Axial emission and spectral broadening in self-focusing of femtosecond Bessel beams

A. Dubietis, P. Polesana , G. Valiulis, A. Stabinis, P. Di Trapani , A. Piskarskas

Department of Quantum Electronics, Vilnius University, Saul tekio Ave. 9, bldg.3, LT-10222 e Vilnius, Lithuania Permanent address: INFM and Department of Physics, University of Insubria, Via Valleggio 11, IT-22100 Como, Italy. audrius.dubietis@ff.vu.lt

Abstract: We report on the experimental observations of on-axis spectral broadening arising from self-focusing of the axicon-generated femtosecond Bessel beam in water. The observed spectral broadening is interpreted by a nonlinearly phase-matched four-wave mixing process involving the intense conical pump, the axial signal and a conical idler wave.
2007 Optical Society of America
OCIS codes: (190.4410) Nonlinear optics, parametric processes; (190.5940) Self-action effects; (320.7110) Ultrafast nonlinear optics

References and links

1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 14. 15. 16. J. Durnin, J. J. Miceli, and J. H. Eberly, Diffraction-free beams, Phys. Rev. Lett. 58, 14991501 (1987). D. McGloin and K. Dholakia Bessel beams: diffraction in a new light, Contemp. Phys. 41, 1528 (2005). I. Golub, Superluminal-source-induced emission, Opt. Lett. 20, 18471849 (1995). S. Klewitz, P. Leiderer, S. Herminghaus, and S. Sogomonian, Tunable stimulated Raman scattering by pumping with Bessel beams, Opt. Lett. 21, 248250 (1996). A. Piskarskas, V. Smilgevi ius, and A. Stabinis, Optical parametric oscillator pumped by a Bessel beam, Appl. c Opt. 36, 77797782 (1997). J. Amako, D. Sawaki, and E. Fujii, Microstructuring transparent materials by use of nondiffracting ultrashort pulse beams generated by diffractive optics, J. Opt. Soc. Am. B 20, 25622568 (2003). E. J. Botcherby, R. Juskaitis, and T. R. Wilson, Scanning two photon uorescence microscopy with extended depth of eld, Opt. Commun. 268, 253260 (2006). P. Johannisson, D. Anderson, M. Lisak, and M. Marklund, Nonlinear Bessel beams, Opt. Commun. 222, 107115 (2003). M. A. Porras, A. Parola, D. Faccio, A. Dubietis, and P. Di Trapani, Nonlinear unbalanced Bessel beams: stationary conical waves supported by nonlinear losses, Phys. Rev. Lett. 93, 153902 (2004). P. Polesana, A. Dubietis, M. A. Porras, E. Ku inskas, D. Faccio, A. Couairon, and P. Di Trapani, Near-eld c dynamics of ultrashort pulsed Bessel beams in media with Kerr nonlinearity, Phys. Rev. E 73, 056612 (2006). R. Gadonas,V. Jarutis, R. Pakauskas, V. Smilgevi ius, A. Stabinis, and V. Vai aitis, Self-action of Bessel beam s c c in nonlinear medium, Opt. Commun. 196, 309316 (2001). E. Gai auskas, E. Vanagas, V. Jarutis, S. Juodkazis, V. Mizeikis, and H. Misawa, Discrete damage traces from z lamentation of Gauss-Bessel pulses, Opt. Lett. 31, 8082 (2006). J. H. Cooley, T. M. Antonsen, H. M. Milchberg, J. Fan, L. Margolin, and L. Pyatnitskii, Parametric instability in the formation of plasma waveguides, Phys. Rev. E 73, 036404 (2006). S. Klewitz, S. Sogomonian, M. Woerner, and S. Herminghaus, Stimulated Raman scattering of femtosecond Bessel pulses, Opt. Commun. 154, 186190 (1998). M. Wittmann and A. Penzkofer, Spectral superbroadening of femtosecond laser pulses, Opt. Commun. 126, 308317 (1996). A. G. Van Engen, S. A. Diddams, and T. S. Clement, Dispersion measurements of water with white-light interferometry, Appl. Opt. 37, 56795686 (1998).

