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Within a generic model we analyze the Stokes linewidth in surface enhancedRaman scattering (SERS) from molecules embedded as bridges in molecularjunctions. We identify four main contributions to the off-resonant Stokessignal and show that under zero voltage bias (a situation pertaining also tostandard SERS experiments) and at low bias junctions only one of thesecontributions is pronounced. The linewidth of this component is determined bythe molecular vibrational relaxation rate, which is dominated by interactionswith the essentially bosonic thermal environment when the relevant molecularelectronic energy is far from the metal(s) Fermi energy(ies). It increases whenthe molecular electronic level is close to the metal Fermi level so that anadditional vibrational relaxation channel due to electron-hole (eh) excition inthe molecule opens. Other contributions to the Raman signal, of considerablybroader linewidths, can become important at larger junction bias.

On the widths of Stokes lines in Raman scattering from molecules adsorbed at metal surfaces and in molecular conduction junctions