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1.
Active Long Path Differential Optical Absorption Spectroscopy (LP-DOAS) measurements of halogen oxides were conducted at Masaya Volcano, in Nicaragua from April 14 to 26, 2007. The active LP-DOAS system allowed night-time halogen measurements and reduced the ClO detection limit by an order of magnitude when compared to previous passive DOAS measurements, as wavelengths below 300 nm could be used for the DOAS retrievals. BrO was detected with an average BrO/SO2 molecular ratio of approximately 3 × 10−5 during the day. However, BrO values were below the detection limit of the instrument for all night-time measurements, a strong indication that BrO is not directly emitted, but rather the result of photochemical formation in the plume itself according to the autocatalytic “bromine explosion” mechanism. Despite the increased sensitivity, both ClO and OClO could not be detected. The achieved upper limits for the X/SO2 ratios were 5 × 10−3 and 7 × 10−6, respectively. A rough calculation suggests that ClO and OClO should be present at similar abundances in volcanic plumes. Since the DOAS technique is orders of magnitude more sensitive for OClO than for ClO, this indicates that OClO should always be detectable in plumes in which ClO is found. However, further LP-DOAS studies are needed to conclusively clarify the role of chlorine oxides in volcanic plumes.  相似文献   

2.
The simultaneous quantitative determination of two-dimensional bromine monoxide (BrO) and sulphur dioxide (SO2) distributions in volcanic gas plumes is described. Measurements at the fumarolic field on the island Vulcano (autumn 2004) and in the plume of Mt. Etna volcano (spring 2005) were carried out with an Imaging DOAS instrument. The SO2 fluxes of several fumaroles were estimated from two-dimensional distributions of SO2. Additionally, the first two-dimensional distributions of BrO within a volcanic plume were successfully retrieved. Slant column densities of up to 2.6 × 1014 molecules per square centimetre were detected in the plume of Mt. Etna. The investigation of the BrO/SO2 ratio, calculated from the two-dimensional distributions of SO2 and BrO, shows an increase from the centre to the edge of the volcanic plume. These results have significance for the involvement of ozone during BrO formation processes in volcanic emissions.  相似文献   

3.
Atmospheric SO2 has a significant impact on the urban environment and global climate. Band Residual Difference Algorithm (BRD) and Differential Optical Absorption Spectroscopy (DOAS) were used respectively by NASA and ESA science team to derive SO2 columns from satellite observations, but there are few studies on the comparison and validation of BRD and DOAS SO2 retrievals under the same observation conditions. In this study, the radiative transfer model SCIATRAN was firstly used to validate the accuracies of BRD and DOAS SO2 retrievals, and analyse the uncertainty of SO2 retrieval caused by band selection, O3 absorption, aerosol, surface reflectance, solar and viewing zenith angle. Finally, BRD and DOAS algorithms were applied to the same radiances from satellite observations, and comparisons of BRD and DOAS SO2 retrievals were conducted over volcanic eruption and North China. Results show that, for the case with low SO2 columns, BRD SO2 retrievals have higher retrieval accuracy than DOAS, but typical seasonal variation with high SO2 column in winter and low in summer can be more clearly discernible in DOAS SO2 retrievals than BRD from satellite observations. For the case with high SO2 columns, the differences between BRD (310.8–314.4 nm) and DOAS (315–327 nm) retrievals are large, and the value and accuracy of BRD (310.8–314.4 nm) SO2 retrievals are lower than those of DOAS (315–327 nm) retrievals. Compared with the SO2 inputs in forward model, both BRD (310.8–314.4 nm) and DOAS (315–327 nm) SO2 retrievals are underestimated for the case with high SO2 columns. The selection of wavelength range can significantly affect the accuracy of SO2 retrieval. The error of BRD SO2 retrieval from 310.8–314.4 nm is lower than other bands in the ultraviolet spectral region (306–327 nm). The increase of wavelength in the ultraviolet spectral region 306–330 nm can reduce the underestimation of DOAS SO2 retrievals in the case of high SO2 column, but slight overestimation of SO2 retrieval is found from the 315–327 nm range in the case of low SO2 column. The values of BRD and DOAS SO2 retrieval decrease with atmospheric O3 column and aerosol optical depth increasing, but increase with surface reflectance increasing. Large solar zenith angle and viewing zenith angle can introduce more errors to the BRD and DOAS SO2 retrievals. This study is important for the improvement of retrieval algorithm and the application of SO2 products from satellite observations.  相似文献   

