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Xray free‐electron lasers (XFELs) enable experiments that would have been impractical or impossible at conventional X‐ray laser facilities. Indeed, more XFEL facilities are being built and planned, with their aim to deliver larger pulse energies and higher peak brilliance. While seeking to increase the pulse power, it is quintessential to consider the maximum pulse fluence that a grazing‐incidence FEL mirror can withstand. To address this issue, several studies were conducted on grazing‐incidence damage by soft X‐ray FEL pulses at the European XFEL facility. Boron carbide (B4C) coatings on polished silicon substrate were investigated using 1 keV photon energy, similar to the X‐ray mirrors currently installed at the soft X‐ray beamlines (SASE3). The purpose of this study is to compare the damage threshold of B4C and Si to determine the advantages, tolerance and limits of using B4C coatings. [ABSTRACT FROM AUTHOR]

Extreme ultraviolet (XUV) capillary-discharge lasers (CDLs) are a suitable source for the efficient, clean ablation of ionic crystals, which are obviously difficult to ablate with conventional, long-wavelength lasers. In the present study, a single crystal of cesium iodide (CsI) was irradiated by multiple, focused 1.5-ns pulses of 46.9-nm radiation delivered from a compact XUV-CDL device operated at either 2-Hz or 3-Hz repetition rates. The ablation rates were determined from the depth of the craters produced by the accumulation of laser pulses. Langmuir probes were used to diagnose the plasma plume produced by the focused XUV-CDL beam. Both the electron density and electron temperature were sufficiently high to confirm that ablation was the key process in the observed CsI removal. Moreover, a CsI thin film on MgO substrate was prepared by XUV pulsed laser deposition; a fraction of the film was detected by X-ray photoelectron spectroscopy.

The availability of reliable modeling tools and input data required for the prediction of surface removal rate from the lithium fluoride targets irradiated by the intense photon beams is essential for many practical aspects. This study is motivated by the practical implementation of soft X-ray (SXR) or extreme ultraviolet (XUV) lasers for the pulsed ablation and thin film deposition. Specifically, it is focused on quantitative description of XUV laser-induced desorption/ablation from lithium fluoride, which is a reference large band-gap dielectric material with ionic crystalline structure. Computational framework was proposed and employed here for the reconstruction of plume expansion dynamics induced by the irradiation of lithium fluoride targets. The morphology of experimentally observed desorption/ablation craters were reproduced using idealized representation (two-zone approximation) of the laser fluence profile. The calculation of desorption/ablation rate was performed using one-dimensional thermomechanic model (XUV-ABLATOR code) taking into account laser heating and surface evaporation of the lithium fluoride target occurring on a nanosecond timescale. This step was followed by the application of two-dimensional hydrodynamic solver for description of laser-produced plasma plume expansion dynamics. The calculated plume lengths determined by numerical simulations were compared with a simple adiabatic expansion (blast-wave) model.

The application of fluorescent crystal media in wide-range X-ray detectors provides an opportunity to directly image the spatial distribution of ultraintense X-ray beams including investigation of the focal spot of free-electron lasers. Here the capabilities of the micro- and nano-focusing X-ray refractive optics available at the High Energy Density instrument of the European XFEL are reported, as measured in situ by means of a LiF fluorescent detector placed into and around the beam caustic. The intensity distribution of the beam focused down to several hundred nanometers was imaged at 9 keV photon energy. A deviation from the parabolic surface in a stack of nanofocusing Be compound refractive lenses (CRLs) was found to affect the resulting intensity distribution within the beam. Comparison of experimental patterns in the far field with patterns calculated for different CRL lens imperfections allowed the overall inhomogeneity in the CRL stack to be estimated. The precise determination of the focal spot size and shape on a sub-micrometer level is essential for a number of high energy density studies requiring either a pin-size backlighting spot or extreme intensities for X-ray heating. [ABSTRACT FROM AUTHOR]

