In this study, we investigate interference between several excited electronic states in resonance enhanced vibrational Raman optical activity (RROA) spectra. A gradient Franck–Condon model for the excited-state potential energy surface is applied in order to include vibronic effects in the description of the RROA intensities. Both sum-over-states and time-dependent expressions for the RROA intensities in case of close-lying excited states are given. As an example, we compare the calculated RROA and resonance Raman spectra of -naproxen- to the experimental ones. Subsequently, we examine the excitation profiles of -naproxen and study the vibration at in more detail in order to demonstrate how the consideration of a second excited electronic state can lead to significant changes in the RROA intensities.
REFERENCES
1.
L. A.
Nafie
, Chem. Phys.
205
, 309
(1996
).2.
M.
Vargek
, T. B.
Freedman
, E.
Lee
, and L. A.
Nafie
, Chem. Phys. Lett.
287
, 359
(1998
).3.
L.
Jensen
, J.
Autschbach
, M.
Krykunov
, and G. C.
Schatz
, J. Chem. Phys.
127
, 134101
(2007
).4.
P.
Stein
, V.
Miskowski
, W. H.
Woodruff
, J. P.
Griffin
, K. G.
Werner
, B. P.
Gaber
, and T. G.
Spiro
, J. Chem. Phys.
64
, 2159
(1976
).5.
K. -S. K.
Shin
and J. I.
Zink
, J. Am. Chem. Soc.
112
, 7148
(1990
).6.
J. L.
Wootton
and J. I.
Zink
, J. Am. Chem. Soc.
119
, 1895
(1997
).7.
M.
Wu
, M.
Ray
, and A. J.
Sedlacek
, J. Chem. Phys.
109
, 1352
(1998
).8.
S. E.
Bailey
, J. S.
Cohan
, and J. I.
Zink
, J. Phys. Chem. B
104
, 10743
(2000
).9.
J. V.
Lockard
, G.
Valverde
, D.
Neuhauser
, and J. I.
Zink
, J. Phys. Chem. A
110
, 57
(2006
).10.
J.
Neugebauer
, E. J.
Baerends
, E. V.
Efremov
, F.
Ariese
, and C.
Gooijer
, J. Phys. Chem. A
109
, 2100
(2005
).11.
T.
Petrenko
, K.
Ray
, K. E.
Wieghardt
, and F.
Neese
, J. Am. Chem. Soc.
128
, 4422
(2006
).12.
C.
Herrmann
, J.
Neugebauer
, M.
Presselt
, U.
Uhlemann
, M.
Schmitt
, S.
Rau
, J.
Popp
, and M.
Reiher
, J. Phys. Chem. B
111
, 6078
(2007
).13.
14.
T.
Petrenko
and F.
Neese
, J. Chem. Phys.
127
, 164319
(2007
).15.
S.
Laimgruber
, T.
Schmierer
, P.
Gilch
, K.
Kiewisch
, and J.
Neugebauer
, Phys. Chem. Chem. Phys.
10
, 3872
(2008
).16.
K.
Kiewisch
, J.
Neugebauer
, and M.
Reiher
, J. Chem. Phys.
129
, 204103
(2008
).17.
A.
Mohammed
, H.
Ågren
, and P.
Norman
, Phys. Chem. Chem. Phys.
11
, 4539
(2009
).18.
A.
Mohammed
, H.
Ågren
, and P.
Norman
, Chem. Phys. Lett.
468
, 119
(2009
).19.
F.
Lahmani
, K. L.
Barbu-Debus
, N.
Seurre
, and A.
Zehnacker-Rentien
, Chem. Phys. Lett.
375
, 636
(2003
).20.
L. A.
Nafie
, Theor. Chem. Acc.
119
, 39
(2008
).21.
L. A.
Nafie
and D.
Che
, in Modern Nonlinear Optics Part 3
, Advances in Chemical Physics
Vol. 85
, edited by M.
