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Alkali trimers, Ak3, located on the surface of He nanodroplets are triply ionized following multiphoton absorption from an intense femtosecond laser pulse, leading to fragmentation into three correlated Ak+ ions. Combining the information from threefold covariance analysis of the emission direction of the fragment ions and their kinetic energy distributions P(Ekin), we find that Na3, K3, and Rb3 have an equilateral triangular structure, corresponding to that of the lowest lying quartet state A 2 ′ 4 , and determine the equilibrium bond distance Req(Na3) = 4.65 ± 0.15 Å, Req(K3) = 5.03 ± 0.18 Å, and Req(Rb3) = 5.45 ± 0.22 Å. For K3 and Rb3, these values agree well with existing theoretical calculations, while for Na3, the value is 0.2–0.3 Å larger than the existing theoretical results. The discrepancy is ascribed to a minor internuclear motion of Na3 during the ionization process. In addition, we determine the distribution of internuclear distances P(R) under the assumption of fixed bond angles. The results are compared to the square of the internuclear wave function |Ψ(R)|2. [ABSTRACT FROM AUTHOR]

Site-selective probing of iodine 4d orbitals at 13.1 nm was used to characterize the photolysis of CH2I2 and CH2BrI initiated at 202.5 nm. Time-dependent fragment ion momenta were recorded using Coulomb explosion imaging mass spectrometry and used to determine the structural dynamics of the dissociating molecules. Correlations between these fragment momenta, as well as the onset times of electron transfer reactions between them, indicate that each molecule can undergo neutral three-body photolysis. For CH2I2, the structural evolution of the neutral molecule was simultaneously characterized along the C–I and I–C–I coordinates, demonstrating the sensitivity of these measurements to nuclear motion along multiple degrees of freedom. [ABSTRACT FROM AUTHOR]

Photoionization can initiate structural reorganization of molecular matter and drive formation of new chemical bonds. Here, we used time-resolved extreme ultraviolet (EUV) pump – EUV probe Coulomb explosion imaging of carbon dioxide dimer ion C O 2 2 + dynamics, that combined with ab initio molecular dynamics simulations, revealed unexpected asymmetric structural rearrangement. We show that ionization by the pump pulse induces rearrangement from the slipped-parallel (C2h) geometry of the neutral C O 2 dimer towards a T-shaped (C2v) structure on the ~100 fs timescale, although the most stable slipped-parallel (C2h) structure of the ionic dimer. Moreover, we find that excited states of the ionized C O 2 dimer can exhibit formation of a CO 3 moiety in the C 2 O 4 + complex that can persist even after a suitably time-delayed second photoionization in a metastable C 2 O 4 2 + dication. Our results suggest that charge asymmetry plays an important role in the ionization-induced dynamics in such dimers that are present in C O 2 rich environments. In a time-resolved Coulomb explosion imaging study using ultrafast extreme ultraviolet pulses, combined with theoretical simulations, authors reveal unexpected asymmetric rearrangement of carbon dioxide dimer ion, including a CO3 moiety formation. [ABSTRACT FROM AUTHOR]

We experimentally studied the three-body fragmentation dynamics of a noble gas cluster (ArKr2) upon its multiple ionization by an intense femtosecond laser pulse. The three-dimensional momentum vectors of correlated fragmental ions were measured in coincidence for each fragmentation event. A novel comet-like structure was observed in the Newton diagram of the quadruple-ionization-induced breakup channel of ArKr 2 4 + → Ar+ + Kr+ + Kr2+. The concentrated head part of the structure mainly originates from the direct Coulomb explosion process, while the broader tail part of the structure stems from a three-body fragmentation process involving electron transfer between the distant Kr+ and Kr2+ ion fragments. Due to the field-driven electron transfer, the Coulomb repulsive force of the Kr2+ and Kr+ ions with respect to the Ar+ ion undergoes exchange, leading to changes in the ion emission geometry in the Newton plot. An energy sharing among the separating Kr2+ and Kr+ entities was observed. Our study indicates a promising approach for investigating the strong-field-driven intersystem electron transfer dynamics by using the Coulomb explosion imaging of an isosceles triangle van der Waals cluster system. [ABSTRACT FROM AUTHOR]

The ion impact multiple ionization and subsequent dissociation of CCl4 is studied using a beam of Ar7+ ion having the energy of about 1 MeV in a linear time- of-flight mass spectrometer, coupled with a position-sensitive detector. The complete, as well as incomplete Coulomb explosion pathways, for CCl 4 2 + and CCl 4 3 + ions are identified and studied. The kinetic energy release distributions of channels, kinetic energies, and momentum distributions of fragmented ions, as well as neutrals, are also calculated. Possible modes of fragmentation pathways, i.e., concerted and/or sequential, for all the identified channels are studied using Newton diagrams, Dalitz plots, and kinetic energy distributions. The dynamical information and fragmentation pathways were analyzed with the Dalitz plot and Newton diagram for the three-body dissociation channel. The nature of the fragmentation process is further investigated with simulated Dalitz plots and Newton diagrams using the simple classical mechanical model. [ABSTRACT FROM AUTHOR]

We report an investigation on the fragmentation dynamics of SO2q+ (q = 2–4) induced by 1 keV electron collision utilizing an ion momentum imaging spectrometer. Six complete Coulomb explosion channels were observed using the time-of-flight correlation map. The kinetic energy release distributions for these channels were obtained and compared with those available in the literature. The fragmentation mechanisms of the three-body dissociation channels were analyzed by the Dalitz plots and Newton diagrams. Both concerted breakup and sequential fragmentation pathways were identified in the channel SO23+ → O+ + O+ + S+, whereas only the concerted breakup mechanism was confirmed for the channels SO24+ → O+ + O+ + S2+ and SO24+ → O2+ + O+ + S+. Using the Coulomb explosion model, we determined the molecular geometry from the concerted fragmentation channels, and the obtained bond lengths and angles from the higher kinetic energy release peaks are close to that of the neutral SO2 obtained by high-level quantum chemical calculation. The present results indicate that the electron impact experiment is a potential tool for the Coulomb explosion imaging of small molecules. [ABSTRACT FROM AUTHOR]

