Using first-principles calculations, we systematically study the dissociation of O$_2$ molecules on different ultrathin Pb(111) films. Based on our previous work revealing the molecular adsorption precursor states for O$_2$, we further explore that why there are two nearly degenerate adsorption states on Pb(111) ultrathin films, but no precursor adsorption states exist at all on the Mg(0001) and Al(111) surfaces. And the reason is concluded to be the different surface electronic structures. For the O$_2$ dissociation, we consider both the reaction channels from gas-like and molecularly adsorbed O$_2$ molecules. We find that the energy barrier for O$_2$ dissociation from the molecular adsorption precursor states is always smaller than from O$_2$ gases. The most energetically favorable dissociation process is found to be the same on different Pb(111) films, and the energy barriers are found to be modulated by the quantum size effects of Pb(111) films.
We analyze X-ray diffraction data used to extract cell parameters of ultrathin films on closely matching substrates. We focus on epitaxial La2/3Sr1/3MnO3 films grown on (001) SrTiO3 single crystalline substrates. It will be shown that, due to extremely high structural similarity of film and substrate, data analysis must explicitly consider the distinct phase of the diffracted waves by substrate and films to extract reliable unit cell parameters. The implications of this finding for the understanding of strain effects in ultrathin films and interfaces will be underlined
We report bcc-like crystal structures in 2-4 ML Fe films grown on fcc Cu(100) using scanning tunneling microscopy. The local bcc structure provides a straightforward explanation for their frequently reported outstanding magnetic properties, i.e., ferromagnetic ordering in all layers with a Curie temperature above 300 K. The non-pseudomorphic structure, which becomes pseudomorphic above 4 ML film thickness is unexpected in terms of conventional rules of thin film growth and stresses the importance of finite thickness effects in ferromagnetic ultrathin films.
We present a first-principles study on the dielectric properties of an NaCl crystal and ultrathin NaCl films under a finite external electric field. Our results show that the high-frequency dielectric constant of the films is not affected by the finite size effect from crystal surfaces and is close to that of the crystal, whereas the static one is sensitive to the thickness of the film due to the difference in the atomic configurations between the surface and inside of the film.
X-ray photoelectron diffraction is used to directly probe the intra-cell polar atomic distortion and tetragonality associated with ferroelectricity in ultrathin epitaxial PbTiO3 films. Our measurements, combined with ab-initio calculations, unambiguously demonstrate non-centro-symmetry in films a few unit cells thick, imply that films as thin as 3 unit cells still preserve a ferroelectric polar distortion, and also show that there is no thick paraelectric dead layer at the surface.
We report layer-resolved measurements of the \textit{unoccupied} electronic structure of ultrathin MgO films grown on Ag(001). The metal-induced gap states at the metal/oxide interface, the oxide band gap as well as a surface core exciton involving an image-potential state of the vacuum are revealed through resonant Auger spectroscopy of the Mg $KL_{23}L_{23}$ Auger transition. Our results demonstrate how to obtain new insights on \textit{empty} states at interfaces of metal-supported ultrathin oxide films.
The ground-state polarization of PbTiO3 thin films is studied using a microscopic effective Hamiltonian with parameters obtained from first-principles calculations. Under short-circuit electrical boundary conditions, (001) films with thickness as low as three unit cells are found to have a perpendicularly polarized ferroelectric ground state with significant enhancement of the polarization at the surface.
