We address, by means of ab-initio calculations, the origin of the correlation that has been observed experimentally between the chemisorption energy of CO on nanoscale Cu(001) supported films and quantum-size effects. The calculated chemisorption energy shows systematic oscillations, as a function of film thickness, with a periodicity corresponding to that of quantum-well states at the surface-Brillouin-zone center crossing the Fermi energy. We explain this trend based on the oscillations, with film thickness, of the decay length on the vacuum side of the quantum-well states at the Fermi energy. Contrary to previous suggestions, we find that the actual oscillations with film thickness of the density of states per atom of the film at the Fermi energy cannot account for the observed trend in the chemisorption energy.
We present the observation of a transverse thermopower, or Planar Nernst Effect, in patterned ultrathin film (8 nm) of La0.7Sr0.3MnO3 (LSMO) driven by heat current applied in-plane of the film and Planar Hall Effect (PHE) in the same LSMO ultrathin film with in-plane current of 100 microA is also investigated. Even for temperature difference of 5 K the Planar Nernst Effect in ultrathin film (8 nm) shows a coercivity of 3 Oe same as observed in Planar Hall Effect measurement and confirms the ferromagnetic nature of thin film. The angular dependence of transverse voltages shows four-fold sin{the…
We discuss the optical response peculiarities for ultrathin plasmonic films of finite lateral size. Due to their plasma frequency spatial dispersion caused by the spatial confinement of the electron motion, the film dielectric permittivity tensor is spatially dispersive as well and so nonlocal. Such a confinement induced nonlocality can result in peculiar magneto-optical effects. For example, the frequency dependence of the magnetic permeability of the film exhibits a sharp resonance structure shifting to the red as the film aspect ratio increases. The properly tuned ultrathin plasmonic films …
Spin-split two-dimensional electronic states have been observed on ultrathin Sn(001) films grown on InSb(001) substrates. Angle-resolved photoelectron spectroscopy (ARPES) performed on these films revealed Dirac-cone-like linear dispersion around the $\barΓ$ point of surface Brillouin zone, suggesting nearly massless electrons belonging to 2D surface states. The states disperse across a bandgap between bulk-like quantum well states in the films. Moreover, both circular dichroism of ARPES and spin-resolved ARPES studies show helical spin polarization of the Dirac-cone-like surface states, sugge…
We present the results of Monte-Carlo studies of the non-equilibrium properties of ferromagnetic Heisenberg films. Aging effects were observed in non-equilibrium critical behavior. The calculations were carried out for both high-temperature and low-temperature initial states. The characteristic correlation time, which diverges at the transition temperature in the thermodynamic limit, was obtained as a function of system size and waiting time.
Ultrathin iron oxide films epitaxially grown on the (111)- and (0001)-oriented metal single crystal supports exhibit unique electronic, catalytic and magnetic properties not observed for the corresponding bulk oxides. These properties originate mainly from the presence of Moiré superstructures which, in turn, disqualify ultrathin films as model systems imitating bulk materials. We present a route for the preparation of a close-packed Moiré-free ultrathin iron oxide film, namely FeO(111) on Ag(111). Experimental scanning tunneling microscopy (STM), low energy electron diffraction (LEED) and x-r…
We have investigated the effect of electric field control on the magnetization and the transport properties in La0.7Ca0.3MnO3 (LCMO) ultrathin film (~10 nm) by using it as the semiconductor channel material of a prototypical field effect device and SiO2 as dielectric gate. A large electroresistance (ER) of ~78% at Vg = -8 V is found in LCMO at 200 K. The direct magnetization measurements confirm the formation of a large ferromagnetic phase with the increase in the applied gate voltage at 200 K.
