Abstract
A strong increase of second-order nonlinear optical signal intensity due to electromagnetic field enhancement, in combination with femtosecond nonlinear optical pump–probe techniques facilitates measuring relaxation time constants τ r in large Na n ( n≈10 5–10 7) clusters, bound to insulator surfaces. Time constants of τ r≈1.8 ps for Na n clusters on mica and τ r≈1.1 ps for Na clusters on lithium fluoride are found. The difference is attributed to either morphological changes or the different thermal properties of the substrates. The subpicosecond-part of the time-resolved response is seen to be dominated by the field-enhancement effect, but is otherwise independent of cluster size for mean radii between 12 and 100 nm.
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