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We have investigated the possibility to track and control correlation dynamics of valence electrons in krypton (Kr) initiated by the absorption of one extreme ultraviolet (XUV) photon. In this investigation, pump-probe experiments have been performed where monochromatized single high-harmonics at photon energies 29.6, 32.8, and 35.9 eV have been used as pump to populate different intermediate excited states. A temporally delayed near-infrared (NIR) pulse probes the population of various decay channels via the detection of Kr²⁺ ion yields and its transient profiles. We observe that by varying the NIR pulse intensity within a range from 0.3 x 10¹³ to 2.6 x 10¹³ W cm⁻², the shape of the Kr²+ transient profile changes significantly. We show that by varying the intensity of the NIR pulse, it is possible—(i) to control the ratio between sequential and non-sequential double ionization of Kr; (ii) to selectively probe quantum beating oscillations between Kr+* satellite states that are coherently excited within the bandwidth of the XUV pulse; and (iii) to specifically probe the relaxation dynamics of doubly excited (Kr**) decay channels. Our studies show that the contribution of different ionization and decay channels (i)–(iii) can be altered by the NIR pulse intensity, thus demonstrating an efficient way to control the ionization dynamics in rare gas atoms.
Ultrafast electron dynamics drive phenomena such as photochemical reactions, catalysis, and light harvesting. To capture such dynamics in real-time, femtosecond to attosecond light sources are extensively used. However, an exact match between the excitation photon energy and a characteristic resonance is crucial. High-harmonic generation sources are advantageous in terms of pulse duration but limited in spectral tunability in the vacuum ultraviolet range. Here, we present a monochromatic femtosecond source continuously tunable around 21eV photon energy utilizing the second harmonic of an optical parametric chirped pulse amplification laser system to drive high-harmonic generation. The unique tunability of the source is verified in an experiment probing the interatomic Coulombic decay in doped He nanodroplets across the He absorption bands. Moreover, we achieved intensities sufficient for driving collective processes in multiply excited helium nanodroplets, which have been previously observed only at free electron lasers.
We study the dynamics of avalanche ionization of pure helium nanodroplets activated by a weak extreme-ultraviolet (XUV) pulse and driven by an intense near-infrared (NIR) pulse. In addition to a transient enhancement of ignition of a nanoplasma at short delay times ${\sim}200$ fs, long-term activation of the nanodroplets lasting up to a few nanoseconds is observed. Molecular dynamics simulations suggest that the short-term activation is caused by the injection of seed electrons into the droplets by XUV photoemission. Long-term activation appears due to electrons remaining loosely bound to photoions which form stable 'snowball' structures in the droplets. Thus, we show that XUV irradiation can induce long-lasting changes of the strong-field optical properties of nanoparticles, potentially opening new routes to controlling avalanche-ionization phenomena in nanostructures and condensed-phase systems.
XUV fluorescence as a probe of interatomic coulombic decay of resonantly excited He nanodroplets
(2026)
Superfluid He nanodroplets resonantly excited by extreme ultraviolet (XUV) pulses can relax via interatomic coulombic decay (ICD), generally considered an ultrafast process. Here, we introduce a novel approach to probe the dynamics of ICD in He nanodroplets over timescales ranging from femtoseconds to nanoseconds. Our method relies on detecting XUV fluorescence emitted from the nanodroplets as they are driven into a nanoplasma by subsequent intense infrared pulses. Nanoplasma ignition is facilitated by tunnel ionization of XUV-excited He∗ atoms attached to the droplets; it thus serves as a sensitive probe of their relaxation dynamics. The observed nanosecond-scale decay is attributed to ICD between pairs of He∗ atoms undergoing roaming motion on the droplet surface, as supported by quantum-mechanical and classical model calculations.
Studies of ultrafast dynamics in substrate-free nanoparticles at ELI using Timepix3 optical camera
(2025)
We present a novel application of the Timepix3 optical camera (Tpx3Cam) for investigating ultrafast dynamics in substrate-free nanoparticles at the Extreme Light Infrastructure European Research Infrastructure Consortium (ELI ERIC). The camera, integrated into an ion imaging system based on a micro-channel plate (MCP) and a fast P47 scintillator, enables individual time-stamping of incoming ions with nanosecond timing precision and high spatial resolution. The detector successfully captured laser-induced ion events originating from free nanoparticles disintegrated by intense laser pulses. Owing to the broad size distribution of the nanoparticles (10-500 nm) and the variation in laser intensities within the interaction volume, the detected events range in occupancy from near-zero to extremely high, approaching the readout limits of the detector. By combining time-of-flight and velocity map imaging (VMI) techniques, detailed post-processing and analysis were performed. The results presented here focus on the performance of Tpx3Cam under high-occupancy conditions, which are of particular relevance to this study. These conditions approach the limitations imposed by the camera readout capabilities and challenge the effectiveness of standard post-processing algorithms. We investigated these limitations and associated trade-offs, and we present improved methods and algorithms designed to extract the most informative features from the data.
Studies of ultrafast dynamics in substrate-free nanoparticles at ELI using Timepix3 optical camera
(2026)
We present a novel application of the Timepix3 optical camera (Tpx3Cam) for investigating ultrafast dynamics in substrate-free nanoparticles at the Extreme Light Infrastructure European Research Infrastructure Consortium (ELI ERIC). The camera, integrated into an ion imaging system based on a micro-channel plate (MCP) and a fast P47 scintillator with nanosecond scale response time, enables individual time-stamping of incoming ions with nanosecond timing precision and high spatial resolution. The detector successfully captured laser-induced ion events originating from free nanoparticles disintegrated by intense laser pulses. Owing to the broad size distribution of the nanoparticles (10–500 nm) and the variation in laser intensities within the interaction volume, the detected events range in occupancy from near-zero to extremely high, approaching the readout limits of the detector. By combining time-of-flight and velocity map imaging (VMI) techniques, detailed post-processing and analysis were performed. The results presented here focus on the performance of Tpx3Cam under high-occupancy conditions, which are of particular relevance to this study. These conditions approach the limitations imposed by the camera’s readout capabilities and challenge the effectiveness of standard post-processing algorithms. We investigated these limitations and associated trade-offs, and we present improved methods and algorithms designed to extract the most informative features from the data.

