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Funder: Alexander von Humboldt Foundation, Funder: Experienced Researcher Fellowship, Funder: DFG Collaborative, Funder: PAPIIT, Funder: Danish National Research Foundation, Funder: JSPS, Funder: STFC Centre for Instrumentation, Funder: UKSA Centre for Earth, Funder: Leverhulme Trust; doi: http://dx.doi.org/10.13039/501100000275, Funder: NRF, Funder: Royal Society; doi: http://dx.doi.org/10.13039/501100000288, Funder: Australian Government; doi: http://dx.doi.org/10.13039/100015539, Funder: Cancer Research UK; doi: http://dx.doi.org/10.13039/501100000289, Funder: University of Warwick; doi: http://dx.doi.org/10.13039/501100000741, Terahertz (THz) radiation encompasses a wide spectral range within the electromagnetic spectrum that extends from microwaves to the far infrared (100 GHz–∼30 THz). Within its frequency boundaries exist a broad variety of scientific disciplines that have presented, and continue to present, technical challenges to researchers. During the past 50 years, for instance, the demands of the scientific community have substantially evolved and with a need for advanced instrumentation to support radio astronomy, Earth observation, weather forecasting, security imaging, telecommunications, non-destructive device testing and much more. Furthermore, applications have required an emergence of technology from the laboratory environment to production-scale supply and in-the-field deployments ranging from harsh ground-based locations to deep space. In addressing these requirements, the research and development community has advanced related technology and bridged the transition between electronics and photonics that high frequency operation demands. The multidisciplinary nature of THz work was our stimulus for creating the 2017 THz Science and Technology Roadmap (Dhillon et al 2017 J. Phys. D: Appl. Phys. 50 043001). As one might envisage, though, there remains much to explore both scientifically and technically and the field has continued to develop and expand rapidly. It is timely, therefore, to revise our previous roadmap and in this 2023 version we both provide an update on key developments in established technical areas that have important scientific and public benefit, and highlight new and emerging areas that show particular promise. The developments that we describe thus span from fundamental scientific research, such as THz astronomy and the emergent area of THz quantum optics, to highly applied and commercially and societally impactful subjects that include 6G THz communications, medical imaging, and climate monitoring and prediction. Our Roadmap vision draws upon the expertise and perspective of multiple international specialists that together provide an overview of past developments and the likely challenges facing the field of THz science and technology in future decades. The document is written in a form that is accessible to policy makers who wish to gain an overview of the current state of the THz art, and for the non-specialist and curious who wish to understand available technology and challenges. A such, our experts deliver a ‘snapshot’ introduction to the current status of the field and provide suggestions for exciting future technical development directions. Ultimately, we intend the Roadmap to portray the advantages and benefits of the THz domain and to stimulate further exploration of the field in support of scientific research and commercial realisation.

Spintronic terahertz emitters are broadband and efficient sources of terahertz radiation, which emerged at the intersection of ultrafast spintronics and terahertz photonics. They are based on efficient spin-current generation, spin-to-charge-current conversion, and current-to-field conversion at terahertz rates. In this Editorial, we review the recent developments and applications, the current understanding of the physical processes, and the future challenges and perspectives of broadband spintronic terahertz emitters.

A material’s magnetic state and its dynamics are of great fundamental research interest and are also at the core of a wide plethora of modern technologies. However, reliable access to magnetization dynamics in materials and devices on the technologically relevant ultrafast timescale, and under realistic device-operation conditions, remains a challenge. Here, we demonstrate a method of ultrafast terahertz (THz) magnetometry, which gives direct access to the (sub-)picosecond magnetization dynamics even in encapsulated materials or devices in a contact-free fashion, in a fully calibrated manner, and under ambient conditions. As a showcase for this powerful method, we measure the ultrafast magnetization dynamics in a laser-excited encapsulated iron film. Our measurements reveal and disentangle distinct contributions originating from (i) incoherent hot-magnon-driven magnetization quenching and (ii) coherent acoustically-driven modulation of the exchange interaction in iron, paving the way to technologies utilizing ultrafast heat-free control of magnetism. High sensitivity and relative ease of experimental arrangement highlight the promise of ultrafast THz magnetometry for both fundamental studies and the technological applications of magnetism., Nature Communications, 11 (1), ISSN:2041-1723

