Observational tests of interstellar methanol formation

Context. It has been established that the classical gas-phase production of interstellar methanol (CH3OH) cannot explain observed abundances. Instead it is now generally thought that the main formation path has to be by successive hydrogenation of solid CO on interstellar grain surfaces. Aims. While theoretical models and laboratory experiments show that methanol is efficiently formed from CO on cold grains, our aim is to test this scenario by astronomical observations of gas associated with young stellar objects (YSOs). Methods. We have observed the rotational transition quartets J = 2K – 1K of 12CH3OH and 13CH3OH at 96.7 and 94.4 GHz, respectively, towards a sample of massive YSOs in different stages of evolution. In addition, the J = 1-0 transitions of 12C18O and 13C18O were observed towards some of these sources. We use the 12C/13C ratio to discriminate between gas-phase and grain surface origin: If methanol is formed from CO on grains, the ratios should be similar in CH3OH and CO. If not, the ratio should be higher in CH3OH due to 13C fractionation in cold CO gas. We also estimate the abundance ratios between the nuclear spin types of methanol (E and A). If methanol is formed on grains, this ratio is likely to have been thermalized at the low physical temperature of the grain, and therefore show a relative over-abundance of A-methanol. Results. We show that the 12C/13C isotopic ratio is very similar in gas-phase CH3OH and C18O, on the spatial scale of about 40 arcsec, towards four YSOs. For two of our sources we find an overabundance of A-methanol as compared to E-methanol, corresponding to nuclear spin temperatures of 10 and 16 K. For the remaining five sources, the methanol E/A ratio is less than unity. Conclusions. While the 12C/13C ratio test is consistent with methanol formation from hydrogenation of CO on grain surfaces, the result of the E/A ratio test is inconclusive.

Ultrahigh-intensity laser-produced plasmas as a compact heavy ion injection source

The possibility of using high-intensity laser-produced plasmas as a source of energetic ions for heavy ion accelerators is addressed. Experiments have shown that neon ions greater than 6 MeV can be produced from gas jet plasmas, and well-collimated proton beams greater than 20 MeV have been produced from high-intensity Laser solid interactions. The proton beams from the back of thin targets appear to be more collimated and reproducible than are high-energy ions generated in the ablated plasma at the front of the target and may be more suitable for ion injection applications. Lead ions have been produced at energies up to 430 MeV.

Generation of bright, extreme-ultraviolet harmonic radiation from a krypton fluoride laser

We present results of experiments studying the efficiency of high harmonic generation from a gas target using the TITANIA krypton fluoride laser at the Rutherford Appleton Laboratory. The variation of harmonic yield for the 7th to 13th harmonics (355-191 Angstrom) is studied as a function of the backing pressure of a solenoid valve gas jet and of the axial position of the laser focus relative to the centre of the gas jet nozzle. Harmonic energies up to 1 mu J were produced in helium and neon targets from laser energies of approximately 200 mJ. This corresponds to absolute conversion efficiencies of up to 5 x 10(-6).

High-order harmonics of 248.6-nm KrF laser from helium and neon ions

We report high harmonic generation from a 248.6-nm KrF laser giving harmonic orders up to the 37th (67 Angstrom) in a helium gas jet and the 35th (71 Angstrom) in neon, for laser intensities up to 4 x 10(17) W/cm(2) in 380-fs pulses. These observations are interpreted using theoretical modeling that identifies the ion species He+, Ne+, and Ne2+ as the sources of the highest harmonics.

Interaction of intense laser pulses with preformed density channels

The interaction of a high-intensity laser pulse with a plasma density channel preformed in a gas jet target has been studied. At neutral densities below 3.0 X 10(19) cm(-3) a strong interaction between the pulse and the channel walls was observed, there was clear evidence of pulse confinement, and the laser irradiance was significantly increased compared to an interaction with neutral gas. At higher gas densities, however, the radial uniformity and length of the channel were both found to be adversely affected by refractive defocusing of the prepulse used to generate the channel.

