See discussions, stats, and author profiles for this publication at: https://www.researchgate.

net/publication/257745492

Investigation of the Material Removal Efficiency During Femtosecond Laser

Machining

Article  in  Procedia CIRP · December 2012

DOI: 10.1016/j.procir.2012.07.081

CITATIONS READS

9 288

3 authors, including:

Panagiotis Stavropoulos George Chryssolouris

Hellenic Air Force University of Patras
211 PUBLICATIONS   4,236 CITATIONS    386 PUBLICATIONS   15,379 CITATIONS   

SEE PROFILE SEE PROFILE

Some of the authors of this publication are also working on these related projects:

EP-20903: RIDER View project

Time prediction algorithm for raster Rapid Prototyping systems View project

All content following this page was uploaded by Konstantinos Efthymiou on 20 September 2014.

The user has requested enhancement of the downloaded file.

 Available online at www.sciencedirect.com

Procedia CIRP 3 (2012) 471 – 476

45th CIRP Conference on Manufacturing Systems 2012

Investigation of the Material Removal Efficiency During

Femtosecond Laser Machining
P. Stavropoulosa, K. Efthymioua, G. Chryssolourisa,*
a
Laboratory for Manufacturing Systems & Automation, Department of Mechanical Engineering & Aeronautics, University of Patras, 26500, Greece
* Corresponding author. Tel.: +30-2610-997262; fax: 30-2610-997744.E-mail address: xrisol@lms.mech.upatras.gr

Abstract

Understanding physical processes accompanying ablation is necessary for the optimal use of Femtosecond Laser pulse material
processing. The current work describes the implementation of a molecular dynamics based approach, developed for simulating the
Laser ablation process of iron at a molecular level. A measure of material removal is formulated and utilized to estimate the effect
of energy and pulse width on material removal. Evaluation of the model is based on comparison with experimental results. Ablation
efficiency dependence of Laser Fluence is discussed.

© 2012
© 2012 The
The Authors.
Authors. Published by Elsevier
Elsevier B.V.
B.V. Selection
Selection and/or
and/or peer-review
peer-reviewunder
underresponsibility
responsibilityofofProfessor
ProfessorD.D.Mourtzis
Mourtzisand
and
Professor G.
Professor G. Chryssolouris.
Chryssolouris.

Keywords: Laser ablation efficiency; Molecular Dynamics; Femtosecond laser

parameters and environmental conditions [2].

1. Introduction Experimental investigations have revealed that with FL,
along with the crater, co-exists a debris formation, the
Laser micro machining is a technology capable of height of which depends on the target matter, the laser
producing parts in the micro and sub micro scale. For energy and the number of pulses fired to the target. The
such applications, lasers with pulse duration in the crater diameters have been found to be greater than those
femtosecond range (femtolasers) are widely used. Laser of the laser beam. Coincidence on the crater shape with
ablation occurs due to the irradiation of the laser beam radiation intensity distribution has been found only at
onto the material causing a combination of sublimation, low laser fluences (≈1 J/cm2). The crater widening is the
vaporization and melting. It is characterized by small result of the laser beam being scattered in the near-
temporal and spatial scales and an extremely high surface plasma and the plasma action on the crater
material temperature and pressure. Femtolaser (FL) formation. The debris generation is the result not only of
drilling uses pulses with duration in the order of tens to the liquid phase explosion, but also of the plasma
hundreds of femtoseconds. During the recent years, the particle recondensation [3]. Laser micro-processing is
FL ablation has shown a rapid development due to its used by many industrial sectors – semiconductors,
distinct advantages compared with those of the longer electronics, medical, automotive, aerospace,
pulse lasers [1]. As a result of its extremely short pulse instrumentation, and communications. Laser ablation of
duration, the heat diffusion is confined, and the heat metals, ceramics, silicon and polymers is a complex
affected zone (HAZ) is rather limited. This high process and the exact nature of their interaction with the
localized heating, in each laser pulse, results in smaller material and laser processing parameters used, is
material volume removal and therefore, more precise specific.
machining results compared with the ones obtained from FL being a rather precise tool needs accurate
longer laser pulses. The laser ablation process depends simulation methods [4]. Molecular Dynamics (MD) is
on the physical properties of solid matter, laser based on the solution of Newton’s second law and aims

