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- Asmussen, J. D., et al.
(author)
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Unravelling the full relaxation dynamics of superexcited helium nanodroplets
- 2021
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In: Physical Chemistry Chemical Physics. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 23:28, s. 15138-15149
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Journal article (peer-reviewed)abstract
- The relaxation dynamics of superexcited superfluid He nanodroplets is thoroughly investigated by means of extreme-ultraviolet (XUV) femtosecond electron and ion spectroscopy complemented by time-dependent density functional theory (TDDFT). Three main paths leading to the emission of electrons and ions are identified: droplet autoionization, pump-probe photoionization, and autoionization induced by re-excitation of droplets relaxing into levels below the droplet ionization threshold. The most abundant product ions are He-2(+), generated by droplet autoionization and by photoionization of droplet-bound excited He atoms. He+ appear with some pump-probe delay as a result of the ejection He atoms in their lowest excited states from the droplets. The state-resolved time-dependent photoelectron spectra reveal that intermediate excited states of the droplets are populated in the course of the relaxation, terminating in the lowest-lying metastable singlet and triplet He atomic states. The slightly faster relaxation of the triplet state compared to the singlet state is in agreement with the simulation showing faster formation of a bubble around a He atom in the triplet state.
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- Michiels, R., et al.
(author)
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Enhancement of above Threshold Ionization in Resonantly Excited Helium Nanodroplets
- 2021
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In: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 127
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Journal article (peer-reviewed)abstract
- Clusters and nanodroplets hold the promise of enhancing high-order nonlinear optical effects due to their high local density. However, only moderate enhancement has been demonstrated to date. Here, we report the observation of energetic electrons generated by above-threshold ionization (ATI) of helium (He) nanodroplets which are resonantly excited by ultrashort extreme ultraviolet (XUV) free-electron laser pulses and subsequently ionized by near-infrared (NIR) or near-ultraviolet (UV) pulses. The electron emission due to high-order ATI is enhanced by several orders of magnitude compared with He atoms. The crucial dependence of the ATI intensities with the number of excitations in the droplets suggests a local collective enhancement effect.
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- Uhl, D., et al.
(author)
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Extreme Ultraviolet Wave Packet Interferometry of the Autoionizing HeNe Dimer
- 2022
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In: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 13:36, s. 8470-8476
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Journal article (peer-reviewed)abstract
- Femtosecond extreme ultraviolet wave packet interferometry (XUV-WPI) was applied to study resonant interatomic Coulombic decay (ICD) in the HeNe dimer. The high demands on phase stability and sensitivity for vibronic XUV-WPI of molecular-beam targets are met using an XUV phase-cycling scheme. The detected quantum interferences exhibit vibronic dephasing and rephasing signatures along with an ultrafast decoherence assigned to the ICD process. A Fourier analysis reveals the molecular absorption spectrum with high resolution. The demonstrated experiment shows a promising route for the real-time analysis of ultrafast ICD processes with both high temporal and high spectral resolution. © 2022 American Chemical Society.
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- Asmussen, J. D., et al.
(author)
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Time-Resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-Doped Helium Nanodroplets
- 2022
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In: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 13:20, s. 4470-4478
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Journal article (peer-reviewed)abstract
- The autoionization dynamics of super excited superfluid He nanodropletsdoped with Na atoms is studied by extreme-ultraviolet (XUV) time-resolved electronspectroscopy. Following excitation into the higher-lying droplet absorption band, the dropletrelaxes into the lowest metastable atomic 1s2s1,3Sstates from which interatomic Coulombicdecay (ICD) takes place either between two excited He atoms or between an excited He atomand a Na atom attached to the droplet surface. Four main ICD channels are identified, andtheir decay times are determined by varying the delay between the XUV pulse and a UV pulsethat ionizes the initial excited state and thereby quenches ICD. The decay times for thedifferent channels all fall in the range of similar to 1 ps, indicating that the ICD dynamics are mainlydetermined by the droplet environment. A periodic modulation of the transient ICD signals istentatively attributed to the oscillation of the bubble forming around the localized Heexcitation
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- Uhl, D., et al.
(author)
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Improved stabilization scheme for extreme ultraviolet quantum interference experiments
- 2022
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In: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 55
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Journal article (peer-reviewed)abstract
- Interferometric pump-probe experiments in the extreme ultraviolet (XUV) domain are experimentally very challenging due to the high phase stability required between the XUV pulses. Recently, an efficient phase stabilization scheme was introduced for seeded XUV free electron lasers (FELs) combining shot-to-shot phase modulation with lock-in detection [A. Wituschek et al., Nat Commun 11, 1 (2020)]. This method stabilized the seed laser beampath on the fundamental ultraviolet wavelength to a high degree. Here, we extend this scheme including the stabilization of the XUV beampath, incorporating phase fluctuations from the FEL high gain harmonic generation process. Our analysis reveals a clear signal improvement with the new method compared to the previous stabilization scheme.
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