In the last three decades, we have witnessed incredible advances in laser technology and in the understanding of nonlinear laser-matter interactions, crowned recently by the award of the Nobel prize to Gérard Mourou and Donna Strickland [1,2]. It is now routinely possible to produce few-cycle femtosecond (1 fs = 10 −15 s) laser pulses in the visible and mid-infrared regimes [3,4]. By focusing such ultrashort laser pulses on gas or solid targets, possibly in a presence of nano-structures [5], the targets are subjected to an ultra-intense electric field, with peak field strengths approaching the binding field inside the atoms themselves. Such fields permit the exploration of the interaction between strong electromagnetic coherent radiation and an atomic or molecular system with unprecedented spatial and temporal resolution [6]. On one hand, HHG nowadays can be used to generate attosecond pulses in the extreme ultraviolet [7,8], or even in the soft X-ray regime [9]. Such pulses themselves may be used for dynamical spectroscopy of matter; despite carrying modest pulse energies, they exhibit excellent coherence properties [10,11]. Combined with femtosecond pulses they can also be used to extract information about the laser pulse electric field itself [12]. HHG sources therefore offer an important alternative to other sources of XUV and X-ray radiation: synchrotrons, free electron lasers, X-ray lasers, and laser plasma sources. Moreover, HHG pulses can provide information about the structure of the target atom, molecule or solid [13][14][15]. Of course, to decode such information from a highly nonlinear HHG signal is a challenge, and that is why a possibly perfect, and possibly "as analytical as possible" theoretical understanding of these processes is in high demand. Here is the first instance where SFA offers its basic services.Since electronic motion is governed by the waveform of the laser electric field, an important quantity to describe the electric field shape is the so-called absolute phase or carrier-envelope phase (CEP). Control over the CEP is paramount for extracting information about electron dynamics, and to retrieve structural information from atoms and molecules [13,16,17]. For instance, in HHG an electron is liberated from an atom or molecule through ionization, which occurs close to the maximum of the electric field. Within the oscillating field, the electron can thus accelerate along oscillating trajectories, which may result in recollision with the parent ion, roughly when the laser field approaches a zero value. Control over the CEP is particularly important for HHG, when targets are driven by laser pulses comprising only one or two optical cycles. In that situation the CEP determines the relevant electron trajectories, i.e. the CEP determines whether emission results in a single or in multiple attosecond bursts of radiation [16,18].The influence of the CEP on electron emission is also extremely important. It was demonstrated for instance in an anti-correlation experiment, in which the number of AT...

Emission of high-order harmonics from solids provides a new avenue in attosecond science. On the one hand, it allows us to investigate fundamental processes of the nonlinear response of electrons driven by a strong laser pulse in a periodic crystal lattice. On the other hand, it opens new paths toward efficient attosecond pulse generation, novel imaging of electronic wave functions, and enhancement of high-order harmonic-generation (HHG) intensity. A key feature of HHG in a solid (as compared to the well-understood phenomenon of HHG in an atomic gas) is the delocalization of the process, whereby an electron ionized from one site in the periodic lattice may recombine in any other. Here, we develop an analytic model, based on the localized Wannier wave functions in the valence band and delocalized Bloch functions in the conduction band. This Wannier-Bloch approach assesses the contributions of individual lattice sites to the HHG process and hence precisely addresses the question of localization of harmonic emission in solids. We apply this model to investigate HHG in a ZnO crystal for two different orientations, corresponding to wider and narrower valence and conduction bands, respectively. Interestingly, for narrower bands, the HHG process shows significant localization, similar to harmonic generation in atoms. For all cases, the delocalized contributions to HHG emission are highest near the band-gap energy. Our results pave the way to controlling localized contributions to HHG in a solid crystal

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Nonlinear susceptibilities are key to ultrafast lightwave driven optoelectronics, allowing petahertz scaling manipulation of the signal. Recent experiments retrieved a 3rd order nonlinear susceptibility by comparing the nonlinear response induced by a strong laser field to a linear response induced by the otherwise identical weak field. The highly nonlinear nature of high harmonic generation (HHG) has the potential to extract even higher order nonlinear susceptibility terms. However, up till now, such characterization has been elusive due to a lack of direct correspondence between high harmonics and nonlinear susceptibilities. Here, we demonstrate a regime where such correspondence can be clearly made, extracting nonlinear susceptibilities (7th, 9th, and 11th) from sapphire of the same order as the measured high harmonics. The extracted high order susceptibilities show angular-resolved periodicities arising from variation in the band structure with crystal orientation. Our results open a door to multi-channel signal processing, controlled by laser polarization.