2212-8271 © 2012 The Authors. Published by Elsevier B.V. Selection and/or peer-review under responsibility of Professor
D. Mourtzis and Professor G. Chryssolouris.
doi:10.1016/j.procir.2012.07.081
472 P. Stavropoulos et al. / Procedia CIRP 3 (2012) 471 – 476

at monitoring the movement of an atom within a system. mechanism and shock wave propagation [10], their
Each particle in the ensemble of N particles is treated as dependence on the initial temperature, the pulse duration
a mass point, interacting through force fields, which in [11] and the mechanism and velocity distribution of
turn, have been derived from interacting potentials. MD molecules or plume, ejected during laser ablation [12].
works through the solution of Newton’s equation of According to [13], the results from the MD modelling of
motion. Therefore, the evolution of the system can be the ultrashort laser pulse ablation of metals (Al, Ni and
calculated in certain time steps, where the total in- Fe), are reported at fluences, and range from the
formation (particle positions, velocities, kinetic and threshold of ablation up to 0.5 J/cm2.
potential energies) of the system is available for each In the present study we define as laser ablation
time step. All further properties as temperature, pressure efficiency the ratio of the ablated material volume to the
and autocorrelation functions can be determined without energy of the laser pulse.
any additional parameters [5]. The reaction process of a Section 2 provides the molecular dynamics model
laser beam with a bulk solid is the interaction between describing the implemented algorithm and the simulation
the electromagnetic field of light and the electric field of details of model including the material and laser beam
the atoms or molecules of the solid material. The light properties. In section 3 the experimental setup, that
absorbed by the solid material can be divided into three validates the model, is determined. The results from the
categories depending on the level of the light energy: 1) molecular dynamics model and the experiments are
The excitation of the electronic state of atoms and presented and discussion in section 4 with special
molecules of the lattice particles, 2) The excitation of the emphasis given on the laser ablation efficiency.
intermolecular vibration state of the lattice molecules
and 3) The excitation of the intermolecular or inter 2. Molecular Dynamics
atomic vibration of rotational state of the lattice
molecules. 2.1. General Description
The majority of the interacting potentials used in MD,
are based on the Pair Potential Approximation (PPA). After energy has been absorbed by the material, the
This is so, due to the fact that PPA provides a good electro and lattice temperatures rise greatly. When the
description of the material’s properties and also material temperature is high enough, certain phase
consumes less computing time than do the potentials change processes occur and part of the material is
utilizing three or more body terms [7]. Potential removed from the bulk. Complicated thermal and
functions that have been “phenomenologically” derived, mechanical processes take place and many factors con-
often present a more realistic view of the atomic tribute to the material being removed. Temperature is the
interactions than do the potentials having been dominant factor that leads to material separation and
exclusively derived. The following types of potentials consequently, to its removal. The electrons and the
fall into the phenomenological category: Buckingham, lattice are heated strongly by the laser irradiation in
Morse, Lennard-Jones (Mie’s reduced form) and Barker order for the increase in the lattice temperature to be
potentials for Krypton and Xenon. Among the above high enough for melting and evaporation to occur. Since
potential functions, the Morse Potential Function (MPF) the lasers, used in micro/nano processing are operating
is considered to be more appropriate for its application in the femtosecond range, the irradiated material is
to metals [5]. The embedded-Atom Method (EAM) is a assumed to be going from a solid to a gas phase without
semi-empirical, many-particle potential for computing having first gone through a melting phase [19]. The
the total energy of a metallic system. The influence [8] target to be irradiated is considered to be of BCC
of the MPF and EAM based potential, on the description structure, at an initial constant environment temperature.
of the properties and the ultrashort laser ablation process The lattice structure of pure Fe changes with the increase
of Fe by MD Simulation technique, has been studied. of temperature. Until 11180 K the crystal structure is off
The accuracy of both potentials in evaluating the melting BCC. After this temperature has been reached and up to
temperature, the linear thermal expansion coefficient and 16630 K the structure is transposed to FCC. From 1663 0
the compression behaviour of Fe, is calculated [9]. K and above the form is of BCC again. It is safe to
Numerous studies have been conducted for the assume that the crystal structure of pure Fe is constant in
decomposition of metals during the FL ablation, the BCC form, due to the ultrafast heating of the bulk
following different approaches, varying from analytical material, provided by the femtosecond Laser pulses. The
mathematical modeling to simulation and experimental incident laser beam irradiates the target as shown in
studies. Studies have applied Hybrid MD Simulations, Figure 1, with a uniform temporal distribution. The laser
Classical MD or MD, combined with the Two beam propagates along the Z axis, perpendicularly to the
Temperature Model (TTM), in order to investigate the surface of the target. The laser beam intensity is
laser ablation phenomena, such as the heat transfer considered being spatially uniform and has Gaussian
 P. Stavropoulos et al. / Procedia CIRP 3 (2012) 471 – 476 473

