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Area of Science:

  • Atmospheric Chemistry
  • Climate Science
  • Computational Chemistry

Background:

  • Atmospheric molecular clusters and secondary aerosols significantly impact climate.
  • New Particle Formation (NPF) studies typically focus on sulfuric acid (SA) with a single base molecule.
  • Understanding the synergistic effects of multiple bases in NPF is crucial.

Purpose of the Study:

  • To investigate the combinations and synergy of several bases in the formation of sulfuric acid clusters.
  • To computationally examine (SA)0-4(base)0-4 clusters with five different bases: ammonia (AM), methylamine (MA), dimethylamine (DMA), trimethylamine (TMA), and ethylenediamine (EDA).
  • To determine the role of different bases in SA-driven NPF rates and cluster stability.

Main Methods:

  • Utilized computational quantum chemistry for configurational sampling (CS) of 316 different clusters.
  • Employed a multilevel funnelling sampling approach enhanced by a machine-learning (ML) step for efficient CS.
  • Evaluated cluster thermodynamics and binding free energies using high-level theory (DLPNO-CCSD(T0)/aug-cc-pVTZ//ωB97X-D/6-31++G(d,p)).

Main Results:

  • Dimethylamine (DMA) and ethylenediamine (EDA) act as primary nucleators for SA clusters, though EDA's effectiveness diminishes in larger clusters.
  • Trimethylamine (TMA) functions as a catalyst in the NPF process.
  • Ammonia (AM) and methylamine (MA) have limited impact when strong bases like DMA or EDA are present.

Conclusions:

  • The study elucidates the complex interplay of multiple bases in atmospheric NPF.
  • Identified distinct roles for different amines (nucleator, catalyst, or minor contributor) in SA cluster formation.
  • Provides critical data for atmospheric models simulating NPF and aerosol formation.