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Tobias Kampfrath

Publications and source records attributed to Tobias Kampfrath.

At least 19 recordsLinked to original sources

Modified Low-Temperature Scanning Tunneling Microscope for Ultrafast Pump-Probe Spectroscopy

Combining scanning tunneling microscopy (STM) with terahertz pulses (THz-STM) enables ultrafast dynamics of phonons, spins, and charge carriers to be probed with atomic-scale spatial and sub-picosecond temporal resolution. However, coupling THz radiation into a low-temperature STM junction presents some technical challenges as it requires optical access for laser illumination while maintaining junction stability. Instead of designing a completely new STM head with customized optical access and optics within the ultra-high vacuum chamber, we modified a Besocke "Beetle" style STM with minimal changes of the cryogenic radiation shields. Despite the given geometrical conditions, we achieved efficient coupling of THz and optical pulses to the STM junction while maintaining temperatures below 6 K. We designed the optical setup on a separate laser table, starting with femtosecond laser pulses that are used to generate THz pulses in a LiNbO$_3$ crystal. We show the obtained THz pulse shapes and determine the effective time resolution using cross-correlation measurements. We further demonstrate the stable performance of the modified STM by measuring THz-induced tunneling currents from monolayer molybdenum disulfide (MoS$_2$) grown on Au(111). The resulting current maps resolve atomic-scale contrast revealing a point defect. The measurements confirm efficient THz coupling and stable low-temperature STM operation with atomic resolution.

cond-mat.mes-hall

Terahertz magneto-photocurrents in the topological insulator Bi$_2$Se$_3$ probe its topological surface states

We study ultrafast magneto-photocurrents in a three-dimensional topological insulator. For this purpose, we excite (In$_r$Bi$_{1-r}$)$_2$Se$_3$ thin films with a femtosecond laser pulse in the presence of an external magnetic field $B_{\text{ext}}$ up to 0.3 T parallel to the film plane. The resulting in-plane photocurrent is measured by detecting the emitted terahertz (THz) electromagnetic pulse. It scales linearly with $B_{\text{ext}}$ and is perpendicular to $B_{\text{ext}}$. Strikingly, for $r\ge$4%, we observe an abrupt photocurrent reduction, which is strongly correlated with the Indium-induced quenching of the topological surface states. The rise time, decay time and amplitude of the THz magneto-photocurrent can consistently be explained by a scenario in which optically excited spin-polarized electrons propagate toward the film surface where the accumulated spin is converted into an in-plane charge current due to spin-velocity locking. Our results are highly relevant for contact-free probing of spin-charge conversion in systems with paramagnetic rather than spontaneous magnetic order.

cond-mat.mes-hall

Terahertz switching of antiferromagnetic order by Néel spin-orbit torques

Ultrafast electric manipulation of magnetic order in solids is critical for the development of future terahertz data processing. A fascinating concept for such high-speed operation is offered in metallic antiferromagnets by Néel spin-orbit torque. It should allow one to coherently rotate the ordered spins by simply applying an electric current of suitable amplitude and polarity. However, such switching has been severely hampered by competing heat-induced effects, and it has not yet been achieved on the intrinsically ultrafast time scales of antiferromagnets. Here, we report robust, direction-controlled and non-thermal rotation of the Néel vector $\mathbf{L}$ by $\pm$90° at room temperature in the antiferromagnet Mn$_2$Au driven by phase-locked terahertz current pulses. All observed features are consistent with ultrafast Néel spin-orbit torque: First, nonlinear optical imaging reveals that the terahertz current direction sets the final orientation of $\mathbf{L}$ in the absence of any bias field for at least two months. Second, transient optical birefringence shows that the switching proceeds ultrafast in less than 15 picoseconds. Finally, atomistic spin-dynamics simulations reproduce the observed dynamics and confirm the minor role of thermal effects. While the switching is already one order of magnitude faster than in ferromagnets at comparable dissipated energy, our simulations predict routes toward switching times and energies which are another order of magnitude lower. Our approach can be transferred to electric-field-driven switching in many more antiferromagnets, including magnetoelectric insulators. The engineering of spin torques, resonance frequencies and read-out mechanisms provides an exciting pathway toward on-chip applications of terahertz antiferromagnetic spin-orbitronics.

