Article on coherent excitation of a two-level atom driven by a far off-resonant classical field.

Diabetes mellitus results from an absolute or relative deficiency of insulin producing pancreatic beta-cells. The adult human beta-cell's turnover rate remains unknown. We employed novel techniques to examine adult human islet beta-cell turnover and longevity in vivo. Subjects enrolled in NIH clinical trials received thymidine analogues [iododeoxyuridine (IdU) or bromodeoxyuridine (BrdU)] 8-days to 4-years prior to death. Archival autopsy samples from ten patients (aged 17-74 years) were employed to assess beta-cell turnover by scoring nuclear analog labeling within insulin staining cells. Human adult beta-cell longevity was determined by estimating the cells genomic DNA integration of atmospheric carbon-14 ({sup 14}C). DNA was purified from pancreatic islets isolated from cadaveric donors; whole islet prep DNA was obtained from a 15 year old donor, and purified beta-cell DNA was obtained from two donors (age 48 and 80 years). {sup 14}C levels were then determined using accelerator mass spectrometry (AMS). Cellular 'birth date' was determined by comparing the subject's DNA {sup 14}C content relative to a well-established {sup 14}C atmospheric prevalence curve. In the two subjects less than age 20 years, 1-2% of the beta-cell nuclei co-stained for BrdU/IdU. No beta-cell nuclei co-stained in the eight patients more than 30 years old. Consistent with …

Monodisperse sub-10 nm (6.5 nm) sized Rh nanocrystals with (111) and (100) surface structures were synthesized by a seedless polyol reduction in ethylene glycol, with poly(vinylpyrrolidone) as a capping ligand. When using [Rh(Ac){sub 2}]{sub 2} as the metal precursor, (111)-oriented Rh nanopolyhedra containing 76% (111)-twined hexagons (in 2D projection) were obtained; whereas, when employing RhCl{sub 3} as the metal precursor in the presence of alkylammonium bromide, such as tetramethylammonium bromide and trimethyl(tetradecyl)ammonium bromide, (100)-oriented Rh nanocubes were obtained with 85% selectivity. The {l_brace}100{r_brace} faces of the Rh nanocrystals are stabilized by chemically adsorbed Br{sup -} ions from alkylammonium bromides, which led to (100)-oriented nanocubes. Monolayer films of the (111)-oriented Rh nanopolyhedra and (100)-oriented Rh nanocubes were deposited on silicon wafers in a Langmuir-Blodgett trough to make model 2D nanoarray catalysts. These nanocatalysts were active for CO oxidation by O{sub 2}, and the turnover frequency was independent of nanoparticle shape, consistent with that previously observed for Rh(111) and Rh(100) single crystals.

Two luminescent terbium(III) complexes have been prepared from chiral ligands containing 2-hydroxyisophthalamide (IAM) antenna chromophores and their non-polarized and circularly-polarized luminescence properties have been studied. These tetradentate ligands, which form 2:1 ligand/Tb{sup III} complexes, utilize diaminocyclohexane (cyLI) and diphenylethylenediamine (dpenLI) backbones, which we reasoned would impart conformational rigidity and result in Tb{sup III} complexes that display both large luminescence quantum yield ({phi}) values and strong circularly polarized luminescence (CPL) activities. Both Tb{sup III} complexes are highly emissive, with {phi} values of 0.32 (dpenLI-Tb) and 0.60 (cyLI-Tb). Luminescence lifetime measurements in H{sub 2}O and D{sub 2}O indicate that while cyLI-Tb exists as a single species in solution, dpenLI-Tb exists as two species: a monohydrate complex with one H{sub 2}O molecule directly bound to the Tb{sup III} ion and a complex with no water molecules in the inner coordination sphere. Both cyLI-Tb and dpenLI-Tb display increased CPL activity compared to previously reported Tb{sup III} complexes made with chiral IAM ligands. The CPL measurements also provide additional confirmation of the presence of a single emissive species in solution in the case of cyLI-Tb, and multiple emissive species in the case of dpenLI-Tb.

