Vibrational spectra of (n + m = 4, 5; k = 1-4) clusters are determined by far-infrared resonant multiple photon dissociation spectroscopy in the range -250 cm−1. The experimental spectra are assigned using density functional theory for geometries obtained by the Birmingham cluster genetic algorithm. Putative global minimum candidates of the Ar complexes are generated by adding Ar atoms to the low energy isomers and subsequent local optimization. Differential Ar binding energies indicate exceptionally strong Au-Ar bonds in Au-rich clusters, leading to fundamental changes to the IR spectra. The stronger Ar binding is attributed to a relativistically enhanced covalent character of the Au-Ar bond, while in Au-rich species charge-induced dipole interactions overcompensate the relativistic affinity to Au. Moreover, not only the absolute composition but also the topologies are essential in the description of Ar binding to a certain cluster.
REFERENCES
1.
P.
Schwerdtfeger
, Angew. Chem., Int. Ed.
42
, 1892
(2003
).2.
R.
Ferrando
, J.
Jellinek
, and R. L.
Johnston
, Chem. Rev.
108
, 845
(2008
).3.
M.
Faraday
, Philos. Trans. R. Soc. London
147
, 145
(1857
).4.
S.
Fedrigo
, W.
Harbich
, and J.
Buttet
, J . Chem. Phys.
99
, 5712
(1993
).5.
B. A.
Collings
, K.
Athanassenas
, D.
Lacombe
, D. M.
Rayner
, and P. A.
Hackett
, J. Chem. Phys.
101
, 3506
(1994
).6.
M. M.
Alvarez
, J. T.
Khoury
, T. G.
Schaaff
, M. N.
Shafigullin
, I.
Vezmar
, and R. L.
Whetten
, J. Phys. Chem. B
101
, 3706
(1997
).7.
M.
Harb
, F.
Rabilloud
, D.
Simon
, A.
Rydlo
, S.
Lecoultre
, F.
Conus
, V.
Rodrigues
, and C.
Félix
, J . Chem. Phys.
129
, 194108
(2008
).8.
A.
Terasaki
, S.
Minemoto
, M.
Iseda
, and T.
Kondow
, Eur. Phys. J. D
9
, 163
(1999
).9.
M.
Haruta
, T.
Kobayashi
, H.
Sano
, and N.
Yamada
, Chem. Lett.
16
, 405
(1987
).10.
L. M.
Molina
, S.
Lee
, K.
Sell
, G.
Barcaro
, A.
Fortunelli
, B.
Lee
, S.
Seifert
, R. E.
Winans
, J. W.
Elam
, and M. J.
Pellin
, Catal. Today
160
, 116
(2011
).11.
D. R.
Kauffman
, D.
Alfonso
, C.
Matranga
, H.
Qian
, and R.
Jin
, J . Phys. Chem. C
117
, 7914
(2013
).12.
C.
Kumara
, C.
Aikens
, and A.
Dass
, J. Phys. Chem. Lett.
5
, 461
(2014
).13.
J. K.
Gansel
, M.
Thiel
, M. S.
Rill
, M.
Decker
, K.
Bade
, V.
Saile
, G.
von Freymann
, S.
Linden
, and M.
Wegener
, Science
325
, 1513
(2009
).14.
S.
Wang
, X.
Meng
, A.
Das
, T.
Li
, Y.
Song
, T.
Cao
, X.
Zhu
, M.
Zhu
, and R.
Jin
, Angew. Chem., Int. Ed. Engl.
53
, 2376
(2014
).15.
16.
M. V.
Petri
, R. A.
Ando
, and P. H.
Camargo
, Chem. Phys. Lett.
531
, 188
(2012
).17.
T. J. A.
Slater
, A.
Macedo
, S. L. M.
Schroeder
, M. G.
Burke
, P.
O’Brien
, P. H. C.
Camargo
, and S. J.
Haigh
, Nano Lett.
14
, 1921
(2014
).18.
N. L.
Rosi
and C. A.
Mirkin
, Chem. Rev.
105
, 1547
(2005
).19.
M.
Larguinho
and P. V.
