arXiv subjects

Tobias Kampfrath

Publications and source records attributed to Tobias Kampfrath.

52 records · Page 3Linked to original sources

arXiv2020

High-throughput techniques for measuring the spin Hall effect

The spin Hall effect in heavy-metal thin films is routinely employed to convert charge currents into transverse spin currents and can be used to exert torque on adjacent ferromagnets. Conversely, the inverse spin Hall effect is frequently used to detect spin currents by charge currents in spintronic devices up to the terahertz frequency range. Numerous techniques to measure the spin Hall effect or its inverse were introduced, most of which require extensive sample preparation by multi-step lithography. To enable rapid screening of materials in terms of charge-to-spin conversion, suitable high-throughput methods for measuring the spin Hall angle are required. Here, we compare two lithography-free techniques, terahertz emission spectroscopy and broadband ferromagnetic resonance, to standard harmonic Hall measurements and theoretical predictions using the binary-alloy series Au$_x$Pt$_{1-x}$ as benchmark system. Despite being highly complementary, we find that all three techniques yield a spin Hall angle with approximately the same $x$~dependence, which is also consistent with first-principles calculations. Quantitative discrepancies are discussed in terms of magnetization orientation and interfacial spin-memory loss.

cond-mat.mes-hall↗

arXiv2020

Phase-resolved Detection of Ultrabroadband THz Pulses inside a Scanning Tunneling Microscope Junction

Coupling phase-stable single-cycle terahertz (THz) pulses to scanning tunneling microscope (STM) junctions enables spatio-temporal imaging with femtosecond temporal and Ångstrom spatial resolution. The time resolution achieved in such THz-gated STM is ultimately limited by the sub-cycle temporal variation of the tip-enhanced THz field acting as an ultrafast voltage pulse, and hence by the ability to feed high-frequency, broadband THz pulses into the junction. Here, we report on the coupling of ultrabroadband (1-30 THz) single-cycle THz pulses from a spintronic THz emitter(STE) into a metallic STM junction. We demonstrate broadband phase-resolved detection of the THz voltage transient directly in the STM junction via THz-field-induced modulation of ultrafast photocurrents. Comparison to the unperturbed far-field THz waveform reveals the antenna response of the STM tip. Despite tip-induced low-pass filtering, frequencies up to 15 THz can be detected in the tip-enhanced near-field, resulting in THz transients with a half-cycle period of 115 fs. We further demonstrate simple polarity control of the THz bias via the STE magnetization, and show that up to 2 V THz bias at 1 MHz repetition rate can be achieved in the current setup. Finally, we find a nearly constant THz voltage and waveform over a wide range of tip-sample distances, which by comparison to numerical simulations confirms the quasi-static nature of the THz pulses. Our results demonstrate the suitability of spintronic THz emitters for ultrafast THz-STM with unprecedented bandwidth of the THz bias, and provide insight into the femtosecond response of defined nanoscale junctions.

physics.app-ph↗

arXiv2020

Energy Transfer within the Hydrogen Bonding Network of Water Following Resonant Terahertz Excitation

Energy dissipation in water is very fast and more efficient than in many other liquids. This behavior is commonly attributed to the intermolecular interactions associated with hydrogen bonding. Here, we investigate the dynamic energy flow in the hydrogen-bond network of liquid water by a pump-probe experiment. We resonantly excite intermolecular degrees of freedom with ultrashort single-cycle terahertz pulses and monitor its Raman response. By using ultrathin sample-cell windows, a background-free bipolar signal whose tail relaxes mono-exponentially is obtained. The relaxation is attributed to the molecular translational motions, using complementary experiments, force-field and ab initio molecular dynamics simulations. They reveal an initial coupling of the terahertz electric field to the molecular rotational degrees of freedom whose energy is rapidly transferred, within the excitation pulse duration, to the restricted-translational motion of neighboring molecules. This rapid energy transfer may be rationalized by the strong anharmonicity of the intermolecular interactions.

cond-mat.soft↗

arXiv2018

Terahertz spectroscopy for all-optical spintronic characterization of the spin-Hall-effect metals Pt, W and Cu$_{80}$Ir$_{20}$

