Probing the electronic and spintronic properties of buried interfaces by extremely low energy photoemission spectroscopy


Probing the electronic and spintronic properties of buried interfaces by extremely low energy photoemission spectroscopy

Play all audios:


ABSTRACT Ultraviolet photoemission spectroscopy (UPS) is a powerful tool to study the electronic spin and symmetry features at both surfaces and interfaces to ultrathin top layers. However,


the very low mean free path of the photoelectrons usually prevents a direct access to the properties of buried interfaces. The latter are of particular interest since they crucially


influence the performance of spintronic devices like magnetic tunnel junctions (MTJs). Here, we introduce spin-resolved extremely low energy photoemission spectroscopy (ELEPS) to provide a


powerful way for overcoming this limitation. We apply ELEPS to the interface formed between the half-metallic Heusler compound Co2MnSi and the insulator MgO, prepared as in state-of-the-art


Co2MnSi/MgO-based MTJs. The high accordance between the spintronic fingerprint of the free Co2MnSi surface and the Co2MnSi/MgO interface buried below up to 4 nm MgO provides clear evidence


for the high interface sensitivity of ELEPS to buried interfaces. Although the absolute values of the interface spin polarization are well below 100%, the now accessible spin- and


symmetry-resolved wave functions are in line with the predicted existence of non-collinear spin moments at the Co2MnSi/MgO interface, one of the mechanisms evoked to explain the


controversially discussed performance loss of Heusler-based MTJs at room temperature. SIMILAR CONTENT BEING VIEWED BY OTHERS DETERMINATION OF THE EMBEDDED ELECTRONIC STATES AT NANOSCALE


INTERFACE VIA SURFACE-SENSITIVE PHOTOEMISSION SPECTROSCOPY Article Open access 27 July 2021 SPIN AND VALLEY DEPENDENT TRANSPORT AND TUNNELING MAGNETORESISTANCE IN IRRADIATED FERROMAGNETIC


WSE2DOUBLE BARRIER JUNCTIONS Article Open access 06 January 2025 GIANT SPIN-TO-CHARGE CONVERSION AT AN ALL-EPITAXIAL SINGLE-CRYSTAL-OXIDE RASHBA INTERFACE WITH A STRONGLY CORRELATED METAL


INTERLAYER Article Open access 26 September 2022 INTRODUCTION Magnetic tunnel junctions (MTJs) are essential parts of many magnetic storage devices. Typically, they can be found in magnetic


hard-disks as high sensitivity read-heads or in non-volatile and fast-access magnetic random access memory elements as basic building block1,2. These structures consist of two ferromagnetic


electrodes separated only by a few-nanometer thin insulating layer. The relative magnetization direction of the two ferromagnetic metals (FM), i.e., the electrodes, is directly reflected in


the tunneling current across the MTJ. While a parallel orientation of the magnetization in the ferromagnetic films results in a high tunneling current, an anti-parallel orientation leads to


a significantly lower tunneling current. Therefore, MTJs show the distinct behavior of a two level system which can be switched by an external magnetic field and hence be employed in a


variety of logical circuits. The applicability of MTJs in storage devices crucially depends on the difference between the resistance of these two states, the so called tunnel


magneto-resistance ratio, which is a direct result of the intrinsic properties of the MTJs. In particular, to improve the performance of the MTJs, the fundamental electronic properties of


the buried ferromagnetic metal/insulator interface have to be revealed. The importance of the interface results from the fact that only electrons from the outermost FM layers can participate


to the tunneling process3,4. For high efficiency MTJs using epitaxial MgO barriers as insulating layer, the spin-dependent tunneling properties crucially depend not only on the interface


spin polarization, but also on the wave function symmetry of the electronic states near _E__F_ at that buried FM/MgO interface5,6. Up to now, spin-resolved ultraviolet photoemission


spectroscopy (UPS) is the only existing method capable of revealing both the electronic spin and symmetry properties at interfaces7. However, sample structures are constrained to FM


substrates with ultrathin insulator top layers of 1–2 ML (i.e. less than 0.5 nm)8, whereas direct access to interfaces buried below thicker insulator layers comparable to actual devices


(i.e. 1–2 nm) is experimentally very challenging due to the very low mean free path of electrons in materials9. This is quite a drawback of UPS, since the interface properties themselves


depend on the thickness of the insulating layer10. Recently, significant process in the development of high brilliant photon sources (3rd generation synchrotron light sources) allowed to


increase the escape depth of electrons to a few nanometers by using hard X-ray photons of several hundreds of electron volts (HAXPES) which resulted in the first studies of the electronic


structure of buried interfaces11. However, the low cross section for the photoemission process in the HAXPES experiment (especially for electronic states close to the Fermi level) is still a


huge challenge when studying the corresponding spin properties of buried interfaces. In addition, the experiment becomes distinctively bulk-sensitive. Consequently, alternative approaches


are essential to extend our knowledge of buried interfaces in electronic and spintronic assemblies. Here, we demonstrate how spin-resolved extremely low energy photoemission spectroscopy


