Volume

8, number

OPTICS COMMUNICATIONS

August

1973

THE INFLUENCE OF ELECTRON PLASMA FORMATION SUPERBROADENING IN LIGHT FILAMENTS N. BLOEMBERGEN*

Philips Research Laboratories, Received Eindhoven, Netherlands

ON

18 June 1973

Avalanche

ionization

limits the maximum

field strength

in small scale filaments,

produced

by laser pulses in aohds

and liquids. The temporal and spatial variations in the index of refraction due to electron plasma formation contribute significantly to the processes of self-phase-modulation. A new interpretation of previous experimental results on frequency superbroadening is presented.

1. Introduction The extensive literature on theoretical and experimental investigations of superbroadening in small scale filaments produced by self-focussed light pulses has been reviewed by Akhmanov et al. [ 11. The interpretation of this frequency broadening in terms of moving focal spots has been reviewed more recently by Low and Shen [2]. In all of this work the diameter of the filaments, or the size of the focal spot, is introduced as a phenomenological parameter which is chosen to conform with experimental observations. Yablonovitch and Bloembergen [3] have demonstrated that the maximum power flux density in a filament or focal spot, even one with a duration of a picosecond, is limited by the onset of dielectric breakdown of the optically transparent medium. The formation of an electron plasma with an electron density N,(t) and an electronic collision time 7 leads to a contribution to the complex index of refraction
Anpl =

(Yis the ionization rate per electron, which is a sensitive function of the intensity. Avalanche ionization is a universal mechanism, which is operative at power flux densities of 1012 W/cm2, or less for longer pulses, in ionic crystals, glasses, atomic and molecular fluids. It is the purpose of this note to investigate the influence of the plasma index modulation Anp,(t, r), given by eqs. (1) and (2), on the spectral broadening by self-phase-moclulation, which is also a universally observed phenomenon in small scale filaments in any material [ 11. ,4lfano and Shapiro [4] observed pronounced broadening when short intense light pulses form filaments in glasses, ionic crystals and liquified noble gases. The Stokes broadening is characteristically several thousand wavenumber, while the anti-Stokes broadening is even 30 to 50% larger. A new interpretation of their results will be given in section 2. The plasma contribution to the observed frequency broadening in filaments in molecular fluids will be discussed in section 3.

LNe&
n0

.1--,
1 + ,V

mw

(1)

2. Plasma index modulation and superbroadening ionic crystals and glasses

in

Here no is the linear index of refraction of the medium. In the case of plasma formation by avalanche ionization the density is an exponential function of the light intensity and the time

* On leave from Harvard

University.

It is a well established fact that the duration of the high intensity in a fixed volume element of a small scale filament is on the order of a picosecond or less [ 11. It is also known that a filament really represents two moving focal spots [2], if the mechanism responsible for the self-focussing action has a response time short compared to the incident laser pulse. We postulate, with 285

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Alfano and Shapiro

with a response

[4] , that the electronic

set

nonlinearity

is the dominant nonlinear index contribution in the crystals of calcite, NaCI, quartz and some glasses used in their experiments. Loy and Shen [Z] argue that the near-instantaneous response of the non-linearity should give rise to high intensity focal spots which also last only about I O-l5 sec. It appears more realistic to USCthe observed filament dimension, a = 90 ~_lm,and determine the time necessary for a light ray to traverse this dimension. A duration of the high intensity spot, b,, = H@~/c x IO-l3 set, is thus estimated. In fig. I the qualitative behaviour of the light intensity on the axis of a filament is sketched. The distance along the length of cell was here chosen as the selffocussing distance for light of half the maximum input intensity. Two sharp intensity focal spots appear on the background of the unfocusscd intensity. Alfano and Shapiro assumed a field strength of nearly IO8 V/cm, and or power flux densities of 1013 W/cm2. Even for such short pulses an electron plasma will be formed already for field strenghts of about 1.5 x IO7 V/cm, or power flux densities below IO W/cmZ. Under these rather extreme conditions the dominant mechanism for the creation of an electron plasma will be either frequency-dependent tunneling or avalanche ionization. The latter process needs about 30 to 40 doubling gcnerations to build up a plasma density N, - I 018/cc. The temporal behaviour of such an exponential build up of the plasma density with a time constant of about t,/30 3 x lo-l5 XC is sketched in fig. 1 as a dotted line. The resulting change in the index of refraction, with the plasma contribution superimposed on the instantaneous nonlinearity of the bound electrons is shown in fig. 1 as the solid line. The electronic nonlinearity tz2 Ikq I2 with tl? - l&l4 for calcite, and E, 6 1OSesu, becomes 10m4 The plasma index change attains the same magnitude for the following numerical values: N, = 1018cm-3, 7 = 3 x 10-15 set and w = 3 x 105 sccM1. This value corresponds to the ruby light frequency, while the collision time r has the appropriate magnitude for low-energy electrons, which constitute the bulk of the plasma, in ionic crystals. Bv substitution in eq. (1) one finds Re (AfzPl) N -10m4. while lm (An,,) = 1O-5. The negative real part is sufficient to compensate the positive contribution tt21Ee12 during the light pulse. For the trailing edge the effective index change is negative, as the plasma density decays much more slowly than the light pulse. through recombination and diffusion. 286

