910111213141512 of 26
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
From clouds over the boreal forest to fog events in polluted plains: New insights on CCN activity and cloud droplet formation through field observations and numerical modeling
Stockholm University, Faculty of Science, Department of Environmental Science.ORCID iD: 0009-0003-7141-9060
2026 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Aerosol–cloud interactions (ACI) remain the largest source of uncertainty in the estimates of anthropogenic radiative forcing from Earth system models (ESMs). In this thesis, we combine theoretical tools including inverse modeling, sensitivity analysis, and cloud parcel model (CPM) simulations with observations from clean and polluted environments (SMEAR II station in Finnish boreal forest, and San Pietro Capofiume station in the Italian Po Valley) to yield new insights on ACI. For the boreal forest, we showed that if bulk chemical composition of submicron aerosol particles is used for cloud condensation nuclei (CCN) prediction, it would lead to significant errors (for e.g. a bias of ~34% at 1.0% supersaturation). Therefore, inverse CCN closures were performed in which optimized size-segregated chemical composition and thus the hygroscopicity parameter (κ) were obtained, which reduced the bias to below 21%. The results further confirmed the lower hygroscopicity of the ultrafine (smaller than about 100 nm in diameter) Aitken mode particles (median κ ≈ 0.1) as compared with the larger accumulation mode (median κ ≈ 0.3) – except in cases with very numerous Aitken mode particles.  We then performed multiple CPM simulations of warm and non-precipitating clouds using a decade-long aerosol and cloud base updraft data from the same location. The median of modelled maximum supersaturation (SSmax) and cloud droplet number concentration at SSmax height level (CDNCmax) were ~0.2-0.3% and ~200 cm⁻³, respectively, increasing to ~0.32% and ~500 cm⁻³ in summer cumulus clouds due to higher updrafts and aerosol number concentrations. Observed CCN showed a moderate correlation with modeled CDNCmax (Spearman correlation coefficient r ≈ 0.5), highlighting the importance of other parameters (particularly SS and κ). Furthermore, in case of the cumulus clouds, the observed peak liquid water path showed low correlation (Spearman correlation coefficient r = 0.26) with the ground observation of total aerosol number concentration. Co-condensation of organic vapors on growing droplets was found to enhance the cloud base CDNC by 16 to 22%, depending on updraft and the type of size distribution. In the Po Valley fog, in contrast to the boreal forest clouds, high aerosol loading and slower cooling rate resulted in low SS (0.01% to 0.03%) and lower CDNC ~12 cm⁻³ leaving, most (~87%) as hydrated haze particles. 

In the boreal forest, the most important factors driving the CDNC varied depending primarily on the size distribution shape. For cases with a relatively large number of accumulation mode particles present, their number and updraft velocities were the most important determining factors. For cases with numerous ultrafine particles, however, the Aitken mode properties (hygroscopicity, concentrations and size) became important as well.  In contrast to the boreal forest, in the Po Valley, the SS driven by the radiative cooling and aerosol number concentration were always the most important parameters for accurate prediction of fog microphysics – instead of the chemical composition. 

This thesis highlights that accurate representation of updraft velocity and aerosol number concentration is consistently needed for reliable CDNC estimates, while chemical composition becomes especially critical when the size distribution includes a large number of ultrafine particles. We recommend continuing current long-term measurements, which can be complemented by campaign-based vertical profiling of aerosol size distributions beneath low stratus and cumulus clouds to help close remaining knowledge gaps. For fog microphysics studies in polluted environments, hydrated particles must be accounted for, as activated and non-activated droplets behave very differently in terms of processes such as evaporation and sedimentation.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science, Stockholm University , 2026. , p. 49
Keywords [en]
Aerosol-cloud interactions, Boreal forests, Po valley, Köhler theory, Cloud parcel model
National Category
Environmental Sciences
Research subject
Environmental Sciences
Identifiers
URN: urn:nbn:se:su:diva-254605ISBN: 978-91-8107-656-1 (print)ISBN: 978-91-8107-657-8 (electronic)OAI: oai:DiVA.org:su-254605DiVA, id: diva2:2055338
Public defence
2026-06-12, Ahlmansalen, Geovetenskapens hus, Svante Arrhenius väg 8, Stockholm, 08:00 (English)
Opponent
Supervisors
Available from: 2026-05-20 Created: 2026-04-23 Last updated: 2026-05-11Bibliographically approved
List of papers
1. Cloud response to co-condensation of water and organic vapors over the boreal forest
Open this publication in new window or tab >>Cloud response to co-condensation of water and organic vapors over the boreal forest
Show others...
2024 (English)In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 24, no 8, p. 5117-5147Article in journal (Refereed) Published
Abstract [en]

