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	Author	Vermeiren, V.; Bogaerts, A.
	Title	Plasma-Based CO₂Conversion: To Quench or Not to Quench?			Type	A1 Journal article
	Year	2020	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	124	Issue	34	Pages	18401-18415
	Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
	Abstract	Plasma technology is gaining increasing interest for CO2 conversion. The gas temperature in (and after) the plasma reactor largely aﬀects the performance. Therefore, we examine the eﬀect of cooling/quenching, during and after the plasma, on the CO2 conversion and energy eﬃciency, for typical “warm” plasmas, by means of chemical kinetics modeling. For plasmas at low speciﬁc energy input (SEI ∼ 0.5 eV/molecule), it is best to quench at the plasma end, while for high-SEI plasmas (SEI ∼ 4 eV/molecule), quenching at maximum conversion is better. For low-SEI plasmas, quenching can even increase the conversion beyond the dissociation in the plasma, known as superideal quenching. To better understand the eﬀects of quenching at diﬀerent plasma conditions, we study the dissociation and recombination rates, as well as the vibrational distribution functions (VDFs) of CO2, CO, and O2. When a high vibrational−translational (VT) nonequilibrium exists at the moment of quenching, the dissociation and recombination reaction rates both increase. Depending on the conversion degree at the moment of quenching, this can lead to a net increase or decrease of CO2 conversion. In general, however, and certainly for equilibrium plasmas at high temperature, quenching after the plasma helps prevent recombination reactions and clearly enhances the ﬁnal CO2 conversion. We also investigate the eﬀect of diﬀerent quenching cooling rates on the CO2 conversion and energy eﬃciency. Finally, we compare plasma-based conversion to purely thermal conversion. For warm plasmas with typical temperatures of 3000−4000 K, the conversion is roughly thermal.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000566481000003	Publication Date	2020-08-27
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	3.7	Times cited		Open Access	OpenAccess
	Notes	Fonds Wetenschappelijk Onderzoek, G.0383.16N ; H2020 European Research Council, 810182 ; This research was supported by the FWO project (grant no. G.0383.16N) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement no. 810182SCOPE ERC Synergy project). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI), and the UAntwerpen.			Approved	Most recent IF: 3.7; 2020 IF: 4.536
	Call Number	PLASMANT @ plasmant @c:irua:172052			Serial	6407
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	Author	van ‘t Veer, K.; Engelmann, Y.; Reniers, F.; Bogaerts, A.
	Title	Plasma-Catalytic Ammonia Synthesis in a DBD Plasma: Role of Microdischarges and Their Afterglows			Type	A1 Journal article
	Year	2020	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	124	Issue	42	Pages	22871-22883
	Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT)
	Abstract	Plasma-catalytic ammonia synthesis is receiving ever increasing attention, especially in packed bed dielectric barrier discharge (DBD) reactors. The latter typically operate in the ﬁlamentary regime when used for gas conversion applications. While DBDs are in principle well understood and already applied in the industry, the incorporation of packing materials and catalytic surfaces considerably adds to the complexity of the plasma physics and chemistry governing the ammonia formation. We employ a plasma kinetics model to gain insights into the ammonia formation mechanisms, paying special attention to the role of ﬁlamentary microdischarges and their afterglows. During the microdischarges, the synthesized ammonia is actually decomposed, but the radicals created upon electron impact dissociation of N2 and H2 and the subsequent catalytic reactions cause a net ammonia gain in the afterglows of the microdischarges. Under our plasma conditions, electron impact dissociation of N2 in the gas phase followed by the adsorption of N atoms is identiﬁed as a rate-limiting step, instead of dissociative adsorption of N2 on the catalyst surface. Both elementary Eley−Rideal and Langmuir−Hinshelwood reaction steps can be found important in plasma-catalytic NH3 synthesis.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000585970300002	Publication Date	2020-10-22
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	3.7	Times cited		Open Access	OpenAccess
	Notes	Fonds Wetenschappelijk Onderzoek, 30505023 GoF9618n ; Fonds De La Recherche Scientifique – FNRS, 30505023 GoF9618n ; H2020 European Research Council, 810182 ;This research was supported by the Excellence of Science FWOFNRS project (FWO grant ID GoF9618n, EOS ID 30505023) and by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no 810182-SCOPE ERC Synergy project). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. The authors would also like to thank Järi Van den Hoek and Dr. Yury Gorbanev for providing the experimentally measured electrical characteristics and Dr. Fatme Jardali for creating the TOC graphics.			Approved	Most recent IF: 3.7; 2020 IF: 4.536
	Call Number	PLASMANT @ plasmant @c:irua:173587			Serial	6428
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	Author	Michiels, R.; Engelmann, Y.; Bogaerts, A.
	Title	Plasma Catalysis for CO₂Hydrogenation: Unlocking New Pathways toward CH₃OH			Type	A1 Journal article
	Year	2020	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	124	Issue	47	Pages	25859-25872
	Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT)
	Abstract	We developed a microkinetic model to reveal the eﬀects of plasma-generated radicals, intermediates, and vibrationally excited species on the catalytic hydrogenation of CO2 to CH3OH on a Cu(111) surface. As a benchmark, we ﬁrst present the mechanisms of thermal catalytic CH3OH formation. Our model predicts that the reverse water-gas shift reaction followed by CO hydrogenation, together with the formate path, mainly contribute to CH3OH formation in thermal catalysis. Adding plasma-generated radicals and intermediates results in a higher CH3OH turnover frequency (TOF) by six to seven orders of magnitude, showing the potential of plasma-catalytic CO2 hydrogenation into CH3OH, in accordance with the literature. In addition, CO2 vibrational excitation further increases the CH3OH TOF, but the eﬀect is limited due to relatively low vibrational temperatures under typical plasma catalysis conditions. The predicted increase in CH3OH formation by plasma catalysis is mainly attributed to the increased importance of the formate path. In addition, the conversion of plasma-generated CO to HCO* and subsequent HCOO* or H2CO* formation contribute to CH3OH formation. Both pathways bypass the HCOO* formation from CO2, which is the main bottleneck in the process. Hence, our model points toward the important role of CO, but also O, OH, and H radicals, as they inﬂuence the reactions that consume CO2 and CO. In addition, our model reveals that the H pressure should not be smaller than ca. half of the O pressure in the plasma as this would cause O* poisoning, which would result in very small product TOFs. Thus, plasma conditions should be targeted with a high CO and H content as this is favorable for CH3OH formation, while the O content should be minimized.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000595545800023	Publication Date	2020-11-25
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	3.7	Times cited		Open Access	Not_Open_Access: Available from 15.07.2021
	Notes	Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, 1114921N ; H2020 European Research Council, 810182 ; We acknowledge the ﬁnancial support from the Fund for Scientiﬁc Research (FWO-Vlaanderen; grant ID 1114921N) and from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 810182 − SCOPE ERC Synergy project) as well as from the DOC-PRO3 and the TOPBOF projects of the University of Antwerp.			Approved	Most recent IF: 3.7; 2020 IF: 4.536
	Call Number	PLASMANT @ plasmant @c:irua:173864			Serial	6443
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	Author	Loenders, B.; Engelmann, Y.; Bogaerts, A.
