We have developed a model to calculate accurately the intensity of the hydrogen bonded XH-stretching vibrational transition in hydrogen bonded complexes. In the Local Mode Perturbation Theory (LMPT) model, the unperturbed system is described by a local mode (LM) model, which is perturbed by the intermolecular modes of the hydrogen bonded system that couple with the intramolecular vibrations of the donor unit through the potential energy surface. We have applied the model to three complexes containing water as the donor unit and different acceptor units, providing a series of increasing complex binding energy: H2O⋯N2, H2O⋯H2O, and H2O⋯NH3. Results obtained by the LMPT model are presented and compared with calculated results obtained by other vibrational models and with previous results from gas-phase and helium-droplet experiments. We find that the LMPT model reduces the oscillator strengths of the fundamental hydrogen bonded OH-stretching transition relative to the simpler LM model.
REFERENCES
1.
K.
Pfeilsticker
, F.
Erle
, and U.
Platt
, J. Atmos. Sci.
54
, 933
–939
(1997
).2.
A. A.
Vigasin
, Molecular Complexes in Earth’s Planetary, Cometary and Interstellar Atmospheres
(World Scientific
, River Edge, NJ
, 1998
).3.
S.
Aloisio
and J. S.
Francisco
, Acc. Chem. Res.
33
, 825
(2000
).4.
V.
Vaida
, H. G.
Kjaergaard
, and K. J.
Feierabend
, Int. Rev. Phys. Chem.
22
, 203
(2003
).5.
P. G.
Sennikov
, S. K.
Ignatov
, and O.
Schrems
, ChemPhysChem
6
, 392
(2005
).6.
V.
Vaida
, J. S.
Daniel
, H. G.
Kjaergaard
, L. M.
Goss
, and A. F.
Tuck
, Q. J. R. Meteorol. Soc.
127
, 1627
(2001
).7.
H. G.
Kjaergaard
, T. W.
Robinson
, D. L.
Howard
, J. S.
Daniel
, J. E.
Headrick
, and V.
Vaida
, J. Phys. Chem. A
107
, 10680
(2003
).8.
J. S.
Daniel
, S.
Solomon
, H. G.
Kjaergaard
, and D. P.
Schofield
, Geophys. Res. Lett.
31
, L06118
(2004
).9.
M.
Kanakidou
et al., Atmos. Chem. Phys.
5
, 1053
(2005
).10.
J.
Almeida
et al., Nature
502
, 359
–363
(2013
).11.
S.
Solomon
, D.
Qin
, M.
Manning
, Z.
Chen
, M.
Marquis
, K.
Averyt
, M.
Tignor
, and H.
Miller
, Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change
(Cambridge University Press
, Cambridge, United Kingdom, and New York, NY, USA
, 2007
).12.
P.
Atkins
, J.
de Paula
, and R.
Friedman
, Quanta, Matter, and Change: A Molecular Approach to Physical Chemistry
, 1st ed. (Oxford University Press
, 2009
).13.
Y.
Scribano
, N.
Goldman
, R. J.
Saykally
, and C.
Leforestier
, J. Phys. Chem. A
110
, 5411
(2006
).14.
S.
Chung
and M.
Hippler
, J. Chem. Phys.
124
, 214316
(2006
).15.
M.
Hippler
, J. Chem. Phys.
127
, 084306
(2007
).16.
L.
Du
, J. R.
Lane
, and H. G.
Kjaergaard
, J. Chem. Phys.
136
, 184305
(2012
).17.
L.
Du
, K.
Mackeprang
, and H. G.
Kjaergaard
, Phys. Chem. Chem. Phys.
15
, 10194
(2013
).18.
N.
Bork
, L.
Du
, and H. G.
Kjaergaard
, J. Phys. Chem. A
118
, 1384
(2014
).19.
N.
Bork
, L.
Du
, H.
Reiman
, T.
Kurtèn
, and H. G.
