Photoelectron spectra of solvated electrons in bulk water, methanol, and ethanol

Horio, Takeshi; Shen, Huan; Adachi, Shunsuke; Suzuki, Toshinori

doi:10.1016/j.cplett.2012.03.051

Cited by 46 publications

(65 citation statements)

References 31 publications

(42 reference statements)

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“…Using liquid micro-jet photoelectron spectroscopy, the VDE was found to be in the range of 3.3 eV to 3.5 eV. 18,21,22,23,30,31 Recently, liquid jet experiments reported the VDE of e - aq in the range of 3.42 – 3.45 eV. 30,31 Using density functional theory (DFT) and considering the effect of full solvent through the non-equilibrated polarized continuum model (NE-PCM), the VDE of e - aq was calculated as ca.…”

Section: Introductionmentioning

confidence: 99%

Do Solvated Electrons (e_aq^–) Reduce DNA Bases? A Gaussian 4 and Density Functional Theory-Molecular Dynamics Study

et al. 2016

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The solvated electron (e-aq) is a primary intermediate after an ionization event that produces reductive DNA damage. Accurate determination of standard redox potentials (E°) of nucleobases and of e-aq determine the extent of reaction of e-aq with nucleobases. In this work, E° of e-aq and of nucleobases have been calculated employing the accurate ab initio Gaussian-4 theory including the polarizable continuum model (PCM). The Gaussian-4-calculated E° of e-aq (-2.86 V) is in excellent agreement with the experimental one (-2.87 V). The Gaussian-4-calculated E° of nucleobases in dimethylformamide (DMF) lie in the range (-2.36 V to -2.86 V); they are in reasonable agreement with the experimental E° in DMF and have a mean unsigned error (MUE) = 0.22 V. However, inclusion of specific water molecules reduces this error significantly (MUE= 0.07). Employing a model of e-aq-nucleobase complex with 6 water molecules, reaction of e-aq with the adjacent nucleobase is investigated using approximate ab initio molecular dynamics (MD) simulations including PCM. Our MD simulations show that e-aq transfers to uracil, thymine, cytosine and adenine, within 10 to 120 fs and e-aq reacts with guanine only when a water molecule forms a hydrogen bond to O6 of guanine which stabilizes the anion radical.

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Section: Introductionmentioning

confidence: 99%

Do Solvated Electrons (e_aq^–) Reduce DNA Bases? A Gaussian 4 and Density Functional Theory-Molecular Dynamics Study

et al. 2016

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“…Since methanol has become a popular target in fuel-cell research (methanol economy), Experiments performed for more than 50 years, have successfully characterized the structure, the dynamics and spectroscopy of solvated electrons in bulk methanol. 3,4,5,6,7,8,9,10 Extension of the experimental techniques to the gas phase has made it possible to investigate solvated electrons in methanol clusters in the last decade. 11,12,13 Due to the fewer degrees of freedom of the solvating molecules, cluster experiments provide more tangible information on the underlying microscopic details of the solute-solvent interaction and dynamics.…”

Section: Introductionmentioning

confidence: 99%

Excess electrons in methanol clusters: Beyond the one-electron picture

Pohl

Mones

Túri

2016

The Journal of Chemical Physics

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“…In order to achieve higher precision and reliability for liquid TRPES, we have constructed a magnetic bottle time-of-flight (TOF) spectrometer (flight length: 1 m), which collects 50% of photoelectrons emitted from the liquid beam and enables measurement of the entire photoelectron energy spectrum on a shot-to-shot basis. 105 In combination with a 100 kHz DUV femtosecond laser we constructed, the new spectrometer improved the signal count level by four to five orders of magnitude in comparison with our old system. The spectra of solvated electrons in H 2 O, D 2 O, methanol, and ethanol measured at a pumpprobe time delay of 2 ns are shown in Figure 19.…”

Section: Time-resolved Photoelectron Spectroscopy Of Liquidsmentioning

confidence: 99%

Nonadiabatic Electronic Dynamics in Isolated Molecules and in Solution Studied by Ultrafast Time–Energy Mapping of Photoelectron Distributions

Suzuki

2014

Bulletin of the Chemical Society of Japan

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Nonadiabatic electronic dynamics contribute to the diversity of chemical reactions. We investigate nonadiabatic dynamics in isolated molecules and aqueous solutions by time-resolved photoelectron spectroscopy. For isolated molecules in the gas phase, we combine two-dimensional imaging detection of electrons and a sub-20 fs deep UV and vacuum UV light source to measure time-evolution of the photoelectron kinetic energy and angular distributions. Time energy mapping of photoelectron angular anisotropy reveals the S 2 ¼ S 1 internal conversion dynamics through conical intersection in pyrazine, benzene, and toluene. The timeenergy mapping is also employed to extract the photoelectron angular distribution in the molecular frame for nitric oxide. For electronic dynamics in aqueous solution, we employ timeresolved photoelectron spectroscopy using a liquid beam and an electrostatic or a time-of-flight electron energy analyzer. Successful observation of ultrafast electron-transfer reactions in aqueous solutions and measurement of electron binding energies of solvated species suggest promising future developments of this very young field.

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Photoelectron spectra of solvated electrons in bulk water, methanol, and ethanol

Cited by 46 publications

References 31 publications

Do Solvated Electrons (e_aq^–) Reduce DNA Bases? A Gaussian 4 and Density Functional Theory-Molecular Dynamics Study

Do Solvated Electrons (e_aq^–) Reduce DNA Bases? A Gaussian 4 and Density Functional Theory-Molecular Dynamics Study

Excess electrons in methanol clusters: Beyond the one-electron picture

Nonadiabatic Electronic Dynamics in Isolated Molecules and in Solution Studied by Ultrafast Time–Energy Mapping of Photoelectron Distributions

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Photoelectron spectra of solvated electrons in bulk water, methanol, and ethanol

Cited by 46 publications

References 31 publications

Do Solvated Electrons (eaq–) Reduce DNA Bases? A Gaussian 4 and Density Functional Theory-Molecular Dynamics Study

Do Solvated Electrons (eaq–) Reduce DNA Bases? A Gaussian 4 and Density Functional Theory-Molecular Dynamics Study

Excess electrons in methanol clusters: Beyond the one-electron picture

Nonadiabatic Electronic Dynamics in Isolated Molecules and in Solution Studied by Ultrafast Time–Energy Mapping of Photoelectron Distributions

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Product

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Do Solvated Electrons (e_aq^–) Reduce DNA Bases? A Gaussian 4 and Density Functional Theory-Molecular Dynamics Study

Do Solvated Electrons (e_aq^–) Reduce DNA Bases? A Gaussian 4 and Density Functional Theory-Molecular Dynamics Study