Accounting for the condensation of organic vapors along with water vapor (co-condensation) has been shown in adiabatic cloud parcel model (CPM) simulations to enhance the number of aerosol particles that activate to form cloud droplets. The boreal forest is an important source of biogenic organic vapors, but the role of these vapors in co-condensation has not been systematically investigated. In this work, the environmental conditions under which strong co-condensation-driven cloud droplet number enhancements would be expected over the boreal biome are identified. Recent measurement technology, specifically the Filter Inlet for Gases and AEROsols (FIGAERO) coupled to an iodide-adduct chemical ionization mass spectrometer (I-CIMS), is utilized to construct volatility distributions of the boreal atmospheric organics. Then, a suite of CPM simulations initialized with a comprehensive set of concurrent aerosol observations collected in the boreal forest of Finland during spring 2014 is performed. The degree to which co-condensation impacts droplet formation in the model is shown to be dependent on the initialization of temperature, relative humidity, updraft velocity, aerosol size distribution, organic vapor concentration, and the volatility distribution. The predicted median enhancements in cloud droplet number concentration (CDNC) due to accounting for the co-condensation of water and organics fall on average between 16 % and 22 %. This corresponds to activating particles 10–16 nm smaller in dry diameter that would otherwise remain as interstitial aerosol. The highest CDNC enhancements (ΔCDNC) are predicted in the presence of a nascent ultrafine aerosol mode with a geometric mean diameter of ∼ 40 nm and no clear Hoppel minimum, indicative of pristine environments with a source of ultrafine particles (e.g., via new particle formation processes). Such aerosol size distributions are observed 30 %–40 % of the time in the studied boreal forest environment in spring and fall when new particle formation frequency is the highest. To evaluate the frequencies with which such distributions are experienced by an Earth system model over the whole boreal biome, 5 years of UK Earth System Model (UKESM1) simulations are further used. The frequencies are substantially lower than those observed at the boreal forest measurement site (< 6 % of the time), and the positive values, peaking in spring, are modeled only over Fennoscandia and the western parts of Siberia. Overall, the similarities in the size distributions between observed and modeled (UKESM1) are limited, which would limit the ability of this model, or any model with a similar aerosol representation, to project the climate relevance of co-condensation over the boreal forest. For the critical aerosol size distribution regime, ΔCDNC is shown to be sensitive to the concentrations of semi-volatile and some intermediate-volatility organic compounds (SVOCs and IVOCs), especially when the overall particle surface area is low. The magnitudes of ΔCDNC remain less affected by the more volatile vapors such as formic acid and extremely low- and low-volatility organic compounds (ELVOCs and LVOCs). The reasons for this are that most volatile organic vapors condense inefficiently due to their high volatility below the cloud base, and the concentrations of LVOCs and ELVOCs are too low to gain significant concentrations of soluble mass to reduce the critical supersaturations enough for droplet activation to occur. A reduction in the critical supersaturation caused by organic condensation emerges as the main driver of the modeled ΔCDNC. The results highlight the potential significance of co-condensation in pristine boreal environments close to sources of fresh ultrafine particles. For accurate predictions of co-condensation effects on CDNC, also in larger-scale models, an accurate representation of the aerosol size distribution is critical. Further studies targeted at finding observational evidence and constraints for co-condensation in the field are encouraged.

