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At least 163 records · Page 9

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DOE OSTI2024

Spatially Resolved Near Field Spectroscopy of Vibrational Polaritons at the Small N Limit

Vibrational polaritons, which have been primarily studied in Fabry–Pérot cavities with a large number of molecules (N ~ 10 6 –10 10 ) coupled to the resonator mode, exhibit various experimentally observed effects on chemical reactions. However, the exact mechanism is elusively understood from the theoretical side, as the large number of molecules involved in an experimental strong coupling condition cannot be represented completely in simulations. This discrepancy between theory and experiment arises from computational descriptions of polariton systems typically being limited to only a few molecules, thus failing to represent the experimental conditions adequately. To address this mismatch, we used surface phonon polariton (SPhP) resonators as an alternative platform for vibrational strong coupling. SPhPs exhibit strong electromagnetic confinement on the surface and thus allow for coupling to a small number of molecules. As a result, this platform can enhance nonlinearity and slow down relaxation to the dark modes. In this study, we fabricated a pillar-shaped quartz resonator and then coated it with a thin layer of cobalt phthalocyanine (CoPc). By employing scattering-type scanning near-field optical microscopy (s-SNOM), we spatially investigated the dependency of vibrational strong coupling on the spatially varying electromagnetic field strength and demonstrated strong coupling with 38,000 molecules only–reaching to the small N limit. Through s-SNOM analysis, we found that strong coupling was observed primarily on the edge of the quartz pillar and the apex of the s-SNOM tip, where the maximum field enhancement occurs. In contrast, a weak resonance signal and lack of coupling were observed closer to the center of the pillar. This work demonstrates the importance of spatially resolved polariton systems in nanophotonic platforms and lays a foundation to explore polariton chemistry and chemical dynamics at the small N limit–one step closer to reconcile with high-level quantum calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

The Liquid Jet Endstation for Hard X-ray Scattering and Spectroscopy at the Linac Coherent Light Source

The ability to study chemical dynamics on ultrafast timescales has greatly advanced with the introduction of X-ray free electron lasers (XFELs) providing short pulses of intense X-rays tailored to probe atomic structure and electronic configuration. Fully exploiting the full potential of XFELs requires specialized experimental endstations along with the development of techniques and methods to successfully carry out experiments. The liquid jet endstation (LJE) at the Linac Coherent Light Source (LCLS) has been developed to study photochemistry and biochemistry in solution systems using a combination of X-ray solution scattering (XSS), X-ray absorption spectroscopy (XAS), and X-ray emission spectroscopy (XES). The pump–probe setup utilizes an optical laser to excite the sample, which is subsequently probed by a hard X-ray pulse to resolve structural and electronic dynamics at their intrinsic femtosecond timescales. The LJE ensures reliable sample delivery to the X-ray interaction point via various liquid jets, enabling rapid replenishment of thin samples with millimolar concentrations and low sample volumes at the 120 Hz repetition rate of the LCLS beam. This paper provides a detailed description of the LJE design and of the techniques it enables, with an emphasis on the diagnostics required for real-time monitoring of the liquid jet and on the spatiotemporal overlap methods used to optimize the signal. Additionally, various scientific examples are discussed, highlighting the versatility of the LJE.

EXAFS↗

NASA NTRS1972

Stability of the Martian atmosphere

A detailed chemical dynamic model is presented for a moist Martian atmosphere. Recombination of CO2 is catalyzed by trace amount of H2O. The abundances of CO and O2 should vary in response to changes in atmospheric H2O and atmospheric mixing.

Mcelroy, M. B.↗

NASA NTRS1975

Stratospheric ozone destruction by aircraft-induced nitrogen oxides

The preliminary results from a three-dimensional dynamic-chemical model applied to the SST-NOx (NO + NO2) problem are reported. Simulations indicate that a depletion of about 12 per cent in total stratospheric O3 would be realized for a continuous NOx injection rate of 1.8 x 10 to the sixth power metric tons per year from a hypothetical fleet of SST's flying at an altitude of 20 km in the midlatitudes of the Northern Hemisphere. Sixteen per cent of the existing O3 would be destroyed on an annual basis. The model assumes a fleet of about 500 aircraft of the now-canceled American Boeing 2707 type; if only present Anglo-French and Russian SST models, which fly at lower, less harmful altitudes, are built, it will take a fleet of a few thousand such craft to attain an effective injection rate equal to the one above.

Alyea, F. N.↗

NASA NTRS1975

Phosphine on Jupiter and implications for the Great Red Spot

A study of the chemistry and photochemistry of the recently discovered phosphine in the atmosphere of Jupiter suggests that the red colorations on this planet result from photochemical production of red phosphorus particles. Chemical-dynamical models of this red phosphorus haze imply that the intensity of the red coloration is a strong function of the strength of vertical turbulent mixing in the atmosphere. If the Jovian Great Red Spot is a region of considerable dynamical activity our model provides a self-consistent explanation for the redness of this region in comparison to the rest of the planet.