Respective Roles of Shallow Convection and Stratiform Rainfall on the Simulation of Madden Julian Oscillation Joshua Xiouhua Fu IPRC, SOEST, University of Hawaii The IPRC/UH Hybrid-coupled GCM (HcGCM), which combined ECHAM-4 AGCM with UH intermediate ocean model, produces robust Tropical Intra-Seasonal Oscillations including the boreal-winter MJO and boreal-summer Monsoon Intra-Seasonal Oscillation. In this study, two sets of sensitivity experiments (i.e., short-term retrospective forecast of one MJO event observed during TOGA COARE and long-term free integrations) have been carried out to understand the respective roles of shallow-convection and stratiform rainfall on the simulations and predictions of the MJO. Major findings are summarized as following: Shallow-convection ahead of MJO deep convection moistens the lower-troposphere and preconditions the movement of the MJO. Present study shows that this process is very important to the eastward propagating speed of the MJO. A significant fraction of stratiform rainfall (~30%; stratiform part vs. total rainfall) is needed for ECHAM-4 to have a robust MJO. The above findings suggest that in addition to deep convection, shallow convection and stratiform rainfall needs to be well represented in conventional GCMs to ensure a robust model MJO.

Decade-long continuous surface-based measurements at Great Southern Plains (SGP) collected by the US Department of Energy’s Atmospheric Radiation Measurement (ARM) Climate Research Facility are first used to evaluate the three major reanalyses (i.e., ERA-Interim, NCEP/NCAR Reanalysis I and NCEP/DOE Reanalysis II) to identify model biases in simulating surface shortwave cloud forcing and total cloud fraction. The results show large systematic lower biases in the modeled surface shortwave cloud forcing and cloud fraction from all the three reanalysis datasets. Then we focus on diagnosing the causes of these model biases using the Active Remote Sensing of Clouds (ARSCL) products (e.g., vertical distribution of cloud fraction, cloud-base and cloud-top heights, and cloud optical depth) and meteorological measurements (temperature, humidity and stability). Efforts are made to couple cloud properties with boundary processes in the diagnosis.

As part of the Indirect and Semi-Direct Aerosol Campaign (ISDAC) an Analytical Spectral Devices (ASD, Inc.) spectroradiometer was deployed at the Barrow NSA site during April and May of 2008, and in April-October of 2009. This instrument recorded one-minute averages of surface downwelling spectral flux in the wavelength interval 350-2200 nm, thus sampling the two major near infrared windows (1.6 and 2.2 microns) in which the flux is influenced by cloud microphysical properties including thermodynamic phase and effective particle size. Aircraft in situ measurements of cloud properties show mostly mixed-phase clouds over Barrow during the campaign, but with wide variability in relative liquid versus ice water content. At fixed total optical depth, this variability in phase composition can yield of order 5-10 Watts per square meter in surface flux variability, with greater cloud attenuation of the surface flux usually occurring under higher ice water content. Thus our data show that changes in cloud phase properties, even within the 'mixed-phase' category, can affect the surface energy balance at the same order of magnitude as greenhouse gas increases. Analysis of this spectral radiometric data provides suggestions for testing new mixed-phase parameterizations in climate models.

Understanding the onset of coalescence in warm clouds is key in our effort to improve cloud representation in numerical models. Coalescence acts at small scales, and its study requires detailed high-resolution dynamical and microphysical measurements from a comprehensive suite of instruments over a wide range of environmental conditions (e.g., aerosol loading). The first AMF is currently in its second year of a two-year deployment at Graciosa Island in the Azores, offering the opportunity to collect a long data set from a stable land-based platform in a marine stratocumulus regime. In this study, recorded WACR Doppler spectra are used to characterize the properties of Doppler spectra from warm clouds with and without drizzle, and from drizzle only, in an effort to observe the transition (onset) to precipitation in clouds. A retrieval technique that decomposes observed Doppler spectra into their cloud and/or drizzle components is applied in order to quantify drizzle growth.

