Coulomb Explosion Research Articles

Evidence for the formation of metallic In after laser irradiation of InP

Structural and electronic changes induced by laser irradiation are currently of interest owing to the possibility to tune the mechanical, optical, and transport properties of the irradiated materials. In this work, we investigate the effects of laser irradiation on indium phosphide, InP, by modifying the electronic temperature, Te, of the system within the density functional theory framework and performing molecular dynamics simulations to prove that the laser irradiation also provokes a local thermalization effect. We found that the process can be described by a two-stage mechanism. First, at low Te values (0–1.0 eV), the laser energy induces electronic transitions, while the InP lattice remains undisturbed and cool. In the second stage (with Te in the range of 1.0–4.0 eV), both electron-electron scattering and electron-phonon coupling processes are triggered, increasing the energy of the lattice so as to provoke a Coulomb explosion, which changes some physical chemical properties of InP. The close agreement between the simulations helps explain the formation of metallic In as it is observed in the transmission electron microscopy images.

Laser-irradiated gold nanoparticles for breast cancer therapy

Current study involves laser-induced gold nanoparticles (GNPs) for breast cancer therapy. GNPs as a therapeutic agent using nanophotolysis approach are discussed. Coulomb explosion of GNPs is studied numerically using MATLAB. Our findings show that [Formula: see text] ions are generated for short pulse laser interaction of 8 ns and laser irradiation of 2 J/cm2 penetrates in the tumor depth of 3.30 cm. Cluster size of 98 nm produced [Formula: see text] nanobullets that target the breast tumor. Short pulse laser of 2.27 ns generates maximum shock front velocity of [Formula: see text] cm/s. Shock front of 20–146 [Formula: see text]m is produced for effectively damaging the breast cancer tissues. A total of 825 cells are damaged by [Formula: see text] ions. Current results are matched with the literature and are in good correlation. Hence, we conclude that laser-irradiated GNPs using nanophotolysis approach are useful for targeted therapy of breast tumor.

Combined Experimental and Theoretical Survey of the Gas-Phase Reactions of Serine-Ca2+ Adducts.

The association of Ca2+ to serine and the subsequent gas-phase unimolecular reactivity of the [Ca(Ser)]2+ (Ser = Serine) adduct was investigated throughout the use of tandem mass spectrometry techniques and B3LYP/6-311+G(3df,2p)//B3LYP/6-311+G(d,p) density functional theory calculations. In a first step, the structure and relative stability of all possible conformers of serine were obtained and analyzed, as well as the most stable [serine-Ca]2+ adducts. For the analysis of the different potential energy surfaces associated with the gas-phase unimolecular reactivity of these adducts, only those that differ by less than 100 kJ·mol-1 from the global minimum were taken into account. In agreement with previous studies, the serine-Ca2+ global minimum corresponds to a charge-solvated structure in which Ca is tricoordinated to neutral serine. The major peaks observed in the nanoelectrospray-MS/MS spectrum of [Ca(Ser)]2+ adduct correspond to both Coulomb explosions, yielding either CaOH+ + [C3,H6,N,O2]+ or [C2,H4,O,N]+ + [Ca(C,H3,O2)]+, and to the loss of neutrals, namely, CH2O and H2O. Our theoretical survey of the energy profile allow us to conclude that, although all the aforementioned fragmentation processes can have their origin at the global minimum, similar fragmentations involving low-lying conformers, both zwitterionic and nonzwitterionic, compete and should be considered to account for the observed reactivity. We have also found that in some specific cases post-transition state dynamics similar to the ones described before in the literature for formamide-Ca2+ reactions, may also play a role.

Structure determination of the tetracene dimer in helium nanodroplets using femtosecond strong-field ionization.

Dimers of tetracene molecules are formed inside helium nanodroplets and identified through covariance analysis of the emission directions of kinetic tetracene cations stemming from femtosecond laser-induced Coulomb explosion. Next, the dimers are aligned in either one or three dimensions under field-free conditions by a nonresonant, moderately intense laser pulse. The experimental angular covariance maps of the tetracene ions are compared to calculated covariance maps for seven different dimer conformations and found to be consistent with four of these. Additional measurements of the alignment-dependent strong-field ionization yield of the dimer narrow the possible conformations down to either a slipped-parallel or parallel-slightly rotated structure. According to our quantum chemistry calculations, these are the two most stable gas-phase conformations of the dimer and one of them is favorable for singlet fission.

