The past ∼10 years have witnessed revolutionary breakthroughs both in synthesis of quantum dots (leading to nearly monodispersed, defect-free nanostructures) and in characterization of such systems, ...revealing ultra narrow spectroscopic lines of <1 meV width, exposing new intriguing effects, such as multiple exciton generation, fine-structure splitting, quantum entanglement, multiexciton recombination and more. These discoveries have led to new technological applications including quantum computing and ultra-high efficiency solar cells. Our work in this project is based on two realizations/observations: First, that the dots exhibiting clean and rich spectroscopic and transport characteristics are rather big. Indeed, the phenomenology indicated above is exhibited only by the well-passivated defect-free quantum dots containing at least a few thousand atoms (colloidal) and even a few hundred thousand atoms (self assembled). Understanding the behavior of nanotechnology devices requires the study of even larger, million-atom systems composed of multiple components such as wires+dots+films. Second, first-principles many-body computational techniques based on current approaches (Quantum Monte-Carlo, GW, Bethe-Salpeter) are unlikely to be adaptable to such large structures and, at the same time, the effective mass-based techniques are too crude to provide insights on the many-body/atomistic phenomenology revealed by experiment. Thus, we have developed a set of methods that use an atomistic approach (unlike effective-mass based techniques) and utilize single-particle + many body techniques that are readily scalable to ∼103−106 atom nanostructures. New mathematical and computational techniques have also been developed to accelerate our calculations and go beyond simple conjugate gradient based methods allowing us to study larger systems. In this short paper based on a poster presented at the DOE SciDAC06 conference we will present the overall structure as well as highlights of our computational nanoscience project.
We present results for applications to nanosystems of state-of-the-art iterative eigensolvers based on conjugate gradients and variants of Davidson in the context of semi-empirical plane wave ...electronic structure calculations. We are concerned with the computation of electronic and optical properties of nanosystems using the Energy SCAN method to compute interior eigenstates around the band gap that determine their properties. Numerically, this interior Hermitian eigenvalue problem poses several challenges, with respect to both accuracy and efficiency. All the iterative eigensolvers are seeking the minimal eigenvalues of the folded operator with reference shift in the band-gap. The tested methods include standard conjugate-gradient (CG)-based Rayleigh quotient minimization, Locally optimal block-preconditioned CG (LOBPCG) and two variants of the (Jacobi-)Davidson method: JDQMR and GD+1. Our experimental results indicated that Davidson-type methods are often the fastest.
Starting from the bio-based platform chemicals 5-hydroxymethylfurfural (HMF) and furfural, a library of anionic surfactants was synthesized using stoichiometric and catalytic reactions. In total, ...seven different surfactants with varying chain lengths were prepared and tested for industrially relevant properties, such as critical micelle concentration (CMC) and interfacial tension towards isopropyl myristate. Surfactants based on 2,5-bis(hydroxymethyl)-tetrahydrofuran (BHMTHF), which are accessible
via
acid-catalysis over zeolites, were identified as the most promising candidates for possible industrial applications. Variants with chain lengths of C
12
-C
14
showed the best results in terms of physico-chemical properties. These lengths represent the usually occurring length of carbon chains in natural oils, opening up a pathway for a possible production of the here used substrates. The other synthesized surfactants, accessible
via
stoichiometric routes, also showed promising results in terms of CMC and interfacial tension.
Starting from the bio-based platform chemicals 5-hydroxymethylfurfural (HMF) and furfural, a library of anionic surfactants was synthesized using stoichiometric and catalytic reactions.
REFERENCE UPPER-AIR OBSERVATIONS FOR CLIMATE Bodeker, G. E.; Bojinski, S.; Cimini, D. ...
Bulletin of the American Meteorological Society,
01/2016, Letnik:
97, Številka:
1
Journal Article
Recenzirano
Odprti dostop
The three main objectives of the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) are to provide long-term high-quality climate records of vertical profiles of selected ...essential climate variables (ECVs), to constrain and calibrate data from more spatially comprehensive global networks, and to provide measurements for process studies that permit an in-depth understanding of the properties of the atmospheric column. In the five years since the first GRUAN implementation and coordination meeting and the printing of an article (Seidel et al.) in this publication, GRUAN has matured to become a functioning network that provides reference-quality observations to a community of users.
This article describes the achievements within GRUAN over the past five years toward making reference-quality observations of upper-air ECVs. Milestones in the evolution of GRUAN are emphasized, including development of rigorous criteria for site certification and assessment, the formal certification of the first GRUAN sites, salient aspects of the GRUAN manual and guide to operations, public availability of GRUAN’s first data product, outcomes of a network expansion workshop, and key results of scientific studies designed to provide a sound scientific foundation for GRUAN operations.