	Title	Plasma-Catalytic Partial Oxidation of Methane on Pt(111): A Microkinetic Study on the Role of Different Plasma Species			Type	A1 Journal article
	Year	2021	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	125	Issue	5	Pages	2966-2983
	Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT)
	Abstract	We use microkinetic modeling to examine the potential of plasma-catalytic partial oxidation (POX) of CH4 as a promising new approach to produce oxygenates. We study how diﬀerent plasma species aﬀect POX of CH4 on the Pt(111) surface, and we discuss the associated kinetic and mechanistic changes. We discuss the eﬀect of vibrationally excited CH4 and O2, as well as plasma-generated radicals and stable intermediates. Our results show that vibrational excitation enhances the turnover frequency (TOF) of catalytic CH4 dissociation and has good potential for improving the selectivities toward CH3OH, HCOOH, and C2 hydrocarbons. Nevertheless, when also considering plasma-generated radicals, we ﬁnd that these species mainly govern the surface chemistry. Additionally, we ﬁnd that plasma-generated radicals and stable intermediates enhance the TOFs of COx and oxygenates, increase the selectivity toward oxygenates, and make the formation of HCOOH more signiﬁcant on Pt(111). We also brieﬂy illustrate the potential impact of Eley−Rideal reactions that involve plasma-generated radicals. Finally, we reveal how various radicals aﬀect the catalyst surface chemistry and we link this to the formation of diﬀerent products. This allows us to make suggestions on how the plasma composition should be altered to improve the formation of desired products.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000619760700017	Publication Date	2021-02-11
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	4.536	Times cited		Open Access	OpenAccess
	Notes	Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, S001619N ; H2020 European Research Council, 810182 ; We thank Tom Butterworth for the interesting discussions regarding the calculation of the vibrational populations of methane and for taking the time to share his thoughts and experiences on the matter. This research is supported by the FWO-SBO project PLASMACATDesign (grant number S001619N). We also acknowledge ﬁnancial support from the TOP-BOF project of the University of Antwerp and from the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant agreement no. 810182SCOPE ERC Synergy project). The calculations were carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (Department EWI), and the University of Antwerp.			Approved	Most recent IF: 4.536
	Call Number	PLASMANT @ plasmant @c:irua:175873			Serial	6672
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	Author	Javdani, Z.; Hassani, N.; Faraji, F.; Zhou, R.; Sun, C.; Radha, B.; Neyts, E.; Peeters, F.M.; Neek-Amal, M.
	Title	Clogging and unclogging of hydrocarbon-contaminated nanochannels			Type	A1 Journal article
	Year	2022	Publication	The journal of physical chemistry letters	Abbreviated Journal	J Phys Chem Lett
	Volume	13	Issue	49	Pages	11454-11463
	Keywords	A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
	Abstract	The recent advantages of the fabrication of artificial nanochannels enabled new research on the molecular transport, permeance, and selectivity of various gases and molecules. However, the physisorption/chemisorption of the unwanted molecules (usually hydrocarbons) inside nanochannels results in the alteration of the functionality of the nanochannels. We investigated contamination due to hydrocarbon molecules, nanochannels made of graphene, hexagonal boron nitride, BC2N, and molybdenum disulfide using molecular dynamics simulations. We found that for a certain size of nanochannel (i.e., h = 0.7 nm), as a result of the anomalous hydrophilic nature of nanochannels made of graphene, the hydrocarbons are fully adsorbed in the nanochannel, giving rise to full uptake. An increasing temperature plays an important role in unclogging, while pressure does not have a significant role. The results of our pioneering work contribute to a better understanding and highlight the important factors in alleviating the contamination and unclogging of nanochannels, which are in good agreement with the results of recent experiments.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000893147700001	Publication Date	2022-12-05
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1948-7185	ISBN		Additional Links	UA library record; WoS full record
	Impact Factor	5.7	Times cited		Open Access	OpenAccess
	Notes				Approved	Most recent IF: 5.7
	Call Number	UA @ admin @ c:irua:192815			Serial	7263
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	Author	Canossa, S.; Ferrari, E.; Sippel, P.; Fischer, J.K.H.; Pfattner, R.; Frison, R.; Masino, M.; Mas-Torrent, M.; Lunkenheimer, P.; Rovira, C.; Girlando, A.