The rotational dynamics of a molecule is sensitive to neighboring atoms or molecules, which can be used to probe the intermolecular interactions in the gas phase. Here, we real-time track the laser-driven rotational dynamics of a single N2 molecule affected by neighboring Ar atoms using coincident Coulomb explosion imaging. We find that the alignment trace of N-N axis decays fast and only persists for a few picoseconds when an Ar atom is nearby. We show that the decay rate depends on the rotational geometry of whether the Ar atom stays in or out of the rotational plane of the N2 molecule. Additionally, the vibration of the van der Waals bond is found to be excited through coupling with the rotational N-N axis. The observations are well reproduced by solving the time-dependent Schrödinger equation after taking the interaction potential between the N2 and Ar into consideration. Our results demonstrate that environmental effects on a molecular level can be probed by directly visualizing the rotational dynamics. The authors demonstrate, using coincident Coulomb explosion imaging, that the rotational dynamics of single nitrogen molecules can be used as a probe to sense the interactions with surrounding Ar atoms in gas-phase clusters. [ABSTRACT FROM AUTHOR]

Improving the energy efficiency in generating high-energy proton or boron ions is crucial for advancing the feasibility of neutronless laser-based proton–boron (p-B11) fusion reactions. The primary objective of this work is to optimize the fusion energy efficiency of a proposed advanced p-B11 fusion scheme. In the proposed scheme, an ultrashort laser pulse is guided by a plasma channel filled with carbon–hydrogen (CH2) clusters. The MeV protons are generated by the Coulomb explosion (CE) of the cluster, which, therefore, interact with surrounding boron to produce alpha particles. To evaluate the fusion energy efficiency under various conditions, 2D particle-in-cell (PIC) simulations are used, supplemented with analytical calculations and estimations. The Bayesian optimization (BO) algorithm is utilized to optimize the key interaction parameters. The BO approach allows us to identify optimal cluster and laser parameters that would have higher fusion energy efficiency.

Nanotechnologists and medical researchers are working hard to develop new and innovative ways to use nanorobots as nanomedicine to improve healthcare outcomes and revolutionize the field of therapeutics. Nanotechnology has the potential to revolutionize healthcare by providing new ways of treating chronic diseases in the field of medicine. A “Gold Nano Thermo Robot” (GNTR) model has been proposed in this research article, which can be considered a nanomedicine that will deliver controlled thermal therapy to targeted malignant tissues without damaging healthy tissues. The proposed nanotherapeutic system, empowered with a nano sensor network, interbody body communication network, and Internet of nanomedical things, has been used to normalize and control hyperthermal waves in real-time that have been used to eliminate breast cancer cells using the “SEE and TREAT” technique. To generate hyperthermia, which has been irradiated by laser pulses to propose GNTR, a Coulomb explosion took place, and a huge amount of dispersed hyperthermia waves were produced. To convert the intensity of dispersed and irregular hyperthermia into a regulated and disciplined format, a Finite Difference Method has been used to develop a “Heat Control System.” A comparative analysis has been provided of the intricate relationship between the required radius of Gold Nano Thermo Robots and the volume depth of the tumor for penetration, with a keen focus on evaluating how different GNTR sizes fit or do not fit for the task of effectively treating tumors at various depths within cancer tumors. Furthermore, the effectiveness of treatment has multifaceted outcomes that have been acquired by the interplay between two critical factors, the temperature limit and therapy duration. By examining a comprehensive matrix of thermal therapy durations (ranging from 25 minutes to 60 minutes) alongside various temperature limits (ranging from 33°C to 60°C). The best fit and the best response therapy session have been verified with a temperature limit of 42 °C for 30 minutes, achieving near-complete tumor ablation with minimum harm to the healthy tissues. The complex physical effects on the Gold Nano Robots surfaces due to the Coulomb explosion procedure are also provided in the form of simulation analysis, and an explanation is given in nine panels.

Multi-ionization and subsequent Coulomb explosion (CE) of the N2O molecule irradiated by a linearly polarized 800 nm laser field is investigated by a reaction microscope, where a number of CE channels of N2Oq+ with q ≤ 5 for two-body fragmentation and q ≤ 8 for three-body fragmentation were observed. For two-body CE, by analyzing the internuclear separations extracted from kinetic energy releases (KERs), dissociation branching fractions, and laser intensity dependence, interestingly, we found that fragmentation N2O5+ → N3+ + NO2+ is produced directly from dissociating N2O3+ via non-sequential stairstep ionization, whereas most of the others result from the sequential stairstep ionization. For three-body CE, 25 fragmentation channels of N2Oq+ (q = 3–8) are distinguished in the present charge-encoded multi-photoion coincidence plot, and the concerted fragmentation mechanism is nominated in a typical Dalitz plot. With the help of the numerical computation with the measured KERs and momentum correlation angles, the geometric structures of molecular ions prior to fragmentation are reconstructed, which display the bending motion and simultaneous two-bond stretching before the CE. Increasing of the bond length for high charged N2Oq+ indicates the dominating stairstep ionization in the three-body fragmentation. [ABSTRACT FROM AUTHOR]