The implosion of a solid deuterium gas-puff Z-pinch was studied on the S-300 pulsed power generator [A. S. Chernenko, et al., Proceedings of 11th Int. Conf. on High Power Particle Beams, 154 (1996)]. The peak neutron yield above [10.sup.10] was achieved on the current level of 2 MA. The fusion neutrons were generated at about 150 ns after the current onset, i.e., during the stagnation and at the beginning of the expansion of a plasma column. The neutron emission lasted on average 25 ns. The neutron energy distribution function was reconstructed from 12 neutron time-of-flight signals by the Monte Carlo simulation. The side-on neutron energy spectra peaked at 2.42 [+ or -] 0.04 MeV with about 450-keV FWHM. In the downstream direction (i.e., the direction of the current flow from the anode toward the cathode), the peak neutron energy and the width of a neutron spectrum were 2.6 [+ or -] 0.1 MeV and 400 keV, respectively. The average kinetic energy of fast deuterons, which produced fusion neutrons, was about 100 keV. The generalized beam-target model probably fits best to the obtained experimental data. Index Terms--Deuterium, fusion reaction, gas puff, Monte Carlo reconstruction, neutron energy spectra, neutrons, Z-pinch.

The high‐energy‐density synthesis of NxOy species is simulated in gas mixtures representing an O2‐free early‐Earth atmosphere by terawatt‐kilojoule‐class laser‐induced dielectric breakdown (LIDB). These experiments differ from previous LIDB experiments due to the 100 times greater energy delivered per pulse and sensitive analysis of products by high‐resolution infrared spectroscopy. The measured yields of NO, N2O, and NO2 are 0.08–8 × 1015, 5 × 1012, and 0.03–7 × 1014 molec J −1. The high N2O yield is above the upper‐limit constraint of previous tabletop LIDB experiments and the expected yield of a thermochemical freeze‐out at any temperature between 2000 and 5000 K, while the NO and NO2 yields are in broad agreement with freeze‐out models. Using a one dimensional chemical model of the Hadean atmosphere and a simple model of late bombardment, we compute the source flux of N2O assuming the same high production yield as measured experimentally and find the steady‐state partial pressure of N2O is insufficient to warm the climate. Plain Language Summary: The climate of the Earth 4.5 to 4 billion years ago is not well known but geological evidence suggests the presence of liquid water, which is at odds with the possibility of a very‐cold early Earth. Extra greenhouse warming by atmospheric gases is thought necessary to keep the surface temperature high enough for liquid water. Nitrous oxide is a possible greenhouse gas and its high‐temperature formation in an atmosphere undergoing intense meteor bombardment may provide additional means of warming the early Earth. In this paper, we mimic the impact formation of nitrogen oxide molecules in the laboratory using a high‐energy laser‐induced plasma. The laser generates pulses 100 times more energetic than in previous studies and the new molecules are measured by infrared spectroscopy. We then compute the stable amount of nitrous oxide that might have existed 4.5 billion years ago and find this is still too small to contribute to greenhouse warming. The effect of large amounts of impact‐formed nitrogen oxides may still lead to significant short‐term consequences of a large impact, or become chemical inputs to the first stages of biochemistry, or be relevant for observational models exoplanet atmospheres in young star systems encountering heavy bombardment. Key Points: A terawatt‐class laser simulation of NxOy formation by impacts finds a large yield of N2OOne‐dimensional atmospheric model shows that impact‐production of N2O is still insufficient to significantly warm the Hadean Earth [ABSTRACT FROM AUTHOR]

The development of ultra-intense electron pulse for applications needs to be accompanied by the implementation of a practical dosimetry system. In this study four different systems were investigated as dosimeters for low doses with a very high-dose-rate source. First, the effects of ultra-short pulses were investigated for the yields of the Fricke dosimeter based on acidic solutions of ferrous sulfate; it was established that the yields were not significantly affected by the high dose rates, so the Fricke dosimeter system was used as a reference. Then, aqueous solutions of three compounds as fluorescence chemical dosimeters were utilized, each operated at a different solution pH: terephthalic acid - basic, trimesic acid - acidic, and coumarin-3-carboxylic acid (C3CA) - neutral. Fluorescence chemical dosimeters offer an attractive alternative to chemical dosimeters based on optical absorption for measuring biologically relevant low doses because of their higher sensitivity. The effects of very intense dose rate (TGy/ s) from pulses of fast electrons generated by a picosecond linear accelerator on the chemical yields of fluorescence chemical dosimeters were investigated at low peak doses (<20 Gy) and compared with yields determined under low-dose-rate irradiation from a 60 Co gamma-ray source (mGy/s). For the terephthalate and the trimesic acid dosimeters changes in the yields were not detected within the estimated (∼10%) precision of the experiments, but, due to the complexity of the mechanism of the hydroxyl radical initiated reactions in solutions of the relevant aromatic compounds, significant reductions of the chemical yield (–60%) were observed when the C3CA dosimeter was irradiated with the ultra-short pulses. [ABSTRACT FROM AUTHOR]

