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1.
The 362.156 GHz absorption spectrum of H2O2 in the Mars atmosphere was observed on September 4 of 2003, employing the James Clerk Maxwell Telescope (JCMT) sub-millimeter facility on Mauna Kea, Hawaii. Radiative transfer analysis of this line absorption yields an average volume mixing ratio of 18±0.4 ppbv within the lower (0-30 km) Mars atmosphere, in general accordance with standard photochemical models (e.g., Nair et al., 1994, Icarus 111, 124-150). Our derived H2O2 abundance is roughly three times greater than the upper limit retrieved by Encrenaz et al. (2002, Astron. Astrophys. 396, 1037-1044) from infrared spectroscopy, although part of this discrepancy may result from the different solar longitudes (Ls) of observation. Aphelion-to-perihelion thermal forcing of the global Mars hygropause generates substantial (>200%) increases in HOx abundances above ∼10 km altitudes between the Ls=112° period of the Encrenaz et al. upper limit measurement and the current Ls=250° period of detection (Clancy and Nair, 1996, J. Geophys. Res. 101, 12785-12590). The observed H2O2 line absorption weakens arguments for non-standard homogeneous (Encrenaz et al., 2002, Astron. Astrophys. 396, 1037-1044) or heterogeneous (Krasnopolsky, 2003a, J. Geophys. Res. 108; 2003b, Icarus 165, 315-325) chemistry, which have been advocated partly on the basis of infrared (8 μm) non-detections for Mars H2O2. Observation of Mars H2O2 also represents the first measurement of a key catalytic specie in a planetary atmosphere other than our own. 相似文献
2.
A sequential fractionation procedure employing a series of selected mild organic solvents of different polarity has been applied for the isolation of chemically different organic fractions from a brown coal humic acid. Elemental composition, molecular weight distribution, i.r. and electron spin resonance analysis were carried out on the isolated humic fractions. They were characterized by: (a) a low polydispersity, (b) a decreasing aliphatic and increasing aromatic character along the series, (c) very different molecular weight which significantly correlated with E4/E6 ratios (particle aggregation and molecular association) and free radical concentrations (chemical and biochemical activity). Significant correlations were found between physico-chemical parameters of the isolated humic fractions, i.e. Mn, Mw, E4/E6 ratios, spins/g contents and the dielectric constants of the solvents used. This suggested the efficiency of the applied procedure in isolating chemically different organic fractions from the bulk, original humic acid. 相似文献
3.
First measurements of SO2 and SO in the Venus mesosphere (70-100 km) are reported. This altitude range is distinctly above the ∼60-70 km range to which nadir-sounding IR and UV investigations are sensitive. Since July 2004, use of ground-based sub-mm spectroscopy has yielded multiple discoveries. Abundance of each molecule varies strongly on many timescales over the entire sub-Earth Venus hemisphere. Diurnal behavior is evident, with more SO2, and less SO, at night than during the day. Non-diurnal variability is also present, with measured SO2 and SO abundances each changing by up to 2× or more between observations conducted on different dates, but at fixed phase, hence identical sub-Earth Venus local times. Change as large and rapid as a 5σ doubling of SO on a one-week timescale is seen. The sum of SO2 and SO abundances varies by an order of magnitude or more, indicating at least one additional sulfur reservoir must be present, and that it must function as both a sink and source for these molecules. The ratio SO2/SO varies by nearly two orders of magnitude, with both diurnal and non-diurnal components. In contrast to the strong time dependence of molecular abundances, their altitude distributions are temporally invariant, with far more SO2 and SO at 85-100 km than at 70-85 km. The observed increase of SO2 mixing ratio with altitude requires that the primary SO2 source be upper mesospheric photochemistry, contrary to atmospheric models which assert upward transport as the only source of above-cloud SO2. Abundance of upper mesospheric aerosol, with assumption that it is composed primarily of sulfuric acid, is at least sufficient to provide the maximum gas phase (SO + SO2) sulfur reported in this study. Sulfate aerosol is thus a plausible source of upper mesospheric SO2. 相似文献
4.
