Theoretical Chemistry in Belgium: A Topical Collection from Theoretical Chemistry Accounts

277 Pages·2014·9.061 MB·English

by  Benoît Champagne, Michael S. Deleuze, Frank De Proft, Tom Leyssens (eds.)

Highlights in Theoretical Chemistry 6
Series Editors:
Christopher J. Cramer · Donald G. Truhlar
Benoît Champagne
Michael S. Deleuze
Frank De Proft
Editors
Tom Leyssens
Theoretical
Chemistry in
Belgium
A Topical Collection from Theoretical Chemistry Accounts
Highlights in Theoretical Chemistry
Vol. 6
Series Editors: Ch.J. Cramer • D.G. Truhlar

Forfurthervolumes:
http://www.springer.com/series/11166

Benoît Champagne • Michael S. Deleuze
Frank De Proft • Tom Leyssens
Volume Editors
Theoretical Chemistry
in Belgium
A Topical Collection from Theoretical Chemistry
Accounts
With contributions from

Jean-Marie André • Guillermo Avendaño-Franco • David Beljonne
Frank Blockhuys • Annemie Bogaerts • Jean-Luc Brédas • Patrick Bultinck
Thomas Carette • Emilie Cauët • Andrés Cedillo • Arnout Ceulemans
Benoît Champagne • Aurélie Chenel • Jérôme Cornil • Frank De Proft
Freija De Vleeschouwer • Dirk E. De Vos • Annelies Delabie
Michael S. Deleuze • Maxime Delsaut • Michèle Desouter-Lecomte
Georges Dive • Adri C. T. van Duin • Joseph G. Fripiat • Uma R. Fogueri
Patrick W. Fowler • Renuka Ganesan • Thomas Gathy • Paul Geerlings
Davy Geldof • Victor Geskin • An Ghysels • Michel Godefroid
Xavier Gonze • Myrta Grüning • Maxime Guillaume • Balázs Hajgató
Frank E. Harris • Pierre O. Hubin • Denis Jacquemin • Amir Karton
Sebastian Kozuch • Alisa Krishtal • Clément Lauzin • Laurence Leherte
Tom Leyssens • Jiguang Li • Vincent Liégeois • Jacques Liévin
Erwin Lijnen • Jérôme Loreau • Roger B. Mallion • Jan M. L. Martin
Christoph Meier • Filippo Morini • Fady Nahra • Cédric Nazé
Mamadou Ndong • Erik C. Neyts • Minh Tho Nguyen • Daniel Peeters
Quan Manh Phung • Kristine Pierloot • Bernard Piraux • Tomaz Pisanski
Geoffrey Pourtois • Françoise Remacle • Olivier Riant • Raphaël Robiette
John S. Sears • Gjergji Sini • Brian Sutcliffe • Truong Ba Tai
Nguyen Minh Tam • Nathalie S. Vaeck • Christian Van Alsenoy
Dimitri Van Neck • Tanguy Van Regemorter • Veronique Van Speybroeck
Steven Vancoillie • Matthias Vandichel • Monique A. van der Veen
Daniel P. Vercauteren • Simon Verdebout • Thomas Vergote
Toon Verstraelen • Stéphane Vranckx • Michel Waroquier • Giuseppe Zanti
Volume Editors
Benoît Champagne Michael S. Deleuze
Laboratory of Theoretical Chemisty Research Group of Theoretical Chemistry
Unit of Physical Chemistry and Molecular Modeling
Chemistry Department Hasselt University
University of Namur Diepenbeek, Belgium
Namur, Belgium
Tom Leyssens
Frank De Proft Laboratory of Crystal Engineering
Faculteit Wetenschappen Institute of Condensed Matter and Nanosciences
Eenheid Algemene Chemie (ALGC) Catholic University of Louvain
Free University of Brussels Louvain-La-Neuve, Belgium
Brussels, Belgium
Originally Published in Theor Chem Acc, Volume 131 (2012) and Volume 132 (2013)
© Springer-Verlag Berlin Heidelberg 2012, 2013
ISSN 2194-8666 ISSN 2194-8674 (electronic)
ISBN 978-3-642-41314-8 ISBN 978-3-642-41315-5 (eBook)
DOI 10.1007/978-3-642-41315-5
SpringerHeidelberg New York DordrechtLondon
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Contents
Preface ............................................................................................................................... 1
Benoît Champagne, Michael S. Deleuze, Frank De Proft, Tom Leyssens
Is there an exact potential energy surface? ...................................................................... 15
Brian Sutcliffe
Self-consistent methods constrained to a fixed number of particles in
a given fragment and its relation to the electronegativity equalization method ......... 27
Andrés Cedillo, Dimitri Van Neck, Patrick Bultinck
Host–guest and guest–guest interactions between xylene isomers
confined in the MIL-47(V) pore system. ......................................................................... 35
An Ghysels, Matthias Vandichel, Toon Verstraelen, Monique A. van der Veen,
Dirk E. De Vos, Michel Waroquier, Veronique Van Speybroeck
Laser control in open quantum systems: preliminary analysis toward
the Cope rearrangement control in methyl-cyclopentadienylcarboxylate dimer. ...... 49
G. Dive, R. Robiette, A. Chenel, M. Ndong, C. Meier, M. Desouter-Lecomte
Ruthenocene and cyclopentadienyl pyrrolyl ruthenium as precursors
for ruthenium atomic layer deposition: a comparative study of dissociation