We study the competing mechanisms involved in the Coulomb explosion of 2-propanol C H 3 2 C H O H 2 + dication, formed by an ultrafast extreme ultraviolet pulse. Over 20 product channels are identified and characterized using 3D coincidence imaging of the ionic fragments. The momentum correlations in the three-body fragmentation channels provide evidence for a dominant sequential mechanism, starting with the cleavage of a C–C bond, ejecting C H 3 + and CH3CHOH+ cations, followed by a secondary fragmentation of the hydroxyethyl cation that can be delayed for up to a microsecond after ionization. The C–O bond dissociation channels are less frequent, involving proton transfer and double proton transfer, forming H2O+ and H3O+ products, respectively, and exhibiting mixed sequential and concerted character. These results can be explained by the high potential barrier for the C–O bond dissociation seen in our ab initio quantum chemical calculations. We also observe coincident COH+ + C2Hn+ ions, suggesting exotic structural rearrangements, starting from the Frank–Condon geometry of the neutral 2-propanol system. Remarkably, the relative yield of the H 3 + product is suppressed compared with methanol and alkene dications. Ab initio potentials and ground state molecular dynamics simulations show that a rapid and direct C–C bond cleavage dominates the Coulomb explosion process, leaving no time for H2 roaming, which is a necessary precursor to the H 3 + formation. [ABSTRACT FROM AUTHOR]

We have recently proposed a new technique of plasma tailoring by laser-driven hydrodynamic shockwaves generated on both sides of a gas jet [Marquès et al., Phys. Plasmas 28, 023103 (2021)]. In a continuation of this numerical work, we study experimentally the influence of the tailoring on proton acceleration driven by a high-intensity picosecond laser in three cases: without tailoring, by tailoring only the entrance side of the picosecond laser, and by tailoring both sides of the gas jet. Without tailoring, the acceleration is transverse to the laser axis, with a low-energy exponential spectrum, produced by Coulomb explosion. When the front side of the gas jet is tailored, a forward acceleration appears, which is significantly enhanced when both the front and back sides of the plasma are tailored. This forward acceleration produces higher-energy protons, with a peaked spectrum, and is in good agreement with the mechanism of collisionless shock acceleration (CSA). The spatiotemporal evolution of the plasma profile is characterized by optical shadowgraphy of a probe beam. The refraction and absorption of this beam are simulated by post-processing 3D hydrodynamic simulations of the plasma tailoring. Comparison with the experimental results allows estimation of the thickness and near-critical density of the plasma slab produced by tailoring both sides of the gas jet. These parameters are in good agreement with those required for CSA. [ABSTRACT FROM AUTHOR]

The paper proposes the hypothesis of the explosive-nature dislocationelectronic mechanism of the deformation cracks in the metals' nucleation. This hypothesis is based on the Coulomb repulsion of the positively-charged ions. when the neutral state of the ion--electron system in the crystal lattice is disturbed that leads to the nanolocal Coulomb explosion and the appearance of the nucleated cracks. [ABSTRACT FROM AUTHOR]

The literary data dealing with the experimental studies concerning the influence of electromagnetic phenomena on the diffusion processes are reviewed and analysed. Based on the scientific facts presented in interdisciplinary experimental studies, a hypothesis is suggested. It is concerned with the influence of electromagnetic phenomena in the process of formation of a diffusion joint during pressure welding through a layer of a hydrocarbon substance. In the welded joint, at the initial moment of current transmission, energy is released during the explosion at the points of contact. When a pulsed electric current is passed through the pyrolysis products in microvolumes between the surfaces to be joined, they are also destroyed. Ionized particles are formed. Under the action of the pinch effect, they move to the centre of the welded joint. A capsule with ionized carbon particles is formed there. The 'Coulomb explosion' occurs in the capsule located in the middle of the joint. Multiple exposures of the surfaces by microexplosions in microvolumes between the surfaces to be joined and the final 'Coulomb explosion' of the capsule create the release of a large number of magnetic monopoles. This can be a determining and synergistic factor among a number of others in the formation of a welded joint. This makes it possible to explain the short time required for welding and the small deformations of the weld formation zone. [ABSTRACT FROM AUTHOR]

Using the all-optical molecular orientation technique with intense nonresonant two-color laser pulses, stronger molecular orientation |⟨cos θ2D⟩| ∼ 0.34 is achieved by employing the following two strategies: (1) carbonyl sulfide molecules lying in the lower rotational states are selected using a home-built molecular deflector and (2) the rising parts of the two wavelengths of the pump pulse are adjusted by introducing a Michelson-type delay line in the optical path. The achieved degree of molecular orientation is higher than that observed in the proof-of-principle experiment [Oda et al., Phys. Rev. Lett. 104, 213901 (2010)] by about an order of magnitude and the highest ever characterized directly by Coulomb explosion imaging with appropriate probe polarization. [ABSTRACT FROM AUTHOR]

The DC-sliced ion velocity map imaging approach was used to analyze the multi-electron ionization and subsequent Coulomb explosion of an IBr molecule exposed to a near-infrared femtosecond laser field. The existence of the molecular ions up to IBr7+ was observed in the experiment, and a series of Coulomb explosion channels are assigned. According to the "ladder-path" ionization model, the multi-electron ionization paths of IBr molecules are determined. We find that the charge transfer process does not occur during ionization, and the presence of higher charge states can be explained by considering the higher-order ionization process. [ABSTRACT FROM AUTHOR]

We propose a new scheme of a few MeV range uni-directional neutral particle generation via charge exchange mechanism (Rajeev et al. in Nat Phys 9:185, 2013) of energetic ions driven by intense laser. A two-dimensional stack of gold nanorods, embedded inside a hydrocarbon foil (CH), are ionized by the action of pulse of intensities more than 10 16 Wcm - 2 . The pre-pulse is diverted toward a gaseous/clustered environment and excites atoms/clusters to Rydberg states, while the main part of the pulse exerts a transverse ponderomotive force on electrons causing its immediate expulsion. Under Coulomb explosion, carbon ions and protons exit quickly, while the gold ions remain practically immobile due to inertia. The potential structure created by the positively charged nano-rod assembly has complete transverse confinement and axial acceleration. Carbon ions and protons are axially accelerated and undergo collision with Rydberg state atoms/cluster causing charge exchange. This scheme addresses the issues of complete transverse confinement, directionality, and in-situ charge exchange environment. Typical 40 femtosecond pulses with normalized amplitude ( a 0 = 1 - 2 ) can generate energetic neutrals of ∼ 0.5 - 5 MeV range. In the present scheme, one also gets the flexibility of using the changed nanorod geometry or alignment or using external magnetic field to control the beam direction prior to charge exchange stage. [ABSTRACT FROM AUTHOR]

