Appl. Phys.

A 63, 109—115 (1996)

Femtosecond, picosecond and nanosecond laser ablation of solids

B.N. Chichkov, C. Momma, S. Nolte, F. von Alvensleben, A. Tünnermann
Laser Zentrum Hannover e.V., Hollerithallee 8, D-30419 Hannover, Germany
(Fax: #49-511/2788-100)

Received: 23 February 1996/Accepted: 27 February 1996

Abstract. Laser ablation of solid targets by 0.2—5000 ps precise material processing, since in this case the energy
Ti : Sapphire laser pulses is studied. Theoretical models deposited into the solid and the heat-affected zones are
and qualitative explanations of experimental results are minimized. We discuss and demonstrate advantages of the
presented. Advantages of femtosecond lasers for precise femtosecond-pulse lasers. We hope that our results can
material processing are discussed and demonstrated. stimulate new investigations in this field. In Sect. 1, char-
acteristic features of the low fluence laser ablation of metal
PACS: 81.15 targets in three different pulse duration regimes: fem-
tosecond, picosecond and nanosecond are considered.
The experimental setup and results are presented in
Sect. 2.
Efficient use of lasers for precise material processing is
impossible without a thorough knowledge of the funda-
mental laws governing the interaction of laser radiation 1 Theoretical background
with matter. For this goal systematic studies of the laser-
matter interaction are necessary. Due to the recent pro- During the interaction of low intensity short laser pulses
gress of laser systems, especially those based on the chir- with metal targets the laser energy is absorbed by free
ped pulse amplification (CPA) technique, such systematic electrons, due to the inverse Bremsstrahlung. Then the
studies have become possible in a very broad range of evolution of the absorbed laser energy involves thermali-
laser parameters. With CPA systems the laser pulse dura- zation within the electron subsystem, energy transfer to
tion can be varied from about one hundred femtoseconds the lattice, and energy losses due to the electron heat
to several nanoseconds leaving other laser parameters transport into the target. If we assume that the thermaliz-
unchanged. This allows to perform a very detailed analy- ation within the electron subsystem is very fast and that
sis of different nonstationary laser-matter interaction pro- the electron and the lattice subsystems can be character-
cesses. As an example, recent investigations of the damage ized by their temperatures (¹ and ¹ ), the energy trans-
threshold [1], of the ablation threshold [2], and of the e i
port into the metal can be described by the following
high-intensity laser ablation [3] can be mentioned. Note one-dimensional, two-temperature diffusion model [7, 8]:
that such systematic studies have just begun, much more
should be done for the understanding and demonstration L¹ LQ(z)
of the potential of femtosecond laser systems for precise C e "! !c (¹ !¹ )#S, (1)
e Lt Lz e i
material processing.
Recently several experiments [4—6] comparing laser L¹
ablation of solid targets by femtosecond and nanosecond C i "c (¹ !¹ ) , (2)
i Lt e i
pulses have been performed. In [4] and [5, 6] advantages
of femtosecond lasers for precise material processing with Q(z) "!k L¹ /Lz, S"I(t) Aa exp (!az) . (3)
dye and excimer laser systems have been demonstrated. In e e
this paper, we present our results on ablation and hole Here z is the direction perpendicular to the target surface,
drilling with a commercial, 10 Hz, femtosecond Ti : Sap- Q(z) is the heat flux, S is the laser heating source term, I(t)
phire laser system which provides laser pulses at 780 nm is the laser intensity, A"1!R and a are the surface
with a pulse energy of up to 100 mJ and a variable pulse transmissivity and the material absorption coefficient,
duration in the range of 0.2 to 5000 ps. Experiments are C and C are the heat capacities (per unit volume) of the
e i
performed in a low fluence regime, slightly above the electron and lattice subsystems, c is the parameter charac-
evaporation threshold. This regime is most interesting for terizing the electron-lattice coupling, k is the electron
e
110

