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ISSN 0018-151X, High Temperature, 2016, Vol. 54, No. 2, pp. 277–280. © Pleiades Publishing, Ltd., 2016.

Original Russian Text © V.M. Batenin, V.V. Kachalov, A.V. Kurilovich, V.Ya. Mendeleev, 2016, published in Teplofizika Vysokikh Temperatur, 2016, Vol. 54, No. 2, pp. 294–297.



Evolution of the Diffraction Pattern

of Probing Radiation Reflected
by a Silver Surface upon Melting
V. M. Batenin, V. V. Kachalov, A. V. Kurilovich, and V. Ya. Mendeleev
Joint Institute for High Temperatures, Russian Academy of Sciences, Moscow, 125412 Russia
e-mail: v_mendeleyev@list.ru
Received June 26, 2015

Abstract—Evolution of the diffraction pattern was studied experimentally using a sample of silver with a mod-
erately rough surface formed by the composition of predominantly unidirectional grooves. The sample was
heated in a tubular electric furnace; its temperature was determined by a thermocouple measurement. At a
temperature close to the liquidus temperature, the appearance of isotropically scattered radiation, concen-
trated near the specular beam, is detected. We analyzed the evolution of these radiation components upon
melting and showed that the nucleation is the source of isotropic scattering. It is found that the evolution of
the diffraction pattern enables one to observe the melting of the surface layer, accompanied by the simulta-
neous existence of the disappearing solid phase and the growing liquid phase. Spreading of the sample melt
over a substrate can be also observed with the diffraction pattern.

DOI: 10.1134/S0018151X16020024

INTRODUCTION studying the scattering of optical radiation from the

inhomogeneous surface [10].
Exposure of materials to intense radiation is a In this paper, we study experimentally the evolu-
promising field of research in solid state physics and in tion of the diffraction pattern of the probing radiation
the development of new methods of laser material pro- scattered by the surface of silver upon melting and
cessing. A typical process accompanying the intense analyze the causes of such an evolution.
radiation action is melting, which is actively studied by
optical methods based on determination of the optical
properties of the material by means of probing radia- EXPERIMENTAL SET-UP AND TEST SAMPLE
tion reflected by the surface. The melting of metals,
semiconductors, and insulators has been investigated This study was conducted in an air atmosphere on
experimentally by reflectometry (measurement of the an experimental set-up, the schematic diagram of
total reflectance and the specular reflectance) [1–4], which is shown in Fig. 1.
nonlinear optics (measurement of the intensity of sec- The set-up includes cylindrical high-temperature
ond-harmonic reflected radiation) [5], ellipsometry tube furnaces 1; platinum platinum–rhodium ther-
(determination of optical constants) [6], and monitor-
ing of images of the surface obtained in paraxial rays
[7]. It is assumed in the theoretical models [1, 2, 6, 7] 9 10 2
based on the experimental data that the spatial struc-
ture of the surface of the material does not change 4 5
during melting. However, melting associated with the
nucleation [8, 9] can lead to a spatially inhomoge- 6
neous surface changing over time. For this reason, the 7
experimental estimates obtained by these methods can 1
depend greatly on both the spatial structure of the sur-
face and the experimental conditions. In this connec-
tion, it is advisable to analyze the evolution of the spa- 8 3
tial structure of the sample surface caused by the for-
mation of a liquid phase upon melting. To solve this
problem, the diffraction method can be used for Fig. 1. Experimental set-up.

278 BATENIN et al.

t, °C surface roughness. Such a surface structure of the

963 sample was used to study the evolution of the solid
phase by the unidirectionally scattered radiation and
the evolution of the liquid phase by the specularly
reflected beam.
960 The thermograph of the test sample, obtained over
a time interval of 47 s at temperatures close to the
959 melting point of silver of 960.8°C [11], is presented in
Fig. 2. The average liquidus temperature of silver is
961.2°C. The standard deviation of the random error
958 of measurement of temperature at a specified time
interval does not exceed ±0.3°C; it is represented in
0 10 20 30 40 50 the graph in the range of 18–33 s. It is seen from Fig. 2
T, s
that, at this liquidus temperature and the measure-
ment error, melting may actually begin earlier than
Fig. 2. Thermograph of the silver sample near the melting follows from the thermograph. Note that in [12, 13],
point: characters are experimental data obtained by ther-
mocouple measurements. the nucleation was recorded before melting measured
by a thermocouple.
The evolution of the diffraction pattern of the radi-
mocouple 2 with analog-to-digital converter 3; laser ation reflected from the sample surface is shown in
source 4 of probing radiation; the channel for record- Fig. 3 in the same time interval (47 s).
ing the diffraction pattern of the probing radiation, A diffraction pattern identical to that obtained at
including screen 5, filters 6 and LightWaySystems room temperature was observed up to a temperature
video digital camera 7; and computer 8. Test sample 9 close to the melting point. In the temperature range
was put in a “dovetail” groove of nickel holder 10 and from 200 to 600°C, the intensity of radiation in the dif-
placed in the central zone of the furnace so that the fraction pattern decreased and then increased. This
surface of the sample was vertical. A thermocouple in behavior can be explained by the completion of the
a two-channel Al2O3 straw was mounted in a nickel oxidation processes on the sample surface at ∼600°C
holder and set with the hot junction to the back side of and the destruction of the oxide film at higher tem-
the sample. A semiconductor laser (DMO-100 ver1) peratures. From T = 23 s and on, three characteristic
was used as the source of probing radiation at a wave- intervals were observed in the evolution of the diffrac-
length of λ = 660 nm. The power of the probing radia- tion pattern observed: 23–27, 28–32, 33–37 s.
tion incident on the sample surface was ∼70 mW, and In the range of 23–27 s, there are a specularly
the angle of incidence was ∼5°. The diffraction pattern reflected beam, isotropically scattered radiation con-
of the probing radiation scattered from the sample sur- centrated in the vicinity of the specular beam, and uni-
face was formed on the screen and recorded by the directionally scattered radiation in the diffraction pat-
camera. The thermocouple signals that have passed tern. The divergence of the specular beam and the
the analog-to-digital converter and the signals of the contribution of isotropic scattering into the diffraction
camera enter the computer at the same time with an pattern increased, while the contribution of unidirec-
interval of 1 s. The duration of heating of the sample from tional scattering decreased.
room temperature to the melting point was ∼150 min.
The test sample of silver (99.9% Ag) had a thick- From time T = 28 s, the reflected radiation con-
ness of 0.5 mm and a size of the surface of 8 × 6 mm. sisted only of isotropically scattered radiation and the
The spatial structure of roughness of the surface specularly reflected beam of a random modulation
reflecting the laser light was formed by surface grind- shape. In the range of 30–32 s, the modulation
ing in the same direction. After grinding, the rough- decreased, and the size of the specularly reflected
ness was a composition of mainly unidirectional beam remained almost unchanged.
grooves. The standard deviation of the surface rough- From time T = 33 s and T = 37 s, the specularly
ness of sample σ, measured by a Talystep 1020 profilo- reflected beam became smaller and took a form close
meter, was 69 nm. The surface of the test sample was to a circle. Then, the reflected beam randomly
moderately rough [10], since the ratio of σ/λ ≈ 0.1. At changed its form and the reflected radiation com-
room temperature, the diffraction pattern of radiation pletely disappeared at T = 47 s.
reflected from the surface contained the images of an Given the results of thermocouple measurements
intense, specularly reflected beam of circular shape and based on the nucleation model of melting [9] and
and low-intensity radiation, unidirectionally scattered the diffraction theory of optical scattering from the
in the direction perpendicular to the grooves of the spatial inhomogeneities of the surface [10, 14], we can

