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Lasers in metallurgy and technology of inorganic materials (Review)

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1974 Sov. J. Quantum Electron. 4 564

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Lasers in metallurgy and technology of inorganic materials
(Review)
A. A. Uglov
A.A. Baikov Institute of Metallurgy, USSR Academy of Sciences
(Submitted November 12, 1973)
Kvant. Elektron. 1, 1037-1055 (May 1974)
A review is given of the applications of high-power cw and pulsed lasers in the
technology of inorganic materials, including local hardening, welding, cutting of metals
and dielectrics, film processing, drilling of holes, and so on. An analysis is made of
the potential applications of high-power cw lasers in metallurgical processes, including
preparation of refractory metals, remelting of high-temperature materials, growth of
single crystals, processing of powder materials, etc.
Lasers can be used in various technological processes
(cutting, welding, surface-hardening, hole drilling, etc.)
because of the special features of the interaction between
high-power radiation and matter. These features include
the precision of processing, high rates of heating and high
temperature gradients in the interaction zone, possibility
of local destruction of practically any material, simplicity
of control of the energy input, and so on. Lasers emitting
at different wavelengths can be used in a flexible manner
in processes with a variety of end products, including ini-
tiation of chemical reactions. Only electron-beam pro-
cessing and, partly, low-temperature plasma units can
compete with lasers in the universality of their processing
applications.
Some of the promising applications of laser radiation
occur in metallurgy. Various metallurgical processes in-
volve the synthesis of new and known materials, surface
oxidation, formation of protective coatings, decomposition
of complex compounds, chemical reduction in controlled
media, conversion and heating of gases, etc. The metal-
lurgical applications of lasers in industry have been less
developed than those in the technology of inorganic materials.
The review is divided into four sections, in accordance
with the various applications of lasers in technological
processes. In Sec. I (Introduction) we shall formulate the
main problems encountered in laser technology and metal-
lurgy. In Sec. II we shall consider the application of
pulsed lasers in technology, including heat treatment,
welding, and drilling of small holes. We shall also dis-
cuss film processing, radiation-initiated thermochemical
treatments, and several other applications. Section III
deals with the use of cw lasers. In this section we shall
consider particularly the welding and cutting of inorganic
and other materials by carbon dioxide laser beams. We
shall discuss the initiation of chemical and thermochem-
ical reactions in gases and on the surfaces of condensed
media. We shall consider briefly the laser separation of
isotopes. In Sec. IV we shall discuss potential applications
of lasers in metallurgy. The purpose of the review is to
identify the problems whose solution will help to extend the
range of practical applications of laser radiation.
I. INTRODUCTION
In the technology of inorganic materials, which in-
cludes the traditional material processing treatments (for
example, welding), an important role is played by heat
564 Sov. J. Quant. Electron., Vol. 4, No. 5, November 1974
sources located on the surface or in the bulk of a material
acted upon by a flux of particles (electron, ion, and photon
beams or low-temperature plasma jets or blobs, etc.).
The theory of the thermal phenomena which occur in
the zone of interaction between highly concentrated (flux
density q > 102 W/cm2) energy sources has been developed
to a considerable degree by N. N. Rykalin and his school,1'2
particularly for the processes of welding, and of mechan-
ical and heat treatments.
Laser radiation focused into a small spot of size r^
on the surface of a material opaque to a given wavelength
can raise the upper limit of the attainable flux density to
q > 1015 W/Cm2. This considerable increase in the energy
flux density (by four or five orders of magnitude compared
with the densities attainable for the older energy sources)
is frequently unnecessary. Moreover, it is sometimes un-
desirable. This is because the radiation incident on a ma-
terial interacts with the gaseous and liquid products of the
treatment. In this way, a considerable proportion of the
energy is wasted in increasing the temperature and kinet-
ic energy of the products of the treatment, which reduces
the effective efficiency of the process as a whole and re-
sults in a loss of precision of localization. Therefore, in
most technological processes, the upper limit to the flux
density is q ^ 109W/cm2. Only in some cases, when the
time of interaction is short (< 10"8 sec), is it desirable to
use radiation of q ^ 109 W/cm2 density.
The development of high-power cw lasers has raised
the possibility of their use in technology and metallurgy.
The advantages of lasers and other highly concentrated
energy sources in large-scale metallurgy include the con-
servation of the environment because — in spite of the
economic advantages of modern large-scale metallurgy
over the laser or even plasma metallurgy — the problems
of pollution of the environment by modern metallurgy re-
quire the development of new processes. These new pro-
cesses may result in a reduction of the pollution of the
atmosphere and oceans. These comments are applicable
to the future development of metallurgy in the next de-
cade or so.
It is useful to divide the existing high-power lasers
into two groups: These are the pulsed and cw lasers. The
concept of "high power" in the case of applications of
pulsed lasers in technology may, for example, mean that
during a pulse of r\ ~ 1 msec duration a zone of radius
Copyright © 1974 American Institute of Physics 564
r^ ~ 10~2 cm on the surface of a material reaches a tem-
perature close to its melting point. In the case of iron,
this definition applies to lasers which can provide power
densities q $ 104 W/cm2. The concept of "high-power" cw
lasers is more conveniently based on the assumption that
the radiation acts for an indefinite time. Then, in the case
of iron, a cw laser can be regarded as a high-power ener-
gy source if P ^ 10 W. We shall consider the principal
applications of the pulsed and cw lasers separately, but we
must remember that such a division is quite arbitrary.
II. APPLICATIONS OF PULSED
LASERS IN TECHNOLOGY
OF INORGANIC MATERIALS
1. H e a t t r e a t m e n t . The focusing of a laser
beam on the surface of a material opaque to laser radia-
tion results in the absorption of some part of the radiation
energy. The reflection coefficient R of a material depends
on the state of its surface (polished, ground, etc.), angle
of incidence of the radiation, temperature of the surface,
and density of the radiation flux. When heat treatments
are performed using radiation of q < 104 W/cm2 density,
we can assume approximately that R is independent of the
temperature and the intensity of the heat source on the
surface of the material is governed by the space—time
characteristics of the radiation. In a large number of
practical cases1'2 we can assume that the spatial charac-
teristics of pulsed laser radiation can be described by the
normal distribution law
q(f) = <7 0 exp(—
where q 0 is the intensity at the center of the heated spot;
r is the radial coordinate; k is the concentration coeffi-
cient related to the nominal spot radius ry- by
B is a constant which depends on a definition of
Knowing the temporal structure of a laser pulse al-
lows us to describe the action of radiation as heating by a
source of heat with specified parameters. Heating of sol-
ids not accompanied by phase transitions of the first kind
is usually called heat treatment. The purpose of heat
treatments is to alter the structure of a material in the
interaction zone by heating and subsequent cooling at a
definite rate.
