Search

$FeCr_2S_4$ is a ferrimagnet with two oppositely-ordered spin sublattices (Fe and Cr), connected via superexchange interaction, giving a non-zero net magnetic moment. We show how the magnetic dynamics of the sublattices can be selectively manipulated by resonantly perturbing the Fe sublattice using ultrashort laser pulses. The mid-infrared excitation through intra-atomic Fe $d-d$ transitions triggers a markedly slower magneto-optical Kerr effect dynamics compared to an off-resonant pumping affecting both the two sublattices simultaneously. The analysis and conclusions are supported by probing resonantly and off-resonantly to the Fe sublattice., Comment: 29 pages, 19 figures

Materials with linear electronic dispersion often feature high carrier mobilities and unusually strong nonlinear optical interactions. In this work, we investigate the THz nonlinear dynamics of one such material, HgCdTe, with an electronic band dispersion heavily dependent on both temperature and stoichiometry. We show how the band gap, carrier concentration and band shape together determine the nonlinear response of the system. At low temperatures, carrier generation from Zener tunneling dominates the nonlinear response with a reduction in the overall transmission. At room temperature, quasi-ballistic electronic dynamics drive the largest observed nonlinear optical interactions, leading to a transmission increase. Our results demonstrate the sensitivity of these nonlinear optical properties of narrow-gap materials to small changes in the electronic dispersion and carrier concentration., Comment: 48 pages, 21 figures

Liquid crystal based technologies have found considerably diversified uses and areas of application over the last few decades, proving to be excellent materials for tunable optical elements from visible to near-infrared frequencies. Currently, much effort is devoted to demonstrating their applicability in the far-infrared or THz spectral frequency (1 - 10 THz), where tremendous advances have been achieved in terms of broadband and intense sources. Yet a detailed understanding of the dynamics triggered by THz light in liquid crystals is far from complete. In this work, we perform broadband THz Time Domain Spectroscopy on the low-frequency modes of 4-cyano-4'-alkylbiphenyl (nCB) and 5-phenylcyclohexanes (PCH5) across different mesophases. DFT calculations on isolated molecules capture the majority of the measured response above 3 THz. In particular, the pronounced modes around 4.5 and 5.5 THz mainly originate from in-plane and out-of-plane bending of the cyano group. In contrast, the broad response below 3 THz, linked to modes of the alkyl chain, disagrees with the single molecule calculation. Here, we identify a clear intermolecular character of the response, supported by dimer and trimer calculations., Comment: 14 pages, 4 figures

Interactions between the different degrees of freedom form the basis of many manifestations of intriguing physics in condensed matter. In this respect, quantifying the dynamics of normal modes that themselves arise from these interactions and how they interact with other excitations is of central importance. Of the different types of coupling that are often important, spin-lattice coupling is relevant to several sub-fields of condensed matter physics; examples include spintronics, high-TC superconductivity, and topological materials. While theories of materials where spin-lattice coupling is relevant can sometimes be used to infer the magnitude and character of this interaction, experimental approaches that can directly measure it are rare and incomplete. Here we use time-resolved X-ray diffraction to directly access the spin-lattice coupling by measuring both ultrafast atomic motion and the associated spin dynamics following the excitation of a coherent electromagnon by an intense THz pulse in a multiferroic hexaferrite. Comparing the dynamics of the two different components, one striking outcome is the different phase shifts relative to the driving field. This phase shift provides insight into the excitation process of such a coupled mode. This direct observation of combined lattice and magnetization dynamics paves the way to access the mode-selective spin-lattice coupling strength, which remains a missing fundamental parameter for ultrafast control of magnetism and is relevant to a wide variety of correlated electron physics., Comment: 4 figures

Using two-dimensional THz spectroscopy in combination with numerical models, we investigate the dynamics linked to carrier multiplication caused by high-field THz excitation of the low-gap semiconductor InSb. In addition to previously observed dynamics connected with quasi-ballistic carrier dynamics, we observe other spectral and temporal features that we attribute to impact ionization for peak fields above 60 kV/cm, which continue up to the maximum investigated peak field of 430 kV/cm. At the highest fields we estimate a carrier multiplication factor greater than 10 due to impact ionization, which is well-reproduced by a numerical simulation of the impact ionization process which we have developed., Comment: 25 pages, 5 figures

We report the coherent generation and detection of terahertz (THz) pulses covering the bandwidth of 0.1-9 THz in a high repetition rate, low pulse energy laser system. In this work we demonstrate the application and evaluation of solid-state biased coherent detection in combination with a spintronic emitter. This combination was used to generate and detect THz pulses in a time-domain spectroscopy (TDS) setup and tested on bulk nonlinear crystals. These results establish a new promising candidate to extend the possibilities for compact, broadband THz TDS systems driven by high repetition rate lasers.

