Optics Communications 233 (2004) 411416 www.elsevier.

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Backward time-resolved spectroscopy from lament induced by ultrafast intense laser pulses
Q. Luo *, S.A. Hosseini, B. Ferland, S.L. Chin
Center dOptique, Photonique et Laser (COPL), Dpartement de physique, de gnie physique et doptique, e e Universit Laval, Qubec, QC, Canada G1K 7P4 e e Received 23 July 2003; received in revised form 7 January 2004; accepted 23 January 2004

Abstract The time-resolved spectral distribution of backscattered light from laments generated by intense ultrafast Ti:sapphire laser pulses propagating in air is studied. Clean uorescence from N2 molecules and ions are detected in the backward direction which could be useful in remote sensing application. 2004 Elsevier B.V. All rights reserved.
PACS: 42.68.Ay; 42.62.Fi Keywords: Ultrafast intense laser pulse; Propagation; Time-resovled spectroscopy

1. Introduction The propagation of intense ultrafast laser pulse propagating in optical materials has been investigated extensively since the chirped pulse amplication (CPA) technique was developed in the 1980s. The peak power of femtosecond laser pulses has reached the petawatt (1015 W) level nowadays. Even at peak power several orders of magnitude lower (101012 W), nonlinear eects already become dominant in the pulse propagation processes. This results in the production of laments [13], which

Corresponding author. Tel.: +1-418-6562131x4482; fax: +1418-6562623. E-mail address: qluo@phy.ulaval.ca (Q. Luo).

are created by a dynamical interplay between two nonlinear eects, i.e., Kerr self-focusing and subsequent defocusing by the plasma that is generated through multiphoton/tunnel ionization of the molecules and atoms. The intensity inside the lament is clamped due to this balancing eect [47]. Self-phase modulation (SPM) and self-steepening of the pulse give rise to a strong broadening of the spectrum. The supercontinuum spectral extent has been observed from near UV to near infrared up to 4.5 lm [8]. Experimental observation indirectly [9] indicates that long laments are formed up to several hundred meters in the atmosphere. This makes this phenomenon very promising for LIDAR application. A terawatt femtosecond Ti:sapphire laser system mounted on a mobile unit (Teramobile)

0030-4018/$ - see front matter 2004 Elsevier B.V. All rights reserved. doi:10.1016/j.optcom.2004.01.056

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was recently built to carry out long-range propagation experiments in air and LIDAR type of measurements in the atmosphere [10]. In air, the so-called clean uorescence of nitrogen molecules and ions is obtained by collecting the uorescence from the side of the lament [6,11]; i.e., the contribution of the supercontinuum and the low density plasma emission is quite low and does not mask the spectral features. This should be contrasted to the strong high density plasma emission from optical breakdown induced by long (nanosecond) pulses. The weak plasma density resulting from intensity clamping inside the lament is at least 34 orders of magnitude lower than that of atmospheric air density [6,1113]. The spectra from air have been assigned to the rst negative band B2 R ! X 2 R of N and the 2 u g second positive band C 3 Pu ! B3 Pg of N2 . The uorescence signal was recently applied to measure the lament length in the backscattering direction for distances up to 100 m [14]. It was shown that the peak intensity inside the series of foci is clamped down to about 5 1013 W/ cm2 in air [46]. Inside the self-focal region of the femtosecond laser pulse, the intensity is high enough to ionize and dissociate the molecules. Due to the complex mechanisms of interaction of the intense femtosecond laser pulses with molecules and atoms, we expect dierent products resulting in distinguishable uorescence. Such dierence in the uorescence spectra from dierent molecules and atoms could be very useful for the LIDAR technique. However, one has to be careful to detect such clean uorescence spectra but not to detect white light generated in the lament in a LIDAR measurement. Although there were hints in our previous experiments that the uorescence from nitrogen but not white light can be detected in the backward direction, it is necessary to make a systematic spectroscopy study to investigate the cleanliness of the backscattered uorescence spectra. In this work we investigate experimentally the time-resolved spectral distribution of the backscattered light when the femtosecond laser pulse propagates in air by using a time-resolved technique. In the backward direction, only clean uorescence from the nitrogen molecules and ions inside the lament is observed.