High order harmonics from relativistic electron spikes

A new regime of relativistic high-order harmonic generation has been discovered (Pirozhkov 2012 Phys. Rev. Lett. 108 135004). Multi-terawatt relativistic-irradiance (>1018 W cm−2) femtosecond (~30–50 fs) lasers focused to underdense (few × 1019 cm−3) plasma formed in gas jet targets produce comb-like spectra with hundreds of even and odd harmonic orders reaching the photon energy of 360 eV, including the 'water window' spectral range. Harmonics are generated either by linearly or circularly polarized pulses from the J-KAREN (KPSI, JAEA) and Astra Gemini (CLF, RAL, UK) lasers. The photon number scalability has been demonstrated with a 120 TW laser, producing 40 μJ sr−1 per harmonic at 120 eV. The experimental results are explained using particle-in-cell simulations and catastrophe theory. A new mechanism of harmonic generation by sharp, structurally stable, oscillating electron spikes at the joint of the boundaries of the wake and bow waves excited by a laser pulse is introduced. In this paper, detailed descriptions of the experiments, simulations and model are provided and new features are shown, including data obtained with a two-channel spectrograph, harmonic generation by circularly polarized laser pulses and angular distribution.

Astrochemistry

In the last 40 years a wide range of molecules, including neutrals, cations and anions, containing up to 13 atoms—in addition to detections of C₆₀ and C₇₀ — have been found in the harsh environment of the interstellar medium. The exquisite sensitivity and very high spectral and, more recently, spatial resolution, of modern telescopes has enabled the physics of star formation to be probed through rotational line emission. In this article, I review the basic properties of interstellar clouds and the processes that initiate the chemistry and generate chemical complexity, particularly in regions of star and planet formation. Our understanding of astrochemistry has evolved over the years. Before 1990, the general consensus was that molecules were formed in binary, gas-phase, or volume, reactions, most importantly ion-neutral reactions despite the very low ionization in clouds. Since then, observations have indicated unambiguously that there is also a contribution from surface processes, particularly on the icy mantles that form around refractory grain cores in cold, dense gas. The balance between these two processes depends on particular physical conditions and can vary during the life cycle of a particular volume of interstellar cloud.The complex chemistry that occurs in space is driven mostly through interaction of thegas with cosmic ray protons, a source of ionization that enables a rich ion-neutral chemistry. In addition, I show that the interaction between the gas and the dust in cold, dense regionsalso leads to additional chemical complexity through reactions that take place in ices at onlya few tens of degrees above absolute zero. Although densities are low compared to those in terrestrial environments, the extremely long life times of interstellar clouds and their enormous sizes, enable complex molecules to be synthesised and detected. I show that in some instances, particularly in reactions involving deuterium, the rotational populations of reactants, together with spin-selection rules, can determine the detailed abundances. Although the review is mainly focused on regions associated with star formation, I also consider chemistry in other interesting astronomical regions — in the early Universe and in the envelopes formed by mass loss during the final stages of stellar evolution.

Characterization and spectroscopic analysis of phenol-ethanol hydrogen bonded clusters

Different hydrogen bonded clusters involving phenol and ethanol are studied theoretically using MP2/aug-cc-pVDZ. Nine different 1: 1 clusters are obtained and analyzed according to their stability and spectroscopic properties. Different isomeric forms of ethanol are considered. Attention is also devoted to the spectral shift of the characteristic pi -> pi* transition of phenol. Using TDHF, CIS, CIS(D) and TDB3LYP in aug-cc-pVDZ basis set, all results agree that a red shift is obtained when phenol is the hydrogen donor and a blue shift is obtained in the opposite case. These results are used to rationalize the red shift observed for phenol in liquid ethanol. (C) 2010 Elsevier B.V. All rights reserved.

