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We study how the color and polarization of ultrashort pulses of visible light can be used to control the demagnetization processes of the antiferromagnetic insulator Cr$_2$O$_3$. We utilize time-resolved second harmonic generation (SHG) to probe how changes in the magnetic and structural state evolve in time. We show that, varying the pump photon-energy to excite either localized transitions within the Cr or charge transfer states, leads to markedly different dynamics. Through a full polarization analysis of the SHG signal, symmetry considerations and density functional theory calculations, we show that, in the non-equilibrium state, SHG is sensitive to {em both} lattice displacements and changes to the magnetic order, which allows us to conclude that different excited states couple to phonon modes of different symmetries. Furthermore, the spin-scattering rate depends on the induced distortion, enabling us to control the timescale for the demagnetization process. Our results suggest that selective photoexcitation of antiferromagnetic insulators allows fast and efficient manipulation of their magnetic state.
The mechanism underlying femtosecond laser pulse induced ultrafast magnetization dynamics remains elusive despite two decades of intense research on this phenomenon. Most experiments focused so far on characterizing magnetization and charge carrier d
We investigate exemplary the longitudinal optical (LO) mode order in compounds with a plasmon or plasmon-like phonon mode and additional phonon modes. When the oscillator strength of the plasmon or plasmon-like mode is gradually increased, a reorderi
The Raman effect -- inelastic scattering of light by lattice vibrations (phonons) -- produces an optical response closely tied to a materials crystal structure. Here we show that resonant optical excitation of IR and Raman phonons gives rise to a Ram
We report a comprehensive muon spin rotation ($mu$SR) study of the prototypical magnetoelectric antiferromagnet Cr$_2$O$_3$. We find the positively charged muon ($mu^+$) occupies several distinct interstitial sites, and displays a rich dynamic behavi
Point defects in crystalline materials often occur in multiple charge states. Although many experimental methods to study and explore point defects are available, techniques to explore the non-equilibrium dynamics of the charge states of these defect