scholarly journals On the discrepancy of HCl processing in the core of the wintertime polar vortices

2018 ◽  
Vol 18 (12) ◽  
pp. 8647-8666 ◽  
Author(s):  
Jens-Uwe Grooß ◽  
Rolf Müller ◽  
Reinhold Spang ◽  
Ines Tritscher ◽  
Tobias Wegner ◽  
...  
Keyword(s):  
Cosmic Rays ◽  
Polar Vortex ◽  
Galactic Cosmic Rays ◽  
Lagrangian Model ◽  
The Arctic ◽  
Late Winter ◽  
Model Simulations ◽  
Ozone Loss ◽  
The Antarctic ◽  
Eulerian Models

Abstract. More than 3 decades after the discovery of the ozone hole, the processes involved in its formation are believed to be understood in great detail. Current state-of-the-art models can reproduce the observed chemical composition in the springtime polar stratosphere, especially regarding the quantification of halogen-catalysed ozone loss. However, we report here on a discrepancy between simulations and observations during the less-well-studied period of the onset of chlorine activation. During this period, which in the Antarctic is between May and July, model simulations significantly overestimate HCl, one of the key chemical species, inside the polar vortex during polar night. This HCl discrepancy is also observed in the Arctic. The discrepancy exists in different models to varying extents; here, we discuss three independent ones, the Chemical Lagrangian Model of the Stratosphere (CLaMS) as well as the Eulerian models SD-WACCM (the specified dynamics version of the Whole Atmosphere Community Climate Model) and TOMCAT/SLIMCAT. The HCl discrepancy points to some unknown process in the formulation of stratospheric chemistry that is currently not represented in the models. We characterise the HCl discrepancy in space and time for the Lagrangian chemistry–transport model CLaMS, in which HCl in the polar vortex core stays about constant from June to August in the Antarctic, while the observations indicate a continuous HCl decrease over this period. The somewhat smaller discrepancies in the Eulerian models SD-WACCM and TOMCAT/SLIMCAT are also presented. Numerical diffusion in the transport scheme of the Eulerian models is identified to be a likely cause for the inter-model differences. Although the missing process has not yet been identified, we investigate different hypotheses on the basis of the characteristics of the discrepancy. An underestimated HCl uptake into the polar stratospheric cloud (PSC) particles that consist mainly of H2O and HNO3 cannot explain it due to the temperature correlation of the discrepancy. Also, a direct photolysis of particulate HNO3 does not resolve the discrepancy since it would also cause changes in chlorine chemistry in late winter which are not observed. The ionisation caused by galactic cosmic rays provides an additional NOx and HOx source that can explain only about 20 % of the discrepancy. However, the model simulations show that a hypothetical decomposition of particulate HNO3 by some other process not dependent on the solar elevation, e.g. involving galactic cosmic rays, may be a possible mechanism to resolve the HCl discrepancy. Since the discrepancy reported here occurs during the beginning of the chlorine activation period, where the ozone loss rates are small, there is only a minor impact of about 2 % on the overall ozone column loss over the course of Antarctic winter and spring.

scholarly journals On the discrepancy of HCl processing in the dark polar vortices

2018 ◽  
Author(s):  
Jens-Uwe Grooß ◽  
Rolf Müller ◽  
Reinhold Spang ◽  
Ines Tritscher ◽  
Tobias Wegner ◽  
...  
Keyword(s):  
Cosmic Rays ◽  
Transport Model ◽  
Polar Vortex ◽  
Galactic Cosmic Rays ◽  
The Arctic ◽  
Late Winter ◽  
Chemistry Transport Model ◽  
Ozone Loss ◽  
The Antarctic ◽  
Eulerian Models