cond-mat.mes-hall

Influence of atomic-scale defects on coherent phonon excitations by THz near fields in an STM

Coherent phonons describe the collective, ultrafast motion of atoms and play a central role in light-induced structural dynamics. Here, we employ terahertz scanning tunneling microscopy (THz-STM) to excite and detect coherent phonons in semiconducting 2H-$MoTe_{2}$ and resolve how their excitation is influenced by atomic-scale defects. In a THz pump-probe scheme, we observe long-lived oscillatory signals that we assign to out-of-plane breathing and in-plane shear modes, which are both forbidden in the bulk. Remarkably, the relative excitation strength of these modes varies near defects, indicating that local band bending modulates the coupling to the THz field. This defect-tunable coupling offers new opportunities to control material properties via selective excitation of vibrational modes at the nanoscale.

cond-mat.mes-hall

Broad-band THz emission by Spin-to-Charge Conversion in Topological Material -- Ferromagnet Heterostructures

Terahertz spintronic devices combine ultrafast operation with low power consumption, making them strong candidates for next-generation memory technologies. In this study, we use time-domain terahertz emission spectroscopy to investigate spin-to-charge conversion (SCC) in bilayer heterostructures comprising topological insulators (TIs) or Weyl semimetals (WSMs) with ferromagnetic metals (FMs). SCC is studied in TI materials \ce{Bi2Se3}, Pb-doped \ce{Bi2Se3}, and (Bi$_{1-x}$Sb$_x$)$_2$Te$_3$, and the WSM NbP. Our results reveal that the dependence of SCC on TI thickness varies with interface quality, indicating that thickness dependence alone is not a reliable criterion for distinguishing between inverse spin Hall effect and the inverse Rashba--Edelstein effect mechanisms. We find efficient SCC in TIs depends on both \textit{in-situ} growth to prevent surface oxidation and proper composition. In NbP$\vert$FM bilayers, we observe THz emission with efficiency and bandwidth comparable to that of TIs, highlighting the broader potential of topological materials. Finally, broadband spectral measurements demonstrate that both TIs and WSMs can generate THz pulses with frequencies extending up to 8\,THz. These findings underscore the promise of topological materials as efficient platforms for ultrafast, broadband spintronic applications.

cond-mat.mtrl-sci

Femtosecond signatures of optically induced magnons before ultrafast demagnetization

Optically induced demagnetization of 3d metallic ferromagnets proceeds as fast as ~100 fs and is a crucial prerequisite for spintronic applications, such as ultrafast magnetization switching and spin transport. On the 100 fs time scale, the magnetization dynamics is widely understood in the context of temperature models considering energy transfers between conduction electrons, magnons and crystal lattice. However, on even faster time scales, the flow of both angular momentum and energy between these subsystems has so far not been studied. Here, we measure ultrafast demagnetization by ultrabroadband THz-emission spectroscopy. We find that the rate of change of the magnetization does not rise instantaneously, but on a time scale as short as 10 fs. This rise is a signature that a transfer of angular momentum from the magnons to conduction electrons proceeds in less than 10 fs, before substantial demagnetization has happened. We further conclude that most of the spin dissipated by the lattice is transferred via magnon-lattice rather than electron-lattice interaction. These results show that the limiting speed of magnetization dynamics is not demagnetization, as generally believed, and harnessing the earliest magnon dynamics could be a new route towards an even faster spintronics.

cond-mat.mes-hall

Femtosecond photocurrents by the Dresselhaus bulk spin-galvanic effect in an inversion-asymmetric ferromagnet

We study ultrafast photocurrents in thin films of a model ferromagnetic metal with broken bulk inversion symmetry, the half-metallic Heusler compound NiMnSb, following excitation with an optical pump pulse with photon energy 1.55 eV. Remarkably, in terms of the direction of the sample magnetization M, all photocurrents are found to be a superposition of a component with Rashba- and Dresselhaus-type symmetry. We explain the Dresselhaus bulk photocurrent as follows: Pump-induced electron heating induces an excess of spin μ_s||M, which transfers spin angular momentum into states with Dresselhaus-type spin-momentum locking. The resulting charge current relaxes on a time scale of 10 fs by momentum relaxation and, thus, follows μ_s quasi-instantaneously. The relaxation of μ_s is governed by the cooling of the electrons and not by the significantly slower spin-lattice relaxation of half-metals. Our findings add the Dresselhaus spin-galvanic effect (SGE) to the set of ultrafast spin-charge-conversion phenomena. They indicate a route to more efficient spintronic terahertz emitters and detectors based on the volume scaling of the bulk SGE.