The observed increase in global mean surface temperature (GMST) over the industrial era is less than 40% of that expected from observed increases in long-lived greenhouse gases together with the best-estimate equilibrium climate sensitivity given by the 2007 Assessment Report of the Intergovernmental Panel on Climate Change. Possible reasons for this warming discrepancy are systematically examined here. The warming discrepancy is found to be due mainly to some combination of two factors: the IPCC best estimate of climate sensitivity being too high and/or the greenhouse gas forcing being partially offset by forcing by increased concentrations of atmospheric aerosols; the increase in global heat content due to thermal disequilibrium accounts for less than 25% of the discrepancy, and cooling by natural temperature variation can account for only about 15%. Current uncertainty in climate sensitivity is shown to preclude determining the amount of future fossil fuel CO2 emissions that would be compatible with any chosen maximum allowable increase in GMST; even the sign of such allowable future emissions is unconstrained. Resolving this situation by empirical determination of Earth’s climate sensitivity from the historical record over the industrial period or through use of climate models whose accuracy is evaluated by their performance over …

To aid in improving model parameterizations of clouds and convection, we examine the capability of models, using explicit convection, to simulate the life cycle of tropical cloud systems in the vicinity of the ARM Tropical Western Pacific sites. The cloud life cycle is determined using a satellite cloud tracking algorithm (Boer and Ramanathan, 1997), and the statistics are compared to those of simulations using the Weather Research and Forecasting (WRF) Model. Using New York Blue, a Blue Gene/L supercomputer that is co-operated by Brookhaven and Stony Brook, simulations are run at a resolution comparable to the observations. Initial results suggest a computational paradox where, even though the size of the simulated systems are about half of that observed, their longevities are still similar. The explanation for this seeming incongruity will be explored.

Numerical weather prediction models (ECMWF, NCEP) are evaluated using ARM observational data collected at the Southern Great Plains (SGP) site. Cloud forecasts generated by the models are compared with cloud microphysical quantities, retrieved using a variety of parameterizations. Information gained from this comparison will be utilized during the FASTER project, as models are evaluated for their ability to reproduce fast physical processes detected in the observations. Here the model performance is quantified against the observations through a statistical analysis. Observations from remote sensing instruments (radar, lidar, radiometer and radiosonde) are used to derive the cloud microphysical quantities: ice water content, liquid water content, ice effective radius and liquid effective radius. Unfortunately, discrepancies in the derived quantities arise when different retrieval schemes are applied to the observations. The uncertainty inherent in retrieving the microphysical quantities using various retrievals is estimated from the range of output microphysical values. ARM microphysical retrieval schemes (Microbase, Mace) are examined along with the CloudNet retrieval processing of data from the ARM sites for this purpose. Through the interfacing of CloudNet and “ARM” processing schemes an ARMNET product is produced and employed as accepted observations in the assessment of cloud model predictions.

This poster describes the Fast Physics Testbed for the new FAst-physics System Testbed and Research (FASTER) project. The overall objective is to provide a convenient and comprehensive platform for fast turn-around model evaluation against ARM observations and to facilitate development of parameterizations for cloud-related fast processes represented in global climate models. The testbed features three major components: a single column model (SCM) testbed, an NWP-Testbed, and high-resolution modeling (HRM). The web-based SCM-Testbed features multiple SCMs from major climate modeling centers and aims to maximize the potential of SCM approach to enhance and accelerate the evaluation and improvement of fast physics parameterizations through continuous evaluation of existing and evolving models against historical as well as new/improved ARM and other complementary measurements. The NWP-Testbed aims to capitalize on the large pool of operational numerical weather prediction products. Continuous evaluations of NWP forecasts against observations at ARM sites are carried out to systematically identify the biases and skills of physical parameterizations under all weather conditions. The highresolution modeling (HRM) activities aim to simulate the fast processes at high resolution to aid in the understanding of the fast processes and their parameterizations. A four-tier HRM framework is established to augment the SCM- and NWP-Testbeds …

