| Records |
| Author |
Hamid, I.; Jalali, H.; Peeters, F.M.; Neek-Amal, M. |
| Title |
Abnormal in-plane permittivity and ferroelectricity of confined water : from sub-nanometer channels to bulk |
Type |
A1 Journal article |
| Year |
2021 |
Publication |
Journal Of Chemical Physics |
Abbreviated Journal |
J Chem Phys |
| Volume |
154 |
Issue |
11 |
Pages |
114503 |
| Keywords |
A1 Journal article; Condensed Matter Theory (CMT) |
| Abstract |
Dielectric properties of nano-confined water are important in several areas of science, i.e., it is relevant in the dielectric double layer that exists in practically all heterogeneous fluid-based systems. Molecular dynamics simulations are used to predict the in-plane dielectric properties of confined water in planar channels of width ranging from sub-nanometer to bulk. Because of suppressed rotational degrees of freedom near the confining walls, the dipole of the water molecules tends to be aligned parallel to the walls, which results in a strongly enhanced in-plane dielectric constant (epsilon (parallel to)) reaching values of about 120 for channels with height 8 angstrom < h < 10 angstrom. With the increase in the width of the channel, we predict that epsilon (parallel to) decreases nonlinearly and reaches the bulk value for h > 70 angstrom. A stratified continuum model is proposed that reproduces the h > 10 angstrom dependence of epsilon (parallel to). For sub-nanometer height channels, abnormal behavior of epsilon (parallel to) is found with two orders of magnitude reduction of epsilon (parallel to) around h similar to 7.5 angstrom, which is attributed to the formation of a particular ice phase that exhibits long-time (similar to mu s) stable ferroelectricity. This is of particular importance for the understanding of the influence of confined water on the functioning of biological systems. |
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Place of Publication |
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Wos |
000629831900001 |
Publication Date |
2021-03-17 |
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Series Title |
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Abbreviated Series Title |
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| Series Volume |
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Series Issue |
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Edition |
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| ISSN |
0021-9606 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| Impact Factor |
2.965 |
Times cited |
9 |
Open Access |
OpenAccess |
| Notes |
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Approved |
Most recent IF: 2.965 |
| Call Number |
UA @ admin @ c:irua:177579 |
Serial |
6967 |
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| Author |
Bal, K.M.; Neyts, E.C. |
| Title |
Extending and validating bubble nucleation rate predictions in a Lennard-Jones fluid with enhanced sampling methods and transition state theory |
Type |
A1 Journal article |
| Year |
2022 |
Publication |
Journal Of Chemical Physics |
Abbreviated Journal |
J Chem Phys |
| Volume |
157 |
Issue |
18 |
Pages |
184113-10 |
| Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| Abstract |
We calculate bubble nucleation rates in a Lennard-Jones fluid through explicit molecular dynamics simulations. Our approach-based on a recent free energy method (dubbed reweighted Jarzynski sampling), transition state theory, and a simple recrossing correction-allows us to probe a fairly wide range of rates in several superheated and cavitation regimes in a consistent manner. Rate predictions from this approach bridge disparate independent literature studies on the same model system. As such, we find that rate predictions based on classical nucleation theory, direct brute force molecular dynamics simulations, and seeding are consistent with our approach and one another. Published rates derived from forward flux sampling simulations are, however, found to be outliers. This study serves two purposes: First, we validate the reliability of common modeling techniques and extrapolation approaches on a paradigmatic problem in materials science and chemical physics. Second, we further test our highly generic recipe for rate calculations, and establish its applicability to nucleation processes. |
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Wos |
000885260600002 |
Publication Date |
2022-11-14 |
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Series Title |
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Abbreviated Series Title |
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| Series Volume |
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Series Issue |
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Edition |
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| ISSN |
0021-9606 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| Impact Factor |
4.4 |
Times cited |
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Open Access |