Electron-induced delayed desorption of solid argon doped with methane

The total yield of particles desorption from solid Ar doped with CH4 under irradiation with an electron beam was studied at 5 K. The measurements were carried out at a CH4 concentration of 1 and 5%. The effect of explosive delayed desorption from the surface of argon matrix was discovered in both mixtures. With a higher concentration of CH4, it appeared at lower doses and was more pronounced. Two types of self-oscillations were observed: long-period bursts (on a time scale of about 25 min) and short-period oscillations (of about 10 s). In pure solid Ar delayed desorption was not observed despite the accumulation of a significant number of excess electrons, exceeding their number in mixtures of Ar and CH4 as it was found by measurements of thermally stimulated exoelectron emission. This finding discards the model of Coulomb explosion for the phenomenon detected. In this paper we focused on the role of hydrogen (one of the radiolysis products) in delayed desorption. The formation of atomic hydrogen in the matrix was traced via cathodoluminescence by the emission band of the excimer Ar2H* at 166 nm. Desorption of excited hydrogen atoms in the excited state was detected by the Ly-α emission line. A decrease of the Ar2H* band intensity at higher concentration of CH4 was found evidencing bleaching these centers likely due to recombination of H atoms with energy release and formation of molecular hydrogen. The data obtained give additional evidence in favor of the hypothesis that the exothermic reactions of radiolysis products serve as a stimulating factor for delayed desorption.

Is radiation damage the limiting factor in high-resolution single particle imaging with X-ray free-electron lasers?

The prospect of single particle imaging with atomic resolution is one of the scientific drivers for the development of X-ray free-electron lasers. The assumption since the beginning has been that damage to the sample caused by intense X-ray pulses is one of the limiting factors for achieving subnanometer X-ray imaging of single particles and that X-ray pulses need to be as short as possible. Based on the molecular dynamics simulations of proteins in X-ray fields of various durations (5 fs, 25 fs, and 50 fs), we show that the noise in the diffracted signal caused by radiation damage is less than what can be expected from other sources, such as sample inhomogeneity and X-ray shot-to-shot variations. These findings show a different aspect of the feasibility of high-resolution single particle imaging using free-electron lasers, where employing X-ray pulses of longer durations could still provide a useful diffraction signal above the noise due to the Coulomb explosion.

Effects of parameters on the proton focusing driven by Coulomb explosion

The effects of laser and plasma parameters on the proton focusing driven by Coulomb explosion in the interaction of a laser pulse with a thin arched carbon-hydrogen target are investigated by two-dimensional particle-in-cell simulations. The influence of the laser polarization, the laser spot size and the geometrical dimension of the arched target has been examined. It is shown that a linearly-polarized laser pulse contributes to the occurrence of the Coulomb explosion in a shorter time, and a larger focal spot is advantageous to produce a homogeneous Coulomb field. The geometrical property of the arched target and the buffer action of heavy ions are appropriate for the forward proton focusing.

High-energy 120 MeV Au9+ ion beam-induced modifications and evaluation of craters in surface morphology of SnO2 and TiO2 nanocomposite thin films

