Irreversibility of crystal growth and dissolution processes at the nanoscale

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Morphological and kinetic characteristics of continuous transition through the saturation point from dissolution to growth on the same monomolecular steps on the crystal surface prove that growth and dissolution in the kinetic regime are irreversible processes at the nanoscale. Experimental modeling to solve the fundamental problem of the reversibility of growth and dissolution was carried out using atomic force microscopy (AFM) at extremely low crystallization rates of a poorly soluble model crystal in low-viscosity solutions. The result obtained extends the understanding of near-equilibrium crystal growth processes and the mechanisms of zonality formation in crystals.

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作者简介

N. Piskunova

Komi Scientific Centre, Urals Branch RAS

编辑信件的主要联系方式.
Email: piskunova@geo.komisc.ru

Yushkin Institute of Geology

俄罗斯联邦, Syktyvkar

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2. Fig. 1. Increased surface energy of particles (left) and increased surface tension (right) at the dislocation exit (D), preventing an increase in the interphase surface, i. e., the addition of matter to the dislocation exit point during growth.

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3. Fig. 2. Upper part — dissolution at the exit point of a screw dislocation (circle). Lower part — transition to growth on this screw dislocation (magnified): the matter attaches to the steps edges but not to the exit point of the dislocation (foursquare). The time from the first snapshot is marked on each image. Scale bars (2 µm) are shown in the upper left corner of the images.

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4. Fig. 3. Dissolution and subsequent growth of monomolecular steps of the same hillock — a growth analogue of the Frank-Read dislocation source. The contour of the left part of one of the steps is marked in white. The moment when the system crossed the saturation point is marked by a red rectangle. The time from the start of the experiment is marked on the images. The image size is 4×7 µm.

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5. Fig. 4. Fragment of the graphical image of the transition from dissolution to growth through the saturation point on the steps of the same dislocation mound. In the left light zone of dissolution, growth zones (dark cells) and arrest regions (red cells) are visible. In the dark growth zone on the right, rare dissolution regions (light cells) and arrest regions (red cells) are found. The colors assigned to the cells are based on calculations using AFM data (callout in the centre).

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6. Fig. 5. Average tangential rate of monomolecular steps on the Frank–Read hillock during the transition from dissolution (left) to growth (right) through the saturation point.

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7. Fig. 6. The average normal rate and its fluctuations during the transition from dissolution to growth through the saturation point. The inset shows three profiles of one hillock composed of monomolecular steps (AFM data): one hour before the saturation point, before dissolution (white shape — 1), at the point of maximum dissolution (red shape — 2), and after one hour of growth (green shape — 3).

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8. Fig. 7. The gradients ∇С, ∇I and ∇K are generated by thermal oscillations in the diffusion layer around the thickness δ evaporation and by convection, respectively. The limiting surface processes near the low rates will be the gradients resulting from the excess (during dissolution) and deficiency (during growth) of the substance near the surface itself and surface migration — the symbols ∇Rd, ∇Rg and Mxy in the callouts.

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9. Fig. 8. Modeling of the instrumental influence on nanoscale crystallization processes. On the left (а, в, д, ж, и) — the black line shows the result of the experiment, the red line shows the character of the influence (explanations in the text). On the right (б, г, е, з, к) — the result of the addition of the red and black curves, i. e. the hypothetical curve of the average tangential rate and its fluctuations in the absence of solution stirring, thermal effect of the laser or mechanical effect of the AFM-tip.

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