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DOE OSTI2020

Antioxidant Activity in Supramolecular Carotenoid Complexes Favored by Nonpolar Environment and Disfavored by Hydrogen Bonding

Carotenoids are well-known antioxidants. They have the ability to quench singlet oxygen and scavenge toxic free radicals preventing or reducing damage to living cells. We have found that carotenoids exhibit scavenging ability towards free radicals that increases nearly exponentially with increasing the carotenoid oxidation potential. With the oxidation potential being an important parameter in predicting antioxidant activity, we focus here on the different factors affecting it. This paper examines how the chain length and donor/acceptor substituents of carotenoids affect their oxidation potentials but, most importantly, presents the recent progress on the effect of polarity of the environment and orientation of the carotenoids on the oxidation potential in supramolecular complexes. The oxidation potential of a carotenoid in a nonpolar environment was found to be higher than in a polar environment. Moreover, in order to increase the photostability of the carotenoids in supramolecular complexes, a nonpolar environment is desired and the formation of hydrogen bonds should be avoided.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Aerosol meteorology of Maritime Continent for the 2012 7SEAS southwest monsoon intensive study – Part 2: Philippine receptor observations of fine-scale aerosol behavior

The largest 7 Southeast Asian Studies (7SEAS) operations period within the Maritime Continent (MC) occurred in the August–September 2012 biomass burning season. Data included were observations aboard the M/Y Vasco , dispatched to the Palawan Archipelago and Sulu Sea of the Philippines for September 2012. At these locations, the Vasco observed MC smoke and pollution entering the southwest monsoon (SWM) monsoonal trough. Here we describe the research cruise findings and the finer-scale aerosol meteorology of this convectively active region. This 2012 cruise complemented a 2-week cruise in 2011 and was generally consistent with previous findings in terms of how smoke emission and transport related to monsoonal flows, tropical cyclones (TC), and the covariance between smoke transport events and the atmosphere's thermodynamic structure. Biomass burning plumes were usually mixed with significant amounts of anthropogenic pollution. Also key to aerosol behavior were squall lines and cold pools propagating across the South China Sea (SCS) and scavenging aerosol particles in their path. However, the 2012 cruise showed much higher modulation in aerosol frequency than its 2011 counterpart. Whereas in 2011 large synoptic-scale aerosol events transported high concentrations of smoke into the Philippines over days, in 2012 measured aerosol events exhibited a much shorter-term variation, sometimes only 3$-$12 h. Strong monsoonal flow reversals were also experienced in 2012. Nucleation events in cleaner and polluted conditions, as well as in urban plumes, were observed. Perhaps most interestingly, several cases of squall lines preceding major aerosol events were observed, as opposed to 2011 observations where these lines largely scavenged aerosol particles from the marine boundary layer. Combined, these observations indicate pockets of high and low particle counts that are not uncommon in the region. These perturbations are difficult to observe by satellite and very difficult to model. Indeed, the Navy Aerosol Analysis and Prediction System (NAAPS) simulations captured longer period aerosol events quite well but largely failed to capture the timing of high-frequency phenomena. Ultimately, the research findings of these cruises demonstrate the real world challenges of satellite-based missions, significant aerosol life cycle questions such as those the future Aerosol/Clouds/Ecosystems (ACE) will investigate, and the importance of small-scale phenomena such as sea breezes, squall lines, and nucleation events embedded within SWM patterns in dominating aerosol life cycle and potential relationships to clouds.

