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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. [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]

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.

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]

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]

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.

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]

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]

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]

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]

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]

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 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 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]

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.

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]

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.

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.

We experimentally demonstrate the dissociative photoionization of CHBrCl2 molecules in a femtosecond laser field by time-of-flight mass spectrum and dc-slice imaging technology. The results suggest that the low kinetic energy components are from the dissociative ionization process of single-charged molecular ions. The angular distribution of fragment Cl+ ions can be attributed to the features of dissociative state and molecular configuration, and that of Br+ ions results from the electronic wave-packet evolution and combination of the multi-dissociation processes. The high kinetic energy components are from the Coulomb explosion of multi-charged molecular ions, and the error of the C-Br distance involved in the Coulomb explosion can be explained by the movement of the effective charge center of the polyatomic molecule. [ABSTRACT FROM AUTHOR]

Nanoparticle mediated laser induced breakdown can be used for Nanoparticle synthesis, cell nanosurgery and laser induced breakdown spectroscopy. To investigate the photo-thermal conversion of gold nanoparticles during pulsed laser irradiation, the electron-phonon two temperature model was established in this study. The impact of laser energy density and pulse width on the thermal conversion and morphology change of gold nanorods were investigated and compared with experimental observations. The results show that the melting threshold of gold nanorods under nanosecond laser irradiation is about twenty times that of femtosecond laser irradiation. The mechanisms of nanorod fragmentation are different between femto and nanosecond laser irradiation: particle melting is more likely to occur in nanosecond laser irradiation, while the Coulomb explosion is highly likely to occur in femtosecond laser irradiation. [ABSTRACT FROM AUTHOR]

Fixing molecules in space is a crucial step for the imaging of molecular structure and dynamics. Here, we demonstrate three-dimensional (3D) field-free alignment of the prototypical asymmetric top molecule indole using elliptically polarized, shaped, off-resonant laser pulses. A truncated laser pulse is produced using a combination of extreme linear chirping and controlled phase and amplitude shaping using a spatial-light-modulator (SLM) based pulse shaper of a broadband laser pulse. The angular confinement is detected through velocity-map imaging of H+ and C2+ fragments resulting from strong-field ionization and Coulomb explosion of the aligned molecules by intense femtosecond laser pulses. The achieved three-dimensional alignment is characterized by comparing the result of ion-velocity-map measurements for different alignment directions and for different times during and after the alignment laser pulse to accurate computational results. The achieved strong three-dimensional field-free alignment of < cos 2 δ > = 0.89 demonstrates the feasibility of both, strong three-dimensional alignment of generic complex molecules and its quantitative characterization. Field-free 3D alignment of complex molecules is an important step toward the imaging of molecular dynamics. Here, the authors demonstrate pulse-shaping of long picosecond pulses for the 3D field-free alignment of the prototypical non-rotation-symmetric molecule indole. [ABSTRACT FROM AUTHOR]

We report on the design and capabilities of a reaction microscope (REMI) end-station at the Shanghai Soft X-ray Free-Electron Laser Facility (SXFEL). This apparatus allows high-resolution and 4 π solid-angle coincidence detection of ions and electrons. The components of REMI, including a supersonic gas injection system, spectrometer, detectors and data acquisition system, are described in detail. By measuring the time of flight and the impact positions of ions and electrons on the corresponding detectors, three-dimensional momentum vectors can be reconstructed to study specific reaction processes. Momentum resolutions of ions and electrons with 0.11 a.u. are achieved, which have been measured from a single ionization experiment of oxygen molecules in an infrared (IR), femtosecond laser field, under vacuum at 1.2 × 10 − 10 torr, in a reaction chamber. As a demonstration, a Coulomb explosion experiment of oxygen molecules in the IR field is presented. These results demonstrate the performance of this setup, which provides a basic tool for the study of atomic and molecular reactions at SXFEL. [ABSTRACT FROM AUTHOR]

