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Sub-two-cycle gigawatt-peak-power LWIR OPA for ultrafast nonlinear spectroscopy of condensed state materials

Vyacheslav Leshchenko, Sha Li, Pierre Agostini, and Louis F. DiMauro

Open Access Open Access

Abstract

The application of high-power, few-cycle, long-wave infrared (LWIR, 8–20 µm) pulses in strong-field physics is largely unexplored due to the lack of suitable sources. However, the generation of intense pulses with >6 µm wavelength range is becoming increasingly feasible with the recent advances in high-power ultrashort lasers in the middle-infrared range that can serve as a pump for optical parametric amplifiers (OPA). Here we experimentally demonstrate the feasibility of this approach by building an OPA pumped at 2.4 µm that generates 93 µJ pulses at 9.5 µm, 1 kHz repetition rate with sub-two-cycle pulse duration, 1.6 GW peak power, and excellent beam quality. The results open a wide range of applications in attosecond physics (especially for studies of condensed phase samples), remote sensing, and biophotonics.

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Data availability

Data underlying the results presented in this paper are not publicly available at this time but may be obtained from the authors upon reasonable request.

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Figures (4)
Fig. 1.
Fig. 1. Phase-matching-based low-signal gain at 2.4 µm pump wavelength as a function of the phase matching angle ($\Theta$) and idler wavelength for (a) GaSe type II (o-signal, e-idler); (b) GaSe type I; (c) AgGaSe2 type II (o-signal, e-idler); (d) AgGaSe2 type I. The color scale is normalized to unity maximum value for every plot separately. Dispersion data from Refs. [12,13] is used in simulations.

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Fig. 2.
Fig. 2. Scheme of the experimental setup: LPF, long-pass filter; WLG, white-light generation.

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Fig. 3.
Fig. 3. (a) Output power stability. (b) Pulse quality (M-squared) measurement. Points are the measured beam size defined as the second moment width (D4$\sigma$), according to the ISO Standard 11146. Lines are the fits of the experimental data, based on which $M_x^2=1.1, M_y^2=1.3$. The range of negative distances was limited by the need to use reflective focusing optics (a spherical mirror) and adding a pair of wedges to reduce the power to a save level for the camera. (c) Beam profile at focus (0 cm distance). (d) Beam profile out of focus (120 cm distance).

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Fig. 4.
Fig. 4. (a) Signal spectrum measured after different amplification stages. (b) Reconstructed spectral intensity and phase. The light blue curve is the idler spectrum calculated from the signal spectrum measured after the third stage; the dark blue curve is the spectrum from the “time-domain observation of an electric field” (TIPTOE) measurement; the green curve is the phase reconstructed from the TIPTOE measurement. (c) TIPTOE signal corresponding to the pulse electric field (blue) and the reconstructed pulse intensity: filled green, reconstructed TIPTOE result; orange, transform limited (TL) pulse. (d) Spectrum of high-order harmonics generated in ZnTe. Vertical dashed lines identify expected positions of harmonics. The gap in the data is caused by the gap between the spectral ranges of the available spectrometers.

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Equations (1)

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W idler / ω idler = W signal / ω signal = W pump / ω pump ,
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