Applied Surface Science 249 (2005) 322–331

www.elsevier.com/locate/apsusc

Pulse width and energy influence on laser micromachining

of metals in a range of 100 fs to 5 ps
R. Le Harzica,c,*, D. Breitlinga, M. Weikerta, S. Sommera, C. Föhlb,
S. Valettec, C. Donnetc, E. Audouardc, F. Dausingera
a
Institut für Strahlwerkzeuge (IFSW), Universität Stuttgart, Pfaffenwaldring 43, 70569 Stuttgart, Germany
b
Forschungsgesellschaft für Strahlwerkzeuge mbH (FGSW), Nobelstrasse 15, 70569 Stuttgart, Germany
c
Laboratoire Traitement du Signal et Instrumentation (TSI), UMR CNRS 5516, Bat F, 10 rue Barrouin, 42000 Saint Etienne, France
Received 7 July 2004; received in revised form 23 September 2004; accepted 7 December 2004
Available online 21 January 2005

Abstract

Micromachining of steel, Cu and Al is studied. Ablation depths per pulse are deduced for laser pulse durations between
100 fs and 5 ps for fluences in the range of 150 mJ cm
2 to 20 J cm
2. The evolution of ablation rates allows to evidence a
low and a high fluence regime. Ablation thresholds and penetration depths are deduced as functions of pulse duration. While
in the low fluence regime the penetration depth is close to the theoretical optical penetration depth, at higher fluences the
effective heat penetration depth is 10–20 times bigger with also higher ablation thresholds. Even in the femtosecond range
thermal ablation processes occur and reduce quality, accuracy and efficiency of micromachining. Additionally, the latter are
influenced by strong beam distortions due to nonlinear interaction between the radiation and the atmospheric gas. In the case
of steel and Cu, the pulse duration seems not to affect microprocessing, but it is demonstrated to play a role for Al for pulses
between 1 and 5 ps.
# 2004 Elsevier B.V. All rights reserved.

PACS: 79.20.Ds; 42.62.Cf; 81.65.Cf

Keywords: Laser; Femtosecond; Picosecond; Ablation; Pulse duration; Energy; Heat penetration; Thermal effects

1. Introduction

With the increasing availability of ultra short laser

* Corresponding author. Present address: JenLab GmbH, Schil-
lerstr. 1, 07745 Jena, Germany, c/o Fraunhofer Institute of Biome-
dical Technology (IBMT), Ensheimer Str. 48, St Ingbert, Germany.
Tel.: +49 6894 9903 815; fax: +49 6894 9903 817.
E-mail address: leharzic@jenlab.de (R. Le Harzic)
URL: www.jenlab.de.
pulses and their application in the field of material
structuring or ablation, there is growing evidence that
high precision processing with pulse widths in the
femtosecond to picosecond time ranges demonstrates
in many cases a significant improvement in quality for

