Recombination dynamics of clusters in intense extreme-ultraviolet and near- infrared fields

We investigate electron-ion recombination processes in clusters exposed to intense extreme-ultraviolet (XUV) or near-infrared (NIR) pulses. Using the technique of reionization of excited atoms from recombination (REAR), recently introduced in Schütte et al (2014 Phys. Rev. Lett. 112 253401), a large population of excited atoms, which are formed in the nanoplasma during cluster expansion, is identified under both ionization conditions. For intense XUV ionization of clusters, we find that the significance of recombination increases for increasing cluster sizes. In addition, larger fragments are strongly affected by recombination as well, as shown for the case of dimers. We demonstrate that for mixed Ar–Xe clusters exposed to intense NIR pulses, excited atoms and ions are preferentially formed in the Xe core. As a result of electron-ion recombination, higher charge states of Xe are efficiently suppressed, leading to an overall reduced expansion speed of the cluster core in comparison to the shell

Recombination dynamics of clusters in intense extreme-ultraviolet and near-infrared fields

We investigate electron-ion recombination processes in clusters exposed to intense extreme-ultraviolet (XUV) or near-infrared (NIR) pulses. Using the technique of reionization of excited atoms from recombination (REAR), recently introduced in Schütte et al (2014 Phys. Rev. Lett. 112 253401), a large population of excited atoms, which are formed in the nanoplasma during cluster expansion, is identified under both ionization conditions. For intense XUV ionization of clusters, we find that the significance of recombination increases for increasing cluster sizes. In addition, larger fragments are strongly affected by recombination as well, as shown for the case of dimers. We demonstrate that for mixed Ar–Xe clusters exposed to intense NIR pulses, excited atoms and ions are preferentially formed in the Xe core. As a result of electron-ion recombination, higher charge states of Xe are efficiently suppressed, leading to an overall reduced expansion speed of the cluster core in comparison to the shell

Recombination dynamics of clusters in intense extreme-ultraviolet and near-infrared fields

We investigate electron-ion recombination processes in clusters exposed to intense extreme-ultraviolet (XUV) or near-infrared (NIR) pulses. Using the technique of reionization of excited atoms from recombination (REAR), recently introduced in Schütte et al (2014 Phys. Rev. Lett. 112 253401), a large population of excited atoms, which are formed in the nanoplasma during cluster expansion, is identified under both ionization conditions. For intense XUV ionization of clusters, we find that the significance of recombination increases for increasing cluster sizes. In addition, larger fragments are strongly affected by recombination as well, as shown for the case of dimers. We demonstrate that for mixed Ar–Xe clusters exposed to intense NIR pulses, excited atoms and ions are preferentially formed in the Xe core. As a result of electron-ion recombination, higher charge states of Xe are efficiently suppressed, leading to an overall reduced expansion speed of the cluster core in comparison to the shell

THz streak camera performance for single-shot characterization of XUV pulses with complex temporal structures

The THz-field-driven streak camera has proven to be a powerful diagnostic-technique that enables the shot-to-shot characterization of the duration and the arrival time jitter of free electron laser (FEL) pulses. Here we investigate the performance of three computational approaches capable to determine the duration of FEL pulses with complex temporal structures from single-shot measurements of up to three simultaneously recorded spectra. We use numerically simulated FEL pulses in order to validate the accuracy of the pulse length retrieval in average as well as in a single-shot mode. We discuss requirements for the THz field strength in order to achieve reliable results and compare our numerical study with the analysis of experimental data that were obtained at the FEL in Hamburg - FLASH. © 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreemen

