论文标题
QuestDB:电子结构社区的高度精确激发能的数据库
QUESTDB: a database of highly-accurate excitation energies for the electronic structure community
论文作者
论文摘要
我们描述了过去几年来创建各种本质($π\ toπ^*$,$ n \toπ^*$,double兴奋,rydberg,rydberg,singlet,doublet,tripet等)的大量高度高度精确的垂直激发能的努力。这些值是使用增量策略获得的,该策略在于使用越来越大的弥漫性基集组合高阶耦合群集和选定的配置交互计算,以达到高精度。所谓的垂直激发Quest数据库的关键方面之一是,它不依赖任何实验值,避免了与实验固有链接的潜在偏差并促进理论交叉比较。遵循此复合协议,我们能够为每个转换中的每一个以及基于基础的校正TBE(即接近完整的基集限制),为它们中的每一个提供了AUG-CC-PVTZ基础设置的理论最佳估计(TBE)。已经使用了TBE/AUG-CC-PVTZ来基准大量(较低的)波函数方法,例如顺式(D),ADC(2),CC2,CC2,Steom-CCSD,CCSD,CCSDR,CCSDR(3),CCSDT-3,CCSDT-3,ADC(3),CC3,CC3,NEVPT2,NEVPT2和其他(包括Spiriment Spinec)。为了收集Quest项目期间产生的大量数据,我们创建了一个网站[https://lcpq.github.io/questdb_website],在其中人们可以轻松地测试和比较给定方法相对于各种变量的准确性,以提供分子大小或其家庭的本质,我们将提供诸如兴奋的状态,我们将提供的综合概述,我们将提供一定的效果。激发态方法的发展。
We describe our efforts of the past few years to create a large set of more than 500 highly-accurate vertical excitation energies of various natures ($π\to π^*$, $n \to π^*$, double excitation, Rydberg, singlet, doublet, triplet, etc) in small- and medium-sized molecules. These values have been obtained using an incremental strategy which consists in combining high-order coupled cluster and selected configuration interaction calculations using increasingly large diffuse basis sets in order to reach high accuracy. One of the key aspect of the so-called QUEST database of vertical excitations is that it does not rely on any experimental values, avoiding potential biases inherently linked to experiments and facilitating theoretical cross comparisons. Following this composite protocol, we have been able to produce theoretical best estimate (TBEs) with the aug-cc-pVTZ basis set for each of these transitions, as well as basis set corrected TBEs (i.e., near the complete basis set limit) for some of them. The TBEs/aug-cc-pVTZ have been employed to benchmark a large number of (lower-order) wave function methods such as CIS(D), ADC(2), CC2, STEOM-CCSD, CCSD, CCSDR(3), CCSDT-3, ADC(3), CC3, NEVPT2, and others (including spin-scaled variants). In order to gather the huge amount of data produced during the QUEST project, we have created a website [https://lcpq.github.io/QUESTDB_website] where one can easily test and compare the accuracy of a given method with respect to various variables such as the molecule size or its family, the nature of the excited states, the type of basis set, etc. We hope that the present review will provide a useful summary of our effort so far and foster new developments around excited-state methods.