Appl. Phys. B 80, 3538 (2005) DOI: 10.

1007/s00340-004-1692-2

Applied Physics B
Lasers and Optics

q. luo1,u s.a. hosseini1 w. liu1 j.-f. gravel1 o.g. kosareva2 n.a. panov2 n. akozbek3 v.p. kandidov2 g. roy4 s.l. chin1

Effect of beam diameter on the propagation of intense femtosecond laser pulses

1 Centre

dOptique, Photonique et Laser (COPL) et D partement de Physique, e de G nie Physique et dOptique, Universit Laval, Qu bec, QC, G1K 7P4, Canada e e e 2 International Laser Center, Physics Department, M.V. Lomonosov Moscow State University, Moscow 119992, Russia 3 Time Domain Corporation, 7057 Old Madison Pike, Huntsville, Alabama 35806, USA 4 The Remote Sensing Group of the Defense Research and Development Center Valcartier (DRDC Valcartier), Val-Belair, QC, G3J 1X5, Canada

Received: 21 July 2004/Revised version: 6 October 2004 Published online: 10 November 2004 Springer-Verlag 2004
ABSTRACT This paper describes the effects observed during the

propagation of intense femtosecond laser pulses in air following the modication of the laser beam diameter with a pair of convexconcave lenses placed/mounted in a telescopic conguration. We observed that by reducing the diameter of the beam the detected back-scattered nitrogen uorescence from the laments becomes more stable on a shot-to-shot basis while, for a larger beam size, greater uctuations are observed that are not correlated to shot-to-shot uctuations in the laser pulse energy. This result leads to a new method to control the uorescence signal which can be very important in remote-sensing applications.
PACS 42.65.Jx;

42.68.Ay; 42.68.Wt

Introduction

The propagation of intense femtosecond laser pulses in air is a relatively complex phenomenon involving the strong reshaping of the spatial and temporal prole of the laser pulse through a combined action of linear and nonlinear effects [13]. The optical Kerr effect causes the beam to self-focus, resulting in an increase of the peak intensity. At high peak intensity, multiphoton/tunnel ionization (MPI/TI) of molecules and atoms in air takes place [4], resulting in the creation of a low-density plasma causing the beam to be de-focused. The dynamic balance between self-focusing and plasma de-focusing repeats itself, resulting in the formation of a plasma channel that is popularly called a lament. The nonlinear uorescence signal from nitrogen molecules (both neutral and ion) inside the lament has been previously reported within the spectral range of 300 420 nm [5, 6]. It has been demonstrated that nitrogen molecules are rst ionized inside the lament through the ejection of either an outermost electron or an inner valence electron [6, 7]. Radiative relaxation from excited states gives rise to nitrogen-ion uorescence. Electronion recombination then leads to the emission of the second positive band of the neutral N2 molecule [8]. Previous studies of the propagation of terawatt Tisapphire femtosecond laser pulses over a distance of 100 m in air have
u Fax: +1-418-6562623, E-mail: qi.luo.1@phy.ulaval.ca

