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journal homepage: www.elsevier.com/locate/optcom
∗ Corresponding author at: State Key Laboratory for Manufacturing Systems Engineering, Xi’an Jiaotong University, Xi’an 710054, China.
E-mail address: xsmei@xjtu.edu.cn (X. Mei).
https://doi.org/10.1016/j.optcom.2019.124384
Received 27 April 2019; Received in revised form 5 July 2019; Accepted 13 August 2019
Available online 17 August 2019
0030-4018/© 2019 Published by Elsevier B.V.
Z. Yan, X. Mei, W. Wang et al. Optics Communications 453 (2019) 124384
2. Mathematical model
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Z. Yan, X. Mei, W. Wang et al. Optics Communications 453 (2019) 124384
Table 1
Thermal and optical properties of titanium [52].
Parameter Value
Density (solid/liquid) 4506/4110 [kg/m3 ]
Melting point 1941 [K]
Boiling point 3533 [K]
Heat capacity (solid/liquid) 25.06/37.68 [J/(mol K)]
Thermal conductivity (solid/liquid) 21.9/15.24 [W/(m K)]
Latent heat (melting/evaporation) 14.15/425 [kJ/mol]
First ionization potential 6.823 [eV]
Second ionization potential 13.583 [eV]
Emissivity 0.49
Viscosity (liquid) 5.2 [m Pa s]
Surface tension coefficient (liquid) −0.26 [m N/(m K)]
Complex refractive index (wavelength = 1064 nm) 3.5+4.02i
𝜕𝛾 𝜕𝑇
𝜎⃖⃗ = 𝜏⃖⃗. (4)
𝜕𝑇 𝜕⃖𝜏⃗
where 𝑝𝑒𝑣𝑎𝑝 , 𝜌𝑣 , and 𝑢𝑜𝑢𝑡 are the pressure, density and velocity of
the gaseous material at the interface of gas and target, respectively.
Furthermore, 𝜕𝛾∕𝜕𝑇 is the surface tension temperature coefficient of
material and 𝜏⃖⃗ is the tangent vector of the surface.
The gas region mainly contains two species, namely the titanium
vapour and the ambient atmosphere. The equation for each species was
solved to track the distribution of titanium vapour species in the back-
ground atmosphere [28]. The calculated results are used to evaluate
the plume attenuation coefficient of laser and the recoil pressure of the
target. The governing equation of the gas region is given by Eq. (5).
𝜕𝜌𝑔
⃖⃖⃗) = 0
+ ∇ ⋅ (𝜌𝑔 𝑈
𝜕𝑡
𝜕𝜌𝑣
Fig. 4. Time evolution of the target surface’s central point temperature with different
⃖⃖⃗) = 0
+ ∇ ⋅ (𝜌𝑣 𝑈
𝜕𝑡 (5)
laser fluences (2, 4, 8 and 12 J/cm2 ). The dashed line presents the normalized laser
𝜕𝑉⃖⃖⃗
power density. 𝜌( ⃖⃖
⃗ ⃖⃖
⃗
+ ∇ ⋅ (𝑈 𝑈 )) + ∇𝑝𝑒𝑣𝑎𝑝 = 0
𝜕𝑡
𝜕𝑇 ⃖⃖⃗𝑇 )) − ∇ ⋅ (𝑘∇𝑇 ) = 0.
𝜌𝐶𝑝 ( + ∇ ⋅ (𝑈
𝜕𝑡
where 𝑉 ⃖⃖⃗ is the velocity of material, resulting from the evaporation
where 𝜌𝑔 , 𝜌𝑣 , 𝑚𝑔 , and 𝑚𝑣 are the density of ambient gas, density of
and the flow of melt material, and 𝜌, 𝜇, 𝐶𝑝 and 𝑘 are the mass titanium vapours, molecular mass of the gas and molecular mass of
density, viscosity, specific heat, and thermal conductivity of titanium, the titanium vapours, respectively. The mixture’s density is defined as:
respectively. The temperature dependence of mass density, viscosity, 𝜌 = 𝜌𝑔 +𝜌𝑣 . Furthermore, 𝑈 ⃖⃖⃗ is the velocity in the gas region. In addition,
specific heat, and thermal conductivity in the simulations were given the total pressure is determined using: 𝑝𝑒𝑣𝑎𝑝 = (𝜌𝑣 ∕𝑚𝑣 + 𝜌𝑔 ∕𝑚𝑔 )𝑘𝑇 .
by Eq. (S17)–(S20) in supplementary Information [50]. Due to the fact When the vapour molecules leave the target surface, the velocity
that laser energy obeys the Gaussian distribution in time and space distribution will transform from a non-equilibrium to an equilibrium
domains [51], the heat conduction equation’s boundary conditions are distribution within a thin layer, which is the so-called Knudsen layer
given by Eq. (2). (KL) [15,53]. Since the thickness of the Knudsen layer is only a few
nanometers, it can be treated as a discontinuity in the thermal model.