Quantum manifestations of various properties of metallic thin films by quantum size effect (QSE) have been studied intensively. Here, using first-principles calculations, we show quantum manifestation in dielectric properties of Al(111) ultrathin films. The QSE on the dielectric function is revealed, which arises from size dependent contributions from both intraband and interband electronic transitions. More importantly, the in-plane interband transitions in the films thinner than 15 monolayers are found to be smaller than the bulk counterpart in the energy range from 1.5~eV to 2.5~eV. This in…
We investigate the sensitive interplay between magnetic, electronic and structural properties in the ferrimagnetic oxide NiFe2O4. Emphasis is placed on the impact of reduced dimensionality in the crossover from bulk-like to ultrathin films. We observed an enhanced saturation magnetization $M_S$ for ultrathin NiFe2O4 films on Nb-SrTiO3 (001) substrates that co-occurs with a reduced out-of-plane lattice constant under compressive in-plane epitaxial strain. We found a bulk-like cationic coordination of the inverse spinel lattice independent of the NiFe2O4 film thickness -- thus ruling out a catio…
Interface effects on the ferroelectric behavior of PbTiO$_3$ ultrathin films deposited on SrTiO$_3$ substrate are investigated using an interatomic potential approach with parameters fitted to first-principles calculations. We find that the correlation of atomic displacements across the film/substrate interface is crucial for the stabilization of the ferroelectric state in films a few unit-cells thick. We show that the minimum film thickness for the appearance of a spontaneous polarized domain state is not an intrinsic property of the ferroelectric film but depends on the polarizability of the…
The magnetization of Pd(100) ultrathin films that show ferromagnetism due to quantum well states was manipulated by changing the quantum well state with an applied bias voltage. The voltage dependence of the magnetic moment of Pd/SrTiO$_{3-x}$/Ti/Au intrinsically depends on the Pd film thickness. The induced change in the magnetic moment is due to the modulation of the phase shift at the interface between the Pd thin film and the semiconductor SrTiO$_{3-x}$ substrate.
We study the ferroelectric stability and surface structural properties of an oxygen-terminated hexagonal YMnO$_3$ ultra-thin film using density functional theory. Under an open circuit boundary condition, the ferroelectric state with the spontaneous polarization normal to the (0001) surface, is found to be metastable in a single domain state despite the presence of a depolarizing field. We establish a connection between the result and the role of improper ferroelectric transition. Our results imply that improper ferroelectric ultrathin films can have rather unique properties that are distincti…
To better understand the electronic and chemical properties of wide-gap oxide surfaces at the atomic scale, experimental work has focused on epitaxial films on metal substrates. Recent findings show that these films are considerably thinner than previously thought. This raises doubts about the transferability of the results to surface properties of thicker films and bulk crystals. By means of density-functional theory and approximate GW corrections for the electronic spectra we demonstrate for three characteristic wide-gap oxides (silica, alumina, and hafnia) the influence of the substrate and…
The strong metal-support interaction (SMSI) leads to substantial changes of the properties of an oxide-supported catalyst after annealing under reducing conditions. The common explanation is the formation of heavily reduced, ultrathin oxide films covering metal particles. This is typically encountered for reducible oxides such as TiO2 or Fe3O4. Zirconia (ZrO2), a typical catalyst support, is difficult to reduce and therefore no obvious candidate for the SMSI effect. In this work, we use inverse model systems with Rh(111), Pt(111), and Ru(0001) as supports. Contrary to expectations, we show tha…
We raise the possibility that the chiral degeneracy of the magnons in ultrathin films can be lifted due to the presence of Dzyaloshinskii-Moriya interactions. By using simple symmetry arguments, we discuss under which conditions such a chiral asymmetry occurs. We then perform relativistic first principles calculations for an Fe monolayer on W(110) and explicitly reveal the asymmetry of the spin-wave spectrum in case of wave-vectors parallel to the (001) direction. Furthermore, we quantitatively interpret our results in terms of a simplified spin-model by using calculated Dzyaloshinskii-Moriya …
The surface evolution model based on geometric partial differential equation is used to numerically study the kinetics of dewetting and dynamic morphologies for the localized pinhole defect in the surface of the ultrathin solid film with the strongly anisotropic surface energy. Depending on parameters such as the initial depth and width of the pinole, the strength of the attractive substrate potential and the strength of the surface energy anisotropy, the pinhole may either extend to the substrate and thus rupture the film, or evolve to the quasiequilibrium shape while the rest of the film sur…
Nitrogen-vacancy magnetic microscopy is employed in quenching mode as a non-invasive, high resolution tool to investigate the morphology of isolated skyrmions in ultrathin magnetic films. The skyrmion size and shape are found to be strongly affected by local pinning effects and magnetic field history. Micromagnetic simulations including static disorder, based on a physical model of grain-to-grain thickness variations, reproduce all experimental observations and reveal the key role of disorder and magnetic history in the stabilization of skyrmions in ultrathin magnetic films. This work opens th…
A first-principles-derived approach is developed to study the effects of uncompensated depolarizing electric fields on the properties of Pb(Zr,Ti)O$_3$ ultrathin films for different mechanical boundary conditions. A rich variety of ferroelectric phases and polarization patterns is found, depending on the interplay between strain and amount of screening of surface charges. Examples include triclinic phases, monoclinic states with in-plane and/or out-of-plane components of the polarization, homogeneous and inhomogeneous tetragonal states, as well as, peculiar laminar nanodomains.
