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Photodetachment and electron reactivity in 1-methyl-1-butyl-pyrrolidinium bis(trifluoromethylsulfonyl)amide
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10.1063/1.4736569
/content/aip/journal/jcp/137/3/10.1063/1.4736569
http://aip.metastore.ingenta.com/content/aip/journal/jcp/137/3/10.1063/1.4736569

Figures

Image of FIG. 1.
FIG. 1.

The absorption spectrum in a 1 mm path length cell. The inset shows the IL molecular structure.

Image of FIG. 2.
FIG. 2.

(a) Change in the probe spectrum following excitation at 266 nm. (b) Time dependence for 50 nm wide regions. The circles represent the data and the lines are the fits as described in the text. The associated fitting parameters are listed in Table I.

Image of FIG. 3.
FIG. 3.

The signal at 980 nm and a pump-probe time delay of 500 ps as a function of the 266 nm pump irradiance. The arrow indicates the pump irradiance used for all other presented data. The circles are the data, the line is the fit with a slope of 0.99 ± 0.16, and the error bars span a total of two standard deviations in the signal.

Image of FIG. 4.
FIG. 4.

Change in the signal at 925 nm following excitation at 266 nm and a pump-probe time delay of 1 ps as a function of laboratory time. The first data point is roughly 10 s after the shutter opened to illuminate the sample.

Image of FIG. 5.
FIG. 5.

Time dependence of changes in the signal at 980 nm following excitation at 266 nm. The data are presented as the fraction of the signal in the absence of HClO4. The circles represent the data and the lines are the fits as described in the text. The associated fitting parameters are listed in Table II.

Image of FIG. 6.
FIG. 6.

Change in the probe spectrum following excitation at 266 nm in the presence of (a) 179 mM HClO4 and (b) 347 mM HClO4. The data are presented as the fraction of the signal in the absence of HClO4.

Image of FIG. 7.
FIG. 7.

Probability distribution of nearest pairwise distances for a random distribution at the concentrations of the HClO4 quencher used. The inset shows a comparison of the fraction of the distribution below 0.9 nm (squares), and the fraction of the quenching fit with the 300 fs decay component (circles), see Table II.

Image of FIG. 8.
FIG. 8.

Plots of Eq. (5) with τsol = 300 fs, k dry = 4.3 × 1012 M−1 s−1 and the indicated proton concentration. (b) A comparison of the decays in (a) for all values of [H+] after subtraction of the offset at large delay times and scaling to the same initial value. (c) Comparison of the quenching at long time in Eq. (5) and the residual amplitude of the fastest quenching component determined from the fits to the data, (1 – a 1), see Table II.

Tables

Generic image for table
Table I.

Fitting parameters for the time dependent changes in optical density shown in Fig. 2(a). The exponential time constants are τ n , the exponential weighting factors are a n , and H is the amplitude of the Heaviside function. Below each value is the 68.2% confidence interval from the nonlinear fitting when all variables are simultaneously optimized.

Generic image for table
Table II.

Fits to the quenching data shown in Fig. 5. The exponential time constants are τ n and the exponential weighting factors are a n . Below each value is the 68.2% confidence interval from the nonlinear fitting when all variables are simultaneously optimized.

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/content/aip/journal/jcp/137/3/10.1063/1.4736569
2012-07-19
2014-04-24
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Photodetachment and electron reactivity in 1-methyl-1-butyl-pyrrolidinium bis(trifluoromethylsulfonyl)amide
http://aip.metastore.ingenta.com/content/aip/journal/jcp/137/3/10.1063/1.4736569
10.1063/1.4736569
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