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17. S. P. Tewari, H. Huang, and R. W. Boyd, Theory of self-phase matching, Phys. Rev. A 51, R2707R2710 (1995). 18. M. Sceats, S. A. Rice, and J. E. Butler, The stimulated Raman spectrum of water and its relationship to liquid structure, J. Chem. Phys. 63, 53905400 (1975). 19. M. A. Porras, A. Parola, D. Faccio, A. Couairon, P. Di Trapani, Collapse-driven spatiotemporal dynamics of lament formation, Phys. Rev. Lett. (submitted). 20. G. P. Agrawal, Modulation instability induced by cross-phase modulation, Phys. Rev. Lett. 59, 880883 (1987).

1.

Introduction

Since the rst experimental realization of so-called non-diffracting light beam in 1987 [1], Bessel beams (BB) continuously attract a broad interest from the scientic community inspired by expanding area of applications in atom optics, acoustics and plasma physics [2]. Pulsed BB are of particular interest in nonlinear optics providing new routes for frequency mixing and conversion [3, 4, 5], material processing [6] and device applications [7]. In spite of this evidence, self-focusing of pulsed BB in Kerr media still remains a poorly investigated phenomenon, especially in the femtosecond regime. In the presence of self-focusing nonlinearity, stationary monochromatic Bessel-like solutions were predicted, featured by a compressed transverse beam prole [8], but shown to be unstable, owing to radial collapse [9]. Nonlinear losses (NLL) were predicted to counteract collapse, leading to radially stable unbalanced BB solutions, featured by a ring-like angular spectrum an by a reduction in near-eld modulation contrast that was also detected in experiments in fused silica [9, 10]. Far-eld detection in case of propagation in benzene with quasi-monochromatic pump, however, has outlined the appearance of an intense axial component, accompanied by an outer ring at the angle fullling longitudinally phase matched four-wave mixing (FWM) interaction [11]. Note that the interference between the produced axial component and the conical one has been proposed as responsible for the creation of periodic modulation of the peak uence during BB nonlinear propagation, which results in a series of regularly spaced damage spots in fused silica [12] or in instabilities in plasma waveguides generated in gasses [13]. As to modications in the time-domain spectrum, Stokes-shifted axial emission due to stimulated Raman scattering (SRS) was also reported in earlier experiments with nonlinear Bessel beams in the femtosecond regime [14]. To the best of our knowledge, the space-time dynamics of pulsed BB has not been investigated so far. In this Letter we report on the rst observation of axial broadband radiation excited by Bessel beam pumping. Differently from the Gaussian pump case, spectral broadening appears free from the intense-pump central peak, the pump beam propagating here out of axis. The largest conversion occurs at frequencies far from the pump, where the FWM interaction is shown to experience large gain due to optimum (longitudinal and transversal) phase matching. The process depends critically on the nonlinear-sample position in the beam path, which can be adjusted in order to excite either SRS or broadband light centered at the carrier frequency. The results are interpreted assuming a key role of BB collapse as the triggering mechanism for axial-component amplication. 2. Experiment

In the experiment, we have investigated the nonlinear propagation of femtosecond BB in water. The 200 fs, 527 nm pump pulse has been generated by a chirped-pulse-amplication Nd:glass laser system (Twinkle, Light Conversion Ltd) followed by a frequency-doubling compressor. A spatially ltered Gaussian beam with 1/e2 radius of w0 = 1.02 mm has been launched into BK7-glass axicon with base angle of = 5.17 deg. In this conguration, the length of the Bessel zone (diffraction free path for the central spot) in water is zF = w0 / = 29 mm, where = (na 1) /nw = 35 mrad is the cone half-angle, na = 1.52 is the BK7-glass refractive
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indexes and nw = 1.33 the refractive indexes of water. The resulting prole leads to a central interference spike with diameter of 9 m (between the zeros of Bessel function), which grows in intensity during propagation reaching its maximum at a distance z 9.5 mm and z 7.5 mm from the axicon for propagation in water and in air, respectively. The cuvette input-facet position was varied from close contact to the axicon to z = 7.5 mm. The rst setting allows the spike to grow in intensity inside water, thus supporting the smoothest possible transition from linear to nonlinear regime. In what follows, this setting is referred therefore as smooth transition case. The second setting, in contrast, provides the most abrupt transition from linear to nonlinear regime, and is referred therefore as sharp transition case. In all measurements, the input-pulse energy was kept to Ein = 19.5 J. 3. Results