(ELEPS) performed with photon energy of 5.9 eV can be used to study the electronic and spintronic properties of buried interfaces between a ferromagnetic metal (FM) and an insulator. As


FM/insulator structure, we choose materials suited for high performance MTJs. One of the most promising ferromagnetic materials in this context are fully spin polarized half-metallic


ferromagnets such as the cobalt-based full Heusler compound Co2MnSi. This material has a high Curie Temperature (985 K)12 and a predicted minority band gap around the Fermi energy (_E__F_)


with a width of 0.4–0.8 eV13,14, that should lead to a full spin polarization at _E__F_. Epitaxial MgO, commonly used as insulating material in magnetic tunnel junctions due to its


symmetry-filtering properties5,6, is grown on top of the Heusler complex. The studied Co2MnSi/MgO interfaces have been deposited using the exact same parameters as in the production of


state-of-the-art Co2MnSi-based MTJs. These devices show superior performance, with TMR ratios between 750% and 1135% at cryogenic temperatures15,16. In our ELEPS experiments we find that the


properties of such Co2MnSi/MgO interfaces are accessible for MgO overlayers with thickness up to 4 nm (20 ML), making ELEPS a unique method for the non-destructive characterization of


buried spintronics interfaces, as found in state-of-the-art Co2MnSi/MgO-based MTJs17. Taking advantage of such interface sensitivity we report a room-temperature interface spin polarization


of ≈40% at the Fermi energy, in striking contrast with Ref. 18, where a nearly full spin polarization (93%) is reported for the free Co2MnSi surface. In principle, there are two possible


explanations for the reduced spin polarization: (i) temperature effects, or (ii) effects inherent to the photoemission process18. Regarding the temperature-related effects (i), we recall


that although Co2MnSi-based MTJs show strongly enhanced tunnel magneto-resistance ratios19 at liquid helium temperature compared to MTJs based on conventional 3_d_ ferromagnetic materials20,


the superiority is lost at room temperature15. This behavior is commonly ascribed to a strong temperature-dependence of the spin polarization at the Co2MnSi/MgO interface, but a clear


microscopic understanding is still lacking. In particular, two different main mechanisms have been proposed, schematically depicted in Fig. 1 (a). The first mechanism is the formation of


additional minority band gap states or the shifting of existing minority states inside the band gap. These processes can arise either from peculiarities of the magnetic sublattices21, from


the existence of non-quasiparticle states22, from spin wave excitations23 or from strong hybridization dependence on temperature24. At room temperature, all such processes lead to finite


minority spectral contributions near _E__F_ that will differ in energy dispersion and symmetry compared to the majority states at same binding energy. The second mechanism is the formation


of non-collinear spin moments inside the half-metal bulk as well as at the interface24,25,26, leading to a mirroring of majority states into the minority channel and hence to minority gap


states with the same wave function symmetry as the majority states. Regarding the photoemission-related mechanisms (ii), it was recently suggested18 that correlation effects in the


photoemission process together with the finite energy resolution of standard spin-detectors can cause a reduction of the detected spin polarization from the nominal 100% down to ≈50%. In


order to distinguish between all the possible contributions resulting in a lowering of the spin-polarization at room temperature, we will make use of the further possibility of ELEPS to


resolve the relevant wave function symmetries (Δ1 and Δ5), demonstrating the high potential of ELEPS for the non-destructive characterization of the spin properties of buried FM/insulator


spintronics interfaces. RESULTS THE CO2MNSI(100) FREE SURFACE As a basis to understand the results on the Co2MnSi/MgO interface, we start discussing here the results obtained from the bare


Co2MnSi(100) surface. Note that the photoemission experiments from the free surface have been performed after those on the interface; to do so we removed the MgO overlayer by Ar+ ion


sputtering (see Methods). In general, the photoemission signal obtained in our experiments stems mainly from initial electronic states near _E__F_ with either Δ5 or Δ1 wavefunction symmetry,


located within the Γ – _X_ part of the Co2MnSi Brillouin zone27 (see Methods). Please note that exactly these states contribute almost exclusively to the tunneling current in the respective


MTJ devices5,28. Changing the light polarization furthermore allows us to distinguish between the two wave function symmetries, as linearly s-polarized light excites only Δ5 states, while


p-polarized light probes additionally Δ1 states7,27. This feature is one huge advantage (amongst others) of spin-resolved photoemission spectroscopy compared to further spin-sensitive


experiments like Point contact Andreev reflection29 or the Meservey & Tedrow technique3. The lower panels of Fig. 1 (b) show the spin-resolved ELEPS spectra measured with s-polarized


(left) and p-polarized laser light (right), while the upper panels exhibit the respective spin polarization. The latter one is calculated from the experimentally obtained majority and


minority spectra (_N_↑ and _N_↓, respectively) as . In this section as well as in the further ones, we will focus on the features found close the Fermi level, the energy region where


spin-polarized charge transport takes place in spintronics devices. In case of s-polarization, we find a rather low photoemission yield directly at _E__F_ (additionally cut by the


