Ferromagnetism and superconductivity are antagonistic phenomena. Their coexistence implies either a modulated ferromagnetic order parameter on a lengthscale shorter than the superconducting coherence length or a weak exchange coupling between the itinerant superconducting electrons and the localized ordered spins. In some iron based pnictide superconductors the coexistence of ferromagnetism and superconductivity has been clearly demonstrated. The nature of the coexistence, however, remains elusive since no clear understanding of the spin structure in the superconducting state has been reached and the reports on the coupling strength are controversial. We show, by a direct optical pump-probe experiment, that the coupling is weak, since the transfer of the excess energy from the itinerant electrons to ordered localized spins is much slower than the electron-phonon relaxation, implying the coexistence without the short-lengthscale ferromagnetic order parameter modulation. Remarkably, the polarization analysis of the coherently excited spin wave response points towards a simple ferromagnetic ordering of spins with two distinct types of ferromagnetic domains.
We systematically investigate temperature-and spectrally-dependent optical reflectivity dynamics in AAs2Fe2, (A=Ba, Sr and Eu), iron-based superconductors parent spin-density-wave (SDW) compounds. Two different relaxation processes are identified. The behavior of the slower process, which is strongly sensitive to the magneto-structural transition, is analyzed in the framework of the relaxation-bottleneck model involving magnons. The results are compared to recent time resolved angular photoemission results (TR-ARPES) and possible alternative assignment of the slower relaxation to the magneto-structural order parameter relaxation is discussed.
We report on systematic excitation-density dependent all-optical femtosecond time resolved study of the spin-density wave state in iron-based superconductors. The destruction and recovery dynamics are measured by means of the standard and a multi-pulse pump-probe technique. The experimental data are analyzed and interpreted in the framework of an extended three temperature model. The analysis suggests that the optical-phonons energy-relaxation plays an important role in the recovery of almost exclusively electronically driven spin density wave order.
Magneto-optical spectroscopy in fields up to 30 Tesla reveals anomalies in the equilibrium and ultrafast magnetic properties of the ferrimagnetic rare-earth-transition metal alloy TbFeCo. In particular, in the vicinity of the magnetization compensation temperature, each of the magnetizations of the antiferromagnetically coupled Tb and FeCo sublattices show triple hysteresis loops. Contrary to state-of-the-art theory, which explains such loops by sample inhomogeneities, here we show that they are an intrinsic property of the rare-earth ferrimagnets. Assuming that the rare-earth ions are paramagnetic and have a non-zero orbital momentum in the ground state and, therefore, a large magnetic anisotropy, we are able to reproduce the experimentally observed behavior in equilibrium. The same theory is also able to describe the experimentally observed critical slowdown of the spin dynamics in the vicinity of the magnetization compensation temperature, emphasizing the role played by the orbital momentum in static and ultrafast magnetism of ferrimagnets.
Temperature and fluence dependence of the 1.55-eV optical transient reflectivity in BaFe2(As1−xPx)2 was measured and analysed in the low and high excitation density limit. The effective magnitude of the superconducting gap of ∼5 meV obtained from the low-fluence-data bottleneck model fit is consistent with the ARPES results for the γ-hole Fermi surface. The superconducting-state nonthermal optical destruction energy was determined from the fluence dependent data. The in-plane optical destruction energy scales well with T 2 c and is found to be similar in a number of different layered superconductors.
Spontaneous vibrational Raman scattering is a ubiquitous form of light–matter interaction whose description necessitates quantization of the electromagnetic field. It is usually considered as an incoherent process because the scattered field lacks any predictable phase relationship with the incoming field. When probing an ensemble of molecules, the question therefore arises: What quantum state should be used to describe the molecular ensemble following spontaneous Stokes scattering? We experimentally address this question by measuring time-resolved Stokes–anti-Stokes two-photon coincidences on a molecular liquid consisting of several sub-ensembles with slightly different vibrational frequencies. When spontaneously scattered Stokes photons and subsequent anti-Stokes photons are detected into a single spatiotemporal mode, the observed dynamics is inconsistent with a statistical mixture of individually excited molecules. Instead, we show that the data are reproduced if Stokes–anti-Stokes correlations are mediated by a collective vibrational quantum, i.e. a coherent superposition of all molecules interacting with light. Our results demonstrate that the degree of coherence in the vibrational state of the liquid is not an intrinsic property of the material system, but rather depends on the optical excitation and detection geometry.
Here we report that femtosecond laser pulses are able to trigger oscillations of the magneto-optical Faraday rotation in the ferromagnetic semiconductor CdCr 2 Se 4 in the presence of an applied magnetic field. The frequency of these oscillations is a linear function of the magnetic field and corresponds to the ferromagnetic resonance (FMR). Tuning the photon energy of the pump pulses we reveal two different mechanisms, which induce FMR precession in this material. In the case of pumping from the valence band deep into the conduction band (photon energy 3.1 eV), the phase of the spin oscillations is not sensitive to the polarization of the pump, but can be reversed over 180 deg by changing the polarity of the applied magnetic field. We assign these oscillations to the coherent spin precession triggered by ultrafast laser-induced heating. This mechanism requires a strong optical absorption in the material and becomes inactive if the pump photon energy is below the band gap. Tuning the photon energy in a wide range from 0.88 to 2.1 eV reveals the second mechanism of optical excitation of coherent spin oscillations with a maximum around 1.2 eV, i.e., very close to the energy of the band gap in the semiconductor. Contrary to the laser-induced heating, this excitation mechanism is pump polarization dependent, being the most efficient if the pump is circularly polarized. The phase of the spin oscillations is independent of the polarity of the applied magnetic field, but changes by 180 deg under reversing the helicity of light. We suggest that the effect can be interpreted in terms of spin transfer torque experienced by the network of the ordered Cr 3+ spins as a result of excitation of electrons from the top of the p-type valence band to the bottom of the s-type conduction band. In particular, a strong spin-orbit interaction experienced by the carriers in the valence band is responsible for the coupling of the spins of the photogenerated carriers and the polarization of light. Due to strong pdand sd-exchange interactions the spins of the photocarriers appear to be coupled to the network of ordered spins of the Cr 3+ ions.
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