Ultrafast investigations of vibrationally hot molecules after internal conversion in solution

Wild, Wolfgang; Seilmeier, A.; Gottfried, N.H.; Kaiser, W.

doi:10.1016/0009-2614(85)80413-9

Cited by 84 publications

(51 citation statements)

References 16 publications

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“…[1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19] An improved knowledge of relevant photophysical processes may result in additional discoveries, leading to the availability of more efficient laser dyes covering the entire spectral range.…”

Section: Introductionmentioning

confidence: 99%

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Ultrafast Vibrational and Thermal Relaxation of Dye Molecules in Solutions

et al. 2003

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Intra-and intermolecular relaxations of dye molecules are studied after the excitation to the high-lying excited states by a femtosecond laser pulse, using femtosecond time-resolved stimulated emission pumping fluorescence depletion spectroscopy (FS TR SEP FD). The biexponential decays indicate a rapid intramolecular vibrational redistribution (IVR) depopulation followed by a slower process, which was contributed by the energy transfer to the solvents and the solvation of the excited solutes. The time constants of IVR in both oxazine 750 and rhodamine 700 are at the 290-360 fs range, which are insensitive to the characters of solvents. The solvation of the excited solutes and the cooling of the hot solute molecules by collisional energy transfer to the surrounding takes place in the several picoseconds that strongly depend on the properties of solvents. The difference of Lewis basicity and states density of solvents is a possible reason to explain this solvent dependence. The more basic the solvent is, which means the more interaction between the solute and the neighboring solvent shell, the more rapid the intermolecular vibrational excess energy transfer from the solute to the surroundings and the solvation of the solutes are. The higher the states density of the solvent is, the more favorable the energy transfer between the solute and solvent molecules is.

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Section: Introductionmentioning

confidence: 99%

“…[1][2][3][4][5][6] This rapid process results in a quasiequilibrium distribution in the vibrational manifold equivalent to an elevated temperature of the molecule. Second, the vibrational hot S 1 state is cooled by energy dissipation to the solvent molecules.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast Vibrational and Thermal Relaxation of Dye Molecules in Solutions

et al. 2003

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“…The time scale is 5-50 ps, depending on the specific solvent and the amount of excess energy. 4 Those studies have been reviewed by some authors. [7][8][9][10][11][12] Acetone is a typical example of an aprotic dipolar liquid.…”

Section: Introductionmentioning

confidence: 99%

“…For several dyes in the S 1 state, energy redistribution among vibrational modes has been observed in 25 to 500 fs. [1][2][3][4][5][6] Second, the vibrational hot S 1 state is cooled by energy transfer to the solvent molecules. The time scale is 5-50 ps, depending on the specific solvent and the amount of excess energy.…”

Section: Introductionmentioning

confidence: 99%

“…[1][2][3][4][5][6][19][20][21][22][23][24][25][26][27][28][29][30] The fluorescence upconversion and pump-probe are the most popular methods. The femtosecond time-resolved stimulated emission pumping fluorescence depletion (FS TR SEP FD), which was developed by Kong and co-workers, 28 has been used to study vibrational relaxation and solvation dynamics of dye molecules and the fast singlet-triplet intersystem crossing of terthiophene.…”

Section: Introductionmentioning

confidence: 99%

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Ultrafast Dynamics of Dye Molecules in Solution as a Function of Temperature

et al. 2003

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Femtosecond time-resolved studies using fluorescence depletion spectroscopy were performed on Rhodamine 700 in acetone solution and on Oxazine 750 in acetone and formamide solutions at different temperatures. The experimental curves that include both fast and slow processes have been fitted using a biexponential function. Time constants of the fast process, which corresponds to the intramolecular vibrational redistribution (IVR) of solute molecules, range from 300 to 420 fs and increase linearly as the temperature of the environment decreases. The difference of the average vibrational energy of solute molecules in the ground state at different temperatures is a possible reason that induces this IVR time-constant temperature dependence. However, the time constants of the slow process, which corresponds to the energy transfer from vibrational hot solute molecules to the surroundings occurred on a time scale of 1-50 ps, changed dramatically at lower temperature, nonlinearly increasing with the decrease of temperature. Because of the C-H‚‚‚O hydrogen-bond between acetone molecules, it is more reasonable that acetone molecules start to be associated, which can influence the energy transfer between dye molecules and acetone molecules efficiently, even at temperatures far over the freezing point.

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Vibrational Relaxation in Condensed Phases

Chesnoy

Gale

1988

Advances in Chemical Physics

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Ultrafast investigations of vibrationally hot molecules after internal conversion in solution

Cited by 84 publications

References 16 publications

Ultrafast Vibrational and Thermal Relaxation of Dye Molecules in Solutions

Ultrafast Vibrational and Thermal Relaxation of Dye Molecules in Solutions

Ultrafast Dynamics of Dye Molecules in Solution as a Function of Temperature

Vibrational Relaxation in Condensed Phases

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