NWPEsSe: an Adaptive-Learning Global Optimization Algorithm for Nanosized Cluster Systems

Zhang, Jun; Glezakou, Vassiliki‐Alexandra; Rousseau, Roger; Nguyen, Manh‐Thuong

doi:10.26434/chemrxiv.11302301.v2

Cited by 5 publications

(6 citation statements)

References 31 publications

(34 reference statements)

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“…In addition, the bond distances of Ge 2 , AgGe, and AuGe predicted by mPW2PLYP are 2.38, 19 2.45, 19 and 2.34 Å, 16 which are in good agreement with the experimental values of 2.368, 48 2.54, 49 and 2.38 Å, 50 respectively. On the other hand, many successful examples of the ABCluster were reported recently, 35 and hence, the results calculated by the ABCluster global search technique combined with the mPW2PLYP scheme should be credible.…”

Section: Theoretical Methodsmentioning

confidence: 97%

Structural Evolution, Electronic Structures, and Vibrational Properties of Anionic LuGe_n (n = 5–17) Clusters: From Lu-Linked to Lu-Encapsulated Configurations

et al. 2021

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The structural evolution pattern and electronic properties of Lu-doped germanium anion clusters, LuGe n − (n = 5− 17), have been investigated using a global search method combined with a double hybrid density functional theory and by comparing the theoretical PES spectra with the experimental ones. It is found that, for the structural growth patterns, a Lu-linked configuration is preferred for n = 10−14 in which the Lu atom as a linker connects two Ge subclusters and a Lu-encapsulated Ge cage-like motif is preferred for n = 15−17. The simulated PES spectra agree with experimental ones, revealing that the current global minimum structures are the true minima. The properties such as relative stability, charge transfer, highest-energy occupied molecular orbital−lowest-energy unoccupied molecular orbital (HOMO− LUMO) gap, IR, Raman, and ultraviolet−visible (UV−vis) spectra have been evaluated. The results of IR and Raman spectra could provide additional ways to experimentally identify the structure of these clusters. The results of stability, HOMO−LUMO gap, and UV−vis spectra could make the LuGe 16 − cluster the most suitable building block for further development as a potential optoelectronic material.

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Section: Theoretical Methodsmentioning

confidence: 97%

Structural Evolution, Electronic Structures, and Vibrational Properties of Anionic LuGe_n (n = 5–17) Clusters: From Lu-Linked to Lu-Encapsulated Configurations

et al. 2021

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“…The recently developed global optimizer NWPEsSe was used to explore the binding interactions of ILs on GO. 46 The resulting IL/GO membranes showed a substantial increase in the selectivity of cation rejection and enhanced the water flux. To better understand the improved separation performance of IL/GO membranes, a further study, involving zeta-potential measurements and a highly sensitive atomic force microscope, demonstrated a synergistic modification of the surface charge and hydrophobicity of the GO membranes due to the imidazolium cation that strongly repels other cations in solutions.…”

Section: ■ Introductionmentioning

confidence: 94%

Tuning the Charge and Hydrophobicity of Graphene Oxide Membranes by Functionalization with Ionic Liquids at Epoxide Sites

Tan

Zhang

Nguyen

et al. 2022

ACS Appl. Mater. Interfaces

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Functionalization of graphene oxide (GO) membranes is generally achieved using carboxyl groups as binding sites for ligands. Herein, by taking advantage of the ability of imidazolium-based ionic liquids (ILs) to undergo an epoxide ring-opening reaction, a new approach of GO modification was established, in which ILs were bonded to the abundant epoxides on GO without sacrificing the carboxyl groups. Computational methods confirmed this unique configuration of ILs on GO, which enabled the dispersion of IL/GO flakes in water for facile casting into laminate membranes. Compared with neat GO, the ILs in IL/GO membranes served as spacers that substantially reduced the multi-valent cation mobility, simultaneously facilitated ion desolvation, and increased the water flux across the membrane. Our studies found that the higher separation efficiency of IL/GO membranes may be attributed to the synergistic modification of the hydrophobicity and surface charge. Specifically, the protonated nitrogen of the imidazolium cations altered the surface charge of GO, thereby generating electrostatic repulsion that enhanced the selectivity of cation rejection. On the other hand, the increased length of the alkyl chains bound to the imidazolium rings was found to increase the hydrophobicity of GO, which, in turn, aided the fine-tuning of the water desolvation/transport dynamics at the GO/IL interface to achieve a high water flux. Additionally, the water retention was reduced on the hydrophobic planes, which inhibited GO swelling during aqueous separations. Molecular dynamics simulations revealed increased water diffusivity when ILs were intercalated within GO layers. We establish that without requiring a high energy input, functionalization of GO membranes with ILs may be a promising approach to achieve efficient ion separation and critical material recovery.

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“…230,231 This is more challenging in general than for the strongly adsorbed adsorbates discussed previously because liquid electrolytes adopt a continuously varying set of structures and are not limited to a few local minima in energy. Often, microsolvation approaches adopt specific prescriptions for creating solvent structures for consistency 232 but must be checked to ensure that an ensemble of such structures reproduce the bulk liquid environment correctly. For molecules in bulk solvent, quasi-chemical theory provides connections between microsolvation results and the thermodynamic ensemble average.…”

Section: Electrolyte Configurations and Solvationmentioning

confidence: 99%

Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

2022

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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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NWPEsSe: an Adaptive-Learning Global Optimization Algorithm for Nanosized Cluster Systems

Cited by 5 publications

References 31 publications

Structural Evolution, Electronic Structures, and Vibrational Properties of Anionic LuGe_n (n = 5–17) Clusters: From Lu-Linked to Lu-Encapsulated Configurations

Structural Evolution, Electronic Structures, and Vibrational Properties of Anionic LuGe_n (n = 5–17) Clusters: From Lu-Linked to Lu-Encapsulated Configurations

Tuning the Charge and Hydrophobicity of Graphene Oxide Membranes by Functionalization with Ionic Liquids at Epoxide Sites

Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

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NWPEsSe: an Adaptive-Learning Global Optimization Algorithm for Nanosized Cluster Systems

Cited by 5 publications

References 31 publications

Structural Evolution, Electronic Structures, and Vibrational Properties of Anionic LuGen (n = 5–17) Clusters: From Lu-Linked to Lu-Encapsulated Configurations

Structural Evolution, Electronic Structures, and Vibrational Properties of Anionic LuGen (n = 5–17) Clusters: From Lu-Linked to Lu-Encapsulated Configurations

Tuning the Charge and Hydrophobicity of Graphene Oxide Membranes by Functionalization with Ionic Liquids at Epoxide Sites

Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

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Product

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Structural Evolution, Electronic Structures, and Vibrational Properties of Anionic LuGe_n (n = 5–17) Clusters: From Lu-Linked to Lu-Encapsulated Configurations

Structural Evolution, Electronic Structures, and Vibrational Properties of Anionic LuGe_n (n = 5–17) Clusters: From Lu-Linked to Lu-Encapsulated Configurations