Calculations of Potential Energy Surfaces Using Monte Carlo Configuration Interaction

We apply the method of Monte Carlo configuration interaction (MCCI) to calculate ground-state potential energy curves for a range of small molecules and compare the results with full configuration interaction. We show that the MCCI potential energy curve can be calculated to relatively good accuracy, as quantified using the non-parallelity error, using only a very small fraction of the FCI space. In most cases the potential curve is of better accuracy than its constituent single-point energies. We finally test the MCCI program on systems with basis sets beyond full configuration interaction: a lattice of fifty hydrogen atoms and ethylene. The results for ethylene agree fairly well with other computational work while for the lattice of fifty hydrogens we find that the fraction of the full configuration interaction space we were able to consider appears to be too small as, although some qualitative features are reproduced, the potential curve is less accurate.Comment: 14 pages, 22 figure

Monte Carlo configuration interaction applied to multipole moments, ionisation energies and electron affinities

The method of Monte Carlo configuration interaction (MCCI) [1,2] is applied to the calculation of multipole moments. We look at the ground and excited state dipole moments in carbon monoxide. We then consider the dipole of NO, the quadrupole of the nitrogen molecule and of BH. An octupole of methane is also calculated. We consider experimental geometries and also stretched bonds. We show that these non-variational quantities may be found to relatively good accuracy when compared with FCI results, yet using only a small fraction of the full configuration interaction space. MCCI results in the aug-cc-pVDZ basis are seen to generally have reasonably good agreement with experiment. We also investigate the performance of MCCI when applied to ionisation energies and electron affinities of atoms in an aug-cc-pVQZ basis. We compare the MCCI results with full configuration-interaction quantum Monte Carlo [3,4] and `exact' non-relativistic results [3,4]. We show that MCCI could be a useful alternative for the calculation of atomic ionisation energies however electron affinities appear much more challenging for MCCI. Due to the small magnitude of the electron affinities their percentage errors can be high, but with regards to absolute errors MCCI performs similarly for ionisation energies and electron affinities.Comment: 12 pages, 20 figure

A Multiwavelength Investigation of the Relationship Between 2CG135+1 and LSI+61o 303

We present the results of a multiwavelength monitoring campaign targeting the gamma-ray source 2CG 135+1 in an attempt to confirm the association of this object with the radio/Be/X-ray binary system LSI +61o 303. The campaign included simultaneous radio, optical, infrared, and hard x-ray/gamma-ray observations carried out with a variety of instruments, covering (not continously) almost three binary cycles of LSI +61o 303 during the period April-July 1994. Three separate OSSE observations of the gamma-ray source were carried out, covering different phases of the radio lightcurve. Hard X-ray/gamma-ray emission was detected from the direction of 2CG 135+1 during the first of these OSSE observations. The signal to noise ratio of the OSSE observations was insufficient to establish a spectral or intensity correlation of the high-energy emission with simultaneous radio, optical and infrared emission of LSI +61o 303. We briefly discuss the theoretical implications of our observations.Comment: 17 pages, 9 figures, 6 tables to be published in Astrophysical Journal, 10 April 199

