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1.
Ryuichi Wada Joseph M. Beames Andrew J. Orr-Ewing 《Journal of Atmospheric Chemistry》2007,58(1):69-87
An open-path cavity ring-down spectroscopy (CRDS) instrument for measurement of atmospheric iodine monoxide (IO) radicals
has been tested in the laboratory and subsequently deployed in Roscoff on the north-west coast of France as part of the Reactive
Halogens in the Marine Boundary Layer (RHaMBLe) project in September 2006. In situ measurements are reported of local IO mixing
ratios in the marine boundary layer. To obtain these mixing ratios, accurate absorption cross sections of IO are required
at the selected wavelengths used for spectroscopic measurements. Absorption cross sections at the bandheads of the IO A2Π3/2–X2Π3/2 (3,0) and (2,0) vibronic bands were thus verified by a combination of spectral simulation methods, inter-comparison of prior
determinations of cross-sections at high and low spectral resolution, and by measurement of rates of loss of IO by its self-reaction.
The performance of the open-path CRDS instrument was tested by measuring concentrations of NO2 in ambient air, both within and outside the laboratory, with results that were in excellent agreement with a previously validated
continuous wave CRDS apparatus for NO2 detection. During the RHaMBLe campaign, the open-path CRDS instrument was located within a few metres of the shoreline and
operated at wavelengths close to 435 nm to detect the absorption of light by trace levels of IO. The IO mixing ratios were
obtained on two days, peaked close to low tide, and were approximately 5–10 times higher than values calculated from column
densities previously reported by long-path, differential optical absorption spectroscopy (DOAS) in coastal regions. The typical
detection limit of the instrument was estimated to be 10 pptv of IO, with some fluctuation around this value depending on
the conditions of wind and atmospheric aerosol particles, and the total accumulation time was 30 s for each data point. The
observations of relatively high concentration of IO, compared to the values previously reported by DOAS, are consistent with
the concurrent observations using a LIF (Laser induced Fluorescence) instrument (Whalley et al. in press). The first such measurements of localized IO by CRDS and LIF should contribute to an improved understanding of the chemistry
of halogen compounds and the formation of iodine oxide aerosol particles in the marine boundary layer. 相似文献
2.
Catherine S. E. Bale Trevor Ingham Roisin Commane Dwayne E. Heard William J. Bloss 《Journal of Atmospheric Chemistry》2008,60(1):51-70
A field instrument has been developed for the purpose of measuring gas-phase atmospheric iodine species in the marine boundary
layer. Vacuum UV resonance-fluorescence (RF), generated using a microwave discharge lamp, is employed to detect atomic iodine
via the (5p46s)–(5p5) transitions around 178–184 nm. The system can be operated in two modes; either to directly measure ambient iodine atoms,
or to measure the total photolabile iodine loading of ambient air, through broadband visible photolysis of photolabile iodine-containing
species, with subsequent RF detection of the iodine atoms released. In both cases the instrument allows for the in situ measurement
of the species detected, which is advantageous for gathering information concerning their local sources and distribution.
The instrument is calibrated through generation of a known concentration of iodine atoms from the photolysis of I2 using a mercury pen-ray lamp. The instrument was deployed for the first time in August 2007 at Mace Head on the west coast
of Ireland; initial results from this field trial are presented. Ambient iodine atoms were measured at levels up to 22 ± 4.8 ppt
during the day, coinciding with the lowest tides, when Laminaria seaweed beds were exposed. The total photolabile iodine loading was also measured during several night-time and day-time
periods and was found to correlate inversely with tidal height. Inferred I2 concentrations based on these measurements indicate levels of several hundred ppt at the Mace Head site. These measurements
represent the first direct observations of ambient iodine atoms and measurement of total photolabile iodine in the atmosphere. 相似文献
3.
