One
of the promising approaches to meet the urgent demand for further
device miniaturization is to create functional devices using single
molecules. Although various single-molecule electronic devices have
been demonstrated recently, single-molecule optical devices which
use external stimulations to control the optical response of a single
molecule have rarely been reported. Here, we propose and demonstrate
a field-effect Raman scattering (FERS) device with a single molecule,
an optical counterpart to field-effect transistors (a key component
of modern electronics). With our devices, the gap size between electrodes
can be precisely adjusted at subangstrom accuracy to form single molecular
junctions as well as to reach the maximum performance of Raman scattering
via plasmonic enhancement. Based on this maximum performance, we demonstrated
that the intensity of Raman scattering can be further enhanced by
an additional ∼40% if the orbitals of the molecules bridged
two electrodes were shifted by a gating voltage. This finding not
only provides a method to increase the sensitivity of Raman scattering
beyond the limit of plasmonic enhancement, but also makes it feasible
to realize addressable functional FERS devices with a gate electrode
array.
Supporting Information were incorrect. The corrected and revised Figure S7 and corresponding figure caption are provided.We also provide a complete Supporting Information file that contains the corrected Figure S7 and figure caption.
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