Evolution of trace gases and particles emitted by a chaparral fire in California

Biomass burning (BB) is a major global source of trace gases and particles. Accurately representing the production and evolution of these emissions is an important goal for atmospheric chemical transport models. We measured a suite of gases and aerosols emitted from an 81 hectare prescribed fire in chaparral fuels on the central coast of California, US on 17 November 2009. We also measured physical and chemical changes that occurred in the isolated downwind plume in the first ~4 h after emission. The measurements were carried out onboard a Twin Otter aircraft outfitted with an airborne Fourier transform infrared spectrometer (AFTIR), aerosol mass spectrometer (AMS), single particle soot photometer (SP2), nephelometer, LiCor CO_2 analyzer, a chemiluminescence ozone instrument, and a wing-mounted meteorological probe. Our measurements included: CO_2; CO; NO_x; NH_3; non-methane organic compounds; organic aerosol (OA); inorganic aerosol (nitrate, ammonium, sulfate, and chloride); aerosol light scattering; refractory black carbon (rBC); and ambient temperature, relative humidity, barometric pressure, and three-dimensional wind velocity. The molar ratio of excess O_3 to excess CO in the plume (ΔO_3/ΔCO) increased from −5.13 (±1.13) × 10^(−3) to 10.2 (±2.16) × 10^(−2) in ~4.5 h following smoke emission. Excess acetic and formic acid (normalized to excess CO) increased by factors of 1.73 ± 0.43 and 7.34 ± 3.03 (respectively) over the same time since emission. Based on the rapid decay of C_2H_4 we infer an in-plume average OH concentration of 5.27 (±0.97) × 10^6 molec cm^(−3), consistent with previous studies showing elevated OH concentrations in biomass burning plumes. Ammonium, nitrate, and sulfate all increased over the course of 4 h. The observed ammonium increase was a factor of 3.90 ± 2.93 in about 4 h, but accounted for just ~36% of the gaseous ammonia lost on a molar basis. Some of the gas phase NH_3 loss may have been due to condensation on, or formation of, particles below the AMS detection range. NO_x was converted to PAN and particle nitrate with PAN production being about two times greater than production of observable nitrate in the first ~4 h following emission. The excess aerosol light scattering in the plume (normalized to excess CO_2) increased by a factor of 2.50 ± 0.74 over 4 h. The increase in light scattering was similar to that observed in an earlier study of a biomass burning plume in Mexico where significant secondary formation of OA closely tracked the increase in scattering. In the California plume, however, ΔOA/ΔCO_2 decreased sharply for the first hour and then increased slowly with a net decrease of ~20% over 4 h. The fraction of thickly coated rBC particles increased up to ~85% over the 4 h aging period. Decreasing OA accompanied by increased scattering/particle coating in initial aging may be due to a combination of particle coagulation and evaporation processes. Recondensation of species initially evaporated from the particles may have contributed to the subsequent slow rise in OA. We compare our results to observations from other plume aging studies and suggest that differences in environmental factors such as smoke concentration, oxidant concentration, actinic flux, and RH contribute significantly to the variation in plume evolution observations

Optical variabilities in Be/X-ray binary system:GRO J2058+42

We present an analysis of long-term optical monitoring observations and optical spectroscopic observations of the counterpart to CXOU J205847.5+414637 (high mass X-ray binary system). We search for a variability in the light curve of Be star. We used differential magnitudes in the time series analysis. The variability search in the optical light curve was made by using different algorithms. The reduction and analysis of spectra were done by using MIDAS and its suitable packages. We have performed a frequency search which gave us the value 2.404 1/day. This value is attributed to the non-radial pulsation of Be star. H alpha emission line profiles always show double-peaked emissions with a mean equivalent width of 2.31 \pm 0.19 \AA ~and a peak separation of 516 \pm 45 km/s. This suggests that Be star disk is still present. CXOU J205847.5+414637 is in X-ray quiescent state.Comment: 8 pages, 9 figures. To appear at Astronomy and Astrophysic

Discovery of diffuse emission in the galaxy cluster A1689

The aim of this work is to investigate the possible presence of extended diffuse synchrotron radio emission associated with the intracluster medium of the complex galaxy cluster A1689. The radio continuum emission of A1689 has been investigated by analyzing archival observations at 1.2 and 1.4 GHz obtained with the Very Large Array in different configurations. We report the detection of an extended, diffuse, low-surface brightness radio emission located in the central region of A1689. The surface brightness profile of the diffuse emission at 1.2 GHz indicates a central radio brightness of ~1.7 \mu Jy/arcsec^2 and the 3\sigma radio isophothes reveal the largest linear size to be 730 kpc. Given its central location, the low-level surface brightness, and the comparatively large extension, we classify the diffuse cluster-wide emission in A1689 as a small radio halo.Comment: 8 pages, 6 figures, A&A accepte