Laboratory Study of O(1S) Formation Process in the Photolysis of O3 and its Atmospheric Implications
Tomoki Nakayama Kenshi Takahashi Yutaka Matsumi Hitoshi Fujiwara 《Journal of Atmospheric Chemistry》2006,53(2):107-122
A high-sensitive technique to detect O(1S) atoms using vacuum ultraviolet laser-induced fluorescence (VUV-LIF) spectroscopy has been applied to study the O(1S) production process from the UV photodissociation of O3, N2O, and H2O2. The quantum yields for O(1S) formation from O3 photolysis at 215 and 220 nm are determined to be (1.4 ± 0.4) × 10−4 and (5 ± 3) × 10−5, respectively. Based on thermochemical considerations, the O(1S) formation from O3 photolysis at 215 and 220 nm is attributed to a spin-forbidden process of O(1S)+O2(X3Σg
−). Analysis of the Doppler profile of O(1S) produced from O3 photolysis at 193 nm also indicates that the O(1S) atoms are produced from the spin-forbidden process. In the photolysis of N2O and H2O2 at 193 nm, no discernible signal of O(1S) atoms has been detected. The upper limit values of the quantum yields for O(1S) production from N2O and H2O2 photolysis at 193 nm are estimated to be 8 × 10−5 and 3 × 10−5, respectively. Using the experimental results, the impact of the O(1S) formation from O3 photolysis on the atmospheric OH radical formation through the reaction of O(1S)+H2O has been estimated. The calculated results show that the contribution of the O(1S)+H2O reaction to the OH production rate is ∼2% of that of the O(1D)+H2O reaction at 30 km altitude in mid-latitude. Implications of the present laboratory experimental results for the terrestrial airglow of O(1S) at 557.7 nm have also been discussed. 相似文献
4.
Eric Schlosser Birger Bohn Theo Brauers Hans-Peter Dorn Hendrik Fuchs Rolf Häseler Andreas Hofzumahaus Frank Holland Franz Rohrer Lutz Olaf Rupp Manfred Siese Ralf Tillmann Andreas Wahner 《Journal of Atmospheric Chemistry》2007,56(2):187-205
At the atmosphere simulation chamber SAPHIR in Jülich both Laser-Induced Fluorescence Spectroscopy (LIF) and Long-Path Differential
Optical Laser Absorption Spectroscopy (DOAS) are operational for the detection of OH radicals at tropospheric levels. The
two different spectroscopic techniques were compared within the controlled environment of SAPHIR based on all simultaneous
measurements acquired in 2003 (13 days). Hydroxyl radicals were scavenged by added CO during four of these days in order to
experimentally check the calculated precisions at the detection limit. LIF measurements have a higher precision (σ= 0.88×106 cm–3) and better time resolution (Δt = 60 s), but the DOAS method (σ= 1.24×106 cm–3, Δt = 135 s) is regarded as primary standard for comparisons because of its good accuracy. A high correlation coefficient of
r = 0.95 was found for the whole data set highlighting the advantage of using a simulation chamber. The data set consists of
two groups. The first one includes 3 days, where the LIF measurements yield (1 – 2) ×106 cm–3 higher OH concentrations than observed by the DOAS instrument. The experimental conditions during these days are characterized
by increased NOx concentration and a small dynamic range in OH. Excellent agreement is found within the other group of 6 days. The regression
to the combined data of this large group yields unity slope without a significant offset. 相似文献
5.
Seasonal carbon dioxide balance and respiration of a high-arctic fen ecosystem in NE-Greenland 总被引:2,自引:0,他引:2
C. Nordstroem H. Soegaard T. R. Christensen T. Friborg B. U. Hansen 《Theoretical and Applied Climatology》2001,70(1-4):149-166
Summary Turbulent fluxes of CO2 were continuously measured by eddy correlation for three months in 1997 over a gramineous fen in a high-arctic environment
at Zackenberg (74°28′12″N, 20°34′23″W) in NE-Greenland. The measurements started on 1 June, when there was still a 1–2 m cover
of dry snow, and ended 26 August at a time that corresponds to late autumn at this high-arctic site. During the 20-day period
with snow cover, fluxes of CO2 to the atmosphere were small, typically 0.005 mg CO2 m−2 s−1 (0.41 g CO2 m−2 d−1), wheres during the thawed period, the fluxes displayed a clear diurnal variation. During the snow-free period, before the
onset of vegetation growth, fluxes of CO2 to the atmosphere were typically 0.1 mg CO2 m−2 s−1 in the afternoon, and daily sums reached values up to almost 9 g CO2 m−2 d−1. After 4 July, downward fluxes of CO2 increased, and on sunny days in the middle of the growing season, the net ecosystem exchange rates attained typical values
of about −0.23 mg m−2 s−1 at midday and max values of daily sums of −12 g CO2 m−2 d−1. Throughout the measured period the fen ecosystem acted as a net-sink of 130 g CO2 m−2. Modelling the ecosystem respiration during the season corresponded well with eddy correlation and chamber measurements.
