Jos Lelieveld’s research while affiliated with Max Planck Institute for Chemistry and other places

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Publications (623)


Low Tropospheric Ozone Over the Indo‐Pacific Warm Pool Related to Non‐Electrified Convection
  • Article

March 2025

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10 Reads

Clara M. Nussbaumer

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Andrea Pozzer

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Michael Hewson

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[...]

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Lightning is the most important source of nitric oxide (NO) in the tropical upper troposphere and controls the formation of tropospheric ozone (). It is associated with deep convection and occurs mostly over continents. The Chemistry of the Atmosphere Field Experiment in the Pacific (CAFE Pacific) was conducted in early 2024 from Cairns, Australia, taking airborne measurements across the Australian continent and the surrounding maritime regions. Based on cloud top properties, lightning data and in situ observations of NO, and carbon monoxide, we show that deep convection occurs over Northern Australia and the Indo‐Pacific Warm Pool. While we identify strong lightning activity over Australia, we observe deep convection in the Warm Pool that is not electrified. Our observations of low in the Warm Pool can be attributed to ‐poor air from the marine boundary layer, which is not replenished by photochemical production from NO at high altitudes.



„Umwelteinflüsse auf die kardiovaskuläre Gesundheit““Environmental influences on cardiovascular health”

February 2025

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16 Reads

Zeitschrift für Herz- Thorax- und Gefäßchirurgie

Noncommunicable diseases (NCD) are the leading cause of premature death worldwide, accounting for over 38 million deaths annually, or approximately 70% of global mortality. The majority of these deaths are caused by cardiovascular diseases. The risk of NCD is closely linked to exposure to environmental stressors such as air pollution, noise pollution, artificial light at night and climatic changes, including extreme heat, sandstorms, and forest fires. In addition to traditional risk factors for cardiovascular diseases, such as diabetes, hypertension, smoking, hypercholesterolemia and genetic predisposition, there is increasing evidence that physicochemical environmental factors substantially contribute to the high numbers of NCD. Urbanization contributes to the amplification and accumulation of these stressors. This review summarizes the epidemiology and pathophysiology of environmental stressors with a particular focus on cardiovascular NCD. In addition, strategies and measures to reduce the impact of environmental risks, especially in the context of cardiovascular diseases, are discussed.


The influence of ammonia emissions on the size-resolved global atmospheric aerosol composition and acidity
  • Preprint
  • File available

February 2025

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15 Reads

Ammonia (NH3) is an abundant alkaline gas in the atmosphere and a key precursor in the formation of particulate matter. While emissions of other aerosol precursors such as SO2 and NOx have decreased significantly, global NH3 emissions are stable or increasing, and this trend is projected to continue. This study investigates the impact of NH3 emission changes on size-resolved aerosol composition and acidity using the atmospheric chemistry-climate model EMAC. Three NH3 emission schemes are analyzed: two bottom-up inventories and one derived using an updated top-down method. The results reveal that sulphate-nitrate-ammonium aerosols in two fine mode size ranges (0–1 µm and 1–2.5 µm) show the greatest sensitivity to NH3 emission changes. Regional responses vary depending on the local chemical environment of secondary inorganic aerosols. In 'NH3-rich' regions (e.g. East Asia and Europe), the abundance of NH3 partially offsets the effects of reduced NH3 emissions when NOx and SO2 are available, especially for aerosols in the 1–2.5 µm range. This highlights the importance of coordinated control strategies for NH3, NOx and SO2 emissions. Further, we find that NH3 has a buffering effect in densely populated areas, maintaining aerosol acidity at moderate levels and mitigating drastic pH shifts. The study emphasizes that pH changes are closely related to NH3 emission variations, with the highest sensitivity observed in the fine mode size ranges. These results highlight the critical role of NH3 in shaping aerosol acidity and argue for size-specific approaches to managing particulate matter.

