Terahertz electron-hole recollisions in GaAs/AlGaAs quantum wells: robustness to scattering by optical phonons and thermal fluctuations

Electron-hole recollisions are induced by resonantly injecting excitons with a near-IR laser at frequency $f_{\text{NIR}}$ into quantum wells driven by a ~10 kV/cm field oscillating at $f_{\text{THz}} = 0.57$ THz. At $T=12$ K, up to 18 sidebands are observed at frequencies $f_{\text{sideband}}=f_{\text{NIR}}+2n f_{\text{THz}}$, with $-8 \le 2n \le 28$. Electrons and holes recollide with total kinetic energies up to 57 meV, well above the $E_{\text{LO}} = 36$ meV threshold for longitudinal optical (LO) phonon emission. Sidebands with order up to $2n=22$ persist up to room temperature. A simple model shows that LO phonon scattering suppresses but does not eliminate sidebands associated with kinetic energies above $E_{\text{LO}}$.Comment: 5 pages, 4 figure

Optical frequency combs from high-order sideband generation

We report on the generation of frequency combs from the recently-discovered phenomenon of high-order sideband generation (HSG). A near-band gap continuous-wave (cw) laser with frequency $f_\text{NIR}$ was transmitted through an epitaxial layer containing GaAs/AlGaAs quantum wells that were driven by quasi-cw in-plane electric fields $F_\text{THz}$ between 4 and 50 kV/cm oscillating at frequencies $f_\text{THz}$ between 240 and 640 GHz. Frequency combs with teeth at $f_\text{sideband}=f_\text{NIR}+nf_\text{THz}$ ($n$ even) were produced, with maximum reported $n>120$, corresponding to a maximum comb span $>80$ THz. Comb spectra with the identical product $f_\text{THz}\times F_\text{THz}$ were found to have similar spans and shapes in most cases, as expected from the picture of HSG as a scattering-limited electron-hole recollision phenomenon. The HSG combs were used to measure the frequency and linewidth of our THz source as a demonstration of potential applications

Dynamical birefringence: Electron-hole recollisions as probes of Berry curvature

The direct measurement of Berry phases is still a great challenge in condensed matter systems. The bottleneck has been the ability to adiabatically drive an electron coherently across a large portion of the Brillouin zone in a solid where the scattering is strong and complicated. We break through this bottleneck and show that high-order sideband generation (HSG) in semiconductors is intimately affected by Berry phases. Electron-hole recollisions and HSG occur when a near-band gap laser beam excites a semiconductor that is driven by sufficiently strong terahertz (THz)-frequency electric fields. We carried out experimental and theoretical studies of HSG from three GaAs/AlGaAs quantum wells. The observed HSG spectra contain sidebands up to the 90th order, to our knowledge the highest-order optical nonlinearity observed in solids. The highest-order sidebands are associated with electron-hole pairs driven coherently across roughly 10% of the Brillouin zone around the \Gamma point. The principal experimental claim is a dynamical birefringence: the sidebands, when the order is high enough (> 20), are usually stronger when the exciting near-infrared (NIR) and the THz electric fields are polarized perpendicular than parallel; the sideband intensities depend on the angles between the THz field and the crystal axes in samples with sufficiently weak quenched disorder; and the sidebands exhibit significant ellipticity that increases with increasing sideband order, despite nearly linear excitation and driving fields. We explain dynamical birefringence by generalizing the three-step model for high order harmonic generation. The hole accumulates Berry phases due to variation of its internal state as the quasi-momentum changes under the THz field. Dynamical birefringence arises from quantum interference between time-reversed pairs of electron-hole recollision pathways

Imperfect Recollisions in High-Harmonic Generation in Solids

We theoretically investigate high-harmonic generation in hexagonal boron nitride with linearly polarized laser pulses. We show that imperfect recollisions between electron-hole pairs in the crystal give rise to an electron-hole-pair polarization energy that leads to a double-peak structure in the subcycle emission profiles. An extended recollision model (ERM) is developed that allows for such imperfect recollisions, as well as effects related to Berry connections, Berry curvatures, and transition-dipole phases. The ERM illuminates the distinct spectrotemporal characteristics of harmonics emitted parallel and perpendicularly to the laser polarization direction. Imperfect recollisions are a general phenomenon and a manifestation of the spatially delocalized nature of the real-space wave packet, they arise naturally in systems with large Berry curvatures, or in any system driven by elliptically polarized light

Expanded view of electron-hole recollisions in solid-state high-order harmonic generation: Full-Brillouin-zone tunneling and imperfect recollisions

