Modulated super-Gaussian laser pulse to populate a dark rovibrational state of acetylene.

A pulse-shaping technique in the mid-infrared spectral range based on pulses with a super-Gaussian temporal profile is considered for laser control. We show a realistic and efficient path to the population of a dark rovibrational state in acetylene (C2H2). The laser-induced dynamics in C2H2 are simulated using fully experimental structural parameters. Indeed, the rotation-vibration energy structure, including anharmonicities, is defined by the global spectroscopic Hamiltonian for the ground electronic state of C2H2 built from the extensive high-resolution spectroscopy studies on the molecule, transition dipole moments from intensities, and the effects of the (inelastic) collisions that are parameterized from line broadenings using the relaxation matrix [A. Aerts, J. Vander Auwera, and N. Vaeck, J. Chem. Phys. 154, 144308 (2021)]. The approach, based on an effective Hamiltonian, outperforms today's ab initio computations both in terms of accuracy and computational cost for this class of molecules. With such accuracy, the Hamiltonian permits studying the inner mechanism of theoretical pulse shaping [A. Aerts et al., J. Chem. Phys. 156, 084302 (2022)] for laser quantum control. Here, the generated control pulse presents a number of interferences that take advantage of the control mechanism to populate the dark state. An experimental setup is proposed for in-laboratory investigation.

Laser control of a dark vibrational state of acetylene in the gas phase-Fourier transform pulse shaping constraints and effects of decoherence.

We propose a methodology to tackle the laser control of a non-stationary dark ro-vibrational state of acetylene (C2H2), given realistic experimental limitations in the 7.7 µm (1300 cm-1) region. Simulations are performed using the Lindblad master equation, where the so-called Lindblad parameters are used to describe the effect of the environment in the dilute gas phase. A phenomenological representation of the parameters is used, and they are extracted from high-resolution spectroscopy line broadening data. An effective Hamiltonian is used for the description of the system down to the rotational level close to experimental accuracy. The quality of both the Hamiltonian and Lindblad parameters is assessed by a comparison of a calculated infrared spectrum with the available experimental data. A single shaped laser pulse is used to perform the control, where elements of optics and pulse shaping using masks are introduced with emphasis on experimental limitations. The optimization procedure, based on gradients, explicitly takes into account the experimental constraints. Control performances are reported for shaping masks of increasing complexity. Although modest performances are obtained, mainly due to the strong pulse shaping constraints, we gain insights into the control mechanism. This work is the first step toward the conception of a realistic experiment that will allow for population characterization and manipulation of a non-stationary vibrational "dark" state. Effects of the collisions on the laser control in the dilute gas phase, leading to decoherence in the molecular system, are clearly shown.

Nematicon-driven injection of amplified spontaneous emission into an optical fiber.

We investigate experimentally the interaction between amplified spontaneous emission (ASE) and a soliton, which are both generated in a dye-doped nematic liquid crystal (LC) cell. A light beam is injected through an optical fiber slid into the cell to form a soliton beam. ASE is then automatically collected by this self-induced waveguide and efficiently coupled into the same optical fiber, in the backward direction. We demonstrate that the presence of the soliton improves the ASE collection by one order of magnitude. We also show that the ASE is highly polarized in the plane of the LC cell and that the ASE spectrum depends on the pump stripe orientation with respect to the LC director. The origin of the spectral anisotropy of the gain curves is determined with the help of femtosecond pump-probe spectroscopy.

Measuring the nonlinear refractive index of graphene using the optical Kerr effect method.

By means of the ultrafast optical Kerr effect method coupled to optical heterodyne detection (OHD-OKE), we characterize the third-order nonlinear response of graphene and compare it to experimental values obtained by the Z-scan method on the same samples. From these measurements, we estimate a negative nonlinear refractive index for monolayer graphene, n2=-1.1×10-13 m2/W. This is in contradiction to previously reported values, which leads us to compare our experimental measurements obtained by the OHD-OKE and the Z-scan method with theoretical and experimental values found in the literature and to discuss the discrepancies, taking into account parameters such as doping.