Magnetic Weyl semimetals are an emerging material class that combines magnetic order and a topologically non-trivial band structure. Here, we study ultrafast optically driven spin injection from thin films of the magnetic Weyl semimetals Co2MnGa and Co2MnAl into an adjacent Pt layer by means of terahertz emission spectroscopy. We find that (i) Co2MnGa and Co2MnAl are efficient terahertz spin-current generators reaching efficiencies of typical 3d-transition-metal ferromagnets such as Fe. (ii) The relaxation of the spin current provides an estimate of the electron-spin relaxation time of Co2MnGa (170 fs) and Co2MnAl (100 fs), which is comparable to Fe (90 fs). Both observations are consistent with a simple analytical model and highlight the large potential of magnetic Weyl semimetals as spin-current sources in terahertz spintronic devices. Finally, our results provide a strategy to identify magnetic materials that offer maximum spin-current amplitudes for a given deposited optical energy density.

Spin transport is crucial for future spintronic devices operating at bandwidths up to the terahertz range. In F|N thin-film stacks made of a ferromagnetic/ferrimagnetic layer F and a normal-metal layer N, spin transport is mediated by (1) spin-polarized conduction electrons and/or (2) torque between electron spins. To identify a crossover from (1) to (2), we study laser-driven spin currents in F|Pt stacks where F consists of model materials with different degrees of electrical conductivity. For the magnetic insulators yttrium iron garnet, gadolinium iron garnet (GIG) and γ−Fe2O3, identical dynamics is observed. It arises from the terahertz interfacial spin Seebeck effect (SSE), is fully determined by the relaxation of the electrons in the metal layer, and provides a rough estimate of the spin-mixing conductance of the GIG/Pt and γ−Fe2O3/Pt interfaces. Remarkably, in the half-metallic ferrimagnet Fe3O4 (magnetite), our measurements reveal two spin-current components with opposite direction. The slower, positive component exhibits SSE dynamics and is assigned to torque-type magnon excitation of the A- and B-spin sublattices of Fe3O4. The faster, negative component arises from the pyrospintronic effect and can consistently be assigned to ultrafast demagnetization of minority-spin hopping electrons. This observation supports the magneto-electronic model of Fe3O4. In general, our results provide a route to the contact-free separation of torque- and conduction-electron-mediated spin currents., The authors acknowledge funding by the German Research Foundation through the collaborative research centers SFB TRR 227 “Ultrafast spin dynamics” (Project ID 328545488, projects A05, B02, and B03), SFB TRR 173 “Spin + X” (Project No. 358671374, projects A01 and B02), the European Union H2020 program through the project CoG TERAMAG(GrantNo.681917), the Spanish Ministry of Science and Innovation (Project No. PID2020-112914RB-I00), the National Natural Science Foundation of China (Grants No. 61988102 and No. 61975110), and the Czech Science Foundation through Project GA CR/Grant No. 21-28876J. P.J.-C. acknowledges the Spanish MECD for support through the FPU program (References No. FPU014/02546 and No. EST17/00382.)

In bilayers consisting of a normal metal (N) with spin-orbit coupling and a ferromagnet (F), the combination of the spin-Hall effect, the spin-transfer torque, and the inverse spin-Hall effect gives a small correction to the in-plane conductivity of N, which is referred to as spin-Hall magnetoresistance (SMR). We here present a theory of the SMR and the associated off-diagonal conductivity corrections for frequencies up to the terahertz regime. We show that the SMR signal has pronounced singularities at the spin-wave frequencies of F, which identifies it as a potential tool for all-electric spectroscopy of magnon modes. A systematic change of the magnitude of the SMR at lower frequencies is associated with the onset of a longitudinal magnonic contribution to spin transport across the F-N interface., Comment: 21 pages, 9 figures

