Optimal finite-range atomic basis sets for liquid water and ice
Optimal finite-range atomic basis sets for liquid water and ice
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DOI：
10.1088/0953-8984/25/43/435504
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发表时间：
2013-10-30
影响因子：
2.7
通讯作者：
Artacho, Emilio
中科院分区：
文献类型：
--
作者：
Corsetti, Fabiano;Fernandez-Serra, M-V;Artacho, Emilio
由于其灵活性和可扩展性，有限范围数值原子轨道是几种第一原理方法选择的基函数。然而，生成和测试此类基础集对于最终用户来说仍然是一个重大挑战。我们讨论了这些问题并提出了一种生成改进的有限范围偏振轨道的新方案。然后，我们开发了一系列水分子的高精度基础集，并报告了它们在描述单体和二聚体、冰的两相以及环境密度和高密度下的液态水方面的性能。这些测试是通过与平面波计算进行比较来进行的，并表明原子轨道基组具有出色的可转移性和一致性。对于能量差和离子力等量，最高阶碱基（四 zeta）显示出与至少类似于 1000 eV 的平面波动能截止相当的精度，并且在总能量和绝对压力方面实现了显着更高的精度。
Finite-range numerical atomic orbitals are the basis functions of choice for several first principles methods, due to their flexibility and scalability. Generating and testing such basis sets, however, remains a significant challenge for the end user. We discuss these issues and present a new scheme for generating improved polarization orbitals of finite range. We then develop a series of high-accuracy basis sets for the water molecule, and report on their performance in describing the monomer and dimer, two phases of ice, and liquid water at ambient and high density. The tests are performed by comparison with plane-wave calculations, and show the atomic orbital basis sets to exhibit an excellent level of transferability and consistency. The highest-order bases (quadruple-zeta) are shown to give accuracies comparable to a plane-wave kinetic energy cutoff of at least similar to 1000 eV for quantities such as energy differences and ionic forces, as well as achieving significantly greater accuracies for total energies and absolute pressures.