Evans
and S.
Kielich
(Wiley
, New York
, 1993
).22.
A.
Hazra
and M.
Nooijen
, Int. J. Quantum Chem.
95
, 643
(2003
).23.
A.
Hazra
, H. H.
Chang
, and M.
Nooijen
, J. Chem. Phys.
121
, 2125
(2004
).24.
J.
Neugebauer
and B. A.
Hess
, J. Chem. Phys.
120
, 11564
(2004
).25.
W. L.
Peticolas
and T.
Rush
III, J. Comput. Chem.
16
, 1261
(1995
).26.
A. B.
Myers
and R. A.
Mathies
, in Biological Applications of Raman Spectroscopy
, Resonance Raman Spectra of Polyenes and Aromatics
Vol. 2
, edited by T. G.
Spiro
(Wiley
, New York
, 1979
), pp. 123
–166
.27.
L. D.
Barron
, Molecular Light Scattering and Optical Activity
, 2nd ed. (Cambridge University Press
, Cambridge
, 2004
).28.
D. A.
Long
, The Raman Effect: A Unified Treatment of the Theory of Raman Scattering by Molecules
(Wiley
, New York
, 2002
).29.
30.
A.
Myers
, R. A.
Mathies
, D. J.
Tannor
, and E. J.
Heller
, J. Chem. Phys.
77
, 3857
(1982
).31.
A. B.
Myers
, J. Raman Spectrosc.
28
, 389
(1997
).32.
S. -Y.
Lee
and E. J.
Heller
, J. Chem. Phys.
71
, 4777
(1979
).33.
34.
M.
Lilichenko
, D.
Tittelbach-Helmrich
, J. W.
Verhoeven
, I. R.
Gould
, and A. B.
Myers
, J. Chem. Phys.
109
, 10958
(1998
).35.
A.
Myers Kelley
, Int. J. Quantum Chem.
104
, 602
(2005
).36.
A.
Schäfer
, C.
Huber
, and R.
Ahlrichs
, J. Chem. Phys.
100
, 5829
(1994
).37.
38.
C.
Lee
, W.
Yang
, and R. G.
Parr
, Phys. Rev. B
37
, 785
(1988
).39.
T. W.
Patapoff
, P. -Y.
Turpin
, and W. L.
Peticolas
, J. Phys. Chem.
90
, 2347
(1986
).40.
D. C.
Blazej
and W. L.
Peticolas
, J. Chem. Phys.
72
, 3134
(1980
).41.
S.
Hassing
and O. S.
Mortensen
, J. Chem. Phys.
73
, 1078
(1980
).42.
L.
Chinsky
, A.
Laigle
, W. L.
Peticolas
, and P. -Y.
Turpin
, J. Chem. Phys.
76
, 1
(1982
).43.
J.
Neugebauer
, C.
Herrmann
, S.
Luber
, and M.
Reiher
, SNF 4.0, a program for the quantum chemical calculation of vibrational spectra, see http://www.reiher.ethz.ch/software/snf.44.
J.
Neugebauer
, M.
Reiher
, C.
Kind
, and B. A.
Hess
, J. Comput. Chem.
23
, 895
(2002
).45.
J.
Neugebauer
, DNR 1.1.0, a program for resonance Raman and vibronic structure calculations.46.
S.
Luber
and M.
Reiher
, Chem. Phys.
346
, 212
(2008
).47.
A. D.
Becke
, Phys. Rev. A
38
, 3098
(1988
).48.
J. P.
Perdew
, Phys. Rev. B
33
, 8822
(1986
).49.
Amsterdam Density Functional Program; Theoretical Chemistry, Vrije Universiteit, Amsterdam, http://www.scm.com.
50.
G.
te Velde
, F. M.
Bickelhaupt
, E. J.
Baerends
, C.
Fonseca Guerra
, S. J. A.
van Gisbergen
, J. G.
Snijders
, and T. J.