𝜕𝑇 ||
+∞
4(1 − 𝑅)𝐼0 2𝑟2 𝑡2
𝑘 = √ exp[− − (4 ln 2) − 𝛼(𝑟, 𝑧)𝑑𝑧]
𝜕𝑛 ||𝛤 2 2 ∫ The temperature, density and other parameters of the material will
𝑡𝑝 𝜋∕ ln 2 𝑟0 𝑡𝑝 𝑧
have a jump across the KL. The jump boundary conditions of the
− 𝑢𝑠 𝜌𝐿𝑒𝑣 − ℎ(𝑇 − 𝑇𝑒𝑛 ) − 𝜀 ⋅ 𝜎(𝑇 4 − 𝑇𝑒𝑛
4
). (2) Knudsen layer are given by Eq. (6) [16,18,54].
√ 2
where 𝐼0 is the laser fluence, 𝑅 is the reflection coefficient, 𝑟0 is the 𝑇𝑣 ⎡ √ (𝛾 − 1)𝑠 ⎤
(𝛾 − 1)𝑠
spot radius, 𝑡𝑝 is the full width at half maximum (FWHM) of the laser = ⎢ 1 + 𝜋( )2 − 𝜋 ⎥ ,
𝑇𝑠 ⎢ 2(𝛾 + 1) 2(𝛾 + 1) ⎥
pulse, and 𝛼(𝑟, 𝑧) is the absorption coefficient of laser-induced plasma. ⎣ ⎦
√ [ ]
𝑢𝑠 is the vaporization rate of target, which will be calculated in the 𝜌𝑣 𝑇𝑠 1 𝑠 (6)
next section, 𝐿𝑒𝑣 is the latent heat of vaporization, and 𝑇𝑒𝑛 is the = (𝑠2 + ) exp(𝑠2 )erf c(𝑠) − √
𝜌𝑠 𝑇𝑣 2 𝜋
environment temperature. Since most of the target region in the bottom [ √ ]
1 𝑇𝑠 2
is unaffected by laser, the heat loss of vaporization and radiation is + 1 − 𝜋𝑠 exp(𝑠 )erf c(𝑠) .
2 𝑇𝑣
assumed to occur only on the top surface of the target and could be
neglected on the other surface. where 𝑇𝑣 and 𝜌𝑣 are the temperature and density of the vapour on
The governing equation’s boundary conditions are given by Eqs. (3) the gas side of KL, respectively, while 𝑇𝑠 and 𝜌𝑠 are the temperature
and (4). and density of the target surface, respectively. In addition, 𝛾 is the
specific heat ratio. The vapour plume is considered as an ideal single-
𝑝𝑟𝑒𝑐𝑜𝑖𝑙 = 𝑝𝑒𝑣𝑎𝑝 + 𝜌𝑣 𝑢2𝑜𝑢𝑡 . (3) particle gas column with the specific heat ratio of 5/3. Additionally,
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Z. Yan, X. Mei, W. Wang et al. Optics Communications 453 (2019) 124384
Fig. 5. Flow velocity distribution of the target for various laser fluences (2, 4, 8 and 12 J/cm2 ) and different times ranging from 15 to 60 ns. The solid line represents the
isotherm with the temperature of 1941 K (the melting point of titanium).
√
𝑠 = 𝛾∕2𝑀, erf c(𝑠) is the complementary error function, and M is the where 𝐴0 is a constant, which relates to pressure and temperature
Mach number of the vapours at the edge of KL. Furthermore, the sat- ratios, and the dependence relations are taken from previous work of
uration vapour pressure 𝑝𝑠 at the surface corresponds to the saturation Ref. [16].
vapour density at 𝑇𝑠 and can be calculated using Clausius–Clapeyron
Then, the velocity of vapour particles, which comes out from the
equation [55] given by Eq. (7). √
surface can be expressed as 𝑢𝑜𝑢𝑡 = 𝑀𝑐𝑠 = 𝑀 𝛾𝑘𝐵 𝑇𝑣 ∕𝑚𝑣 , where 𝑐𝑠 is
𝐿𝑒𝑣 𝑇
𝑝𝑠 (𝑇𝑠 ) = 𝑝0 exp( (1 − 0 )). (7) the local sound speed, and 𝑘𝐵 is the Boltzmann constant. Additionally,
𝑅𝑇0 𝑇𝑠
the ablation velocity of the target is obtained by solving the mass
where 𝑝0 is the saturation vapour pressure at 𝑇0 (in this model 𝑝0 = conservation equation, given by Eq. (9).
