High-harmonic generation in isolated atoms and molecules has been widely utilized in extreme ultraviolet photonics and attosecond pulse metrology. Recently, high-harmonic generation has been observed in solids, which could lead to important applications such as all-optical methods to image valance charge density and reconstruct electronic band structures, as well as compact extreme ultraviolet light sources. So far these studies are confined to crystalline solids; therefore, decoupling the respective roles of long-range periodicity and high density has been challenging. Here we report the observation of high-harmonic generation from amorphous fused silica. We decouple the role of long-range periodicity by comparing harmonics generated from fused silica and crystalline quartz, which contain the same atomic constituents but differ in long-range periodicity. Our results advance current understanding of the strong-field processes leading to high-harmonic generation in solids with implications for the development of robust and compact extreme ultraviolet light sources.

Solid-state high-harmonic sources offer the possibility of compact, high-repetition-rate attosecond light emitters. However, the time structure of high harmonics must be characterized at the sub-cycle level. We use strong two-cycle laser pulses to directly control the time-dependent nonlinear current in single-crystal MgO, leading to the generation of extreme ultraviolet harmonics. We find that harmonics are delayed with respect to each other, yielding an atto-chirp, the value of which depends on the laser field strength. Our results provide the foundation for attosecond pulse metrology based on solid-state harmonics and a new approach to studying sub-cycle dynamics in solids.

We generate high-order harmonics in a-cut (11–20) ZnO at a high repetition rate of 50 kHz, using the tunable mid-infrared pulses (3–4 μm wavelength) from a high-power optical parametric amplifier. For driving laser pulses with 3.8 μm central wavelength, we observe nonperturbative harmonic spectra that well exceed the material band gap. The harmonic spectra depend strongly on the orientation of the crystal with respect to the laser polarization, with odd harmonics exhibiting periodicities of π/2 for a polarization within the (11–20) crystal plane. Energy conversion efficiencies of ∼10−6 per harmonic are measured for the 9th–13th harmonics, yielding an average power of more than 0.2 μW for the 13th harmonic.

We carried out a joint theoretical and experimental study of the polarization of high-order harmonics generated from ZnO by intense infrared laser pulses. Experimentally we found that the dependence of parallel and perpendicular polarizations on the crystal orientation for all odd harmonics are nearly identical, but they are quite different from even harmonics which also show little order dependence. A one-dimensional two-band model, combined with a linear coupled excitation model, is shown to be able to explain the observed polarization behavior, including low-order harmonics. We further note that the same odd/even order contrast have been reported in a number of other crystals, despite that the harmonics were perceived to be generated via entirely different mechanisms. We demonstrated that this universality is governed by crystal symmetry, not by specific mechanisms. Thus, polarization measurements of harmonics offers a powerful pure optical method for determining the crystal axes as well as monitoring their ultrafast changes when crystals are undergoing deformation. In addition, the ellipticity of harmonic has been studied. It shows that ellipticity of high-order harmonics from solids can be tuned precisely by changing the bond structure of the sample.

We investigate the potential of a multi-plate medium consisting of thin fused silica plates to generate few-cycle pulses from a moderately high energy (400 μJ) and average power (20 W) Yb:KGW laser centered at 1025 nm. By optimizing the thicknesses and positions of the plates, we mitigate the losses associated with spatial and spectral distortions that can accompany self-focusing in bulk solids. Pulses with an initial duration of ∼280 fs were compressed using chirped mirrors, after spectral broadening in a multi-plate medium consisting of 6 mm of fused silica in total, by a factor of >5 to 50 fs. Further spectral broadening in a second stage also consisting of 6 mm of fused silica in total enabled compression to 18 fs with 40 μJ pulse energy, with the energy efficiency limited primarily by the geometry of the chirped mirror compressors.