	Title	Tetramethylbenzidine-TetrafluoroTCNQ (TMB-TCNQF(4)) : a narrow-gap semiconducting salt with room-temperature relaxor ferroelectric behavior			Type	A1 Journal article
	Year	2021	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	125	Issue	46	Pages	25816-25824
	Keywords	A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
	Abstract	We present an extension and revision of the spectroscopic and structural data of the mixed-stack charge-transfer (CT) crystal 3,3 ',5,5 '-tetramethylbenzidine-tetrafluorotetracyano-quinodimethane (TMB-TCNQF4), associated with new electric and dielectric measurements. Refinement of synchrotron structural data at low temperature has led to revise the previously reported C2/m structure. The revised structure is P2(1)/m, with two dimerized stacks per unit cell, and is consistent with the low temperature vibrational data. However, polarized Raman data in the low-frequency region also indicate that by increasing temperature above 200 K, the structure presents an increasing degree of disorder, mainly along the stack axis. X-ray diffraction data at room temperature have confirmed that the correct structure is P2(1)/ m -no phase transitions -but did not allow substantiating the presence of disorder. On the other hand, dielectric measurements have evidenced a typical relaxor ferroelectric behavior already at room temperature, with a peak in the real part of dielectric constant epsilon'(T,v) around 200 K and 0.1 Hz. The relaxor behavior is explained in terms of the presence of spin solitons separating domains of opposite polarity that yield to ferroelectric nanodomains. TMB-TCNQF(4) is confirmed to be a narrow-gap band semiconductor (Ea similar to 0.3 eV) with a room-temperature conductivity of similar to 10(-4) Omega(-1) cm(-1).
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000731170500008	Publication Date	0000-00-00
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	4.536	Times cited		Open Access	Not_Open_Access
	Notes	A.G. thanks Prof. Pascale Foury-Leylekian for very helpful discussions about the crystallographic issues. R.F. thanks Prof. Anthony Linden for his help in the X-ray diffraction data collection. J.K.H.F. and P.L. acknowledge funding from the Deutsche Forschungsgemeinschaft (DFG) via the Transregional Collaborative Research Center TRR80 (Augsburg, Munich). R.P. and M.M.-T. acknowledge support from the Marie Curie Cofund, Beatriu de Pinós Fellowships (Grant nos. AGAUR 2017 BP 00064). This work was also supported by the Spanish Ministry project GENESIS PID2019-111682RBI00, the “Severo Ochoa” Programme for Centers of Excellence in R&D (FUNFUTURE, CEX2019-000917-S), and the Generalitat de Catalunya (2017-SGR-918). The Elettra Synchrotron (CNR Trieste) is acknowledged for granting the beamtime at the single-crystal diffraction beamline XRD1 (Proposal ID 20185483). In Parma, the work has benefited from the equipment and support of the COMP-HUB Initiative, funded by the “Departments of Excellence” program of the			Approved	Most recent IF: 4.536
	Call Number	UA @ admin @ c:irua:184866			Serial	7066
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	Author	Teunissen, J.L.; Braeckevelt, T.; Skvortsova, I.; Guo, J.; Pradhan, B.; Debroye, E.; Roeffaers, M.B.J.; Hofkens, J.; Van Aert, S.; Bals, S.; Rogge, S.M.J.; Van Speybroeck, V.
	Title	Additivity of Atomic Strain Fields as a Tool to Strain-Engineering Phase-Stabilized CsPbI₃Perovskites			Type	A1 Journal Article
	Year	2023	Publication	The Journal of Physical Chemistry C	Abbreviated Journal	J. Phys. Chem. C
	Volume	127	Issue	48	Pages	23400-23411
	Keywords	A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
	Abstract	CsPbI3 is a promising perovskite material for photovoltaic applications in its photoactive perovskite or black phase. However, the material degrades to a photovoltaically inactive or yellow phase at room temperature. Various mitigation strategies are currently being developed to increase the lifetime of the black phase, many of which rely on inducing strains in the material that hinder the black-to-yellow phase transition. Physical insight into how these strategies exactly induce strain as well as knowledge of the spatial extent over which these strains impact the material is crucial to optimize these approaches but is still lacking. Herein, we combine machine learning potential-based molecular dynamics simulations with our in silico strain engineering approach to accurately quantify strained large-scale atomic structures on a nanosecond time scale. To this end, we first model the strain fields introduced by atomic substitutions as they form the most elementary strain sources. We demonstrate that the magnitude of the induced strain fields decays exponentially with the distance from the strain source, following a decay rate that is largely independent of the specific substitution. Second, we show that the total strain field induced by multiple strain sources can be predicted to an excellent approximation by summing the strain fields of each individual source. Finally, through a case study, we illustrate how this additive character allows us to explain how complex strain fields, induced by spatially extended strain sources, can be predicted by adequately combining the strain fields caused by local strain sources. Hence, the strain additivity proposed here can be adopted to further our insight into the complex strain behavior in perovskites and to design strain from the atomic level onward to enhance their sought-after phase stability.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	001116862000001	Publication Date	2023-12-07
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447	ISBN		Additional Links	UA library record; WoS full record
	Impact Factor	3.7	Times cited		Open Access	OpenAccess
	Notes	This work was supported by iBOF-21-085 PERsist (Special Research Fund of Ghent University, KU Leuven Research Fund, and the Research Fund of the University of Antwerp). S.M.J.R., T.B., and B.P. acknowledge financial support from the Research Foundation-Flanders (FWO) through two postdoctoral fellow- ships [grant nos. 12T3522N (S.M.J.R.) and 1275521N (B.P.)] and an SB-FWO fellowship [grant no. 1SC1319 (T.B.)]. E.D., M.B.J.R., and J.H. acknowledge financial support from the Research Foundation-Flanders (FWO, grant nos. G.0B39.15, G.0B49.15, G098319N, S002019N, S004322N, and ZW15_09- GOH6316). J.H. acknowledges support from the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04) and the MPI as an MPI fellow. S.V.A. and S.B. acknowledge financial support from the Research Foundation-Flanders (FWO, grant no. G0A7723N). S.M.J.R. and V.V.S. acknowledge funding from the Research Board of Ghent University (BOF). The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation- Flanders (FWO) and the Flemish Government�department EWI.; KU Leuven, iBOF-21-085 PERsist ; Universiteit Antwerpen, iBOF-21-085 PERsist ; Universiteit Gent, iBOF-21-085 PERsist ; Vlaamse regering, CASAS2, Meth/15/04 ; Fonds Wetenschappelijk Onderzoek, G.0B39.15 G098319N G.0B49.15 1SC1319 12T3522N ZW15 09-GOH6316 G0A7723N 1275521N S004322N S002019N ;			Approved	Most recent IF: 3.7; 2023 IF: 4.536
	Call Number	EMAT @ emat @c:irua:202124			Serial	8985
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	Author	Delfino, C.L.; Hao, Y.; Martin, C.; Minoia, A.; Gopi, E.; Mali, K.S.; Van der Auweraer, M.; Geerts, Y.H.; Van Aert, S.; Lazzaroni, R.; De Feyter, S.
