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Kennedy 1995 I
Kennedy 1995 I
Abstract-An analytic, first-order model has been developed formation, bubble collapse, and propagation of shock and
to calculate irradiance thresholds for laser-induced breakdown acoustic waves [6], [7], [10]-[15]. Measurement and modeling
(LIB) in condensed media, including ocular and aqueuus media.
of LIB thresholds in ocular and aqueous media seems the
The model is derived from the simple rate equation formalism
obvious starting point.
of Shen for cascade breakdown in solids and from the the
ory of multiphoton ionization in condensed media developed This paper documents the development of an analytic, first
by Keldysh. Analytic expressions have been obtained for the order model for computation of LIB thresholds in condensed
irradiance thresholds corresponding to multiphoton breakdown, media, including ocular and aqueous media. The model is
to cascade breakdown, and to initiation of cascade breakdown by
based on the simple rate equation formalism of Shen [16] for
multiphoton ionization of seed electrons (multiphoton initiation
threshold). The model has been incorporated into a computer
cascade breakdown in solids and on the model developed by
code and code results compared to experimentally measured Keldysh [17] for multiphoton ionization in condensed media.
irradiance thresholds for breakdown of ocular and aqueous The model has been incorporated into a computer code and
media by nanosecond, picosecond, and femtosecond laser pulses code results have been compared to experimentally measured
in the visible and near-infrared. The code and comparison of code
irradiance thresholds for breakdown of ocular and aqueous me
results to experiment have been documented in a second paper
(Part II). dia by nanosecond, picosecond, and femtosecond laser pulses
in the visible and near-infrared. The code and comparison of
code results to experiment have been documented in a second
paper.
I. INTRODUCTION
produces a plasma dense enough to significantly absorb laser For cascade breakdown at least, experimental measurements
light. The latter is typically defined to be approximately 1018 in water show a field dependence similar to that found in
electrons/cm3 [3], [18]. solids [3], [31]. To obtain a simple, first-order model for
There are two mechanisms which can lead to LIB: Direct liquid breakdown, we will assume that liquids can be treated
ionization of the medium by multiphoton absorption [16], [17], as amorphous solids with (effective) conduction and valence
[19]-[22] or cascade ionization, also called avalanche ioniza bands. This appears to be a reasonable approximation for
tion [15], [16], [18], [21]-[26]. The latter process requires pure liquid water and for water doped with halide salts [29],
one or more free electrons to be present in the focal volume [30]. The models of Shen [16], for cascade breakdown in
at the beginning of the pulse. These "seed" electrons absorb solids, and Keldysh [17], for multiphoton ionization in crystals,
light photons through collision witli atoms or molecules, a have tlierefore been adapted to model breakdown in aqueous
process known as inverse brcmsstrahlung absorption. Having media. Altliough the model was developed for application to
achieved an energy greater than the ionization potential, a free aqueous solutions, it can be applied to breakdown in any
electron may ionize a molecule by collision. This produces two condensed medium which can he treated as a semiconductor
free electrons of lower energy, which in tum absorb energy or amorphous semiconductor.
from the laser and ionize two more, tlie process continuing
geometrically in an electron "cascade" leading to breakdown. m. MODIFIED RATE EQUATION FOR
In an impure medium seed electrons are most likely to come CONDENSED MATTER BREAKDOWN
from easily ionized impurities which act as shallow donors.
For nanosecond and sub-nanosecond pulses, we will have
The ionization may occur through tliennally induced collisions
three breakdown regimes. 1) A long pulse regime dominated
or by optical absorption of one or more photons. In a pure
by cascade ionization where multiphoton ionization plays no
mcdium with a high ionization potential, ionization of a few
significant role except (perhaps) for providing seed electrons.
molecules in the medium by multiphoton absorption may be
2) A short pulse regime where both types of ionization are
required to produce seed electrons and start a cascade.
significant. In this regime the pulse may be so short that a
Multiphoton ionization is a nonlinear optical process which
cascade cannot build up during the pulse unless the initial
typically becomes significant only at high irradiances and for
carrier density is very high. This high initial density would
wavelengtlis in tlie near-IR or shorter. For "pure" multiphoton
have to be provided by multiphoton ionization; i.e., multipho
breakdown each electron is independently ionized, requiring
ton processes would ')ump start" the cascade. For irradiances
no seed electrons and no collisions or particle-particle interac
high enough to achieve tliis, continuing multiphoton ionization
tions. The breakdown process is thus independent of impurities
might contribute to and accelerate the cascade process. 3)
and can occur even in media too diffuse to allow many
An ultrashort pulse regime, where only "pure" multiphoton
collisions during the pulse duration. It is potentially much
ionization is fast enough to allow breakdown to occur. over
faster than the buildup of an electron cascade and can tlierefore
the timewidtli of tlie pulse.
occur even for the shortest laser pulses.
