The transition from localized to collective electronic states in a silver quantum dots monolayer examined by nonlinear optical response

F. Remacle, C. P. Collier, J. R. Heath, R. D. Levine

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Abstract

The optical second-harmonic response of a finite hexagonal lattice is computed as a function of the inter particle separation. In agreement with experiments on Langmuir monolayers of silver quantum dots, the computed response exhibits a peak due to a transition from localized electronic states to a band-like structure. The localization is due to the fluctuations in the particle size and position. For a perfect lattice the variation of the nonlinear response with the inter particle separation is qualitatively different. The role of the symmetry breaking is demonstrated at the tight binding level of electronic structure computations.

Original languageEnglish
Pages (from-to)453-458
Number of pages6
JournalChemical Physics Letters
Volume291
Issue number3-4
DOIs
StatePublished - Jul 17 1998
Externally publishedYes

Funding

We thank Professor S. Efrima for discussions. FR is Chercheur Qualifié, FNRS, Belgium. This work was partly supported by the James Franck program (FR and RDL) and NSF-National Young Investigator program and ONR order N00014-95-F-0099 (JRH) and used the computational facilities of UCLA and of SFB 377.

FundersFunder number
NSF-National
Office of Naval ResearchN00014-95-F-0099
University of California, Los AngelesSFB 377

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