The irradiation of SrTiO$_3$ single crystals with swift heavy ions leads to modifications of the surface. The details of the morphology of these modifications depends strongly on the angle of incidence and can be characterized by atomic force microscopy. At glancing angles, discontinuous chains of nanosized hillocks appear on the surface. The latent track radius can be determined from the variation of the length of the chains with the angle of incidence. This radius is material specific and allows the calculation of the electron-phonon-coupling constant for SrTiO$_3$. We show that a theoretical description of the nanodot creation is possible within a two-temperature model if the spatial electron density is taken into account. The appearance of discontinuous features can be explained easily within this model, but it turns out that the electronic excitation dissipates on a femtosecond time scale and thus too rapidly to feed sufficient energy into the phonon system in order to induce a thermal melting process. We demonstrate that this can be solved if the temperature dependent diffusion coefficient is introduced into the model.
We experimentally discovered that Al2O3 and MgO exhibit well-pronounced nanometric modifications on the surfaces when irradiated under grazing incidence with 23 MeV I beam, in contrast to normal incidence irradiation with the same ion beam when no damage was found. Moreover, ions in these two materials produce notably different structures: grooves surrounded with nanohillocks on MgO surfaces vs. smoother, roll-like discontinuous structures on the surfaces of Al2O3. To explain these results, detailed numerical simulations were performed. We identified that a presence of the surface inhibits rec…
We present an investigation of the near-surface tetragonal phase transition in SrTiO3, using the complementary techniques of beta-detected nuclear magnetic resonance and grazing-incidence X-ray diffraction. The results show a clear depth dependence of the phase transition on scales of a few microns. The measurements support a model in which there are tetragonal domains forming in the sample at temperatures much higher than the bulk phase transition temperature. Moreover, we find that these domains tend to form at higher temperatures preferentially near the free surface of the crystal. The deta…
The ability to generate a change of the lattice parameter in a near-surface layer of a controllable thickness by ion implantation of strontium titanate is reported here using low energy He+ ions. The induced strain follows a distribution within a typical near-surface layer of 200 nm as obtained from structural analysis. Due to clamping effect from the underlying layer, only perpendicular expansion is observed. Maximum distortions up to 5-7% are obtained with no evidence of amorphisation at fluences of 1E16 He+ ions/cm2 and ion energies in the range 10-30 keV.
The high energy density of electronic excitations due to the impact of swift heavy ions can induce structural modifications in materials. We present a X-ray diffractometer called ALIX, which has been set up at the low-energy IRRSUD beamline of the GANIL facility, to allow the study of structural modification kinetics as a function of the ion fluence. The X-ray setup has been modified and optimized to enable irradiation by swift heavy ions simultaneously to X-ray pattern recording. We present the capability of ALIX to perform simultaneous irradiation - diffraction by using energy discrimination…
The time-resolved photoconductance of amorphous and crystalline LaAlO$_3$/SrTiO$_3$ interfaces, both hosting an interfacial 2-dimensional electron gas, is investigated under irradiation by variable-wavelengths, visible or ultraviolet photons. Unlike bare SrTiO$_3$ single crystals, showing relatively small photoconductance effects, both kinds of interfaces exhibit an intense and highly persistent photoconductance with extraordinarily long characteristic times. The temporal behaviour of the extra photoinduced conductance persisting after light irradiation shows a complex dependence on interface …
Transient Ferromagnetism in Ultrafast Phase Transitions in Perovskites under XUV Irradiation: A Comparative Study of SrTiO3 and KTaO3
Institute of Physics, Czech Academy of Sciences（捷克科学院物理研究所）；Faculty of Nuclear Sciences and Physical Engineering, Czech Technical University in Prague（布拉格捷克理工大学核科学与物理工程学院）；Institute of Plasma Physics, Czech Academy of Sciences（捷克科学院等离子体物理研究所）
In this paper we show how single layer graphene can be utilized to study swift heavy ion (SHI) modifications on various substrates. The samples were prepared by mechanical exfoliation of bulk graphite onto SrTiO$_3$, NaCl and Si(111), respectively. SHI irradiations were performed under glancing angles of incidence and the samples were analysed by means of atomic force microscopy in ambient conditions. We show that graphene can be used to check whether the irradiation was successful or not, to determine the nominal ion fluence and to locally mark SHI impacts. In case of samples prepared in situ…
We have used grazing-angle infrared spectroscopy to detect the Berreman effect (BE) in the quasi-two-dimensional electron system (q-2DES) which forms spontaneously at the interface between SrTiO$_{3}$ (STO) and a thin film of LaAlO$_3$ (LAO). From the BE, which allows one to study longitudinal optical excitations in ultrathin films like the q-2DES, we have extracted at different temperatures its thickness, the charge density and mobility of the carriers under crystalline LAO (sample A), and the charge density under amorphous LAO (sample B). This quantity turns out to be higher than in sample A…
Mastery of order-disorder processes in highly non-equilibrium nanostructured oxides has significant implications for the development of emerging energy technologies. However, we are presently limited in our ability to quantify and harness these processes at high spatial, chemical, and temporal resolution, particularly in extreme environments. Here we describe the percolation of disorder at the model oxide interface LaMnO$_3$ / SrTiO$_3$, which we visualize during in situ ion irradiation in the transmission electron microscope. We observe the formation of a network of disorder during the initia…
