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We consider several fundamental optical phenomena involving single moleculesin biased metal-molecule-metal junctions. The molecule is represented by itshighest occupied and lowest unoccupied molecular orbitals, and the analysisinvolves the simultaneous consideration of three coupled fluxes: the electroniccurrent through the molecule, energy flow between the molecule andelectron-hole excitations in the leads and the incident and/or emitted photonflux. Using a unified theoretical approach based on the non-equilibrium Greenfunction method we derive expressions for the absorption lineshape (not anobservable but a ueful reference for considering yields of other opticalprocesses) and for the current induced molecular emission in such junctions. Wealso consider conditions under which resonance radiation can induce electroniccurrent in an unbiased junction. We find that current driven molecular emissionand resonant light induced electronic currents in single molecule junctions canbe of observable magnitude under appropriate realizable conditions. Inparticular, light induced current should be observed in junctions involvingmolecular bridges that are characterized by strong charge transfer opticaltransitions. For observing current induced molecular emission we find that inaddition to the familiar need to control the damping of molecular excitationsinto the metal substrate the phenomenon is also sensitive to the way in whichthe potential bias si distributed on the junction.Comment: 56 pages, 8 figures; submitted to JC

Optical properties of current carrying molecular wires