Nanoplasma Formation Research Articles

Nanoplasma formation and expansion ignited by an intense FEL: a study using pump-probe electron spectroscopy

Abstract We demonstrate real-time observations of nanoplasma formation and expansion using intense extreme-ultraviolet (XUV) and near-infrared (NIR) pump--probe electron spectroscopy. We identified the formation of a nanoplasma by the sudden enhancement of low-energy electron emission within a few tens of femtoseconds after XUV excitation, which indicates considerable heating of the clusters by the NIR field. 
We probed the subsequent expansion of the nanoplasma by monitoring the transient resonant enhancement of high-energy electron emission. The dependence of the resonance on the XUV intensity is explained by the expansion speed of the XUV-induced nanoplasma.

Ion imaging of spatially inhomogeneous nanoplasmas in NaCl particles.

Studying photoemission from free, unsupported aerosol particles is a powerful method for gaining insight into light-matter interactions at the nanoscale. We used single-shot velocity map imaging to experimentally measure kinetic energy and angular distributions of ions emitted following interaction of sub-micrometer NaCl particles with femtosecond pulses of near infrared (NIR, 800 nm) and ultraviolet (UV, 266 nm) light. We combined this with time-dependent simulations of light propagation through the particles and a rate equation approach to computationally address the origin of the observed ion emission. For both NIR and UV pulses, ion emission is caused by the formation of an under-dense nanoplasma with similar densities, although using an order of magnitude weaker UV intensities. Such conditions result in remarkably similar ion fragments with similar kinetic energies, and no obvious influence of the plasma formation mechanism (photoionization or collisional ionization). Our data suggests that Coulomb explosion does not play a significant role for ion emission, and we discuss alternative mechanisms that can lead to material ablation from under-dense nanoplasma. Finally, we show how finite size effects play an important role in photoemission through generation of spatially inhomogeneous nanoplasmas, which result in asymmetric ion emission that depends on particle size and laser wavelength. By utilizing the single-particle information available from our experiments, we show how finite size effects and inhomogeneous nanoplasma formation can be exploited to retrieve the size and orientation of individual submicrometer aerosol particles.

Ionization of Xenon Clusters by a Hard X-ray Laser Pulse

Ultrashort pulse X-ray free electron lasers (XFFLs) provided us with an unprecedented regime of X-ray intensities, revolutionizing ultrafast structure determination and paving the way to the novel field of non-linear X-ray optics. While pioneering studies revealed the formation of a nanoplasma following the interaction of an XFEL pulse with nanometer-scale matter, nanoplasma formation and disintegration processes are not completely understood, and the behavior of trapped electrons in the electrostatic potential of highly charged species is yet to be decrypted. Here we report the behavior of the nanoplasma created by a hard X-ray pulse interacting with xenon clusters by using electron and ion spectroscopy. To obtain a deep insight into the formation and disintegration of XFEL-ignited nanoplasma, we studied the XFEL-intensity and cluster-size dependencies of the ionization dynamics. We also present the time-resolved data obtained by a near-infrared (NIR) probe pulse in order to experimentally track the time evolution of plasma electrons distributed in the XFEL-ignited nanoplasma. We observed an unexpected time delay dependence of the ion yield enhancement due to the NIR pulse heating, which demonstrates that the plasma electrons within the XFEL-ignited nanoplasma are inhomogeneously distributed in space.

Surface plasma resonance in Xe clusters studied by EUV pump-NIR probe experiments

The ionization dynamics of Xe cluster was analyzed by extreme ultraviolet (EUV) pump-near infrared (NIR) probe experiments. The experiments were carried out for Xe clusters containing around 5000 atoms on average at the SPring-8 Compact SASE Source (SCSS) test accelerator in Japan. We recorded ion spectra emitted from Xe clusters as a function of the time delay between the EUV and NIR pulses. The ion yields up to highly-charged states were substantially enhanced when Xe clusters excited by the EUV pulses were illuminated by the NIR laser pulses at 1 to 2 ps after the pump pulse, providing a compelling evidence for nano-plasma formation and subsequent NIR absorption via surface plasma resonance. We also observed emergence of low kinetic energy Xe+ at long time delay, which can be attributed to the ionization of excited neutral atoms resulting from the electron-ion recombination in the expanding nano-plasma.

