This work presents the first ab initio molecular dynamics study of trivalent lutetium in aqueous solution. The hybrid quantum and molecular mechanics simulation has been carried out on Hartree-Fock level and the results were compared to extended X-ray absorption fine structure and X-ray diffraction data. In addition to the structural characterisation via radial and angular distribution functions, the influence of the ion on the surrounding solvent was further investigated by local-density-corrected three-body distribution functions and frequency calculations. The obtained results for the mean Lu–O bond distance and force constant were in very good agreement with the literature. Furthermore, deeper insight into the dynamics and geometry of the solvation shell and the number of involved solvent molecules was obtained.
REFERENCES
1.
S.
Taylor
and S.
McClennan
, The Continental Crust: Its Composition and Evolution
(Blackwell Scientific Publications
, Oxford, UK
, 1985
).2.
J.
Emsley
, Nature's Building Blocks: An A–Z Guide to the Elements
(Oxford University Press
, 2001
).3.
Y.
Wei
and R.
Brainard
, Advanced Processes for 193-NM Immersion Lithography
(SPIE Press
, 2009
).4.
P.
Enghag
, Encyclopedia of the Elements: Technical Data - History - Processing - Applications
(Wiley
, 2008
).5.
F.
Daghighian
, P.
Shenderov
, K. S.
Pentlow
, M. C.
Graham
, B.
Eshagian
, C. L.
Melcher
, and J. S.
Schweitzer
, IEEE T. Nucl. Sci.
40
, 1045
(1993
).6.
Y.
Güzel
, M.
Rainer
, M.
Mirza
, and G.
Bonn
, Anal. Bioanal. Chem.
403
, 1323
(2012
).7.
M.
Mirza
, M.
Rainer
, Y.
Güzel
, and G.
Bonn
, Anal. Bioanal. Chem.
404
, 853
(2012
).8.
9.
M.
Gargaud
, M.
Hervé
, and P.
Claeys
, Lectures in Astrobiology
(Springer
, 2007
).10.
I.
Persson
, P.
D'Angelo
, S. D.
Panifilis
, M.
Sandström
, and L.
Eriksson
, Chem.-Eur. J.
14
, 3056
(2008
).11.
A.
Abbasi
, P.
Lindqvist-Reis
, L.
Eriksson
, D.
Sandstrm
, S.
Lidin
, and M.
Sandström
, Chem.-Eur. J.
11
, 4065
(2005
).12.
R.
Gerkin
and W.
Reppart
, Acta Crystallogr.
C40
, 781
(1984
).13.
A.
Chatterjee
, E.
Maslen
, and K.
Watson
, Acta Crystallogr.
B44
, 381
(1988
).14.
T.
Yamaguchi
, M.
Nomura
, H.
Wakita
, and H.
Ohtaki
, J. Chem. Phys.
89
, 5153
(1988
).15.
C.
Cossy
, A. C.
Barnes
, and J. E.
Enderby
, J. Chem. Phys.
90
, 3254
(1989
).16.
C.
Cossy
, L.
Helm
, D. H.
Powell
, and A. E.
Merbach
, New J. Chem.
19
, 27
(1995
).17.
T.
Timofte
, A.
Babai
, G.
Meyer
, and A. V.
Murdring
, Acta Crystallogr., Sect. E: Struct. Rep. Online
61
, i87
(2005
).18.
P. C.
Junk
, L. I.
Semenova
, B. W.
Skelton
, and A. H.
White
, Aust. J. Chem.
52
, 531
(1999
).19.
F. H.
Spedding
, M. J.
Pikal
, and B. O.
Ayers
, J. Phys. Chem.
70
, 2440
(1966
).20.
F. H.
Spedding
and K.
Jones
, J. Phys. Chem.
70
, 2450
(1966
).21.
F.
Spedding
and M.
Pikal
, J. Phys. Chem.
70
, 2430
(1966
).22.
S. I.
Ishiguro
, R.
Kato
, R.
Takahashi
, and S.
Nakasone
, Rare Earth Mod. Sci. Technol.
27
, 61
(1995
).23.
M. E.
Tuckerman
, Statistical Mechanics: Theory and Molecular Simulation
(Oxford University Press
, New York
, 2010
).24.
25.
T. S.
Hofer
, B. M.
Rode
, A. B.
Pribil
, and B. R.
Randolf
, Adv. Inorg. Chem.
62
, 143
(2010
).26.
B.
Rode
, T.
Hofer
, B.
Randolf
, C.
Schwenk
, D.