thermal conductivity. In the above equations a thermal Note that the problem of the hot electron relaxation
conductivity in the lattice subsystem (phonon component) dynamics in metals after the excitation by a femtosecond
is neglected. The electronic heat capacity is much less than laser pulse has been intensively studied during the last
the lattice heat capacity, therefore electrons can be heated years [14—16]. It has been shown that the time scale for
to very high transient temperatures. When the electron the fast electron cooling and a considerable energy trans-
temperature (in units of energy) remains smaller than the fer to the lattice is of the order of 1 ps.
Fermi energy, the electron heat capacity and the The significant evaporation occurs when C ¹ be-
i i
nonequilibrium electron thermal conductivity are given comes larger than o), where o is the density and ) is
by C "C@ ¹ (where C@ is a constant) and k "k (¹ )· the specific (per unit mass) heat of evaporation. Using (7),
e e e e e 0 i
¹ /¹ (where k (¹ ) is the conventional equilibrium ther- we can write the condition for strong evaporation in the
e i 0 i
mal conductivity of a metal) [9—11]. Expressions for the form
coupling constant c are given in [7, 12] and results of
recent measurements in [11, 13, 14]. F 5F exp (az) , (8)
a th
Equations (1—3) have three characteristic time scales q ,
e where F Ko)/a is the threshold laser fluence for evapo-
th
q and q , where q "C /c is the electron cooling time,
i L e e ration with femtosecond pulses. Then the ablation depth
q "C /c is the lattice heating time (q @q ) and q is the
i i e i L per pulse ¸ is
duration of the laser pulse. These parameters define three
different regimes of the laser-metal interaction which we ¸ K a~1 ln (F /F ) . (9)
call femtosecond, picosecond and nanosecond regimes. a th
The logarithmic dependence of the ablation depth on the
laser pulse fluence is well known for the laser ablation of
Femtosecond pulses organic polymers. Recently the logarithmic dependence of
the ablation depth per pulse has been demonstrated for
First we consider the case when the laser pulse duration is metal targets with femtosecond KrF-laser pulses [5].
shorter than the electron cooling time, q @q . For t@q , Due to the very short time scales involved in the
L e e ablation with femtosecond laser pulses the ablation pro-
which is equivalent to C ¹ /tAc¹ , the electron-lattice
e e e cess can be considered as a direct solid-vapor (or solid-
coupling can be neglected. In this case (1) can be easily
solved. Since the general solution of this equation is quite plasma) transition. In this case the lattice is heated on
complicated, we neglect the electron heat conduction term a picosecond time scale which results in the creation of
in our formulas. This can be done when the following vapor and plasma phases followed by a rapid expansion in
condition is fulfilled D q (a~2, where D "k /C is the vacuum. During all these processes thermal conduction
e L e e e into the target can be neglected in a first approximation.
electron thermal diffusivity. In this case (1) reduces to
These advantages of femtosecond laser pulses allow very
C@ L¹2 /Lt"2I a exp (!az) (4) precise and pure laser-processing of metals (and other
e e a solids) which is experimentally demonstrated below.
and gives

A B
2I a 1@2
¹ (t)" ¹2# a t exp (!az) . (5) Picosecond pulses
e 0 C@
e
Here I(t)"I is assumed constant, I "I A, and Now we turn to the discussion of ablation with
0 a 0 picosecond laser pulses when the following condition is
¹ "¹ (0) is the initial temperature. At the end of the
0 e fulfilled q @q @q .
laser pulse the electron temperature is given by e L i
At a time tAq which is equivalent to C ¹ /t@c¹ ,
e e e e

A B
2F a 1@2 (1) for the electron temperature becomes quasistationary,
¹ (q )K a exp (!z/d) , (6)
e L C@ and (1—3) reduce to
e
where ¹ (q )A¹ is assumed, F "I q is the absorbed L/Lz (k L¹ /Lz)!c(¹ !¹ )#I a exp (!az)"0, (10)
e L 0 a a L e e e i a
laser fluence, and d"2/a is the skin depth. t

P A B
The evolution of the electron and lattice temperatures 1 t!h
¹" exp ! ¹ (h) dh#¹ . (11)
after the laser pulse is described by (1—3) with S"0. Initial i q q e 0
conditions for the electron and lattice temperatures are i i
0
given by (6) and ¹ "¹ . After the laser pulse the elec-
i 0 Here (2) for the lattice temperature is written in the inte-
trons are rapidly cooled due to the energy transfer to the
lattice and heat conduction into the bulk. Since this elec- gral form. These equations describe heating of metal tar-
gets by the laser pulses with q Aq . When the condition
tron cooling time is very short, (2) can be written as L e
t@q is fulfilled, (11) can be simplified due to the quasi-
¹ K¹ (q ) t/q (here the initial lattice temperature is
i e L i i
neglected). The attainable lattice temperature is deter- stationary character of the electron temperature. Neglect-
ing ¹ , we get
mined by the average cooling time of the electrons 0
qa"C@ ¹ (q )/2c and is given by ¹ ^ ¹ (1!exp (!t/q )) ^ (t/q ) ¹ .
e e e L i e i i e
(12)
C@ F a As can be seen from this expression, in the picosecond
¹ ^¹2 (q ) e K a exp (!az) . (7)
i e L 2C C regime the lattice temperature remains much less than the
i i
 111