Sub-millimeter 12CO (346 GHz) and 13CO (330 GHz) line absorptions, formed in the mesosphere and lower thermosphere of Venus (70–120 km), have been mapped across the nightside Venus disk during 2001–2009 inferior conjunctions, employing the James Clerk Maxwell Telescope (JCMT). Radiative transfer analysis of these thermal line absorptions supports temperature and CO mixing profile retrievals, as well as Doppler wind fields (described in the companion paper, Clancy et al., 2012). Temporal sampling over the hourly, daily, weekly and interannual timescales was obtained over 2001–2009. On timescales inferred as several weeks, we observe changes between very distinctive CO and temperature nightside distributions. Retrieved nightside CO, temperature distributions for January 2006 and August 2007 observations display strong local time, latitudinal gradients consistent with early morning (2–3 am), low-to-mid latitude (0–40NS) peaks of 100–200% in CO and 20–30 K in temperature. The temperature increases are most pronounced above 100 km altitudes, whereas CO variations extend from 105 km (top altitude of retrieval) down to below 80 km in the mesosphere. In contrast, the 2004 and 2009 periods of observation display modest temperature (5–10 K) and CO (30–60%) increases, that are centered on antisolar (midnight) local times and equatorial latitudes. Doppler wind derived global (zonal and should be SSAS) circulations from the same data do not exhibit variations correlated with these CO, temperature short-term variations. However, large-scale residual wind fields not fit by the zonal, SSAS circulations are observed in concert with the strong temperature, CO gradients observed in 2006 and 2007 (Clancy et al., 2010). These short term variations in nightside CO, temperature distributions may also be related to observed nightside variations in O2 airglow (Hueso, H., Sánchez-Lavega, A., Piccioni, G., Drossart, P., Gérard, J.C., Khatuntsev, I., Zasova, L., Migliorini, A. [2008]. J. Geophys. Res. 113, E00B02. doi:10.1029/2008JE003081) and upper mesospheric SO and SO2 layers (Sandor, B.J., Clancy, R.T., Moriarty-Schieven, G.H., Mills, F.P. [2010]. Icarus 208, 49–60).The retrieved temperature profiles also exhibit 20 K long-term (2001–2009) variations in nightside (whole disk) average mesospheric (80–95 km) temperatures, similar to 1982–1991 variations identified in previous millimeter CO line observations (Clancy et al., 1991). Global average diurnal variations in lower thermospheric temperatures and mesospheric CO abundances decreased by a factor-of-two between 2000–2002 versus 2007–2009 periods of combined dayside and nightside observations. The infrequency and still limited temporal extent of the observations make it difficult to assign specific timescales to such longer term variations, which may be associated with longer term variations observed for cloud top SO2 (Esposito, L.W., Bertaux, J.-L., Krasnopolsky, V., Moroz, V.I., Zasova, L.V. [1997]. Chemistry of lower atmosphere and clouds. In: Bougher, S.W., Hunten, D.M., Phillips, R.J. (Eds.), VENUS II, 1362pp) and mesospheric water vapor (Sandor, B.J., Clancy, R.T. [2005]. Icarus 177, 129–143) abundances. 相似文献
5.
The Venus mesosphere constitutes a highly variable transition region between the zonal rotation of the lower atmosphere and the diurnal circulation of the upper atmosphere. It further serves as the primary photochemical region of the Venus atmosphere. We obtained James Clerk Maxwell Telescope (JCMT, Mauna Kea Hawaii) sub-millimeter line observations of mesospheric 12CO and 13CO during coordinated space (MESSENGER and Venus Express) and ground-based observations of Venus in June of 2007. Such CO spectra line measurements support temperature, CO mixing ratio, and wind retrievals over the 80-110 km altitude range, encompassing the upper mesosphere and lower thermosphere of Venus. Five-point beam integrations were obtained across the observed Venus disk, allowing distinction of afternoon (noon to 6 p.m.) versus evening (6 p.m. to midnight) local times and northern (0-60N) versus southern (0-60S) latitudes. Distinctive diurnal variations (noon to midnight) are retrieved for both temperatures above 95 km and CO mixing ratios above 85 km altitudes. Separate CO line maps obtained on (UT) June 2, 3, 6, and 11 indicate moderate daily variability in afternoon and evening CO mixing ratios (20-50%) and temperatures (5-10 K). Average Venus mesospheric temperatures over this period were 10 K warmer than returned from 1978 to 1979 Pioneer Venus or 2000-01 sub-millimeter measurements, without evidence for the very large temperature inversions indicated by Venus Express SPICAV measurements at 90-100 km altitudes (Bertaux, J.L., Vandaele, A.-C., Korablev, O., Villard, E., Fedorova, A., Fussen, D., Quémerais, E., Belyaev, D., Mahieux, A., Montmessin, F., Muller, C., Neefs, E., Nevejans, D., Wilquet, V., Dubois, J.P. Hauchecorne, A., Stepanov, A., Vinogradov, I., Rodin, A., Bertaux, J.-L., Nevejans, D., Korablev, O., Montmessin, F., Vandaele, A.-C., Fedorova, A., Cabane, M., Chassefière, E., Chaufray, J.Y., Dimarellis, E., Dubois, J.P., Hauchecorne, A., Leblanc, F., Lefèvre, F., Rannou, P., Quémerais, E., Villard, E., Fussen, D., Muller, C., Neefs, E., Van Ransbeeck, E., Wilquet, V., Rodin, A., Stepanov, A., Vinogradov, I., Zasova, L., Forget, F., Lebonnois, S., Titov, D., Rafkin, S., Durry, G., Gérard, J.C., Sandel, B., 2007. A warm layer in Venus’ cryosphere and high-altitude measurements of HF, HCl, H2O and HDO. Nature 450, 646-649). Measured Doppler shifts associated with June 2 and 11 12CO line center absorptions indicate nearly supersonic (200 m/s, Mach 1) afternoon-to-evening (retrograde) circulation; composed of additive subsolar-to-antisolar (SSAS) and zonal retrograde wind components, which are not separable due to the particular observational geometry. 相似文献
6.