Der Einsatz elektrochemischer Methoden für die Untersuchung superschwerer Elemente

Das Hauptziel der vorliegenden Arbeit war die Entwicklung eines Experimentaufbaus für die elektrochemische Abscheidung von Transactiniden mit anschließender Detektion. Zu diesem Zweck wurden Experimente mit den Homologen dieser Elemente durchgeführt. Die Elektrodeposition von Tracermengen an Fremdelektroden führt zu einer Elektrodenbedeckung von weniger als einer Monolage. Die erforderlichen Abscheidepotentiale sind häufig positiver, als nach der Nernst’schen Gleichung zu erwarten ist. Dieses Phänomen nennt man Unterpotentialabscheidung. In zahlreichen Versuchen mit Radiotracern wurde die Abscheideausbeute als Funktion des Elektrodenpotentials bestimmt, wobei abzuscheidendes Ion, Elektrodenmaterial und Elektrolyt variiert wurden. Es wurden kritische Potentiale, bei denen eine nennenswerte Abscheidung gerade begann, ermittelt sowie Potentiale für die Abscheidung von 50 % der in der Lösung befindlichen Atome. Diese Werte wurden mit theoretisch vorhergesagten Potentialen und Werten aus der Literatur verglichen. Die Abscheidung von Pb als Homologem von Element 114 funktionierte sehr gut an Elektroden aus Palladium oder palladinierten Nickelelektroden unter Verwendung von 0,1 M HCl als Elektrolyt. Zur Charakterisierung der Unterpotentialabscheidung wurde neben der Radiotracer-Methode auch die Cyclovoltammetrie eingesetzt. Hier findet die Abscheidung der ersten Monolage auf der Elektrode ebenfalls häufig bei positiveren Potentialen statt, als die der Hauptmenge. Die mit beiden Methoden ermittelten Werte wurden einander gegenübergestellt. Die Elektrodeposition von kurzlebigen Isotopen muss sehr schnell erfolgen. Es konnte gezeigt werden, dass eine hohe Temperatur und damit verbunden eine niedrige Viskosität des Elektrolyten die Abscheidung beschleunigt. Ebenfalls wichtig ist ein gutes Rühren der Lösung, um eine kleine Nernst’sche Diffusionsschichtdicke zu erzielen. Das Verhältnis von Elektrodenfläche zu Elektrolytvolumen muss möglichst groß sein. Auf der Grundlage dieser Ergebnisse wurde eine für schnelle Elektrolysen optimierte Elektrolysezelle entwickelt. Unter Einsatz dieser Zelle wurden die Abscheidegeschwindigkeiten für verschiedene Ionen- und Elektrodenkombinationen gemessen. Es wurden Experimente zur Kopplung von Gasjet und Elektrolysezelle durchgeführt, dabei wurde sowohl mit am Reaktor erzeugten Spaltprodukten, mit Pb-Isotopen aus einer emanierenden Quelle und mit am Beschleuniger erzeugten Isotopen gearbeitet. Mit den dort gewonnenen Erkenntnissen wurde ein Experimentaufbau für die kontinuierliche Abscheidung und Detektion von kurzlebigen Isotopen realisiert. Am Beschleuniger wurden u. a. kurzlebige Hg- und Pb-Isotope erzeugt und mit einem Gasjet aus der Targetkammer zum ALOHA-System transportiert. Dort wurden sie in einem quasi-kontinuierlichen Prozess in die wässrige Phase überführt und zu einer Elektrolyszelle transportiert. In dieser erfolgte die Elektrodeposition auf eine bandförmige Elektrode aus Nickel oder palladiniertem Nickel. Nach der Abscheidung wurde das Band zu einer Detektorphalanx gezogen, wo der -Zerfall der neutronenarmen Isotope registriert wurde. Es wurden charakteristische Größen wie die Abscheidegeschwindigkeit und die Gesamtausbeute der Elektrolyse ermittelt. Das System wurde im Dauerbetrieb getestet. Es konnte gezeigt werden, dass der gewählte Aufbau prinzipiell für die Abscheidung von kurzlebigen, am Beschleuniger erzeugten Isotopen geeignet ist. Damit ist eine wichtige Voraussetzung für den zukünftigen Einsatz der Methode zum Studium der chemischen Eigenschaften der superschweren Elemente geschaffen.