We use time-resolved hard x-ray diffraction to investigate the structural dynamics of the multiferroic insulator TbMnO$_3$ in the low temperature antiferromagnetic and ferroelectrically ordered phase. The lattice response following photoexcitation at 1.55 eV is detected by measuring the (0 2 4) and (1 3 -5) Bragg reflections. A 0.02% tensile strain, normal to the surface, is seen to arise within 20 - 30 ps. The magnitude of this transient strain is over an order of magnitude lower than that predicted from laser-induced heating, which we attribute to a bottleneck in the energy transfer between the electronic and lattice subsystems. The timescale for the transient expansion is consistent with that of previously reported demagnetization dynamics. We discuss a possible relationship between structural and demagnetization dynamics in TbMnO$_3$, in which photoinduced atomic motion modulates the exchange interaction, leading to a destruction of the magnetic order in the system., Comment: 3 figures, 4 footnotes

Understanding ultrafast magnetization dynamics on the microscopic level is of strong current interest due to the potential for applications in information storage. In recent years, the spin-lattice coupling has been recognized to be essential for ultrafast magnetization dynamics. Magnetoelectric multiferroics of type II possess intrinsic correlations among magnetic sublattices and electric polarization (P) through spin-lattice coupling, enabling fundamentally coupled dynamics between spins and lattice. Here we report on ultrafast magnetization dynamics in a room-temperature multiferroic hexaferrite possessing ferrimagnetic and antiferromagnetic sublattices, revealed by time-resolved resonant x-ray diffraction. A femtosecond above-bandgap excitation triggers a coherent magnon in which the two magnetic sublattices entangle and give rise to a transient modulation of P. A novel microscopic mechanism for triggering the coherent magnon in this ferrimagnetic insulator based on the spin-lattice coupling is proposed. Our finding opens up a novel but general pathway for ultrafast control of magnetism., Comment: 18 pages, 7 figures + 21 pages supplementary information

In ionic Raman scattering, infrared-active phonons mediate a scattering process that results in the creation or destruction of a Raman-active phonon. This mechanism relies on nonlinear interactions between phonons and has in recent years been associated with a variety of emergent lattice-driven phenomena in complex transition-metal oxides, but the underlying mechanism is often obscured by the presence of multiple coupled order parameters in play. Here, we use time-resolved spectroscopy to compare coherent phonons generated by ionic Raman scattering with those created by more conventional electronic Raman scattering on the nonmagnetic and non-strongly-correlated wide band-gap insulator LaAlO$_3$. We find that the oscillatory amplitude of the low-frequency Raman-active $E_g$ mode exhibits a sharp peak when we tune our pump frequency into resonance with the high-frequency infrared-active $E_u$ mode, consistent with first-principles calculations. Our results suggest that ionic Raman scattering can strongly dominate electronic Raman scattering in wide band-gap insulating materials. We also see evidence of competing scattering channels at fluences above 28~mJ/cm$^2$ that alter the measured amplitude of the coherent phonon response., Comment: 10 pages, 6 figures

The general idea of using ultrashort light pulses to control ferroic order parameters has recently attracted attention as a means to achieve control over material properties on unprecedented time scales. Much of the challenge in such work is in understanding the mechanisms by which this control can be achieved, and in particular how observables can be connected to structural and electronic properties. Here we report on a combination of experimental and computational methods to study the electronic structure of the semiconducting ferroelectric GeTe when driven out of equilibrium by absorption of a femtosecond pulse of light. We observe coherent modulations of second harmonic generations on the order of 50%, which we attribute to a combination of atomic and electronic structure changes due to a coherently excited soft mode. Comparison of the observed experimental data with model calculations indicates that this effect is predominantly due to an ultrafast modulation of the covalency of the bonding between Ge and Te ions. This stands in contrast to previously held assumptions in other systems, indicating that care should be exercised in using indirect measurements of electronic structure to make strong conclusions about the magnitude of nuclear motions.

