Laser-cluster Interaction Research Articles

Ionization dynamics of sub-micrometer-sized clusters in intense ultrafast laser pulses

Sub-micrometer-sized targets are found in intense laser–cluster interaction experiments and laser-based material processing. Here, we investigate the internal field localization due to Mie scattering and its effect on ionization dynamics in sub-micrometer-sized clusters using Mie calculation and particle-in-cell simulations. As a result of intertwined processes of pulse propagation and ionization, sub-micrometer nanofocusing dominates at lower intensity and gives rise to an ionization hotspot at the rear of the targets while plasma shielding wins over at a higher intensity, stopping further rear side ionization. As ionization is often the precursor of other processes, understanding the ionization dynamics of ultrafast laser pulses with wavelength-sized nanostructure can be relevant for intense laser-cluster experiments and femtosecond laser micro-/nanomachining.

Cluster size determination using shadowgraphy measurements

Cluster-jet beams offer a wide variety of possible applications. The advantages of an internal and windowless cluster-jet target make it suitable for many experiments. It is important to know all the properties of the cluster-jet to prepare it for the desired conditions of the respective experiments. An essential property is the size of the clusters and their size distribution. To investigate the size of the clusters shadowgraphy measurements are performed. This article provides an overview of the shadowgraphy method and presents first results of these analyses using hydrogen clusters. These show an average cluster size of a few micrometers, which will also be of high interest, besides the here shown laser cluster interaction, for other installations using cluster beams.

Laser cluster interaction in ambient magnetic fields for accelerating electrons in two stages without external injection

In the few-cycle pulse regime of laser-cluster interaction (intensity >10^{16},text{ W/cm}^{2}, wavelength > 780 nm), laser absorption is mostly collisionless and may happen via anharmonic resonance (AHR) process in the overdense (cluster) plasma potential. Many experiments, theory and simulation show average absorbed energy per cluster-electron ({mathcal {E}_A}) close to the electron’s ponderomotive energy (U_mathrm {p}) in the collisionless regime. In this work, by simple rigid sphere model (RSM) and detailed particle-in-cell (PIC) simulation, we show enhanced {mathcal {E}_A}approx 30–70U_mathrm {p}—a 15–30 fold increase—with an external (crossed) magnetic field near the electron-cyclotron resonance (ECR). Due to relativistic mass increase, electrons quickly deviate from the standard (non-relativistic) ECR, but time-dependent relativistic-ECR (RECR) happens which also contributes to enhanced {mathcal {E}_A}. Here laser is coupled to electrons in two stages, i.e, AHR and ECR/RECR. To probe further we retrieve the phase-difference Delta psi between the driving electric field and corresponding velocity component for each electron (in PIC and RSM). We find absorption by electron via AHR happens in a very short interval Delta tau for less than half a laser period where Delta psi remains close to pi (necessary condition for maximum laser absorption) and then Delta psi drops to its initial pi /2 (meaning no absorption) after such short-lived AHR. On the contrary, auxiliary magnetic field near the ECR modifies AHR scenario inside the cluster and also helps maintaining the required phase Delta psi approx pi for the liberated cluster-electron accompanied by frequency matching for ECR/RECR for a prolonged Delta tau (which covers 50–60% of the laser pulse through pulse maxima) even after AHR—leading to jump in {mathcal {E}_A}approx 30–70U_mathrm {p}. We note that to realize the second stage of enhanced energy coupling via ECR/RECR, the first stage via AHR is necessary.

Investigation of electrical conductivity effects on cluster characteristics of Ar and Xe

The phenomenon of cluster interaction with high-intensity laser pulses is of great scientific importance as well as potential applications. To explain such phenomena, in rare gasses, several models have been proposed, among which the nanoplasma model is the most successful one since it considers interaction that take into account the processes of ionization, heating and explosion simultaneously. However, the reported results need to be completed, enriched and quantified either experimentally or theoretically. In this context, we investigate the effects of femtosecond laser-cluster interactions in argon and xenon noble gasses on several parameters and their interdependences: electrical conductivity, σ, Debye length,λD2, coupling parameter,Γc, loss tangent, tanδ. To do so, we carry out numerical simulations based on the characteristics and assumptions of the nanoplasma model. Several interesting results were deduced for both Ar and Xe, such as: a linear increase of tanδ with ImgλD2 for all investigated values of σ, an increase in σ with normalized Debye length as well as normalized 1/ΓC (with a sharper initial increase) and the imaginary part of 1/ΓC increases linearly with tanδ. It should be noted that all these variations were quantified and new semi empirical formula were deduced. It was also put into evidence that the same mechanism is responsible for the variations of both coupling parameter and the Debye length.

