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Aerosol–cloud interactions are one of the most uncertain processes in climate models due to their nonlinear complexity. A key complexity arises from the possibility that clouds can respond to perturbed aerosols in two opposite ways, as characterized by the traditional “cloud lifetime” hypothesis and more recent “buffered system” hypothesis. Their importance in climate simulations remains poorly understood. Here we investigate the response of the liquid water path (LWP) to aerosol perturbations for warm clouds from the perspective of general circulation model (GCM) and A-Train remote sensing, through process-oriented model evaluations. A systematic difference is found in the LWP response between the model results and observations. The model results indicate a near-global uniform increase of LWP with increasing aerosol loading, while the sign of the response of the LWP from the A-Train varies from region to region. The satellite-observed response of the LWP is closely related to meteorological and/or macrophysical factors, in addition to the microphysics. The model does not reproduce this variability of cloud susceptibility (i.e., sensitivity of LWP to perturbed aerosols) because the parameterization of the autoconversion process assumes only suppression of rain formation in response to increased cloud droplet number, and does not consider macrophysical aspects that serve as a mechanism for the negative responses of the LWP via enhancements of evaporation and precipitation. Model biases are also found in the precipitation microphysics, which suggests that the model generates rainwater readily even when little cloud water is present. This essentially causes projections of unrealistically frequent and light rain, with high cloud susceptibilities to aerosol perturbations.
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The production of atmospheric organic nitrates (RONO<sub>2</sub>) has a large impact on air quality and climate due to their contribution to secondary organic aerosol and influence on tropospheric ozone concentrations. Since organic nitrates control the fate of gas phase NO<sub><i>x</i></sub> (NO + NO<sub>2</sub>), a byproduct of anthropogenic combustion processes, their atmospheric production and reactivity is of great interest. While the atmospheric reactivity of many relevant organic nitrates is still uncertain, one significant reactive pathway, condensed phase hydrolysis, has recently been identified as a potential sink for organic nitrate species. The partitioning of gas phase organic nitrates to aerosol particles and subsequent hydrolysis likely removes the oxidized nitrogen from further atmospheric processing, due to large organic nitrate uptake to aerosols and proposed hydrolysis lifetimes, which may impact long-range transport of NO<sub><i>x</i></sub>, a tropospheric ozone precursor. Despite the atmospheric importance, the hydrolysis rates and reaction mechanisms for atmospherically derived organic nitrates are almost completely unknown, including those derived from <i>α</i>-pinene, a biogenic volatile organic compound (BVOC) that is one of the most significant precursors to biogenic secondary organic aerosol (BSOA). To better understand the chemistry that governs the fate of particle phase organic nitrates, the hydrolysis mechanism and rate constants were elucidated for several organic nitrates, including an <i>α</i>-pinene-derived organic nitrate (APN). A positive trend in hydrolysis rate constants was observed with increasing solution acidity for all organic nitrates studied, with the tertiary APN lifetime ranging from 8.3 min at acidic pH (0.25) to 8.8 h at neutral pH (6.9). Since ambient fine aerosol pH values are observed to be acidic, the reported lifetimes, which are much shorter than that of atmospheric fine aerosol, provide important insight into the fate of particle phase organic nitrates. Along with rate constant data, product identification confirms that a unimolecular specific acid-catalyzed mechanism is responsible for organic nitrate hydrolysis under acidic conditions. The free energies and enthalpies of the isobutyl nitrate hydrolysis intermediates and products were calculated using a hybrid density functional (<i>ω</i>B97X-V) to support the proposed mechanisms. These findings provide valuable information regarding the organic nitrate hydrolysis mechanism and its contribution to the fate of atmospheric NO<sub><i>x</i></sub>, aerosol phase processing, and BSOA composition.