0169-4332/$ – see front matter # 2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.apsusc.2004.12.027
 R. Le Harzic et al. / Applied Surface Science 249 (2005) 322–331
various materials such as metals in comparison to
nanosecond or longer-laser pulses [1–7]. If ultra
short laser pulses can eventually play a role in
industrial materials microstructuring, it is obviously
desirable to understand the limitations in processing
possibilities and important parameters determining
these limitations for various classes of materials in
order to decide on the optimum laser system for a
particular application. The quality of the structuring
or processing is, however, extremely material and
wavelength dependent and the shorter laser pulse is
not always the better for the precision and controll-
ability of the material ablation. It is commonly said
for the case of metals that no drastical changes in
terms of quality and thermal effects are observed up
to 10 ps pulse duration [8,9]. For an industrial
transfer, the main question of using ultra short (fs) or
short pulses (few ps) is open because of a higher
simplicity of amplified picosecond laser chains and
their better cost-effectivness and reliability. In this
paper we report on the laser pulse width and energy
dependence of ablation in a range of 100 fs to 5 ps
for three different metals, copper, aluminum and
steel known for their different thermo-mechanical
properties, and we bring some quantitative data to
help answering this crucial question.
2. Experimental setup
The short-pulse laser system used in our experi-
ment consists on a femtosecond Ti–sapphire laser.
Pulses are extracted from an oscillator (‘‘Mai Tai’’,
Spectra Physics, 8.75 nJ/pulse, 80 MHz, 800 nm and
100 fs). An additional stage (‘‘Hurricane’’, Spectra
Physics) including an optical pulse stretcher, a
regenerative amplifier pumped by a diode Nd:YLF
laser and a pulse compressor, was used to obtain
pulses centered near 800 nm in wavelength. A single
pulse energy of 1 mJ is typically obtained at 1 kHz
repetition rate and with a duration of 120 fs, which
was measured using a Clark MXR autocorrelator. The
laser pulses were p polarized.
To allow a low energy regime (typically 0.05–
0.5 mJ/pulse), the laser pulses were obtained from the
regenerative amplifier and a system with two
polarizing plates was introduced in the laser beam
path to decrease and control the energy required.
323
Metal samples of copper (purity: 99.9%), alumi-
num (purity: 99.95%) and steel (Fe/Cr18/Ni10) with
thickness of 500 mm were placed on a motorized
translation stage with 48 of displacement, x, y, z and u
to allow a perfect control in the space and a high
precision (accuracy of the translation stage is given to
be 0.5 mm).
An accurate imaging system by means of a far-field
CCD camera allows to visualize precisely the zone of
ablation on the sample. Grooves were machined by
1–20 scans in front of the fixed beam. In all results
presented here, the scan speed of the motorized stages
was fixed at 2 mm s
1 to obtain reproducible and
correct average overlapping pulses.
The laser beam was focalized down with a 100 mm
focal objective and achieved a spot diameter greater
than 18 mm. Several series on each sample were
machined from 0.2 to 30 J cm
2 at different pulses
widths from 100 fs to 5 ps (upper limit of the
CPA system), which were obtained by varying the
gratings distance of the compressor and controlled by
accurate autocorrelation measurements. Fluences
were deduced from a Gaussian spatial shape and
were averaged for each measurement.
To analyse depths and roughness of the grooves, an
accurate mechanical profilometer and laser scanning
microscopy (LSM) were used. Optical microscopy
and (a more precise) scanning electron microscopy
(SEM) allow great visual comparison in term of
quality, structure and removed matter.
3. Results
In Fig. 1 the laser fluence dependence of the
ablation rate in nm per pulse is shown for different
pulse durations of 100, 250, 500, 1000, 2500 and
4500 fs in (a) steel, (b) copper and (c) aluminum.
Ablation rates have been deduced by average
calculations including pulse overlap, scan speed, spot
diameter, repetition rate and depth. As a first remark,
the graphs present a huge database for ablation
knowledge in metals and can be used to deduce the
parameters necessary for applications in microma-
chining, microengraving or etching. As it has already
been mentioned in the literature [2,10], we observe
two regimes of ablation for the different metals: for
low fluences up to 1–1.5 J cm
2 and (for) high
324 R. Le Harzic et al. / Applied Surface Science 249 (2005) 322–331

fluences up to 20 J cm
2. The ablation depth per pulse
can be described by the well-known logarithmic law,
e.g. Eq. (1) [11]:
L ¼ l lnðF=Fth Þ
where l = a
1 is the optical penetration depth and Fth
the ablation threshold fluence. It has to be noticed that
this threshold is extrapolated from the ablation data,
and is usually different from a direct measurement of
the threshold with dedicated experiments.
If we take a close look at the low fluence regime in
Fig. 2, the ablation rate decreases with the pulse
duration, additionally these results show that increas-
ing the pulse duration also increases the threshold
fluence. If we pay attention to the slope of the straight
lines, for the case of steel (Fig. 2(a)) there is no break
of the slopes and they seem to be quite parallel from
100 fs to 4.5 ps, even though the absolutes values
decrease slowly and regularly with increasing pulse
(1)
duration. That is also quite true for the case of Cu
(Fig. 2(b)). The behaviour of Al (Fig. 2(c)), however,
seems to be different. The evolution of the slopes
is much more chaotic and they strongly decrease
above 1 ps.
For all metals, by fitting the data shown in Figs. 1
and 2 using Eq. (1), we can deduce directly fluence
thresholds and energy penetration depths. The slopes
of the straight lines provide the values of the
penetration depths and the interception points repre-
sent fluence thresholds. These results are shown in

