Theoretical research program to study transition metal trimers and embedded clusters

Small transition metal clusters were studied at a high level of approximation, including all the valence electrons in the calculation and extensive electron correlation, in order to understand the electronic structure of these small metal clusters. By comparison of dimers, trimers, and possibly higher clusters, the information obtained was used to provide insights into the electronic structure of bulk transition metals. Small metal clusters are currently of considerable experimental interest and some information is becomming available both from matrix electron spin resonance studies and from gas phase spectroscopy. Collaboration between theorists and experimentalists is thus expected to be especially profitable at this time since there is some experimental information which can serve to guide the theoretical work

Crystalline silicates as a probe of disk formation history

We present a new perspective on the crystallinity of dust in protoplanetary disks. The dominant crystallization by thermal annealing happens in the very early phases of disk formation and evolution. Both the disk properties and the level of crystallinity are thereby directly linked to the properties of the molecular cloud core from which the star+disk system was formed. We show that, under the assumption of single star formation, rapidly rotating clouds produce disks which, after the main infall phase (i.e. in the optically revealed class II phase), are rather massive and have a high accretion rate but low crystallinity. Slowly rotating clouds, on the other hand, produce less massive disks with lower accretion rate, but high levels of crystallinity. Cloud fragmentation and the formation of multiple stars complicates the problem and necessitates further study. The underlying physics of the model is insufficiently understood to provide the precise relationship between crystallinity, disk mass and accretion rate. But the fact that with `standard' input physics the model produces disks which, in comparison to observations, appear to have either too high levels of crystallinity or too high disk masses, demonstrates that the comparison of these models to observations can place strong contraints on the disk physics. The question to ask is not why some sources are so crystalline, but why some other sources have such a low level of crystallinity.Comment: Accepted for publication in ApJ

The SILCC (SImulating the LifeCycle of molecular Clouds) project: I. Chemical evolution of the supernova-driven ISM

The SILCC project (SImulating the Life-Cycle of molecular Clouds) aims at a more self-consistent understanding of the interstellar medium (ISM) on small scales and its link to galaxy evolution. We simulate the evolution of the multi-phase ISM in a 500 pc x 500 pc x 10 kpc region of a galactic disc, with a gas surface density of $\Sigma_{_{\rm GAS}} = 10 \;{\rm M}_\odot/{\rm pc}^2$. The Flash 4.1 simulations include an external potential, self-gravity, magnetic fields, heating and radiative cooling, time-dependent chemistry of H$_2$ and CO considering (self-) shielding, and supernova (SN) feedback. We explore SN explosions at different (fixed) rates in high-density regions (peak), in random locations (random), in a combination of both (mixed), or clustered in space and time (clustered). Only random or clustered models with self-gravity (which evolve similarly) are in agreement with observations. Molecular hydrogen forms in dense filaments and clumps and contributes 20% - 40% to the total mass, whereas most of the mass (55% - 75%) is in atomic hydrogen. The ionised gas contributes <10%. For high SN rates (0.5 dex above Kennicutt-Schmidt) as well as for peak and mixed driving the formation of H$_2$ is strongly suppressed. Also without self-gravity the H$_2$ fraction is significantly lower ($\sim$ 5%). Most of the volume is filled with hot gas ($\sim$90% within $\pm$2 kpc). Only for random or clustered driving, a vertically expanding warm component of atomic hydrogen indicates a fountain flow. Magnetic fields have little impact on the final disc structure. However, they affect dense gas ($n\gtrsim 10\;{\rm cm}^{-3}$) and delay H$_2$ formation. We highlight that individual chemical species, in particular atomic hydrogen, populate different ISM phases and cannot be accurately accounted for by simple temperature-/density-based phase cut-offs.Comment: 30 pages, 23 figures, submitted to MNRAS. Comments welcome! For movies of the simulations and download of selected Flash data see the SILCC website: http://www.astro.uni-koeln.de/silc

The influence of the turbulent perturbation scale on prestellar core fragmentation and disk formation