Identifying materials with an efficient spin-to-charge conversion is crucial for future spintronic applications. The spin Hall effect is a central mechanism as it allows for the interconversion of spin and charge currents. Spintronic material research aims at maximizing its efficiency, quantified by the spin Hall angle $Θ_{\textrm{SH}}$ and the spin-current relaxation length $λ_{\textrm{rel}}$. We develop an all-optical method with large sample throughput that allows us to extract $Θ_{\textrm{SH}}$ and $λ_{\textrm{rel}}$. Employing terahertz spectroscopy, we characterize magnetic metallic heterostructures involving Pt, W and Cu$_{80}$Ir$_{20}$ in terms of their optical and spintronic properties. We furthermore find indications that the interface plays a minor role for the spin-current transmission. Our analytical model is validated by the good agreement with literature DC values. These findings establish terahertz emission spectroscopy as a reliable tool complementing the spintronics workbench.

cond-mat.mtrl-sci↗

arXiv2018

Dissecting spin-phonon equilibration in ferrimagnetic insulators by ultrafast lattice excitation

To gain control over magnetic order on ultrafast time scales, a fundamental understanding of the way electron spins interact with the surrounding crystal lattice is required. However, measurement and analysis even of basic collective processes such as spin-phonon equilibration have remained challenging. Here, we directly probe the flow of energy and angular momentum in the model insulating ferrimagnet yttrium iron garnet. Following ultrafast resonant lattice excitation, we observe that magnetic order reduces on distinct time scales of 1 ps and 100 ns. Temperature-dependent measurements, a spin-coupling analysis and simulations show that the two dynamics directly reflect two stages of spin-lattice equilibration. On the 1-ps scale, spins and phonons reach quasi-equilibrium in terms of energy through phonon-induced modulation of the exchange interaction. This mechanism leads to identical demagnetization of the ferrimagnet's two spin-sublattices and a novel ferrimagnetic state of increased temperature yet unchanged total magnetization. Finally, on the much slower, 100-ns scale, the excess of spin angular momentum is released to the crystal lattice, resulting in full equilibrium. Our findings are relevant for all insulating ferrimagnets and indicate that spin manipulation by phonons, including the spin Seebeck effect, can be extended to antiferromagnets and into the terahertz frequency range.

cond-mat.mtrl-sci↗

arXiv2017

Experimentally Probing the Libration of Interfacial Water: the Rotational Potential of Water is Stiffer at the Air/Water Interface than in Bulk Liquid

Most properties of liquid water are determined by its hydrogen-bond network. Because forming an aqueous interface requires termination of this network, one might expect the molecular level properties of interfacial water to markedly differ from water in bulk. Intriguingly, much prior experimental and theoretical work has found that, from the perspective of their time-averaged structure and picosecond structural dynamics, hydrogen-bonded OH groups at an air/water interface behave the same as hydrogen-bonded OH groups in bulk liquid water. Here we report the first experimental observation of interfacial water's libration (i.e. frustrated rotation) using the laser-based technique vibrational sum frequency spectroscopy. We find this mode has a frequency of 834 cm$^{-1}$, $\approx 165$ cm$^{-1}$ higher than in bulk liquid water at the same temperature and similar to bulk ice. Because libration frequency is proportional to the stiffness of water's rotational potential, this increase suggests that one effect of terminating bulk water's hydrogen bonding network at the air/water interface is retarding rotation of water around intact hydrogen bonds. Because in bulk liquid water the libration plays a key role in stabilizing reaction intermediates and dissipating excess vibrational energy, we expect the ability to probe this mode in interfacial water to open new perspectives on the kinetics of heterogeneous reactions at aqueous interfaces.

physics.chem-ph↗

arXiv2017

Complex THz and DC inverse spin Hall effect in YIG/Cu$_{1-x}$Ir$_{x}$ bilayers across a wide concentration range

