摘要

We have performed density functional theory (BL3YP) and ab initio (MP2) calculations to investigate the energetics of the cluster formation for (NH3)m(H2SO4) and (NH3)(H2SO4)(n) (m, n = 1-6) in the atmospherically-relevant temperature range between 200 and 300 K. For (NH3)(m)(H2SO4) clusters, the binding increases from m = 1 to 6 at 200 K, while the most stable complex at 300 K is the cluster with m = 2. For (NH3)(H2SO4) n clusters, the binding is more stable for those with larger n. There is a strong temperature dependence for the (NH3)(m)(H2SO4) cluster formation; the lowest free energy shifts from m = 6 at T = 200 K to m = 5 around T = 240 K and further to m = 2 at T %26gt;= 280 K. The temperature effects on (NH3) (H2SO4)(n) clusters are much less stronger, while there is still a similar trend which favors larger n in the entire temperature range from 200 to 300 K.

  • 出版日期2014-3-3