First-principals calculations show that up-spin and down-spin carriers are accumulating adjacent to opposite surfaces of BiFeO3(BFO) film with applying external bias. The spin carriers are equal in magnitude and opposite in direction, and down-spin carriers move to the direction opposing the external electric field while up-spin ones along the field direction. This novel spin transfer properties make BFO film an intriguing candidate for application in spin capacitor and BFO-based multiferroic field-effect device.
Previous studies showed that, as ferroelectric films become thinner, their Curie temperature (Tc) and polarization below Tc both typically decrease. In contrast, a recent experiment [Chang et al., Science 353, 274 (2016)] observed that atomic-thick SnTe films have a higher Tc than their bulk counterpart, which was attributed to extrinsic effects. Here, we find, using first-principles calculations, that the 0K energy barrier for the polarization switching (which is a quantity directly related to Tc) is higher in most investigated defect-free SnTe ultrathin films than that in bulk SnTe, and that…
Metal-insulator transition is observed in the La0.8Sr0.2MnO3 thin films with thickness larger than 5 unit cells. Insulating phase at lower temperature appeared in the ultrathin films with thickness ranging from 6 unit cells to 10 unit cells and it is found that the Mott variable range hopping conduction dominates in this insulating phase at low temperature with a decrease of localization length in thinner films. A deficiency of oxygen content and a resulted decrease of the Mn valence have been observed in the ultrathin films with thickness smaller than or equal to 10 unit cells by studying the…
Using a first-principles-based approach, we determine the ferroelectric pattern in PbZr$_{0.5}$Ti$_{0.5}$O$_3$ ultrathin film. It is found that vortex stripes are formed in the system and they are responsible for the 180$^\circ$ domains observed. When a local external field is exerted, the vortex stripe transforms into the vortex loop structure, which leads to the formation of a smaller domain with the polarization antiparallel to the field in the center of the field region. This may provide a convenient way to manipulate nanodomains in thin films.
The impact of oxygen vacancies on local tunneling properties across rf-sputtered MgO thin films was investigated by optical absorption spectroscopy and conducting atomic force microscopy. Adding O$_2$ to the Ar plasma during MgO growth alters the oxygen defect populations, leading to improved local tunneling characteristics such as a lower density of current hotspots and a lower tunnel current amplitude. We discuss a defect-based potential landscape across ultrathin MgO barriers.