Sub-millimeter 12CO (346 GHz) and 13CO (330 GHz) line absorptions, formed within the mesospheric to lower thermospheric altitude (70–120 km) region of the Venus atmosphere, have been mapped across the nightside disk of Venus during 2001–2009 inferior conjunctions, employing the James Clerk Maxwell Telescope (JCMT). Radiative transfer analysis of these thermal line absorptions supports temperature and CO mixing profile retrievals, as described in a companion paper (Clancy et al., 2012). Here, we consider the analysis of the sharp line absorption cores of these CO spectra in terms of accurate Doppler wind profile measurements at 95–115 km altitudes versus local time (～8 pm–4 am) and latitude (～60N–60S). These Doppler wind measurements support determinations of the nightside zonal and subsolar-to-antisolar (SSAS) circulation components over a variety of timescales. The average behavior fitted from 21 retrieved maps of 12CO Doppler winds (obtained over hourly, daily, weekly, and interannual intervals) indicates stronger average zonal (85 m/s retrograde) versus SSAS (65 m/s) circulation at the 1 μbar pressure (108–110 km altitude) level. However, the absolute and relative magnitudes of these circulation components exhibit extreme variability over daily to weekly timescales. Furthermore, the individual Doppler wind measurements within each nightside mapping observation generally show significant deviations (20–50 m/s, averaged over 5000 km horizontal scales) from the simple zonal/SSAS solution, with distinct local time and latitudinal characters that are also time variable. These large scale residual circulations contribute 30–70% of the observed nightside Doppler winds at any given time, and may be most responsible for global variations in nightside lower thermospheric trace composition and temperatures, as coincidentally retrieved CO abundance and temperature distributions do not correlate with solution retrograde zonal and SSAS winds (see companion paper, Clancy et al., 2012). Limited comparisons of these nightside submillimeter results with dayside infrared Doppler wind measurements suggest distinct dayside versus nightside circulations, in terms of zonal winds in particular. Combined 12CO and 13CO Doppler wind mapping observations obtained since 2004 indicate that the average zonal and SSAS wind components increase by 50–100% between altitudes of 100 and 115 km. If gravity waves originating from the cloud levels are responsible for the extension of zonal winds into the thermosphere (Alexander, M.J. [1992]. Geophys. Res. Lett. 19, 2207–2210), such waves deposit substantial momentum (i.e., break) in the lower nightside thermosphere. 相似文献
7.
Guillaume Desbois Janos L. Urai Peter A. Kukla Uwe Wollenberg Fabián Pérez-Willard Zsolt Radí Sandor Riholm 《Contributions to Mineralogy and Petrology》2012,163(1):19-31
We report observations from room temperature static recrystallization experiments (annealing times from minutes to year) of
cold-pressed, synthetic, coarse-grained, wet sodium chloride, prepared by broad ion beam polishing and SEM observations at
cryogenic temperature to observe directly the brine in grain boundaries. At all stages of annealing, the majority of the brine
in the samples is connected in 2D sections along grain boundaries. Another part of the brine is in isolated brine inclusion
arrays along grain boundaries and in brine inclusions left behind by migrating brine-filled grain boundaries. Most of these
boundaries are mobile because the aggregate is coarsening. We interpret that the boundaries without observable brine films
(<15 nm) and brine inclusion arrays are healed and immobile. Evolution of grain boundary structure involves three major processes.
First, dissolution on one side of the grain boundary and precipitation on the other side, resulting in grain boundary migration.
Second, the development of facets formed by low-index crystallographic planes of the grains bounding the grain boundary brine.
When both sides of a grain boundary are able to develop low-index facets in a thick brine film, the resulting impingement
boundary is interpreted to be immobile and may prevent the new grain from migrating into a deformed neighbor. When one side
of a faceted boundary consists of low-index crystallographic planes and the other side passively follows this faceted shape
along irrational surfaces, the boundary is mobile. Third, the healing of grain boundary brine films, producing solid–solid
grain boundaries without resolvable brine films. 相似文献
8.
