Ultrafast imaging of laser-controlled non-adiabatic dynamics in NO2 from time-resolved photoelectron emission

2019 ◽  
Vol 21 (19) ◽  
pp. 10038-10051 ◽  
Author(s):  
Maria Richter ◽  
Jesús González-Vázquez ◽  
Zdeněk Mašín ◽  
Danilo S. Brambila ◽  
Alex G. Harvey ◽  
...  
Keyword(s):  
Conical Intersection ◽  
Photoelectron Emission ◽  
Time Resolved ◽  
Ultrafast Imaging ◽  
Adiabatic Dynamics

Imaging and controlling the ultrafast conical intersection dynamics in NO2 using the latest advances in attosecond and light-synthesizer technology.

scholarly journals Excited state non-adiabatic dynamics of pyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study

2015 ◽  
Vol 142 (7) ◽  
pp. 074302 ◽  
Author(s):  
Guorong Wu ◽  
Simon P. Neville ◽  
Oliver Schalk ◽  
Taro Sekikawa ◽  
Michael N. R. Ashfold ◽  
...  
Keyword(s):  
Excited State ◽  
Photoelectron Spectroscopy ◽  
Quantum Dynamics ◽  
Time Resolved ◽  
Adiabatic Dynamics

scholarly journals Excited state non-adiabatic dynamics of N-methylpyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study

2016 ◽  
Vol 144 (1) ◽  
pp. 014309 ◽  
Author(s):  
Guorong Wu ◽  
Simon P. Neville ◽  
Oliver Schalk ◽  
Taro Sekikawa ◽  
Michael N. R. Ashfold ◽  
...  
Keyword(s):  
Excited State ◽  
Photoelectron Spectroscopy ◽  
Quantum Dynamics ◽  
Time Resolved ◽  
Adiabatic Dynamics

scholarly journals Resolving Competing Conical Intersection Pathways: Time-Resolved X-ray Absorption Spectroscopy of trans-1,3-Butadiene

2021 ◽  
Author(s):  
Issaka Seidu ◽  
Simon Neville ◽  
Ryan J MacDonell ◽  
Michael S. Schuurman
Keyword(s):  
Absorption Spectroscopy ◽  
Conical Intersection ◽  
Theoretical Studies ◽  
Nuclear Dynamics ◽  
Time Resolved ◽  
X Ray ◽  
Excited Molecules ◽  
X Ray Absorption

Time-resolved X-ray absorption spectroscopy is emerging as a uniquely powerful tool to probe coupled electronic-nuclear dynamics in photo-excited molecules. Theoretical studies to date have established that time-resolved X-ray absorption spectroscopy...

scholarly journals Unveiling the spatial distribution of molecular coherences at conical intersections by covariance X-ray diffraction signals

2021 ◽  
Vol 118 (22) ◽  
pp. e2105046118
Author(s):  
Stefano M. Cavaletto ◽  
Daniel Keefer ◽  
Jérémy R. Rouxel ◽  
Flavia Aleotti ◽  
Francesco Segatta ◽  
...  
Keyword(s):  
Spatial Distribution ◽  
Three Dimensional ◽  
Laser Pulses ◽  
Conical Intersection ◽  
Conical Intersections ◽  
X Ray Diffraction ◽  
Time Resolved ◽  
X Ray ◽  
Diffraction Imaging ◽  
The Rich

The outcomes and timescales of molecular nonadiabatic dynamics are decisively impacted by the quantum coherences generated at localized molecular regions. In time-resolved X-ray diffraction imaging, these coherences create distinct signatures via inelastic photon scattering, but they are buried under much stronger background elastic features. Here, we exploit the rich dynamical information encoded in the inelastic patterns, which we reveal by frequency-dispersed covariance ultrafast powder X-ray diffraction of stochastic X-ray free-electron laser pulses. This is demonstrated for the photoisomerization of azobenzene involving the passage through a conical intersection, where the nuclear wave packet branches and explores different quantum pathways. Snapshots of the coherence dynamics are obtained at high frequency shifts, not accessible with conventional diffraction measurements. These provide access to the timing and to the confined spatial distribution of the valence electrons directly involved in the conical intersection passage. This study can be extended to full three-dimensional imaging of conical intersections with ultrafast X-ray and electron diffraction.

scholarly journals Monitoring nonadiabatic dynamics in molecules by ultrafast X-Ray diffraction

2019 ◽  
Vol 205 ◽  
pp. 09032
Author(s):  
Markus Kowalewski ◽  
Kochise Bennett ◽  
Shaul Mukamel
Keyword(s):  
Inelastic Scattering ◽  
Nonadiabatic Dynamics ◽  
X Ray Diffraction ◽  
Time Resolved ◽  
X Ray ◽  
Avoided Crossing ◽  
Adiabatic Dynamics ◽  
Nuclear Configuration

We theoretically examine time-resolved diffraction from molecules which undergo non-adiabatic dynamics and identify contributions from inelastic scattering that indicate the presence of an avoided crossing and the corresponding nuclear configuration.

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