Fall-back time for photo-ionized Cs atoms attached to superfluid 4He nanodroplets

Coppens, François; Vangerow, J. von; Leal, Antonio; Barranco, M.; Halberstadt, Nadine; Mudrich, M.; Pí, M.; Stienkemeier, F.

doi:10.1140/epjd/e2019-90692-0

Cited by 7 publications

(51 citation statements)

References 42 publications

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“…Using time-dependent 4 He-DFT simulations, the same authors have found that excited-state Cs atoms desorb after excitation to the 6p 2 Σ 1/2 state, while for the 6p 2 Π 1/2 state, the atoms are predicted to desorb from the droplet only if the excitation wavenumber E pump /(hc) is ≥11200 cm −1 . The results of the theoretical studies also imply that CsHe exciplex formation is supported for excitation to the 6p 2 Π 3/2 and 6p 2 Π 1/2 states only, and that the desorption of the exciplex in the 6p 2 Π 3/2 state is due to non-radiative relaxation to the 6p 2 Π 1/2 state [36].…”

Section: Resultsmentioning

confidence: 72%

“…The interaction between an electronically excited Cs atom and a He nanodroplet is often repulsive owing to the high delocalization of the valence electron in excited-state Cs [26,35]. The 6p 2 Π 1/2 , 6p 2 Π 3/2 and 6p 2 Σ 1/2 molecular states, which are excited near the 6p ← 6s transitions in atomic Cs, have bound-state character, but resonant excitation near the equilibrium position of the Cs-He N complex is predicted to produce excited-state Cs atoms in molecular states far above the dissociation limit, so that a desorption of the excited Cs atom from the droplet is expected [36]. Using time-dependent 4 He-DFT simulations, the same authors have found that excited-state Cs atoms desorb after excitation to the 6p 2 Σ 1/2 state, while for the 6p 2 Π 1/2 state, the atoms are predicted to desorb from the droplet only if the excitation wavenumber E pump /(hc) is ≥11200 cm −1 .…”

Section: Resultsmentioning

confidence: 99%

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Dynamics of photo-excited Cs atoms attached to helium nanodroplets

Rendler,

Scognamiglio,

Dulitz

et al. 2021

Preprint

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We present an experimental study of the dynamics following the photo-excitation and subsequent photo-ionization of single Cs atoms on the surface of helium nanodroplets. The dynamics of excited-Cs-atom desorption and re-adsorption as well as CsHe exciplex formation are measured using femtosecond pump-probe velocity-map-imaging spectroscopy and ion-time-of-flight spectrometry. The timescales for the desorption of excited Cs atoms off helium nanodroplets as well as the timescales for CsHe exciplex formation are experimentally determined for the 6p states of Cs. For the 6p 2 Π 1/2 state, our results confirm that the excited Cs atoms only desorb from the nanodroplet when the excitation wavenumber is blue-shifted from the 6p 2 Π 1/2 ← 6s 2 Σ 1/2 resonance. Our results suggest that the dynamics following excitation to the 6p 2 Π 3/2 state can be described by an evaporationlike desorption mechanism, whereas the dynamics arising from excitation to the 6p 2 Σ 1/2 state is indicative for a more impulsive desorption process. Furthermore, our results suggest a heliuminduced spin-orbit relaxation from the the 6p 2 Σ 1/2 state to the 6p 2 Π 1/2 state. Our findings largely agree with the results of time-dependent 4 He-density-functional theory (DFT) simulations published earlier [Coppens et al., Eur. Phys. J. D 73, 94 (2019)].