In modeling condensed matter breakdown by ultrashort
Both multiphoton and cascade breakdown can occur in
pulses, it is clearly desirable to have a formalism which
solids, liquids, or gases. For cascade breakdown inside con
includes both cascade and multiphoton effects. In this section,
densed media, however, the term "free electron" takes on a
tlie rate equation formalism of Shen [16], which modcls cas
somewhat different meaning tlian witli gases. In condensed
cade breakdown only, will be modified to include multiphoton
media we have both electrons which are bound to a particular
ionization. A solution to this modified rate equation will be
molecule or lattice site and electrons which are free or quasi
sought in Section IV.
free; i.e., tlieir kinetic energy is great enough that they can
Shen divides the breakdown process into two parts: seed
move through the liquid or solid lattice without being trapped
electron generation and cascade ionization. An initial free
by localized potential wells. As long as these quasi-free
carrier density Po is assumed, which may come from multi
electrons have sufficient mobility to undergo collisions and
photon ionization or ionization due to thermalizing collisions.
absorb photons, an electron cascade can occur. In modeling
Breakdown is assumed to occur when the free electron density
condensed matter breakdown, transitions between bound and
p reaches a critical value Per"'" 10 1 8 /cm3 . The rate equation
quasi-free states are the equivalent of molecular ionization in
is solved to obtain HIe free carrier density as a function of
gases.
time, pet). This solution is combined witli the breakdown
Numerous researchers have modeled cascade and multi
criteria and witli a classical model for free carrier absorption of
photon ionization in gases [16], [17], [19]-[24] and solids
optical field energy. The result is an equation for the threshold
[16]-[18], [25]-[28], with results that give a reasonable match
irradiance needed to raise the carrier density from Po to Per
to experimental data. Breakdown in liquids, sllch as water
by cascade ionization during a pulse of duration Tp. A more
and aqueous solutions, has been experimentally investigated
general form of the rate equation will now be derived which
[3]-[15]; but is less well understood tlieoretically than solid
includes multiphoton contributions to carrier buildup during
or gas breakdown. The amorphous nature of tlie medium, the
the cascade phase as well as during seed electron generation.
consequent vmiation in the localized potential seen by the
Variation in electron density as a function of time can be
quasi-free electron, and the fact that molecules in liquid water
expressed in tlie generalized form [16], [18]
tend to associate or cluster in an undetermined fashion [29],
[30], all make electron mobility in water highly complex [3]. 8p/at = (17 - g)p + (8p/at)m, (1)
KENNEDY: A FIRST-ORDER MODEL FOR COMPUTATION OF LASER-INDUCED BREAKDOWN THRESHOLDS: PART I-THEORY 2243
where c is a constant of integration. Equation (7) gives "7 = [(e2E2/m) - (2mEavw2/M)]T/(w2T2 + l)Eion. (16)
where Co is the permittivity of free space, c is the vacuum D. Multiplwton Ionization Rate
speed of light, and no is the index of refraction of the medium L V. Keldysh [17] has derived approximate expressions
at frequency w. Equation (16) now becomes for the probability of mulliphoton' ionization, both in gases
and in condensed media. Ionization in the latter case refers to
71 = [(e2 lo/menoco) - (2mcavW2/M)]T/(w2T2 + l)Eion.
an electron transition from the valence, band to a conduction
(18)
or exciton band, creating an electron-hole p�ir. The condensed
media expression should be applicable to multiphoton ioniza
C. Electron Loss Rate
tion in water and aqueous solutions, which can be treated as
The electron loss rate, g, consists of contributions from amorphous scmiconductors [29].