aerosols↗

DOE OSTI2018

Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes

The response of marine low cloud systems to changes in aerosol concentrationrepresents one of the largest uncertainties in climate simulations. Majorcontributions to this uncertainty are derived from poor understanding of aerosolunder natural conditions and the perturbation by anthropogenic emissions. Theeastern North Atlantic (ENA) is a region of persistent but diverse marineboundary layer (MBL) clouds, whose albedo and precipitation are highlysusceptible to perturbations in aerosol properties. In this study, we examineMBL aerosol properties, trace gas mixing ratios, and meteorologicalparameters measured at the Atmospheric Radiation Measurement Climate ResearchFacility's ENA site on Graciosa Island, Azores, Portugal, during a 3-yearperiod from 2015 to 2017. Measurements impacted by local pollution onGraciosa Island and during occasional intense biomass burning and dust eventsare excluded from this study. Submicron aerosol size distribution typicallyconsists of three modes: Aitken (At, diameter <~100 nm),accumulation (Ac, D p within ~100 to ~300 nm), andlarger accumulation (LA, D p > ~ 300 nm) modes, with averagenumber concentrations (denoted as N At , N Ac , and N LA below) of 330, 114, and 14 cm -3 , respectively. N At , N Ac , and N LA show contrasting seasonalvariations, suggesting different sources and removal processes. N LA is dominated by sea spray aerosol (SSA) and is higher in winter andlower in summer. This is due to the seasonal variations of SSA production,in-cloud coalescence scavenging, and dilution by entrained free troposphere(FT) air. In comparison, SSA typically contributes a relatively minorfraction to N At (10 %) and N Ac (21 %) on an annual basis. Inaddition to SSA, sources of Ac-mode particles include entrainment of FTaerosols and condensation growth of Aitken-mode particles inside the MBL, whilein-cloud coalescence scavenging is the major sink of N Ac . The observedseasonal variation of N Ac , being higher in summer and lower in winter,generally agrees with the steady-state concentration estimated from majorsources and sinks. N At is mainly controlled by entrainment of FTaerosol, coagulation loss, and growth of Aitken-mode particles into theAc-mode size range. Our calculation suggests that besides the directcontribution from entrained FT Ac-mode particles, growth of entrained FTAitken-mode particles in the MBL also represent a substantial source ofcloud condensation nuclei (CCN), with the highest contribution potentiallyreaching 60 % during summer. The growth of Aitken-mode particles to CCN sizeis an expected result of the condensation of sulfuric acid, a product fromdimethyl sulfide oxidation, suggesting that ocean ecosystems may have asubstantial influence on MBL CCN populations in the ENA.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Seasonal variations in fire conditions are important drivers in the trend of aerosol optical properties over the south-eastern Atlantic

Abstract. From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MACBC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MACBC, providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Tropospheric aerosols over the western North Atlantic Ocean during the winter and summer deployments of ACTIVATE 2020: life cycle, transport, and distribution

The Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) is a NASA mission to characterize aerosol–cloud interactions over the western North Atlantic Ocean (WNAO). Such characterization requires understanding of life cycle, composition, transport pathways, and distribution of aerosols over the WNAO. This study uses the GEOS-Chem model to simulate aerosol distributions and properties that are evaluated against aircraft, ground-based, and satellite observations during the winter and summer field deployments in 2020 of ACTIVATE. Transport in the boundary layer (BL) behind cold fronts was a major mechanism for the North American continental outflow of pollution to the WNAO in winter. Turbulent mixing was the main driver for the upward transport of sea salt within and ventilation out of BL in winter. The BL aerosol composition was dominated by sea salt, which increased in the summer, followed by organics and sulfate. Aircraft in situ aerosol measurements provided useful constraints on wet scavenging in GEOS-Chem. The model generally captured observed features such as continental outflow, land–ocean gradient, and mixing of anthropogenic aerosols with sea salt. Model sensitivity experiments with elevated smoke injection heights to the mid-troposphere (versus within BL) better reproduced observations of smoke aerosols from the western US wildfires over the WNAO in the summer. Model analysis suggests strong hygroscopic growth of sea salt particles and their seeding of marine BL clouds over the WNAO (< 35° N). Future modeling efforts should focus on improving parameterizations for aerosol wet scavenging, implementing realistic smoke injection heights, and applying high-resolution models that better resolve vertical transport.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

Description and evaluation of a new four-mode version of the Modal Aerosol Module (MAM4) within version 5.3 of the Community Atmosphere Model

Atmospheric carbonaceous aerosols play an important role in the climate system by influencing the Earth's radiation budgets and modifying the cloud properties. Despite the importance, their representations in large-scale atmospheric models are still crude, which can influence model simulated burden, lifetime, physical, chemical and optical properties, and the climate forcing of carbonaceous aerosols. In this study, we improve the current three-mode version of the Modal Aerosol Module (MAM3) in the Community Atmosphere Model version 5 (CAM5) by introducing an additional primary carbon mode to explicitly account for the microphysical ageing of primary carbonaceous aerosols in the atmosphere. Compared to MAM3, the four-mode version of MAM (MAM4) significantly increases the column burdens of primary particulate organic matter (POM) and black carbon (BC) by up to 40 % in many remote regions, where in-cloud scavenging plays an important role in determining the aerosol concentrations. Differences in the column burdens for other types of aerosol (e.g., sulfate, secondary organic aerosols, mineral dust, sea salt) are less than 1 %. Evaluating the MAM4 simulation against in situ surface and aircraft observations, we find that MAM4 significantly improves the simulation of seasonal variation of near-surface BC concentrations in the polar regions, by increasing the BC concentrations in all seasons and particularly in cold seasons. However, it exacerbates the overestimation of modeled BC concentrations in the upper troposphere in the Pacific regions. As a result, the comparisons suggest that, to address the remaining model POM and BC biases, future improvements are required related to (1) in-cloud scavenging and vertical transport in convective clouds and (2) emissions of anthropogenic and biomass burning aerosols.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1980