shown that the back-scattered nitrogen uorescence signal (BSF) emitted from multiple laments was clearly detectable over the whole range using a lidar system [9]. However, the BSF signal uctuated signicantly on a shot-to-shot basis despite the rather stable laser pulse energy. By uctuations, we mean that the signal intensity distribution along the propagation path as well as the starting point of the lamentation varied randomly. The physical origin of these uctuations in the BSF signal can be attributed to a competition among multiple laments, which is a complex dynamical process evolving in the direction of the pulse propagation [10]. Numerical simulations and experiments have recently shown that an inhomogeneous intensity distribution in the transverse cross section of the pulse, which can originate from either initial laser imperfection or previous propagation through any non-homogeneous optical medium, ultimately leads to the formation of multiple laments co-propagating in air [1114]. Each initially independent lament (or so-called parent lament) emits radiation conically with respect to the propagation axis, giving rise to the routinely observed ring structure [15]. The interference of the divergent elds of neighboring laments initiates the formation and denes the position of new secondary laments (or so called child laments) if the resulting peak power of the perturbation formed due to the constructive interference is sufcient to induce self-focusing and lament formation [16]. The scenario of multiple-lament competition is very sensitive to the relative location of the initial perturbations. If the parent laments are initially far apart, the interference will be weak and the parent laments will compete with each other for energy with the surrounding (background) reservoir [1719]. Numerical simulations from different groups showed that when several laments are conned in a small volume, they can interact and self-maintain over much longer distances, whereas those distributed in a larger area decay much faster [10, 14, 17]. As a result, the plasma channels and the amplied back-scattered uorescence signal strongly depend on the intensity uctuations in the beam prole and on the relative distance between the initial laments. On the other hand, if the parent laments are closely spaced, the interference of the ring structure of these laments will generate a larger number of child laments, thus leading to a more

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Applied Physics B Lasers and Optics

intense plasma channel and therefore a stronger nitrogen uorescence signal. In order to investigate more about the competition of laments and ultimately have a better control of this process, we have forced the multiple laments to be closer to one another. This was achieved by decreasing the beam diameter with a convexconcave lens system. Since there is a close correlation between the plasma density and the uorescence signal, the characteristics of the BSF signal of nitrogen were monitored to follow the impact of these modications on the lamentation process.
2 Experimental setup

The experimental setup has been described elsewhere [9]. Briey, a femtosecond laser beam with a repetition rate of 10 Hz, 42 fs duration (FWHM), central wavelength of 800 nm with a bandwidth of 23 nm (FWHM) and linearly polarized is used in this experiment. The pulse energy can vary from a few mJ to 85 mJ. The standard deviation of the uctuations of the laser energy is 4.4%. The beam is guided from a vacuum compressor (103 Torr) to a corridor (length 101 m) through a 10 m vacuum pipe terminated with a 1.5 cm thick CaF2 window. In our experiments, a laser beam with two different diameters is used. The output beam diameter after the vacuum pipe is 25 mm (1/ e2 ). A telescope system consisting of a convex lens and a concave lens with 100 cm and -30 cm focal lengths, respectively, is introduced to decrease the beam diameter to 8 mm (1/ e2 ). The divergence of the small beam can be changed by varying the position of the concave lens. The BSF of nitrogen is collected with a lidar system and detected by a photomultiplier tube (PMT, Hamamatsu R7400P, with 1 ns response time; gain = 7 106). Considering that the lifetime of the N2 uorescence signal is around 1 2 ns [20], the resolution of this detection system is around 30 60 cm. The eld of view of the lidar is equal to 16 mrad. In most of our experiments, the lidar is put just behind the last mirror of the laser beam path and set at an on-axis position. In this conguration, the eld of view of the lidar system covers the whole range of the laser propagation, i.e. the geometrical overlapping factor is always 1 for any distance. In one of the experiments using the small-size laser beam, the lidar was moved to an off-axis position and a pinhole is set in front of the PMT in order to detect only the uorescence signal after the rst 35 m propagation distance of the laser pulse. The geometrical overlapping factor is 1 after 35 m. Two broadband dielectric mirrors reecting around 800 25 nm are placed in front of the PMT to eliminate any backscattering of the fundamental laser light. These are followed by a band-pass lter (UG 11, 4 mm thick, band pass 200 to 400 nm) transmitting the major spectral lines from nitrogen molecules and ions in the 300 400 nm region.
3 Experimental results and discussion

FIGURE 1 Two pictures of the laments. a The large beam diameter with 40 mJ input laser energy is used. Image is taken at 35 m from the last mirror where the laments start to develop. b The small beam diameter with 25 mJ input laser energy is used. Image is taken at 2.5 m from the last mirror where the laments start to develop