Structural imaging of transient excited-state species is a key goal of molecular physics, promising to unveil rich information about the dynamics underpinning photochemical transformations. However, separating the electronic and nuclear contributions to the spectroscopic observables is challenging, and typically requires the application of high-level theory. Here, we employ site-selective ionisation via ultrashort soft X-ray pulses and time-resolved Coulomb explosion imaging to interrogate structural dynamics of the ultraviolet photochemistry of carbon disulfide. This prototypical system exhibits the complex motifs of polyatomic photochemistry, including strong non-adiabatic couplings, vibrational mode couplings, and intersystem crossing. Immediately following photoexcitation, we observe Coulomb explosion signatures of highly bent and stretched excited-state geometries involved in the photodissociation. Aided by a model to interpret such changes, we build a comprehensive picture of the photoinduced nuclear dynamics that follows initial bending and stretching motions, as the reaction proceeds towards photodissociation. Coulomb Explosion imaging is a promising technique to study the ultrafast nuclear dynamics which underpin molecular photochemistry. By initiating Coulomb explosion through soft X-ray ionization, the authors are able to image ultrafast nuclear dynamics of a prototypical photoreaction. [ABSTRACT FROM AUTHOR]

Structural imaging of transient excited-state species is a key goal of molecular physics, promising to unveil rich information about the dynamics underpinning photochemical transformations. However, separating the electronic and nuclear contributions to the spectroscopic observables is challenging, and typically requires the application of high-level theory. Here, we employ site-selective ionisation via ultrashort soft X-ray pulses and time-resolved Coulomb explosion imaging to interrogate structural dynamics of the ultraviolet photochemistry of carbon disulfide. This prototypical system exhibits the complex motifs of polyatomic photochemistry, including strong non-adiabatic couplings, vibrational mode couplings, and intersystem crossing. Immediately following photoexcitation, we observe Coulomb explosion signatures of highly bent and stretched excited-state geometries involved in the photodissociation. Aided by a model to interpret such changes, we build a comprehensive picture of the photoinduced nuclear dynamics that follows initial bending and stretching motions, as the reaction proceeds towards photodissociation. Coulomb Explosion imaging is a promising technique to study the ultrafast nuclear dynamics which underpin molecular photochemistry. By initiating Coulomb explosion through soft X-ray ionization, the authors are able to image ultrafast nuclear dynamics of a prototypical photoreaction. [ABSTRACT FROM AUTHOR]

Real-time imaging of transient structure of the electronic excited state is fundamentally critical to understand and control ultrafast molecular dynamics. The ejection of electrons from the inner-shell and valence level can lead to the population of different excited states, which trigger manifold ultrafast relaxation processes, however, the accurate imaging of such electronic state-dependent structural evolutions is still lacking. Here, by developing the laser-induced electron recollision-assisted Coulomb explosion imaging approach and molecular dynamics simulations, snapshots of the vibrational wave-packets of the excited (A) and ground states (X) of D2O+ are captured simultaneously with sub-10 picometre and few-femtosecond precision. We visualise that θDOD and ROD are significantly increased by around 50∘ and 10 pm, respectively, within approximately 8 fs after initial ionisation for the A state, and the ROD further extends 9 pm within 2 fs along the ground state of the dication in the present condition. Moreover, the ROD can stretch more than 50 pm within 5 fs along autoionisation state of dication. The accuracies of the results are limited by the simulations. These results provide comprehensive structural information for studying the fascinating molecular dynamics of water, and pave the way towards to make a movie of excited state-resolved ultrafast molecular dynamics and light-induced chemical reaction. Capturing the detailed structural evolution of electronic excited states is a challenging but critical step to understand and control ultrafast molecular dynamics. Here, combining a Coulomb explosion imaging approach and molecular dynamics simulations, the authors retrieve the transient geometry of the ground and excited states of D2O mono- and dication with few femtosecond, few picometre accuracy. [ABSTRACT FROM AUTHOR]

The behavior of nitrosyl chloride (ClNO) exposed to ionizing radiation was studied by direct probing valence-shell electrons in temporal coincidence with ions originating from the fragmentation process of the transient ClNO2+. Such a molecular dication was produced by double photoionization with synchrotron radiation in the 24–70 eV photon energy range. The experiment has been conducted at the Elettra Synchrotron Facility of Basovizza (Trieste, Italy) using a light beam linearly polarized with the direction of the polarization vector parallel to the ClNO molecular beam axis. ClNO molecules crossing the photon beam at right angles in the scattering region are generated by effusive expansion and randomly oriented. The threshold energy for the double ionization of ClNO (30.1 ± 0.1 eV) and six dissociation channels producing NO+/Cl+, N+/Cl+, N+/O+, O+/Cl+, ClN+/O+, NO+/Cl2+ ion pairs, with their relative abundance and threshold energies, have been measured. [ABSTRACT FROM AUTHOR]

Tpx3Cam is a newly developed time-stamped camera. With the ability to record the arrival time and position of each event simultaneously, it becomes a powerful tool in atomic and molecular research. As an inherent weakness, the time-walk effect resulting in a deviation in the arrival time is a major obstacle in improving the experimental resolution and reconstruction of momentum along the time-of-flight. We developed an analytic expression to describe and correct the time-walk effect, which is independent of different fragments once the parameters of the spectrometer, the microchannel plate (MCP), the phosphor screen, and the Tpx3Cam, such as voltages on the spectrometer and MCP, are fixed. With the time-walk correction, 3D momentum distributions of N+ and N2+ from the N2 molecule's Coulomb explosion were well extracted, paving a way for filming molecular dynamics in three dimensions with time-stamped velocity map imaging. Simultaneously, a denoising method based on data filtering is presented for Tpx3Cam. [ABSTRACT FROM AUTHOR]

