Ultrafast optical observation of spin-pumping induced dynamic exchange coupling in ferromagnetic semiconductor/metal bilayer.

Spin angular momentum transfer in magnetic bilayers offers the possibility of ultrafast and low-loss operation for next-generation spintronic devices. We report the field- and temperature- dependent measurements on the magnetization precessions in Co2FeAl/(Ga,Mn)As by time-resolved magneto-optical Kerr effect. Analysis of the effective Gilbert damping and phase shift indicates a clear signature of an enhanced dynamic exchange coupling between the two ferromagnetic (FM) layers due to the reinforced spin pumping at resonance. The temperature dependence of the dynamic exchange-coupling reveals a primary contribution from the ferromagnetism in (Ga,Mn)As.

Spin-polarized current injection induced magnetic reconstruction at oxide interface.

Electrical manipulation of magnetism presents a promising way towards using the spin degree of freedom in very fast, low-power electronic devices. Though there has been tremendous progress in electrical control of magnetic properties using ferromagnetic (FM) nanostructures, an opportunity of manipulating antiferromagnetic (AFM) states should offer another route for creating a broad range of new enabling technologies. Here we selectively probe the interface magnetization of SrTiO3/La0.5Ca0.5MnO3/La0.7Sr0.3MnO3 heterojunctions and discover a new spin-polarized current injection induced interface magnetoelectric (ME) effect. The accumulation of majority spins at the interface causes a sudden, reversible transition of the spin alignment of interfacial Mn ions from AFM to FM exchange-coupled, while the injection of minority electron spins alters the interface magnetization from C-type to A-type AFM state. In contrast, the bulk magnetization remains unchanged. We attribute the current-induced interface ME effect to modulations of the strong double-exchange interaction between conducting electron spins and local magnetic moments. The effect is robust and may serve as a viable route for electronic and spintronic applications.

Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes.

Optical control of spin is of central importance in the research of ultrafast spintronic devices utilizing spin dynamics at short time scales. Recently developed optical approaches such as ultrafast demagnetization, spin-transfer and spin-orbit torques open new pathways to manipulate spin through its interaction with photon, orbit, charge or phonon. However, these processes are limited by either the long thermal recovery time or the low-temperature requirement. Here we experimentally demonstrate ultrafast coherent spin precession via optical charge-transfer processes in the exchange-coupled Fe/CoO system at room temperature. The efficiency of spin precession excitation is significantly higher and the recovery time of the exchange-coupling torque is much shorter than for the demagnetization procedure, which is desirable for fast switching. The exchange coupling is a key issue in spin valves and tunnelling junctions, and hence our findings will help promote the development of exchange-coupled device concepts for ultrafast coherent spin manipulation.

Exchange bias of the interface spin system at the Fe/MgO interface.

The ferromagnet/oxide interface is key to developing emerging multiferroic and spintronic technologies with new functionality. Here we probe the Fe/MgO interface magnetization, and identify a new exchange bias phenomenon manifested only in the interface spin system, and not in the bulk. The interface magnetization exhibits a pronounced exchange bias, and the hysteresis loop is shifted entirely to one side of the zero field axis. However, the bulk magnetization does not, in marked contrast to typical systems where exchange bias is manifested in the net magnetization. This reveals the existence of an antiferromagnetic exchange pinning layer at the interface, identified here as FeO patches that exist even for a nominally 'clean' interface. These results demonstrate that atomic moments at the interface are non-collinear with the bulk magnetization, and therefore may affect the net anisotropy or serve as spin scattering sites. We control the exchange bias magnitude by varying the interface oxygen concentration and Fe-O bonding.

Quadratic scaling of intrinsic Gilbert damping with spin-orbital coupling in L10 FePdPt films: experiments and Ab initio calculations.

The dependence of the intrinsic Gilbert damping parameter α(0) on the spin-orbital coupling strength ξ is investigated in L1(0) ordered FePd(1-x) Pt(x) films by time-resolved magneto-optical Kerr effect measurements and spin-dependent ab initio calculations. Continuous tuning of α(0) over more than one order of magnitude is realized by changing the Pt/Pd concentration ratio showing that α(0) is proportional to ξ(2) as changes of other leading parameters are found to be negligible. The perpendicular magnetic anisotropy is shown to have a similar variation trend with x. The present results may facilitate the design and fabrication of new magnetic alloys with large perpendicular magnetic anisotropy and tailored damping properties.

