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Register a new userOptical band edge shift of anatase cobalt-doped titanium dioxide
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We report on the optical properties of magnetic cobalt-doped anatase phase titanium dioxide Ti_{1-x}Co_{x}O_{2-d} films for low doping concentrations, 0 <= x <= 0.02, in the spectral range 0.2 to 5 eV. For well oxygenated films (d << 1) the optical conductivity is characterized by an absence of optical absorption below an onset of interband transitions at 3.6 eV and a blue shift of the optical band edge with increasing Co concentration. The absence of below band gap absorption is inconsistent with theoretical models which contain midgap magnetic impurity bands and suggests that strong on-site Coulomb interactions shift the O-band to Co-level optical transitions to energies above the gap.
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Based on first-principles calculations, we predict that the magnetic anisotropy energy (MAE) of Co-doped TiO$_2$ sensitively depends on carrier accumulation. This magnetoelectric phenomenon provides a promising route to directly manipulate the magnetization direction of diluted magnetic semiconductor by external electric-fields. We calculate the band structures and reveal the origin of carrier-dependent MAE in k-space. In fact, the carrier accumulation shifts the Fermi energy and regulates the competing contributions to MAE. The first-principles calculations provide a straightforward way to design spintronics materials with electrically controllable spin direction.
The recent identification of strongly bound excitons in room temperature anatase TiO$_2$ single crystals and nanoparticles underscores the importance of bulk many-body effects in samples used for applications. Here, for the first time, we unravel the interplay between many-body interactions and correlations in highly-excited anatase TiO$_2$ nanoparticles using ultrafast two-dimensional deep-ultraviolet spectroscopy. With this approach, under non-resonant excitation, we disentangle the optical nonlinearities contributing to the bleach of the lowest direct exciton peak. This allows us to clock the ultrafast timescale of the hot electron thermalization in the conduction band with unprecedented temporal resolution, which we determine to be < 50 fs, due to the strong electron-phonon coupling in the material. Our findings call for the design of alternative resonant excitation schemes in photonics and nanotechnology.
Doping of the band insulator FeS$_2$ with Co on the Fe site introduces a small density of itinerant carriers and magnetic moments. The lattice constant, AC and DC magnetic susceptibility, magnetization, and specific heat have been measured over the $0le xle 0.085$ range of Co concentration. The variation of the AC susceptibility with hydrostatic pressure has also been measured in a small number of our samples. All of these quantities show systematic variation with $x$ including a paramagnetic to disordered ferromagnetic transition at $x=0.007pm 0.002$. A detailed analysis of the changes with temperature and magnetic field reveal small power law dependencies at low temperatures for samples near the critical concentration for magnetism, and just above the Curie temperature at higher $x$. In addition, the magnetic susceptibility and specific heat are non-analytic around H=0 displaying an extraordinarily sharp field dependence in this same temperature range. We interpret this behavior as due to the formation of Griffiths phases that result from the quenched disorder inherent in a doped semiconductor.
We have studied magnetism in anatase Ti$_{1-x}$Co$_x$O$_{2-delta}$ ({it x} = 0.05) thin films with various electron carrier densities, by soft x-ray magnetic circular dichroism (XMCD) measurements at the Co $L_{2,3}$ absorption edges. For electrically conducting samples, the magnetic moment estimated by XMCD was $<$ 0.3 $mu_B$/Co using the surface-sensitive total electron yield (TEY) mode, while it was 0.3-2.4 $mu_B$/Co using the bulk-sensitive total fluorescence yield (TFY) mode. The latter value is in the same range as the saturation magnetization 0.6-2.1 $mu_B$/Co deduced by SQUID measurement. The magnetization and the XMCD intensity increased with carrier density, consistent with the carrier-induced origin of the ferromagnetism.
The Hall effect and resistivity of the carrier doped magnetic semiconductor Fe$_{1-x}$Co$_x$S$_2$ were measured for $0le x le 0.16$, temperatures between 0.05 and 300 K, and fields of up to 9 T. Our Hall data indicate electron charge carriers with a density of only 10 to 30% of the Co density of our crystals. Despite the previous identification of magnetic Griffiths phase formation in the magnetic and thermodynamic properties of this system for the same range of $x$, we measure a temperature independent resistivity below 0.5 K indicating Fermi liquid-like transport. We also observe no indication of quantum corrections to the conductivity despite the small values of the product of the Fermi wave vector and the mean-free-path, $1.5 le k_Fell le 15$, over the range of $x$ investigated. This implies a large inelastic scattering rate such that the necessary condition for the observation of quantum contributions to the carrier transport, quantum coherence over times much longer than the elastic scattering time, is not met in our samples. Above 0.5 K we observe a temperature and magnetic field dependent resistivity that closely resembles a Kondo anomaly for $x$ less than that required to form a long range magnetic state, $x_c$. For $x>x_c$, the resistivity and magnetoresistance resemble that of a spin glass with a reduction of the resistivity by as much as 35% in 5 T fields. We also observe an enhancement of the residual resistivity ratio by almost a factor of 2 for samples with $xsim x_c$ indicating temperature dependent scattering mechanisms beyond simple carrier-phonon scattering. We speculate that this enhancement is due to charge carrier scattering from magnetic fluctuations which contribute to the resistivity over a wide temperature range.
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