On the basis of the eddy correlation data and the predicted respiration effluxes, an estimate of the annual CO2 balance the calender year 1997 was calculated to be a net-sink of 20 g CO2 m−2 yr−1.
Received October 6, 1999 Revised May 2, 2000 相似文献
6.
Carsten Blindauer Vladimir Rozanov John Philip Burrows 《Journal of Atmospheric Chemistry》1996,24(1):1-21
The accurate radiative transfer model GOMETRAN, initially designed to yield radiances at TOA in the wavelength range 240–790 nm, has been extended to allow for the computation of actinic fluxes down to 175 nm and for the calculation of photolysis frequencies in the atmosphere. The capability of the extended model PHOTOGT (PHOTOGOMETRAN) is demonstrated in a number of successful comparison studies both with recent experiments (ground-based, balloonborne, airborne) and model calculations of radiances, actinic fluxes and photolysis frequencies in the stratosphere and troposphere. In an atmospheric case study, the impact of new quantum yield data for the O3 » O2+O(1
d) photodissociation channel on the photolytic production of O(1
d) atoms in the lower atmosphere has been quantified. 相似文献
7.
Kinetics of the reactions of soot surface-bound polycyclic aromatic hydrocarbons with NO<Subscript>2</Subscript> 总被引:1,自引:0,他引:1
Mai Lan Nguyen Yuri Bedjanian Angélique Guilloteau 《Journal of Atmospheric Chemistry》2009,62(2):139-150
The kinetics of heterogeneous reactions of NO2 with 17 polycyclic aromatic hydrocarbons (PAHs) adsorbed on laboratory generated kerosene soot surface was studied over the
temperature range (255–330) K in a low pressure flow reactor combined with an electron-impact mass spectrometer. The kinetics
of soot-bound PAH consumption due to their desorption and reaction with NO2 were monitored using off-line HPLC measurements of their concentrations in soot samples as a function of reaction time, NO2 concentrations in the gas phase being analyzed by mass spectrometer. No measurable decay of PAHs due to the reaction with
NO2 was observed under experimental conditions of the study (maximum NO2 concentration of 5.5 × 1014 molecule cm−3 and reaction time of 45 min), which allowed to determine the upper limits of the first-order rate constants for the heterogeneous
reactions of 17 soot-bound PAHs with NO2: k < 5.0 × 10−5 s−1 (for most PAHs studied). Comparison of these results to previous studies carried on different carbonaceous substrates, showed
that heterogeneous reactivity of PAHs towards NO2 is, probably, dependent on the substrate nature even for resembling, although different carbonaceous materials. Results show
that particulate PAHs degradation by NO2 alone is of minor importance in the atmosphere 相似文献
8.
Both aerosol and rainwater samples were collected and analyzed for ionic species at a coastal site in Southeast Asia over
a period of 9 months (January–September 2006) covering different monsoons. In general, the occurrence and distribution of
ionic species showed a distinct seasonal variation in response to changes in air mass origins. Real-time physical characterization
of aerosol particles during rain events showed changes in particle number distributions which were used to assess particle
removal processes associated with precipitation, or scavenging. The mean scavenging coefficients for particles in the range
10–500 nm and 500–10 μm were 7.0 × 10−5 ± 2.8 × 10−5 s−1 and 1.9 × 10−4 ± 1.6 × 10−5 s−1, respectively. A critical analysis of the scavenging coefficients obtained from this study suggested that the wet removal
of aerosol particles was greatly influenced by rain intensity, and was particle size-dependent as well. The scavenging ratios,
another parameter used to characterize particle removal processes by precipitation, for NH4
+, Cl−, SO4
2−, and NO3
− were found to be higher than those of Na+, K+, and Ca2+ of oceanic and crustal origins. This enrichment implied that gaseous species NH3, HCl, and HNO3 could also be washed out readily. These additional sources of ions in precipitation presumably counter-balanced the dilution
effect caused by high total precipitation volume in the marine and tropical area. 相似文献
9.