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Deforestation maps used for the deforestation tree PFTs in LPJ-GUESS. The products are derived from HYDE v3.2 based on data from the year 2015.
Changes in tree and grass cover fractions (areas covered by vegetation per unit ground area). Panels (a) and (c) show the tree PFTs, while panels (b) and (d) show the grass PFTs. Panels (a) and (b) show the global distribution of the vegetation fractions in the PNV scenario. Panels (c) and (d) show the changes with respect to the deforestation (DCGL-PNV) scenario.
Isoprene and monoterpene surface fluxes for the PNV scenario (a–b). Panels (c) and (d) show the spatial differences in isoprene and monoterpene emission fluxes (DCGL-PNV). Monthly emissions are based on the 10-year global averages for isoprene (e) and monoterpenes (f). The shading represents 1 standard deviation, derived from the monthly averages based on 10 simulated years. Fluxes in the Southern Hemisphere were shifted by 6 months to align with the seasonal cycle.
Total column bSOA from the PNV scenario (a) and changes in bSOA from the deforestation (DCGL-PNV) scenario (b). Panels (c), (d), and (e) show the vertical profiles of bSOA, represented by box–whisker plots for different pressure bins. The white line marks the median, the box corresponds to the lower and upper quartiles, and the whiskers represent the 5th and 95th percentiles of the spatial mean over the 10 years simulated. The latitude ranges are defined as follows: high latitudes (90–55° S and 55–90° N), midlatitudes (55–30° S and 30–55° N), and low latitudes (30° S–30° N). A log scale is used for the x axis in panels (c), (d), and (e). Panel (b) includes diagonal crosshatching to indicate areas that are not statistically significant, based on a two-tailed Student's t test with a 90 % confidence level.
Spatial maps of the total column aerosol optical thickness (AOT) at 550 nm for organic carbon (OC) (a) and total aerosol (e). Vertical profiles of aerosol extinction at 550 nm for the DCGL and PNV scenarios, along with the relative differences ((DCGL-PNV)/PNV) in different latitude bands. Panels (b), (c), and (d) correspond to organic carbon, and panels (f), (g), and (h) correspond to total aerosol. The latitude ranges are defined as follows: high latitudes (90–55° S and 55–90° N), midlatitudes (55–30° S and 30–55° N), and low latitudes (30° S–30° N). The grey area represents 1 standard deviation of the spatio-temporal mean (grey line). Please note the different scales for the relative differences. Panels (a) and (e) include diagonal crosshatching to indicate areas that are not statistically significant, based on a two-tailed Student's t test with a 90 % confidence level.

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Influence of land cover change on atmospheric organic gases, aerosols, and radiative effects

January 2025

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32 Reads

Biogenic volatile organic compounds (BVOCs) are emitted in large quantities from the terrestrial biosphere and play a significant role in atmospheric gaseous and aerosol compositions. Secondary organic aerosols (SOAs) resulting from BVOC oxidation affect the radiation budget both directly, through the scattering and absorption of sunlight, and indirectly, by modifying cloud properties. Human activities have extensively altered natural vegetation cover, primarily by converting forests into agricultural land. In this work, a global atmospheric chemistry–climate model, coupled with a dynamic global vegetation model, was employed to study the impacts of perturbing the biosphere through human-induced land use change, thereby exploring changes in BVOC emissions and the atmospheric aerosol burden. A land use scheme was implemented to constrain tree plant functional type (PFT) cover based on land transformation fraction maps from the year 2015. Two scenarios were evaluated: (1) one comparing present-day land cover, which includes areas deforested for crops and grazing land, with potential natural vegetation (PNV) cover simulated by the model, and (2) an extreme reforestation scenario in which present-day grazing land is restored to natural vegetation levels. We find that, compared to the PNV scenario, present-day deforestation results in a 26 % reduction in BVOC emissions, which decreases the global biogenic SOA (bSOA) burden by 0.16 Tg (a decrease of 29 %), while the total organic aerosol (OA) burden decreases by 0.17 Tg (a reduction of 9 %). On the other hand, the extreme reforestation scenario, compared to present-day land cover, suggests an increase in BVOC emissions of 22 %, which increases the bSOA burden by 0.11 Tg and the total OA burden by 0.12 Tg – increases of 26 % and 6 %, respectively. For the present-day deforestation scenario, we estimate a positive total radiative effect (aerosol + cloud) of 60.4 mW m⁻² (warming) relative to the natural vegetation scenario, while for the extreme reforestation scenario, we report a negative (cooling) effect of 38.2 mW m⁻² relative to current vegetation cover.