temporal distribution. The number of photons, Assuming that the target is infinitely large, in the lateral
corresponding to the laser energy, is deposited to the directions, the Periodic Boundary Conditions (PBC)
material exponentially, following the Beer-Lambert law. were applied. The top surface of the target, where the
This photon energy is transferred to the atoms of the laser beam irradiates, has been subjected to the Free
system within a characteristic time, the time for the Boundary Conditions (FBC) allowing particles to move
electron lattice energy transfer and the establishment of and be removed. At the bottom surface, the Reflecting
equilibrium temperature. The energy deposited to the Boundary Conditions are applied (RBC) to ensure
system’s atoms contributes to their kinetic energy being velocity damping. The laser beam has a Gaussian profile
increased. This work uses an MD developed approach in time and space [15]. However, it is the combination of
implemented in a code, based on the Morse Potential the uniform distribution in space and the Gaussian
Function for the simulation of laser ablation processes. distribution in time that is preferred [16]. A number of
The approach and the implementation code, as illustrated photons corresponding to the energy produced by the
in previous study [14], consists of four basic sections. laser are deposited into the bulk material target. The
Phase change and material removal will be illustrated deposition is exponential and follows the Beer Lambert
from the MD retrieved data. The Morse Potential law. By absorbing photons, the particles of the crystal
Function is being used for the description of the inter- increase their kinetic energy and consequently, their
atomic potential and the potential energy within the velocity is also increased. Hence, their new velocities
system’s particles. The initial positions of the atoms are have to be recalculated following their irradiation. The
determined according to the BCC lattice and the initial particle removal criterion is based on the cohesive
velocities are randomly ascribed to the atoms according energy, one of the most significant factors in an MD
to the Maxwell–Boltzmann distribution at room simulation, as it determines the amount of energy that
temperature. can be absorbed by an entity.

2.2. Simulation Details

Iron (Fe) is being selected as the metal with a very

broad industrial application. The parameters of Fe used
in the simulation model are shown in Table 1 and are
assumed to be constant during the simulation time
intervals.

Table 1. Parameters of Fe

λ (nm) R (%) Tm (K) Tv (K)

775 65 1811 3134

The MD simulation system region is formed from

BCC unit cells, in the dimensions of 3.8x3.8x726.5nm
[10446.3nm3] and consists of a total number of 719,756
particles. The velocity Verlet algorithm has been applied
to the system for integrating the equations of motion.
The interaction among the atoms in the system is
described in the Morse Potential Function. According to
Fig. 1. Schematic of the problem description this potential, the Morse parameters of Fe are computed
from the energy of sublimation, the lattice constants and
A standard method for the solution of ordinary the compressibility for a perfect lattice are shown in
differential equations is the finite difference approach. Table 2.
Given the particle positions, velocities and accelerations
Table 2. Morse parameters of Fe [6]
at instant t, the positions, velocities, accelerations at a
later instant t+δt are obtained with a sufficient degree of
D (eV) a (Å-1) r0 (Å-1)
accuracy. The Verlet algorithm has been used for
integrating the equations of motion throughout the 0.4174 1.3885 2.845
simulation steps. The Velocity Autocorrelation function
(VAF) criterion is applied to ensure that the particles’ The initial velocities are randomly ascribed to the
velocities follow the Maxwell Boltzmann distribution. particles according to the Maxwellian distribution at
474 P. Stavropoulos et al. / Procedia CIRP 3 (2012) 471 – 476