1.01 × 105 Pa and 𝑇0 = 3533 K— the boiling point of titanium under a
standard atmospheric pressure), 𝐿𝑒𝑣 is the latent heat of vaporization, 𝜌𝑠 𝑢𝑠 = 𝜌𝑣 𝑢𝑜𝑢𝑡 . (9)
and 𝑅 is the specific gas constant.
The Mach number is determined based upon the pressure ratio where 𝜌𝑠 , and 𝜌𝑣 are the density of target surface and vapour, respec-
𝑝∕𝑝𝑠 . If the ratio is less than unity, the surface vaporization process tively.
dominates the re-condensation. If the ratio is larger than unity, the Due to the material flow and ablation rate, the moving mesh ve-
vapour re-condensation dominates. The Mach number can be given by locity of the interface between gas and target can be determined using
Eq. (8) [53].
Eq. (10).
1 − (𝑝∕𝑝𝑠 )−0.275
𝑀= . (8) ⃖⃖⃗ + 𝑢𝑠 .
𝑢 = 𝑛⃖⃗ ⋅ 𝑉 (10)
1 − 𝐴0 −0.275
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Z. Yan, X. Mei, W. Wang et al. Optics Communications 453 (2019) 124384
Fig. 6. The total pressure of titanium vapour and ambient air above the target surface for various fluences (2, 4, 8 and 12 J/cm2 ) and time period ranging from 15 to 45 ns.
2.3. Laser-vapour interaction and plasma shielding effect of the incident laser is much larger than the electron collision time
of titanium, the vapour can be treated as local thermal equilibrium.
The laser-induced plasma, created by the vapours, is partially ion- Due to this reason, the density of free electrons in the vapours can
ized at high temperatures above the target. Since the pulse width be calculated using the Saha–Eggert equation [24,26,56], given by
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Z. Yan, X. Mei, W. Wang et al. Optics Communications 453 (2019) 124384
Fig. 7. The particle density of titanium vapour above the target surface for various fluences (2, 4, 8 and 12 J/cm2 ) and time period ranging from 15 to 45 ns.
Eq. (11). where 𝛼𝑖 , 𝑔𝑖 and 𝜀𝑖 are the ionization degree, degeneracy and ionization
𝛼𝑖2 2(2𝜋𝑚𝑒 𝑘𝐵 𝑇 )3∕2 𝑔𝑖+1 −𝜀𝑖
= exp( ). (11) energy of the ions, respectively.
1 − 𝛼𝑖 𝑛0 ℎ3 𝑔𝑖 𝑘𝐵 𝑇
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Z. Yan, X. Mei, W. Wang et al. Optics Communications 453 (2019) 124384
Fig. 8. (a) Temporal profile of the normalized effective power density of laser pulse reaching the target after the attenuation of plasma shield at different fluences (2, 4, 8 and
12 J/cm2 ). (b) The energy ratio of plasma shield effect at different laser fluences.
The plasma shielding effect mainly contains two parts: reflection using a plano-convex lens (𝑓 ′ = 100 mm). A motorized xyz stage
and absorption. The reflection coefficient is given by Fresnel equation: (OWIS, PS-30) controlled by computer is used for precise positioning of
| |2 the samples. In this study, the surface roughness of polished commercial
𝑅 = |(𝜀1∕2 − 1)∕(𝜀1∕2 + 1)| . And the corresponding dielectric function
| |
of plasma is given by Drude relation [57–59]: pure titanium was about 300 nm. For the present experiment, at the
fixed repetition frequency of 100 Hz, the wavelength of 1064 nm,
𝜔2𝑝
𝜀(𝜔) = 1 − . (12) the pulses with the peak laser fluences of 2, 4, 8 and 12 J/cm2 were
𝜔(𝜔 − 𝑖𝑣𝑒𝑓 𝑓 ) employed to explore the effect of laser fluence on the ablated depth and
Here, 𝜔 is the light frequency, 𝑣𝑒𝑓 𝑓 is the effective collision fre- surface morphologies of titanium under laser irradiation. The surface
quency, and 𝜔2𝑝 = (4𝜋𝑛𝑒 𝑒2 ∕𝑚∗𝑒 )1∕2 is the electron plasma frequency, morphologies of samples with different laser fluences were observed
where e is the electron charge, 𝑚𝑒 is the effective electron mass, and using confocal microscopy (OLS4000), which contains UIS2 optical
𝑛𝑒 is the density of free electrons in the plasma. System, 5-100x Objectives and resolution of 0.05 μm.