We measure the inverse spin Hall effect of Cu$_{1-x}$Ir$_{x}$ thin films on yttrium iron garnet over a wide range of Ir concentrations ($0.05 \leqslant x \leqslant 0.7$). Spin currents are triggered through the spin Seebeck effect, either by a DC temperature gradient or by ultrafast optical heating of the metal layer. The spin Hall current is detected by, respectively, electrical contacts or measurement of the emitted THz radiation. With both approaches, we reveal the same Ir concentration dependence that follows a novel complex, non-monotonous behavior as compared to previous studies. For small Ir concentrations a signal minimum is observed, while a pronounced maximum appears near the equiatomic composition. We identify this behavior as originating from the interplay of different spin Hall mechanisms as well as a concentration-dependent variation of the integrated spin current density in Cu$_{1-x}$Ir$_{x}$. The coinciding results obtained for DC and ultrafast stimuli show that the studied material allows for efficient spin-to-charge conversion even on ultrafast timescales, thus enabling a transfer of established spintronic measurement schemes into the terahertz regime.

cond-mat.mtrl-sci↗

arXiv2017

Anharmonic Coupling between Intermolecular Motions of Water Revealed by Terahertz Kerr Effect

Formation of local molecular structures in liquid water is believed to have marked effect on the bulk properties of water, however, resolving such structural motives in an experiment is challenging. This challenge might be handled if the relevant low-frequency structural motion of the liquid is directly driven with an intense electromagnetic pulse. Here, we resonantly excite diffusive reorientational motions in water with intense terahertz pulses and measure the resulting transient optical birefringence. The observed response is shown to arise from a particular configuration, namely the restricted trans-lational motion of water molecules whose motions are predominantly orthogonal to the dipole moment of the excited neighboring water molecules. Accordingly, we estimate the strength of the anharmonic coupling between the rotational and the restricted translational degrees of freedom of water.

cond-mat.soft↗

arXiv2017

The sign of the polarizability anisotropy of polar molecules is obtained faithfully from terahertz Kerr effect

Optically heterodyned detected terahertz Kerr effect of gases of polar molecules is reported. Strikingly, the birefringence signal from fluoroform is found to have opposite polarity compared to water and acetonitrile. This behavior is a hallmark of the opposite sign of the polarizability anisotropy of these molecules. Resonant excitation of the rotational degrees of freedom of the molecules aligns their permanent dipoles along the terahertz electric field. This alignment is translated into an optical birefringence through the polarizability anisotropy of each molecule. Therefore, the resulting net signal scales with the polarizability anisotropy, whose sign is imprinted faithfully onto the transient birefringence signal.

physics.optics↗

arXiv2017

Terahertz sum-frequency excitation of a Raman-active phonon

In stimulated Raman scattering, two incident optical waves induce a force oscillating at the difference of the two light frequencies. This process has enabled important applications such as the excitation and coherent control of phonons and magnons by femtosecond laser pulses. Here, we experimentally and theoretically demonstrate the so far neglected up-conversion counterpart of this process: THz sum-frequency excitation of a Raman-active phonon mode, which is tantamount to two-photon absorption by an optical transition between two adjacent vibrational levels. Coherent control of an optical lattice vibration of diamond is achieved by an intense terahertz pulse whose spectrum is centered at half the phonon frequency of 40 THz. Remarkably, the carrier-envelope phase of the driving pulse is directly imprinted on the lattice vibration. New prospects in infrared spectroscopy, light storage schemes and lattice trajectory control in the electronic ground state emerge.

cond-mat.mtrl-sci↗

arXiv2016

Transient birefringence of liquids induced by terahertz electric-field torque on permanent molecular dipoles

Microscopic understanding of low-frequency molecular motions in liquids has been a longstanding goal in soft-matter science. So far, such low-frequency motions have mostly been accessed indirectly by off-resonant optical pulses. A more direct approach would be to interrogate the dynamic structure of liquids with terahertz (THz) radiation. Here, we provide evidence that resonant excitation with intense THz pulses is capable of driving reorientational-librational modes of aprotic polar liquids through coupling to the permanent molecular dipole moments. We observe a hallmark of this enhanced coupling: a transient optical birefringence up to an order of magnitude higher than obtained with optical excitation. Our results open up the path to applications such as efficient molecular alignment and systematic study of the coupling of rotational motion to other collective motions in liquids.

cond-mat.soft↗

arXiv2015

Ultrafast photocurrents at the surface of the three-dimensional topological insulator $\mathrm{Bi}_2\mathrm{Se}_3$