Figures 1(a) and 1(b) show typical axial spectra obtained for the smooth and sharp-transition conguration, respectively, as measured by means of ber spectrometer (QE6500, Ocean Optics). Here cuvette lengths have been set to L = 29 mm and L = 22 mm, respectively, so to ensure the same output-facet position (at the very end of the Bessel zone), in both cases. The corresponding angular distributions of the generated radiation are shown in Figs. 2(b) and 2(c), where far elds detected by means of digital photo-camera (Fujilm Finepix S7000) are reported. Figure 3 shows the dependence of the axial-beam energy on cuvette length, both for the smooth and sharp transition regimes. Sample lengths have been here modied by tuning the output-facet position, while keeping the input as specied above. Figure 4 proposes few examples of sharp-transition axial spectra relative to different sample lengths.

(a)
I (a.u.)

Intensity (a.u.)

450 500 550 600 650 700

(b)
I (a.u.)
450 500 550 600 650 700

Wavelength (nm)
Fig. 1. Frequency spectra of axial emission (right) and corresponding experimental settings (left), which lead to (a) SRS and (b) broadband radiation centered at the carrier frequency. The bold line shows the peak intensity in the central core of the Bessel beam in air with maximum at z=7 mm from the axicon.

The results shown in Figures 1-3 clearly outline a substantial difference between the nonlinear dynamics developed in the smooth and sharp transition regimes. When the BB peak intensity is made to grow smoothly inside the sample, a clean SRS axial emission takes place, with pulse energy growing exponentially with propagation and reaching the value of EStokes 750 nJ at the end of the Bessel zone. We note that SRS axial emission is peaked at = 650 nm, i.e. at a
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Fig. 2. Photographs of the far-eld of the (a) linearly propagating (low energy) Bessel beam, (b) SRS, and (c) broadband radiation centered at the carrier frequency. Intensities of the spectral components are not to scale.

13 mm red-shifted value respect to what is expected for quasi plane and monochromatic pump waves [15]. The Stokes axial emission is here accompanied by an off-axis anti-Stokes radiation, emitted over a cone with half-aperture angle aS 6 . Further measurements (data not shown) revealed the bandwidth of the Stokes-shifted axial radiation to increase on increasing pump energy, in line with the result reported in Ref. [14].
300 900
Stokes energy Linear fit Exponential fit

Continuum Energy (nJ)

700 500 300 100

200 150 100 50 0 8 10

12

14

16

18

20

22

24

26

28

Distance from the axicon (mm)

Fig. 3. Energy of the axial broadband radiation (full circles) and Stokes component (open circles) vs distance from the axicon. Note that the cuvette is shifted by 7 mm with respect to the axicon in the rst case.

For the sharp-transition setting, in contrast, no SRS is detected for the entire range of investigated sample lengths. The axial radiation appears initially (i.e. for short samples) around the pump wavelength. The axial-spectrum keeps broadening with further propagation, developing a sharply modulated structure featured by large peaks at the external sidebands (Fig. 4). A spectral width of > 4000 cm1 is measured for sample length L = 18 mm. The axial-pulse energy increases linearly with propagation, reaching the value Econt 250 nJ for the same L = 18 mm that is after 25 mm from the axicon (Fig. 3), which corresponds to 1.3 % energy conversion from the pump pulse. The axial component is accompanied by the appearance of an outer idler ring. Further measurements (data not shown) reveal the idler to be composed by a broadband radiation featured by angular dispersion, with minimum half-aperture cone angle i 3.3 at degeneracy and with quadratically increasing angles on increasing the frequency shift. As to the axial beam quality, near-eld detection revealed the mode to be shaped as a well-conned Gaussian beam of 17 m waist radius (at 1/e2 ). At higher pump energy Ein = 30 J an explosive broadening of the axial spectrum due to self-focusing of the axial beam itself was observed, accompanied by a beam-quality deterioration and by the appearance of multiple colored rings (conical emission) inside the cone of the input BB. We mention that any intermediate position
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Stokes Energy (nJ)

250

Continuum energy

of the cuvette yields the generation of both SRS and broadband axial emission components.
z = 10 mm 8 4 8 4 0 500 550 600 650 450 500 550 600 650 z = 13 mm

Intensity (a.u.)