4.
This paper presents a method to reconstruct the gas distribution inside a vertical cross section of a gas plume by combining data from two or more scanning DOAS instruments using a tomographic algorithm. The method can be applied to gas plumes from any single, elevated point source, such as a volcano or industrial chimney. Such two-dimensional concentration distributions may prove to be useful for example in plume chemistry, dispersion and environmental impact studies. Here we show the case with one scanning DOAS instrument located on each side of the plume, which is the easiest and most economic setup as well as the most useful in routine monitoring of e.g. volcanic gas emissions. The paper investigates the conditions under which tomographic reconstructions can be performed and discusses limitations of this setup. The proposed method has been studied theoretically by numerical simulations and has been experimentally tested during two field campaigns, with measurements of SO2 emissions from a volcano and a power plant. The simulations show that, under good measurement conditions, the algorithm presented performs well, which is further confirmed by the experimental results.  相似文献   

5.
Data from a series of laboratory experiments show the relationships between measured correlation spectrometer (COSPEC) sulfur-dioxide (SO2) burdens, automatic gain control (AGC) deflections, and visible wavelength opacities in ash-laden plumes. The data show that the COSPEC reliably measures (within a 10% accuracy) SO2 burdens up to AGC deflections of 2 V and visible wavelength opacities of 50%. Beyond these limits, the under measurement of the SO2 burden is not well constrained. During typical COSPEC runs, these limits are rarely violated. The 10% error introduced by measuring ash-laden plumes is acceptable because the error is small relative to other error sources associated with the technique, especially plume velocity; and the error is correctable which allows for a wider range of plume conditions to be measured.These results imply that the densest SO2 concentrations near the volcanic source can be measured. This is important so that SO2 is not lost from the volcanic plume due to physical and chemical processes and that measurements are conducted under maximum signal to noise ratios.  相似文献   

6.
Imaging Differential Optical Absorption Spectroscopy (IDOAS) is an optical remote-sensing method using scattered sunlight as light source. It combines a “pushbroom” imaging spectrometer with the DOAS technique and thus allows imaging two-dimensional trace gas distributions, e.g., in volcanic plumes. The highly sensitive and specific detection of many trace gases simultaneously (specific molecules, not just elements, e.g. SO2, BrO, NO2, O3, HCHO, etc.) is possible, and the temporal and spatial variation of these gases can be measured. The IDOAS system presented here enables the taking of two-dimensional images of trace gas distributions in a volcanic plume with a spatial resolution of 100 pixels horizontally × 64 pixels vertically, each with a field of view of 0.087° in horizontal and 0.208° in vertical directions. Therefore, IDOAS provides useful information about the chemical composition and chemical variability in a volcanic plume and allows studying plume dispersal and chemical transformations. The technique was applied to map the SO2 distribution in the plume of Mt. Etna volcano for the first time in October 2003.  相似文献   

7.
Our knowledge of the physico-chemical properties of volcanic plumes remains at an embryonic state, mainly because of the prohibitive cost of measurements made from aircraft, which alone can provide samples representative of the total aerosol and gaseous emission from a volcanic source. The authors show that a small Remotely Piloted Vehicle (R.P.V.), similar in design to the one they used for some probative flights over Mt. Etna, may be of great use in this field. They can, for instance, insure frequent measurement of the SO2/HCl ratio in volcanic emanations close to active craters at times when the eruptive vents themselves cannot be sampled directly. In June 1978, we were thus able to measure a mean ratio of SO2/HCl (7.6) in the Mt. Etna volcanic plume. In addition, a correlation spectrometer was in operation during the airborne sampling and allowed us to obtain order of magnitude values for the Mt. Etna discharge in water vapour (170000 tons/day), sulphur dioxide (1700 t/d), hydrochloric acid (340 t/d) and hydrofluoric acid (40 t/d). Widespread use of such R.P.V’s would insure the collection of a great deal of physicochemical data from volcanic plumes, data which are presently lacking and which could extensively enhance the efficiency of chemical methods of volcano surveillance.  相似文献   