The use of forward models as an alternative approach to compare models with observations contains advantages and challenges. Radar Doppler spectra simulators are not new; their application in high- resolution models with bin microphysics schemes could help to compare model output with the Doppler spectra recorded from the vertically pointing cloud radars at the ARM Climate Research Facility sites. The input parameters to a Doppler spectra simulator are both microphysical (e.g., particle size, shape, phase, and number concentration) and dynamical (e.g., resolved wind components and sub-grid turbulent kinetic energy). Libraries for spherical and non-spherical particles are then used to compute the backscattering cross-section and fall velocities, while the turbulence is parameterized as a Gaussian function with a prescribed width. The Signal-to-Noise Ratio (SNR) is used to determine the amount of noise added throughout the spectrum, and the spectral smoothing due to spectral averages is included to reproduce the averaging realized by cloud radars on successive returns. Thus, realistic Doppler spectra are obtained, and several parameters that relate to the morphological characteristics of the synthetically generated spectra are computed. Here, the results are compared to the new ARM microARSCL data products in an attempt to validate the simulator. Drizzling data obtained …

The Midlatitude Continental Convective Cloud Experiment (MC3E) will take place in central Oklahoma during the April-May 2011 period. The experiment is a collaborative effort between the U.S. Department of Energy Atmospheric Radition Measurement Program and the National Aeronautics and Space Administration's (NASA) Global Precipitation Measurement (GPM) mission Ground Validation program. The Intensive Observation Period leverages the unprecedented observing infrastructure currently available in the central United States, combined with an extensive sounding array, remote sensing and in situ aircraft observations, NASA GPM ground validation remote sensors and new ARM instrumentation purchased with American Recovery and Reinvestment Act funding. The overarching goal is to provide the most complete characterization of convective cloud systems, precipitation and the environment that has ever been obtained, providing constraints for model cumulus parameterizations and space-based rainfall observations over land that have never before been available. Several different components of convective processes tangible to the convective parameterization problem are targeted such as, pre-convective environment and convective initiation, updraft / downdraft dynamics, condensate transport and detrainment, precipitation and cloud microphysics, influence on the environment and radiation and a detailed description of the large-scale forcing. MC3E will use a new multi-scale observing strategy with the participation of a network of …

As part of the federal government’s 2009 American Recovery and Reinvestment Act (ARRA), the U.S. DOE Office of Science allocated funds for the capital upgrade of the Atmospheric Radiation Measurement (ARM) Climate Research Facility to improve and expand observational capabilities related to cloud and aerosol properties. The ARM Facility was established as a national user facility for the global scientific community to conduct a wide range of interdisciplinary science. Part of the ARRA-funded expansion of the ARM Facility includes four new Aerosol Observing Systems (AOS) to be designed, instrumented, and mentored by BNL. The enclosures will be customized SeaTainers. These new platforms ([AMF2]: ARM Mobile Facility-2; [TWP-D]: Tropical Western Pacific at Darwin; and [MAOS-A]/[MAOS-C]: Mobile Aerosol Observing System-Aerosol/-Chemistry) will provide a laboratory environment for fielding instruments to collect data on aerosol life cycle, microphysics, and optical/physical properties. The extensive instrument suite includes both established methods and initial deployments of new techniques to add breadth and depth to the AOS data sets. The platforms are designed: (1) to have all instruments pre-installed before deployment, allowing a higher measurement duty cycle; (2) with a standardized configuration improving the robustness of data inter-comparability; (3) to provide remote access capability for instrument mentors; and …

The Cumulus Humilis Aerosol Processing Study (CHAPS) provided a unique opportunity to study aerosol and cloud processing. Clouds play an active role in the processing and cycling of atmospheric constituents. Gases and particles can partition to cloud droplets by absorption and condensation as well as activation and impact scavenging. The U.S. Department of Energy (DOE) G-1 aircraft was used as one of the main platforms in CHAPS. Flight tracks were designed and implemented to characterize freshly emitted aerosols at cloud top and cloud base as well as within the cloud, i.e., cumulus humilis (or fair-weather cumulus), in the vicinity of Oklahoma City. Measurements of interstitial aerosols and residuals of activated condensation cloud nuclei were conducted simultaneously. The interstitial aerosols were measured downstream of an isokinetic inlet, and the activated particles downstream of a counter-flow virtual impactor (CVI). The sampling line to the Aerodyne Aerosol Mass Spectrometer (AMS) was switched between the isokinetic inlet and the CVI to allow characterization of non-activated interstitial particles outside of clouds in contrast to particles activated in clouds. Trace gases including ozone, carbon monoxide, sulfur dioxide, and a series of volatile organic compounds (VOCs) were also measured, as were key meteorological state parameters including liquid …