Topological insulators constitute a new and fascinating class of matter with insulating bulk yet metallic surfaces that host highly mobile charge carriers with spin-momentum locking. Remarkably, the direction and magnitude of surface currents can be controlled with tailored light beams, but the underlying mechanisms are not yet well understood. To directly resolve the "birth" of such photocurrents we need to boost the time resolution to the scale of elementary scattering events ($\sim$ 10 fs). Here, we excite and measure photocurrents in the three-dimensional model topological insulator $\mathrm{Bi}_2\mathrm{Se}_3$ with a time resolution as short as 20 fs by sampling the concomitantly emitted broadband THz electromagnetic field from 1 to 40 THz. Remarkably, the ultrafast surface current response is dominated by a charge transfer along the Se-Bi bonds. In contrast, photon-helicity-dependent photocurrents are found to have orders of magnitude smaller magnitude than expected from generation scenarios based on asymmetric depopulation of the Dirac cone. Our findings are also of direct relevance for optoelectronic devices based on topological-insulator surface currents.

cond-mat.mtrl-sci↗

arXiv2013

Sub-cycle control of terahertz waveform polarization using all-optically induced transient metamaterials

Coherent radiation with frequencies ranging from 0.3 to 30 THz has recently become accessible by femtosecond laser technology. Terahertz (THz) waves have already found many applications in spectroscopy and imaging, and they can be manipulated using static optical elements such as lenses, polarizers, and filters. However, ultrafast modulation of THz radiation is required as well, for instance in short-range wireless communication or for preparing shaped THz transients for coherent control of numerous material excitations. Here, we demonstrate an all-optically created transient metamaterial that permits to manipulate the polarization of THz waveforms with sub-cycle precision. The polarization-modulated pulses are potentially interesting for controlling elementary motions such as vibrations of crystal lattices, rotations of molecules, and the precession of spins.

physics.optics↗

arXiv2012

Ultrafast tuneable optical delay line based on indirect photonic transitions

We introduce the concept of an indirect photonic transition and demonstrate its use in a dynamic delay line to alter the group velocity of an optical pulse. Operating on an ultrafast time scale, we show continuously tuneable delays of up to 20 ps, using a slow light photonic crystal waveguide only 300 $μ$m in length. Our approach is flexible, in that individual pulses in a pulse stream can be controlled independently, which we demonstrate by operating on pulses separated by just 30 ps. The two-step indirect transition is demonstrated here with a 30% conversion efficiency.

physics.optics↗

arXiv2012

Ultrafast tilting of the dispersion of a photonic crystal and adiabatic spectral compression of light pulses

We demonstrate, by theory and experiment, the ultrafast tilting of the dispersion curve of a photonic-crystal waveguide following the absorption of a femtosecond pump pulse. By shaping the pump-beam cross section with a nanometric shadow mask, different waveguide eigenmodes acquire different spatial overlap with the perturbing pump, leading to a local flattening of the dispersion by up to 11 %. We find that such partial mode perturbation can be used to adiabatically compress the spectrum of a light pulse traveling through the waveguide.

physics.optics↗

arXiv2009

Active control of light trapping by means of local magnetic coupling.pdf

The ability to actively tune the properties of a nanocavity is crucial for future applications in photonics and quantum information. Two important man-made classes of materials have emerged to mold the flow of electromagnetic waves. Firstly, photonic crystals are dielectric nanostructures that can be used to confine and slow down light and control its emission. They act primarily on the electric component of the light field. More recently, a novel class of metallo-dielectric nanostructures has emerged. These so-called metamaterials enable fascinating phenomena, such as negative refraction, super-focusing and cloaking. This second class of materials realizes light control through effective interactions with both electric and magnetic component. In this work, we combine both concepts to gain an active and reversible control of light trapping on subwavelength length scales. By actuating a nanoscale magnetic coil close to a photonic crystal nanocavity, we interact with the rapidly varying magnetic field and accomplish an unprecedented control of the optical properties of the cavity. We achieve a reversible enhancement of the lifetime of photons in the cavity. By successfully combining photonic crystal and metamaterials concepts, our results open the way for new light control strategies based on interactions which include the magnetic component of light.

physics.optics↗