We report on measured neutron cross section data for super-cooled water and ice by time-of-flight (TOF) neutron transmission imaging. In particular, we demonstrate the use of high duty cycle (HDC)-TOF measurements to determine the local aggregate state of water with spatial resolution, by exploiting the neutron cross section dependence on the mobility of hydrogen atoms for long neutron wavelengths (>4 Å). While one can envision many different applications for this method, one example is to provide insights into the freezing mechanism during the start-up of polymer electrolyte fuel cells from below zero degrees. Unlike for other wavelength selective measurements (e.g., Bragg edge imaging), only a limited wavelength resolution is required for this method. With a chopper setup with HDC (30%), we reached a high contrast-to-noise ratio (CNR) with a contrast between ice and super-cooled water of 8%. To maximize the CNR, we optimized the duty cycle, pulse period, and image processing parameters. Moreover, we present a theoretical framework for performing such optimization calculations, which can be used to maximize CNR for any beam line and any substances. For the optimization procedure presented in this publication, we used cross section values for ice and super-cooled water measured with high wavelength resolution using wavelength frame multiplication choppers. Our results show that the aggregate state of water of a sufficiently thick layer of water (>0.5 mm) can be reliably determined for a small area (1 mm2) and with a reasonable short acquisition time of 5 min.

1.
N.
Kardjilov
,
I.
Manke
,
R.
Woracek
,
A.
Hilger
, and
J.
Banhart
,
Mater. Today
21
,
652
(
2018
).
2.
P.
Boillat
,
E. H.
Lehmann
,
P.
Trtik
, and
M.
Cochet
,
Curr. Opin. Electrochem.
5
,
3
(
2017
).
3.
J. P.
Owejan
,
T. A.
Trabold
,
J. J.
Gagliardo
,
D. L.
Jacobson
,
R. N.
Carter
,
D. S.
Hussey
, and
M.
Arif
,
J. Power Sources
171
,
626
(
2007
).
4.
I.
Manke
,
C.
Hartnig
,
M.
Grunerbel
,
J.
Kaczerowski
,
W.
Lehnert
,
N.
Kardjilov
,
A.
Hilger
,
J.
Banhart
,
W.
Treimer
, and
M.
Strobl
,
Appl. Phys. Lett.
90
,
184101
(
2007
).
5.
A.
Lange
,
A.
Kupsch
,
M. P.
Hentschel
,
I.
Manke
,
N.
Kardjilov
,
T.
Arlt
, and
R.
Grothausmann
,
J. Power Sources
196
,
5293
(
2011
).
6.
P.
Boillat
,
P.
Oberholzer
,
A.
Kaestner
,
R.
Siegrist
,
E. H.
Lehmann
,
G. G.
Scherer
, and
A.
Wokaun
,
J. Electrochem. Soc.
159
,
F210
(
2012
).
7.
P.
Stahl
,
J.
Biesdorf
,
P.
Boillat
,
J.
Kraft
, and
K. A.
Friedrich
,
J. Electrochem. Soc.
162
,
F677
(
2015
).
8.
C.
Lee
,
R.
Banerjee
,
N.
Ge
,
J. K.
Lee
,
B. Z.
Zhao
,
E.
Baltic
,
J. M.
LaManna
,
D. S.
Hussey
,
D. L.
Jacobson
,
R.
Abouatallah
,
R.
Wang
, and
A.
Bazylak
,
Electrochim. Acta
279
,
91
(
2018
).
9.
O. F.
Selamet
,
U.
Pasaogullari
,
D.
Spernjak
,
D. S.
Hussey
,
D. L.
Jacobson
, and
M. D.
Mat
,
Int. J. Hydrogen Energy
38
,
5823
(
2013
).
10.
J.
Seweryn
,
J.
Biesdorf
,
T. J.
Schmidt
, and
P.
Boillat
,
J. Electrochem. Soc.
163
,
F3009
(
2016
).
11.
R.
Hassanein
,
H. O.
Meyer
,
A.
Carminati
,
M.
Estermann
,
E.
Lehmann
, and
P.
Vontobel
,
J. Phys. D: Appl. Phys.
39
,
4284
(
2006
).
12.
P.
Zhang
,
F. H.
Wittmann
,
P.
Lura
,
H. S.
Muller
,
S. B.
Han
, and
T. J.
Zhao
,
Cem. Concr. Res.
108
,
152
(
2018
).
13.
H.
Justnes
,
K.
Bryhn-Ingebrigtsen
, and
G. O.
Rosvold
,
Adv. Cem. Res.
6
,
67
(
1994
).
14.
P.
Trtik
,
B.
Münch
,
W. J.
Weiss
,
A.
Kaestner
,
I.
