Achieving parametric excitation in an oscillating physical system involves periodically adjusting one of its parameters to modulate the oscillator's natural frequency. This phenomenon has been observed in numerous systems within physics and engineering, profoundly transforming modern science and technology. Despite rapid progress, the parametric control of collective excitations, such as phonons, remains a challenge while promising to generate novel and intriguing effects in a largely unexplored field. Here, we investigate the terahertz (THz) field-induced dynamics of Raman-active phonons in the perovskite structure of LaAlO_{3}. Utilizing intense THz pulses, we demonstrate a novel mechanism of parametric phonon excitation marked by substantial subharmonic components. Theoretical analysis can successfully capture the hallmarks of the observed phenomena in a physical scenario with the THz field inducing a parametric coupling between the Raman mode and pairs of acoustic phonon excitations.
Ultrafast electric-field control of emergent electronic and magnetic states at oxide interfaces offers exciting prospects for the development of the next generation of energy-efficient devices. Here, it is demonstrated that the electronic structure and emergent ferromagnetic interfacial state in epitaxial LaNiO3/CaMnO3 superlattices can be effectively controlled using intense, single-cycle THz electric-field pulses. A suite of advanced X-ray spectroscopic techniques is employed to measure a detailed magneto-optical profile and the thickness of the ferromagnetic interfacial layer. Then, a combination of time-resolved and temperature-dependent optical measurements is used to disentangle several correlated electronic and magnetic processes driven by ultrafast, high-field THz pulses. Sub-picosecond non-equilibrium Joule heating of the electronic system is observed, ultrafast demagnetization of the ferromagnetic interfacial layer, and slower dynamics indicative of a change in the magnetic state of the superlattice due to the transfer of spin-angular momentum to the lattice. These findings suggest a promising avenue for the efficient control of 2D ferromagnetic states at oxide interfaces using ultrafast electric-field pulses.
The emergence of collective order in matter is among the most fundamental and intriguing phenomena in physics. In recent years, the ultrafast dynamical control and creation of novel ordered states of matter not accessible in thermodynamic equilibrium is receiving much attention. Among those, the theoretical concept of dynamical multiferroicity has been introduced to describe the emergence of magnetization by means of a time-dependent electric polarization in non-ferromagnetic materials. In simple terms, a large amplitude coherent rotating motion of the ions in a crystal induces a magnetic moment along the axis of rotation. However, the experimental verification of this effect is still lacking. Here, we provide evidence of room temperature magnetization in the archetypal paraelectric perovskite SrTiO$_3$ due to this mechanism. To achieve it, we resonantly drive the infrared-active soft phonon mode with intense circularly polarized terahertz electric field, and detect a large magneto-optical Kerr effect. A simple model, which includes two coupled nonlinear oscillators whose forces and couplings are derived with ab-initio calculations using self-consistent phonon theory at a finite temperature, reproduces qualitatively our experimental observations on the temporal and frequency domains. A quantitatively correct magnitude of the effect is obtained when one also considers the phonon analogue of the reciprocal of the Einsten - de Haas effect, also called the Barnett effect, where the total angular momentum from the phonon order is transferred to the electronic one. Our findings show a new path for designing ultrafast magnetic switches by means of coherent control of lattice vibrations with light.
Terahertz (THz)-based science is growing rapidly thanks to its unique capability to investigate, excite and master degree of freedom in matter. In contrast to the existing thermal excitation mechanisms, which rely on high energy excitations, terahertz radiation, in resonance with low-energy excitations and quasiparticles, offers a non-thermal excitation pathway that is able to selectively populate excited states. In less than 10 years, scientists have made outstanding progresses in terahertz-based science and are now able to excite and control structural, electronic and spin dynamics that ultimately may result in phase transitions. Intriguingly, a terahertz-driven out-of-equilibrium configuration can reveal hidden states of matter, inaccessible in the static configuration.
The THz Kerr effect measures the birefringence induced in an otherwise isotropic material by a strong THz pulse driving the Raman-active excitations of the systems. Here we provide experimental evidence of a sizable Kerr response in insulating SrTiO3 due to infrared-active lattice vibrations. Such a signal, named ionic Kerr effect, is associated with the simultaneous excitation of multiple phonons. Thanks to a theoretical modeling of the time, polarization and temperature dependence of the birefringence we can disentangle the ionic Kerr effect from the off-resonant electronic excitations, providing an alternative tunable mechanism to modulate the refractive index on ultrashort time-scales via infra-red active phonons.
We investigate the role of domain walls in the ultrafast magnon dynamics of an antiferromagnetic NiO single crystal in a pump-probe experiment with variable pump photon energy. Analyzing the amplitude of the energy-dependent photoinduced ultrafast spin dynamics, we detect a yet unreported coupling between the material's characteristic terahertz- and gigahertz-magnon modes. We explain this unexpected coupling between two orthogonal eigenstates of the corresponding Hamiltonian by modeling the magnetoelastic interaction between spins in different domains. We find that such interaction, in the nonlinear regime, couples the two different magnon modes via the domain walls and it can be optically exploited via the exciton-magnon resonance.
By means of muon spin relaxation measurements we unraveled the temperature spin dynamics in monodisperse maghemite spherical nanoparticles with different surface to volume ratio, in two samples wit ...
