A critical disadvantage of primal-dual interior-point methods compared to dual interior-point methods for large scale semidefinite programs (SDPs) has been that the primal positive semidefinite matrix variable becomes fully dense in general even when all data matrices are sparse. Based on some fundamental results about positive semidefinite matrix completion, this article proposes a general method of exploiting the aggregate sparsity pattern over all data matrices to overcome this disadvantage. Our method is used in two ways. One is a conversion of a sparse SDP having a large scale positive semidefinite matrix variable into an SDP having multiple but smaller positive semidefinite matrix variables to which we can effectively apply any interior-point method for SDPs employing a standard block-diagonal matrix data structure. The other way is an incorporation of our method into primal-dual interior-point methods which we can apply directly to a given SDP. In Part II of this article, we will investigate an implementation of such a primal-dual interior-point method based on positive definite matrix completion, and report some numerical results.

The variational approach for electronic structure based on the two-body reduced density matrix is studied, incorporating two representability conditions beyond the previously used P, Q, and G conditions. The additional conditions (called T1 and T2 here) are implicit in the work of Erdahl [Int. J. Quantum Chem. 13, 697 (1978)] and extend the well-known three-index diagonal conditions also known as the Weinhold-Wilson inequalities. The resulting optimization problem is a semidefinite program, a convex optimization problem for which computational methods have greatly advanced during the past decade. Formulating the reduced density matrix computation using the standard dual formulation of semidefinite programming, as opposed to the primal one, results in substantial computational savings and makes it possible to study larger systems than was done previously. Calculations of the ground state energy and the dipole moment are reported for 47 different systems, in each case using an STO-6G basis set and comparing with Hartree-Fock, singly and doubly substituted configuration interaction, Brueckner doubles (with triples), coupled cluster singles and doubles with perturbational treatment of triples, and full configuration interaction calculations. It is found that the use of the T1 and T2 conditions gives a significant improvement over just the P, Q, and G conditions, and provides in all cases that we have studied more accurate results than the other mentioned approximations.

The ground-state fermion second-order reduced density matrix ͑2-RDM͒ is determined variationally using itself as a basic variable. As necessary conditions of the N-representability, we used the positive semidefiniteness conditions, P, Q, and G conditions that are described in terms of the 2-RDM. The variational calculations are performed by using recently developed semidefinite programming algorithm ͑SDPA͒. The calculated energies of various closed-and open-shell atoms and molecules are excellent, overshooting only slightly the full-CI energies. There was no case where convergence was not achieved. The calculated properties also reproduce well the full-CI results.

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The reduced density matrix (RDM) method, which is a variational calculation based on the second-order reduced density matrix, is applied to the ground state energies and the dipole moments for 57 different states of atoms, molecules, and to the ground state energies and the elements of 2-RDM for the Hubbard model. We explore the well-known N-representability conditions (P, Q, and G) together with the more recent and much stronger T1 and T2(') conditions. T2(') condition was recently rederived and it implies T2 condition. Using these N-representability conditions, we can usually calculate correlation energies in percentage ranging from 100% to 101%, whose accuracy is similar to CCSD(T) and even better for high spin states or anion systems where CCSD(T) fails. Highly accurate calculations are carried out by handling equality constraints and/or developing multiple precision arithmetic in the semidefinite programming (SDP) solver. Results show that handling equality constraints correctly improves the accuracy from 0.1 to 0.6 mhartree. Additionally, improvements by replacing T2 condition with T2(') condition are typically of 0.1-0.5 mhartree. The newly developed multiple precision arithmetic version of SDP solver calculates extraordinary accurate energies for the one dimensional Hubbard model and Be atom. It gives at least 16 significant digits for energies, where double precision calculations gives only two to eight digits. It also provides physically meaningful results for the Hubbard model in the high correlation limit.