enthalpies ........................................................................................................................... 61
Quan Manh Phung, Steven Vancoillie, Annelies Delabie, Geoffrey Pourtois,
Kristine Pierloot
The Boron conundrum: the case of cationic clusters (cid:1776)(cid:2878) with n = 2–20 ...................... 71
(cid:2196)
Truong Ba Tai, Nguyen Minh Tam, Minh Tho Nguyen
Quantum chemical study of self-doping PPV oligomers: spin distribution
of the radical forms. .......................................................................................................... 87
D. Geldof, A. Krishtal, F. Blockhuys, C. Van Alsenoy
Electron momentum spectroscopy of metal carbonyls: a reinvestigation
of the role of nuclear dynamics. ....................................................................................... 95
Balázs Hajgató, Filippo Morini, Michael S. Deleuze
Radical electrophilicities in solvent ................................................................................. 111
Freija De Vleeschouwer, Paul Geerlings, Frank De Proft
S graphs as model systems for icosahedral Jahn–Teller problems .......................... 125
5
A. Ceulemans, E. Lijnen, P. W. Fowler, R. B. Mallion, T. Pisanski
Mechanism of ketone hydrosilylation using NHC–Cu(I) catalysts:
a computational study. .................................................................................................... 135
Thomas Vergote, Thomas Gathy, Fady Nahra, Olivier Riant,
Daniel Peeters, Tom Leyssens
From atoms to biomolecules: a fruitful perspective .................................................... 149
E. Cauët, T. Carette, C. Lauzin, J. G. Li, J. Loreau, M. Delsaut,
C. Nazé, S. Verdebout, S. Vranckx, M. Godefroid, J. Liévin, N. Vaeck
v
vi Contents
Stabilization of merocyanine by protonation, charge, and external electric
fields and effects on the isomerization of spiropyran: a computational study.......... 167
Renuka Ganesan, F. Remacle
Ewald-type formulas for Gaussian-basis studies of one-dimensionally
periodic systems .............................................................................................................. 181
Joseph G. Fripiat, Frank E. Harris
Smoothed Gaussian molecular fields: an evaluation of molecular
alignment problems ........................................................................................................ 189
Laurence Leherte, Daniel P. Vercauteren
Ab initio quantum chemical and ReaxFF-based study of the intramolecular
iminium–enamine conversion in a proline-catalyzed reaction. .................................. 205
Pierre O. Hubin, Denis Jacquemin, Laurence Leherte, Jean-Marie André,
Adri C. T. van Duin, Daniel P. Vercauteren
Density functional theory for the description of charge-transfer processes
at TTF/TCNQ interfaces ................................................................................................ 217
Tanguy Van Regemorter, Maxime Guillaume, Gjergji Sini, John S. Sears,
Victor Geskin, Jean-Luc Brédas, David Beljonne, Jérôme Cornil
Implementation in the Pyvib2 program of the localized mode method
and application to a helicene. ......................................................................................... 225
Vincent Liégeois, Benoît Champagne
Time-dependent density functional theory study of charge transfer
in collisions. ...................................................................................................................... 241
Guillermo Avendaño-Franco, Bernard Piraux, Myrta Grüning,
Xavier Gonze
A simple DFT-based diagnostic for nondynamical correlation. ................................. 251
Uma R. Fogueri, Sebastian Kozuch, Amir Karton, Jan M. L. Martin
Electronic structure analysis of small gold clusters Au (m (cid:148) 16)
m
by density functional theory. .......................................................................................... 261
Giuseppe Zanti, Daniel Peeters
Combining molecular dynamics with Monte Carlo simulations:
implementations and applications. ................................................................................ 277
Erik C. Neyts, Annemie Bogaerts
TheorChemAcc(2013)132:1372
DOI10.1007/s00214-013-1372-6
EDITORIAL
Preface
Benoˆıt Champagne • Michael S. Deleuze •
Frank De Proft • Tom Leyssens
Publishedonline:19May2013
(cid:2)Springer-VerlagBerlinHeidelberg2013
In Belgium, theoretical chemistry began more than quickenborne at Katholieke Universiteit Leuven (KUL),
50 years ago, with an initial focus on quantum chemistry, and Piet van Leuven at Antwerpen (RUCA).