We present a new technique for detecting chirality in the gas phase: Chiral molecules are spatially aligned in three dimensions by a moderately strong elliptically polarized laser field. The momentum distributions of the charged fragments, produced by laser-induced Coulomb explosion, show distinct three-dimensional orientation of the enantiomers when the laser polarization ellipse is rotated by a non-right angle with respect to the norm vector of the detector plane. The resulting velocity-map-image asymmetry is directly connected to the enantiomeric excess and to the absolute handedness of molecules. We demonstrated our scheme computationally for camphor (C10H16O), with its methyl groups as marker fragments, using quantum-mechanical simulations geared toward experimentally feasible conditions. Computed sensitivity to enantiomeric excess is comparable to other modern chiroptical approaches. The present method can be readily optimized for any chiral molecule with an anisotropic polarizability tensor by adjusting the polarization state and intensity profile of the laser field. [ABSTRACT FROM AUTHOR]

CO2 single-photon double photoionization, Coulomb explosion, and dissociative ionization are studied with ultrafast extreme-ultraviolet pump and time-delayed near-infrared probe pulses. Kinetic energy release and momentum correlations for the two-body CO+ + O+ and three-body O+ + C+ + O fragmentation products are determined by 3D coincidence fragment imaging. The transient enhancement of the ratio of two-body vs three-body Coulomb explosion events and the time dependence of low and high kinetic energy release dissociation events are discussed in terms of dissociative ionization and Coulomb explosion dynamics. [ABSTRACT FROM AUTHOR]

Coulomb explosion velocity-map imaging is a new and potentially universal probe for gas-phase chemical dynamics studies, capable of yielding direct information on (time-evolving) molecular structure. The approach relies on a detailed understanding of the mapping between the initial atomic positions within the molecular structure of interest and the final velocities of the fragments formed via Coulomb explosion. Comprehensive on-the-fly ab initio trajectory studies of the Coulomb explosion dynamics are presented for two prototypical small molecules, formyl chloride and cis-1,2-dichloroethene, in order to explore conditions under which reliable structural information can be extracted from fragment velocity-map images. It is shown that for low parent ion charge states, the mapping from initial atomic positions to final fragment velocities is complex and very sensitive to the parent ion charge state as well as many other experimental and simulation parameters. For high-charge states, however, the mapping is much more straightforward and dominated by Coulombic interactions (moderated, if appropriate, by the requirements of overall spin conservation). This study proposes minimum requirements for the high-charge regime, highlights the need to work in this regime in order to obtain robust structural information from fragment velocity-map images, and suggests how quantitative structural information may be extracted from experimental data. [ABSTRACT FROM AUTHOR]

The laser energy per unit surface, necessary to trigger material removal, decreases with the pulse shortening, becoming pulse–time independent in the sub-picosecond range. These pulses are shorter than the electron-to-ion energy transfer time and electronic heat conduction time, minimising the energy losses. Electrons receiving an energy larger than the threshold drag the ions off the surface in the mode of electrostatic ablation. We show that a pulse shorter than the ion period (Shorter-the-Limit (StL)) ejects conduction electrons with an energy larger than the work function (from a metal), leaving the bare ions immobile in a few atomic layers. Electron emission is followed by the bare ion's explosion, ablation, and THz radiation from the expanding plasma. We compare this phenomenon to the classic photo effect and nanocluster Coulomb explosions, and show differences and consider possibilities for detecting new modes of ablation experimentally via emitted THz radiation. We also consider the applications of high-precision nano-machining with this low intensity irradiation. [ABSTRACT FROM AUTHOR]

The process of gas ionization-recombination and dust particle charging under the effect of X-ray radiation in the conditions of space plasma has been investigated. Conditions have been found under which, as a result of radiation exposure, dust particles in a protoplanetary disk can acquire a positive charge even under low gas ionization. [ABSTRACT FROM AUTHOR]

Accelerator mass spectrometry (AMS) measurements of 10Be almost invariably utilize the BeO- molecular negative ion. Molecular ions experience the process of 'Coulomb explosion' when dissociated by a stripper in the high-voltage terminal of a tandem accelerator, resulting in energy and angular spread of the subsequently-accelerated positive ions. In this paper, the phenomenon is studied in detail for both foil and gas stripping of BeO, using the 14UD pelletron accelerator at the Australian National University operating at 8.5 MV. In a companion paper by Suter et al. [1], a model is developed to interpret, inter alia, these results. [ABSTRACT FROM AUTHOR]

Filming atomic motion within molecules is an active pursuit of molecular physics and quantum chemistry. A promising method is laser-induced Coulomb Explosion Imaging (CEI) where a laser pulse rapidly ionizes many electrons from a molecule, causing the remaining ions to undergo Coulomb repulsion. The ion momenta are used to reconstruct the molecular geometry which is tracked over time (i.e., filmed) by ionizing at an adjustable delay with respect to the start of interatomic motion. Results are distorted, however, by ultrafast motion during the ionizing pulse. We studied this effect in water and filmed the rapid "slingshot" motion that enhances ionization and distorts CEI results. Our investigation uncovered both the geometry and mechanism of the enhancement which may inform CEI experiments in many other polyatomic molecules. Laser-induced Coulomb explosion imaging allows the study of molecular geometries over time, but the results are often distorted by ultrafast motion during the ionizing laser pulse. Here, the authors film the rapid slingshot motion in D2O that induces this distortion and elucidate the underlying mechanism of enhanced ionization. [ABSTRACT FROM AUTHOR]