We use the terahertz (THz) emission spectroscopy to study femtosecond photocurrent dynamics in the prototypical 2D semiconductor, transition metal dichalcogenide MoSe$_2$. We identify several distinct mechanisms producing THz radiation in response to an ultrashort ($30\,$fs) optical excitation in a bilayer (BL) and a multilayer (ML) sample. In the ML, the THz radiation is generated at a picosecond timescale by out-of-plane currents due to the drift of photoexcited charge carriers in the surface electric field. The BL emission is generated by an in-plane shift current. Finally, we observe oscillations at about $23\,$THz in the emission from the BL sample. We attribute the oscillations to quantum beats between two excitonic states with energetic separation of $\sim100\,$meV., Comment: This is the Accepted Manuscript version of an article accepted for publication in 2D Materials. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at https://doi.org/10.1088/2053-1583/abd527 7 pages, 9 figures

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., Comment: 9 pages, 3 figures

Following the success and relevance of the 2014 and 2017 Magnetism Roadmap articles, this 2020 Magnetism Roadmap edition takes yet another timely look at newly relevant and highly active areas in magnetism research. The overall layout of this article is unchanged, given that it has proved the most appropriate way to convey the most relevant aspects of today's magnetism research in a wide variety of sub-fields to a broad readership. A different group of experts has again been selected for this article, representing both the breadth of new research areas, and the desire to incorporate different voices and viewpoints. The latter is especially relevant for thistype of article, in which one's field of expertise has to be accommodated on two printed pages only, so that personal selection preferences are naturally rather more visible than in other types of articles. Most importantly, the very relevant advances in the field of magnetism research in recent years make the publication of yet another Magnetism Roadmap a very sensible and timely endeavour, allowing its authors and readers to take another broad-based, but concise look at the most significant developments in magnetism, their precise status, their challenges, and their anticipated future developments. While many of the contributions in this 2020 Magnetism Roadmap edition have significant associations with different aspects of magnetism, the general layout can nonetheless be classified in terms of three main themes: (i) phenomena, (ii) materials and characterization, and (iii) applications and devices. While these categories are unsurprisingly rather similar to the 2017 Roadmap, the order is different, in that the 2020 Roadmap considers phenomena first, even if their occurrences are naturally very difficult to separate from the materials exhibiting such phenomena. Nonetheless, the specifically selected topics seemed to be best displayed in the order presented here, in particular, because many of the phenomena or geometries discussed in (i) can be found or designed into a large variety of materials, so that the progression of the article embarks from more general concepts to more specific classes of materials in the selected order. Given that applications and devices are based on both phenomena and materials, it seemed most appropriate to close the article with the application and devices section (iii) once again. The 2020 Magnetism Roadmap article contains 14 sections, all of which were written by individual authors and experts, specifically addressing a subject in terms of its status, advances, challenges and perspectives in just two pages. Evidently, this two-page format limits the depth to which each subject can be described. Nonetheless, the most relevant and key aspects of each field are touched upon, which enables the Roadmap as whole to give its readership an initial overview of and outlook into a wide variety of topics and fields in a fairly condensed format. Correspondingly, the Roadmap pursues the goal of giving each reader a brief reference frame of relevant and current topics in modern applied magnetism research, even if not all sub-fields can be represented here. The first block of this 2020 Magnetism Roadmap, which is focussed on (i) phenomena, contains five contributions, which address the areas of interfacial Dzyaloshinskii–Moriya interactions, and two-dimensional and curvilinear magnetism, as well as spin-orbit torque phenomena and all optical magnetization reversal. All of these contributions describe cutting edge aspects of rather fundamental physical processes and properties, associated with new and improved magnetic materials' properties, together with potential developments in terms of future devices and technology. As such, they form part of a widening magnetism 'phenomena reservoir' for utilization in applied magnetism and related device technology. The final block (iii) of this article focuses on such applications and device-related fields in four contributions relating to currently active areas of research, which are of course utilizing magnetic phenomena to enable specific functions. These contributions highlight the role of magnetism or spintronics in the field of neuromorphic and reservoir computing, terahertz technology, and domain wall-based logic. One aspect common to all of these application-related contributions is that they are not yet being utilized in commercially available technology; it is currently still an open question, whether or not such technological applications will be magnetism-based at all in the future, or if other types of materials and phenomena will yet outperform magnetism. This last point is actually a very good indication of the vibrancy of applied magnetism research today, given that it demonstrates that magnetism research is able to venture into novel application fields, based upon its portfolio of phenomena, effects and materials. This materials portfolio in particular defines the central block (ii) of this article, with its five contributions interconnecting phenomena with devices, for which materials and the characterization of their properties is the decisive discriminator between purely academically interesting aspects and the true viability of real-life devices, because only available materials and their associated fabrication and characterization methods permit reliable technological implementation. These five contributions specifically address magnetic films and multiferroic heterostructures for the purpose of spin electronic utilization, multi-scale materials modelling, and magnetic materials design based upon machine-learning, as well as materials characterization via polarized neutron measurements. As such, these contributions illustrate the balanced relevance of research into experimental and modelling magnetic materials, as well the importance of sophisticated characterization methods that allow for an ever-more refined understanding of materials. As a combined and integrated article, this 2020 Magnetism Roadmap is intended to be a reference point for current, novel and emerging research directions in modern magnetism, just as its 2014 and 2017 predecessors have been in previous years., Journal of Physics D: Applied Physics, 53 (45), ISSN:0022-3727, ISSN:1361-6463

