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@ARTICLE{Baric:51224,
author = {Baric, D. and Kovacevic, B. and Maksic, Z. B. and Müller,
T.},
title = {{A} {N}ovel {A}pproach in {A}nalyzing {A}romaticity by
{H}omo- and {I}sostructural {R}eactions: {A}n ab {I}nitio
{S}tudy of {F}luorobenzenes},
journal = {The journal of physical chemistry / A},
volume = {109},
issn = {1089-5639},
address = {Washington, DC},
publisher = {Soc.},
reportid = {PreJuSER-51224},
pages = {10594},
year = {2005},
note = {Record converted from VDB: 12.11.2012},
abstract = {The influence of fluorine substitutions on the stability of
benzene is examined by using the Hartree-Fock (HF) and MP2
models. It is conclusively demonstrated that homodesmotic
reactions based on the open-chain zigzag polyenes are
unsatisfactory. A comparison of the intramolecular
interactions of educts and products shows that they are not
well balanced. Hence, these reactions should be abandoned in
discussing aromaticity. A much better vehicle for exploring
aromaticity is provided by homostructural reactions, which
employ cyclic monoene and diene as reference model
compounds. Their heavy atoms are enforced to assume planar
geometries to enable sigma/pi separation. The HF/cc-pVTZ
calculations show that extrinsic aromaticity of benzene B
DeltaE(ease)(B)() arises both from the sigma- and
pi-contributions. They are -14.8 and -23.1 in kcal/mol,
respectively, if the stockholder energy partitioning scheme
is employed. This result implies that both the sigma- and
pi-frameworks contribute to the aromatic stabilization of B,
the latter being more important. The total aromatic
stabilization DeltaE(ease)(B)() is -37.9 kcal/mol.
Schleyer's indene-isoindene isomerization approach also
strongly indicates that the decisive factor in determining
the aromatic stability of the benzene moiety is the
pi-electron framework. The origin of extrinsic aromaticity
is identified as the increased nuclear-electron attraction
of both sigma- and pi-electrons, if 1,3-cyclohexadiene is
used as a gauge compound. Further, by using a system of
isostructural reactions, it is conclusively demonstrated
that fluorobenzenes exhibit a remarkable additivity of the
substituent effects, as far as the stability of multiply
substituted benzenes is concerned. This additivity rule is
so accurate that it enables delineation of the fluorine
repulsions and the aromaticity defect DeltaE(AD). It appears
that the DeltaE(AD) values increase upon sequential fluorine
substitution at the next nearest (vicinal) position thus
making multiply fluorinated benzenes less stable.},
keywords = {Butadienes: chemistry / Chemistry, Physical / Ethylenes:
chemistry / Fluorobenzenes: chemistry / Hydrocarbons,
Aromatic: chemistry / Hydrocarbons, Cyclic: chemistry /
Hydrocarbons, Fluorinated: chemistry / Models, Chemical /
Molecular Structure / Physicochemical Phenomena / Butadienes
(NLM Chemicals) / Ethylenes (NLM Chemicals) / Fluorobenzenes
(NLM Chemicals) / Hydrocarbons, Aromatic (NLM Chemicals) /
Hydrocarbons, Cyclic (NLM Chemicals) / Hydrocarbons,
Fluorinated (NLM Chemicals) / 1,3-butadiene (NLM Chemicals)
/ ethylene (NLM Chemicals) / J (WoSType)},
cin = {ZAM},
ddc = {530},
cid = {I:(DE-Juel1)VDB62},
pnm = {Betrieb und Weiterentwicklung des Höchstleistungsrechners},
pid = {G:(DE-Juel1)FUEK254},
shelfmark = {Chemistry, Physical / Physics, Atomic, Molecular $\&$
Chemical},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:16834316},
UT = {WOS:000233436900016},
doi = {10.1021/jp0532871},
url = {https://juser.fz-juelich.de/record/51224},
}