We present an experimental investigation of the magnetic and magnetocaloric properties of sputter... more We present an experimental investigation of the magnetic and magnetocaloric properties of sputtered epitaxial and amorphous Tb thin films. We grew epitaxial Nb (50-nm)/Tb (100-nm) bilayer thin films on Al 2 O 3 (1120) substrate using DC magnetron sputtering at high temperature, with excellent crystalline quality of the hcp Tb(0001) layer. While the amorphous Tb thin film exhibits more isotropic magnetocaloric properties, we show that the epitaxial Tb thin film displays large anisotropic magnetocaloric properties, with a large maximum magnetic entropy change of 6.27 J kg −1 K −1 at the Néel temperature as well as a large relative cooling power of 225 J kg −1 with a magnetic field change H = 20 kOe applied along the in-plane direction. These large and anisotropic magnetocaloric properties are much larger than those measured for the amorphous Tb thin film, or previously reported for Tb-based thin-film structures. Our findings highlight the opportunities for growing epitaxial rare-earth thin films using sputtering techniques and demonstrate the importance of crystallographic control on the magnetocaloric effect in Tb thin films.
Investigation of the spin Hall effect in gold has triggered increasing interest over the past dec... more Investigation of the spin Hall effect in gold has triggered increasing interest over the past decade, since gold combines the properties of a large bulk spin diffusion length and strong interfacial spin-orbit coupling. However, discrepancies between the values of the spin Hall angle of gold reported in the literature have brought into question the microscopic origin of the spin Hall effect in Au. Here, we investigate the thickness dependence of the spin-charge conversion efficiency in single Au films and ultrathin Au/Si multilayers by non-local transport and spin-torque ferromagnetic resonance measurements. We show that the spin-charge conversion efficiency is strongly enhanced in ultrathin Au/Si multilayers, reaching exceedingly large values of 0.99 +/- 0.34 when the thickness of the individual Au layers is scaled down to 2 nm. These findings reveal the coexistence of a strong interfacial spin-orbit coupling effect which becomes dominant in ultrathin Au, and bulk spin Hall effect w...
Tuning the Dzyaloshinskii-Moriya interaction (DMI) using electric (E)-fields in magnetic devices ... more Tuning the Dzyaloshinskii-Moriya interaction (DMI) using electric (E)-fields in magnetic devices has opened up new perspectives for controlling the stabilization of chiral spin structures. Recent efforts have used voltage-induced charge redistribution at magnetic/oxides interfaces to modulate the DMI. This approach is attractive for active devices but tends to be volatile, making it energy-demanding. Here we demonstrate nonvolatile E-field manipulation of the DMI by ionic-liquid gating of Pt/Co/HfO2 ultra thin films. The E-field effect on the DMI is linked to the migration of oxygen species from the HfO2 layer into the Co and Pt layers and subsequent anchoring. This effect permanently changes the properties of the material, showing that E-fields can be used not only for local gating in devices but also as a material design tool for post growth tuning of the DMI.
All‐optical control and detection of magnetic states for high‐density recording necessitate nanop... more All‐optical control and detection of magnetic states for high‐density recording necessitate nanophotonic approaches to amplify local light intensity below the diffraction limit. Sculpting the near‐field phase and polarization can additionally strengthen magneto‐optical effects that rely on circularly polarized pulses, such as all‐optical helicity‐dependent switching, imaging, and spin‐wave excitation. Here, high‐refractive‐index dielectric nanoantennas illuminated with circularly polarized light resonantly enhance local electric field rotation by more than sixfold within [Pt/Co]N thin films. Sub‐wavelength arrays of amorphous Si nanodisks, or metasurfaces, patterned on perpendicularly magnetized films support Mie‐type resonances that modulate reflection and transmission dissymmetry by >±2% in experiments. Spatial and spectral interference between dipolar modes, proximity effects, and gain are evaluated by varying disk aspect ratio, metasurface–metal separation, and magnetic film thickness, respectively. Simulated enhancements in magnetic circular birefringence and differential absorption are correlated with amplified local field rotation at electric dipolar modes. Greater achievable amplifications are shown via simulations with single‐crystalline Si metasurfaces exhibiting lower losses, including a 12‐fold strengthened electric field rotation within ferromagnetic layers. The metasurface design rules established here could enable nanoscale localization of all‐optical magnetic switching with lowered laser fluence thresholds, as well as enhanced magneto‐optical responses for light‐assisted reading in spintronic devices.
