1,064 research outputs found
Current induced light emission and light induced current in molecular tunneling junctions
The interaction of metal-molecule-metal junctions with light is considered
within a simple generic model. We show, for the first time, that light induced
current in unbiased junctions can take place when the bridging molecule is
characterized by a strong charge-transfer transition. The same model shows
current induced light emission under potential bias that exceeds the molecular
excitation energy. Results based on realistic estimates of molecular-lead
coupling and molecule-radiation field interaction suggest that both effects
should be observable.Comment: 5 pages, 3 figures, RevTeX
Observation and analysis of Fano-like lineshapes in the Raman spectra of molecules adsorbed at metal interfaces
Surface enhanced Raman spectra from molecules (bipyridyl ethylene) adsorbed
on gold dumbells are observed to become increasingly asymmetric (Fano-like) at
higher incident light intensity. The electronic temperature (inferred from the
anti-Stokes (AS) electronic Raman signal increases at the same time while no
vibrational AS scattering is seen. These observations are analyzed by assuming
that the molecule-metal coupling contains an intensity dependent contribution
(resulting from light-induced charge transfer transitions as well as
renormalization of the molecule metal tunneling barrier). We find that
interference between vibrational and electronic inelastic scattering routes is
possible in the presence of strong enough electron-vibrational coupling and can
in principle lead to the observed Fano-like feature in the Raman scattering
profile. However the best fit to the observed results, including the dependence
on incident light intensity and the associated thermal response is obtained
from a model that disregards this coupling and accounts for the structure of
the continuous electronic component of the Raman scattering signal. The
temperatures inferred from the Raman signal are argued to be only of
qualitative value.Comment: 20 pages, 12 figure
Kubo-Anderson theory of polariton lineshape
We apply the Kubo-Anderson stochastic theory of molecular spectral lineshape
to the case of polaritons formed in the collective strong coupling regime. We
investigate both the fast and slow limits of the random frequency modulation of
the emitter as well as the intermediate regime and show how the interplay
between the characteristic timescales of the cavity and the molecular disorder
is expressed in the observed polaritons lineshapes. The analytical solution
obtained for the slow limit is valid for any ratio between the inhomogeneous
broadening of the molecules and the Rabi splitting, especially relevant for
molecular polaritons where these two quantities can be of the same order of
magnitude
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