We present the results of an integrated laboratory and modeling investigation into the impact of stellar X-rays on cosmic dust. Carbonaceous grains were prepared in a cooled (<200 K) supersonic expansion from aromatic molecular precursors, and were later irradiated with 970 eV X-rays. Silicate (enstatite) grains were prepared via laser ablation, thermally annealed, and later irradiated with 500 eV X-rays. Infrared spectra of the 3.4 ÎĽ m band of the carbon sample prepared with benzene revealed 84% ± 5% band area loss for an X-ray dose of 5.2 Ă—1023 eV.cmâˆ'2. Infrared spectra of the 8â€"12 ÎĽ m Siâ€"O band of the silicate sample revealed band area loss up to 63% ± 5% for doses of 2.3 Ă— 1023 eV.cmâˆ'2. A hybrid Monte Carlo particle trajectory approach was used to model the impact of X-rays and ensuing photoelectrons, Auger and collisionally ionized electrons through the bulk. As a result of X-ray ionization and ensuing Coulomb explosions on surface molecules, the calculated mass loss is 60% for the carbonaceous sample and 46% for the silicate sample, within a factor of 2 of the IR band loss, supporting an X-ray induced mass-loss mechanism. We apply the laboratory X-ray destruction rates to estimate the lifetimes of dust grains in protoplanetary disks surrounding 1 M ⊙ and 0.1 M ⊙ G and M stars. In both cases, X-ray destruction timescales are short (a few million years) at the disk surface, but are found to be much longer than typical disk lifetimes (≳10 Myr) over the disk bulk. [ABSTRACT FROM AUTHOR]

We discuss how Coulomb explosion imaging (CEI), triggered by intense femtosecond laser pulses and combined with laser-induced alignment and covariance analysis of the angular distributions of the recoiling fragment ions, provides new opportunities for imaging the structures of molecules and molecular complexes. First, focusing on gas phase molecules, we show how the periodic torsional motion of halogenated biphenyl molecules can be measured in real time by timed CEI, and how CEI of one-dimensionally aligned difluoroiodobenzene molecules can uniquely identify four structural isomers. Next, focusing on molecular complexes formed inside He nano-droplets, we show that the conformations of noncovalently bound dimers or trimers, aligned in one or three dimensions, can be determined by CEI. Results presented for homodimers of CS2, OCS, and bromobenzene pave the way for femtosecond time-resolved structure imaging of molecules undergoing bimolecular interactions and ultimately chemical reactions. [ABSTRACT FROM AUTHOR]

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. [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.

Coulomb explosion imaging is a promising experimental tool to study individual molecules. In this work simulation data for the x-ray induced Coulomb explosion of 2-iodopyridine is analyzed and the involved fragmentation dynamics are described. It is found that particular final ion momenta show correlations that reflect a collision of two atoms during the explosion. Variations of the proton kinetic energies can be associated with variations in the charge build-up time. Covariances of the forces during the explosion can be utilized to simplify the description of the dynamics in reduced dimensionality using only four collective coordinates. [ABSTRACT FROM AUTHOR]

Using single-shot velocity map imaging technique, explosion imaging of different ion species ejected from 50 nm SiO2 nanoparticles are obtained excitedly by strong near-infrared and ultraviolet femtosecond laser fields. Characteristic momentum distributions showing forward emission of the ions at low excitation intensities and shock wave behaviors at high intensities are observed. When the excitation intensity is close to the dissociative ionization threshold of the surface molecules, the resulting ion products can be used to image the instant near-field distributions. The underlying dynamics of shock formation are simulated by using a Coulomb explosion model. Our results allow one to distinguish the ultrafast strong-field response of various molecular species in nanosystems and will open a new way for further exploration of the underlying dynamics of laser-and-nanoparticle interactions. [ABSTRACT FROM AUTHOR]

We have deduced the structure of the bromobenzeneâ€"I2 heterodimer and the (bromobenzene)2 homodimer inside helium droplets using a combination of laser-induced alignment, Coulomb explosion imaging (CEI), and three-dimensional ion imaging. The complexes were fixed in a variety of orientations in the laboratory frame, then in each case multiply ionized by an intense laser pulse. A three dimensional ion imaging detector, including a Tpx3Cam detector allowed us to measure the correlations between velocity vectors of different fragments and, in conjunction with classical simulations, work backward to the initial structure of the complex prior to explosion. For the heterodimer, we find that the I2 molecular axis intersects the phenyl ring of the bromobenzene approximately perpendicularly. The homodimer has a stacked parallel structure, with the two bromine atoms pointing in opposite directions. These results illustrate the ability of CEI to determine the structure of large complexes, and point the way toward real-time measurements of bimolecular reactions inside helium droplets. [ABSTRACT FROM AUTHOR]