The washout of combustion-generated hydrogen chloride

The coefficient for the washout from a rocket exhaust cloud of HCl generated by the combustion of an ammonium perchlorate-based solid rocket propellant such as that to be used for the Space Shuttle Booster is determined. A mathematical model of HCl scavenging by rain is developed taking into account rain droplet size, fall velocity and concentration under various rain conditions, partitioning of exhaust HCl between liquid and gaseous phases, the tendency of HCl to promote water vapor condensation and the concentration and size of droplets within the exhaust cloud. The washout coefficient is calculated as a function of total cloud water content, total HCl content at 100% relative humidity, condensation nuclei concentration and rain intensity. The model predictions are compared with experimental results obtained in scavenging tests with solid rocket exhaust and raindrops of different sizes, and the large reduction in washout coefficient at high relative humidities predicted by the model is not observed. A washout coefficient equal to 0.0000512 times the -0.176 power of the mass concentration of HCl times the 0.773 power of the rainfall intensity is obtained from the experimental data.

Fenton, D. L.↗

NASA NTRS1986

Silicon production in a fluidized bed reactor

Part of the development effort of the JPL in-house technology involved in the Flat-Plate Solar Array (FSA) Project was the investigation of a low-cost process to produce semiconductor-grade silicon for terrestrial photovoltaic cell applications. The process selected was based on pyrolysis of silane in a fluidized-bed reactor (FBR). Following initial investigations involving 1- and 2-in. diameter reactors, a 6-in. diameter, engineering-scale FBR was constructed to establish reactor performance, mechanism of silicon deposition, product morphology, and product purity. The overall mass balance for all experiments indicates that more than 90% of the total silicon fed into the reactor is deposited on silicon seed particles and the remaining 10% becomes elutriated fines. Silicon production rates were demonstrated of 1.5 kg/h at 30% silane concentration and 3.5 kg/h at 80% silane concentration. The mechanism of silicon deposition is described by a six-path process: heterogeneous deposition, homogeneous decomposition, coalescence, coagulation, scavenging, and heterogeneous growth on fines. The bulk of the growth silicon layer appears to be made up of small diameter particles. This product morphology lends support to the concept of the scavenging of homogeneously nucleated silicon.

Rohatgi, N. K.↗

NASA NTRS1988

Holographic particle detection

The feasibility was studied of developing a novel particle track detector based on the detection of 1p-1s emission radiation from electron bubbles in liquid helium. The principles, design, construction, and initial testing of the detection system have been described in previous reports. The main obstacle encountered was the construction of the liquid-helium tight infrared windows. Despite numerous efforts in testing and redesigning the windows, the problem of window leakage at low temperature persisted. Due to limited time and resources, attention was switched to investigating the possibility of using room-temperature liquid as the detection medium. A possible mechanism was the detection of de-excitation radiation emitted from localized electrons in common liquids where electrons exhibit low mobilities, as suggested in the previous report. The purity of the liquid is critical in this method as the dissolved impurities (such as oxygen), even in trace amounts, will act as scavengers of electrons. Another mechanism is discussed whereby the formation of the superoxide ions by electron scavenging behavior of dissolved oxygen is exploited to detect the track of ionizing particles. An experiment to measure the ionization current produced in a liquid by a pulsed X-ray beam in order to study propertiies of the ions is also reported.

Bowen, Theodore↗

NASA NTRS1988

A 3-dimensional numerical simulation of the atmospheric injection of aerosols by a hypothetical basaltic fissure eruption

Researchers simulated the atmospheric response to a hypothetical basaltic fissure eruption using heating rates based on the Roza flow eruption. The simulation employs the Colorado State University Regional Atmospheric Model (RAMS) with scavenging effects. The numerical model is a three-dimensional non-hydrostatic time-split compressible cloud/mesoscale model. Explicit microphysics include prediction of cloud, rain, crystal, and hail precipitation types. Nucleation and phoretic scavenging are predicted assuming that the pollutant makes an effective cloud droplet nucleus. Smoke is carried as a passive tracer. Long and short wave radiation heating tendencies, including the effects of the smoke, are parameterized. The longwave emission by the lava surface is neglected in the parameterization and included as an explicit heating term instead. A regional scale domain of 100 x 100 km in the horizontal and 22 km high is used. The horizontal grid spacing is taken to be 2 km and the vertical spacing is taken to be 0.75 km. The initial atmospheric state is taken to be horizontally homogenous and based on the standard atmospheric sounding. The fissure is assumed to be 90 km long and oriented in a zig/zag pattern.

