Mapping light-dressed Floquet bands by highly nonlinear optical excitations and valley polarization

Ultrafast nonlinear optical phenomena in solids have been attracting major interest as novel methodologies for femtosecond spectroscopy of electron dynamics and control of material properties. Here, we theoretically investigate strong-field nonlinear optical transitions in a prototypical two-dimensional material, hBN, and show that the k-resolved conduction band charge occupation patterns induced by an elliptically-polarized laser can be understood in a multi-photon resonant picture; but remarkably, only if using the Floquet light-dressed states instead of the undressed matter states. Consequently, our work establishes a direct measurable signature for band-dressing in nonlinear optical processes in solids, and opens new paths for ultrafast spectroscopy and valley manipulation

Band nonlinearity-enabled manipulation of Dirac nodes, Weyl cones, and valleytronics with intense linearly polarized light

We study monochromatic linearly-polarized laser-induced band structure modifications in material systems with valley (graphene and hexagonal-Boron-Nitride), and topological (Dirac and Weyl semimetals), properties. We find that for Dirac-like linearly-dispersing bands, the laser dressing effectively moves the Dirac nodes away from their original position by up to ~10% of the Brillouin zone (opening a large pseudo-gap in their original position). The direction of the movement can be fully controlled by rotating the laser polarization axis. We prove that this effect originates from band nonlinearities away from the Dirac nodes (without which the effect completely vanishes, and which are often neglected). We demonstrate that this physical mechanism is applicable beyond two-dimensional Dirac semimetals, and can move the positions of the valley minima in hexagonal materials to tune valley selectivity, split and move Weyl cones in higher-order Weyl semimetals, and merge Dirac nodes in three-dimensional topological Dirac semimetals. The model results are validated with ab-initio time-dependent density functional theory calculations. Our results directly affect theoretical and experimental efforts for exploring light-dressed electronic-structure, suggesting that one can benefit from band nonlinearity for tailoring material properties. They also highlight the importance of describing the full band structure in nonlinear optical phenomena in solids

New photonic conservation laws in parametric nonlinear optics

Conservation laws are one of the most generic and useful concepts in physics. In nonlinear optical parametric processes, conservation of photonic energy, momenta and parity often lead to selection rules, restricting the allowed polarization and frequencies of the emitted radiation. Here we present a new scheme to derive conservation laws in optical parametric processes in which many photons are annihilated and a single new photon is emitted. We then utilize it to derive two new such conservation laws. Conservation of reflection-parity (RP) arises from a generalized reflection symmetry of the polarization in a superspace, analogous to the superspace employed in the study of quasicrystals. Conservation of space-time-parity (STP) similarly arises from space-time reversal symmetry in superspace. We explore these new conservation laws numerically in the context of high harmonic generation and outline experimental set-ups where they can be tested

Attosecond magnetization dynamics in non-magnetic materials driven by intense femtosecond lasers

Irradiating solids with ultrashort laser pulses is known to initiate femtosecond timescale magnetization dynamics. However, sub-femtosecond spin dynamics have not yet been observed or predicted. Here, we explore ultrafast light-driven spin dynamics in a highly non-resonant strong-field regime. Through state-of-the-art ab-initio calculations, we predict that a non-magnetic material can be transiently transformed into a magnetic one via dynamical extremely nonlinear spin-flipping processes, which occur on attosecond timescales and are mediated by a combination of multi-photon and spin-orbit interactions. These are non-perturbative non-resonant analogues to the inverse Faraday effect that build up from cycle-to-cycle as electrons gain angular momentum. Remarkably, we show that even for linearly polarized driving, where one does not intuitively expect any magnetic response, the magnetization transiently oscillates as the system interacts with light. This oscillating response is enabled by transverse anomalous light-driven currents in the solid, and typically occurs on timescales of ~500 attoseconds. We further demonstrate that the speed of magnetization can be controlled by tuning the laser wavelength and intensity. An experimental set-up capable of measuring these dynamics through pump-probe transient absorption spectroscopy is outlined and simulated. Our results pave the way for new regimes of ultrafast manipulation of magnetism.Comment: 21 pages, 14 figure

Are There Universal Signatures of Topological Phases in High-Harmonic Generation? Probably Not

High harmonic generation (HHG) has developed in recent years as a promising tool for ultrafast materials spectroscopy. At the forefront of these advancements, several works proposed using HHG as an all-optical probe for topology of quantum matter by identifying its signatures in the emission spectra. However, it remains unclear if such spectral signatures are indeed a robust and general approach for probing topology. To address this point, we perform a fully ab initio study of HHG from prototypical two-dimensional topological insulators in the Kane-Mele quantum spin-Hall and anomalous-Hall phases. We analyze the spectra and previously proposed topological signatures by comparing HHG from the topological and trivial phases and across the phase transition. We demonstrate and provide detailed microscopic explanations of why, in these systems, none of the observables proposed thus far uniquely and universally probes material topology. Specifically, we find that the (i) HHG helicity, (ii) anomalous HHG ellipticity, (iii) HHG elliptical dichroism, and (iv) temporal delays in HHG emission are all unreliable signatures of topological phases. Our results suggest that extreme care must be taken when interpreting HHG spectra for topological signatures and that contributions from the crystal symmetries and chemical nature might be dominant over those from topology. They hint that a truly universal topological signature in nonlinear optics is unlikely and raise important questions regarding possible utilization and detection of topology in out-of-equilibrium systems