Modelling the effect of nuclear motion on the attosecond time-resolved photoelectron spectra of ethylene

Abstract

Using time dependent density functional theory (TDDFT) we examine the energy, angular and timeresolved photoelectron spectra (TRPES) of ethylene in a pump-probe setup. To simulate TRPES we expose ethylene to an ultraviolet (UV) femtosecond pump pulse, followed by a time delayed extreme ultraviolet (XUV) probe pulse. Studying the photoemission spectra as a function of this delay provides us direct access to the dynamic evolution of the molecule's electronic levels. Further, by including the nuclei's motion, we provide direct chemical insight into the chemical reactivity of ethylene. These results show how angular and energy resolved TRPES could be used to directly probe electron and nucleus dynamics in molecules.

High-order-harmonic generation in benzene with linearly and circularly polarized laser pulses

“…While it has mainly been used to study the electronic response [13,29,30,37,38], some implementations combine TDDFT with a classical description of the ionic motion [39][40][41][42][43][44]. To date, very few implementations combine the treatment of ionic motion with approximations to the exchange-correlation functional that include self-interaction corrections [45,46]. However, these calculations have generally considered the interaction with high-frequency laser pulses.…”

Modeling electron dynamics coupled to continuum states in finite volumes with absorbing boundaries

“…The points in Fig. 9 represent the reflection error for an MFA associated to V S CAP (x) through (24). The behavior here is slightly different from what we observed in the previous section; for E > 0.15 eV, ǫ(E, L) closely reproduces the results obtained with V S CAP (x), while for lower energies it absorbs better.…”

“…8 (b). It shows that (24) yields two numerically identical absorbing properties and that, for practical applications, the two methods are equivalent. Further, the results indicate that the value of a mask function at the edge of the box is connected with the position of the minimum in ǫ(E, L).…”

“…They are the cornerstone of split-domain propagation schemes [20,21] where they act as matching layers between two different domains. In the literature they have been mainly associated with few-body problems (two or three particles), but in recent works they have also been used to study electron photoemission in multi-electron systems combined with time-dependent density functional theory [22][23][24].…”

Efficient and accurate modeling of electron photoemission in nanostructures with TDDFT

“…Both of them were extensively and successfully used for the calculation of photoelectron spectra of atoms, molecules, and clusters [55], model systems for nano-tips [56], and for various experimental setups from time-resolved (pump-probe) spectroscopy [57,58] to strong-field ionization of atoms exposed the x-rays [59]. However, both methods present limitations in practical applications.…”