Tripoli, Gregory J.↗

NASA NTRS1990

Model simulations of rainout and washout from a warm stratiform cloud

Calculations utilizing a one-dimensional, time-dependent stratiform cloud model with parameterized microphysics to study the washout and rainout of soluble trace gases are presented. It is shown that the in-cloud concentrations of relatively insoluble species remain essentially unaffected by the presence of cloudwater and rainwater, while the concentrations of highly soluble species are rapidly depleted within the cloud. Due to this depletion it is shown that for highly soluble species the below-cloud scavenging via washout can dominate over in-cloud scavenging via rainout; in-cloud, aqueous-phase cloudwater and rainwater concentrations can differ considerably and, near the cloudbase, cloudwater concentrations can exceed rainwater concentrations by factors of two to ten.

Xing, Lin↗

NASA NTRS1992

Aluminum-fueled rockets for the space transportation system

Aluminum-fueled engines, used to propel orbital transfer vehicles (OTV's), offer benefits to the Space Transportation System (STS) if scrap aluminum can be scavenged at a reasonable cost. Aluminum scavenged from Space Shuttle external tanks could replace propellants hauled from Earth, thus allowing more payloads to be sent to their final destinations at the same Shuttle launch rate. To allow OTV use of aluminum fuel, two new items would be required: a facility to reprocess aluminum from external tanks and an engine for the OTV which could burn aluminum. Design of the orbital transfer vehicle would have to differ substantially from current concepts for it to carry and use the aluminum fuel. The aluminum reprocessing facility would probably have a mass of under 15 metric tons and would probably cost less that $200,000,000. Development of an aluminum-burning engine would no doubt be extremely expensive (1 to 2 billion dollars), but this amount would be adequately repaid by increased STS throughput. Engine production cost is difficult to estimate, but even an extremely high cost (e.g., $250,000,000 per engine) would not significantly increase orbit-raising expenses.

Cutler, Andrew Hall↗

NASA NTRS1988

AGBT Advanced Counter-Rotating Gearbox Detailed Design Report

An Advanced Counter-Rotating (CR) Gearbox was designed and fabricated to evaluate gearbox efficiency, durability and weight characteristics for emerging propfan-powered airplanes. Component scavenge tests showed that a constant volume collector had high scavenge effectiveness, which was uneffected by added airflow. Lubrication tests showed that gearbox losses could be reduced by controlling the air/oil mixture and by directing the oil jets radially, with a slight axial component, into the sun/planet gears.

Howe, D. C.↗

NASA NTRS1998

Vertical Distribution of Saharan Dust from the Goddard Three Dimensional Transport Model: Comparison with LITE Data

Spatial distributions of Saharan dust are simulated by the Goddard 3D chemistry transport model driven by meteorological fields from the Goddard Earth Observing System Data Assimilation System, GEOS-2 DAS. An aerosol module accounts for gravitational settling and the aerosol source function is based on surface moisture content and wind speed. The simulated aerosol fields are compared with Total Ozone Mapping Spectrometer (TOMS) by P. Ginoux in this session. The main focus is how ventilation of the assimilation winds will impact the simulated aerosol vertical distribution. Excessive ventilation would transport too much aerosol in the upper troposphere and lead to errors in the long range transport as well as errors in any radiative forcing calculations derived from the simulated aerosol fields. Simulated aerosol fields using GEOS-1 DAS wind fields for September 1994 will be compared with lidar observations during the Lidar In-space Technology Experiment (LITE). The lidar return signal clearly delineates the vertical extent and horizontal variability of the aerosol layer allowing rigorous comparison with the simulated fields. A second focus is the simulation of aerosol scavenging due to moist processes. Three-dimensional precipitation fields can be derived from two possible sources: Assimilated precipitation fields from GEOS-DAS or fields obtained from the Special Sensor Microwave/imager (SSM/1). Of interest is the sensitivity of the modeled aerosol fields to the different precipitation fields driving the moist scavenging module.