Fig. 1. Ablation rate (nm/pulse) vs. the incident laser fluence for different pulse durations of 100, 250, 500, 1000, 2500 and 4500 fs for (a) steel,
(b) copper and (c) aluminum.
 R. Le Harzic et al. / Applied Surface Science 249 (2005) 322–331 325

Fig. 3. It displays fluence threshold and penetration
depth dependences as functions of the pulse duration
for steel (Fig. 3(a)), Cu (Fig. 3(b)) and Al (Fig. 3(c))
for the low (in insert) and high fluence regimes. We
can deduce for fluences less than 1.6 J cm
2 that steel
has a very low fluence threshold ranging from
20 mJ cm
2 at 100 fs to 50 mJ cm
2 at 4.5 ps in
comparison to Al and Cu, which have fluence
thresholds from 110 to 190 mJ cm
2, respectively,
at 100 fs to 250 and 600 mJ cm
2 at 4.5 ps,
respectively. These results are in quite good agreement
with literature [4,10–13]. Accordingly, increasing
pulse duration reduces the effective energy penetration
depth. As mentioned by Nolte et al. [2], both effects
can be explained by plasma shielding of the laser
radiation, and increased heat conduction losses. The
machining of steel, being one of the most widely used
materials for practical applications, provides good
results. However, steel being an alloy it is difficult to
give a detailed physical explanation. Moreover, we
have to keep in mind in the analysis of the results that
the simple model used for a first exploitation of the
ablation depth measurements cannot take into account
the complexity of mechanisms that occurs near the
threshold, where more detailed studies are needed. In
the same way, for the high fluence range it is known
that complex mechanisms (such as plasma effects and
shock waves) have to be taken into account, and
saturation in the ablation rate evolution is usually
observed [14].

Fig. 2. Details of the ablation rate (nm/pulse) vs. the incident laser fluence in the low fluence regime for pulse durations of 100, 250, 500, 1000,
2500 and 4500 fs for (a) steel, (b) copper and (c) aluminum. The solid lines represent the best fits according to Eq. (1).
326 R. Le Harzic et al. / Applied Surface Science 249 (2005) 322–331

Fig. 3. Comparison of fluence threshold and penetration depth for the high and low (insert) fluence regimes for pulse durations of 100, 250, 500,
1000, 2500 and 4500 fs for (a) steel, (b) copper and (c) aluminum (the left-hand scale of each graph represents the fluence threshold and the right-
hand scale the penetration depth).

4. Discussion At low fluences in the case of steel, one can observe

For Cu and Al at 100 fs, experimental results of
penetration depth for low fluences are found to be two
or three times higher than the theoretical optical
penetration depth as reported in Table 1. With
increasing pulse duration, the penetration depths are
relatively constant for Cu but strongly decreases for
Al. For high fluences, quite similar phenomena are
observed but the values for the penetration depths are
much higher. Ablation thresholds are found to be 1 and
1.7 J cm
2, respectively, for Al and Cu which exceed
those of the low fluence regime by a factor of 10.
Penetration depths are higher than the theoretical
optical penetration depth by a factor of 10–20.
a relatively constant penetration depth with the
increasing pulse duration. For Al, there is a
pronounced break down taking place at about 1 ps.
We conclude, hence, that for steel and Cu, no
modification of the ablation mechanism should occur
for pulse duration below 5 ps. In the case of Cu it can
be explained by a weak electron–phonon coupling
constant g (Table 1), which governs an electron–
phonon relaxation time tep in the range of 10 ps [15].
Thermodynamic equilibrium between the electron gas
and the lattice, i.e. heat transfer, cannot be reached
before 10 ps. Pulse duration has then a significant
effect for values longer than 10 ps. For Al, with a
stronger electron–phonon coupling, tep is reached at
 R. Le Harzic et al. / Applied Surface Science 249 (2005) 322–331 327