The electronic excitation and modification in the properties of the target material occur due to the kinetic energy loss of incident ions mainly through the inelastic collision with atomic electrons in the process of electronic energy stopping. Nanocomposite tin oxide (SnO2) and titanium dioxide (TiO2) thin film were grown on silicon and ITO substrates using RF magnetron-sputtering process. These thin films were irradiated by 120 MeV Au9+ Swift Heavy Ion (SHI) beam with varying fluence from 5 × 1011 ions cm−2 to 2 × 1013 ions cm−2 to induce modifications in thin films by dense electronic excitation. Surface morphology and depth profile of craters (approx. 85 nm) have been characterized by multimode atomic force microscopy (AFM). Grain mapping of AFM images provided the variation in grain size in the range of 72–279 nm and RMS roughness increased (4.01–23.6 nm) with increasing the ion fluence. Scanning Electron Microscopy (SEM) was also carried out to confirm the formation of craters in the irradiated film. X-ray diffraction (XRD) technique has been used for the structural analysis of virgin and irradiated thin films. XRD patterns established the formation of film in mixed (rutile and gamma) phase. Further, the crystallite size was evaluated using the Debye–Scherrer and Williamson–Hall method. It was found that crystallite size lie in the range of 36–54 nm which increased for the lower fluence and then decreased for higher fluence. The ion irradiation-induced strain has been explained by Thermal spike and Coulomb explosion model. UV–Vis study showed that the optical band gap reduced from 3.87 to 3.72 eV with increasing the ion fluence which can be ascribed to the formation of intermediate states and free radicals between the valance and band conduction band. Rutherford Backscattering Spectrometry (RBS) ensured that the film thickness decreased from 210 to 183 nm with increasing the ion fluence. The simulation of the RBS spectra provides the elemental composition of Sn (0.37), Ti (0.65) and O (0.85) in SnO2 and TiO2 nanocomposite thin films.

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 1016 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.

Fusion hindrance effects in laser-induced non-neutral plasmas

Inertial confinement fusion hotspots and cluster Coulomb explosion plasmas may develop a positive net electric charge. The Coulomb barrier penetrability and the rate of nuclear fusion reactions at ultra-low energies (≲10keV) are altered by such an environment. These effects are here studied via the screening potential approach. Approximate analytical results are developed by evaluating the average screening potential for some scenarios of interest. It is found that fusion is hindered for reactions between thermal fuel nuclei, while an enhancement is expected for secondary and “beam-target” reactions. Depending on the plasma conditions, the variations can be relevant even for relatively small net charges (several % difference or more in the fusion rate for an average net charge per nucleus of 10−5 proton charges).

Stereo‐dynamical ion‐pair formation in collisions of highly‐charged ions with argon dimers

Multiple ionization process of a rare gas dimer BC collided with a slow highly charged ion Aq+ is investigated with the three‐center Coulombic over‐barrier model previously developed by the present authors. To reveal stereodynamical effects, we calculate asymmetric ion‐pair formation cross sections σ(QB,QC) as a function of the orientation angle. We introduce a pair of atomic impact parameters bB and bC with which we distinguish the near and far sites. Furthermore, we distinguish the forward and backward emitted ions produced as a result of Coulomb explosion. Partial screening effects are also considered.

Controlled Enantioselective Orientation of Chiral Molecules with an Optical Centrifuge.

We report on the first experimental demonstration of enantioselective rotational control of chiral molecules with a laser field. In our experiments, two enantiomers of propylene oxide are brought to accelerated unidirectional rotation by means of an optical centrifuge. Using Coulomb explosion imaging, we show that the centrifuged molecules acquire preferential orientation perpendicular to the plane of rotation, and that the direction of this orientation depends on the relative handedness of the enantiomer and the rotating centrifuge field. The observed effect is in agreement with theoretical predictions and is reproduced in numerical simulations of the centrifuge excitation followed by Coulomb explosion of the centrifuged molecules. The demonstrated technique opens new avenues in optical enantioselective control of chiral molecules with a plethora of potential applications in differentiation, separation, and purification of chiral mixtures.

Dynamics of three-particle fragmentation of (CO2)23+ ions produced by intense femtosecond laser fields