Energy flow in the hydrogen bonding network of water is traced by resonant terahertz excitation and off-resonant optical probing., 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 monoexponentially 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.

Coupling phase-stable single-cycle terahertz (THz) pulses to scanning tunneling microscope (STM) junctions enables spatio-temporal imaging with femtosecond temporal and \r{A}ngstrom 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., Comment: 5 figures, supporting information available

Reliable modulation of terahertz electromagnetic waveforms is important for many applications. Here, we rapidly modulate the direction of the electric field of linearly polarized terahertz electromagnetic pulses with 1–30 THz bandwidth by applying time-dependent magnetic fields to a spintronic terahertz emitter. Polarity modulation of the terahertz field with more than 99% contrast at a rate of 10 kHz is achieved using a harmonic magnetic field. By adding a static magnetic field, we modulate the direction of the terahertz field between angles of, for instance, −53° and 53° at kilohertz rates. We believe our approach makes spintronic terahertz emitters a promising source for low-noise modulation spectroscopy and polarization-sensitive techniques such as ellipsometry at 1–30 THz.

We demonstrate antenna-coupled spintronic terahertz (THz) emitters excited by 1550 nm, 90 fs laser pulses. Antennas are employed to optimize THz outcoupling and frequency coverage of ferromagnetic/nonmagnetic metallic spintronic structures. We directly compare the antenna-coupled devices to those without antennas. Using a 200 μm H-dipole antenna and an ErAs:InGaAs photoconductive receiver, we obtain a 2.42-fold larger THz peak-peak signal, a bandwidth of 4.5 THz, and an increase in the peak dynamic range (DNR) from 53 dB to 65 dB. A 25 μm slotline antenna offered 5 dB larger peak DNR and a bandwidth of 5 THz. For all measurements, we use a comparatively low laser power of 45 mW from a commercial fiber-coupled system that is frequently employed in table-top THz time-domain systems.We demonstrate antenna-coupled spintronic terahertz (THz) emitters excited by 1550 nm, 90 fs laser pulses. Antennas are employed to optimize THz outcoupling and frequency coverage of ferromagnetic/nonmagnetic metallic spintronic structures. We directly compare the antenna-coupled devices to those without antennas. Using a 200 μm H-dipole antenna and an ErAs:InGaAs photoconductive receiver, we obtain a 2.42-fold larger THz peak-peak signal, a bandwidth of 4.5 THz, and an increase in the peak dynamic range (DNR) from 53 dB to 65 dB. A 25 μm slotline antenna offered 5 dB larger peak DNR and a bandwidth of 5 THz. For all measurements, we use a comparatively low laser power of 45 mW from a commercial fiber-coupled system that is frequently employed in table-top THz time-domain systems.

We systematically study the pump-wavelength dependence of terahertz pulse generation in thin-film spintronic THz emitters composed of a ferromagnetic Fe layer between adjacent nonmagnetic W and Pt layers. We find that the efficiency of THz generation is essentially at for excitation by 150 fs pulses with center wavelengths ranging from 900 to 1500 nm, demonstrating that the spin current does not depend strongly on the pump photon energy. We show that the inclusion of dielectric overlayers of TiO2 and SiO2, designed for a particular excitation wavelength, can enhance the terahertz emission by a factor of of up to two in field., 7 pages including 2 supplementary

The anomalous Hall effect (AHE) is a fundamental spintronic charge-to-charge-current conversion phenomenon and closely related to spin-to-charge-current conversion by the spin Hall effect. Future h ...