Aerosol and rain samples were collected between 48°N and 55°S during the KH-08-2 and MR08-06 cruises conducted over the North
and South Pacific Ocean in 2008 and 2009, to estimate dry and wet deposition fluxes of atmospheric inorganic nitrogen (N).
Inorganic N in aerosols was composed of ~68% NH4+ and ~32% NO3– (median values for all data), with ~81% and ~45% of each species being present on fine mode aerosol, respectively. Concentrations
of NH4+ and NO3− in rainwater ranged from 1.7–55 μmol L−1 and 0.16–18 μmol L−1, respectively, accounting for ~87% by NH4+ and ~13% by NO3− of total inorganic N (median values for all data). A significant correlation (r = 0.74, p < 0.05, n = 10) between NH4+ and methanesulfonic acid (MSA) was found in rainwater samples collected over the South Pacific, whereas no significant correlations
were found between NH4+ and MSA in rainwater collected over the subarctic (r = 0.42, p > 0.1, n = 6) and subtropical (r = 0.33, p > 0.5, n = 6) western North Pacific, suggesting that emissions of ammonia (NH3) by marine biological activity from the ocean could become a significant source of NH4+ over the South Pacific. While NO3− was the dominant inorganic N species in dry deposition, inorganic N supplied to surface waters by wet deposition was predominantly
by NH4+ (42–99% of the wet deposition fluxes for total inorganic N). We estimated mean total (dry + wet) deposition fluxes of atmospheric
total inorganic N in the Pacific Ocean to be 32–64 μmol m−2 d−1, with 66–99% of this by wet deposition, indicating that wet deposition plays a more important role in the supply of atmospheric
inorganic N than dry deposition. 相似文献
10.
Melanie Louise Inez Witt Stephen Skrabal Robert Kieber Joan Willey 《Journal of Atmospheric Chemistry》2007,58(2):89-109
Significant quenching of fluorescence by Cu in rainwater samples from southeastern North Carolina demonstrates that chromophoric
dissolved organic matter (CDOM) is an effective ligand for Cu in rainwater. A strong inverse correlation between the decrease
in fluorescence upon Cu addition and CDOM abundance suggests the presence of excess binding sites for Cu in high CDOM samples.
Electroanalytical studies indicate that CDOM extracted from C18 cartridges formed Cu complexes with concentrations and conditional stability constants similar to ligands found in ambient
rainwater. When authentic rainwater samples were photolyzed with simulated sunlight both photoproduction and photodestruction
of ligands were observed, suggesting the photochemical response of Cu-complexing ligands in rainwater is the result of two
competing reactions. The rate of CDOM photobleaching was directly related to changes in strong ligands (KCuL ∼ 1015) whereas weaker ligands (KCuL < 1013) were not correlated, suggesting the photolabile CDOM resides in the strong ligand class. A photolysis study comparing filtered
and unfiltered rainwater samples indicated that Cu-complexing ligands adsorbed onto or otherwise associated with particles
are photodegraded much more rapidly than dissolved ligands. Photolysis with UV radiation appears to be most effective at engendering
changes in Cu ligands, however a significant photochemical response was also observed when samples were exposed to photosynthetically
active radiation with wavelengths greater than 400 nm. Results from this study demonstrate that complexation of Cu by CDOM
has important ramifications for controlling both the speciation of the metal and the reactivity of CDOM in rainwater. 相似文献
11.
A Laser-induced Fluorescence Instrument for Detecting Tropospheric OH and HO2: Characteristics and Calibration 总被引:1,自引:0,他引:1
Ian C. Faloona David Tan Robert L. Lesher Nathan L. Hazen Christopher L. Frame James B. Simpas Hartwig Harder Monica Martinez Piero Di Carlo Xinrong Ren William H. Brune 《Journal of Atmospheric Chemistry》2004,47(2):139-167
12.