Jerjen
,
L.
Josic
,
E.
Lehmann
, and
P.
Lura
,
Nucl. Instrum. Methods Phys. Res., Sect. A
651
,
244
(
2011
).
15.
P.
Benard
,
E.
Kroener
,
P.
Vontobel
,
A.
Kaestner
, and
A.
Carminati
,
Adv. Water Resour.
95
,
190
(
2016
).
16.
M.
Sedighi-Gilani
,
M.
Griffa
,
D.
Mannes
,
E.
Lehmann
,
J.
Carmeliet
, and
D.
Derome
,
Int. J. Heat Mass Transfer
55
,
6211
(
2012
).
17.
M.
Zarebanadkouki
,
A.
Carminati
,
A.
Kaestner
,
D.
Mannes
,
M.
Morgano
,
S.
Peetermans
,
E.
Lehmann
, and
P.
Trtik
,
Phys. Procedia
69
,
292
(
2015
).
18.
P.
Oberholzer
,
P.
Boillat
,
R.
Siegrist
,
R.
Perego
,
A.
Kästner
,
E.
Lehmann
,
G. G.
Scherer
, and
A.
Wokaun
,
J. Electrochem. Soc.
159
,
B235
(
2011
).
19.
A.
Santamaria
,
H. Y.
Tang
,
J. W.
Park
,
G. G.
Park
, and
Y. J.
Sohn
,
Int. J. Hydrogen Energy
37
,
10836
(
2012
).
20.
J.
Mishler
,
Y.
Wang
,
P. P.
Mukherjee
,
R.
Mukundan
, and
R. L.
Borup
,
Electrochim. Acta
65
,
127
(
2012
).
21.
R.
Mukundan
,
J.
Davey
,
R.
Lujan
,
J.
Spendelow
,
Y. S.
Kim
,
D. S.
Hussey
,
D.
Jacobson
,
M.
Arif
, and
R. L.
Borup
,
ECS Trans.
16
,
1939
(
2008
).
22.
R.
Mukundan
,
Y. S.
Kim
,
T.
Rockward
,
J. R.
Davey
,
B.
Pivovar
,
D. S.
Hussey
,
D. L.
Jacobson
,
M.
Arif
, and
R.
Borup
,
ECS Trans.
11
,
543
(
2007
).
23.
R.
Mukundan
,
R.
Lujan
,
J. R.
Davey
,
J. S.
Spendelow
,
D. S.
Hussey
,
D. L.
Jacobson
,
M.
Arif
, and
R.
Borup
,
ECS Trans.
25
,
345
(
2009
).
24.
N.
Macauley
,
R. W.
Lujan
,
D.
Spernjak
,
D. S.
Hussey
,
D. L.
Jacobson
,
K.
More
,
R. L.
Borup
, and
R.
Mukundan
,
J. Electrochem. Soc.
163
,
F1317
(
2016
).
25.
Y.
Ishikawa
,
H.
Hamada
,
M.
Uehara
, and
M.
Shiozawa
,
J. Power Sources
179
,
547
(
2008
).
26.
Y.
Ishikawa
,
M.
Shiozawa
,
M.
Kondo
, and
K.
Ito
,
Int. J. Heat Mass Transfer
74
,
215
(
2014
).
27.
N.
Wakatake
,
Y.
Tabe
, and
T.
Chikahisa
,
ECS Trans.
75
,
623
(
2016
).
29.
Z.
Yang
,
Q.
Du
,
S.
Huo
, and
K.
Jiao
,
Int. J. Hydrogen Energy
42
,
25372
(
2017
).
30.
D.
Ko
,
S.
Doh
,
D. I.
Yu
,
H. S.
Park
, and
M. H.
Kim
,
Fuel Cells
18
,
413
(
2018
).
31.
S. H.
Ge
and
C. Y.
Wang
,
Electrochem. Solid-State Lett.
9
,
A499
(
2006
).
32.
S. H.
Ge
and
C. Y.
Wang
,
Electrochim. Acta
52
,
6395
(
2007
).
33.
I.
Mayrhuber
,
F.
Marone
,
M.
Stampanoni
,
T. J.
Schmidt
and
F. N.
Büchi
,
ChemElectroChem
2
,
1551
(
2015
).
34.
J.
Roth
,
M.
Zurbrug
,
S.
Irvine
,
F.
Marone
,
M.
Stampanoni
, and
F. N.
Buchi
,
ECS Trans.
58
,
453
(
2013
).
35.
J.
Biesdorf
,
P.
Oberholzer
,
F.
Bernauer
,
A.
Kaestner
,
P.
Vontobel
,
E.
Lehmann
,
T. J.
Schmidt
, and
P.