In the interaction of radiation resulting in the forma-
tion of a definite heating zone, it is important to know the
main characteristics of the process which are the rate of
heating and cooling, time taken to reach a given tempera-
ture, temperature gradients and their distribution through-
out the treated material, and dimensions of the heat-treat-
ment zone. The difficulties encountered in the experimen-
tal determination of these parameters are very great, so
that calculation methods have become very important.
Since high radiation flux densities result in a high rate of
heating, the critical points Ac may shift during heating
toward higher temperatures3 and the shift may amount to
tens or hundreds of degrees (a critical point Ac repre-
sents the temperature of a phase transition of the second
kind, which occurs during heating and depends on the rate
of heating).
565 Sov. J. Quant. Electron., Vol. 4, No. 5, November 1974
The determination of the temperature field in the bulk
of a material can be regarded as the boundary-value prob-
lem in heat conduction subject to boundary conditions of
the second kind in linear or nonlinear formulation. In the
latter case, we can allow not only for the temperature de-
pendence of the thermal parameters but also for the vari-
ation of R with temperature. Since three-dimensional non-
linear heat transfer can be treated only by numerical cal-
culations, we shall consider briefly the relationships nec-
essary for the calculation of the parameters of heating
processes. It is worth noting that, in most technological
processes, one can ignore the finite nature of the rate of
propagation of heat.
For example, the time needed to reach the melting
point of a material Tm on the surface of a semiinfinite
body subjected to a source of heat with a normal distribu-
tion can be found from 4
rm = (4o£)-1tg (K -\^nkTm/q0). (3)
Here, \ is the thermal conductivity and a is the thermal
diffusivity.
In heat treatments of surfaces by laser radiation, it
is important to know the flux density which does not re-
sult in surface melting for given duration of a pulse and
for a given material. The critical flux density, qc can be
estimated from 4
(4)
The rate of heating of a semiinfinite body by a source
(1) of the type described by Eq. (1) is defined as the rate of
rise of the temperature of a given point v = 8T/9r and it
can be found from 78
? 0 exp [ — zV4at — r 2 /(4aT +
(5)
(2)
where z is the axial coordinate. Typical rates of heating
and cooling by laser radiation are much higher than the
corresponding rates used in quenching or even those used
in electric heating.
Knowing the laws governing the changes in the tem-
perature field we can derive the necessary heat cycle1'2
resulting in the required changes in the structure of the
zone of interaction and adjoining regions. The geometry
of a workpiece can affect considerably the distribution of
heat in the interaction zone. The influence of various fac-
tors on the temperature field and on the removal of heat
from the interaction zone are analyzed in a linear formu-
lation in refs. 4-9. Allowance for the influence of the tem-
perature dependence of the absorptivity on the kinetics of
heating is considered in ref. 10 for the one-dimensional
case. An analysis of the characteristic features of the
thermal effects of laser radiation is not always acceptable
without allowance for other factors because physicochem-
ical changes, including chemical reactions, can take place
on the surface of a material. Activation of these reactions
during heating in an oxidizing atmosphere may alter the
absorptivity and kinetics of heating. This problem will be
discussed in detail later.
Laser heat treatment can increase the microhardness.
The question of changes in the structure of materials, in-
cluding carbon-iron alloys, is discussed in detail in ref.
A. A. Uglov 565
11. The mechanism of this increase in microhardness is
related to the formation of nonequilibrium structures, gen-
eration of large numbers of dislocations because of con-
siderable thermal stresses, fragmentation of structure
blocks in the thermal influence zone, etc. Topochemical
reactions and the diffusion of nitrogen from the atmo-
sphere, resulting in the formation of nitrides, can play an
important role in such treatments.
In machine building it is very desirable to achieve lo-
cal hardening in those cases when a localized hard region
is produced in a relatively cheap material because this
reduces the cost of the final product. Important practical
applications include hardening of the cutting edges of
drills, cutters, and other machining tools. Surface hard-
ening can be produced by doping the liquid phase formed
in this way12 or without such doping. Work on these ap-
plications has started relatively recently and should even-
tually produce results suitable for adoption in industry.
2 . L a s e r w e l d i n g . Welding is one of the most
effective applications of lasers in technology. In laser
welding, one does not have to place the workpiece in vac-
uum (as has to be done in electron-beam welding) but the
process can be carried out in a controlled medium pass-
ing laser radiation through walls (windows) transparent
to a given wavelength. In view of the short duration of the
pulses, one can avoid damage to such heat-sensitive ele-
ments as p—n junctions and so on, and one can also avoid
distortion in welding of thin plates.
Laser welding methods cover a wide range, including
welding of thin-walled parts, wires to plates and larger
parts, wires to one another, etc. Investigations of the
mechanical properties of laser-welded parts have shown
that the strength of the welded joints is usually not infe-
rior to the strength of the bulk metal.13
Although laser welding is basically a melting process,
one can also visualize processes in which radiation ac-
tivates the surface, raising its temperature to values at
which the material does not melt but becomes plastic (sol-
id-state welding). A quartz or sapphire capillary can be
used to apply pressure to the parts being welded together.
The knowledge of the laws governing heating, which
are used in the selection of the parameters of the radia-
tion pulses, plays an important role in laser welding.
There have been many investigations of the characteristics
of heat sources and temperature fields in laser welding
but most have provided only estimates.14"24
Laser melting can be considered (like laser heat
treatment) as a problem of heat conduction in three di-
mensions with a specified surface source of heat. In de-
scribing the heating processes, considerable difficulties
are encountered in allowing for the thermal contact be-
tween materials of different kinds.18 Allowance for the
heat of melting complicates considerably the solution of
the problem because three-dimensional Stefan problems
can be analyzed only by numerical methods25 (the Stefan
problems are those involving calculations of the rates of
motion of the boundaries of phase transitions and of the
distribution of the potentials, including temperature, in
both phases; the Stefan problems are strongly nonlinear).
