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Investigation of Environmental Effects on Iron-Sulfur Clusters through Linear-Response Density Matrix Embedding Theory

Subject Area Theoretical Chemistry: Electronic Structure, Dynamics, Simulation
Theoretical Chemistry: Molecules, Materials, Surfaces
Term from 2021 to 2024
Project identifier Deutsche Forschungsgemeinschaft (DFG) - Project number 495279997
 
Final Report Year 2024

Final Report Abstract

The quantum mechanical interaction of electrons is at the origin of various essential processes ranging from biology to exotic material properties like superconductivity. Gaining microscopic insights into how these quantum mechanical interactions enable these processes is of great interest, as it would allow the rational design of artificial systems with similar or even amplified properties. Unfortunately, such a microscopic understanding is experimentally often only indirectly accessible. In contrast, the numerical solution of the (electronic) Schrödinger equation directly enables the understanding of the mechanisms responsible for these phenomena. In practice, the exact solution is only achievable for systems consisting of a small number of electrons due to the exponential increase in computational cost with increasing system size. Developing approaches that find reliable approximations to the Schrödinger equation is therefore essential. Quantum embedding (QE) strategies achieve this goal by partitioning the system into a region of interest (impurity) and an environment. The success of these methods originates from the fact that the reduced dimensionality of the impurity allows for an (almost) exact solution of the Schrödinger equation, while the effect of the environment’s electronic structure is accounted for using more approximate (and computationally less demanding) approaches. One of the methods enabling such a description is Density Matrix Embedding Theory (DMET). Here, the goal of the project is the “Investigation of Environmental Effects on Iron-Sulfur Clusters through Linear-Response Density Matrix Embedding Theory”. Preliminary work on response properties within DMET indicated that the proposed ansatz seemed unsuitable for the description of excited states in molecular systems with strong electron correlation, i.e., iron-sulfur clusters. An alternative strategy towards achieving this goal has therefore been pursued. By unifying diagrammatic methods used in quantum chemistry and theoretical condensed matter physics, a new route towards the efficient determination of such excitations has been found. These new developments will allow for a rigorous extension of these methods to strongly interacting systems for the first time. The original goal—“Investigation of Environmental Effects on Iron-Sulfur Clusters through Linear-Response Density Matrix Embedding Theory”—is therefore within reach, albeit using a different methodology. Fortunately, we identified linear-response DMET as a promising tool in a different context. It enables the identification of superconducting phase transitions in strongly correlated quantum materials. This is made possible by the recent application of DMET in the ab initio simulation of superconducting trends in cuprates. These developments represent an important step toward understanding the microscopic origin of high-temperature superconductivity in real materials, which has been a challenge for theory and experiments for decades.

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