Takuya Higuchi

Strong-Field Perspective on High-Harmonic Radiation from Bulk Solids

Mechanisms of high-harmonic generation from crystals are described by treating the electric field of a laser as a quasistatic strong field. Under the quasistatic electric field, electrons in periodic potentials form dressed states, known as Wannier-Stark states. The energy differences between the dressed states determine the frequencies of the radiation. The radiation yield is determined by the magnitudes of the interband and intraband current matrix elements between the dressed states. The generation of attosecond pulses from solids is predicted. Ramifications for strong-field physics are discussed.

Visualizing the interfacial evolution from charge compensation to metallic screening across the manganite metal–insulator transition

Electronic changes at polar interfaces between transition metal oxides offer the tantalizing possibility to stabilize novel ground states yet can also cause unintended reconstructions in devices. The nature of these interfacial reconstructions should be qualitatively different for metallic and insulating films as the electrostatic boundary conditions and compensation mechanisms are distinct. Here we directly quantify with atomic-resolution the charge distribution for manganite-titanate interfaces traversing the metal-insulator transition. By measuring the concentration and valence of the cations, we find an intrinsic interfacial electronic reconstruction in the insulating films. The total charge observed for the insulating manganite films quantitatively agrees with that needed to cancel the polar catastrophe. As the manganite becomes metallic with increased hole doping, the total charge build-up and its spatial range drop substantially. Direct quantification of the intrinsic charge transfer and spatial width should lay the framework for devices harnessing these unique electronic phases.

Light-field-driven currents in graphene

The ability to steer electrons using the strong electromagnetic field of light has opened up the possibility of controlling electron dynamics on the sub-femtosecond (less than 10−15 seconds) timescale. In dielectrics and semiconductors, various light-field-driven effects have been explored, including high-harmonic generation, sub-optical-cycle interband population transfer and the non-perturbative change of the transient polarizability. In contrast, much less is known about light-field-driven electron dynamics in narrow-bandgap systems or in conductors, in which screening due to free carriers or light absorption hinders the application of strong optical fields. Graphene is a promising platform with which to achieve light-field-driven control of electrons in a conducting material, because of its broadband and ultrafast optical response, weak screening and high damage threshold. Here we show that a current induced in monolayer graphene by two-cycle laser pulses is sensitive to the electric-field waveform, that is, to the exact shape of the optical carrier field of the pulse, which is controlled by the carrier-envelope phase, with a precision on the attosecond (10−18 seconds) timescale. Such a current, dependent on the carrier-envelope phase, shows a striking reversal of the direction of the current as a function of the driving field amplitude at about two volts per nanometre. This reversal indicates a transition of light–matter interaction from the weak-field (photon-driven) regime to the strong-field (light-field-driven) regime, where the intraband dynamics influence interband transitions. We show that in this strong-field regime the electron dynamics are governed by sub-optical-cycle Landau–Zener–Stückelberg interference, composed of coherent repeated Landau–Zener transitions on the femtosecond timescale. Furthermore, the influence of this sub-optical-cycle interference can be controlled with the laser polarization state. These coherent electron dynamics in graphene take place on a hitherto unexplored timescale, faster than electron–electron scattering (tens of femtoseconds) and electron–phonon scattering (hundreds of femtoseconds). We expect these results to have direct ramifications for band-structure tomography and light-field-driven petahertz electronics.

A nanoscale vacuum-tube diode triggered by few-cycle laser pulses

We propose and demonstrate a nanoscale vacuum-tube diode triggered by few-cycle near-infrared laser pulses. It represents an ultrafast electronic device based on light fields, exploiting near-field optical enhancement at surfaces of two metal nanotips. The sharper of the two tips displays a stronger field-enhancement, resulting in larger photoemission yields at its surface. One laser pulse with a peak intensity of 4.7u2009×u20091011u2009W/cm2 triggers photoemission of ∼16 electrons from the sharper cathode tip, while emission from the blunter anode tip is suppressed by 19u2009dB to ∼0.2 electrons per pulse. Thus, the laser-triggered current between two tips exhibit a rectifying behavior, in analogy to classical vacuum-tube diodes. According to the kinetic energy of the emitted electrons and the distance between the tips, the total operation time of this laser-triggered nanoscale diode is estimated to be below 1 ps.