	Title	Conformation-Dependent Monolayer and Bilayer Structures of an Alkylated TTF Derivative Revealed using STM and Molecular Modeling			Type	A1 Journal Article
	Year	2023	Publication	The Journal of Physical Chemistry C	Abbreviated Journal	J. Phys. Chem. C
	Volume	127	Issue	47	Pages	23023-23033
	Keywords	A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
	Abstract	In this study, the multi-layer self-assembled molecular network formation of an alkylated tetrathiafulvalene compound is studied at the liquid-solid interface between 1-phenyloctane and graphite. A combined theoretical/experimental approach associating force-field and quantum-chemical calculations with scanning tunnelling microscopy is used to determine the two-dimensional self-assembly beyond the monolayer, but also to further the understanding of the molecular adsorption conformation and its impact on the molecular packing within the assemblies at the monolayer and bilayer level.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	001111637100001	Publication Date	2023-11-30
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447	ISBN		Additional Links	UA library record; WoS full record
	Impact Factor	3.7	Times cited		Open Access	OpenAccess
	Notes	Financial support from the Research Foundation-Flanders (FWO G081518N, G0A3220N) and KU Leuven–Internal Funds (C14/19/079) is acknowledged. This work was in part supported by FWO and F. R. S.-FNRS under the Excellence of Science EOS program (project 30489208 and 40007495). C.M. acknowledges the financial support: Grants PID2021-128761OA-C22 and CNS2022-136052 funded by MCIN/AEI/10.13039/501100011033 by the “European Union” and SBPLY/21/180501/000127 funded by JCCM and by the EU through “Fondo Europeo de Desarollo Regional” (FEDER). Research in Mons is also supported by the Belgian National Fund for Scientific Research (FRS-FNRS) within the Consortium des Équipements de Calcul Intensif – CÉCI, under Grant 2.5020.11, and by the Walloon Region (ZENOBE Tier-1 supercomputer, under grant 1117545).			Approved	Most recent IF: 3.7; 2023 IF: 4.536
	Call Number	EMAT @ emat @c:irua:201671			Serial	8974
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	Author	Gerrits, N.; Jackson, B.; Bogaerts, A.
	Title	Accurate Reaction Probabilities for Translational Energies on Both Sides of the Barrier of Dissociative Chemisorption on Metal Surfaces			Type	A1 Journal Article
	Year	2024	Publication	The Journal of Physical Chemistry Letters	Abbreviated Journal	J. Phys. Chem. Lett.
	Volume	15	Issue	9	Pages	2566-2572
	Keywords	A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
	Abstract	Molecular dynamics simulations are essential for a better understanding of dissociative chemisorption on metal surfaces, which is often the rate-controlling step in heterogeneous and plasma catalysis. The workhorse quasi-classical trajectory approach ubiquitous in molecular dynamics is able to accurately predict reactivity only for high translational and low vibrational energies. In contrast, catalytically relevant conditions generally involve low translational and elevated vibrational energies. Existing quantum dynamics approaches are intractable or approximate as a result of the large number of degrees of freedom present in molecule−metal surface reactions. Here, we extend a ring polymer molecular dynamics approach to fully include, for the first time, the degrees of freedom of a moving metal surface. With this approach, experimental sticking probabilities for the dissociative chemisorption of methane on Pt(111) are reproduced for a large range of translational and vibrational energies by including nuclear quantum effects and employing full-dimensional simulations.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	001177959900001	Publication Date	2024-03-07
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1948-7185	ISBN		Additional Links	UA library record; WoS full record
	Impact Factor	5.7	Times cited		Open Access
	Notes	Nick Gerrits has been financially supported through a Dutch Research Council (NWO) Rubicon grant (019.202EN.012). The computational resources and services used in this work were provided by the high performance computing (HPC) core facility CalcUA of the Universiteit Antwerpen and the Flemish Supercomputer Center (VSC) funded by the Research Foundation−Flanders (FWO) and the Flemish Government. The authors thank Mark Somers for useful discussions.			Approved	Most recent IF: 5.7; 2024 IF: 9.353
	Call Number	PLASMANT @ plasmant @c:irua:204818			Serial	9114
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	Author	Cai, Y.; Michiels, R.; De Luca, F.; Neyts, E.; Tu, X.; Bogaerts, A.; Gerrits, N.
	Title	Improving Molecule–Metal Surface Reaction Networks Using the Meta-Generalized Gradient Approximation: CO₂Hydrogenation			Type	A1 Journal Article
	Year	2024	Publication	The Journal of Physical Chemistry C	Abbreviated Journal	J. Phys. Chem. C
	Volume	128	Issue	21	Pages	8611-8620
	Keywords	A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
	Abstract	Density functional theory is widely used to gain insights into molecule−metal surface reaction networks, which is important for a better understanding of catalysis. However, it is well-known that generalized gradient approximation (GGA) density functionals (DFs), most often used for the study of reaction networks, struggle to correctly describe both gas-phase molecules and metal surfaces. Also, GGA DFs typically underestimate reaction barriers due to an underestimation of the selfinteraction energy. Screened hybrid GGA DFs have been shown to reduce this problem but are currently intractable for wide usage. In this work, we use a more affordable meta-GGA (mGGA) DF in combination with a nonlocal correlation DF for the first time to study and gain new insights into a catalytically important surface reaction network, namely, CO2 hydrogenation on Cu. We show that the mGGA DF used, namely, rMS-RPBEl-rVV10, outperforms typical GGA DFs by providing similar or better predictions for metals and molecules, as well as molecule−metal surface adsorption and activation energies. Hence, it is a better choice for constructing molecule−metal surface reaction networks.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos		Publication Date	2024-05-30
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447	ISBN		Additional Links
	Impact Factor	3.7	Times cited		Open Access
	Notes	H2020 Marie Sklodowska-Curie Actions, 813393 ; Fonds Wetenschappelijk Onderzoek, 1114921N ; H2020 European Research Council, 810182 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 019.202EN.012 ;			Approved	Most recent IF: 3.7; 2024 IF: 4.536
	Call Number	PLASMANT @ plasmant @			Serial	9248
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	Author	Borah, R.; Verbruggen, S.W.