Auswirkungen von Umweltstressoren auf die kardiovaskuläre GesundheitThe effects of environmental stressors on cardiovascular health

December 2024

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20 Reads

Die Innere Medizin

Noncommunicable diseases (NCDs) are responsible for the premature deaths of more than 38 million people each year, making them the leading cause of the global burden of disease, accounting for 70% of global mortality. The majority of these deaths are caused by cardiovascular diseases. The risk of NCDs is closely related to exposure to environmental stressors such as air pollution, noise pollution, artificial light at night, and climate change, including extreme heat, sandstorms, and wildfires. In addition to the traditional risk factors for cardiovascular diseases such as diabetes, high blood pressure, smoking, hypercholesterolemia and genetic predisposition, there is increasing evidence that physicochemical factors in the environment significantly contribute to the high NCD numbers. In addition, urbanization is related to the accumulation and intensification of these stressors. This expert review will summarize the epidemiology and pathophysiology of environmental stressors with a focus on cardiovascular NCDs. In addition, solutions and measures to mitigate the effects of environmental risks, especially concerning cardiovascular diseases, will be discussed.


Heat Surge Animation: Middle East & North Africa's Future Under High Greenhouse Emissions (RCP—8.5)

December 2024

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10 Reads

This animation illustrates future summer warming in the Middle East and North Africa (MENA) relative to the pre-industrial climate (1850–1900). It also shows how the global annual mean temperature will change in future. Animation highlights when warming exceeds specific tipping points at national, regional, and global scales. The warming is based on the average of 21 statistically downscaled Global Climate Models at 31 km using a High-end greenhouse gas emission scenario (RCP—8.5). Please refer to the publication below for more information on temperature changes in MENA and globally. Cite: Malik, A., Stenchikov, G., Mostamandi, S., Parajuli, S., Lelieveld, J., Zittis, G., et al. (2024). Accelerated historical and future warming in the Middle East and North Africa. Journal of Geophysical Research: Atmospheres, 129, e2024JD041625. https://doi.org/10.1029/2024JD041625


Influence of ambient NO and NO 2 on the quantification of total peroxy nitrates (∑PNs) and total alkyl nitrates (∑ANs) by thermal dissociation cavity ring-down spectroscopy (TD-CRDS)

December 2024

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12 Reads

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1 Citation

Measurement of total peroxy nitrates (∑PNs) and alkyl nitrates (∑ANs) by instruments that use thermal dissociation (TD) inlets to convert the organic nitrate to detectable NO2 may suffer from systematic bias (both positive and negative) resulting from unwanted secondary chemistry in the heated inlets. Here we review the sources of the bias and the methods used to reduce it and/or correct for it and report new experiments using (for the first time) atmospherically relevant, unsaturated, biogenic alkyl nitrates as well as two different peroxyacetyl nitrate (PAN) sources. We show that the commonly used commercial C3-alkyl-nitrate (isopropyl nitrate, IPN) inlet for characterising the chemistry of ANs is not appropriate for real-air samples that contain longer chain nitrates. ANs generated in the NO3-induced oxidation of limonene are strongly positively biased in the presence of NO. By detecting NOX rather than NO2, we provide a simple solution to avoid the bias caused by the conversion of NO to NO2 by primary and secondary peroxy radicals resulting from the complex chemistry in the thermal degradation of long-chain, alkyl nitrates in air at TD-temperatures. We also show that using a photochemical source of PAN to characterise the TD-inlets can result in a much stronger apparent bias from NO to NO2 conversion than for a diffusion source of synthesised (“pure”) PAN at similar mixing ratios. This is explained by the presence of thermally labile trace gases such as peracetic acid (CH3C(O)OOH) and hydrogen peroxide (H2O2).