Prinn, R. G.↗

NASA NTRS1978

Photochemistry and dynamics of the ozone layer

The paper presents a broad review of the photochemical and dynamic theories of the ozone layer. The two theories are combined into the MIT three-dimensional dynamic-chemical quasi-geostrophic model with 26 levels in the vertical spaced in logarithmic pressure coordinates between the ground and 72-km altitude. The chemical scheme incorporates the important odd nitrogen, odd hydrogen, and odd oxygen chemistry, but is simplified in the sense that it requires specification of the distributions of NO2, OH and HO2. The prognostic equations are the vorticity equation, the perturbation thermodynamic equation, and the global mean and perturbation continuity equations for ozone; diagnostic equations include the hydrostatic equation, the balance condition, and the mass continuity equation. The model is applied to the investigation of the impact of supersonic aircraft on the ozone layer.

Prinn, R. G.↗

NASA NTRS1978

On the coupled nature of atmospheric phenomena

The interactions that take place in the stratosphere and the troposphere which are important to the maintenance of the chemical, dynamic, and thermal state and of the middle atmosphere, and which may be important in the determination of the state of the lower atmosphere are reviewed. Examples of these interactions due to either natural or anthropogenic processes are discussed, and promising areas for future research are indicated. Specific topics include: (1) coupling between temperature and chemistry via temperature dependent rate constants; (2) the effect of latitudinal temperature variations on zonal winds; (3) the effect of clouds, surface albedo, and the lower atmosphere on stratospheric chemistry due to the scattering and reflection of solar radiation; (4) the effect of trace constituents on thermal structure and thermal balance; (5) the effect of the stratosphere on tropospheric climate; (6) the effect of solar UV variability on stratospheric chemistry and temperature; and (7) the effect of trace constituents on stratospheric dynamics.

Callis, L. B.↗

NASA NTRS1979

Middle atmosphere processes revealed by satellite observations

The present paper deals with satellite measurements carried out over the past decade, which include radiance measurements (closely associated with temperatures in the lower stratosphere), temperature measurements in the mesopause, and ozone distributions. Some information obtained from satellite data on chemical, dynamical, energy-balance, and transport processes is reviewed, and data suitable for testing dynamical and photochemical theories are noted.

Gille, J. C.↗

NASA NTRS1984

The zonally averaged circulation, temperature, and compositional structure of the lower thermosphere and variations with geomagnetic activity

A zonally averaged chemical-dynamical model of the thermosphere is used to examine the effect of high-latitude particle and Joule heating on the neutral composition, temperature, and winds at solstice for solar minimum conditions. The meridional circulation forced by solar heating alone is a summer-to-winter flow, with a winter enhancement in atomic oxygen. The high-latitude heat sources drive mean circulation cells that reinforce the solar-driven circulation in the summer hemisphere and oppose this circulation in the winter hemisphere. The changes in wind and temperature caused by the high-latitude heat sources increase the relative concentration of N2 and O2 in the high-latitude upper thermosphere and decrease the O concentration in the high-latitude lower thermosphere. For prolonged moderate levels of geomagnetic activity the peak atomic oxygen density in the polar regions can decrease by factors of 2-3 from geomagnetic quiet conditions.

Roble, R. G.↗

NASA NTRS1986

Evolution of primoridal gas clouds

The dynamical, chemical, and thermal evolution of zero-metal gas clouds was modeled to study conditions of star formation in the early universe. Numerical results are given for the collapse of spherical clouds of mass 1000 and 50000 solar mass. Cooling by H2 lines and by photons emitted in H + e(-) yields H(-) = h (sup nu) maintains collapse until formation of an equilibrium protostellar core of mass 0.02 solar mass. The cooling by photons produced with H is essential for low mass star formation. If the cloud is fragmented, the evolution of the pieces is similar to that of the parent cloud, but the equilibrium core has larger density and mass.

Bodenheimer, P. H.↗

NASA NTRS1987

Chemical evolution of molecular clouds

The principles behind the coupled chemical-dynamical evolution of molecular clouds are described. Particular attention is given to current problems involving the simplest species (i.e., C. CO, O2, and H2) in quiescent clouds. The results of a comparison made between the molecular abundances in the Orion ridge and the hot core (Blake, 1986) are presented.

Prasad, Sheo S.↗

NASA NTRS1990

Carbon deposition model for oxygen-hydrocarbon combustion. Task 6: Data analysis and formulation of an empirical model

The formation and deposition of carbon (soot) was studied in the Carbon Deposition Model for Oxygen-Hydrocarbon Combustion Program. An empirical, 1-D model for predicting soot formation and deposition in LO2/hydrocarbon gas generators/preburners was derived. The experimental data required to anchor the model were identified and a test program to obtain the data was defined. In support of the model development, cold flow mixing experiments using a high injection density injector were performed. The purpose of this investigation was to advance the state-of-the-art in LO2/hydrocarbon gas generator design by developing a reliable engineering model of gas generator operation. The model was formulated to account for the influences of fluid dynamics, chemical kinetics, and gas generator hardware design on soot formation and deposition.

