Charge transfer to solvent dynamics in iodide aqueous solution studied at ionization threshold

Kothe, Alexander; Wilke, Martin; Moguilevski, Alexandre; Engel, Nicholas; Winter, Bernd; Kiyan, Igor Yu.; Aziz, Emad F.

doi:10.1039/c4cp02482f

Cited by 13 publications

(18 citation statements)

References 140 publications

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“…In an attempt to probe interfacial CTTS dynamics of iodide, time-resolved photoelectron spectroscopy coupled with the liquid microject technique has recently been used. 6,[9][10][11][12][13] Results from such experiments showed that the observable dynamics are very similar to those seen in the bulk.…”

mentioning

confidence: 69%

“…A particularly useful means of initiating CTTS reactions is photoexcitation to CTTS absorption bands of certain aqueous anions. The most studied of these has been the CTTS of iodide [2][3][4][5][6][7][8][9][10][11][12][13] and a schematic of the solvation dynamics are shown in Figure 1. However, these studies have focussed on the bulk dynamics, while arguably, electron transfer reactions are of most interest at interfaces, be it on an aerosol particle, on an interstellar dust-grain, or at a water/biomolecule interface.…”

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confidence: 99%

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Charge Transfer to Solvent Dynamics at the Ambient Water/Air Interface

Nowakowski

Woods

Verlet

2016

J. Phys. Chem. Lett.

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confidence: 69%

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confidence: 99%

Charge Transfer to Solvent Dynamics at the Ambient Water/Air Interface

Nowakowski

Woods

Verlet

2016

J. Phys. Chem. Lett.

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“…The study of electronic and structural dynamics in solutions and at interfaces received much attention during the past years [1][2][3][4][5][6][7][8][9]. The interest and the importance of these studies arise from the fact that solutions represent a natural environment for most biochemical complexes [10][11][12][13].…”

Section: Introductionmentioning

confidence: 99%

“…Various non-radiative electronic transitions can be initiated by light in biochemical complexes. Charge transfer [14], electron solvation [1,15], spin crossover [16,17], and photooxidation [18] represent some of them. Depending on the transition character, the time scale of the complex dynamics can lie in the femtosecond range, requiring application of ultrafast spectroscopies to study photoreactions in detail.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast photoelectron spectroscopy of solutions: space-charge effect

et al. 2015

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The method of time-resolved XUV photoelectron spectroscopy is applied in a pump-probe experiment on a liquid micro-jet. We investigate how the XUV energy spectra of photoelectrons are influenced by the space charge created due to ionization of the liquid medium by the pump laser pulse. XUV light from high-order harmonic generation is used to probe the electron population of the valence shell of iron hexacyanide in water. By exposing the sample to a short UV pump pulse of 266 nm wavelength and ∼55 fs duration, we observe an energy shift of the spectral component associated with XUV ionization from the Fe 3d(t 2g ) orbital as well as a shift of the water spectrum. Depending on the sequence of the pump and probe pulses, the arising energy shift of photoelectrons acquires a positive or negative value. It exhibits a sharp positive peak at small time delays, which facilitates to determine the temporal overlap between pump and probe pulses. The negative spectral shift is due to positive charge accumulated in the liquid medium during ionization. Its dissipation is found to occur on a (sub)nanosecond time scale and has a biexponential character. A simple meanfield model is provided to interpret the observations. A comparison between the intensity dependencies of the spectral shift and the UV ionization yield shows that the space-charge effect can be significantly reduced when the pump intensity is attenuated below the saturation level of water ionization. For the given experimental conditions, the saturation intensity lies at 6 10 10 W cm −2 .

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“…Kothe et al assume excitation of iodide by two-photon absorption. 1 and that the temporal overlap is shifted. In Kothe's work, the concentration of water molecules is about 2000 times larger than the iodide concentration.…”

Section: Hans-hermann Ritze and Andrea Lübcke*mentioning

confidence: 99%