Time-resolved Rayleigh scattering measurements of methane clusters for laser-cluster fusion experiments.

We present a time-resolved analysis of Rayleigh scattering measurements to determine the average size of methane clusters and find the optimum timing for laser-cluster fusion experiments. We measure Rayleigh scattering and determine the average size of methane clusters varying the backing pressure (P0) from 11 bar to 69 bar. Regarding the onset of clustering, we estimate that the average size of methane clusters at the onset of clustering is Nc0≅20 at 11 bar. According to our measurements, the average cluster radius r follows the power law of r∝P01.86. Our ion time-of-flight measurements indicate that we have produced energetic deuterium ions with kT = 52±2 keV after laser-cluster interaction using CD4 gas at 50 bar. We find that this ion temperature agrees with the predicted temperature from CD4 clusters at 50 bar with r = 14 nm assuming the Coulomb explosion model.

Efficient coupling of picosecond laser pulses with (CCl4)n clusters: Linear vs circular polarization

Ionic outcome and electron energy distribution, upon interaction of carbon tetrachloride clusters ((CCl4)n) with picosecond laser pulses of 1064 nm was investigated, to understand influence of linear and circular polarization on the mechanism of laser-cluster interaction. Contrary to the perception regarding higher proficiency of circular polarized laser pulses in collisional heating of ionized cluster, higher yield of multiply charged atomic ions (up to C5+ (I.E. ~ 392 eV) and Cl10+ (I.E. ~ 456.7 eV)) was obtained for linear polarization. Though marginally higher peak and mean electron energy were recorded for circular polarized laser pulses, with electron energy distribution extending up to ~ 300–350 eV. Present studies provide insight about the crucial steps of complex laser-cluster interaction mechanism, where inverse Bremsstrahlung energization of quasi-free electrons and screening effect within the ionized cluster are found to play a decisive role in determining efficiency of laser-cluster interaction.

Generation of Multiply Charged Argon Ions in Nanosecond Laser Field Ionization of Argon Clusters.

Zhang and co-workers ( J. Phys. Chem. Lett. 2020, 11, 1100-1105) have recently reported results of experiments involving irradiation of argon clusters doped with bromofluorene chromophores by nanosecond-long pulses of 532 nm laser light. Multiply charged ions of atomic argon (Arn+, 1 ≤ n ≤ 7) and carbon (Cn+, 1 ≤ n ≤ 4) are observed, which are sought to be rationalized using an evaporation model. The distinguishing facet of exploding clusters being progenitors of energetic ions and electrons constitutes the key driver for contemporary research in laser-cluster interactions; it is, therefore, important to point out inconsistencies that are intrinsic to the model of Zhang and co-workers. In light of similar reports already in the literature, we show that their model is of limited utility in describing the dynamics that govern how fast, multiply charged atomic ions result from laser irradiation of gas-phase clusters. We posit that it is plasma behavior that underpins cluster heating and cluster explosion dynamics.

Spatiotemporal characteristics of high-density gas jet and absolute determination of size and density of gas clusters

Properties of gas clusters such as the size and number density when expanding into the vacuum after passing through a conical nozzle are analyzed for argon at an average density of 1020/cm3. Temporally and spatially resolved size and density distribution were measured from all-optical methods of Rayleigh scattering measurement and Nomarski interferometry using a CW laser. At the gas backing pressure of 80 bar, Ar clusters as large as 100 nm were obtained, which differs significantly from the size estimated by the conventional Hagena scaling law. The two independent methods of cluster characterization presented here would be useful to precisely determine the initial conditions in a variety of intense laser-cluster interaction driven applications such as neutron generation, thermonuclear fusion, efficient x-ray emission, and energetic ion acceleration.