A first-principles-derived method is used to study the morphology and electric-field-induced evolution of stripe nanodomains in (001) BaTiO3 (BTO) ultrathin films, and to compare them with those in (001) Pb(Zr,Ti)O3 (PZT) ultrathin films. The BaTiO3 systems exhibit 180o periodic stripe domains at null electric field, as in PZT ultrathin films. However, the stripes alternate along [1-10] in BTO systems versus [010] in PZT systems, and no in-plane surface dipoles occur in BTO ultrathin films (unlike in PZT materials). Moreover, the evolution of the 180o stripe domains in the BaTiO3 systems, when…
We present a synchrotron grazing incidence x-ray diffraction analysis of the domain structure and polar symmetry of highly strained BiFeO3 thin films grown on LaAlO3 substrate. We revealed the existence of periodic elastic nanodomains in the pure tetragonal-like BFO ultrathin films down to a thickness of 6 nm. A unique shear strain accommodation mechanism is disclosed. We further demonstrated that the periodicity of the nanodomains increases with film thickness but deviates from the classical Kittel's square root law in ultrathin thickness regime (6 - 30 nm). Temperature-dependent experiments …
Graphene is attractive for spintronics due to its long spin life time and high mobility. So far only thick and polycrystalline slabs have been used as ferromagnetic electrodes. We report the growth of flat, epitaxial ultrathin Co films on graphene. These display perpendicular magnetic anisotropy in the thickness range 0.5-1nm, which is confirmed by theory. PMA, epitaxy and ultrathin thickness bring new perspectives for graphene-based spintronic devices such as the zero-field control of an arbitrary magnetization direction, band matching between electrodes and graphene, and interface effects su…
Transport in ultrathin films of LaNiO3 evolves from a metallic to a strongly localized character as the film's thickness is reduced and the sheet resistance reaches a value close to h/e2, the quantum of resistance in two dimensions. In the intermediate regime, quantum corrections to the Drude low- temperature conductivity are observed; they are accurately described by weak localization theory. Remarkably, the negative magnetoresistance in this regime is isotropic, which points to magnetic scattering associated with the proximity of the system to either a spin glass state or the charge ordered …
Switching kinetics in ultrathin epitaxial BaTiO3 films confirms the existence of the homogeneous switching (without domains) in ultrathin ferroelectric films. We suppose that the homogeneous switching in ultrathin films is a common phenomenon for all ferroelectric materials.
First-principles density-functional theory calculations show switching magnetization by 90 degree can be achieved in ultrathin BFO film by applying external electric-field. Up-spin carriers appear to the surface with positive field while down-spin ones to the negative field surface, arising from the redistribution of Fe-t2g orbital. The half-metallic behavior of Fe-3d states in the surface of R phase film makes it a promising candidate for AFM/FM bilayer heterostructure possessing electric-field tunable FM magnetization reversal and opens a new way towards designing spintronic multiferroics. T…
We have performed ab initio density functional calculations of thin Ag films on the Pd(111) surface. We have calculated the structural properties and the electronic bands of the Ag/Pd systems. There is a band gap in the electronic density of states around the centre of the two-dimensional Brillouin zone of the Pd(111) surface, which makes possible the formation of localised states in the adsorbed silver films. We find that quantum well states may form at binding energies around 4 eV.
The coupling between the electrical transport properties of La2/3Sr1/3MnO3 (LSMO) thin films and structural phase transitions of SrTiO3 (STO) substrates at Ts = 105 K has been investigated. We found that the electrical resistivity of LSMO films exhibit a cusp at Ts, which is greatly amplified by tuning films to the verge of metallic and insulating phases, i.e., to the boundary of two delicate competing electronic states. Our results demonstrate that small amounts of strain can tip the subtle balance of competing interactions and tune the electronic properties in correlated electron materials.
The spin and orbital magnetic moments of the Fe3O4 epitaxial ultrathin film synthesized by plasma assisted simultaneous oxidization on MgO(100) have been studied with X-ray magnetic circular dichroism (XMCD). The ultrathin film retains a rather large total magnetic moment, i.e. (2.7+-0.15) uB/f.u., which is ~ 70% of that for the bulk-like Fe3O4. A significant unquenched orbital moment up to (0.54+-0.05) uB/f.u. was observed, which could come from the symmetry breaking at the Fe3O4/MgO interface. Such sizable orbital moment will add capacities to the Fe3O4-based spintronics devices in the magne…