Spin-dependent and enantioselective electron-molecule scattering occurs in photoelectron transmis... more Spin-dependent and enantioselective electron-molecule scattering occurs in photoelectron transmission through chiral molecular films. This spin selectivity leads to electron spin filtering by molecular helices, with increasing magnitude, concomitant with increasing numbers of helical turns. Using ultraviolet photoelectron spectroscopy, we measured spin-selective surface charging accompanying photoemission from ferromagnetic substrates functionalized with monolayers of mercurated DNA hairpins that constitute only one helical turn. Mercury ions bind specifically at thymine-thymine mismatches within self-hybridized single-stranded DNA, enabling precise control over the number and position of Hg 2+ along the helical axis. Differential charging of the organic layers, manifested as substrate magnetization-dependent photoionization energies, was observed for DNA hairpins containing Hg 2+ ; no differences were measured for hairpin monolayers in the absence of Hg 2+. Inversion of the DNA helical secondary structure at increased metal loading led to complementary inversion in spin selectivity. We attribute these results to increased scattering probabilities from relativistic enhancement of spin-orbit interactions in mercurated DNA.
The observation of all-optical helicity-dependent switching (AO-HDS) in ferri-and ferro-magnetic ... more The observation of all-optical helicity-dependent switching (AO-HDS) in ferri-and ferro-magnetic materials depends not only on the saturation magnetization, but on the magnetic domain size which takes into account the competition between the demagnetizing energy and the domain wall (DW) energy. In this paper, we study Suppression of all-optical switching in He +-irradiated Co/Pt multilayers 2 the optical response of Co/Pt multilayers for which perpendicular magnetic anisotropy can be tuned using He +-irradiation. This allows us to correlate the observation of AO-HDS with the magnetic properties of the He +-irradiated multilayer. These results give direct evidence of the crucial role of the DW energy in the laser-induced switching process.
The possibility to tune the Dzyaloshinskii Moriya interaction (DMI) by electric (E) field gating ... more The possibility to tune the Dzyaloshinskii Moriya interaction (DMI) by electric (E) field gating in ultra-thin magnetic materials has opened new perspectives in terms of controlling the stabilization of chiral spin structures. Most recent efforts have used voltage-induced charge redistribution at the interface between a metal and an oxide to modulate DMI. This approach is attractive for active devices but it tends to be volatile, making it energy demanding, and it is limited by Coulomb screening in the metal. Here we have demonstrated the non-volatile E-field manipulation of DMI by ionic liquid gating of Pt/Co/HfO2 ultra-thin films. The E-field effect on DMI scales with the E-field exposure time and is proposed to be linked to the migration and subsequent anchoring of oxygen species from the HfO2 layer into the Co and Pt layers. This effect permanently changes the properties of the material showing that E-fields can not only be used for local gating in devices but also as a highly scalable materials design tool for post-growth tuning of DMI.
Domain wall displacement in Co/Pt thin films induced by not only fs-but also ps-laser pulses is d... more Domain wall displacement in Co/Pt thin films induced by not only fs-but also ps-laser pulses is demonstrated using time-resolved magneto-optical Faraday imaging. We evidence multi-pulse helicity-dependent laser-induced domain wall motion in all-optical switchable Co/Pt multilayers with a laser energy below the switching threshold. Domain wall displacement of ∼ 2 nm per 2ps pulse is achieved. By investigating separately the effect of linear and circular polarization, we reveal that laser-induced domain wall motion results from a complex interplay between pinning, temperature gradient and helicity effect. Then, we explore the microscopic origin of the helicity effect acting on the domain wall. These experimental results enhance the understanding of the mechanism of all-optical switching in ultra-thin ferromagnetic films.