	Title	Coupled plasmon modes in 2D gold nanoparticle clusters and their effect on local temperature control			Type	A1 Journal article
	Year	2019	Publication	The journal of physical chemistry: C : nanomaterials and interfaces	Abbreviated Journal	J Phys Chem C
	Volume	123	Issue	50	Pages	30594-30603
	Keywords	A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
	Abstract	Assemblies of closely separated gold nanoparticles exhibit a strong collective plasmonic response due to coupling of the plasmon modes of the individual nanostructures. In the context of self-assembly of nanoparticles, close-packed two-dimensional (2D) clusters of spherical nanoparticles present an important composite system that promises numerous applications. The present study probes the collective plasmonic characteristics and resulting photothermal behavior of close-packed 2D Au nanoparticle clusters to delineate the effects of the cluster size, interparticle distance, and particle size. Smaller nanoparticles (20 and 40 nm in diameter) that exhibit low individual scattering and high absorption were considered for their relevance to photothermal applications. In contrast to typical literature studies, the present study compares the optical response of clusters of different sizes ranging from a single nanoparticle up to large assemblies of 61 nanoparticles. Increasing the cluster size induces significant changes to the spectral position and optophysical characteristics. Based on the model outcome, an optimal cluster size for maximum absorption per nanoparticle is also determined for enhanced photothermal effects. The effect of the particle size and interparticle distance is investigated to elucidate the nature of interaction in terms of near-field and far-field coupling. The photothermal effect resulting from absorption is compared for different cluster sizes and interparticle distances considering a homogeneous water medium. A strong dependence of the steady-state temperature of the nanoparticles on the cluster size, particle position in the cluster, incident light polarization, and interparticle distance provides new physical insight into the local temperature control of plasmonic nanostructures.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000503919500061	Publication Date	2019-11-20
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	4.536	Times cited		Open Access
	Notes				Approved	Most recent IF: 4.536
	Call Number	UA @ admin @ c:irua:164530			Serial	5938
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	Author	Zhou, X.-G.; Yang, C.-Q.; Sang, X.; Li, W.; Wang, L.; Yin, Z.-W.; Han, J.-R.; Li, Y.; Ke, X.; Hu, Z.-Y.; Cheng, Y.-B.; Van Tendeloo, G.
	Title	Probing the electron beam-induced structural evolution of halide perovskite thin films by scanning transmission electron microscopy			Type	A1 Journal article
	Year	2021	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	125	Issue	19	Pages	10786-10794
	Keywords	A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
	Abstract	A deep understanding of the fine structure at the atomic scale of halide perovskite materials has been limited by their sensitivity to the electron beam that is widely used for structural characterization. The sensitivity of a gamma-CsPbIBr2 perovskite thin film under electron beam irradiation is revealed by scanning transmission electron microscopy (STEM) through a universal large-range electron dose measurement, which is based on discrete single-electron events in the STEM mode. Our research indicates that the gamma-CsPbIBr2 thin film undergoes structural changes with increasing electron overall dose (e(-).A(-2)) rather than dose rate (e(-).A(-2).s(-1)), which suggests that overall dose is the key operative parameter. The electron beam-induced structural evolution of gamma-CsPbIBr2 is monitored by fine control of the electron beam dose, together with the analysis of high-resolution (S)TEM, diffraction, and energy-dispersive X-ray spectroscopy. Our results show that the gamma-CsPbIBr2 phase first forms an intermediate phase [e.g., CsPb(1-x)(IBr)((3-y))] with a superstructure of ordered vacancies in the pristine unit cell, while a fraction of Pb2+ is reduced to Pb-0. As the electron dose increases, Pb nanoparticles precipitate, while the remaining framework forms the Cs2IBr phase, accompanied by some amorphization. This work provides guidelines to minimize electron beam irradiation artifacts for atomic-resolution imaging on CsPbIBr2 thin films.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000655640900061	Publication Date	2021-05-11
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	4.536	Times cited		Open Access	Not_Open_Access
	Notes				Approved	Most recent IF: 4.536
	Call Number	UA @ admin @ c:irua:179187			Serial	6880
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	Author	Bafekry, A.; Faraji, M.; Fadlallah, M.M.; Mortazavi, B.; Ziabari, A.A.; Khatibani, A.B.; Nguyen, C., V; Ghergherehchi, M.; Gogova, D.
	Title	Point defects in a two-dimensional ZnSnN₂ nanosheet : a first-principles study on the electronic and magnetic properties			Type	A1 Journal article
	Year	2021	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	125	Issue	23	Pages	13067-13075
	Keywords	A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
	Abstract	The reduction of dimensionality is a very effective way to achieve appealing properties in two-dimensional materials (2DMs). First-principles calculations can greatly facilitate the prediction of 2DM properties and find possible approaches to enhance their performance. We employed first-principles calculations to gain insight into the impact of different types of point defects (vacancies and substitutional dopants) on the electronic and magnetic properties of a ZnSnN2 (ZSN) monolayer. We show that Zn, Sn, and N + Zn vacancy-defected structures are p-type conducting, while the defected ZSN with a N vacancy is n-type conducting. For substitutional dopants, we found that all doped structures are thermally and energetically stable. The most stable structure is found to be B-doping at the Zn site. The highest work function value (5.0 eV) has been obtained for Be substitution at the Sn site. Li-doping (at the Zn site) and Be-doping (at the Sn site) are p-type conducting, while B-doping (at the Zn site) is n-type conducting. We found that the considered ZSN monolayer-based structures with point defects are magnetic, except those with the N vacancy defects and Be-doped structures. The ab initio molecular dynamics simulations confirm that all substitutionally doped and defected structures are thermally stable. Thus, our results highlight the possibility of tuning the magnetism in ZnSnN2 monolayers through defect engineering.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000664312500063	Publication Date	2021-06-03
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	4.536	Times cited		Open Access	Not_Open_Access
	Notes				Approved	Most recent IF: 4.536
	Call Number	UA @ admin @ c:irua:179741			Serial	7012
Permanent link to this record



	Author	Nematollahi, P.; Neyts, E.C.