Dispersive wave emission and supercontinuum generation in a silicon wire waveguide pumped around the 1550 nm telecommunication wavelength.

We experimentally and numerically study dispersive wave emission, soliton fission, and supercontinuum generation in a silicon wire at telecommunication wavelengths. Through dispersion engineering, we experimentally confirm a previously reported numerical study and show that the emission of resonant radiation from the solitons can lead to the generation of a supercontinuum spanning over 500 nm. An excellent agreement with numerical simulations is observed.

Nonlinear symmetry breaking induced by third-order dispersion in optical fiber cavities.

We study analytically, numerically, and experimentally the nonlinear symmetry breaking induced by broken reflection symmetry in an optical fiber system. In particular, we investigate the modulation instability regime and reveal the key role of the third-order dispersion on the asymmetry in the spectrum of the dissipative structures. Our theory explains early observations, and the predictions are in excellent agreement with our experimental findings.

Z-scan measurement of the nonlinear refractive index of graphene.

Under strong laser illumination, few-layer graphene exhibits both a transmittance increase due to saturable absorption and a nonlinear phase shift. Here, we unambiguously distinguish these two nonlinear optical effects and identify both real and imaginary parts of the complex nonlinear refractive index of graphene. We show that graphene possesses a giant nonlinear refractive index n(2)≃10(-7) cm(2) W(-1), almost 9 orders of magnitude larger than bulk dielectrics. We find that the nonlinear refractive index decreases with increasing excitation flux but slower than the absorption. This suggests that graphene may be a very promising nonlinear medium, paving the way for graphene-based nonlinear photonics.

Pattern formation without diffraction matching in optical parametric oscillators with a metamaterial.

We consider a degenerate optical parametric oscillator containing a left-handed material. We show that the inclusion of a left-handed material layer allows for controlling the strength and sign of the diffraction coefficient at either the pump or the signal frequency. Subsequently, we demonstrate the existence of stable dissipative structures without diffraction matching, i.e., without the usual relationship between the diffraction coefficients of the signal and pump fields. Finally, we investigate the size scaling of these light structures with decreasing diffraction strength.

Three-dimensional structures in nonlinear cavities containing left-handed materials.

We study the coupling between negative diffraction and direct dispersion in a nonlinear ring cavity containing slabs of Kerr nonlinear right-handed and left-handed materials. Within the mean field approximation, we show that a portion of the homogeneous response curve is affected by a three-dimensional modulational instability. We show numerically that the light distribution evolves through a sequence of three-dimensional dissipative structures with different lattice symmetry. These structures are unstable with respect to the upswitching process, leading to a premature transition to the upper branch in the homogeneous hysteresis cycle.

Dissipative structures in left-handed material cavity optics.

We study the spatiotemporal dynamics of spatially extended nonlinear cavities containing a left-handed material. Such materials, which have a negative index of refraction, have been experimentally demonstrated recently, and allow for novel electromagnetic behavior. We show that the insertion of a left-handed material in an optical resonator allows for controlling the value and the sign of the diffraction coefficient in dispersive Kerr resonators and degenerate optical parametric oscillators. We give an overview of our analytical and numerical studies on the stability and formation of dissipative structures in systems with negative diffraction.

Fast self-pulsing through nonlinear incoherent feedback.

We consider a double-pass ring cavity with nonlinear incoherent optical feedback and analyze its response when it is driven by a continuous laser beam. This particular cavity is equivalent, in the temporal domain, to a simple spatial-pattern-generating system made from a Kerr slice and a feedback mirror. After formulating the evolution equations, we investigate the behavior of small-amplitude solutions and obtain an expression for the round-trip gains. We then explore the important effect of dispersion in the nonlinear medium. Finally, we show that stable modes are possible by solving numerically the full nonlinear equations.

Experimental observation of the elliptically polarized fundamental vector soliton of isotropic Kerr media.

We report the experimental observation of the elliptically polarized fundamental vector soliton of isotropic Kerr media and its unique polarization evolution. This was achieved in the spatial domain in a nonbirefringent CS2 planar waveguide.