Ultrafast Laser-Induced Dynamics of Non-Equilibrium Electron Spill-Out in Nanoplasmonic Bilayers.

Contemporary quantum plasmonics capture subtle corrections to the properties of plasmonic nano-objects in equilibrium. Here, we demonstrate non-equilibrium spill-out redistribution of the electronic density at the ultrafast time scale. As revealed by time-resolved 2D spectroscopy of nanoplasmonic Fe/Au bilayers, an injection of the laser-excited non-thermal electrons induces transient electron spill-out thus changing the plasma frequency. The response of the local electronic density switches the electronic density behavior from spill-in to strong (an order of magnitude larger) spill-out at the femtosecond time scale. The superdiffusive transport of hot electrons and the lack of a direct laser heating indicate significantly non-thermal origin of the underlying physics. Our results demonstrate an ultrafast and non-thermal way to control surface plasmon dispersion through transient variations of the spatial electron distribution at the nanoscale. These findings expand quantum plasmonics into previously unexplored directions by introducing ultrashort time scales in the non-equilibrium electronic systems.

Surface Plasmon-Enhanced Photomagnetic Excitation of Spin Dynamics in Au/YIG:Co Magneto-Plasmonic Crystals.

We report strong amplification of the photomagnetic spin precession in Co-doped YIG employing a surface plasmon excitation in a metal-dielectric magneto-plasmonic crystal. Plasmonic enhancement is accompanied by the localization of the excitation within the 300 nm thick layer inside the transparent dielectric garnet. Experimental results are nicely reproduced by numerical simulations of the photomagnetic excitation. Our findings demonstrate the magneto-plasmonic concept of subwavelength localization and amplification of the photomagnetic excitation in dielectric YIG:Co, which can potentially be employed for all-optical magnetization switching below the diffraction limit, with energy efficiency approaching the fundamental limit for magnetic memories.

Giant magneto-refractive effect in mid-infrared second-harmonic generation from plasmonic antennas.

Active modulation of nonlinear-optical response from metallic nanostructures can be realized with an external magnetic field. We report a resonant 20% magneto-refractive modulation in second-harmonic generation (SHG) from spintronic multilayer antennas in the mid-infrared. We discuss mechanisms of this modulation and show that it cannot be explained by an unequal enhancement of the electromagnetic field. Instead, we propose a novel, to the best of our knowledge, contribution to the nonlinear susceptibility, which relies on the spin-dependent electron mean free path. In contrast to magneto-optics in ferromagnets, our approach allows simultaneous observation of the enhanced SHG and its large modulation.

Controlling the Infrared Dielectric Function through Atomic-Scale Heterostructures.

Surface phonon polaritons (SPhPs), the surface-bound electromagnetic modes of a polar material resulting from the coupling of light with optic phonons, offer immense technological opportunities for nanophotonics in the infrared (IR) spectral region. However, once a particular material is chosen, the SPhP characteristics are fixed by the spectral positions of the optic phonon frequencies. Here, we provide a demonstration of how the frequency of these optic phonons can be altered by employing atomic-scale superlattices (SLs) of polar semiconductors using AlN/GaN SLs as an example. Using second harmonic generation (SHG) spectroscopy, we show that the optic phonon frequencies of the SLs exhibit a strong dependence on the layer thicknesses of the constituent materials. Furthermore, new vibrational modes emerge that are confined to the layers, while others are centered at the AlN/GaN interfaces. As the IR dielectric function is governed by the optic phonon behavior in polar materials, controlling the optic phonons provides a means to induce and potentially design a dielectric function distinct from the constituent materials and from the effective-medium approximation of the SL. We show that atomic-scale AlN/GaN SLs instead have multiple Reststrahlen bands featuring spectral regions that exhibit either normal or extreme hyperbolic dispersion with both positive and negative permittivities dispersing rapidly with frequency. Apart from the ability to engineer the SPhP properties, SL structures may also lead to multifunctional devices that combine the mechanical, electrical, thermal, or optoelectronic functionality of the constituent layers. We propose that this effort is another step toward realizing user-defined, actively tunable IR optics and sources.

Femtosecond formation dynamics of the spin Seebeck effect revealed by terahertz spectroscopy.

Understanding the transfer of spin angular momentum is essential in modern magnetism research. A model case is the generation of magnons in magnetic insulators by heating an adjacent metal film. Here, we reveal the initial steps of this spin Seebeck effect with <27 fs time resolution using terahertz spectroscopy on bilayers of ferrimagnetic yttrium iron garnet and platinum. Upon exciting the metal with an infrared laser pulse, a spin Seebeck current js arises on the same ~100 fs time scale on which the metal electrons thermalize. This observation highlights that efficient spin transfer critically relies on carrier multiplication and is driven by conduction electrons scattering off the metal-insulator interface. Analytical modeling shows that the electrons' dynamics are almost instantaneously imprinted onto js because their spins have a correlation time of only ~4 fs and deflect the ferrimagnetic moments without inertia. Applications in material characterization, interface probing, spin-noise spectroscopy and terahertz spin pumping emerge.

Strong Coupling of Epsilon-Near-Zero Phonon Polaritons in Polar Dielectric Heterostructures.

