In this work, we show that injecting a single space-time-coupled light pulse-beam into a multimode graded-index fiber generates a train of multimode solitons. Space-time couplings excite the spatial modes with distinct temporal profiles. Due to nonlinear interactions, with a properly chosen input power these profiles split into several unique multimode solitons. In the case of a spatially chirped input pulse, two solitons composed of modes LP_01 and LP_11 are formed. In the case of the injection of a space-time optical vortex, characterized by its topological charge ℓ, a train composed of |ℓ| + 1 multimode solitons is generated. Their energy and modal composition are directly determined by the absolute value of the topological charge.

The initial conditions in multimode fibers pumped by ultrashort laser pulses strongly determine the following nonlinear optical interactions. In this work we firstly compare the detailed spatial mode content of simple initial conditions, transverse offset and tilt. We then show how those initial conditions can both be used to achieve beam self-cleaning into higher-order spatial modes of a model graded-index fiber, with their own slight differences and advantages. Going beyond purely spatial initial conditions, we introduce self-cleaning results using spatial chirp at the input facet, whereby the different temporal envelopes of the spatial modes allows for tuning the self-cleaning process. Our results open up investigations into higher-dimensional tuning of nonlinear processes in multimode fibers using initial conditions.

The non-intuitive spatiotemporal modal content of space-time optical vortices (STOVs) is calculated in a graded-index fiber supporting a large number of propagating modes. We discuss how a fiber supporting many modes allows to truly couple higher-order STOVs, the number of modes necessary to support a STOV of a certain order, and conversely the truncation effect in a few-mode fiber. Based on the excited modes and their temporal profiles, we show numerical results for the linear and nonlinear propagation of STOVs in multimode fibers, specifically the linear space-time beating at short propagation distances, and the nonlinear trapping effect between modes producing stable states on long propagation distances. Our results underline how STOVs present a rich platform for multimode nonlinear optics and technology.

The initial conditions in multi-mode fibers pumped by ultrashort laser pulses strongly determine the following nonlinear optical interactions. In this work we firstly compare the detailed spatial mode content of simple initial conditions, transverse offset and tilt. We then show how those initial conditions can both be used to achieve a nonlinear modal energy transfer into higher-order spatial modes of a model graded-index fiber, with their own slight differences and advantages. Going beyond purely spatial initial conditions, we introduce nonlinear modal energy transfer results using spatial chirp at the input facet, whereby the different temporal envelopes of the spatial modes allow for tuning the nonlinear modal energy transfer process. Our results open up investigations into higher-dimensional tuning of nonlinear processes in multi-mode fibers using initial conditions.

An example of a beam with angular dispersion in its focus coupled to a graded-index fiber is used to demonstrate one way to merge free-space and waveguide space-time optics.

Guided wave optics, including most prominently fiber optics and integrated photonics, very often considers only one or very few spatial modes of the waveguides. Despite being known and utilized for decades, multi-mode guided wave optics is currently rapidly increasing in sophistication in parallel with technological improvements and advancing simulation tools. The physics of multi-mode interactions are usually driven by some initial energy distribution in a number of spatial modes. In this work we introduce how, with free-space input beams having space-time couplings, the different modes can be excited with different complex frequency or time profiles. We cover fundamentals, the coupling with a few simple space-time aberrations, different waveguides, and a number of technical nuances. This concept of space-time initial conditions in multi-mode waveguides will provide yet another tool to study the rich nonlinear interactions in such systems.

Bidimensional materials are ideally viewed as having no thickness, as their name suggests. Their optical response have been previously modelled by a purely bidimensional surface current or by a very thin film with some contradictory results. The advent of multilayer stacks of bidimensional materials and combinations of different materials in vertical van der Waals heterostructures highlights, however, that these materials have a finite thickness. In this article, we propose a new model that reconciles both approaches and we show how volume properties of stacked bidimensional layers can be calculated from the bidimensional response of each individual layer, and conversely. In our approach, each bidimensional layers is surrounded by vacuum and described as a kind of transfer matrix with intrinsic parameters that do not depend on the external medium. This provides a link between continuous thin films and discrete layers. We show how to model heterostructures of bidimensional materials and identify the parameters of the current sheet that represents the bidimensional material in the zero -thickness limit, namely the in-plane surface susceptibility and the out-of-plane displacement susceptibility. We show that our unified model is perfectly compatible with existing ellipsometric data with the same reliability as the existing interface model but with different values of the surface susceptibility or bulk dielectric function. We discuss in detail the origin of the discrepancies and show that our approach allows to determine intrinsic properties of the bidimensional materials with the advantage that multilayer and monolayer systems are described in a same framework.

2D materials offer a large variety of optical properties, from transparency to plasmonic excitation. They can be structured and combined to form heterostructures that expand the realm of possibility to manipulate light interactions at the nanoscale. Appropriate and numerically efficient models accounting for the high intrinsic anisotropy of 2D materials and heterostructures are needed. In this article, we retrieve the relevant intrinsic parameters that describe the optical response of a homogeneous 2D material from a microscopic approach. Well-known effective models for vertical heterostructure (stacking of different layers) are retrieved. We found that the effective optical response model of horizontal heterostructures (alternating nano-ribbons) depends of the thickness. In the thin layer model, well adapted for 2D materials, a counter-intuitive in-plane isotropic behavior is predicted. We confront the effective model formulation with exact reference calculations such as ab-initio calculations for graphene, hexagonal boron nitride (hBN), as well as corrugated graphene with larger thickness but also with classical electrodynamics calculations that exactly account for the lateral structuration.

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.