The original observation of the Einstein-de Haas effect was a landmark experiment in the early history of modern physics that illustrates the relationship between magnetism and angular momentum. Today the effect is still discussed in elementary physics courses to demonstrate that the angular momentum associated with the aligned electron spins in a ferromagnet can be converted to mechanical angular momentum by reversing the direction of magnetisation using an external magnetic field. In recent times, a related problem in magnetism concerns the time-scale over which this angular momentum transfer can occur. It is known experimentally for several metallic ferromagnets that intense photoexcitation leads to a drop in the magnetisation on a time scale shorter than 100 fs, a phenomenon called ultrafast demagnetisation. The microscopic mechanism for this process has been hotly debated, with one key question still unanswered: where does the angular momentum go on these sub-picosecond time scales? Here we show using femtosecond time-resolved x-ray diffraction that a large fraction of the angular momentum lost from the spin system on the laserinduced demagnetisation of ferromagnetic iron is transferred to the lattice on sub-picosecond timescales, manifesting as a transverse strain wave that propagates from the surface into the bulk. By fitting a simple model of the x-ray data to simulations and optical data, we roughly estimate that the angular momentum occurs on a time scale of 200 fs and corresponds to 80% of the angular momentum lost from the spin system. Our results show that interaction with the lattice plays an essential role in the process of ultrafast demagnetisation in this system., Comment: 39 pages, 2 tables, 7 figures

Light-matter interaction at the nanoscale in magnetic materials is a topic of intense research in view of potential applications in next-generation high-density magnetic recording. Laser-assisted switching provides a pathway for overcoming the material constraints of high-anisotropy and high-packing density media, though much about the dynamics of the switching process remains unexplored. We use ultrafast small-angle x-ray scattering at an x-ray free-electron laser to probe the magnetic switching dynamics of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. We observe that the combination of laser excitation and applied static magnetic field, one order of magnitude smaller than the coercive field, can overcome the magnetic anisotropy barrier between "up" and "down" magnetization, enabling magnetization switching. This magnetic switching is found to be inhomogeneous throughout the material, with some individual FePt nanoparticles neither switching nor demagnetizing. The origin of this behavior is identified as the near-field modification of the incident laser radiation around FePt nanoparticles. The fraction of not-switching nanoparticles is influenced by the heat flow between FePt and a heat-sink layer.

All-optical switching (AOS) of magnetic domains by femtosecond laser pulses was first observed in the transition metal-rare earth (TM-RE) alloy GdFeCo1-5; this phenomenon demonstrated the potential for optical control of magnetism for the development of ever faster future magnetic recording technologies. The technological potential of AOS has recently increased due to the discovery of the same effect in other materials, including RE-free magnetic multilayers6,7. However, to be technologically meaningful, AOS must compete with the bit densities of conventional storage devices, restricting optically-switched magnetic areas to sizes well below the diffraction limit. Here, we demonstrate reproducible and robust all-optical switching of magnetic domains of 53 nm size in a ferrimagnetic TbFeCo alloy using gold plasmonic antenna structures. The confined nanoscale magnetic reversal is imaged around and beneath plasmonic antennas using x-ray resonant holographic imaging. Our results demonstrate the potential of future AOS-based magnetic recording technologies., Comment: 15 pages (including Supplementary Materials)

Employing plasmonic antennas for subdiffraction focusing of light on recording media requires to take into account the complete structure of the medium, including dielectric cover layers. We find, with finite difference time domain simulations, that optical energy transfer to the magnetic recording layer is most efficient for an off-resonant antenna. Furthermore, we show that the focal spot in the magnetic film is well below the diffraction limit, making nanoscale all-optical magnetic data recording achievable., Comment: 11 pages, 4 figures

By exploiting photo-induced reorientation in azo-polymer thin films, we demonstrate all-optical polarization-encoded information storage with a scanning near-field optical microscope. In the writing routine, 5-level bits are created by associating different bit values to different birefringence directions, induced in the polymer after illumination with linearly polarized light. The reading routine is then performed by implementing polarization-modulation techniques on the same near-field microscope, in order to measure the encoded birefringence direction., Comment: 13 pages, 5 figures