	Title	Distribution pattern of metal atoms in bimetal-doped pyridinic-N₄ pores determines their potential for electrocatalytic N₂ reduction			Type	A1 Journal article
	Year	2022	Publication	Journal Of Physical Chemistry A	Abbreviated Journal	J Phys Chem A
	Volume	126	Issue	20	Pages	3080-3089
	Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
	Abstract	Doping two single transition-metal (TM) atoms on a substrate host opens numerous possibilities for catalyst design. However, what if the substrate contains more than one vacancy site? Then, the combination of two TMs along with their distribution patterns becomes a design parameter potentially complementary to the substrate itself and the bimetal composition. In this study, we investigate ammonia synthesis under mild electrocatalytic conditions on a transition-metal-doped porous C24N24 catalyst using density functional theory (DFT). The TMs studied include Ti, Mn, and Cu in a 2:4 dopant ratio (Ti2Mn4@C24N24 and Ti2Cu4@N-24(24)). Our computations show that a single Ti atom in both catalysts exhibits the highest selectivity for N-2 fixation at ambient conditions. This work is a good theoretical model to establish the structure-activity relationship, and the knowledge earned from the metal-N-4 moieties may help studies of related nanomaterials, especially those with curved structures.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000804119800003	Publication Date	2022-05-12
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1089-5639; 1520-5215	ISBN		Additional Links	UA library record; WoS full record
	Impact Factor	2.9	Times cited		Open Access	OpenAccess
	Notes				Approved	Most recent IF: 2.9
	Call Number	UA @ admin @ c:irua:189023			Serial	7146
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	Author	Nematollahi, P.; Neyts, E.C.
	Title	Identification of a unique pyridinic FeN₄C_x electrocatalyst for N₂ reduction : tailoring the coordination and carbon topologies			Type	A1 Journal article
	Year	2022	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	126	Issue	34	Pages	14460-14469
	Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
	Abstract	Although the heterogeneity of pyrolyzed Fe???N???C materials is known and has been reported previously, the atomic structure of the active sites and their detailed reaction mechanisms are still unknown. Here, we identified two pyridinic Fe???N4-like centers with different local C coordinates, i.e., FeN4C8 and FeN4C10, and studied their electrocatalytic activity for the nitrogen reduction reaction (NRR) based on density functional theory (DFT) calculations. We also discovered the influence of the adsorption of NH2 as a functional ligand on catalyst performance on the NRR. We confirmed that the NRR selectivity of the studied catalysts is essentially governed either by the local C coordination or by the dynamic structure associated with the FeII/FeIII. Our investigations indicate that the proposed traditional pyridinic FeN4C10 has higher catalytic activity and selectivity for the NRR than the robust FeN4C8 catalyst, while it may have outstanding activity for promoting other (electro)catalytic reactions. <comment>Superscript/Subscript Available</comment
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000859545200001	Publication Date	2022-08-17
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record
	Impact Factor	3.7	Times cited		Open Access	OpenAccess
	Notes				Approved	Most recent IF: 3.7
	Call Number	UA @ admin @ c:irua:191469			Serial	7268
Permanent link to this record



	Author	Gerrits, N.
	Title	Accurate simulations of the reaction of H₂ on a curved Pt crystal through machine learning			Type	A1 Journal article
	Year	2021	Publication	Journal Of Physical Chemistry Letters	Abbreviated Journal	J Phys Chem Lett
	Volume	12	Issue	51	Pages	12157-12164
	Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
	Abstract	Theoretical studies on molecule-metal surface reactions have so far been limited to small surface unit cells due to computational costs. Here, for the first time molecular dynamics simulations on very large surface unit cells at the level of density functional theory are performed, allowing a direct comparison to experiments performed on a curved crystal. Specifically, the reaction of D-2 on a curved Pt crystal is investigated with a neural network potential (NNP). The developed NNP is also accurate for surface unit cells considerably larger than those that have been included in the training data, allowing dynamical simulations on very large surface unit cells that otherwise would have been intractable. Important and complex aspects of the reaction mechanism are discovered such as diffusion and a shadow effect of the step. Furthermore, conclusions from simulations on smaller surface unit cells cannot always be transfered to larger surface unit cells, limiting the applicability of theoretical studies of smaller surface unit cells to heterogeneous catalysts with small defect densities.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000734045900001	Publication Date	2021-12-17
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1948-7185	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	9.353	Times cited		Open Access	OpenAccess
	Notes				Approved	Most recent IF: 9.353
	Call Number	UA @ admin @ c:irua:184717			Serial	7413
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	Author	Demiroglu, I.; Karaaslan, Y.; Kocabas, T.; Keceli, M.; Vazquez-Mayagoitia, A.; Sevik, C.
	Title	Computation of the thermal expansion coefficient of graphene with Gaussian approximation potentials			Type	A1 Journal article
	Year	2021	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	125	Issue	26	Pages	14409-14415
	Keywords	A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
	Abstract	Direct experimental measurement of thermal expansion coefficient without substrate effects is a challenging task for two-dimensional (2D) materials, and its accurate estimation with large-scale ab initio molecular dynamics is computationally very expensive. Machine learning-based interatomic potentials trained with ab initio data have been successfully used in molecular dynamics simulations to decrease the computational cost without compromising the accuracy. In this study, we investigated using Gaussian approximation potentials to reproduce the density functional theory-level accuracy for graphene within both lattice dynamical and molecular dynamical methods, and to extend their applicability to larger length and time scales. Two such potentials are considered, GAP17 and GAP20. GAP17, which was trained with pristine graphene structures, is found to give closer results to density functional theory calculations at different scales. Further vibrational and structural analyses verify that the same conclusions can be deduced with density functional theory level in terms of the reasoning of the thermal expansion behavior, and the negative thermal expansion behavior is associated with long-range out-of-plane phonon vibrations. Thus, it is argued that the enabled larger system sizes by machine learning potentials may even enhance the accuracy compared to small-size-limited ab initio molecular dynamics.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000672734100027	Publication Date	2021-06-24
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	4.536	Times cited		Open Access	OpenAccess
	Notes				Approved	Most recent IF: 4.536
	Call Number	UA @ admin @ c:irua:179850			Serial	7719
Permanent link to this record



	Author	Van de Sompel, P.; Khalilov, U.; Neyts, E.C.
