The linear and nonlinear (chi((2))) optical responses of Langmuir mono
layers of organically functionalized silver quantum dots were measured
as a continuous function of interparticle separation under near-ambie
nt conditions. As the distance between metal surfaces was decreased fr
om 12 to similar to 5 angstroms, both quantum and classical effects we
re observed in the optical signals. When the separation was less than
5 angstroms, the optical second-harmonic generation (SHG) response exh
ibited a sharp discontinuity, and the linear reflectance and absorbanc
e began to resemble those of a thin metallic film, indicating that an
insulator-to-metal transition occurred. This transition was reversible
.