Unmasking the cis-Stilbene Phantom State via Vacuum Ultraviolet Time-Resolved Photoelectron Spectroscopy and Ab Initio Multiple Spawning

Author(s):  
Monika Williams ◽  
Ruaridh Forbes ◽  
Hayley Weir ◽  
Kévin Veyrinas ◽  
Ryan J. MacDonell ◽  
...  
2014 ◽  
Vol 16 (23) ◽  
pp. 11770-11779 ◽  
Author(s):  
T. J. A. Wolf ◽  
T. S. Kuhlman ◽  
O. Schalk ◽  
T. J. Martínez ◽  
K. B. Møller ◽  
...  

Time-resolved photoelectron spectroscopy and ab initio multiple spawning dynamical simulations of hexamethylcyclopentadiene reveal wavepacket evolution in a distinct degree of freedom.


2021 ◽  
Author(s):  
Federico Pressacco ◽  
Davide Sangalli ◽  
Vojtěch Uhlíř ◽  
Dmytro Kutnyakhov ◽  
Jon Ander Arregi ◽  
...  

Abstract Femtosecond light-induced phase transitions between different macroscopic orders provide the possibility to tune the functional properties of condensed matter on ultrafast timescales. In first-order phase transitions, transient non-equilibrium phases and inherent phase coexistence often preclude non-ambiguous detection of transition precursors and their temporal onset. Here, we present a study combining time-resolved photoelectron spectroscopy and ab-initio electron dynamics calculations elucidating the transient subpicosecond processes governing the photoinduced generation of ferromagnetic order in antiferromagnetic FeRh. The transient photoemission spectra are accounted for by assuming that not only the occupation of electronic states is modified during the photoexcitation process. Instead, the photo-generated non-thermal distribution of electrons modifies the electronic band structure. The ferromagnetic phase of FeRh, characterized by a minority band near the Fermi energy, is established 350 ± 30 fs after the laser excitation. Ab-initio calculations indicate that the phase transition is initiated by a photoinduced Rh-to-Fe charge transfer.


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Federico Pressacco ◽  
Davide Sangalli ◽  
Vojtěch Uhlíř ◽  
Dmytro Kutnyakhov ◽  
Jon Ander Arregi ◽  
...  

AbstractFemtosecond light-induced phase transitions between different macroscopic orders provide the possibility to tune the functional properties of condensed matter on ultrafast timescales. In first-order phase transitions, transient non-equilibrium phases and inherent phase coexistence often preclude non-ambiguous detection of transition precursors and their temporal onset. Here, we present a study combining time-resolved photoelectron spectroscopy and ab-initio electron dynamics calculations elucidating the transient subpicosecond processes governing the photoinduced generation of ferromagnetic order in antiferromagnetic FeRh. The transient photoemission spectra are accounted for by assuming that not only the occupation of electronic states is modified during the photoexcitation process. Instead, the photo-generated non-thermal distribution of electrons modifies the electronic band structure. The ferromagnetic phase of FeRh, characterized by a minority band near the Fermi energy, is established 350 ± 30 fs after the laser excitation. Ab-initio calculations indicate that the phase transition is initiated by a photoinduced Rh-to-Fe charge transfer.


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