Experiments show that in the case of typical metals (steel,
566 Sov. J. Quant. Electron., Vol. 4, No. 5, November 1974
copper, etc.) it is important to allow not so much for the
heat of melting as for the occurrence of a situation in
which surface evaporation deforms the liquid phase and
the source of heat penetrates deeper into the material.26
The critical flux density qc, which does not result in a
significant deviation of the depth and shape of the molten
zone from that predicted by the linear theory of heat con-
duction, can be estimated employing a relationship similar
to Eq. (4):
qe = (6)
where TD is the boiling temperature under normal pres-
sure. For example, in the case of copper with T^ =
2300°C, we!have qc = 2 • 105 W/cm2. The experimental
values of qc are close to those found by calculation em-
ploying Eq. (6).
The kinetics of melting depends on the temporal struc-
ture of a laser radiation pulse. The splashing of liquid out
of the molten zone, which usually impairs the quality of a
welded joint, is due to several factors. They include ir-
regularity of the pulse (spike structure), insufficient clean-
ness of the materials being welded and their saturation
with gases, conditions of focusing of the incident radiation,
and contacts between the materials. The causes of splash-
ing of the liquid phase have not yet been investigated in
sufficient detail. The use of regular pulses or quasicon-
tinuous radiation27 increases the stability of the melting
process and reduces the probability of the formation of
defects in the welding zone. The spike structure of a pulse
may tend to cause deeper melting because of deformation
of the liquid phase.
The size of the thermal influence zone can be calcu-
lated allowing for the boundary conditions on free surfaces
and on surfaces in contact. In calculations relating to la-
ser welding, the assumption of a point source of heat may
result in considerable errors even if the size of the weld-
ing zone is only several tens of microns.28
Spot laser welding is used industrially in electronic
technology, microelectronics, instrument construction,
the watch and clock industry, precision machine construc-
tion, etc. It has to compete with other methods for joining
materials, which include electron-beam welding, heat-
compression welding and its various varieties, ultrasonic
welding, etc. However, in some cases, laser welding is
the only acceptable method becaus e of a combination of sev-
eral factors (the need to limit the thermal influence zone, im-
possibility of applying mechanical stresses, presence of
a closed volume, etc.). Spot laser welding can also be
used to produce welded seams if the repetition frequency
/ of separate pulses, producing a seam by a partial overlap
of the separate melting zones, is sufficiently high (f > 1
Hz). Laser welding can be performed not only when the
materials are in direct contact but also when they are sep-
arated by an easily fusible material (welding—soldering
operation) or through a spacer made of a material which
ensures the weldability of different materials, and so on.
The number of various laser melting methods is very large
but still does not cover all the various cases specific to
particular situations.
3. D r i l l i n g of s m a l l h o l e s . If q exceeds the
critical value for the onset of damage, a through or blind
A. A. Uglov 566
hole is produced. The physical processes which occur in
the interaction zone above the critical intensity are known
only qualitatively. In considering the interaction process
(i.e., in estimating temperatures, pressures, depth and di-
ameter of the damage zone or in evaluating the proportions
of the liquid and gaseous fractions in the ejected products,
etc.) in the q ^ 109 W/cm range, it is usual to employ the
thermal damage theory29 or the gas-dynamic theory of the
interaction between radiation and condensed media.30 In
spite of the different approach to the damage caused by
high-power fluxes, these two theories predict approximate-
ly the same results in the technological range of flux den-
sities (106-109 W/cm2). Neither of these theories gives
quantitative estimates because the thermal theory is lim-
ited to the one-dimensional approximation and ignores the
presence of the liquid phase on the surface of the material
(this is allowed for in ref. 31) and the gas-dynamic theory
is also limited to the one-dimensional approximation, ig-
nores the presence of the condensed medium, and is con-
cerned only with the motion of a plasma and its interaction
with the incident radiation.
In some estimates concerned with hole drilling, both
approximations are satisfactory only during the initial
stage of the interaction, when the process can be regarded
as one-dimensional.
Thus, there is practically no theory which can give a
consistent description of all the phenomena resulting from
the interaction of high-power radiation with metals and
other materials.
The formation of holes is accompanied by the ejection
of the liquid phase and, according to the thermal theory,
this is due to the melting—erosion mechanism. 29 The pres-
ence of various inclusions, dissolved gases, particles of
contamination, etc. in a material, which are all conse-
quences of the technology of preparation, may favor addi-
tional ejection of liquid and solid matter from the inter-
action zone.32"35 A preliminary hardening of a material
(for example, by quenching) also tends to increase the
proportion of the condensed material ejected from the
interaction zone.11'36
A physical analysis of the processes of interaction
between laser radiation and matter in the q~ 109 W/cm2
range predicts interesting consequences in the case when
the temperature exceeds the critical value. In drilling
holes a considerable increase in the flux density in milli- terial from the surface of an insulating substrate (making
second pulses is usually undesirable because of a consid-
erable enhancement of the interaction between the incident ment of nominal values) of resistors, etc. Although there
radiation and the ejection products. The screening of the
radiation by these products becomes considerable for
steels even for q ~ 105 W/cm2, i.e., in the "welding" range.
If q ~ 109 W/cm2, the hole drilling becomes ineffective be- laser radiation on film materials because the processes
cause of the strong screening. On the other hand, the
presence of a liquid phase on the walls of a hole, set in
6 2
motion by the interaction with radiation of q ~ 10 W/cm
intensity, is a frequent hindrance in precision drilling,
particularly in the case of materials with a high thermal
conductivity. Under these conditions, a drilled hole fills
up with a liquid during a pulse and the process is quasi-
periodic.37 The motion of the liquid phase frequently pre-
vents the formation of complex and noncircular holes be-
cause, after a time, the melting destroys the intended
shape of the hole.
