Sarsa Antonio, Bacić Zlatko, Moskowitz Jules W, Schmidt Kevin E
International School for Advanced Studies, SISSA, Via Beirut 2/4, I-34014 Trieste, Italy.
Phys Rev Lett. 2002 Mar 25;88(12):123401. doi: 10.1103/PhysRevLett.88.123401. Epub 2002 Mar 11.
We present diffusion quantum Monte Carlo calculations of the interchange tunneling splitting of (4)He(n)(HF)(2) clusters, n = 1-10. The tunneling splitting decreases rapidly for n = 1-4 clusters, and much more slowly for n>4. The decrease calculated for (4)He(n)(HF)(2) represents 74% of the reduction in the tunneling splitting measured recently for HF dimer in nanodroplets of more than 2000 He atoms. The first four He atoms quench the interchange tunneling very efficiently by virtue of occupying the equatorial ring which encircles the C(2h) transition state of the tunneling pathway.
我们展示了对(4)He(n)(HF)(2)团簇(n = 1 - 10)交换隧穿分裂的扩散量子蒙特卡罗计算结果。对于n = 1 - 4的团簇,隧穿分裂迅速减小,而对于n > 4的团簇,减小速度要慢得多。(4)He(n)(HF)(2)计算得出的减小量占最近在超过2000个He原子的纳米液滴中测量的HF二聚体隧穿分裂减小量的74%。前四个He原子通过占据环绕隧穿路径的C(2h)过渡态的赤道环,非常有效地淬灭了交换隧穿。