Abstract The trihydrogen ion has a central role in creating complex molecules in the interstellar medium. Therefore, its formation and destruction mechanisms in high photon energy environments involving organic molecules are drawing significant experimental and theoretical attention. Here, we employ a combination of time‐resolved ultrafast extreme‐ultraviolet pump and near‐infrared probe spectroscopy applied to the deuterated CH3OD methanol molecule. Similar to other double‐ionization studies, the isotopic labeling reveals two competing pathways for forming trihydrogen: A) H3++COH+ and B) H3++HCO+. We validate our high‐level ab initio nonadiabatic molecular dynamic simulations by showing that it closely reproduces the essential features of the measured kinetic energy release distribution and branching ratios of the two pathways of the deuterated system. The success of ab initio simulation in describing single photon double‐ionization allows for an unprecedented peek into the formation pathways for the undeuterated species, beyond present experimental reach. For this case, we find that the kinetic energy release of pathway B shifts to lower energies by more than 0.6 eV due to a dynamical isotope effect. We also determine the mechanism for trihydrogen formation from excited states of the dication and elucidate the isotope effect's role in the observed dynamics.

We report the comprehensive measurement of the Coulomb explosion of the double and triple ionization of N2 in collisions with slow highly-charged ions. The experiments are carried out with ion beams of different charge states for a given velocity (1 a.u.) and at three different velocities for a given charge state (O6+). By analyzing the kinetic energy release distributions of and molecular ions, the effects of projectile velocity and charge state on the population of different molecular states are inferred. We explain such a systematic variation in the population of different molecular states considering the energy deposition to N2 by the projectile ions. [ABSTRACT FROM AUTHOR]

The Jahn-Teller effect is an essential mechanism of spontaneous symmetry breaking in molecular and solid state systems, and has far-reaching consequences in many fields. Up to now, to directly image the onset of Jahn-Teller symmetry breaking remains unreached. Here we employ ultrafast ion-coincidence Coulomb explosion imaging with sub-10 fs resolution and unambiguously image the ultrafast dynamics of Jahn-Teller deformations of CH 4 + cation in symmetry space. It is unraveled that the Jahn-Teller deformation from C3v to C2v geometries takes a characteristic time of 20 ± 7 fs for this system. Classical and quantum molecular dynamics simulations agree well with the measurement, and reveal dynamics for the build-up of the C2v structure involving complex revival process of multiple vibrational pathways of the CH 4 + cation. The Jahn-Teller effect is the spontaneous symmetry breaking of the molecular structure caused by the coupling of electrons and nuclei. Here the authors use ultrafast Coulomb explosion imaging to map the evolution of the fundamental symmetry lowering process in photoionized methane within around 20fs. [ABSTRACT FROM AUTHOR]

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We experimentally demonstrate the dissociative photoionization of CHBrCl2 molecules in a femtosecond laser field by time-of-flight mass spectrum and dc-slice imaging technology. The results suggest that the low kinetic energy components are from the dissociative ionization process of single-charged molecular ions. The angular distribution of fragment Cl+ ions can be attributed to the features of dissociative state and molecular configuration, and that of Br+ ions results from the electronic wave-packet evolution and combination of the multi-dissociation processes. The high kinetic energy components are from the Coulomb explosion of multi-charged molecular ions, and the error of the C-Br distance involved in the Coulomb explosion can be explained by the movement of the effective charge center of the polyatomic molecule.

XUV multiphoton ionization of molecules is commonly used in free-electron laser experiments to study charge transfer dynamics. However, molecular dissociation and electron dynamics, such as multiple photon absorption, Auger decay, and charge transfer, often happen on competing time scales, and the contributions of individual processes can be difficult to unravel. We experimentally investigate the Coulomb explosion dynamics of methyl iodide upon core–hole ionization of the shallow inner-shell of iodine (4d) and classically simulate the fragmentation by phenomenologically introducing ionization dynamics and charge transfer. Under our experimental conditions with medium fluence and relatively long XUV pulses (∼75 fs), we find that fast Auger decay prior to charge transfer significantly contributes to the charging mechanism, leading to a yield enhancement of higher carbon charge states upon molecular dissociation. Furthermore, we argue for the existence of another charging mechanism for the weak fragmentation channels leading to triply charged carbon atoms. This study shows that classical simulations can be a useful tool to guide the quantum mechanical description of the femtosecond dynamics upon multiphoton absorption in molecular systems. [ABSTRACT FROM AUTHOR]

With an intense femtosecond two-color pulse optimized for the generation of even-order harmonics from CO molecules, we directly measure the actual degrees of orientation by utilizing the Coulomb explosion imaging technique with appropriate probe polarization. We find that the macroscopic orientation of CO molecules is negligible even when significant even-order harmonics are observed. This finding shows that the generation of even-order harmonics cannot be ascribed to the macroscopic orientation of CO molecules. The rotational wave packet of CO molecules created with an intense femtosecond two-color pulse is thought to be in an uninvestigated quantum state, which cannot be explained by the theoretical model based on the Born–Oppenheimer approximation, without inversion symmetry at any of the three steps of high-order harmonic generation, leading to the generation of even-order harmonics. [ABSTRACT FROM AUTHOR]