Laura T. Iraci Brent G. Riffel Carly B. Robinson Rebecca R. Michelsen Rachel M. Stephenson 《Journal of Atmospheric Chemistry》2007,58(3):253-266
The aqueous phase acid-catalyzed reaction of methanol (CH3OH) with nitric acid (HNO3) to yield methyl nitrate (CH3ONO2) under atmospheric conditions has been investigated using gas-phase infrared spectroscopy. Reactions were conducted in aqueous
sulfuric acid solutions (50.5–63.6 wt.%) with [CH3OH] = 0.00005–0.005 M and [HNO3] = 0.02–0.21 M, at 278.2–328.6 K. Methyl nitrate production rates increased linearly with CH3OH and HNO3 concentrations and exponentially with sulfuric acid weight percent within the regime studied. Rates increased linearly with
nitronium ion concentration, indicating that the reaction involves as the nitrating agent under these conditions. At 298 K, the rate of methyl nitrate production can be calculated from k
obs
[CH3OH][HNO3], where k
obs
= 2.337 × 10−13(exp(0.3198*wt.% H2SO4)) when the solubility of CH3ONO2 in acidic solution is approximated by H* for pure water. The temperature dependence of the rate coefficient is related to solution composition, with activation energies
of 59 and 49 kJ/mol at 51.1 and 63.6 wt.% H2SO4, respectively, when k is calculated from rate. The temperature dependence has also been parameterized for application to the atmosphere, but the small quantities of present in aerosol particles will result in methyl nitrate production rates too small to be of significance under most atmospheric
conditions.
An erratum to this article can be found at 相似文献
13.
The I-atom sensitised decomposition of ozone in air at 1 atm pressure and ambient temperature has been investigated. Iodine atoms were produced by photolysis of I2 using visible light or of CH3I using ultraviolet light. In both cases, the quantum yield for O3 decomposition was 1.25 (±0.11) per I atom. An important role is proposed for the self-reaction of IO radicals leading to higher oxides of iodine, IO+IO(+M)I2O2(+M)higher oxides, which predominated over the bimolecular reaction leading to regeneration of I atoms, IO+IO2I+O2, with k
2a/k
2b4. Simple computer modelling calculations indicate that reaction (2a) may be important in determining the fate of photolabile iodine species in the atmosphere. The consequences for the behaviour of radioiodine releases are also discussed. 相似文献
14.
Continuous weekly monitoring on the concentration of gases and aerosols in urban ambient air by a four-stage filter-pack method
was carried out for 7 years in order to study not only the acid-base balance of acid-related (HNO3, NO3
−, and non-sea-salt-(nss-)SO4
2−) and alkali-related (NH3, NH4
+, and nss-Ca2+) chemical species but also its influence on the acidification of precipitation. The concentrations of the total nitrate (=
NO3− + HNO3) and nss-SO42− showed a similar seasonal variation: high in the summer and low in the winter. The total nitrate and nss-SO42− accounted for 0.43 and 0.57 of the acid-related species, respectively, on an equivalent basis. The total ammonium (= NH3 + NH4+) accounted for more than 0.9 of the alkali-related species, except for a springtime nss-Ca2+ episodic peak. The alkali-related species were generally overabundant compared with the acid-related species in the HNO3-NO3−-nss-SO42−-NH3-NH4+-nss-Ca2+ system. The alkali-rich distribution was especially pronounced in the winter, but the acid-related species was comparable
to the alkali-related species in the summer, which was attributed to the larger H+ deposition by precipitation in the summer. This study can provide a methodology to associate survey results obtained by a
filter-pack method with those of precipitation. 相似文献
15.
R. R. Reddy K. Rama Gopal L. Siva Sankara Reddy K. Narasimhulu K. Raghavendra Kumar Y. Nazeer Ahammed C. V. Krishna Reddy 《Journal of Atmospheric Chemistry》2008,59(1):47-59
In the present study, an attempt has been made to examine the governing photochemical processes of surface ozone (O3) formation in rural site. For this purpose, measurements of surface ozone and selected meteorological parameters have been
made at Anantapur (14.62°N, 77.65°E, 331 m asl), a semi-arid zone in India from January 2002 to December 2003. The annual
average diurnal variation of O3 shows maximum concentration 46 ppbv at noon and minimum 25 ppbv in the morning with 1σ standard deviation. The average seasonal
variation of ozone mixing ratios are observed to be maximum (about 60 ppbv) during summer and minimum (about 22 ppbv) in the
monsoon period. The monthly daytime and nighttime average surface ozone concentration shows a maximum (55 ± 7 ppbv; 37 ± 7.3 ppbv)
in March and minimum (28 ± 3.4 ppbv; 22 ± 2.3 ppbv) in August during the study period. The monthly average high (low) O3 48.9 ± 7.7 ppbv (26.2 ± 3.5 ppbv) observed at noon in March (August) is due to the possible increase in precursor gas concentration
by anthropogenic activity and the influence of meteorological parameters. The rate of increase of surface ozone is high (1.52 ppbv/h)
in March and lower (0.40 ppbv/h) in July. The average rate of increase of O3 from midnight to midday is 1 ppbv/h. Surface temperature is highest (43–44°C) during March and April months leading to higher
photochemical production. On the other hand, relative humidity, which is higher during the rainy season, shows negative correlation
with temperature and ozone mixing ratio. It can be seen that among the two parameters are measured, correlation of surface
ozone with wind speed is better (R
2=0.84) in compare with relative humidity (R
2=0.66). 相似文献
16.