The thickness evolution of in-plane magnetization reversal in ultrathin films is studied with a theoretical model that takes account of surface roughness typical of epitaxial growth. Guided by Néel's model, step edge sites of monolayer-height islands are assigned a two-fold anisotropy in addition to a four-fold anisotropy at all sites. Coercivity is found to depend essentially on both the film thickness and the partial coverage of the topmost layer. Its qualitative features are determined primarily by sample geometry and the size of the step anisotropy compared to the domain wall energy. Magne…
The origin of the correlation between surface reactivity and quantum-size effects, observed in recent experiments on the oxidation of ultrathin magnesium films, is addressed by means of ab-initio calculations and model predictions. We show that the decay length in vacuum of the electronic local density of states at the Fermi energy exhibits systematic oscillations with film thickness, with local maxima induced when a quantum well state at k// = 0 crosses the Fermi energy. The predicted changes in the decay length are expected to have a major impact on the electron transfer rate by tunneling, w…
In this work we are investigating the effect of strain in ultrathin Mn-Ga thin films on the magnetic properties at room temperature. Two different Mn-Ga compositions of which one is furthermore doped with Co were grown on Cr buffered MgO (001) substrates. Films with a thickness below 12nm are highly strained and it was observed that the ratio c/a vs. thickness is depending on composition. Using c/a as an order parameter the PMA is shown to be drastically reduced with increasing strain. These findings should be considered when generalizing and downscaling results obtained from films >20nm. Furt…
Ferromagnetism was observed in a Pt(100) ultrathin film deposited on a SrTiO3(100) substrate. The ferromagnetism, which appears in films with thicknesses of 2.2-4.4 nm, periodically changes with a period of approximately 1 nm (5-6 monolayers) depending on the film thickness. This is consistent with the period derived from the quantum-well states formed in the thin film. X-ray magnetic circular dichroism measurements show the evidence of appearance of intrinsic ferromagnetism in Pt(100) ultra-thin film. In addition, present results suggest a possibility that the orbital magnetic moment of pure …
The mean-field Landau-type theory is used to analyze the polarization properties of epitaxial ferroelectric thin films grown on dissimilar cubic substrates, which induce biaxial compressive stress in the film plane. The intrinsic effect of the film surfaces on the spontaneous polarization is taken into account via the concept of the extrapolation length. The theory simultaneously allows for the influence of the misfit strain imposed on the film lattice by a thick substrate. Numerical calculations are performed for PbTiO3 and BaTiO3 films under an assumption of the polarization reduction in sur…
We study the crystal structure of Pd(100) ultrathin films, which show ferromagnetism induced by the quantum confinement effect, using in-situ X-ray crystal truncation rod measurement and density functional calculation. The energy gain due to the appearance of ferromagnetism in Pd results in flatter and uniform film growth of ferromagnetic Pd films compared with paramagnetic Pd. In addition, ferromagnetic Pd films expand the lattice constant in order to suppress the increase in kinetic energy of electrons accompanied by the occurrence of exchange splitting. Although the traditional theory of ma…
Competition between electronic and atomic reconstruction is a constantly recurring theme in transition-metal oxides. We use density functional theory calculations to study this competition for a model system consisting of a thin film of the polar, infinite-layer structure ACuO2 (A=Ca, Sr, Ba) grown on a nonpolar, perovskite SrTiO3 substrate. A transition from the bulk planar structure to a chain-type thin film accompanied by substantial changes to the electronic structure is predicted for a SrCuO2 film fewer than five unit cells thick. An analytical model explains why atomic reconstruction bec…
We present a combined study with conventional far-infrared and time-domain terahertz ellipsometry of the temperature dependent optical response of SrTiO3 thin films (85 and 8.5 nm) that are grown by pulsed-laser deposition on LSAT substrates. We demonstrate that terahertz ellipsometry is very sensitive to the optical response of these thin films, in particular, to the soft mode of SrTiO3. We show that for the 85 nm film the eigenfrequency of the soft mode is strongly reduced by annealing at 1200 C, whereas for the 8.5 nm film it is hardy affected. For the latter, after annealing the mode remai…
A first-principles-based scheme is developed to simulate properties of (001) PbO-terminated Pb(Zr$_{1-x}$Ti$_{x}$)O$_3$ thin films that are under stress-free and open-circuit boundary conditions. Their low-temperature spontaneous polarization never vanishes down to the minimal thickness, and continuously rotates between the in-plane <010> and <110> directions when varying the Ti composition around x=0.50. Such rotation dramatically enhances piezoelectricity and dielectricity. Furthermore, the order of some phase transitions changes when going from bulk to thin films.
