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This paper identifies the off-diagonal low rank (ODLR) property in key matrices used in computational chemistry, such as the Coulomb matrix and Fock matrix, which allows for more efficient storage and computation. By demonstrating that these matrices exhibit low numerical ranks in their off-diagonal blocks when appropriately ordered, the authors highlight a significant mathematical insight that has been underutilized in the field. The key result shows that Fock matrices and localized molecular orbital coefficient matrices adhere to the ODLR property, enabling linear scaling electronic structure calculations in gapless systems at zero electronic temperature.
Discovering that Fock matrices and LMO coefficient matrices exhibit off-diagonal low rank could revolutionize computational chemistry by enabling linear scaling calculations for complex systems.
Many matrices in computational chemistry are neither sparse nor low-rank, making the design of low-scaling algorithms difficult. In this Perspective, we point out that many important matrices in computational chemistry, such as the Coulomb matrix, the electronic repulsion integral tensor, the density matrix, the localized molecular orbital (LMO) coefficient matrix, the Fock matrix, and the nuclear Hessian matrix share the same property: when their basis functions are suitably ordered, their off-diagonal blocks have low numerical ranks (despite that they as a whole have high numerical ranks). This property, termed off-diagonal low rank (ODLR), has been extensively studied in the mathematics community, but has surprisingly found very little use in computational chemistry. This Perspective reviews the existing mathematical literature on how to use the ODLR property of matrices to compactly store, as well as efficiently calculate or use them. Subsequently, we review the use of the ODLR property in computational chemistry, and point out possible future opportunities of devising new low-scaling methods for dense, full-rank matrices, exploiting the ODLR property. In particular, we prove for the first time that Fock matrices and LMO coefficient matrices satisfy the ODLR property, even if the system is gapless (in which case the matrices are dense). This paves the way to linear scaling electronic structure calculations of gapless systems at zero electronic temperature.