2. Experiment setup The high power femtosecond laser system consists of a Ti:sapphire oscillator (Spectra Physics Maitai) followed by a regenerative amplier (Spectra Physics Spitre), a two-pass Ti:sapphire amplier pumped by a Quanta-Ray Nd:YAG laser and a compressor. The seed beam passes through a spatial lter before entering into the 2-pass amplier to obtain good beam quality. The pulse duration at the output of the compressor is about 42 fs measured by a single-shot autocorrelator and the central wavelength is 810 nm with a band width of 23 nm (FWHM). The maximum output energy is about 15 mJ per pulse at the repetition rate of 10 Hz. The experimental setup is shown in Fig. 1. The laser beam propagates in air without any lens. At 3 m after the compressor, a dielectric mirror (M1) with high reectivity at around 800 nm (bandwidth 100 nm) and high transmission for UV light is used to reect the beam at 45 incident angle. In the inset of Fig. 1, the transmission curve of M1 is shown. Along the propagation direction of the

filament

6m

10 Hz, 42fs pulses

T%

80

M1

40 0 300 600 900 1200

M2 Spectrometer+ICCD

Wavelength (nm)

Fig. 1. The experimental setup. M1: dielectric mirror for 800 nm for 45 incident angle; M2: dielectric mirror for 800 nm for 0 incident angle. The inset is the transmission curve of M1 and M2.

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laser beam, the lament is generated. A beam dump blocks the laser beam before the wall in order to reduce the strong scattering from the wall. The distance between the last mirror and the beam dump is around 6 m. The backscattered uorescence from the lament in air is collected by a fused-silica lens (2 in. diameter) and then sent into a spectrometer (spectropro500i) connected to an ICCD camera (PI-MAX 512RB). A dielectric coated fused-silica mirror (M2) which has the same transmission curve as M1 is put before the slit in order to lter out the scattered laser light. For all the spectra shown in this work, the slit size is opened to 200 lm and a 300 g/mm grating blazed at 500 nm is used. The timing for the laser pulses arriving at the last mirror in the beam path is 140 ns earlier than the trigger signal for the ICCD camera. The gate width of the ICCD in this work is 5 ns which corresponds to 0.75 m resolution in distance. We have measured that the nitrogen uorescence lifetime is 23 ns which is less than 5 ns [15] and the white light generation and scattering processes happen instantaneously with the laser pulse excitation. Therefore by controlling the dierent gating time of the ICCD, the backscattered signal from dierent ranges can be resolved and detected.

/100

(h) 5.25-6m (g) 4.5-5.25m (f) 3.75-4.5m

Signal (arb. units)

(d) 2.25-3m

(c) 1.5-2.25m (b) 0.75-1.5m (a) 0-0.75m

200 400 600 800 1000

Wavelength (nm)
Fig. 2. The spectra for dierent ranges between the last mirror and the beam dump. In (a)(g), the vertical scale is linear scale. In (h), the spectrum is calibrated by the transmission curve of M1 and M2 and the vertical scale is in log scale. The input laser energy is 13 mJ.

3. Experimental results and discussion Fig. 2 shows the spectra scanned from 2501000 nm using dierent gating time of ICCD with input laser energy of 13 mJ. Each of the spectra is an accumulation of 200 shots. We take the last mirror (M1) in the beam path as zero position. In Fig. 2(a), there is a peak corresponding to the laser spectrum that is caused by the strong scattering of the laser pulses hitting the last mirror in the beam path. At 1.53 m region, a group of peaks appear in 300400 nm region which are from nitrogen molecules and ions [11,12] as shown in Fig. 2(d) and (c). In the longer wavelength, there is no signal. The spectra from nitrogen molecules and ions are very clean, i.e., there is no detectable continuum background mixed with the uorescence peaks. In the following regions, there are almost no signals (Fig. 2(e)(g)). In Fig. 2(h), a

strong continuum band is observed at 6 m where the beam dump is located. We move the beam dump 2 m closer to the last mirror and take the spectra. For this conguration, the strong continuum band appears at 4 m position. This shows that the continuum band is caused by the scattering from the beam dump. The ranged resolved spectra with dierent input laser energies are also measured. The uorescence spectra appears later with decreasing laser energy while the strong continuum band is always detected at the 6 m position. When an intense femtosecond pulse starts to propagate in air, it takes a certain distance to form the lament. This self-focal distance is determined by the input laser power. Before the self-focal distance, the scattering from air is too weak to be detected as shown in Fig. 2(b). At the self-focal distance, the plasma is induced and the lament is created from there on. Nitrogen molecules will go through ionization and recombination processes and are populated in the excited states followed by uorescence (Fig. 2(c)). When the laser power