The plasma absorbs a part of the incoming laser radiation and
shields the target surface. Additionally, it consists of different species, 4. Results and discussion
such as electrons, ions, and neutral particles. Due to this, the absorption
of the laser by plasma occurs through three different mechanisms, In order to compare the simulation results with experimental mea-
namely the inverse Bremsstrahlung (IB), photoionization (PI) and Mie surements, the parameters of the mathematical model must conform
scattering absorption [30]. The absorption of laser radiation by free to the actual experiments. Therefore, the beam waist radius of laser
electrons in the plasma is described by the IB mechanism, while the that reached the surface was set to be 40 μm. The FWHM of laser
absorption by excited ions and neutral atoms is described by the PI pulse duration was 10 ns, as shown in Fig. 3. The thermal and optical
mechanism. Furthermore, the absorption by vapour clusters inside the parameters of the titanium target are given in Table 1. In the gas
plasma is described by Mie absorption. However, PI and Mie scattering region, the ambient gas is considered as air and the initial temperatures
could be neglected due to its very small contribution to the absorption and pressure is 293 K and 1.01 × 105 PA, respectively. The effect of
of laser. Due to this reason, the absorption coefficient of laser-induced chemical reaction is neglected and the ambient gas is considered to
plasma is expressed using Eq. (13) [27,29,56,60]. be transparent to the laser. The molar mass of the ambient gas is:
2 2 3 𝑚𝑔 = 29 g∕mol. Furthermore, the maximum degree of ionization of
2𝜋 1∕2 𝑒0 3 4𝑛𝑒 𝑍𝑖 𝑛𝑖 𝜆 ℎ𝑐∕𝜆 vapour ions is taken to be 2.
𝛼=( ) ( ) (1 − exp(− )). (13)
3𝑚3𝑒 𝑘B 4𝜋𝜀0 3ℎ𝑐 4 𝑇 1∕2 𝑘B 𝑇
where 𝑚𝑒 , 𝑛𝑒 and 𝑒0 are the mass, number density and electric charge of 4.1. Temperature and flow velocity of target region
electron, respectively. 𝑛𝑖 and 𝑍𝑖 are the number density and the average
ionized degree of ions. Furthermore, 𝑘B is the Boltzmann constant, When the laser irradiates the target surface, most of the laser energy
ℎ is the Planck constant, 𝜀0 is the vacuum permittivity, and 𝜆 is the is concentrated on a very thin and small region around the central
wavelength of laser. point. In the target region, the temperature–time evolution of the
surface’s central point at different fluences is shown in Fig. 4. During
3. Experiment setup the laser pulse duration, the temperature of the central point did not
always increase due to the latent heat of vaporization and plasma
For studying the nanosecond laser ablation of titanium, A Nd:VAN shielding phenomena. With the laser fluence of 2, 4, 8 and 12 J/cm2 ,
nanosecond laser system (InnoLas, SpitLight Compact 100) based on the temperature reached the maximum values at 18.65 ns, 14.95 ns,
pulse regenerative amplification was used. The laser system delivers 10- 16 ns, and 15.55 ns. Obviously, the higher laser fluence had a much
ns full width at half maximum (FWHM) pulse duration with a maximum higher heating rate at the beginning of laser interaction. The energy
pulse energy of 100 mJ and works at optional wavelength of 1064 nm, loss was not comparable to the laser power, which was absorbed by
532 nm, and 266 nm. The energy density distribution of the laser beam the target and due to which, the temperature continuously increased
is Gaussian shape with beam quality factor (M2 ) ∼ 1.3. And the interval during the early stage of the laser pulse. After the temperature ex-
between laser pulses is 10 ms. The experimental setup is depicted in ceeded the boiling point, the vaporization began and the vaporization
Fig. 3. The number of pulses is controlled using an electromechanical rate depended on temperature. Additionally, the evaporated material
shutter. A diaphragm is used further to shape the laser beam, and a hindered the laser propagation and decreased laser energy absorbed by
pyroelectric detector is used to monitor the laser power in real time the target. Therefore, the maximum temperature not happened at the
with conjunction with a beam splitter in the primary laser path. The end of the laser pulse and raised slower with the increment of laser
laser beam is focused and normally incident onto the surface of sample fluence.
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Z. Yan, X. Mei, W. Wang et al. Optics Communications 453 (2019) 124384
Fig. 9. Spatial and temporal evolution of the laser power density that reached the target surface after plasma shielding attenuation for different fluences (2, 4, 8 and 12 J/cm2 ).