which gradually developed into a general interest in dif- Nowadays, Belgium counts around 200 theoretical
ferent domains of theoretical chemistry. In the Florile`ge chemists, spread over 10 universities (Fig. 1). This special
desSciences enBelgique [1], Louis d’Orcites asfounding issue includes contributions from the different theoretical
members of quantum chemistry in Belgium: Jean-Claude chemistry groups, illustrating the diversity and richness of
Lorquet at the Universite´ de Lie`ge, Georges Leroy at the the field whereas this Editorial is the occasion to sketch
Universite´ catholique de Louvain (UCL), Georges Ver- some aspects of the evolution of quantum chemistry and
haegen at Universite´ libre de Bruxelles (ULB), Luc Van- theoretical chemistry in our country.
Keyelementsinthedevelopmentsofthefieldhavealso
been the collaborations, the creation of working groups,
and the organization of conferences, of which the two-
yearly meeting Quantum Chemistry in Belgium, that was
thestimulusforpreparingthisspecial issue.Thefirstissue
Publishedaspartofthespecialcollectionofarticlescelebrating
theoreticalandcomputationalchemistryinBelgium. of the meeting took place in 1995 at the University of
Namur,andduringthelast17 years(1996inLeuven,1997
B.Champagne(&) inULB,1999inAntwerpen,2001inLie`ge,2003inGhent,
LaboratoryofTheoreticalChemistry,UnitofPhysical
2006inMons,2008inHasselt,2010inLouvain-la-Neuve,
Chemistry,ChemistryDepartment,UniversityofNamur,Ruede
Bruxelles,61,5000Namur,Belgium 2012inVUB),ithasbeenorganizedinalltheuniversities.
e-mail:[email protected] The second round will start in 2014 in Namur.
Progresses in theoretical chemistry have always been
M.S.Deleuze
associated with the development of computational resour-
ResearchGroupofTheoreticalChemistryandMolecular
Modeling,HasseltUniversity,AgoralaanGebouwD, ces, from more local architectures to the larger centers
3590Diepenbeek,Belgium recently installed in the two regions of the country, the
e-mail:[email protected]
Vlaams Supercomputer Center and the Consortium des
E´quipements de Calcul Intensif (CE´CI). Theoretical
F.DeProft
FaculteitWetenschappen,EenheidAlgemeneChemie(ALGC), chemistry in Belgium has over the years largely benefited
VrijeUniversiteitBrussel(VUB),Pleinlaan2,1050Brussels, fromfundingbyscientificagenciessuchastheFondsvoor
Belgium
Wetenschappelijk Onderzoek (FWO-Vlaanderen) and the
e-mail:[email protected]
Instituut voor Wetenschap en Technologie on the Flemish
T.Leyssens side, the Fonds de la Recherche Scientifique (F.R.S.–
LaboratoryofCrystalEngineering,InstituteofCondensed FNRS) and the Fonds de la Recherche pour la Formation
MatterandNanosciences,Universite´ CatholiquedeLouvain,
dans l’Industrie et dans l’Agriculture on the French
PlaceLouisPasteur1,bteL4.01.03,1348Louvain-La-Neuve,
speakingside,aswellastheBelgiumSciencePolicyOffice
Belgium
e-mail:[email protected] at the national level.