Autoionization following nanoplasma formation in atomic and molecular clusters

Nanoplasmas resulting from the ionization of nano-scale particles by intense laser pulses are typically described by quasiclassical models, where electron emission is understood to take place via thermal processes. Recently, we discovered that, following the interaction of intense near-infrared (NIR) laser pulses with molecular oxygen clusters, electron emission from nanoplasmas can also occur from atomic bound states via autoionization [Schütte et al., Phys. Rev. Lett. 114, 123002 (2015)]. Here we extend these studies and demonstrate that the formation and decay of doubly-excited atoms and ions is a very common phenomenon in nanoplasmas. We report on the observation of autoionization involving spin-orbit excited states in molecular oxygen and carbon dioxide clusters as well as in atomic krypton and xenon clusters ionized by intense NIR pulses, for which we find clear bound-state signatures in the electron kinetic energy spectra. By applying terahertz (THz) streaking, we show that the observed autoionization processes take place on a picosecond to nanosecond timescale after the interaction of the NIR laser pulse with the clusters

Plasma channel formation in NIR laser-irradiated carrier gas from an aerosol nanoparticle injector

Aerosol nanoparticle injectors are fundamentally important for experiments where container-free sample handling is needed to study isolated nanoparticles. The injector consists of a nebuliser, a differential pumping unit, and an aerodynamic lens to create and deliver a focused particle beam to the interaction point inside a vacuum chamber. The tightest focus of the particle beam is close to the injector tip. The density of the focusing carrier gas is high at this point. We show here how this gas interacts with a near infrared laser pulse (800 nm wavelength, 120 fs pulse duration) at intensities approaching 10(16) Wcm(-2). We observe acceleration of gas ions to kinetic energies of 100s eV and study their energies as a function of the carrier gas density. Our results indicate that field ionisation by the intense near-infrared laser pulse opens up a plasma channel behind the laser pulse. The observations can be understood in terms of a Coulomb explosion of the created underdense plasma channel. The results can be used to estimate gas background in experiments with the injector and they open up opportunities for a new class of studies on electron and ion dynamics in nanoparticles surrounded by a low-density gas

Correlated electronic decay in expanding clusters triggered by intense XUV pulses from a Free-Electron-Laser

Irradiation of nanoscale clusters and large molecules with intense laser pulses transforms them into highly-excited non- equilibrium states. The dynamics of intense laser-cluster interaction is encoded in electron kinetic energy spectra, which contain signatures of direct photoelectron emission as well as emission of thermalized nanoplasma electrons. In this work we report on a so far not observed spectrally narrow bound state signature in the electron kinetic energy spectra from mixed Xe core - Ar shell clusters ionized by intense extreme-ultraviolet (XUV) pulses from a free-electron-laser. This signature is attributed to the correlated electronic decay (CED) process, in which an excited atom relaxes and the excess energy is used to ionize the same or another excited atom or a nanoplasma electron. By applying the terahertz field streaking principle we demonstrate that CED-electrons are emitted at least a few picoseconds after the ionizing XUV pulse has ended. Following the recent finding of CED in clusters ionized by intense near-infrared laser pulses, our observation of CED in the XUV range suggests that this process is of general relevance for the relaxation dynamics in laser produced nanoplasmas

Mapping ultrafast ionization of atoms and clusters with terahertz-streaking delay

We apply THz-field streaking to temporally resolve the ultrafast ionization of neutral cluster vs atomic targets exposed to intense ultrashort soft x-ray pulses from a free-electron laser (FEL). In the experiment pristine Xe and mixed Xe/Ar clusters as well as Xe atoms are ionized in the vicinity of the $4d→ɛf$ giant resonance of Xe. We compare the relative streaking delay between the center-of-mass oscillations of electrons that have final kinetic energies in the spectral region of the Xe($4d$) photoline. Our results show that clusters are ionized at the beginning of the 100 fs FEL pulse as supported by calculations of target frustration in the focal volume. We have identified a significantly larger 40 fs relative streaking delay between mixed Xe-Ar clusters vs Xe atoms compared to a 15 fs relative delay found for pristine Xe clusters. This is attributed to the high sensitivity of our spectroscopic measurement to the degree of condensation of the cluster target. Our results show that THz streaking is a powerful technique to temporally study electron emission from extended targets under intense FEL radiation on time scales that are significantly shorter than the FEL pulse duration