Magnetic refrigeration based on the magneto-caloric effect is one of the best alternatives to com... more Magnetic refrigeration based on the magneto-caloric effect is one of the best alternatives to compete with vapor-compression technology. The viability of a magnetic refrigeration system for magnetic cooling can be tested by exploiting the materials in various forms, ranging from bulk to nanostructured materials. In order to achieve a wide refrigerating temperature range in magnetic refrigeration, we study in this paper a 100 nm-thick Gd-Co alloys-based multilayer stack. The stack is made of four individual Gd-Co alloy layers with different values of concentration and Curie temperature (T C). A magnetic entropy change associated with the second-order magnetic phase transition was determined from the magnetic isotherms. Moreover, the relative cooling power (RCP) of the studied Gd-Cobased multilayer is enhanced compared to the one of bulk Gd, and reaches a value of 200 J/kg. Such an enhancement of the RCP is not due to an enhanced maximum variation of entropy, but this is due to a much broader magnetic entropy peak. This study demonstrates the potential of nanostructured Gd-Co multilayer stack for magnetic cooling applications.
To understand the necessary condition for the observation of all-optical helicity-dependent switc... more To understand the necessary condition for the observation of all-optical helicity-dependent switching (AO-HDS) of magnetization in thin films, we investigated ferromagnetic Co/Pt and Co/Ni multilayers as well as ferrimagnetic TbCo alloys as a function of magnetic layer compositions and thicknesses. We show that both ferro-and ferri-magnets with high saturation magnetization show AO-HDS if their magnetic thickness is strongly reduced below a material-dependent threshold thickness. By taking into account the demagnetizing energy and the domain wall energy, we are able to define a criterion to predict whether AO-HDS or thermal demagnetization (TD) will be observed. This criterion for the observation of AO-HDS is that the equilibrium size of magnetic domains forming during the cooling process should be larger than the laser spot size. From these results we anticipate that more magnetic materials are expected to show AO-HDS. However, the effect of the optical pulses' helicity is hidden by the formation of small magnetic domains during the cooling process.
Using a time-dependent electrical investigation of the all-optical switching in ferrimagnetic and... more Using a time-dependent electrical investigation of the all-optical switching in ferrimagnetic and ferromagnetic Hall crosses via the anomalous Hall effect, intriguing new insights into the rich physics underlying the all-optical switching are provided. We demonstrate that two different all-optical magnetization switching mechanisms can be distinguished; a "single pulse" switching for ferrimagnetic GdFeCo alloys, and a "two regimes" switching process for both ferrimagnetic TbCo alloys and ferromagnetic Pt/Co multilayers. We show that the latter takes place at two different timescales, and consists in a step-like helicity-independent multiple-domain formation within the first 1 ms followed by a helicity-dependent remagnetization on several tens of ms.
Since the first observation of ultrafast demagnetization in Ni thin films by Beaurepaire et al 20... more Since the first observation of ultrafast demagnetization in Ni thin films by Beaurepaire et al 20 years ago, understanding the interaction between ultrashort laser pulses and magnetization has become a topic of huge interest. In 2007, an intriguing discovery related to ultrafast demagnetization was the observation of all-optical switching (AOS) of magnetization in ferrimagnetic GdFeCo alloy films using only femtosecond laser pulses. This review discusses the recent studies elucidating several key issues regarding the all-optical switching phenomenon. Although AOS had long been restricted to GdFeCo alloys, it turned out to be a more general phenomenon for a variety of ferrimagnetic as well as ferromagnetic materials. This discovery helped pave the way for the integration of all-optical writing in data storage industries. Nevertheless, theoretical models explaining the switching in GdFeCo alloy films do not appear to apply in the other materials, thus questioning the uniqueness of the microscopic origin of all-optical switching. By investigating the integration of all-optical switching in spintronic devices, two types of all-optical switching mechanism have been distinguished: a single-pulse heat-only switching in ferrimagnetic GdFeCo alloys, and a two regime helicity-dependent switching in both ferrimagnetic TbCo alloys and ferromagnetic Co/Pt multilayers. Another key issue discussed in this review is the necessary condition for the observation of all-optical switching. Many models have been proposed but are strongly challenged by the discovery of such switching in ferromagnets. A comprehensive investigation of the magnetic parameters governing all-optical switching demonstrate that its observation requires magnetic domains larger than the laser spot size during the cooling process; such a criterion is common for both ferri- and ferro-magnets. These investigations strongly improve our understanding and give intriguing insights into the rich physics of the ultrafast manipulation of magnetic order.