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We find that wintertime temperature anomalies near 4 hPa and 50° N/S are related, through dynamics, to anomalies in ozone and temperature, particularly in the tropical stratosphere but also throughout the upper stratosphere and mesosphere. These mid-latitude anomalies occur on timescales of up to a month, and are related to changes in wave forcing. A change in the meridional Brewer–Dobson circulation extends from the middle stratosphere into the mesosphere and forms a temperature-change quadrupole from Equator to pole. We develop a dynamical index based on detrended, deseasonalised mid-latitude temperature. When employed in multiple linear regression, this index can account for up to 60 % of the total variability of temperature, peaking at ∼ 5 hPa and dropping to 0 at ∼ 50 and ∼ 0.5 hPa, respectively, and increasing again into the mesosphere. Ozone similarly sees up to an additional 50 % of variability accounted for, with a slightly higher maximum and strong altitude dependence, with zero improvement found at 10 hPa. Further, the uncertainty on all equatorial multiple-linear regression coefficients can be reduced by up to 35 and 20 % in temperature and ozone, respectively, and so this index is an important tool for quantifying current and future ozone recovery.
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In situ flight data from two distinct campaigns during winter and summer seasons in the San Joaquin Valley (SJV) of California are used to calculate boundary-layer entrainment rates, ozone photochemical production rates, and regional methane emissions. Flights near Fresno, California, in January and February 2013 were conducted in concert with the NASA DISCOVER-AQ project. The second campaign (ArvinO3), consisting of 11 days of flights spanning June through September 2013 and 2014, focused on the southern end of the SJV between Bakersfield and the small town of Arvin, California – a region notorious for frequent violations of ozone air quality standards. Entrainment velocities, the parameterized rates at which free tropospheric air is incorporated into the atmospheric boundary layer (ABL), are estimated from a detailed budget of the inversion base height. During the winter campaign near Fresno, we find an average midday entrainment velocity of 1.5 cm s<sup>−1</sup>, and a maximum of 2.4 cm s<sup>−1</sup>. The entrainment velocities derived during the summer months near Bakersfield averaged 3 cm s<sup>−1</sup> (ranging from 0.9 to 6.5 cm s<sup>−1</sup>), consistent with stronger surface heating in the summer months. Using published data on boundary-layer heights we find that entrainment rates across the Central Valley of California have a bimodal annual distribution peaking in spring and fall when the lower tropospheric stability (LTS) is changing most rapidly.<br><br>Applying the entrainment velocities to a simple mixed-layer model of three other scalars (O<sub>3</sub>, CH<sub>4</sub>, and H<sub>2</sub>O), we solve for ozone photochemical production rates and find wintertime ozone production (2.8 ± 0.7 ppb h<sup>−1</sup>) to be about one-third as large as in the summer months (8.2 ± 3.1 ppb h<sup>−1</sup>). Moreover, the summertime ozone production rates observed above Bakersfield–Arvin exhibit an <i>inverse</i> relationship to a proxy for the volatile organic compound (VOC) : NO<sub><i>x</i></sub> ratio (aircraft [CH<sub>4</sub>] divided by surface [NO<sub>2</sub>]), consistent with a NO<sub><i>x</i></sub>-limited photochemical environment. A similar budget closure approach is used to derive the regional emissions of methane, yielding 100 (±100) Gg yr<sup>−1</sup> for the winter near Fresno and 170 (±125) Gg yr<sup>−1</sup> in the summer around Bakersfield. These estimates are 3.6 and 2.4 times larger, respectively, than current state inventories suggest. Finally, by performing a boundary-layer budget for water vapor, surface evapotranspiration rates appear to be consistently ∼ 55 % of the reference values reported by the California Irrigation Management Information System (CIMIS) for nearby weather stations.
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Wind tunnel experiments of dust emissions from different soil surfaces are carried out to better understand dust emission mechanisms. The effects of surface renewal on aerodynamic entrainment and saltation bombardment are analyzed in detail. It is found that flow conditions, surface particle motions (saltation and creep), soil dust content and ground obstacles all strongly affect dust emission, causing its rate to vary over orders of magnitude. Aerodynamic entrainment is highly effective, if dust supply is unlimited, as in the first 2–3 min of our wind tunnel runs. While aerodynamic entrainment is suppressed by dust supply limits, surface renewal through the motion of surface particles appears to be an effective pathway to remove the supply limit. Surface renewal is also found to be important to the efficiency of saltation bombardment. We demonstrate that surface renewal is a significant mechanism affecting dust emission and recommend that this mechanism be included in future dust models.