Two defining attributes of GRUAN are 1) that every measurement is accompanied by a traceable estimate of the measurement uncertainty and 2) that data quality and continuity are maximized because network changes are minimized and managed. This article summarizes how these imperatives are being achieved for existing and planned data products and provides an outlook for the future, including expected new data streams, network expansion, and critical needs for the ongoing success of GRUAN.
Celotno besedilo
Dostopno za:
BFBNIB, DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
We present a method of identifying the tropical tropopause transition layer (TTL) using chemical tracer‐tracer relationships. Coincident ozone (O3) and water vapor (H2O) measurements over Alajuela, ...Costa Rica (~10°N), in July and August 2007 are used to demonstrate the concept. In the tracer‐tracer space, the O3 and H2O relationship helps to separate the transition layer air mass from the background troposphere and stratosphere. This tracer relationship‐based transition layer is found to span an approximately 40 K potential temperature range between 340 and 380 K and is largely confined between the level of minimum stability (LMS) and the cold point tropopause (CPT). This chemical composition‐based transition layer is, therefore, consistent with a definition of the TTL based on the thermal structure, for which the LMS and CPT are the lower and upper boundaries of TTL, respectively. We also examine the transition layer over the region of Asian summer monsoon (ASM) anticyclone using the measurements over Kunming, China (~25°N), and compare its behavior with the TTL structure in the deep tropics. The comparison shows that the transition layer over the ASM is similar to the TTL, although the data suggest the ASM transition layer lies at higher potential temperature levels and is potentially prone to the influence of extratropical processes.
Key Points
The TTL is identified using the ozone and water vapor relationship
The tracer TTL is consistent with the CPT and LMS as upper and lower boundaries
The transition layer in the Asian monsoon region is compared to the TTL
Nitric acid trihydrate (NAT) particles in the polar stratosphere have been shown to be responsible for vertical redistribution of reactive nitrogen (NOy). Recent observations by Cloud–Aerosol Lidar ...with Orthogonal Polarization (CALIOP) aboard the CALIPSO satellite have been explained in terms of heterogeneous nucleation of NAT on foreign nuclei, revealing this to be an important formation pathway for the NAT particles. In state of the art global- or regional-scale models, heterogeneous NAT nucleation is currently simulated in a very coarse manner using a constant, saturation-independent nucleation rate. Here we present first simulations for the Arctic winter 2009/2010 applying a new saturation-dependent parametrisation of heterogeneous NAT nucleation rates within the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulation shows good agreement of chemical trace species with in situ and remote sensing observations. The simulated polar stratospheric cloud (PSC) optical properties agree much better with CALIOP observations than those simulated with a constant nucleation rate model. A comparison of the simulated particle size distributions with observations made using the Forward Scattering Spectrometer Probe (FSSP) aboard the high altitude research aircraft Geophysica, shows that the model reproduces the observed size distribution, except for the very largest particles above 15 μm diameter. The vertical NOy redistribution caused by the sedimentation of the NAT particles, in particular the denitrification and nitrification signals observed by the ACE-FTS satellite instrument and the in situ SIOUX instrument aboard the Geophysica, are reproduced by the improved model, and a small improvement with respect to the constant nucleation rate model is found.
Here we present extensive observations of stratospheric and upper tropospheric water vapor using the balloon‐borne Cryogenic Frost point Hygrometer (CFH) in support of the Aura Microwave Limb Sounder ...(MLS) satellite instrument. Coincident measurements were used for the validation of MLS version 1.5 and for a limited validation of MLS version 2.2 water vapor. The sensitivity of MLS is on average 30% lower than that of CFH, which is fully compensated by a constant offset at stratospheric levels but only partially compensated at tropospheric levels, leading to an upper tropospheric dry bias. The sensitivity of MLS observations may be adjusted using the correlation parameters provided here. For version 1.5 stratospheric observations at pressures of 68 hPa and smaller MLS retrievals and CFH in situ observations agree on average to within 2.3% ± 11.8%. At 100 hPa the agreement is to within 6.4% ± 22% and at upper tropospheric pressures to within 23% ± 37%. In the tropical stratosphere during the boreal winter the agreement is not as good. The “tape recorder” amplitude in MLS observations depends on the vertical profile of water vapor mixing ratio and shows a significant interannual variation. The agreement between stratospheric observations by MLS version 2.2 and CFH is comparable to the agreement using MLS version 1.5. The variability in the difference between observations by MLS version 2.2 and CFH at tropospheric levels is significantly reduced, but a tropospheric dry bias and a reduced sensitivity remain in this version. In the validation data set a dry bias at 177.8 hPa of −24.1% ± 16.0% is statistically significant.