We present an experimental investigation of the magnetic and magnetocaloric properties of sputter... more We present an experimental investigation of the magnetic and magnetocaloric properties of sputtered epitaxial and amorphous Tb thin films. We grew epitaxial Nb (50-nm)/Tb (100-nm) bilayer thin films on Al 2 O 3 (1120) substrate using DC magnetron sputtering at high temperature, with excellent crystalline quality of the hcp Tb(0001) layer. While the amorphous Tb thin film exhibits more isotropic magnetocaloric properties, we show that the epitaxial Tb thin film displays large anisotropic magnetocaloric properties, with a large maximum magnetic entropy change of 6.27 J kg −1 K −1 at the Néel temperature as well as a large relative cooling power of 225 J kg −1 with a magnetic field change H = 20 kOe applied along the in-plane direction. These large and anisotropic magnetocaloric properties are much larger than those measured for the amorphous Tb thin film, or previously reported for Tb-based thin-film structures. Our findings highlight the opportunities for growing epitaxial rare-earth thin films using sputtering techniques and demonstrate the importance of crystallographic control on the magnetocaloric effect in Tb thin films.
Investigation of the spin Hall effect in gold has triggered increasing interest over the past dec... more Investigation of the spin Hall effect in gold has triggered increasing interest over the past decade, since gold combines the properties of a large bulk spin diffusion length and strong interfacial spin-orbit coupling. However, discrepancies between the values of the spin Hall angle of gold reported in the literature have brought into question the microscopic origin of the spin Hall effect in Au. Here, we investigate the thickness dependence of the spin-charge conversion efficiency in single Au films and ultrathin Au/Si multilayers by non-local transport and spin-torque ferromagnetic resonance measurements. We show that the spin-charge conversion efficiency is strongly enhanced in ultrathin Au/Si multilayers, reaching exceedingly large values of 0.99 +/- 0.34 when the thickness of the individual Au layers is scaled down to 2 nm. These findings reveal the coexistence of a strong interfacial spin-orbit coupling effect which becomes dominant in ultrathin Au, and bulk spin Hall effect w...
Tuning the Dzyaloshinskii-Moriya interaction (DMI) using electric (E)-fields in magnetic devices ... more Tuning the Dzyaloshinskii-Moriya interaction (DMI) using electric (E)-fields in magnetic devices has opened up new perspectives for controlling the stabilization of chiral spin structures. Recent efforts have used voltage-induced charge redistribution at magnetic/oxides interfaces to modulate the DMI. This approach is attractive for active devices but tends to be volatile, making it energy-demanding. Here we demonstrate nonvolatile E-field manipulation of the DMI by ionic-liquid gating of Pt/Co/HfO2 ultra thin films. The E-field effect on the DMI is linked to the migration of oxygen species from the HfO2 layer into the Co and Pt layers and subsequent anchoring. This effect permanently changes the properties of the material, showing that E-fields can be used not only for local gating in devices but also as a material design tool for post growth tuning of the DMI.
All‐optical control and detection of magnetic states for high‐density recording necessitate nanop... more All‐optical control and detection of magnetic states for high‐density recording necessitate nanophotonic approaches to amplify local light intensity below the diffraction limit. Sculpting the near‐field phase and polarization can additionally strengthen magneto‐optical effects that rely on circularly polarized pulses, such as all‐optical helicity‐dependent switching, imaging, and spin‐wave excitation. Here, high‐refractive‐index dielectric nanoantennas illuminated with circularly polarized light resonantly enhance local electric field rotation by more than sixfold within [Pt/Co]N thin films. Sub‐wavelength arrays of amorphous Si nanodisks, or metasurfaces, patterned on perpendicularly magnetized films support Mie‐type resonances that modulate reflection and transmission dissymmetry by >±2% in experiments. Spatial and spectral interference between dipolar modes, proximity effects, and gain are evaluated by varying disk aspect ratio, metasurface–metal separation, and magnetic film thickness, respectively. Simulated enhancements in magnetic circular birefringence and differential absorption are correlated with amplified local field rotation at electric dipolar modes. Greater achievable amplifications are shown via simulations with single‐crystalline Si metasurfaces exhibiting lower losses, including a 12‐fold strengthened electric field rotation within ferromagnetic layers. The metasurface design rules established here could enable nanoscale localization of all‐optical magnetic switching with lowered laser fluence thresholds, as well as enhanced magneto‐optical responses for light‐assisted reading in spintronic devices.