8.
The Eyjafjallajökull volcanic eruption, which occurred on April 14, 2010, caused many environmental, air traffic and health problems. An attempt has been made to demonstrate for the first time that certain improvements could be made in the quantitative prediction of the volcanic ash parameters, and in the accounting of the processes in the immediate vicinity of the volcano, using a cloud-resolving model. This type of explicit modeling by treatment of volcanic ash and sulfate chemistry parameterization, with input of a number parameters describing the volcanic source, is the way forward for understanding the complex processes in plumes and in the future plume dispersion modeling. Results imply that the most significant microphysical processes are those related to accretion of cloud water, cloud ice and rainwater by snow, and accretion of rain and snow by hail. The dominant chemical conversion rates that give a great contribution to the sulfate budget are nucleation and dynamic scavenging and oxidation processes. A three-dimensional numerical experiment has shown a very realistic simulation of volcanic ash and other chemical compounds evolution, with a sloping structure strongly influenced by the meteorological conditions. In-cloud oxidation by H2O2 is the dominant pathway for SO2 oxidation and allows sulfate to be produced within the SO2 source region. The averaged cloud water pH of about 5.8 and rainwater pH of 4.5 over simulation time show quantitatively how the oxidation may strongly influence the sulfate budget and acidity of volcanic cloud. Compared to observations, model results are close in many aspects. Information on the near field volcanic plume behavior is essential for early preparedness and evacuation. This approach demonstrates a potential improvement in quantitative predictions regarding the volcanic plume distribution at different altitudes. It could be a useful tool for modeling volcanic plumes for better emergency measures planning.  相似文献   

9.
A portable multi-sensor system was developed to measure volcanic plumes in order to estimate the chemical composition and temperature of volcanic gases. The multi-sensor system consists of a humidity–temperature sensor, SO2 electrochemical sensor, CO2 IR analyzer, pump and flow control units, pressure sensor, data logger, and batteries; the whole system is light (∼5 kg) and small enough to carry in a medium-size backpack. Volcanic plume is a mixture of atmosphere and volcanic gas; therefore volcanic gas composition and temperature can be estimated by subtracting the atmospheric gas background from the plume data. In order to obtain the contrasting data of the plume and the atmosphere, measurements were repeated in and out of the plume. The multi-sensor technique was applied to measure the plume of Tarumae, Tokachi, and Meakan volcanoes, Hokkaido, Japan. Repeated measurements at each volcano gave a consistent composition with ±10–30% errors, depending on the stability of the background atmospheric conditions. Fumarolic gas samples were also collected at the Tokachi volcano by a conventional method, and we found a good agreement (the difference <10%) between the composition estimated by the multi-sensor technique and conventional method. Those results demonstrated that concentration ratios of major volcanic gas species (i.e., H2O, CO2, and SO2) and temperature can be estimated by the new technique without any complicated chemical analyses even for gases emitted from an inaccessible open vent. Estimation of a more detailed gas composition can be also achieved by the combination of alkaline filter techniques to measure Cl/F/S ratios in the plume and other sensors for H2S and H2.  相似文献   

10.
A fundamental problem with all ground-based remotely sensed measurements of volcanic gas flux is the difficulty in accurately measuring the velocity of the gas plume. Since a representative wind speed and direction are used as proxies for the actual plume velocity, there can be considerable uncertainty in reported gas flux values. Here we present a method that uses at least two time-synchronized simultaneously recording UV spectrometers (FLYSPECs) placed a known distance apart. By analyzing the time varying structure of SO2 concentration signals at each instrument, the plume velocity can accurately be determined. Experiments were conducted on Kīlauea (USA) and Masaya (Nicaragua) volcanoes in March and August 2003 at plume velocities between 1 and 10 m s−1. Concurrent ground-based anemometer measurements differed from FLYSPEC-measured plume speeds by up to 320%. This multi-spectrometer method allows for the accurate remote measurement of plume velocity and can therefore greatly improve the precision of volcanic or industrial gas flux measurements. Editorial responsibility: A. Woods  相似文献   

