Quantum embedding for material chemistry based on domain separation and open subsystems

Mosquera, Martín A.; Jones, Leighton O.; Ratner, Mark A.; Schatz, George C.

doi:10.1002/qua.26184

Cited by 6 publications

(11 citation statements)

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“…However, when considering a fragment in a molecule as an open system interacting with its environment, it is often convenient to treat that environment as a bath of electrons with which the fragment can exchange electrons and acquire, on average, a partial charge. This situation is especially relevant when describing intermolecular charge transfer.. [109] Mosquera et al [110] describe how their recent method that locally couples open subsystems [111] can naturally account for fractional electron numbers in the fragments. They also describe a related method for domain separation in DFT (DS-DFT) that can be used for many embedding applications, including wavefunction embedding.…”

Section: Qm/mm and Continuum Dielectrics Embeddingmentioning

confidence: 99%

Quantum embedding electronic structure methods

Wasserman

Pavanello

2020

Int J of Quantum Chemistry

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This editorial serves as an introduction to a series of 10 papers collected under the special issue "Quantum Embedding Electronic Structure Methods." The idea to assemble a special issue came during a symposium at the Spring 2019 meeting of the American Chemical Society where we (Adam and Michele) organized a Physical Chemistry symposium bearing the same name as the special issue. The symposium ran for the entire week and featured many flavors of embedding: from density embedding to embedding within lattice models, as well as continuum models and many-body expansions. While it may seem that these approaches are far removed from each other, the symposium highlighted common goals, such as the reduction of the computational effort through "divide-and-conquer" strategies, and stressed the importance of establishing a common language across all embedding methods. It is clear that human interaction is key for scientific progress, and traveling to conferences is an important aspect of scientific research. Unfortunately, we write this introduction during a pandemic of historic proportions, when working on theoretical and computational chemistry may seem like an unacceptable luxury or an unjustified distraction. It is striking to remember how we interacted prior to the outbreak. Figure 1 provides a glimpse into the social nature of the symposium participants and the massive crowds at the conference. The editorial is organized into three sections: Origins, where we briefly discuss the origins of embedding methods for newcomers to the field; Present, where we highlight some of the current efforts with an emphasis on the contributions submitted to this Special Issue of IJQC; and Future, where we enumerate a few of the open challenges in the field and speculate on some of its possible future directions. 2 | ORIGINS Modern embedding methods can be broadly classified into three groups: density embedding, density-matrix and Green's function (GF) embedding, and classical (quantum mechanics / molecular mechanics (QM/MM) and continuum dielectrics) embedding. We briefly discuss the origins of these three approaches separately. orbitals. The KSCED follows by requiring that E[n] be minimized directly with regard to variations of the n α (r). A different set of equations is

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Section: Qm/mm and Continuum Dielectrics Embeddingmentioning

confidence: 99%

Quantum embedding electronic structure methods

Wasserman

Pavanello

2020

Int J of Quantum Chemistry

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“…In this section, we describe the steps we follow in the implementation of DS-DFT and DS-TDDFT calculations. The formal theoretical background is presented in ref , and additional details are discussed in refs and .…”

Section: Theory Implementationmentioning

confidence: 99%

“…In analogy with standard HF algorithms, the computation of the domain-screened HF exchange energy can be carried out through an exchange matrix: where ϕ μ denotes a basis function. As suggested in ref , the above matrix can be computed by means of “orbital” fitting. First, we define the orbital: …”

Section: Theory Implementationmentioning

confidence: 99%

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Domain Separated Density Functional Theory for Reaction Energy Barriers and Optical Excitations

et al. 2020

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We recently proposed domain separated density functional theory (DS-DFT), a framework that allows for the combination of different levels of theory for the computation of the electronic structure of molecules. This work discusses the application of DS-DFT to the computation of transition-state energy barriers and optical absorption spectra. We considered several hydrogen abstraction reactions and optical spectra of molecule/metal cluster systems, including the absorption of individual species such as carbon monoxide, methane, and molecular hydrogen to a Li6 cluster. We present and discuss two domain-separated methods: (i), the screened-density approximation (SDA) and (ii) linearly weighted exchange (LWE). We find that SDA, which is applied as a hybridization based on atomic domains, could be useful to computing energy barriers, whereas LWE is suited for the analysis of electronic properties such as ground-state gaps, excitation energies, and oscillator strengths.

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“…44 We mention here that alternative QM/QM approaches, avoiding the use of KEDFs and allowing also for fragmentation in subsystems through covalent bonds, have been recently proposed (see for instance Ref. 14,15,[45][46][47][48][49][50][51] ).…”

Section: Introductionmentioning

confidence: 99%