time of I O-l5

10

-12

2 .10-2sec
An

Fig. 1. Schematic temporal behaviour on the axis of a small scale filament at a distance where the intensity at half maximum of the incident pulse is self-focussed by a fast electronic nonlinear index change. Intensity: dashed line. Plasma density: dotted line. Change in index of refraction: solid line

The very steep negative slope will produce an antiStokes frequency sweep, which in order of magnitude is given by, 6~ = -- WC-!

an/at.

(3)

The path length 1 cannot be chosen larger than the absorption length in the plasma of the assumed density. In our numerical example 1 c CT ZY- ~ 1 7,~ lm(Atzpl) = q)

abq

Z cm

For crystals longer than this length, the resultant broadening is independent of the assumed plasma density and consequently independent of the radial position in the filament, because an/at is proportional and I is inversely proportional to the electron density. The maximum frequency sweep that may be expected is obtained when we take Watlm;LY 30Re(Atzp,)/tp which leads to (60),, = (307/tp&, or (60/o),, = 1. The frequency shift can be of the same order of magnitude as the light frequency. Since the anti-Stokes frequency sweep is so large and the swept light is initially contained in a very narrow section, the effects of linear colour dispersion of the host lattice are very important. Light that is up-shifted by 10% in frequency will have an index of refraction change, AtlLin = (an/aw)Aw = 5 x 1O-3 for typical dispersion constants in these materials. After a distance z = 200Ctp/tz0 = 0.5 cm in the crystal, this shifted light will have fallen behind the high intensity focus. It is then

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1973

3. Spectral broadening

in molecular

fluids

, 0

__,/__jL&
,0-l* --

2x10-'2sec

Fig. 2. Schematic temporal behaviour on the axis of a small scale filament which is formed by the self-focussing of the tail end of the incident pulse by transient molecular reorientation. Intensity: dashed line. Plasma density: dotted line. Change in index of refraction: solid line.

diffracted out of the filament by the negative plasma index of refraction, and these rays of upshifted light are now coincident in space and time with laser light in the trailing edge of the pulse which is not (yet) focussed. The conditions for a phase-matched four-wave parametric interaction are now fulfilled. Thus one of the outer curves*, or frequency swept cones of light observed by Alfano and Shapiro, may indeed be explained in the manner suggested by them [4]. The second wing could be formed in the following manner: anti-Stokes light remaining in the filament, with wave vector k,, parallel lto it, travels more slowly and is overtaken by the second moving focal spot. Laser rays in the trailing edge of the pulse move here at an angle to the filament with wave vector k,. The second diffuse cone is determined by the momentum matching condition 2k,, = k, + kl,. The combinatiosn of the large temporal and spatial gradients in the plasma density with the large frequency shift and colour dilspersion would require more refined calculations than have been customary [l] to predict the observed spectral density. The admittedly crude estimates given here show that the index changes associated with the plasma formation account for most of the observed details of superbroadening without making strained assumptions about the magnitude of physical parameters.

* See figure 5 2 in ref.