Properties of laser beam passed through cluster plasma studied with diffraction pattern method

The diffraction method is used to study the properties of laser radiation interacting with a gas-cluster plasma. Based on the simulation of propagation a laser beam with a wavelength 800 nm through a hexagon Cu-mesh and subsequently compared with the obtained experimental diffraction pattern, the contribution of the second harmonic to the laser radiation was considered. The capability of this method to reveal the spectral composition of laser radiation is discussed. Also, the dependence of the visibility of the diffraction pattern on the intensity of the laser beam is considered. Besides, the contribution of x-ray radiation generated from the laser-cluster interaction into the observed diffraction pattern signal was estimated.

Modeling radiative-shocks created by laser–cluster interactions

Radiative-shocks induced by laser–cluster interactions are modeled using radiation-hydrodynamic simulations. A good agreement—in both shock velocity and density profiles—is obtained between experiment and simulations, indicating that non-local thermodynamic equilibrium (NLTE) radiative effects are important in the experimental regime examined, particularly at early times (≤30 ns) due to the elevated temperatures (≥35 eV). The enhanced NLTE radiative emission causes the shock to be reduced in amplitude, increased in width, and reduced in propagation velocity, while the amplitude of the radiative precursor is increased. As the density and temperature conditions are relatively modest, this potentially has important implications for the scalings that are used in laboratory–astrophysics to transform between laboratory and astrophysical scales, which do not hold for non-LTE systems.

Quasimonoenergetic Proton Bunch Acceleration Driven by Hemispherically Converging Collisionless Shock in a Hydrogen Cluster Coupled with Relativistically Induced Transparency.

An approach for accelerating a quasimonoenergetic proton bunch via a hemispherically converging collisionless shock created in laser-cluster interactions at the relativistically induced transparency (RIT) regime is studied using three-dimensional particle-in-cell simulations. By the action of focusing a petawatt class laser pulse onto a micron-size spherical hydrogen cluster, a crescent-shaped collisionless shock is launched at the laser-irradiated hemisphere and propagates inward. The shock converges at the sphere center in concurrence with the onset of the RIT, thereby allowing the proton bunch to be pushed out from the shock surface in the laser propagation direction. The proton bunch experiences further acceleration both inside and outside of the cluster to finally exhibit a quasimonoenergetic spectral peak around 300MeV while maintaining a narrow energy spread (∼10%) and a small half-divergence angle (∼5°) via the effect of the RIT. This mechanism works for finite ranges of parameters with threshold values concerning the laser peak intensity and the cluster radius, resulting from the synchronization of the multiple processes in a self-consistent manner. The present scheme utilizing the internal and external degrees of freedom ascribed to the spherical cluster leads to the proton bunch alternative to the plain target, which allows the operation with a high repetition rate and impurity free.

Simulations of a polar molecule (sulfur dioxide) in a supersonic jet

Clustering of polar molecules (SO2) in a supersonic jet was investigated by simulation. The cluster size Nc was calculated under different gas backing pressures P0 and source temperatures T0. Based on these results, the dependence of Nc on P0 or T0 was compared with that for the gases of non-polar molecules. It is found that SO2 molecules condense very easily into clusters even when P0 is very low. This result implies that large clusters can be produced using polar molecules, which could be useful in the studies of laser-cluster interactions. Also, SO2 gas is an important component of air pollution, so the knowledge of the clustering properties of SO2 could be helpful in the study of air pollution and environment.

Dynamical resonance shift and unification of resonances in short-pulse laser-cluster interaction