Fermi-Dirac distribution), getting more intense for binding energies higher then 0.4 eV. This is expected from bulk band structure calculations, which predict Δ1 and Δ5 bands along the Γ –


_X_ direction with strong dispersion around the Fermi energy and becoming rather flat at approx. 0.5 eV binding energy12,28. The respective spin polarization shows a maximum at _E_ − _E__F_


= −0.2 _eV_ with a value of +45%. Both spectra and spin-polarization change dramatically at _E__F_ when p-polarized light is used for excitation. In this case the minority channel exhibits a


prominent peak directly at _E__F_, leading to a distinct negative spin polarization of −20%. This peak can be ascribed to a minority surface state with Δ1-like symmetry for three reasons:


(i) it can only be excited by p-polarized light30; (ii) several theoretical works27,31 predict minority surface states for Co2MnSi(001) and have been already confirmed experimentally for


off-stoichiometric Co2MnSi in our previous work27; (iii) the state vanishes when the surface is covered by MgO, as described in detail in the following section. The values of the spin


polarization at _E__F_ (45% for s-polarized light and −20% for p-polarized light) are in apparent disagreement with the value of 93% recently measured by spin-resolved UPS18. We first recall


that the photoemission calculations reported in Ref. 18 have shown that even considering a fully spin polarized Co2MnSi sample, the broadening due to electronic correlations and the


experimental energy resolution reduce the measured spin polarization to values below 55% if only bulk photoemission transitions are considered. This value is indeed very close to the spin


polarization measured by ELEPS with s-polarized light, which is mostly sensitive to bulk electric states. In the UPS measurements of Ref. 18, the used photon energy of 21.2 eV excites


further surface resonances in the majority channel, leading to the measured high spin polarization. Indeed the majority ELEPS spectra measured with p-polarized light, which is additionally


sensitive to surface features, show a higher photoemission yield near _E__F_ than the spectra measured with s-polarized light. However, in ELEPS the 5.9 eV photons induce a resonant


excitation of a pure surface state in the minority channel, as clearly visible in the minority spectra in Fig. 1 (b) (p-polarization). This resonant excitation reduces the spin polarization


down to negative values instead of increasing it up to 93% as in UPS. It is thus possible to reconcile our ELEPS results to previous UPS measurements18. However, we add here that the reduced


spin polarization of the Co2MnSi surface might also have thermal origin, as discussed in detail in the next section. THE BURIED CO2MNSI/MGO INTERFACE Let us now turn to the results obtained


for the Co2MnSi/MgO(10 ML) system (1 ML MgO equals 0.21 nm). Figure 2 (a) shows conventional spin-resolved UPS spectra measured with a photon energy of hν = 21.2 eV (bottom panel) and the


corresponding spin-polarization (upper panel). In these spectra almost no photoemission signal is detected close to _E__F_. For lower binding energies a distinct feature centered at _E_ −


_E__F_ = −5 _eV_ stemming from the oxygen 2p states of MgO11,32 is observed (inset of Fig. 2 (a)). As expected, the UPS study performed with hν = 21.2 eV gives mainly spectroscopic


information about the MgO surface and not about the interface to Co2MnSi, since the MgO top layer thickness (ca. 2 nm) is larger than the electronic mean free path in MgO, the latter being


≤1 nm for photon energies between 20 and 500 eV (NIST Electron Inelastic-Mean-Free-Path Database). Further confirmation is given by the clearly visible MgO band gap ranging from _E__F_ down


to 4 eV binding energy, the onset of the MgO valence band. The spin-resolved ELEPS spectra (measured with hν = 5.9 eV) show a completely different behavior: Most remarkable, the spectra for


p- (shown in Fig. 2 (b)) and s-polarized laser light (not shown here) resemble the ones obtained at the free Co2MnSi surface using s-polarized laser light (c.f. Fig. 1(b)). Even the inferred


spin polarization shows high similarity to the free Co2MnSi surface (in case of s-polarized light) with a maximum value of 40% in vicinity of the Fermi energy, dropping down to roughly 20%


at higher binding energies. In addition, the total photoemission yield of the Co2MnSi/MgO(10 ML) structure is not lowered distinctively compared to the free Co2MnSi surface. These findings


prove that - in contrast to conventional UPS - ELEPS allows to determine the spin-polarization of the buried interface throughout a MgO thickness of 10 ML. Even more surprising, this


observation still holds for thicker MgO films as demonstrated by the spin-resolved ELEPS spectra measured from the Co2MnSi/MgO(20 ML) sample shown in Fig. 2 (c). This underlines the large


mean free path of the electrons in insulating materials excited by extremely low photon energy which must be in the range of at least 4 nm, i.e., the thickness of the 20 ML MgO film. The


small spectroscopic discrepancies between the free Co2MnSi surface and the buried interfaces originate solely from interface spectra smearing due to both quasi-elastic and inelastic


scattering at defects directly at the interface. These defects are inevitably induced by the finite lattice mismatch between Co2MnSi and MgO33. Besides, these disloscations lead to a


thickness-dependent surface defect density of the MgO layer and thus to MgO thickness-dependent work functions, as reported in Ref. 34 and visible in Fig. 2. Let us now explain the origin of


the remarkable interface sensitivity. Figure 3 illustrates the principle of ELEPS. If applied to metals, this method is strongly surface sensitive27 and hence comparable to conventional