Kjaergaard
, J. Phys. Chem. A
118
, 5316
(2014
).20.
A. S.
Hansen
, L.
Du
, and H. G.
Kjaergaard
, J. Phys. Chem. Lett.
5
, 4225
(2014
).21.
A. S.
Hansen
, L.
Du
, and H. G.
Kjaergaard
, Phys. Chem. Chem. Phys.
16
, 22882
(2014
).22.
C. L.
Andersen
, C. S.
Jensen
, K.
Mackeprang
, L.
Du
, S.
Jørgensen
, and H. G.
Kjaergaard
, J. Phys. Chem. A
118
, 11074
(2014
).23.
P.
Atkins
and R.
Friedman
, Molecular Quantum Mechanics
, 4th ed. (Oxford University Press
, 2008
).24.
J. R.
Lane
and H. G.
Kjaergaard
, J. Chem. Phys.
132
, 174304
(2010
).25.
B. J.
Miller
, L.
Du
, T. J.
Steel
, A. J.
Paul
, A. H.
Södergren
, J. R.
Lane
, B. R.
Henry
, and H. G.
Kjaergaard
, J. Phys. Chem. A
116
, 290
(2012
).26.
Y.
Wang
, S.
Carter
, B. J.
Braams
, and J. M.
Bowman
, J. Chem. Phys.
128
, 071101
(2008
).27.
E.
Sälli
, T.
Salmi
, and L.
Halonen
, J. Phys. Chem. A
115
, 11594
(2011
).28.
K.
Mackeprang
, H. G.
Kjaergaard
, T.
Salmi
, V.
Hänninen
, and L.
Halonen
, J. Chem. Phys.
140
, 184309
(2014
).29.
H. G.
Kjaergaard
, A. L.
Garden
, G. M.
Chaban
, R. B.
Gerber
, D. A.
Matthews
, and J. F.
Stanton
, J. Phys. Chem. A
112
, 4324
(2008
).30.
J.
Vazquez
and J. F.
Stanton
, Mol. Phys.
104
, 377
(2006
).31.
H. G.
Kjaergaard
, B. R.
Henry
, H.
Wei
, S.
Lefebvre
, T.
Carrington
, Jr.
, O. S.
Mortensen
, and M. L.
Sage
, J. Chem. Phys.
100
, 6228
(1994
).32.
K.
Raghavachari
, G. W.
Trucks
, J. A.
Pople
, and M.
Head-Gordon
, Chem. Phys. Lett.
157
, 479
(1989
).33.
R. J.
Bartlett
, J.
Watts
, S.
Kucharski
, and J.
Noga
, Chem. Phys. Lett.
165
, 513
(1990
).34.
T. H.
Dunning
, J. Chem. Phys.
90
, 1007
(1989
).35.
K.
Kuyanov-Prozument
, M. Y.
Choi
, and A. F.
Vilesov
, J. Chem. Phys.
132
, 014304
(2010
).36.
T.
Salmi
, V.
Hänninen
, A. L.
Garden
, H. G.
Kjaergaard
, J.
Tennyson
, and L.
Halonen
, J. Phys. Chem. A
112
, 6305
(2008
).37.
H.-J.
Werner
et al., molpro, version 2010.1, a package of ab initioprograms, 2010, see http://www.molpro.net.38.
H.-J.
Werner
et al., molpro, version 2012.1, a package of ab initioprograms, 2012, see http://www.molpro.net.39.
T. B.
Adler
, G.
Knizia
, and H.-J.
Werner
, J. Chem. Phys.
127
, 221106
(2007
).40.
G.
Knizia
, T. B.
Adler
, and H.-J.
Werner
, J. Chem. Phys.
130
, 054104
(2009
).41.
H.-J.
Werner
, G.
Knizia
, and F. R.
Manby
, Mol. Phys.
109
, 407
(2011
).42.
K. A.
Peterson
, T. B.
Adler
, and H.-J.