Identifying materials with an efficient spin-to-charge conversion is crucial for future spintronic applications. In this respect, 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 and the spin-current relaxation length . We develop an all-optical contact-free method with large sample throughput that allows us to extract and . Employing terahertz spectroscopy and an analytical model, magnetic metallic heterostructures involving Pt, W and Cu80Ir20 are characterized in terms of their optical and spintronic properties. The validity of our analytical model is confirmed by the good agreement with literature DC values. For the samples considered here, we find indications that the interface plays a minor role for the spin-current transmission. Our findings establish terahertz emission spectroscopy as a reliable tool complementing the spintronics workbench., Journal of Physics D: Applied Physics, 51 (36), ISSN:0022-3727, ISSN:1361-6463

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, 14 pages, 5 figures

We report on measurements of magnetic field and temperature dependence of antiferromagnetic resonances in the prototypical antiferromagnet NiO. The frequencies of the magnetic resonances in the vicinity of 1 THz have been determined in the time-domain via time-resolved Faraday measurements after selective excitation by narrow-band superradiant terahertz (THz) pulses at temperatures down to 3K and in magnetic fields up to 10 T. The measurements reveal two antiferromagnetic resonance modes, which can be distinguished by their characteristic magnetic field dependencies. The nature of the two modes is discussed by comparison to an eight-sublattice antiferromagnetic model, which includes superexchange between the next-nearest-neighbor Ni spins, magnetic dipolar interactions, cubic magneto-crystalline anisotropy, and Zeeman interaction with the external magnetic field. Our study indicates that a two-sublattice model is insufficient for the description of spin dynamics in NiO, while the magnetic-dipolar interactions and magneto-crystalline anisotropy play important roles., 5 pages, 5 figures

We measure the inverse spin Hall effect of Cu1-xIrx thin films on yttrium iron garnet over a wide range of Ir concentrations (0.05 ⩽ x ⩽ 0.7). Spin currents are triggered through the spin Seebeck effect, either by a continuous (dc) temperature gradient or by ultrafast optical heating of the metal layer. The spin Hall current is detected by electrical contacts or measurement of the emitted terahertz radiation. With both approaches, we reveal the same Ir concentration dependence that follows a novel complex, nonmonotonous behavior as compared to previous studies. For small Ir concentrations a signal minimum is observed, whereas 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 Cu1-xIrx. The coinciding results obtained for dc and ultrafast stimuli provide further support that the spin Seebeck effect extends to terahertz frequencies, thus enabling a transfer of established spintronic measurement schemes into the terahertz regime. Our findings also show that the studied material allows for efficient spin-to-charge conversion even on ultrafast time scales.

Recent advancements of accelerator technology enable the generation of carrier-envelope-phase stable THz pulses with high fields at adjustable high repetition rates. The appropriate choice of THz radiator allows generation of narrow-band, spectrally dense, multicycle THz transients of tunable THz frequency which are ideally suited to selectively excite low-energy excitations such as magnons or phonons. They also allow one to study the frequency dependence of nonresonant THz-field interactions with various order parameters with high dynamic range. In this paper, we discuss the future prospects of this new type of THz light source for studying the coherent control of magnetic order based on recent results.

Control and detection of spin order in ferromagnetic materials is the main principle enabling magnetic information to be stored and read in current technologies. Antiferromagnetic materials, on the other hand, are far less utilized, despite having some appealing features. For instance, the absence of net magnetization and stray fields eliminates crosstalk between neighbouring devices, and the absence of a primary macroscopic magnetization makes spin manipulation in antiferromagnets inherently faster than in ferromagnets. However, control of spins in antiferromagnets requires exceedingly high magnetic fields, and antiferromagnetic order cannot be detected with conventional magnetometry. Here we provide an overview and illustrative examples of how electromagnetic radiation can be used for probing and modification of the magnetic order in antiferromagnets. We also discuss possible research directions that are anticipated to be among the main topics defining the future of this rapidly developing field. An overview of how electromagnetic radiation can be used for probing and modification of the magnetic order in antiferromagnets, and possible future research directions.

