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.
Phase-locked ultrashort pulses in the rich terahertz spectral range have provided key insights into phenomena as diverse as quantum confinement, first-order phase transitions, high-temperature ...superconductivity and carrier transport in nanomaterials. Ultrabroadband electro-optic sampling of few-cycle field transients can even reveal novel dynamics that occur faster than a single oscillation cycle of light. However, conventional terahertz spectroscopy is intrinsically restricted to ensemble measurements by the diffraction limit. As a result, it measures dielectric functions averaged over the size, structure, orientation and density of nanoparticles, nanocrystals or nanodomains. Here, we extend ultrabroadband time-resolved terahertz spectroscopy to the sub-nanoparticle scale (10 nm) by combining sub-cycle, field-resolved detection (10 fs) with scattering-type near-field scanning optical microscopy (s-NSOM). We trace the time-dependent dielectric function at the surface of a single photoexcited InAs nanowire in all three spatial dimensions and reveal the ultrafast (<50 fs) formation of a local carrier depletion layer.
Atomically thin two-dimensional crystals have revolutionized materials science. In particular, monolayer transition metal dichalcogenides promise novel optoelectronic applications, owing to their ...direct energy gaps in the optical range. Their electronic and optical properties are dominated by Coulomb-bound electron-hole pairs called excitons, whose unusual internal structure, symmetry, many-body effects and dynamics have been vividly discussed. Here we report the first direct experimental access to all 1s A excitons, regardless of momentum--inside and outside the radiative cone--in single-layer WSe2. Phase-locked mid-infrared pulses reveal the internal orbital 1s-2p resonance, which is highly sensitive to the shape of the excitonic envelope functions and provides accurate transition energies, oscillator strengths, densities and linewidths. Remarkably, the observed decay dynamics indicates an ultrafast radiative annihilation of small-momentum excitons within 150 fs, whereas Auger recombination prevails for optically dark states. The results provide a comprehensive view of excitons and introduce a new degree of freedom for quantum control, optoelectronics and valleytronics of dichalcogenide monolayers.
Ultrafast charge transport in strongly biased semiconductors is at the heart of high-speed electronics, electro-optics and fundamental solid-state physics. Intense light pulses in the terahertz ...spectral range have opened fascinating vistas. Because terahertz photon energies are far below typical electronic interband resonances, a stable electromagnetic waveform may serve as a precisely adjustable bias. Novel quantum phenomena have been anticipated for terahertz amplitudes, reaching atomic field strengths. We exploit controlled (multi-)terahertz waveforms with peak fields of 72 MV cm-1 to drive coherent interband polarization combined with dynamical Bloch oscillations in semiconducting gallium selenide. These dynamics entail the emission of phase-stable high-harmonic transients, covering the entire terahertz-to-visible spectral domain between 0.1 and 675 THz. Quantum interference of different ionization paths of accelerated charge carriers is controlled via the waveform of the driving field and explained by a quantum theory of inter- and intraband dynamics. Our results pave the way towards all-coherent terahertz-rate electronics.
Magnonics as an emerging nanotechnology offers functionalities beyond current semiconductor technology. Spin waves used in cellular nonlinear networks are expected to speed up technologically, ...demanding tasks such as image processing and speech recognition at low power consumption. However, efficient coupling to microelectronics poses a vital challenge. Previously developed techniques for spin-wave excitation (for example, by using parametric pumping in a cavity) may not allow for the relevant downscaling or provide only individual point-like sources. Here we demonstrate that a grating coupler of periodically nanostructured magnets provokes multidirectional emission of short-wavelength spin waves with giantly enhanced amplitude compared with a bare microwave antenna. Exploring the dependence on ferromagnetic materials, lattice constants and the applied magnetic field, we find the magnonic grating coupler to be more versatile compared with gratings in photonics and plasmonics. Our results allow one to convert, in particular, straight microwave antennas into omnidirectional emitters for short-wavelength spin waves, which are key to cellular nonlinear networks and integrated magnonics.
We demonstrate a new technique for frequency-swept laser operation--Fourier domain mode locking (FDML)--and its application for swept-source optical coherence tomography (OCT) imaging. FDML is ...analogous to active laser mode locking for short pulse generation, except that the spectrum rather than the amplitude of the light field is modulated. High-speed, narrowband optical frequency sweeps are generated with a repetition period equal to the fundamental or a harmonic of cavity round-trip time. An FDML laser is constructed using a long fiber ring cavity, a semiconductor optical amplifier, and a tunable fiber Fabry-Perot filter. Effective sweep rates of up to 290 kHz are demonstrated with a 105 nm tuning range at 1300 nm center wavelength. The average output power is 3mW directly from the laser and 20 mW after post-amplification. Using the FDML laser for swept-source OCT, sensitivities of 108 dB are achieved and dynamic linewidths are narrow enough to enable imaging over a 7 mm depth with only a 7.5 dB decrease in sensitivity. We demonstrate swept-source OCT imaging with acquisition rates of up to 232,000 axial scans per second. This corresponds to 906 frames/second with 256 transverse pixel images, and 3.5 volumes/second with a 256x128x256 voxel element 3-DOCT data set. The FDML laser is ideal for swept-source OCT imaging, thus enabling high imaging speeds and large imaging depths.