In the recently developed ultrafast Li-ion conductor, Li10GeP2S12, our ab initio and molecular dynamics simulations have revealed a unique Li ion transport mechanism. The Li ions are discovered to migrate in a highly correlated fashion, stemming from the large Coulombic interaction between the mobile ions. The stringlike cooperative ionic motion is found to entail a rather low energy barrier, contributing to the unusually high ionic conductivity of this solid-state electrolyte. Such a collective migration mechanism may also be operative in other Li-ion battery electrolytes with high concentrations of mobile Li ions.

1.
P. G.
Bruce
,
S. A.
Freunberger
,
L. J.
Hardwick
, and
J. M.
Tarascon
,
Nat. Mater.
11
,
19
(
2012
).
2.
M.
Park
,
X.
Zhang
,
M.
Chung
,
G. B.
Less
, and
A. M.
Sastry
,
J. Power Sources
195
,
7904
(
2010
).
3.
E.
Quartarone
and
P.
Mustarelli
,
Chem. Soc. Rev.
40
,
2525
(
2011
).
4.
P.
Knauth
,
Solid State Ionics
180
,
911
(
2009
).
5.
N.
Kamaya
,
K.
Homma
,
Y.
Yamakawa
,
M.
Hirayama
,
R.
Kanno
,
M.
Yonemura
,
T.
Kamiyama
,
Y.
Kato
,
S.
Hama
,
K.
Kawamoto
, and
A.
Mitsui
,
Nat. Mater.
10
,
682
(
2011
).
6.
Y. F.
Mo
,
S. P.
Ong
, and
G.
Ceder
,
Chem. Mater.
24
,
15
(
2012
).
7.
S.
Adams
and
R. P.
Rao
,
J. Mater. Chem.
22
,
7687
(
2012
).
8.
G.
Kresse
and
J.
Furthmuller
,
Comput. Mater. Sci.
6
,
15
(
1996
).
9.
P. E.
Blöchl
,
Phys. Rev. B
50
,
17953
(
1994
).
10.
J. P.
Perdew
,
K.
Burke
, and
M.
Ernzerhof
,
Phys. Rev. Lett.
77
,
3865
(
1996
).
11.
K. J.
Laidler
,
J. Chem. Educ.
61
,
494
(
1984
).
12.
E. J.
Cussen
,
Chem. Commun.
412
(
2006
).
13.
C.
Donati
,
J. F.
Douglas
,
W.
Kob
,
S. J.
Plimpton
,
P. H.
Poole
, and
S. C.
Glotzer
,
Phys. Rev. Lett.
80
,
2338
(
1998
).
14.
J. P.
Hansen
and
I. R.
McDonald
,
Theory of Simple Liquids
(
Academic
,
London
,
1986
).
15.
C.
Otjacques
,
J. Y.
Raty
,
M. V.
Coulet
,
M.
Johnson
,
H.
Schober
,
C.
Bichara
, and
J. P.
Gaspard
,
Phys. Rev. Lett.
103
,
245901
(
2009
).
16.
G.
Mills
,
H.
Jónsson
, and
G. K.
Schenter
,
Surf. Sci.
324
,
305
(
1995
).
17.
S.
Adams
and
R. P.
Rao
,
J. Mater. Chem.
22
,
1426
(
2012
).
18.
M.
Xu
,
M. S.
Park
,
J. M.
Lee
,
T. Y.
Kim
,
Y. S.
Park
, and
E.
Ma
,
Phys. Rev. B
85
,
052301
(
2012
).
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