Baptista
, J. Proteomics
75
, 2811
(2012
).20.
J. C.
Fabbi
, J. D.
Langenberg
, Q. D.
Costello
, M. D.
Morse
, and L.
Karlsson
, J. Chem. Phys.
115
, 7543
(2001
).21.
Y.
Negishi
, Y.
Nakamura
, A.
Nakajima
, and K.
Kaya
, J. Chem. Phys.
115
, 3657
(2001
).22.
G.-F.
Zhao
, J.-M.
Sun
, and Z.
Zeng
, Chem. Phys.
342
, 267
(2007
).23.
X.-D.
Zhang
, M.-L.
Guo
, D.
Wu
, P.-X.
Liu
, Y.-M.
Sun
, L.-A.
Zhang
, Y.
She
, Q.-F.
Liu
, and F.-Y.
Fan
, Int. J. Mol. Sci.
12
, 2972
(2011
).24.
X.
López-Lozano
, C.
Mottet
, and H.-C.
Weissker
, J . Phys. Chem. C
117
, 3062
(2013
).25.
H.-Ch.
Weissker
, R. L.
Whetten
, and X.
López-Lozano
, Phys. Chem. Chem. Phys.
16
, 12495
(2014
).26.
P.
Weis
, O.
Welz
, E.
Vollmer
, and M. M.
Kappes
, J. Chem. Phys.
120
, 677
(2004
).27.
V.
Bonačić-Koutecký
, J.
Burda
, R.
Mitrić
, M.
Ge
, G.
Zampella
, and P.
Fantucci
, J. Chem. Phys.
117
, 3120
(2002
).28.
A.
Shayeghi
, R. L.
Johnston
, and R.
Schäfer
, Phys. Chem. Chem. Phys.
15
, 19715
(2013
).29.
A.
Shayeghi
, C. J.
Heard
, R. L.
Johnston
, and R.
Schäfer
, J. Chem. Phys.
140
, 054312
(2014
).30.
31.
S.
Heiles
, A. J.
Logsdail
, R.
Schäfer
, and R. L.
Johnston
, Nanoscale
4
, 1109
(2012
).32.
L. M.
Ghiringhelli
, P.
Gruene
, J. T.
Lyon
, D. M.
Rayner
, G.
Meijer
, A.
Fielicke
, and M.
Scheffler
, New J. Phys.
15
, 083003
(2013
).33.
L. A.
Mancera
and D. M.
Benoit
, J. Phys. Chem. A
119
, 3075
(2015
).34.
L. M.
Ghiringhelli
and S. V.
Levchenko
, Inorg. Chem. Commun.
55
, 153
(2015
).35.
A.
Fielicke
, I.
Rabin
, and G.
Meijer
, J. Phys. Chem. A
110
, 8060
(2006
).36.
P.
Pyykkö
, J. Am. Chem. Soc.
117
, 2067
(1995
).37.
D.
Schröder
, H.
Schwarz
, J.
Hrusak
, and P.
Pyykkö
, Inorg. Chem.
37
, 624
(1998
).38.
J. P.
Read
and A. D.
Buckingham
, J. Am. Chem. Soc.
119
, 9010
(1997
).39.
R.
Wesendrup
, T.
Hunt
, and P.
Schwerdtfeger
, J. Chem. Phys.
112
, 9356
(2000
).40.
D.
Bellert
and W. H.
Breckenridge
, Chem. Rev.
102
, 1595
(2002
).41.
W. H.
Breckenridge
, V. L.
Ayles
, and T. G.
Wright
, J. Phys. Chem. A
112
, 4209
(2008
).42.
T.
Zeng
and M.
Klobukowski
, J. Phys. Chem. A
112
, 5236
(2008
).43.
L.
Belpassi
, I.
Infante
, F.
Tarantelli
, and L.
Visscher
, J. Am. Chem. Soc.
130
, 1048
(2008
).44.
P.
Zhang
, Y.
Zhao
, F.
Hao
, X.
Song
, G.
Zhang
, and Y.
Wang
, J. Mol. Struct.: THEOCHEM
899
, 111
(2009
).45.