Bidimensional materials are ideally viewed as having no thickness, as their name suggests. Their optical response have been previously modelled by a purely bidimensional surface current or by a very thin film with some contradictory results. The advent of multilayer stacks of bidimensional materials and combinations of different materials in vertical van der Waals heterostructures highlights however that these materials have a finite thickness. In this article, we propose a new model that reconciles both approaches and we show how volume properties of stacked bidimensional layers can be calculated from the bidimensional response of each individual layer, and conversely. In our approach, each bidimensionnal layers is surrounded by vacuum and described as a kind of transfer matrix with intrinsic parameters that do not depend on the external medium. This provides a link between continuous thin films and discrete layers. We show how to model heterostructures of bidimensional materials and identify the parameters of the current sheet that represents the bidimensional material in the zero-thickness limit, namely the in-plane surface susceptibility and the out-of-plane displacement susceptibility. We show that our unified model is perfectly compatible with existing ellipsometric data with the same reliability as the existing interface model but with different values of the surface susceptibility or bulk dielectric function. We discuss in details the origin of the discrepancies and show that our approach allows to determine intrinsic properties of the bidimensional materials with the advantage that multilayer and monolayer systems are described in a same framework.

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.

Using an enhanced optically heterodyned optical Kerr effect method and a theoretical description of the interactions between an optical beam, a single layer of graphene, and its substrate, we provide experimental answers to questions raised by theoretical models of graphene third-order nonlinear optical response. In particular, we measure separately the time response of the two main tensor components of the nonlinear susceptibility, we validate the assumption that the out-of plane tensor components are small, and we quantify the optical impact of the substrate on the measured coefficients. Our method can be applied to other 2D materials, as it relies mainly on the small ratio between the thickness and the wavelength.

Two-dimensional (2D) materials are intrinsically anisotropic, and an accurate description of their out-of-plane response to an electromagnetic field is more and more important as new materials with diverse properties are proposed. Their electromagnetic properties are often modeled using a single sheet with a surface susceptibility or conductivity or by means of a thin film of finite thickness with an effective bulk permittivity. The discordances between these two approaches lead to two irreconcilable interpretations of the optical characterizations and uncertain predictions of electromagnetic responses. Here, we fully account for the particular anisotropy of 2D materials and reconcile both approaches. We propose a unified description for the electromagnetic properties that applies to 2D heterostructures for all polarizations and at all angles of incidence. In particular, we determine the class of materials for which both models can be used indifferently and when particular care should be taken to select the thickness and the tensorial response of the effective thin film. We illustrate our conclusions on extensively studied experimental quantities such as transmittance and ellipsometric data of graphene and metal dichalcogenides. We discuss similarities and discrepancies reported in the literature when single-sheet or thin-film models are used.

A uniform lying helix (ULH) alignment of cholesteric liquid crystals (LCs) is obtained using a solvent evaporation technique. The solvent evaporation method allows for the spontaneous formation of a virtually defect-free alignment, even in the absence of an external electric field. A small amount of solvent diffuses into the LC and changes its phase into isotropic state where the individual LC molecules are more mobile. As the solvent diffuses out of the LC and consequently evaporates, additional mobility provided by the solvent allows the molecules to reach the lowest energy configuration, dictated by the boundary conditions, the solvent evaporation direction and the elastic forces among the molecules. Compared to a shear-flow-induced alignment, the solvent-induced ULH exhibits a contrast ratio between the bright and dark states that is a factor of 4 times larger, due to the low number of defects in the structure. From measurements of the flexoelectro-optic effect, the difference between the splay and bend flexoelectric coefficients, , for the nematic LC E7 is found to be in agreement with the measured values reported in the literature (12.11.0 pC/m), demonstrating that the solvent self-aligning does not change the electric response of the medium, while improving its optical properties. [GRAPHICS] .

We present modeling of the spatial instabilities in nematicon propagation where the long range interaction in liquid crystals is taken into account with a correlated noise. The experimental measurements support the numerical results.

Starting from the de Gennes theory of director fluctuations in nematics, we report on a model of the spatial fluctuations in nematicon propagation. We demonstrate that, when the long-range correlation that characterizes nematic liquid crystals is taken into account in the thermal noise, it is possible to account for the spatial oscillations and propagation losses experienced by nematicons. Increasing the power of the nematicon, the oscillation amplitudes increase and the propagation losses decrease. The nematicon is then more strongly confined and deviates more, but is less scattered by the thermally induced perturbations of the refractive index. All the results are in good agreement with the experimental observations.

Using an enhanced optically heterodyned optical Kerr effect method and a theoretical description of the interactions between an optical beam, a single layer of graphene, and its substrate, we provide experimental answers to questions raised by theoretical models of graphene third-order nonlinear optical response. In particular, we measure separately the time response of the two main tensor components of the nonlinear susceptibility, we validate the assumption that the out-of-plane tensor components are small, and we quantify the optical impact of the substrate on the measured coefficients. Our method can be applied to other two-dimensional materials, as it relies mainly on the small ratio between the thickness and the wavelength.

Graphene, with its high and broadband optical nonlinearity, has attracted the interest of many researchers the last few years, as it appears to be a promising candidate for integrated photonics. In our work, we report the use of the ultrafast optical Kerr effect method with optical heterodyne detection (OHD-OKE) for the characterization of the third order optical nonlinearity of monolayer CVD graphene on quartz, at telecom wavelength. Our measurements show that the nonlinear refractive index of graphene is negative, in contrast to previously reported results. We also performed measurements of the nonlinear absorption of graphene and we studied the temperature dependence of the nonlinearity, as well as the relaxation time of the OHD-OKE signal.