Light scattering by aerosols plays an important role in Earth’s radiative balance, and quantification of this phenomenon is important in understanding and accounting for anthropogenic influences on Earth’s climate. Light scattering by an aerosol particle is determined by its radius and index of refraction, and for aerosol particles that are hygroscopic, both of these quantities vary with relative humidity RH. Here exact expressions are derived for the dependences of the radius ratio (relative to the volume-equivalent dry radius) and index of refraction on RH for aqueous solutions of single solutes. Both of these quantities depend on the apparent molal volume of the solute in solution and on the practical osmotic coefficient of the solution, which in turn depend on concentration and thus implicitly on RH. Simple but accurate approximations are also presented for the RH dependences of both radius ratio and index of refraction for several atmospherically important inorganic solutes over the entire range of RH values for which these substances can exist as solution drops. For all substances considered, the radius ratio is accurate to within a few percent, and the index of refraction to within ~0.02, over this range of RH. Such parameterizations will be useful in radiation …

A dimensionless theory for new particle formation (NPF) was developed, using an aerosol population balance model incorporating recent developments in nucleation rates and measured particle growth rates. Based on this theoretical analysis, it was shown that a dimensionless parameter Lg, characterizing the ratio of the particle scavenging loss rate to the particle growth rate, exclusively determined whether or not NPF would occur on a particular day. This parameter determines the probability that a nucleated particle will grow to a detectable size before being lost by coagulation with the pre-existing aerosol. Cluster-cluster coagulation was shown to contribute negligibly to this survival probability under conditions pertinent to the atmosphere. Data acquired during intensive measurement campaigns in Tecamac (MILAGRO), Atlanta (ANARChE), Boulder, and Hyytiala (QUEST II, QUEST IV, and EUCAARI) were used to test the validity of Lg as an NPF criterion. Measurements included aerosol size distributions down to 3 nm and gas-phase sulfuric acid concentrations. The model was applied to 77 NPF events and 19 non-events (characterized by growth of pre-existing aerosol without NPF) measured in diverse environments with broad ranges in sulfuric acid concentrations, ultrafine number concentrations, aerosol surface areas, and particle growth rates (nearly two orders of magnitude). Across this …

The influences of atmospheric aerosols on cloud properties (i.e., aerosol indirect effects) strongly depend on the aerosol CCN concentrations, which can be effectively predicted from detailed aerosol size distribution, mixing state, and chemical composition using Köhler theory. However, atmospheric aerosols are complex and heterogeneous mixtures of a large number of species that cannot be individually simulated in global or regional models due to computational constraints. Furthermore, the thermodynamic properties or even the molecular identities of many organic species present in ambient aerosols are often not known to predict their cloud-activation behavior using Köhler theory. As a result, simplified presentations of aerosol composition and mixing state are necessary for large-scale models. In this study, aerosol microphysics, CCN concentrations, and chemical composition measured at the T0 urban super-site in Mexico City during MILAGRO are analyzed. During the campaign in March 2006, aerosol size distribution and composition often showed strong diurnal variation as a result of both primary emissions and aging of aerosols through coagulation and local photochemical production of secondary aerosol species. The submicron aerosol composition was ~1/2 organic species. Closure analysis is first carried out by comparing CCN concentrations calculated from the measured aerosol size distribution, mixing state, and chemical composition …