Time series of radicals, trace gases and aerosol particles
Measurements were performed on 23 January 2023 over the Amazon basin north of Manaus (RF 19). a, OH and HO2. b, Isoprene, sum of the first-generation isoprene oxidation products methyl vinyl ketone (MVK), methacrolein (MACR) and isoprene hydroxy hydroperoxide (ISOPOOH) and NO. c, Isoprene-derived organonitrates C5H11O4(ONO2) and C5H10O2(ONO2)2. d, Particle concentrations N2–4 and N4–5, as well as pressure altitude. The light-red bar (T9) indicates the period between 10:05 and 10:10 local time, during which the strongest NPF was detected. Grey bars (T1–T8) represent previous sampling periods of the air mass examined at T9, traced by backward trajectories originating from the position of the aircraft during that period. The ambient temperature was about −58 °C at a flight altitude of 12.3 km during T1–T9. During the 4–5 min of the NPF event encounters, the aircraft travels more than 50 km.
Source Data
Flight path and air-mass back trajectories
a, Flight path for RF 19 (grey). The diamond-shaped pattern ABCD was flown repeatedly and the NPF air mass was encountered several times (thick-coloured sections T4–T9) also before the NPF event started (T1–T3). Coloured sections T1–T8 are each slightly shifted to the right to prevent overlap. Thin yellow lines with 1-h markers indicate 3 h of back trajectories from the NPF period T9 used to calculate and identify periods T1–T8. b, Back trajectories from the locations of the aircraft between 08:05 and 08:15 local time (black and red markers) to 140 min before (yellow-centred markers) and infrared satellite image (GOES-16, band 13: 10.3 µm; https://ftp.cptec.inpe.br/goes/goes16/retangular/ch13/2023/01/) indicating the approximate cloud-top temperatures at 05:50 local time. Temperatures below −50 °C are coloured. The back-trajectory calculations used the horizontal wind speed and direction measured by the research aircraft. The air parcels in which NPF was detected (red circles) trace back to the convective cloud and were in contact with convection more recently (relative to the sampling time) than those in which NPF was not detected (black circles). Satellite picture data in a obtained from https://wvs.earthdata.nasa.gov, NASA Worldview Snapshots.
Source Data
Molecular composition detected with the CI-APi-TOF mass spectrometer during the strongest NPF event of RF 19 (T9, 10:06–10:10 local time)
a, Mass defect versus mass-to-charge ratio with labelling of the molecular composition for prominent peaks. For clarity, the nitrate reagent ion (NO3⁻, m/z = 62) has been omitted from all labels. Circle size indicates peak intensity and colour indicates isoprene oxidation products without a nitrate group (IP0N, green), mononitrates (IP1N, magenta), dinitrates (IP2N, blue) and MSA signals (orange). b, Saturation vapour pressure C* of isoprene and its oxidation products as calculated with the SIMPOL model⁴⁹. The compounds C5H12O6, C5H11O4(ONO2) and C5H10O2(ONO2)2 are ELVOCs at −58 °C. c, Reaction scheme leading to the formation of C5H12O6, C5H11O4(ONO2) and C5H10O2(ONO2)2. The molecular structures shown are exemplary. IVOCs, intermediate-volatility organic compounds; LVOCs, low-volatility organic compounds; SVOCs, semivolatile organic compounds.
Source Data
Diurnal cycle and altitude dependence of NPF events, N2–5 particles and precursor gases
Pixels are calculated as bins of 1 km altitude and 30 min time and combine data from 11 research flights over the Amazon basin. a, Frequency of occurrence of NPF events, defined as the ratio of NPF events to the total number of measurements for each pixel. b, Concentrations of N2–5 particles. c–e, Isoprene organonitrates IP0N (c), mononitrates IP1N (d) and dinitrates IP2N (e). Panels b–e show the 95th percentile of the concentration, that is, 5% of the data contributing to a pixel are even higher than the value indicated by the colour. In the upper troposphere, high concentrations of organonitrates and N2–5 particles occurred frequently, whereas concentrations were low in the lower and middle tropospheres and during the night. Data influenced by the Manaus plume and by biomass burning have been removed. For direct comparability, all concentration data are normalized to standard conditions (273.15 K, 1,000 hPa).
Source Data
Isoprene nitrates drive new particle formation in Amazon’s upper troposphere

December 2024

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325 Reads

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10 Citations

Nature

New particle formation (NPF) in the tropical upper troposphere is a globally important source of atmospheric aerosols1, 2, 3–4. It is known to occur over the Amazon basin, but the nucleation mechanism and chemical precursors have yet to be identified². Here we present comprehensive in situ aircraft measurements showing that extremely low-volatile oxidation products of isoprene, particularly certain organonitrates, drive NPF in the Amazonian upper troposphere. The organonitrates originate from OH-initiated oxidation of isoprene from forest emissions in the presence of nitrogen oxides from lightning. Nucleation bursts start about 2 h after sunrise in the outflow of nocturnal deep convection, producing high aerosol concentrations of more than 50,000 particles cm⁻³. We report measurements of characteristic diurnal cycles of precursor gases and particles. Our observations show that the interplay between biogenic isoprene, deep tropical convection with associated lightning, oxidation photochemistry and the low ambient temperature uniquely promotes NPF. The particles grow over time, undergo long-range transport and descend through subsidence to the lower troposphere, in which they can serve as cloud condensation nuclei (CCN) that influence the Earth’s hydrological cycle, radiation budget and climate1,4, 5, 6, 7–8.