UPS. If applied to a metal/insulator system like Co2MnSi/MgO, the high penetration depth of the used laser wavelength in MgO results in an excitation of electrons near _E__F_ in the


uppermost metallic (Co2MnSi) layers which will traverse the metal/insulator interface. Inside the insulator (MgO) these electrons will transiently occupy states in the conduction band until


reaching the surface and getting finally photoemitted. In the exemplary case of MgO, we extract from the UPS spectra in Fig. 2 the valence band onset at −4 eV. Assuming a band gap of 7.8 


eV10,35 we can infer the conduction band minimum of MgO at a binding energy of 3.8 eV above _E__F_. Since the excitation energy is 5.9 eV, only the lowest 2.1 eV of the conduction band will


be accessible to the traversing electrons. In contrast to conventional UPS with excitation energies higher than 20 eV, these electrons will not be able to scatter inelastically with the MgO


valence band electrons (in general, this process is the actual reason for the high surface sensitivity of UPS), since no final states for the potential scattering partners can be found: even


for a maximum possible energy exchange of 5.9 eV, the MgO band gap is still larger and hence prohibits inelastic scattering. This is the ultimate reason for the extremely large mean free


path of low energy electrons in insulating materials, translating in the interface sensitivity of the ELEPS method at FM/insulator interfaces. ELECTRONIC PROPERTIES OF THE CO2MNSI/MGO


INTERFACE After we have provided experimental evidence for the high interface sensitivity of ELEPS, we now turn to the discussion of the electronic and spintronic properties of the


Co2MnSi/MgO interface. A close inspection of the spectra in Fig. 1 and Fig. 2 (b) shows that the Δ1 minority surface state does not convert into an interface state when the Co2MnSi/MgO


interface is formed. If this would be the case, like e.g. at the CoFe/MgO interface7, the resulting interface state should again lead to a distinct feature in the minority spectra and hence


to a negative spin polarization near _E__F_ when p-polarized light is used. Since no additional features appear in the interface spectra compared to the free surface, we can thus infer that


no interface states with either Δ1 or Δ5 symmetry are formed at the Co2MnSi/MgO interface in the investigated energy range. Although such interface states are predicted theoretically at


_E__F_28,36, they do not cross the Fermi level near the Γ point37. This explains not only the shape of our photoemission spectra, but also the high tunneling magneto resistance ratios


obtained with CMS/MgO-based MTJs at low temperatures. In fact, Δ1 states contribute most to the tunneling current of such devices38 and the presence of minority states with Δ1 symmetry in


the band gap would significantly reduce the MTJs performance. WAVE FUNCTION SYMMETRIES AT THE INTERFACE Here we evaluate the energy-dependent p-s asymmetry, defined as: ; where are the spin-


and energy-resolved photoemission intensities recorded respectively for p(s)-polarized light. In Fig. 4 we plot the asymmetry of the minority (↓) and majority (↑) electrons for both the


Co2MnSi surface (upper panel) and the Co2MnSi/MgO(10 ML) interface (lower panel). _A_↑,↓ allows to determine the relative spin-resolved Δ1/Δ5 contributions of the electronic wave functions


probed by the photoemission process27. In fact, in our experimental set-up p-polarized light probes both Δ1 and Δ5 electronic states, while s-polarized light only probes Δ5 states. Thus, an


increase of the p-s asymmetry at a certain energetic position means that additional Δ1 states contribute to the spectra at this energy. At the free Co2MnSi surface the majority channel shows


enhanced asymmetry values near _E__F_ compared to higher binding energies due to majority surface resonances exhibiting Δ1-like symmetry, in line with recent spin-resolved UPS


experiments18. The increase is even stronger in the minority channel, since the 5.9 eV photons additionally excite resonantly a minority surface state. At the Co2MnSi/MgO interface, the


majority channel exhibits an almost energy-independent asymmetry, as expected from bulk band structure calculations28. Crucially, the minority channel shows a very similar behavior. This


finding can be explained by temperature-related effects, as we discuss in the following. We first recall that the strong temperature dependence of the spin polarization of the Co2MnSi/MgO


interface - that is assumed in order to explain the lowered performance of Co2MnSi/MgO-based MTJs at room temperature- can be ascribed theoretically to two competing mechanisms (c.f. Fig. 1


