Tuning the Multiferroic Properties of BiFeO_{3} under Uniaxial Strain.

More than twenty years ago, multiferroic compounds combining in particular magnetism and ferroelectricity were rediscovered. Since then, BiFeO_{3} has emerged as the most outstanding multiferroic by combining at room temperature almost all the fundamental or applicative properties that may be desired: electroactive spin wave excitations called electromagnons, conductive domain walls, or a low band gap of interest for magnonic devices. All these properties have so far only been discontinuously strain engineered in thin films according to the lattice parameter imposed by the substrate. Here we explore the ferroelectricity and the dynamic magnetic response of BiFeO_{3} bulk under continuously tunable uniaxial strain. Using elasto-Raman spectroscopy, we show that the ferroelectric soft mode is strongly enhanced under tensile strain and driven by the volume preserving deformation at low strain. The magnonic response is entirely modified with low energy magnon modes being suppressed for tensile strain above pointing out a transition from a cycloid to an homogeneous magnetic state. Effective Hamiltonian calculations show that the ferroelectric and the antiferrodistortive modes compete in the tensile regime. In addition, the homogeneous antiferromagnetic state becomes more stable compared to the cycloidal state above a +2% tensile strain close to the experimental value. Finally, we reveal the ferroelectric and magnetic orders of BiFeO_{3} under uniaxial strain and how the tensile strain allows us to unlock and to modify in a differentiated way the polarization and the magnetic structure.

400 kHz repetition rate THz-TDS with 24†mW of average power driven by a compact industrial Yb-laser.

We demonstrate a high average power terahertz time-domain spectroscopy (THZ-TDS) set-up based on optical rectification in the tilted-pulse front geometry in lithium niobate at room temperature, driven by a commercial, industrial femtosecond-laser operating with flexible repetition rate between 40 kHz - 400 kHz. The driving laser provides a pulse energy of 41 µJ for all repetition rates, at a pulse duration of 310 fs, allowing us to explore repetition rate dependent effects in our TDS. At the maximum repetition rate of 400 kHz, up to 16.5 W of average power are available to drive our THz source, resulting in a maximum of 24 mW of THz average power with a conversion efficiency of ∼ 0.15% and electric field strength of several tens of kV/cm. At the other available lower repetition rates, we show that the pulse strength and bandwidth of our TDS is unchanged, showing that the THz generation is not affected by thermal effects in this average power region of several tens of watts. The resulting combination of high electric field strength with flexible and high repetition rate is very attractive for spectroscopy, in particular since the system is driven by an industrial and compact laser without the need for external compressors or other specialized pulse manipulation.

Elastic and magnetoelastic properties of TbMnO3single crystal by nanosecond time resolved acoustics and first-principles calculations.

Time resolved pump and probe acoustics and first-principles calculations were employed to assess elastic properties of the TbMnO3perovskite manganite having orthorhombic symmetry. Measuring sound velocities of bulk longitudinal and shear acoustic waves propagating along at least two different directions in the high symmetry planes (100), (010) and (001), provided a powerful mean to selectively determine the six diagonal elastic constantsC11= 227 GPa,C22= 349 GPa,C33= 274 GPa,C44= 71 GPa,C55= 57 GPa,C66= 62 GPa. Among the three remaining off-diagonal ones,C23= 103 GPa was determined with a bissectrice direction. Density functional theory calculations with colinear spin-polarized provided complementary insights on their optical, elastic and magnetoelastic properties.

Giant optical nonlinearity interferences in quantum structures.

Second-order optical nonlinearities can be greatly enhanced by orders of magnitude in resonantly excited nanostructures. These resonant nonlinearities continually attract attention, particularly in newly discovered materials. However, they are frequently not as heightened as currently predicted, limiting their exploitation in nanostructured nonlinear optics. Here, we present a clear-cut theoretical and experimental demonstration that the second-order nonlinear susceptibility can vary by orders of magnitude as a result of giant destructive, as well as constructive, interference effects in complex systems. Using terahertz quantum cascade lasers as a model source to investigate interband and intersubband nonlinearities, we show that these giant interferences are a result of an unexpected interplay of the second-order nonlinear contributions of multiple light and heavy hole states. As well as of importance to understand and engineer the resonant optical properties of nanostructures, this advanced framework can be used as a novel, sensitive tool to elucidate the band structure properties of complex materials.

2D THz spectroscopic investigation of ballistic conduction-band electron dynamics in InSb.

Using reflective cross-polarized 2D THz time-domain spectroscopy in the range of 1-12 THz, we follow the trajectory of the out-of-equilibrium electron population in the low-bandgap semiconductor InSb. The 2D THz spectra show a set of distinct features at combinations of the plasma-edge and vibration frequencies. Using finite difference time domain simulations combined with a tight binding model of the band structure, we assign these features to electronic nonlinearities and show that the nonlinear response in the first picoseconds is dominated by coherent ballistic motion of the electrons. We demonstrate that this technique can be used to investigate the landscape of the band curvature near the Γ-point, as illustrated by the observation of anisotropy in the (100)-plane.

Optical sideband generation up to room temperature with mid-infrared quantum cascade lasers.

Mid-infrared (MIR) sideband generation on a near infrared (NIR) optical carrier is demonstrated within a quantum cascade laser (QCL). By employing an externally injected NIR beam, E(NIR), that is resonant with the interband transitions of the quantum wells in the QCL, the nonlinear susceptibility is enhanced, leading to both frequency mixing and sideband generation. A GaAs-based MIR QCL (E(QCL) = 135 meV) with an aluminum-reinforced waveguide was utilized to overlap the NIR and MIR modes with the optical nonlinearity of the active region. The resulting difference sideband (E(NIR) - E(QCL)) shows a resonant behavior as a function of NIR pump wavelength and a maximum second order nonlinear susceptibility, χ((2)), of ~1 nm/V was obtained. Further, the sideband intensity showed little dependence with the operating temperature of the QCL, allowing sideband generation to be realized at room temperature.