The new EUV Lithography tools for IC High Volume Manufacture at 22nm make use of EUV radiation at λ= 13.5nm. High power Laser (LPP) and Discharge (DPP)EUV light sources are based on Sn plasmas for the optimum conversion of electrical power to in-band radiation. Sn-fueled sources emit debris such as Sn particles in a rather wide energy spectrum: from thermalized Sn to several tens keV fast ions. Tin interaction with the collector mirrors surfaces facing the high power EUV light source leads to the degradation of the optical performance and productivity of the litho tool, therefore debris must b…
Effects of X-ray irradiation on the electronic structure of LaAlO$_3$/SrTiO$_3$ (LAO/STO) samples, grown at low oxygen pressure and post-annealed ex-situ till recovery of their stoichiometry, were investigated by soft-X-ray ARPES. The irradiation at low sample temperature below ~100K creates oxygen vacancies (VOs) injecting Ti t2g-electrons into the interfacial mobile electron system (MES). At this temperature the oxygen out-diffusion is suppressed, and the VOs are expected to appear mostly in the top STO layer. However, we observe a pronounced three-dimensional (3D) character of the X-ray gen…
A metallic surface is realized on stoichiometric and insulating (100) SrTiO$_3$ by Ar$^+$ - ion irradiation. The sheet carrier density and Hall mobility of the layer are $\sim$$4.0$ $\times$ $10^{14}$ $/cm^2$ and $\sim$$2$ $\times$ $10^3$ $cm^2/Vs$ respectively at 15 K for the irradiation dose of $\sim$4.2 $\times 10^{18}$ $ions/cm^2$. These samples display ultraviolet light sensitive photoconductivity (PC) which is enhanced abruptly below the temperature ($\approx$100 K) where SrTiO$_3$ crystal undergoes an antiferrodistortive cubic-to-tetragonal ($O_h^1$ $\rightarrow$ $D_{4h}^{18}$) structur…
SrTiO$_3$ is a highly efficient photocatalyst for the overall water splitting reaction under UV irradiation. However, an atomic-level understanding of the active surface sites responsible for the oxidation and reduction reactions is still lacking. Here we present a unified experimental and computational account of the photocatalytic activity at the SrO- and TiO$_2$- terminations of aqueous-solvated [001] SrTiO$_3$. Our experimental findings show that the overall water-splitting reaction proceeds on the SrTiO$_3$ surface only when the two terminations are simultaneously exposed to water. Our si…
The novel electronic properties emerging at interfaces between transition metal oxides, and in particular the discovery of conductivity in heterostructures composed of LaAlO$_3$ (LAO) and SrTiO$_3$ (STO) band insulators, have generated new challenges and opportunities in condensed matter physics. Although the interface conductivity is stabilized when LAO matches or exceeds a critical thickness of 4 unit cells (u.c.), other phenomena such as a universal metallic state found on the bare surface of STO single crystals and persistent photon-triggered conductivity in otherwise insulating STO-based …
The aim of this work is to investigate feasibility of the ion beam analysis techniques for monitoring swift heavy ion track formation. First, use of the in situ Rutherford backscattering spectroscopy in channeling mode to observe damage build-up in quartz SiO2 after MeV heavy ion irradiation is demonstrated. Second, new results of the in situ grazing incidence time-of-flight elastic recoil detection analysis used for monitoring the surface elemental composition during ion tracks formation in various materials are presented. Ion tracks were found on SrTiO3, quartz SiO2, a-SiO2 and muscovite mic…
The effects of ion beam induced atomic mixing and subsequent thermal treatment in Si/C multilayer structures are investigated by use of the technique of grazing incidence X-ray diffraction (GIXRD) and Raman spectroscopy. The [Si (3.0 nm) / C (2.5 nm)]x10 /Si multilayer films were prepared by electron beam evaporation under ultra high vacuum (UHV) environment. The layer thicknesses were measured using in-situ quartz crystal oscillator. These multilayer films were subjected to 40 keV Ar+ ion irradiation with fluences 5E-16 (low fluence) and 1E-17 ions / cm2 (high fluence).The as-prepared and irr…
With infrared (IR) ellipsometry and DC resistance measurements we investigated the photo-doping at the (001) and (110) surfaces of SrTiO$_3$ (STO) single crystals and at the corresponding interfaces of LaAlO$_3$/SrTiO$_3$ (LAO/STO) heterostructures. In the bare STO crystals we find that the photo-generated charge carriers, which accumulate near the (001) surface, have a similar depth profile and sheet carrier concentration as the confined electrons that were previously observed in LAO/STO (001) heterostructures. A large fraction of these photo-generated charge carriers persist at low temperatu…
We present theoretical and experimental data on the threshold behaviour of nanodot creation with swift heavy ions. A model calculation based on a two-temperature model taking the spatially resolved electron density into account gives a threshold of 12 keV/nm below which the energy density at the end of the track is no longer high enough to melt the material. In the corresponding experiments we irradiated SrTiO$_3$ surfaces under grazing incidence with swift heavy ions. The resulting chains of nanodots were analyzed by atomic force microscopy. In addition, samples irradiated under normal incide…
Molecular contamination of a grazing incidence collector for extreme ultraviolet (EUV) lithography was experimentally studied. A carbon film was found to have grown under irradiation from a pulsed tin plasma discharge. Our studies show that the film is chemically inert and has characteristics that are typical for a hydrogenated amorphous carbon film. It was experimentally observed that the film consists of carbon (~70 at. %), oxygen (~20 at. %) and hydrogen (bound to oxygen and carbon), along with a few at. % of tin. Most of the oxygen and hydrogen are most likely present as OH groups, chemica…
In recent experiments the irradiation of insulators of perovskite type with swift heavy ions under glancing incidence has been shown to provide a unique means to generate periodically arranged nanodots at the surface. The physical origin of these patterns has been suggested to stem from a highly anisotropic electron density distribution within the bulk. In order to show the relevance of the electron density distribution of the target we present a model calculation for the system Xe$^{+23}$ $\to$ SrTiO$_{3}$ that is known to produce the aforementioned surface modifications. On the basis of the …