Size-dependent wet removal of black carbon in Canadian biomass burning plumes

Wet deposition is the dominant mechanism for removing black carbon (BC) from the atmosphere and is key in determining its atmospheric lifetime, vertical gradient and global transport. Despite the importance of BC in the climate system, especially in terms of its ability to modulate the radiative energy budget, there are few quantitative case studies of wet removal in ambient environments. We present a case study of BC wet removal by examining aerosol size distributions and BC coating properties sampled in three Canadian boreal biomass burning plumes, one of which passed through a precipitating cloud. This depleted the majority of the plume’s BC mass, and the largest and most coated BCcontaining particles were found to be preferentially removed, suggesting that nucleation scavenging was likely the dominant mechanism. Calculated single-scattering albedo (SSA) showed little variation, as a large number of non-BC particles were also present in the precipitation-affected plume. The remaining BC cores were smaller than those observed in previous studies of BC in post-precipitation outflow over Asia, possibly due to the thick coating by hydrophilic compounds associated with the Canadian biomass burning particles. This study provides measurements of BC size, mixing state and removal efficiency to constrain model parameterisations of BC wet removal in biomass burning regions, which will help to reduce uncertainty in radiative forcing calculations

XMM-Newton observations of the Galactic Supernova Remnant CTB 109 (G109.1-1.0)

We present the analysis of the X-ray Multi-Mirror Mission (XMM-Newton) European Photon Imaging Camera (EPIC) data of the Galactic supernova remnant (SNR) CTB 109 (G109.1-1.0). CTB 109 is associated with the anomalous X-ray pulsar (AXP) 1E 2259+586 and has an unusual semi-circular morphology in both the X-ray and the radio, and an extended X-ray bright interior region known as the `Lobe'. The deep EPIC mosaic image of the remnant shows no emission towards the west where a giant molecular cloud complex is located. No morphological connection between the Lobe and the AXP is found. We find remarkably little spectral variation across the remnant given the large intensity variations. All spectra of the shell and the Lobe are well fitted by a single-temperature non-equilibrium ionization model for a collisional plasma with solar abundances (kT = 0.5 - 0.7 keV, tau = n_e t = 1 - 4 x 10^11 s cm^-3, N_H = 5 - 7 x 10^21 cm^-2). There is no indication of nonthermal emission in the Lobe or the shell. We conclude that the Lobe originated from an interaction of the SNR shock wave with an interstellar cloud. Applying the Sedov solution for the undisturbed eastern part of the SNR, and assuming full equilibration between the electrons and ions behind the shock front, the SNR shock velocity is derived as v_s = 720 +/- 60 km s^-1, the remnant age as t = (8.8 +/- 0.9) x 10^3 d_3 yr, the initial energy as E_0 = (7.4 +/- 2.9) x 10^50 d_3^2.5 ergs, and the pre-shock density of the nuclei in the ambient medium as n_0 = (0.16 +/- 0.02) d_3^-0.5 cm^-3, at an assumed distance of D = 3.0 d_3 kpc. Assuming CTB 109 and 1E 2259+586 are associated, these values constrain the age and the environment of the progenitor of the SNR and the pulsar.Comment: Accepted for publication in ApJ. 9 figures. Figs. 1 + 2 are in color (fig1.jpg, fig2.jpg

Aerosol emissions from prescribed fires in the United States: A synthesis of laboratory and aircraft measurements