We report the first observation of epsilon-near-zero (ENZ) phonon polaritons in an ultrathin AlN film fully hybridized with surface phonon polaritons (SPhP) supported by the adjacent SiC substrate. Employing a strong coupling model for the analysis of the dispersion and electric field distribution in these hybridized modes, we show that they share the most prominent features of the two precursor modes. The novel ENZ-SPhP coupled polaritons with a highly propagative character and deeply subwavelength light confinement can be utilized as building blocks for future infrared and terahertz nanophotonic integration and communication devices.

Surface Plasmon-Mediated Nanoscale Localization of Laser-Driven sub-Terahertz Spin Dynamics in Magnetic Dielectrics.

We report spatial localization of the effective magnetic field generated via the inverse Faraday effect employing surface plasmon polaritons (SPPs) at Au/garnet interface. Analyzing both numerically and analytically the electric field of the SPPs at this interface, we corroborate our study with a proof-of-concept experiment showing efficient SPP-driven excitation of coherent spin precession with 0.41 THz frequency. We argue that the subdiffractional confinement of the SPP electric field enables strong spatial localization of the SPP-mediated excitation of spin dynamics. We demonstrate two orders of magnitude enhancement of the excitation efficiency at the surface plasmon resonance within a 100 nm layer of a dielectric garnet. Our findings broaden the horizons of ultrafast spin-plasmonics and open pathways toward nonthermal opto-magnetic recording on the nanoscale.

Femtosecond Spin Current Pulses Generated by the Nonthermal Spin-Dependent Seebeck Effect and Interacting with Ferromagnets in Spin Valves.

Using the sensitivity of optical second harmonic generation to currents, we demonstrate the generation of 250-fs long spin current pulses in Fe/Au/Fe/MgO(001) spin valves. The temporal profile of these pulses indicates ballistic transport of hot electrons across a sub-100 nm Au layer. The pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Considering the calculated spin-dependent Fe/Au interface transmittance we conclude that a nonthermal spin-dependent Seebeck effect is responsible for the generation of ultrashort spin current pulses. The demonstrated rotation of spin polarization of hot electrons upon interaction with noncollinear magnetization at Au/Fe interfaces holds high potential for future spintronic devices.

Nanoscale interface confinement of ultrafast spin transfer torque driving non-uniform spin dynamics.

Spintronics had a widespread impact over the past decades due to transferring information by spin rather than electric currents. Its further development requires miniaturization and reduction of characteristic timescales of spin dynamics combining the sub-nanometre spatial and femtosecond temporal ranges. These demands shift the focus of interest towards the fundamental open question of the interaction of femtosecond spin current (SC) pulses with a ferromagnet (FM). The spatio-temporal properties of the impulsive spin transfer torque exerted by ultrashort SC pulses on the FM open the time domain for probing non-uniform magnetization dynamics. Here we employ laser-generated ultrashort SC pulses for driving ultrafast spin dynamics in FM and analysing its transient local source. Transverse spins injected into FM excite inhomogeneous high-frequency spin dynamics up to 0.6 THz, indicating that the perturbation of the FM magnetization is confined to 2 nm.

Resonant Enhancement of Second-Harmonic Generation in the Mid-Infrared Using Localized Surface Phonon Polaritons in Subdiffractional Nanostructures.

We report on the strong enhancement of mid-infrared second-harmonic generation (SHG) from SiC nanopillars due to the resonant excitation of localized surface phonon polaritons within the Reststrahlen band. A strong dependence of the SHG enhancement upon the optical mode distribution was observed. One such mode, the monopole, exhibits an enhancement that is beyond what is anticipated from field localization and dispersion of the linear and nonlinear SiC optical properties. Comparing the results for the identical nanostructures made of 4H and 6H SiC polytypes, we demonstrate the interplay of localized surface phonon polaritons with zone-folded weak phonon modes of the anisotropic crystal. Tuning the monopole mode in and out of the region where the zone-folded phonon is excited in 6H-SiC, we observe a further prominent increase of the already enhanced SHG output when the two modes are coupled. Envisioning this interplay as one of the showcase features of mid-infrared nonlinear nanophononics, we discuss its prospects for the effective engineering of nonlinear-optical materials with desired properties in the infrared spectral range.

Extended π-conjugated ruthenium zinc-porphyrin complexes with enhanced nonlinear-optical properties.

Zinc porphyrin dimers and trimers, in which the porphyrins are connected via a ruthenium metal core, exhibit large third-order nonlinear optical absorption coefficients and refractive indices. These properties are a result of the presence of multiple porphyrins, which lead to an extension of the π-conjugated system and the octupolar effect.

Ultrafast transport of laser-excited spin-polarized carriers in Au/Fe/MgO(001).

Hot carrier-induced spin dynamics is analyzed in epitaxial Au/Fe/MgO(001) by a time domain approach. We excite a spin current pulse in Fe by 35 fs laser pulses. The transient spin polarization, which is probed at the Au surface by optical second harmonic generation, changes its sign after a few hundred femtoseconds. This is explained by a competition of ballistic and diffusive propagation considering energy-dependent hot carrier relaxation rates. In addition, we observe the decay of the spin polarization within 1 ps, which is associated with the hot carrier spin relaxation time in Au.