We investigate the optical properties of an ultrathin film of a topological insulator in the presence of an in-plane magnetic field. We show that due to the combination of the overlap between the surface states of the two layers and the magnetic field, the optical conductivity can show strong anisotropy. This leads to the effective optical activity of the ultrathin film by influencing the circularly polarized incident light. Intriguingly, for a range of magnetic fields, the reflected and transmitted lights exhibit elliptic character. Even for certain values almost linear polarizations are obta…
We study the modification of micromagnetic configurations in nanostructures, due to the Dzyaloshinskii-Moriya interaction (DMI) that appear at the interface of an ultrathin film. We show that this interaction leads to new micromagnetic boundary conditions that bend the magnetization at the edges. We explore several cases of ultrathin film nanostructures that allow analytical calculations (1D systems, domain walls, cycloids and skyrmions), compare with fully numerical calculations, and show that a good physical understanding of this new type of micromagnetics can be reached. We particularly foc…
Employing Brillouin spectroscopy, strong interfacial Dzyaloshinskii-Moriya interactions have been observed in an ultrathin Pt/CoFeB film. Our micromagnetic simulations show that spin-wave nonreciprocity due to asymmetric surface pinning is insignificant for the 0.8nmthick CoFeB film studied. The observed high asymmetry of the monotonic spin wave dispersion relation is thus ascribed to strong Dzyaloshinskii-Moriya interactions present at the Pt/CoFeB interface. Our findings should further enhance the significance of CoFeB as an important material for magnonic, spintronic and skyrmionic applicat…
Electronic density of states (DOS) at Fermi level has been investigated in ultrathin Ag films grown on Si(111)-(7x7) down to the two dimensional limit of a single atomic layer. Measurement of DOS at Fermi level by scanning tunneling spectroscopy shows an approximate (1 - γ/d) dependence, where γ is a constant and d is the film thickness. The results are explained in the light of an analytical theory as well as our density functional theory (DFT) calculations. DFT results also show that in the proximity of the interface the DOS values of the film and the substrate are mutually affected by each …
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.
Against expectations, robust switchable ferroelectricity has been recently observed in ultrathin (1 nm) ferroelectric films exposed to air [V. Garcia $et$ $al.$, Nature {\bf 460}, 81 (2009)]. Based on first-principles calculations, we show that the system does not polarize unless charged defects or adsorbates form at the surface. We propose electrochemical processes as the most likely origin of this charge. The ferroelectric polarization of the film adapts to the bound charge generated on its surface by redox processes when poling the film. This, in turn, alters the band alignment at the botto…
We present a theoretical study of the collective quasiparticle excitations responsible for the electromagnetic response of ultrathin plane-parallel homogeneous periodic single-wall carbon nanotube arrays and weakly inhomogeneous single-wall carbon nanotube films. We show that in addition to varying film composition, the collective response can be controlled by varying the film thickness. For single-type nanotube arrays, the real part of the dielectric response shows a broad negative refraction band near a quantum interband transition of the constituent nanotube, whereby the system behaves as a…
The reflectance difference (RD) as a function of film thickness was measured during Pb deposition on Si(111)-(6x6)Au surface at 105 K. The oblique incident s- and p-polarized light with energy range 0.25-0.60 eV was used. The component of the dielectric function tensor parallel to the surface was determined from the data of experiments and it oscillation due to quantum size effects (QSE) with period of 2 ML within the Pb monolayer-by-monolayer growth was observed.