11.
Volcán Fuego in the Central American Republic of Guatemala erupted violently in October, 1974. A remote sensing correlation spectrometer. COSPEC IV, which utilizes the characteristic molecular absorption of SO2 in the ultraviolet was used to monitor the SO2 content of the volcanic plume. Over a 60-day period measurements were made on 37 days between and following major eruptive phases. SO2 emission rates corrected for atmospheric scattering of the spectral signal average 423 metric tons/day with a standard deviation of 252 metric tons/days. Late stage peaks in SO2 emission at Fuego are consistent with the presence of anomalously high contents of soluble materials on the stratigraphically highest ashes from other Central American eruptions. Indications are that the SO2 concentration within the volcanic plume increased as activity waned. These features imply that remote spectroscopic sensing of SO2 and perhaps other gases in a volcanic plume may provide a relatively easy and inexpensive means of determining the cessation of violent eruptive activity.  相似文献   

12.
Measurements of perturbations in the atmospheric potential gradient around volcanic plumes at multiple (from two to five) sites, and measurements of the charge-mass ratio of ash particles falling from volcanic plumes, were carried out at Sakurajima Volcano, Japan. Results from 28 and 29 October 1995, show that the nature of the perturbations depends on the intensity of plume activity. Although plume activity was vigorous on 28 October, negative perturbations were predominant. As plume activity peaked, the magnitude of negative perturbations decreased just below the plume and increased at an off-axis site. During the peak period, positively charged ash particles fell out from the plume. This suggests that the active plume dominantly contained negatively charged materials, and that positively and negatively charged materials were added to the lower and upper parts of the plume, respectively, during the peak period. On the other hand, as plume activity became less vigorous on 29 October, the perturbations were characterized by a positive anomaly followed by a negative anomaly. Because wind velocity increased with altitude that day, we infer that positive and negative charges were distributed in the upper and lower parts of the plume, respectively. The differences in perturbations observed on 28 and 29 October suggest that volcanic plumes are generally composed of three parts: an upper part with positively charged gas and aerosol, a middle part with negatively charged fine ash particles, and a lower part with positively charged coarse ash particles. The compilation of present and previous results from Sakurajima and other volcanoes indicates that the effect of the negative charge in the middle part was predominant in most cases, although positive perturbations caused by the upper part were observed around some weak plumes. The effect of positively charged particles in the lower part was observable only when plume activity was sufficiently strong because positively charged coarse particles tended to fall out near the vent.  相似文献   

13.
The correlation spectrometer (COSPEC), the principal tool for remote measurements of volcanic SO2, is rapidly being replaced by low-cost, miniature, ultraviolet (UV) spectrometers. We compared two of these new systems with a COSPEC by measuring SO2 column amounts at Kīlauea Volcano, Hawaii. The two systems, one calibrated using in-situ SO2 cells, and the other using a calibrated laboratory reference spectrum, employ similar spectrometer hardware, but different foreoptics and spectral retrieval algorithms. Accuracy, signal-to-noise, retrieval parameters, and precision were investigated for the two configurations of new miniature spectrometer. Measurements included traverses beneath the plumes from the summit and east rift zone of Kīlauea, and testing with calibration cells of known SO2 concentration. The results obtained from the different methods were consistent with each other, with <8% difference in estimated SO2 column amounts up to 800 ppm m. A further comparison between the COSPEC and one of the miniature spectrometer configurations, the ‘FLYSPEC’, spans an eight month period and showed agreement of measured emission rates to within 10% for SO2 column amounts up to 1,600 ppm m. The topic of measuring high SO2 burdens accurately is addressed for the Kīlauea measurements. In comparing the foreoptics, retrieval methods, and resultant implications for data quality, we aim to consolidate the various experiences to date, and improve the application and development of miniature spectrometer systems.  相似文献   