Featured Application: laser surface-processing. Monocrystalline barium fluoride (BaF2) slab targets were irradiated by focused 46.9-nm laser radiation at various fluence levels above the ablation threshold. Well-developed ablation patterns with sharp edges were studied by AFM (atomic force microscopy). Their inner surfaces were uniformly covered by periodic structures. The spatial period of the ripples depends on the laser fluence. When the sample is rotated by 45°, the orientation of the grating-like structure changes accordingly. Thus, the grating vector of the periodic structure seems to be coupled to the crystallographic planes of the single crystal. This means that the XUV-laser induced ripples reported here differ from LIPSS (laser-induced periodic surface structures) associated with interference phenomena occurring on illuminated surfaces. Therefore, other mechanisms are discussed to explain the formation of the periodic nanostructures reported in this article. [ABSTRACT FROM AUTHOR]

We present a computational case study of X-ray single-particle imaging of hydrated proteins on an example of 2-Nitrogenase–Iron protein covered with water layers of various thickness, using a start-to-end simulation platform and experimental parameters of the SPB/SFX instrument at the European X-ray Free-Electron Laser facility. The simulations identify an optimal thickness of the water layer at which the effective resolution for imaging the hydrated sample becomes significantly higher than for the non-hydrated sample. This effect is lost when the water layer becomes too thick. Even though the detailed results presented pertain to the specific sample studied, the trends which we identify should also hold in a general case. We expect these findings will guide future single-particle imaging experiments using hydrated proteins. [ABSTRACT FROM AUTHOR]

Terrestrial volcanism has been one of the dominant geological forces shaping our planet since its earliest existence. Its associated phenomena, like atmospheric lightning and hydrothermal activity, provide a rich energy reservoir for chemical syntheses. Based on our laboratory simulations, we propose that on the early Earth volcanic activity inevitably led to a remarkable production of formic acid through various independent reaction channels. Large‐scale availability of atmospheric formic acid supports the idea of the high‐temperature accumulation of formamide in this primordial environment. [ABSTRACT FROM AUTHOR]

Laser-assisted microanalysis offers the advantage of determining the spatially resolved compositions in 3D. Scanning a material with a sequence of sampling laser pulses and acquiring online the related spectra allow one to map the lateral and depth distribution of elements and molecules. However, the requirement to analyse smaller and smaller length-scales is challenged by focal diffraction as well as reduction of sensitivity at the nano-scale. Electron-based microprobes still offer unmatched spatial resolution. Disruptive improvements in laser technology are however demonstrated utilizing recently self-developed extreme ultraviolet or soft X-ray lasers. Firstly, a significant enhancement of the resolution is accomplished thanks to a much shorter wavelength, with respect to state-of-the-art commercial lasers. Furthermore, as the most innovative aspect, the sampling efficiency is enhanced using "ionizing radiation", i.e. directly activating the target material. The high photon-energy (20–100 eV) makes the sampling process essentially single-photon, whatever bond or ionization energy. Furthermore, the analytical setup is simplified to a sampling source and detector, i.e. without the need for a secondary ionization or excitation source as in some state-of-the-art analytical systems. In this review, fundamental aspects of X-ray laser desorption and ablation are discussed, and a survey of the available literature is presented. The main objective is to convince the reader that desorption or ablation in this spectral domain is a significantly cleaner sampling process, with large potential, still requiring investigation for a complete fundamental understanding. Applications of laser microanalysis are thus entering the nano-scale era, which shrinks the gap with electron-based microprobes. [ABSTRACT FROM AUTHOR]

A standard Fricke dosimeter was used to measure the absorbed dose via the oxidation yields of Fe3+ ions in an aqueous environment induced by soft X rays within the "water window" spectral range. We also exploited the property of a neutral solution containing terephthalic acid as a tool for selective detection of OH radicals. Both dosimetric systems were irradiated using the experimental pulsed laser-plasma soft X-ray source as well as conventional 1.25-MeV gamma rays. Radiation chemical yields of Fe3+ ions and OH radicals were determined to be (5.13 ± 0.94) × 10–1 µmol·J–1 (4.95 ± 0.91 100eV–1) and (2.33 ± 0.35) × 10–2 µmol·J–1 (0.23 ± 0.03 100eV–1), respectively. Measurements were supported by Monte Carlo simulations to estimate the linear energy transfer of the water window radiation. The simulation results are in good agreement with expected linear energy transfer of ions inducing the same Fe3+ ion and OH radical radiation chemical yield. [ABSTRACT FROM AUTHOR]