The AquaVIT-1 intercomparison of atmospheric water vapor measurement techniques was conducted at the aerosol and cloud simulation chamber AIDA (Aerosol Interaction and Dynamics in the Atmosphere) at ...the Karlsruhe Institute of Technology, Germany, in October 2007. The overall objective was to intercompare state-of-the-art and prototype atmospheric hygrometers with each other and with independent humidity standards under controlled conditions. This activity was conducted as a blind intercomparison with coordination by selected referees. The effort was motivated by persistent discrepancies found in atmospheric measurements involving multiple instruments operating on research aircraft and balloon platforms, particularly in the upper troposphere and lower stratosphere, where water vapor reaches its lowest atmospheric values (less than 10 ppm). With the AIDA chamber volume of 84 m3, multiple instruments analyzed air with a common water vapor mixing ratio, by extracting air into instrument flow systems, by locating instruments inside the chamber, or by sampling the chamber volume optically. The intercomparison was successfully conducted over 10 days during which pressure, temperature, and mixing ratio were systematically varied (50 to 500 hPa, 185 to 243 K, and 0.3 to 152 ppm). In the absence of an accepted reference instrument, the absolute accuracy of the instruments was not established. To evaluate the intercomparison, the reference value was taken to be the ensemble mean of a core subset of the measurements. For these core instruments, the agreement between 10 and 150 ppm of water vapor is considered good with variation about the reference value of about ±10% (±1σ). In the region of most interest between 1 and 10 ppm, the core subset agreement is fair with variation about the reference value of ±20% (±1σ). The upper limit of precision was also derived for each instrument from the reported data. The implication for atmospheric measurements is that the substantially larger differences observed during in-flight intercomparisons stem from other factors associated with the moving platforms or the non-laboratory environment. The success of AquaVIT-1 provides a template for future intercomparison efforts with water vapor or other species that are focused on improving the analytical quality of atmospheric measurements on moving platforms.
We compare Tropospheric Emission Spectrometer (TES) version 2 (V002) nadir ozone profiles with ozonesonde profiles from the Intercontinental Chemical Transport Experiment Ozonesonde Network Study, ...the World Ozone and Ultraviolet Data Center, the Global Monitoring Division of the Earth System Research Laboratory, and the Southern Hemisphere Additional Ozonesonde archives. Approximately 1600 coincidences spanning 72.5°S–80.3°N from October 2004 to October 2006 are found. The TES averaging kernel and constraint are applied to the ozonesonde data to account for the TES measurement sensitivity and vertical resolution. TES sonde differences are examined in six latitude zones after excluding profiles with thick high clouds. Values for the bias and standard deviation are determined using correlations of mean values of TES ozone and sonde ozone in the upper troposphere (UT) and lower troposphere (LT). The UT biases range from 2.9 to 10.6 ppbv, and the LT biases range from 3.7 to 9.2 ppbv, excluding the Arctic and Antarctic LT where TES sensitivity is low. A similar approach is used to assess seasonal differences in the northern midlatitudes where the density and frequency of sonde measurements are greatest. These results are briefly compared to TES V001 ozone validation work which also used ozonesondes but was carried out prior to improvements in the radiometric calibration and ozone retrieval in V002. Overall, the large number of TES and sonde comparisons indicate a positive bias of approximately 3–10 ppbv for the TES V002 nadir ozone data set and have helped to identify areas of potential improvement for future retrieval versions.
Acquiring accurate measurements of water vapor at the low mixing ratios (< 10 ppm) encountered in the upper troposphere and lower stratosphere (UT/LS) has proven to be a significant analytical ...challenge evidenced by persistent disagreements between high‐precision hygrometers. These disagreements have caused uncertainties in the description of the physical processes controlling dehydration of air in the tropical tropopause layer and entry of water into the stratosphere and have hindered validation of satellite water vapor retrievals. A 2011 airborne intercomparison of a large group of in situ hygrometers onboard the NASA WB‐57F high‐altitude research aircraft and balloons has provided an excellent opportunity to evaluate progress in the scientific community toward improved measurement agreement. In this work we intercompare the measurements from the Midlatitude Airborne Cirrus Properties Experiment (MACPEX) and discuss the quality of agreement. Differences between values reported by the instruments were reduced in comparison to some prior campaigns but were nonnegligible and on the order of 20% (0.8 ppm). Our analysis suggests that unrecognized errors in the quantification of instrumental background for some or all of the hygrometers are a likely cause. Until these errors are understood, differences at this level will continue to somewhat limit our understanding of cirrus microphysical processes and dehydration in the tropical tropopause layer.
Key Points
Agreement among in situ measurements of UT/LS water vapor is improved
Scientifically significant disagreements between instruments still exist
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