Electronic energy relaxation and transition frequency jumps of single molecules at 30 mK - art. no. 015504

Transition frequency jumps for single terrylene molecules in a polyethylene matrix caused by resonant laser irradiation are investigated at 30 mK. The se jumps are not accompanied by substantial sample heating. A model for the effect is: proposed, based on the interaction of tunneling two-level syste ms (TLSs) surrounding the single molecule with high-energy nonthermal phono ns emitted by the molecule during electronic energy relaxation. The radius of the effective interaction volume is estimated to be r(m) approximate to 12.5 nm, and the interaction cross section for nonequilibrium phonon -TLS s cattering is estimated as similar to 10(-22) cm(-2).