Structure Formation, Melting, and the Optical Properties of Gold/DNA Nanocomposites: Effects of Relaxation Time

We present a model for structure formation, melting, and optical properties of gold/DNA nanocomposites. These composites consist of a collection of gold nanoparticles (of radius 50 nm or less) which are bound together by links made up of DNA strands. In our structural model, the nanocomposite forms from a series of Monte Carlo steps, each involving reaction-limited cluster-cluster aggregation (RLCA) followed by dehybridization of the DNA links. These links form with a probability $p_{eff}$ which depends on temperature and particle radius $a$. The final structure depends on the number of monomers (i. e. gold nanoparticles) $N_m$, $T$, and the relaxation time. At low temperature, the model results in an RLCA cluster. But after a long enough relaxation time, the nanocomposite reduces to a compact, non-fractal cluster. We calculate the optical properties of the resulting aggregates using the Discrete Dipole Approximation. Despite the restructuring, the melting transition (as seen in the extinction coefficient at wavelength 520 nm) remains sharp, and the melting temperature $T_M$ increases with increasing $a$ as found in our previous percolation model. However, restructuring increases the corresponding link fraction at melting to a value well above the percolation threshold. Our calculated extinction cross section agrees qualitatively with experiments on gold/DNA composites. It also shows a characteristic ``rebound effect,'' resulting from incomplete relaxation, which has also been seen in some experiments. We discuss briefly how our results relate to a possible sol-gel transition in these aggregates.Comment: 12 pages, 10 figure

Herschel observations of EXtra-Ordinary Sources (HEXOS): Observations of H2O and its isotopologues towards Orion KL

We report the detection of more than 48 velocity-resolved ground rotational state transitions of H 16 2 O, H 18 2 O, and H 17 2 O – most for the first time – in both emission and absorption toward Orion KL using Herschel/HIFI. We show that a simple fit, constrained to match the known emission and absorption components along the line of sight, is in excellent agreement with the spectral profiles of all the water lines. Using the measured H 18 2 O line fluxes, which are less affected by line opacity than their H 16 2 O counterparts, and an escape probability method, the column densities of H 18 2 O associated with each emission component are derived. We infer total water abundances of 7.4 × 10−5, 1.0× 10−5, and 1.6 × 10−5 for the plateau, hot core, and extended warm gas, respectively. In the case of the plateau, this value is consistent with previous measures of the Orion-KL water abundance as well as those of other molecular outflows. In the case of the hot core and extended warm gas, these values are somewhat higher than water abundances derived for other quiescent clouds, suggesting that these regions are likely experiencing enhanced water-ice sublimation from (and reduced freeze-out onto) grain surfaces due to the warmer dust in these sources

Herschel observations of EXtra-Ordinary Sources (HEXOS): Detection of hydrogen fluoride in absorption towards Orion KL

We report a detection of the fundamental rotational transition of hydrogen fluoride in absorption towards Orion KL using Herschel/HIFI. After the removal of contaminating features associated with common molecules (“weeds”), the HF spectrum shows a P-Cygni profile, with weak redshifted emission and strong blue-shifted absorption, associated with the low-velocity molecular outflow. We derive an estimate of 2.9 × 1013 cm−2 for the HF column density responsible for the broad absorption component. Using our best estimate of the H2 column density within the low-velocity molecular outflow, we obtain a lower limit of ∼1.6 × 10−10 for the HF abundance relative to hydrogen nuclei, corresponding to ∼0.6% of the solar abundance of fluorine. This value is close to that inferred from previous ISO observations of HF J = 2−1 absorption towards Sgr B2, but is in sharp contrast to the lower limit of 6 × 10−9 derived by Neufeld et al. for cold, foreground clouds on the line of sight towards G10.6-0.4

Herschel observations of deuterated water towards Sgr B2(M)

Observations of HDO are an important complement for studies of water, because they give strong constraints on the formation processes – grain surfaces versus energetic process in the gas phase, e.g. in shocks. The HIFI observations of multiple transitions of HDO in Sgr B2(M) presented here allow the determination of the HDO abundance throughout the envelope, which has not been possible before with ground-based observations only. The abundance structure has been modeled with the spherical Monte Carlo radiative transfer code RATRAN, which also takes radiative pumping by continuum emission from dust into account. The modeling reveals that the abundance of HDO rises steeply with temperature from a low abundance (2.5 × 10−11) in the outer envelope at temperatures below 100 K through a medium abundance (1.5 × 10−9) in the inner envelope/outer core at temperatures between 100 and 200 K, and finally a high abundance ( 3.5 × 10−9) at temperatures above 200 K in the hot core

Reversal of infall in SgrB2(M) revealed by Herschel/HIFI observations of HCN lines at THz frequencies

Aims. To investigate the accretion and feedback processes in massive star formation, we analyze the shapes of emission lines from hot molecular cores, whose asymmetries trace infall and expansion motions. Methods. The high-mass star forming region SgrB2(M) was observed with Herschel/HIFI (HEXOS key project) in various lines of HCN and its isotopologues, complemented by APEX data. The observations are compared to spherically symmetric, centrally heated models with density power-law gradient and different velocity fields (infall or infall+expansion), using the radiative transfer code RATRAN. Results. The HCN line profiles are asymmetric, with the emission peak shifting from blue to red with increasing J and decreasing line opacity (HCN to H13CN). This is most evident in the HCN 12–11 line at 1062 GHz. These line shapes are reproduced by a model whose velocity field changes from infall in the outer part to expansion in the inner part. Conclusions. The qualitative reproduction of the HCN lines suggests that infall dominates in the colder, outer regions, but expansion dominates in the warmer, inner regions. We are thus witnessing the onset of feedback in massive star formation, starting to reverse the infall and finally disrupting the whole molecular cloud. To obtain our result, the THz lines uniquely covered by HIFI were critically important