Spin-dependent and enantioselective electron-molecule scattering occurs in photoelectron transmis... more Spin-dependent and enantioselective electron-molecule scattering occurs in photoelectron transmission through chiral molecular films. This spin selectivity leads to electron spin filtering by molecular helices, with increasing magnitude, concomitant with increasing numbers of helical turns. Using ultraviolet photoelectron spectroscopy, we measured spin-selective surface charging accompanying photoemission from ferromagnetic substrates functionalized with monolayers of mercurated DNA hairpins that constitute only one helical turn. Mercury ions bind specifically at thymine-thymine mismatches within self-hybridized single-stranded DNA, enabling precise control over the number and position of Hg 2+ along the helical axis. Differential charging of the organic layers, manifested as substrate magnetization-dependent photoionization energies, was observed for DNA hairpins containing Hg 2+ ; no differences were measured for hairpin monolayers in the absence of Hg 2+. Inversion of the DNA helical secondary structure at increased metal loading led to complementary inversion in spin selectivity. We attribute these results to increased scattering probabilities from relativistic enhancement of spin-orbit interactions in mercurated DNA.
The observation of all-optical helicity-dependent switching (AO-HDS) in ferri-and ferro-magnetic ... more The observation of all-optical helicity-dependent switching (AO-HDS) in ferri-and ferro-magnetic materials depends not only on the saturation magnetization, but on the magnetic domain size which takes into account the competition between the demagnetizing energy and the domain wall (DW) energy. In this paper, we study Suppression of all-optical switching in He +-irradiated Co/Pt multilayers 2 the optical response of Co/Pt multilayers for which perpendicular magnetic anisotropy can be tuned using He +-irradiation. This allows us to correlate the observation of AO-HDS with the magnetic properties of the He +-irradiated multilayer. These results give direct evidence of the crucial role of the DW energy in the laser-induced switching process.
The possibility to tune the Dzyaloshinskii Moriya interaction (DMI) by electric (E) field gating ... more The possibility to tune the Dzyaloshinskii Moriya interaction (DMI) by electric (E) field gating in ultra-thin magnetic materials has opened new perspectives in terms of controlling the stabilization of chiral spin structures. Most recent efforts have used voltage-induced charge redistribution at the interface between a metal and an oxide to modulate DMI. This approach is attractive for active devices but it tends to be volatile, making it energy demanding, and it is limited by Coulomb screening in the metal. Here we have demonstrated the non-volatile E-field manipulation of DMI by ionic liquid gating of Pt/Co/HfO2 ultra-thin films. The E-field effect on DMI scales with the E-field exposure time and is proposed to be linked to the migration and subsequent anchoring of oxygen species from the HfO2 layer into the Co and Pt layers. This effect permanently changes the properties of the material showing that E-fields can not only be used for local gating in devices but also as a highly scalable materials design tool for post-growth tuning of DMI.
Domain wall displacement in Co/Pt thin films induced by not only fs-but also ps-laser pulses is d... more Domain wall displacement in Co/Pt thin films induced by not only fs-but also ps-laser pulses is demonstrated using time-resolved magneto-optical Faraday imaging. We evidence multi-pulse helicity-dependent laser-induced domain wall motion in all-optical switchable Co/Pt multilayers with a laser energy below the switching threshold. Domain wall displacement of ∼ 2 nm per 2ps pulse is achieved. By investigating separately the effect of linear and circular polarization, we reveal that laser-induced domain wall motion results from a complex interplay between pinning, temperature gradient and helicity effect. Then, we explore the microscopic origin of the helicity effect acting on the domain wall. These experimental results enhance the understanding of the mechanism of all-optical switching in ultra-thin ferromagnetic films.
