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Single attosecond pulses from high harmonics driven by self-compressed laments

Himadri S. Chakraborty* and Mette B. Gaarde
Department of Physics and Astronomy, Louisiana State University, Baton Rouge, Louisiana 70803-4001

Arnaud Couairon
Centre de Physique Thorique, cole Polytechnique, CNRS F-91128, Palaiseau, France Received June 5, 2006; revised August 8, 2006; accepted September 19, 2006; posted September 22, 2006 (Doc. ID 71650); published November 22, 2006 We show that isolated subfemtosecond, extreme ultraviolet (XUV) pulses can be generated via harmonic generation in argon by few-cycle infrared pulses formed through lamentation-induced self-compression in neon. Our calculations show that the time structure of the XUV pulses depends sensitively on both the amplitude and the phase modulation that are induced in the driving pulse during the self-compression process. 2006 Optical Society of America OCIS codes: 190.7110, 320.5520, 320.7120.

It has recently been experimentally and theoretically demonstrated that few-cycle laser pulses can be efciently generated via lamentation-driven selfcompression in noble gases.14 This process has resulted in the compression of 800 nm, 30 40 fs pulses to durations of 4 8 fs and thus presents a viable alternative to the generation of few-cycle pulses in hollow bers.5 There is considerable interest in using these pulses to drive ultrafast nonlinear optics in general, and attosecond science in particular.6,7 Isolated attosecond extreme ultraviolet (XUV) pulses can be generated via the process of high harmonic generation (HHG) driven by a few-cycle infrared laser pulse. The highest harmonic energies are generated only at the peak of the laser pulse, and the spectral selection of a range of energies close to the harmonic cutoff energy therefore leads to the formation of a single pulse of subfemtosecond duration.6,8 In this Letter we present a theoretical study of attosecond pulse generation via HHG driven by lamentation-compressed few-cycle laser pulses. We show that an isolated and well-collimated 560 as burst of XUV light can be generated in argon when one is using an 800 nm driving pulse that has been compressed via lamentation in neon to a duration of 4 fs and a peak intensity of a few times 1014 W / cm2. We nd that both the rapid variation of the intensity envelope and the frequency chirp induced by selfphase modulation in the lament play important roles for the time structure of the XUV radiation. Our calculations are performed in two steps: (i) propagation, lamentation, and self-compression down to 1 2 cycles of the 800 nm, 30 fs laser pulse in a long neon gas cell at atmospheric pressure and (ii) harmonic generation in a separate, short argon gas cell at much lower pressure, driven by the laser pulse extracted from the neon lament at the desired propagation length. Such an extraction of the compressed pulse should be possible, for instance, using the recently proposed scenario of self-compression in a lament with a density gradient.2 Here we do not dwell upon the details of this extraction stage.
0146-9592/06/243662-3/$15.00

In step (i), we describe the lamentation process using numerical simulations of the nonlinear envelope equation. The model accounts for diffraction, group velocity dispersion with high-order terms, Kerr self-focusing, multiphoton absorption, plasma generation and plasma defocusing, spacetime focusing and self-steepening.3 Optical eld ionization constitutes the main contribution to plasma generation and is described from the modied Ammosov, Delone, and Krainov (ADK) theory.9,10 In step (ii),11 we solve the wave equation for the driving and the generated harmonic elds using the slowly evolving wave approximation,12 coupled with the solution of the time-dependent Schrdinger equation using the strong eld approximation.13 The time-dependent Schrdinger equation solution yields the single atom time-dependent dipole moment, and thereby the nonlinear polarization eld that leads to the formation of harmonics in the wave equation. The source term for the driving eld due to plasma oscillations is calculated using ADK ionization rates.9 This term is small, and the laser pulse propagates through the argon gas almost unaltered. Our main result is summarized in Fig. 1. First, an 800 nm, 30 fs, and 4 mJ Gaussian input pulse selffocuses in a 2 m long neon gas cell with an initial gas density of 2.5 1019 cm3. The formation of a lament over the z-range of 60 130 cm is evident in the beam width R z shown in Fig. 1(a). R z is calculated as the full width at half-maximum (FWHM) of the time-integrated intensity. During the lamentation stage, the peak intensity and the electron density exceed 3 1014 W / cm2 and 5 1016 cm3, respectively. The pulse duration, calculated as the FWHM of the intensity envelope radially integrated over 50 m, is also shown in Fig. 1(a). A strong compression of the pulse occurs progressively during the lamentation, resulting in the shortest duration of approximately 4 fs at z = 130 cm. The time prole of the laser pulse at this point is shown in Fig. 1(b). Next, this maximally compressed pulse is used to generate harmonics in a 1 mm long argon gas cell with a density of
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Fig. 1. (Color online) (a) Propagation dynamics of laser pulse during lamentation. Beam width (dashed curve, right axis) and pulse duration (solid curve, left axis) are shown versus propagation length z. (b) Laser pulse time prole at the point of maximum compression, z = 130 cm. This pulse is used to generate harmonics in the subsequent step. (c) Time prole of 40 eV XUV radiation, produced via HHG in a 1 mm argon gas cell.