HIGH TEMPERATURE Vol. 54 No. 2 2016


T=1s T = 23 s T = 27 s T = 28 s

T = 29 s T = 30 s T = 32 s T = 33 s

T = 37 s T = 47 s
Fig. 3. Evolution of the diffraction pattern of radiation scattered by the sample surface.

assume that the observed features of the diffraction The subsequent evolution of the beam shape in the
pattern in these three time intervals are caused by the range of 33–37 s can be explained by the silver melt
following. spreading over the nickel substrate. The surface curva-
In the range of 23–27 s, unidirectional scattering ture of the liquid phase decreased, and the divergence
mainly disappears and isotropic scattering increases. of the specularly reflected beam decreased corre-
The concentration of isotropically scattered radiation spondingly. The chaotic change in the beam shape
near the specularly reflected beam indicates that inho- (T = 47 s) and the disappearance of the reflected light
mogeneities do not constitute isotropically rough sur- were caused by the molten silver leaking off the nickel
face scattering the radiation hemispherically [10]. The
observed scattering is characteristic of inhomogene- substrate from the area illuminated by the probing
ities arranged randomly on the surface and having an light under the force of gravity. A photograph of the
average transverse dimension substantially greater molten sample in the nickel holder is shown in Fig. 4.
than the wavelength of the probing radiation [14]. Tak-
ing into account the results of thermocouple measure-
ments, one can assume that the nucleation sites of the
liquid phase are those surface irregularities that scatter
the probing radiation isotropically. Thus, in the specified
time interval, the diffraction patterns show the simulta-
neous existence of disappearing solid phase and growing
liquid phase in a surface layer of the sample. An increase
in divergence of the specularly reflected beam indicates
the beginning of coalescence of nuclei and increasing
surface curvature of the liquid phase.
Interference of waves formed by the diffraction of
the probing radiation at the fragments of the liquid
phase resulting from the coalescence of nuclei can be
regarded as a reason for the modulation of the specularly
reflected beam at T ≥ 28 s. In the range of 29–32 s, frag-
ments of the liquid phase coalesces and the spatial
structure of the surface became more uniform, thereby
reducing the specular beam modulation. The invari-
ance of divergence of the specularly reflected beam in
the range of 30–32 s can be attributed to the comple-
tion of melting of the surface layer and the beginning
of propagating of the melting wave into the sample. Fig. 4. Molten sample in the nickel holder.

HIGH TEMPERATURE Vol. 54 No. 2 2016

280 BATENIN et al.

CONCLUSIONS 3. Sokolowski-Tinten, K., Biakowski, J., and von der

Linde, D., Phys. Rev. B: Condens. Matter Mater. Phys.,
In the range of temperatures close to the melting 1995, vol. 51, no. 20, p. 14186.
point, we studied experimentally the thermograph of
the silver sample and the evolution of the diffraction 4. Bityukov, V.K., Petrov, V.A., and Smirnov, I.V., High
Temp., 2015, vol. 53, no. 1, p. 27.
pattern of the probing laser beam reflected from the
surface of the sample. At a temperature close to the 5. Tom, H.W.K., Heinz, T.F., and Shen, Y.R., Phys. Rev.
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scattered radiation is recorded in the diffraction pat- 6. Schmid, M., Zehnder, S., Schwaller, P., Neuenschwan-
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ACKNOWLEDGMENTS Physical Quantities: A Reference Book) Kikoin, I.K.,
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This work was supported by the Russian Founda- 12. Lyakhovitskii, M.M., Roshchupkin, V.V., Pokrasin, M.A.,
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