3,829 research outputs found
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Design Principles for High-Capacity Mn-Based Cation-Disordered Rocksalt Cathodes
Mn-based Li-excess cation-disordered rocksalt (DRX) oxyfluorides are promising candidates for next-generation rechargeable battery cathodes owing to their large energy densities, the earth abundance, and low cost of Mn. In this work, we synthesized and electrochemically tested four representative compositions in the Li-Mn-O-F DRX chemical space with various Li and F content. While all compositions achieve higher than 200 mAh gâ1 initial capacity and good cyclability, we show that the Li-site distribution plays a more important role than the metal-redox capacity in determining the initial capacity, whereas the metal-redox capacity is more closely related to the cyclability of the materials. We apply these insights and generate a capacity map of the Li-Mn-O-F chemical space, LixMn2-xO2-yFy (1.167 †x †1.333, 0 †y †0.667), which predicts both accessible Li capacity and Mn-redox capacity. This map allows the design of compounds that balance high capacity with good cyclability
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Ultrahigh power and energy density in partially ordered lithium-ion cathode materials
The rapid market growth of rechargeable batteries requires electrode materials that combine high power and energy and are made from earth-abundant elements. Here we show that combining a partial spinel-like cation order and substantial lithium excess enables both dense and fast energy storage. Cation overstoichiometry and the resulting partial order is used to eliminate the phase transitions typical of ordered spinels and enable a larger practical capacity, while lithium excess is synergistically used with fluorine substitution to create a high lithium mobility. With this strategy, we achieved specific energies greater than 1,100 Wh kgâ1 and discharge rates up to 20 A gâ1. Remarkably, the cathode materials thus obtained from inexpensive manganese present a rare case wherein an excellent rate capability coexists with a reversible oxygen redox activity. Our work shows the potential for designing cathode materials in the vast space between fully ordered and disordered compounds
Dicarboxylic acids, ketocarboxylic acids, α-dicarbonyls, fatty acids and benzoic acid in PM2.5 aerosol collected during CAREBeijing-2007: an effect of traffic restriction on air quality
Thirty water-soluble organic species, including dicarboxylic acids, ketocarboxylic acids, α-dicarbonyls, fatty acids and benzoic acid were determined as well as organic carbon (OC), elemental carbon (EC) and water-soluble organic carbon (WSOC) in PM2.5 samples collected during the Campaign of Air Quality Research in Beijing 2007 (CAREBeijing-2007) in the urban and suburban areas of Beijing. The objective of this study is to identify the influence of traffic emissions and regional transport to the atmosphere in Beijing during summer. PM2.5 samples collected with or without traffic restriction in Beijing are selected to evaluate the effectiveness of local traffic restriction measures on air pollution reduction. The average concentrations of the total quantified bifunctional organic compounds (TQBOCs), total fatty acids and benzoic acid during the entire sampling period were 1184±241, 597±159 and 1496±511 ng mâ3 in Peking University (PKU), and 1050±303, 475±114 and 1278±372 ng mâ3 in Yufa, Beijing. Oxalic acid (C2) was found as the most abundant dicarboxylic acid at PKU and Yufa followed by phthalic acid (Ph). A strong even carbon number predominance with the highest level at stearic acid (C18:0), followed by palmitic acid (C16:0) was found for fatty acids. According to the back trajectories modeling results, the air masses were found to originate mainly from the northeast, passing over the southeast or south of Beijing (heavily populated, urbanized and industrialized areas), during heavier pollution events, whereas they are mainly from the north or northwest sector (mountain areas without serious anthropogenic pollution sources) during less pollution events. The data with wind only from the same sector (minimizing the difference from regional contribution) but with and without traffic restriction in Beijing were analyzed to evaluate the effectiveness of local traffic restriction measures on the reduction of local air pollution in Beijing. The results suggested that the traffic restriction measures can reduce the air pollutants, but the decrease of pollutants is generally smaller in Yufa compared to that in PKU. Moreover, an enhancement of EC value indicates more elevated primary emissions in Yufa during restriction periods than in non-restriction periods. This study demonstrates that even when primary exhaust was controlled by traffic restriction, the contribution of secondary organic species formed from photochemical processes was critical with long-range atmospheric transport of pollutants.published_or_final_versio
Partially linear censored quantile regression
Censored regression quantile (CRQ) methods provide a powerful and flexible approach to the analysis of censored survival data when standard linear models are felt to be appropriate. In many cases however, greater flexibility is desired to go beyond the usual multiple regression paradigm. One area of common interest is that of partially linear models: one (or more) of the explanatory covariates are assumed to act on the response through a non-linear function. Here the CRQ approach of Portnoy (J Am Stat Assoc 98:1001â1012, 2003) is extended to this partially linear setting. Basic consistency results are presented. A simulation experiment and unemployment example justify the value of the partially linear approach over methods based on the Cox proportional hazards model and on methods not permitting nonlinearity
Nonlinear response of the vacuum Rabi resonance
On the level of single atoms and photons, the coupling between atoms and the
electromagnetic field is typically very weak. By employing a cavity to confine
the field, the strength of this interaction can be increased many orders of
magnitude to a point where it dominates over any dissipative process. This
strong-coupling regime of cavity quantum electrodynamics has been reached for
real atoms in optical cavities, and for artificial atoms in circuit QED and
quantum-dot systems. A signature of strong coupling is the splitting of the
cavity transmission peak into a pair of resolvable peaks when a single resonant
atom is placed inside the cavity - an effect known as vacuum Rabi splitting.
