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Volcanic plumes are common and far-reaching manifestations of volcanic activity during and between eruptions. Observations of the rate of emission and composition of volcanic plumes are essential to recognize and, in some cases, predict the state of volcanic activity. Measurements of the size and location of the plumes are important to assess the impact of the emission from sporadic or localized events to persistent or widespread processes of climatic and environmental importance. These observations provide information on volatile budgets on Earth, chemical evolution of magmas, and atmospheric circulation and dynamics. Space-based observations during the last decades have given us a global view of Earth's volcanic emission, particularly of sulfur dioxide (SO2). Although none of the satellite missions were intended to be used for measurement of volcanic gas emission, specially adapted algorithms have produced time-averaged global emission budgets. These have confirmed that tropospheric plumes, produced from persistent degassing of weak sources, dominate the total emission of volcanic SO2. Although space-based observations have provided this global insight into some aspects of Earth's volcanism, it still has important limitations. The magnitude and short-term variability of lower-atmosphere emissions, historically less accessible from space, remain largely uncertain. Operational monitoring of volcanic plumes, at scales relevant for adequate surveillance, has been facilitated through the use of ground-based scanning differential optical absorption spectrometer (ScanDOAS) instruments since the beginning of this century, largely due to the coordinated effort of the Network for Observation of Volcanic and Atmospheric Change (NOVAC). In this study, we present a compilation of results of homogenized post-analysis of measurements of SO2 flux and plume parameters obtained during the period March 2005 to January 2017 of 32 volcanoes in NOVAC. This inventory opens a window into the short-term emission patterns of a diverse set of volcanoes in terms of magma composition, geographical location, magnitude of emission, and style of eruptive activity. We find that passive volcanic degassing is by no means a stationary process in time and that large sub-daily variability is observed in the flux of volcanic gases, which has implications for emission budgets produced using short-term, sporadic observations. The use of a standard evaluation method allows for intercomparison between different volcanoes and between ground- and space-based measurements of the same volcanoes. The emission of several weakly degassing volcanoes, undetected by satellites, is presented for the first time. We also compare our results with those reported in the literature, providing ranges of variability in emission not accessible in the past. The open-access data repository introduced in this article will enable further exploitation of this unique dataset, with a focus on volcanological research, risk assessment, satellite-sensor validation, and improved quantification of the prevalent tropospheric component of global volcanic emission. Published version Initial implementation of the network was funded by the EU FP6 NOVAC project (https://cordis.europa.eu/ project/rcn/75513/factsheet/en, last access: 1 October 2020). Recent funding for this work was provided by the Alfred P. Sloan Foundation’s Deep Carbon Observatory programme (https://deepcarbon. net/, last access: 1 October 2020), Chalmers University of Technology, the Swedish National Space Agency (career grant no. 149/18), and the ECMWF CAMS_81 Global and Regional Emissions project. The authors are thankful for the valuable support from the USGS–USAID Volcano Disaster Assistance Program (https: //volcanoes.usgs.gov/vdap/, last access: 1 October 2020) provided to NOVAC since 2015.

Volcanic plumes are common and far-reaching manifestations of volcanic activity during and between eruptions. Observations of the rate of emission and composition of volcanic plumes are essential to recognize, and in some cases predict, the state of volcanic activity. Measurements of the size and location of the plumes are important to assess the impact of the emission from sporadic or localized events to persistent or widespread processes of climatic and environmental importance. These observations provide information on volatile budgets on Earth, chemical evolution of magmas and atmospheric circulation and dynamics. Space-based observations during the last decades have given us a global view of Earth’s volcanic emission, particularly of sulphur dioxide (SO2). Although none of the satellite missions were intended to be used for measurement of volcanic gas emission, specially adapted algorithms have produced time-averaged global emission budgets. These have confirmed that tropospheric plumes, produced from persistent degassing of weak sources, dominate the total emission of volcanic SO2. Although space-based observations have provided this global insight into some aspects of Earth's volcanism, it still has important limitations. The magnitude and short-term variability of lower-atmosphere emissions, historically less accessible from space, remain largely uncertain. Operational monitoring of volcanic plumes, at scales relevant for adequate surveillance, has been facilitated through the use of ground-based scanning-differential optical absorption spectrometers (ScanDOAS) since the beginning of this century, largely due to the coordinated effort of the Network for Observation of Volcanic and Atmospheric Change (NOVAC). In this study, we present a compilation of results of homogenized post-analysis of measurements of SO2 flux and plume parameters obtained during the period March 2005 to January 2017 on 32 volcanoes in NOVAC. This inventory opens a window into the short-term emission patterns of a diverse set of volcanoes in terms of magma composition, geographical location, magnitude of emission, and style of eruptive activity. We find that passive volcanic degassing is by no means a stationary process in time and that large sub-daily variability is observed in the flux of volcanic gases, which has implications for emission budgets produced using short-term, sporadic observations. The use of a standard evaluation method allows intercomparison between different volcanoes and between ground- and space-based measurements of the same volcanoes. The emission of several weakly degassing volcanoes, undetected by satellites, is presented for the first time. We also compare our results with those reported in the literature, providing ranges of variability in emission, not accessible in the past. The open-access data repository, introduced in this article, will enable further exploitation of this unique dataset, with a focus on volcanological research, risk assessment, satellite-sensors validation, and improved quantification of the prevalent tropospheric component of global volcanic emission. Data sets for each volcano are made available at https://novac.chalmers.se, under license CC-BY 4, or through the DOI-links provided in Table 1.

