Ultrafast α –CC bond cleavage of acetone upon excitation to 3p and 3d Rydberg states by femtosecond time-resolved photoelectron imaging

2016 ◽  
Vol 145 (21) ◽  
pp. 214312 ◽  
Author(s):  
O. Hüter ◽  
F. Temps
Keyword(s):  
Bond Cleavage ◽  
Rydberg States ◽  
Photoelectron Imaging ◽  
Time Resolved

scholarly journals Ultrafast Relaxation Dynamics of the S1 (nπ*) State and the 3p and 3d Rydberg States in Cyclohexanone by Femtosecond Photoelectron Imaging

2019 ◽  
Author(s):  
Ole Hüter ◽  
Niklas Helle ◽  
Friedrich Temps
Keyword(s):  
Imaging Spectroscopy ◽  
Rydberg States ◽  
Population Transfer ◽  
Relaxation Dynamics ◽  
Photoelectron Imaging ◽  
Time Resolved ◽  
Flight Mass Spectrometry ◽  
Vibronic Interactions ◽  
Photon Excitation ◽  
Photoelectron Imaging Spectroscopy

<div>The radiationless decay dynamics of the S1 (nπ*) state and the 3p and 3d Rydberg states of cyclohexanone are investigated using femtosecond time-resolved time-of- flight mass spectrometry and photoelectron imaging spectroscopy. After two-photon excitation of the 3p and 3d states, an ultrafast population transfer to the 3s state is observed within < 120 fs. We ascribe this behavior to strong vibronic interactions of the excited Rydberg states with the <sup>1</sup>ππ* valence state that enable an ultrafast population transfer via an avoided crossing and the subsequent passage of a conical intersection between the respective electronic states. Eventually, the 3s state deactivates by internal conversion to the S<sub>1</sub> (nπ*) state, which in turn is found to be long-lived with a decay time of ~ 300 - 800 ps.</div>

scholarly journals Ultrafast valence to non-valence excited state dynamics in a common anionic chromophore

2019 ◽  
Vol 10 (1) ◽  
Author(s):  
James N. Bull ◽  
Cate S. Anstöter ◽  
Jan R. R. Verlet
Keyword(s):  
Excited State ◽  
Internal Conversion ◽  
Rydberg States ◽  
Bound State ◽  
Photoactive Yellow Protein ◽  
Coumaric Acid ◽  
Photoelectron Imaging ◽  
Time Resolved ◽  
Valence States

AbstractNon-valence states in neutral molecules (Rydberg states) have well-established roles and importance in photochemistry, however, considerably less is known about the role of non-valence states in photo-induced processes in anions. Here, femtosecond time-resolved photoelectron imaging is used to show that photoexcitation of the S1(ππ*) state of the methyl ester of deprotonated para-coumaric acid – a model chromophore for photoactive yellow protein (PYP) – leads to a bifurcation of the excited state wavepacket. One part remains on the S1(ππ*) state forming a twisted intermediate, whilst a second part leads to the formation of a non-valence (dipole-bound) state. Both populations eventually decay independently by vibrational autodetachment. Valence-to-non-valence internal conversion has hitherto not been observed in the intramolecular photophysics of an isolated anion, raising questions into how common such processes might be, given that many anionic chromophores have bright valence states near the detachment threshold.

scholarly journals Ultrafast Relaxation Dynamics of the S1 (nπ*) State and the 3p and 3d Rydberg States in Cyclohexanone by Femtosecond Photoelectron Imaging

2019 ◽  
Author(s):  
Ole Hüter ◽  
Niklas Helle ◽  
Friedrich Temps
Keyword(s):  
Imaging Spectroscopy ◽  
Rydberg States ◽  
Population Transfer ◽  
Relaxation Dynamics ◽  
Photoelectron Imaging ◽  
Time Resolved ◽  
Flight Mass Spectrometry ◽  
Vibronic Interactions ◽  
Photon Excitation ◽  
Photoelectron Imaging Spectroscopy

<div>The radiationless decay dynamics of the S1 (nπ*) state and the 3p and 3d Rydberg states of cyclohexanone are investigated using femtosecond time-resolved time-of- flight mass spectrometry and photoelectron imaging spectroscopy. After two-photon excitation of the 3p and 3d states, an ultrafast population transfer to the 3s state is observed within < 120 fs. We ascribe this behavior to strong vibronic interactions of the excited Rydberg states with the <sup>1</sup>ππ* valence state that enable an ultrafast population transfer via an avoided crossing and the subsequent passage of a conical intersection between the respective electronic states. Eventually, the 3s state deactivates by internal conversion to the S<sub>1</sub> (nπ*) state, which in turn is found to be long-lived with a decay time of ~ 300 - 800 ps.</div>

scholarly journals Time-resolved photoelectron imaging using a femtosecond UV laser and a VUV free-electron laser

2010 ◽  
Vol 81 (3) ◽  
Author(s):  
S. Y. Liu ◽  
Y. Ogi ◽  
T. Fuji ◽  
K. Nishizawa ◽  
T. Horio ◽  
...  
Keyword(s):  
Free Electron ◽  
Free Electron Laser ◽  
Uv Laser ◽  
Photoelectron Imaging ◽  
Time Resolved

Dynamics of dipole- and valence bound anions in iodide-adenine binary complexes: A time-resolved photoelectron imaging and quantum mechanical investigation

2015 ◽  
Vol 143 (10) ◽  
pp. 104308 ◽  
Author(s):  
Anne B. Stephansen ◽  
Sarah B. King ◽  
Yuki Yokoi ◽  
Yusuke Minoshima ◽  
Wei-Li Li ◽  
...  
Keyword(s):  
Quantum Mechanical ◽  
Photoelectron Imaging ◽  
Time Resolved ◽  
Binary Complexes ◽  
Mechanical Investigation

scholarly journals Ultrafast Internal Conversion Dynamics of 2-Chloropyridine by Femtosecond Time-Resolved Photoelectron Imaging

2012 ◽  
Vol 28 (11) ◽  
pp. 2543-2548
Author(s):  
GHAZAl Ahmed-Yousif ◽  
◽  
QIU Xue-Jun ◽  
QIN Chao-Chao ◽  
LONG Jin-You ◽  
...  
Keyword(s):  
Internal Conversion ◽  
Photoelectron Imaging ◽  
Time Resolved

Unraveling the electronic relaxation dynamics in photoexcited 2,4-difluoroaniline via femtosecond time-resolved photoelectron imaging

2018 ◽  
Vol 148 (14) ◽  
pp. 144311 ◽  
Author(s):  
Fengzi Ling ◽  
Shuai Li ◽  
Jie Wei ◽  
Kai Liu ◽  
Yanmei Wang ◽  
...  
Keyword(s):  
Electronic Relaxation ◽  
Relaxation Dynamics ◽  
Photoelectron Imaging ◽  
Time Resolved

Ultrafast Internal Conversion Dynamics of Benzyl Chloride by Femtosecond Time-Resolved Photoelectron Imaging

2012 ◽  
Vol 28 (12) ◽  
pp. 2761-2766
Author(s):  
DING Zhong-Hua ◽  
◽  
◽  
QIU Xue-Jun ◽  
XU Yan-Qi ◽  
...  
Keyword(s):  
Benzyl Chloride ◽  
Internal Conversion ◽  
Photoelectron Imaging ◽  
Time Resolved
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