Table 1
Data from literature for Au, Cu, Al, Ni and Fe
Metal
Au Cu Al Ni Fe
6
3
1
Thermal capacity, Ci (10 J m K ) 2.5 3.46 2.43 4.1 3.5
Electron specific heat coefficient, Ce0 (J m
3 K
2) 71 97 135 1065 498
Electron–phonon coupling constant, g (1016 W m
3 K
1) 2.1 10 56.9 36
Melting temperature, Tm (K) 1337 1358 933 1728 1811
Vaporization temperature, Tv (K) 3081 2835 2740 3003 3134
Thermal conductivity, K [W m
1 K
1] 318 401 238 91 80
Thermal diffusivity, k [cm2 s
1] 1.26 1.16 0.98 0.18 0.23
Absorption coefficient, a (105, cm
1) 6.9 6.3 5.9 6.6 5.2
Optical penetration depth, l (nm) 11.8 13.5 7.5 14.5 18.3
Latent heat of melting, Lm (J g
1) 64.9 205 388 292 272
Latent heat of evaporation, Lv (J g
1) 1738 4796 10800 6378 6095

approximately 1 ps [15]. Energy transfer and a
potential thermal expansion can only occur for pulse
durations longer than 1 ps. This is in strong agreement
with observed decrease of the energy penetration
depth. The fact that the penetration depth decreases
with pulse duration for an irradiation at the same
energy density indicates that energy is absorbed
differently and probably not diffused in the bulk. The
deposited energy stays in the vicinity of the surface
and contributes to thermal effects or structural
modifications. For higher pulse energies, however,
the influence of electronic heat conduction certainly
becomes important and the second ablation regime
appears with deeper penetration depths.
One can use similar arguments to comment the
scanning electron microscopy results shown in Fig. 4
(low fluence regime) and Fig. 5 (high fluence regime).
One can observe a superior ablation quality, little
matter removal but an observable difference for Al at
100 fs (Fig. 4(e)) and 4.5 ps (Fig. 4(f)) in terms of
quality on the borders of the grooves, which confirms
our previous observations on ablation rates. In the high
fluence regime no evident difference can be observed
in all cases, but one can observe stronger structural
modifications than in the low fluence regime for Al.
One might think that completely melt-free processing
should be impossible for metal machining, however, it
is clear that the reduction of fluence minimizes the
melt layer thickness. Heat affected zones have been
found to be very small for short laser pulses in
comparison to nanosecond laser pulses in the low
fluence regime [16,17] but at high fluences thermal
effects even occur in the femtosecond range and thus
can strongly affect the microprocessing efficiency
[8,18].
Finally we can compare the values of the critical
pulse width, determined from equations reported in
Table 2 [19,20,21]. It is defined as the time separating
ultra short from short or long laser pulse durations. For
pulses longer than the critical pulse width the
penetration depth is described by the well-known
equation [22,23], which depends on thermal diffusiv-
ity k and pulse duration tH, expressing a linear thermal
law:
pffiffiffiffiffiffiffiffi
lth ¼ 2 ktH (2)
Even if the estimated values differ strongly, obviously
the critical pulse width is much longer for Cu, which is

Table 2
Critical pulse width (ps) for Cu and Al deduced from literature, (a) [19], (b) [20] and (c) [21]
Metal (a) tcl ¼ ð8=pÞ1=4 ðCi3 =Ce0 Tm Þ1=2 =g (ps) (b) tc2 = Ci/g (ps) (c) tc3 = (1/a)2/2k (ps)

