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Maia Magrakvelidze

Publications and source records attributed to Maia Magrakvelidze.

6 recordsLinked to original sources

Attosecond correlated electron dynamics at C$_{60}$ giant plasmon resonance

Fullerenes have unique physical and chemical properties that are associated with their delocalized conjugated electronic structure. Among them, there is a giant ultra-broadband - and therefore ultrafast - plasmon resonance, which for C$_{60}$ is in the extreme-ultraviolet energy range. While this peculiar resonance has attracted considerable interest for the potential downscaling of nanoplasmonic applications such as sensing, drug delivery and photocatalysis at the atomic level, its electronic character has remained elusive. The ultrafast decay time of this collective excitation demands attosecond techniques for real-time access to the photoinduced dynamics. Here, we uncover the role of electron correlations in the giant plasmon resonance of C$_{60}$ by employing attosecond photoemission chronoscopy. We find a characteristic photoemission delay of up to 200 attoseconds pertaining to the plasmon that is purely induced by coherent large-scale correlations. This result provides novel insight into the quantum nature of plasmonic resonances, and sets a benchmark for advancing nanoplasmonic applications.

physics.atom-ph↗

Attosecond delay of xenon $4d$ photoionization at the giant resonance and Cooper minimum

A Kohn-Sham time-dependent local-density-functional scheme is utilized to predict attosecond time delays of xenon 4d photoionization that involves the 4d giant dipole resonance and Cooper minimum. The fundamental effect of electron correlations to uniquely determine the delay at both regions is demonstrated. In particular, for the giant dipole resonance, the delay underpins strong collective effect, emulating the recent prediction at C60 giant plasmon resonance [T. Barillot et al, Phys. Rev. A 91, 033413 (2015)]. For the Cooper minimum, a qualitative similarity with a photorecombination experiment near argon 3p minimum [S. B. Schoun et al, Phys. Rev. Lett. 112, 153001 (2014)] is found. The result should encourage attosecond measurements of Xe 4d photoemission.

physics.atom-ph↗

First prediction of inter-Coulombic decay of C60 inner vacancies through the continuum of confined atoms

Considering the photoionization of Ar@C60 and Kr@C60 endofullerenes, the decay of C60 innershell excitations through the outershell continuum of the confined atom via the inter-Coulombic decay (ICD) pathway is detailed. Excitations to atom-C60 hybrid states demonstrate coherence between ICD and electron-transfer mediated decay (ETMD). This should be the dominant above-threshold decay process for a variety of confined systems, and the strength of these resonances is such that they should be amenable for study by photoelectron spectroscopy.

physics.atm-clus↗

Coherence of Auger and inter-Coulombic decay processes in the photoionization of Ar@C60 versus Kr@C60

For the asymmetric spherical dimer of an endohedrally confined atom and a host fullerene, an innershell vacancy of either system can decay through the continuum of an outer electron hybridized between the systems. Such decays, viewed as coherent superpositions of the single-center Auger and two-center inter-Coulombic (ICD) amplitudes, are found to govern leading decay mechanisms in noble-gas endofullerenes, and are likely omnipresent in this class of nanomolecules. A comparison between resulting autoionizing resonances calculated in the photoionization of Ar@C60 and Kr@C60 exhibits details of the underlying processes.

physics.atm-clus↗

Attosecond time delay in valence photoionization and photorecombination of argon: a TDLDA study

We determine and analyze the quantum phases and time delays in photoionization and photorecombination of valence 3p and 3s electrons of argon using the Kohn-Sham local density functional approach. The time-dependent local density approximation (TDLDA) is used to account for the electron correlation. Resulting attosecond Wigner-Smith time delays show excellent agreements with two recent independent experiments on argon that measured the relative 3s-3p time delay in photoionization [Physical Review Letters {\bf 106}, 143002 (2011)] and the delay in 3p photorecombination [Physical Review Letters {\bf 112}, 153002 (2014)]

physics.atom-ph↗

Fullerene photoemission time delay explores molecular cavity in attoseconds

Photoelectron spectroscopy earlier probed oscillations in C60 valence emissions, producing series of minima whose energy separation depends on the molecular cavity. We show here that the quantum phase at these cavity minima exhibits variations from strong electron correlations in C60, causing rich structures in the emission time delay. Hence, these minima offer unique spectral zones to directly explore multielectron forces via attosecond RABITT interferometry not only in fullerenes, but also in clusters and nanostructures for which such minima are likely abundant.

physics.atm-clus↗