(a)): The formation of new minority states inside the gap21,22,23,24 as well as the mirroring of the majority density of states into the minority channel. The latter process is assumed to be


only marginal in the bulk of half-metals24, however latest theoretical considerations regarding the Co2MnSi/MgO interface found a distinctively weakened exchange coupling and hence


non-collinear alignment of atomic interface moments at elevated temperatures, causing a significant TMR ratio decrease compared to Fe/MgO-based MTJs26. The latter process leads to a


projection of majority states onto the minority band gap within the interface region and hence will influence the spin-resolved ELEPS spectra. In fact, this scenario agrees perfectly with


our observation that both the minority and majority channel possess almost an identical spectral shape as well as the same Δ1/Δ5 asymmetry near _E__F_. These findings are furthermore in


accordance with other experiments focused on temperature-dependent measurements at Co2MnSi39,40. Please note that bulk-sensitive magnetization measurements can not reveal this process, since


only the interface magnetic moments are affected. The formation of other temperature-induced minority gap states, on the other hand, can be ruled out, as such states would posses a


different Δ1/Δ5 asymmetry than the majority states present in the energetic region of the band gap. Before concluding, we note that at the buried Co2MnSi/MgO interface, surface contributions


are suppressed by the MgO top layer and no further interface states are formed. The interface electronic structure thus resembles the Co2MnSi bulk properties and hence the measured


interface spin polarization is in qualitative agreement with the bulk photoemission calculations (including correlation effects) of Ref. 18. CONCLUSIONS On the example of the bilayer


Co2MnSi/MgO, we were able to study the electronic spin- and symmetry properties of a buried ferromagnetic/insulator interface by spin-resolved ELEPS. Even for insulator thicknesses of 4 nm,


the electronic fingerprint of the free ferromagnetic surface is almost unchanged in the ELEPS experiment. This proves the sensitivity of ELEPS for interfaces buried below insulating


materials. We applied this novel technique in order to reveal the fundamental properties of the very same buried Co2MnSi/MgO interface implemented in state-of-the art Heusler-based magnetic


tunnel junctions. We found a complete suppression of the Δ1 minority surface state present at the Co2MnSi surface (whose presence would be detrimental for MTJs) and no indication for the


formation of additional interface states. A detailed analysis of the spectral dependence, spin polarization and wave function symmetry of the interface-related photoemission spectra allowed


us to rule out the presence of several temperature-induced minority states in the band gap, while both thermally activated non-collinear interface spin moments and photoemission related


effects can explain our experimental data. METHODS SAMPLE FABRICATION AND PREPARATION Four samples with the stacking structure were fabricated17 to investigate the electron wavefunction


symmetry and spin polarization of the Co2MnSi/MgO interface as well as the free Co2MnSi surface. Additionally Mn-rich samples16 served to prove the truly interface-sensitive property of


ELEPS. In all cases both epitaxial Co2MnSi and MgO grew as (001) layers with preferential L21 crystal structure, i.e. highest ordering16,17. Crystalline structure and chemical composition of


the Co2MnSi/MgO bilayers as well as the Co2MnSi surface were controlled by low energy electron diffraction and Auger electron spectroscopy. In agreement with previous investigations34, the


samples showed high structural order and stoichiometric composition. Auger electron spectroscopy was further used to ensure the complete removal of the MgO top layer by gentle 500 eV _Ar_+


ion sputtering, performed at the Co2MnSi/MgO(10 ML) samples in order to investigate the bare Co2MnSi surface. A very short _Ar_+ ion sputtering cycle with a removal of max. 1 ML of MgO was


also applied prior to photoemission experiments on the Co2MnSi/MgO(10 ML) system to remove residual carbon contaminations from the MgO surface. As expected, preferential sputtering at MgO


did not take place41. Since the Co2MnSi/MgO(20 ML) sample showed in the Auger spectra only marginal carbon adsorption at the MgO surface due to less surface defects34, it was not _Ar_+ ion


sputtered. As the final step before the photoemission experiments, all the samples were annealed to 450°C for at least 30 minutes. Hence, the interfaces studied in this work are identical to


the one present in state-of-the-art devices fabricated by some of the authors16,17. All four samples with stoichiometric Co2MnSi showed identical interface spin polarizations and wave


function asymmetries. For three of the samples, the MgO top layer was removed to study the free Co2MnSi surface, with fully reproducible results. PHOTOEMISSION EXPERIMENTS For the


spin-resolved ELEPS experiments we used the fourth harmonic of a femtosecond Ti:Sa oscillator with photon energy _hν_ = 5.9 _eV_ as the light source42. A plate allows to switch between p-


and s-polarization of the laser beam, which illuminates the sample under a degree of 45°. Because of the optical dipole selection rules43,44, s-polarized light excites only electrons with Δ5


symmetry at the Co2MnSi(100) surface, while p-polarized light probes both Δ1 and Δ5 states in case of an incoming beam angle of 45°7,27. For comparison with standard photoemission methods


(performed typically with higher photon energies), spin-resolved ultraviolet photoemission spectroscopy (UPS) spectra were recorded using a commercial He VUV gas discharge lamp providing


unpolarized light with _hν_ = 21.2 _eV_ (He I line). A spin detector (Omicron CSA-SPLEED) allows for energy- and spin-resolution of the photoemitted electrons. The energy resolution is set


to 210 meV for ELEPS and decreased to 420 meV for UPS in order to compensate the lower photoemission yield. All measurements were conducted at room temperature in an ultrahigh vacuum chamber


with a base pressure lower than 10−10 mbar. The sample surface normal points to the electron analyzer entry slit in [001] crystal direction, which is equivalent to the Γ – _X_ direction of