laser propagating direction

(e) 3-3.75m

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(energy) increases, the self-focal distance is shorter. Hence the positions where uorescence spectra appear vary with the input laser energy. We check the laments length by using a burn paper to look at the strong spots in the beam. It is found that the lament extends into the beam dump. But the uorescence spectra are observed only at the rst 1.5 m of the lament. To check it, we performed another experiment. An interference lter (center wavelength 337 nm, bandwidth 5 nm) is used to choose one of the nitrogen uorescence. The backscattered uorescence is detected by a PMT (2 ns time resolution). We chose this line at 337 nm because the spectrum of the white light generated in air only extends to 350 nm [8]. At this wavelength, the signal detected by the PMT only includes the uorescence signal but not the white light. As shown in Fig. 3, one strong peak followed by another weaker peak is detected in the 1.53.5 m region which corresponds to the uorescence spectra in Fig. 2(c) and (d). The time-resolved spectra cannot distinguish the two peaks because of the long time resolution (5 ns) of the ICCD system. After that, the uorescence signal is still detectable but is roughly 10 times weaker. Since the ICCD measures the signals dispersed by the spectrometer and has less gain compared to the

PMT, the sensitivity of the spectral measurement system (ICCD and spectrometer) is less than that of the PMT. Thus the time-resolved spectra using ICCD only showed the uorescence in the beginning of the lament. In the regions after the strong peaks, the uorescence is too low to be measured by the ICCD, even though there was a small degree of uorescence. In Fig. 3 there is another strong peak at 6 m position caused by the scattering of the beam dump. When the lament is formed, the laser pulse self-transforms into a white light pulse [16] due to SPM and self-steepening that is stopped by the beam dump. The strong white light comes from the scattering by the dump. Note that no backscattered white light is detected before the beam hits the dump. In Fig. 4, a spectrum from air scanned from 3001000 nm is shown. The laser beam is focused by f 1 m lens and input laser energy is 13 mJ. The uorescence signals and the scattered lights are collected at right angle to the laser propagation direction and the spectra are measured using an imaging spectrometer (Acton Research Corp., Spectrapro-150) with150 g/mm grating and a CCD camera (Princeton Instruments 770E). The spectrum has been calibrated by the grating eciency

6
Fluorescence intensity (arb. units)

5 4

1,0 0,8 0,6 0,4 0,2 0,0

Distance (m)

3 2 1 0 0.0 0.2 0.4 0.6 0.8 Signal (arb. units) 1.0

400

600 800 Wavelength (nm)

1000

Fig. 3. The uorescence signal at 337 nm detected by the PMT. The input laser energy is 13 mJ.

Fig. 4. The spectrum from 3001000 nm collected at right angle to the laser propagation. The laser beam is focused by f 1 m lens and input laser energy is 13 mJ.

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curve and CCD Quantum eciency. In Fig. 4, it is shown that the intensity of the scattered 810 nm laser light is roughly of the same order of magnitude as the uorescence signal from nitrogen. It has been measured that the intensity of the broadened anti-Stokes and Stokes spectra, especially in the 300400 nm region where nitrogen uorescence exists, is more than 3 orders of magnitude lower than that at the central wavelength of 810 nm [8]. Thus the white light scattering is expected to be 3 orders of magnitude lower than the uorescence signal. This is also true in the backward direction since the scattering and the uorescence radiations are isotropic. Recently we have proved that the uorescence from nitrogen molecules is amplied when it propagates back along the lament [17], i.e., the uorescence signal should be even stronger in the backward direction. In the case of laser free-propagation in air, the plasma density and laser intensity inside the lament would be the roughly the same as that generated in a focusing geometry due to intensity clamping inside the lament [46]; thus the scattering and uorescence processes would give rise to similar results as in the case of a focusing geometry. Therefore in Fig. 2, the scattering signal from the white light, which is expected to be 1000 times weaker than the uorescence signal, is too weak to be observed. In our lab, the dust density level is 105 per cubic-foot which is much cleaner than the outside atmosphere. There are no strong scattering produced by dust or large particles such as aerosol. The backscattered white light signal is thus much weaker than the uorescence signal from nitrogen molecules and ions and cannot be detected in our experiment inside our laboratory. In an outdoor atmosphere environment, the scattering processes are expected to be dierent from that in a clean laboratory. Further experiment needs to be done to investigate the outdoor backscattered uorescence spectra in the future.

of an intense femtosecond laser pulse in air are measured. Strong and clean uorescence signals from nitrogen molecules and ions are detected at the position where lament forms. The white light scattering is too weak to be detected in our experiments.

Acknowledgements We would like to acknowledge Prof. H. Schroeder for the constructive and fruitful discussion. This work was supported in part by DRDC-Valcartier, NSERC, CFI, CIPI, FQRNT and Canada Research Chairs. The collaboration of Spectra Physics in setting up the versatile laser system in Laval University is particularly appreciated.

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4. Conclusion The spectral components of backscattered light from dierent ranges during the free-propagation

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