0 450

z = 17 mm 8 4 0 450 500 550 600 650 8 4 0 450

z = 25 mm

500

550

600

650

Wavelength (nm)
Fig. 4. Single-shot spectra of axial emission versus propagation distance z.

4.

Discussion

In order to provide a consistent scenario for interpreting the observed phenomenology we consider in what follows a generic, Kerr-driven, FWM process which involves: (i) two pump waves at 0 , whose wavevectors kp = k0 coincide with those of the Bessel beam; (ii) a signal wave s = 0 + , with ks oriented on axis; (iii) an idler wave, with frequency i = 0 fullling energy conservation 20 = s + i and with ki oriented at the angle which permits the longitudinal phase matching relation 2k0 = ks + ki to be fullled. We dene k0 = k(0 ), ks = k(0 + ) and ki = k(0 ), where is the frequency shift relative to carrier frequency. The angle, at which the idler wave is longitudinally phase-matched is frequency dependent and, in the low intensity limit, reads as 2k(0 ) cos k(0 + ) , (1) k(0 ) where k( ) = n( ) /c obeys the dispersion relation for water as given in Ref. [16]. In small angle and second-order dispersion approximation the cone angle for the idler wave is

i ( ) = arccos

i ( ) = 2 2 +

2k ( )2 , k0

(2)

where k = 2 k/ 2 |0 denotes the group-velocity dispersion coefcient. Assuming that in the case of BB one has to account for various azimuthal components giving their contribution to the generated axial beam, the transverse phase matching is expressed by the transverse phase-matching integral [17], which in the low-intensity limit is given by: T=
0 r0 2 J0 (k(0 ) sin r)J0 (k(0 ) sin i r)rdr,

(3)

where r is the radial coordinate and r0 = 1.5 mm is the upper integration limit set by BB apodization. By substituting i from Eq. (1) to Eq. (3) and assuming that an intense BB pump
#79377 - $15.00 USD Received 24 January 2007; revised 8 March 2007; accepted 8 March 2007

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modies by cross-phase modulation the refraction index seen by the weak axial signal, i.e n(0 + ) = n0 (0 + ) + 2n2 I, we obtain T ( , I) = with cos2 i ( , I) = 20 n0 cos (0 + )[n0 (0 + ) + 2n2 I] , (0 )n0 (0 ) (5)
r0 0 2 J0 (k(0 ) sin r)J0 [k(0 ) 1 cos2 i ( , I)]rdr,

(4)

where n2 = 4.1 1016 cm2 /W is the nonlinear refraction index, I is the peak intensity and n0 = n0 (0 ). Here we assumed that both pump and idler waves propagate linearly, owing to expected negligible off-axis nonlinear phase accumulation. Figure 5 shows transverse phase matching integral as computed from Eq. (4). In FWM process, the gain experienced by the spectral component 0 + of the signal is proportional to the product of Kerr nonlinearity, I and T ( , I). The full black line shows the case of low-intensity limit, for a given pump cone angle = 35 mrad. The lines in color represent modications of the gain prole in high-intensity propagation regime. Note how phase-matched peaks shift toward the center in the presence of the intense pump wave. And nally, the peak position of the transverse phase matching integral strongly depends of the cone angle , as shown by a dashed line, which represents the computed T ( , I) in the case of a 40 % larger BB cone angle.

Fig. 5. Transverse phase matching integral as function of wavelength, = 2 c/(0 + ). Solid and dashed black curves depict the case of low-intensity regime for cone angles of 35 and 50 mrad, respectively, while those in color demonstrate how the sidebands shift towards the carrier frequency with increasing the intensity.

