Spin-dependent electron dynamics in front of a ferromagnetic surface

Exchange splitting and dynamics of image-potential states in front of a 3 monolayer iron film on Cu(100) have been studied with time-, energy-, and spin-resolved bichromatic two-photon photoemission. For the first image-potential state n=1 we observe an exchange splitting of 56 +/- 10 meV and spin-dependent lifetimes of 16 +/- 2 fs for majority-spin and of 11 +/- 2 fs for minority-spin electrons, respectively. The time-resolved studies of both the population and the linewidth of image-potential states manifest that at the magnetic surface not only inelastic but also quasielastic scattering processes are spin dependent.     

Spin-orbit hybridization points in the face-centered-cubic cobalt band structure

Linear magnetic dichroism is observed in spin-, time-, and energy-resolved two-photon photoemission from valence bands of epitaxial fcc cobalt on Cu(001). With image-potential states as spectator states we identify initial bulk and surface states with minority spin character as the source for dichroic intensities and apparent dichroic lifetimes. Excellent agreement with ab initio fully relativistic calculations of the cobalt fcc band structure allows us to precisely determine spin-orbit hybridization points close to the Fermi level. These spin hot spots enhance spin-flip scattering by several orders of magnitude and are therefore assumed to be crucial in ultrafast demagnetization.     

Dynamics of image-potential states on stepped Cu(001) surfaces

The dynamical properties of image-potential states on stepped Cu(117) and Cu(118) surfaces were studied by time- and angle-resolved two-photon photoelectron spectroscopy. The interaction with the step-induced potential leads to quasielastic anisotropic scattering between image-potential-state bands. In particular, resonant interband scattering from image-potential states with quantum numbers n2 to the n=1 band and quasielastic intraband scattering within the n=1 band show high efficiency. In spite of the higher step density of Cu(117), resonant scattering is about four times larger on Cu(118). This distinction is attributed to the different step distributions of the two surfaces and to the concomitant correlation of the step arrangement on short- and long-range scales, which has been studied by scanning tunneling microscopy. Details of the surface band structure lead to different boundary conditions and may weakly affect scattering probabilities. PACS 73.20.At; 79.60.Bm; 79.60.Dp; 79.60.Ht     

Electron scattering at steps: image-potential states on Cu(119)

The dynamics of image-potential states on Cu(119) have been studied with two-photon photoemission. Direction-dependent quasielastic scattering processes with large momentum transfer are attributed to the finite terrace-width distribution on the stepped surface. This effectively couples image-potential states via interband scattering and leads to an asymmetry of the decay rate. Electrons in the first image-potential state live apparently longer when running upstairs.     

Spin-polarized tunneling spectroscopy of co(0001) surface States

Spin-polarized tunneling was studied on Co surfaces of exchange coupled Co/Cu/Co samples, using an Fe tip. A spin-polarized surface state of Co(0001) was found to exist at -0.43 eV relative to E(F), with FWHM of 0.23 eV in the spectra. The state exhibits negative magnetoresistance with an effective spin polarization of less than -23%, suggesting negatively high spin polarization of the surface state. Our first-principles calculations have supported the existence of the surface state. From the calculation, the state is identified as a minority spin Gamma-centered d(2)(z)-like surface state.     

Scattering of hot electrons by adatoms at metal surfaces

The scattering of electrons in image-potential states by Cu adatoms on Cu(001) surfaces has been investigated by means of time- and angle-resolved two-photon photoemission. Several interband and intraband-scattering mechanisms have been identified and their contributions to the total decay of the states determined quantitatively. The adsorbates mainly cause quasielastic scattering processes. Inelastic processes in contrast are due to interactions with electrons in the substrate and are not significantly increased by Cu adatoms. Quasielastic scattering into bulk bands contributes significantly to the depopulation of surface states.     

Ab initio study of mirages and magnetic interactions in quantum corrals

The state of the art ab initio calculations of quantum mirages, the spin polarization of surface-state electrons, and the exchange interaction between magnetic adatoms in Cu and Co corrals on Cu(111) are presented. We find that the spin polarization of the surface-state electrons caused by magnetic adatoms can be projected to a remote location and can be strongly enhanced in corrals, compared to an open surface. Our studies give clear evidence that quantum corrals could permit one to tailor the exchange interaction between magnetic adatoms at large separations.     

