Spin-Momentum Locking and Ultrafast Spin-Charge Conversion in Ultrathin Epitaxial Bi1 - x Sbx Topological Insulator.

The helicity of three-dimensional (3D) topological insulator surface states has drawn significant attention in spintronics owing to spin-momentum locking where the carriers' spin is oriented perpendicular to their momentum. This property can provide an efficient method to convert charge currents into spin currents, and vice-versa, through the Rashba-Edelstein effect. However, experimental signatures of these surface states to the spin-charge conversion are extremely difficult to disentangle from bulk state contributions. Here, spin- and angle-resolved photo-emission spectroscopy, and time-resolved THz emission spectroscopy are combined to categorically demonstrate that spin-charge conversion arises mainly from the surface state in Bi1 - x Sbx ultrathin films, down to few nanometers where confinement effects emerge. This large conversion efficiency is correlated, typically at the level of the bulk spin Hall effect from heavy metals, to the complex Fermi surface obtained from theoretical calculations of the inverse Rashba-Edelstein response. Both surface state robustness and sizeable conversion efficiency in epitaxial Bi1 - x Sbx thin films bring new perspectives for ultra-low power magnetic random-access memories and broadband THz generation.

Vacuum-field-induced THz transport gap in a carbon nanotube quantum dot.

The control of light-matter interaction at the most elementary level has become an important resource for quantum technologies. Implementing such interfaces in the THz range remains an outstanding problem. Here, we couple a single electron trapped in a carbon nanotube quantum dot to a THz resonator. The resulting light-matter interaction reaches the deep strong coupling regime that induces a THz energy gap in the carbon nanotube solely by the vacuum fluctuations of the THz resonator. This is directly confirmed by transport measurements. Such a phenomenon which is the exact counterpart of inhibition of spontaneous emission in atomic physics opens the path to the readout of non-classical states of light using electrical current. This would be a particularly useful resource and perspective for THz quantum optics.

Author Correction: Diffraction-limited ultrabroadband terahertz spectroscopy.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Ultra-long carrier lifetime in neutral graphene-hBN van der Waals heterostructures under mid-infrared illumination.

Graphene/hBN heterostructures are promising active materials for devices in the THz domain, such as emitters and photodetectors based on interband transitions. Their performance requires long carrier lifetimes. However, carrier recombination processes in graphene possess sub-picosecond characteristic times for large non-equilibrium carrier densities at high energy. An additional channel has been recently demonstrated in graphene/hBN heterostructures by emission of hBN hyperbolic phonon polaritons (HPhP) with picosecond decay time. Here, we report on carrier lifetimes in graphene/hBN Zener-Klein transistors of ~30 ps for photoexcited carriers at low density and energy, using mid-infrared photoconductivity measurements. We further demonstrate the switching of carrier lifetime from ~30 ps (attributed to interband Auger) down to a few picoseconds upon ignition of HPhP relaxation at finite bias and/or with infrared excitation power. Our study opens interesting perspectives to exploit graphene/hBN heterostructures for THz lasing and highly sensitive THz photodetection as well as for phonon polariton optics.

Giant optical nonlinearity interferences in quantum structures.

Second-order optical nonlinearities can be greatly enhanced by orders of magnitude in resonantly excited nanostructures. These resonant nonlinearities continually attract attention, particularly in newly discovered materials. However, they are frequently not as heightened as currently predicted, limiting their exploitation in nanostructured nonlinear optics. Here, we present a clear-cut theoretical and experimental demonstration that the second-order nonlinear susceptibility can vary by orders of magnitude as a result of giant destructive, as well as constructive, interference effects in complex systems. Using terahertz quantum cascade lasers as a model source to investigate interband and intersubband nonlinearities, we show that these giant interferences are a result of an unexpected interplay of the second-order nonlinear contributions of multiple light and heavy hole states. As well as of importance to understand and engineer the resonant optical properties of nanostructures, this advanced framework can be used as a novel, sensitive tool to elucidate the band structure properties of complex materials.

High-speed THz spectroscopic imaging at ten kilohertz pixel rate with amplitude and phase contrast.