We report the growth of ultrathin pyrolytic carbon (PyC) films on nickel substrate by using chemical vapor deposition at 1000 °C under methane ambience. We find that the ultra-fast cooling is crucial for PyC film uniformity by controlling the segregation of carbon on nickel. We characterize the in-plane crystal size of PyC film by using Raman spectroscopy. The Raman peaks at ~1354 cm-1 and ~1584 cm-1 wavenumbers are used to extract the D and G bands. The corresponding peak intensities are then used in an excitation energy dependent equation to calculate the in-plane crystal size. Using Raman a…
We employ metadynamics simulations to calculate the free energy landscape of thin ferromagnetic films and perform a systematic study of the temperature dependence of magnetic anisotropy and of the spin-reorientation transitions. By using a simple spin model we recover the well-known power-law behavior of the magnetic anisotropy energy against magnetization and present a rather detailed analysis of the spin-reorientation transitions in ultrathin films. Based on tensorial exchange interactions and anisotropy parameters derived from first-principles calculations we perform simulations for Fe doub…
We study theoretically confinement related effects in the optical response of thin plasmonic films of controlled variable thickness. While being constant for relatively thick films, the plasma frequency is shown to acquire spatial dispersion typical of two-dimensional materials such as graphene, gradually shifting to the red with the film thickness reduction. The dissipative loss, while decreasing at any fixed frequency, gradually goes up at the plasma frequency as it shifts to the red with the film thickness reduced. These features offer a controllable way to tune spatial dispersion and relat…
Anderson localization, the absence of diffusive transport in disordered systems, has been manifested as hopping transport in numerous electronic systems, whereas in recently discovered topological insulators it has not been directly observed. Here we report experimental demonstration of transition from diffusive transport in the weak antilocalization regime to variable range hopping transport in the Anderson localization regime with ultrathin (Bi$_{1-x}$Sb$_x$)$_2$Te$_3$ films. As disorder becomes stronger, negative magnetoconductivity due to the weak antilocalization is gradually suppressed, …
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…
For a ultrathin NiO(001) film of 4 monolayers (ML) thickness grown on Ag(001), the vibrational properties have been determined by high-resolution electron energy loss spectroscopy (HREELS). For the well-ordered pseudomorphically grown film, nine phonon modes have been identified and their dispersions have been revealed along the Gamma-X high-symmetry direction. The comparison with phonon data for a 25 ML thick NiO(001) film shows that the NiO (001) phonon properties are already fully developed at 4 ML. Significant differences are found for the surface-localized phonon S6 which has an increased…
By combining first principles theoretical calculations and experimental optical and structural characterization such as spectroscopic ellipsometry, X-ray spectroscopy, and electron microscopy, we study the dielectric permittivity and plasmonic properties of ultrathin TiN films at an atomistic level. Our results indicate a remarkably persistent metallic character of ultrathin TiN films and a progressive red shift of the plasmon energy as the thickness of the film is reduced. The microscopic origin of this trend is interpreted in terms of the characteristic two-band electronic structure of the s…
The properties of ultrathin films have been studied within the framework of Ising model and the method of random-field interactions. It is shown that the Curie temperature is inversely proportional to the number of layers. Critical exponent $ν$ has been obtained and it is shown that it does not depend on the type of crystalline lattice.
Microscopy and diffraction measurements are presented of ultrathin binary alloy films of ruthenium and molybdenum that are obtained by standard sputter deposition. For compositions close to Ru50Mo50, we find the films to be amorphous. The amorphicity of the films is accompanied by a significant reduction of the roughness with respect to the roughness of equally thick films of either ruthenium or molybdenum. We ascribe this to the absence of the grain structure that is characteristic of the polycrystalline films of the separate elements.
A theoretical model for understanding the formation of interfacial thin films is presented, which combines density functional theory calculations for interface energies with thermodynamic modeling techniques for multicomponent bulk systems. The theory is applied to thin film formation in VC-doped WC-Co cemented carbides. It is predicted that ultrathin VC films may exist in WC/Co interfaces at the high temperature sintering conditions where most of the WC grain growth occurs, which provides an explanation of the grain growth inhibiting effect of VC additions in the WC-Co system.
We present the observation of strain induced sign reversal of anisotropic magnetoresistance (AMR) in LCMO (LCMO) ultrathin films (thickness 4 nm) deposited on STO (001) substrate (STO). We have also observed unusually large AMR in LCMO/STO thin films with thickness of 6 nm below but close to its Curie temperature (TC) which decrease as the film thickness increases. The sign reversal of AMR (with a maximum value of - 6) with magnetic field or temperature for the 4 nm thin film may be attributed to the increase in tensile strain in the plane of the thin film which in turn facilitates the rotatio…
We predict spin Hall angles up to 80% for ultrathin noble metal films with substitutional Bi impurities. The colossal spin Hall effect is caused by enhancement of the spin Hall conductivity in reduced sample dimension and a strong reduction of the charge conductivity by resonant impurity scattering. These findings can be exploited to create materials with high efficiency of charge to spin current conversion by strain engineering.