OpenAccess |
| Notes |
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Approved |
Most recent IF: 4.4 |
| Call Number |
UA @ admin @ c:irua:192076 |
Serial |
7266 |
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| Author |
Bal, K.M. |
| Title |
Nucleation rates from small scale atomistic simulations and transition state theory |
Type |
A1 Journal article |
| Year |
2021 |
Publication |
Journal Of Chemical Physics |
Abbreviated Journal |
J Chem Phys |
| Volume |
155 |
Issue |
14 |
Pages |
144111 |
| Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| Abstract |
The evaluation of nucleation rates from molecular dynamics trajectories is hampered by the slow nucleation time scale and impact of finite size effects. Here, we show that accurate nucleation rates can be obtained in a very general fashion relying only on the free energy barrier, transition state theory, and a simple dynamical correction for diffusive recrossing. In this setup, the time scale problem is overcome by using enhanced sampling methods, in casu metadynamics, whereas the impact of finite size effects can be naturally circumvented by reconstructing the free energy surface from an appropriate ensemble. Approximations from classical nucleation theory are avoided. We demonstrate the accuracy of the approach by calculating macroscopic rates of droplet nucleation from argon vapor, spanning 16 orders of magnitude and in excellent agreement with literature results, all from simulations of very small (512 atom) systems. |
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Wos |
000755502100008 |
Publication Date |
2021-09-30 |
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Series Title |
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Abbreviated Series Title |
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| Series Volume |
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Series Issue |
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Edition |
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| ISSN |
0021-9606 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| Impact Factor |
2.965 |
Times cited |
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Open Access |
OpenAccess |
| Notes |
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Approved |
Most recent IF: 2.965 |
| Call Number |
UA @ admin @ c:irua:184937 |
Serial |
8320 |
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| Author |
Ramesha, B.M.; Pawlak, B.; Arenas Esteban, D.; Reekmans, G.; Bals, S.; Marchal, W.; Carleer, R.; Adriaensens, P.; Meynen, V. |
| Title |
Partial hydrolysis of diphosphonate ester during the formation of hybrid Tio₂ nanoparticles : role of acid concentration |
Type |
A1 Journal article |
| Year |
2023 |
Publication |
ChemPhysChem : a European journal of chemical physics and physical chemistry |
Abbreviated Journal |
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| Volume |
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Issue |
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Pages |
e202300437-13 |
| Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA) |
| Abstract |
In the present work, a method was utilized to control the in‐situ partial hydrolysis of a diphosphonate ester in presence of a titania precursor and in function of acid content and its impact on the hybrid nanoparticles was assessed. The hydrolysis degree of organodiphosphonate ester linkers during the formation of hybrid organic‐inorganic metal oxide nanoparticles, are relatively underexplored . Quantitative solution NMR spectroscopy revealed that during the synthesis of TiO2 nanoparticles, an increase in acid concentration introduces a higher degree of partial hydrolysis of the TEPD linker into diverse acid/ester derivatives of TEPD. Increasing the HCl/Ti ratio from 1 to 3, resulted in an increase in degree of partial hydrolysis of the TEPD linker in solution from 4% to 18.8% under the here applied conditions. As a result of the difference in partial hydrolysis, the linker‐TiO2 bonding was altered. Upon subsequent drying of the colloidal TiO2 solution, different textures, at nanoscale and macroscopic scale, were obtained dependent on the HCl/Ti ratio and thus the degree of hydrolysis of TEPD. Understanding such linker‐TiO2 nanoparticle surface dynamics is crucial for making hybrid organic‐inorganic materials (i.e. (porous) metal phosphonates) employed in applications such as electronic/photonic devices, separation technology and heterogeneous catalysts. |
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Wos |
001071673900001 |
Publication Date |
2023-09-05 |
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Series Title |
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Abbreviated Series Title |
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| Series Volume |
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Series Issue |
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Edition |
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| ISSN |