Single-shot pictures of the laser beam cross section are shown in Fig. 1 for (a) a large beam diameter and (b) a small beam diameter. These pictures were taken by a commercial digital camera (Canon A40) after 35 m from the last mirror, where the laments just start to develop. A whitepaper screen was inserted perpendicularly in the beam path

and the image created at the surface of the paper screen was captured by the camera. For the large beam (Fig. 1a), multiple laments are clearly observed since they are far from each other. One can clearly observe that one of the laments (in the center) is much brighter than the others. In contrast, in Fig. 1b, one can observe that the laments are squeezed together and cannot be resolved. Thus only one very bright spot is observed in the center. In Fig. 2, a three-dimensional graph of 300 shots at 30 mJ/pulse with large beam diameter (25 mm) is presented. The experiment was done with different energies of the laser pulse. In this graph the x axis is the direction of propagation of the beam that is calibrated from the time scale of the oscilloscope and the y axis represents the laser shot number. The rst small peaks at 0.0 m are due to the scattering of the pump pulse from the last mirror in the setup and the last peaks are from the beam stop that is xed at the end of the corridor. The middle peaks are BSF signals. A close analysis

LUO et al.

Effect of beam diameter on the propagation of intense femtosecond laser pulses

37

of the BSF signal distributions shown in Fig. 2 demonstrates that the uorescence signals change drastically from shot to shot. This irregularity is well explained in our competition model [10]. The BSF signal varies from shot to shot due to the random uctuation of the distance between the hot spots in the beam cross-sectional area. This leads to either a favorable or an unfavorable situation for the plasma channel formation. In the favorable case, the distances between the initial hot spots are shorter; the interference of the ring structure of these laments generates a larger number of child laments. It thus results in a large number of secondary plasma columns. Thus, more intense plasma channels stretching over longer distances can be observed. In the unfavorable case, the larger separation distance between the initial hot spots causes less powerful perturbations arising due to the interference and more competition for energy between these perturbations. The resulting uorescence signal is weaker. In Fig. 3, the BSF signal with the smaller beam size (8 mm) at 30 mJ/pulse is plotted. Here the telescope changes the beam size and forces the initial perturbations in the beam to be closer to each other. The signals show a dramatic change compared to Fig. 2. The BSF signals appear closer to the detector, i.e. the laments start earlier. This is due to the smaller beam size. The most important thing is that the signals are quite stable and strong from shot to shot, as our theoretical model predicted [10]. The beam size is so small that it forces the initial laments to develop closer to each other. The distance between the initial hot spots is shorter even than in the favorable case of the relative location of perturbations in the large beam. Indeed, the variation in the separation distance between the initial perturbations in the case of a large beam is of the order of 23% [10]. The beam is squeezed three times

FIGURE 3 300 shots of BSF waveform detected by PMT. The laser energy was xed at 30 mJ/pulse. By using the telescope the beam diameter is reduced to 8 mm

FIGURE 2 300 shots of BSF waveform detected by PMT. The laser energy was xed at 30 mJ/pulse. The diameter of the beam is 25 mm

when the diameter is decreased from 25 to 8 mm. Therefore, one might expect roughly a three times decrease in the separation distance between the initial perturbations, which are the seeds for the parent laments. Smaller separation between the parent laments leads to earlier formation and closer location of child laments. The average width of the laments and the corresponding plasma channels become larger. As a consequence, in the case of a smaller beam diameter more free electrons are generated. Hence, we can expect a much stronger BSF signal (Fig. 3). Even with random shot-to-shot uctuations in the separation distance between the initial perturbations, the plasma density remains high enough to provide a BSF signal at each shot. Thus, not only stronger but also more stable BSF signals are observed in the case of a smaller beam size. It is interesting to note that the strong signal lasts only up to a distance of around 10 m. After this region, it seems that no more uorescence signal can be detected. To further check the signal, we moved the lidar system to the off-axis position and put a pinhole in front of the PMT. In this setup, the lidar system cannot collect the signal from the rst 35 m of the laser beam propagation, so that the strong signal at the beginning is not detected. A higher sensitivity is obtained by increasing the high voltage of the PMT and using the more sensitive scale of the oscilloscope. We observed a uorescence signal for the whole range limited by the corridor. In Fig. 4, the average BSF signal of 300 shots is shown for the case of a smaller input beam size. This signal consists of two parts: the rst 40 m is taken from the rst set of experiments with an on-axis lidar position and the rest is from the second set of experiments with an off-axis lidar position. The signal is calibrated by taking into account the different gain of the PMT with different high voltages, the different os-