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Section: Resultsmentioning

confidence: 72%

Section: Resultsmentioning

confidence: 99%

Dynamics of photo-excited Cs atoms attached to helium nanodroplets

Rendler,

Scognamiglio,

Dulitz

et al. 2021

Preprint

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“…These software packages have been designed to become powerful and universal instruments of computational research in the field of MBN Science, which should play a role of a "virtual microscope" and a "camera" capable to explore, simulate, record and visualize both structure and dynamics of the MBN-world with an atomistic level of accuracy, in order to both reproduce its known features and predict the new ones. In this Topical Issue, many contributions [12][13][14][15][16][17][18][19][20][21][22][24][25][26][27][28][29][30][31][32][33][34][35] provide case studies conducted with these packages and demonstrate their application to a broad variety of topical areas in MBN science as listed at the beginning of this Editorial. To be noted that these universal and powerful software packages are fully applicable to a broad variety of the topical areas of the MBN Science listed above in the introductory part of the Editorial.…”

Section: Discussionmentioning

confidence: 99%

“…A theoretical study [16] investigated helium nanodroplets with impurities. Here the impurities were modeled through cesium atoms and the Coppens et al studied the dynamic evolution of a Cs atom photo-excited from 6s to 6p and 7s states on a helium droplet using timedependent DFT simulations.…”

Section: Clusters and Nanoparticlesmentioning

confidence: 99%

Special issue: Dynamics of systems on the nanoscale (2018). Editorial

et al. 2020

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The structure, formation and dynamics of both animate and inanimate matter on the nanoscale are a highly interdisciplinary field of rapidly emerging research engaging a broad community encompassing experimentalists, theorists, and technologists. It is relevant for a large variety of molecular and nanosystems of different origin and composition and concerns numerous phenomena originating from physics, chemistry, biology, or materials science. This Topical Issue presents a collection of original research papers devoted to different aspects of structure and dynamics on the nanoscale. Some of the contributions discuss specific applications of the research results in several modern technologies and in next generation medicine. Most of the works of this topical issue were reported at the Fifth International Conference on Dynamics of Systems on the Nanoscale (DySoN)-the premier forum for the presentation of cutting-edge research in this field that was held in Potsdam, Germany in October of 2018.

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“…27-32, and earlier works have simulated photon absorption spectra of alkali atoms attached to vortex-free helium nanodroplets using different functionals and/or He-alkali pair potentials. [27,28,[33][34][35][36][37] We have repeated them in order to ensure comparison with vortex-hosting droplets with exactly the same parameters. To the best of our knowledge, the spectrum of alkali atoms attached to vortex-hosting droplets has not been previously addressed theoretically.…”

Section: Please Cite This Article As Doi:101063/50008923mentioning

confidence: 99%

Alkali atoms attached to vortex-hosting helium nanodroplets

García-Alfonso

Coppens

Barranco

et al. 2020

The Journal of Chemical Physics

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Light absorption or accordingly fluorescence excitation spectroscopy of alkali atoms attached to 4 He droplets is investigated as a possible way of detecting the presence of vortices. To this end, we have calculated the equilibrium configuration and energetics of alkali atoms attached to a 4 He1000 droplet hosting a vortex line using 4 He density functional theory. We use them to study how the dipole absorption spectrum of the alkali atom is modified when the impurity is attached to a vortex line. Spectra are found to be shifted to the blue (higher frequencies) and broadened compared to vortex-free droplets, because the dimple in which the alkali atom sits at the intersection of the vortex line and the droplet surface is deeper. This effect is smaller for lighter alkali atoms, and all the more so when using a quantum description since in this case, they sit further away from the droplet surface on average due to their zero-point motion. Spectral modifications due to the presence of a vortex line are minor for np ← ns excitation, and therefore insufficient for vortex detection. In the case of higher n p ← ns or n s ← ns (n > n) excitations the shifts are larger, as the excited state orbital is more extended and therefore more sensitive to changes in the surrounding helium density.

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Fall-back time for photo-ionized Cs atoms attached to superfluid 4He nanodroplets

Cited by 7 publications

References 42 publications

Dynamics of photo-excited Cs atoms attached to helium nanodroplets

Dynamics of photo-excited Cs atoms attached to helium nanodroplets

Special issue: Dynamics of systems on the nanoscale (2018). Editorial

Alkali atoms attached to vortex-hosting helium nanodroplets

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