The collapse of weakly turbulent prestellar cores is a critical stage in the process of star formation. Being highly non-linear and stochastic, the outcome of collapse can only be explored theoretically by performing large ensembles of numerical simulations. Standard practice is to quantify the initial turbulent velocity field in a core in terms of the amount of turbulent energy (or some equivalent) and the exponent in the power spectrum (n \equiv -d log Pk /d log k). In this paper, we present a numerical study of the influence of the details of the turbulent velocity field on the collapse of an isolated, weakly turbulent, low-mass prestellar core. We show that, as long as n > 3 (as is usually assumed), a more critical parameter than n is the maximum wavelength in the turbulent velocity field, {\lambda}_MAX. This is because {\lambda}_MAX carries most of the turbulent energy, and thereby influences both the amount and the spatial coherence of the angular momentum in the core. We show that the formation of dense filaments during collapse depends critically on {\lambda}_MAX, and we explain this finding using a force balance analysis. We also show that the core only has a high probability of fragmenting if {\lambda}_MAX > 0.5 R_CORE (where R_CORE is the core radius); that the dominant mode of fragmentation involves the formation and break-up of filaments; and that, although small protostellar disks (with radius R_DISK <= 20 AU) form routinely, more extended disks are rare. In turbulent, low-mass cores of the type we simulate here, the formation of large, fragmenting protostellar disks is suppressed by early fragmentation in the filaments.Comment: 11 pages, 7 figures; accepted for publication by MNRA

The SILCC project: III. Regulation of star formation and outflows by stellar winds and supernovae

We study the impact of stellar winds and supernovae on the multi-phase interstellar medium using three-dimensional hydrodynamical simulations carried out with FLASH. The selected galactic disc region has a size of (500 pc)$^2$ x $\pm$ 5 kpc and a gas surface density of 10 M$_{\odot}$/pc$^2$. The simulations include an external stellar potential and gas self-gravity, radiative cooling and diffuse heating, sink particles representing star clusters, stellar winds from these clusters which combine the winds from indi- vidual massive stars by following their evolution tracks, and subsequent supernova explosions. Dust and gas (self-)shielding is followed to compute the chemical state of the gas with a chemical network. We find that stellar winds can regulate star (cluster) formation. Since the winds suppress the accretion of fresh gas soon after the cluster has formed, they lead to clusters which have lower average masses (10$^2$ - 10$^{4.3}$ M$_{\odot}$) and form on shorter timescales (10$^{-3}$ - 10 Myr). In particular we find an anti-correlation of cluster mass and accretion time scale. Without winds the star clusters easily grow to larger masses for ~5 Myr until the first supernova explodes. Overall the most massive stars provide the most wind energy input, while objects beginning their evolution as B-type stars contribute most of the supernova energy input. A significant outflow from the disk (mass loading $\gtrsim$ 1 at 1 kpc) can be launched by thermal gas pressure if more than 50% of the volume near the disc mid-plane can be heated to T > 3x10$^5$ K. Stellar winds alone cannot create a hot volume-filling phase. The models which are in best agreement with observed star formation rates drive either no outflows or weak outflows.Comment: 23 pages; submitted to MNRA

Diffusion and desorption of SiH3 on hydrogenated H:Si(100)-(2x1) from first principles

We have studied diffusion pathways of a silyl radical adsorbed on the hydrogenated Si (100)-(2x1) surface by density-functional theory. The process is of interest for the growth of crystalline silicon by plasma-enhanced chemical vapor deposition. Preliminary searches for migration mechanisms have been performed using metadynamics simulations. Local minima and transition states have been further refined by using the nudged-elastic-band method. Barriers for diffusion from plausible adsorption sites as low as 0.2 eV have been found, but trap states have also been spotted, leading to a more stable configuration, with escape barriers of 0.7 eV. Diffusion among weakly bound physisorbed states is also possible with very low activation barriers (<50 meV). However, desorption mechanisms (either as SiH3 or as SiH4) from physisorbed or more strongly bound adsorption configurations turn out to have activation energies similar to diffusion barriers. Kinetic Monte Carlo simulations based on ab initio activation energies show that the silyl radical diffuses at most by a few lattice spacing before desorbing at temperatures in the range 300-1000 K

On the resolution requirements for modelling molecular gas formation in solar neighbourhood conditions