Construction and commissioning of a collinear laser spectroscopy setup at TRIGA Mainz and laser spectroscopy of magnesium isotopes at ISOLDE (CERN)

Collinear laser spectroscopy has been used as a tool for nuclear physics for more than 30 years. The unique possibility to extract nuclear properties like spins, radii and nuclear moments in a model-independent manner leads to important physics results to test the predictive power of existing nuclear models. rnThis work presents the construction and the commissioning of a new collinear laser spectroscopy experiment TRIGA-LASER as a part of the TRIGA-SPEC facility at the TRIGA research reactor at the University of Mainz. The goal of the experiment is to study the nuclear structure of radioactive isotopes which will be produced by neutron-induced fission near the reactor core and transported to an ion source by a gas jet system. rnThe versatility of the collinear laser spectroscopy technique will be exploited in the second part of this thesis. The nuclear spin and the magnetic moment of the neutron-deficient isotope Mg-21 will be presented, which were measured by the detection of the beta-decay asymmetry induced by nuclear polarization after optical pumping. A combination of this detection method with the classical fluorescence detection is then used to determine the isotope shifts of the neutron-rich magnesium isotopes from Mg-24 through Mg-32 to study the transition to the ''island of inversion''.

Ion acceleration in underdense plasmas by ultra-short laser pulses

We report on the ion acceleration mechanisms that occur during the interaction of an intense and ultrashort laser pulse ( λ > μ I 2 1018 W cm−2 m2) with an underdense helium plasma produced from an ionized gas jet target. In this unexplored regime, where the laser pulse duration is comparable to the inverse of the electron plasma frequency ωpe, reproducible non-thermal ion bunches have been measured in the radial direction. The two He ion charge states present energy distributions with cutoff energies between 150 and 200 keV, and a striking energy gap around 50 keV appearing consistently for all the shots in a given density range. Fully electromagnetic particle-in-cell simulations explain the experimental behaviors. The acceleration results from a combination of target normal sheath acceleration and Coulomb explosion of a filament formed around the laser pulse propagation axis

Gasification of rubberwood in a downdraft gasifier

The objectives of this research were to investigate the perforamnce of a rubberwood gasifier and engine with electricity generation and to identify opportunities for the implementation of such a system in Malaysia. The experimental work included the design, fabrication and commissioning of a throated downdraft gasifier in Malaysia. The gasifier was subsequently used to investigate the effect of moisture content, dry wood capacity and particle size of rubberwood on gasifier performance. Additional experiments were also conducted to investigate the influence of two different nozzle numbers and two different throat diameters on tar cracking. A total of 101 runs were completed during the duration of the research. From the experimental data, the average mass balance was found to be 92.65%. The average energy balance over the gasifier to hot raw gas was 98.7%, to cold clean gas was 102.4% and over the complete system was 101.9%. The heat loss from the gasifier was estimated to range from 10-26% of the chemical energy of the feedstock. From the downstream operation, the heat loss was estimated to range from 17-37% of the chemical energy of rubberwood feedstock. The maximum throughput for stable operation was found to be 60-70% of the maximum dry wood capacity. The gasifier was found to have a maximum turndown ratio of 5:1. It is also postulated that the phenomenon of turndown of the gasifier is due to a `bubble theory' occurring at the gasification zone, and this hypothesis is explained. For stable power output, the working range of the engine was found to be 5-33.5 kWe. The thermal efficiency and diesel displacement of the engine was found to be 17-18% and 65-70% respectively. The research also showed that rubberwood gasification in Malaysia is feasible if the price of diesel is above MR35/l and the price of wood is below MR120/tonne.

Experimental measurements of the collisional absorption of XUV radiation in warm dense aluminium

The collisional (or free-free) absorption of soft x rays in warm dense aluminium remains an unsolved problem. Competing descriptions of the process exist, two of which we compare to our experimental data here. One of these is based on a weak scattering model, another uses a corrected classical approach. These two models show distinctly different behaviors with temperature. Here we describe experimental evidence for the absorption of 26-eV photons in solid density warm aluminium (Te≈1 eV). Radiative x-ray heating from palladium-coated CH foils was used to create the warm dense aluminium samples and a laser-driven high-harmonic beam from an argon gas jet provided the probe. The results indicate little or no change in absorption upon heating. This behavior is in agreement with the prediction of the corrected classical approach, although there is not agreement in absolute absorption value. Verifying the correct absorption mechanism is decisive in providing a better understanding of the complex behavior of the warm dense state.