	Title	Contrasting H-etching to OH-etching in plasma-assisted nucleation of carbon nanotubes			Type	A1 Journal article
	Year	2021	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	125	Issue	14	Pages	7849-7855
	Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
	Abstract	To gain full control over the growth of carbon nanotubes (CNTs) using plasma-enhanced chemical vapor deposition (PECVD), a thorough understanding of the underlying plasma-catalyst mechanisms is required. Oxygen-containing species are often used as or added to the growth precursor gas, but these species also yield various radicals and ions, which may simultaneously etch the CNT during the growth. At present, the effect of these reactive species on the growth onset has not yet been thoroughly investigated. We here report on the etching mechanism of incipient CNT structures from OH and O radicals as derived from combined (reactive) molecular dynamics (MD) and force-bias Monte Carlo (tfMC) simulations. Our results indicate that the oxygen-containing radicals initiate a dissociation process. In particular, we show how the oxygen species weaken the interaction between the CNT and the nanocluster. As a result of this weakened interaction, the CNT closes off and dissociates from the cluster in the form of a fullerene. Beyond the specific systems studied in this work, these results are generically important in the context of PECVD-based growth of CNTs using oxygen-containing precursors.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000641307100032	Publication Date	2021-04-06
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record
	Impact Factor	4.536	Times cited		Open Access	OpenAccess
	Notes				Approved	Most recent IF: 4.536
	Call Number	UA @ admin @ c:irua:178393			Serial	7729
Permanent link to this record



	Author	Kocabas, T.; Ozden, A.; Demiroglu, I.; Cakir, D.; Sevik, C.
	Title	Determination of Dynamically Stable Electrenes toward Ultrafast Charging Battery Applications			Type	A1 Journal article
	Year	2018	Publication	The journal of physical chemistry letters	Abbreviated Journal
	Volume	9	Issue	15	Pages	4267-4274
	Keywords	A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
	Abstract	Electrenes, an atomically thin form of layered electrides, are very recent members of the 2D materials family. In this work, we employed first principle calculations to determine stable, exfoliatable, and application-promising 2D electrene materials among possible M2X compounds, where M is a group II-A metal and X is a nonmetal element (C, N, P, As, and Sb). The promise of stable electrene compounds for battery applications is assessed via their exfoliation energy, adsorption properties, and migration energy barriers toward relevant Li, Na, K, and Ca atoms. Our calculations revealed five new stable electrene candidates in addition to previously known Ca2N and Sr2N. Among these seven dynamically stable electrenes, Ba2As, Ba2P, Ba2Sb, Ca2N, Sr2N, and Sr2P are found to be very promising for either K or Na ion batteries due to their extremely low migration energy barriers (5-16 meV), which roughly demonstrates 105 times higher mobility than graphene and two to four times higher mobility than other promising 2D materials such as MXene (Mo2C).
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000440956500020	Publication Date	2018-07-11
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1948-7185	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor		Times cited		Open Access
	Notes				Approved	no
	Call Number	UA @ admin @ c:irua:193765			Serial	7779
Permanent link to this record



	Author	Nematollahi, P.; Ma, H.; Schneider, W.F.; Neyts, E.C.
	Title	DFT and microkinetic comparison of ru-doped porphyrin-like graphene and nanotubes toward catalytic formic acid decomposition and formation			Type	A1 Journal article
	Year	2021	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	125	Issue	34	Pages	18673-18683
	Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
	Abstract	Immobilization of single metal atoms on a solid host opens numerous possibilities for catalyst designs. If that host is a two-dimensional sheet, sheet curvature becomes a design parameter potentially complementary to host and metal composition. Here, we use a combination of density functional theory calculations and microkinetic modeling to compare the mechanisms and kinetics of formic acid decomposition and formation, chosen for their relevance as a potential hydrogen storage medium, over single Ru atoms anchored to pyridinic nitrogen in a planar graphene flake (RuN4-G) and curved carbon nanotube (RuN4-CNT). Activation barriers are lowered and the predicted turnover frequencies are increased over RuN4-CNT relative to RuN4-CNT. The results highlight the potential of curvature control as a means to achieve high performance and robust catalysts.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000693413400013	Publication Date	2021-08-22
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	4.536	Times cited		Open Access	OpenAccess
	Notes				Approved	Most recent IF: 4.536
	Call Number	UA @ admin @ c:irua:181538			Serial	7805
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	Author	Gjerding, M.N.; Cavalcante, L.S.R.; Chaves, A.; Thygesen, K.S.
	Title	Efficient Ab initio modeling of dielectric screening in 2D van der Waals materials : including phonons, substrates, and doping			Type	A1 Journal article
	Year	2020	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	124	Issue	21	Pages	11609-11616
	Keywords	A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
	Abstract	The quantum electrostatic heterostructure (QEH) model allows for efficient computation of the dielectric screening properties of layered van der Waals (vdW)-bonded heterostructures in terms of the dielectric functions of the individual two-dimensional (2D) layers. Here, we extend the QEH model by including (1) contributions to the dielectric function from infrared active phonons in the 2D layers, (2) screening from homogeneous bulk substrates, and (3) intraband screening from free carriers in doped 2D semiconductor layers. We demonstrate the potential of the extended QEH model by calculating the dispersion of coupled phonons in multilayer stacks of hexagonal boron-nitride (hBN), the strong hybridization of plasmons and optical phonons in graphene/hBN heterostructures, the effect of substrate screening on the exciton series of monolayer MoS2, and the properties of hyperbolic plasmons in a doped phosphorene sheet. The new QEH code is distributed as a Python package with a simple command line interface and a comprehensive library of dielectric building blocks for the most common 2D materials, providing an efficient open platform for dielectric modeling of realistic vdW heterostructures.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000614615900022	Publication Date	2020-05-04
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	3.7	Times cited		Open Access
	Notes				Approved	Most recent IF: 3.7; 2020 IF: 4.536
	Call Number	UA @ admin @ c:irua:176187			Serial	7852
Permanent link to this record



	Author	Korkmaz, Y.A.; Bulutay, C.; Sevik, C.