567 Sov. J. Quant. Electron., Vol. 4, No. 5. November 1974
The solution to this problem in the precision drilling
of small-diameter holes is provided by many-pulse
treatment.38 In such treatment, the main parameter which
is controlled is the pulse repetition frequency, but there
are some industrial processes in which the energy of the
individual pulses is varied in accordance with a specified
program. Obviously, in order to obtain holes of specified
shape, depth, diameter, and surface finish, one has to
employ amplitude—frequency modulation of a train of
pulses. This method is already employed in other forms
of processing of very hard and refractory materials by
highly concentrated energy sources such as the electron
beam.
The drilling of a hole in a plate is usually accompan-
ied by changes in the composition and structure of the
material in the interaction zone.11'39 This is due to the
mass transfer processes, diffusion in liquid and solid
phases, differences between the vapor pressures of the
components of the material, etc. When holes are drilled
in steels of complex composition, it is usual to harden
such steels before drilling.40
We shall now mention some applications of laser hole
drilling in metal and dielectric plates. One of the prom-
ising applications of lasers is in the drilling of a large
number of holes of small diameter ( ~ 10~2-10~3cm), such
as are needed for the processing of ferrite plates used in
computer memory cells. The difficulties in this process
arise from the brittleness of ferrites and the appearance of
cracks due to thermal stresses.
The drilling of holes in various hard iron alloys which
are used in dies in the manufacture of chemical (synthe-
tic) fibers is one important application. It has been mas-
tered only partly: Only rough holes can be drilled by a
laser.38 The laser drilling must be followed by additional
grooving.
Another important application is the drilling of small
holes in ruby, diamond, and other hard materials em-
ployed in watches, clocks, and other industrial products.
4. F i l m p r o c e s s i n g . Laser radiation has also
important applications in the processing of thin films.
This type of processing is encountered in electronic tech-,
nology and microelectronics. The important tasks are the
preparation of photographic masks, removal of excess ma-
windows), recrystallization of films, 41 trimming (adjust-
are other ways of performing these tasks, the use of la-
sers promises to increase the efficiency.
We shall consider briefly only the thermal action of
of initiation of thermochemical reactions on the surfaces
of thin films are discussed elsewhere.
Radiation produced by free-oscillation and Q-switched
lasers is used in processing thin films. 42 The simpler
tasks, such as the trimming of resistors, can be performed
by removing a part of a film until the required value of the
resistance is reached. This process can be automated.
Another method for adjusting the values of resistors is to
alter the structure of the film by heating. The thermal
physics problems encountered in processing films by la-
A. A. Uglov 567
ser radiation are considered in refs. 43-46. Estimates
make it possible to specify the characteristics of a radia-
tion source needed for the performance of a given opera-
tion. Since the threshold density of the radiation flux re-
quired for the destruction of thin films is relatively low,
one can use gas,47 semiconductor, and other lasers.48'49
A projection method, suggested by V. P. Veiko and
M. N. Libenson,50 and some of its variants51 are among
the most promising. In the projection method, a workpiece
is placed in the plane of the image of a mask with a pre-
scribed profile which must be transferred to the work-
piece. The mask is placed between the exit objective of
the laser and the objective which transfers the image (to
the required scale) to the plane of the substrate carrying
the film. The main advantage of the method is that it can
be used to transfer a complex figure. Moreover, the re-
solving power is sufficiently high. The projection method
permits treating up to several square centimeters of the
surface simultaneously and the minimum size of an ele-
ment of a figure is ~ 1 /*. The main distortions in the film
are due to the melting of the boundaries of the figure, which
occurs when heat travels during the action of a pulse. A
radical method for avoiding such melting is to reduce the
duration of radiation pulses. Q-switched lasers are usual-
ly employed in the projection method.
5. Thermochemical processes initiated
by p u l s e d l a s e r r a d i a t i o n . The chemical inter-
action between laser radiation and matter may be due to a
variety of causes. They include: local heating, absorption
of photons by molecules which become dissociated or ion-
ized, or are excited to a level at which a reaction with an-
other molecule requires only a small activation energy,
all of which may happen without a significant rise of the
general temperature of the medium; excitation of radia-
tion—chemical transformations analogous to the processes
resulting from the passage of fast charged particles
through a medium which generate ions, radicals, and ex-
cited atoms and molecules; macroscopic heating of a me-
dium as a whole.
Surface thermochemical reactions initiated by pulsed
laser radiation are of considerable interest in various
branches of technology: These reactions include thermal
decomposition, oxidation and reduction of metals, and
synthesis of substances from simpler components. In
practice, such reactions alter the properties of the sur-
faces of bulk or film materials by changing the electrical
conductivity, 52 ' 53 mechanical strength,11 resistance to
chemical action, etc.
Surface thermochemical reactions proceed generally
as follows.54 A workpiece whose surface is subjected to
laser radiation is placed in a chemically active gaseous
medium. The laser radiation raises the temperature and
this activates a surface chemical reaction whose rate is
proportional to exp(—u/kT), where u is the activation en-
ergy of the process and k the Boltzmann constant. In the
subsequent stage, the rate of reaction is controlled to a
great extent by the rate of supply of the reagents via a
layer of the reacted substance (this is limited by diffusion)
rather than by the rate of the reaction itself.
Pulsed and continuous laser radiation provides a
promising means for surface chemical (topochemical) re-
568 Sov. J. Quant. Electron., Vol. 4, No. 5, November 1974
actions on substrates of materials of the type used in
electronic technology and microelectronics. In this case,
it is usual to combine laser illumination and subsequent
chemical treatments.
We shall consider some examples of the use of such
thermochemical reactions. One of the simplest reactions
is thermal decomposition.54 The original substance in
the form of, for example, a suspension is deposited on a
substrate heated by laser radiation within the desired area
by the projection method. The flux density is selected so
as to ensure a temperature sufficient for the decomposi-
tion of the substance throughout the thickness of the sam-
ple. The flux density should be within the range q j < q <
q2, where q2 is the flux density causing the evaporation of
the material and q t is the flux density at which the tem-
perature of the material at the contact with the substrate
reaches the decomposition temperature.
