Research School of Chemistry, Australian National University, Australian Capital Territory 0200, Australia.
Phys Rev Lett. 2013 Jun 28;110(26):263202. doi: 10.1103/PhysRevLett.110.263202. Epub 2013 Jun 26.
A wide variety of molecular systems that have recently come into the reach of experimental and theoretical investigation is dominated by quantum phenomena. However, even state of the art quantum propagation techniques are either unsuitable for general application to molecular systems with strong interference and tunneling characteristics or are computationally prohibitive for systems with more than a few degrees of freedom. In this Letter, we introduce a novel quantum propagation technique with wide applicability, controllable accuracy, and efficient utilization of computational resources. Its performance is validated for tunneling and dissociating systems with 1, 2, and 3 degrees of freedom, and the scaling behavior with respect to system dimensionality and requested accuracy is discussed.
各种分子体系，这些体系最近已经进入实验和理论研究的范围，主要由量子现象主导。然而，即使是最先进的量子传播技术，要么不适合于具有强烈干涉和隧道特性的分子系统的一般应用，要么对于自由度超过几个的系统来说，计算上是不可行的。在这封信中，我们引入了一种新的量子传播技术，它具有广泛的适用性、可控的准确性和高效利用计算资源的特点。我们验证了它在具有 1、2 和 3 个自由度的隧道和离解系统中的性能，并讨论了它与系统维数和所需精度的缩放行为。