electron temperature. This allows to neglect the lattice can be written as

temperature in (10). The analysis of (10, 12) is especially
simple when the condition k ¹ a2@c¹ is fulfilled. o)D1@2
e e e I'I \ , F'F \o)D1@2]q1@2 (15)
In this case the electron cooling is due to the energy th q1@2 th L
L
exchange with the lattice. The electron temperature and
the lattice temperature at the end of the laser pulse are for laser intensity and fluence, respectively. The threshold
given by laser fluence which is necessary for evaporation with long
laser pulses grows as q1@2 .
L
I a F a In case of ablation with long laser pulses there is
¹ ^ a exp (!az), ¹ ^ a exp (!az) . (13)
e c i C enough time for the thermal wave to propagate into the
i target and to create a relatively large layer of melted
Note that the attainable lattice temperature after the laser material. In this case the evaporation occurs from the
pulse is again determined by the electron cooling time. liquid metal, which makes precise material processing of
Since q @q , the attainable lattice temperature and metal targets in vacuum with nanosecond pulses very
e L complicated.
the lattice temperature at the end of the laser pulse are
approximately equal. In femtosecond and picosecond
regimes (7) and (13) give the same expressions for the
lattice temperature. Therefore, the condition for strong 2 Experimental setup and results
evaporation given by (8), the fluence threshold and
the ablation depth per pulse given by (9) remain un- Now we turn to the discussion of experimental results on
changed. a low fluence laser ablation of metals and other solids. In
Thus, the logarithmic dependence of the ablation our experiments a commercial femtosecond Ti : Sapphire
depth on the laser pulse fluence is also possible in the laser system (BMI Alpha 10A) based on the chirped-pulse
picosecond range. In our derivations we have neglected amplification (CPA) technique [21] is used. A detailed
the electron heat conduction into the target. This is a very description of the principal setup is given in [22]. This
crude assumption for the description of laser ablation of system provides laser pulses at 780 nm with a variable
metal targets in the picosecond regime. Laser ablation in pulse energy of up to 100 mJ. Due to the CPA technique
this case is accompanied by the electron heat conduction the pulse duration can be varied from 200 fs up to 400 ps.
and formation of a melted zone inside the target. In spite In this pulse duration range the spectral pulse width
that at the surface we can again consider evaporation as remains constant (approximately 8 nm). Pulse duration
a direct solid-vapor (or solid-plasma) transition, the pres- measurements for pulses shorter than 10 ps are performed
ence of the liquid phase inside the target reduces the by a background free second order autocorrelator and for
precision of laser processing of metals in this regime (see pulses longer than 10 ps by a picosecond streak camera
below). (Hadland, IMACON 500). Pulse widths of 3—5 ns are
obtained when the regenerative amplifier (see [22]) is not
seeded by the femtosecond oscillator (Coherent, Mira
Nanosecond pulses Basic). In this case the regenerative amplifier operates as
an oscillator, and the spectral width of the generated
Here we briefly discuss ablation with nanosecond laser pulses is significantly reduced. The time durations of the
pulses when the condition q Aq is fulfilled. In this case nanosecond pulses have been measured by a photodiode
L i in combination with a fast sampling oscillograph and by
the electron and lattice temperatures are equal
¹ "¹ "¹, and (1—3) reduce to the streak camera.
e i Our experiments are performed in the low fluence
C L¹/Lt"L/Lz (k L¹/Lz)#I a exp (!az) . (14) regime (F"0.1—5 J/cm2) with an imaging geometry. An
i 0 a aperture (d"5 mm), mounted in the beam pass, is imaged
Laser heating of metal targets by long laser pulses has (with demagnification factor of ^1/30) onto the target
been a subject of many experimental and theoretical stud- surface by a f"140 mm suprasil lense. The laser beam
ies [17—20]. In this regime the absorbed laser energy first diameter is approximately 20 mm. As target materials
heats the target surface to the melting point and then to steel, copper, AlN and silicon plates are used. These plates
the vaporization temperature. Note that metals need are attached to a computer controlled x,y,z-translation
much more energy to vaporize than to melt. During the stage which is mounted in a vacuum cell at a pressure
interaction the main source of energy losses is the heat below 10~4 mbar. The number of pulses which are neces-
conduction into the solid target. The heat penetration sary to drill through the target plate is controlled by
depth is given by l\(Dt)1@2, where D is the heat diffusion a photodiode mounted behind the targets.
coefficient, D"k /C . Note that for long-pulse laser abla- First we present our results on the laser processing of
0 i
tion of metal targets the condition Dq a2A1 is usually metal targets. We compare holes drilled in 100 lm thick
L
fulfilled. The energy deposited inside the target per unit steel foils (in vacuum) with 104 laser pulses in three differ-
mass is given by E \I t/ol. When at a certain moment ent regimes: femtosecond, picosecond and nanosecond. In
m a
t"t this energy becomes larger than the specific heat of Fig. 1 schematic of femtosecond-pulse laser ablation and
th
evaporation ), significant evaporation occurs. From the the hole drilled with 200 fs, 120 lJ, F"0.5 J/cm2 laser
condition E \) we get t \D ()o/I)2 (see [17]). Thus, pulses are shown. As can be seen, there is no trace of the
m th
the condition for strong evaporation, E ') (or q 't ), molten material. Only a vapor dust ring around the hole.
m L th
112

