Ultrafast dynamics of electron transfer at polar adsorbate/metal interfaces studied with time-resolved photoelectron spectroscopy

2008 ◽  
Author(s):  
Martin Wolf
Keyword(s):  
Electron Transfer ◽  
Photoelectron Spectroscopy ◽  
Ultrafast Dynamics ◽  
Time Resolved ◽  
Metal Interfaces

Ultrafast dynamics of water molecules excited to electronic F̃ states: A time-resolved photoelectron spectroscopy study

2019 ◽  
Vol 32 (1) ◽  
pp. 53-58
Author(s):  
Dong-yuan Yang ◽  
Yan-jun Min ◽  
Zhen Chen ◽  
Zhi-gang He ◽  
Zhi-chao Chen ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Water Molecules ◽  
Ultrafast Dynamics ◽  
Spectroscopy Study ◽  
Time Resolved

scholarly journals The Role of Structural Flexibility in Plasmon-Driven Coupling Reactions: Kinetic Limitations in the Dimerization of Nitro-Benzenes

2021 ◽  
Author(s):  
Wouter Koopman ◽  
Evgenii Titov ◽  
Radwan Mohamed Sarhan ◽  
Tina Gaebel ◽  
Robin Schürmann ◽  
...  
Keyword(s):  
Electron Transfer ◽  
Photoelectron Spectroscopy ◽  
Density Functional ◽  
Bond Activation ◽  
Density Functional Theory Calculations ◽  
Surface Enhanced Raman Spectroscopy ◽  
Bimolecular Reaction ◽  
Structural Flexibility ◽  
Coupling Reactions ◽  
Time Resolved

<div>The plasmon-driven dimerization of 4-nitrothiophenol (4NTP) to 4-4’-dimercaptoazobenzene (DMAB) has become a testbed for understanding bimolecular photoreactions enhanced by nanoscale metals, in particular, regarding the relevance of electron transfer and heat transfer from the metal to the molecule. By adding a methylene group between the thiol bond and the nitrophenyl, we add structural flexibility to the reactant molecule. Time-resolved surface-enhanced Raman-spectroscopy proves that this (4-nitrobenzyl)mercaptan (4NBM) molecule has a larger dimerization rate and dimerization yield than 4NTP and higher selectivity towards dimerization. X-ray photoelectron spectroscopy and density functional theory calculations show that the electron transfer would prefer activation of 4NTP over 4NBM. We conclude that the rate limiting step of this plasmonic reaction is the dimerization step, which is dramatically enhanced by the additional flexibility of the reactant. This study may serve as an example for using nanoscale metals to simultaneously provide charge carriers for bond activation and localized heat for driving bimolecular reaction steps. The molecular structure of reactants can be tuned to control the reaction kinetics.<br></div>

scholarly journals Time-Resolved Dynamics in Iodide-Uracil-Water Clusters upon Excitation of the Nucleobase

2019 ◽  
Author(s):  
Alice Kunin ◽  
Valerie S. McGraw ◽  
Daniel Neumark
Keyword(s):  
Electron Transfer ◽  
Photoelectron Spectroscopy ◽  
Cross Correlation ◽  
Water Clusters ◽  
Laser Pulses ◽  
Probe Laser ◽  
Time Resolved ◽  
Pump And Probe ◽  
The Cross

The dynamics of iodide-uracil-water (I<sup>−</sup>·U·H<sub>2</sub>O) clusters following π-π* excitation of the nucleobase are probed using time-resolved photoelectron spectroscopy (TRPES). Photoexcitation of this cluster at 4.77 eV results in electron transfer from the iodide moiety to the uracil, creating a valence-bound (VB) anion within the cross-correlation of the pump and probe laser pulses. This species can decay by a number of channels, including autodetachment and dissociation to I<sup>−</sup> or larger anion fragments. Comparison of the energetics of the photoexcited cluster and its decay dynamics with those of the bare iodide-uracil (I<sup>−</sup>·U) complex provide a sensitive probe of the effects of microhydration on these species. The results are also compared with TRPES experiments on I<sup>−</sup>·U·H<sub>2</sub>O at lower pump photon energies, where both the initial photoinduced dynamics and the decay of the photoexcited cluster are qualitatively different.

Time-Resolved Dynamics in Iodide-Uracil-Water Clusters upon Excitation of the Nucleobase

2019 ◽  
Author(s):  
Alice Kunin ◽  
Valerie S. McGraw ◽  
Katharine G. Lunny ◽  
Daniel Neumark
Keyword(s):  
Electron Transfer ◽  
Photoelectron Spectroscopy ◽  
Cross Correlation ◽  
Water Clusters ◽  
Laser Pulses ◽  
Probe Laser ◽  
Time Resolved ◽  
Pump And Probe ◽  
The Cross

The dynamics of iodide-uracil-water (I<sup>−</sup>·U·H<sub>2</sub>O) clusters following π-π* excitation of the nucleobase are probed using time-resolved photoelectron spectroscopy (TRPES). Photoexcitation of this cluster at 4.77 eV results in electron transfer from the iodide moiety to the uracil, creating a valence-bound (VB) anion within the cross-correlation of the pump and probe laser pulses. This species can decay by a number of channels, including autodetachment and dissociation to I<sup>−</sup> or larger anion fragments. Comparison of the energetics of the photoexcited cluster and its decay dynamics with those of the bare iodide-uracil (I<sup>−</sup>·U) complex provide a sensitive probe of the effects of microhydration on these species.