The optical emission spectroscopy technique with temporal resolution is employed to explain the mechanisms involved in the creation of large-scale plasma in gas mixtures containing carbon dioxide by the high-power laser-induced dielectric breakdown strategy. The production of the carbon monoxide cations is shown to be enhanced by the Penning ionization mechanism.

An overall optical emission of high-powered laser-induced dielectric breakdown (LIDB) in various molecular gases and their mixtures were measured and analyzed. It is concluded that the presence of the cold molecular gas surrounding the hot core of the LIDB plasma is a necessary condition for formation of complex molecular species.

Unexpected strong ultraviolet emission has been observed from the merger of two low-pressure supersonic gas-flows previously leaving two radiofrequency (RF) discharges, one containing Ar, He, O2 and traces of NO, the other He and plasma-chemically produced C2F4. Analysis of the spectral emission data over a range of 190 to 710 nm shows that the main energy carriers in this radiofrequency powered flowing discharge afterglow are He, C2F4 (or CF2) and NO. Plasma-chemical excitation and energy transfer amongst the main energy carriers result in a spectrum dominated by a vibronic structure, covering the spectral range from 190 to 300 nm, which is assigned to the spontaneous emission from excited nitric oxide. The strongest line located at 236.2 nm is due to the NO(A2Σ+, 0–1) transition. The distance between the point of observation and the nearest RF discharge together with the residence time of gases in this region excludes any direct excitation of NO by the RF discharge itself. The observed phenomenon has potential as a plasma-chemical gas-flow laser emitting at a fundamental frequency in the mid-ultraviolet spectral region. [ABSTRACT FROM AUTHOR]

The experimental study of damage to tungsten (W), molybdenum (Mo), and silicon carbide (SiC) surfaces induced by focused extreme ultraviolet laser radiation (λ ~ 47 nm/~1.5 ns/21–40 µJ) is presented. It was found that W and Mo behaved similarly: during the first shot, the damaged area is covered by melted and re-solidified material, in which circular holes appear – residua of just opened pores/bubbles, from which pressurized gas/vapors escaped. Next cracks and ruptures appear and the W has a tendency to delaminate its surface layer. Contrary, single-crystalline SiC has negligible porosity and sublimates; therefore, no escape of "pressurized" gas and no accompanying effects take place. Moreover, SiC at sublimating temperature decomposes to elements; therefore, the smooth crater morphology can be related to local laser energy density above ablation threshold. When more shots are accumulated, in all three investigated materials, the crater depth increases non-linearly with number of these shots. The surface morphology was investigated by an atomic force microscope, the surface structure was imaged by a scanning electron microscope (SEM), and the structure below the surface was visualized by SEM directed into a trench that is milled by focused ion beam. Additionally, structural changes in SiC were revealed by Raman spectroscopy. [ABSTRACT FROM AUTHOR]

The durability of grazing- and normal-incidence optical coatings has been experimentally assessed under free-electron laser irradiation at various numbers of pulses up to 16 million shots and various fluence levels below 10% of the single-shot damage threshold. The experiment was performed at FLASH, the Free-electron LASer in Hamburg, using 13.5 nm extreme UV (EUV) radiation with 100 fs pulse duration. Polycrystalline ruthenium and amorphous carbon 50 nm thin films on silicon substrates were tested at total external reflection angles of 20° and 10° grazing incidence, respectively. Mo/Si periodical multilayer structures were tested in the Bragg reflection condition at 16° off-normal angle of incidence. The exposed areas were analysed post-mortem using differential contrast visible light microscopy, EUV reflectivity mapping and scanning X-ray photoelectron spectroscopy. The analysis revealed that Ru and Mo/Si coatings exposed to the highest dose and fluence level show a few per cent drop in their EUV reflectivity, which is explained by EUV-induced oxidation of the surface. [ABSTRACT FROM AUTHOR]