Cu 224 34.6 0.69

Al 23.7 4.27 1.47
328 R. Le Harzic et al. / Applied Surface Science 249 (2005) 322–331

Fig. 4. SEM photographs of grooves machined by 10 scans at a scan speed of 2 mm s
1 and with an energy density of 0.8 J cm
2 for two
different pulse durations of 120 fs (left) and 4.5 ps (right) for (a, b) steel, (c, d) copper and (e, f) aluminum.

of the order of tens of picoseconds to 200 ps, and thus expansion in the case of Al after 1–4.5 ps with calcu-
relatively far from the maximal pulse width of 4.5 ps lated values of 1–23 ps. These results for Al are in
used in our ablation experiments. Coincidence is agreement with experimental results of Zhu [24] who
found with our conclusion of a possible thermal estimated a critical pulse width of 3.7 ps. Once again,
 R. Le Harzic et al. / Applied Surface Science 249 (2005) 322–331 329

Fig. 5. SEM photographs of grooves machined by 20 scans at a scan speed of 2 mm s
1 and with an energy density of 18 J cm
2 for two different
pulse durations of 120 fs (left) and 4.5 ps (right) for (a, b) steel, (c, d) copper and (e, f) aluminum.

we can conclude that, in the investigated energy 5. Conclusion

density range, the ablation mechanisms are governed
by electron–phonon coupling, which should allow to Investigations of the pulse width and energy
manage the pulse duration effects in metals. density dependence on laser micromachining of
330 R. Le Harzic et al. / Applied Surface Science 249 (2005) 322–331
metals in a range of 100 fs to 5 ps are presented.
Two fluence regimes have been observed as already
described in literature. Ablation thresholds and
penetration depths are deduced as functions of the
pulse duration. Increasing pulse duration increases
the threshold fluence and reduces the effective
energy penetration depth. While in the low fluence
regime the penetration depth is close to the
theoretical optical penetration depth and ablation
thresholds are weak, at higher fluences the effec-
tive heat penetration depth is 10–20 times bigger
with also higher ablation thresholds. Even in the
femtosecond range, thermal ablation processes occur
and reduce quality, accuracy and efficiency of
micromachining. One can conclude that at high
enough fluences a simple thermal model can be used
to describe, and thus control ablation. As expected,
in the low fluence regime the quality is increased and
thermal diffusion is minimized, but a more refined
model has to be used to describe ablation. Never-
theless, the distinction between the two regimes can
be evidenced by the measurements presented in this
paper in each case. For steel and Cu, the pulse
duration does not seem to affect microprocessing,
but it is demonstrated to play a role for Al for pulses
from 1 to 4.5 ps. The best results are obtained in the
low fluence regime but associated with significantly
lower ablation rates. This loss of efficiency must be
compensated by higher pulse repetition rates. Indeed,
today the lack of available laser sources with high
average power and repetition rates and the resulting
low processing efficiency are still the strongest
limitations for the introduction of ultra short laser
pulses in industry. As a first tentative conclusion,
pulse duration up to 5–10 ps do not drastically affect
micromachining of metals since in these cases, the
main mechanism of ablation in the optimal energy