In a momentum coincidence measurement experiment, we studied the three-body fragmentation dynamics of carbon dioxide dimers in intense femtosecond laser fields. The three-dimensional momentum vectors and kinetic energies of the fragments were recorded in a cold-target recoil-ion momentum spectrometer. An analysis shows that ${({\mathrm{CO}}_{2})}_{2}{}^{3+}$ breaks up into ${\mathrm{CO}}_{2}{}^{+}+{\mathrm{CO}}^{+}+{\mathrm{O}}^{+}$ ions through both concerted and sequential fragmentation channels. These two fragmentation channels are consistent with the instantaneous and metastable dissociation channels in the dissociation dynamics of ${\mathrm{CO}}_{2}{}^{2+}$ ion breakup into ${\mathrm{CO}}^{+}$ and ${\mathrm{O}}^{+}$ ions. From Coulomb explosion imaging, our results show that, for the parallel sliding structure of the carbon dioxide dimer molecules, the angle between the C=O bond and the van der Waals bond is $48{}^{\ensuremath{\circ}}$, and the intermolecular nuclear distance $R({\mathrm{CO}}_{2}\text{\ensuremath{-}}{\mathrm{CO}}_{2})$ is 4.0 \AA{}. By tracing the direction of the fragmentation ions, the ${\mathrm{O}}^{+}$ was found to be produced from the C=O bond that is closer to the center of the C-C bond during direct dissociation. These results indicate that the dynamic characteristics of the monomer is retained and gives rise to new dynamics in the molecular cluster complexes. Finally, we have measured angular distributions of ion fragments produced by different dissociation channels of ${({\mathrm{CO}}_{2})}_{2}$, and the results reveal that the structure of the dimer and its relative orientation in the laser field govern the ionization dynamics.

Dissociative ionization of the H2O molecule bombarded by swift singly charged and slow highly charged ions

Fragment ion energy spectra of the water molecule have been measured in conventional crossed‐beam experiments by the impact of 46 keV/u energy, singly charged ions (SCIs) and 4.3 keV/u energy, highly charged ions (HCIs). Double differential cross sections have been determined and a comparative analysis has been performed. We found that the fragmentation spectra for SCIs and HCIs are very similar, indicating that both collisions lead to the same fragmentation channels. This suggests that the Coulomb explosion of the water molecule is dominantly determined by the charge state of the transient molecular ions, and it is almost independent from the primary ionization mechanism. Differences were observed not only between the SCI and HCI impact‐induced fragmentation cross sections, but between those obtained by the 60 keV N6+ and 70 keV O7+ projectiles. The differences were attributed to the selectivity of the electron capture process for HCIs. Multiple target ionization cross sections have been deduced from the fragment ion spectra. We found contributions of up to fivefold ionization for SCIs and up to sixfold ionization for HCIs.

Modifying the second order dispersion of femtosecond laser pulses to crack silver nanoparticles and control their dimensions

The potential application of metallic nanoparticles had been attracting attention and interest from different areas of academia and industry. The nanoparticles properties and applications depend heavily on their dimension and shape, thus special interest is aimed to controlling the nanoparticles sizes. Ultrashort laser pulses are known to change metallic nanoparticles characteristics, but the interaction mechanism is still not completely understood. In this work we reduced the dimension of silver nanoparticles with ultrashort pulses and demonstrated that there is a dependence of the particles size on the second order dispersion introduced in the pulses, which became smaller as the dispersion becomes more negative. Based on the results, we propose that the Coulomb explosion that reduces the nanoparticles size is predominantly initiated by multiphotonic ionization for the intensities used (1014 W/cm2).

Ultradense protium p(0) and deuterium D(0) and their relation to ordinary Rydberg matter: a review

The extremely large density of ultra-dense hydrogen H(0) has been proved in numerous experiments by three laser-induced methods, namely Coulomb explosions observed by particle time-of-flight (TOF) and TOF mass spectrometry, rotational emission spectroscopy in the visible, and annihilation-like meson ejecting nuclear reaction processes. The density of H(0) at the quite common spin level s = 2 is of the order of 100 kg cm−3. The theory of ultra-dense hydrogen H(0) is described briefly, especially the ‘mixed’ spin quantum number s and its relation to the internuclear distances. The orbital angular momentum of the bonding electrons in H(0) is l = 0, which gives the H(0) designation. At s = 2 with electron total angular momentum L = ħ, the internuclear distance is 2.24 pm, and at s = 1 thus L = ħ/2, it is as small as 0.56 pm. The internuclear distances are measured by optical rotational spectroscopy with a precision as good as 10−3, thus with femtometer resolution. The dimensional factor (ratio of internuclear distance to the electron orbit radius) was determined to be 2.9 by electrostatic stability calculations for ordinary Rydberg matter. This value is found to be valid with high precision also for H(0) clusters with different shapes. Superfluidity and a Meissner effect at room temperature are only found for the long chain clusters H2N(0), while the small H3(0) and H4(0) clusters do not have any super properties. Instead, they are the clusters in which most of the nuclear reaction processes take place. These processes give meson showers (most types of kaons and pions) and, after meson decay, large fluxes of muons and other leptons. Published applications of these results already exist in the field of nuclear reactions, energy production (patented fusion reactor), space physics (the solar wind), and in astrophysics (dark matter and the interstellar medium).

