Related papers: Geometric Constraints on Two-electron Reduced Dens…
The exponential computational cost of describing strongly correlated electrons can be mitigated by adopting a reduced density-matrix (RDM)-based description of the electronic structure. While variational two-electron RDM (v2RDM) methods can…
Encoding the electronic structure of molecules using 2-electron reduced density matrices (2RDMs) as opposed to many-body wave functions has been a decades-long quest as the 2RDM contains sufficient information to compute the exact molecular…
Correlation-driven phenomena in molecular periodic systems are challenging to predict computationally not only because such systems are periodically infinite but also because they are typically strongly correlated. Here we generalize the…
Machine learning is rapidly accelerating materials and chemical discovery, but most current models target energies, forces, or selected molecular properties rather than the underlying many-body electronic structure. Learning…
The computation of strongly correlated quantum systems is challenging because of its potentially exponential scaling in the number of electron configurations. Variational calculation of the two-electron reduced density matrix (2-RDM)…
The direct variational optimization of the two-electron reduced density matrix (2RDM) can provide a reference-independent description of the electronic structure of many-electron systems that naturally captures strong or nondynamic…
The last several decades have seen significant advances in the theoretical modeling of materials within the fields of solid-state physics and materials science, but many methods commonly applied to this problem struggle to capture strong…
The two-electron reduced density matrix (2RDM) carries enough information to evaluate the electronic energy of a many-electron system. The variational 2RDM (v2RDM) approach seeks to determine the 2RDM directly, without knowledge of the wave…
The second-order reduced density matrix method (the RDM method) has performed well in determining energies and properties of atomic and molecular systems, achieving coupled-cluster singles and doubles with perturbative triples (CC SD(T))…
The electronic and magnetic properties of many strongly-correlated systems are controlled by a limited number of states, located near the Fermi level and well isolated from the rest of the spectrum. This opens a formal way for combining the…
Reduced density matrices are central to describing observables in many-body quantum systems. In electronic structure theory, the two-particle reduced density matrix (2-RDM) suffices to determine the energy and other key properties. Recent…
Two-body reduced density matrices (2RDMs) encode the essential two-electron physics of electronic states, but their quartic storage cost poses a major limitation in practical workflows. We investigate a simple protocol to compress both…
We introduce a data-driven framework for approximating the convex set of $N$-representable two-electron reduced density matrices (2-RDMs). Traditional approaches characterize this set through linear matrix inequalities that define its…
The variational two-electron reduced density matrix (v2RDM) method is generalized for the description of total angular momentum ($J$) and projection of total angular momentum ($M_{J}$) states in atomic systems described by non-relativistic…
Minimizing the energy of an $N$-electron system as a functional of a two-electron reduced density matrix (2-RDM), constrained by necessary $N$-representability conditions (conditions for the 2-RDM to represent an ensemble $N$-electron…
We present a second-order formulation of multi-reference algebraic diagrammatic construction theory [Sokolov, A. Yu. J. Chem. Phys. 2018, 149, 204113] for simulating photoelectron spectra of strongly correlated systems (MR-ADC(2)). The…
Variational calculation of the ground state energy and its properties using the second-order reduced density matrix (2-RDM) is a promising approach for quantum chemistry. A major obstacle with this approach is that the $N$-representability…
Correlations between electrons and the effective dimensionality are crucial factors that shape the properties of an interacting electron system. For example, the onsite Coulomb repulsion, U, may inhibit, or completely block the intersite…
Parametric two-electron reduced-density-matrix (p-2RDM) methods have enjoyed much success in recent years; the methods have been shown to exhibit accuracies greater than coupled cluster with single and double substitutions (CCSD) for both…
Here we present a many-body theory based on a solution of the $N$-representability problem in which the ground-state two-particle reduced density matrix (2-RDM) is determined directly without the many-particle wave function. We derive an…