Pronounced maximum absorption of laser light irradiating a rare-gas or metal cluster is widely expected during the linear resonance (LR) when Mie-plasma wavelength $\lambdaM$ of electrons equals the laser wavelength $\lambda$. On the contrary, by performing molecular dynamics (MD) simulations of an argon cluster irradiated by short 5-fs (fwhm) laser pulses it is revealed that, for a given laser pulse energy and a cluster, at each peak intensity there exists a $\lambda$ -- shifted from the expected $\lambdaM$ -- that corresponds to a {\em unified dynamical} LR at which evolution of the cluster happens through very effective unification of possible resonances in various stages, including (i) the LR in the initial time of plasma creation, (ii) the LR in the Coulomb expanding phase in the later time and (iii) anharmonic resonance in the marginally over-dense regime for a relatively longer pulse duration, leading to maximum laser absorption accompanied by maximum removal of electrons from cluster and also maximum allowed average charge states for the argon cluster. Increasing the laser intensity, the absorption maxima is found to shift to a higher wavelength in the band of $\lambda\approx (1-1.5)\lambdaM$ than permanently staying at the expected $\lambdaM$. A naive rigid sphere model also corroborates the wavelength shift of the absorption peak as found in MD and un-equivocally proves that maximum laser absorption in a cluster happens at a shifted $\lambda$ in the marginally over-dense regime of $\lambda\approx (1-1.5)\lambdaM$ in stead of $\lambdaM$ of LR. Present study may find importance for guiding an optimal condition laser-cluster interaction experiment in the short pulse regime.

(TMT)n clusters as dilute debris-free tin source for generation of multiply charged tin ions-of relevance in extreme ultraviolet (EUV) lithography, under intense laser irradiation.

Multiply charged tin ions ([Sn]8+ to [Sn]13+ ) are considered as ideal-emitters at extreme ultraviolet (EUV) wavelength ~ 13.5 nm, pertinent to advanced micro-electronic device fabrication. Solid tin targets have been widely explored for the generation of these ions, but debris generation has restricted their utilization. Tin-containing molecular clusters have, however, the potential to act as dilute and debris-free sources for the generation of tin ions, as investigated in the present study. Efficient coupling of laser energy with clusters has been utilized for the generation of multiply charged tin ions. The ions generated have been characterized using time-of-flight mass spectrometry. By varying experimental parameters, the yield of multiply charged tin ions has been manipulated, for tetramethyltin (TMT) clusters. In addition, the energetic electrons and photons liberated upon laser-cluster interaction have been probed utilizing an in-house developed retarding field analyser. Interaction of tetramethyltin clusters with 1064 nm picosecond laser pulses of intensity ~ 1013 W/cm2 leads to the generation of multiply charged tin ions (up to [Sn]14+ ) and carbon ions (up to [C]4+ ). Efficient laser-cluster interaction is evident from the generation of multiply charged tin ions with ionization energy ~ 282 eV ([Sn]14+ ). By varying the experimental conditions, the distribution of multiply charged tin ions can be influenced to obtain significant relative ion yield of multiply charged tin ions from [Sn]8+ to [Sn]13+ . Tetramethyltin clusters have the potential to act as dilute and debris-free source for EUV lithographic applications, in contrast to bulk tin targets. The inherent properties of clusters, such as higher local density and the pulsed nature of the cluster source, are appropriate for EUV lithographic applications.

Induced transparency in the XUV: a pump-probe test of laser-cluster interactions

An experiment is proposed to distinguish between different laser-cluster atomistic models and their predictions. The induced transparency of rare-gas clusters, post-interaction with an extreme ultraviolet (XUV) pump-pulse, is predicted by using an atomistic hybrid quantum–classical molecular dynamics model. We find there is an intensity range for which an XUV probe-pulse has no lasting effect on the average charge state of a cluster after being saturated by an XUV pump-pulse: the cluster is transparent to the probe-pulse. Multiple complete experimental signals are calculated which include the effect of the pulse’s spatial distribution as well as the cluster size distribution. The calculated experimental signals and trends are also accomplished with the addition of an ionization potential lowering model that results in effectively removing the induced transparency effect. Thus, the proposed experiment is expected to either find the new phenomenon of induced transparency in clusters or give strong evidence for the existence of the enhanced ionization phenomenon, ionization potential lowering, in nanoplasmas.