5 1018 cm3. Finally, from the harmonic eld at the end of the argon cell we calculate the time prole of a 15 eV range of XUV radiation near the 40 eV cutoff energy of the harmonic spectrum. The resulting XUV time prole, shown in Fig. 1(c), presents a wellcollimated, isolated burst of XUV radiation with a duration of 560 as and an energy of a few pJ. The results presented in Fig. 1 are robust with respect to the choice of generating conditions as long as they lead to self-compression. Changing the noble gas species, the gas pressure, or the initial pulse energy or using different (multiphoton) ionization rates in the lamentation calculation leads to similar compression. The peak intensity of the maximally compressed pulse varies, with the most intense pulses obtained in neon, since its large ionization potential means that self-focusing is only balanced by plasma defocusing at high intensity. We have generated harmonics with pulses compressed in several different noble gases. In general, the XUV radiation around the harmonic cutoff energy is emitted in a single burst with duration of a few hundred attoseconds. We have also varied the carrier envelope phase of the driving pulse (which is locked to the phase of the initial 30 fs laser pulse1) and nd that several other, but not all, carrier envelope phases lead to single attosecond pulse generation. We next examine the inuence of the lamentation and self-compression dynamics on the HHG process, and in particular on the prospect for single attosecond pulse formation. Few-cycle pulses generated by self-compression in laments are in general not transform limited. Self-phase modulation, plasma defocusing, and self-steepening typically lead to an asymmetric pulse shape with a slowly increasing leading edge and a steep trailing edge [see Fig. 1(b)], accompanied by a rapid blueshift occurring over the peak of the pulse.4,14 Figure 2 shows harmonic spectra generated in argon by three different driving pulses extracted

from the lament at propagation lengths of z = 110, 120, 130 cm. Over this range of z, the peak intensity is approximately constant 3 1014 W / cm2 and the pulse duration decreases progressively from 10 to 4 fs [Fig. 1(a)]. The cutoff law would predict a cutoff energy of Ip + 3Up 45 0, where Ip is the argon ionization potential, 0 is the frequency corresponding to 800 nm, and the ponderomotive energy Up is proportional to the laser intensity and to the wavelength squared.15 However, the cutoff energy of each of the spectra in Fig. 2 is signicantly lower than 45 0 and furthermore decreases as the driving pulse is more strongly compressed [going from Fig. 2(a) to Fig. 2(c)]. We interpret the variation of the cutoff energy as a consequence of the rapid blueshift experienced by the laser pulse during self-compression. Figure 3 shows the on-axis time prole of the intensity and frequency of the driving eld at the point of extraction. The laser frequency increases to approximately 2 0 at the peak of the pulse, and even higher in the trailing edge. This frequency chirp means that the cutoff energy is reduced compared with that of an unchirped pulse with the same peak intensity. This is illustrated in Fig. 3 by the instantaneous cutoff energy curve, calculated by using the time-dependent laser intensity and frequency in the cutoff law, which indicates the highest harmonic energies that can be generated at any time during the pulse. These maximum energies are in good agreement with the cutoff energies observed in Fig. 2: Because of the large blueshift, the highest energy appears well before the peak of the laser pulse and is therefore lower than 45 0. Furthermore, the highest energy decreases going from Fig. 2(a) to Fig. 2(c). The blueshift also has consequences for the time structure of the XUV pulses. The time proles of a 10 0 range of harmonics close to the cutoff energies in the three different cases are shown in Figs.

Fig. 2. (Color online) Radially integrated harmonic spectra at the end of the argon gas, driven by laser pulses extracted at z = 110 (a), 120 (b), and 130 (c) cm. The spectral ranges synthesizing the XUV pulses are indicated.

