Electrochemically Switchable Multimode Strong Coupling in Plasmonic Nanocavities

The strong-coupling interaction between quantum emitters and cavities provides the archetypical platform for fundamental quantum electrodynamics. Here we show that methylene blue (MB) molecules interact coherently with subwavelength plasmonic nanocavity modes at room temperature. Experimental results show that the strong coupling can be switched on and off reversibly when MB molecules undergo redox reactions which transform them to leuco-methylene blue molecules. In simulations we demonstrate the strong coupling between the second excited plasmonic cavity mode and resonant emitters. However, we also show that other detuned modes simultaneously couple efficiently to the molecular transitions, creating unusual cascades of mode spectral shifts and polariton formation. This is possible due to the relatively large plasmonic particle size resulting in reduced mode splittings. The results open significant potential for device applications utilizing active control of strong coupling

Synthesis of satellite (MODIS), aircraft (ICARTT), and surface (IMPROVE, EPA-AQS, AERONET) aerosol observations over eastern North America to improve MODIS aerosol retrievals and constrain surface aerosol concentrations and sources

We use an ensemble of satellite (MODIS), aircraft, and ground-based aerosol observations during the ICARTT field campaign over eastern North America in summer 2004 to (1) examine the consistency between different aerosol measurements, (2) evaluate a new retrieval of aerosol optical depths (AODs) and inferred surface aerosol concentrations (PM2.5) from the MODIS satellite instrument, and (3) apply this collective information to improve our understanding of aerosol sources. The GEOS-Chem global chemical transport model (CTM) provides a transfer platform between the different data sets, allowing us to evaluate the consistency between different aerosol parameters observed at different times and locations. We use an improved MODIS AOD retrieval based on locally derived visible surface reflectances and aerosol properties calculated from GEOS-Chem. Use of GEOS-Chem aerosol optical properties in the MODIS retrieval not only results in an improved AOD product but also allows quantitative evaluation of model aerosol mass from the comparison of simulated and observed AODs. The aircraft measurements show narrower aerosol size distributions than those usually assumed in models, and this has important implications for AOD retrievals. Our MODIS AOD retrieval compares well to the ground-based AERONET data (R = 0.84, slope = 1.02), significantly improving on the MODIS c005 operational product. Inference of surface PM2.5 from our MODIS AOD retrieval shows good correlation to the EPA-AQS data (R = 0.78) but a high regression slope (slope = 1.48). The high slope is seen in all AOD-inferred PM2.5 concentrations (AERONET: slope = 2.04; MODIS c005: slope = 1.51) and could reflect a clear-sky bias in the AOD observations. The ensemble of MODIS, aircraft, and surface data are consistent in pointing to a model overestimate of sulfate in the mid-Atlantic and an underestimate of organic and dust aerosol in the southeastern United States. The sulfate overestimate could reflect an excessive contribution from aqueous-phase production in clouds, while the organic carbon underestimate could possibly be resolved by a new secondary pathway involving dicarbonyls

Synthetic CO emission and the XCOX_{\rm CO} factor of young molecular clouds: a convergence study

The properties of synthetic CO emission from 3D simulations of forming molecular clouds are studied within the SILCC-Zoom project. Since the time scales of cloud evolution and molecule formation are comparable, the simulations include a live chemical network. Two sets of simulations with an increasing spatial resolution (d$x=3.9$ pc to d$x=0.06$ pc) are used to investigate the convergence of the synthetic CO emission, which is computed by post-processing the simulation data with the RADMC-3D radiative transfer code. To determine the excitation conditions, it is necessary to include atomic hydrogen and helium alongside H$_2$, which increases the resulting CO emission by ~7-26 per cent. Combining the brightness temperature of $^{12}$CO and $^{13}$CO, we compare different methods to estimate the excitation temperature, the optical depth of the CO line and hence, the CO column density. An intensity-weighted average excitation temperature results in the most accurate estimate of the total CO mass. When the pixel-based excitation temperature is used to calculate the CO mass, it is over-/underestimated at low/high CO column densities where the assumption that $^{12}$CO is optically thick while $^{13}$CO is optically thin is not valid. Further, in order to obtain a converged total CO luminosity and hence factor, the 3D simulation must have d$x\lesssim0.1$ pc. The evolves over time and differs for the two clouds; yet pronounced differences with numerical resolution are found. Since high column density regions with a visual extinction larger than 3~mag are not resolved for d$x\gtrsim 1$~pc, in this case the H$_2$ mass and CO luminosity both differ significantly from the higher resolution results and the local $X_{\rm CO}$ is subject to strong noise. Our calculations suggest that synthetic CO emission maps are only converged for simulations with d$x\lesssim 0.1$ pc.Comment: 23 pages, 22 figures, accepted for publication in MNRA

Climate Change and invasibility of the Antarctic benthos

Benthic communities living in shallow-shelf habitats in Antarctica (<100-m depth) are archaic in their structure and function. Modern predators, including fast-moving, durophagous (skeleton-crushing) bony fish, sharks, and crabs, are rare or absent; slow-moving invertebrates are the top predators; and epifaunal suspension feeders dominate many soft substratum communities. Cooling temperatures beginning in the late Eocene excluded durophagous predators, ultimately resulting in the endemic living fauna and its unique food-web structure. Although the Southern Ocean is oceanographically isolated, the barriers to biological invasion are primarily physiological rather than geographic. Cold temperatures impose limits to performance that exclude modern predators. Global warming is now removing those physiological barriers, and crabs are reinvading Antarctica. As sea temperatures continue to rise, the invasion of durophagous predators will modernize the shelf benthos and erode the indigenous character of marine life in Antarctica

