Diffusion Monte Carlo Study on Relative Stabilities of Boron Nitride Polymorphs
Diffusion Monte Carlo Study on Relative Stabilities of Boron Nitride Polymorphs
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DOI：
10.1021/acs.jpcc.1c10943
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发表时间：
2021-11
期刊：
影响因子：
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通讯作者：
Yutaka Nikaido;Tom Ichibha;K. Hongo;F. Reboredo;K. C. Kumar;P. Mahadevan;R. Maezono;K. Nakano
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作者：
Yutaka Nikaido;Tom Ichibha;K. Hongo;F. Reboredo;K. C. Kumar;P. Mahadevan;R. Maezono;K. Nakano
尽管氮化硼(BN)是一种广泛用于工程和科学目的的著名化合物，但其最基本的性质之一--多晶型的相稳定性仍然存在争议。由于难以捉摸的Van der Waals相互作用，用从头算方法确定BN多晶型(如六方闪锌矿)的基态是困难的，这种相互作用在某些多晶型中起着决定性的作用，这使得定量预测具有很大的挑战性。因此，尽管有多种理论研究，但对于基态还没有达成共识，这主要是因为相互矛盾的报告。在这项研究中，我们应用最先进的从头算框架固定节点扩散蒙特卡罗(FNDMC)方法，对四种著名的BN多晶型，即六方、菱面体、纤锌矿和闪锌矿BN进行了研究。我们的FNDMC计算表明，在0 K和300K下，hBN是四种晶型中热力学上最稳定的。这一结果与Corrigan等人的实验数据相吻合。还有福永。所得结论与用耦合团簇等其他高水平方法得到的结果一致。我们证明了FNDMC是一种有效的方法来解决表现出各种形式的键的多晶型。当可靠的实验数据丢失或难以获取时，它还提供有价值的信息，如可靠的参考能量。我们的发现将促进FNDMC在其他范德华材料中的应用。
Although Boron nitride (BN) is a well-known compound widely used for engineering and scientific purposes, the phase stability of its polymorphs, one of its most fundamental properties, is still under debate. The ab initio determination of the ground state of the BN polymorphs, such as hexagonal and zinc-blende, is difficult because of the elusive Van der Waals interaction, which plays a decisive role in some of the polymorphs, making quantitative prediction highly challenging. Hence, despite multiple theoretical studies, there has been no consensus on the ground state yet, primarily due to contradicting reports. In this study, we apply a state-of-the-art ab initio framework fixed-node diffusion Monte Carlo (FNDMC), to four well known BN polymorphs, namely hexagonal, rhombohedral, wurtzite, and zinc-blende BNs. Our FNDMC calculations show that hBN is thermodynamically the most stable among the four polymorphs at 0 K as well as at 300K. This result agrees with the experimental data of Corrigan et al. and Fukunaga. The conclusions are consistent with those obtained using other high-level methods, such as coupled cluster. We demonstrate that the FNDMC is a powerful method to address polymorphs that exhibit bonds of various forms. It also provides valuable information, like reliable reference energies, when reliable experimental data are missing or difficult to access. Our findings should promote the application of FNDMC for other van der Waals materials.