Imaging plasma formation in isolated nanoparticles with ultrafast resonant scattering

We have recorded the diffraction patterns from individual xenon clusters irradiated with intense extreme ultraviolet pulses to investigate the influence of light-induced electronic changes on the scattering response. The clusters were irradiated with short wavelength pulses in the wavelength regime of different 4d inner-shell resonances of neutral and ionic xenon, resulting in distinctly different optical properties from areas in the clusters with lower or higher charge states. The data show the emergence of a transient structure with a spatial extension of tens of nanometers within the otherwise homogeneous sample. Simulations indicate that ionization and nanoplasma formation result in a light-induced outer shell in the cluster with a strongly altered refractive index. The presented resonant scattering approach enables imaging of ultrafast electron dynamics on their natural timescale.

Electron spectroscopic study of nanoplasma formation triggered by intense soft x-ray pulses.

Using electron spectroscopy, we investigated the nanoplasma formation process generated in xenon clusters by intense soft x-ray free electron laser (FEL) pulses. We found clear FEL intensity dependence of electron spectra. Multistep ionization and subsequent ionization frustration features are evident for the low FEL-intensity region, and the thermal electron emission emerges at the high FEL intensity. The present FEL intensity dependence of the electron spectra is well addressed by the frustration parameter introduced by Arbeiter and Fennel [New J. Phys. 13, 053022 (2011)].

Recombination-Enhanced Surface Expansion of Clusters in Intense Soft X-Ray Laser Pulses.

We studied the nanoplasma formation and explosion dynamics of single large xenon clusters in ultrashort, intense x-ray free-electron laser pulses via ion spectroscopy. The simultaneous measurement of single-shot diffraction images enabled a single-cluster analysis that is free from any averaging over the cluster size and laser intensity distributions. The measured charge state-resolved ion energy spectra show narrow distributions with peak positions that scale linearly with final ion charge state. These two distinct signatures are attributed to highly efficient recombination that eventually leads to the dominant formation of neutral atoms in the cluster. The measured mean ion energies exceed the value expected without recombination by more than an order of magnitude, indicating that the energy release resulting from electron-ion recombination constitutes a previously unnoticed nanoplasma heating process. This conclusion is supported by results from semiclassical molecular dynamics simulations.

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 [Schutte 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.

Ionization Avalanching in Clusters Ignited by Extreme-Ultraviolet Driven Seed Electrons.

We study the ionization dynamics of Ar clusters exposed to ultrashort near-infrared (NIR) laser pulses for intensities well below the threshold at which tunnel ionization ignites nanoplasma formation. We find that the emission of highly charged ions up to Ar^{8+} can be switched on with unit contrast by generating only a few seed electrons with an ultrashort extreme-ultraviolet (XUV) pulse prior to the NIR field. Molecular dynamics simulations can explain the experimental observations and predict a generic scenario where efficient heating via inverse bremsstrahlung and NIR avalanching is followed by resonant collective nanoplasma heating. The temporally and spatially well-controlled injection of the XUV seed electrons opens new routes for controlling avalanching and heating phenomena in nanostructures and solids, with implications for both fundamental and applied laser-matter science.

Hydrodynamic model for expansion and collisional relaxation of x-ray laser-excited multi-component nanoplasma

The irradiation of an atomic cluster with a femtosecond x-ray free-electron laser pulse results in a nanoplasma formation. This typically occurs within a few hundred femtoseconds. By this time the x-ray pulse is over, and the direct photoinduced processes no longer contributing. All created electrons within the nanoplasma are thermalized. The nanoplasma thus formed is a mixture of atoms, electrons, and ions of various charges. While expanding, it is undergoing electron impact ionization and three-body recombination. Below we present a hydrodynamic model to describe the dynamics of such multi-component nanoplasmas. The model equations are derived by taking the moments of the corresponding Boltzmann kinetic equations. We include the equations obtained, together with the source terms due to electron impact ionization and three-body recombination, in our hydrodynamic solver. Model predictions for a test case, expanding spherical Ar nanoplasma, are obtained. With this model, we complete the two-step approach to simulate x-ray created nanoplasmas, enabling computationally efficient simulations of their picosecond dynamics. Moreover, the hydrodynamic framework including collisional processes can be easily extended for other source terms and then applied to follow relaxation of any finite non-isothermal multi-component nanoplasma with its components relaxed into local thermodynamic equilibrium.

Correlated electronic decay following intense near-infrared ionization of clusters

We report on a novel correlated electronic decay process following extensive Rydberg atom formation in clusters ionized by intense near-infrared fields. A peak close to the atomic ionization potential is found in the electron kinetic energy spectrum. This new contribution is attributed to an energy transfer between two electrons, where one electron decays from a Rydberg state to the ground state and transfers its excess energy to a weakly bound cluster electron in the environment that can escape from the cluster. The process is a result of nanoplasma formation and is therefore expected to be important, whenever intense laser pulses interact with nanometer-sized particles.

