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93 result(s) for "639/301/1019/584"
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High-harmonic generation from an atomically thin semiconductor
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 timescales 1 , 2 , 3 , 4 , 5 , 6 . The generation process has been discussed in the context of strongly driven electron dynamics in single-particle bands 7 , 8 , 9 , 10 , 11 , 12 , 13 , 14 . Two-dimensional materials exhibit distinctive electronic properties compared to the bulk that could significantly modify the HHG process 15 , 16 , including different symmetries 17 , 18 , 19 , access to individual valleys 20 , 21 and enhanced many-body interactions 22 , 23 , 24 , 25 . Here we demonstrate non-perturbative HHG from a monolayer MoS 2 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.
Light-field-driven currents in graphene
Light-field-driven control of electrons in a conductor is demonstrated by inducing a current by laser pulses in graphene that is sensitive to the carrier-envelope phase. A light on current advances in graphene A new field of ultrafast electronics has emerged in recent years that uses strong electromagnetic (light) fields to steer electrons. It is difficult to explore such effects in metals because of screening by the charge carriers, so mainly insulators and semiconductors have been studied in this area. However, different physics applies to graphene, a two-dimensional material in which only weak screening is present. Takuya Higuchi et al . have now generated electric currents in graphene with ultrafast light fields. The current is sensitive 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 timescale. The results open up new opportunities for creating light-field-driven petahertz electronics. 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 1 , 2 , 3 , 4 , sub-optical-cycle interband population transfer 5 and the non-perturbative change of the transient polarizability 6 , 7 . 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 6 , 8 . 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 9 , 10 . 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 11 , 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) 12 , 13 , 14 . We expect these results to have direct ramifications for band-structure tomography 2 and light-field-driven petahertz electronics 8 .
Regulation of the luminescence mechanism of two-dimensional tin halide perovskites
Two-dimensional (2D) Sn-based perovskites are a kind of non-toxic environment-friendly luminescent material. However, the research on the luminescence mechanism of this type of perovskite is still very controversial, which greatly limits the further improvement and application of the luminescence performance. At present, the focus of controversy is defects and phonon scattering rates. In this work, we combine the organic cation control engineering with temperature-dependent transient absorption spectroscopy to systematically study the interband exciton relaxation pathways in layered A 2 SnI 4 (A = PEA + , BA + , HA + , and OA + ) structures. It is revealed that exciton-phonon scattering and exciton-defect scattering have different effects on exciton relaxation. Our study further confirms that the deformation potential scattering by charged defects, not by the non-polar optical phonons, dominates the excitons interband relaxation, which is largely different from the Pb-based perovskites. These results enhance the understanding of the origin of the non-radiative pathway in Sn-based perovskite materials. Exciton scattering in perovskite is an important phenomenon dictating the optoelectronic performance. Here, the authors confirm the deformation potential scattering by charged defects, not by the non-polar optical phonons, dominates the excitons interband relaxation in 2D Sn-based perovskites.
Orbitronics: light-induced orbital currents in Ni studied by terahertz emission experiments
Orbitronics is based on the use of orbital currents as information carriers. Orbital currents can be generated from the conversion of charge or spin currents, and inversely, they could be converted back to charge or spin currents. Here we demonstrate that orbital currents can also be generated by femtosecond light pulses on Ni. In multilayers associating Ni with oxides and nonmagnetic metals such as Cu, we detect the orbital currents by their conversion into charge currents and the resulting terahertz emission. We show that the orbital currents extraordinarily predominate the light-induced spin currents in Ni-based systems, whereas only spin currents can be detected with CoFeB-based systems. In addition, the analysis of the time delays of the terahertz pulses leads to relevant information on the velocity and propagation length of orbital carriers. Our finding of light-induced orbital currents and our observation of their conversion into charge currents opens new avenues in orbitronics, including the development of orbitronic terahertz devices. Several recent works have highlighted the importance of the orbital currents in transferring angular momentum within materials. In combination with spin-orbit coupling, such orbital currents can be used to alter the magnetization of a material. Herein, the authors demonstrate the inverse effect, showing orbital current driven terahertz emission in Nickel based heterostructures.
A light-induced phononic symmetry switch and giant dissipationless topological photocurrent in ZrTe5
Dissipationless currents from topologically protected states are promising for disorder-tolerant electronics and quantum computation. Here, we photogenerate giant anisotropic terahertz nonlinear currents with vanishing scattering, driven by laser-induced coherent phonons of broken inversion symmetry in a centrosymmetric Dirac material ZrTe 5 . Our work suggests that this phononic terahertz symmetry switching leads to formation of Weyl points, whose chirality manifests in a transverse, helicity-dependent current, orthogonal to the dynamical inversion symmetry breaking axis, via circular photogalvanic effect. The temperature-dependent topological photocurrent exhibits several distinct features: Berry curvature dominance, particle–hole reversal near conical points and chirality protection that is responsible for an exceptional ballistic transport length of ~10 μm. These results, together with first-principles modelling, indicate two pairs of Weyl points dynamically created by B 1u phonons of broken inversion symmetry. Such phononic terahertz control breaks ground for coherent manipulation of Weyl nodes and robust quantum transport without application of static electric or magnetic fields. Femtosecond optical pulses are used to generate coherent phonons that break inversion symmetry and drive anisotropic terahertz photocurrents in the topological material ZrTe 5 .