14.
Airborne correlation spectrometry (COSPEC) was used to measure the rate of SO2 emission at White Island on three dates, i.e., November 1983, 1230 ± 300 t/d; November 1984, 320 ± 120 t/d; and January 1985, 350 ± 150 t/d (t = metric tons). The lower emission rates are likely to reflect the long-term emission rates, whereas the November 1983 rate probably reflects conditions prior to the eruption of December 1983. The particle flux in the White Island plume, as determined with a quartz crystal microbalance/cascade in November 1983, was 1.3 t/d, unusually low for volcanic plumes. The observed plume particles, as shown from scanning electron microscopy, include halite, native sulfur, and silicates and are broadly similar to other volcanic plumes.Gas analyses from high-temperature volcanic fumaroles collected from June 1982 through November 1984 werde used together with the COSPEC data to estimate the flux of other gas species from White Island. The rates estimated are indicative of the long-term volcanic emission, i.e., 8000–9000 t/d H2O, 900–1000 t/d CO2, 70–80 t/d HCl, 1.5–2 t/d HF, and about 0.2 t/d NH3. The long-term thermal power output at White Island is estimated at about 400 MW.  相似文献   

15.
A list of volcanic eruption plumes observed to ascend into or near the stratosphere since 1883 shows that the volcanoes divide readily into two groups, one at low and one at higher latitudes. A model for the rise of a buoyant volcanic plume rise as applied to volcanic eruptions is corrected for realistic temperature profiles and for the finite vertical extent of the resultant debris clouds. The utility of the model can be questioned, however, owing to the highly uncertain and variable nature of the efficiency of use of heat energy of buoyant rise. The observed correlation of stratospheric plumes with climatic effects indicates that those plumes nearer the equator have the largest impact on surface temperatures. Analysis of the observations also suggests that injection of debris into the stratosphere is more important in determining the effect on climate than either the total volcanic explosivity of the eruption or the actual height reached within the stratosphere.  相似文献   

16.
The continuous measurement of molecular hydrogen (H2) emissions from passively degassing volcanoes has recently been made possible using a new generation of low-cost electrochemical sensors. We have used such sensors to measure H2, along with SO2, H2O and CO2, in the gas and aerosol plume emitted from the phonolite lava lake at Erebus volcano, Antarctica. The measurements were made at the crater rim between December 2010 and January 2011. Combined with measurements of the long-term SO2 emission rate for Erebus, they indicate a characteristic H2 flux of 0.03?kg s–1 (2.8?Mg? day–1). The observed H2 content in the plume is consistent with previous estimates of redox conditions in the lava lake inferred from mineral compositions and the observed CO2/CO ratio in the gas plume (~0.9 log units below the quartz–fayalite–magnetite buffer). These measurements suggest that H2 does not combust at the surface of the lake, and that H2 is kinetically inert in the gas/aerosol plume, retaining the signature of the high-temperature chemical equilibrium reached in the lava lake. We also observe a cyclical variation in the H2/SO2 ratio with a period of ~10?min. These cycles correspond to oscillatory patterns of surface motion of the lava lake that have been interpreted as signs of a pulsatory magma supply at the top of the magmatic conduit.  相似文献   

17.
Digital cameras, sensitive to specific regions of the ultra-violet (UV) spectrum, have been employed for quantifying sulfur dioxide (SO2) emissions in recent years. The instruments make use of the selective absorption of UV light by SO2 molecules to determine pathlength concentration. Many monitoring advantages are gained by using this technique, but the accuracy and limitations have not been thoroughly investigated. The effect of some user-controlled parameters, including image exposure duration, the diameter of the lens aperture, the frequency of calibration cell imaging, and the use of the single or paired bandpass filters, have not yet been addressed. In order to clarify methodological consequences and quantify accuracy, laboratory and field experiments were conducted. Images were collected of calibration cells under varying observational conditions, and our conclusions provide guidance for enhanced image collection. Results indicate that the calibration cell response is reliably linear below 1500 ppm m, but that the response is significantly affected by changing light conditions. Exposure durations that produced maximum image digital numbers above 32 500 counts can reduce noise in plume images. Sulfur dioxide retrieval results from a coal-fired power plant plume were compared to direct sampling measurements and the results indicate that the accuracy of the UV camera retrieval method is within the range of current spectrometric methods.  相似文献   