Effects of laser-polarization and wiggler magnetic fields on electron acceleration in laser-cluster interaction

We examine the electron dynamics during laser-cluster interaction. In addition to the electrostatic field of an individual cluster and laser field, we consider an external transverse wiggler magnetic field, which plays a pivotal role in enhancing the electron acceleration. Single-particle simulation has been presented with a short pulse linearly polarized as well as circularly polarized laser pulses for electron acceleration in a cluster. The persisting Coulomb field allows the electron to absorb energy from the laser field. The stochastically heated electron finds a weak electric field at the edge of the cluster from where it is ejected. The wiggler magnetic field connects the regions of the stochastically heated, ejected electron from the cluster and high energy gain by the electron from the laser field outside the cluster. This increases the field strength and hence supports the electron to meet the phase of the laser field for enhanced acceleration. A long duration resonance appears with an optimized magnetic wiggler field of about 3.4 kG. Hence, the relativistic energy gain by the electron is enhanced up to a few 100 MeV with an intense short pulse laser with an intensity of about 1019 W cm−2 in the presence of a wiggler magnetic field.

Tailoring Ion Charge State Distribution in Tetramethyltin Clusters under Influence of Moderate Intensity Picosecond Laser Pulse: Role of Laser Wavelength and Rate of Energy Deposition.

Systematic manipulation of ionic-outcome in laser-cluster interaction process has been realized for studies carried out on tetramethyltin (TMT) clusters under picosecond laser conditions, determined by choice of laser wavelength and intensity. As a function of laser intensity, TMT clusters exhibit gradual enhancement in overall ionization of its cluster constituents, up to a saturation level of ionization, which was distinct for different wavelengths (266, 355, and 532 nm). Simultaneously, systematic appearance of higher multiply charged atomic ions and shift in relative abundance of multiply charged atomic ions towards higher charge state was observed, using time-of-flight mass spectrometer. At saturation level, multiply charged atomic ions up to (C2+, Sn2+) at 266 nm, (C4+, Sn4+) at 355 nm, and (C4+, Sn6+) at 532 nm were detected. In addition, at 355 nm intra-cluster ion chemistry within the ionized cluster leads to generation of molecular hydrogen ion (H2+) and triatomic molecular hydrogen ion (H3+). Generation of multiply charged atomic ions is ascribed to efficient coupling of laser pulse with the cluster media, facilitated by inner-ionized electrons produced within the cluster, at the leading edge of laser pulse. Role of inner-ionized electrons is authenticated by measuring kinetic energy distribution of electrons liberated upon disintegration of excessively ionized cluster, under the influence of picosecond laser pulse. Graphical Abstract ᅟ.

Tracing transient charges in expanding clusters

We study transient charges formed in methane clusters following ionization by intense near-infrared laser pulses. Cluster ionization by 400 fs ($I=1 \times 10^{14}$ W/cm$^2$) pulses is highly efficient, resulting in the observation of a dominant C$^{3+}$ ion contribution. The C$^{4+}$ ion yield is very small, but is strongly enhanced by applying a time-delayed weak near-infrared pulse. We conclude that most of the valence electrons are removed from their atoms during the laser-cluster interaction, and that electrons from the nanoplasma recombine with ions and populate Rydberg states when the cluster expands, leading to a \textit{decrease} of the average charge state of individual ions. Furthermore, we find clear bound-state signatures in the electron kinetic energy spectrum, which we attribute to Auger decay taking place in expanding clusters. Such nonradiative processes lead to an \textit{increase} of the final average ion charge state that is measured in experiments. Our results suggest that it is crucial to include both recombination and nonradiative decay processes for the understanding of recorded ion charge spectra.

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.

Influence of the electron density on the characteristics of terahertz waves generated under laser–cluster interaction

A theory of generation of terahertz radiation under laser–cluster interaction, developed earlier for an overdense cluster plasma [A. A. Frolov, Plasma Phys. Rep. 42. 637 (2016)], is generalized for the case of arbitrary electron density. The spectral composition of radiation is shown to substantially depend on the density of free electrons in the cluster. For an underdense cluster plasma, there is a sharp peak in the terahertz spectrum at the frequency of the quadrupole mode of a plasma sphere. As the electron density increases to supercritical values, this spectral line vanishes and a broad maximum at the frequency comparable with the reciprocal of the laser pulse duration appears in the spectrum. The dependence of the total energy of terahertz radiation on the density of free electrons is analyzed. The radiation yield is shown to increase significantly under resonance conditions, when the laser frequency is close to the eigenfrequency of the dipole or quadrupole mode of a plasma sphere.