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gate for the XUV emission with the highest photon energies. A single attosecond XUV pulse can therefore be synthesized by spectrally selecting the XUV radiation at and beyond the harmonic cutoff energy. The authors gratefully acknowledge fruitful discussions with M. Franco, A. Mysyrowicz, J. Biegert, and U. Keller. This material is based upon work supported by the Louisiana Board of Regents through grant LEQSF(2004-07)-RD-A-09 and by the National Science Foundation through grant PHY-0449235. M. Gaardes e-mail address is gaarde@phys.lsu.edu. *Present address, Department of Chemistry and Physics, Northwest Missouri State University, Maryville, Missouri 64468. References
1. C. P. Hauri, W. Kornelis, F. W. Helbing, A. Heinrich, A. Couairon, A. Mysyrowicz, J. Biegert, and U. Keller, Appl. Phys. B 79, 673 (2004). 2. A. Couairon, M. Franco, A. Mysyrowicz, J. Biegert, and U. Keller, Opt. Lett. 30, 2657 (2005). 3. A. Couairon, J. Biegert, C. P. Hauri, W. Kornelis, F. W. Helbing, U. Keller, and A. Mysyrowicz, J. Mol. Spectrosc. 53, 75 (2006). 4. G. Stibenz, N. Zhavoronkov, and G. Steinmeyer, Opt. Lett. 31, 274 (2006). 5. M. Nisoli, S. de Silvestri, O. Svelto, R. Szipcz, K. Ferencz, C. Spielmann, S. Sartania, and F. Krausz, Opt. Lett. 22, 522 (1997). 6. M. Hentschel, R. Kienberger, Ch. Spielmann, G. A. Reider, N. Milosevic, T. Brabec, P. Corkum, U. Heinzmann, M. Drescher, and F. Krausz, Nature 414, 509 (2001). 7. P. M. Paul, E. S. Toma, P. Breger, G. Mullot, F. Aug, Ph. Balcou, H. G. Muller, and P. Agostini, Science 292, 1689 (2001). 8. R. Kienberger, E. Goulielmakis, M. Uiberacker, A. Baltuska, V. Yakovlev, F. Bammer, A. Scrinzi, T. Westerwalbesloh, U. Kleineberg, U. Heinzmann, M. Drescher, and F. Krausz, Nature 427, 817 (2004). 9. M. V. Ammosov, N. B. Delone, and V. P. Krainov, Sov. Phys. JETP 64, 1191 (1986). 10. F. A. Ilkov, J. E. Decker, and S. L. Chin, J. Phys. B 25, 4005 (1992). 11. M. B. Gaarde, K. J. Schafer, A. Heinrich, J. Biegert, and U. Keller, Phys. Rev. A 72, 013411 (2005). 12. T. Brabec and F. Krausz, Rev. Mod. Phys. 72, 545 (2000). 13. M. Lewenstein, P. Balcou, M. Y. Ivanov, A. LHuillier, and P. B. Corkum, Phys. Rev. A 49, 2117 (1994). 14. A. L. Gaeta, Phys. Rev. Lett. 84, 3582 (2000). 15. J. L. Krause, K. J. Schafer, and K. C. Kulander, Phys. Rev. Lett. 68, 3535 (1992).

Fig. 3. (Color online) On-axis time structure of the driving eld intensity and frequency (dashed and dotted curves) extracted at z = 110 cm (a), 120 cm (b), and 130 cm (c). The thin solid lines show the resulting instantaneous harmonic cutoff energies. Radially integrated XUV time proles (in arbitrary units) at the end of the argon gas are shown by thick solid curves. The spectral ranges synthesizing the XUV pulses are indicated.

3(a)3(c). These harmonic energies are generated only around the peak of the instantaneous cutoff curves, and thus before the peak of the intensity envelope. Clearly, while the rising edge of the XUV pulse is shaped mainly by the increase in the IR intensity, the end of the XUV emission happens because the driving frequency becomes too high. It is this combined intensityfrequency effect that allows for the generation of a single 560 as pulse by the 4 fs driving pulse in Fig. 3(c).16 This mechanism is different from the generation of single attosecond pulses by transform-limited 4 5 fs pulses in which the duration of the XUV emission is restricted by the intensity variation only.8 In summary, we have studied the generation of attosecond XUV pulses by lamentation-driven selfcompressed few-cycle laser pulses. One advantage of these laser pulses is that they are naturally collimated while still having high peak intensities. The near absence of intensity and phase variation along the propagation axis leads to improved phase matching during the HHG process,17,18 and in our case to well-collimated XUV harmonics. We found that the rapid dynamic blueshift of the laser frequency, which leads to a reduction of the harmonic cutoff energy, in combination with the short duration of the selfcompressed pulse presents a steep timefrequency

16. Similar time/frequency gates are obtained in selfcompressed pulses extracted from a lament using a pressure gradient.
17. Y. Tamaki, J. Itatani, Y. Nagata, M. Obara, and K. Midorikawa, Phys. Rev. Lett. 82, 1422 (1999). 18. E. A. Gibson, A. Paul, N. Wagner, R. Tobey, S. Backus, I. P. Christov, M. M. Murnane, and H. C. Kapteyn, Phys. Rev. Lett. 92, 033001 (2004).