Erratum: “Interfacial water asymmetry at ideal electrochemical interfaces” [J. Chem. Phys. 156, 014705 (2022)]

Shandilya, Abhishek; Schwarz, Kathleen; Sundararaman, Ravishankar

doi:10.1063/5.0089796

Cited by 4 publications

(4 citation statements)

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“…The simplest version of this amounts to shifting the plane of electrode charge in classical MD toward the electrolyte, effectively reducing the gap and increasing the capacitance . This is equivalent to adding a surface dipole potential (Figure a), , whose magnitude is determined empirically or from electronic DFT calculations of the electrode under an applied electric field. , More generally, the classical MD charge density can be replaced by an electron density profile calculated using DFT, thus including nonlinear changes of the electronic response with electrode potential that can affect the shape of the capacitance curves (Figure b). , Alternately, the mean electrostatic potential from classical MD of the electrolyte can be incorporated into electronic DFT of the electrode to include a degree of self-consistency in the interfacial response …”

Section: Classical Molecular Dynamics Accuracymentioning

confidence: 99%

“…Underestimation of electrochemical capacitance by classical MD can be fixed by (a) a dipole correction that accounts for the electronic induced charge distribution, or equivalently, (b) a shift of the electrode charge density toward the electrolyte. , (c) Additionally, a semiclassical Thomas–Fermi model can approximately incorporate electronic screening of the electrode to decrease the overall capacitance for electrodes that are not perfect conductors . (a) Adapted with permission from ref .…”

Section: Classical Molecular Dynamics Accuracymentioning

confidence: 99%

“…113,114 More generally, the classical MD charge density can be replaced by an electron density profile calculated using DFT, thus including nonlinear changes of the electronic response with electrode potential that can affect the shape of the capacitance curves (Figure 9b). 21,115 Alternately, the mean electrostatic potential from classical MD of the electrolyte can be incorporated into electronic DFT of the electrode to include a degree of self-consistency in the interfacial response. 116 For electrodes that are not perfect conductors, efforts have been made to account for both the electronic polarizability of the electrode and the electrode screening.…”

Section: Electronic Polarizability Correctionsmentioning

confidence: 99%

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Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

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Atomistic simulation of the electrochemical double layer is an ambitious undertaking, requiring quantum mechanical description of electrons, phase space sampling of liquid electrolytes, and equilibration of electrolytes over nanosecond time scales. All models of electrochemistry make different trade-offs in the approximation of electrons and atomic configurations, from the extremes of classical molecular dynamics of a complete interface with point-charge atoms to correlated electronic structure methods of a single electrode configuration with no dynamics or electrolyte. Here, we review the spectrum of simulation techniques suitable for electrochemistry, focusing on the key approximations and accuracy considerations for each technique. We discuss promising approaches, such as enhanced sampling techniques for atomic configurations and computationally efficient beyond density functional theory (DFT) electronic methods, that will push electrochemical simulations beyond the present frontier.

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Section: Classical Molecular Dynamics Accuracymentioning

confidence: 99%

Section: Classical Molecular Dynamics Accuracymentioning

confidence: 99%

Section: Electronic Polarizability Correctionsmentioning

confidence: 99%

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Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

2022

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“…12–14 Furthermore, the non-radiative charge recombination and passivation defect approaches may increase critical parameters such as open circuit voltage, fill factor, and hysteresis potentially improving the performance of PSCs. 15…”

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confidence: 99%

Harnessing solar energy with NH₄Cl-doped hole transport layers in inverted perovskite solar cells

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et al. 2023

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Solvent effects determine the sign of the charges of maximum entropy and capacitance at silver electrodes

Sundararaman

Schwarz

2023

The Journal of Chemical Physics

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Fully harnessing electrochemical interfaces for reactions requires a detailed understanding of solvent effects in the electrochemical double layer. Predicting the significant impact of solvent on entropic and electronic properties of electrochemical interfaces has remained an open challenge of computational electrochemistry. Using molecular dynamics simulations of silver-water and silver-acetonitrile interfaces, we show that switching the solvent changes the signs for both the charges of maximum capacitance (CMC) and maximum entropy (CME). Contrasting the capacitance and CME behavior of these two interfaces, we demonstrate that the preferred orientation of the solvent molecule and the corresponding charge density determine the sign of the CMC and CME, and hence, the qualitatively-different charge asymmetry of the electrochemical interface.

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Erratum: “Interfacial water asymmetry at ideal electrochemical interfaces” [J. Chem. Phys. 156, 014705 (2022)]

Cited by 4 publications

References 1 publication

Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

Harnessing solar energy with NH₄Cl-doped hole transport layers in inverted perovskite solar cells

Solvent effects determine the sign of the charges of maximum entropy and capacitance at silver electrodes

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Erratum: “Interfacial water asymmetry at ideal electrochemical interfaces” [J. Chem. Phys. 156, 014705 (2022)]

Cited by 4 publications

References 1 publication

Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

Harnessing solar energy with NH4Cl-doped hole transport layers in inverted perovskite solar cells

Solvent effects determine the sign of the charges of maximum entropy and capacitance at silver electrodes

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Product

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Harnessing solar energy with NH₄Cl-doped hole transport layers in inverted perovskite solar cells