123
Reprinted from the journal 1
TheorChemAcc(2013)132:1372
Fig.1 MapofBelgium
representingthecitieswherethe
differentuniversitiesdiscussed
belowarelocated
1 University of Antwerp differencesinbondlengthsandvibrationalamplitudesfrom
abinitio(HF)gradientcalculationswereusedasconstraints
TheUniversitaireInstellingAntwerpen(UIA)wasfounded in the refinement of ED-experimental data. A code was
in 1971. On October 1, 2003, it became part of the Uni- thereby setup todo geometryrefinements, force field, and
versity of Antwerp (UA) which united RUCA (State Uni- vibrationalfrequencycalculations,alongwithnormal-mode
versity Centre Antwerp), UFSIA (University Faculties fitting. The second line of research involved the further
Saint Ignatius Antwerp) and UIA (University Institution development and implementation of the MIA into Pulay’s
Antwerp).Since the foundation oftheUIA,research using TEXASquantumchemicalpackage.Thiscode,afterfurther
quantum chemical methods has been performed in the refinement and optimization, evolved into the program
‘‘Structural Chemistry’’ group led by H.J. Geise working BRABO, a package which besides enabling SCF (HF and
on electron diffraction (ED) and by A.T.H. Lenstra work- DFT)calculationsinparallelalsocontainssoftwaretorelax
ing on X-ray diffraction. At that time, mainly semi- the molecular structure in geometry optimization, to con-
empirical calculations such as MINDO/3 were performed struct clusters based on fractional coordinates and space
to assist in the interpretation ofthe experimental data with group symmetry, to calculate and plot molecular density
these techniques. C. Van Alsenoy joined this group in (-difference) maps, and to partition molecular quantities
1978.Duringthisperiod,structuralchemistsbecameaware using the Hirshfeld approach.
of the enormous potential of P. Pulay’s force method in To date, the MIA approach can be applied routinely in
their research field. With this in mind, C. Van Alsenoy HF and DFT calculations as well as CPHF and CPKS
went to the USA for two postdoctoral stays, the first one calculations of polarizabilities and NMR chemical shifts.
with L. Scha¨fer at the University of Arkansas and the These developments were used in numerous studies,
second one with J. Boggs at the University of Texas (at among others for unraveling the structure of the crambin
Austin) where he worked under the guidance of P. Pulay peptide.Atthetime,thisachievementwasrecognizedbyI.
for a period of 6 months. During this period, the basis for Levine in his book ‘‘quantum chemistry’’ as the largest
the Multiplicative Integral Approximation (MIA) was ever performed quantum chemical calculation. Other
established, which later evolved into the Multiplicative studies involved cluster calculations in order to explain
Integral Approach. structural differences and vibrational frequency shifts in
When C. Van Alsenoy returned to the University of molecules between the gas-phase and the crystal-phase
Antwerp, research in the group of quantum chemistry was structures, depending on the space group. Another impor-
directedmainlyalongtwolines.Afirstpurposewastomake tant and more recent line of research in C. Van Alsenoy’s
the Molecular Orbital Constrained Electron Diffraction research group is devoted to the study and use of the
(MOCED) approach routinely available to people doing Hirshfeld approach for partitioning molecular properties
ElectronDiffractioninthegroup.IntheMOCEDapproach, suchastotalchargedistributions,molecularpolarizabilities
123
2 Reprinted from the journal
TheorChemAcc(2013)132:1372
as well as the total molecular energy into atomic contri- plasma formation) (in 2002). In 2001, A. Bogaerts was
butions,atvariouslevelsoftheory(HF,DFT,andMP2).A prize winner of the Royal Flemish Academy of Belgium
very promising extension along these lines of research is for Sciences and Arts. In 2003, she was appointed as a
the use of Hirshfeld partitioned quantities of multipole professor. After the retirement of R. Gijbels in 2004, the
polarizabilities in the study of dispersion effects comple- group was renamed as ‘‘PLASMANT’’.In 2011, E. Neyts,
menting DFT calculations. who made his PhD and postdoctoral work in the group on
In parallel to the work by C. van Alsenoy, research by molecular dynamics (MD) simulations for plasma deposi-
RenaatGijbelsandAnnemieBogaertsinAntwerpledover tionofcoatingsandcarbonnanotube growth,respectively,
the years to the foundation of an interdisciplinary research started in the group as a tenure track professor.