We theoretically investigate electron-hole recollisions in high-harmonic generation (HHG) in band-gap solids irradiated by linearly and elliptically polarized drivers. We find that in many cases the emitted harmonics do not originate in electron-hole pairs created at the minimum band gap, where the tunneling probability is maximized, but rather in pairs created across an extended region of the Brillouin zone (BZ). In these situations, the analogy to gas-phase HHG in terms of the short- and long-trajectory categorizations is inadequate. Our analysis methodology comprises three complementary levels of theory: the numerical solutions to the semiconductor Bloch equations, an extended semiclassical recollision model, and a quantum wave packet approach. We apply this methodology to two general material types with representative band structures: a bulk system and a hexagonal monolayer system. In the bulk, the interband harmonics generated using elliptically-polarized drivers are found to originate not from tunneling at the minimum band gap $\Gamma$, but from regions away from it. In the monolayer system driven by linearly-polarized pulses, tunneling regions near different symmetry points in the BZ lead to distinct harmonic energies and emission profiles. We show that the imperfect recollisions, where an electron-hole pair recollide while being spatially separated, are important in both bulk and monolayer materials. The excellent agreement between our three levels of theory highlights and characterizes the complexity behind the HHG emission dynamics in solids, and expands on the notion of interband HHG as always originating in trajectories tunnelled at the minimum band gap. Our work furthers the fundamental understanding of HHG in periodic systems and will benefit the future design of experiments.Comment: 18 pages, 13 figure

Direct evidences for inner-shell electron-excitation by laser induced electron recollision

Extreme ultraviolet (XUV) attosecond pulses, generated by a process known as laser-induced electron recollision, are a key ingredient for attosecond metrology, providing a tool to precisely initiate and probe sub-femtosecond dynamics in the microcosms of atoms, molecules and solids[1]. However, with the current technology, extending attosecond metrology to scrutinize the dynamics of the inner-shell electrons is a challenge, that is because of the lower efficiency in generating the required soft x-ray \hbar\omega>300 eV attosecond bursts and the lower absorption cross-sections in this spectral range. A way around this problem is to use the recolliding electron to directly initiate the desired inner-shell process, instead of using the currently low flux x-ray attosecond sources.Such an excitation process occurs in a sub-femtosecond timescale, and may provide the necessary "pump" step in a pump-probe experiment[2]. Here we used a few cycle infrared \lambda_{0}~1800nm source[3] and observed direct evidences for inner-shell excitations through the laser-induced electron recollision process. It is the first step toward time-resolved core-hole studies in the keV energy range with sub-femtosecond time resolution.Comment: 6 pages, 4 figure

Dynamics of multiply charged ions in intense laser fields

We numerically investigate the dynamics of multiply charged hydrogenic ions in near-optical linearly polarized laser fields with intensities of order 10^16 to 10^17 W/cm^2. Depending on the charge state Z of the ion the relation of strength between laser field and ionic core changes. We find around Z=12 typical multiphoton dynamics and for Z=3 tunneling behaviour, however with clear relativistic signatures. In first order in v/c the magnetic field component of the laser field induces a Z-dependent drift in the laser propagation direction and a substantial Z-dependent angular momentum with repect to the ionic core. While spin oscillations occur already in first order in v/c as described by the Pauli equation, spin induced forces via spin orbit coupling only appear in the parameter regime where (v/c)^2 corrections are significant. In this regime for Z=12 ions we show strong splittings of resonant spectral lines due to spin-orbit coupling and substantial corrections to the conventional Stark shift due to the relativistic mass shift while those to the Darwin term are shown to be small. For smaller charges or higher laser intensities, parts of the electronic wavepacket may tunnel through the potential barrier of the ionic core, and when recombining are shown to give rise to keV harmonics in the radiation spectrum. Some parts of the wavepacket do not recombine after ionisation and we find very energetic electrons in the weakly relativistic regime of above threshold ionization.Comment: submitte

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

Accelerating and colliding particles has been a key strategy to explore the texture of matter. Strong lightwaves can control and recollide electronic wavepackets, generating high-harmonic (HH) radiation which encodes the structure and dynamics of atoms and molecules and lays the foundations of attosecond science. The recent discovery of HH generation in bulk solids combines the idea of ultrafast acceleration with complex condensed matter systems and sparks hope for compact solid-state attosecond sources and electronics at optical frequencies. Yet the underlying quantum motion has not been observable in real time. Here, we study HH generation in a bulk solid directly in the time-domain, revealing a new quality of strong-field excitations in the crystal. Unlike established atomic sources, our solid emits HH radiation as a sequence of subcycle bursts which coincide temporally with the field crests of one polarity of the driving terahertz waveform. We show that these features hallmark a novel non-perturbative quantum interference involving electrons from multiple valence bands. The results identify key mechanisms for future solid-state attosecond sources and next-generation lightwave electronics. The new quantum interference justifies the hope for all-optical bandstructure reconstruction and lays the foundation for possible quantum logic operations at optical clock rates