Mm-wave spectra of HDO in the Venus mesosphere (65-100 km) were obtained over the period March 1998 to June 2004. Each spectrum is a measurement of the hemispheric-average H2O vapor mixing ratio in the Venus mesosphere. Observations were conducted for wide ranges of Venus solar elongations (46° W to 47° E), and fractional disk illuminations (f=0% to 99%), yielding water vapor abundances on 17 dates and over a full range of local solar time (LST) at the sub-Earth point on Venus. Our mesopheric H2O values are more numerous and far more precise than the earliest mm-derived H2O measurements [Encrenaz, Th., Lellouch, E., Paubert, G., Gulkis, S., 1991. First detection of HDO in the atmosphere of Venus at radio wavelengths: An estimate of the H2O vertical distribution. Astron. Astrophys. 246, L63-L66; Encrenaz, Th., Lellouch, E., Cernicharo, J., Paubert, G., Gulkis, S., Spilker, T., 1995. The thermal profile and water abundance in the Venus mesosphere from H2O and HDO millimeter observations. Icarus 117, 162-172], allowing an analysis of variability that was previously impossible. Measured 65-100 km H2O ranged from 0.0±0.06 to 3.5±0.3 ppmv, with significantly different variability than found in previous infrared (lower altitude, cloudtop) studies. Strong global variability on a 1-2 month timescale is clear and unambiguous. A limited number of excellent s/n measurements tentatively indicate the 1-2 month variability manifests most rapidly as change in the lower mesosphere, and more slowly as change in the upper mesosphere. Neither long term (1998-2004) nor diurnal variability in 65-100 km H2O is evident. While six-year and/or diurnal variabilities are not ruled out, they are weaker than the 1-2 month timescale variation. These conclusions are supported by initial (2004) sub-mm measurements. 相似文献
9.
Rapid temporal variability of SO2 and SO in the Venus 85–100 km mesosphere (Sandor, B.J., Clancy, R.T., Moriarty-Schieven G.H. [2007]. Bull. Am. Astron. Soc. 39, 503; Sandor, B.J., Clancy, R.T., Moriarty-Schieven, G.H., Mills, F.P. [2010]. Icarus 208, 49–60) requires in situ sources and sinks for these molecules. While many loss mechanisms are recognized, no process for in situ production is known. Observational investigations to find, or constrain other potential sulfur reservoirs offer one method toward understanding the applicable photochemistry. Here, we report upper limits for gas-phase H2SO4 (sulfuric acid) abundances in Venus’ 85–100 km upper mesosphere, derived from 16 ground-based sub-mm spectroscopic observations in the period 2004–2008. Unlike the ubiquitous sulfuric acid solid/liquid aerosol, the gas phase would be photochemically active, potentially both source and sink for SO and SO2. H2SO4 is retrieved from sub-mm lines located in the same bandpass as the SO2 and SO lines described by Sandor et al. (Sandor, B.J., Clancy, R.T., Moriarty-Schieven, G.H., Mills, F.P. [2010]. Icarus 208, 49–60). H2SO4 upper limits reported here are thus simultaneous and spatially coincident with measurements of SO2 and SO, providing for analysis of the three sulfur species collectively. The average H2SO4 abundance over 16 observations is 1 ± 2 ppb (i.e. <3 ppb). Upper limits for individual observations range from 3 to 44 ppb, where quality of the observing weather is the dominant constraint on measurement precision. The sum of H2SO4, SO2 and SO varies widely. In one comparison, the sum [H2SO4 + SO2 + SO] measured on one date differs by 10-σ from the sum measured 2 months later. We conclude that upper mesospheric sulfur atoms are not conserved among the three molecules, that H2SO4 is not a significant sulfur reservoir for balancing the observed variations of [SO2 + SO], and is not relevant to the (still unknown) photochemistry responsible for observed behavior of SO2 and SO. Having ruled out H2SO4, we infer that elemental sulfur is the most probable candidate for the needed third reservoir. 相似文献
10.
Farmers in the Zuni area of the semiarid American Southwest have successfully cultivated maize and other crops for over three millennia without using artificial fertilizers. Zuni agricultural fields are among the oldest, more or less continuously cultivated areas in the United States. Traditional Zuni agriculture is based on runoff farming, a system whereby runoff and organic‐rich sediment generated in small watersheds are captured and directed onto fields for crop use. We conducted a study to compare soil properties associated with paired and unpaired cultivated, abandoned, and uncultivated fields to evaluate the long‐term effects of cultivation on soil quality. Sampling and analytical methods of this research are especially applicable to geoarchaeological studies of anthropogenic effects on soil fertility and agricultural sustainability in ancient and traditional historical farming systems. Results of the Zuni soil study indicate that cultivation has altered some soil properties, including bulk density, organic carbon, total nitrogen, and C:N ratios in paired fields, but there is no indication that agricultural soils are degraded. This assessment supports the perception of Zuni farmers that long‐term cultivation has not caused a decline in agricultural productivity. © 2005 Wiley Periodicals, Inc. 相似文献