group ‘‘PLASMANT’’ (Plasma, Laser Ablation and Sur- Currently, the group consists of about 20 people (PhD
face Modeling—ANTwerp) where theoretical chemistry students and postdoctoral researchers; under the supervi-
alsoformsanimportant lineofresearch. R.Gijbelsstarted sion of A. Bogaerts and E. Neyts, and one technical-
his PhD work at Ghent University in 1961, in the research administrative coworker). As the name says, the group is
group of J. Hoste, which later evolved to the Institute of mainly performing computer modeling for (i) plasmas, (ii)
NuclearSciences.Histopicwasthedeterminationoftraces laserablation(laser–surfaceinteractions),and(iii)plasma–
of noble metals in other, high-purity noble metals, via surface interactions. The first two fields are under the
neutron activation analysis (NAA). After a few years, D. supervisionofA.Bogaerts,whereasthethirdtopicisunder
Desoete and R. Gijbels, together with J. Hoste, embarked the supervision of E. Neyts, especially the combination of
on the preparation of a monograph on Neutron Activation modeling both the plasma itself and its interaction with
Analysis. R. Gijbels took care of the more ‘‘fundamental’’ surfaces gives the group a unique expertise.
chapters and realized that NAA practitioners were not Theoretical chemistry activities in the University of
enough aware of a number of basic concepts, elastic and Antwerp are discussed in the papers by Geldolf et al. [2]
inelastic scatterings, excited states and metastable states, and by Neyts and Bogaerts [3] of the present issue.
among others. So, he started to study and to clarify these
concepts in the book. As a consequence, a number of PhD
works started in the group, for example, for the determi- 2 Free University of Brussels
nation of average cross-sections of so-called threshold
reactionsinducedbyfissionneutrons,byJ.P.Franc¸ois(see 2.1 Universite´ Libre de Bruxelles (ULB)
his contribution at the University of Hasselt).
R. Gijbels continued to follow this double track: theory Quantum chemical research at the Universite´ Libre de
anddifferentpracticalapplicationsbyNAAinavarietyof Bruxelles started in the mid-sixties. In 1965, Reginald
nuclear reactors. Modelingreceivedagainaboost with the Colin (RC) and Georges Verhaegen (GV) completed their
arrival of a postdoc from the Hungarian Academy of Sci- PhD theses in high-temperature chemistry in the Labora-
ences, A. Vertes who started a 1-D model for laser-solid tory of P. Goldfinger. The main characteristic of these
interaction. Another even more fruitful line of research studies was the discovery of numerous new molecules by
startedwiththearrival,in1986,ofJanM.L.Martinforhis massspectrometry.Itwastheurgetolearnmoreaboutthe
master thesis in Antwerp. R. Gijbels had seen a large structureofthesenewspeciesthatdeterminedthefieldsof
variety of carbon cluster ions in spark source and laser postdoctoral studies they both chose: RC went to the
induced mass spectra, and wondered what their structure HerzbergInstituteinOttawatoworkwithA.E.Douglasin
could be. J. Martin performed quantum chemical calcula- Molecular Spectroscopy; GV went to the ‘‘Centre de
tions to model these clusters, in close collaboration with Me´canique Ondulatoire Applique´e’’ (CMOA) of R. Dau-
J.-P. Franc¸ois, at the University of Hasselt. del in Paris to work with C. Moser in quantum chemistry.
In1993,A.BogaertsjoinedthegroupasaPhDstudent, The first publications of GV in this emerging field con-
and she developed a computer model for a glow discharge cerned the molecules BeO and MgO, both treated in his
plasma, used as an ion source for glow discharge mass thesis.
spectrometry. After finishing her PhD thesis in 1996, she Ab initio calculations have always demanded, and still
became an FWO postdoc in the group and started a sub- demand, the largest possible computing possibilities, both
grouponplasmamodeling,alsoforotherapplicationsthan interms ofspeed andcapacity. Back fromthe CMOA, the
analytical spectrometry (see below). This group was available computer in the ULB-VUB Center was then an
gradually growing, and new activities started, that is, on IBM 650, much too small to accomplish anything, but a
classical molecular dynamics simulations for plasma–sur- moderate LCAO-SCF calculation on very small atoms.
face interactions (in 2001) and on modeling for laser Therefore, after discussions with the FNRS, GV was able
ablation(i.e.,laser–solidinteraction,plumeexpansion,and to set up the then well-known SCF diatomic molecular
123
Reprinted from the journal 3