The chemistry of glycolaldehyde (hydroxyacetaldehyde) relevant to the troposphere has been investigated using UV absorption spectrometry and FTIR absorption spectrometry in an environmental chamber. Quantitative UV absorption spectra have been obtained for the first time. The UV spectrum peaks at 277 nm with a maximum cross section of (5.5± 0.7)×10–20 cm2 molecule–1. Studies of the ultraviolet photolysis of glycolaldehyde ( = 285 ± 25 nm) indicated that the overall quantum yield is > 0.5 in one bar of air, with the major products being CH2OH and HCO radicals. Rate coefficients for the reactions of Cl atoms and OH radicals with glycolaldehyde have been determined to be (7.6± 1.5)×10–11 and (1.1± 0.3)×10–11 cm3 molecule–1 s–1, respectively, in good agreement with the only previous study. The lifetime of glycolaldehyde in the atmosphere is about 1.0 day for reaction with OH, and > 2.5 days for photolysis, although both wet and dry deposition should also be considered in future modeling studies. 相似文献
17.
Rebecca S. Anderson Lin Huang Richard Iannone Jochen Rudolph 《Journal of Atmospheric Chemistry》2007,56(3):275-291
The carbon kinetic isotope effects (KIEs) in the reactions of several unsaturated hydrocarbons with chlorine atoms were measured
at room temperature and ambient pressure using gas chromatography combustion isotope ratio mass spectrometry (GCC-IRMS). All
measured KIEs, defined as the ratio of the rate constants for the unlabeled and labeled hydrocarbon reaction k
12/k
13, are greater than unity or normal KIEs. The KIEs, reported in per mil according to Cl
ɛ = (k
12/k
13−1) × 1000‰ with the number of experimental determinations in parenthesis, are as follows: ethene, 5.65 ± 0.34 (1); propene,
5.56 ± 0.18 (2); 1-butene, 5.93 ± 1.16 (1); 1-pentene, 4.86 ± 0.63 (1); cyclopentene, 3.75 ± 0.14 (1); toluene, 2.89 ± 0.31
(2); ethylbenzene, 2.17 ± 0.17 (2); o-xylene, 1.85 ± 0.54 (2). To our knowledge, these are the first reported KIE measurements for reactions of unsaturated NMHC
with Cl atoms. Relative rate constants were determined concurrently to the KIE measurements. For the reactions of cyclopentene
and ethylbenzene with Cl atoms, no rate constant has been reported in refereed literature. Our measured rate constants are:
cyclopentene (7.32 ± 0.88) relative to propene (2.68 ± 0.32); ethylbenzene (1.15 ± 0.04) relative to o-xylene (1.35 ± 0.21), all × 10−10 cm3 molecule−1 s−1. The KIEs in reactions of aromatic hydrocarbons with Cl atoms are similar to previously reported KIEs in Cl-reactions of
alkanes with the same numbers of carbon atoms. Unlike the KIEs for previously studied gas-phase hydrocarbon reactions, the
KIEs for alkene–Cl reactions do not exhibit a simple inverse dependence on carbon number. This can be explained by competing
contributions of normal and inverse isotope effects of individual steps in the reaction mechanism. Implications for the symmetries
of the transition state structures in these reactions and the potential relevance of Cl-atom reactions on stable carbon isotope
ratios of atmospheric NMHC are discussed. 相似文献
18.