	Title	k · p parametrization and linear and circular dichroism in strained monolayer (Janus) transition metal dichalcogenides from first-principles			Type	A1 Journal article
	Year	2021	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
	Volume	125	Issue	13	Pages	7439-7450
	Keywords	A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
	Abstract	Semiconductor monolayer transition metal dichalcogenides (TMDs) have brought a new paradigm by introducing optically addressable valley degree of freedom. Concomitantly, their high flexibility constitutes a unique platform that links optics to mechanics via valleytronics. With the intention to expedite the research in this direction, we investigated ten TMDs, namely MoS2, MoSe2, MoTe2, WS2, WSe2, WTe2, MoSSe, MoSeTe, WSSe, and WSeTe, which particularly includes their so-called janus types (JTMDs). First, we obtained their electronic band structures using regular and hybrid density functional theory (DFT) calculations in the presence of the spin-orbit coupling and biaxial or uniaxial strain. Our DFT results indicated that against the expectations based on their reported piezoelectric behavior, JTMDs typically interpolated between the standard band properties of the constituent TMDs without producing a novel feature. Next, by fitting to our DFT data we generated both spinless and spinful k center dot p parameter sets which are quite accurate over the K valley where the optical activity occurs. As an important application of this parametrization, we considered the circular and linear dichroism under strain. Among the studied (J)TMDs, WTe2 stood out with its largest linear dichroism under uniaxial strain because of its narrower band gap and large K valley uniaxial deformation potential. This led us to suggest WTe2 monolayer membranes for optical polarization-based strain measurements, or conversely, as strain tunable optical polarizers.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000639044400045	Publication Date	2021-03-26
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	4.536	Times cited		Open Access	OpenAccess
	Notes				Approved	Most recent IF: 4.536
	Call Number	UA @ admin @ c:irua:178264			Serial	8136
Permanent link to this record



	Author	Tchakoua, T.; Powell, A.D.; Gerrits, N.; Somers, M.F.; Doblhoff-Dier, K.; Busnengo, H.F.; Kroes, G.-J.
	Title	Simulating highly activated sticking of H₂ on Al(110) : quantum versus quasi-classical dynamics			Type	A1 Journal article
	Year	2023	Publication	The journal of physical chemistry: C : nanomaterials and interfaces	Abbreviated Journal
	Volume	127	Issue	11	Pages	5395-5407
	Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
	Abstract	We evaluate the importance of quantum effects on the sticking of H2 on Al(110) for conditions that are close to those of molecular beam experiments that have been done on this system. Calculations with the quasi-classical trajectory (QCT) method and with quantum dynamics (QD) are performed using a model in which only motion in the six molecular degrees of freedom is allowed. The potential energy surface used has a minimum barrier height close to the value recently obtained with the quantum Monte Carlo method. Monte Carlo averaging over the initial rovibrational states allowed the QD calculations to be done with an order of magnitude smaller computational expense. The sticking probability curve computed with QD is shifted to lower energies relative to the QCT curve by 0.21 to 0.05 kcal/mol, with the highest shift obtained for the lowest incidence energy. Quantum effects are therefore expected to play a small role in calculations that would evaluate the accuracy of electronic structure methods for determining the minimum barrier height to dissociative chemisorption for H2 + Al(110) on the basis of the standard procedure for comparing results of theory with molecular beam experiments.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000971346700001	Publication Date	2023-03-14
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1932-7447; 1932-7455	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	3.7	Times cited		Open Access	OpenAccess
	Notes				Approved	Most recent IF: 3.7; 2023 IF: 4.536
	Call Number	UA @ admin @ c:irua:196071			Serial	8525
Permanent link to this record



	Author	Mazzola, F.; Hassani, H.; Amoroso, D.; Chaluvadi, S.K.; Fujii, J.; Polewczyk, V.; Rajak, P.; Koegler, M.; Ciancio, R.; Partoens, B.; Rossi, G.; Vobornik, I.; Ghosez, P.; Orgiani, P.
	Title	Unveiling the electronic structure of pseudotetragonal WO₃ thin films			Type	A1 Journal article
	Year	2023	Publication	The journal of physical chemistry letters	Abbreviated Journal
	Volume	14	Issue	32	Pages	7208-7214
	Keywords	A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
	Abstract	WO3 isa 5d compound that undergoes severalstructuraltransitions in its bulk form. Its versatility is well-documented,with a wide range of applications, such as flexopiezoelectricity,electrochromism, gating-induced phase transitions, and its abilityto improve the performance of Li-based batteries. The synthesis ofWO(3) thin films holds promise in stabilizing electronicphases for practical applications. However, despite its potential,the electronic structure of this material remains experimentally unexplored.Furthermore, its thermal instability limits its use in certain technologicaldevices. Here, we employ tensile strain to stabilize WO3 thin films, which we call the pseudotetragonal phase, and investigateits electronic structure using a combination of photoelectron spectroscopyand density functional theory calculations. This study reveals theFermiology of the system, notably identifying significant energy splittingsbetween different orbital manifolds arising from atomic distortions.These splittings, along with the system's thermal stability,offer a potential avenue for controlling inter- and intraband scatteringfor electronic applications.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	001044522400001	Publication Date	2023-08-08
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1948-7185	ISBN		Additional Links	UA library record; WoS full record
	Impact Factor	5.7	Times cited		Open Access	OpenAccess
	Notes				Approved	Most recent IF: 5.7; 2023 IF: 9.353
	Call Number	UA @ admin @ c:irua:198391			Serial	8951
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