We report on the design and capabilities of a reaction microscope (REMI) end-station at the Shanghai Soft X-ray Free-Electron Laser Facility (SXFEL). This apparatus allows high-resolution and 4π solid-angle coincidence detection of ions and electrons. The components of REMI, including a supersonic gas injection system, spectrometer, detectors and data acquisition system, are described in detail. By measuring the time of flight and the impact positions of ions and electrons on the corresponding detectors, three-dimensional momentum vectors can be reconstructed to study specific reaction processes. Momentum resolutions of ions and electrons with 0.11 a.u. are achieved, which have been measured from a single ionization experiment of oxygen molecules in an infrared (IR), femtosecond laser field, under vacuum at 1.2×10−10 torr, in a reaction chamber. As a demonstration, a Coulomb explosion experiment of oxygen molecules in the IR field is presented. These results demonstrate the performance of this setup, which provides a basic tool for the study of atomic and molecular reactions at SXFEL.

This paper treats the characteristic topics of MeV/atom cluster ion beams produced using tandem accelerators both in the production stage and in the penetration stage from the viewpoint of fundamental processes. The former is related to atomic collisions in that production and decay of a cluster ion Cn+ (n=1−4) colliding with a charge-changing rare gas underlined through the electron-loss process. Regarding the latter, relatively small carbon clusters Cn+ (n=2−10) are treated. The reduction effect of the average charge of cluster ions in a material is first presented. Next, the electronic stopping power and the energy loss, the polarization force, and the coulomb explosion under cluster-ion impact are described in the dielectric function form. Alignment and structure effects are stressed. As a large and highly symmetric cluster, the electronic stopping power and the average charge are shown for a C60 cluster ion moving inside a solid. Throughout the paper, it is emphasized that the vicinage effect originating from correlation on spatial structure and orientation of constituent ions plays the key role. Moreover, results obtained in cluster production and penetration phenomena are mostly different from multiplication of those under single-ion impact.

Van der Waals clusters are weakly bound atomic/molecular systems and are an important medium for understanding micro-environmental chemical phenomena in bio-systems. The presence of neighboring atoms may open channels otherwise forbidden in isolated atoms/molecules. In hydrogen-bond clusters, proton transfer plays a crucial role, which involves mass and charge migration over large distances within the cluster and results in its fragmentation. Here we report an exotic transfer channel involving a heavy N+ ion observed in a doubly charged cluster produced by 1 MeV Ne8+ ions: (N2Ar)2+→N++NAr+. The neighboring Ar atom decreases the N 2 2 + barrier height and width, resulting in significant shorter lifetimes of the metastable molecular ion state N 2 2 + ( X 1 Σ g + ). Consequently, the breakup of the covalent N+−N+ bond, the tunneling out of the N+ ion from the N 2 2 + potential well, as well as the formation of an N−Ar+ bound system take place almost simultaneously, resulting in a Coulomb explosion of N+ and NAr+ ion pairs. There are multiple ways by which energy and charge transfer occur in weakly bound systems. Here the authors reveal a heavy ion N+ transfer in a doubly charged Van der Waals cluster produced in collisions of the highly charged Ne8+ ion with N2Ar, leading to fragmentation of N+ and NAr+ via Coulomb explosion. [ABSTRACT FROM AUTHOR]

In the probe-before-destroy methodology, developed with the advent of X-ray free-electron lasers, the investigated system is probed with an ultra-short (femtosecond) X-ray pulse within time shorter than that the X-ray-induced damage needs to propagate. Radiation damage is typically considered in terms of the Coulomb explosion which needs about 50 fs to induce observable effects in the material structure. It has been, however, shown that the much faster electronic structure change has also a significant influence on the X-ray emission spectroscopy data and may alter the X-ray diffraction patterns. This work reports on energy and time distribution of photo-electrons induced in water by an X-ray pulse with properties typical for an X-ray free-electron laser operated in the intensity regime below the sequential photoionization regime. The electron flux was simulated on the basis of a kinetic model and was found to be significant over the course of the X-ray pulse duration. The presented findings call for consideration of the X-ray-induced electrons in studies on solutions and samples embedded in matrices. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]