Makel, Darby B.↗

NASA NTRS1989

Global three-dimensional model calculations of the budgets and present-day atmospheric lifetimes of CF2ClCFCl2 (CFC-113) and CHClF2 (CFC-22)

The annual percentage increases in concentrations of the chlorofluorocarbons CFC-113 (an industrial solvent) and CFC-22 (a refrigerant) are the highest among major chlorofluorocarbons in the atmosphere today. The present-day atmospheric lifetimes for these species are computed using a global three-dimensional dynamical-chemical model. The present-day lifetimes of both are long (15.5 years for CFC-22 and 136 or 195 years for CFC-113, depending on assumed O2 absorption cross sections), underscoring the need to decrease their emissions in order to minimize their future role in ozone destruction and greenhouse warming.

Golombek, Amram↗

NASA NTRS1990

Measurements of total reactive nitrogen during the Airborne Arctic Stratospheric Expedition

Composite distributions of measured total reactive nitrogen NO(y), from the NASA ER-2 during the Airborne Arctic Stratospheric Expedition are presented. The observed features of these distributions are discussed in terms of the controlling dynamical, chemical and microphysical processes. In the latitudinal profile from 58 deg N to within about 4 deg poleward of the polar vortex boundary, NO(y) conforms closely to predictions of NO(y) based on N2O measurements. Poleward of 5 deg of latitude within the boundary, the average NO(y) decreases sharply and is significantly lower than that predicted from N2O. This feature is consistent with loss of NO(y) through sedimentation of particles containing NO(y) in polar stratospheric clouds.

Kawa, S. R.↗

NASA NTRS1994

Three-dimensional modelling of trace species in the Arctic lower stratosphere

A three-dimensional radiative-dynamical-chemical model has been developed and used to study some aspects of modeling the polar lower stratosphere. The model includes a comprehensive gas-phase chemistry scheme as well as a treatment of heterogeneous reactions occurring on the surface of polar stratospheric clouds. Tracer transport is treated by an accurate, nondispersive scheme with little diffusion suited to the representation of strong gradients. Results from a model simulation of early February 1990 are presented and used to illustrate the importance of the model transport scheme. The model simulation is also used to examine the potential for Arctic ozone destruction and the relative contributions of the chemical cycles responsible.

Chipperfield, Martyn↗

NASA NTRS1994

Report on concentrations, lifetimes, and trends of CFCs, halons, and related species

The atmospheric lifetimes of molecules containing chlorine and bromine are the dominant parameters influencing their ability to promote enhanced ozone destruction in the stratosphere. The purpose of this report is to assess the present state of knowledge of the lifetimes of halocarbons using two complementary approaches. First, a time series of measurements of gas concentrations is used together with information on their emissions histories and a computational model of atmospheric circulation and chemistry to infer lifetimes through a mass balance approach. Second, an atmospheric chemical-dynamical model is used with detailed information on the chemistry and spectroscopy of the molecules of interest to calculate lifetimes. The lifetimes determined by these two methods are then compared. Attention is focused most closely on fully halogenated chlorine- and bromine-containing molecules, primarily the chlorofluorocarbons, and the halons, because of their ability to deliver chlorine and bromine to the stratosphere. Some attention will be given to those molecules containing hydrogen, which are subject to removal in the troposphere primarily by reaction with OH and by other processes.

Kaye, J. A.↗

NASA NTRS1994

NASA atmospheric effects of aviation projects: Status and plans

NASA's Atmospheric Effects of Aviation Project is developing a scientific basis for assessment of the atmospheric impact of subsonic and supersonic aviation. Issues addressed include predicted ozone changes and climatic impact, and related uncertainties. A primary goal is to assist assessments of United Nations scientific organizations and, hence, consideration of emission standards by the International Civil Aviation Organization. Project focus is on simulation of atmospheric processes by computer models, but studies of aircraft operations, laboratory studies, and remote and in situ observations of chemical, dynamic, and radiative processes are also included.

Wesoky, Howard L.↗

NASA NTRS1994

NLC-91: An experimental study of the polar summer mesosphere

In the summer of 1991, a major scientific campaign (NLC-91) involving 31 rocket flights was conducted from ESRANGE, Kiruna, Sweden and from Heiss Island, Russia to investigate the chemical, dynamical, and electrodynamical properties of the polar summer mesosphere. The rocket flights were also coordinated with two coherent radar facilities, EISCAT (European Incoherent Scatter Scientific Association) and CUPRI (Cornell University Portable Radar Instrument), as well as other ground facilities, to provide continual monitoring of the mesosphere by remote sensing techniques. The primary objectives of the campaign were to study noctilucent clouds (NLC's) and polar mesospheric summer echoes (PMSE's), including their possible relationship to local aerosols and/or small scale turbulence. The program involved scientific participation from eight countries, and promises to produce many results during the next few years. This overview considers the scientific campaign and briefly discusses preliminary results. These results are provided in more detail in papers following this overview.

Goldberg, R. A.↗