Observation of correlated electronic decay in expanding clusters triggered by near-infrared fields.

When an excited atom is embedded into an environment, novel relaxation pathways can emerge that are absent for isolated atoms. A well-known example is interatomic Coulombic decay, where an excited atom relaxes by transferring its excess energy to another atom in the environment, leading to its ionization. Such processes have been observed in clusters ionized by extreme-ultraviolet and X-ray lasers. Here, we report on a correlated electronic decay process that occurs following nanoplasma formation and Rydberg atom generation in the ionization of clusters by intense, non-resonant infrared laser fields. Relaxation of the Rydberg states and transfer of the available electronic energy to adjacent electrons in Rydberg states or quasifree electrons in the expanding nanoplasma leaves a distinct signature in the electron kinetic energy spectrum. These so far unobserved electron-correlation-driven energy transfer processes may play a significant role in the response of any nano-scale system to intense laser light.

Ionization dynamics of Xe nanoplasma formation studied with XUV fluorescence spectroscopy

Intense pulses from a short wavelength free-electron laser turn xenon nanoparticles into a high energy density nanoplasma within femtoseconds. Recently, the generation of multiply charged xenon ions during the initial phase of plasma evolution has been studied by energy-resolved XUV fluorescence detection as a function of cluster size and cluster composition []. In the present contribution we give a detailed analysis of the corresponding radiative transitions after resonant excitation of the 4d electron shell at intensities of 2 × 1012 − 2.45 × 1015 W cm−2. The evaluation of charge-state specific fluorescence yields as a function of FEL power density demonstrates that plasma effects such as ionization potential lowering, electron impact excitation, ionization, and energy redistribution govern the laser-induced non-equilibrium dynamics in xenon clusters.

Nanoplasma Formation by High Intensity Hard X-rays.

Using electron spectroscopy, we have investigated nanoplasma formation from noble gas clusters exposed to high-intensity hard-x-ray pulses at ~5 keV. Our experiment was carried out at the SPring-8 Angstrom Compact free electron LAser (SACLA) facility in Japan. Dedicated theoretical simulations were performed with the molecular dynamics tool XMDYN. We found that in this unprecedented wavelength regime nanoplasma formation is a highly indirect process. In the argon clusters investigated, nanoplasma is mainly formed through secondary electron cascading initiated by slow Auger electrons. Energy is distributed within the sample entirely through Auger processes and secondary electron cascading following photoabsorption, as in the hard x-ray regime there is no direct energy transfer from the field to the plasma. This plasma formation mechanism is specific to the hard-x-ray regime and may, thus, also be important for XFEL-based molecular imaging studies. In xenon clusters, photo- and Auger electrons contribute more significantly to the nanoplasma formation. Good agreement between experiment and simulations validates our modelling approach. This has wide-ranging implications for our ability to quantitatively predict the behavior of complex molecular systems irradiated by high-intensity hard x-rays.

Transformations induced in bulk amorphous silica by ultrafast laser direct writing

A transmission electron microscopy study of nanogratings formed in bulk amorphous silica by direct writing with an ultrafast pulsed laser with a radiation wavelength of 1030 nm and pulse duration of 560 fs is presented. The results achieved show that the nanogratings are composed of planar nanostructures with an average periodicity of 250 nm and typical thickness of about 30 nm, consisting of alternating layers of heavily damaged material and layers of material where a dense precipitation of nanocrystals occurred. The crystallization of silica to form these nanocrystals can be explained by the large pressures and temperatures reached in these regions as a result of nanoplasma formation and recombination.

Frustration of photoionization of Ar nanoplasma produced by extreme ultraviolet FEL pulses

We report on the laser power dependence of photoabsorptions of Ar clusters irradiated by extreme ultraviolet–free electron laser (EUV–FEL) at the wavelength of 62 nm. We measured kinetic energy distributions of fragment ions with our ion momentum spectrometer. From the measured kinetic energy distributions, we estimated charge states of irradiated Ar clusters using the classical uniformly charged sphere model. Our results show that the EUV–FEL irradiation of Ar clusters results in the frustration of direct photoionization leading to nanoplasma formation and subsequent strong electron–ion charge recombination.

