☆ 4.6 Article

Aggregates of quadrupolar dyes for two-photon absorption: the role of intermolecular interactions

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2016)

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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 18, 期 40, 页码 28198-28208

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ROYAL SOC CHEMISTRY
DOI: 10.1039/c6cp05153g

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Chemistry, Physical Physics, Atomic, Molecular & Chemical

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  1. People Programme (Marie Curie Actions) of the European Union's Seventh Framework Programme FP7 under REA grant [607721]
  2. Italian MIUR [PRIN2012T9XHH7_002]
  3. CINECA [IsC35_MMMOptic]

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We present a theoretical investigation of small aggregates of quadrupolar (A-pi-D-pi-A or D-pi-A-pi-D) charge-transfer dyes, with attention focused on the role of intermolecular interactions in determining their optical properties. We tackle the theoretical issue by adopting essential-state models (ESMs), which describe an isolated molecule in terms of a minimal number of electronic states, corresponding to the resonance structures. ESMs quite naturally describe intermolecular interactions relaxing the dipolar approximation and accounting for molecular polarizabilities. The approach is applied to curcuminoid and squaraine dyes, two families of chromophores with weak and strong quadrupolar character, respectively. The method is validated against experiment and for curcuminoids also against time-dependent density functional theory. ESMs rationalize the strong ultra-excitonic effects recurrently observed in the experimental optical spectra of aggregates of highly polarizable quadrupolar dyes, offering a valuable tool to exploit the supramolecular design of material properties.

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