Nucleation, the birth of a stable cluster from a disorder, is inherently stochastic. Yet up to date, there are no quantitative studies on NaCl nucleation that accounts for its stochastic nature. Here, we report the first stochastic treatment of NaCl-water nucleation kinetics. Using a recently developed microfluidic system and evaporation model, our measured interfacial energies extracted from a modified Poisson distribution of nucleation time show an excellent agreement with theoretical predictions. Furthermore, analysis of nucleation parameters in 0.5, 1.5, and 5.5 pl microdroplets reveals an interesting interplay between confinement effects and shifting of nucleation mechanisms. Overall, our findings highlight the need to treat nucleation stochastically rather than deterministically to bridge the gap between theory and experiment.
REFERENCES
1.
J.
Lee
, J.
Yang
, S. G.
Kwon
, and T.
Hyeon
, Nat. Rev. Mater.
1
(8
), 16034
(2016
).2.
J. H.
Um
, A.
Jin
, X.
Huang
, J.
Seok
, S. S.
Park
, J.
Moon
, M.
Kim
, S. H.
Kim
, H. S.
Kim
, S.-P.
Cho
, H. D.
Abruña
, and S.-H.
Yu
, Energy Environ. Sci.
15
(4
), 1493
–1502
(2022
).3.
R. D.
Davis
, S.
Lance
, J. A.
Gordon
, S. B.
Ushijima
, and M. A.
Tolbert
, Proc. Natl. Acad. Sci. U. S. A.
112
(52
), 15815
(2015
).4.
J.
Desarnaud
, H.
Derluyn
, J.
Carmeliet
, D.
Bonn
, and N.
Shahidzadeh
, J. Phys. Chem. Lett.
5
(5
), 890
–895
(2014
).5.
G. S.
Frankel
, J. D.
Vienna
, J.
Lian
, X.
Guo
, S.
Gin
, S. H.
Kim
, J.
Du
, J. V.
Ryan
, J.
Wang
, W.
Windl
, C. D.
Taylor
, and J. R.
Scully
, Chem. Rev.
121
(20
), 12327
–12383
(2021
).6.
E. M.
Winkler
and P. C.
Singer
, Geol. Soc. Am. Bull.
83
(11
), 3509
–3514
(1972
).7.
M. J.
Qazi
, R. W.
Liefferink
, S. J.
Schlegel
, E. H. G.
Backus
, D.
Bonn
, and N.
Shahidzadeh
, Langmuir
33
(17
), 4260
–4268
(2017
).8.
N. E. R.
Zimmermann
, B.
Vorselaars
, J. R.
Espinosa
, D.
Quigley
, W. R.
Smith
, E.
Sanz
, C.
Vega
, and B.
Peters
, J. Chem. Phys.
148
(22
), 222838
(2018
).9.
K. E.
Blow
, D.
Quigley
, and G. C.
Sosso
, J. Chem. Phys.
155
(4
), 040901
(2021
).10.
N. E. R.
Zimmermann
, B.
Vorselaars
, D.
Quigley
, and B.
Peters
, J. Am. Chem. Soc.
137
(41
), 13352
–13361
(2015
).11.
D.
Zahn
, Phys. Rev. Lett.
92
(4
), 040801
(2004
).12.
R.
Bahadur
, L. M.
Russell
, and S.
Alavi
, J. Phys. Chem. B
111
(41
), 11989
–11996
(2007
).13.
G.
Lanaro
and G. N.
Patey
, J. Phys. Chem. B
120
(34
), 9076
–9087
(2016
).14.
H.
Jiang
, A.
Haji-Akbari
, P. G.
Debenedetti
, and A. Z.
Panagiotopoulos
, J. Chem. Phys.
148
(4
), 044505
(2018
).15.
Y.
Gao
, L. E.
Yu
, and S. B.
Chen
, J. Phys. Chem. A
111
(42
), 10660
–10666
(2007
).16.
H.-S.
Na
, S.
Arnold
, and A. S.
Myerson
, J. Cryst. Growth
139
(1
), 104
–112
(1994
).17.
L.-T.
Deck
and M.
Mazzotti
, Cryst. Growth Des.
23
(2
), 899
–914
(2022
).18.
N.
Candoni
, Z.
Hammadi
, R.
Grossier
, M.
Ildefonso
, S.
Zhang
, R.
Morin
, and S.
Veesler
, in Advances in Organic Crystal Chemistry: Comprehensive Reviews 2015
, edited by R.
Tamura
and M.
Miyata
(Springer
, Japan, Tokyo
, 2015
), pp. 95
–113
.19.
R.
Grossier
, Z.
Hammadi
, R.
Morin
, and S.
Veesler
, Phys. Rev. Lett.
107
(2
), 025504
(2011
).20.
T.
Nakamuro
, M.