Boillat
,
ECS Trans.
58
,
309
(
2013
).
36.
J.
Biesdorf
,
P.
Oberholzer
,
F.
Bernauer
,
A.
Kaestner
,
P.
Vontobel
,
E. H.
Lehmann
,
T. J.
Schmidt
, and
P.
Boillat
,
Phys. Rev. Lett.
112
,
248301
(
2014
).
37.
P.
Stahl
,
J.
Biesdorf
,
P.
Boillat
, and
K. A.
Friedrich
,
J. Electrochem. Soc.
163
,
F1535
(
2016
).
38.
R.
Woracek
,
J.
Santisteban
,
A.
Fedrigo
, and
M.
Strobl
,
Nucl. Instrum. Methods Phys. Res., Sect. A
878
,
141
(
2018
).
39.
L.
Torres
,
J. R.
Granada
, and
J. J.
Blostein
,
Nucl. Instrum. Methods Phys. Res., Sect. B
251
,
304
(
2006
).
40.
J.
Biesdorf
, Ph.D. thesis,
ETH-Zürich
,
2016
.
41.
M.
Strobl
,
M.
Bulat
, and
K.
Habicht
,
Nucl. Instrum. Methods Phys. Res., Sect. A
705
,
74
(
2013
).
42.
K.
Heinloth
,
Z. Phys.
163
,
218
(
1961
), EXFOR 21341002.
43.
S. B.
Stepanov
and
V. E.
Zhitarev
,
Sov. At. Energy
41
,
743
(
1976
), EXFOR 41620002.
44.
R.
Woracek
,
T.
Hofmann
,
M.
Bulat
,
M.
Sales
,
K.
Habicht
,
K.
Andersen
, and
M.
Strobl
,
Nucl. Instrum. Methods Phys. Res., Sect. A
839
,
102
(
2016
).
45.
A. S.
Tremsin
,
V.
Dangendorf
,
K.
Tittelmeier
,
B.
Schillinger
,
M.
Schulz
,
M.
Lerche
, and
W. B.
Feller
,
J. Instrum.
10
,
P07008
(
2015
).
47.
A. S.
Tremsin
,
J. V.
Vallerga
,
J. B.
McPhate
, and
O. H. W.
Siegmund
,
J. Instrum.
9
,
C05026
(
2014
).
48.
P.
Boillat
,
C.
Carminati
,
F.
Schmid
,
C.
Grunzweig
,
J.
Hovind
,
A.
Kaestner
,
D.
Mannes
,
M.
Morgano
,
M.
Siegwart
,
P.
Trtik
,
P.
Vontobel
, and
E. H.
Lehmann
,
Opt. Express
26
,
15769
(
2018
).
49.
C.
Carminati
,
P.
Boillat
,
F.
Schmid
,
P.
Vontobel
,
J.
Hovind
,
M.
Morgano
,
M.
Raventos
,
M.
Siegwart
,
D.
Mannes
,
C.
Gruenzweig
,
P.
Trtik
,
E.
Lehmann
,
M.
Strobl
, and
A.
Kaestner
,
PLoS One
14
,
e0210300
(
2019
).
50.
A.
Furrer
,
J.
Mesot
, and
T.
Strassle
, (
World Scientific
,
2009
).
51.
R.
Macfarlane
,
D. W.
Muir
,
R. M.
Boicourt
,
I.
Kahler
,
C.
Albert
, and
J. L.
Conlin
, Report LA-UR-17-20093,
Los Alamos National Laboratory (LANL)
,
Los Alamos, NM, USA
,
2017
.
52.
J. I.
Márquez Damian
,
J. R.
Granada
, and
D. C.
Malaspina
,
Ann. Nucl. Energy
65
,
280
(
2014
).
53.
J. I.
Márquez Damian
,
D. C.
Malaspina
, and
J. R.
Granada
,
J. Chem. Phys.
139
,
024504
(
2013
).
54.
S.
Herdade
,
M.
Bechara
,
C.
Rodriguez
, and
L.
Vinhas
, “
Brazilian report to the I.N.D.C.
,” Report No. 2, EXFOR 30229003,
1969
, p.
22
.
55.
J. L.
Russell
,
J. M.
Neill
, and
J. R.
Brown
, General Atomic Div. Reports, Report No. 7581, EXFOR 11162003,
1966
.
56.
A. S.
Tremsin
,
J. V.
Vallerga
,
J. B.
McPhate
, and
O. H. W.
Siegmund
,
Nucl. Instrum. Methods Phys. Res., Sect. A
787
,
20
(
2015
).
57.
J.
Hayya
,
D.
Armstrong
, and
N.
Gressis
,
Manage. Sci.
21
,
1338
(
1975
).
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