range for micromachining (between the low fluence
range near the threshold and the high fluence range
where the ablation rates saturate) can be considered
as purely thermal in nature as demonstrated also by
theoretical results [25]. In this frame, the effect of
pulse duration can be understood and simulated
using the usual thermal characteristics of metals.
Of course, the specific properties of each metal have
to be considered as shown by the experimental
differences between aluminum and copper. A
specific study of the Al case should be of special
interest with a more detailed study of the role of the
energy density [26]
Acknowledgements
The authors would like to thank the French Région
Rhônes-Alpes and the Bundesministerium für Bildung
und Forschung bmb + f (German Ministry for Educa-
tion and Research, project PRIMUS (FZK 13 N 7710/
6)) for financial support.
References
[1] C. Momma, B.N. Chichkov, S. Nolte, F. von Alvensleben, A.
Tunnermann, H. Welling, B. Wellegehausen, Opt. Commun.
129 (1996) 134.
[2] S. Nolte, C. Momma, H. Jacobs, A. Tunnermann, B.N. Chich-
kov, B. Wellegehausen, H. Welling, J. Opt. Soc. Am. B 14
(1997) 2716.
[3] H.K. Tönshoff, F. Von Alvensleben, A. Ostendorf, G. Kamlage,
S. Nolte, IJEM Rev. (1999) 1.
[4] X. Zhu, A. Naumov, D. Villeneuve, P. Corkum, Appl. Phys. A
69 (1999) 1.
[5] M. Weikert, C. Föhl, F. Dausinger, Proc. SPIE 5063 (2003)
208.
[6] C. Föhl, F. Dausinger, Proc. SPIE 5063 (2003) 346.
[7] R. Le Harzic, N. Sanner, N. Huot, C. Donnet, E. Audouard, P.
Laporte, Proc. SPIE 5063 (2003) 352.
[8] F. Dausinger, Proc. SPIE 4830 (2003) 471.
[9] D. Breitling, A. Ruf, F. Dausinger, Proc. SPIE 5339 (2004)
49.
[10] B. Le Drogoff, F. Vidal, Y. Von Kaenel, M. Chaker, T.W.
Johnston, S. Laville, J. Appl. Phys. 89 (2004) 8247.
[11] S. Preuss, A. Demchuk, M. Stuke, Appl. Phys. A 61 (1) (1995)
33.
[12] S. Amoruso, X. Wang, C. Altucci, C. de Lisio, M. Armenante,
R. Bruzzese, R. Velotta, Appl. Phys. Lett. 77 (23) (2000) 3728.
[13] J. Jandeleit, G. Urbasch, H.D. Hoffmann, H.G. Treusch, E.W.
Kreutz, Appl. Phys. A 63 (2) (1996) 117.
[14] J.Ph. Colombier, E. Audouard, P. Combis, F. Bonneau, R. Le
Harzic, Proc. SPIE 5448 (2004) 853.
[15] S. Valette, Ph.D. Thesis, Saint Etienne, 2003.
[16] R. Le Harzic, N. Huot, E. Audouard, C. Jonin, P. Laporte, S.
Valette, A. Fraczkiewicz, R. Fortunier, Appl. Phys. Lett. 80
(2002) 3886.
[17] S. Valette, E. Audouard, R. Le Harzic, N. Huot, P. Laporte, R.
Fortunier, Appl. Surf. Sci. 239 (2005) 381.
[18] A. Luft, U. Franz, A. Emsermann, J. Kaspar, Appl. Phys. A 63
(1996) 93.
[19] P.B. Corkum, F. Brunel, N.K. Sherman, T. Srinivasan-Rao,
Phys. Rev. Lett. 61 (1988) 2886.
 R. Le Harzic et al. / Applied Surface Science 249 (2005) 322–331 331

[20] B.N. Chichkov, C. Momma, S. Nolte, F. von Alvensleben, A.
Tunnermann, Appl. Phys. A 63 (1996) 109.
[21] G.A. Mourou, D. Du, S.K. Dutta, V. Elner, R. Kurtz, P.R.
Lichter, X. Liu, (1997) US Patent 5,656,186.
[22] J.F. Figueira, S.J. Thomas, IEEE J. Quantum Electron. 18
(1982) 1381.
[23] M. Sparks, E. Loh, J. Opt. Soc. Am. 69 (1976) 847.
[24] X. Zhu, Appl. Surf. Sci. 167 (2000) 230.
[25] J.P. Colombier, P. Combis, F. Bonneau, E. Audouard, R. Le
Harzic, to be published in Phys. Rev. B.
[26] R. Le Harzic, D. Breitling, M. Weikert, S. Sommer, C. Foehl,
S. Valette, C. Donnet, E. Audouard, F. Dausinger, Proc. SPIE,
in press.