COOL CORE CYCLES: COLD GAS AND AGN JET FEEDBACK IN CLUSTER CORES

Using high-resolution 3D and 2D (axisymmetric) hydrodynamic simulations in spherical geometry, we study the evolution of cool cluster cores heated by feedback-driven bipolar active galactic nuclei (AGNs) jets. Condensation of cold gas, and the consequent enhanced accretion, is required for AGN feedback to balance radiative cooling with reasonable efficiencies, and to match the observed cool core properties. A feedback efficiency (mechanical luminosity approximate to epsilon(M) over dot(acc)c(2); where (M) over dot(acc). is the mass accretion rate at 1 kpc) as small as 6 x 10(-5) is sufficient to reduce the cooling/accretion rate by similar to 10 compared to a pure cooling flow in clusters (with M-200 less than or similar to 7 x 10(14) M-circle dot). This value is much smaller compared to the ones considered earlier, and is consistent with the jet efficiency and the fact that only a small fraction of gas at 1 kpc is accreted onto the supermassive black hole (SMBH). The feedback efficiency in earlier works was so high that the cluster core reached equilibrium in a hot state without much precipitation, unlike what is observed in cool-core clusters. We find hysteresis cycles in all our simulations with cold mode feedback: condensation of cold gas when the ratio of the cooling-time to the free-fall time (t(cool)/t(ff)) is less than or similar to 10 leads to a sudden enhancement in the accretion rate; a large accretion rate causes strong jets and overheating of the hot intracluster medium such that t(cool)/t(ff) > 10; further condensation of cold gas is suppressed and the accretion rate falls, leading to slow cooling of the core and condensation of cold gas, restarting the cycle. Therefore, there is a spread in core properties, such as the jet power, accretion rate, for the same value of core entropy t(cool)/t(ff). A smaller number of cycles is observed for higher efficiencies and for lower mass halos because the core is overheated to a longer cooling time. The 3D simulations show the formation of a few-kpc scale, rotationally supported, massive (similar to 10(11) M-circle dot) cold gas torus. Since the torus gas is not accreted onto the SMBH, it is largely decoupled from the feedback cycle. The radially dominant cold gas (T < 5 x 10(4) K; vertical bar v(r)vertical bar >vertical bar v(phi vertical bar)) consists of fast cold gas uplifted by AGN jets and freely infalling cold gas condensing out of the core. The radially dominant cold gas extends out to 25 kpc for the fiducial run (halo mass 7 x 10(14) M-circle dot and feedback efficiency 6 x 10(-5)), with the average mass inflow rate dominating the outflow rate by a factor of approximate to 2. We compare our simulation results with recent observations.

Femtosecond Rotational Raman Coherence Spectroscopy of Cyclohexane in a Pulsed Supersonic Jet

We combine the technique of femtosecond degenerate four-wave mixing (fs-DFWM) with a high repetition-rate pulsed supersonic jet source to obtain the rotational coherence spectrum (RCS) of cold cyclohexane (C(6)H(12)) with high signal/noise ratio. In the jet expansion, the near-parallel flow pattern combined with rapid translational cooling effectively eliminate dephasing collisions, giving near-constant RCS signal intensities over time delays up to 5 ns. The vibrational cooling in the jet eliminates the thermally populated vibrations that complicate the RCS coherences of cyclohexane at room temperature [Bragger, G.; et al. J. Phys. Chem. A 2011, 115, 9567]. The rotational cooling reduces the high-J rotational-state population, yielding the most accurate ground-state rotational constant to date, B(0) = 4305.859(9) MHz. Based on this B(0), a reanalysis of previous room-temperature gas-cell RCS measurements of cydohexane gives improved vibration rotation interaction constants for the v(32), v(6), v(16), and v(24) vibrational states. Combining the experimental B(0)(C(6)H(12)) with CCSD(T) calculations yields a very accurate semiexperimental equilibrium structure of the chair isomer of cyclohexane