300K room temperature. The ablation is investigated up The Scanning Electron Microscope (SEM) is used for
to several tens of femtoseconds. The Periodic Boundary observing the ablated area while the laser Scanning
Conditions (PBC) have been applied, in the X and Y Microscope (LSM) for measuring the ablation depth.
directions of the computational domain, for simulating The ablation depth per pulse is evaluated by measuring
an infinite medium. A velocity dampening technique is the total depth of the drilled hole and divided by the
applied, at the bottom of the computational cell along number of pulses used.
with the RBC, in order to prevent the artificial ablation
effects that may arise from the shock wave reflection. Table 4. Properties of Fe Samples [17]
The number of photons, corresponding to the laser
Material R% α (cm-1) 1/α Tm (K) Tv (K)
energy, is deposited in the material exponentially (nm)
following the Beer-Lambert law. The laser wavelength is
99.99% 65 0.54 x 18.5 1811 3145
set at 800 nm. The pulse duration, the total interaction
Fe 10
time of the laser and the material are fixed for all
experiments, whilst the laser fluence ranges from 0.1
J/cm2 to 30 J/cm2. 4. Discussion of the Results

3. Experimental Setup The ultrashort laser ablation has been investigated

computationally and experimentally in the range of laser
For the verification of the model, a set of fluences from the threshold up to 10 J/cm2. Both
femtosecond laser ablation experiments was conducted. computational and experimental results define the
The laser system used in the experiments consisted of a different ablation regimes of an ablation threshold.
mode-locked Ti:Sapphire laser system (CPA-2101,
Clark-MRX, Inc) pumped with a CW, solid state, 4.1. Ablation Depth and Laser Fluence
Nd:YVO4 laser (Millenia Vs, Spectra Physics). This
system is tunable from 400 to 800 nm and provides The ablation depth, per laser pulse, has been used as a
ultrashort laser pulses in the femtosecond regime validation means of the theoretical model. Figure 2,
(duration < 100 fs). A 5-fold expanding telescope was presents a comparison of the ablation depth in the
used for expanding the laser beam in order to uniformly experimental and computational results. For the majority
illuminate the back-aperture of an oil immersion of the laser fluences applied, there is observed a good
objective lens (100x; N.A., 1.2). This tight focusing agreement of the results.
geometry has made available the high fluences, required
for the ablation of the samples. The irradiation power
was controlled with a combination of a motorized λ/2
plate and an ultrafast polarizer (Melles Griot,
16PPB200) and was measured at the back aperture of the
lens used for excitation. To control the desired total
interaction time of the laser beam with the material
target, a fast mechanical shutter (rise system time 3ms,
Newport 845HP) has been integrated into the setup.

Table 3. Parameters of the laser system

Laser Type Wavelength Pulse Spot Diameter

(nm) Duration (μm)
Range (Fs)
Fig. 2. Computation and experimental ablation depths vs applied laser
Ti: Sapphire 400-8000 50-80 3134 fluence
Laser

Starting from the lowest applied laser fluence up to

The laser radiation is focused on the material surface the value of 0.1 J/cm2, the ablation depth per pulse,
by a lens having a 10 mm focal length. The beam follows a linear increment with the corresponding
diameter, at the focal point, ranges form 1 to 5μm. The fluence, as shown in Figure 3. For the experimental
targets are 0.5 mm thick and 99.99% pure Fe plates, results the smallest measured depth is 0.5nm for a 0.07
placed on a piezoelectric XYZ table vertically to the J/cm2 pulse. This is due to the fact that the LSM does not
laser beam cross-sectional surface. Table 4, contains the provide accurate measurements for depths smaller than
properties of the Fe specimens used in the experiments. 25 nm. However, the SEM images of the specimens
 P. Stavropoulos et al. / Procedia CIRP 3 (2012) 471 – 476 475

show material removal from the surface for fluences

even smaller than 0.07 J/cm2. Computational results
indicate that the ablation phenomenon starts at 0.06
J/cm2.