recombination, trapping, and diffusion [22J. We will assume In modeling ionization by a strong electromagnetic wave, a
that the lifetime of the quasi-free electron is longer than the key parameter is the ratio, ry, of the opticaJ frequency wand
interaction time for pulsewidths of interest (Tp S 10-8 sec), the tunneling frequency Wt:
especially when the electron is absorbing energy from an
intense optical field. Electron-hole recombination during the
,=w/wt=w(m'6.)1/2/eE. (25)
breakdown process will therefore be neglected. In (25) m' represents the exciton reduced mass
Trapping in localized potential wells or solvated states is a
well known phenomenon in liquid water [34J-[36J. Binding lim'= l/m + l/mh, (26)
energies of these states, however, are low enough (�1.5 ±
where m and mh are the electron and hole masscs, respec
0.5 eV) that they can be easily reionized by cascading free
tively, and 6. is the transition energy across the band gap,
electrons or by single photon absorption. We will assume for
equivalcnt to the ionization energy Eion in our notation.
our first-order model that solvation and desolvation do not
Keldysh first derived a general formula, valid for any value
significantly effect the breakdown process at fields close to
of ,. He then obtained approximate fonllulas for the low
the breakdown threshold.
frequency (, � 1) and high frequency (ry � 1) limits,
With the above assumptions the loss rate is the rate of
cOITesponding to tunneling ionization and ionization through
diffusion out of the focal volume, given by [22J, [23]
multiphoton absorption, respectively.
For multiphoton ionization it is useful to define an effective
(19)
ionization potential in the field E:
where Td is the average time the electron stays in the focal
volume, D is the electron diffusion coefficient, and A is the
6.' = 6. + e2 E2 /4m' wZ = 6.[1 + 1/4ry21. (27)
characteristic diffusion length. The diffusion coefficient is [23], The number of photons required to ionize is then
[24]
K = (1 + 6.' /fiw), (28)
D = 2cav/3mv, (20)
where the symbol (x) denotes the integer prui of the number
where Cav is once again the average electron energy. For x, Ft = h/27r, and h is Planck's constant. Using (25), (27), and
a cylindrical focal volume of diameter d and length e, the (28), Keldysh's expression for the probability of mllltiphoton
diffusion length is given by [22] ionization in condensed media takes the form
where A is the optical wavelength and To is the gaussian waist 2....= [z2nH /n!(2n + 1)]. (31)
n=O;oc>
radius. The focal volume is given by
Equation (29) has a rather complex dependence on the
(24)
optical field E, which can be greatly simplified by using the
Smaller focal volumes and spot sizes will produce a higher limiting condition, ry � 1, to obtain:
rate of diffusion loss and should cause a higher breakdown
1 ± 1/4ry2 ;:;::;1, (32)
threshold for pulses longer than the diffusion time (Tp � Td)'
6.' ;:;::; 6., (33)
According to Bloembergen [18], for pulses of 10-8 sec or
less we will usually have Td ::; Tp in condensed media, making K;:;::; (1 + 6./,hw) , (34)
diffusion losses during the pulse interaction time small. z ;:;::; [2K .26./nw]1/2. (35)
KENNEDY: A FIRST-ORDER MODEL FOR COMPUTATION OF LASER-INDUCED BREAKDOWN THRESHOLDS: PART I-THEORY 2245
With these changes the field dependence is confined to the last and (37), we obtain the free electron density generated in time
term. Using (25) and (17), we can convert to a dependence on !:J.t by interaction with a pulse of irradiance 10:
irradiance:
(46 )
(36)
Assuming the initial density is that generated on the leading
Finally, using (32)-(36) in (29), the dependence of mul edge of the pulse, we follow Sacchi [3] and somewhat arbitrar
tiphoton ionization on optical irradiance takes the familiar ily set 6t = Tp/IO. We further assume that if Tp represents the
form full width half maximum (FWHM) in irradiance of the pulse,
then on the leading edge the irradiance will be roughly half
W =A[Blo]K, (37) the peak irradiance 10, We now have
A = (2/97r)w(rn'w/tt)3/2 exp [2K]<T>(z)(1/16)K, (38)
(47)
B = [e2/rn'6w 2cEono]. (39)
The initial density generated by thermal excitation can be
All quantities above are in MKS units. B has units of inverse estimated by assuming that the molecules are a thermalized
irradiance [rn2/Wj and A has units of inverse time and volume Maxwell-Boltzmann distribution with temperature T. The
[sec-1 m-3]. bound electrons correspond to thc ground state of the distribu
The probability W gives thc number of ionizations (or free tion and the ionized electrons to the excited state, where Eion
carriers gencratcd) per unit volume per unit time. It is thus is the transition energy between states. Maxwell-Boltzmann
equivalent to the time rate of change of the free carrier density statistics give a probability
P due to multiphoton ionization, which is also given by (4)
and (6b): (48)
as a function of the input il!adiance 10, just as we did for the (49)
cascade ionization rate 7].
