Quantum–Quantum and Quantum–Quantum-Classical Schemes for Near-Gap Excitations with Projection-Based-Embedded <i>GW</i>-Bethe–Salpeter Equation

Sundaram, Vivek; Baumeier, Björn

doi:10.1021/acs.jctc.4c00163

J. Chem. Theory Comput.

2024

DOI: 10.1021/acs.jctc.4c00163

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Quantum–Quantum and Quantum–Quantum-Classical Schemes for Near-Gap Excitations with Projection-Based-Embedded GW-Bethe–Salpeter Equation

Vivek Sundaram,

Björn Baumeier

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2024

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Cited by 2 publications

References 68 publications

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From Many-Body Ab Initio to Effective Excitonic Models: A Versatile Mapping Approach Including Environmental Embedding Effects

Rodriguez-Mayorga,

Blase,

Duchemin

et al. 2024

J. Chem. Theory Comput.

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We present an original multistate projective diabatization scheme based on Green's function formalisms that allows the systematic mapping of many-body ab initio calculations onto effective excitonic models. This method inherits the ability of the Bethe−Salpeter equation to describe Frenkel molecular excitons and intermolecular charge-transfer states equally well, as well as the possibility for an effective description of environmental effects in a QM/MM framework. The latter is found to be a crucial element in order to obtain accurate model parameters for condensed phases and to ensure their transferability to excitonic models for extended systems. The method is presented through a series of examples illustrating its quality, robustness, and internal consistency.

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From Many-Body Ab Initio to Effective Excitonic Models: A Versatile Mapping Approach Including Environmental Embedding Effects

Rodriguez-Mayorga,

Blase,

Duchemin

et al. 2024

J. Chem. Theory Comput.

View full text Add to dashboard Cite

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Optical Gaps of Ionic Materials from GW/BSE-in-DFT and CC2-in-DFT

Sharma,

Sierka

2024

J. Chem. Theory Comput.

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This work presents a density functional theory (DFT)-based embedding technique for the calculation of optical gaps in ionic solids. The approach partitions the supercell of the ionic solid and embeds a small molecule-like cluster in a periodic environment using a cluster-in-periodic embedding method. The environment is treated with DFT, and its influence on the cluster is captured by a DFT-based embedding potential. The optical gap is estimated as the lowest singlet excitation energy of the embedded cluster, obtained using a wave function theory method: secondorder approximate coupled-cluster singles and doubles (CC2), and a many-body perturbation theory method: GW approximation combined with the Bethe−Salpeter equation (GW/BSE). The calculated excitation energies are benchmarked against the periodic GW/BSE values, equation-of-motion coupled-cluster singles and doubles (EOM-CCSD) results, and experiments. Both CC2-in-DFT and GW/BSE-in-DFT deliver excitation energies that are in good agreement with experimental values for several ionic solids (MgO, CaO, LiF, NaF, KF, and LiCl) while incurring negligible computational costs. Notably, GW/BSE-in-DFT exhibits remarkable accuracy with a mean absolute error (MAE) of just 0.38 eV with respect to experiments, demonstrating the effectiveness of the embedding strategy. In addition, the versatility of the method is highlighted by investigating the optical gap of a 2D MgCl 2 system and the excitation energy of an oxygen vacancy in MgO, with results in good agreement with reported values.

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Quantum–Quantum and Quantum–Quantum-Classical Schemes for Near-Gap Excitations with Projection-Based-Embedded GW-Bethe–Salpeter Equation

Cited by 2 publications

References 68 publications

From Many-Body Ab Initio to Effective Excitonic Models: A Versatile Mapping Approach Including Environmental Embedding Effects

From Many-Body Ab Initio to Effective Excitonic Models: A Versatile Mapping Approach Including Environmental Embedding Effects

Optical Gaps of Ionic Materials from GW/BSE-in-DFT and CC2-in-DFT

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