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2015 ; 5
(ä): 14555
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Competition between diagonal and off-diagonal coupling gives rise to
charge-transfer states in polymeric solar cells
#MMPMID26412693
Yao Y
; Zhou N
; Prior J
; Zhao Y
Sci Rep
2015[Sep]; 5
(ä): 14555
PMID26412693
show ga
It has long been a puzzle on what drives charge separation in artificial
polymeric solar cells as a consensus has yet to emerge among rivaling theories
based upon electronic localization and delocalization pictures. Here we propose
an alternative using the two-bath spin-boson model with simultaneous diagonal and
off-diagonal coupling: the critical phase, which is born out of the competition
of the two coupling types, and is neither localized nor delocalized. The
decoherence-free feature of the critical phase also helps explain sustained
coherence of the charge-transfer state. Exploiting Hamiltonian symmetries in an
enhanced algorithm of density-matrix renormalization group, we map out boundaries
of the critical phase to a precision previously unattainable, and determine the
bath spectral densities inducive to the existence of the charge-transfer state.