Weaver, Clark J.↗

NASA NTRS2000

Influence of the Latitudinal Temperature Gradient on Soil Dust Concentration and Deposition in Greenland

To investigate the effects of changes in the latitudinal temperature gradient and the global mean temperature on dust concentration in the Northern Hemisphere, experiments with the GISS GCM (Goddard Institute for Space Studies General Circulation Model) are performed. The dust concentration over Greenland is calculated from sources in central and eastern Asia, which are integrated on-line in the model. The results show that an increase in the latitudinal temperature gradient increases both the Asian dust source strength and the concentration over Greenland. The source increase is the result of increased surface winds, and to a minor extent, the increase in Greenland dust is also associated with increased northward transport. Cooling the climate in addition to this increased gradient leads to a decrease in precipitation scavenging, which helps produce a further (slight) increase in Greenland dust in this experiment. Reducing the latitudinal gradient reduces the surface wind and hence the dust source, with a subsequent reduction in Greenland dust concentrations. Warming the climate in addition to this reduced gradient leads to a further reduction in Greenland dust due to enhanced precipitation scavenging. These results can be used to evaluate the relationship of Greenland ice core temperature changes to changes in the latitudinal and global temperatures.

Tegen, Ina↗

NASA NTRS2000

Influence of the Latitudinal Temperature Gradient on Soil Dust Concentration and Deposition in Greenland

To investigate the effects of changes in the latitudinal temperature gradient and the global mean temperature on dust concentration in the Northern Hemisphere, experiments with the Goddard Institute for Space Studies General Circulation Model (GISS GCM) are performed. The dust concentration over Greenland is calculated from sources in central and eastern Asia, which are integrated on-line in the model. The results show that an increase in the latitudinal temperature gradient increases both the Asian dust source strength and the concentration over Greenland. The source increase is the result of increased surface winds, and to a minor extent, the increase in Greenland dust is also associated with increased northward transport. Cooling the climate in addition to this increased gradient leads to a decrease in precipitation scavenging, which helps produce a further (slight) increase in Greenland dust in this experiment. Reducing the latitudinal gradient reduces the surface wind and hence the dust source, with a subsequent reduction in Greenland dust concentrations. Warming the climate in addition to this reduced gradient leads to a further reduction in Greenland dust due to enhanced precipitation scavenging. These results can be used to evaluate the relationship of Greenland ice core temperature changes to changes in the latitudinal and global temperatures.

Tegen, Ina↗

NASA NTRS1997

Free Radicals Generated by Ionizing Radiation Signal Nuclear Translocation of p53

The p53 tumor suppressor is a transcription factor that regulates several pathways, which function collectively to maintain the integrity of the genome. Nuclear localization is critical for wild-type function. However, the signals that regulate subcellular localization of p53 have not been identified. Here, we examine the effect of ionizing radiation on the subcellular localization of p53 in two cell lines in which p63 is normally sequestered in the cytoplasm and found that ionizing radiation caused a biphasic translocation response. p53 entered the nucleus 1-2 hours postirradiation (early response), subsequently emerged from the nucleus, and then again entered the nucleus 12-24 hours after the cells had been irradiated (delayed response). These changes in subcellular localization could be completely blocked by the free radical scavenger, WR1065. By comparison, two DNA-damaging agents that do not generate free radicals, mitomycin C and doxorubicin, caused translocation only after 12-24 h of exposure to the drugs, and this effect could not be inhibited by WR1065. Hence, although all three DNA-damaging agents induced relocalization of p53 to the nucleus, only the translocation caused by radiation was sensitive to free radical scavenging. We suggest that the free radicals generated by ionizing radiation can signal p53 translocation to the nucleus.

Martinez, J. D.↗

NASA NTRS2003

H2O-Silicate Microphysics in Ascending Volcanic Plumes on Mars

Physical adsorption of water vapor plays a much more significant role in eruptive plume energetics on Mars than on Earth. The total surface area in martian plumes is likely comparable to terrestrial ash, while the erupting magma and ambient atmosphere are drier. Plumes cool rapidly during ascent, and a limited population of H2O molecules find adsorption sites to be increasingly stable. Release of latent heat of condensation and the onset of moist convection are diminished, delayed, or even prevented by adsorptive interaction We have developed a 5-component numerical model of the behavior of water in eruptive plumes under Mars-like conditions. We have used the model to study the fate of both juvenile and ambient atmospheric water in the eruption column. Here we investigate the adsorptive interaction of water and silicates as they effect plume dynamics and the partitioning and distribution of H2O to the martian environment. Our focus is on the role of adsorption in scavenging H2O from the ascending eruption column, and the possibility that adsorptive scavenging depresses the vapor pressure in the column below the level considered in most eruptive models.

A P Zent↗