Strategies for the Synthesis of Spiropiperidines - A Review of the Last 10 Years

Spiropiperidines have gained in popularity in drug discovery programmes as medicinal chemists explore new areas of three-dimensional chemical space. This review focuses on the methodology used for the construction of 2-, 3- and 4- spiropiperidines, covering the literature from the last 10 years. It classifies the synthesis of each of the types of spiropiperidine by synthetic strategy: the formation of the spiro-ring on a preformed piperidine ring, and the formation of the piperidine ring on a preformed carbo- or heterocyclic ring. While 3- and 4-spiropiperidines are predominantly synthesised for drug discovery projects, 2-spiropiperidines are synthesised en route to natural products. The lack of 2- spiropiperidines in drug discovery is presumably due to limited general procedures for their synthesis

Incremental bounded model checking for embedded software

Program analysis is on the brink of mainstream usage in embedded systems development. Formal verification of behavioural requirements, finding runtime errors and test case generation are some of the most common applications of automated verification tools based on bounded model checking (BMC). Existing industrial tools for embedded software use an off-the-shelf bounded model checker and apply it iteratively to verify the program with an increasing number of unwindings. This approach unnecessarily wastes time repeating work that has already been done and fails to exploit the power of incremental SAT solving. This article reports on the extension of the software model checker CBMC to support incremental BMC and its successful integration with the industrial embedded software verification tool BTC EMBEDDED TESTER. We present an extensive evaluation over large industrial embedded programs, mainly from the automotive industry. We show that incremental BMC cuts runtimes by one order of magnitude in comparison to the standard non-incremental approach, enabling the application of formal verification to large and complex embedded software. We furthermore report promising results on analysing programs with arbitrary loop structure using incremental BMC, demonstrating its applicability and potential to verify general software beyond the embedded domain

Shallow stratigraphic control on pockmark distribution in north temperate estuaries

This paper is not subject to U.S. copyright. The definitive version was published in Marine Geology 329-331 (2012): 34-45, doi:10.1016/j.margeo.2012.09.006.Pockmark fields occur throughout northern North American temperate estuaries despite the absence of extensive thermogenic hydrocarbon deposits typically associated with pockmarks. In such settings, the origins of the gas and triggering mechanism(s) responsible for pockmark formation are not obvious. Nor is it known why pockmarks proliferate in this region but do not occur south of the glacial terminus in eastern North America. This paper tests two hypotheses addressing these knowledge gaps: 1) the region's unique sea-level history provided a terrestrial deposit that sourced the gas responsible for pockmark formation; and 2) the region's physiography controls pockmarks distribution. This study integrates over 2500 km of high-resolution swath bathymetry, Chirp seismic reflection profiles and vibracore data acquired in three estuarine pockmark fields in the Gulf of Maine and Bay of Fundy. Vibracores sampled a hydric paleosol lacking the organic-rich upper horizons, indicating that an organic-rich terrestrial deposit was eroded prior to pockmark formation. This observation suggests that the gas, which is presumably responsible for the formation of the pockmarks, originated in Holocene estuarine sediments (loss on ignition 3.5–10%), not terrestrial deposits that were subsequently drowned and buried by mud. The 7470 pockmarks identified in this study are non-randomly clustered. Pockmark size and distribution relate to Holocene sediment thickness (r2 = 0.60), basin morphology and glacial deposits. The irregular underlying topography that dictates Holocene sediment thickness may ultimately play a more important role in temperate estuarine pockmark distribution than drowned terrestrial deposits. These results give insight into the conditions necessary for pockmark formation in nearshore coastal environments.Graduate support for Brothers came from a Maine Economic Improvement Fund Dissertation Fellowship

Simultaneous monitoring of the photometric and polarimetric activity of the young star PV Cep in the optical/near-infrared bands

We present the results of a simultaneous monitoring, lasting more than 2 years, of the optical and near-infrared photometric and polarimetric activity of the variable protostar PV Cep. During the monitoring period, an outburst has occurred in all the photometric bands, whose declining phase ($\Delta$J $\approx$ 3 mag) lasted about 120 days. A time lag of $\sim$ 30 days between optical and infrared light curves has been measured and interpreted in the framework of an accretion event. This latter is directly recognizable in the significant variations of the near-infrared colors, that appear bluer in the outburst phase, when the star dominates the emission, and redder in declining phase, when the disk emission prevails. All the observational data have been combined to derive a coherent picture of the complex morphology of the whole PV Cep system, that, in addition to the star and the accretion disk, is composed also by a variable biconical nebula. In particular, the mutual interaction between all these components is the cause of the high value of the polarization ($\approx$ 20%) and of its fluctuations. The observational data concur to indicate that PV Cep is not a genuine EXor star, but rather a more complex object; moreover the case of PV Cep leads to argue about the classification of other recently discovered young sources in outburst, that have been considered, maybe over-simplifying, as EXor.Comment: Accepted for publication on Ap