Werner
, J. Chem. Phys.
128
, 084102
(2008
).43.
B. J.
Miller
, J. R.
Lane
, and H. G.
Kjaergaard
, Phys. Chem. Chem. Phys.
13
, 14183
(2011
).44.
See supplementary material at http://dx.doi.org/10.1063/1.4913737 for details of our perturbation model, a detailed discussion of the donor potential, the various modes, convergence and overtone transitions, g-matrix elements of the intermolecular modes, results for the donor bending motion, force fields and dipole moment surfaces used in the perturbation part.
45.
L.
Halonen
and T.
Carrington,
, Jr., J. Chem. Phys.
88
, 4171
(1988
).46.
E. L.
Sibert
, J. T.
Hynes
, and W. P.
Reinhardt
, J. Phys. Chem.
87
, 2032
(1983
).47.
H. M.
Pickett
, J. Chem. Phys.
56
, 1715
(1972
).48.
R.
Meyer
and H. H.
Günthard
, J. Chem. Phys.
49
, 1510
(1968
).49.
E. B.
Wilson
, J. C.
Decius
, and P. C.
Cross
, Molecular Vibrations
(Dover
, New York
, 1980
).50.
B.
Podolsky
, Phys. Rev.
32
, 812
(1928
).51.
H. G.
Kjaergaard
and O. S.
Mortensen
, Am. J. Phys.
58
, 344
(1990
).52.
R.
Meyer
, J. Chem. Phys.
52
, 2053
(1970
).53.
MATLAB and Statistics Toolbox Release R2013a (The MathWorks Inc., Natick, Massachusetts, United States).
54.
H. G.
Kjaergaard
, H.
Yu
, B.
Schattka
, B.
Henry
, and A.
Tarr
, J. Chem. Phys.
93
, 6239
(1990
).55.
K. M.
de Lange
and J. R.
Lane
, J. Chem. Phys.
135
, 064304
(2011
).56.
J. D.
McMahon
and J. R.
Lane
, J. Chem. Phys.
135
, 154309
(2011
).57.
U.
Buck
and F.
Huisken
, Chem. Rev.
100
, 3863
(2000
).58.
A. K.
Mollner
, B. E.
Casterline
, L. C.
Ch’ng
, and H.
Reisler
, J. Phys. Chem. A
113
, 10174
(2009
).59.
S.
Kuma
, M. N.
Slipchenko
, T.
Momose
, and A. F.
Vilesov
, Chem. Phys. Lett.
439
, 265
(2007
).60.
S.
Kuma
, M. N.
Slipchenko
, K. E.
Kuyanov
, T.
Momose
, and A. F.
Vilesov
, J. Phys. Chem. A
110
, 10046
(2006
).61.
A.
Shank
, Y.
Wang
, A.
Kaledin
, B. J.
Braams
, and J. M.
Bowman
, J. Chem. Phys.
130
, 144314
(2009
).62.
C.
Leforestier
, K.
Szalewicz
, and A.
van der Avoird
, J. Chem. Phys.
137
, 014305
(2012
).63.
C.
Leforestier
, Philos. Trans. R. Soc., A
370
, 2675
(2012
).64.
J.
Ceponkus
, P.
Uvdal
, and B.
Nelander
, J. Phys. Chem. A
112
, 3921
(2008
).65.
E.
Arunan
et al., Pure Appl. Chem.
83
, 1619
(2011
).66.
J.
Sadlej
, R.
Moszynski
, J. C.
Dobrowolski
, and A. P.
Mazurek
, J. Phys. Chem. A
103
, 8528
(1999
).67.
D. L.
Howard
and H. G.
Kjaergaard
, J. Phys. Chem. A
110
, 9597
(2006
).68.
L.
Du
and H. G.
Kjaergaard
, J. Phys. Chem. A
115
, 12097
(2011
).© 2015 AIP Publishing LLC.
2015
AIP Publishing LLC
You do not currently have access to this content.