1439-4235; 1439-7641 |
ISBN |
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Additional Links |
UA library record; WoS full record |
| Impact Factor |
2.9 |
Times cited |
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Open Access |
OpenAccess |
| Notes |
This work was supported by the Research Foundation-Flanders (FWO Vlaanderen) Project G.0121.17 N. The work was further supported by Hasselt University and the Research Foundation – Flanders (FWO Vlaanderen) via the Hercules project AUHL/15/2 – GOH3816 N. V. M. acknowledges the Research Foundation Flanders (FWO) for project K801621 N. B. M. R. acknowledges, Prof. Dr. Christophe Detavernier and Dr. Davy Deduystche (COCOON, Ghent University) for PXRD and VT-XRD measurements, Prof. Dr. Christophe Van De Velde (iPRACS, University of Antwerp) and Dr. Radu Ciocarlan (LADCA, University of Antwerp) for helpful discussions on PXRD measurements and Dr. Nick Gys (University of Antwerp and VITO) for ICP-OES measurements. |
Approved |
Most recent IF: 2.9; 2023 IF: 3.075 |
| Call Number |
UA @ admin @ c:irua:198934 |
Serial |
8911 |
| Permanent link to this record |
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| Author |
Nikolaev, A.V.; Lamoen, D.; Partoens, B. |
| Title |
Extension of the basis set of linearized augmented plane wave (LAPW) method by using supplemented tight binding basis functions |
Type |
A1 Journal article |
| Year |
2016 |
Publication |
The journal of chemical physics |
Abbreviated Journal |
J Chem Phys |
| Volume |
145 |
Issue |
145 |
Pages |
014101 |
| Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) |
| Abstract |
In order to increase the accuracy of the linearized augmented plane wave (LAPW) method, we present a new approach where the plane wave basis function is augmented by two different atomic radial components constructed at two different linearization energies corresponding to two different electron bands (or energy windows). We demonstrate that this case can be reduced to the standard treatment within the LAPW paradigm where the usual basis set is enriched by the basis functions of the tight binding type, which go to zero with zero derivative at the sphere boundary. We show that the task is closely related with the problem of extended core states which is currently solved by applying the LAPW method with local orbitals (LAPW+LO). In comparison with LAPW+LO, the number of supplemented basis functions in our approach is doubled, which opens up a new channel for the extension of the LAPW and LAPW+LO basis sets. The appearance of new supplemented basis functions absent in the LAPW+LO treatment is closely related with the existence of the ul-component in the canonical LAPW method. We discuss properties of additional tight binding basis functions and apply the extended basis set for computation of electron energy bands of lanthanum (face and body centered structures) and hexagonal close packed lattice of cadmium. We demonstrate that the new treatment gives lower total energies in comparison with both canonical LAPW and LAPW+LO, with the energy difference more pronounced for intermediate and poor LAPW basis sets. |
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Place of Publication |
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Wos |
000379584700003 |
Publication Date |
2016-07-05 |
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Abbreviated Series Title |
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Series Issue |
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Edition |
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| ISSN |
0021-9606 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| Impact Factor |
2.965 |
Times cited |
11 |
Open Access |
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| Notes |
A.V.N. acknowledges useful discussions with B. Verberck, E. V. Tkalya, and A. V. Bibikov. |
Approved |
Most recent IF: 2.965 |
| Call Number |
c:irua:134290 |
Serial |
4099 |
| Permanent link to this record |
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| Author |
Bal, K.M.; Fukuhara, S.; Shibuta, Y.; Neyts, E.C. |
| Title |
Free energy barriers from biased molecular dynamics simulations |
Type |
A1 Journal article |
| Year |
2020 |
Publication |
Journal Of Chemical Physics |
Abbreviated Journal |
J Chem Phys |
| Volume |
153 |
Issue |
11 |
Pages |
114118 |
| Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| Abstract |