We develop the multi-band BCS model of superconductivity in the ultrathin films using the orthogonal tight-binding approximation for constructing the electron wavefunctions. This allows for relatively simple determination of the band structure near the Fermi level as well as the electron-electron interaction matrix elements of the BCS type. The model is applied to the ultrathin MgB$_2$(0001) films, for which the critical temperature values are calculated in the thickness range 2...10 MgB$_2$ layers. The importance of the boundary conditions is emphasised, as either boron or magnesium layers ma…
Well-ordered ultrathin films of NiO have been prepared on an Ag(001) substrate using molecular beam epitaxy. With the help of angle-resolved two-photon photoemission (2PPE) a series of image potential states (IPS) for film thicknesses of 2--4 monolayers (ML) has been identified. By time-resolved 2PPE, the lifetimes of the first three IPS and their dependence on the oxide film thickness have been determined. While the lifetimes of the (n=1) IPS are all in the range of 27--42 fs, the values for the (n=2) IPS decrease from 85 fs for 2 ML to 33 fs for 4 ML. These differences are discussed in terms…
We theoretically investigate the exchange interaction between magnetic impurities in ultrathin Bi$_2$Se$_3$ topological insulator films by taking into account the low-energy states produced by the impurities. We find that the locally induced impurity resonances strongly influence the exchange interaction between magnetic moments. In particular, we find a non-collinear alignment being more favorable than the collinear ferromagnetic alignment preferred when impurity states are ignored and only the pristine topological insulator band structure is considered. Moreover, we show that by applying of …
Ultrathin FeSe films grown on SrTiO$_{3}$ substrates are a recent milestone in atomic material engineering due to their important role in understanding unconventional superconductivity in Fe-based materials. Using femtosecond time- and angle-resolved photoelectron spectroscopy, we study phonon frequencies in ultrathin FeSe/SrTiO$_{3}$ films grown by molecular beam epitaxy. After optical excitation, we observe periodic modulations of the photoelectron spectrum as a function of pump-probe delay for 1 unit cell, 3 unit cell, and 60 unit cell thick FeSe films. The frequencies of the coherent inten…
We studied the spectral dynamics of single fluorescent dye molecules embedded in ultrathin films (5 - 100 nm) of the amorphous polymer polyisobutylene at cryogenic temperatures and its variation with film thickness. Noticeable portion of molecules in the ensemble show a behavior which is inconsistent with the standard tunneling model: Their spectral lines are subject to irreversible spectral jumps, continuous shifting, and abrupt chaotic changes of the linewidth or jumping rate. In films thinner than 100 nm, the occurrence of "non-standard" spectral behavior increases with decreasing sample th…
We analyze the finite temperature phase diagram of ultrathin magnetic films by introducing a mean field theory, valid in the low anisotropy regime, i.e., close to de Spin Reorientation Transition. The theoretical results are compared with Monte Carlo simulations carried out on a microscopic Heisenberg model. Connections between the finite temperature behavior and the ground state properties of the system are established. Several properties of the stripes pattern, such as the presence of canted states, the stripes width variation phenomenon and the associated magnetization profiles are also ana…
Recently, there have been intense efforts in searching for new topological insulator (TI) materials. Based on first-principles calculations, we find that all the ultrathin Bi (111) films are characterized by a nontrivial Z2 number independent of the film thickness, without the odd-even oscillation of topological triviality as commonly perceived. The stable nontrivial Z2 topology is retained by the concurrent band gap inversions at multiple time-reversal-invariant k-points and associated with the intermediate inter-bilayer coupling of the multi-bilayer Bi film. Our calculations further indicate…
Uniform and large area synthesis of bulk insulating ultrathin films is an important subject toward applications of a surface of three dimensional topological insulators (3D-TIs) in various electronic devices. Here we report epitaxial growth of bulk insulating three dimensional topological insulator (3D-TI) Bi2-xSbxTe3-ySey (BSTS) ultrathin films, ranging from a few quintuple to several hundreds of layaers, on mica in a large-area (1 cm2) via catalyst free physical vapor deposition. These films can nondestructively be exfoliated using deionized water and transferred to various kinds of substrat…