The formation of molecular hydrogen (H$_2$) and carbon monoxide (CO) is sensitive to the volume and column density distribution of the turbulent interstellar medium. In this paper, we study H$_2$ and CO formation in a large set of hydrodynamical simulations of periodic boxes with driven supersonic turbulence, as well as in colliding flows with the \textsc{Flash} code. The simulations include a non-equilibrium chemistry network, gas self-gravity, and diffuse radiative transfer. We investigate the spatial resolution required to obtain a converged H$_2$ and CO mass fraction and formation history. From the numerical tests we find that H$_2$ converges at a spatial resolution of $\lesssim0.2$~pc, while the required resolution for CO convergence is $\lesssim 0.04$~pc in gas with solar metallicity which is subject to a solar neighbourhood interstellar radiation field. We derive two critical conditions from our numerical results: the simulation has to at least resolve the densities at which (1) the molecule formation time in each cell in the computational domain is equal to the dissociation time, and (2) the formation time is equal to the the typical cell crossing time. For both H$_2$ and CO, the second criterion is more restrictive. The formulae we derive can be used to check whether molecule formation is converged in any given simulation.Comment: 22 pages, 21 figures, submitte

From parallel to perpendicular -- On the orientation of magnetic fields in molecular clouds

We present synthetic dust polarization maps of simulated molecular clouds (MCs) with the goal to systematically explore the origin of the relative orientation of the magnetic field ($\bf{B}$) with respect to the MC sub-structures identified in density ($n$; 3D) and column density ($N$; 2D). The polarization maps are generated with the radiative transfer code POLARIS, including self-consistently calculated efficiencies for radiative torque alignment. The MCs are formed in two sets of 3D MHD simulations: in (i) colliding flows (CF), and (ii) the SILCC-Zoom simulations. In 3D, for the CF simulations with an initial field strength below $\sim$5 $\mu$G, $\bf{B}$ is oriented parallel or randomly with respect to the $n$-structures. For CF runs with stronger initial fields and all SILCC-Zoom simulations, which have an initial field strength of 3 $\mu$G, a flip from parallel to perpendicular orientation occurs at high densities of $n_\text{trans}$ $\simeq$ 10$^2$ - 10$^3$ cm$^{-3}$. We suggest that this flip happens if the MC's mass-to-flux ratio, $\mu$, is close to or below the critical value of 1. This corresponds to a field strength around 3 - 5 $\mu$G. In 2D, we use the Projected Rayleigh Statistics (PRS) to study the orientation of $\bf{B}$. If present, the flip in orientation occurs at $N_\text{trans}$ $\simeq$ 10$^{21 - 21.5}$ cm$^{-2}$, similar to the observed transition value from sub- to supercritical magnetic fields in the ISM. However, projection effects can reduce the power of the PRS method: Depending on the MC or LOS, the projected maps of the SILCC-Zoom simulations do not always show the flip, although expected from the 3D morphology. Such projection effects can explain the variety of recently observed field configurations, in particular within a single MC. Finally, we do not find a correlation between the observed orientation of $\bf{B}$ and the $N$-PDF.Comment: 20 pages, 12 figures, accepted for publication in MNRA

Graphene-based LbL deposited films: further study of electrical and gas sensing properties

Graphene-surfactant composite materials obtained by the ultrasonic exfoliation of graphite powder in the presence of ionic surfactants (either CTAB or SDS) were utilised to construct thin films using layer-by-layer (LbL) electrostatic deposition technique. A series of graphene-based thin films were made by alternating layers of either graphene-SDS with polycations (PEI or PAH) or graphene-CTAB with polyanions (PSS). Also, graphene-phthalocyanine composite films were produced by alternating layers of graphene-CTAB with tetrasulfonated nickel phthalocyanine. Graphene-surfactant LbL films exhibited good electric conductivity (about 0.1 S/cm) of semiconductor type with a band gap of about 20 meV. Judging from UV-vis spectra measurements, graphene-phthalocyanine LbL films appeared to form joint π-electron system. Gas sensing testing of such composite films combining high conductivity of graphene with the gas sensing abilities of phthalocyanines showed substantial changes (up to 10%) in electrical conductivity upon exposure to electro-active gases such as HCl and NH3