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The Toulouse electron spectrometer flown on the Russian project INTERBALL-Tail performs electron measurements from 10 to 26 000 eV over a 4<pi> solid angle in a satellite rotation period. The INTERBALL-Tail probe was launched on 3 August 1995 together with a subsatellite into a 65° inclination orbit with an apogee of about 30 <i>R<sub>E</sub></i>. The INTERBALL mission also includes a polar spacecraft launched in August 1996 for correlated studies of the outer magnetosphere and of the auroral regions. We present new observations concerning the low-latitude boundary layers (LLBL) of the magnetosphere obtained near the dawn magnetic meridian. LLBL are encountered at the interface between two plasma regimes, the magnetosheath and the dayside extension of the plasma sheet. Unexpectedly, the radial extent of the region where LLBL electrons can be sporadically detected as plasma clouds can reach up to 5 <i>R<sub>E</sub></i> inside the magnetopause. The LLBL core electrons have an average energy of the order of 100 eV and are systematically field-aligned and counterstreaming. As a trend, the temperature of the LLBL electrons increases with decreasing distance to Earth. Along the satellite orbit, the apparent time of occurrence of LLBL electrons can vary from about 5 to 20 min from one pass to another. An initial first comparison between electron- and magnetic-field measurements indicates that the LLBL clouds coincide with a strong increase in the magnetic field (by up to a factor of 2). The resulting strong magnetic field gradient can explain why the plasma-sheet electron flux in the keV range is strongly depressed in LLBL occurrence regions (up to a factor of sim10). We also show that LLBL electron encounters are related to field-aligned current structures and that wide LLBL correspond to northward interplanetary magnetic field. Evidence for LLBL/plasma-sheet electron leakage into the magnetosheath during southward IMF is also presented.
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A short description of the SAS (subsatellite analyser of spectra) wave experiment on board the Magion-4 subsatellite is given. We present first measurements of the magnetic-field fluctuations in the frequency range 32–2000 Hz obtained in the magnetotail during the disturbed period at the magnetopause and in the polar cusp.
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PROMICS-3 is a plasma experiment flown in the Russian project Interball. It performs three-dimensional (3D) measurements of ions in the energy range 4 eV–70 keV with mass separation and of electrons in the energy range 12 eV–35 keV. The Interball project consists of two main satellites, the Tail Probe and the Auroral Probe, each with one subsatellite. The Interball Tail Probe was launched on 3 August 1995, into a 65° inclination orbit with apogee at about 30 R<sub>E</sub>. Both main satellites carry identical PROMICS-3 instruments and thus direct comparisons of the particle distributions will be possible once the Auroral Probe is launched. Furthermore, PROMICS-3-Tail is the first instrument measuring the 3D ion distribution function in the magnetospheric boundary layers at high latitudes. In this paper we describe the PROMICS-3 instrument and show initial results from the Tail probe, measurements of the magnetosheath, plasma sheet, and ring current plasmas.
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The fast plasma analyzer EU-1 of the SCA-1 complex plasma spectrometer is installed onboard the Interball Tail Probe (Interball-1). It provides fast three-dimensional measurements of the ion distribution function on the low-spin-rate Prognoz satellite (about 2min). The EU-1 ion spectrometer with virtual aperture consists of two detectors with 16 E/Q narrow-angle analyzers and electrostatic scanners. This configuration allows one to measure the ion distribution function in three dimensions (over 15 energy steps in 50 eV/Q–5.0 keV/Q energy range in 64 directions) in 7.5 s, which makes it independent of the slow rotation speed of the satellite. A description of the instrument and its capabilities is given. We present here the preliminary results of measurements of ions for two cases of the dawn low- and mid-latitude magnetopause crossings. The properties of observed ion structures and their tentative explanation are presented. The 12 September 1995 pass at low latitude at about 90° solar-zenith angle on the dawn side of the magnetosphere is considered in more detail. Dispersive ions are seen at the edge of the magnetopause and at the edges of subsequently observed plasma structures. Changes in ion velocity distribution in plasma structures observed after the first magnetopause crossing suggest that what resembles multiple magnetopause crossings may be <i>plasma blobs</i> penetrating the magnetosphere. Observed variations of plasma parameters near magnetopause structures suggest nonstationary reconnection as the most probable mechanism for observed structures.