Lanthanide-doped inorganic nanoparticles turn molecular triplet excitons bright
The generation, control and transfer of triplet excitons in molecular and hybrid systems is of great interest owing to their long lifetime and diffusion length in both solid-state and solution phase systems, and to their applications in light emission 1 , optoelectronics 2 , 3 , photon frequency conversion 4 , 5 and photocatalysis 6 , 7 . Molecular triplet excitons (bound electron–hole pairs) are ‘dark states’ because of the forbidden nature of the direct optical transition between the spin-zero ground state and the spin-one triplet levels 8 . Hence, triplet dynamics are conventionally controlled through heavy-metal-based spin–orbit coupling 9 – 11 or tuning of the singlet–triplet energy splitting 12 , 13 via molecular design. Both these methods place constraints on the range of properties that can be modified and the molecular structures that can be used. Here we demonstrate that it is possible to control triplet dynamics by coupling organic molecules to lanthanide-doped inorganic insulating nanoparticles. This allows the classically forbidden transitions from the ground-state singlet to excited-state triplets to gain oscillator strength, enabling triplets to be directly generated on molecules via photon absorption. Photogenerated singlet excitons can be converted to triplet excitons on sub-10-picosecond timescales with unity efficiency by intersystem crossing. Triplet exciton states of the molecules can undergo energy transfer to the lanthanide ions with unity efficiency, which allows us to achieve luminescent harvesting of the dark triplet excitons. Furthermore, we demonstrate that the triplet excitons generated in the lanthanide nanoparticle–molecule hybrid systems by near-infrared photoexcitation can undergo efficient upconversion via a lanthanide–triplet excitation fusion process: this process enables endothermic upconversion and allows efficient upconversion from near-infrared to visible frequencies in the solid state. These results provide a new way to control triplet excitons, which is essential for many fields of optoelectronic and biomedical research. Optically dark (non-emitting) triplet excitons on organic molecules may be rendered bright by coupling the molecules to lanthanide-doped nanoparticles, providing a way to control such excitons in optoelectronic systems.
Materials for chiral light control
Solution-processable semiconductors based on small molecules, polymers or halide perovskites combine sustainable manufacturing with exceptional optoelectronic properties that can be chemically tailored to achieve flexible and highly efficient optoelectronic and photonic devices. A new exciting research direction is the study of the influence of chirality on light–matter interactions in these soft materials and its exploitation for the simultaneous control of charge, spin and light. In this Viewpoint, researchers working on different types of chiral semiconductors discuss the most interesting directions in this rapidly expanding field.
Ultrafast switching of tunable infrared plasmons in indium tin oxide nanorod arrays with large absolute amplitude
All-optical control of plasmons can enable optical switches with high speeds, small footprints and high on/off ratios. Here we demonstrate ultrafast plasmon modulation in the near-infrared (NIR) to mid-infrared (MIR) range by intraband pumping of indium tin oxide nanorod arrays (ITO-NRAs). We observe redshifts of localized surface plasmon resonances arising from a change of the plasma frequency of ITO, which is governed by the conduction band non-parabolicity. We generalize the plasma frequency for non-parabolic bands, quantitatively model the fluence-dependent plasma frequency shifts, and show that different from noble metals, the lower electron density in ITO enables a remarkable change of electron distributions, yielding a significant plasma frequency modulation and concomitant large transient bleaches and induced absorptions, which can be tuned spectrally by tailoring the ITO-NRA geometry. The low electron heat capacity explains the sub-picosecond kinetics that is much faster than noble metals. Our work demonstrates a new scheme to control infrared plasmons for optical switching, telecommunications and sensing. Ultrafast plasmon modulation has been realized in the near- to mid-infrared range by intraband pumping of indium tin oxide nanorod arrays.
Coupling of terahertz light with nanometre-wavelength magnon modes via spin–orbit torque
Spin-based technologies can operate at terahertz frequencies but require manipulation techniques that work at ultrafast timescales to become practical. For instance, devices based on spin waves, also known as magnons, require efficient generation of high-energy exchange spin waves at nanometre wavelengths. To achieve this, a substantial coupling is needed between the magnon modes and an electro-magnetic stimulus such as a coherent terahertz field pulse. However, it has been difficult to excite non-uniform spin waves efficiently using terahertz light because of the large momentum mismatch between the submillimetre-wave radiation and the nanometre-sized spin waves. Here we improve the light–matter interaction by engineering thin films to exploit relativistic spin–orbit torques that are confined to the interfaces of heavy metal/ferromagnet heterostructures. We are able to excite spin-wave modes with frequencies of up to 0.6 THz and wavelengths as short as 6 nm using broadband terahertz radiation. Numerical simulations demonstrate that the coupling of terahertz light to exchange-dominated magnons originates solely from interfacial spin–orbit torques. Our results are of general applicability to other magnetic multilayered structures, and offer the prospect of nanoscale control of high-frequency signals.Engineering of the spin–orbit interactions in a magnetic multilayered structure makes it possible to coherently generate coherent spin waves using terahertz radiation, which could benefit the development of spintronic devices.
Active tuning of surface phonon polariton resonances via carrier photoinjection
Surface phonon polaritons (SPhPs) are attractive alternatives to infrared plasmonics for subdiffractional confinement of infrared light. Localized SPhP resonances in semiconductor nanoresonators are narrow, but that linewidth and the limited extent of the Reststrahlen band limit spectral coverage. To address this limitation, we report active tuning of SPhP resonances in InP and 4H-SiC by photoinjecting free carriers into nanoresonators, taking advantage of the coupling between the carrier plasma and optic phonons to blueshift SPhP resonances. We demonstrate state-of-the-art tuning figures of merit upon continuous-wave excitation (in InP) or pulsed excitation (in 4H-SiC). Lifetime effects cause the tuning to saturate in InP, and carrier redistribution leads to rapid (<50 ps) recovery of the resonance in 4H-SiC. This work demonstrates the potential for this method and opens a path towards actively tuned nanophotonic devices, such as modulators and beacons, in the infrared, and identifies important implications of coupling between electronic and phononic excitations.