Excitation of coupled spin–orbit dynamics in cobalt oxide by femtosecond laser pulses

Ultrafast control of magnets using femtosecond light pulses attracts interest regarding applications and fundamental physics of magnetism. Antiferromagnets are promising materials with magnon frequencies extending into the terahertz range. Visible or near-infrared light interacts mainly with the electronic orbital angular momentum. In many magnets, however, in particular with iron-group ions, the orbital momentum is almost quenched by the crystal field. Thus, the interaction of magnons with light is hampered, because it is only mediated by weak unquenching of the orbital momentum by spin–orbit interactions. Here we report all-optical excitation of magnons with frequencies up to 9u2009THz in antiferromagnetic CoO with an unquenched orbital momentum. In CoO, magnon modes are coupled oscillations of spin and orbital momenta with comparable amplitudes. We demonstrate excitations of magnon modes by directly coupling light with electronic orbital angular momentum, providing possibilities to develop magneto-optical devices operating at several terahertz with high output-to-input ratio.Light pulses can control magnetism in a material, and the effective creation of magnetic oscillations leads to spintronic devices with higher efficiency. Here, the authors increase the efficiency of magnon excitation by using a material in which orbital angular momenta are not quenched.

Control of antiferromagnetic domain distribution via polarization-dependent optical annealing.

The absence of net magnetization inside antiferromagnetic domains has made the control of their spatial distribution quite challenging. Here we experimentally demonstrate an optical method for controlling antiferromagnetic domain distributions in MnF2. Reduced crystalline symmetry can couple an order parameter with non-conjugate external stimuli. In the case of MnF2, time-reversal symmetry is macroscopically broken reflecting the different orientations of the two magnetic sublattices. Thus, it exhibits different absorption coefficients between two orthogonal linear polarizations below its antiferromagnetic transition temperature under an external magnetic field. Illumination with linearly polarized laser light under this condition selectively destructs the formation of a particular antiferromagnetic order via heating. As a result, the other antiferromagnetic order is favoured inside the laser spot, achieving spatially localized selection of an antiferromagnetic order. Applications to control of interface states at antiferromagnetic domain boundaries, exchange bias and control of spin currents are expected.

Landau-Zener-Stückelberg interferometer on attosecond timescales in graphene

When solids are exposed to intense optical fields, the intraband electron motion may influence interband transitions, potentially causing a transition of light-matter interaction from a quantum (photon-driven) regime to a semi-classical (field-driven) regime. We demonstrate this transition in monolayer graphene. We observe a carrier-envelope-phasedependent current in graphene irradiated with phase-stable two-cycle laser pulses, showing a striking reversal of the current direction as a function of the driving field amplitude at ~2 V/nm. This reversal indicates the transition into the field-driven (or strong-field) regime. We show furthermore that in this regime electron dynamics are governed by suboptical-cycle Landau-Zener-Stückelberg interference, comprised of coherent repeated Landau-Zener transitions. We expect these results to have direct ramifications for light-wave driven electronics in graphene.

High spatial coherence in multiphoton-photoemitted electron beams

Nanometer-sharp metallic tips are known to be excellent electron emitters. They are used in highest-resolution electron microscopes in cold field emission mode to generate the most coherent electron beam in continuous-wave operation. For time-resolved operation, sharp metal needle tips have recently been triggered with femtosecond laser pulses. We show here that electrons emitted with near-infrared femtosecond laser pulses at laser oscillator repetition rates show the same spatial coherence properties as electrons in cold field emission mode in cw operation. From electron interference fringes, obtained with the help of a carbon nanotube biprism beam splitter, we deduce a virtual source size of less than

Electron dynamics in graphene reaching the light-field-driven regime

(0.65pm0.06),

Strong-field physics: Harmonic radiation from crystals

nm for both operation modes, a factor of ten smaller than the geometrical source size. These results bear promise for ultrafast electron diffraction, ultrafast electron microscopy and other techniques relying on highly coherent and ultrafast electron beams.