Time-Dependent Density Matrix Renormalization Group Algorithms for Nearly Exact Absorption and Fluorescence Spectra of Molecular Aggregates at Both Zero and Finite Temperature

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 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 multi-layer 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.Comment: 10 figure

Computing covariant vectors, Lyapunov vectors, Oseledets vectors, and dichotomy projectors: a comparative numerical study

Covariant vectors, Lyapunov vectors, or Oseledets vectors are increasingly being used for a variety of model analyses in areas such as partial differential equations, nonautonomous differentiable dynamical systems, and random dynamical systems. These vectors identify spatially varying directions of specific asymptotic growth rates and obey equivariance principles. In recent years new computational methods for approximating Oseledets vectors have been developed, motivated by increasing model complexity and greater demands for accuracy. In this numerical study we introduce two new approaches based on singular value decomposition and exponential dichotomies and comparatively review and improve two recent popular approaches of Ginelli et al. (2007) and Wolfe and Samelson (2007). We compare the performance of the four approaches via three case studies with very different dynamics in terms of symmetry, spectral separation, and dimension. We also investigate which methods perform well with limited data

Randomized Dynamic Mode Decomposition

This paper presents a randomized algorithm for computing the near-optimal low-rank dynamic mode decomposition (DMD). Randomized algorithms are emerging techniques to compute low-rank matrix approximations at a fraction of the cost of deterministic algorithms, easing the computational challenges arising in the area of `big data'. The idea is to derive a small matrix from the high-dimensional data, which is then used to efficiently compute the dynamic modes and eigenvalues. The algorithm is presented in a modular probabilistic framework, and the approximation quality can be controlled via oversampling and power iterations. The effectiveness of the resulting randomized DMD algorithm is demonstrated on several benchmark examples of increasing complexity, providing an accurate and efficient approach to extract spatiotemporal coherent structures from big data in a framework that scales with the intrinsic rank of the data, rather than the ambient measurement dimension. For this work we assume that the dynamics of the problem under consideration is evolving on a low-dimensional subspace that is well characterized by a fast decaying singular value spectrum