In order to clarify its electric double layer (EDL) structure under external voltage, an interface between the ionic liquid N,N-diethyl-N-methyl-N-(2-methoxyethyl)ammonium bis(trifluoromethanesulfonyl)imide and a Au (111) surface was studied by x-ray reflectometry. A clear change in reflectivity was observed as a function of applied voltage. The electron density profile of the ionic liquid around the interface was calculated using liquid structure models. Switching of the external electric field reversed the polarity of the EDL, and the magnitude of the applied voltage controlled the magnitude of the layering structure as well as molecular position fluctuation.

1.
A. A.
Kornyshev
,
J. Phys. Chem. B
111
,
5545
(
2007
).
2.
Y.-Z.
Su
,
Y.-C.
Fu
,
Y.-M.
Wei
,
J.-W.
Yan
,
B.-W.
Mao
,
Chem. Phys. Chem.
11
,
2764
(
2010
).
3.
M.
Galiński
,
A.
Lewandowski
, and
I.
Stȩpniak
,
Electrochim. Acta
51
,
5567
(
2006
).
4.
H.
Shimotani
,
H.
Asanuma
,
A.
Tsukazaki
,
A.
Ohtomo
,
M.
Kawasaki
, and
Y.
Iwasa
,
Appl. Phys. Lett.
91
,
082106
(
2007
).
5.
H.
Yuan
,
H.
Shimotani
,
A.
Tsukazaki
,
A.
Ohtomo
,
M.
Kawasaki
, and
Y.
Iwasa
,
Adv. Funct. Mater.
19
,
1046
(
2009
).
6.
T.
Uemura
,
M.
Yamagishi
,
S.
Ono
, and
J.
Takeya
,
Appl. Phys. Lett.
95
,
103301
(
2009
).
7.
K.
Ueno
,
S.
Nakamura
,
H.
Shimotani
,
H. T.
Yuan
,
N.
Kimura
,
T.
Nojima
,
H.
Aoki
,
Y.
Iwasa
, and
M.
Kawasaki
,
Nat. Nanotechnol.
6
,
408
412
(
2011
).
8.
H. T.
Yuan
,
H.
Shimotani
,
J.
Ye
,
S.
Yoon
,
H.
Aliah
,
A.
Tsukazaki
,
M.
Kawasaki
, and
Y.
Iwasa
,
J. Am. Chem. Soc.
132
,
18402
(
2010
).
9.
V.
Lockett
,
M.
Horne
,
R.
Sedev
,
T.
Rodopoulos
, and
J.
Ralston
,
Phys. Chem. Chem. Phys.
39
,
12499
(
2010
).
10.
M. M.
Islam
,
M. T.
Alam
, and
T.
Ohsaka
,
J. Phys. Chem. C
112
,
16568
(
2008
).
11.
M. V.
Fedorov
and
A. A.
Kornyshev
,
Electrochim. Acta
53
,
6835
(
2008
).
12.
M.
Sha
,
G.
Wu
,
Q.
Dou
,
Z.
Tang
, and
H.
Fang
,
Langmuir
26
,
12667
(
2010
).
13.
M. Z.
Bazant
,
B. D.
Storey
, and
A. A.
Kornyshev
,
Phys. Rev. Lett.
106
,
046102
(
2011
).
14.
S.
Baldelli
,
Acc. Chem. Res.
41
,
421
(
2008
).
15.
T.
Cremer
,
M.
Stark
,
A.
Deyko
,
H.-P.
Steinrück
, and
F.
Maier
,
Langmuir
27
,
3662
(
2011
).
16.
S.
Bovio
,
A.
Podest
,
C.
Lenardi
, and
P.
Milani
,
J. Phys. Chem. B
113
,
6600
(
2009
).
17.
Y.
Yokota
,
T.
Harada
, and
K.
Fukui
,
Chem. Commun.
46
,
8627
(
2010
).
18.
R.
Hayes
,
N.
Borisenko
,
M. K.
Tam
,
P. C.
Howlett
,
F.
Endres
, and
R.
Atkin
,
J. Phys. Chem. C
115
,
6855
(
2011
).
19.
M.
Mezger
,
H.
Schröder
,
H.
Reichert
,
S.
Schramm
,
J. S.
Okasinski
,
S.
Schröder
,
V.
Honkimäki
,
M.
Deutsch
,
B. M.
Ocko
,
J.
Ralston
,
M.
Rohwerder
,
M.
Stratmann
, and
H.
Dosch
,
Science
322
,
424
(
2008
).
20.
L.
Cheng
,
P.
Fenter
,
K. L.
Nagy
,
M. L.
Schlegel
, and
N. C.
Sturchio
,
Phys. Rev. Lett.
87
,
156103
(
2001
).
21.
P.
Fenter
and
N. C.
Sturchio
,
Prog. Surf. Sci.
77
,
171
(
2004
).
22.
E.
Sloutskin
,
B. M.
Ocko
,
L.
Tamam
,
I.
Kuzmenko
,
T.
Gog
, and
M.
Deutsch
,
J. Am. Chem. Soc.
127
,
7796
(
2005
).
23.
M.
Mezger
,
S.
Schramm
,
H.
Schröder
,
H.
Reichert
,
M.
Deutsch
,
E. J.
De Souza
,
J. S.
Okasinski
,
B. M.
Ocko
,
V.
Honkimäki
, and
H.
Dosch
,
J. Chem. Phys.
131
,
094701
(
2009
).
24.
H.
Sakuma
,
T.
Kondo
,
H.
Nakao
,
K.
Shiraki
, and
K.
Kawamura
,
J. Phys. Chem. C
115
,
15959
(
2011
).
25.
N.
Nishi
,
Y.
Yasui
,
T.
Uruga
,
H.
Tanida
,
T.
Yamada
,
S.
Nakayama
,
H.
Matsuoka
, and
T.
Kakiuchi
,
J. Chem. Phys.
132
,
164705
(
2010
).
26.
Y.-J.
Kim
,
Y.
Matsuzawa
,
S.
Ozaki
,
K. C.
Park
,
C.
Kim
,
M.
Endo
,
H.
Yoshida
,
G.
Masuda
,
T.
Sato
, and
M. S.
Dresselhaus
,
J. Electrochem. Soc.
152
,
A710
(
2005
).
27.
E. I.
Rogers
,
B.
Šljukić
,
C.
Hardacre
, and
R. G.
Compton
,
J. Chem. Eng. Data
54
,
2049
(
2009
).
28.

Reflectivity or CTR intensity was extracted from rocking curve measurements at various ζ-positions to eliminate voltage dependence of the bulk ionic-liquid structure, if any. Rocking curves were measured at each ζ with +V applied voltage, followed by the same measurement with –V to minimize systematic error, such as any effect of drift of the optics, in the reflectivity profile for ±V.

29.
O. M.
Magnussen
,
B. M.
Ocko
,
M. J.
Regan
,
K.
Penanen
,
P. S.
Pershan
, and
M.
Deutsch
,
Phys. Rev. Lett.
74
,
4444
(
1995
).
You do not currently have access to this content.