National Category
Meteorology and Atmospheric Sciences
Identifiers
urn:nbn:se:su:diva-231178 (URN)10.5194/acp-24-5117-2024 (DOI)001236960000001 ()2-s2.0-85192057149 (Scopus ID)
Available from: 2024-06-25 Created: 2024-06-25 Last updated: 2026-04-23Bibliographically approved
2. Optimizing CCN predictions through inferred modal aerosol composition – a boreal forest case study
Open this publication in new window or tab >>Optimizing CCN predictions through inferred modal aerosol composition – a boreal forest case study
Show others...
2025 (English)In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 25, no 23, p. 17275-17300Article in journal (Refereed) Published
Abstract [en]

The contribution of natural aerosol particles from boreal forests to total aerosol loadings may increase with reduction in anthropogenic emissions. Aitken and accumulation mode particles in boreal regions differ significantly in hygroscopicity, and ignoring this size dependence can cause large uncertainty in Cloud Condensation Nuclei (CCN) prediction. We applied κ-Köhler theory to a multi-year dataset (2016–2020) from Hyytiälä, Finland, to evaluate different representations of aerosol chemical composition for CCN prediction. Overpredictions by forward closures using either bulk chemical composition from an Aerosol Chemical Speciation Monitor (ACSM) or a constant κ= 0.18 were mitigated to a great extent by optimizing size-resolved composition using two inverse modeling approaches: (1) Nelder–Mead method with the size distribution fixed to its median during each 2 h CCN measurement cycle, and (2) MCMC (Markov Chain Monte Carlo) accounting also for the variability in the size distribution during each cycle. Both methods improved closure at SS =  0.2 %–1.0 % (with Geometric Mean Bias GMB values 1.12–1.20 and 0.95–1.05, respectively), with moderate improvement at 0.1 % (GMBs of 1.53 and 1.32, respectively). The Aitken mode was enriched in organics in 77 % of cases using method (1) and 46 % using method (2) – with typical κ values of ∼ 0.1 for Aitken and ∼ 0.3 for accumulation modes. The results generally align with known size-dependent chemical composition in Hyytiälä and indicate that variability in CCN hygroscopicity is largely driven by Aitken mode composition. Our results demonstrate the potential of inverse CCN closure methods for obtaining valuable information of the size-dependent chemical composition.

National Category
Meteorology and Atmospheric Sciences
Identifiers
urn:nbn:se:su:diva-250585 (URN)10.5194/acp-25-17275-2025 (DOI)001628197000001 ()2-s2.0-105023679571 (Scopus ID)
Available from: 2025-12-18 Created: 2025-12-18 Last updated: 2026-04-23Bibliographically approved
3. Modeling cloud droplet properties using aerosol physicochemical properties and cloud base updrafts over a boreal forest station
Open this publication in new window or tab >>Modeling cloud droplet properties using aerosol physicochemical properties and cloud base updrafts over a boreal forest station
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Boreal forests contribute to climate cooling through aerosol–cloud interactions. As rising temperatures are expected to modify the aerosol emissions, an improved understanding of aerosol activation and cloud microphysical properties over boreal regions is required. Here, we present, for the first time, long-term statistics of the maximum parcel supersaturation(SSmax) and the corresponding cloud droplet number concentration at the SSmax height level (CDNCmax) in adiabatic warm clouds. We use a comprehensive multiyear (2014–2024) observational dataset of cloud-base updraft velocity from warm, non-precipitating clouds, together with aerosol size-distribution and chemical composition measurements from Station for Measuring Ecosystem–Atmosphere Relations II (SMEAR II) measurement site in Hyytiälä, Finland, to perform cloud parcel model(CPM) simulations. We find median values of SSmax = 0.23% and CDNCmax = 213 cm−3. We further show that different approaches to representing updraft velocity lead to similar results: using a simple Gaussian probability density function (PDF) yields CDNCmax values about 15% lower than those obtained with an updraft-weighted PDF. Accounting for size-segregated aerosol composition reduces CDNCmax by 4–21% while increasing SSmax by 1–12%, depending on the specific updraft representation method employed for simulations. Simulations of 70 cumulus cloud cases observed between May and October in 2018 and 2019, characterized by stronger median positive updrafts (1.34 m s−1) compared to the long-term median(0.36 m s−1), produced median values of SSmax = 0.32% and CDNCmax = 542 cm−3. Sensitivity analyses, conducted using multiple approaches, revealed that updraft velocity and aerosol number concentration are the dominant controls on simulated cloud properties. However, chemical composition can become an important control under conditions with a large number of Aitken mode particles with a small mode diameter and low accumulation mode concentration.

