Ultrafast and octave-spanning optical nonlinearities from strongly phase-mismatched cascaded interactions

Cascaded nonlinearities have attracted much interest, but ultrafast applications have been seriously hampered by the simultaneous requirements of being near phase-matching and having ultrafast femtosecond response times. Here we show that in strongly phase-mismatched nonlinear frequency conversion crystals the pump pulse can experience a large and extremely broadband self-defocusing cascaded Kerr-like nonlinearity. The large cascaded nonlinearity is ensured through interaction with the largest quadratic tensor element in the crystal, and the strong phase-mismatch ensures an ultrafast nonlinear response with an octave-spanning bandwidth. We verify this experimentally by showing few-cycle soliton compression with noncritical cascaded second-harmonic generation: Energetic 47 fs infrared pulses are compressed in a just 1-mm long bulk lithium niobate crystal to 17 fs (under 4 optical cycles) with 80% efficiency, and upon further propagation an octave-spanning supercontinuum is observed. Such ultrafast cascading is expected to occur for a broad range of pump wavelengths spanning the near- and mid-IR using standard nonlinear crystals.Comment: resubmitted, revised version, accepted for Phys. Rev. Let

Generating mid-IR octave-spanning supercontinua and few-cycle pulses with solitons in phase-mismatched quadratic nonlinear crystals

We discuss a novel method for generating octave-spanning supercontinua and few-cycle pulses in the important mid-IR wavelength range. The technique relies on strongly phase-mismatched cascaded second-harmonic generation (SHG) in mid-IR nonlinear frequency conversion crystals. Importantly we here investigate the so-called noncritical SHG case, where no phase matching can be achieved but as a compensation the largest quadratic nonlinearities are exploited. A self-defocusing temporal soliton can be excited if the cascading nonlinearity is larger than the competing material self-focusing nonlinearity, and we define a suitable figure of merit to screen a wide range of mid-IR dielectric and semiconductor materials with large effective second-order nonlinearities $d_{\rm eff}$. The best candidates have simultaneously a large bandgap and a large $d_{\rm eff}$. We show selected realistic numerical examples using one of the promising crystals: in one case soliton pulse compression from 50 fs to 15 fs (1.5 cycles) at 3.0\mic is achieved, and at the same time a 3-cycle dispersive wave at 5.0\mic is formed that can be isolated using a long-pass filter. In another example we show that extremely broadband supercontinua can form spanning the near-IR to the end of the mid-IR (nearly 4 octaves).Comment: submitted to Optics Materials Express special issue on mid-IR photonic

Scaling laws for soliton pulse compression by cascaded quadratic nonlinearities

We present a detailed study of soliton compression of ultra-short pulses based on phase-mismatched second-harmonic generation (\textit{i.e.}, the cascaded quadratic nonlinearity) in bulk quadratic nonlinear media. The single-cycle propagation equations in the temporal domain including higher-order nonlinear terms are presented. The balance between the quadratic (SHG) and the cubic (Kerr) nonlinearity plays a crucial role: we define an effective soliton number -- related to the difference between the SHG and the Kerr soliton numbers -- and show that it has to be larger than unity for successful pulse compression to take place. This requires that the phase mismatch be below a critical level, which is high in a material where the quadratic nonlinearity dominates over the cubic Kerr nonlinearity. Through extensive numerical simulations we find dimensionless scaling laws, expressed through the effective soliton number, which control the behaviour of the compressed pulses. These laws hold in the stationary regime, in which group-velocity mismatch effects are small, and they are similar to the ones observed for fiber soliton compressors. The numerical simulations indicate that clean compressed pulses below two optical cycles can be achieved in a $\beta$-barium borate crystal at appropriate wavelengths, even for picosecond input pulses.Comment: 11 pages, 8 figures, resubmitted version, to appear in October issue of J. Opt. Soc. Am. B. Substantially revised, updated mode

Limits to compression with cascaded quadratic soliton compressors

We study cascaded quadratic soliton compressors and address the physical mechanisms that limit the compression. A nonlocal model is derived, and the nonlocal response is shown to have an additional oscillatory component in the nonstationary regime when the group-velocity mismatch (GVM) is strong. This inhibits efficient compression. Raman-like perturbations from the cascaded nonlinearity, competing cubic nonlinearities, higher-order dispersion, and soliton energy may also limit compression, and through realistic numerical simulations we point out when each factor becomes important. We find that it is theoretically possible to reach the single-cycle regime by compressing high-energy fs pulses for wavelengths $\lambda=1.0-1.3 \mu{\rm m}$ in a $\beta$-barium-borate crystal, and it requires that the system is in the stationary regime, where the phase mismatch is large enough to overcome the detrimental GVM effects. However, the simulations show that reaching single-cycle duration is ultimately inhibited by competing cubic nonlinearities as well as dispersive waves, that only show up when taking higher-order dispersion into account.Comment: 16 pages, 5 figures, submitted to Optics Expres

Optical Cherenkov radiation by cascaded nonlinear interaction: an efficient source of few-cycle energetic near- to mid-IR pulses

When ultrafast noncritical cascaded second-harmonic generation of energetic femtosecond pulses occur in a bulk lithium niobate crystal optical Cherenkov waves are formed in the near- to mid-IR. Numerical simulations show that the few-cycle solitons radiate Cherenkov (dispersive) waves in the \lambda=2.2-4.5\mic range when pumping at \lambda_1=1.2-1.8\mic. The exact phase-matching point depends on the soliton wavelength, and we show that a simple longpass filter can separate the Cherenkov waves from the solitons. The Cherenkov waves are born few-cycle with an excellent Gaussian pulse shape, and the conversion efficiency is up to 25%. Thus, optical Cherenkov waves formed with cascaded nonlinearities could become an efficient source of energetic near- to mid-IR few-cycle pulses.Comment: Extended version of Nonlinear Optics 2011 contribution http://www.opticsinfobase.org/abstract.cfm?URI=NLO-2011-NTuA7. Submitted for Optics Express special issue for NLO conferenc

Quantum spatial correlations in high-gain parametric down-conversion measured by means of a CCD camera

We consider travelling-wave parametric down-conversion in the high-gain regime and present the experimental demonstration of the quantum character of the spatial fluctuations in the system. In addition to showing the presence of sub-shot noise fluctuations in the intensity difference, we demonstrate that the peak value of the normalized spatial correlations between signal and idler lies well above the line marking the boundary between the classical and the quantum domain. This effect is equivalent to the apparent violation of the Cauchy-Schwartz inequality, predicted by some of us years ago, which represents a spatial analogue of photon antibunching in time. Finally, we analyse numerically the transition from the quantum to the classical regime when the gain is increased and we emphasize the role of the inaccuracy in the determination of the symmetry center of the signal/idler pattern in the far-field plane.Comment: 21 pages, 11 figures, submitted to J. Mod. Opt. special issue on Quantum Imagin

Nonlocal explanation of stationary and nonstationary regimes in cascaded soliton pulse compression

We study soliton pulse compression in materials with cascaded quadratic nonlinearities, and show that the group-velocity mismatch creates two different temporally nonlocal regimes. They correspond to what is known as the stationary and nonstationary regimes. The theory accurately predicts the transition to the stationary regime, where highly efficient pulse compression is possible.Comment: 3 pages, 2 figures, published verison in Optics Letters. Contains revised equations, including an updated mode