The controlled manipulation and switching of single atoms and molecule
s raise the prospect of ultra-high-density data storage, Switching by
motion of a single atom has been reported(1), and techniques of single
-molecule optical detection and spectroscopy(2) in the condensed phase
have been refined to a degree that allows the modification of the abs
orption properties of a single chromophore(3). Light-induced jumps in
single-molecule excitation frequencies have been reported(3-5), but in
none of these cases could the process be controlled: the jumps varied
from molecule to molecule, they were interrupted by spontaneous jumps
, and the new excitation frequencies could not be identified unambiguo
usly, Here we report light-induced reversible frequency jumps of singl
e molecules of the aromatic hydrocarbon terrylene embedded in a partic
ular site of a p-terphenyl host crystal(6) at temperatures of around 2
K. The changes in absorption frequency for different terrylene molecu
les were identical (within 0.5%) for all samples studied, Thus we were
able to switch single-molecule absorption lines in a controlled way b
etween well-defined frequency positions.