If the field interacts with the medium for a time 6t, then If there are multiple sources for seed electrons (medium,
the fraction of bound electrons ionized in the focal volume is impurities, traps), then (47)-(49) must be solved for each
source, with the appropriate binding energy and bound electron
a = 7]'6t = P/Pb' (42) density in each case. Each term in (45) would then represent
the sum of contributions from all carrier sources present. Note
The free electron density generated by multiphoton ionization
that seed electrons contributed by impurities can significantly
is
lower the breakdown threshold for some impure media at some
and the number of free electrons in the focal volume is V. BREAKDOWN THRESHOLDS
(44) From (8) and the expressions derived previously for 7], g,
a, r/, b, and Po, we can predict the electron density p( t)
E. Initial Free Carrier Density
at some time t during the passage of a pulse of width Tp,
for pure multiphoton breakdown and for initiation of cascade arbitrary and alternate values could be used. The values above,
breakdown by multiphoton ionization of seed electrons. Before however, seem to work well in the comparison of theory to
deriving these expressions, a clearer definition of breakdown experimental data.
criteria is needed for future use in comparing the results of A problem arises in attempting to use the standard endpoint
the model to experiment. to detect breakdown by pulses shorter than 10 ps; i.e., the
intensity of the plasma radiation decreases as the pulsewidth
criterion.
The flash endpoint also introduces a constraint on the time
fo = fth in (18); and further that this is the value of 17 for
whi h (8) yieJds the breakdown condition P (0.5 Tp) = Per.
allowed for breakdown. During the timewidth of the pulse, �
Settmg b = 0, to eliminate multiphoton contributions, and
Tp, both plasma formation (breakdown) and plasma heating to using (6a) gives
visibly eniitting temperatures must occur. Reichel et al., [38],
found that breakdown occurred during the first half of a 20 ns
Nd : YAG laser pulse, with the remaining pulse energy going
p(t) :::::: Po exp [(17 - g)t]. (53)
to plasma heating. Future calculations for the flash endpoint
will use Tp/2 as an estimated breakdown time, regardless of Now we apply the breakdown criteria to obtain
Setting (5�) equal to the expression for 'fIer obtained by setting initial density Po � po(min). The second, the multiphoton
fa = fth m (18), the threshold is initiation threshold Im, represents tlJe irradiance needed to
nit ate a cascade by providing
� � Po (min) through multiphoton
Ith = [mcnocoEion(1 + W2 'T2 )/c2'T][g + 2(7p)-1 In (Per/Po)] .
101llzatlOn.
+ 2m2EavW2 (cnoE:o)/e21Vf, (56) Equation (47 ) gave the initial density Pam generated through
multiphoton ionization by the leading edge (Llt = 0.1 'T ) of
,:here all quantities are in MKS units [Ith in W/m2]. A
SImpler form can be obtained if we assume that the average
a pulse witlJ peak irradiance Io. To compute tlJe thre hold :
electron energy is
10 = Im, we set Pam = po(min) and obtain
(57) (61)
(59) (62)
The three terms of (58) represent, in order, diffusion losses, D. Time Constraints for Cascade Breakdown
carrier buildup through cascade ionization, and collisional
In addition to the minimum initial density constraint given
energy losses.
above, there is also a time constraint on the initial density
The dependence of the cascade breakdown threshold on
needed for cascade breakdown during a time 0.5 'Tp. Bloember
various experimental parameters can be seen from (58) and
gen [18] estimates that the time between collisions, for a quasi
(59). The threshold is directly proportional to tlJe ionization
free electron in a condensed medium, is approximately 'T �
energy Eion. For optical frequencies and photon energies high
lO-lu s. Since collision and photon absorption is occurring
enough to give W2'T2 � 1, fth is proportional to w2 (or to 1/.\2
on a femtosecond time scale, a cascade could conceivably
as it is more commonly expressed). When tlJe loss terms are
small, as they are likely to be for short pUlses, the threshold is
raise p( t) by a factor of 1012 in a picosecond or less [28].
For subpicosecond pulses, however, it may not be possible to
inversely proportional to the pulsewidth 'Tp. Finally, for pulses
long enough to make diffusion a factor ('Tp > 'Td), smaller spot
achieve cascade multiplication from po(min) to Per over an
interaction time 0.5 'Tp. In this case a higher minimum initial
sizes will produce higher thresholds, due to a higher rate of
density, p�(min), must be defined; for which breakdown can
diffusion loss from the smaller focal volume.
be achieved over this time.