Abstract. More than three decades after the discovery of the ozone hole, the processes involved in its formation are believed to be understood in great detail. Current state-of-the-art models are able to reproduce the observed chemical composition in the springtime polar stratosphere, especially regarding the quantification of halogen-catalysed ozone loss. However, here we report on a discrepancy between simulations and observations during the less-well studied period of the onset of chlorine activation. During this period, which in the Antarctic is between May and July, model simulations significantly overestimate HCl, one of the key chemical species, inside the polar vortex during polar night. This HCl discrepancy is also observed in the Arctic and present, to varying extents, in three independent models, the Lagrangian chemistry transport model CLaMS as well as the Eulerian models WACCM and TOMCAT/SLIMCAT. The HCl discrepancy points to some unknown process in the formulation of stratospheric chemistry that is currently not represented in the models. Here we characterise the HCl discrepancy in space and time for the Lagrangian Chemistry Transport Model CLaMS, in which HCl in the polar vortex core stays about constant from June to August in the Antarctic while the observations indicate a continuous HCl decrease over this period. The somewhat smaller discrepancies in the models WACCM and TOMCAT/SLIMCAT are also presented. Numerical diffusion in the Eulerian models is identified to be a likely cause for the inter-model differences. Although the missing process has not yet been identified, we investigate different hypotheses on the basis of the characteristics of the discrepancy. An under-estimated uptake of HCl into the PSC particles that consist mainly of H2O and HNO3 cannot explain the discrepancy due to the temperature correlation of the discrepancy. Also, a direct photolysis of particulate HNO3 does not explain the discrepancy since it would also cause changes in late winter which are not observed. The ionisation caused by Galactic Cosmic Rays provides an additional NOx and HOx source that can explain only around 20 % of the discrepancy. A hypothetical decomposition of particulate HNO3 by some other process not dependent on the solar elevation, e.g. involving Galactic Cosmic Rays, may be a possible mechanism to resolve the HCl discrepancy. Since the discrepancy reported here occurs during the beginning of the chlorine activation period, where the ozone loss rates are slow, there is only a minor impact of about 2 % on the overall ozone column loss over the course of Antarctic winter and spring.

scholarly journals The impact of mid-latitude intrusions into the polar vortex on ozone loss estimates

2002 ◽  
Vol 2 (6) ◽  
pp. 2489-2506
Author(s):  
J.-U. Grooß ◽  
R. Müller
Keyword(s):  
Loss Rate ◽  
Polar Vortex ◽  
Lagrangian Model ◽  
The Arctic ◽  
Mixing Ratio ◽  
Match Method ◽  
Air Masses ◽  
Model Simulations ◽  
Ozone Loss ◽  
The Impact

Abstract. Current stratospheric chemical model simulations underestimate substantially the large ozone loss rates that are derived for the Arctic from ozone sondes for January of some years. Until now, no explanation for this discrepancy has been found. Here, we examine the influence of intrusions of mid-latitude air into the polar vortex on these ozone loss estimates. This study focuses on the winter 1991/92. It is based on simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulations for January 1992 show that the intrusions induce a reduction of vortex average ozone mixing ratio corresponding to a systematic offset of the ozone loss rate of about 12 ppb per day. Further, the results of the Match method are influenced by the intrusions, since the intruded air masses are deformed and reach dimensions below the Match radius. From our calculations we deduce a systematic offset of the Match ozone loss rate by about 10 ppb/day, which may explain about 28% of the published discrepancy between Match and box model simulations for the winter 1991/92.

scholarly journals Chemical ozone loss and ozone mini-hole event during the Arctic winter 2010/2011 as observed by SCIAMACHY and GOME-2

2014 ◽  
Vol 14 (7) ◽  
pp. 3247-3276 ◽  
Author(s):  
R. Hommel ◽  
K.-U. Eichmann ◽  
J. Aschmann ◽  
K. Bramstedt ◽  
M. Weber ◽  
...  
Keyword(s):  
Transport Model ◽  
Polar Vortex ◽  
The Arctic ◽  
Optical Absorption Spectroscopy ◽  
Late Winter ◽  
Total Column Ozone ◽  
Bromine Oxide ◽  
Ozone Loss ◽  
Catalytic Cycles ◽  
Total Column