By combining the advantages of the high-speed ASOPS technology and efficient THz generation, we have realized a high-speed laser-based spectroscopic THz imaging system with more than 10,000 pixels per second acquisition speed and an excellent signal-to-noise ratio of more than 100. Unlike THz line cameras or mm-wave intensity detectors, the present device allows for a much higher spatial resolution and attributes each imaging pixel with phase and amplitude information up to several THz while simultaneously maintaining a very high scanning speed unmatched by any other technique presented so far. The high-speed acquisition allows for samples to be scanned even at sample velocities of 5 m/s or higher while preserving the fundamental resolution limit of the THz radiation, which is on the order of 500 µm in the present case.

Diffraction-limited ultrabroadband terahertz spectroscopy.

Diffraction is the ultimate limit at which details of objects can be resolved in conventional optical spectroscopy and imaging systems. In the THz spectral range, spectroscopy systems increasingly rely on ultra-broadband radiation (extending over more 5 octaves) making a great challenge to reach resolution limited by diffraction. Here, we propose an original easy-to-implement wavefront manipulation concept to achieve ultrabroadband THz spectroscopy system with diffraction-limited resolution. Applying this concept to a large-area photoconductive emitter, we demonstrate diffraction-limited ultra-broadband spectroscopy system up to 14.5 THz with a dynamic range of 10(3). The strong focusing of ultrabroadband THz radiation provided by our approach is essential for investigating single micrometer-scale objects such as graphene flakes or living cells, and besides for achieving intense ultra-broadband THz electric fields.

Engineered far-fields of metal-metal terahertz quantum cascade lasers with integrated planar horn structures.

The far-field emission profile of terahertz quantum cascade lasers (QCLs) in metal-metal waveguides is controlled in directionality and form through planar horn-type shape structures, whilst conserving a broad spectral response. The structures produce a gradual change in the high modal confinement of the waveguides and permit an improved far-field emission profile and resulting in a four-fold increase in the emitted output power. The two-dimensional far-field patterns are measured at 77 K and are agreement in with 3D modal simulations. The influence of parasitic high-order transverse modes is shown to be controlled by engineering the horn structure (ridge and horn widths), allowing only the fundamental mode to be coupled out.

Optical sideband generation up to room temperature with mid-infrared quantum cascade lasers.

Mid-infrared (MIR) sideband generation on a near infrared (NIR) optical carrier is demonstrated within a quantum cascade laser (QCL). By employing an externally injected NIR beam, E(NIR), that is resonant with the interband transitions of the quantum wells in the QCL, the nonlinear susceptibility is enhanced, leading to both frequency mixing and sideband generation. A GaAs-based MIR QCL (E(QCL) = 135 meV) with an aluminum-reinforced waveguide was utilized to overlap the NIR and MIR modes with the optical nonlinearity of the active region. The resulting difference sideband (E(NIR) - E(QCL)) shows a resonant behavior as a function of NIR pump wavelength and a maximum second order nonlinear susceptibility, χ((2)), of ~1 nm/V was obtained. Further, the sideband intensity showed little dependence with the operating temperature of the QCL, allowing sideband generation to be realized at room temperature.

20 THz broadband generation using semi-insulating GaAs interdigitated photoconductive antennas.

We demonstrate broadband (20 THz), high electric field, terahertz generation using large area interdigitated antennas fabricated on semi-insulating GaAs. The bandwidth is characterized as a function of incident pulse duration (15-35 fs) and pump energy (2-30 nJ). Broadband spectroscopy of PTFE is shown. Numerical Drude-Lorentz simulations of the generated THz pulses are performed as a function of the excitation pulse duration, showing good agreement with the experimental data.

Terahertz generation by dynamical photon drag effect in graphene excited by femtosecond optical pulses.

Graphene has been proposed as a particularly attractive material for the achievement of strong optical nonlinearities, in particular generation of terahertz radiation. However, owing to the particular symmetries of the C-lattice, second-order nonlinear effects such as difference-frequency or rectification processes are predicted to vanish in a graphene layer for optical excitations (ℏω ≫ 2EF) involving the two relativistic dispersion bands. Here we experimentally demonstrate that graphene excited by femtosecond optical pulses generate a coherent THz radiation ranging from 0.1 to 4 THz via a second-order nonlinear effect. We fully interpret its characteristics with a model describing the electron and hole states beyond the usual massless relativistic scheme. This second-order nonlinear effect is dynamical photon drag, which relies on the transfer of light momentum to the carriers by the ponderomotive electric and magnetic forces. The model highlights the key roles of next-C-neighbor couplings and of unequal electron and hole lifetimes in the observed second-order response. Finally, our results indicate that dynamical photon drag effect in graphene can provide emission up to 60 THz, opening new routes for the generation of ultrabroadband terahertz pulses.