The speed of writing of state-of-the-art ferromagnetic memories is physically limited by an intrinsic gigahertz threshold. Recently, realization of memory devices based on antiferromagnets, in which spin directions periodically alternate from one atomic lattice site to the next has moved research in an alternative direction. We experimentally demonstrate at room temperature that the speed of reversible electrical writing in a memory device can be scaled up to terahertz using an antiferromagnet. A current-induced spin-torque mechanism is responsible for the switching in our memory devices throughout the 12-order-of-magnitude range of writing speeds from hertz to terahertz. Our work opens the path toward the development of memory-logic technology reaching the elusive terahertz band., Science Advances, 4 (3), ISSN:2375-2548

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 THz pulse is directly transferred into the phase of the lattice vibration. New prospects in general infrared spectroscopy, action spectroscopy, and lattice trajectory control in the electronic ground state emerge.

To explore the capabilities of metallic spintronic thin-film stacks as a source of intense and broadband terahertz electromagnetic fields, we excite a W/CoFeB/Pt trilayer on a large-area glass substrate (diameter of 7.5 cm) by a femtosecond laser pulse (energy 5.5 mJ, duration 40 fs, wavelength 800 nm). After focusing, the emitted terahertz pulse is measured to have a duration of 230 fs, a peak field of 300 kV cm$^{-1}$ and an energy of 5 nJ. In particular, the waveform exhibits a gapless spectrum extending from 1 to 10 THz at 10% of amplitude maximum, thereby facilitating nonlinear control over matter in this difficult-to-reach frequency range and on the sub-picosecond time scale., 7 pages, 4 figures

A review on the recent development of intense laser-driven terahertz (THz) sources is provided here. The technologies discussed include various types of sources based on optical rectification (OR), spintronic emitters, and laser-filament-induced plasma. The emphasis is on OR using pump pulses with tilted intensity front. Illustrative examples of newly emerging applications are briefly discussed, in particular strong-field THz control of materials and acceleration and manipulation of charged particles.

Three-dimensional topological insulators are fascinating materials with insulating bulk yet metallic surfaces that host highly mobile charge carriers with locked spin and momentum. Remarkably, surface currents with tunable direction and magnitude can be launched with tailored light beams. To better understand the underlying mechanisms, the current dynamics need to be resolved on the timescale of elementary scattering events (∼10 fs). Here, we excite and measure photocurrents in the model topological insulator Bi2Se3 with a time resolution of 20 fs by sampling the concomitantly emitted broadband terahertz (THz) electromagnetic field from 0.3 to 40 THz. Strikingly, the surface current response is dominated by an ultrafast charge transfer along the Se–Bi bonds. In contrast, photon-helicity-dependent photocurrents are found to be orders of magnitude smaller than expected from generation scenarios based on asymmetric depopulation of the Dirac cone. Our findings are of direct relevance for broadband optoelectronic devices based on topological-insulator surface currents., Surface currents in topological insulators can be controlled by light, but the underlying mechanisms are not well understood. Here, Braun et al. report an ultrafast shift photocurrent at the surface of Ca-doped Bi2Se3, whereas injection currents are much smaller than expected from asymmetric depopulation of the Dirac cone.

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., Comment: Manuscript: 14 pages, 3 figures Supplementary Information: 12 pages, 10 figures

Few cycle THz transients pump electronic transitions coupled to the spin system in thulium orthoferrite to trigger coherent magnons. Exploiting this novel driving mechanism we realize the first nonlinear interaction between THz pulses and spins.

Future information technologies, such as ultrafast data recording, quantum computation or spintronics, call for ever faster spin control by light1-16. Intense terahertz pulses can couple to spins on the intrinsic energy scale of magnetic excitations5,11. Here, we explore a novel electric dipole-mediated mechanism of nonlinear terahertz-spin coupling that is much stronger than linear Zeeman coupling to the terahertz magnetic field5,10. Using the prototypical antiferromagnet thulium orthoferrite (TmFeO3), we demonstrate that resonant terahertz pumping of electronic orbital transitions modifies the magnetic anisotropy for ordered Fe3+ spins and triggers large-amplitude coherent spin oscillations. This mechanism is inherently nonlinear, it can be tailored by spectral shaping of the terahertz waveforms and its efficiency outperforms the Zeeman torque by an order of magnitude. Because orbital states govern the magnetic anisotropy in all transition-metal oxides, the demonstrated control scheme is expected to be applicable to many magnetic materials.