Coherent spin precession via photoinduced antiferromagnetic interactions in La0.67Ca0.33MnO3.

Pronounced spin precessions are observed in a geometry with negligible canting of the magnetization in ferromagnetic La(0.67)Ca(0.33)MnO(3) thin films using the time-resolved magneto-optical Kerr effect. The precession amplitude monotonically decreases with increasing field, indicating that the coherent spin rotation may be triggered by a transient exchange field and not by demagnetization and/or anisotropy field modulation. We attribute the transient exchange field to emergent antiferromagnetic interactions due to charge transfer and modification of the kinetic energy of e(g) electrons under optical excitation.

Giant enhancement of hydrogen transport in rutile TiO2 at low temperatures.

Measurements of the O-H and O-D vibrational lifetimes show that the room-temperature hydrogen diffusion rate in rutile TiO2 can be enhanced by 9 orders of magnitude when stimulated by resonant infrared light. We find that the local oscillatory motion of the proton quickly couples to a wag-mode-assisted classical transfer process along the c channel with a jump rate of greater than 1 THz and a barrier height of 0.2 eV. This increase in proton transport rate at moderate temperatures provides new insight into hydrogen transport in solids, which could play a role in applications ranging from fuel cells to hydrogen production.

Proton tunneling: a decay channel of the O-H stretch mode in KTaO3.

The vibrational lifetimes of the O-H and O-D stretch modes in the perovskite oxide KTaO3 are measured by pump-probe infrared spectroscopy. Both stretch modes are exceptionally long lived and exhibit a large "reverse" isotope effect, due to a phonon-assisted proton-tunneling process, which involves the O-Ta-O bending motion. The excited-state tunneling rate is found to be 7 orders of magnitude larger than from the ground state in the proton conducting oxide, BaCeO3 [Phys. Rev. B 60, R3713 (1999)].

Viscous spin exchange torque on precessional magnetization in (LaMnO3)2n/(SrMnO3)n superlattices.

Photoinduced magnetization dynamics is investigated in chemically ordered (LaMnO3)2n/(SrMnO3)n superlattices using the time-resolved magneto-optic Kerr effect. A monotonic frequency-field dependence is observed for the n=1 superlattice, indicating a single spin population consistent with a homogeneous hole distribution. In contrast, for n> or =2 superlattices, a large precession frequency is observed at low fields indicating the presence of an exchange torque in the dynamic regime. We attribute the emergence of exchange torque to the coupling between two spin populations-viscous and fast spins.

Vibrational lifetimes and frequency-gap law of hydrogen bending modes in semiconductors.

Vibrational lifetimes of hydrogen and deuterium related bending modes in semiconductors are measured by transient bleaching spectroscopy and high-resolution infrared absorption spectroscopy. We find that the vibrational lifetimes follow a universal frequency-gap law; i.e., the decay time increases exponentially with increasing decay order, with values ranging from 1 ps for a one-phonon process to 265 ps for a four-phonon process. The temperature dependence of the lifetime shows that the bending mode decays by lowest-order multiphonon process. Our results provide new insights into vibrational decay and the giant isotope effect of hydrogen in semiconductor systems.

Interface magnetization reversal and anisotropy in Fe/AlGaAs(001).

The reversal process of the Fe interface layer magnetization in Fe/AlGaAs heterostructures is measured directly using magnetization-induced second-harmonic generation, and is compared with the reversal of the bulk magnetization as obtained from magneto-optic Kerr effect. The switching characteristics are distinctly different due to interface-derived anisotropy--single step switching occurs at the interface layer, while two-jump switching occurs in the bulk Fe for the magnetic field orientations employed. The angle between the interface and bulk magnetization may be as large as 40-85 degrees. Such interface switching will dominate the behavior of nanoscale structures.

Ultrafast photoinduced reflectivity transients in doped manganite.

The temperature and magnetic field dependence of ultrafast photoinduced spin and quasiparticle relaxation dynamics is reported in La(0.67)Ca(0.33)MnO(3) and LaMnO(3) single crystals and thin films. Both manganites reveal an unusually slow ( approximately 10 micros) carrier relaxation process attributed to the spin-lattice relaxation in localized states. The quasiparticle dynamics is governed by the temperature- and magnetic field-dependent pseudogap in La(0.67)Ca(0.33)MnO(3), and by the temperature-independent Jahn-Teller gap in LaMnO(3). The loss of spectral weight near the Fermi level in La(0.67)Ca(0.33)MnO(3) strongy affects the quasiparticle relaxation dynamics as temperature increases from below T(C). Our results show that the coupled dynamics of charge, spin and lattice is strongly correlated with the distinct gap structures in these manganites.