The temperature distributions of the target region with different due to the surface curvature at the hump. Therefore, the hump grew
laser fluences are shown in Figure s3 of Supplementary Information. bigger at the edge of melt zone. The position of humps is mainly
The temperature was usually the highest at the central point, where determined by the first mechanism, whereas the size of humps is mainly
absorbs relatively high laser intensity. Similarly, the melt zone’s area determined by the second mechanism.
enlarged with the increment of laser influence. The temperature dis-
tribution for the target region is strongly dependent on the local 4.2. Vapour gas dynamics and plasma shielding effect
laser intensity that irradiates the surface of titanium. Therefore, the
distribution of target temperature is quite similar to the shape of laser Based on the temperature distribution of target, the boundary con-
energy distribution. With the increase in laser fluence, the centre of ditions in the gas region can be obtained from Knudsen relations. The
temperature distribution turned to be uniform in radial direction. There total pressure and the particle density of vapours in the gas region with
are two reasons for the change in temperature distribution. As the laser different laser fluences (2, 4, 8 and 12 J/cm2 ) from 15 to 45 ns are
fluence increases, the plasma shielding effect becomes more substantial, shown in Figs. 6 and 7.
due to which the laser energy distribution becomes even at the centre. Similar to the temperature distribution, the evaporation rate was
Another factor is that the radial flow velocity brings the heat of the highest at the centre of target. Therefore, the pressure and the particle
centre to the surrounding area. density were the highest at the centre of target surface at any laser
The flow velocity distributions of the target region with different fluence. Due to the difference in time, during which the target reached
laser fluences are shown in Fig. 5. The flow velocity was the highest the maximum temperature under different laser fluences, the total
at the outer part of melt zone and the maximum velocity reached 121 pressure and the vapour particle density reached maximum at different
m/s at 60 ns with the laser fluence of 12 J/cm2 . There are two possible times. With the laser fluence of 12 J/cm2 and at time 𝑡 = 15 ns, as the
mechanisms. Firstly, when the central temperature is above the boiling strong evaporation just began, the total pressure reached more than 107
point, strong recoil pressure is generated above the centre of melt zone Pa and the vapour particle density reached more than 300 mol/m3 ,
due to vaporization and pushes the liquid phase to the peripheral area. which caused a huge recoil pressure on the target surface. With the
Secondly, at the outer part of the melt zone, although the temperature is increase in laser fluence, the maximum pressure and the vapour particle
relatively low, there is a steep temperature gradient, which on average density also seemed to be saturated while the vaporized area became
lies within the order of 108 K/m and causes a strong local thermo- larger.
capillary force to push the liquid phase outside. In other words, at the The high laser fluence also increased the speed of vapours at the
edge of melt zone, the liquid phase has nowhere to go except upwards interface. The high-speed vapours were ejected out from the target
and hence, produces a hump of molten material. interface. The speed of vapours increased with the increase in laser
Moreover, the first mechanism dominated during the laser pulse. fluence and the front of vapours could reach the height of 80 μm at
Then, the outer surface formed a small hump and the curvature the time 𝑡 = 45 ns with the laser fluence of 12 J/cm2 .
changed due to the strong recoil pressure with the radial gradient. It can also be seen that the vapour caused a huge pressure gradient
After the laser pulse, with the cooling of materials, the recoil pressure around the centre of interface during laser processing. With the increase
decreased and the thermo-capillary force predominated. Additionally, in laser fluence, the position of maximum pressure gradient became
at the outer part of the melt zone, the thermo-capillary force intensified farther from the centre. Due to this reason, in the target region, the
8
Z. Yan, X. Mei, W. Wang et al. Optics Communications 453 (2019) 124384
9
Z. Yan, X. Mei, W. Wang et al. Optics Communications 453 (2019) 124384
Fig. 11. Target surface morphology cross-sectional profile after 5 pulses at different laser fluences (2, 4, 8 and 12 J/cm2 ). Solid line: Experimental results. Dashed line: Simulation
results.
Acknowledgements [2] G.D. Gautam, A.K. Pandey, Pulsed Nd:YAG laser beam drilling: A review, Opt.
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[3] R. Eason, Pulsed Laser Deposition of Thin Films: Applications-Led Growth of
This work was supported by the National Natural Science Founda- Functional Materials, Wiley-Interscience, 2007.
tion of China (Grant No. 51735010) and the Program for Changjiang [4] J. Huotari, V. Kekkonen, T. Haapalainen, M. Leidinger, T. Sauerwald, J. Pu-
Scholars and Innovative Research Team in University, China (Grant No. ustinen, J. Liimatainen, J. Lappalainen, Pulsed laser deposition of metal oxide
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