Co2MnSi in k-space. Hence all electrons originating from this part of the Brillouin zone are probed by our set-up. Furthermore, due to a finite detector acceptance angle of ±15° and an


applied biasing voltage of −4 V, the Γ – _K_ crystal direction is probed additionally by approx. 15% (at _hν_ = 5.9 eV). Prior to the photoemission experiments, the samples were magnetized


in remanence along the easy magnetization axis, i.e. the [110] crystal direction of Co2MnSi. The remanent magnetization of the samples, showing a squared hysteresis along the easy axis, is


nearly 100% of the saturation magnetization45. The measured spin polarization is the projection of the spin polarization vector along this direction. REFERENCES * Moodera, J. S., Kinder, L.


R., Wong, T. M. & Meservey, R. Large Magnetoresistance at Room Temperature in Ferromagnetic Thin Film Tunnel Junctions. Phys. Rev. Lett. 74, 3273–3276 (1995). ADS  CAS  PubMed  Google


Scholar  * Chappert, C., Fert, A. & Van Dau, F. N. The emergence of spin electronics in data storage. Nature Mater. 6, 813–823 (2007). ADS  CAS  Google Scholar  * Meservey, R. &


Tedrow, P. M. Spin-polarized electron tunneling. Phys. Rep. 238, 173–243 (1994). ADS  Google Scholar  * Velev, J., Dowben, P., Tsymbal, E., Jenkins, S. & Caruso, A. Interface effects in


spin-polarized metal/insulator layered structures. Surf. Sci. Rep. 63, 400–425 (2008). ADS  CAS  Google Scholar  * Butler, W. H. Tunneling magnetoresistance from a symmetry filtering effect.


Sci. Technol. Adv. Mater. 9, 014106 (2008). PubMed  PubMed Central  Google Scholar  * Yuasa, S. & Djayaprawira, D. D. Giant tunnel magnetoresistance in magnetic tunnel junctions with a


crystalline MgO(001) barrier. J. Phys. D: Appl. Phys. 40, R337 (2007). ADS  CAS  Google Scholar  * Bonell, F. et al. Spin-Polarized Electron Tunneling in bcc FeCo/MgO/FeCo(001) Magnetic


Tunnel Junctions. Phys. Rev. Lett. 108, 176602 (2012). ADS  CAS  PubMed  Google Scholar  * Plucinski, L., Zhao, Y., Sinkovic, B. & Vescovo, E. MgO/Fe(100) interface: A study of the


electronic structure. Phys. Rev. B 75, 214411 (2007). ADS  Google Scholar  * Hüfner, S. Photoelectron Spectroscopy (Springer, Heidelberg, 1994). * Klaua, M. et al. Growth, structure,


electronic and magnetic properties of MgO/Fe(001) bilayers and Fe/MgO/Fe(001) trilayers. Phys. Rev. B 64, 134411 (2001). ADS  Google Scholar  * Fecher, G. H. et al. Detection of the valence


band in buried Co2MnSi-MgO tunnel junctions by means of photoemission spectroscopy. Appl. Phys. Lett. 92, 193513 (2008). ADS  Google Scholar  * Balke, B. et al. Properties of the quaternary


half-metal-type Heusler alloy Co2Mn1−_x_Fe_x_Si. Phys. Rev. B 74, 104405 (2006). ADS  Google Scholar  * Sakuraba, Y. et al. Direct observation of half-metallic energy gap in Co2MnSi by


tunneling conductance spectroscopy. Appl. Phys. Lett. 89, 052508 (2006). ADS  Google Scholar  * Picozzi, S., Continenza, A. & Freeman, A. J. Co2MnX (X = Si, Ge, Sn) Heusler compounds: An


ab initio study of their structural, electronic and magnetic properties at zero and elevated pressure. Phys. Rev. B 66, 094421 (2002). ADS  Google Scholar  * Tsunegi, S., Sakuraba, Y.,


Oogane, M., Takanashi, K. & Ando, Y. Large tunnel magnetore-sistance in magnetic tunnel junctions using a Co2MnSi Heusler alloy electrode and a MgO barrier. Appl. Phys. Lett. 93, 112506


(2008). ADS  Google Scholar  * Ishikawa, T. et al. Influence of film composition in Co2MnSi electrodes on tunnel magnetore-sistance characteristics of Co2MnSi/MgO/Co2MnSi magnetic tunnel


junctions. Appl. Phys. Lett. 95, 232512 (2009). ADS  Google Scholar  * Tsunegi, S. et al. Enhancement in tunnel magnetoresistance effect by inserting CoFeB to the tunneling barrier interface


in Co2MnSi/MgO/CoFe magnetic tunnel junctions. Appl. Phys. Lett. 94, 252503 (2009). ADS  Google Scholar  * Jourdan, M. et al. Direct observation of half-metallicity in the Heusler compound