The Nevado del Ruiz volcano is considered one of the most active volcanoes in Colombia, which can potentially threaten approximately 600,000 inhabitants. The existence of a glacier and several streams channelling in some main rivers, flowing downslope, increases the risk for the population living on the flank of the volcano in case of unrest, because of the generation of lahars and mudflows. Indeed, during the November 1985 subplinian eruption, a lahar generated by the sudden melting of the glacier killed twenty thousand people in the town of Armero. Moreover, the involvement of the local hydrothermal system has produced in the past phreatic and phreatomagmatic activity, as occurred in 1989. Therefore, the physico-chemical conditions of the hydrothermal system as well as its contribution to the shallow thermal groundwater and freshwater in terms of enthalpy and chemicals require a close monitoring. The phase of unrest occurred since 2010 and culminated with an eruption in 2012, after several years of relative stability, still maintains a moderate alert, as required by the high seismicity and SO 2 degassing. In October 2013, a sampling campaign has been performed on thermal springs and stream water, located at 2600–5000 m of elevation on the slope of Nevado del Ruiz, analyzed for water chemistry and stable isotopes. Some of these waters are typically steam-heated (low pH and high sulfate content) by the vapour probably separating from a zoned hydrothermal system. By applying a model of steam-heating, based on mass and enthalpy balances, we have estimated the mass rate of hydrothermal steam discharging in the different springs. The composition of the hottest thermal spring (Botero Londono) is probably representative of a marginal part of the hydrothermal system, having a temperature of 250 °C and low salinity (Cl ~ 1500 mg/l), which suggest, along with the retrieved isotope composition, a chiefly meteoric origin. The vapour discharged at the steam vent “Nereidas” (3600 m asl) is hypothesized to be separated from a high-temperature hydrothermal system. Based on its composition and on literature data on fluid inclusions, we have retrieved the P-T-X conditions of the deep hydrothermal system, as well as its pH and f O 2 . The vapour feeding Nereidas would separate from a biphasic hydrothermal system characterized by the following parameters: t = 315 °C, P = 15 MPa, NaCl = 10 wt%, CO 2 = 5 wt%, and similar proportion between liquid and vapour. Considering also the equilibria involving S-bearing gases and HCl, pH would approach the value of 1.5 while f O 2 would correspond to the FeO-Fe 2 O 3 buffer. Chlorine content is estimated at 10,300 mg/l. Changes in the magmatic input into the hydrothermal system could modify its degree of vapourization and/or P-T-X conditions, thus inducing corresponding variations in vapour discharges and thermal waters. These findings, paralleled by contemporary measurements of water flow rates, could give significant clues on risk evaluation.

Cerro Machin volcano in Colombia recently (2009–2013) exhibited new seismic activity. A geochemical characterization of emitted fluids was carried out based on the chemical and isotopic compositions of fumaroles and thermal springs discharged in this volcanic area with the aim of improving the volcano monitoring program. The isotopic composition of fumaroles located in the upper part of the dome was characterized by depleted δD and δ 18 O relative to the meteoric recharge fluids, which is due to a separation of the liquid phase in the lower part of the dome. A clear magmatic He signature was found in the fumaroles, with an increased magmatic contribution observed in the discharged fluids during 2011–2013 corroborating the increase in recorded seismic activity. Coupling the geochemical and seismic information has highlighted a clear awakening of Cerro Machin volcanic activity, indicating that this volcano is still active deserve an improvement of volcanic monitoring activity by the scientific community.