Example new particle formation experiment from IP-OOM at −50 °C, without NOx
a–c, Evolution of vapour concentrations (a), particle-nucleation rates at 1.7 nm, J1.7 (b), and naturally charged negative particle number size distribution (dN/dlogDp) and growth rates measured between 3.2 and 8.0 nm, GR3.2-8 (nm h⁻¹), for total (naturally charged + neutral) particles (c). The black lines in c depict the linear fits of 50% appearance time of particles between 3.2 and 8.0 nm. The vertical dashed lines and labels indicate the start of a new stage, at which the experimental conditions were adjusted. Trace sulfuric and iodic acid contaminants are present at the start of the run at concentrations of 1–5 × 10⁴ cm⁻³. Sulfur dioxide is injected and progressively increased during stages 5–8, which produces steps in H2SO4. The dotted black curve in b shows the expected H2SO4–NH3 nucleation rate, conservatively assuming that NH3 is present at the 4 pptv limit of detection. Stages 1 and 3 are, respectively, under neutral (ion-free) and beam (ion-enhanced) conditions, whereas all of the other stages are under galactic cosmic ray (GCR; natural ion concentrations) conditions. The experimental conditions are: isoprene = 0.20–0.41 ppbv (6.2–13.0 × 10⁹ cm⁻³), O3 = 84–96 ppbv (2.6–3.0 × 10¹² cm⁻³), I2 = 3.7–23.0 × 10⁵ cm⁻³, SO2 = 0–4 × 10⁹ cm⁻³, OH = 1–3 × 10⁶ cm⁻³, HO2 = 4.7–6.0 × 10⁷ cm⁻³, HO2/OH ratio = 18–37, RH = 62%, NO less than limit of detection (7 pptv) and temperature = −49 °C.
Particle-nucleation rates from IP-OOM at −30 °C and −50 °C, with variable NOx
a–d, Nucleation rates at 1.7 nm, J1.7, versus IP0N without NOx present (a), IP0N with NOx (b), HIOx + H2SO4 with and without NOx (c) and the product (HIOx + H2SO4) × IP0N with and without NOx (d). Measurements without NOx are indicated by diamonds (without acids) and circles (with acids). Measurements with NOx are indicated by triangles (without acids) and squares (with acids). Hollow symbols indicate −30 °C and solid symbols indicate −50 °C. In c, nucleation rates measured at contaminant acid concentrations are assigned the acid limit of detection (around 2 × 10⁴ cm⁻³). The solid lines in c show the nucleation rates expected for H2SO4 with 4 pptv NH3 at −30 °C (red) and −50 °C (blue), both at 60% RH (ref. ⁴⁴). The dashed and solid lines in d represent fits to the equation 10a×log10(x)+b, in which, for the dashed line, a = 1.241 and b = −15.065, and for the solid line, a = 1.505 and b = −19.948. Panels a–c show that both IP0N and total acid (HIOx + H2SO4) contribute to the nucleation rate. Panel d indicates that it is the product of IP0N and total acid (that is, the dimer formation rate) that best describes the nucleation rate, J1.7, as the data points cluster into two groups primarily characterized by temperature alone. IP1-2N also contribute to particle nucleation but they are less effective than IP0N (Extended Data Fig. 5). The experimental conditions are: isoprene = 0.04–1.50 ppbv (0.1–4.2 × 10¹⁰ cm⁻³), O3 = 1–590 ppbv (3.7 × 10¹⁰ to 1.8 × 10¹³ cm⁻³), I2 = 0–7.5 × 10⁷ cm⁻³, SO2 = 0–4.6 × 10⁹ cm⁻³, OH = 0.11–6.90 × 10⁷ cm⁻³, HO2 = 0.6–17.0 × 10⁸ cm⁻³, HO2/OH ratio = 11–118, NO = 0–0.22 ppbv, NO2 = 0–0.77 ppbv, RH = 29–70% and temperature = −30 °C and −50 °C. The error bars represent the standard deviation of the measurement at steady state. All measurements are made under galactic cosmic ray conditions (natural ionization amounts).
Molecular composition of charged and neutral clusters during IP-OOM nucleation without acids at −50 °C
