Accelerate stochastic calculation of random-phase approximation correlation energy difference with an atom-based correlated sampling
Accelerate stochastic calculation of random-phase approximation correlation energy difference with an atom-based correlated sampling
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使用基于原子的相关采样加速随机相位近似相关能量差的随机计算
DOI：
10.1088/2516-1075/abde94
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发表时间：
2021
影响因子：
2.6
通讯作者：
Huang, C.
中科院分区：
文献类型：
--
作者：
Chi, Y-C.;Huang, C.
提出了一种计算随机位相近似(RPA)关联能量的核多项式方法。在该方法中，RPA关联能由库仑势和密度线性响应函数的乘积矩阵表示。通过用切比雪夫多项式展开矩阵的状态密度来计算矩阵特征值上的积分。通过随机抽样获得展开式中的系数。由于实际中经常关注的是两个系统之间的能量差，因此本工作的另一个重点是开发一种相关采样方案，以加速两个相似系统之间的RPA关联能量差的随机计算的收敛。该方案被称为基于原子的相关采样(ACS)。通过计算丙酮生成2-丙烯醇的异构化能和水-气变换反应的能量来考察该催化剂的性能。使用蚁群算法，这两个算例的收敛速度分别提高了3.6倍和4.5倍。这些方法有望用于计算发生在局部区域的反应的RPA水平的反应能，例如计算分子在过渡金属表面上的吸附能以模拟表面催化。
A kernel polynomial method is developed to calculate the random phase approximation (RPA) correlation energy. In the method, the RPA correlation energy is formulated in terms of the matrix that is the product of the Coulomb potential and the density linear response functions. The integration over the matrix's eigenvalues is calculated by expanding the density of states of the matrix in terms of the Chebyshev polynomials. The coefficients in the expansion are obtained through stochastic sampling. Since it is often the energy difference between two systems that is of much interest in practice, another focus of this work is to develop a correlated sampling scheme to accelerate the convergence of the stochastic calculations of the RPA correlation energy difference between two similar systems. The scheme is termed the atom-based correlated sampling (ACS). The performance of ACS is examined by calculating the isomerization energy of acetone to 2-propenol and the energy of the water–gas shift reaction. Using ACS, the convergences of these two examples are accelerated by 3.6 and 4.5 times, respectively. The methods developed in this work are expected to be useful for calculating RPA-level reaction energies for the reactions that take place in local regions, such as calculating the adsorption energies of molecules on transition metal surfaces for modeling surface catalysis.
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影响因子：
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作者：
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通讯作者：
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影响因子：
4.4
作者：
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影响因子：
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影响因子：
5.5
作者：
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DOI：
--
发表时间：
1994
期刊：
Physical Review B (Condensed Matter)
影响因子：
--
作者：
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通讯作者：
Lin