Herschel observations of EXtra-Ordinary Sources (HEXOS): The present and future of spectral surveys with Herschel/HIFI

We present initial results from the Herschel GT key program: Herschel observations of EXtra-Ordinary Sources (HEXOS) and outline the promise and potential of spectral surveys with Herschel/HIFI. The HIFI instrument offers unprecedented sensitivity, as well as continuous spectral coverage across the gaps imposed by the atmosphere, opening up a largely unexplored wavelength regime to high-resolution spectroscopy. We show the spectrum of Orion KL between 480 and 560 GHz and from 1.06 to 1.115 THz. From these data, we confirm that HIFI separately measures the dust continuum and spectrally resolves emission lines in Orion KL. Based on this capability we demonstrate that the line contribution to the broad-band continuum in this molecule-rich source is ∼20−40% below 1 THz and declines to a few percent at higher frequencies. We also tentatively identify multiple transitions of HD18O in the spectra. The first detection of this rare isotopologue in the interstellar medium suggests that HDO emission is optically thick in the Orion hot core with HDO/H2O ∼ 0.02. We discuss the implications of this detection for the water D/H ratio in hot cores

Herschel observations of EXtra-Ordinary Sources (HEXOS): The Terahertz spectrum of Orion KL seen at high spectral resolution

We present the first high spectral resolution observations of Orion KL in the frequency ranges 1573.4–1702.8 GHz (band 6b) and 1788.4–1906.8 GHz (band 7b) obtained using the HIFI instrument on board the Herschel Space Observatory. We characterize the main emission lines found in the spectrum, which primarily arise from a range of components associated with Orion KL including the hot core, but also see widespread emission from components associated with molecular outflows traced by H2O, SO2, and OH. We find that the density of observed emission lines is significantly diminished in these bands compared to lower frequency Herschel/HIFI bands

Origin of the hot gas in low-mass protostars, Herschel-PACS spectroscopy of HH 46

Aims. “Water In Star-forming regions with Herschel” (WISH) is a Herschel key programme aimed at understanding the physical and chemical structure of young stellar objects (YSOs) with a focus on water and related species. Methods. The low-mass protostar HH 46 was observed with the Photodetector Array Camera and Spectrometer (PACS) on the Herschel Space Observatory to measure emission in H2O, CO, OH, [O i], and [C ii] lines located between 63 and 186 μm. The excitation and spatial distribution of emission can disentangle the different heating mechanisms of YSOs, with better spatial resolution and sensitivity than previously possible. Results. Far-IR line emission is detected at the position of the protostar and along the outflow axis. The OH emission is concentrated at the central position, CO emission is bright at the central position and along the outflow, and H2O emission is concentrated in the outflow. In addition, [O i] emission is seen in low-velocity gas, assumed to be related to the envelope, and is also seen shifted up to 170 km s−1 in both the red- and blue-shifted jets. Envelope models are constructed based on previous observational constraints. They indicate that passive heating of a spherical envelope by the protostellar luminosity cannot explain the high-excitation molecular gas detected with PACS, including CO lines with upper levels at >2500 K above the ground state. Instead, warm CO and H2O emission is probably produced in the walls of an outflow-carved cavity in the envelope, which are heated by UV photons and non-dissociative C-type shocks. The bright OH and [Oi] emission is attributed to J-type shocks in dense gas close to the protostar. In the scenario described here, the combined cooling by far-IR lines within the central spatial pixel is estimated to be 2 × 10−2 L, with 60–80% attributed to J- and C-type shocks produced by interactions between the jet and the envelope

Herschel observations of EXtra-Ordinary Sources (HEXOS): detecting spiral arm clouds by CH absorption lines

We have observed CH absorption lines (J = 3/2, N = 1 ← J = 1/2, N = 1) against the continuum source Sgr B2(M) using the Herschel/HIFI instrument. With the high spectral resolution and wide velocity coverage provided by HIFI, 31 CH absorption features with different radial velocities and line widths are detected and identified. The narrower line width and lower column density clouds show “spiral arm” cloud characteristics, while the absorption component with the broadest line width and highest column density corresponds to the gas from the Sgr B2 envelope. The observations show that each “spiral arm” harbors multiple velocity components, indicating that the clouds are not uniform and that they have internal structure. This line-of-sight through almost the entire Galaxy offers unique possibilities to study the basic chemistry of simple molecules in diffuse clouds, as a variety of different cloud classes are sampled simultaneously. We find that the linear relationship between CH and H2 column densities found at lower AV by UV observations does not continue into the range of higher visual extinction. There, the curve flattens, which probably means that CH is depleted in the denser cores of these clouds

Herschel/HIFI measurements of the ortho/para ratio in water towards Sagittarius B2(M) and W31C

We present Herschel/HIFI observations of the fundamental rotational transitions of ortho- and para-H16 2 O and H18 2 O in absorption towards Sagittarius B2(M) and W31C. The ortho/para ratio in water in the foreground clouds on the line of sight towards these bright continuum sources is generally consistent with the statistical high-temperature ratio of 3, within the observational uncertainties. However, somewhat unexpectedly, we derive a low ortho/para ratio of 2.35±0.35, corresponding to a spin temperature of ∼27 K, towards Sagittarius B2(M) at velocities of the expanding molecular ring. Water molecules in this region appear to have formed with, or relaxed to, an ortho/para ratio close to the value corresponding to the local temperature of the gas and dust