Ronca Enrico, Li Zhendong, Jimenez-Hoyos Carlos A, Chan Garnet Kin-Lic
Division of Chemistry and Chemical Engineering, California Institute of Technology , Pasadena, California 91125, United States.
J Chem Theory Comput. 2017 Nov 14;13(11):5560-5571. doi: 10.1021/acs.jctc.7b00682. Epub 2017 Oct 13.
We study the dynamical density matrix renormalization group (DDMRG) and time-dependent density matrix renormalization group (td-DMRG) algorithms in the ab initio context to compute dynamical correlation functions of correlated systems. We analyze the strengths and weaknesses of the two methods in small model problems and propose two simple improved formulations, DDMRG and td-DMRG, that give increased accuracy at the same bond dimension at a nominal increase in cost. We apply DDMRG to obtain the oxygen core-excitation energy in the water molecule in a quadruple-zeta quality basis, which allows us to estimate the remaining correlation error in existing coupled cluster results. Further, we use DDMRG to compute the local density of states and gaps and td-DMRG to compute the complex polarization function, in linear hydrogen chains with up to 50 H atoms, to study metallicity and delocalization as a function of bond length.
我们在从头算的背景下研究动态密度矩阵重整化群（DDMRG）和含时密度矩阵重整化群（td-DMRG）算法，以计算相关系统的动态关联函数。我们在小模型问题中分析了这两种方法的优缺点，并提出了两种简单的改进形式，即DDMRG和td-DMRG，它们在相同键维度下以名义上增加的成本提供了更高的精度。我们应用DDMRG在四重zeta质量基组下获得水分子中的氧芯激发能，这使我们能够估计现有耦合簇结果中剩余的相关误差。此外，我们使用DDMRG计算多达50个H原子的线性氢链中的局域态密度和能隙，并使用td-DMRG计算复极化函数，以研究金属性和离域化与键长的函数关系。