Studying spatial and temporal trends in volcanic gas compositions and fluxes is crucial both to volcano monitoring and to constrain the origin and recycling efficiency of volatiles at active convergent margins. New volcanic gas compositions and volatile fluxes are here reported for Nevado del Ruiz, Galeras, and Purace, three of the most persistently degassing volcanoes located in the Colombian Arc Segment of the Northern Volcanic Zone. At Nevado del Ruiz, from 2014 to 2017, plume emissions showed an average molar CO2/S-T ratio of 3.9 +/- 1.6 (S-T is total sulfur, S). Contemporary, fumarolic chemistry at Galeras progressively shifted toward low-temperature, S-depleted fumarolic gas discharges with an average CO2/S-T ratio in excess of 10 (6.0-46.0, 2014-2017). This shift in volcanic gas compositions was accompanied by a concurrent decrease in SO2 emissions, confirmed on 21 March 2017 by high-resolution ultraviolet camera-based SO2 fluxes of similar to 2.5 kg/s (similar to 213 t/day). For comparison, SO2 emissions remained high at Nevado del Ruiz (weighted average of 8 kg/s) between 2014 and 2017, while Purace maintained rather low emission levels (

Scanning Differential Optical Absorption Spectroscopy (DOAS) networks using scattered solar radiation have become an increasingly important tool for monitoring volcanic sulphur dioxide (SO2) emissions. In order to get absolute column densities (CDs), the DOAS evaluation requires a Fraunhofer Reference Spectrum (FRS) that is free of absorption structures of the trace gas of interest. At volcanoes, this requirement can be formulated in a weaker form, if there is a plume free viewing direction within the spectra of a scan through the complete sky. In this case, it is possible to use a specific viewing direction (e.g. zenith) as FRS and correcting for possible plume contamination in the FRS by calculating and subtracting an SO2 offset (e.g. the lowest SO2 CD) from all viewing directions of the respective scan. This procedure is followed in the standard evaluations of data from the Network for Observation of Volcanic and Atmospheric Change (NOVAC). While this procedure is very efficient in removing Fraunhofer structures and instrumental effects it has the disadvantage that one can never be sure that there is no SO2 from the plume in the FRS. Therefore, using a modelled FRS (based on a high-resolution Solar atlas) is of great advantage. We followed this approach and investigated an SO2 retrieval algorithm using a modelled FRS. In this manuscript, we present results from two volcanoes that are monitored by NOVAC stations and which also often show a large volcanic plume. Results from a DOAS SO2 evaluation using a modelled FRS are presented for data from Nevado del Ruiz (Colombia) recorded between January 2010 and June 2012 and from Tungurahua (Ecuador) recorded between January 2009 and December 2011. Instrumental effects were identified with help of a Principal Component Analysis (PCA) of the residual structures of the DOAS evaluation. The SO2 retrieval performed extraordinarily well with an SO2 DOAS retrieval error of 1−2 × 1016 [molecules/cm2]. Compared to a regular evaluation (using a FRS recorded directly before the scan), we found systematic differences of the differential Slant Column Density (dSCD) of only up to 15 % when looking at the variation of the SO2 within one scan. The major advantage of our new retrieval is that it yields absolute SO2 CDs and that it does not require complicated instrumental calibration in the field, since the method exploits the information available in the measurements.

International audience; The geochemical behaviour of Rare Earth Elements, Zr and Hf was investigated in the thermal waters of Nevado del Ruiz volcano system. A wide range of pH, between 1.0 and 8.8, characterizes these fluids. The acidic waters are sulphate dominated with different Cl/SO4 ratios. The important role of the pH and the ionic complexes for the distribution of REE, Zr and Hf in the aqueous phase was evidenced. The pH rules the precipitation of authigenic Fe and Al oxyhydroxides producing changes in REE, Zr, Hf amounts and strong anomalies of Cerium. The precipitation of alunite and jarosite removes LREE from the solution, changing the REE distribution in acidic waters.Y–Ho and Zr–Hf (twin pairs) have a different behaviour in strong acidic waters with respect to the water with pH near-neutral. Yttrium and Ho behave as Zr and Hf in waters with pH near neutral-to-neutral, showing super-chondritic ratios. The twin pairs showed to be sensitive to the co-precipitation and/or adsorption onto the surface of authigenic particulate (Fe-, Al-oxyhydroxides), suggesting an enhanced scavenging of Ho and Hf with respect to Y and Zr, leading to superchondritic values. In acidic waters, a different behaviour of twin pairs occurs with chondritic Y/Ho ratios and sub-chondritic Zr/Hf ratios. For the first time, Zr and Hf were investigated in natural acidic fluids to understand the behaviour of these elements in extreme acidic conditions and different major anion chemistry. Zr/Hf molar ratio changes from 4.75 to 49.29 in water with pH < 3.6. In strong acidic waters the fractionation of Zr and Hf was recognized as function of major anion contents (Cl and SO4), suggesting the formation of complexes leading to sub-chondritic Zr/Hf molar ratios.