18.
We present a study on the retrieval sensitivity of the column-averaged dry-air mole fraction of CO2 (XCO2) for the Chinese carbon dioxide observation satellite (TanSat) with a full physical forward model and the optimal estimation technique. The forward model is based on the vector linearized discrete ordinate radiative transfer model (VLIDORT) and considers surface reflectance, gas absorption, and the scattering of air molecules, aerosol particles, and cloud particles. XCO2 retrieval errors from synthetic TanSat measurements show solar zenith angle (SZA), albedo dependence with values varying from 0.3 to 1 ppm for bright land surface in nadir mode and 2 to 8 ppm for dark surfaces like snow. The use of glint mode over dark oceans significantly improves the CO2 information retrieved. The aerosol type and profile are more important than the aerosol optical depth, and underestimation of aerosol plume height will introduce a bias of 1.5 ppm in XCO2. The systematic errors due to radiometric calibration are also estimated using a forward model simulation approach.  相似文献   

19.
Volcanic lightning, perhaps the most spectacular consequence of the electrification of volcanic plumes, has been implicated in the origin of life on Earth, and may also exist in other planetary atmospheres. Recent years have seen volcanic lightning detection used as part of a portfolio of developing techniques to monitor volcanic eruptions. Remote sensing measurement techniques have been used to monitor volcanic lightning, but surface observations of the atmospheric electric Potential Gradient (PG) and the charge carried on volcanic ash also show that many volcanic plumes, whilst not sufficiently electrified to produce lightning, have detectable electrification exceeding that of their surrounding environment. Electrification has only been observed associated with ash-rich explosive plumes, but there is little evidence that the composition of the ash is critical to its occurrence. Different conceptual theories for charge generation and separation in volcanic plumes have been developed to explain the disparate observations obtained, but the ash fragmentation mechanism appears to be a key parameter. It is unclear which mechanisms or combinations of electrification mechanisms dominate in different circumstances. Electrostatic forces play an important role in modulating the dry fall-out of ash from a volcanic plume. Beyond the local electrification of plumes, the higher stratospheric particle concentrations following a large explosive eruption may affect the global atmospheric electrical circuit. It is possible that this might present another, if minor, way by which large volcanic eruptions affect global climate. The direct hazard of volcanic lightning to communities is generally low compared to other aspects of volcanic activity.  相似文献   

20.
On December 1, 2007, the solar absorption infrared spectra of the Popocatépetl volcanic plume was recorded during an eruptive event and complementarily on November 17, 2008, the passive quiescent degassing was measured from the same site. A portable FTIR spectrometer with a scanning mirror for fast tracking of the sun provided the flexibility, quality, and simplicity needed for field deployment. Slant columns of the gases SO2, HCl, HF, and SiF4 were retrieved and strong differences could be observed when comparing gas ratios in both time periods. During the explosive eruption, the SO2/HCl ratio was three times greater and the HF/HCl ratio was slightly smaller than during passive degassing.While the ratios among SO2, HCl, HF, and SiF4 describe the chemical composition of the volcanic gas mixture, the SiF4/HF ratio provides information about the equilibrium temperatures of the stored gases which in this study were calculated at 150° and 185 °C for the explosive and quiescent degassing episodes, respectively. We conclude that cooling of lava domes in the crater precedes Vulcanian explosions as suggested by Schaaf et al (2005). Based on SO2 flux (Grutter et al., 2008) and measurements and data from the November 2008 event, the average fluxes for HCl, HF, SiF4, and F through quiescent degassing are estimated to be 204, 22.7, 9.8, and 31.7 tons/day, respectively. These values are similar to those reported by Love et al. (1998) more than 10 yrs ago.  相似文献   

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