Oxidation of the surfaces of materials by focused
pulsed laser radiation is considered in the case of chrom-
ium in ref. 54. The growth of an oxide film was analyzed
in ref. 54 by the Cabrera-Mott theory.55 A characteristic
feature of the oxidation and the majority of other hetero-
geneous reactions is that the formation of a thin surface
layer of the reaction products is followed by later stages
governed by the rate of diffusion rather than the rate of
the chemical reaction proper. An estimate of the thick-
ness of the chromium oxide film obtained in ref. 54 was in
good agreement with the experimental results for pulses
up to 0.6 msec duration. Veiko et al.54 also oxidized with
laser radiation alloys such as Fe—Ni—Co and Cr—SiOand
studied thermal decomposition of copper formate (HCOO)2 •
Cu. To obtain a film of copper on a substrate, Veiko et
al. dissolved copper formate in ethylene glycol and mixed it
with an easily fusible enamel before depositing on the
surface of a glass-ceramic substrate. The sample was
then illuminated with laser radiation. At 295-325°Cthe
formate was decomposed and the volatile components
driven off so that a film of copper formed at the sur-
face. The unreacted residue was washed away in water.
The thickness of a film of copper produced in this way was
less than 1/ji.
Studies of surface reactions under the action of laser
radiation are still in their early stages.
6. Other a p p l i c a t i o n s of pulsed lasers
in t e c h n o l o g y . Large numbers of vacancies and dis-
locations can be generated in a surface layer of a material
by applying giant laser pulses. Such defects enhance the
diffusion coefficients of many substances. Since the ac-
tion of giant laser pulses lasting several tens of nanosec-
onds gives rise to explosive phenomena accompanied by
the propagation of shock waves into the bulk of a sample,
the effect can also be used for the hardening of materials.
Investigations of the practical use of giant laser pulses
for technological purposes other than film processing are
still in the laboratory stage.78
It is worth mentioning the possibility of using pulsed
lasers in the precipitation of thin films. Here again, there
are some difficulties associated with the phase composi-
tion of the products of damage which include a consider-
able proportion in the form of liquid drops. One of the
methods for reducing the liquid phase content in the ejec-
A. A. Uglov 568
tion products is to use quas[continuous radiation which
results in "gentle" heating. Some of the other technolo-
gical applications of lasers are mentioned in ref. 79.
It is appropriate to ask what new contribution has
been made by lasers to the technology of inorganic ma-
terials. The answer lies in a comparison of the "prelaser
era" in technology with the achievements in the last 10 or
12 years from the moment of appearance of the first
"technological" lasers. Lasers have made it possible to
tackle a number of tasks which have been impossible up
to now. They include microwelding inside enclosed spaces,
formation of local regions with a very high microhardness,
drilling of small holes in very hard materials, etc. The
most important achievements of laser technology have been
recorded in those cases in which traditional processing
methods are highly labor-intensive. The main achieve-
ments of laser technology also include the stimulus it has
given to further improvements in other processing meth-
ods. This has resulted both from competition posed by
the laser and from a better understanding of the physics
of the processes in the zones of interaction between highly
concentrated energy sources, which have many features
in common irrespective of the nature of the source.
III. APPLICATIONS OF CW LASERS
1. C O 2 l a s e r w e l d i n g . Gas-dynamic and elec-
tric-discharge CO and CO2 lasers, whose theory and prac-
tical construction have been investigated intensively in
many countries, are characterized by high output powers
of tens of kilowatts under continuous operating conditions.58
The radiation of these lasers focused into a small spot can
be used in large-volume processing of metals or ceramics.
A characteristic of lasers emitting at X = 10.6 n is
the high coefficient of reflection of metallic materials and
the low coefficient of the majority of dielectrics. The ab-
sorptivity of metals can be increased by a suitable surface
treatment, oxidation, deposition of a thin nonmetallic film,
and so on.56 The high absorption at the wavelength of 10.6
H causes difficulties in the selection of the optical mate-
rials used in focusing the radiation.
The spatial distribution of the intensity of CO2 laser
beams can be described by a diffraction curve.57 There-
fore, the thermal processes under the action of such
beams can be described using the normal distribution given
by Eq. (1). For an average power of 102-104 W and a fo-
cusing spot of ~10~2 cm2 area, the flux densities are q0 »
103-105 W/cm2 for metals and q0 » 104-106 W/cm2 for di-
electrics. At these flux densities we can consider heating
by applying the theory of concentrated heat sources.1
It is worth noting the special characteristics of the
interaction of the CO2 laser radiation with metals in ox-
idizing atmospheres. The surfaces of most metals carry
a thin oxide film whose thickness has a strong influence
on the absorption coefficient. This coefficient increases
with the oxide film thickness. Therefore, the process of
heating such metals as iron in an oxidizing atmosphere
can be divided into two stages.80 In the initial stage, when
the oxide film is still thin, the heating is relatively slow.
Beginning from a time r*, when the process of oxidation
becomes considerably accelerated, the rate of heating
rises strongly (second stage). During the first stage, the
569 Sov. J. Quant. Electron., Vol. 4, No. 5, November 1974
action of the CO2 laser radiation is practically indistin-
guishable from the action of such heat sources as an elec-
tric arc. In the second stage, we must allow for the change
in the absorption coefficient due to the growth of the oxide
film.
When high-power laser radiation reaches a metal, a
cloud of ionized vapor usually forms above the surface and
this cloud screens the interaction zone from the incident
radiation.58 This effect occurs only above a certain power
threshold and it prevents the appearance of deep molten
zones. The screening can be prevented by blowing away
the cloud with a gas jet, which can be directed parallel or
normal to the surface which absorbs radiation.
The screening of the zone of interaction between the
CO2 laser radiation and matter is also observed in the
case of dielectrics and, because of the molecular nature
of the absorption, the screening appears at lower power
densities. For example, experiments59 on the action of
CO2 laser radiation of q ~ (0.5-2) • 104 W/cm2 density on
quartz glass, optical glasses of the TF-5, K-8, and LK-5
grades, neodymium glass of the KGSS-7 grade, glass ce-
ramics, and other materials have demonstrated the oc-
currence of evaporation pulsating at an irregular frequen-
cy of 5-10 Hz. The pulsating nature of the development of
a crater on the surface is due to the competition between
two processes, which are the expansion of the gaseous
phase and the screening of the incident radiation.
