Modeling of a tunable-barrier non-adiabatic electron pump beyond the decay cascade model

We generalize the decay cascade model of charge capture statistics for a tunable-barrier non-adiabatic electron pump dominated by the backtunneling error at the quantum dot decoupling stage. The energy scales controlling the competition between the thermal and the dynamical mechanisms for accurate trapped charge quantization are discussed. Empirical fitting formula incorporating quantum dot re-population errors due to particle-hole fluctuations in the source lead is suggested and tested against an exactly solvable rate equation model.Comment: 2-page summary paper for CPEM Digest'201

Quantum fluctuations and coherence in high-precision single-electron capture

The phase of a single quantum state is undefined unless the history of its creation provides a reference point. Thus quantum interference may seem hardly relevant for the design of deterministic single-electron sources which strive to isolate individual charge carriers quickly and completely. We provide a counterexample by analyzing the non-adiabatic separation of a localized quantum state from a Fermi sea due to a closing tunnel barrier. We identify the relevant energy scales and suggest ways to separate the contributions of quantum non-adiabatic excitation and backtunneling to the rare non-capture events. In the optimal regime of balanced decay and non-adiabaticity, our simple electron trap turns into a single-lead Landau-Zener-backtunneling interferometer, revealing the dynamical phase accumulated between the particle capture and leakage. The predicted "quantum beats in backtunneling" may turn the error of a single-electron source into a valuable signal revealing essentially non-adiabatic energy scales of a dynamic quantum dot.Comment: 7 pages, supplementary info in 3 appendices, final PRL versio

Thermal disorder and correlation effects in anti-perovskite-type copper nitride

This work has been supported by the Latvian National Research Program IMIS2. The EXAFS experiment has been financed from the European Community's Seventh Framework Programme under grant agreement No. 226716 (Project I-20100098 EC). J.T. also gratefully acknowledges support from the National Science Foundation under the DMREF program Grant No. CHE-1534184.Reverse Monte Carlo simulations coupled with evolutionary algorithm were employed for the analysis of the temperature dependent (10–300 K) Cu K-edge extended X-ray absorption fine structure (EXAFS) spectra of polycrystalline copper nitride (Cu3N) with the goal to extract information on the thermal disorder and interatomic correlations in anti-perovskite-type crystal lattice. The obtained results are discussed in comparison with metallic copper and perovskite-type rhenium trioxide. The analysis of EXAFS spectra suggests that the anisotropy of copper atom vibrations is significantly enhanced upon increasing temperature, leading to pronounced tilting motion of NCu6 octahedra. Strong correlation in the motion of atoms was found along –N–Cu–N– atomic chains but it reduces rapidly with an increase of interatomic distance. Finally, anticorrelated motion of neighboring Cu atoms occurs along Cu–Cu bonds and is consistent with breathing-type motion of NCu6 octahedra.National Science Foundation CHE-1534184; Seventh Framework Programme 226716; Institute of Solid State Physics, University of Latvia as the Center of Excellence has received funding from the European Union’s Horizon 2020 Framework Programme H2020-WIDESPREAD-01-2016-2017-TeamingPhase2 under grant agreement No. 739508, project CAMART

Treatment of disorder effects in X-ray absorption spectra beyond the conventional approach

The contribution of static and thermal disorder is one of the largest challenges for the accurate determination of the atomic structure from the extended X-ray absorption fine structure (EXAFS). Although there are a number of generally accepted approaches to solve this problem, which are widely used in the EXAFS data analysis, they often provide less accurate results when applied to outer coordination shells around the absorbing atom. In this case, the advanced techniques based on the molecular dynamics and reverse Monte Carlo simulations are known to be more appropriate: their strengths and weaknesses are reviewed here.Latvian Council of Science project no. lzp-2018/2-0353; Institute of Solid State Physics, University of Latvia as the Center of Excellence has received funding from the European Union’s Horizon 2020 Framework Programme H2020-WIDESPREAD-01-2016-2017-TeamingPhase2 under grant agreement No. 739508, project CAMART

Interpretation of the Cu K-edge EXAFS spectra of Cu3N using ab initio molecular dynamics

Financial support provided by ERDF project No. 1.1.1.2/VIAA/l/16/147 (1.1.1.2/16/I/001) under the activity “Post-doctoral research aid” realized at the Institute of Solid State Physics, University of Latvia is greatly acknowledged. This work was supported by a grant from the Swiss National Supercomputing Centre (CSCS) under the project ID s681 .Cubic copper nitride (Cu3N) has anti-perovskite structure, and its properties are strongly affected by anisotropic thermal vibrations of copper atoms. Ab initio molecular dynamics (AIMD) simulations were performed in the temperature range from 300 K to 700 K in order to probe the details of Cu3N lattice dynamics. The Cu K-edge extended X-ray absorption fine structure (EXAFS) spectrum of bulk Cu3N was used to validate AIMD simulations at 300 K. The AIMD results suggest strong anharmonicity of the Cu–N and Cu–Cu bonds, the rigidity of NCu6 octahedra and strong correlation in atomic motion within –N–Cu–N– atom chains as well as support anisotropy of copper thermal vibrations.National Centre for Supercomputing Applications; Institute of Solid State Physics, Chinese Academy of Sciences; European Regional Development Fund 1.1.1.2/16/I/001,1.1.1.2/VIAA/l/16/147; Swiss National Supercomputing Centre grant under the project ID s681; Institute of Solid State Physics, University of Latvia as the Center of Excellence has received funding from the European Union’s Horizon 2020 Framework Programme H2020-WIDESPREAD-01-2016-2017-TeamingPhase2 under grant agreement No. 739508, project CAMART