The nonreciprocal propagation of spin waves in an ultrathin Pt/Co/Ni film has been measured by Brillouin light scattering. The frequency nonreciprocity, due to the interfacial Dzyaloshinskii-Moriya interaction (DMI), has a sinusoidal dependence on the in-plane angle between the magnon wavevector and the applied magnetic field. The results, which are in good agreement with analytical predictions reported earlier, yield a value of the DMI constant which is the same as that obtained previously from a study of the magnon dispersion relations. We have demonstrated that our magnon-dynamics based met…
The ultrathin film limit has been shown to be a rich playground for unusual low dimensional physics. Taking the example of SrRuO$_3$ which is ferromagnetic and metallic at the bulk limit, one finds that it becomes antiferromagnetic and insulating at the three monolayers limit when grown on SrTiO$_3$. The origin of the insulating state is traced to strongly orbital dependent exchange splittings. A modest compressive strain of 1% of the SrTiO$_3$ substrate is then found to drive the system into a highly confined two-dimensional 100% spin polarized metallic state. This metal-insulator transition …
Thin FeRh film was extensively studied recently, and an emergent substrate- and capping-dependent interfacial ferromagnetism (FM) was widely observed in experiments. However, the voltage modulation of this interfacial ferromagnetism is barely studied, which would have profound applications in antiferromagnetic (AFM) FeRh-based magnetoelectric-random access memory (MeRAM). Using ab initio techniques, we comparatively study the interfacial ferromagnetic properties and magnetoelectric responses of ultrathin FeRh films capped by heavy transition metal Ta. We find that Ta capping reverses the phase…
The fluid dynamics of the classical dewetting instability in ultrathin films is a non-linear process. However, the physical manifestation of the instability in terms of characteristic length and time scales can be described by a linearized form of the initial conditions of the films's dynamics. Alternately, the thermodynamic approach based on equating the rate of free energy decrease to the viscous dissipation [de Gennes, C. R. Acad. Paris.v298, 1984] can give similar information. Here we have evaluated dewetting in the presence of thermocapillary forces arising from a film-thickness (h) depen…
The evolution of tetragonality with thickness has been probed in epitaxial c-axis oriented PbTiO3 films with thicknesses ranging from 500 down to 24 Angstroms. High resolution x-ray pointed out a systematic decrease of the c-axis lattice parameter with decreasing film thickness below 200 Angstroms. Using a first-principles model Hamiltonian approach, the decrease in tetragonality is related to a reduction of the polarization attributed to the presence of a residual unscreened depolarizing field. It is shown that films below 50 Angstroms display a significantly reduced polarization but still re…
We propose a model for the description of the transport properties of metallic films on a large scale of slab thickness. This model is based on solving the linearized Boltzmann equation in relaxation-time approximation using {\it ab initio} calculations within the framework of the density functional theory. The expression for the relaxation time is derived from the microscopic treatment of the scattering processes and provides the correct thickness dependence for very thin as well as very thick films. The method is applied to the calculation of the in-plane conductivity and the Drude-type plas…
Spin waves in perpendicularly-magnetized Pt/Co/AlO$_x$/Pt ultrathin films with varying Co thicknesses (0.6-1.2 nm) have been studied with Brillouin light spectroscopy in the Damon-Eshbach geometry. The measurements reveal a pronounced nonreciprocal propagation, which increases with decreasing Co thicknesses. This nonreciprocity is attributed to an interfacial Dzyaloshinskii-Moriya interaction (DMI), which is significantly stronger than asymmetries resulting from surface anisotropies for such modes. Results are consistent with an interfacial DMI constant $D_s = -1.7 \pm 0.11$ pJ/m, which favors…
Ferromagnetic materials dominate as the magnetically active element in spintronic devices, but come with drawbacks such as large stray fields, and low operational frequencies. Compensated ferrimagnets provide an alternative as they combine the ultrafast magnetization dynamics of antiferromagnets with a ferromagnet-like spin-orbit-torque (SOT) behavior. However to use ferrimagnets in spintronic devices their advantageous properties must be retained also in ultrathin films (t < 10 nm). In this study, ferrimagnetic Gdx(Fe87.5Co12.5)1-x thin films in the thickness range t = 2-20 nm were grown on h…