We begin by obtaining an estimate of the minimum time
C. Irradiance Threshold for Multiphoton Initiation
needed to go from po(min) to per by cascade ionization. The
Although (58) neglects multiphoton contributions during multiplication factor during this event is
carrier buildup, multiphoton ionization may still contribute to
the generation of the initial free carrier density po. To initiate
(63)
cascade ionization tlJere must be at least one seed electron in
the focal volume, Vj. In fact, only one seed electron makes
where y represents the number of times the density doubles
cascade initiation uncertain and 10 seed electrons would be a
during the cascade. The time required for one free electron to
more dependabJe starting point, especially for ps and fs pulses,
ionize another is approximately
where the short pulse duration requires rapid initiation. We
assume a minimum value of tlJe initial free electron density
(64)
(60)
where Neall is tlJe number of collisions needed to absorb one
where No(min) represents the minimum number of seed
photon and K is the number of photons needed to ionize. The
electrons required in Vj. In our calculations No(min) was
ionization time is also tlJe minimum doubling time 'Tdb; i.e., the
set to 1 for ns pulses and to 10 for ps and fs pulses.
time during which the number of free electrons N in the focal
For some condensed media, such as semiconductors, ther
volume will double, assuming tlJere are no losses. With these
mal ionization at room temperature will supply sufficient free
definitions, the minimum breakdown time can be estimated as
carriers, 108 /cm3 to satisfy tlJis condition [18]. For pure
Pot � ,
If O.5'Tp 2' 'FIR., then full cascade breakdown from p o { min ) be obtained from (46) with !It = 0.5 'p' 10 = IMP; and
is possible and no recalculation of the thresholds in Section P =
Per:
V -C is needed. Otherwise, we compute
(74)
y' O.5'Tp/'db,
= (66)
' . ) Since multiphoton absorption is a nonlinear optical process
' = 2Y = Pcr/ Po/ ( mIn, (67)
.1:
requiring very high irradiance, IMP is likely to be higher than
p� ( mi n) = Pcr/X', (68)
cascade breakdown thresholds in almost all cases. Tn the fem
where y' is the largest number of doublings possible in the tosecond pulse regime, however, time constraints on cascade
time allowed, x' is the corresponding multiplication factor, and formation cause a gradual shift to rnultiphoton ionization as
p� ( min) is the new minimum initial density. From (47), we can the dominant mechanism.
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Paul K. Kennedy received the B.S., M.S., and
[21] C. DeMichelis, "Laser induced gas breakdown: A bibliographical re Ph.D. degrees in physics from North Texas State
view," IEEE J. Quantum Electron., vol. QE-5, pp. 1 88-202, 1969. University in 1976, 1980, and 1983, respectively.
[22] D. C. Smith and R. G. Meyerand, Jr., "Laser radiation induced gas In 1983, he joined the Rocketdyne Division of
breakdown," in Principles ofLaser Plasmas, G. Bekefi, Ed. New York: Rockwell International, where he served as a the
Wiley, 1976, pp. 457-507. oretical analyst and scientific programmer support
[23] N. Kroll and K. M. Watson, 'Theoretical study of ionization of air by ing research and development of high energy free
intense laser pulses," Phys. Rev. A, vol. 5, pp. 1 883-1905, 1972. electron, excimer, and oxygen-iodine lasers. Since
[24] Y. B. Zel'dovich and Y. P. Raizer, "Cascade ionization of a gas by a 1992, he has been a research biophysicist in the Op
light pulse," SOy. Phys. JETP, vol. 20, pp. 772-780, 1965. tical Radiation Division of Armstrong Laboratory,
[25] M. Bass and H. H. Barrett, "Laser-induced damage probability at 1 .06 characterizing and modeling the interaction of laser
Jl-m and 0.69 Ilm," Appl. Opt., vol. 12, pp. 690-699, 1973. and other optical radiation with biological systems. His current area of interest
[26] __ , "Avalanche breakdown and the probabilistic nature of laser is the physics of laser-induced breakdown in the eye and its relationship to
induced damage," IEEE J. Quantum Electron., vol. QE-8, pp. 338-343, observed ocular damage from ultrashort pulse exposures.
1972. Dr. Kennedy is a member of Sigma Pi Sigma, APS, and OSA.