Unravelling the full relaxation dynamics of superexcited helium nanodroplets

D., Asmussen, Jakob; Michiels, Rupert; Dulitz, Katrin; Ngai, A.; Bangert, Ulrich; Barranco, M.; Binz, Marcel; Bruder, Lukas; Danailov, Miltcho; Fraia, Michele Di; Eloranta, Jussi; Feifel, Raimund; Giannessi, L.; Pí, M.; Plekan, Oksana; Squibb, Richard J.; Uhl, Daniel; Wituschek, Andreas; Zangrando, Marco; Callegari, Carlo; Stienkemeier, F.; Mudrich, M.

doi:10.1039/d1cp01041g

Cited by 15 publications

(39 citation statements)

References 72 publications

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“…From our investigation of the relaxation dynamics, it was found that the complete relaxation to the two lowest metastable states happens on a similar time-scale as ICD, but that the electronic (interband) relaxation is faster, and thus happens before the He superfluid dynamics sets in. 32 ICD of dopants appears to be driven by a similar medium-dominated dynamics as the He*+He* ICD process in pure droplets.…”

Section: Decay (Icd) Takes Places Either Between Two Excited He Atoms...mentioning

confidence: 91%

“…For a discussion of the relaxation dynamics of superexcited pure He nanodroplets, we refer to our recent paper. 32 We start by presenting the results of static measurements (XUV only) for various doping levels of Na. Figure 1 shows photoelectron spectra (PES) of pure and Na-doped He nanodroplets of average size 4.1×10 4 atoms per droplet and a FEL intensity of 1.7×10 10 Wcm −2 .…”

Section: Decay (Icd) Takes Places Either Between Two Excited He Atoms...mentioning

confidence: 99%

“…18,37,38 The spectra show that the main contributions to ICD are from the metastable 1s2s 1 S and 3 S excited states after electronic relaxation from the initial superexcited state, matching previous measurements for pure and doped He nanodroplets. 13,25 Thus, electronic relaxation 30,32 proceeds much faster than ICD. The four main Figure 2: Yield of the 4 main ICD channels involving the lowest excited states 1s2s 1, 3 S as a function of doping strength (in units of tabulated Na vapor pressure times the length of the doping region).…”

Section: Decay (Icd) Takes Places Either Between Two Excited He Atoms...mentioning

confidence: 99%

“…The lower part shows photoelectrons due to ionization of the excited He atoms with either one or two photons of the UV probe. 32 The upper part shows electrons generated by ICD which is quenched around 0 ps pump-probe delay where the excited state is photoionized before ICD has happened. The panel on the top left shows an electron spectrum at negative delay (UV first), where the ICD process is unperturbed.…”

Section: Decay (Icd) Takes Places Either Between Two Excited He Atoms...mentioning

confidence: 99%

“…For further analysis of the low-energy part of the TRPES, we refer to our recent paper on the relaxation dynamics of superexcited He droplets. 32 In this phase, ICD begins to outcompete photoionization and ICD electrons reappear. The time constant of ICD can be determined from the reappearance time following depletion.…”

Section: Decay (Icd) Takes Places Either Between Two Excited He Atoms...mentioning

confidence: 99%

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Time-resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-doped Helium Nanodroplets

D.¹,

Michiels²,

Bangert³

et al. 2022

Preprint

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Section: Decay (Icd) Takes Places Either Between Two Excited He Atoms...mentioning

confidence: 91%

Section: Decay (Icd) Takes Places Either Between Two Excited He Atoms...mentioning

confidence: 99%

Section: Decay (Icd) Takes Places Either Between Two Excited He Atoms...mentioning

confidence: 99%

Section: Decay (Icd) Takes Places Either Between Two Excited He Atoms...mentioning

confidence: 99%

Section: Decay (Icd) Takes Places Either Between Two Excited He Atoms...mentioning

confidence: 99%

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Time-resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-doped Helium Nanodroplets

D.¹,

Michiels²,

Bangert³

et al. 2022

Preprint

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Ultrafast Dynamics in Helium Droplets

Bruder

Koch

Mudrich

et al. 2022

Topics in Applied Physics

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Helium nanodroplets are peculiar systems, as condensed superfluid entities on the nanoscale, and as vessels for studies of molecules and molecular aggregates and their quantum properties at very low temperature. For both aspects, the dynamics upon the interaction with light is fundamental for understanding the properties of the systems. In this chapter we focus on time-resolved experiments in order to study ultrafast dynamics in neat as well as doped helium nanodroplets. Recent experimental approaches are reviewed, ranging from time-correlated photon detection to femtosecond pump-probe photoelectron and photoion spectroscopy, coherent multidimensional spectroscopy as well as applications of strong laser fields and novel, extreme ultraviolet light sources. The experiments examined in more detail investigate the dynamics of atomic and molecular dopants, including coherent wave packet dynamics and long-lived vibrational coherences of molecules attached to and immersed inside helium droplets. Furthermore, the dynamics of highly-excited helium droplets including interatomic Coulombic decay and nanoplasma states are discussed. Finally, an outlook concludes on the perspectives of time-resolved experiments with helium droplets, including recent options provided by new radiation sources of femto- or even attosecond laser pulses up to the soft X-ray range.

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Time-Resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-Doped Helium Nanodroplets

Michiels

Bangert

et al. 2022

J. Phys. Chem. Lett.

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The autoionization dynamics of superexcited superfluid He nanodroplets doped with Na atoms is studied by extreme-ultraviolet (XUV) time-resolved electron spectroscopy. Following excitation into the higher-lying droplet absorption band, the droplet relaxes into the lowest metastable atomic 1s2s 1,3 S states from which interatomic Coulombic decay (ICD) takes place either between two excited He atoms or between an excited He atom and a Na atom attached to the droplet surface. Four main ICD channels are identified, and their decay times are determined by varying the delay between the XUV pulse and a UV pulse that ionizes the initial excited state and thereby quenches ICD. The decay times for the different channels all fall in the range of ∼1 ps, indicating that the ICD dynamics are mainly determined by the droplet environment. A periodic modulation of the transient ICD signals is tentatively attributed to the oscillation of the bubble forming around the localized He excitation.

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Unravelling the full relaxation dynamics of superexcited helium nanodroplets

Abstract: The relaxation dynamics of superexcited superfluid He nanodroplets is fully unravelled by means of extreme-ultraviolet (XUV) femtosecond electron and ion spectroscopy complemented by time-dependent density functional theory (TDDFT). Three main...

Cited by 15 publications

References 72 publications

Time-resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-doped Helium Nanodroplets

Time-resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-doped Helium Nanodroplets

Ultrafast Dynamics in Helium Droplets

Time-Resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-Doped Helium Nanodroplets

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