We have studied the magneto-optical spectra of ultrathin magnetic films deposited on Si substrates coated with an oxide layer (SiOx). We find that the Kerr rotation angle and the ellipticity of ~1 nm thick CoFeB thin films, almost transparent to visible light, show a strong dependence on the thickness of the SiOx layer. The Kerr signal from the 1 nm CoFeB thin film can be larger than that of ~100 nm thick CoFeB films for a given SiOx thickness and light wavelength. The enhancement of the Kerr signal occurs when optical interference takes place within the SiOx layer. Interestingly, under such r…
We theoretically study the generic behavior of the penetration depth of the edge states in two-dimensional quantum spin Hall systems. We found that the momentum-space width of the edge-state dispersion scales with the inverse of the penetration depth. As an example of well-localized edge states, we take the Bi(111) ultrathin film. Its edge states are found to extend almost over the whole Brillouin zone. Correspondingly, the bismuth (111) 1-bilayer system is proposed to have well-localized edge states in contrast to the HgTe quantum well.
We explore a new type of domain wall structure in ultrathin films with perpendicular anisotropy, that is influenced by the Dzyaloshinskii-Moriya interaction due to the adjacent layers. This study is performed by numerical and analytical micromagnetics. We show that these walls can behave like Neel walls with very high stability, moving in stationary conditions at large velocities under large fields. We discuss the relevance of such walls, that we propose to call Dzyaloshinskii domain walls, for current-driven domain wall motion under the spin Hall effect.
The discovery of high-temperature superconductivity in FeSe/STO has trigged great research interest to reveal a range of exotic physical phenomena in this novel material. Here we present a temperature dependent magnetotransport measurement for ultrathin FeSe/STO films with different thickness and protection layers. Remarkably, a surprising linear magnetoresistance (LMR) is observed around the superconducting transition temperatures but absent otherwise. The experimental LMR can be reproduced by magnetotransport calculations based on a model of magnetic field dependent disorder induced by spin …
We demonstrate that topological-chiral magnetic interactions can play a key role for magnetic ground states in ultrathin films at surfaces. Based on density functional theory we show that significant chiral-chiral interactions occur in hexagonal Mn monolayers due to large topological orbital moments which interact with the emergent magnetic field. Due to the competition with higher-order exchange interactions superposition states of spin spirals such as the 2Q state or a distorted 3Q state arise. Simulations of spin-polarized scanning tunneling microscopy images suggest that the distorted 3Q s…
A film-coupled metamaterial structure is numerically investigated for enhancing the light absorption in an ultrathin photovoltaic layer of crystalline gallium arsenide (GaAs). The top subwavelength concave grating and the bottom metallic film could not only effectively trap light with the help of wave interference and magnetic resonance effects excited above the bandgap, but also practically serve as electrical contacts for photon-generated charge collection. The energy absorbed by the active layer is greatly enhanced in the film-coupled metamaterial structure, resulting in significant enhance…
We report broadband ferromagnetic resonance (FMR) measurements based on a coplanar waveguide (CPW) of ultrathin magnetic film structures that comprise in-plane/out-of-plane decoupled layers deposited on nonmagnetic buffer layers of various thickness or other buffer structures with a diverse sheet resistance. We show that the excitation of the fundamental mode can be substantially (up to 10 times) enhanced in the structures deposited on buffer layers with a low sheet resistance in comparison to the structures deposited on thin or weakly conducting buffer layers. The results are analyzed in term…
