The dynamics of water at supercooled temperatures in aqueous solutions of different types of solutes has been deeply analyzed in the literature. In these previous works and in most of the cases, a single relaxation of water molecules is observed. In this work, we analyze the dynamics of water in solutions for which a dual relaxation of water molecules is experimentally measured. We discuss the criteria for observing these two water relaxations in these specific solutions and their most likely origins. We also discuss how these two water relaxations relate to the relaxation behavior of bulk water and how the slower one is coupled to the solute dynamics and is essential for the dynamics and functional properties of proteins.

1.
S.
Ebbinghaus
 et al.,
Proc. Natl. Acad. Sci. U. S. A.
104
,
20749
(
2007
).
2.
L. W.
Luyuan Zhang
,
Y.-T.
Kao
,
W.
Qiu
,
Y.
Yang
,
O.
Okobiah
, and
D.
Zhong
,
Proc. Natl. Acad. Sci. U. S. A.
104
,
18461
(
2007
).
3.
N. Q.
Vinh
,
S. J.
Allen
, and
K. W.
Plaxco
,
J. Am. Chem. Soc.
133
,
8942
(
2011
).
4.
L.
Nilsson
and
B.
Halle
,
Proc. Natl. Acad. Sci. U. S. A.
102
,
13867
(
2005
).
5.
G.
Camisasca
 et al.,
J. Chem. Phys.
145
,
044503
(
2016
).
6.
D.
Corradini
 et al.,
Sci. Rep.
3
,
1218
(
2013
).
7.
D.
Laage
,
T.
Elsaesser
, and
J. T.
Hynes
,
Chem. Rev.
117
,
10694
(
2017
).
8.
S. C.
Harvey
and
P.
Hoekstra
,
J. Phys. Chem.
76
,
2987
(
1972
).
9.
G.
Otting
,
Prog. Nucl. Magn. Reson. Spectrosc.
31
,
259
(
1997
).
10.
N.
Shinyashiki
 et al.,
J. Phys. Chem. B
113
,
14448
(
2009
).
11.
A.
Panagopoulou
 et al.,
Biochim. Biophys. Acta, Proteins Proteomics
1814
,
1984
(
2011
).
12.
S. A.
Lusceac
,
M. R.
Vogel
, and
C. R.
Herbers
,
Biochim. Biophys. Acta, Proteins Proteomics
1804
,
41
(
2010
).
13.
S.
Cerveny
,
I.
Combarro-Palacios
, and
J.
Swenson
,
J. Phys. Chem. Lett.
7
,
4093
(
2016
).
14.
J.
Swenson
and
S.
Cerveny
,
J. Phys.: Condens. Matter
27
,
033102
(
2015
).
15.
I.
Combarro Palacios
 et al.,
J. Chem. Phys.
150
,
124902
(
2019
).
16.
P.
Papadopoulos
 et al.,
J. Chem. Phys.
122
,
224906
(
2005
).
17.
A.
Gitsas
 et al.,
Biomacromolecules
9
,
1959
(
2008
).
18.
S.
Maeda
,
C.
Chizuru Sasaki
, and
K.
Kunimoto
, in
NMR Spectroscopy of Polymers: Innovative Strategies for Complex Macromolecules Vol. 1077 ACS Symposium Series
, edited by
H. N.
Cheng
,
T.
Asakura
, and
A. D.
English
(
American Chemical Society
,
2011
), pp.
317
335
.
19.
S.
Jia
 et al.,
Int. J. Mol. Sci.
10
,
3358
(
2009
).
20.
A.
Panagopoulou
 et al.,
J. Phys. Chem. B
116
,
4593
(
2012
).
21.
H.
Jansson
and
J.
Swenson
,
Biochim. Biophys. Acta
1804
,
20
(
2010
).
22.
S. A.
Lusceac
 et al.,
J. Non-Cryst. Solids
357
,
655
(
2011
).
23.
J.
Kong
and
S.
Yu
,
Acta Biochim. Biophys. Sin.
39
,
549
(
2007
).
24.
A.
Dong
,
P.
Huang
, and
W. S.
Caughey
,
Biochemistry
29
,
3303
(
1990
).
25.
S. C.
Shukla
 et al.,
Biochem. Eng. J.
65
,
70
(
2012
).
26.
S.
Maeda
 et al.,
Polym. Bull.
68
,
745
(
2011
).
27.
K.
Amann-Winkel
 et al.,
Proc. Natl. Acad. Sci. U. S. A.
110
,
17720
(
2013
).
28.
J.
Sjostrom
 et al.,
J. Chem. Phys.
128
,
154503
(
2008
).
29.
M.
Sattig
and
M.
Vogel
,
J. Phys. Chem. Lett.
5
,
174
(
2014
).
30.
S.
Cerveny
 et al.,
J. Non-Cryst. Solids
356
,
3037
(
2010
).
31.
M.
Weigler
 et al.,
J. Phys. Chem. B
123
,
2123
(
2019
).
32.
R.
Buchner
,
G. T.
Hefter
, and
J.
Barthel
,
J. Chem. Soc., Faraday Trans.
90
,
2475
(
1994
).
33.
S.
Cerveny
 et al.,
Phys. Rev. Lett.
93
,
245702
(
2004
).
34.
S.
Cerveny
,
J.
Colmenero
, and
A.
Alegria
,
Eur. Phys. J.: Spec. Top.
141
,
49
(
2007
).
35.
G. P.
Johari
,
A.
Hallbrucker
, and
E.
Mayer
,
Nature
330
,
552
(
1987
).
36.
J.
Swenson
and
J.
Teixeira
,
J. Chem. Phys.
132
,
014508
(
2010
).
37.
S. A.
McCartney
and
V.
Sadtchenko
,
J. Chem. Phys.
138
,
084501
(
2013
).
38.
J.
Qvist
,
H.
Schober
, and
B.
Halle
,
J. Chem. Phys.
134
,
144508
(
2011
).
39.
J. J.
Shephard
and
C. G.
Salzmann
,
J. Phys. Chem. Lett.
7
,
2281
(
2016
).
40.
J.
Swenson
,
Phys. Chem. Chem. Phys.
20
,
30095
(
2018
).
41.
C. G.
Salzmann
 et al.,
Phys. Chem. Chem. Phys.
13
,
18468
(
2011
).
43.
D.
Bhattacharya
,
C. N.
Payne
, and
V.
Sadtchenko
,
J. Phys. Chem. A
115
,
5965
(
2011
).
44.
K.
Sasaki
 et al.,
J. Phys. Chem. B
121
,
265
(
2017
).
45.
H.
Frauenfelder
 et al.,
Proc. Natl. Acad. Sci. U. S. A.
106
,
5129
(
2009
).
46.
J. S.
Hansen
 et al.,
Phys. Rev. Lett.
116
,
237601
(
2016
).
47.
J.
Gabriel
,
F.
Pabst
, and
T.
Blochowicz
,
J. Phys. Chem. B
121
,
8847
(
2017
).
48.
N.
Müller
and
M.
Vogel
,
J. Chem. Phys.
150
,
064502
(
2019
).

Supplementary Material

You do not currently have access to this content.