Co2MnSi. Nature Commun. 5, 4974 (2014). Google Scholar  * Liu, H.-x. et al. Giant tunneling magnetoresistance in epitaxial Co2MnSi/MgO/Co2MnSi magnetic tunnel junctions by half-metallicity


of Co2MnSi and coherent tunneling. Appl. Phys. Lett. 101, 132418 (2012). ADS  Google Scholar  * Ikeda, S. et al. Tunnel magnetoresistance of 604% at 300 K by suppression of Ta diffusion in


CoFeB/MgO/CoFeB pseudo-spin-valves annealed at high temperature. Appl. Phys. Lett. 93, 082508 (2008). ADS  Google Scholar  * Dowben, P. A. & Skomski, R. Finite-temperature spin


polarization in half-metallic ferromagnets. J. Appl. Phys. 93, 7948–7950 (2003). ADS  CAS  Google Scholar  * Chioncel, L. et al. Nonquasiparticle States in Co2MnSi Evidenced through Magnetic


Tunnel Junction Spectroscopy Measurements. Phys. Rev. Lett. 100, 086402 (2008). ADS  CAS  PubMed  Google Scholar  * Long, N. H., Ogura, M. & Akai, H. Effects of spin-wave excitations in


half-metallic materials. Phys. Rev. B 85, 224437 (2012). ADS  Google Scholar  * Ležaić, M., Mavropoulos, P., Enkovaara, J., Bihlmayer, G. & Blügel, S. Thermal collapse of spin


polarization in half-metallic ferromagnets. Phys. Rev. Lett. 97, 026404 (2006). ADS  PubMed  Google Scholar  * Sakuma, A., Toga, Y. & Tsuchiura, H. Theoretical study on the stability of


magnetic structures in the surface and interfaces of Heusler alloys, Co2MnAl and Co2MnSi. J. Appl. Phys. 105, 07C910 (2009). Google Scholar  * Miura, Y., Abe, K. & Shirai, M. Effects of


interfacial noncollinear magnetic structures on spin-dependent conductance in Co2MnSi/MgO/Co2MnSi magnetic tunnel junctions: A firstprinciples study. Phys. Rev. B 83, 214411 (2011). ADS 


Google Scholar  * Wüstenberg, J.-P. et al. Surface spin polarization of the nonstoichiometric Heusler alloy Co2MnSi. Phys. Rev. B 85, 064407 (2012). ADS  Google Scholar  * Miura, Y., Uchida,


H., Oba, Y., Nagao, K. & Shirai, M. Coherent tunnelling conductance in magnetic tunnel junctions of half-metallic full Heusler alloys with MgO barriers. J. Phys.: Condens. Matter 19,


365228 (2007). Google Scholar  * Soulen, R. J., Jr. et al. Measuring the spin polarization of a metal with a superconducting point contact. Science 282, 85–88 (1998). ADS  CAS  Google


Scholar  * Hansson, G. V. & Flodström, S. A. Angular-resolved photoemission from low-index crystal faces of silverbulk and surface contributions. Phys. Rev. B 17, 473–483 (1978). ADS 


CAS  Google Scholar  * Hashemifar, S. J., Kratzer, P. & Scheffler, M. Preserving the Half-Metallicity at the Heusler Alloy Co2MnSi(001) Surface: A Density Functional Theory Study. Phys.


Rev. Lett. 94, 096402 (2005). ADS  PubMed  Google Scholar  * Tjeng, L., Vos, A. & Sawatzky, G. Electronic structure of MgO studied by angle-resolved ultraviolet photoelectron


spectroscopy. Surf. Sci. 235, 269–279 (1990). ADS  CAS  Google Scholar  * Miyajima, T. et al. Direct Observation of Atomic Ordering and Interface Structure in Co2MnSi/MgO/Co2MnSi Magnetic


Tunnel Junctions by High-Angle Annular Dark-Field Scanning Transmission Electron Microscopy. Appl. Phys. Express 2, 093001 (2009). ADS  Google Scholar  * Fetzer, R. et al. Structural,


chemical and electronic properties of the Co2MnSi(001)/MgO interface. Phys. Rev. B 87, 184418 (2013). ADS  Google Scholar  * Roessler, D. M. & Walker, W. C. Electronic Spectrum and


Ultraviolet Optical Properties of Crystalline MgO. Phys. Rev. 159, 733–738 (1967). ADS  CAS  Google Scholar  * Miura, Y., Uchida, H., Oba, Y., Abe, K. & Shirai, M. Half-metallic


interface and coherent tunneling in Co2YZ/MgO/Co2YZ (YZ = MnSi,CrAl) magnetic tunnel junctions: A firstprinciples study. Phys. Rev. B 78, 064416 (2008). ADS  Google Scholar  * Hülsen, B.,


Scheffler, M. & Kratzer, P. Structural Stability and Magnetic and Electronic Properties of _Co_2_MnSi_(001)/_MgO_ Heterostructures: A Density-Functional Theory Study. Phys. Rev. Lett.


