Reformulating time-dependent density functional theory with non-orthogonal localized molecular orbitals.
Repository Usage Stats
Time-dependent density functional theory (TDDFT) has broad application in the study of electronic response, excitation and transport. To extend such application to large and complex systems, we develop a reformulation of TDDFT equations in terms of non-orthogonal localized molecular orbitals (NOLMOs). NOLMO is the most localized representation of electronic degrees of freedom and has been used in ground state calculations. In atomic orbital (AO) representation, the sparsity of NOLMO is transferred to the coefficient matrix of molecular orbitals (MOs). Its novel use in TDDFT here leads to a very simple form of time propagation equations which can be solved with linear-scaling effort. We have tested the method for several long-chain saturated and conjugated molecular systems within the self-consistent charge density-functional tight-binding method (SCC-DFTB) and demonstrated its accuracy. This opens up pathways for TDDFT applications to large bio- and nano-systems.
Published Version (Please cite this version)10.1039/b916688b
Publication InfoCui, Ganglong; Fang, Weihai; & Yang, Weitao (2010). Reformulating time-dependent density functional theory with non-orthogonal localized molecular orbitals. Phys Chem Chem Phys, 12(2). pp. 416-421. 10.1039/b916688b. Retrieved from https://hdl.handle.net/10161/4117.
This is constructed from limited available data and may be imprecise. To cite this article, please review & use the official citation provided by the journal.
More InfoShow full item record
Philip Handler Distinguished Professor of Chemistry
Prof. Yang, the Philip Handler Professor of Chemistry, is developing methods for quantum mechanical calculations of large systems and carrying out quantum mechanical simulations of biological systems and nanostructures. His group has developed the linear scaling methods for electronic structure calculations and more recently the QM/MM methods for simulations of chemical reactions in enzymes.