Abstract. Record breaking loss of ozone (O3) in the Arctic stratosphere has been reported in winter–spring 2010/2011. We examine in detail the composition and transformations occurring in the Arctic polar vortex using total column and vertical profile data products for O3, bromine oxide (BrO), nitrogen dioxide (NO2), chlorine dioxide (OClO), and polar stratospheric clouds (PSC) retrieved from measurements made by SCIAMACHY (Scanning Imaging Absorption SpectroMeter for Atmospheric CHartography) on-board Envisat (Environmental Satellite), as well as total column ozone amount, retrieved from the measurements of GOME-2 (Global Ozone Monitoring Experiment) on MetOp-A (Meteorological Experimental Satellite). Similarly we use the retrieved data from DOAS (Differential Optical Absorption Spectroscopy) measurements made in Ny-Ålesund (78.55° N, 11.55° E). A chemical transport model (CTM) has been used to relate and compare Arctic winter–spring conditions in 2011 with those in the previous year. In late winter–spring 2010/2011 the chemical ozone loss in the polar vortex derived from SCIAMACHY observations confirms findings reported elsewhere. More than 70% of O3 was depleted by halogen catalytic cycles between the 425 and 525 K isentropic surfaces, i.e. in the altitude range ~16–20 km. In contrast, during the same period in the previous winter 2009/2010, a typical warm Arctic winter, only slightly more than 20% depletion occurred below 20 km, while 40% of O3 was removed above the 575 K isentrope (~23 km). This loss above 575 K is explained by the catalytic destruction by NOx descending from the mesosphere. In both Arctic winters 2009/2010 and 2010/2011, calculated O3 losses from the CTM are in good agreement to our observations and other model studies. The mid-winter 2011 conditions, prior to the catalytic cycles being fully effective, are also investigated. Surprisingly, a significant loss of O3 around 60%, previously not discussed in detail, is observed in mid-January 2011 below 500 K (~19 km) and sustained for approximately 1 week. The low O3 region had an exceptionally large spatial extent. The situation was caused by two independently evolving tropopause elevations over the Asian continent. Induced adiabatic cooling of the stratosphere favoured the formation of PSC, increased the amount of active chlorine for a short time, and potentially contributed to higher polar ozone loss later in spring.

scholarly journals The impact of mid-latitude intrusions into the polar vortex on ozone loss estimates

2003 ◽  
Vol 3 (2) ◽  
pp. 395-402 ◽  
Author(s):  
J.-U. Grooß ◽  
R. Müller
Keyword(s):  
Large Scale ◽  
Loss Rate ◽  
Polar Vortex ◽  
Control Measures ◽  
Lagrangian Model ◽  
The Arctic ◽  
Match Method ◽  
Ozone Loss ◽  
The Impact ◽  
Loss Rates

Abstract. Current stratospheric chemical model simulations underestimate substantially the large ozone loss rates that are derived for the Arctic from ozone sondes for January of some years. Until now, no explanation for this discrepancy has been found. Here, we examine the influence of intrusions of mid-latitude air into the polar vortex on these ozone loss estimates. This study focuses on the winter 1991/92, because during this winter the discrepancy between simulated and experimentally derived ozone loss rates is reported to be the largest. Also during the considered period the vortex was disturbed by a strong warming event with large-scale intrusions of mid-latitude air into the polar vortex, which is quite unusual for this time of the year. The study is based on simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). Two methods for determination the ozone loss are investigated, the so-called vortex average approach and the Match method. The simulations for January 1992 show that the intrusions induce a reduction of vortex average ozone mixing ratio corresponding to a systematic offset of the ozone loss rate of about 12 ppb per day. This should be corrected for in the vortex average method. The simulations further suggest, that these intrusions do not cause a significant bias for the Match method due to effective quality control measures in the Match technique.

scholarly journals Comparison of Inorganic Chlorine in the Southern Hemispheric lowermost stratosphere during Late Winter 2019

2021 ◽  
Author(s):  
Markus Jesswein ◽  
Heiko Bozem ◽  
Hans-Christoph Lachnitt ◽  
Peter Hoor ◽  
Thomas Wagenhäuser ◽  
...  
Keyword(s):  
Degradation Products ◽  
Polar Vortex ◽  
Boundary Region ◽  
Early Spring ◽  
Active Chlorine ◽  
The Arctic ◽  
Late Winter ◽  
Annual Variations ◽  
The Difference ◽  
The Antarctic

