Extreme ultraviolet (EUV) high-harmonic radiation emerging from laser-driven atoms, molecules or plasmas underlies powerful attosecond spectroscopy techniques and provides insight into fundamental structural and dynamic properties of matter. The advancement of these spectroscopy techniques to study strong-field electron dynamics in condensed matter calls for the generation and manipulation of EUV radiation in bulk solids, but this capability has remained beyond the reach of optical sciences. Recent experiments and theoretical predictions paved the way to strong-field physics in solids by demonstrating the generation and optical control of deep ultraviolet radiation in bulk semiconductors, driven by femtosecond mid-infrared fields or the coherent up-conversion of terahertz fields to multi-octave spectra in the mid-infrared and optical frequencies. Here we demonstrate that thin films of SiO2 exposed to intense, few-cycle to sub-cycle pulses give rise to wideband coherent EUV radiation extending in energy to about 40 electronvolts. Our study indicates the association of the emitted EUV radiation with intraband currents of multi-petahertz frequency, induced in the lowest conduction band of SiO2. To demonstrate the applicability of high-harmonic spectroscopy to solids, we exploit the EUV spectra to gain access to fine details of the energy dispersion profile of the conduction band that are as yet inaccessible by photoemission spectroscopy in wide-bandgap dielectrics. In addition, we use the EUV spectra to trace the attosecond control of the intraband electron motion induced by synthesized optical transients. Our work advances lightwave electronics in condensed matter into the realm of multi-petahertz frequencies and their attosecond control, and marks the advent of solid-state EUV photonics.

Extreme ultraviolet high-harmonic spectroscopy of solids

When intense light interacts with an atomic gas, recollision between an ionizing electron and its parent ion creates high-order harmonics of the fundamental laser frequency. This sub-cycle effect generates coherent soft X-rays and attosecond pulses, and provides a means to image molecular orbitals. Recently, high harmonics have been generated from bulk crystals, but what mechanism dominates the emission remains uncertain. To resolve this issue, we adapt measurement methods from gas-phase research to solid zinc oxide driven by mid-infrared laser fields of 0.25 volts per angstrom. We find that when we alter the generation process with a second-harmonic beam, the modified harmonic spectrum bears the signature of a generalized recollision between an electron and its associated hole. In addition, we find that solid-state high harmonics are perturbed by fields so weak that they are present in conventional electronic circuits, thus opening a route to integrate electronics with attosecond and high-harmonic technology. Future experiments will permit the band structure of a solid to be tomographically reconstructed.

/pdf/linking-high-harmonics-from-gases-and-solids-4rtfjbqvr5.pdf

Linking high harmonics from gases and solids

Observations of high-harmonic generation from a single layer of a transition metal dichalcogenide opens the door to studying strong-field and attosecond phenomena in two-dimensional materials. High-harmonic generation (HHG) in bulk solids permits the exploration of materials in a new regime of strong fields and attosecond timescales1,2,3,4,5,6. The generation process has been discussed in the context of strongly driven electron dynamics in single-particle bands7,8,9,10,11,12,13,14. Two-dimensional materials exhibit distinctive electronic properties compared to the bulk that could significantly modify the HHG process15,16, including different symmetries17,18,19, access to individual valleys20,21 and enhanced many-body interactions22,23,24,25. Here we demonstrate non-perturbative HHG from a monolayer MoS2 crystal, with even and odd harmonics extending to the 13th order. The even orders are predominantly polarized perpendicular to the pump and are compatible with the anomalous transverse intraband current arising from the material’s Berry curvature, while the weak parallel component suggests the importance of interband transitions. The odd harmonics exhibit a significant enhancement in efficiency per layer compared to the bulk, which is attributed to correlation effects. The combination of strong many-body Coulomb interactions and widely tunable electronic properties in two-dimensional materials offers a new platform for attosecond physics.

High-harmonic generation from an atomically thin semiconductor

Acceleration and collision of particles has been a key strategy for exploring the texture of matter. Strong light waves can control and recollide electronic wavepackets, generating high-harmonic radiation that encodes the structure and dynamics of atoms and molecules and lays the foundations of attosecond science. The recent discovery of high-harmonic generation in bulk solids combines the idea of ultrafast acceleration with complex condensed matter systems, and provides hope for compact solid-state attosecond sources and electronics at optical frequencies. Yet the underlying quantum motion has not so far been observable in real time. Here we study high-harmonic generation in a bulk solid directly in the time domain, and reveal a new kind of strong-field excitation in the crystal. Unlike established atomic sources, our solid emits high-harmonic radiation as a sequence of subcycle bursts that coincide temporally with the field crests of one polarity of the driving terahertz waveform. We show that these features are characteristic of a non-perturbative quantum interference process that involves electrons from multiple valence bands. These results identify key mechanisms for future solid-state attosecond sources and next-generation light-wave electronics. The new quantum interference process justifies the hope for all-optical band-structure reconstruction and lays the foundation for possible quantum logic operations at optical clock rates.