Vibrational lifetimes and isotope effects of interstitial oxygen in silicon and germanium.

Decay dynamics of local vibrational modes provides unique information about energy relaxation processes to solid-state phonon bath. In this Letter the lifetimes of the asymmetric stretch mode of interstitial 16O and 17O isotopes in Si are measured at 10 K directly by time-resolved, transient bleaching spectroscopy to be 11.5 and 4.5 ps, respectively. A calculation of the three-phonon density of states shows that the 17O mode lies in the highest phonon density resulting in the shortest lifetime. The lifetime of the 16O mode in Ge is measured to be 125 ps, i.e., approximately 10 times longer than in Si. The interaction between the local modes and the lattice vibrations is discussed according to the activity of phonon combinations.

Structure-dependent vibrational lifetimes of hydrogen in silicon.

The lifetimes of the Si-H vibrational stretch modes of the H(*)(2) ( 2062 cm(-1)) and HV.VH((110)) ( 2072.5 cm(-1)) defects in crystalline Si are measured directly by transient bleaching spectroscopy from 10 K to room temperature. The interstitial-type defect H(*)(2) has a lifetime of 4.2 ps at 10 K, whereas the lifetime of the vacancy-type complex HV.VH((110)) is 2 orders of magnitude longer, 295 ps. The temperature dependence of the lifetime of H(*)(2) is governed by TA phonons, while HV.VH((110)) is governed by LA phonons. This behavior is attributed to the distinctly different local structure of these defects and the accompanying local vibrational modes.

Lifetimes of hydrogen and deuterium related vibrational modes in silicon.

Lifetimes of hydrogen and deuterium related stretch modes in Si are measured by high-resolution infrared absorption spectroscopy and transient bleaching spectroscopy. The lifetimes are found to be extremely dependent on the defect structure, ranging from 2 to 295 ps. Against conventional wisdom, we find that lifetimes of Si-D modes typically are longer than for the corresponding Si-H modes. The potential implications of the results on the physics of electronic device degradation are discussed.

Vibrational lifetime of bond-center hydrogen in crystalline silicon

The lifetime of the stretch mode of bond-center hydrogen in crystalline silicon is measured to be T1 = 7.8+/-0.2 ps with time-resolved, transient bleaching spectroscopy. The low-temperature spectral width of the absorption line due to the stretch mode converges towards its natural width for decreasing hydrogen concentration C(H), and nearly coincides with the natural width for C(H) approximately 1 ppm. The lifetimes of the Si-H stretch modes of selected hydrogen-related defects are estimated from their spectral widths and shown to range from 1.6 to more than 37 ps.

Exact separation of surface and bulk contributions to anisotropic second-harmonic generation from cubic centrosymmetric media.

We solve this long-standing problem theoretically by recognizing that the ranks of the tensors that describe the surface and bulk second-order nonlinear susceptibilities differ in this class of media. We show that this implies that the phenomenologies of the anisotropic optical second-harmonic (SH) responses of the two sources differ for all possible crystal facial orientations except (111). To demonstrate the result, we apply the theory to separate the surface and bulk contributions to SH generation from an oxidized vicinal Si(001) wafer for p-polarized 775-nm fundamental and s-polarized SH radiation. It is shown that knowledge of the phase of the SH field is necessary to achieve a unique separation.

Optical second-harmonic generation as a probe of electric-field-induced perturbation of centrosymmetric media.

Polarization-selective optical second-harmonic generation (SHG) is applied to monitor nonuniform polarization distributions in centrosymmetric media modulated by an external dc electric field. Two different systems are investigated: first, optical SHG from a Au-Si(100) Schottky Barrier is shown to be a direct probe of the electric field polarity near such a metal-semiconductor interface. Second, a poled polymer exhibits a strong anisotropic SHG signal under normal incidence, indicating a nonuniform field enhancement at the edges of the poling electrode. The results demonstrate the sensitivity of SHG to small symmetry perturbations. Consequences for device applications are discussed.