Summary Net ecosystem CO2 exchange was measured over a mountain birch forest in northern Finland throughout the growing season. The maximal net CO2 uptake rate of about − 0.5 mg(CO2) m−2 s−1 was observed at the end of July. The highest nocturnal respiration rates in early August were 0.2 mg(CO2) m−2 s−1. The daily CO2 balances during the time of maximal photosynthesis were about −15 g(CO2) m−2 d−1. The mountain birch forest acted as a net sink of CO2 from 30 June to 28 August. During that period the net CO2 balance was −448 g(CO2)m−2. The interannual representativeness of the observed balances was studied using a simplified daily balance model, with daily
mean global radiation and air temperature as the input parameters. The year-to-year variation in the phenological development
was parameterised as a function of the cumulative effective temperature sum. The daily balance model was used for estimating
the variability in the seasonal CO2 balances due to the timing of spring and meteorological factors. The sink term of CO2 in 1996 was lower than the 15-year mean, mainly due to the relatively late emergence of the leaves.
Received October 11, 1999 Revised April 25, 2000 相似文献
19.
Absorption and fluorescence properties of rainwater during the cold season at a town in Western Portugal 总被引:1,自引:0,他引:1
Patrícia S. M. Santos Regina M. B. O. Duarte Armando C. Duarte 《Journal of Atmospheric Chemistry》2009,62(1):45-57
This study aims at evaluating the variability of the optical properties of chromophoric dissolved organic matter (CDOM) of
rainwater during the cold season, specifically between Autumn and Winter periods. The spectroscopic characteristics of rainwater
samples collected at a town (Aveiro) in western Portugal were assessed by UV-Vis absorbance and three-dimensional excitation-emission
matrix (EEM) fluorescence spectroscopies. Rainwater samples showed similar characteristics to those of natural humic substances
when analysed by UV-Vis absorbance spectroscopy, but a significant difference was observed in the volume weight average (VWA)
of absorbances between Autumn and Winter. In general, the EEM fluorescence spectra of the Autumn and Winter samples disclosed
the presence of six fluorophores with different VWA specific fluorescence intensities: three humic-like (λ
excitation/λ
emission ≈ 230/415 nm; 290/415 nm; and 340/415 nm) and three protein-like (λ
excitation/λ
emission ≈ 230/350 nm; 280/340 nm; and 225/300 nm), but one of the humic-like peaks (≈340/415 nm) does not always appear in the EEM
fluorescence spectra of the Winter samples. During the cold season, chromophoric compounds are important constituents of rainwater
dissolved organic matter and the presence of these highly absorbing and fluorescing compounds may exert a determining effect
in atmospheric absorption of solar radiation. 相似文献
20.
O. A. Tarasova C. A. M. Brenninkmeijer S. S. Assonov N. F. Elansky T. Röckmann M. A. Sofiev 《Journal of Atmospheric Chemistry》2007,57(2):135-152
The concentration, radiocarbon (14C) and stable isotope (13C and 18O) content of CO have been determined in air samples collected across Russia (about 8,500 km) and along the Ob river during
the summer of 1999 to study the CO sources and sinks. An instrumented carriage on the Trans-Siberian railway and a boat on
the river Ob were used as atmospheric measurement platforms. In general, CO mixing ratios, CO stable isotope ratios, as well
as the abundances of 14CO over West Siberia were similar to those found at remote northern hemispheric baseline monitoring stations. Identified sources
of CO along the Ob appear to be connected to methane oxidation based on an inferred δ13Csource = −36.8 ± 0.6‰, while the value for δ18Osource = 9.0 ± 1.6‰ identifies it as burning. Thus flaring in the oil and gas production can be supposed to be a source. The extreme
13C depletion and concomitant 18O enrichment for two of the boat samples unambiguously indicates contamination by CO from combustion of natural gas (inferred
values δ13Csource = −40.3‰ and δ18Osource = 17.5‰). For these two samples, that have strongly elevated 14CO concentrations, the industrial area near Tomsk is identified as a source area using meteorological calculations. Along
the Trans-Siberian Railroad background CO was to various degrees contaminated with CO from methane combustion (δ13Csource = −35.7 ± 6.2‰ and δ18Osource = 10.3 ± 1.8‰). The impact of industrial burning was discernable in the vicinity of Perm-Kungur. 相似文献