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Ultrafast Excited State Deactivation of Triphenylmethane Dyes†
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Abstract
We have carried out ultrafast pump−probe measurement of four TPM dyes, malachite green (MG), brilliant green (BG), crystal violet (CV), and ethyl violet (EV), with a time resolution of 30 fs. The pump−probe signal showed that solvent dependence arose first in the femtosecond time regime, e.g., the decay of n-butanol solution was clearly slower than the methanol solution just 50 fs after the initial photoexcitation. The signal decays in a multiexponential manner and the slower components showed stronger linear dependence on the solvent viscosity than did the faster components. We have also carried out temperature-dependent measurement of ethanol solution and calculated the activation energies from the Arrhenius plots of each components. The activation energies and effective volumes were larger for slower decays. The activation energy of the viscosity of ethanol was larger than that of the decay components of TPM dyes. These observations are explained with a combined effect of microviscosity and intramolecular relaxation. The lifetime of the transient absorption appearing at the red edge of the ground state absorption was longer than any of the reported lifetimes of the excited state absorption around 400 nm. Therefore, the red-edge absorption is assigned to the unrelaxed ground state molecule with the twisted phenyl group.
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This article has been cited by 15 ACS Journal articles (5 most recent appear below).
Ultrafast Nonradiative Decay of Electronically Excited States of Malachite Green: Ab Initio Calculations
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Akira Nakayama and Tetsuya TaketsuguThe Journal of Physical Chemistry A2011 Article ASAPWe have investigated the nonradiative deactivation process of malachite green in the singlet excited states, S1 and S2, by high-level ab initio quantum chemical calculations using the CASPT2//CASCF approach. The deactivation pathways connecting the Franck–...
Ultrafast Twisting Dynamics in the Excited State of Auramine
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Ultrafast Surface Enhanced Resonance Raman Scattering Detection in Droplet-Based Microfluidic Systems
Michael P. Cecchini, Jongin Hong, Chaesung Lim, Jaebum Choo, Tim Albrecht, Andrew J. deMello, and Joshua B. EdelAnalytical Chemistry2011 83 (8), 3076-3081Ultrafast Surface Enhanced Resonance Raman Scattering Detection in Droplet-Based Microfluidic Systems
Michael P. Cecchini, Jongin Hong, Chaesung Lim, Jaebum Choo, Tim Albrecht, Andrew J. deMello, and Joshua B. EdelAnalytical Chemistry2011 83 (8), 3076-3081The development of ultrafast Raman-based detection is one of the most interesting challenges underpinning the application of droplet-based microfluidics. Herein, we describe the use of surface-enhanced resonance Raman spectroscopy (SERRS) with ...
Microviscosity inside a Nanocavity: A Femtosecond Fluorescence Up-Conversion Study of Malachite Green
Shahnawaz Rafiq, Rajeev Yadav, and Pratik SenThe Journal of Physical Chemistry B2010 114 (44), 13988-13994Microviscosity inside a Nanocavity: A Femtosecond Fluorescence Up-Conversion Study of Malachite Green
Shahnawaz Rafiq, Rajeev Yadav, and Pratik SenThe Journal of Physical Chemistry B2010 114 (44), 13988-13994Femtosecond fluorescence up-conversion measurements of malachite green (MG) have been carried out to confirm the relaxation pathway and subsequently to probe the microviscosity of water trapped in a nanoconfined environment using an AOT (sodium ...
Salt Effect on the Formation of Dye Aggregates at Liquid/Liquid Interfaces Studied by Time-Resolved Surface Second Harmonic Generation
Marina Fedoseeva, Piotr Fita, Angela Punzi and Eric VautheyThe Journal of Physical Chemistry C2010 114 (32), 13774-13781Salt Effect on the Formation of Dye Aggregates at Liquid/Liquid Interfaces Studied by Time-Resolved Surface Second Harmonic Generation
Marina Fedoseeva, Piotr Fita, Angela Punzi and Eric VautheyThe Journal of Physical Chemistry C2010 114 (32), 13774-13781The present study reports on the effect caused by sodium salts added to a solution of malachite green in a liquid/liquid interfacial system probed by the time-resolved surface second harmonic generation (TRSSHG) technique. This effect is known as “salting-...
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History
- Published In Issue March 14, 2002
- Received June 5, 2001
Revised November 1, 2001
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