針對(duì)固體可靠而準(zhǔn)確的穩(wěn)定性第一性原理的詳細(xì)概述

可靠而準(zhǔn)確的穩(wěn)定性第一性原理計(jì)算對(duì)材料的合成、反應(yīng)性和性質(zhì)的研究至關(guān)重要，對(duì)于探索新的化學(xué)空間和難以觀察的相結(jié)構(gòu)來(lái)說(shuō)也很重要。穩(wěn)定性涉及化學(xué)穩(wěn)定能力（不同化學(xué)環(huán)境中化學(xué)計(jì)量組成保持不變的能力）和結(jié)構(gòu)選擇（一定化學(xué)計(jì)量組成的晶體結(jié)構(gòu)取向）兩個(gè)方面，對(duì)于已知材料，可用實(shí)驗(yàn)測(cè)量生成焓來(lái)預(yù)測(cè)。然而對(duì)于新材料和化學(xué)組成相同而空間結(jié)構(gòu)不同的材料來(lái)說(shuō)，則不可能或難以用實(shí)測(cè)生成焓來(lái)預(yù)測(cè)。來(lái)自美國(guó)的華裔科學(xué)家Haowei Peng 和 Jianwei Sun，應(yīng)用密度泛函理論結(jié)合最近開(kāi)發(fā)的強(qiáng)約束-適當(dāng)規(guī)范（strongly constrained and appropriately normed, SCAN）泛函，對(duì)材料穩(wěn)定問(wèn)題的兩個(gè)方面（化學(xué)穩(wěn)定能力&結(jié)構(gòu)選擇）作了研究，發(fā)現(xiàn)該方法能對(duì)主要化合物群組的穩(wěn)定性作可信的、有效的預(yù)測(cè)，而對(duì)過(guò)渡金屬化合物穩(wěn)定性預(yù)測(cè)，雖有進(jìn)展，但仍是一個(gè)挑戰(zhàn)。他們認(rèn)為，SCAN函數(shù)為元素周期表的重要部分提供了一個(gè)穩(wěn)健的模型，為新材料的開(kāi)發(fā)和精細(xì)相變研究提供了良方。

Efficient first-principles prediction of solid stability: Towards chemical accuracy

Yubo Zhang,Daniil A. Kitchaev,Julia Yang,Tina Chen,Stephen T. Dacek,Rafael A. Sarmiento-Pérez,Maguel A. L. Marques,Haowei Peng,Gerbrand Ceder,John P. Perdew&Jianwei Sun

AbstractThe question of material stability is of fundamental importance to any analysis of system properties in condensed matter physics and materials science. The ability to evaluate chemical stability, i.e., whether a stoichiometry will persist in some chemical environment, and structure selection, i.e. what crystal structure a stoichiometry will adopt, is critical to the prediction of materials synthesis, reactivity and properties. Here, we demonstrate that density functional theory, with the recently developed strongly constrained and appropriately normed (SCAN) functional, has advanced to a point where both facets of the stability problem can be reliably and efficiently predicted for main group compounds, while transition metal compounds are improved but remain a challenge. SCAN therefore offers a robust model for a significant portion of the periodic table, presenting an opportunity for the development of novel materials and the study of fine phase transformations even in largely unexplored systems with little to no experimental data.