An evolution partial differential equation for the surface of a non-wetting single-crystal film in an attractive substrate potential is derived and used to study the dynamics of a pinhole for the varying initial depth of a pinhole and the strengths of the potential and the surface energy anisotropy. The results of the simulations demonstrate how the corresponding parameters may lead to complete or partial dewetting of the film. Anisotropy of the surface energy, through faceting of the pinhole walls, is found to most drastically affect the time to film rupture. In particular, the similations su…
Ultrathin films of Na3Bi on insulating substrates are desired for opening a bulk band gap and generating the quantum spin Hall effect from a topological Dirac semimetal, though continuous films in the few nanometer regime have been difficult to realize. Here, we utilize alternating layer molecular beam epitaxy (MBE) to achieve uniform and continuous single crystal films of Na3Bi(0001) on insulating Al2O3(0001) substrates and demonstrate electrical transport on films with 3.8 nm thickness (4 unit cells). The high material quality is confirmed through in situ reflection high-energy electron diff…
NiFe$_2$O$_4$ thin films with varying thickness were grown on SrTiO$_3$(001) by reactive molecular beam epitaxy. Soft and hard x-ray photoelectron spectroscopy measurements reveal a homogeneous cation distribution throughout the whole film with stoichiometric Ni:Fe ratios of 1:2 independent of the film thickness. Low energy electron diffraction and high resolution (grazing incidence) x-ray diffraction in addition to x-ray reflectivity experiments were conducted to obtain information of the film surface and bulk structure, respectively. For ultrathin films up to 7.3 nm, lateral tensile and vert…
In this paper, a method is presented to create and characterize mechanically robust, free standing, ultrathin, oxide films with controlled, nanometer-scale thickness using Atomic Layer Deposition (ALD) on graphene. Aluminum oxide films were deposited onto suspended graphene membranes using ALD. Subsequent etching of the graphene left pure aluminum oxide films only a few atoms in thickness. A pressurized blister test was used to determine that these ultrathin films have a Young's modulus of 154 \pm 13 GPa. This Young's modulus is comparable to much thicker alumina ALD films. This behavior indic…
A long standing problem of domain switching process - how domains nucleate - is examined in ultrathin ferroelectric films. We demonstrate that the large depolarization fields in ultrathin films could significantly lower the nucleation energy barrier (U*) to a level comparable to thermal energy (kBT), resulting in power-law like polarization decay behaviors. The "Landauer's paradox": U* is thermally insurmountable is not a critical issue in the polarization switching of ultrathin ferroelectric films. We empirically find a universal relation between the polarization decay behavior and U*/kBT.
We have used a first-principles-based scheme to compute the temperature-versus-misfit strain ``Pertsev'' phase diagram of ultrathin films of {\sl incipient} ferroelectric KTaO$_3$. Our results suggest that, at variance with the bulk material, KTaO$_3$ ultrathin films cannot be described as quantum paraelectrics. Rather, the behavior of the films is largely determined by surface/interface effects that favor ferroelectricity and the imperfect screening of the depolarizing fields. This leads to Pertsev phase diagrams that are qualitatively similar to those of {\sl normal} ferroelectrics such as B…
The melting of ultrathin lubricant film by friction between atomically flat surfaces is studied. The additive noises of the elastic shear stress and strain, and the temperature are introduced for building a phase diagram with the domains of sliding, stick-slip, and dry friction. It is shown that increase of the strain noise intensity causes the lubricant film melting even at low temperatures of the friction surfaces.
Experimental efforts to stabilize ferromagnetism in ultrathin films of transition metal oxides have so far failed, despite expectations based on density functional theory (DFT) and DFT+U. Here, we investigate one of the most promising materials, SrRuO$_3$, and include correlation effects beyond DFT by means of dynamical mean field theory. In agreement with experiment we find an intrinsic thickness limitation for metallic ferromagnetism in SrRuO$_3$ thin films. Indeed, we demonstrate that the realization of ultrathin ferromagnetic films is out of reach of standard thin-film techniques. Proposin…