Keywords
CDNC
National Category
Environmental Sciences
Identifiers
urn:nbn:se:su:diva-254573 (URN)
Available from: 2026-04-22 Created: 2026-04-22 Last updated: 2026-04-23
4. Importance of hydrated aerosol particles for aerosol-fog relationships in the Italian Po Valley
Open this publication in new window or tab >>Importance of hydrated aerosol particles for aerosol-fog relationships in the Italian Po Valley
(English)Manuscript (preprint) (Other (popular science, discussion, etc.))
Abstract [en]

Air pollution and fog are closely connected, influencing both visibility and human health. As relative humidity rises, aerosol particles absorb water and grow hygroscopically, potentially activating into fog droplets when supersaturation is reached. However, distinguishing between hydrated (non-activated) aerosols and activated droplets is critical, as their differing thermodynamic states influence fog chemistry and dissipation. This study quantifies the impact of hydrated aerosol particles on fog microphysical properties and visibility in the Po Valley, one of Europe’s most polluted regions. We analyzed detailed aerosol–fog observations from the 2021/22 FAIRARI campaign at San Pietro Capofiume, Italy, using κ-Köhler theory and the Large Eddy Simulation (LES) model MIMICA. The median hygroscopicity κ-value of fog residuals (0.45) exceeded that of interstitial particles (0.40) and out-of-fog aerosols (0.34), reflecting enhanced inorganic content in fog droplets. Hygroscopic growth calculations show that hydrated particles can reach several micrometers in diameter, significantly influencing inferred fog microphysical properties. Excluding hydrated aerosols led to an 81 % increase in effective diameter (from 11.6 μm to 21.0 μm) and an 87 % decrease in cloud droplet number concentration (from 97.4 to 12.4 cm-3). Hydrated particles contributed on average 21 % to liquid water content and accounted for 36 % of sub-kilometer visibility events without droplet activation. LES results emphasize that fog prediction depends strongly on the largest dry aerosol particles. Our findings demonstrate the need to distinguish between hydrated and activated particles when interpreting fog observations and modeling fog development in polluted environments.

National Category
Earth and Related Environmental Sciences
Research subject
Environmental Sciences
Identifiers
urn:nbn:se:su:diva-254312 (URN)10.5194/2025-5419, 2025 (DOI)
Note

The paper is already in Diva as Identifiers URN: urn:nbn:se:su:diva-245313OAI: oai:DiVA.org:su-245313DiVA, id: diva2:1987021

But I cannot see it in my list on login. That's why registering it.

Available from: 2026-04-20 Created: 2026-04-20 Last updated: 2026-04-23

Open Access in DiVA

From clouds over the boreal forest to fog events in polluted plains(6404 kB)20 downloads
File information
File name FULLTEXT01.pdfFile size 6404 kBChecksum SHA-512
c67bd86734f4eeca0f583dad43d514b21c150f36eff92ff745dbaca53a60ef4ee40fa4a6d38ab319e89b286ab340cdc900939c4401ddb18082b060180ecf7fd6
Type fulltextMimetype application/pdf

Authority records

Ranjan, Rahul

Search in DiVA

By author/editor
Ranjan, Rahul
By organisation
Department of Environmental Science
Environmental Sciences

Search outside of DiVA

GoogleGoogle Scholar
The number of downloads is the sum of all downloads of full texts. It may include eg previous versions that are now no longer available

isbn
urn-nbn

Altmetric score

isbn
urn-nbn
Total: 93 hits
910111213141512 of 26
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf