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Optics Communications 453 (2019) 124384

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Optics Communications
journal homepage: www.elsevier.com/locate/optcom

Numerical simulation on nanosecond laser ablation of titanium considering


plasma shield and evaporation-affected surface thermocapillary convection
Zhaoxuan Yan, Xuesong Mei ∗, Wenjun Wang, Aifei Pan, Qingyan Lin, Chenchen Huang
State Key Laboratory for Manufacturing Systems Engineering, Xi’an Jiaotong University, Xi’an 710054, China
Shaanxi Key Laboratory of Intelligent Robots, Xi’an 710049, China

ARTICLE INFO ABSTRACT


Keywords: Nanosecond laser ablation of metal is a complicated process, which consists of many strongly coupled physical
Nanosecond laser ablation phenomena, including material heating, melting, evaporation, vapour dynamics, and plasma shield. In this
Vapour dynamics work, the nanosecond laser ablation process of titanium is investigated at 1064 nm wavelength. A multi-
Plasma shield
physics axisymmetric two-dimensional (2D) model is presented. The evolution and the distribution of titanium
Surface morphology
target’s temperature were solved using governing equations and the vapour dynamics was determined using
the Knudsen relations. The maximum temperature of titanium grown slower with the increase in laser fluence
and the maximum flow velocity of liquid materials reached 121 m/s with the laser fluence of 12 J/cm2 . In
addition, the plasma shield effect was taken into account to correct the energy distribution of the incident laser.
As the laser fluence increases, the energy efficiency decreases. At the laser fluence of 12 J/cm only 55.9% of
the energy was absorbed at the centre of titanium. Furthermore, the surface morphology profiles were analysed
after the laser ablation on different laser fluences lying within the range of 2 - 12 J/cm2 . The results showed
that the surface morphology after ablation has a crater-like form and the increment of laser fluence leads to a
slower non-linear increment in ablation depth and diameter of melt zone. The calculated results are in good
agreement with the experimental results. The study provides useful information for nanosecond laser precision
fabrication.

1. Introduction focused on the mechanism of phase explosion removal [19–22]. Most


of them concentrated on the study of nucleation rate of liquid mate-
In recent years, many studies have focused on the process of rials, and the material was considered to be removed at the critical
nanosecond laser ablation owing to its expanding applications such temperature. It was widely accepted that the vaporization was the main
as precision machining [1,2], pulsed laser deposition [3,4], nanopar- removal mechanism of nanosecond laser ablation under low energy
ticle fabrication [5,6], synthesizing materials [7] and laser-induced density [23,24].
breakdown spectrometry (LIBS) [8]. This wide range of applications Furthermore, the removed gasification material will continue to
is due to high flexibility and precision of nanosecond laser ablation
interact with the laser and being converted to locally ionized plasma,
which necessitates accurate control over material morphology and
which exhibited a significant effect on the laser processing. The evap-
thermodynamic conditions. Therefore, the fundamental laser ablation
orated material expands rapidly above the surface and absorbs a
mechanism received lots of attention.
part of the laser energy, which called plasma shielding phenomenon.
However, most of the theoretical studies were devoted to one-
dimensional laser ablation models, which were based on heat conduc- There were also many theoretical and experimental studies focusing
tion [9–14]. With regards to the material removal mechanism, Knight on the vaporization of materials and the subsequent formation of
et al. proposed the concept of the Knudsen layer, which was used to plasma [25–27]. The absorption by plasma mainly consists of in-
do calculations about the state equilibrium of the surface evaporation verse bremsstrahlung (IB) and photo-ionization (PI) processes [28,29].
atoms during the rapid phase change process of the material [15]. Experiment research shows that the laser-induced plasma forms hemi-
There were many studies about the thermodynamics phenomena during spherical structure compresses the surrounding gas and generates a
the laser processing, including atomic flux from the material, change shock wave during the laser pulse [30,31]. Due to the plasma shielding
in surface pressure and dynamics of the vapours, which were all based phenomenon, the laser ablation depth tended to saturate with the
on the theory of Knudsen layer [16–18]. Additionally, many studies increase in laser energy [32].

∗ 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

However, there were a few studies, which focused on the surface


morphology after nanosecond laser ablation. Most of these studies
only considered evaporation for predicting the ablation depth and
diameter [33–35]. Otto et al. proposed a computational fluid dynamics
model, which involved melting, evaporation and gas dynamics in the
pulsed laser ablation of metals [36–38]. However, they did not consider
the plasma shield effect in laser processing, due to which, the simulated
depth turned out to be larger than the experimental value. There
were some studies that took into account the influence of plasma
shielding during laser processing for metals and films [39–42]. Tani
et al. proposed a laser milling model with an experimental coefficient
which described the ratio of absorbed laser energy [43–46]. It showed
that plasma shielding attenuated laser energy and had a significant
impact on the target surface state.
In this study, a two-dimensional (2D) axisymmetric model for
the nanosecond ablation of titanium was presented. The influence
of plasma shield on laser energy, corresponding with the vapour
dynamics, was carefully investigated. In addition, the flow of molten
material under the recoil pressure and surface tension was solved to
trace changes in surface morphology after laser ablation. As a conse-
quence, the simulated surface morphologies satisfactorily verified the
experimental results. Based on the results, a better understanding of the
surface morphology can be obtained after nanosecond ablation coupled
with the plasma shielding phenomenon. The results also provide a good Fig. 1. Physical phenomena under nanosecond laser irradiation.
guide for nanosecond laser precision machining.

2. Mathematical model

Since a nanosecond is much longer than the phonon–electron re-


laxation time, the interaction of nanosecond laser with the material is
essentially a photo-thermal process. When the material is exposed to
a pulsed laser, the material will absorb extremely high-power density.
During the process, the laser energy is converted to heat deposition
on the surface of the material and result in the rapid temperature
increment of the irradiated area.
The temperature of the material quickly exceeds the melting point
or even the boiling point, due to which, the surface appears to be
liquefied material, and some of the material is vaporized. At this
stage, vaporization is the main removal mechanism because the energy
density is relatively low. The vapour molecules will first form a very
thin Knudsen layer on the surface of the material, and the velocity and
pressure will regain the equilibrium distribution. Subsequently, the va-
porized material with high temperature leaves Knudsen layer and rises
into the air environment. Then, a layer of ionized plasma is produced
above the material, which hinders the continuous absorption of poste-
rior laser energy of the pulse (plasma shielding phenomenon) [47]. A
very complex physical and chemical coupling reaction takes place in a
short time, as shown in Fig. 1.
In this work, a 2D axisymmetrical model is proposed to solve for
several physical phenomena, including material melting, vaporization,
surface flow, and plasma shielding during the laser processing. The
model uses the commercial software COMSOL Multiphysics 5.3a as
modelling platform. In the proposed model, the region of melt and Fig. 2. Geometry and mesh of the simulation model.
the solid material are classified as the target region. And the region
above the target, which comprises of ambient air and metallic vapour
is called the gas region. Fig. 2 presents the geometry and mesh details
2.1. Laser-target interaction
of the 2D axisymmetrical FEM model. The orthogonal quadrilateral
grids were generated with the maximum size of 0.75 μm in the centre
and the adaptive quadrilateral grids were generated in the periphery In the target region, a two-dimensional governing equation is used
area. Moreover, the time step of numerical simulation is set to 0.05 ns. to model the flow and the heat transfer process (see Eq. (1)).
The PARDISO solver was used to solve the governing equations and ⃖⃖⃗ = 0
∇⋅𝑉
boundary flux computation in two regions with relative and absolute
𝜕𝑉⃖⃖⃗
tolerance as 10−2 and 10−4 , respectively. The interface of gas/target is 𝜌( + ∇ ⋅ (𝑉 ⃖⃖⃗)) + 𝜇∇2 𝑉
⃖⃖⃗𝑉 ⃖⃖⃗ + ∇𝑝 = 0 (1)
𝜕𝑡
solved using the ALE moving mesh method [48,49]. The detailed model [ ]
𝜕𝑇 ⃖⃖⃗𝑇 ) − ∇ ⋅ (𝑘∇𝑇 ) = 0.
implement is shown in Figure s1 of Supplementary Information. 𝜌𝐶𝑝 + ∇ ⋅ (𝑉
𝜕𝑡

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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

Fig. 3. Schematic diagram of the experimental setup.

𝜕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.

2.2. Vapour gas dynamics

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

vapour dynamics produced a high recoil pressure gradient outside of


the melt zone and moved the initial position of target hump out as
the laser fluence increased. Additionally, because the vapour particle
density near the surface was very high during the laser pulse, the
plasma shielding phenomenon dramatically reduced the laser energy
that reached the target’s surface. Therefore, the surface temperature
decreased due to the heat loss of vaporization and plasma shield, which
reduced the rate of evaporation. At the end of the laser pulse duration,
the pressure and the vapour particle density gradually decreased at the
target interface.
As time grew, the total pressure propagated from the centre to
periphery, gradually pushing the air away and generating a shock wave,
which matched well with the experimental observation [28,31]. At
45 ns, the shock wave was fully developed, as shown in Fig. 4. In
addition, the vapour particle moved upwards and diffused into the
ambient air. The horizontal expansion increased the vapour width.
With the movement of vapour, the airflow vortices appeared near the
interface.
When the laser pulse energy reached the target surface, the intensity
was substantially modified after its propagation through the vapour Fig. 10. Ablation depth and diameter of melt zone after 5 laser pulses for various
plume. However, based on the vapours dynamics, the attenuation coef- laser fluences. The solid line represents the experimental results, while the dashed line
ficient of plasma shielding phenomenon can be obtained. The temporal represents the simulation results.

profile of the normalized laser effective power density at the centre of


surface is shown in Fig. 8. At the early stage of laser pulse, there is
no plasma shield effect until the beginning of evaporation. Apparently, results, similar to the simulation results, the surface morphology had a
with the higher laser fluence, the evaporation occurred earlier and crater-like form. There were pits and humps at the edge of heat effect
more intense, which resulted in a higher attenuation coefficient of zone, while the centre was the deepest. However, in the simulation
plasma shield. Therefore, the energy efficiency decreases with the results, the centre was not the deepest at the laser fluence of 12 J/cm2 .
increase in laser fluence. At the laser fluence of 12 J/cm2 , only 55.9% There was a very small uplift at the centre due to the flow convection.
of energy was absorbed at the centre of target. There were about Moreover, there is a small deviation between the simulation and exper-
30.5% of energy was reflected and 13.6% of energy was absorbed by imental results. One possible explanation is that the actual laser pulse
the plasma. With the diffusion and convection of vapours, the particle is not an ideal Gaussian shape distribution because of the energy loss
density and the temperature were decreased and diluted by the ambient in the laser propagation and the positional error of the optical devices.
air. Therefore the attenuation coefficient of plasma shield gradually The laser energy distribution becomes more dispersed, which increased
decreased at the end of the laser pulse duration. the melt zone’s diameter and decreased the ablation depth. Besides, the
Additionally, the plasma shielding phenomenon affected the laser surface roughness may cause a minor effect on the morphology result.
energy’s spatial distribution on the target surface. The spatial and
However, good agreement was observed between the simulation
temporal profile of laser power density, which irradiated the target
(dash lines) and experimental data (solid lines) of surface morphol-
surface, is shown in Fig. 9. Similar to the particle density distribution,
ogy after 5 laser pulses at different laser fluences (2, 4, 8 and 12
the attenuation coefficient caused by the plasma shield was higher at
J/cm2 ), which validates the proposed model in predicting the surface
the centre than the periphery area.
morphology of titanium after laser ablation at different laser fluences.
4.3. Surface morphology after ablation
5. Conclusions
After the laser pulse finished, the molten material still existed for
hundreds of nanoseconds. The material in liquid phase was pushed and In this article, a comprehensive two-dimensional (2D) model of laser
accumulated on the edge of the melt zone due to the recoil pressure ablation titanium with nanosecond pulses at 1064 nm wavelength is
and surface tension. The accumulated material formed a hump and
proposed. The results shows that the temperature was the highest at
the surface curvature changed. Additionally, the surface tension force
the centre and grow slower with the increment of laser fluence. The
generated small pits near the hump of molten material. Then, with
recoil pressure and the surface tension force continuously pushed the
the cooling of the material, the molten material solidified around the
liquid phase and formed a hump at the edge of melt zone. Moreover, the
ablation area and formed a crater-like surface.
simulation of laser beam absorption and reflection by the plasma was
The changes in surface morphology after one laser pulse ablation are
improved by correct the energy distribution of the incident laser. The
only several hundred nanometers. It brings difficulties to compare the
high laser fluence lowered the energy efficiency. At the laser fluence
experimental results with the theoretical analysis. In order to avoid the
of 12 J/cm2 , only 55.9% of the energy was absorbed by the target.
measurement error, the surface morphology of titanium after 5 laser
pulses ablation was used to compare the experimental and simulated Furthermore, the surface morphology results showed that the increase
results. In the experiments, the interval between laser pulses was in laser fluence led to a slower non-linear increase in ablation depth and
10 ms, which was long enough to cool the target. Additionally, in the diameter of melt zone. The morphology of the target surface formed
simulation, the surface morphology after previous pulse ablation was a crater-like shape and produced pits and humps at the edge of the
set to be the input of the next laser pulse’s simulation. melt zone after laser ablation in both the experiments and simulations,
The ablation depth of the centre point and the diameter of the melt which obtains good consistency.
zone are shown in Fig. 10. The increase in laser fluence led to a slower This study provides a general model for predicting the titanium
non-linear increase in the ablation depth and the diameter of melt surface morphology after nanosecond laser ablation, which provides
zone in the simulation and experimental results. The cross-sectional useful information for the practical application of nanosecond laser
profile of surface morphology is shown in Fig. 11. In the experimental processing.

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.

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