Atomistic simulation methods for the quantification of free energies are in wide use. These methods operate by sampling the probability density of a system along a small set of suitable collective variables (CVs), which is, in turn, expressed in the form of a free energy surface (FES). This definition of the FES can capture the relative stability of metastable states but not that of the transition state because the barrier height is not invariant to the choice of CVs. Free energy barriers therefore cannot be consistently computed from the FES. Here, we present a simple approach to calculate the gauge correction necessary to eliminate this inconsistency. Using our procedure, the standard FES as well as its gauge-corrected counterpart can be obtained by reweighing the same simulated trajectory at little additional cost. We apply the method to a number of systems—a particle solvated in a Lennard-Jones fluid, a Diels–Alder reaction, and crystallization of liquid sodium—to demonstrate its ability to produce consistent free energy barriers that correctly capture the kinetics of chemical or physical transformations, and discuss the additional demands it puts on the chosen CVs. Because the FES can be converged at relatively short (sub-ns) time scales, a free energy-based description of reaction kinetics is a particularly attractive option to study chemical processes at more expensive quantum mechanical levels of theory. |
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Place of Publication |
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Editor |
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Wos |
000574665600004 |
Publication Date |
2020-09-21 |
| Series Editor |
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Series Title |
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Abbreviated Series Title |
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| Series Volume |
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Series Issue |
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Edition |
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| ISSN |
0021-9606 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| Impact Factor |
4.4 |
Times cited |
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Open Access |
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| Notes |
Japan Society for the Promotion of Science, 19H02415 18J22727 ; Fonds Wetenschappelijk Onderzoek, 12ZI420N ; This work was supported, in part, by a Grant-in-Aid for Scientific Research (B) (Grant No. 19H02415) and Grant-in-Aid for a JSPS Research Fellow (Grant No. 18J22727) from the Japan Society for the Promotion of Science (JSPS), Japan. K.M.B. was funded as a junior postdoctoral fellow of the FWO (Research Foundation – Flanders), Grant No. 12ZI420N. S.F. was supported by JSPS through the Program for Leading Graduate Schools (MERIT). The computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the FWO and the Flemish Government. The authors are grateful to Pablo Piaggi for making the pair entropy CV code publicly available. |
Approved |
Most recent IF: 4.4; 2020 IF: 2.965 |
| Call Number |
PLASMANT @ plasmant @c:irua:172456 |
Serial |
6420 |
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| Author |
Payne, L.M.; Masia, F.; Zilli, A.; Albrecht, W.; Borri, P.; Langbein, W. |
| Title |
Quantitative morphometric analysis of single gold nanoparticles by optical extinction microscopy: Material permittivity and surface damping effects |
Type |
A1 Journal article |
| Year |
2021 |
Publication |
Journal Of Chemical Physics |
Abbreviated Journal |
J Chem Phys |
| Volume |
154 |
Issue |
4 |
Pages |
044702 |
| Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
| Abstract |
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Place of Publication |
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Editor |
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Wos |
000630495600001 |
Publication Date |
2021-01-28 |
| Series Editor |
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Series Title |
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Abbreviated Series Title |
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| Series Volume |
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Series Issue |
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Edition |
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| ISSN |
0021-9606 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| Impact Factor |
2.965 |
Times cited |
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Open Access |
OpenAccess |
| Notes |
This work was supported by the Welsh Government Life Sciences Bridging Fund (Grant No. LSBF/R6-005), the UK EPSRC (Grant Nos. EP/I005072/1 and EP/M028313/1), and the European Commission (Grant No. EUSMI E191000350). P.B. acknowledges the Royal Society for her Wolfson research merit award (Grant No. WM140077). F.M. acknowledges the Ser Cymru II programme (Case ID 80762-CU-148) which is part-funded by Cardiff University and the European Regional Development Fund through the Welsh Government. W.A. acknowledges an Individual Fellowship from the Marie Skłodowska-Curie actions (MSCA) under the EU’s Horizon 2020 program (Grant No. 797153, SOPMEN) and Sara Bals for supporting the STEM measurements. The brightfield TEM was performed by Thomas Davies at Cardiff University. We acknowledge Iestyn Pope for technical support of the optical equipment. |
Approved |
Most recent IF: 2.965 |
| Call Number |
EMAT @ emat @c:irua:177566 |
Serial |
6748 |
| Permanent link to this record |