New particle formation (NPF) in the atmospheric is a two-step process: Nucleation leads to the birth of stable nuclei that subsequently grow to sizes that can be detected and affect the atmosphere’s radiative properties. Our group is studying both of these processes. Our nucleation research is largely supported by NSF and involves measurements of neutral molecular clusters formed by nucleation with a new custom-designed mass spectrometer (the Cluster-CIMS) and measurements of nanoparticle size distributions as small as 1 nm with a new aerosol spectrometer (the DEG SMPS). These measurements are providing new insights into aspects of cluster behavior that affect nucleation rates. The U.S. DOE supports our research on nanoparticle growth rates. This research couples physical and chemical measurements of aerosol properties and behavior. The TDCIMS, which enables real-time measurements of composition for freshly nucleated particles as small as 8 nm and was developed with support from DOE, is the most important tool in this work. Our most important discoveries about processes that affect growth rates are summarized in a recent PNAS article (doi:10.1073/pnas.0912127107). In short, this work has shown that alkylammonium-carboxylate salts, formed, for example, by reactions between amines and carboxylic acids, account for 20–50% of the mass of …

The contribution of aerosol absorption on direct radiative forcing is still an active area of research, in part, because aerosol extinction is dominated by light scattering and, in part, because the primary absorbing aerosol of interest, soot, exhibits complex aging behavior that alters its optical properties. The consequences of this can be evidenced by the work of Ramanathan and Carmichael (2008) who suggest that incorporating the atmospheric heating due to brown clouds (plumes containing soot byproducts from automobiles, biomass burning, wood-burning kitchen stoves, and coal-fired power plants) will increase black carbon (BC) radiative forcing from the Intergovernmental Panel on Climate Change best estimate of 0.34 Wm-2 (±0.25 Wm-2) (IPCC 2007) to 0.9 Wm-2. This noteworthy degree of uncertainty is due largely to the interdependence of BC optical properties on particle mixing state and aggregate morphology, each of which changes as the particle ages in the atmosphere and becomes encapsulated within a coating of inorganic and/or organic substances. In July 2008, a laboratory-based measurement campaign, led by Boston College and Aerodyne, was initiated to begin addressing this interdependence. To achieve insights into the interdependence of BC optical properties on particle mixing state and aggregate morphology, measurements of both the optical and …

A cursory examination of historical ARSCL data indicates a common cloud feature in the tropics are thin detrainment shelves (Attendant Shelf Clouds, or ASCs) near the melting level (see figure for example). We use the ARSCL product to identify ASCs by defining them as cloud layers with bases above 4 km, a corresponding top below 6 km, and a thickness of less than 1 km. In order to prevent biases in determination of the diurnal cycle of cloud occurrence, we require that both the MMCR and MPL are operating well. In this study we use a total of 55 months of data collected over 14 years of deployments at the Manus, Nauru, and Darwin ARM sites in the Tropical Western Pacific to define the frequency of occurrence (~ 14% of the time) and diurnal cycle of these clouds, along with the atmospheric thermodynamic profile. We further investigate the horizontal extent, cloud radiative forcing, and cloud particle phase through a series of “golden cases” where there is a general absence of additional cloud types in the column and nearby deep convection. These cases indicate that the clouds can cover horizontal areas on the order of a GCM gridbox, have significant (but …

In order to better use the long-term ARM measurements to evaluate parameterizations of fast processes used in global climate models --- mainly those related to clouds, precipitation and aerosols, the DOE Earth System Modeling (ESM) program funds a new multi-institution project led by the Brookhaven National Laboratory, FAst -physics System Testbed and Research (FASTER). This poster will present an overview of this new project and its scientific relationships to the ASR sciences and ARM measurements.

The aim of the FAst-physics System TEstbed and Research (FASTER) project is to evaluate and improve the parameterizations of fast physics (involving clouds, precipitation, aerosol) in numerical models using ARM measurements. One objective within FASTER is to evaluate model representations of fast physics with long-term continuous cloud observations by use of an 'NWP testbed'. This approach was successful in the European Cloudnet project. NWP model data (NCEP, ECMWF, etc.) is routinely output at ARM sites, and model evaluation can potentially be achieved in quasi-real time. In this poster, we will outline our progress in the development of the NWP testbed and discuss the successful integration of ARM algorithms, such as ARSCL, with algorithms and lessons learned from Cloudnet. Preliminary results will be presented of the evaluation of the ECMWF, NCEP, and UK Met Office models over the SGP site using this approach.