Ionization heating in rare-gas clusters under intense XUV laser pulses

The interaction of intense extreme ultraviolet (XUV) laser pulses ($\ensuremath{\lambda}=32 \mathrm{nm}$, $I={10}^{11}--{10}^{14}$ W/cm${}^{2}$) with small rare-gas clusters (${\mathrm{Ar}}_{147}$) is studied by quasiclassical molecular dynamics simulations. Our analysis supports a very general picture of the charging and heating dynamics in finite samples under short-wavelength radiation that is of relevance for several applications of free-electron lasers. First, up to a certain photon flux, ionization proceeds as a series of direct photoemission events producing a jellium-like cluster potential and a characteristic plateau in the photoelectron spectrum as observed in Bostedt et al. [Phys. Rev. Lett. 100, 133401 (2008)]. Second, beyond the onset of photoelectron trapping, nanoplasma formation leads to evaporative electron emission with a characteristic thermal tail in the electron spectrum. A detailed analysis of this transition is presented. Third, in contrast to the behavior in the infrared or low vacuum ultraviolet range, the nanoplasma energy capture proceeds via ionization heating, i.e., inner photoionization of localized electrons, whereas collisional heating of conduction electrons is negligible up to high laser intensities. A direct consequence of the latter is a surprising evolution of the mean energy of emitted electrons as function of laser intensity.

Extreme multielectron ionization of elemental clusters in ultraintense laser fields

AbstractIn this paper we present computational and theoretical studies of extreme multielectron ionization in Xen clusters (n = 55‐2171, initial cluster radii R0 = 8.7‐31.0 Å) driven by ultraintense Gaussian infrared laser fields (peak intensity IM = 1015‐1020 W cm−2, temporal pulse length τ = 10‐100 fs, and frequency v = 0.35fs−1). The microscopic approach, which rests on three sequential‐parallel processes of inner ionization, nanoplasma formation, and outer ionization, properly describes the high ionization levels (with the formation of {Xeq+}n with q = 5‐36), the inner/outer cluster ionization mechanisms, and the nanoplasma response. The cluster size and laser intensity dependence of the inner ionization levels are determined by a complex superposition of laser‐induced barrier suppression ionization (BSI), with the contributions of the inner field BSI manifesting ignition enhancement and screening retardation effects, together with electron impact ionization. The positively charged nanoplasma produced by inner ionization reveals intensity‐dependent spatial inhomogeneity and spatial anisotropy, and can be either persistent (at lower intensities) or transient (at higher intensities). The nanoplasma is depleted by outer ionization that was semiquantitatively described by the cluster barrier suppression electrostatic model, which accounts for the cluster size, laser intensity, and pulse length dependence of the outer ionization yield.

Extreme ionization of Xe clusters driven by ultraintense laser fields

We applied theoretical models and molecular dynamics simulations to explore extreme multielectron ionization in Xe(n) clusters (n=2-2171, initial cluster radius R(0)=2.16-31.0 A) driven by ultraintense infrared Gaussian laser fields (peak intensity I(M)=10(15)-10(20) W cm(-2), temporal pulse length tau=10-100 fs, and frequency nu=0.35 fs(-1)). Cluster compound ionization was described by three processes of inner ionization, nanoplasma formation, and outer ionization. Inner ionization gives rise to high ionization levels (with the formation of [Xe(q+)](n) with q=2-36), which are amenable to experimental observation. The cluster size and laser intensity dependence of the inner ionization levels are induced by a superposition of barrier suppression ionization (BSI) and electron impact ionization (EII). The BSI was induced by a composite field involving the laser field and an inner field of the ions and electrons, which manifests ignition enhancement and screening retardation effects. EII was treated using experimental cross sections, with a proper account of sequential impact ionization. At the highest intensities (I(M)=10(18)-10(20) W cm(-2)) inner ionization is dominated by BSI. At lower intensities (I(M)=10(15)-10(16) W cm(-2)), where the nanoplasma is persistent, the EII contribution to the inner ionization yield is substantial. It increases with increasing the cluster size, exerts a marked effect on the increase of the [Xe(q+)](n) ionization level, is most pronounced in the cluster center, and manifests a marked increase with increasing the pulse length (i.e., becoming the dominant ionization channel (56%) for Xe(2171) at tau=100 fs). The EII yield and the ionization level enhancement decrease with increasing the laser intensity. The pulse length dependence of the EII yield at I(M)=10(15)-10(16) W cm(-2) establishes an ultraintense laser pulse length control mechanism of extreme ionization products.