Time-resolved photoelectron angular distributions as a means of studying polyatomic nonadiabatic dynamics

2000 ◽  
Vol 113 (5) ◽  
pp. 1677-1680 ◽  
Author(s):  
Tamar Seideman
Keyword(s):  
Angular Distributions ◽  
Nonadiabatic Dynamics ◽  
Time Resolved ◽  
Photoelectron Angular Distributions

Observation of multi-channel non-adiabatic dynamics in aniline derivatives using time-resolved photoelectron imaging

2016 ◽  
Vol 194 ◽  
pp. 185-208 ◽  
Author(s):  
Magdalena M. Zawadzki ◽  
Marco Candelaresi ◽  
Lisa Saalbach ◽  
Stuart W. Crane ◽  
Martin J. Paterson ◽  
...  
Keyword(s):  
Excited State ◽  
Angular Distributions ◽  
Relaxation Dynamics ◽  
Photoelectron Imaging ◽  
Time Resolved ◽  
Valence States ◽  
Ultimate Fate ◽  
Site Selective ◽  
Photoelectron Angular Distributions ◽  
Electronic Character

We present results from a recent time-resolved photoelectron imaging (TRPEI) study investigating the non-adiabatic relaxation dynamics of N,N-dimethylaniline (N,N-DMA) and 3,5-dimethylaniline (3,5-DMA) following excitation at 240 nm. Analysis of the experimental data is supported by ab initio coupled-cluster calculations evaluating excited state energies and the evolution of several excited state physical properties as a function of N–H/N–CH3 bond extension – a critical reaction coordinate. The use of site-selective methylation brings considerable new insight to the existing body of literature concerning photochemical dynamics in the related system aniline at similar excitation wavelengths. The present work also builds on our own previous investigations in the same species at 250 nm. The TRPEI method provides highly differential energy- and angle-resolved data and, in particular, the temporal evolution of the photoelectron angular distributions afforded by the imaging approach offers much of the new dynamical information. In particular, we see no clear evidence of the second excited 2ππ* state non-adiabatically coupling to the lower-lying S1(ππ*) state or the mixed Rydberg/valence S2(3s/πσ*) state. This, in turn, potentially raises some unresolved questions about the overall nature of the dynamics operating in these systems, especially in regard to the 2ππ* state's ultimate fate. More generally, the findings for the aromatic systems N,N-DMA and 3,5-DMA, taken along with our recent TRPEI results for several aliphatic amine species, highlight interesting questions about the nature of electronic character evolution in mixed Rydberg-valence states as a function of certain key bond extensions and the extent of system conjugation. We begin exploring these ideas computationally for a systematically varied series of tertiary amines.

scholarly journals Femtosecond Time-Resolved Photoelectron Angular Distributions Probed during Photodissociation ofNO2

2000 ◽  
Vol 84 (26) ◽  
pp. 5983-5986 ◽  
Author(s):  
J. A. Davies ◽  
R. E. Continetti ◽  
D. W. Chandler ◽  
C. C. Hayden
Keyword(s):  
Angular Distributions ◽  
Time Resolved ◽  
Photoelectron Angular Distributions

scholarly journals Time-resolved photoelectron angular distributions from nonadiabatically aligned CO2 molecules with SX-FEL at SACLA

2018 ◽  
Vol 2 (11) ◽  
pp. 115015
Author(s):  
Shinichirou Minemoto ◽  
Hiroyuki Shimada ◽  
Kazma Komatsu ◽  
Wataru Komatsubara ◽  
Takuya Majima ◽  
...  
Keyword(s):  
Angular Distributions ◽  
Time Resolved ◽  
Photoelectron Angular Distributions

scholarly journals Ultrafast Relaxation Dynamics Observed Through Time-Resolved Photoelectron Angular Distributions†

2010 ◽  
Vol 114 (42) ◽  
pp. 11216-11224 ◽  
Author(s):  
Julien Lecointre ◽  
Gareth M. Roberts ◽  
Daniel A. Horke ◽  
Jan R. R. Verlet
Keyword(s):  
Angular Distributions ◽  
Relaxation Dynamics ◽  
Time Resolved ◽  
Ultrafast Relaxation ◽  
Photoelectron Angular Distributions

scholarly journals Imaging molecular structure through femtosecond photoelectron diffraction on aligned and oriented gas-phase molecules

2014 ◽  
Vol 171 ◽  
pp. 57-80 ◽  
Author(s):  
Rebecca Boll ◽  
Arnaud Rouzée ◽  
Marcus Adolph ◽  
Denis Anielski ◽  
Andrew Aquila ◽  
...  
Keyword(s):  
Gas Phase ◽  
Angular Distributions ◽  
Nanosecond Laser Pulse ◽  
Nanosecond Laser ◽  
Time Resolved ◽  
Pump Probe ◽  
X Ray ◽  
Photoelectron Diffraction ◽  
Gas Phase Molecules ◽  
Photoelectron Angular Distributions

This paper gives an account of our progress towards performing femtosecond time-resolved photoelectron diffraction on gas-phase molecules in a pump–probe setup combining optical lasers and an X-ray free-electron laser. We present results of two experiments aimed at measuring photoelectron angular distributions of laser-aligned 1-ethynyl-4-fluorobenzene (C8H5F) and dissociating, laser-aligned 1,4-dibromobenzene (C6H4Br2) molecules and discuss them in the larger context of photoelectron diffraction on gas-phase molecules. We also show how the strong nanosecond laser pulse used for adiabatically laser-aligning the molecules influences the measured electron and ion spectra and angular distributions, and discuss how this may affect the outcome of future time-resolved photoelectron diffraction experiments.

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