Document Detail


Spin Dynamics of Radical Pairs with Restricted Geometries and Strong Exchange Coupling: The Role of Hyperfine Coupling.
MedLine Citation:
PMID:  24870373     Owner:  NLM     Status:  Publisher    
Abstract/OtherAbstract:
Sub-nanosecond radical pair formation by electron transfer from an excited singlet state or by bond breaking produces two correlated spins coupled by their spin-spin exchange (J) and magnetic dipole (D) interactions. In the high magnetic field limit, the two-spin system can be described by a singlet state (S) and three triplet states (T0, T+1, T-1). When J is small relative to the electron Zeeman interaction, |T0⟩ is the only triplet state that is populated by coherent spin mixing with the |S⟩ state because the |T+1⟩ and |T-1⟩ are well-separated from |S⟩ by a large energy gap. Herein we describe the spin dynamics for RPs having restricted geometries in which J is similar in magnitude to the electron Zeeman interaction and does not fluctuate significantly. Under these circumstances, depending on the sign of J, the energies of |T+1⟩ or |T-1⟩ are close to that of |S⟩, so that weak isotropic electron-nuclear hyperfine coupling leads to population of |T+1⟩ or |T-1⟩. An approximate relationship for the triplet quantum yield is developed for a RP in the large J regime, where one or both electrons interact with nearby spin-1/2 nuclei. This relationship also yields the net spin polarization transfer to the nuclear spins.
Authors:
Mehdi Zarea; Raanan Carmieli; Mark A Ratner; Michael R Wasielewski
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Publication Detail:
Type:  JOURNAL ARTICLE     Date:  2014-5-28
Journal Detail:
Title:  The journal of physical chemistry. A     Volume:  -     ISSN:  1520-5215     ISO Abbreviation:  J Phys Chem A     Publication Date:  2014 May 
Date Detail:
Created Date:  2014-5-29     Completed Date:  -     Revised Date:  -    
Medline Journal Info:
Nlm Unique ID:  9890903     Medline TA:  J Phys Chem A     Country:  -    
Other Details:
Languages:  ENG     Pagination:  -     Citation Subset:  -    
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