Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Particle Size Distribution Dynamics Can Help Constrain the Phase State of Secondary Organic Aerosol

Journal Article · · Environmental Science & Technology
 [1];  [1];  [2];  [3];  [4];  [1];  [5];  [6];  [7];  [1];  [1]
  1. Colorado State University
  2. City University of Hong Kong
  3. Georgia Institute of Technology
  4. COLORADO STATE UNIVERSITY
  5. University of California, Irvine
  6. BATTELLE (PACIFIC NW LAB)
  7. University of California, Davis

Particle phase state is a property of atmospheric aerosols that has important implications for the formation, evolution, and gas/particle partitioning of secondary organic aerosol (SOA). In this work, we use a size-resolved chemistry and microphysics model (SOM-TOMAS), updated to include an explicit treatment of particle phase state, to constrain the bulk diffusion coefficient (Db) of SOA produced from ??- pinene ozonolysis. By leveraging data from laboratory experiments performed in the absence of a seed and under dry conditions, we find that the Db for SOA can be constrained (1-7 ×10-15 cm2 s-1 in these experiments) by simultaneously reproducing the time-varying SOA mass concentrations and the evolution of the particle size distribution. Another version of our model that used the predicted SOA composition to calculate the glass transition temperature, viscosity, and, ultimately, Db (~10-15 cm2 s-1) of the SOA was able to reproduce the mass and size distribution measurements when we included oligomer formation (oligomers accounted for about a fifth of the SOA mass). Our work highlights the potential of a size resolved SOA model to constrain the particle phase state of SOA by utilizing historical measurements of the evolution of the particle size distribution.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1767151
Report Number(s):
PNNL-SA-156556
Journal Information:
Environmental Science & Technology, Vol. 55, Issue 3
Country of Publication:
United States
Language:
English

References (63)

Evolution of Organic Aerosols in the Atmosphere journal December 2009
Particulate matter, air quality and climate: lessons learned and future needs journal January 2015
Equilibration timescale of atmospheric secondary organic aerosol partitioning journal December 2012
Gas uptake and chemical aging of semisolid organic aerosol particles journal June 2011
Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol journal June 2017
Multiphase reactivity of polycyclic aromatic hydrocarbons is driven by phase separation and diffusion limitations journal May 2019
Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions journal March 2010
Heterogeneous ice nucleation and water uptake by field-collected atmospheric particles below 273 K: ICE NUCLEATION BY ATMOSPHERIC PARTICLES journal September 2012
Competition between water uptake and ice nucleation by glassy organic aerosol particles journal January 2014
The viscosity of atmospherically relevant organic particles journal March 2018
Technical Note: New methodology for measuring viscosities in small volumes characteristic of environmental chamber particle samples journal January 2013
Integrating phase and composition of secondary organic aerosol from the ozonolysis of  -pinene journal May 2014
Estimating the Viscosity Range of SOA Particles Based on Their Coalescence Time journal December 2013
Formation and evolution of molecular products in α-pinene secondary organic aerosol journal November 2015
Hygroscopic Influence on the Semisolid-to-Liquid Transition of Secondary Organic Materials journal November 2014
Effect of varying experimental conditions on the viscosity of α -pinene derived secondary organic material journal January 2016
Growth Kinetics and Size Distribution Dynamics of Viscous Secondary Organic Aerosol journal January 2018
Particle-Phase Diffusion Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary Organic Aerosol journal January 2020
Experimental determination of chemical diffusion within secondary organic aerosol particles journal January 2013
Kinetic limitations in gas-particle reactions arising from slow diffusion in secondary organic aerosol journal January 2013
Evaporation kinetics and phase of laboratory and ambient secondary organic aerosol journal January 2011
Factors controlling the evaporation of secondary organic aerosol from α‐pinene ozonolysis journal March 2017
Modeling kinetic partitioning of secondary organic aerosol and size distribution dynamics: representing effects of volatility, phase state, and particle-phase reaction journal January 2014
Coupled Partitioning, Dilution, and Chemical Aging of Semivolatile Organics journal April 2006
Organic condensation: a vital link connecting aerosol formation to cloud condensation nuclei (CCN) concentrations journal January 2011
Quantification of the volatility of secondary organic compounds in ultrafine particles during nucleation events journal January 2011
The role of low-volatility organic compounds in initial particle growth in the atmosphere journal May 2016
Influence of seed aerosol surface area and oxidation rate on vapor wall deposition and SOA mass yields: a case study with α -pinene ozonolysis journal January 2016
Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition journal January 2018
Secondary organic aerosol formation from the β-pinene+NO 3 system: effect of humidity and peroxy radical fate journal January 2015
Multi-generation gas-phase oxidation, equilibrium partitioning, and the formation and evolution of secondary organic aerosol journal January 2012
Multi-generational oxidation model to simulate secondary organic aerosol in a 3-D air quality model journal January 2015
Predicting global aerosol size distributions in general circulation models journal January 2002
Contribution of primary carbonaceous aerosol to cloud condensation nuclei: processes and uncertainties evaluated with a global aerosol microphysics model journal January 2007
Secondary organic aerosol formation from evaporated biofuels: comparison to gasoline and correction for vapor wall losses journal January 2020
Oxygenated Aromatic Compounds are Important Precursors of Secondary Organic Aerosol in Biomass-Burning Emissions journal June 2020
Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol journal January 2019
A large source of low-volatility secondary organic aerosol journal February 2014
Production of extremely low volatile organic compounds from biogenic emissions: Measured yields and atmospheric implications journal May 2015
Ion-induced nucleation of pure biogenic particles journal May 2016
Global distribution of particle phase state in atmospheric secondary organic aerosols journal April 2017
Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities journal January 2019
Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors journal January 2019
Formation of Glasses from Liquids and Biopolymers journal March 1995
Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes–Einstein and fractional Stokes–Einstein relations journal January 2019
Isothermal Evaporation of α-Pinene Ozonolysis SOA: Volatility, Phase State, and Oligomeric Composition journal September 2018
A study of volatility by composition, heating, and dilution measurements of secondary organic aerosol from 1,3,5-trimethylbenzene journal January 2019
Oligomer formation within secondary organic aerosols: equilibrium and dynamic considerations journal January 2014
Equilibration time scales of organic aerosol inside thermodenuders: Evaporation kinetics versus thermodynamics journal February 2010
Diffusion-Limited Versus Quasi-Equilibrium Aerosol Growth journal August 2012
Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation journal July 2013
Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere journal January 2011
Kinetics, products, and mechanisms of secondary organic aerosol formation journal January 2012
Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM journal January 2014
Measurements of Kinetics and Equilibria for the Condensed Phase Reactions of Hydroperoxides with Carbonyls to Form Peroxyhemiacetals journal February 2020
The rate of equilibration of viscous aerosol particles journal January 2016
Water diffusion in atmospherically relevant α-pinene secondary organic material journal January 2015
Relative humidity-dependent viscosities of isoprene-derived secondary organic material and atmospheric implications for isoprene-dominant forests journal January 2015
Is the gas-particle partitioning in alpha-pinene secondary organic aerosol reversible? journal January 2007
Optimization of process models for determining volatility distribution and viscosity of organic aerosols from isothermal particle evaporation data journal January 2019
Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs journal March 2018
Size dependence of phase transitions in aerosol nanoparticles journal January 2015
Predicting the influence of particle size on the glass transition temperature and viscosity of secondary organic material journal September 2020

Similar Records

Related Subjects