[ 1]

In fluids with anisotropic molecules the self-focussing is initiated by the orientational Kerr effect, even if the relaxation time for molecular reorientation is longer than the laser pulse duration [5]. III this situation only the trailing part of the incident pulse is focussed into a filament [2, 61. Its diameter can again be stabilized by initial plasma formation, although other mechanisms are still under active discussion [7] In fig. 2 the schematic behaviour of the intensity on the axis of the filament, the plasma density and the index of refraction is sketched. It is assumed that the orientational Kerr effect is integrated over the laser pulse. The index of refraction due this effect increases monotonically during the pulse, as was demonstrated experimentally in nitrobenzene [S] At the end of the pulse the index decreases rather suddenly due to incipient plasma formation. This effect would not be detectable in birefringence experiments. It is believed that this plasma contribution is largely responsible for the antistokes broadening observed in fluids with long molecular relaxation times. The case of CS, which has been most widely investigated is a borderline situation because the laser pulse duration and the molecular reorientation have comparable magnitude in this case. Loy and Shen argue that an assumed radial variation of the form shown in fig. 2 could contribute to antistokes broadening in CS,, because a diffraction term causes a variation of the phase. Cubeddu [8] et al. previously invoked a fast librational contribution to the intensity dependent index to explain the observed antistokes broadening. A librational contribution to the birefringence is, however, not observed [6]. The plasma variation is consistent with the observed broadening without straining numerical parameters. It is also consistent with the lack of radial dependence of the frequency broadening and with the leaking of light out of the filamentary region, as explained in the preceding section. Furthermore the plasma index variation will be helpful in promoting parametric interactions between four light waves. Under the simultaneous presence of two light waves with a frequency difference Aw, the plasma density will be modulated. This modulation will be effective up to frequencies r;{ or 30t;, i.e. for Ao e 1000 cm-l. The contribution from the bound electron nonlinearity is numerically smaller and has been ignored in this brief discussion of self-focussing and self-phase modulation in small scale filaments in molecular fluids. 287

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4. Conclusion It is universally pulses create The quadratic be of purely association accepted that short, resonsible in tense Ias may and

References
R.V. Khokhlov and A.P. Sukhorukov, Ch. I-3 in Laser Handbook, Vol. 2, eds. F.T. Arecchi and F.O. Schulz-DuBois, North Ilolland Publ. Co, Amsterdam 1972. This review contains comprehensive references to the eutensivc literature. I21 M.M.?. Loy and Y.R. Shen, I.E.E.E. .I. Quantum Electr. QE9 ( 1973) 409. and N. Bloembergen, Phys. Rev. Letters 131 ii. Yablonovitch 29 (I 972) 907. I41 R.R. Alfano and S.L. Shapiro, Phys. Rev. Letters 24 (I 970) 584, 592 and 1217. 1st J. Retntjcs and R.L. (arman, Phyr. Rev. Lcttcrs 28 (1972) 1697. Fundamental and Applied Laser Physics, I51 N. IIloembcrgen, Proc. of the 1971 Esfahan Symp., Feld, Javan and Kurnit cds. (Academic Press. New York, 1973). 171 A.11. Piekara and T.K. Gustavson, Optics Commun. 7 (I 973) 197. 181 R. Cubcddu, R. Polloni. C.A. Sacchi and 0. Svelte, Phys. Rev. Letters 26 (1971) 1009. 191 1j.W. I:radin, N. Bloembcrgen and 3.1. Letellier, submitted to .4ppl. Phys. Letters.

111 S.A. Akhmanov,

small scale filaments Kerr effect electronic in others.

I II

due to self-focussing. for this effect reorientation

origin in some classes of-matceither ~ase localized regions

rials, and may arise fronl molecular are formed in the material where reaches values [II) to IO I 2 W/cm2

the light intensity during times of one plasma formation [3, 91 The spatial

picosecond or less. Incipient electron takes place under these circumstances

and temporal index changes associated with this pla.~~~a formation have a profound influence 011 the geometry and sire of the filamentary regions. and on the sclf-phascmodulation occurring in them. Numerical calculations of suIerbroadelling should take this process into account.

288