Lifetimes of image-potential states on the Pt(111) surface probed by time-resolved two-photon photoemission spectroscopy

We have investigated the population dynamics of image-potential states on the clean Pt(111) surface. The first two image-potential states have been resolved exhibiting lifetimes of 26±7 fs and 62±7 fs. Those lifetimes are in contrast to the (111) surfaces of Ag and Cu, where the n=2 state is degenerate with bulk states leading to lifetimes shorter than 20 fs. Received: 30 March 2000 / Accepted: 2 September 2000 / Published online: 12 October 2000     

Quantum coherence of image-potential states

The quantum dynamics of the two-dimensional image-potential states in front of the Cu(100) surface is measured by scanning tunneling microscopy and spectroscopy. The dispersion relation and the momentum resolved phase-relaxation time of the first image-potential state are determined from the quantum interference patterns in the local density of states at step edges. It is demonstrated that the tip-induced Stark shift does not affect the motion of the electrons parallel to the surface.     

Time-resolved two-color interferometric photoemission of image-potential states on Cu(100)

We describe an interferometric time-resolved photoemission technique that makes it possible to simultaneously observe the decay of optical induced polarizations and populations at surfaces in a two-color excitation scheme. In this scheme initially unoccupied electronic surface states are coherently excited by the interaction of laser pulses with frequency ω_a and the two-photon polarization which is induced by laser pulses with frequency ω_a/2. Interference is observed by changing the delay between both laser pulses using an actively stabilized two-color Mach–Zehnder interferometer. We demonstrate this technique for excitation of the n=1 image-potential state on a Cu(100) surface. PACS 78.47.+p; 79.60.Bm; 73.20.-r; 82.53.Kp; 42.50.Md     

Interferometric control of spin-polarized electron populations at a metal surface observed by multiphoton photoemission

In an interferometric pump-probe experiment, we demonstrate the phase tuning of the spin polarization of photoelectrons emitted in a three-photon process from Cu(001). A phase shift of pi between delayed ultrafast circularly polarized light pulses can switch the spin polarization from +/-20% to -/+40%. In the delay regime of overlapping pulses, we show the dominating role of optical interference effects in determining the spin polarization. For longer delays, we detect the influence of the coherent material response, manifested in both the final state electron population as well as the final state spin polarization.     

Image-potential states on stepped Cu (001) surfaces

Image-potential states on Cu (117) and Cu (119) surfaces were studied by means of two-photon photoelectron spectroscopy. The regular array of steps generates a lateral potential on the vicinal surfaces, which modifies the surface-electronic structure. Compared to Cu (001), the band bottom of the n=1 image-potential states shifts by 40 meV to lower binding energy. The periodicity of the step-induced superlattice manifests itself as back-folding of the n=1 and 2 dispersion bands. At the surface Brillouin zone boundary a mini-gap opens with a width of 135 meV for the first image-potential state on Cu (117). On the vicinal surfaces the lifetime of the image-potential states is reduced by a factor of three as compared to Cu (001). This is attributed to a narrowing of the surface-projected bulk-band gap when projected along the [11n] direction. While the dephasing rate of the first image-potential state is close to the decay rate, higher members of the Rydberg-like series show negligible dephasing. Received: 16 October 2001 / Revised version: 9 April 2002 / Published online: 6 June 2002     

自旋极化对Kondo系统基态的影响

Anderson模型中的自旋极化效应是一个普遍存在的问题.本文从Anderson杂质模型出发,利用变分及对角化方法分析了自旋极化所引起的系统基态性质的改变,分别研究了自旋极化对Kondo单态以及高温超导两分量模型中Zhang-Rice单态稳定性的影响问题.     

Reversal of spin polarization in Fe/GaAs (001) driven by resonant surface states: first-principles calculations

A minority-spin resonant state at the Fe/GaAs(001) interface is predicted to reverse the spin polarization with the voltage bias of electrons transmitted across this interface. Using a Green's function approach within the local spin-density approximation, we calculate the spin-dependent current in a Fe/GaAs/Cu tunnel junction as a function of the applied bias voltage. We find a change in sign of the spin polarization of tunneling electrons with bias voltage due to the interface minority-spin resonance. This result explains recent experimental data on spin injection in Fe/GaAs contacts and on tunneling magnetoresistance in Fe/GaAs/Fe magnetic tunnel junctions.     

