# Direct Comparison of Many-Body Methods for Realistic Electronic Hamiltonians

@article{Williams2020DirectCO, title={Direct Comparison of Many-Body Methods for Realistic Electronic Hamiltonians}, author={Kiel T. Williams and Yuan Yao and Jia Li and Li Chen and Hao Shi and Mario Motta and Chun-Jiang Niu and Ushnish Ray and Sheng Guo and Robert J Anderson and Junhao Li and Lan Nguyen Tran and Chia-Nan Yeh and Bastien Mussard and Sandeep Sharma and Fabien Bruneval and Mark van Schilfgaarde and George H. Booth and Garnet Kin-Lic Chan and Shiwei Zhang and Emanuel Gull and Dominika Zgid and Andrew J. Millis and C. J. Umrigar and Lucas K. Wagner}, journal={Physical Review X}, year={2020} }

A large collaboration carefully benchmarks 20 first principles many-body electronic structure methods on a test set of 7 transition metal atoms, and their ions and monoxides. Good agreement is attained between the 3 systematically converged methods, resulting in experiment-free reference values. These reference values are used to assess the accuracy of modern emerging and scalable approaches to the many-electron problem. The most accurate methods obtain energies indistinguishable from…

## 54 Citations

### Ab initio electronic density in solids by many-body plane-wave auxiliary-field quantum Monte Carlo calculations

- Physics
- 2021

We present accurate many-body results of the electronic densities in several solid materials, including Si, NaCl, and Cu. These results are obtained using the ab initio auxiliary-field quantum Monte…

### The Ground State Electronic Energy of Benzene.

- PhysicsThe journal of physical chemistry letters
- 2020

We report on the findings of a blind challenge devoted to determining the frozen-core, full configuration interaction (FCI) ground-state energy of the benzene molecule in a standard…

### Orbital Optimization in Selected Configuration Interaction Methods.

- PhysicsJournal of chemical theory and computation
- 2021

It is demonstrated that taking the coupling into account is crucial for fast convergence and recommend two quasi-fully coupled methods for such applications: accelerated diagonal Newton and Broyden-Fletcher-Goldfarb-Shanno.

### Ab Initio Full Cell GW+DMFT for Correlated Materials

- PhysicsPhysical Review X
- 2021

Quantitative prediction of electronic properties in correlated materials requires simulations without empirical truncations and parameters. We present a method to achieve this goal through a new ab…

### The performance of CIPSI on the ground state electronic energy of benzene.

- Physics, ChemistryThe Journal of chemical physics
- 2020

The performance of the configuration interaction using a perturbative selection made iteratively method on the non-relativistic frozen-core correlation energy of the benzene molecule in the cc-pVDZ basis is reported.

### Quantification of electron correlation for approximate quantum calculations.

- PhysicsThe Journal of chemical physics
- 2022

State-of-the-art many-body wave function techniques rely on heuristics to achieve high accuracy at an attainable computational cost to solve the many-body Schrödinger equation. By far, the most…

### Almost exact energies for the Gaussian-2 set with the semistochastic heat-bath configuration interaction method.

- ChemistryThe Journal of chemical physics
- 2020

The recently developed semistochastic heat-bath configuration interaction (SHCI) method is a systematically improvable selected configuration interaction plus perturbation theory method capable of…

### Ab initio self-energy embedding for the photoemission spectra of NiO and MnO

- Physics
- 2020

The accurate ab initio simulation of periodic solids with strong correlations is one of the grand challenges of condensed matter. While mature methods exist for weakly correlated solids, the ab…

### Vibrational heat-bath configuration interaction.

- PhysicsThe Journal of chemical physics
- 2021

VHCI is a selected CI approach that uses a simple criterion to identify important basis states with a pre-sorted list of anharmonic force constants and produces vibrational spectra of tens or hundreds of states with sub-wavenumber accuracy at low computational cost.

### Toward a systematic improvement of the fixed-node approximation in diffusion Monte Carlo for solids-A case study in diamond.

- PhysicsThe Journal of chemical physics
- 2020

A computational method is presented that produces trial wavefunctions with systematically improvable nodes for DMC calculations of periodic solids and indicates a very good error cancellation in carbon diamond between the bulk and atomic total fixed-node energies when using single-determinant nodes.

## References

SHOWING 1-10 OF 105 REFERENCES

### Do Practical Standard Coupled Cluster Calculations Agree Better than Kohn-Sham Calculations with Currently Available Functionals When Compared to the Best Available Experimental Data for Dissociation Energies of Bonds to 3d Transition Metals?

- ChemistryJournal of chemical theory and computation
- 2015

The available experimental data do not provide a justification for using conventional single-reference CC theory calculations to validate or test xc functionals for systems involving 3d transition metals, and the T1 diagnostics correlate the errors better than either the M diagnostics or the B1 DFT-based diagnostics.

### Comparing many-body approaches against the helium atom exact solution

- PhysicsSciPost Physics
- 2019

Over time, many different theories and approaches have been developed
to tackle the many-body problem in quantum chemistry, condensed-matter
physics, and nuclear physics. Here we use the helium atom,…

### Towards the solution of the many-electron problem in real materials: equation of state of the hydrogen chain with state-of-the-art many-body methods

- Physics
- 2017

We present numerical results for the equation of state of an infinite chain of hydrogen atoms. A variety of modern many-body methods are employed, with exhaustive cross-checks and validation.…

### Accurate Ab initio calculation of ionization potentials of the first-row transition metals with the configuration-interaction quantum Monte Carlo technique.

- PhysicsPhysical review letters
- 2015

Accurate ionization potentials of the first-row transition-metal atoms are obtained via the initiator full configuration quantum Monte Carlo technique, performing a stochastic integration of the…

### Generalized Self-Energy Embedding Theory.

- PhysicsThe journal of physical chemistry letters
- 2017

Ab initio quantum chemistry calculations for systems with large active spaces are notoriously difficult and cannot be successfully tackled by standard methods. We generalize a Green's function QM/QM…

### Correlated electron pseudopotentials for 3d-transition metals.

- Physics, ChemistryThe Journal of chemical physics
- 2015

The CEPPs give better results in the correlated-electron calculations than Hartree-Fock-based pseudopotentials available in the literature, and to include relativistic effects.

### Communication: DFT treatment of strong correlation in 3d transition-metal diatomics.

- ChemistryThe Journal of chemical physics
- 2017

This work tests B13 on bond energies of transition-metal diatomics in this work, with promising results.

### Shape and energy consistent pseudopotentials for correlated electron systems.

- PhysicsThe Journal of chemical physics
- 2017

The eCEPPs provide a significant improvement in optimised geometries and dissociation energies for small molecules, with errors for the latter being an order-of-magnitude smaller than for Hartree-Fock-based pseudopotentials available in the literature.

### Helium Atom Excitations by the GW and Bethe-Salpeter Many-Body Formalism.

- PhysicsPhysical review letters
- 2017

The accuracy of the BSE and GW approximations is not significantly limited by self-interaction and self-screening problems even in this few electron limit, and the results are compared to those obtained by time-dependent density-functional theory.

### Quantum Monte Carlo simulations of solids

- Physics
- 2001

This article describes the variational and fixed-node diffusion quantum Monte Carlo methods and how they may be used to calculate the properties of many-electron systems. These stochastic…