these figures. The presence of liquid phase leads to an

unstable drilling process (see Fig. 2a). In case of ablation
with nanosecond pulses there is enough time for the
thermal wave to propagate into the metal target and
to create a relatively large molten layer. In this case the
target material is removed both in vapor and liquid
phases, since the vaporization process creates a recoil
pressure that expels the liquid. In Fig. 2b a ‘‘corona’’
created due to the recoil vapor pressure is clearly seen.
Note that these are the best results which we obtain with
80 ps and 3.3 ns laser pulses at fluences as low as possible.
When the laser fluence is reduced further the drilling
through the 100 lm steel plate in vacuum becomes im-
possible.
Comparing Fig. 1 and Fig. 2, the advantages of fem-
tosecond-pulse lasers for precise material processing be-
come evident. Moreover, due to the absence of thermal
losses in the femtosecond regime, holes in metal targets
can be drilled with much lower laser fluences.
Below we present additional illustrative information
on femtosecond-pulse laser ablation of different targets
with the second harmonic of Ti : Sapphire laser radiation
(j"390). The second harmonic is used to minimize dif-
fraction effects and to improve the quality of image projec-
tion. In Fig. 3 the development of the ablation process
with the increasing number of 250 fs, 0.5 mJ, and
Fig. 1. Schematic of femtosecond-pulse laser ablation and a SEM F"2.5 J/cm2 laser pulses a) 10, b) 100, c) 103 and
photograph of a hole drilled in a 100 lm thick steel foil with 200 fs, d) 5]103 is shown. The target is a 0.5 mm steel plate. In
120 lJ, F"0.5 J/cm2 laser pulses at 780 nm Fig. 3c the creation of characteristic structures is clearly
seen. These structures appear due to the instability of
In Fig. 2 schematic of nanosecond-pulse laser ablation a plane evaporation front [23].
and the holes drilled with (a) 80 ps, 900 lJ, F"3.7 J/cm2; In Fig. 4 the evolution of femtosecond-pulse laser
and (b) 3.3 ns, 1 mJ, and F"4.2 J/cm2 laser pulses are ablation of a 1 mm thick copper target is shown with:
shown. The trace of the molten material can be seen in a) 10, b) 100, c) 103, and d) 3]104 pulses. In Fig. 5

Fig. 2a, b. Schematic of

nanosecond-pulse laser ablation
and holes drilled in a 100 lm
thick steel foil with (a) 80 ps,
900 lJ, F"3.7 J/cm2; and
(b) 3.3 ns, 1 mJ, and
F"4.2 J/cm2 laser pulses at
780 nm
a b
 113

Fig. 3a–d. Femtosecond-pulse

laser processing of a 0.5 mm
steel plate with 250 fs, 0.5 mJ,
and F"2.5 J/cm2 second
harmonic radiation
(j"390 nm) and different
number of pulses: (a) 10,
(b) 100, (c) 1000 and (d) 5000
laser pulses

Fig. 4a–d. Evolution of

femtosecond-pulse laser
ablation of a 1 mm thick copper
target with: (a) 10, (b) 100,
(c) 103, and (d) 3]104 pulses.
Laser parameters are the same
as in Fig. 3

results of laser ablation of a 0.3 mm thick silicon target are In Fig. 6 the ablation of a 0.8 mm AlN target with: a) 10,
demonstrated with: a) 10, b) 100, c) 5]103, and d) 104 b) 103, and c) 3.5]104 laser pulses is illustrated. The
pulses. Redeposition of the ablated material on the target laser parameters in Figs. 4, 5 and 6 are approximately the
surface is much stronger than in the case of metal targets. same as in Fig. 3.
114

Fig. 5a–d. Laser ablation of

a 0.3 mm thick silicon target
with: (a) 10, (b) 100, (c) 5]103,
and (d) 104 pulses. Laser
parameters are the same as in
Fig. 3

Fig. 6a–c. Ablation of a 0.8 mm

AlN target with: (a) 10, (b) 103,
and (c) 3.5]104 laser pulses.
Laser parameters are
approximately the same as in
Fig. 3

Closing this section we summarize the main features absence of the liquid phase allows better control during
of femtosecond laser material processing: very rapid the drilling process. Therefore, the reproducibility
creation of vapor and plasma phases, negligible heat of our results with femtosecond laser pulses is very
conduction and the absence of liquid phase. The good.
 115

3 Conclusion 7. M.I. Kaganov, I.M. Lifshitz, L.V. Tanatarov: Sov. Phys. —JETP
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