Abstract. Inorganic chlorine (Cly) is the sum of the degradation products of long-lived chlorinated source gases. These include the reservoir species (HCl and ClONO2) and active chlorine species (i.e. ClOx). The active chlorine species drive catalytic cycles that deplete ozone in the polar winter stratosphere. This work presents calculations of inorganic chlorine (Cly) derived from chlorinated source gas measurements on board the High Altitude and Long Range Research Aircraft (HALO) during the Southern hemisphere Transport, Dynamic and Chemistry (SouthTRAC) campaign in late winter and early spring 2019. Results are compared to Cly of the Northern Hemisphere derived from measurements of the POLSTRACC-GW-LCYCLE-SALSA (PGS) campaign in the Arctic winter of 2015/2016. A scaled correlation was used for PGS data, since not all source gases were measured. Cly from a scaled correlation was compared to directly determined Cly and agreed well. An air mass classification based on in situ N2O measurements allocates the measurements to the vortex, the vortex boundary region, and mid-latitudes. Although the Antarctic vortex was weakened in 2019 compared to previous years, Cly reached 1687 ± 20 ppt at 385 K, therefore up to around 50 % of total chlorine could be found in inorganic form inside the Antarctic vortex, whereas only 15 % of total chlorine could be found in inorganic form in the southern mid-latitudes. In contrast, only 40 % of total chlorine could be found in inorganic form in the Arctic vortex during PGS and roughly 20 % in the northern mid-latitudes. Differences inside the respective vortex reaches up to 565 ppt more Cly in the Antarctic vortex 2019 than in the Arctic vortex 2016 (at comparable distance to the local tropopause). As far as is known, this is the first comparison of inorganic chlorine within the respective polar vortex. Based on the results of these two campaigns, the difference of Cly inside the respective vortex is significant and larger than reported inter annual variations.

scholarly journals Mixing and Chemical Ozone Loss during and after the Antarctic Polar Vortex Major Warming in September 2002

2005 ◽  
Vol 62 (3) ◽  
pp. 848-859 ◽  
Author(s):  
Paul Konopka ◽  
Jens-Uwe Grooß ◽  
Karl W. Hoppel ◽  
Hildegard-Maria Steinhorst ◽  
Rolf Müller
Keyword(s):  
Potential Temperature ◽  
Polar Vortex ◽  
Vertical Shear ◽  
Lagrangian Model ◽  
Ozone Loss ◽  
Time Period ◽  
The Difference ◽  
Antarctic Polar Vortex ◽  
The Antarctic ◽  
Vortex Split

Abstract The 3D version of the Chemical Lagrangian Model of the Stratosphere (CLAMS) is used to study the transport of CH4 and O3 in the Antarctic stratosphere between 1 September and 30 November 2002, that is, over the time period when unprecedented major stratospheric warming in late September split the polar vortex into two parts. The isentropic and cross-isentropic velocities in CLAMS are derived from ECMWF winds and heating/cooling rates calculated with a radiation module. The irreversible part of transport, that is, mixing, is driven by the local horizontal strain and vertical shear rates with mixing parameters deduced from in situ observations. The CH4 distribution after the vortex split shows a completely different behavior above and below 600 K. Above this potential temperature level, until the beginning of November, a significant part of vortex air is transported into the midlatitudes up to 40°S. The lifetime of the vortex remnants formed after the vortex split decreases with the altitude with values of about 3 and 6 weeks at 900 and 700 K, respectively. Despite this enormous dynamical disturbance of the vortex, the intact part between 400 and 600 K that “survived” the major warming was strongly isolated from the extravortex air until the end of November. According to CLAMS simulations, the air masses within this part of the vortex did not experience any significant dilution with the midlatitude air. By transporting ozone in CLAMS as a passive tracer, the chemical ozone loss was estimated from the difference between the observed [Polar Ozone and Aerosol Measurement III (POAM III) and Halogen Occultation Experiment (HALOE)] and simulated ozone profiles. Starting from 1 September, up to 2.0 ppmv O3 around 480 K and about 70 Dobson units between 450 and 550 K were destroyed until the vortex was split. After the major warming, no additional ozone loss can be derived, but in the intact vortex part between 450 and 550 K, the accumulated ozone loss was “frozen in” until the end of November.

scholarly journals Chemical ozone loss in Arctic and Antarctic polar winter/spring season derived from SCIAMACHY limb measurements 2002–2009