An increasing awareness about novel medical applications of smaller, inorganic-based nanoparticles, possessing unique properties at the nanoscale, has led to a burst of research activities in the development of "nanoprobes" for diagnostic medicine and agents for novel, externally activated therapies. In this research field magnetic nanoparticles are prominent due to fundamental peculiar properties particularly appealing for their use in materials and biomedical applications. Aiming to study the relationship between the topology of the magnetic nanoparticles and their efficacy as MRI contrast agents (relaxometric properties), we prepared three different stable colloidal suspension (ferrofluid) of magnetic nanobeads (MNBs) constituted by a discrete number of maghemite nanoparticles, arranged in disordered clusters or ordered in a polymeric matrix. An accurate morpho-dimensional and magnetic characterization displays the close correlation between the magnetic fundamental properties and the topology of our spin systems. The NMR relaxometry profiles confirmed the nature of the physical mechanisms inducing the increase of nuclear relaxation rates at low (magnetic anisotropy) and high (Curie relaxation) magnetic fields. Moreover the transverse relaxivity (r₂) values for all the MNBs are higher than those of common contrast agents and the differences between the three MNBs are suggested to be due to the spin topology effect.
An experimental 1H NMR relaxometry investigation on iron oxide nanoparticles with different magnetic core size and coated with PolyAcrylic Acid (PAA), is presented. A full structural, morphodimensional and magnetic characterization of the nanoparticles has been performed by means of X-ray diffraction, Dynamic Light Scattering, Transmission Electron Microscopy, Atomic Force Microscopy and SQUID DC magnetometry. The application of a heuristic model for the field dependence of the NMR relaxivity curves allowed us to evaluate the distance of minimum approach of the solvent molecules from the magnetic centers, and to conclude that the local correlation times, namely the Neél time τN and the diffusion time τD related to the magnetization reversal and to the diffusion process respectively, depend strongly on the core size. A preliminary evaluation of their r2 efficiency as Magnetic Resonance Imaging (MRI) contrast agents is also performed by means of a universal scaling law model. The results of our experimental investigation should allow to tailor the physical properties of the nanoparticles for obtaining systems with a resultant contrast efficiency optimized for the in-vivo application of MRI at pre-clinical and clinical level.
Colloidal magnetic nanoparticles (MNPs) based on a nearly monodisperse iron oxide core and capped by oleic acid have been used as model systems for investigating the superparamagnetic spin dynamics by means of magnetometry measurements and nuclear magnetic resonance (1H NMR) relaxometry. The key magnetic properties (saturation magnetization, coercive field, and frequency dependent "blocking" temperature) of MNPs with different core size (3.5 nm, 8.5 nm, and 17.5 nm), shape (spherical and cubic), and dispersant (hexane and water-based formulation) have been determined. 1H NMR dispersion profiles obtained by measuring the r1 (longitudinal) and r2 (transverse) nuclear relaxivities in the frequency range 0.01-60 MHz confirmed that in all samples the physical mechanisms that drive the nuclear relaxation are the Néel reversal at low temperature and the Curie relaxation at high frequency. The magnetization reversal time at room temperature extracted from the fitting of NMR data falls in the typical range of superparamagnetic systems (10-9-10-10 s). Furthermore, from the distance of minimum approach we could conclude that water molecules do not arrive in close vicinity of the magnetic core. Our findings contribute to elucidate the local spin dynamics mechanisms in colloidal superparamagnetic nanoparticles which are useful in biomedical application as, e.g., contrast agents for magnetic resonance imaging.
We report a systematic experimental study of the evolution of the magnetic and relaxometric properties as a function of metal (Co, Ni) doping in iron oxide nanoparticles. A set of five samples, having the same size and ranging from stoichiometric cobalt ferrite (CoFe2O4) to stoichiometric nickel ferrite (NiFe2O4) with intermediate doping steps, was ad hoc synthesized. Using both DC and AC susceptibility measurements, the evolution of the magnetic anisotropy depending on the doping is qualitatively discussed. In particular, we observed that the height of the magnetic anisotropy barrier is directly proportional to the amount of Co, while the Ni has an opposite effect. By Nuclear Magnetic Resonance Dispersion (NMR-D) experiments, the experimental longitudinal r1 and transverse r2 relaxivity profiles were obtained, and the heuristic theory of Roch et al. was used to analyze the data of both r1 and, for the first time, r2. While the experimental and fitting results obtained from r1 profiles were satisfying and confirmed the anisotropy trend, the model applied to r2 hardly explains the experimental findings.
Superparamagnetic iron oxide particles find their main application as contrast agents for cellular and molecular magnetic resonance imaging. The contrast they bring is due to the shortening of the transverse relaxation time T 2 of water protons. In order to understand their influence on proton relaxation, different theoretical relaxation models have been developed, each of them presenting a certain validity domain, which depends on the particle characteristics and proton dynamics. The validation of these models is crucial since they allow for predicting the ideal particle characteristics for obtaining the best contrast but also because the fitting of T 1 experimental data by the theory constitutes an interesting tool for the characterization of the nanoparticles. In this work, T 2 of suspensions of iron oxide particles in different solvents and at different temperatures, corresponding to different proton diffusion properties, were measured and were compared to the three main theoretical models (the motional averaging regime, the static dephasing regime, and the partial refocusing model) with good qualitative agreement. However, a real quantitative agreement was not observed, probably because of the complexity of these nanoparticulate systems. The Roch theory, developed in the motional averaging regime (MAR), was also successfully used to fit T 1 nuclear magnetic relaxation dispersion (NMRD) profiles, even outside the MAR validity range, and provided a good estimate of the particle size. On the other hand, the simultaneous fitting of T 1 and T 2 NMRD profiles by the theory was impossible, and this occurrence constitutes a clear limitation of the Roch model. Finally, the theory was shown to satisfactorily fit the deuterium T 1 NMRD profile of superparamagnetic particle suspensions in heavy water.