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<!--StartFragment--><p class="MsoNormal" style="margin-right:14.05pt;tab-stops:63.8pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size: 10pt; font-style: normal;" class="">Dear Member of the 3DEM List,</span></p><p class="MsoNormal" style="margin-right:14.05pt;tab-stops:63.8pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size: 10pt; font-style: normal;" class="">We all enjoyed the good news about Alasdair McDowall. </span></p><p class="MsoNormal" style="margin-right:14.05pt;tab-stops:63.8pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size: 10pt; font-style: normal;" class="">There is more. </span></p><p class="MsoNormal" style="margin-right:14.05pt;tab-stops:63.8pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size: 10pt; font-style: normal;" class="">An article by Tulk at all in the 23d of May issue of Nature</span><span style="font-size: 10pt;" class=""> offers, for the first time in my view, a plausible hint about the real nature of the vitreous water that Alasdair was the first to produce and see in an electron cryo-microscope, nearly 4 decades ago. In case you haven't noticed this article, read the following</span></p><p class="MsoNormal" style="margin-right:14.05pt;tab-stops:63.8pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size: 10pt; font-style: normal;" class="">I will be thankful for any comment. </span></p><div class="">Jacques Dubochet</div><div class="">University of Lausanne</div><div class="">Switzerland</div><p class="MsoNormal" style="margin-right:14.05pt;tab-stops:63.8pt;mso-layout-grid-align:
none;text-autospace:none"><u class=""><span lang="EN-US" style="font-size:10.0pt;
mso-ansi-language:EN-US" class="">What is vitrification that owes me a Nobel
prize ? A mystery which seems, at last, to become more understandable.</span></u></p><p class="MsoNormal" style="margin-right:14.05pt;tab-stops:63.8pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-ansi-language:EN-US" class="">Once,
in the early 80s, while we were trying to do something really useful out of
electron cryo-microscopy, Alasdair McDowall decided to freeze water in liquid
ethane rather than in liquid nitrogen. And so, for the first time, we could see
vitreous water. Our observation submitted to Nature was shortly rejected with
the remarkable comment, “you can’t bend Nature”. The editor was wrong. He
should have known it since the discovery that vitreous water can be obtained by
flash cooling of liquid water was already published, or was in press, in the
same journal (Mayer and Brüggeller,1980). Nevertheless, the severe comment had
its good reasons. Fifty years of work had shown that cooling of pure water
always results in ice crystals. Experiments and theory – in particular by Father Basile Luyet and his gifted colleagues such as D. H. Rasmussen and A. Mackenzie
– led to this apparently unavoidable conclusion. <o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;mso-layout-grid-align:none;
text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-ansi-language:EN-US" class="">What
is then “our” mysterious vitreous water which is so useful to electron
cryo-microscopists?<o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;mso-layout-grid-align:none;
text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-ansi-language:EN-US" class="">The
situation became more complicated when Mishima et al. (1984, 1985) found that a
form of vitreous water can be obtained by squeezing normal ice (ice I) by high
pressure at liquid nitrogen temperature (77 K) . The material remains stable
when brought to normal pressure. They called it HDA for high density amorphous
water. The next observation - truly remarkable - is that, upon warming at ambient
pressure, HDA does not crystallise but is first transformed into another form of
vitreous water, LDA, low density amorphous, which seems to be very similar to
“our” vitreous water. Further work indicated that the transition from HDA to
LDA can be reversed and that the transformation seems to be discontinuous like any
<i class="">bona fide </i>first order transition.
Apparently there are two well-distinct states of vitreous water. <o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;mso-layout-grid-align:none;
text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-ansi-language:EN-US" class="">This
is difficult to swallow. As I understand it, it means that there are two kinds
of orders in vitreous water and that each water molecule knows which one it
belongs to. Things are simple when we consider liquid water and ice I, for example.
