BORDAT, Patrice; ORRIT, M.; BROWN, Ross; WÜRGER, Aloïs

doi:10.1016/S0301-0104(00)00173-7

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BORDAT, Patrice
Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux [IPREM]

ORRIT, M.
Centre de physique moléculaire optique et hertzienne [CPMOH]

BROWN, Ross
Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux [IPREM]

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Chemical Physics. 2000, vol. 258, n° 1, p. 63-72

Elsevier

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Single terrylene molecules embedded in a p-terphenyl crystal behave like well-defined optical switches. Recent measurements of the shift of their optical lines under an applied electric field (Stark effect) have revealed surprising anomalies: unexpectedly large and widely spread differences of polarizability between the ground and excited states, even in crystals of excellent quality. Some molecules even had a greater polarizability in the ground than in the excited state. We propose to explain these results by a symmetry breaking in the supermolecule (including the terrylene molecule and the first shells of p-terphenyl neighbours), leading to two distorted conformations with opposite dipole moments. Tunnelling between these conformations gives rise to a quadratic Stark effect with a large effective polarizability. The model is internally consistent, and provides reasonable orders of magnitude for the tunnel barrier. We argue that this tunnelling involves correlated movements of groups of atoms, 1 nm apart, and therefore the system is particularly sensitive to small residual strains in otherwise perfect crystals.< Leer menos

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The anomalous Stark effect of single terrylene molecules in p-terphenyl crystals

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