a–d, Mass defect (difference from integer mass) versus m/z during IP-OOM nucleation events without acid and without added NOx (a,b) or with NOx (c,d). The data points are coloured by the number of carbon (a,b) or nitrogen (c,d) atoms. The symbol area in a and c is proportional to the normalized signal intensity by total signal, whereas that in b and d is proportional to IP-OOM concentrations. The charger ions (Br⁻, NO3⁻ and NH4⁺) are removed from the molecular formula in b and d. The data show that IP-OOM—which are around C5 for the monomer or C10 for the dimer—nucleate at −50 °C. The experimental conditions in a–d are: isoprene = 0.19, 0.07, 0.28 and 0.07 ppbv, O3 = 196.0, 129.0, 1.9 and 1.8 ppbv, OH = 0.3, 0.3, 1.6 and 4.6 × 10⁷ cm⁻³, HO2 = 1.8, 2.2, 3.4 and 6.8 × 10⁸ cm⁻³, NO = 0, 0, 0.07 and 0.18 ppbv, NO2 = 0, 0, 0.10 and 0.54 ppbv, RH = 31, 57, 66 and 29% and temperature = −49, −49, −48 and −48 °C, respectively. The concentrations of IP0N were unmeasured (instrument was not available), 3.4 × 10⁷, unmeasured and 2.5 × 10⁷ cm⁻³ and the concentrations of IP1-2N were unmeasured, 0, unmeasured and 1.5 × 10⁸ cm⁻³, respectively. The bromide chemical-ionization mass spectrometer was converted to measure charged clusters for the experiments shown in a and c, under ground-level and upper-tropospheric ion concentrations, respectively.
Particle growth rates and particle composition
a,b, Particle growth rates from 3.2 to 8.0 nm, GR3.2-8, versus IP0N (a) and IP0-2N (b). The solid lines show the predicted GR3.2-8 at the kinetic limit assuming monomer condensation and without considering any dipole enhancement. The prediction assumes that IP-OOM have a general formula of C5H12O6 and a density of 1.34 g cm⁻³ (ref. ⁵⁰). The dashed lines are linear fits to the experimental data of the form GR3.2-8 = 2.04 × 10⁻⁷ × IP0N (a) and GR3.2-8 = 1.23 × 10⁻⁷ × IP0-2N (b). c,d, Mass-defect plots showing the molecular composition of particles measured with the FIGAERO at −30 °C (Br-FIGAERO) and −50 °C (I-FIGAERO), with particle geometric mean sizes ranging from 6 to 20 nm. The colour legends indicate the number of atoms of carbon (c) and nitrogen (d). The symbol area is proportional to the normalized signal by the sum of measured signals. The charger ions are removed from the molecular formula. The annotations show the molecular formula of the particle-phase compounds. Our measurements show that both IP0N and IP1-2N drive rapid early particle growth and that C5H12O5-6 are the main condensing vapours in IP0N. The experimental conditions in a and b are: isoprene = 0.05–1.50 ppbv (0.15–4.40 × 10¹⁰ cm⁻³), O3 = 1–592 ppbv (3.6 × 10¹⁰ to 1.8 × 10¹³ cm⁻³), I2 = 0–1.1 × 10⁸ cm⁻³, SO2 = 0–4.9 × 10⁹ cm⁻³, OH = 0.09–7.40 × 10⁷ cm⁻³, HO2 = 0.6–19.0 × 10⁸ cm⁻³, NO = 0–0.26 ppbv, NO2 = 0–0.80 ppbv, RH = 29–72% and temperature = −30 °C and −50 °C. The experimental conditions for in c are: isoprene = 1.1 ppbv, O3 = 184 ppbv, I2 = 2.9 × 10⁷ cm⁻³, SO2 = 2.7 × 10⁷ cm⁻³, OH = 2.3 × 10⁶ cm⁻³, HO2 = 0.8 × 10⁸ cm⁻³, NO = 0 ppbv, NO2 = 0 ppbv, RH = 72%, temperature = −30 °C and DMS = 0 ppbv and those for in d are: isoprene = 0.2 ppbv, O3 = 1 ppbv, I2 = 0, SO2 = 1.2 × 10⁸ cm⁻³, OH = 5.2 × 10⁷ cm⁻³, HO2 = 1.2 × 10⁹ cm⁻³, NO = 0.11 ppbv, NO2 = 0.65 ppbv, RH = 38%, temperature = −48 °C and DMS = 0.16 ppbv. The vertical error bars represent the statistical uncertainty in the appearance-time growth-rate measurements derived from the 95% confidence interval on the growth-rate fit. The horizontal error bars represent the standard deviation of measured IP0N or IP0-2N during the growth period.
Schematic of new particle formation from isoprene in the upper troposphere
Isoprene from forests is efficiently transported at night by deep convective clouds into the upper troposphere. During daylight, the isoprene accumulated overnight, together with daytime-convected isoprene, reacts with hydroxyl radicals and NOx from lightning to produce IP-OOM. The IP-OOM combine with trace ambient acids to produce high particle-number concentrations at cold temperatures below −30 °C. The newly formed particles grow rapidly over several hours to days while following the descending air masses. This mechanism may provide an extensive source of CCN for shallow continental and marine clouds, which strongly influence Earth’s radiative balance.
New particle formation from isoprene under upper-tropospheric conditions