Correlated ion stopping in dense plasmas

Correlated ion stopping arising from an intense cluster ion beam (CIB) interacting with an ultradense plasma target of relevance to inertial confinement fusion (ICF) is first investigated in a two-body approximation in an arbitrarily degenerate electron fluid target. The specific advantages of CIB-driven ICF are first demonstrated through 1D simulations, highlighting the very fine focusing of the ion beam on the target pellet. Then, the N-body configurations of ion debris resulting from the impact of heavy cluster ions are determined in terms of their specific topology. The validities of the usual assumptions of equal ion fragment charge and negligible coupling between stopping and Coulomb explosion are assessed.

Making Sense of Coulomb Explosion Imaging.

A multifaceted agreement between ab initio theoretical predictions and experimental measurements, including branching ratios, channel-specific kinetic energy release, and three-body momentum correlation spectra, leads to the identification of new mechanisms in Coulomb-explosion (CE) induced two- and three-body breakup processes in methanol. These identified mechanisms include direct nonadiabatic Coulomb explosion responsible for CO bond-breaking, a long-range " inverse harpooning" dominating the production of H2+ + HCOH+, a transient proton migration leading to surprising energy partitioning in three-body fragmentation and other complex dynamics forming products such as H2O+ and H3+. These mechanisms provide general concepts that should be useful for analyzing future time-resolved Coulomb explosion imaging of methanol as well as other molecular systems. These advances are enabled by a combination of recently developed experimental and computational techniques, using weak ultrafast EUV pulses to initiate the CE and a high-level quantum chemistry approach to follow the resulting field-free nonadiabatic molecular dynamics.

Experimental Detection of the Signs of a Coulomb Explosion in Micropinch Plasma

A flow of ions with energies of about 3 MeV propagating in the direction perpendicular to the symmetry axis of discharge has been detected in high-current low inductance vacuum spark. Estimations show that the measured ion energies quite well correspond to the value that can be achieved as a result of “Coulomb explosion” of the waist of a plasma channel of discharge current at the stage preceding its radiation compression.

Bond-breakage-dependent dissociative ionization of an asymmetric molecule in an intense femtosecond laser field

A coincidence momentum imaging method is used to investigate the dissociative ionization of carbonyl sulfide (OCS) irradiated by linearly polarized 800 nm femtosecond laser pulses. As a typical asymmetric molecule, kinetic-energy release (KER) distributions of two-body Coulomb explosion (CE) along C-S or C-O bond breakage from $\mathrm{OC}{\mathrm{S}}^{q+}$ ($q=2$, 3, 4) exhibit a different behavior when the parent charge state increases. Two processes, i.e., concerted enhanced multiple ionization and ladder-climbing-type sequential ionization, are proposed for the C-S and C-O bond breakage, respectively. With the help of the potential-energy curves (PEC) obtained from the multistate density-functional-theory method, the KER values are calculated for these CE channels of $\mathrm{OC}{\mathrm{S}}^{q+}$. The overall good quantitative agreement between the experiment and calculation confirms the validity of the ionization mechanism assumed. In our approach, the global minimum of cationic PEC for the OCS can be treated as ${R}_{c}$ for enhanced ionization. Furthermore, a bimodal KER distribution was observed for the channel of $\mathrm{OC}{\mathrm{S}}^{2+}\ensuremath{\rightarrow}{\mathrm{O}}^{+}+\mathrm{C}{\mathrm{S}}^{+}$, and with the help of PEC, we believe that both of the ionization processes are involved in the dynamics of its formation.