Continuous high-power laser radiation can also be
used in seam welding. When the radiation power is in-
creased, the depth of the molten zone increases and this
makes it possible to increase the rate of welding. In many
respects, the properties of seams welded with the CO2 la-
ser radiation are similar to those of the seams obtained
using electron-beam units. In particular, gas-dynamic
lasers can produce deep molten craters in metals with
high values of the ratio h/d, where h is the depth of the
crater and d is its diameter. The results of a study of the
interaction between the radiation emitted by a gas-dynamic
laser (20 kW) or an electric-discharge laser (8 kW) with
steel are described in ref. 58. When the gas-dynamic la-
ser was used, the rate of welding of steel plates was 2.1
cm/sec, the depth of the molten craters was 1.9 cm, and
the ratio h/d was 6. The depth of the craters decreased
to 1.27 cm when the rate of welding was increased to 4.2
cm/sec. An almost complete melting of a steel plate
~ 0.95 cm thick was achieved at a welding rate of 1.27
cm/sec when the electric-discharge laser was used. When
this rate was increased to 1.7 cm/sec, a welded seam
could be produced by the complete melting of a steel plate
0.635 cm thick. If, by analogy with ref. 58, we were to
introduce the concept of efficiency e as the ratio of the
power required solely for the melting of the material to
the total radiation power (allowing for the heat-conduction
losses), we would find that e«= 45% for the 20-kW gas-
dynamic laser and e «= 28% for the 8-kW electric-dis-
charge laser. A reduction in the power of the electric-
discharge laser to 3.8 kW reduced e to 22%.
Estimates show that in order to melt 1 cm of a ma-
terial, one would require 4 kW for stainless steel, 14 kW
for low-carbon steel, 16 kW for aluminum, and 60 kW
for copper. Welding involving deep melting can also be
achieved at lower powers but the efficiency is less.
A. A. Uglov 569
 Welding with CO2 laser radiation is usually carried
out supplying argon to the interaction zone (the argon jet
is at right angles to the surface or parallel to it). The
strongest melting is achieved when the argon jet is normal
to the interaction zone but, in this case, the welding seam
becomes longitudinally inhomogeneous and may have dis-
continuities. When the argon jet is parallel to the surface,
a narrow continuous seam with homogeneous properties
along its length is obtained.
If the process of formation of a narrow and deep
channel in a material is ignored, we can describe seam
welding using the theory of moving heat sources.1*2 In
particular, the simplest model for the description of deep
melting of thick materials is the thermal model of a linear
source of heat moving at a constant rate across a material.
It is interesting to estimate the minimum radiation
power needed to melt the material. If we assume that the
Hagen—Rubens relationship56 applies to polished metals,
we find that the power Pm (for X = 10.6 IJL) is given by
where TJ is the dc resistance at the melting temperature
Tm. Estimates based on Eq. (7) give Pm = 200 W for ti-
tanium, 200 W for stainless steel, 300-400 W for iron and
zirconium, and 9-10 kW for copper and silver.
Obviously, the development of high-power cw tunable
lasers would make it possible to increase considerably the
efficiency of laser welding.
2^. C u t t i n g of m a t e r i a l s . The processes of
separation of materials1) are among the most promising
applications of high-power cw lasers. For this reason,
the number of foreign patents on laser cutting is larger
than the number of patents for any.other technological
processes utilizing laser radiation. It is usual to employ
the CC-2 and yttrium aluminum garnet (YAG) lasers in
cutting. The CO2 lasers are most effective in such ap-
plications and the efficiency of these applications is high
(~ 15-20%); moreover, the X = 10.6M radiation is ab-
sorbed by a large number of materials, including metal
oxides, glasses, ceramics, quartz, natural organic mate-
rials (wood, leather, etc.), synthetic materials, plastics,
and so on. The cutting process can be automated to obtain
complex shapes.
Thermal cleaving results from the generation of
stresses and microcracks in a material, followed by frac-
ture along the line of action of a heat source. The process
is, to some extent, analogous to the cutting of glasses or
6, mm m/min 8, mm m/min 6. mm M/M'HH 8, mm m/min 0, mm m/min
Material
100 W 200 W
Steel:
low-carbon 1.0 1.6 4.75 0.635 0.5
stainless 1.0 0.94 0.46 0.635 0.5
Titanium - - 0.51 0.203* 0.6
Wood
17,5 0.203 18
Glass 0.38 0. 10 4.0
Plexiglas . — 25.4
Quartz —
1 .2 0.5
Ceramic — — — —
Rubber —. 0
2 —
1.9 — — — —
— — — —
570 Sov. J. Quant. Electron., Vol. 4, No. 5, November 1974
ceramics by scratching the surface of a material with a
diamond cutter, followed by the application of mechanical
forces to produce fracture.
Cutting a material usually requires the application of
a jet of gas to the cutting zone. This jet helps to remove
the cutting products, which are dangerous in the case of
inflammable materials, such as cardboard, etc., and it
initiates the chemical reaction in the zone of interaction
between the laser beam and metals. Neutral gases are
used for the removal of chemical reaction products and
oxygen is used for the initiation of reactions.
Laser beam cutting combined with an oxygen jet (gas-
jet laser cutting) was proposed by Sullivan and Hould-
croft.61 The cutting aided by an oxygen jet is analogous to
the oxygen—acetylene cutting in which an exothermal chem-
ical reaction is used as the source of a considerable pro-
portion of the energy. A focused radiation replaces an
oxygen—acetylene flame as the source of heat for heating
the metal to the chemical reaction temperature. The la-
ser beam is a more strongly concentrated source of ener-
gy and this reduces the width of the cut as well as the di-
mensions of the thermal influence zone, and makes it pos-
sible to cut materials faster than by any other method.
The width of the cut is close to the diameter of the
heating spot in the focal pane, or it can be somewhat
smaller, whereas the size of the thermal influence zone
is 0.05-0.2 mm. When the laser power is increased, the
rate of cutting increases; this rate also depends strongly
on the thermal properties of the material and the thickness
of the sheet being cut. When the power is 300-500 W, the
rate of cutting of such materials as steel or titanium may
reach several meters per second but it is still insufficient
for the cutting of materials with a high thermal conductiv-
ity such as copper or aluminum. However, at power levels
of 15-20 kW it is also possible to cut copper and aluminum
and this can be done without a gas jet in the cutting zone.58
Table 1 gives information on the rates of cutting of vari-
ous metals and other materials of different thicknesses
using lasers of different power outputs.58'62'65
Cutting with a cw laser beam aided by a neutral gas
jet is particularly effective in the case of brittle and easily
flammable materials (ceramics, glasses, plastics, paper,
wood, etc.), which absorb strongly the X= 10.6/n radiation.