103, 046802 (2009). ADS  PubMed  Google Scholar  * Butler, W. H., Zhang, X.-G., Schulthess, T. C. & MacLaren, J. M. Spin-dependent tunneling conductance of _Fe_|_MgO_|_Fe_ sandwiches.


Phys. Rev. B 63, 054416 (2001). ADS  Google Scholar  * Miyamoto, K. et al. Absence of temperature dependence of the valence-band spectrum of _Co_2_MnSi_. Phys. Rev. B 79, 100405(R) (2009).


ADS  Google Scholar  * Tsunegi, S. et al. Observation of magnetic moments at the interface region in magnetic tunnel junctions using depth-resolved x-ray magnetic circular dichroism. Phys.


Rev. B 85, 180408 (2012). ADS  Google Scholar  * Henrich, V. The surfaces of metal oxides. Rep. Prog. Phys. 48, 1481–1541 (1985). ADS  CAS  Google Scholar  * Cinchetti, M. et al. Towards a


full Heusler alloy showing room temperature half-metallicity at the surface. J. Phys. D: Appl. Phys. 40, 1544–1547 (2007). ADS  CAS  Google Scholar  * Hermanson, J. Final-state symmetry and


polarization effects in angle-resolved photoemission spectroscopy. Solid State Commun. 22, 9–11 (1977). ADS  CAS  Google Scholar  * Eberhardt, W. & Himpsel, F. J. Dipole selection rules


for optical transitions in the fcc and bcc lattices. Phys. Rev. B 21, 5572–5576 (1980). ADS  CAS  Google Scholar  * Gaier, O. et al. Influence of the L21 ordering degree on the magnetic


properties of Co2MnSi Heusler films. J. Appl. Phys. 103, 103910 (2008). ADS  Google Scholar  Download references ACKNOWLEDGEMENTS This work was financially supported by the JST-DFG Research


Unit 1464 ASPIMATT. The work at Hokkaido University was partly supported by a Grantin-Aid for Scientific Research (A) (Grant No. 23246055) from MEXT, Japan. AUTHOR INFORMATION AUTHORS AND


AFFILIATIONS * Department of Physics and Research Center OPTIMAS, University of Kaiserslautern, Erwin-Schrödinger Str. 46, 67663, Kaiserslautern, Germany Roman Fetzer, Benjamin Stadtmüller, 


Martin Aeschlimann & Mirko Cinchetti * Department of Applied Physics, Graduate School of Engineering, Tohoku University, aoba-yama 6-6-05, 980-8579, Sendai, Japan Yusuke Ohdaira, Hiroshi


Naganuma, Mikihiko Oogane & Yasuo Ando * Division of Electronics for Informatics, Hokkaido University, Kita 14 Nishi 9, 060-0814, Sapporo, Japan Tomoyuki Taira, Tetsuya Uemura & 


Masafumi Yamamoto Authors * Roman Fetzer View author publications You can also search for this author inPubMed Google Scholar * Benjamin Stadtmüller View author publications You can also


search for this author inPubMed Google Scholar * Yusuke Ohdaira View author publications You can also search for this author inPubMed Google Scholar * Hiroshi Naganuma View author


publications You can also search for this author inPubMed Google Scholar * Mikihiko Oogane View author publications You can also search for this author inPubMed Google Scholar * Yasuo Ando


View author publications You can also search for this author inPubMed Google Scholar * Tomoyuki Taira View author publications You can also search for this author inPubMed Google Scholar *


Tetsuya Uemura View author publications You can also search for this author inPubMed Google Scholar * Masafumi Yamamoto View author publications You can also search for this author inPubMed 


Google Scholar * Martin Aeschlimann View author publications You can also search for this author inPubMed Google Scholar * Mirko Cinchetti View author publications You can also search for


this author inPubMed Google Scholar CONTRIBUTIONS R.F., B.S., M.A. and M.C. wrote the main manuscript text. R.F. and M.C. prepared all figures. R.F. conducted all presented experiments. Y.O.


and T.T. fabricated the investigated samples. H.N., M.O., Y.A., T.U. and M.Y. supervised sample fabrication, contributed to the respective methods section as well as to the discussion of


the results. All authors reviewed the manuscript. ETHICS DECLARATIONS COMPETING INTERESTS The authors declare no competing financial interests. RIGHTS AND PERMISSIONS This work is licensed


under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless


indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder in order to reproduce


the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ Reprints and permissions ABOUT THIS ARTICLE CITE THIS ARTICLE Fetzer, R., Stadtmüller, B.,


Ohdaira, Y. _et al._ Probing the electronic and spintronic properties of buried interfaces by extremely low energy photoemission spectroscopy. _Sci Rep_ 5, 8537 (2015).


https://doi.org/10.1038/srep08537 Download citation * Received: 07 October 2014 * Accepted: 23 January 2015 * Published: 23 February 2015 * DOI: https://doi.org/10.1038/srep08537 SHARE THIS


ARTICLE Anyone you share the following link with will be able to read this content: Get shareable link Sorry, a shareable link is not currently available for this article. Copy to clipboard


Provided by the Springer Nature SharedIt content-sharing initiative