In interpreting the SRS process, we note that: (i) owing to the chosen BB cone angle, and to the related tilt in the pump-pulse amplitude front, the effective pump group-velocity component in the axial direction matches with good accuracy that of the axial Stokes pulse, leading to pump-to-Stokes splitting length of 8 mm for 200 fs pulse duration (see Ref. [14] for derivation); (ii) the SRS under plane-monochromatic pump leads to Stokes S = 637 nm [15], very close
#79377 - $15.00 USD Received 24 January 2007; revised 8 March 2007; accepted 8 March 2007

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to optimum condition for linearly phase matched FWM process. The observed red shift of the Stokes wavelength might be attributed to peculiarities of nonlinear propagation regime as suggested in Ref. [18]. The smooth-transient conguration provides therefore the ideal setting for efcient SRS and subsequent parametric FWM amplication, this being the conguration that ensures: (i) the large interaction path for the vacuum-state uctuations to be readily amplied and (ii) the condition for the signal to be amplied without severe pump-phase distortion, these being expected to be detrimental for the FWM parametric process. We assume the triggering mechanism for the occurrence of broadband radiation to be the production of axial seed at degenerate frequency, which in turn is a consequence of self-action experienced by intense BB as discussed in Ref. [11]. In accordance to the results of Fig. 5, this seed is not expected to experience degenerate amplication, in the smooth-transient regime. The key factor which we believe characterizes the sharp-transient regime is the occurrence of Kerr-driven BB collapse-type transverse-beam dynamics [9], which enhances peak intensity and relaxes constrain for transverse momentum conservation. In accordance to our calculations, these two elements should greatly enhance the degenerate axial-signal gain, thus permitting the instability to begin. As axial intensity descends with propagation, as illustrated in Fig. 1 (b), the occurrence of larger gain at larger frequency shift is then expected to contribute in settling a coherent spectral broadening of the signal, where axial sidebands are produced and are boosted away from degeneracy with propagation, in the presence of conjugated off-axis idler components. The experimental observation of spectral width dynamics versus z presented in Fig. 4 is in qualitative agreement with calculation results outlined in Fig. 5. We mention that the outlined scenario does not consider the further impact of the temporal modication of the pump-pulse prole. Indeed, in analogy to what recently described for the spatio-temporal instability of the Townes beam, pulse splitting is expected to occur also for the present pulsed BB, seeded by interference between the pump and the amplied axial and conical waves [19]. Notably, a recursive temporal splitting of the pulse during propagation has to be forecasted in this case, owing to the replenishment feature of the conical propagation geometry. In analogy to what described by Agrawal [20] for the case of spectral broadening in bers, the pulse splitting dynamics might substantially impact (via cross-phase modulation) the instability gain prole, leading to the appearance of sidebands in normal dispersion as well. The interplay between this effect and what we have described above deserves therefore to be investigated. 5. Conclusion

In conclusion, we have demonstrated that differently from the Gaussian beam case, the broadband radiation excited by the BB appears here free from the exponential-like decay of intensity with increasing frequency shift, and free from the intense-pump component. Therefore it could be particularly useful for many applications demanding spectrally broadened (continuum) light pulses without strong residual radiation at the central frequency. The key factor which allows spectral broadening to overcome SRS was found to be important modication of transverse phase-matching condition by the nonlinearity that accompanies the abrupt transition between BB linear and nonlinear regimes. In fact, spectral broadening is quenched where the nonlinear dynamics is approached by focusing smoothly in the sample. The possible contribution of spatiotemporal modication of the pump pulse prole is also considered. Acknowledgment Authors thank E. Ku inskas for his valuable contribution in the early stages of the experiment. c P. P. acknowledges the support from Sixth EU Framework Programme Contract No. MESTCF-2004-008048 (ATLAS), P.D.T. acknowledges the support from Marie Curie Chair project STELLA, Contract No. MEXC-CT-2005-025710. This work is performed in the framework of
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VINO (the Virtual Institute for Nonlinear Optics) collaboration: www.vino-stella.eu.

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Received 24 January 2007; revised 8 March 2007; accepted 8 March 2007

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