December 2024

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322 Reads

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9 Citations

Nature

Aircraft observations have revealed ubiquitous new particle formation in the tropical upper troposphere over the Amazon1,2 and the Atlantic and Pacific oceans3,4. Although the vapours involved remain unknown, recent satellite observations have revealed surprisingly high night-time isoprene mixing ratios of up to 1 part per billion by volume (ppbv) in the tropical upper troposphere⁵. Here, in experiments performed with the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber, we report new particle formation initiated by the reaction of hydroxyl radicals with isoprene at upper-tropospheric temperatures of −30 °C and −50 °C. We find that isoprene-oxygenated organic molecules (IP-OOM) nucleate at concentrations found in the upper troposphere, without requiring any more vapours. Moreover, the nucleation rates are enhanced 100-fold by extremely low concentrations of sulfuric acid or iodine oxoacids above 10⁵ cm⁻³, reaching rates around 30 cm⁻³ s⁻¹ at acid concentrations of 10⁶ cm⁻³. Our measurements show that nucleation involves sequential addition of IP-OOM, together with zero or one acid molecule in the embryonic molecular clusters. IP-OOM also drive rapid particle growth at 3–60 nm h⁻¹. We find that rapid nucleation and growth rates persist in the presence of NOx at upper-tropospheric concentrations from lightning. Our laboratory measurements show that isoprene emitted by rainforests may drive rapid new particle formation in extensive regions of the tropical upper troposphere1,2, resulting in tens of thousands of particles per cubic centimetre.


Citations (43)


... Recent direct measurements above the Amazon together with laboratory studies have now conrmed these earlier results. 3,26 Whereas these efforts have shed light on NPF mechanisms in the upper troposphere above Amazon, formation pathways of SOA and the role of isoprene photooxidation remain to be fully constrained in this environment. Shrivastava et al. 27 have found that they need to evoke transport of directly emitted 2-methyltetrols to the upper troposphere and subsequent condensation onto pre-existing particles to explain IEPOX-SOA fractions in OA observed at 12-14 km altitude above the Amazon, as the presumably glassy state of the high-altitude OA due to low temperature and humidity would inhibit reactive uptake of IEPOX. ...

Reference:

Direct high-altitude observations of 2-methyltetrols in the gas- and particle phase in air masses from Amazonia
New particle formation from isoprene under upper-tropospheric conditions

Nature

... Recent direct measurements above the Amazon together with laboratory studies have now conrmed these earlier results. 3,26 Whereas these efforts have shed light on NPF mechanisms in the upper troposphere above Amazon, formation pathways of SOA and the role of isoprene photooxidation remain to be fully constrained in this environment. Shrivastava et al. 27 have found that they need to evoke transport of directly emitted 2-methyltetrols to the upper troposphere and subsequent condensation onto pre-existing particles to explain IEPOX-SOA fractions in OA observed at 12-14 km altitude above the Amazon, as the presumably glassy state of the high-altitude OA due to low temperature and humidity would inhibit reactive uptake of IEPOX. ...

Isoprene nitrates drive new particle formation in Amazon’s upper troposphere

Nature

... In addition to these types of techniques to determine the truthfulness and validity of a model, they also provide information about the model's predictive power. Investigators compare model output with past climate data and draw lines of mismatch which they can adjust in the models such that the modelling of future climate change in the Gulf and Middle East region will improve [62]. It's absolutely essential to the process of model validation, that that model validation guarantees the accuracy of the climate forecast. ...