Coherent storage of photoexcited triplet states using 29Si nuclear spins in silicon

Pulsed electron paramagnetic resonance spectroscopy of the photoexcited, metastable triplet state of the oxygen-vacancy center in silicon reveals that the lifetime of the m(s)=±1 sublevels differs significantly from that of the m(s)=0 state. We exploit this significant difference in decay rates to the ground singlet state to achieve nearly ~100% electron-spin polarization within the triplet. We further demonstrate the transfer of a coherent state of the triplet electron spin to, and from, a hyperfine-coupled, nearest-neighbor (29)Si nuclear spin. We measure the coherence time of the (29)Si nuclear spin employed in this operation and find it to be unaffected by the presence of the triplet electron spin and equal to the bulk value measured by nuclear magnetic resonance.     

Time-resolved two-photon photoemission of unoccupied electronic states of periodically rippled graphene on Ru(0001)

The unoccupied electronic states of epitaxially grown graphene on Ru(0001) have been explored by time- and angle-resolved two-photon photoemission. We identify a Ru derived resonance and a Ru/graphene interface state at 0.91 and 2.58?eV above the Fermi level, as well as three image-potential derived states close to the vacuum level. The most strongly bound, short-lived, and least dispersing image-potential state is suggested to have some quantum-well character with a large amplitude below the graphene hills. The two other image-potential states are attributed to a series of slightly decoupled states. Their lifetimes and dispersions are indicative of electrons moving almost freely above the valley areas of the moiré superstructure of graphene.     

Controlling the spin polarization of nanostructures on magnetic substrates

It is shown that, by utilizing spin-selective quantum interference, the spin polarization of nanostructures deposited on a magnetic substrate with a surface state can be strongly modulated locally and energetically by an appropriate structural design. This finding is deduced from state-of-the-art ab initio calculations and interpreted within an analytical model. We present results for hexagonal Cu corrals and mesoscopic triangular Co islands on Co-covered Cu(111). These systems are experimentally feasible, and the effect should be detectable with current technology.     

Scattering by Cu adatoms between image-potential bands on Cu(001)

With the increasing resolution and sensitivity of photoelectron spectroscopy, the influence of defects is becoming more and more obvious. Scattering processes induced by adsorbate atoms can be studied by time- and angle-resolved two-photon photoemission. We have examined the dynamics of electrons in image-potential states on the Cu(001) surface for statistically distributed Cu adatoms and have identified different scattering mechanisms. Scattering of electrons from the second (n=2) to the bottom of the first (n=1) image-potential band is observed, which we attribute to inelastic interband scattering with electrons in the bulk. At energies above the bottom of the n=2 band, resonant interband scattering from the n=2 to the n=1 image-potential band is found. The rate for these processes can be determined by modeling the time-resolved measurements via optical Bloch equations of a four-level system. Comparison of the transition and decay rates reveals that the decay rate of the n=2 electrons is almost exclusively changed by additional resonant interband-scattering processes upon adsorption. PACS 73.20.At; 79.60.Ht; 68.49.Jk     

Transport properties and electronic structure of epitaxial tunnel junctions

We present ab initio calculations for the electronic ground-state and transport properties of epitaxial Fe/semiconductor/Fe (0 0 1) tunnel junctions. The ground state properties are determined by the ab initio Screened KKR Green's function method and the transport properties by a Green's function formulation of the Landauer–Büttiker formalism. We focus on tunnel junctions with a semiconducting ZnSe barrier and compare them to results for junctions with Si and GaAs barriers. We comment on the presence of metal-induced gap states (MIGS) in the semiconductor, the spin polarization of which strongly depends on the nature of the barrier. We investigate furthermore the influence of one atomic layer at the interface of a non-magnetic metal (Cu, Ag, Al) and of a magnetic 3d transition metal.     

Observing spin polarization of individual magnetic adatoms

We have used spin-polarized scanning tunneling spectroscopy to observe the spin polarization state of individual Fe and Cr atoms adsorbed onto Co nanoislands. These magnetic adatoms exhibit stationary out-of-plane spin polarization, but have opposite sign of the exchange coupling between electron states of the adatom and the Co island surface state: Fe adatoms exhibit parallel spin polarization to the Co surface state while Cr adatoms exhibit antiparallel spin polarization. First-principles calculations predict ferromagnetic and antiferromagnetic alignment of the spin moment for individual Fe and Cr adatoms on a Co film, respectively, implying negative spin polarization for Fe and Cr adatoms over the energy range of the Co surface state.