We shall now consider in a simple manner the process
of cutting by a cw laser beam. A heat source, equivalent
to the action of the laster beam, can be represented by a
point or normally distributed source.66
o,
P. kW
250 W 850 W >1 kW |
0.63 2,2 1.8 6,3 2.3 15
2.6 9 0,36 4.7 1 .27 20
0.2* 0.5 3.24
- - -
0. 1 0.25 4.5"
0.1* 9.5 1.52 20
1.52 8
—
6.5 0—
.6»«
— — — —
— — —
A. A. Uglov 570
 The source moving on the surface of a plate at a con-
stant velocity heats the plate and, if the velocity v is high,
the temperature can be found from 67
PL exp
where t0 = (1/4)ak; a is the thermal diffusivity, y is the
density; 6 is the thickness of the plate; PL is the laser
power.
If the interaction zone is subjected to a jet of gas
which initiates a chemical reaction, the zeroth approxima-
tion for the power P of a heat source equivalent to the ac-
tion of the laser beam gives66
P = PL + PC~&P,
where PC is the additional power due to the chemical re-
action and AP is the power removed by the gas jet.
The minimum power Pm of a heat source can be found
using the relationship
:A&) !4 >
where T 0 is the damage temperature.
The efficiency of laser cutting can be improved when
we understand better the processes taking place during
cutting and develop computation models which allow for
the motion of the liquid phase and for the interaction be-
tween the gas jet and the molten material.
3. Initiation of c h e m i c a l and t h e r m o -
c h e m i c a l r e a c t i o n s . Continuous laser radiation can
be used for the initiation of surface chemical and thermo-
chemical reactions. In this case, its interaction with con-
densed media is similar to the action of laser pulses.
We shall consider briefly some general aspects of the
activation of chemical reactions in gases by laser radia-
tion.68'69 A chemical reaction can be due to different
causes, depending on the intensity and the wavelength of
the laser radiation and the state of the medium. In parti-
cular, we can have photochemical or thermal reaction
mechanisms which are interchangeable.
The initiation of a chemical reaction requires not only
translational but also vibrational and rotational energies.
During later stages the vibrational energy of molecules
predominates. Therefore, a basically new approach to the
problem of chemical transformations can be made by in-
fluencing not the molecule as a whole but its individual
bonds. Then, molecules with temperatures of the excited
vibrations amounting to several thousands of degrees can
take part in selective chemical reactions.
The selectivity of laser radiation is based on two main
factors: 1) the selective excitation of some energy states;
2) the selective excitation of a mixture of substances which
can absorb radiation. Lasers open up new possibilities
associated with the excitation of vibrational levels because
other light sources do not have the required spectral den-
sity of infrared radiation. The high monochromaticity of
the radiation should make it possible to influence selec-
tively one level. Laser-chemical reactions of this type
should be characterized not only by selectivity but also by
a large difference between the vibrational and translation-
al temperatures.
571 Sov. J. Quant. Electron., Vol. 4, No. 5, November 1974
It was pointed out in ref. 70 that laser-chemical re-
actions differ from the reactions involving equilibrium
molecules and can be regarded as a new type of reaction
of selectively excited molecules. This suggests ways of
(8) controlling chemical reactions by exciting the required
bonds in a molecule and localizing the excitation up to the
moment of simple reaction.
Photochemical laser reactions involve the appearance
of bleaching and screening waves at high radiation intensi-
ties. The action of continuous laser radiation on gases
may result in the propagation of supersonic perturbations
in the form of traveling chemical-reaction zones, known
as photochemical waves. 71 ' 72 Basov et al. 73 investigated
the chemical behavior of mixtures of N 2 F 4 and SF6 with
(9) various gases (NO, CF 4 , C 2 F 6 , N2, and N20) absorbing the
CO2 laser radiation. Basov et al. also studied the behav-
ior of the same gases mixed with absorbing compounds
BC13, PF5, and SiH4. All the investigated laser-chemical
reactions occurred at explosive rates and were accom-
panied by the emission of light. The composition of the
reaction products was quite different from that obtained
(10) by the conventional heating of gases. Karlov et al. 75 re-
ported the initiation of a chain reaction in a mixture of
BC13 and H2 gases resulting from a multistage dissocia-
tion of the BC13 molecules under the action of the CO2
laser radiation. The dissociation of the BC13 molecules
resulted in the detachment of boron atoms and the appear-
ance of atomic chlorine, which initiated the chain reaction.
Equilibrium heating of a gas with laser radiation pro-
duces the same chemical transformations as equilibrium
heating by any other method. In the case of resonant ab-
sorption of radiation in vibrational transitions, a gas can
be heated to ~ 1000°C in a fraction of a second even when
the flux density is only q ~ 102 W/cm2. The difference be-
tween such heating and the conventional process is that the
energy is supplied along one channel of vibrations which
are excited by the laser beam and is then transferred to
other degrees of freedom. This aspect of resonant ab-
sorption may be of interest in metallurgical processes.
The resonant absorption of radiation of a certain
wavelength can be used to separate isotopes. We shall
consider briefly only the principle of such separation. The
process involves selective excitation of molecules in a
mixture of gases. Such a mixture contains two or more
types of molecule and when these molecules are excited
by laser radiation they can participate in chemical reac-
tions. One of the molecules contains an element with dif-
ferent isotopic abundances. The presence of isotopes re-
sults in a difference berween the energy states of chem-
ically identical molecules. Therefore, the laser-radia-
tion-excited components of the required isotopic composi-
tion enter selectively into a chemical reaction and are
thus removed by "burning" from the mixture of gases.
The task of isotope separation then reduces to the separa-
tion of different chemical compounds which is much sim-
pler. In principle, we can "burn out" separately different
components with a given isotopic composition by varying
the illumination wavelength.
Investigations of laser chemistry, which have started
only relatively recently, have yet to produce a method
suitable for direct application in industry. However, there
is no doubt that such investigations are likely to be very
A. A. Uglov 571
valuable. One of the main problems in the future laser
chemistry is likely to be the requirement of a high output
from a single unit, which would need the development of
lasers capable of producing high powers continuously.68
This difficulty also faces laser metallurgy.