Ziegler
, J. Comput. Chem.
22
, 931
(2001
).51.
S. J. A.
van Gisbergen
, J. G.
Snijders
, and E. J.
Baerends
, Comput. Phys. Commun.
118
, 119
(1999
).52.
P. R. T.
Schipper
, O. V.
Gritsenko
, S. J. A.
van Gisbergen
, and E. J.
Baerends
, J. Chem. Phys.
112
, 1344
(2000
).53.
O. V.
Gritsenko
, P. R. T.
Schipper
, and E. J.
Baerends
, Chem. Phys. Lett.
302
, 199
(1999
).54.
O. V.
Gritsenko
, P. R. T.
Schipper
, and E. J.
Baerends
, Int. J. Quantum Chem.
76
, 407
(2000
).55.
M.
Parac
and S.
Grimme
, Chem. Phys.
292
, 11
(2003
).56.
A.
Köhn
and C.
Hättig
, J. Chem. Phys.
119
, 5021
(2003
).57.
T.
Helgaker
, K.
Ruud
, K. L.
Bak
, P.
Jørgensen
, and J.
Olsen
, Faraday Discuss.
99
, 165
(1994
).58.
K.
Ruud
, T.
Helgaker
, and P.
Bouř
, J. Phys. Chem. A
106
, 7448
(2002
).59.
M.
Pecul
and K.
Ruud
, Int. J. Quantum Chem.
104
, 816
(2005
).60.
V.
Liégeois
, O.
Quinet
, and B.
Champagne
, J. Chem. Phys.
122
, 214304
(2005
).61.
V.
Liégeois
, O.
Quinet
, B.
Champagne
, J.
Haesler
, G.
Zuber
, and W.
Hug
, Vib. Spectrosc.
42
, 309
(2006
).62.
V.
Liégeois
, O.
Quinet
, and B.
Champagne
, Int. J. Quantum Chem.
106
, 3097
(2006
).63.
M.
Reiher
, V.
Liégeois
, and K.
Ruud
, J. Phys. Chem. A
109
, 7567
(2005
).64.
M.
Pecul
, E.
Lamparska
, C.
Cappelli
, L.
Frediani
, and K.
Ruud
, J. Phys. Chem. A
110
, 2807
(2006
).65.
J.
Kapitán
, V.
Baumruk
, and P.
Bouř
, J. Am. Chem. Soc.
128
, 2438
(2006
).66.
C.
Herrmann
, K.
Ruud
, and M.
Reiher
, ChemPhysChem
7
, 2189
(2006
).67.
V.
Liégeois
, K.
Ruud
, and B.
Champagne
, J. Chem. Phys.
127
, 204105
(2007
).68.
C.
Herrmann
, K.
Ruud
, and M.
Reiher
, Chem. Phys.
343
, 200
(2008
).69.
J.
Kapitán
, F.
Zhu
, L.
Hecht
, J.
Gardiner
, D.
Seebach
, and L. D.
Barron
, Angew. Chem., Int. Ed.
47
, 6392
(2008
).70.
J.
Kapitán
, F.
Zhu
, L.
Hecht
, J.
Gardiner
, D.
Seebach
, and L. D.
Barron
, Angew. Chem.
120
, 6492
(2008
).71.
S.
Luber
, C.
Herrmann
, and M.
Reiher
, J. Phys. Chem. B
112
, 2218
(2008
).72.
C. R.
Jacob
, S.
Luber
, and M.
Reiher
, ChemPhysChem
9
, 2177
(2008
).73.
74.
J.
Neugebauer
, E. J.
Baerends
, and M.
Nooijen
, J. Phys. Chem. A
109
, 1168
(2005
).75.
J.
Neugebauer
, E. J.
Baerends
, M.
Nooijen
, and J.
Autschbach
, J. Chem. Phys.
122
, 234305
(2005
).© 2010 American Institute of Physics.
2010
American Institute of Physics
You do not currently have access to this content.