Sakakibara
, H.
Nada
, K.
Harano
, and E.
Nakamura
, J. Am. Chem. Soc.
143
(4
), 1763
–1767
(2021
).21.
R.
Cedeno
, R.
Grossier
, M.
Lagaize
, D.
Nerini
, N.
Candoni
, A.
Flood
, and S.
Veesler
, Faraday Discuss.
235
, 183
–197
(2022
).22.
R.
Cedeno
, R.
Grossier
, V.
Tishkova
, N.
Candoni
, A. E.
Flood
, and S.
Veesler
, Langmuir
38
(31
), 9686
–9696
(2022
).23.
L.
Goh
, K.
Chen
, V.
Bhamidi
, G.
He
, N. C. S.
Kee
, P. J. A.
Kenis
, C. F.
Zukoski
III, and R. D.
Braatz
, Cryst. Growth Des.
10
(6
), 2515
–2521
(2010
). 24.
X. Y.
Liu
, Langmuir
16
(18
), 7337
–7345
(2000
).25.
F. C.
Meldrum
and C.
O’Shaughnessy
, Adv. Mater.
32
(31
), 2001068
(2020
).26.
R.
Grossier
and S.
Veesler
, Cryst. Growth Des.
9
(4
), 1917
–1922
(2009
).27.
O. A.
Bempah
and O. E.
Hileman
, Jr., Can. J. Chem.
51
(20
), 3435
–3442
(1973
).28.
R.
Grossier
, V.
Tishkova
, R.
Morin
, and S.
Veesler
, AIP Adv.
8
(7
), 075324
(2018
).29.
B.
Peters
, J. Cryst. Growth
317
(1
), 79
–83
(2011
).30.
N.
Shahidzadeh
, M. F. L.
Schut
, J.
Desarnaud
, M.
Prat
, and D.
Bonn
, Sci. Rep.
5
(1
), 10335
(2015
).31.
P.
Koß
, A.
Statt
, P.
Virnau
, and K.
Binder
, Phys. Rev. E
96
(4
), 042609
(2017
).32.
M. W.
Anderson
, M.
Bennett
, R.
Cedeno
, H.
Cölfen
, S. J.
Cox
, A. J.
Cruz-Cabeza
, J. J.
De Yoreo
, R.
Drummond-Brydson
, M. K.
Dudek
, K. A.
Fichthorn
, A. R.
Finney
, I.
Ford
, J. M.
Galloway
, D.
Gebauer
, R.
Grossier
, J. H.
Harding
, A.
Hare
, D.
Horváth
, L.
Hunter
, J.
Kim
, Y.
Kimura
, C. E. A.
Kirschhock
, A. A.
Kiselev
, W.
Kras
, C.
Kuttner
, A. Y.
Lee
, Z.
Liao
, L.
Maini
, S. O.
Nilsson Lill
, N.
Pellens
, S. L.
Price
, I. B.
Rietveld
, J. D.
Rimer
, K. J.
Roberts
, J.
Rogal
, M.
Salvalaglio
, I.
Sandei
, G.
Schuszter
, J.
Sefcik
, W.
Sun
, J. H.
ter Horst
, M.
Ukrainczyk
, A. E. S.
Van Driessche
, S.
Veesler
, P. G.
Vekilov
, V.
Verma
, T.
Whale
, H. P.
Wheatcroft
, and J.
Zeglinski
, Faraday Discuss.
235
, 219
–272
(2022
).33.
S.
Karthika
, T. K.
Radhakrishnan
, and P.
Kalaichelvi
, Cryst. Growth Des.
16
(11
), 6663
(2016
).34.
M. A.
Durán-Olivencia
, P.
Yatsyshin
, S.
Kalliadasis
, and J. F.
Lutsko
, New J. Phys.
20
(8
), 083019
(2018
).35.
H.
Hwang
, Y. C.
Cho
, S.
Lee
, Y.-H.
Lee
, S.
Kim
, Y.
Kim
, W.
Jo
, P.
Duchstein
, D.
Zahn
, and G. W.
Lee
, Chem. Sci.
12
(1
), 179
–187
(2021
).36.
C. P.
Lamas
, J. R.
Espinosa
, M. M.
Conde
, J.
Ramírez
, P.
Montero de Hijes
, E.
G. Noya
, C.
Vega
, and E.
Sanz
, Phys. Chem. Chem. Phys.
23
(47
), 26843
–26852
(2021
).37.
A. P.
Olsen
, R. C.
Flagan
, and J. A.
Kornfield
, Rev. Sci. Instrum.
77
(7
), 073901
(2006
).38.
A.
Naillon
, P.
Joseph
, and M.
Prat
, J. Cryst. Growth
463
, 201
–210
(2017
).© 2023 Author(s). Published under an exclusive license by AIP Publishing.
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