Xenides
, and V.
Vchirawongkwin
, Theor. Chem. Acc.
115
, 77
(2006
).27.
T.
Hofer
and B. M.
Rode
, Pure Appl. Chem.
78
, 525
(2006
).28.
A. K. H.
Weiss
and T. S.
Hofer
, RSC Adv.
3
, 1606
–1635
(2013
).29.
T.
Hofer
, A.
Weiss
, B.
Randolf
, and B.
Rode
, Chem. Phys. Lett.
512
, 139
(2011
).30.
O.
Lutz
, T.
Hofer
, B.
Randolf
, and B.
Rode
, Chem. Phys. Lett.
539–540
, 50
(2012
).31.
O.
Lutz
, T.
Hofer
, B.
Randolf
, and B.
Rode
, Chem. Phys. Lett.
536
, 50
(2012
).32.
T. S.
Hofer
, H.
Scharnagl
, B. R.
Randolf
, and B. M.
Rode
, Chem. Phys.
327
, 31
(2006
).33.
T. S.
Hofer
, B.
Randolf
, and B. M.
Rode
, Phys. Chem. Chem. Phys.
7
, 1382
(2005
).34.
T. S.
Hofer
, B.
Randolf
, and B. M.
Rode
, J. Phys. Chem. B
112
, 11726
(2008
).35.
R.
Frick
, A. B.
Pribil
, T. S.
Hofer
, B. R.
Randolf
, A.
Bhattacharjee
, and B. R.
Rode
, Inorg. Chem.
48
, 3993
(2009
).36.
C. B.
Messner
, T. S.
Hofer
, B.
Randolf
, and B. M.
Rode
, Phys. Chem. Chem. Phys.
13
, 224
(2011
).37.
O.
Lutz
, T.
Hofer
, B.
Randolf
, A.
Weiss
, and B.
Rode
, Inorg. Chem.
51
, 6746
(2012
).38.
D.
Bakowies
and W.
Thiel
, J. Phys. Chem.
100
, 10580
(1996
).39.
P.
Bash
, J.
Field
, and M.
Karplus
, J. Am. Chem. Soc.
109
, 8092
(1987
).40.
M. P.
Allen
and D. J.
Tildesley
, Computer Simulation of Liquids
(Oxford Science Publications
, Oxford
, 1990
).41.
M. J.
Frisch
, G. W.
Trucks
, H. B.
Schlegel
et al, GAUSSIAN 09, Revision A.1, Gaussian, Inc., Wallingford, CT, 2009
.42.
X.
Cao
and M.
Dolg
, J. Chem. Phys.
115
, 7348
(2001
).43.
44.
H.
Berendsen
, J.
Postma
, and W.
van Gunsteren
, J. Phys. Chem.
81
, 3684
(1984
).45.
D.
Adams
, E.
Adams
, and G.
Hills
, Mol. Phys.
38
, 387
(1979
).46.
47.
P.
Bopp
, G.
Jancs
, and K.
Heinzinger
, Chem. Phys. Lett.
98
, 129
(1983
).48.
F.
Stillinger
and A.
Rahman
, J. Chem. Phys.
68
, 666
(1978
).49.
G.
Jancs
, P.
Bopp
and K.
Heinzinger
, Chem. Phys.
85
, 377
(1984
).50.
TURBOMOLE V6.2 2010, a development of University of Karlsruhe and Forschungszentrum Karlsruhe GmbH, 1989-2007, TURBOMOLE GmbH, since 2007; see http://www.turbomole.com.
51.
D.
Feller
, J. Comput. Chem.
17
, 1571
(1996
).52.
A.
Bhattacharjee
, T.
Hofer
, and B.
Rode
, Phys. Chem. Chem. Phys.
10
, 6653
(2008
).53.
T.
Moin
, T.
Hofer
, A.
Pribil
, and B.
Rode
, Inorg. Chem.
49
, 5101
(2010
).54.
F. M.
Floris
and A.
Tani
, J. Chem. Phys.
115
, 4750
(2001
).55.
Th.
Kowall
, F.
Foglia
, L.
Helm
, and A. E.
Merbach
, J. Phys. Chem.
99
, 13078
(1995
).56.
D.
Xenides
, B.
Randolf
, and B.
Rode
, J. Chem. Phys.
122
, 174506
(2005
).57.
H.
Kanno
and J.
Hiraishi
, Chem. Phys. Lett.
151
, 315
(1988
).© 2013 AIP Publishing LLC.
2013
AIP Publishing LLC
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