cond-mat.mtrl-sci

Ultrafast electron heating as the dominant driving force of photoinduced terahertz spin currents

Ultrafast spintronics strongly relies on the generation, transport, manipulation and detection of terahertz spin currents (TSCs). In F|HM stacks consisting of a ferromagnetic layer F and a heavy-metal layer HM, ultrafast spin currents are typically triggered by femtosecond optical laser pulses. A key open question is whether the initial step, optical excitation and injection of spin currents, can be controlled by tuning the photon energy of the femtosecond pulse. While many theoretical works suggest a marked impact of photon-energy and of highly excited non-thermal electrons, profound experimental evidence is lacking. Here, we use terahertz-emission spectroscopy to study TSCs triggered with two different photon energies of 1.5 eV and 3 eV. We study a wide range of magnetic systems covering metallic ferromagnets, ferrimagnetic insulators, half-metals, as well as systems including tunneling barriers, and rare-earth metallic alloys. We find that variation of the exciting photon energy does not change the dynamics and only slightly the amplitude of the induced TSC in all sample systems. Our results reveal that the ultrafast pump-induced heating of electrons is a highly efficient process for generating TSCs, whereas highly excited primary photoelectrons are of minor importance.

cond-mat.mes-hall

Terahertz time-domain signatures of the inverse Edelstein effect in topological-insulator|ferromagnet heterostructures

Three-dimensional topological insulators possess topologically protected surface states with spin-momentum locking, which enable spin-charge-current interconversion (SCI) by the inverse Edelstein effect (IEE). However, it remains experimentally challenging to separate the surface-related IEE from the bulk-type inverse spin Hall effect (ISHE). Here, we search for distinct time-domain signatures of the two SCI phenomena in a $\mathcal{F}$|TI model stack of a ferromagnetic-metal layer $\mathcal{F}$ (Co and Fe) and a topological-insulator layer TI (Bi$_2$Te$_3$, SnBi$_2$Te$_4$ and Bi$_{1-x}$Sb$_x$ with $x$ = 0.15 and 0.3), where the focus is on Bi$_2$Te$_3$. A femtosecond laser pulse serves to induce a transient spin voltage $μ_s^{\mathcal{F}}$ in $\mathcal{F}$ and, thus, drive an ultrafast spin current out of $\mathcal{F}$. SCI results in a transverse charge current with a sheet density $I_c$ that is detected by sampling the emitted terahertz electric field. Analysis of the dynamics of $I_c(t)$ vs time $t$ relative to $μ_s^{\mathcal{F}}(t)$ reveals two components with distinct time scales: (i) a quasi-instantaneous response and (ii) a longer-lived response with a relaxation time of 270 fs, which is independent of the chosen $\mathcal{F}$ material. Component (i) is consistently ascribed to the ISHE. In contrast, we interpret component (ii) as a signature of interfacial spin accumulation and the IEE at the $\mathcal{F}$/Bi$_2$Te$_3$ interface, with a fraction of $< 10^{-2}$ of the incident spins participating. This assignment is fully consistent with respect to its dynamics and magnitude. We rate other possible signal contributions, such as spin trapping in intermediate states, as less likely. Our results show that the femtosecond dynamics of photocurrents provide important insights into the mechanisms of spin transport and SCI in $\mathcal{F}$|TI stacks.