Z.
Jamshidi
, K.
Eskandari
, and S. M.
Azami
, Int. J. Quantum Chem.
113
, 1981
(2013
).46.
A.
Shayeghi
, R. L.
Johnston
, D. M.
Rayner
, R.
Schäfer
, and A.
Fielicke
, “Messenger or modifier? The nature of argon bonds to mixed gold-silver trimers
,” Angew. Chem., Int. Ed.
(in press). 47.
A.
Fielicke
, G.
von Helden
, and G.
Meijer
, Eur. Phys. J. D
34
, 83
(2005
).48.
A.
Fielicke
, A.
Kirilyuk
, C.
Ratsch
, J.
Behler
, M.
Scheffler
, G.
von Helden
, and G.
Meijer
, Phys. Rev. Lett.
93
, 023401
(2004
).49.
D.
Oepts
, A. F. G.
van der Meer
, and P. W.
van Amersfoort
, Infrared Phys. Technol.
36
, 297
(1995
).50.
P.
Gruene
, B.
Butschke
, J. T.
Lyon
, D. M.
Rayner
, and A.
Fielicke
, Z. Phys. Chem.
228
, 337
(2014
).51.
A. M.
Rappe
, K. M.
Rabe
, E.
Kaxiras
, and J. D.
Joannopoulos
, Phys. Rev. B
41
, 1227
(1990
).52.
J.
Perdew
, K.
Burke
, and M.
Ernzerhof
, Phys. Rev. Lett.
77
, 3865
(1996
).53.
M.
Valiev
, E. J.
Bylaska
, N.
Govind
, K.
Kowalski
, T. P.
Straatsma
, H. J. J.
Van Dam
, D.
Wang
, J.
Nieplocha
, E.
Apra
, T. L.
Windus
, and W. A.
de Jong
, Comput. Phys. Commun.
181
, 1477
(2010
).54.
F.
Weigend
and R.
Ahlrichs
, Phys. Chem. Chem. Phys.
7
, 3297
(2005
).55.
O. A.
Vydrov
and G. E.
Scuseria
, J. Chem. Phys.
125
, 234109
(2006
).56.
M. A.
Rohrdanz
, K. M.
Martins
, and J. M.
Herbert
, J. Chem. Phys.
130
, 054112
(2009
).57.
D. W.
Silverstein
and L.
Jensen
, J. Chem. Phys.
132
, 194302
(2010
).58.
J. V.
Koppen
, M.
Hapka
, M. M.
Szcześniak
, and G.
Chalasinski
, J. Chem. Phys.
137
, 114302
(2012
).59.
F.
Rabilloud
, J. Phys. Chem. A
117
, 4267
(2013
).60.
A.
Shayeghi
, R. L.
Johnston
, and R.
Schäfer
, J. Chem. Phys.
141
, 181104
(2014
).61.
Z.
Jamshidi
, M. F.
Far
, and A.
Maghari
, J. Phys. Chem. A
116
, 12510
(2012
).62.
See supplementary material at http://dx.doi.org/10.1063/1.4923255 for atomic coordinates and harmonic IR linespectra of the considered isomers.
63.
S.
Grimme
, Wiley Interdiscip. Rev.: Comput. Mol. Sci.
1
, 211
(2011
).64.
S. M.
Lang
, P.
Claes
, N. T.
Cuong
, M. T.
Nguyen
, P.
Lievens
, and E.
Janssens
, J. Chem. Phys.
135
, 224305
(2011
).65.
P.
Weis
, Int. J. Mass Spectrom.
245
, 1
(2005
).66.
A.
Schweizer
, J. M.
Weber
, S.
Gilb
, H.
Schneider
, D.
Schooss
, and M. M.
Kappes
, J. Chem. Phys.
119
, 3699
(2003
).67.
M.
Neumaier
, F.
Weigend
, O.
Hampe
, and M. M.
Kappes
, J. Chem. Phys.
125
, 104308
(2006
).68.
See http://www.bear.bham.ac.uk/bluebear for a description of the BlueBEAR HPC facility.
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