open access

https://hdl.handle.net/2115/54784

Linear response theory for the density matrix renormalization group : efficient algorithms for strongly correlated excited states

英語

2014-01-14

American Institute of Physics

Journal of chemical physics

140(2)

024108-1-024108-13

Linear response theory for the density matrix renormalization group (DMRG-LRT) was first presented in terms of the DMRG renormalization projectors [J. J. Dorando, J. Hachmann, and G. K.-L. Chan, J. Chem. Phys. 130, 184111 (2009)]. Later, with an understanding of the manifold structure of the matrix product state (MPS) ansatz, which lies at the basis of the DMRG algorithm, a way was found to construct the linear response space for general choices of the MPS gauge in terms of the tangent space vectors [J. Haegeman, J. I. Cirac, T. J. Osborne, I. Pizorn, H. Verschelde, and F. Verstraete, Phys. Rev. Lett. 107, 070601 (2011)]. These two developments led to the formulation of the Tamm-Dancoff and random phase approximations (TDA and RPA) for MPS. This work describes how these LRTs may be efficiently implemented through minor modifications of the DMRG sweep algorithm, at a computational cost which scales the same as the ground-state DMRG algorithm. In fact, the mixed canonical MPS form implicit to the DMRG sweep is essential for efficient implementation of the RPA, due to the structure of the second-order tangent space. We present ab initio DMRG-TDA results for excited states of polyenes, the water molecule, and a [2Fe-2S] iron-sulfur cluster.

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Copyright 2014 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in Journal of Chemical Physics 140, 024108 (2014) and may be found at http://scitation.aip.org/content/aip/journal/jcp/140/2/10.1063/1.4860375.

0021-9606

1089-7690

AA00694991