2011 ◽  
Vol 11 (2) ◽  
pp. 6555-6599 ◽  
Author(s):  
T. Sonkaew ◽  
C. von Savigny ◽  
K.-U. Eichmann ◽  
M. Weber ◽  
A. Rozanov ◽  
...  
Keyword(s):  
Mass Loss ◽  
Total Ozone ◽  
Stratospheric Ozone ◽  
Polar Vortex ◽  
The Arctic ◽  
Absorption Bands ◽  
Data Set ◽  
Ozone Loss ◽  
The Difference ◽  
The Antarctic

Abstract. Stratospheric ozone profiles are retrieved for the period 2002–2009 from SCIAMACHY measurements of limb-scattered solar radiation in the Hartley and Chappuis absorption bands of ozone. This data set is used to determine the chemical ozone loss in both the Arctic and Antarctic polar vortices using the vortex average method. The chemical ozone loss at isentropic levels between 450 K and 600 K is derived from the difference between observed ozone abundances and the ozone modelled considering diabatic cooling, but no chemical ozone loss. The results show chemical ozone losses of up to 20–40% between the beginning of January and the end of March inside the Arctic polar vortex. Strong inter-annual variability of the Arctic ozone loss is observed, with the cold winters 2004/2005 and 2006/2007 showing the largest chemical ozone losses. The ozone mass loss inside the polar vortex is also estimated. In the coldest Arctic winter 2004/2005 the total ozone mass loss is about 30 million tons inside the polar vortex between the 450 K and 600 K isentropic levels from the beginning of January until the end of March. The Antarctic vortex averaged ozone loss as well as the size of the polar vortex do not vary much from year to year. At the 475 K isentropic level ozone losses of 70–80% between mid-August and mid-November are observed every year inside the vortex, also in the anomalous year 2002. The total ozone mass loss inside the Antarctic polar vortex between the 450 K and 600 K isentropic levels is about 55–75 million tons for the period between mid-August and mid-November. Comparisons of the vertical variation of ozone loss derived from SCIAMACHY observations with several independent techniques for the Arctic winter 2004/2005 show very good agreement.

scholarly journals Dynamical Elliptical Diagnostics of the Antarctic Polar Vortex

2019 ◽  
Vol 77 (3) ◽  
pp. 1167-1180
Author(s):  
M. Mester ◽  
J. G. Esler
Keyword(s):  
Data Assimilation ◽  
Polar Vortex ◽  
The Arctic ◽  
Late Winter ◽  
Phase Plane Analysis ◽  
Background Flow ◽  
Planetary Scale ◽  
Plane Analysis ◽  
Antarctic Polar Vortex ◽  
The Antarctic

Abstract Elliptical diagnostics provide dynamical and climatological information about the behavior of the Arctic and Antarctic stratospheric polar vortices. Here Kida’s model, describing the evolution of a uniform vortex in a linear, but possibly unsteady, background flow, is used to interpret the observed evolution of the Antarctic vortex in late winter during 1999–2018. Kida’s model has oscillatory solutions that can undergo an amplitude bifurcation, which serves as a simple model for the onset of vortex-splitting stratospheric sudden warmings (SSWs). A data assimilation method is used to find solutions of Kida’s equations consistent with the observations. A phase-plane analysis reveals large interannual variability in the amplitude of oscillations of the vortex. In 2002, the year of the only observed vortex-splitting Antarctic SSW, the system is found to cross a separatrix in phase space, associated with the SSW amplitude bifurcation, in late September. An output of the data assimilation is the linear background flow experienced by the vortex. The rotational component of this linear flow is consistent with the vortex being embedded in an anticyclonic background. The time-mean strain flow is weak but has a clear orientation, consistent with the presence of stationary forcing due to planetary-scale topography and land–sea contrast. The time-varying strain flow is comparatively large in magnitude, illustrating the relative importance of the planetary-scale component of the turbulent dynamics occurring at tropopause level. Unlike in the Northern Hemisphere, therefore, the direction of future Antarctic vortex splits will not necessarily align with the direction of the 2002 split.

scholarly journals The implementation of the CLaMS Lagrangian transport core into the chemistry climate model EMAC 2.40.1: application on age of air and transport of long-lived trace species