Terahertz radiation from magnetic excitations in diluted magnetic semiconductors.

We probed, in the time domain, the THz electromagnetic radiation originating from spins in CdMnTe diluted magnetic semiconductor quantum wells containing high-mobility electron gas. Taking advantage of the efficient Raman generation process, the spin precession was induced by low power near-infrared pulses. We provide a full theoretical first-principles description of spin-wave generation, spin precession, and of emission of THz radiation. Our results open new perspectives for improved control of the direct coupling between spin and an electromagnetic field, e.g., by using semiconductor technology to insert the THz sources in cavities or pillars.

Mode-locking of a terahertz laser by direct phase synchronization.

A novel scheme to achieve mode-locking of a multimode laser is demonstrated. Traditional methods to produce ultrashort laser pulses are based on modulating the cavity gain or losses at the cavity roundtrip frequency, favoring the pulsed emission. Here, we rather directly act on the phases of the modes, resulting in constructive interference for the appropriated phase relationship. This was performed on a terahertz quantum cascade laser by multimode injection seeding with an external terahertz pulse, resulting in phase mode-locked terahertz laser pulses of 9 ps duration, characterized unambiguously in the time domain.

Integrated injection seeded terahertz source and amplifier for time-domain spectroscopy.

We used a terahertz (THz) quantum cascade laser (QCL) as an integrated injection seeded source and amplifier for THz time-domain spectroscopy. A THz input pulse is generated inside a QCL by illuminating the laser facet with a near-IR pulse from a femtosecond laser and amplified using gain switching. The THz output from the QCL is found to saturate upon increasing the amplitude of the THz input power, which indicates that the QCL is operating in an injection seeded regime.

Ultrafast dynamics of coherences in a quantum Hall system.

Using three-pulse four-wave-mixing optical spectroscopy, we study the ultrafast dynamics of the quantum Hall system. We observe striking differences as compared to an undoped system, where the 2D electron gas is absent. In particular, we observe a large off-resonant signal with strong oscillations. Using a microscopic theory, we show that these are due to many-particle coherences created by interactions between photoexcited carriers and collective excitations of the 2D electron gas. We extract quantitative information about the dephasing and interference of these coherences.

Parametric oscillation in vertical triple microcavities.

Optical parametric oscillation is a nonlinear process that enables coherent generation of 'signal' and 'idler' waves, shifted in frequency from the pump wave. Efficient parametric conversion is the paradigm for the generation of twin or entangled photons for quantum optics applications such as quantum cryptography, or for the generation of new frequencies in spectral domains not accessible by existing devices. Rapid development in the field of quantum information requires monolithic, alignment-free sources that enable efficient coupling into optical fibres and possibly electrical injection. During the past decade, much effort has been devoted to the development of integrated devices for quantum information and to the realization of all-semiconductor parametric oscillators. Nevertheless, at present optical parametric oscillators typically rely on nonlinear crystals placed into complex external cavities, and pumped by powerful external lasers. Long interaction lengths are typically required and the phase mismatch between the parametric waves propagating at different velocities results in poor parametric conversion efficiencies. Here we report the demonstration of parametric oscillation in a monolithic semiconductor triple microcavity with signal, pump and idler waves propagating along the vertical direction of the nanostructure. Alternatively, signal and idler beams can also be collected at finite angles, allowing the generation of entangled photon pairs. The pump threshold intensity is low enough to envisage the realization of an all-semiconductor electrically pumped micro-parametric oscillator.

Polariton parametric amplifier pump dynamics in the coherent regime.

We studied the pump coherent dynamics in a II-VI microcavity parametric amplifier, using angle-resolved four-wave mixing. The polariton parametric amplification is found to result in a strong quenching and saturation of the pump coherence lifetime above the threshold. For the polariton scattering processes that remain below the amplification threshold, we find an angle-dependent collision broadening associated with the efficiency of the polariton scattering towards the excitonic reservoir.

Unified picture of polariton propagation in bulk GaAs semiconductors

High-resolution amplitude and phase linear spectroscopy of high-quality bulk GaAs are reported. The detailed structure of the observed full complex transmission is consistently explained by polariton effects on the basis of microscopic calculations. The coupled equations for the excitonic polarization and the light field in the slab configuration are evaluated using appropriate boundary conditions for the electromagnetic field and the excitonic wave function without reference to additional boundary conditions for the macroscopic polarization.