Fig. 5. Computation and experimental ablation depths vs applied laser

fluence for the third ablation region from 1 to 10 J/cm2

The accuracy of the MD model is verified by

Fig. 3. Computation and experimental ablation depths vs applied laser
comparing the ablation depth with the experimental data
fluence for the first ablation region from 0.01 to 0.1 J/cm2 obtained. Both experimental and theoretical results
clearly define three (3) different ablation areas, each
The second distinct ablation area in relation to the governed by different ablation mechanisms. At laser
applied laser fluence varies in-between 0.1 and 1 J/cm2 fluences, near the ablation threshold (0.1 J/cm2), the
as shown in Figure 4. Ablation starts to become intense, removal of the material is governed by the photothermal
producing depths that start from 2 nm to 12 nm per mechanism. Increase in the fluence results in
pulse. The ablation depths show an exponential growth photomechanical mechanisms responsible for the
in relation to the laser fluence applied to both the material’s removal and in thermo-elastic stresses being
computational and experimental results. developed due to fast heating. Here, the ablated material
starts being composed of big clusters. The increase of
the fluence results in a strong overheating of the
absorbed volume and in a subsequent phase explosion,
while it leads to the decomposition of the ablated
material into liquid droplets and single particles. At the
ablation areas, there is a transitional limits co-existence
of more than one ablation mechanisms being responsible
for the material’s removal [18]. Figures 3 to 5, show the
dependence of the ablation depth per pulse on the Laser
fluence. There is a good agreement between the MD and
the experimental values. The discrepancy observed
could refer to the lack of knowledge of the reliable data
for the thermo-physical parameters of the electron
system.

4.2. Laser Ablation Efficiency

Fig. 4. Computation and experimental ablation depths vs applied laser As it is defined in chapter 1, laser ablation efficiency
fluence for the second ablation region from 0.1 to 1 J/cm2 is considered the ratio of the ablated material volume to
the energy of the laser pulse. The diagram of Figure 6
In-between the limits of 1 and 10 J/cm2 lies the third can be divided in three areas based on the behavior of
ablation area. The ablation process is intense, resulting the laser efficiency.
in the production of holes whose depths vary from 12 The first area is up to laser fluence 1 J/cm2. Within
nm to 500 nm per pulse. The ablation depths continue this area the laser efficiency presents a linear increase of
having an exponential growth in relation to the laser a small slope. The second area has a range from 1 J/cm2
fluence applied to both computational and experimental up to 10 J/cm2. In contrast to the behaviour of the laser
results.
 476 P. Stavropoulos et al. / Procedia CIRP 3 (2012) 471 – 476