A droplet charged above the Rayleigh limit is unstable. In the resulting dynamical process, referred to as a Coulomb explosion, smaller droplets with higher charge-to-mass ratios are ejected, reducing the charge of the parent droplet below the Rayleigh limit. Furthermore, if the droplet is sufficiently small, the electric field on its surface can promote ion field emission. Ion emission can lower the charge of a spherical droplet below its Rayleigh limit, keeping it stable, or reduce the charge of a deforming droplet, changing its dynamics and potentially preventing the Coulomb explosion. This article develops a continuum phase field electrohydrodynamic model to study the interplay between Coulomb explosions and ion emission, using charged nanodroplets of the ionic liquid 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMI-Im) as a case study. In small droplets (diameter $D \lesssim 20$  nm for EMI-Im), the electric field is strong enough to emit ions in the early phase of the droplet's evolution, suppressing the Coulomb explosion. For $20 \lesssim D \lesssim 45$  nm, the electric field on the EMI-Im droplet may not promote significant ion emission; however, as the unstable droplet becomes ellipsoidal, ions are emitted from its vertices, ultimately suppressing the Coulomb explosion while shedding $20\unicode{x2013}40\,\%$ of the initial charge. For larger EMI-Im droplets, $45 \lesssim D \lesssim 100$  nm, the evolution typical of a Coulomb explosion is observed, accompanied by ion emission which is however insufficient to prevent the Coulomb explosion. Ion emission and the smaller progeny droplets account for $24\,\%$ and $16\,\%$ of the initial charge, respectively. [ABSTRACT FROM AUTHOR]

We have studied the fragmentation of the brominated cyclic hydrocarbons bromocyclo-propane, bromocyclo-butane, and bromocyclo-pentane upon Br(3d) and C(1s) inner-shell ionization using coincidence ion momentum imaging. We observe a substantial yield of CH3+ fragments, whose formation requires intramolecular hydrogen (or proton) migration, that increases with molecular size, which contrasts with prior observations of hydrogen migration in linear hydrocarbon molecules. Furthermore, by inspecting the fragment ion momentum correlations of three-body fragmentation channels, we conclude that CHx+ fragments (with x = 0, ..., 3) with an increasing number of hydrogens are more likely to be produced via sequential fragmentation pathways. Overall trends in the molecular-size-dependence of the experimentally observed kinetic energy releases and fragment kinetic energies are explained with the help of classical Coulomb explosion simulations. [ABSTRACT FROM AUTHOR]

We study ion-induced secondary electron emission from solid surfaces. This work focuses on the dependence of the energy distribution of secondary electrons on the orientation of Si-dimers impinging on thin carbon foils. The orientation was determined by the foil-induced Coulomb explosion method. Furthermore, the electron energy was measured with a retarding field analyzer. The correlation between the electron energy distribution and the cluster orientation was obtained through simultaneous measurements. A comparison of the electron energy distribution for parallel and perpendicular orientations indicated that the electron yields at an energy below 20 eV are lower for parallel orientation. This reduction can be explained by the orientation dependence of the energy loss of Si 2 + in carbon. It was suggested that the orientation effect is due to the distant collision between the cluster and the target atom, in which low-energy electrons are produced. [ABSTRACT FROM AUTHOR]

We investigate the fragmentation of the CH4 cluster by fast electron impact at stagnation pressures from 0.5 bar to 16 bar. By measuring the time of flight spectrum (TOF), two types of ions, including (CH4)n−1CH5+ and (CH4)n−2(C2Hm)+, are observed. In the 1D TOF spectrum, it is shown that for the stagnation pressure larger than 4 bar, the former ion is predominant for each n, similar to the previous experimental result. However, as the pressure decreases to 0.5 or 2 bar, the contribution of the C2Hm+ ion is dominant over that of the CH4CH5+ ion. In the 2D coincident TOF spectrum, the above two patterns of ions are also distinguished, and the enhancement of C2Hm+ is observed at 4 bar pressure. The phenomena appearing in 2D and 1D TOF spectra imply that the C2Hm+ ion prefers to survive in a smaller cluster, while the stabilization of the protonated ion needs a more massive cluster environment. [ABSTRACT FROM AUTHOR]

The DC-sliced ion velocity map imaging approach was used to analyze the multi-electron ionization and subsequent Coulomb explosion of an IBr molecule exposed to a near-infrared femtosecond laser field. The existence of the molecular ions up to IBr7+ was observed in the experiment, and a series of Coulomb explosion channels are assigned. According to the “ladder-path” ionization model, the multi-electron ionization paths of IBr molecules are determined. We find that the charge transfer process does not occur during ionization, and the presence of higher charge states can be explained by considering the higher-order ionization process.

We performed reaction dynamics simulations to demonstrate that the vibrational dynamics of C60 induced by infrared (IR) pulses can be traced by triggering Coulomb explosion with intense femtosecond X-ray free electron laser (XFEL) probe pulses. The time series of the angular anisotropy β(t) of fast C+ and C2+ fragments of C6060+ produced by such an XFEL pulse reflects the instantaneous structure of C60 vibrationally excited by IR pulses. The phases and amplitudes of excited vibrational modes and the coupling between excited modes can be successfully extracted from the expansion of β(t) in terms of vibrational modes. This proof-of-principle simulation clearly demonstrates that various information of the structures and reaction dynamics of large clusters or biomolecules can be retrieved by decomposing the experimentally determined β(t) into vibrational modes. [ABSTRACT FROM AUTHOR]

Charge transfer (CT) at avoided crossings of excited ionized states of argon dimers is observed using a two-color pump-probe experiment at the free-electron laser in Hamburg (FLASH). The process is initiated by the absorption of three 27-eV-photons from the pump pulse, which leads to the population of Ar2+*–Ar states. Due to nonadiabatic coupling between these one-site doubly ionized states and two-site doubly ionized states of the type Ar+*–Ar+, CT can take place leading to the population of the latter states. The onset of this process is probed by a delayed infrared (800 nm) laser pulse. The latter ionizes the dimers populating repulsive Ar2+ –Ar+ states, which then undergo a Coulomb explosion. From the delay-dependent yields of the obtained Ar2+ and Ar+ ions, the lifetime of the charge-transfer process is extracted. The obtained experimental value of (531 ± 136) fs agrees well with the theoretical value computed from Landau-Zener probabilities. [ABSTRACT FROM AUTHOR]