scholarly journals Time-Resolved Dynamics in Iodide-Uracil-Water Clusters upon Excitation of the Nucleobase

2019 ◽  
Author(s):  
Alice Kunin ◽  
Valerie S. McGraw ◽  
Katharine G. Lunny ◽  
Daniel Neumark
Keyword(s):  
Electron Transfer ◽  
Photoelectron Spectroscopy ◽  
Cross Correlation ◽  
Water Clusters ◽  
Laser Pulses ◽  
Probe Laser ◽  
Time Resolved ◽  
Pump And Probe ◽  
The Cross

The dynamics of iodide-uracil-water (I<sup>−</sup>·U·H<sub>2</sub>O) clusters following π-π* excitation of the nucleobase are probed using time-resolved photoelectron spectroscopy (TRPES). Photoexcitation of this cluster at 4.77 eV results in electron transfer from the iodide moiety to the uracil, creating a valence-bound (VB) anion within the cross-correlation of the pump and probe laser pulses. This species can decay by a number of channels, including autodetachment and dissociation to I<sup>−</sup> or larger anion fragments. Comparison of the energetics of the photoexcited cluster and its decay dynamics with those of the bare iodide-uracil (I<sup>−</sup>·U) complex provide a sensitive probe of the effects of microhydration on these species.

Probing ultrafast dynamics during and after passing through conical intersections

2019 ◽  
Vol 21 (26) ◽  
pp. 13902-13905 ◽  
Author(s):  
Shunsuke Adachi ◽  
Tom Schatteburg ◽  
Alexander Humeniuk ◽  
Roland Mitrić ◽  
Toshinori Suzuki
Keyword(s):  
Photoelectron Spectroscopy ◽  
Ultrafast Dynamics ◽  
Conical Intersections ◽  
Time Resolved ◽  
Vacuum Uv

Time-resolved photoelectron spectroscopy using vacuum-UV probe pulses enables observing ultrafast dynamics during and after passing through conical intersections.

scholarly journals The Role of Structural Flexibility in Plasmon-Driven Coupling Reactions: Kinetic Limitations in the Dimerization of Nitro-Benzenes

2021 ◽  
Author(s):  
Wouter Koopman ◽  
Evgenii Titov ◽  
Radwan Mohamed Sarhan ◽  
Tina Gaebel ◽  
Robin Schürmann ◽  
...  
Keyword(s):  
Electron Transfer ◽  
Photoelectron Spectroscopy ◽  
Density Functional ◽  
Bond Activation ◽  
Density Functional Theory Calculations ◽  
Surface Enhanced Raman Spectroscopy ◽  
Bimolecular Reaction ◽  
Structural Flexibility ◽  
Coupling Reactions ◽  
Time Resolved

<div>The plasmon-driven dimerization of 4-nitrothiophenol (4NTP) to 4-4’-dimercaptoazobenzene (DMAB) has become a testbed for understanding bimolecular photoreactions enhanced by nanoscale metals, in particular, regarding the relevance of electron transfer and heat transfer from the metal to the molecule. By adding a methylene group between the thiol bond and the nitrophenyl, we add structural flexibility to the reactant molecule. Time-resolved surface-enhanced Raman-spectroscopy proves that this (4-nitrobenzyl)mercaptan (4NBM) molecule has a larger dimerization rate and dimerization yield than 4NTP and higher selectivity towards dimerization. X-ray photoelectron spectroscopy and density functional theory calculations show that the electron transfer would prefer activation of 4NTP over 4NBM. We conclude that the rate limiting step of this plasmonic reaction is the dimerization step, which is dramatically enhanced by the additional flexibility of the reactant. This study may serve as an example for using nanoscale metals to simultaneously provide charge carriers for bond activation and localized heat for driving bimolecular reaction steps. The molecular structure of reactants can be tuned to control the reaction kinetics.<br></div>

scholarly journals Attosecond intra-valence band dynamics and resonant-photoemission delays in W(110)

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
S. Heinrich ◽  
T. Saule ◽  
M. Högner ◽  
Y. Cui ◽  
V. S. Yakovlev ◽  
...  
Keyword(s):  
Valence Band ◽  
Photoelectron Spectroscopy ◽  
Electronic Band Structure ◽  
Photoelectric Effect ◽  
Final State ◽  
Electronic Band ◽  
Time Resolved ◽  
Resonant Photoemission ◽  
Pulse Trains ◽  
Electron Correlation Effects

AbstractTime-resolved photoelectron spectroscopy with attosecond precision provides new insights into the photoelectric effect and gives information about the timing of photoemission from different electronic states within the electronic band structure of solids. Electron transport, scattering phenomena and electron-electron correlation effects can be observed on attosecond time scales by timing photoemission from valence band states against that from core states. However, accessing intraband effects was so far particularly challenging due to the simultaneous requirements on energy, momentum and time resolution. Here we report on an experiment utilizing intracavity generated attosecond pulse trains to meet these demands at high flux and high photon energies to measure intraband delays between sp- and d-band states in the valence band photoemission from tungsten and investigate final-state effects in resonant photoemission.

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