2014 ◽  
Vol 7 (2) ◽  
pp. 1759-1790 ◽  
Author(s):  
C. M. Hoppe ◽  
L. Hoffmann ◽  
P. Konopka ◽  
J.-U. Grooß ◽  
F. Ploeger ◽  
...  
Keyword(s):  
Coupled Model ◽  
Polar Vortex ◽  
Model System ◽  
Lagrangian Model ◽  
The Arctic ◽  
Trace Gas ◽  
Late Winter ◽  
Tracer Transport ◽  
Lagrangian Transport ◽  
Airborne Measurements

Abstract. Lagrangian transport schemes have proven to be useful tools for modelling stratospheric trace gas transport since they are less diffusive than classical Eulerian schemes and therefore especially well suited for maintaining steep tracer gradients. Here, we present the implementation of the full-Lagrangian transport core of the Chemical Lagrangian Model of the Stratosphere (CLaMS) into the ECHAM/MESSy Atmospheric Chemistry model (EMAC). We performed a ten-year time-slice simulation to evaluate the coupled model system EMAC/CLaMS. Simulated zonal mean age of air distributions are compared to age of air derived from airborne measurements, showing a good overall representation of the stratospheric circulation. Results from the new Lagrangian transport scheme are compared to tracer distributions calculated with the standard flux-form semi-Lagrangian (FFSL) transport scheme in EMAC. The differences in the resulting tracer distributions are most pronounced in the regions of strong transport barriers. The polar vortices are presented as an example and simulated trace gas distributions are compared to satellite measurements. The analysis of CFC-11, N2O, CH4, and age of air in the polar vortex regions shows that the CLaMS Lagrangian transport scheme produces a stronger, more realistic transport barrier at the edge of the polar vortex than the FFSL transport scheme of EMAC. Differences in simulated age of air range up to one year in the Arctic polar vortex in late winter/early spring. The new coupled model system EMAC/CLaMS thus constitutes a suitable tool for future model studies of stratospheric tracer transport.

scholarly journals Dynamics and chemistry of vortex remnants in late Arctic spring 1997 and 2000: Simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS)

2003 ◽  
Vol 3 (3) ◽  
pp. 839-849 ◽  
Author(s):  
P. Konopka ◽  
J.-U. Grooß ◽  
S. Bausch ◽  
R. Müller ◽  
D. S. McKenna ◽  
...  
Keyword(s):  
Ozone Depletion ◽  
Polar Vortex ◽  
Lagrangian Model ◽  
The Arctic ◽  
Summer Circulation ◽  
Air Masses ◽  
Ozone Loss ◽  
Mixing Ratios ◽  
Photochemical Decomposition ◽  
The Impact

Abstract. High-resolution simulations of the chemical composition of the Arctic stratosphere during late spring 1997 and 2000 were performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulations were performed for the entire northern hemisphere on two isentropic levels 450 K (~18 km) and 585 K (~24 km). The spatial distribution and the lifetime of the vortex remnants formed after the vortex breakup in May 1997 display different behavior above and below 20 km. Above 20 km, vortex remnants propagate southward (up to 40°N) and are "frozen in'' in the summer circulation without significant mixing. Below 20 km the southward propagation of the remnants is bounded by the subtropical jet. Their lifetime is shorter by a factor of 2 than that above 20 km, owing to significant stirring below this altitude. The behavior of vortex remnants formed in March 2000 is similar but, due to an earlier vortex breakup, dominated during the first 6 weeks after the vortex breakup by westerly winds, even above 20 km. Vortex remnants formed in May 1997 are characterized by large mixing ratios of HCl indicating negligible, halogen-induced ozone loss. In contrast, mid-latitude ozone loss in late boreal spring 2000 is dominated, until mid-April, by halogen-induced ozone destruction within the vortex remnants, and subsequent transport of the ozone-depleted polar air masses (dilution) into the mid-latitudes. By varying the intensity of mixing in CLaMS, the impact of mixing on the formation of ClONO2 and ozone depletion is investigated. We find that the photochemical decomposition of HNO3 and not mixing with NOx-rich mid-latitude air is the main source of NOx within the vortex remnants in March and April 2000. Ozone depletion in the remnants is driven by ClOx photolytically formed from ClONO2. At the end of May 1997, the halogen-induced ozone deficit at 450 K poleward of 30°N amounts to ~12% with ~10% in the polar vortex and ~2% in well-isolated vortex remnants after the vortex breakup.

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