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<p>Given the significant climatic role of sulfuric acid (SA) and methanesulfonic acid (MSA), this work examines the hydration-driven formation of ternary MSA(SA)(W)<sub><i>n</i>=1–10</sub> clusters <i>via</i> DFT (M06-2X, X3LYP, APF-D, PW6B95 combined with Def2-TZVP). We report structures, Boltzmann populations, binding energies and binding free energies (ΔE, ΔG), and binding energies per-water moleculs (ΔE/W, ΔG/W). While clusters of size <i>n</i> = 7–10 are inherently stable, their atmospheric equilibrium concentrations are low. The MSA(SA)(W)<sub>4</sub> cluster is an exception, with a concentration of ~ 10³ molecules/cm³ and a low evaporation rate. Clusters of size <i>n</i> = 4,7,8 exhibit slow evaporation ( &lt; ~ 10⁵ s⁻¹), suggesting extended atmospheric lifetimes. All DFT methods yield consistent trends, with M06-2X closest to PW91/6-311 + + G(3df,3pd) reference values. Cluster concentrations are sensitive to relative humidity (20, 50, and 100%). SA/MSA evaporation is minimal versus water loss. We assess the net climatic effect by quantifying cluster radiative forcing and Rayleigh scattering intensities.</p>

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Sulfuric Acid-methansulfonic Acid-water Cluster Formation Promoting Aerosol Nucleation: Atmospheric Impact

  • 期刊论文

  • 发表日期：

    2026年5月18日

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  • Oumarou Oussoumanou,
  • Olivier Holtomo,
  • Anne Justine Etindélé,
  • Ousmanou Motapon

摘要

Given the significant climatic role of sulfuric acid (SA) and methanesulfonic acid (MSA), this work examines the hydration-driven formation of ternary MSA(SA)(W)n=1–10 clusters via DFT (M06-2X, X3LYP, APF-D, PW6B95 combined with Def2-TZVP). We report structures, Boltzmann populations, binding energies and binding free energies (ΔE, ΔG), and binding energies per-water moleculs (ΔE/W, ΔG/W). While clusters of size n = 7–10 are inherently stable, their atmospheric equilibrium concentrations are low. The MSA(SA)(W)4 cluster is an exception, with a concentration of ~ 10³ molecules/cm³ and a low evaporation rate. Clusters of size n = 4,7,8 exhibit slow evaporation ( < ~ 10⁵ s⁻¹), suggesting extended atmospheric lifetimes. All DFT methods yield consistent trends, with M06-2X closest to PW91/6-311 + + G(3df,3pd) reference values. Cluster concentrations are sensitive to relative humidity (20, 50, and 100%). SA/MSA evaporation is minimal versus water loss. We assess the net climatic effect by quantifying cluster radiative forcing and Rayleigh scattering intensities.