PtSe$_2$ ultrathin films are used as the channel of back-gated field-effect transistors (FETs) that are investigated at different temperatures and under super-continuous white laser irradiation. The temperature-dependent behavior confirms the semiconducting nature of multilayer PtSe$_2$, with p-type conduction, a hole field-effect mobility up to 40 cm2/(Vs) and significant gate modulation. Electrical conduction measured along different directions shows isotropic transport. A reduction of PtSe$_2$ channel conductance is observed under exposure to light. Such negative photoconductivity is explai…
The structure and strain of ultrathin CoO films grown on a Pt(001) substrate and on a ferromagnetic PtFe pseudomorphic layer on Pt(001) have been determined with insitu and real time surface x-ray diffraction. The films grow epitaxially on both surfaces with an in-plane hexagonal pattern that yields a pseudo-cubic CoO(111) surface. A refined x-ray diffraction analysis reveals a slight monoclinic distortion at RT induced by the anisotropic stress at the interface. The tetragonal contribution to the distortion results in a ratio c/a > 1, opposite to that found in the low temperature bulk CoO pha…
We consider the diffusion of markers in a layered medium, with the lateral diffusion coefficient being the function of hight. We show that the probability density of the lateral displacements follows one-dimensional Batchelor's equation with time-dependent diffusion coefficient governed by the particles' redistribution in height. For the film of a finite thickness the resulting mean squared displacement exhibits superdiffusion at short times and crosses over to normal diffusion at long times. The approach is used for description of experimental results on inhomogeneous molecular diffusion in t…
Recent emergence of two-dimensional (2D) crystalline superconductors has provided a promising platform to investigate novel quantum physics and potential applications. To reveal essential quantum phenomena therein, ultralow temperature transport investigation on high quality ultrathin superconducting films is critically required, although it has been quite challenging experimentally. Here we report a systematic transport study on the ultrathin crystalline PdTe2 films grown by molecular beam epitaxy (MBE). Interestingly, a new type of Ising superconductivity in 2D centrosymmetric materials is r…
Here we report a method to fabricate high quality Bi2Se3 thin films using molecular beam epitaxy with a radio frequency cracker cell as an atomic selenium source. With rates close to exact stoichiometry, optimal layer-by-layer growth of high quality Bi2Se3 thin films with smooth surfaces, has been achieved on CaF2(111) substrates and Si(111) substrates with a thin CaF2 buffer layer(CaF2/Si). Transport measurements show a characteristic weak antilocalization mangnetoresistance, with emergence of weak localization in the ultrathin film limit. Quantum Oscillations attributed to the topological su…
By means of ab initio calculations, we have investigated the effect of H adsorption in the structural, electronic and magnetic properties of ultrathin Co films on Ru(0001). Our calculations predict that H occupies hollow sites preserving the two-dimensional 3-fold symmetry. The formation of a complete H overlayer leads to a very stable surface with strong H-Co bonds. H tends to suppress surface features, in particular, the enhancement of the magnetic moments of the bare film. The H-induced effects are mostly confined to the Co atoms bonded to H, independent of the H coverage or of the thicknes…
Hanle magnetoresistance (HMR) is a type of magnetoresistance where interplay of the spin Hall effect, Hanle-type spin precession, and spin-dependent scattering at the top/bottom surfaces in a heavy metal controls the effect. In this study, we modulate HMR in ultrathin Pt by ionic gating, where the surface Rashba field created by a strong electric field at the interface between the ionic gate and Pt plays the dominant role in the modulation. This finding can facilitate investigations of gate-tunable, spin-related effects and fabrication of spin devices.
We use the continuum micromagnetic framework to derive the formulas for compact skyrmion lifetime due to thermal noise in ultrathin ferromagnetic films with relatively weak interfacial Dzyaloshinskii-Moriya interaction. In the absence of a saddle point connecting the skyrmion solution to the ferromagnetic state, we interpret the skyrmion collapse event as ``capture by an absorber'' at microscale. This yields an explicit Arrhenius collapse rate with both the barrier height and the prefactor as functions of all the material parameters, as well as the dynamical paths to collapse.