Formation yields of ṖOH radicals were precisely determined in aqueous solutions of coumarin-3-carboxylic acid and ferrous sulfate (i.e., Fricke dosimeter) exposed to 253.7 nm radiation delivered from a continuous source. Quantum yield of ṖOH radicals was determined as ∼0.08, i.e., roughly one out of twelve photons, efficiently absorbed in UV-illuminated solutions, produced one ṖOH radical. Energetically, a water molecule should undergo a correlated action of at least two 4.9 eV photons delivering enough energy for direct H–OH dissociation (5.0–5.4 eV). We suggest a mechanism based on an interaction of two water molecules, both in long-living triplet states. An intermolecular transfer of excitation energy provided a sufficient amount of energy for the dissociation of one water molecule into ṖOH and HṖ radicals. In an aqueous solution of phospholipids, quantum yields of hydroperoxides formed under these irradiation conditions decreased with total effectively absorbed energy (i.e. a dose), similar to the radiation chemical yields obtained during an exposure to ionizing radiation, such as gamma rays from radionuclide sources. Under 253.7 nm irradiation, one ṖOH radical causes a peroxidation of 34 phospholipid molecules. This implicates chain mechanism of the reaction. [ABSTRACT FROM AUTHOR]

The problem of spontaneous magnetic field generation with nanosecond laser pulses raises a series of fundamental questions, including the intrinsic magnetization mechanisms in laser-driven plasmas and the understanding of charge-discharge processes in the irradiated target. These two issues are tightly bound as the charge-discharge processes are defined by the currents, which have in turn a feedback by magnetic fields in the plasma. Using direct polaro-interferometric measurements and theoretical analysis, we show that at parameters related to the PALS laser system (1.315 µm, 350 ps, and 1016 W/cm²), fast electrons play a decisive role in the generation of magnetic fields in the laser-driven plasma. Spatial distributions of electric currents were calculated from the measured magnetic field and plasma density distributions. The obtained results revealed the characteristics of strong currents observed in capacitor-coil magnetic generation schemes and open a new approach to fundamental studies related to magnetized plasmas. [ABSTRACT FROM AUTHOR]

Large-scale plasma was created in gas mixtures containing methane using high-power laser-induced dielectric breakdown (LIDB). The composition of the mixtures corresponded to a cometary and/or meteoritic impact into the early atmosphere of either Titan or Earth. A multiple-centimeter-sized fireball was created by focusing a single 100 J, 450 ps near-infrared laser pulse into the center of a 15 L gas cell. The excited reaction intermediates formed during the various stages of the LIDB plasma chemical evolution were investigated using optical emission spectroscopy (OES) with temporal resolution. The chemical consequences of laser-produced plasma generation in a CH4–N2–H2O mixture were investigated using high resolution Fourier-transform infrared absorption spectroscopy (FTIR) and gas selected ion flow tube spectrometry (SIFT). Several simple inorganic and organic compounds were identified in the reaction mixture exposed to ten laser sparks. Deuterated water (D2O) in a gas mixture was used to separate several of the produced isotopomers of acetylene, which were then quantified using the FTIR technique. [ABSTRACT FROM AUTHOR]

We present the x-ray optical design of the soft x-ray materials science instrument at the Linac Coherent Light Source, consisting of a varied line-spaced grating monochromator and Kirkpatrick-Baez refocusing optics. Results from the commissioning of the monochromator are shown. A resolving power of 3000 was achieved, which is within a factor of two of the design goal. [ABSTRACT FROM AUTHOR]

Conditions for ultrasound toluene extraction of synthetic C60 added to powdered bituminous coal were tested. High-performance liquid chromatography (HPLC) was used to determine the fullerene content in the obtained extracts. The results indicated a possible negative effect of sample demineralization (HCl/HF) and N2 purging on the extraction yield of C60. On the contrary, a 30% yield increase was registered when the coal was pre-extracted with pentane or pentane/toluene. The best conditions for C60 recovery in the investigated mixtures are 30 min of sonication at 280-285 K. The effects of sample filtration, sequential extraction, ultrasound bath power and treatments of C60 solution alone are also discussed. [ABSTRACT FROM AUTHOR]

