On-the-Fly Femtosecond Action Spectroscopy of Charged Cyanine Dyes: Electronic Structure versus Geometry - Archive ouverte HAL Access content directly
Journal Articles Journal of Physical Chemistry Letters Year : 2019

On-the-Fly Femtosecond Action Spectroscopy of Charged Cyanine Dyes: Electronic Structure versus Geometry

Abstract

Understanding optical properties of molecular dyes is required to drive progress in molecular photonics. This requires a fundamental comprehension of the role of electronic structure, geometry, and interactions with the environment in order to guide molecular engineering strategies. In this context, we studied charged cyanine dye molecules in the gas phase with a controlled microenvironment to unravel the origin of the spectral tuning of this class of molecules. This was performed using a new approach combining femtosecond multiple-photon action spectroscopy of on-the-fly mass-selected molecular ions and high-level quantum calculations. While arguments based on molecular geometry are often used to design new polymethine dyes, we provide experimental evidence that electronic structure is of primary importance and hence the decisive criterion as suggested by recent theoretical investigations.
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hal-02364934 , version 1 (15-11-2019)

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Marius Hervé, Richard Bredy, Gabriel Karras, Bruno Concina, Jeffery Brown, et al.. On-the-Fly Femtosecond Action Spectroscopy of Charged Cyanine Dyes: Electronic Structure versus Geometry. Journal of Physical Chemistry Letters, 2019, 10 (9), pp.2300-2305. ⟨10.1021/acs.jpclett.9b00435⟩. ⟨hal-02364934⟩
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