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Experimental Methods for Spin- and Angle-Resolved Photoemission Spectroscopy Combined with Polarization-Variable Laser
Published on: June 28, 2018
Theoretical study of dynamic electron-spin-polarization via the doublet-quartet quantum-mixed state (II). Population
Takafumi Matsumoto1, Yoshio Teki
1Division of Molecular Material Science, Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585, Japan.
Abstract:
The population transfer to the spin-sublevels of the unique quartet (S = 3/2) high-spin state of the strongly exchange-coupled (SC) radical-triplet pair (for example, an Acceptor-Donor-Radical triad (A-D-R)) via a doublet-quartet quantum-mixed (QM) state is theoretically investigated by a stochastic Liouville equation. In this work, we have treated the loss of the quantum coherence (de-coherence) due to the de-phasing during the population transfer and neglected the effect of other de-coherence mechanisms. The dependences on the magnitude of the exchange coupling or the fine-structure parameter of the QM state are investigated. The dependence on the velocity of the population transfer (by the electron transfer or the energy-transfer) from the QM state to the SC quartet state is also clarified. It is revealed that the de-coherence during the population transfer mainly originates from the fine-structure term of the QM state in the doublet-triplet exchange coupled systems. This de-coherence leads to the unique dynamic electron polarization (DEP) on the high-field spin sublevels of the SC state, which is similar to the unique DEP pattern of the photo-excited triplet states of the reaction centers of photosystems I and II. The magnetic field dependence of the population transfer leading to the populations of the spin-sublevels of the SC states is also calculated. The possibility of the control of energy transport, spin transport and information technology by using the QM state is discussed based on these results. The knowledge obtained in this work is useful in the spin dynamics of any doublet-triplet exchange coupled systems.
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