efficiency in the first area, within the second area the References
growth of the laser efficiency is exponential. The last
[1] Kautek, W., Kruger, J., Lenzner, M., Sartania, S., Spielmann, C.
area is dedicated for laser fluence after the value of 10 Krausz, F., 1996. Laser Ablation of Dielectrics with Pulse
J/cm2. Within this area the laser efficiency follows an Durations between 20 fs and 3ps, Applied Physics Letters 69, p.
exponential decrease. It is evident that the laser fluence 3146.
[2] Semerok, A., Chaleard, C., Detalle, V., Lacour, J.-L., Mauchien, P.,
region around 8-10 J/cm2 present the highest values of Meynadier., P., Nouvellon, C., Salle, B., Palianov, P., Perdix, M.,
laser efficiency. Thus the laser fluence of 10 J/cm2 can Petite, G., 1999. Experimental investigations of laser ablation
be considered as a threshold for laser efficiency that it efficiency of pure metals with femto, pico and nanosecond pulses,
should not be transpassed, since after this value the laser Applied Surface Science 138, p. 311.
[3] Kelly, R., Miotello, A., 1994. Laser-pulse sputtering of atoms and
efficiency only decreases. molecules Part II. Recondensation effects, Nuclear Instruments
The explanation of the laser efficiency decrease can and Methods in Physics Research Section B: Beam Interactions
be found in four main reasons. Firstly, shock waves with Materials and Atoms 91, p. 682.
[4] Stavropoulos, P., Chryssolouris, G., 2006. “Nanomanufacturing
appear and affect significantly the mechanism of the Processes and Simulation: A Critical Review", Proceedings of
laser ablation after the laser fluence increase. Secondly, the 4th International Symposium on Nanomanufacturing (ISNM),
the material volume shrinks due to the high pressures Cambridge, MA, USA, p. 46.
[5] Rieth, M., 2000. Molecular dynamics calculations for
occurred by the shock waves. Ejected atoms or nanostructured systems, University of Patras, School of
molecules ionized facilitating the plasma or plume Engineering, Engineering Science Department, PhD Thesis.
creation consisting of free electros and ions. Finally, [6] Gibbon, P., Forster, E., 1996. Short-pulse laser-plasma interactions,
Plasma Physics Control Fusion 38, p. 769.
plasma detachment reduces the absorption properties of [7] Allen, M.P., Tildesley, D.J, 1989. Computer simulation of liquids,
the material leading to a further laser efficiency Oxford Clarendon Press.
decrease. [8] Imamova, S.E., Atanasov, P.A., Nedialkov, N.N., Dausinger, F.,
Berger, P., 2005. Molecular dynamics simulation using pair and
many body interatomic potentials: Ultrashort Laser ablation of Fe,
Nuclear Instruments and Methods in Physics Research Section B:
Beam Interactions with Materials and Atoms 227, p. 490.
[9] Cheng, C., Xu, X., 2005. Mechanisms of decomposition of metal
during femtosecond Laser ablation, Physical Review B 72, p.
165415.
[10] Zhigilei, L.V., Kodali, P.B.S. Garrison, B.J., 1998 A Microscopic
View of Laser Ablation, The Journal of Physical Chemistry B
102, p. 2845.
[11] Zhigilei, L.V. Garrison, B.J, 1999. Mechanisms of Laser Ablation
from Molecular Dynamics Simulations: Dependence on the
Initial Temperature and Pulse Duration, Applied Physics A 69, p.
S75.
[12] Zhigilei, L.V. Garrison, B.J., 1997. Velocity Distribution of
Molecules Ejected in Laser Ablation, Applied Physics Letters 71,
p. 551.
[13] Nedialkov, N.N., Imamova, S.E., Atanasov, P.A., Berger, P.,
Dausinger, F., 2005. Mechanism of ultrashort laser ablation of
Fig. 6. Laser ablation efficiency as a function of the laser fluence metals: Molecular dynamics simulation, Applied Surface Science
247, p. 243.
[14] Stavropoulos, P. Chryssolouris G., 2007. Molecular Dynamics
5. Conclusion
Simulations of Laser Ablation: The Morse Potential Function
Approach, International Journal of Nanomanufacturing 1, p. 736.
This study presents results of the MD modelling and [15] Nedialkov, N.N., Atanasov, P.A., Imamova, S.E., Ruf, A., Berger,
experimentation with femtosecond laser pulses, P., Dausinger, F., 2004. Dynamics of the ejected material in
ultra-short Laser ablation of metals, Applied Physics A 79, p.
regarding the ablation mechanisms Fe, at fluences 1121.
ranging from 0.01 up to 10 J/cm2 and emphasizes on the [16] Wang, X., Xu, X., 2003. Molecular dynamics simulation of
laser efficiency. The theoretical results produced by the thermal and thermomechanical phenomena in picosecond Laser
material interaction, International Journal of Heat and Mass
MD analysis are in agreement with the experimental Transfer 46, p. 45.
results. Three main ablation areas are identified, the first [17] Alfa Aesar GmbH & Co KG Chemicals, 2006. Alfa Aesar
ranges from 0.01 up to 0.1 J/cm2, the second from 0.1 to Material Catalogue 2006-2007.
[18] Stavropoulos, P., Stournaras, A., Salonitis, K., Chryssolouris, G.,
1 J/cm2 and the last one from 1 to 10 J/cm2. The ablation 2010. Experimental and Theoretical Investigation of the Ablation
phenomenon based on computational results that are in Mechanisms During Femptosecond Laser Machining,
line with theoretical is initiated around 0.06 J/cm2. The International Journal of Nanomanufacturing 6, p. 55.
ablation efficiency behaviour is divided into three areas, [19] Yahng J. S., Chon B. H., Jeoung S. C., 2006. Nonlinear
enhancement of femtosecond laser ablation efficiency by
and the maximum ablation efficiency is identified in the hybridization with nanosecond laser, Optics Express 14, p. 9544.
area of 8-10 J/cm2.

View publication stats