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, T e , 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 T e values (0–1.0 eV), the laser energy induces electronic transitions, while the InP lattice remains undisturbed and cool. In the second stage (with T e 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. [ABSTRACT FROM AUTHOR]

The long-time correlated decay dynamics of strong-field exposed helium nanodroplets is studied by means of photoelectron spectroscopy. As a result of the adiabatic expansion of the laser-produced, fully inner-ionized nanoplasma, delocalized electrons in the deep confining mean field potential are shifted towards the vacuum level. Meanwhile, part of the electrons localize in bound levels of the helium ions. The simple hydrogenlike electronic structure of He+ results in clear signatures in the experimentally observed photoelectron spectra, which can be traced back to bound-free and bound-bound transitions. Auger electron emission takes place as a result of the transfer of transition energy to weakly bound electrons in the quasifree electron band. Hence, the spatial and temporal development of the nanoplasma cloud is encoded in the experimental spectra, whereas the electronic properties of He+ help resolve the different contributions. [ABSTRACT FROM AUTHOR]

The photodissociation dynamics of CH3I and CH2ClI at 272 nm were investigated by time-resolved Coulomb explosion imaging, with an intense non-resonant 815 nm probe pulse. Fragment ion momenta over a wide m/z range were recorded simultaneously by coupling a velocity map imaging spectrometer with a pixel imaging mass spectrometry camera. For both molecules, delay-dependent pump-probe features were assigned to ultraviolet-induced carbon-iodine bond cleavage followed by Coulomb explosion. Multi-mass imaging also allowed the sequential cleavage of both carbon-halogen bonds in CH2ClI to be investigated. Furthermore, delay-dependent relative fragment momenta of a pair of ions were directly determined using recoil-frame covariance analysis. These results are complementary to conventional velocity map imaging experiments and demonstrate the application of time-resolved Coulomb explosion imaging to photoinduced real-time molecular motion. [ABSTRACT FROM AUTHOR]

The dissociation dynamics of CS2 molecules in collisions with 1.0 keV electrons is studied. We observe a series of two- and three-body fragmentation channels which are identified from the correlation map between fragment ions. For all of the channels, the kinetic energy release (KER) distributions are obtained. The Dalitz plot and Newton diagram are adopted to analyze the fragmentation dynamics of the three-body dissociation channels. For C S 2 3 + and C S 2 4 + , both the concerted and sequential fragmentation mechanisms are observed where the concerted mechanism dominates. For C S 2 5 + , only the concerted mechanism is observed. Two types of Coulomb explosion models considering the molecular vibration are adopted to simulate the experimental KER distributions of the three-body channels. While obvious deviations are observed considering each ion during the whole dissociation process with an integer charge, good agreement can be achieved within deviation less than 5% if the charge state of the ions are adopted from ab initio calculations. [ABSTRACT FROM AUTHOR]

Dimers and trimers of carbonyl sulfide (OCS) molecules embedded in helium nanodroplets are aligned by a linearly polarized 160 ps long moderately intense laser pulse and Coulomb exploded with an intense 40 fs long probe pulse in order to determine their structures. For the dimer, recording of 2D images of OCS+ and S+ ions and covariance analysis of the emission directions of the ions allow us to conclude that the structure is a slipped-parallel shape similar to the structure found for gas phase dimers. For the trimer, the OCS+ ion images and the corresponding covariance maps reveal the presence of a barrel-shaped structure (as in the gas phase) but also other structures not present in the gas phase, most notably a linear chain structure. [ABSTRACT FROM AUTHOR]

BackgroundThe research of molecular fragmentation dynamics has attracted extensive attention in the fields of physics, chemistry and biology. The major challenge in this field is to understand the selectivity of molecular bond breaking and to elucidate which parameters control bond fission.PurposeThis study aims to reveal the mechanism of two and three-body fragmentation of CO2 in strong laser fields and to elucidate the dynamics information of the ion fragmentation in the Coulomb explosion.MethodsThe time-of-flight (TOF) and three-dimensional momentum distributions of ion fragments were obtained using a cold-target recoil ion momentum spectroscopy (COLTRIMS). Precise identification of the two-body and three-body dissociation channels of CO2 was determined by the photoion-photoion coincidence (PIPICO) and the photoion-photoion-photoion coincidence (PIPIPICO) techniques. The occurrence of sequential and non-sequential fragmentation during three-body dissociation was revealed by the momentum correlation between two O ions. Finally, the dynamics of the three-body fragmentation process was visualized by the Newton diagram.ResultsFour two-body dissociation channels and three three-body dissociation channels for CO2q+ (q≤4) are identified with the coincidence technique. The kinetic energy release (KER) distribution of these dissociation channels is obtained from the three-dimensional momentum.ConclusionsThe experiments reveal that the dynamic collimation mechanism plays a dominant role in the two-body fragmentation channels, and the ion fragments of the four two-body fragmentation channels are mainly emitted along the laser polarization direction with the significant anisotropic distribution. Non-sequential and sequential fragmentation of CO2 is separated and identified in the momentum correlation and Newtonian diagrams. In the first step of the sequential fragmentation of CO24+, the O2+ and CO2+ ionic fragments are always produced. It is further shown that the vibration and rotation of the CO2+ ion are shown to occur before the fragmentation of the second step.