The circuit QED architecture is ideally suited for going beyond this linear
response effect. Here, we show that increasing the drive power results in two
unique nonlinear features in the transmitted heterodyne signal: the
supersplitting of each vacuum Rabi peak into a doublet, and the appearance of
additional peaks with the characteristic sqrt(n) spacing of the Jaynes-Cummings
ladder. These constitute direct evidence for the coupling between the quantized
microwave field and the anharmonic spectrum of a superconducting qubit acting
as an artificial atom.Comment: 6 pages, 4 figures. Supplementary Material and Supplementary Movies
are available at http://www.eng.yale.edu/rslab/publications.htm
Coherent optical wavelength conversion via cavity-optomechanics
We theoretically propose and experimentally demonstrate coherent wavelength
conversion of optical photons using photon-phonon translation in a
cavity-optomechanical system. For an engineered silicon optomechanical crystal
nanocavity supporting a 4 GHz localized phonon mode, optical signals in a 1.5
MHz bandwidth are coherently converted over a 11.2 THz frequency span between
one cavity mode at wavelength 1460 nm and a second cavity mode at 1545 nm with
a 93% internal (2% external) peak efficiency. The thermal and quantum limiting
noise involved in the conversion process is also analyzed, and in terms of an
equivalent photon number signal level are found to correspond to an internal
noise level of only 6 and 4x10-3 quanta, respectively.Comment: 11 pages, 7 figures, appendi
Theory of Photon Blockade by an Optical Cavity with One Trapped Atom
In our recent paper [1], we reported observations of photon blockade by one
atom strongly coupled to an optical cavity. In support of these measurements,
here we provide an expanded discussion of the general phenomenology of photon
blockade as well as of the theoretical model and results that were presented in
Ref. [1]. We describe the general condition for photon blockade in terms of the
transmission coefficients for photon number states. For the atom-cavity system
of Ref. [1], we present the model Hamiltonian and examine the relationship of
the eigenvalues to the predicted intensity correlation function. We explore the
effect of different driving mechanisms on the photon statistics. We also
present additional corrections to the model to describe cavity birefringence
and ac-Stark shifts. [1] K. M. Birnbaum, A. Boca, R. Miller, A. D. Boozer, T.
E. Northup, and H. J. Kimble, Nature 436, 87 (2005).Comment: 10 pages, 6 figure
An ATP and Oxalate Generating Variant Tricarboxylic Acid Cycle Counters Aluminum Toxicity in Pseudomonas fluorescens
Although the tricarboxylic acid (TCA) cycle is essential in almost all aerobic organisms, its precise modulation and integration in global cellular metabolism is not fully understood. Here, we report on an alternative TCA cycle uniquely aimed at generating ATP and oxalate, two metabolites critical for the survival of Pseudomonas fluorescens. The upregulation of isocitrate lyase (ICL) and acylating glyoxylate dehydrogenase (AGODH) led to the enhanced synthesis of oxalate, a dicarboxylic acid involved in the immobilization of aluminum (Al). The increased activity of succinyl-CoA synthetase (SCS) and oxalate CoA-transferase (OCT) in the Al-stressed cells afforded an effective route to ATP synthesis from oxalyl-CoA via substrate level phosphorylation. This modified TCA cycle with diminished efficacy in NADH production and decreased CO2-evolving capacity, orchestrates the synthesis of oxalate, NADPH, and ATP, ingredients pivotal to the survival of P. fluorescens in an Al environment. The channeling of succinyl-CoA towards ATP formation may be an important function of the TCA cycle during anaerobiosis, Fe starvation and O2-limited conditions
Control of microwave signals using circuit nano-electromechanics
Waveguide resonators are crucial elements in sensitive astrophysical
detectors [1] and circuit quantum electrodynamics (cQED) [2]. Coupled to
artificial atoms in the form of superconducting qubits [3, 4], they now provide
a technologically promising and scalable platform for quantum information
processing tasks [2, 5-8]. Coupling these circuits, in situ, to other quantum
systems, such as molecules [9, 10], spin ensembles [11, 12], quantum dots [13]
or mechanical oscillators [14, 15] has been explored to realize hybrid systems
with extended functionality. Here, we couple a superconducting coplanar
waveguide resonator to a nano-coshmechanical oscillator, and demonstrate
all-microwave field controlled slowing, advancing and switching of microwave
signals. This is enabled by utilizing electromechanically induced transparency
[16-18], an effect analogous to electromagnetically induced transparency (EIT)
in atomic physics [19]. The exquisite temporal control gained over this
phenomenon provides a route towards realizing advanced protocols for storage of
both classical and quantum microwave signals [20-22], extending the toolbox of
control techniques of the microwave field.Comment: 9 figure
Kahler-Einstein metrics emerging from free fermions and statistical mechanics
We propose a statistical mechanical derivation of Kahler-Einstein metrics,
i.e. solutions to Einstein's vacuum field equations in Euclidean signature
(with a cosmological constant) on a compact Kahler manifold X. The microscopic
theory is given by a canonical free fermion gas on X whose one-particle states
are pluricanonical holomorphic sections on X (coinciding with higher spin
states in the case of a Riemann surface). A heuristic, but hopefully physically
illuminating, argument for the convergence in the thermodynamical (large N)
limit is given, based on a recent mathematically rigorous result about
exponentially small fluctuations of Slater determinants. Relations to effective
bosonization and the Yau-Tian-Donaldson program in Kahler geometry are pointed
out. The precise mathematical details will be investigated elsewhere.Comment: v1: 22 pages v2: 25 pages. The relation to quantum gravity has been
further developed by working over the moduli space of all complex structures.
Relations to Donaldson's program pointed out. References adde
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