Terahertz magnetic fields with amplitudes of up to 0.4 Tesla drive magnon resonances in nickel oxide while the induced dynamics is recorded by femtosecond magneto-optical probing. We observe distinct spin-mediated optical nonlinearities, including oscillations at the second harmonic of the 1 THz magnon mode. The latter originate from coherent dynamics of the longitudinal component of the antiferromagnetic order parameter, which are probed by magneto-optical effects of second order in the spin deflection. These observations allow us to dynamically disentangle electronic from lattice-related contributions to magnetic linear birefringence and dichroism---information so far only accessible by ultrafast THz spin control. The nonlinearities discussed here foreshadow physics that will become essential in future subcycle spin switching.

We use slow-light photonic crystals to enhance optical switching and modulation in silicon. By using dispersion-engineered designs, a switch as short as 5 ¿m was achieved, in which we have demonstrated rerouting of optical pulses on a 3-ps time scale through the absorption of a femtosecond pulse. We additionally demonstrate a modulator with a Mach-Zehnder interferometer (MZI) configuration with flat-band slow-light photonic crystal phase shifters that is designed to give a large group-index-bandwidth product. An extinction ratio in excess of 15 dB is obtained over the entire 11-nm bandwidth of the modulator.

We apply intense terahertz (THz) electromagnetic pulses with field strengths exceeding 2 MV cm(-1) at ~1 THz to window and substrate materials commonly used in THz spectroscopy and determine the induced optical birefringence. Materials studied are diamond, sapphire, magnesium oxide (MgO), polymethylpentene (TPX), low-density polyethylene (LDPE), silicon nitride membrane (SiN) and crystalline quartz. We observe a Kerr-effect-type transient birefringence in all samples, except in quartz and Si, where, respectively, a linear electrooptic signal and a response beyond the perturbative regime are found. We extract the nonlinear refractive indices and the electrooptic coefficient (in the case of quartz) of these materials and discuss implications for their use as windows or substrates in THz pump-optical probe spectroscopy.

Terahertz electromagnetic radiation is extremely useful for numerous applications such as imaging and spectroscopy. Therefore, it is highly desirable to have an efficient table-top emitter covering the 1-to-30-THz window whilst being driven by a low-cost, low-power femtosecond laser oscillator. So far, all solid-state emitters solely exploit physics related to the electron charge and deliver emission spectra with substantial gaps. Here, we take advantage of the electron spin to realize a conceptually new terahertz source which relies on tailored fundamental spintronic and photonic phenomena in magnetic metal multilayers: ultrafast photo-induced spin currents, the inverse spin-Hall effect and a broadband Fabry-P\'erot resonance. Guided by an analytical model, such spintronic route offers unique possibilities for systematic optimization. We find that a 5.8-nm-thick W/CoFeB/Pt trilayer generates ultrashort pulses fully covering the 1-to-30-THz range. Our novel source outperforms laser-oscillator-driven emitters such as ZnTe(110) crystals in terms of bandwidth, terahertz-field amplitude, flexibility, scalability and cost., Comment: 18 pages, 10 figures

Topological insulators are candidates to open up a novel route in spin based electronics. Different to traditional ferromagnetic materials, where the carrier spin-polarization and magnetization are based on the exchange interaction, the spin properties in topological insulators are based on the coupling of spin- and orbit interaction connected to its momentum. Specific ways to control the spin-polarization with light have been demonstrated: the energy momentum landscape of the Dirac cone provides spin-momentum locking of the charge current and its spin. We investigate a spin-related signal present only during the laser excitation studying real and imaginary part of the complex Kerr angle by disentangling spin and lattice contributions. This coherent signal is only present at the time of the pump-pulses’ light field and can be described in terms of a Raman coherence time. The Raman transition involves states at the bottom edge of the conduction band. We demonstrate a coherent femtosecond control of spin-polarization for electronic states at around the Dirac cone., National Science Foundation (U.S.) (DMR-1207469), United States. Office of Naval Research (N00014-13-1-0301), National Science Foundation (U.S.). Materials Research Science and Engineering Centers (Program) (Award DMR-0819762), National Science Foundation (U.S.). Science and Technology Center for Integrated Quantum Materials (Grant DMR-1231319)