IV. HIGH-POWER LASERS IN METALLURGY
One of the fundamental tasks of modern industry is
the production of metals and alloys with different physical
properties for different purposes. Potential applications
of lasers in metallurgy arise from the high power of con-
tinuous radiation, localization of the interaction zone, and
universality of lasers as heat sources.
At the present stage, the tasks in laser metallurgy
should be very similar to the corresponding tasks of plas-
ma metallurgy, 76 subject to allowance for the special fea-
tures of the interaction of laser radiation with matter. Al-
though the power available as continuous laser radiation
(~ 10-100 kW) is less than the power which can be obtained
from plasma jets (~ 1-10 MW) and the efficiency of laser
units (~ 20%) is much lower than the efficiency of low-
temperature plasma generators (~ 70%), the potential ad-
vantages of lasers are the ability to reach higher temper-
atures and, consequently, higher pressures. Moreover,
laser radiation power can be transferred directly to the
material being processed by photon absorption or via a
plasma cloud and not only by a gas heated in a plasma jet.
The efficiency of the utilization of lasers in metal-
lurgy can be checked in the same processes which have
been considered in the first investigations of the applica-
tion of low-temperature plasma generators, i.e., the prep-
aration of refractory materials by reduction of oxides and
chlorides,reduction and oxidation of sulfides of nonferrous
metals, oxidation of chlorides, synthesis of nitrides, car-
bides, oxides, hydrides, powders of composite materials,
etc.
In Sec. Ill we have considered some aspects of the
resonant interaction between laser radiation and a gas or
a mixture of gases, which are specific to lasers. The
resonant action of radiation on chemical bonds should make
it possible to perform metallurgical operations at low tem-
peratures but in the required direction. Such an interac-
tion can occur in the presence of one or more reagents in
the gaseous phase. We shall now consider briefly the met-
allurgical processes which can be produced by the resonant
interaction of radiation with matter.
Metallurgical processes involving gaseous media can
be divided into three groups: 1) reactions in the gaseous
phase; 2) oxidation—reduction reactions involving gases
and condensed media; 3) synthesis processes accompan-
ied by the formation of new phases.
The first group includes the processes of conversion
of sulfide gases and conversion of natural, producer, and
water gases, and so on.76 They can be initiated by raising
the temperature to a suitable level in the presence of het-
erogeneous catalysts. Oxidation—reduction reactions (sec-
ond group) occur under the catalytic influence of the sur-
face of a condensed medium and of reaction products. The
catalytic effect of the reagents is of little importance in
the synthesis reactions (third group).
572 Sov. J. Quant. Electron., Vol. 4, No. 5, November 1974
A small numbe'r of gases (including oxygen, hydrogen,
CO, chlorine, nitrogen, CO2, SO2, SO3, H2O, CH4, and am-
monia) is used in ferrous and nonferrous metallurgy. The
activation of metallurgical processes with the aid of these
gases is possible because of the resonant excitation of the
gas molecules whose vibration frequencies lie in the in-
frared range (the corresponding wavelengths are 2-20 M)«
Laser radiation can be used to prepare high-purity
materials by decomposing carbonyls and organometallic
compounds. These processes can be realized technically
in a great variety of ways. In particular, it seems prom-
ising to use a suspended layer of powdered material which
is penetrated by a laser beam. In this way, it should be
possible to treat powder materials of particle size (~ 10~2
cm) exceeding the radiation wavelength.
Applications of lasers in metallurgy may encounter
the problem of "windows," i.e., the problem of the intro-
duction of radiation into an enclosure with a controlled
atmosphere at a given pressure because the number of
materials which satisfy the conditions of mechanical
strength and low absorption at X = 10.6 n is very limited.
One of the possible ways of solving this problem is to de-
velop high-power tunable lasers.
Estimates show that one of the urgent tasks would be
the development of high-power cw lasers with an output
power in the range ~ 102-103 kW.
Other possible applications of laser radiation in met-
allurgy involve the use of beams as highly concentrated
heat sources. For example, remelting of refractory met-
als or of high-temperature ceramics should be possible
by analogy with plasma or solar heating. This is required
in the refining of materials and improvement of their prop-
erties. One of the advantages of laser melting might be
the attainment of high temperatures for a relatively small
power input, flexibility in control of the flux density, and
ability to carry out the process in a wide range of pres-
sures of the ambient medium (up to tens of atmospheres).
However, we must remember that at high pressures the
interaction zone may be screened by a plasma cloud.
High-power laser radiation can also be used as a
heat source in the growth of single crystals of refractory,
rare-metal, semiconducting, and other materials, as well
as in the zone refining of materials. For example, a unit
for growing barium and strontium crystals is described
in ref. 77: A hot zone is produced by heating with the CO2
laser radiation of over 1 kW/m specific power.
Laser radiation can be used in the fabrication of com-
posite materials by one of the methods in which one or
more substances have to be evaporated and then condensed
on the required surface, which may be a bundle of fibers.
Further development of cw lasers may result in in-
teresting metallurgical applications involving the resonant
interaction between radiation and gaseous media or in-
volving thermochemical reactions. Therefore, one of the
main requirements, apart from the high power, is the tun-
ability in the wavelength range 2-20 ^. There are as yet
no such tunable lasers.
separation of materials is the process of obtaining two or more parts
A. A. Uglov 572
 36
from a single piece. The separation in which part of the original material N. N. Rykalin, A. A. Uglov, and A. N. Kokora, Fiz. Khim. Obrab. Mater.,
is lost will be called cutting and the separation without such loss will be No. 6, 14(1972).
37
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sented at Scientific-Technical Conference on the Use of Lasers in Modern
X
Science and Technology [in Russian], Znanie, Leningrad (1973), p. 14.
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2
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A. A. Uglov, A. N. Kokora, and M. A. Krishtal, Fiz. Khim. Obrab. Mater.,
3
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6
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8
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9
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10
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U
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12
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13
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14
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15
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16
Yu. N. Lokhov, G. V. Rozhnov, and I. L Shvyrkova, Fiz. Khim. Obrab. S
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18
N. N. Rykalin, A. A. Uglov. and N. I. Makarov, Dokl. Akad. Nauk SSSR, 55
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34
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