cond-mat.mes-hall

Local and Global Reciprocity in Orbital-Charge-Coupled Transport

The coupled transport of charge and orbital angular momentum (OAM) lies at the core of orbitronics. Here, we examine the reciprocal relation in orbital-charge-coupled transport in thin films, treating bulk and surface contributions on equal footing. We argue that the conventional definition of orbital current is ill-defiled, as it violates reciprocity due to the nonconservation of OAM. This issue is resolved by adopting the so-called \emph{proper} orbital current, which is directly linked to orbital accumulation. We establish the reciprocal relation for the \emph{global} (spatially integrated) response between orbital and charge currents, while showing that their \emph{local} (spatially resolved) responses can differ significantly. In particular, we find large surface contributions that may lead to nonreciprocity when currents are measured locally. These findings are supported by first-principles calculations on W(110) and Pt(111) thin films. In W(110), orbital-charge interconversion is strongly nonreciprocal at the layer level, despite exact reciprocity in the integrated response. Interestingly, spin-charge interconversion in W(110) remains nearly reciprocal even locally. In contrast, Pt(111) exhibits local nonreciprocity for both orbital-charge and spin-charge conversions, which we attribute to strong spin-orbit coupling. We propose that such local distinctions can be exploited to experimentally differentiate spin and orbital currents.

cond-mat.mes-hall

Hallmarks of terahertz magnon currents in an antiferromagnetic insulator

The efficient transport of spin angular momentum is expected to play a crucial role in future spintronic devices, which potentially operate at frequencies reaching the terahertz range. Antiferromagnetic insulators exhibit significant potential for facilitating ultrafast pure spin currents by terahertz magnons. Consequently, we here use femtosecond laser pulses to trigger ultrafast spin currents across antiferromagnetic NiO thin films in Py|NiO|Pt stacks, where permalloy (Py) and Pt serve as spin-current source and detector respectively. We find that the spin current pulses traversing NiO reach a velocity up to 40 nm/ps and experience increasing delay and broadening as the NiO thickness is increased. We can consistently explain our observations by ballistic transport of incoherent magnon. Our approach has high potential to characterize terahertz magnon transport in magnetic insulators with any kind of magnetic order.

cond-mat.mes-hall

Magnon-mediated terahertz spin transport in metallic Gd|Pt stacks

We study femtosecond spin transport in a Gd|Pt stack induced by a laser pulse. Remarkably, the dynamics of the spin current from Gd to Pt suggests that its dominant driving force is the ultrafast spin Seebeck effect. As the contribution of a transient spin voltage in the metal Gd is minor, Gd acts akin a magnetic insulator here. This view is supported by time- and spin-resolved photoemission, which indicates that a buildup of spin voltage is suppressed by exchange scattering, leading to similar amplitudes and relaxation rates of hot majority- and minority-spin electron populations.

cond-mat.mes-hall

Accessing ultrafast spin-transport dynamics in copper using broadband terahertz spectroscopy

We study the spatiotemporal dynamics of ultrafast electron spin transport across nanometer-thick copper layers using broadband terahertz spectroscopy. Our analysis of temporal delays, broadening and attenuation of the spin-current pulse revealed ballistic-like propagation of the pulse peak, approaching the Fermi velocity, and diffusive features including a significant velocity dispersion. A comparison to the frequency-dependent Ficks law identified the diffusion-dominated transport regime for distances larger than 2 nm. The findings lie the groundwork for designing future broadband spintronic devices.

cond-mat.mes-hall

All-optical magnetometric characterization of the antiferromagnetic exchange-spring system Mn$_2$Au|Py by terahertz spin-torques

Antiferromagnetic materials have great potential for spintronic applications at terahertz (THz) frequencies. However, in contrast to ferromagnets, experimental studies of antiferromagnets are often challenging due to a lack of straightforward external control of the Néel vector $\mathbf{L}$. Here, we study an AFM|FM stack consisting of an antiferromagnetic metal layer (AFM) of the novel material Mn2Au and a ferromagnetic metal layer (FM) of NiFe. In this exchange-spring system, $\mathbf{L}$ of AFM Mn2Au can be controlled by the application of an external magnetic field B_ext. To characterize the AFM|FM stack as a function of the quasi-static $\mathbf{B}_{\mathrm{ext}}$, we perform THz-pump magneto-optic probe experiments. We identify signal components that can consistently be explained by the in-plane antiferromagnetic magnon mode excited by field-like Néel spin-orbit torques (NSOTs). Remarkably, we find that the $\mathbf{B}_{\mathrm{ext}}$- and THz-pump-induced changes in the optical response of the sample are dominated exclusively by the spin degrees of freedom of AFM. We fully calibrate the magnetic circular and magnetic linear optical birefringence of AFM and extract the efficiency of the NSOTs. Finally, by selective excitation of domains with different orientation of $\mathbf{L}$, we are able to determine the relative volume fraction of 0°, 90°, 180° and 270° domains distribution during the quasi-static reversal of $\mathbf{L}$ by $\mathbf{B}_{\mathrm{ext}}$. Our insights are an important prerequisite for future studies of ultrafast coherent switching of spins by THz NSOTs and show that THz-pump magneto-optic-probe experiments are a powerful tool to characterize magnetic properties of antiferromagnets.