The break-up of molecules in the stripper of an AMS facility induces an energy and angular spread in the beam. This can cause beam losses, thereby reducing the performance of an AMS facility. With an appropriate design, these effects can be minimised and the efficiency enhanced. As an example, the break-up of BeO molecules is discussed here. First the basic physics is described and corresponding models and computer codes are explained. Then experimental data are shown and compared with the models. For gas stripping, beam profiles are available for small and large facilities. All show tails which can be attributed to the dissociation of the molecules. The size of the effect depends on various parameters such as beam energy, selected charge state, stripping gas type and ion optics. Foil stripping leads to energy distributions which are much wider, and show typically a double peak. [ABSTRACT FROM AUTHOR]

In this work we instigated the fragmentation of Au microparticles supported on a thin amorphous carbon film by irradiating them with a gradually convergent electron beam inside the Transmission Electron Microscope. This phenomenon has been generically labeled as "electron beam-induced fragmentation" or EBIF and its physical origin remains contested. On the one hand, EBIF has been primarily characterized as a consequence of beam-induced heating. On the other, EBIF has been attributed to beam-induced charging eventually leading to Coulomb explosion. To test the feasibility of the charging framework for EBIF, we instigated the fragmentation of Au particles under two different experimental conditions. First, with the magnetic objective lens of the microscope operating at full capacity, i.e. background magnetic field B = 2 T, and with the magnetic objective lens switched off (Lorenz mode), i.e. B = 0 T. We observe that the presence or absence of the magnetic field noticeably affects the critical current density at which EBIF occurs. This strongly suggests that magnetic field effects play a crucial role in instigating EBIF on the microparticles. The dependence of the value of the critical current density on the absence or presence of an ambient magnetic field cannot be accounted for by the beam-induced heating model. Consequently, this work presents robust experimental evidence suggesting that Coulomb explosion driven by electrostatic charging is the root cause of EBIF. [Display omitted] • Experimental study of the magnetic field effect on the e-beam induced fragmentation • Theoretical framework explaining the difference of critical current densities • The simulated Coulomb explosion occuring in pico-second order • Raman, XRD, SAED studies of the amorphous carbon films and 4-probe resistance measurements [ABSTRACT FROM AUTHOR]

The behavior of nitrosyl chloride (ClNO) exposed to ionizing radiation was studied by direct probing valence-shell electrons in temporal coincidence with ions originating from the fragmentation process of the transient ClNO2+. Such a molecular dication was produced by double photoionization with synchrotron radiation in the 24–70 eV photon energy range. The experiment has been conducted at the Elettra Synchrotron Facility of Basovizza (Trieste, Italy) using a light beam linearly polarized with the direction of the polarization vector parallel to the ClNO molecular beam axis. ClNO molecules crossing the photon beam at right angles in the scattering region are generated by effusive expansion and randomly oriented. The threshold energy for the double ionization of ClNO (30.1 ± 0.1 eV) and six dissociation channels producing NO+/Cl+, N+/Cl+, N+/O+, O+/Cl+, ClN+/O+, NO+/Cl2+ ion pairs, with their relative abundance and threshold energies, have been measured.

Intermolecular interactions involving aromatic rings are ubiquitous in biochemistry and they govern the properties of many organic materials. Nevertheless, our understanding of the structures and dynamics of aromatic clusters remains incomplete, in particular for systems beyond the dimers, despite their high presence in many macromolecular systems such as DNA and proteins. Here, we study the fragmentation dynamics of benzene trimer that represents a prototype of higher-order aromatic clusters. The trimers are initially ionized by electron-collision with the creation of a deep-lying carbon 2s−1 state or one outer-valence and one inner-valence vacancies at two separate molecules. The system can thus relax via ultrafast intermolecular decay mechanisms, leading to the formation of C 6 H 6 + ⋅ C 6 H 6 + ⋅ C 6 H 6 + trications and followed by a concerted three-body Coulomb explosion. Triple-coincidence ion momentum spectroscopy, accompanied by ab-initio calculations and further supported by strong-field laser experiments, allows us to elucidate the details on the fragmentation dynamics of benzene trimers. Higher-order aromatic clusters are prevalent in biochemical systems, but a full understanding of their structural and dynamical properties is lacking. Here, the authors demonstrate that inner-valence ionization can induce ultrafast relaxation and further fragmentation mechanisms in benzene trimers. [ABSTRACT FROM AUTHOR]

Coulomb explosion experiments using linearly polarized intense 60 fs laser pulses were conducted for structural characterization of three dichloroethylene (DCE) isomers, 1,1-DCE, cis-1,2-DCE, and trans-1,2-DCE. Under relatively low laser intensity at 1.8 × 1014 W/cm2, mass-resolved momentum imaging (MRMI) for selected fragment ions of 35Cl+ and C2+ revealed different patterns for the three isomers. The C2+ ion fragmented from multiply charged trans-1,2-DCE was forced to leave perpendicularly to the direction of the laser polarization, due to recoil forces from adjacent cations. In contrast, the fast ions of C2+ from cis-1,2-DCE exhibited an isotropic distribution, whereas the fast ions of C2+ from 1,1-DCE recoiled along the laser polarization together with the slow C2+ ions, and thereby distinction of the three isomers was demonstrated. Coulomb explosion occurs predominantly at specific orientation, which is useful for potential applications of MRMI analysis to molecular structure assays. [ABSTRACT FROM AUTHOR]

Additive manufacturing (AM) will empower the next breakthroughs in nanotechnology by combining unmatched geometrical freedom with nanometric resolution. Despite recent advances, no micro-AM technique has been able to synthesize functional nanostructures with excellent metal quality and sub-100 nm resolution. Here, significant breakthroughs in electrohydrodynamic redox 3D printing (EHD-RP) are reported by directly fabricating high-purity Cu (>98 at.%) with adjustable voxel size from >6µm down to 50 nm. This unique tunability of the feature size is achieved by managing in-flight solvent evaporation of the ion-loaded droplet to either trigger or prevent the Coulomb explosion. In the first case, the landing of confined droplets on the substrate allows the fabrication of high-aspect-ratio 50 nm-wide nanopillars, while in the second, droplet disintegration leads to large-area spray deposition. It is discussed that the reported pillar width corresponds to the ultimate resolution achievable by EHD printing. The unrivaled feature size and growth rate (>100 voxel s -1 ) enable the direct manufacturing of 30 µm-tall atom probe tomography (APT) tips that unveil the pristine microstructure and chemistry of the deposit. This method opens up prospects for the development of novel materials for 3D nano-printing., (© 2024 The Author(s). Small published by Wiley‐VCH GmbH.)