Despite extensive work on high-temperature superconductors, the critical behavior of an incipient condensate has so far been studied exclusively under equilibrium conditions. Here, we excite Bi2Sr2CaCu2O8+d with a femtosecond laser pulse and monitor the subsequent nonequilibrium dynamics of the mid-infrared conductivity. Our data allow us to discriminate temperature regimes where superconductivity is either coherent, fluctuating or vanishingly small. Above the transition temperature Tc, we make the striking observation that the relaxation to equilibrium exhibits power-law dynamics and scaling behavior, both for optimally and underdoped superconductors. Our findings can in part be modeled using time-dependent Ginzburg-Landau theory and provide strong indication of universality in systems far from equilibrium., Comment: 5 pages, 4 figures

Spin-dependent conduction in metals underlies all modern magnetic memory technologies, such as giant magnetoresistance (GMR). The charge current in ferromagnetic transition metals is carried by two non-mixing populations of sp-band Fermi-level electrons: one of majority-spin and one of minority-spin. These electrons experience spin-dependent momentum scattering with localized electrons, which originate from the spin-split d-band. The direct observation of magnetotransport under such fundamental conditions, however, requires magnetotransport measurements on the same timescale as the electron momentum scattering, which takes place in the sub-100 fs regime. Using terahertz electromagnetic probes, we directly observe the magnetotransport in a metallic system under the fundamental conditions, and determine the spin-dependent densities and momentum scattering times of conduction electrons. We show that traditional measurements significantly underestimate the spin asymmetry in electron scattering, a key parameter responsible for effects such as GMR. Furthermore, we demonstrate the possibility of magnetic modulation of terahertz waves, along with heat- and contact-free GMR readout using ultrafast terahertz signals. Terahertz radiation is used to directly probe magnetotransport in metallic multilayers on the timescale of electron momentum scattering—the fundamental conditions of Nevill Mott’s model of spin-dependent conduction in metals.

Understanding dynamics on ultrafast timescales enables unique and new insights into important processes in the materials and life sciences. In this respect, the fundamental pump-probe approach based on ultra-short photon pulses aims at the creation of stroboscopic movies. Performing such experiments at one of the many recently established accelerator-based 4th-generation light sources such as free-electron lasers (FELs) or superradiant THz sources allows an enormous widening of the accessible parameter space for the excitation and/or probing light pulses. Compared to table-top devices, critical issues of this type of experiment are fluctuations of the timing between the accelerator and external laser systems and intensity instabilities of the accelerator-based photon sources. Existing solutions have so far been only demonstrated at low repetition rates and/or achieved a limited dynamic range in comparison to table-top experiments, while the 4th generation of accelerator-based light sources is based on superconducting radio-frequency (SRF) technology which enables operation at MHz or even GHz repetition rates. In this article, we present the successful demonstration of ultra-fast accelerator-laser pump-probe experiments performed at an unprecedentedly high repetition rate in the few-hundred-kHz regime and with a currently achievable optimal time resolution of 13 femtoseconds (fs) (rms). Our scheme, based on the pulse-resolved detection of multiple beam parameters relevant for the experiment, allows us to achieve an excellent sensitivity in real-world ultra-fast experiments, as demonstrated for the example of THz-field-driven coherent spin precession.

Terahertz electromagnetic pulses are frequently generated by optical rectification of femtosecond laser pulses. In many cases, the efficiency of this process is known to saturate with increasing intensity of the generation beam because of two-photon absorption. Here, we demonstrate two routes to reduce this effect in ZnTe(110) crystals and enhance efficiency, namely, by (i) recycling the generation pulses and by (ii) splitting each generation pulse into two pulses before pumping the crystal. In both methods, the second pulse arrives ∼1 ns after the first one, sufficiently long for optically generated carriers to relax. Enhancement is achieved by coherently superimposing the two resulting terahertz fields.