Real-time observation of interfering crystal electrons in high-harmonic generation

High-harmonic generation in atomic gases has been studied for decades, and has formed the basis of attosecond science. Observation of high-order harmonics from bulk crystals was, however, reported much more recently, in 2010. This Review surveys the subsequent efforts aimed at understanding the microscopic mechanism of solid-state harmonics in terms of what it can tell us about the electronic structure of the source materials, how it can be used to probe driven ultrafast dynamics and its prospects for novel, compact short-wavelength light sources. Although most of this work has focused on bulk materials as the source, recent experiments have investigated high-harmonic generation from engineered structures, which could form flexible platforms for attosecond photonics. This Review surveys recent efforts at understanding and characterizing generation of high harmonics from solid-state materials.

High-harmonic generation from solids

We investigate theoretically high-harmonic generation (HHG) in bulk crystals exposed to intense midinfrared lasers with photon energies smaller than the band gap. The two main mechanisms, interband and intraband HHG, are explored. Our analysis indicates that the interband current neglected so far is the dominant mechanism for HHG. Saddle point analysis in the Keldysh limit yields an intuitive picture of interband HHG in solids similar to atomic HHG. Interband and intraband HHG exhibit a fundamentally different wavelength dependence. This signature can be used to experimentally distinguish between the two mechanisms in order to verify their importance.

Theoretical Analysis of High-Harmonic Generation in Solids

High harmonic generation (HHG) in solids is investigated. We find that interband emission is dominant for the midinfrared laser driver frequencies, whereas intraband emission dominates the far-infrared range. Interband HHG is similar to atomic HHG and therewith opens the possibility to apply atomic attosecond technology to the condensed matter phase. Interband emission is investigated with a quasiclassical method, by which HHG can be modeled based on the classical trajectory analysis of electron-hole pairs. This analysis yields a simple approximate cutoff law for HHG in solids. Differences between HHG in atoms and solids are identified that are important for adapting atomic attosecond technology to make it applicable to condensed matter.

/pdf/semiclassical-analysis-of-high-harmonic-generation-in-bulk-14r9lvwooa.pdf

Semiclassical analysis of high harmonic generation in bulk crystals

In a seminal paper, Keldysh published a theory of ionization of atoms and solids in intense sinusoidally varying laser fields. In this paper the Keldysh parameter was introduced, which separates optical field ionization into tunnel ionization and multi-photon ionization for and , respectively. Keldysh showed that the Keldysh parameter can be written as a product of laser frequency ω and of the Keldysh tunnel time , i.e. . Over the past 50 years there has been much debate about the meaning and the significance of the Keldysh tunnel time and of the tunnel time in general. This debate has been rekindled by recent attosecond experiment measurements of the tunnel time that are in contradiction with the Keldysh tunnel time and with other definitions of the tunnel time. This paper focuses on an analytical and numerical investigation of the Keldysh tunnel time. It is proven that the tunnel time in atoms represents a response time needed for the groundstate wavefunction to react to the laser field and to develop into the quasi-static resonance state, where full tunnel ionization occurs. Based on this definition, methods to measure the tunnel time of atoms in intense fields are discussed.

http://iopscience.iop.org/article/10.1088/0953-4075/47/20/204002/pdf

Tunnelling time, what does it mean?

By using first-principles arguments, based on the time-energy uncertainty principle in the form given by Mandelstam and Tamm, we show that the Keldysh time represents a lower limit for the tunnel time. We use the definition of the tunnel time as identified in a recent numerical investigation [C. R. McDonald et al., Phys. Rev. Lett. 111, 090405 (2013)]; it is the time it takes for the unperturbed initial ground-state wave function to evolve into the field-perturbed final eigenstate which is the quasistatic field dressed resonance.

Identification of the Keldysh time as a lower limit for the tunneling time

High-harmonic generation (HHG) in bulk crystals exposed to intense mid-infrared lasers with photon energies below the bandgap is investigated theoretically. A three dimensional, two-band model that considers both interband and intraband currents is used. It is shown that the interband current is the dominant mechanism for HHG in solids. A physical interpretation of interband HHG – similar to atomic HHG – is provided by saddle point analysis. The effects of dephasing time and driving field wavelength on the harmonic specrum are investigated.

https://iopscience.iop.org/article/10.1088/1742-6596/594/1/012021/pdf

Theory of high-harmonic generation in solids

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