cond-mat.mes-hall

Rotating spintronic terahertz emitter optimized for microjoule pump-pulse energies and megahertz repetition rates

Spintronic terahertz emitters (STEs) are powerful sources of ultra-broadband single-cycle terahertz (THz) field transients. They work with any pump wavelength, and their polarity and polarization direction are easily adjustable. However, at high pump powers and high repetition rates, STE operation is hampered by a significant increase in the local temperature. Here, we resolve this issue by rotating the STE at a few 100 Hz, thereby distributing the absorbed pump power over a larger area. Our approach permits stable STE operation at a fluence of ~1 mJ/cm$^2$ with up to 18 W pump power at megahertz repetition rates, corresponding to pump-pulse energies of a few 10 $μ$J and a power density far above the melting threshold of metallic films. The rotating STE is of interest for all ultra-broadband high-power THz applications requiring high repetition rates. As an example, we show that THz pulses with peak fields of 10 kV/cm can be coupled to a THz-lightwave-driven scanning tunneling microscope at 1 MHz repetition rate, demonstrating that the rotating STE can compete with standard THz sources such as LiNbO$_3$.

physics.optics

Radiation hardness of ultrabroadband spintronic terahertz emitters: en-route to a space-qualified terahertz time-domain gas spectrometer

The radiation hardness of ultrabroadband, spintronic terahertz emitters against gamma and proton irradiation is investigated. We find that irradiation doses equivalent to those experienced by a space instrument en-route to and operated on Mars have a minor effect on the performance of the emitter. In particular, the ultrawide emission spectrum 0.1-30 THz, which covers a large part of the vibrational fingerprint region, remains unchanged. These results make this emitter type highly interesting as essential building block for broad-band gas sensors based on terahertz time-domain spectroscopy for future space missions.

physics.ins-det

Quartz as an Accurate High-Field Low-Cost THz Helicity Detector

The advent of high-field THz sources has opened the field of nonlinear THz physics and unlocked access to fundamental low energy excitations for ultrafast material control. Recent advances towards controlling and employing chiral excitations, or generally angular momentum of light, not only rely on the measurement of undistorted intense THz fields, but also on the precise knowledge about sophisticated THz helicity states. A recently reported and promising detector material is $α$-quartz. However, its electrooptic response function and contributing nonlinear effects have remained elusive. Here, we establish z-cut $α$-quartz as a precise electrooptic THz detector for full amplitude, phase and polarization measurement of intense THz fields, all at a fraction of costs of conventional THz detectors. We experimentally determine its complex detector response function, which is in good agreement with our model based on predominantly known literature values. It also explains previously observed thickness-dependent waveforms. These insights allow us to develop a swift and reliable protocol to precisely measure arbitrary THz polarization and helicity states. This two-dimensional electrooptic sampling (2D-EOS) in $α$-quartz fosters rapid and cost-efficient THz time-domain ellipsometry, and enables the characterization of polarization-tailored fields for driving chiral or other helicity-sensitive quasiparticles and topologies.

physics.optics

Shaping THz emission spectra by using sub-wavelength nanopatterned spintronic THz emitters

We show in theory and experiment that in periodically patterned spintronic THz emitters (STE), charge dynamics can modify the emission spectrum in a well-controlled way. Characterization of sub-wavelength patterned STE at frequencies up to 30 THz shows that the STE's emission spectrum systematically changes with emitter size. The spectral intensity exhibits significant reductions at frequencies below 4 THz, accompanied by pronounced dips at around 15 THz and 24 THz. While reducing the STE size enhances the modulation of all features, it does not alter the dip frequencies. The effect originates from the charging of the structure's edges by THz currents, causing a backflow that interferes with the primary current pulse. An analytical model quantitatively reproduces these results and agrees well with control experiments. Our findings enable a detailed investigation of the charge dynamics in STE and provide additional means for controlled shaping of STE emission spectra by nano patterning.

physics.app-ph