Accelerated Historical and Future Warming in the Middle East and North Africa

... One of the possible sources is vertical transport 85 during precipitation events, where ultrafine particles formed in the upper troposphere and were subsequently injected into the PBL by convective downdrafts Andreae et al., 2018;Machado et al., 2021). Despite that, Machado et al. (2024) recently analyzed aerosol and trace gas changes during downdrafts and attributed the characteristic particle bursts to boundary layer NPF, driven by a sudden increase in ozone and decrease in the condensation sink. 90 ...

Frequent rainfall-induced new particle formation within the canopy in the Amazon rainforest

... Hence, understanding these factors helps tailor interventions that align with the day-to-day realities of an individual. Environmental factors, such as air quality (23-28), climate (29)(30)(31)(32)(33)(34)(35)(36), and exposure to pollutants (37)(38)(39)(40)(41)(42)(43)(44)(45)(46), also play significant roles in determining health outcomes. By continuously monitoring and analyzing these elements, healthcare providers can create dynamic health plans that adapt to real-time changes. ...

Challenges posed by climate hazards to cardiovascular health and cardiac intensive care: implications for mitigation and adaptation
  • Citing Article
  • October 2024

European Heart Journal: Acute Cardiovascular Care

... Insufficient proline accumulation and high electrolyte leakage can compromise cellular stability, leading to reduced photosynthetic efficiency, weakened plant health, and ultimately, reduced yield (27,30). Cold stress at this critical bolling stage can negatively impact pollination, seed development,and seed quality, resulting in fewer, smaller and less viable seeds that lower both the economic value and regeneration potential of the crop (11). Similarly, in regions with a Mediterranean climate, like parts of the Middle East, where cool, wet winters with mean monthly temperatures between −3 °C and 18 °C are common (33), prolonged exposure to low temperatures can further impair safflower growth and productivity. ...

A Global Analysis of Historical and Future Changes in Mediterranean Climate‐Type Regions

... At nighttime, ground-level NO3 mixing ratios can vary greatly from < 1 pptv to > 100 pptv depending on atmospheric composition (Ng et al., 2017;Brown and Stutz, 2012), i.e. their production and loss terms. During ACROSS, the NO3 230 reactivity within the canopy was generally high at nighttime due to the emission of biogenic volatile organic compounds (BVOCs, by vegetation) and NO (from soil) into a shallow, poorly mixed nocturnal surface layer Andersen et al., 2024). This led to NO3 mixing ratios, at the ground, of < 0.5 pptv, which were generally lower than the limit of detection of instrumentation at the site. ...

Measurement report: Sources, sinks, and lifetime of NOx in a suburban temperate forest at night

... T he cardiovascular effects of heavy metal exposure are well-documented. 1,2 Historical reports, dating back over a century, highlighted a rise in hypertension and stroke cases among workers exposed to lead. 1 Since then, extensive epidemiologic and experimental research has established a robust link between exposure to various (heavy) metals-such as arsenic, lead, cadmium, mercury, and copper-and adverse cardiovascular disease outcomes, highlighting their cardiotoxic effects. 1,3 Importantly, uranium contamination of soil and water represents a global health concern that remains insufficiently studied, with significant regional variation in uranium concentrations due to both natural (geogenic) and human-made (anthropogenic) sources. ...

Soil and water pollution and cardiovascular disease

Nature Reviews Cardiology

... HO 2 was measured with the HORUS instrument and has an uncertainty of approximately 50%. Due to the difficulty in determining an experimental calibration factor for the HO 2 data set, a value of 2.5 was estimated based on comparison with the EMAC model and its performance in measuring hydrogen peroxide (H 2 O 2 ) (Hamryszczak et al., 2023). ...

Measurement report: Hydrogen peroxide in the upper tropical troposphere over the Atlantic Ocean and western Africa during the CAFE-Africa aircraft campaign

... year for which coincident emission inventories and measurement data were available, based on recently published results 55 . We concentrate on long-term -rather than acute-exposure because chronic oxidative stress and inflammatory responses are associated with cardiovascular, cardiometabolic, and cerebrovascular diseases 56 . ...

Numerical simulation and evaluation of global ultrafine particle concentrations at the Earth's surface