Aerosol emissions from prescribed fires can affect air quality on regional scales. Accurate representation of these emissions in models requires information regarding the amount and composition of the emitted species. We measured a suite of submicron particulate matter species in young plumes emitted from prescribed fires (chaparral and montane ecosystems in California; coastal plain ecosystem in South Carolina) and from open burning of over 15 individual plant species in the laboratory. We report emission ratios and emission factors for refractory black carbon (rBC) and submicron nonrefractory aerosol and compare field and laboratory measurements to assess the representativeness of our laboratory-measured emissions. Laboratory measurements of organic aerosol (OA) emission factors for some fires were an order of magnitude higher than those derived from any of our aircraft observations; these are likely due to higher-fuel moisture contents, lower modified combustion efficiencies, and less dilution compared to field studies. Nonrefractory inorganic aerosol emissions depended more strongly on fuel type and fuel composition than on combustion conditions. Laboratory and field measurements for rBC were in good agreement when differences in modified combustion efficiency were considered; however, rBC emission factors measured both from aircraft and in the laboratory during the present study using the Single Particle Soot Photometer were generally higher than values previously reported in the literature, which have been based largely on filter measurements. Although natural variability may account for some of these differences, an increase in the BC emission factors incorporated within emission inventories may be required, pending additional field measurements for a wider variety of fires

Evolution of Trace Gases and Particles Emitted by a Chaparral Fire in California

Biomass burning (BB) is a major global source of trace gases and particles. Accurately representing the production and evolution of these emissions is an important goal for atmospheric chemical transport models. We measured a suite of gases and aerosols emitted from an 81 hectare prescribed fire in chaparral fuels on the central coast of California, US on 17 November 2009. We also measured physical and chemical changes that occurred in the isolated down-wind plume in the first similar to 4 h after emission. The measurements were carried out onboard a Twin Otter aircraft outfitted with an airborne Fourier transform infrared spectrometer (AFTIR), aerosol mass spectrometer (AMS), single particle soot photometer (SP2), nephelometer, LiCor CO2 analyzer, a chemiluminescence ozone instrument, and a wing-mounted meteorological probe. Our measurements included: CO2; CO; NOx; NH3; non-methane organic compounds; organic aerosol (OA); inorganic aerosol (nitrate, ammonium, sulfate, and chloride); aerosol light scattering; refractory black carbon (rBC); and ambient temperature, relative humidity, barometric pressure, and three-dimensional wind velocity. The molar ratio of excess O-3 to excess CO in the plume (Delta O-3/Delta CO) increased from -5.13 (+/- 1.13) x 10(-3) to 10.2 (+/- 2.16) x 10(-2) in similar to 4.5 h following smoke emission. Excess acetic and formic acid (normalized to excess CO) increased by factors of 1.73 +/- 0.43 and 7.34 +/- 3.03 (respectively) over the same time since emission. Based on the rapid decay of C2H4 we infer an in-plume average OH concentration of 5.27 (+/- 0.97) x 10(6) molec cm(-3), consistent with previous studies showing elevated OH concentrations in biomass burning plumes. Ammonium, nitrate, and sulfate all increased over the course of 4 h. The observed ammonium increase was a factor of 3.90 +/- 2.93 in about 4 h, but accounted for just similar to 36% of the gaseous ammonia lost on a molar basis. Some of the gas phase NH3 loss may have been due to condensation on, or formation of, particles below the AMS detection range. NOx was converted to PAN and particle nitrate with PAN production being about two times greater than production of observable nitrate in the first similar to 4 h following emission. The excess aerosol light scattering in the plume (normalized to excess CO2) increased by a factor of 2.50 +/- 0.74 over 4 h. The increase in light scattering was similar to that observed in an earlier study of a biomass burning plume in Mexico where significant secondary formation of OA closely tracked the increase in scattering. In the California plume, however, Delta OA/Delta CO2 decreased sharply for the first hour and then increased slowly with a net decrease of similar to 20% over 4 h. The fraction of thickly coated rBC particles increased up to similar to 85% over the 4 h aging period. Decreasing OA accompanied by increased scattering/particle coating in initial aging may be due to a combination of particle coagulation and evaporation processes. Recondensation of species initially evaporated from the particles may have contributed to the subsequent slow rise in OA. We compare our results to observations from other plume aging studies and suggest that differences in environmental factors such as smoke concentration, oxidant concentration, actinic flux, and RH contribute significantly to the variation in plume evolution observations