Neural Network Approach for Characterizing Structural Transformations by X-Ray Absorption Fine Structure Spectroscopy

AIF acknowledge support by the US Department of Energy, Office of Basic Energy Sciences under Grant No. DE-FG02 03ER15476. AIF acknowledges support by the Laboratory Directed Research and Development Program through LDRD 18-047 of Brookhaven National Laboratory under U.S. Department of Energy Contract No. DE-SC0012704 for initiating his research in machine learning methods. The help of the beamline staff at ELETTRA (project 20160412) synchrotron radiation facility is acknowledged. RMC-EXAFS and MD-EXAFS simulations were performed on the LASC cluster-type computer at Institute of Solid State Physics of the University of Latvia.The knowledge of the coordination environment around various atomic species in many functional materials provides a key for explaining their properties and working mechanisms. Many structural motifs and their transformations are difficult to detect and quantify in the process of work (operando conditions), due to their local nature, small changes, low dimensionality of the material, and/or extreme conditions. Here we use an artificial neural network approach to extract the information on the local structure and its in situ changes directly from the x-ray absorption fine structure spectra. We illustrate this capability by extracting the radial distribution function (RDF) of atoms in ferritic and austenitic phases of bulk iron across the temperature-induced transition. Integration of RDFs allows us to quantify the changes in the iron coordination and material density, and to observe the transition from a body-centered to a face-centered cubic arrangement of iron atoms. This method is attractive for a broad range of materials and experimental conditions.Laboratory Directed Research and Development LDRD 18-047; U.S. Department of Energy DE-FG02 03ER15476; Brookhaven National Laboratory DE-SC0012704; Institute of Solid State Physics, University of Latvia as the Center of Excellence has received funding from the European Union’s Horizon 2020 Framework Programme H2020-WIDESPREAD-01-2016-2017-TeamingPhase2 under grant agreement No. 739508, project CAMART

Amorphous p-Type Conducting Zn-x Ir Oxide (x > 0.13) Thin Films Deposited by Reactive Magnetron Cosputtering

Zinc-iridium oxide (Zn-Ir-O) thin films have been demonstrated as a p-type conducting material. However, the stability of p-type conductivity with respect to chemical composition or temperature is still unclear. In this study we discuss the local atomic structure and the electrical properties of Zn-Ir-O films in the large Ir concentration range. The films are deposited by reactive DC magnetron co-sputtering at two different substrate temperatures-without intentional heating and at 300 {\deg}C. Extended X-ray absorption fine structure (EXAFS) analysis reveals that strongly disordered ZnO4 tetrahedra are the main Zn complexes in Zn-Ir-O films with up to 67.4 at% Ir. As the Ir concentration increases, an effective increase of Ir oxidation state is observed. Reverse Monte Carlo analysis of EXAFS at Zn K-edge shows that the average Zn-O interatomic distance and disorder factor increase with the Ir concentration. We observed that the nano-crystalline w-ZnO structure is preserved in a wider Ir concentration range if the substrate is heated during deposition. At low Ir concentration, the transition from n- to p-type conductivity is observed regardless of the temperature of the substrates. Electrical resistivity decreases exponentially with the Ir concentration in the Zn-Ir-O films

Local structure of A-atom in ABO3 perovskites studies by RMC-EXAFS

The measurements of Sr K-edge XAFS were performed under the approval of Proposal No. 97G042 of Photon Factory (KEK) and partially supported by the Research Grants of Hirosaki University. This work was supported by Bruce Ravel providing data for BTO. Boby Joseph acknowledges IISc Bangalore and ICTP Trieste for financial support through the award of the IISc-ICTP fellowship.The ferroelectric distortions in perovskites were a subject of numerous investigations for a long time. However, some controversial results still exist, coming from the analysis of diffraction (X-ray, neutron or electron) data and X-ray absorption spectra. In this study, our goal was to revisit these classical materials using recently developed methods without imposing any predefined structural model. Local environment around A-type atom in ABO3 perovskites (SrTiO3, BaTiO3, EuTiO3) was studied by X-ray absorption spectroscopy (XAS) in a wide range of temperatures (20–400 K). Using reverse Monte Carlo method enhanced by evolutionary algorithm, the 3D structure was extracted from the extended X-ray absorption fine structure (EXAFS) and interpreted in terms of the radial distribution functions (RDFs). Our findings show that both diffraction and XAS data are consistent, but reflect the structure of the material from different points of view. In particular, when strong correlations in the motion of certain atoms are present, the information obtained by XAS might lead to a different from expected shape of the RDF. At the same time, the average positions of all atoms are in good agreement with those given by diffraction. This makes XAS an important technique for studying interatomic correlations and lattice dynamics.Abdus Salam International Centre for Theoretical Physics; Institute of Solid State Physics, University of Latvia as the Center of Excellence has received funding from the European Union’s Horizon 2020 Framework Programme H2020-WIDESPREAD-01-2016-2017-TeamingPhase2 under grant agreement No. 739508, project CAMART

Local Structure of Multiferroic MnWO 4 and Mn 0.7 Co 0.3 WO 4 Revealed by the Evolutionary Algorithm

A novel reverse Monte Carlo/evolutionary algorithm scheme was applied to the analysis of the W L 3 -edge and Mn(Co) K-edges EXAFS spectra from multiferroic MnWO 4 and Mn 0.7 Co 0.3 WO 4 . A 3D structural model, consistent with the experimental data, was obtained, and the influence of composition and temperature on the local structure of tungstates is discussed