Magnetic refrigeration based on the magneto-caloric effect is one of the best alternatives to com... more Magnetic refrigeration based on the magneto-caloric effect is one of the best alternatives to compete with vapor-compression technology. The viability of a magnetic refrigeration system for magnetic cooling can be tested by exploiting the materials in various forms, ranging from bulk to nanostructured materials. In order to achieve a wide refrigerating temperature range in magnetic refrigeration, we study in this paper a 100 nm-thick Gd-Co alloys-based multilayer stack. The stack is made of four individual Gd-Co alloy layers with different values of concentration and Curie temperature (T C). A magnetic entropy change associated with the second-order magnetic phase transition was determined from the magnetic isotherms. Moreover, the relative cooling power (RCP) of the studied Gd-Cobased multilayer is enhanced compared to the one of bulk Gd, and reaches a value of 200 J/kg. Such an enhancement of the RCP is not due to an enhanced maximum variation of entropy, but this is due to a much broader magnetic entropy peak. This study demonstrates the potential of nanostructured Gd-Co multilayer stack for magnetic cooling applications.
To understand the necessary condition for the observation of all-optical helicity-dependent switc... more To understand the necessary condition for the observation of all-optical helicity-dependent switching (AO-HDS) of magnetization in thin films, we investigated ferromagnetic Co/Pt and Co/Ni multilayers as well as ferrimagnetic TbCo alloys as a function of magnetic layer compositions and thicknesses. We show that both ferro-and ferri-magnets with high saturation magnetization show AO-HDS if their magnetic thickness is strongly reduced below a material-dependent threshold thickness. By taking into account the demagnetizing energy and the domain wall energy, we are able to define a criterion to predict whether AO-HDS or thermal demagnetization (TD) will be observed. This criterion for the observation of AO-HDS is that the equilibrium size of magnetic domains forming during the cooling process should be larger than the laser spot size. From these results we anticipate that more magnetic materials are expected to show AO-HDS. However, the effect of the optical pulses' helicity is hidden by the formation of small magnetic domains during the cooling process.
Using a time-dependent electrical investigation of the all-optical switching in ferrimagnetic and... more Using a time-dependent electrical investigation of the all-optical switching in ferrimagnetic and ferromagnetic Hall crosses via the anomalous Hall effect, intriguing new insights into the rich physics underlying the all-optical switching are provided. We demonstrate that two different all-optical magnetization switching mechanisms can be distinguished; a "single pulse" switching for ferrimagnetic GdFeCo alloys, and a "two regimes" switching process for both ferrimagnetic TbCo alloys and ferromagnetic Pt/Co multilayers. We show that the latter takes place at two different timescales, and consists in a step-like helicity-independent multiple-domain formation within the first 1 ms followed by a helicity-dependent remagnetization on several tens of ms.
Since the first observation of ultrafast demagnetization in Ni thin films by Beaurepaire et al 20... more Since the first observation of ultrafast demagnetization in Ni thin films by Beaurepaire et al 20 years ago, understanding the interaction between ultrashort laser pulses and magnetization has become a topic of huge interest. In 2007, an intriguing discovery related to ultrafast demagnetization was the observation of all-optical switching (AOS) of magnetization in ferrimagnetic GdFeCo alloy films using only femtosecond laser pulses. This review discusses the recent studies elucidating several key issues regarding the all-optical switching phenomenon. Although AOS had long been restricted to GdFeCo alloys, it turned out to be a more general phenomenon for a variety of ferrimagnetic as well as ferromagnetic materials. This discovery helped pave the way for the integration of all-optical writing in data storage industries. Nevertheless, theoretical models explaining the switching in GdFeCo alloy films do not appear to apply in the other materials, thus questioning the uniqueness of the microscopic origin of all-optical switching. By investigating the integration of all-optical switching in spintronic devices, two types of all-optical switching mechanism have been distinguished: a single-pulse heat-only switching in ferrimagnetic GdFeCo alloys, and a two regime helicity-dependent switching in both ferrimagnetic TbCo alloys and ferromagnetic Co/Pt multilayers. Another key issue discussed in this review is the necessary condition for the observation of all-optical switching. Many models have been proposed but are strongly challenged by the discovery of such switching in ferromagnets. A comprehensive investigation of the magnetic parameters governing all-optical switching demonstrate that its observation requires magnetic domains larger than the laser spot size during the cooling process; such a criterion is common for both ferri- and ferro-magnets. These investigations strongly improve our understanding and give intriguing insights into the rich physics of the ultrafast manipulation of magnetic order.
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