Time-Dependent Density Matrix Renormalization Group Algorithms for Nearly Exact Absorption and Fluorescence Spectra of Molecular Aggregates at Both Zero and Finite Temperature
Time-Dependent Density Matrix Renormalization Group Algorithms for Nearly Exact Absorption and Fluorescence Spectra of Molecular Aggregates at Both Zero and Finite Temperature
复制标题
零温度和有限温度下分子聚集体近乎精确的吸收和荧光光谱的瞬态密度矩阵重整化群算法
DOI：
10.1021/acs.jctc.8b00628
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发表时间：
2018-10-01
影响因子：
5.5
通讯作者：
Chan, Garnet Kin-Lic
中科院分区：
文献类型：
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作者：
Ren, Jiajun;Shuai, Zhigang;Chan, Garnet Kin-Lic
我们实现并应用含时密度矩阵重整化群（TD-DMRG）算法在零温度和有限温度下计算分子聚集体的线性吸收和荧光光谱。我们的实现是在一个矩阵产品状态/运营商框架内的激子和振动自由度的显式治疗，它使用的零激子空间中的哈密顿量的局部性，以提高计算的效率和准确性。我们证明了几个分子聚集体模型的计算方法的力量，比较我们的结果对那些从多层多组态随时间变化的Hartree和n-粒子近似。我们发现，TD-DMRG提供了一个准确和有效的路线来计算分子聚集体的光谱。
We implement and apply time-dependent density matrix renormalization group (TD-DMRG) algorithms at zero and finite temperature to compute the linear absorption and fluorescence spectra of molecular aggregates. Our implementation is within a matrix product state/operator framework with an explicit treatment of the excitonic and vibrational degrees of freedom, and it uses the locality of the Hamiltonian in the zero-exciton space to improve the efficiency and accuracy of the calculations. We demonstrate the power of the method by calculations on several molecular aggregate models, comparing our results against those from multilayer multiconfiguration time-dependent Hartree and n-particle approximations. We find that TD-DMRG provides an accurate and efficient route to calculate the spectrum of molecular aggregates.