Upon warming at normal pressure all the water molecules of an ice crystal know
that they are approaching zero °C and that they can’t remain in this state if
more heat is brought to the system. The specific vibrations of the ice lattice
(phonons) is the messenger that keeps each molecule informed. But what happens
between two states of vitreous water ? What tells each molecule that it belong to HLA or LDA? What is the corresponding long range order that must necessarily
hide somewhere ? For me, this situation was painfully mysterious. <o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;mso-layout-grid-align:none;
text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-ansi-language:EN-US" class="">The
present work by Tulk at all. (2019) (also read the explanation by J.S.Tse
(2019)) is for me a big relief. What they did is simple, in principle; they just
took time ! Along the line initiated by Mishima, they compressed ice I at 100 K
but they did it in incremental steps, waiting an hour at each step. No HDA was
formed under these conditions but, with increasing pressure, the material was
transformed into different forms of crystalline ice. Confirming previous
results, HDA was produced when the pressure was increased without pausing. They
conclude that HDA is the kinetically arrested transformation between ice I and some
forms of high density ice crystals; it is not a thermodynamically defined
state.<o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;mso-layout-grid-align:none;
text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-ansi-language:EN-US" class="">I
feel comfortable with the idea that “our” vitreous water can be understood
along the same principle: it is not a thermodynamically define state capable of
first order phase transition but a kinetically arrested volume of liquid water in
its way towards some form of ice crystal. <o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;mso-layout-grid-align:none;
text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-ansi-language:EN-US" class="">At
least one question remains. What is the “feeling” of a biological structure embedded
in vitreous ice? Does it “suffer” during vitrification ? How far can we trust
what we observe by electron cryo-microscopy ? <o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;mso-layout-grid-align:none;
text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-ansi-language:EN-US" class="">I am
confident that members of the 3DEM community will address these questions in
the light of the above Tulk at all results and I look forward to learning about
their answers.</span></p><div class="">Thank you in advance. </div><div class=""><span style="font-size: 10pt;" class=""> </span></div><p class="MsoNormal" style="margin-right:12.85pt;text-indent:-.55pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-bidi-font-size:
12.0pt;mso-fareast-font-family:"MS Mincho";mso-fareast-theme-font:minor-fareast;
mso-bidi-font-family:Helvetica;mso-ansi-language:EN-US" class="">Mayer, E., &
Brüggeller, P. (1980). Complete vitrification in pure liquid water and dilute
aqueous solutions. </span><i class=""><span lang="FR" style="font-size:10.0pt;mso-bidi-font-size:
12.0pt;mso-fareast-font-family:"MS Mincho";mso-fareast-theme-font:minor-fareast;
mso-bidi-font-family:Helvetica;mso-ansi-language:FR" class="">Nature, 288</span></i><span lang="FR" style="font-size:10.0pt;mso-bidi-font-size:12.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-bidi-font-family:Helvetica;
mso-ansi-language:FR" class="">(5791 (11.12.1980)), 569-571. <o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;text-indent:-.55pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-bidi-font-size:
12.0pt;mso-fareast-font-family:"MS Mincho";mso-fareast-theme-font:minor-fareast;
mso-bidi-font-family:Helvetica;mso-ansi-language:EN-US" class="">Mishima, O., Calvert,
L. D., & Whalley, E. (1984). "Melting ice" I at 77 K and 10 kbar
: a new method of making amorphous solids. </span><i class=""><span lang="FR" style="font-size:10.0pt;mso-bidi-font-size:12.0pt;mso-fareast-font-family:"MS Mincho";
mso-fareast-theme-font:minor-fareast;mso-bidi-font-family:Helvetica;mso-ansi-language:
FR" class="">Nature, 310</span></i><span lang="FR" style="font-size:10.0pt;mso-bidi-font-size:
12.0pt;mso-fareast-font-family:"MS Mincho";mso-fareast-theme-font:minor-fareast;
mso-bidi-font-family:Helvetica;mso-ansi-language:FR" class="">, 393-395. <o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;text-indent:-.55pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-bidi-font-size:
12.0pt;mso-fareast-font-family:"MS Mincho";mso-fareast-theme-font:minor-fareast;
mso-bidi-font-family:Helvetica;mso-ansi-language:EN-US" class="">Mishima, O., Calvert,
L. D., & Whalley, E. (1985). An apparently first-order transition between
tow amorphous phases of ice induced by pressure. <i class="">Nature, 314</i>, 76-78. <o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;text-indent:-.55pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-bidi-font-size:
12.0pt;mso-fareast-font-family:"MS Mincho";mso-fareast-theme-font:minor-fareast;
mso-bidi-font-family:Helvetica;mso-ansi-language:EN-US" class="">Tse, J. S. (2019). A
twist in the tale of the structure of ice. <i class="">Nature, 569</i>(7757), 495-496.<o:p class=""></o:p></span></p><p class="MsoNormal" style="margin-right:12.85pt;mso-layout-grid-align:none;
text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-ansi-language:EN-US" class="">
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<!--EndFragment--></span></p><p class="MsoNormal" style="margin-right:12.85pt;text-indent:-.55pt;mso-layout-grid-align:
none;text-autospace:none"><span lang="EN-US" style="font-size:10.0pt;mso-bidi-font-size:
12.0pt;mso-fareast-font-family:"MS Mincho";mso-fareast-theme-font:minor-fareast;
mso-bidi-font-family:Helvetica;mso-ansi-language:EN-US" class="">Tulk, C. A., Molaison,
J. J., Makhluf, A. R., Manning, C. E., & Klug, D. D. (2019). Absence of
amorphous forms when ice is compressed at low temperature. </span><i class=""><span lang="FR" style="font-size:10.0pt;mso-bidi-font-size:12.0pt;mso-fareast-font-family:
"MS Mincho";mso-fareast-theme-font:minor-fareast;mso-bidi-font-family:Helvetica;
mso-ansi-language:FR" class="">Nature, 569</span></i><span lang="FR" style="font-size:
10.0pt;mso-bidi-font-size:12.0pt;mso-fareast-font-family:"MS Mincho";
mso-fareast-theme-font:minor-fareast;mso-bidi-font-family:Helvetica;mso-ansi-language:
FR" class="">(7757), 542-545.<o:p class=""></o:p></span></p>
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