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Applied Physics B Lasers and Optics

cilloscope scales and geometrical overlapping factors due to different lidar positions. The signal is corrected for different distances by multiplying the measured signal by r 2 , where r is the distance between the signal and the lidar system. The BSF signals are very strong at the beginning of lament formation and decrease signicantly after about 10 m. After that, the weak signal stays at almost the same amplitude and extends to the end of the corridor. The weak signal shows that the plasma column could extend to a very long distance. However, we are limited by the corridor length and do not know what the total extent of the plasma column would be. The total extent of the plasma column due to multiple lamentation starts from the initial self-focal point where the powerful pulse at several hundred critical powers for self-focusing rst self-focuses and, in principle, would end where the peak power inside the pulse is decreased to just above the critical power for self-focusing. Even if the corridor is long enough, we might be limited by the sensitivity of our system and might still not be able to measure the total extent. We thus estimate what our current system could measure and dene this measurable extent of the plasma column as the effective length. In order to estimate the effective length in our current experiment, the average data of 300 shots (without r 2 correction) taken from the off-axis lidar position is plotted in the inset of Fig. 4. As described in [9], we t the tail part of the BSF signal using the lidar equation exp (r)/r 2 , where is the attenuation factor (dashed line). This curve can be extrapolated to the baseline of the BSF signal, which corresponds to the limit of our detection system. It suggests roughly an effective length of 564 m for laments that can be measured under this experimental condition provided that laments exist for this whole range. For the large-beam case, the detectable maximum effective lament length at 60 mJ is only 196 m [9]. It is important to note that a small region can be determined at the beginning of the lament in which the signal is strong. This could be very important for locating the position of the pollutant precisely in a remote-sensing application. This small region at the beginning of self-focusing can be moved, in principle, by varying any or all of the following parameters: beam divergence, chirp, beam diameter and pulse energy (peak power). More experimentation needs to be done on this separate engineering subject.

Summary and conclusions

We measured the back-scattered uorescence signal from nitrogen molecules in the laments in air generated from an intense femtosecond laser pulse with two different beam diameters, 25 mm and 8 mm. When the beam size is decreased, the separation of the initial perturbations gets closer. The interference of these initial laments leads to the formation of a larger number of child laments and, as a consequence, a more intense and stable plasma channel, which gives rise to a higher uorescence signal. The understanding of the initiations of multiple laments, consequent propagation and interaction dynamics is important in the control of random uctuations of the input laser pulse that may lead to longer propagation distances. This is particularly important for potential lidar applications in atmospheric sensing and pollutant measurement.
ACKNOWLEDGEMENTS We would like to acknowledge the technical support of M. Martin. This work was supported in part by NSERC, DRDC Valcartier, Canada Research Chairs, CIPI and FQRNT. O.G. Kosareva, N.A. Panov and V.P. Kandidov acknowledge the support of the European Research Ofce of the US Army under Contract No. N6255804-P-6051 the and Russian Foundation for Basic Research (Grant No. 0302-16939). V.P. Kandidov, O.G. Kosareva and S.L. Chin acknowledge the support of the NATO Linkage (Grant No. PST.CLG.976981).

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FIGURE 4

The averaged BSF signal for 300 shots. The inset is the tail part of the signal, the dashed line is the tted curve. Initial beam diameter is 8 mm