We study the behavior of poly(methyl methacrylate) (PMMA) exposed to femtosecond pulses of extreme ultraviolet and X-ray laser radiation in the single-shot damage regime. The employed microscopic simulation traces induced electron cascades, the thermal energy exchange of electrons with atoms, nonthermal modification of the interatomic potential, and a triggered atomic response. We identify that the nonthermal hydrogen decoupling triggers ultrafast fragmentation of PMMA strains at the absorbed threshold dose of ~0.07 eV/atom. At higher doses, more hydrogen atoms detach from their parental molecules, which, at the dose of ~0.5 eV/atom, leads to a complete separation of hydrogens from carbon and oxygen atoms and fragmentation of MMA molecules. At the dose of ~0.7 eV/atom, the band gap completely collapses indicating that a metallic liquid is formed with complete atomic disorder. An estimated single-shot ablation threshold and a crater depth as functions of fluence agree well with the experimental data collected. [ABSTRACT FROM AUTHOR]

In a mixture of molecular gases with compositions (CO2–N2–H2O and CO–N2–H2O) and total pressure close to that of the Earth’s early atmospheres, a centimeter-sized plasma was created by focusing a single 85-J, 450-ps near-infrared laser pulse in a center of 15-L gas cell. Chemical consequences of the laser-produced plasma generation in such a mixture were investigated using high-performance liquid chromatography with mass-spectrometric detection (HPLC/MS). Amino acids were identified in the reaction mixture containing CO2 as well as in that one based on CO, both exposed to 10 laser shots. [Copyright &y& Elsevier]

Large laser sparks created by a single shot of a high-power laser system were used for the laboratory simulation of the chemical consequences of high-energy-density events (lightning, high-velocity impact) in planetary atmospheres, e.g., the early Earth's atmosphere. [ABSTRACT FROM PUBLISHER]

Abstract: A large-scale plasma was created in CO–N2–H2O gas mixtures by high-power laser-induced dielectric breakdown. The composition of the mixtures used corresponded to a cometary and/or meteoritic impact into the Earth’s early atmosphere. A multiple-centimeter-sized fireball was created by focusing near-infrared laser pulse into the centre of cell. The laser–plasma formation in the mixtures mainly leads to a production of CO2. The competition of the CO+CO→CO2 +C and CO+OH→CO2 +H reactions in the CO2 production was investigated using 18O labeled water. An analysis of the isotopomers was carried out by means of high-resolution FTIR spectroscopy. [Copyright &y& Elsevier]

Abstract: This article gives an account of chemical reactions initiated by laser-induced dielectric breakdown (LIDB) in homogeneous molecular gases. The systematic part of the article describes the laser-plasma-chemical behavior of simple inorganic gases and their mixtures, metal carbonyls and organometallics, and organic molecular gases. Research on LIDB-initiated chemical reactions producing well-defined fine solid particles has been triggered again recently by the advent of nanotechnologies. Laser ignition of fuel mixtures is also a well researched branch of laser-plasma chemistry because of strong commercial and military interests. However, the strongest current impulses for studying laser-spark chemistry come from planetary sciences, where laser sparks have been used as a laboratory model of high-energy-density phenomena (e.g., impact of extraterrestrial bodies, lightning) in planetary atmospheres. A single pulse from a high-power laser system was used to develop an improved method for investigating this phenomenon. The particular processes responsible for the chemical action of a laser spark are identified and described in detail by the end of the article. [Copyright &y& Elsevier]

Fullerene oxides were the first observed fullerene derivatives and they have naturally attracted attention of both experiment and theory. C60O has represented a long standing case of experiment–theory disagreement, and there has been a similar problem with C60O2—both cases were explained by kinetic rather than thermodynamic control. In this contribution, we report the first computations of C84O. The computations are carried out with the PM3 quantum-chemical semiempirical method. Thermodynamic stabilities are evaluated for the electronic singlet and triplet states. The triplet states are computed at both restricted open-shell Hartree–Fock (ROHF) and unrestricted open-shell Hartree–Fock levels. The computations focus on the two most abundant C84 isomers—D2 and D2d, and especially deal with additions to their shortest and longest bonds. The D2/long structure is the lowest-energy species. The PM3/ROHF energy ordering of the C84O isomers in the first triplet electronic state is exactly the same as in the singlet electronic state and the relative energies are also quite similar. On the other hand, the kinetic stability order is just reversed compared to the thermodynamic order. Hence, for relatively short reaction times the C84O D2/short isomer should primarily be formed (in spite of the fact that it should be, thermodynamically, the least stable in the studied set). The computations point out various stability selection rules controlling production of fullerene-based materials. [Copyright &y& Elsevier]