieved a steady state or have been flashed. Expressions are given for the donor quantum yields, the decay of excited donor molecules for flashed and steady-state systems, and the steady-state population of excited donor molecules.

DOI
10.1063/1.1725941

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The effects of dipole—dipole resonance transfer on the population and decay of excited donor molecules are discussed. The limitation of the previous treatments of this problem to flash excitation is demonstrated. The present treatment is applicable to systems which have achieved a steady state or have been flashed. Expressions are given for the donor quantum yields, the decay of excited donor molecules for flashed and steady-state systems, and the steady-state population of excited donor molecules.
The dynamic quenching of dual fluorescence is simulated based on solving a system of equations for matrix elements of the statistical operator of a five-level model molecule three levels of which belong to its excited states. It is assumed that one of the excited states is resonantly populated by monochromatic irradiation, while the other two states are populated as a result of subsequent relaxation processes. These two states are initial states for transitions that emit dual fluorescence photons. Expressions for the population of the excited molecular states in the case of steady-state fluorescence are obtained taking into account their decay (quenching) due to collisions with foreign molecules of the environment. As applied to molecules with intramolecular hydrogen bonds, the dual fluorescence quenching is described more completely and in more detail compared to the description given in the literature based on the molecular model with two excited levels.
The two-photon transitions of a system of two dissimilar molecules are studied in the dipole approximation. Special attention is paid to transitions in which both molecules participate simultaneously. By use of a reduced Hamiltonian the influence of long-range intermolecular forces is also studied. The three main transitions considered occur when: (i) no molecular level is in resonance with a primary photon, (ii) one primary photon excites a molecular level, and (iii) two primary photons excite a molecular level. It is shown that in no case can the mixing of excited states by intermolecular forces be represented as a change to an effective transition dipole moment for one of the molecules. The one-photon decay of a state in which both molecules are excited is also treated.
The influence of excited-state absorption (ESA) and two-exciton processes on a coherent population transfer with intense ultrashort chirped pulses in molecular systems in solution has been studied. A unified treatment of adiabatic rapid passage (ARP) in such systems has been developed using a three-state electronic system with relaxation treated as a diffusion on electronic potential energy surfaces. We have shown that ESA has a profound effect on coherent population transfer in large molecules that necessitates a more accurate interpretation of experimental data. A simple and physically clear model for ARP in molecules with three electronic states in solution has been developed by extending the Landau-Zener calculations putting in a third level to random crossing of levels. A method for quantum control of two-exciton states in molecular complexes has been proposed. 1.
A theoretical treatment of the relaxation and transfer of atomic multipole moments due to interatomic collisions is presented, applicable to systems of emitters and perturbers with any angular momenta. Expressions are obtained for the rate constants, within the impact approximation, in terms of the elements of the scattering matrix evaluated as a function of impact parameter for an emitter-perturber collision. Processes in which the total electronic excitation energy is not conserved are excluded and collisions are assumed to occur isotropically. Explicit evaluation of rate constants has been carried out using the first-order dipole-dipole (resonance) interaction, assuming the classical straight line path approximation. Four special cases have been treated by numerical integration of the Schrodinger equation in the interaction representation. These are: J g (ground state angular momentum)=0, J e (excited state)=1; j g = 1 / 2 , J e = 1 / 2 ; J g = 1 / 2 , J e = 3 / 2 ; J g =1, J e =1. The ( 1 / 2 , 1 / 2 ) rate constants are shown to be simply related to those for the (0, 1) case. Within the context of the various approximations, numerical accuracy is expected to be better than 1%.
We study coherent energy transfer of a single excitation and quantum entanglement in a dimer, which consists of a donor and an acceptor modeled by two two-level systems. Between the donor and the acceptor, there exists a dipole-dipole interaction, which provides the physical mechanism for coherent energy transfer and entanglement generation. The donor and the acceptor couple to two independent heat baths with diagonal couplings that do not dissipate the energy of the noncoupling dimer. Special attention is paid to the effect on single-excitation energy transfer and entanglement generation of the energy detuning between the donor and the acceptor and the temperatures of the two heat baths. It is found that, the probability for single-excitation energy transfer largely depends on the energy detuning in the low temperature limit. Concretely, the positive and negative energy detunings can increase and decrease the probability at steady state, respectively. In the high temperature limit, however, the effect of the energy detuning on the probability is negligibly small. We also find that the probability is negligibly dependent on the bath temperature difference of the two heat baths. In addition, it is found that quantum entanglement can be generated in the process of coherent energy transfer. As the bath temperature increases, the generated steady-state entanglement decreases. For a given bath temperature, the steady-state entanglement decreases with the increase of the absolute value of the energy detuning.