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1.
Phys Rev Lett ; 128(15): 157205, 2022 Apr 15.
Article in English | MEDLINE | ID: mdl-35499884

ABSTRACT

Triggering and switching magnetic moments is of key importance for applications ranging from spintronics to quantum information. A noninvasive ultrafast control at the nanoscale is, however, an open challenge. Here, we propose a novel laser-based scheme for generating atomic-scale charge current loops within femtoseconds. The associated orbital magnetic moments remain ferromagnetically aligned after the laser pulses have ceased and are localized within an area that is tunable via laser parameters and can be chosen to be well below the diffraction limit of the driving laser field. The scheme relies on tuning the phase, polarization, and intensities of two copropagating Gaussian and vortex laser pulses, allowing us to control the spatial extent, direction, and strength of the atomic-scale charge current loops induced in the irradiated sample upon photon absorption. In the experiment we used He atoms driven by an ultraviolet and infrared vortex-beam laser pulses to generate current-carrying Rydberg states and test for the generated magnetic moments via dichroic effects in photoemission. Ab initio quantum dynamic simulations and analysis confirm the proposed scenario and provide a quantitative estimate of the generated local moments.

2.
J Phys Chem C Nanomater Interfaces ; 126(12): 5435-5442, 2022 Mar 31.
Article in English | MEDLINE | ID: mdl-35392436

ABSTRACT

X-ray Raman spectroscopy (XRS) is an emerging spectroscopic technique that utilizes inelastic scattering of hard X-rays to study X-ray absorption edges of low Z elements in bulk material. It was used to identify and quantify the amount of carbonyl bonds in a cathode sample, in order to track the redox reaction inside metal-organic batteries during the charge/discharge cycle. XRS was used to record the oxygen K-edge absorption spectra of organic polymer cathodes from different multivalent metal-organic batteries. The amount of carbonyl bond in each sample was determined by modeling the oxygen K-edge XRS spectra with the linear combination of two reference compounds that mimicked the fully charged and the fully discharged phases of the battery. To interpret experimental XRS spectra, theoretical calculations of oxygen K-edge absorption spectra based on density functional theory were performed. Overall, a good agreement between the amount of carbonyl bond present during different stages of battery cycle, calculated from linear combination of standards, and the amount obtained from electrochemical characterization based on measured capacity was achieved. The electrochemical mechanism in all studied batteries was confirmed to be a reduction of double carbonyl bond and the intermediate anion was identified with the help of theoretical calculations. X-ray Raman spectroscopy of the oxygen K-edge was shown to be a viable characterization technique for accurate tracking of the redox reaction inside metal-organic batteries.

3.
Sensors (Basel) ; 20(23)2020 Nov 24.
Article in English | MEDLINE | ID: mdl-33255163

ABSTRACT

In this work, we characterise the performance of a Sharp optical aerosol sensor model GP2Y1010AU0F. The sensor was exposed to different environments: to a clean room, to a controlled atmosphere with known aerosol size distribution and to the ambient atmosphere on a busy city street. During the exposure, the output waveforms of the sensor pulses were digitised, saved and a following offline analysis enabled us to study the behaviour of the sensor pulse-by-pulse. A linear response of the sensor on number concentration of the monosized dispersed PSL particles was shown together with an almost linear dependence on particle diameters in the 0.4 to 4 micrometer range. The gathered data about the sensor were used to predict its response to an ambient atmosphere, which was observed simultaneously with a calibrated optical particle counter.

4.
Rev Sci Instrum ; 91(7): 073108, 2020 Jul 01.
Article in English | MEDLINE | ID: mdl-32752866

ABSTRACT

We report an electron scattering experiment on argon gas where a keV electron beam is used as a probe and electrons are collected with a magnetic bottle spectrometer. For this purpose, we have built a thermionic gun that produces electron pulses with nanosecond duration by sweeping the beam across a small aperture. To reach the target, electrons must pass through the hole in an axially symmetric arrangement of strong permanent magnets required to operate the magnetic bottle. From the recorded multi-hit sequence of electron arrival times on the microchannel plate detector, a kinetic energy spectrum is built that allows an analysis of the elastic and inelastic electron scattering channels by means of the coincidence technique. After a description of the instrumental configuration and discussion of suitable working parameters, the results of an angle-integrated (e, 2e) experiment are presented for 800 eV electron scattering on argon atoms.

6.
Sci Rep ; 6: 21012, 2016 Feb 18.
Article in English | MEDLINE | ID: mdl-26888159

ABSTRACT

In this paper we report an X-ray emission study of bulk aqueous sulfuric acid. Throughout the range of molarities from 1 M to 18 M the sulfur Kß emission spectra from H2SO4 (aq) depend on the molar fractions and related deprotonation of H2SO4. We compare the experimental results with results from emission spectrum calculations based on atomic structures of single molecules and structures from ab initio molecular dynamics simulations. We show that the S Kß emission spectrum is a sensitive probe of the protonation state of the acid molecules. Using non-negative matrix factorization we are able to extract the fractions of different protonation states in the spectra, and the results are in good agreement with the simulation for the higher part of the concentration range.

7.
Anal Chem ; 87(11): 5632-9, 2015 Jun 02.
Article in English | MEDLINE | ID: mdl-25927339

ABSTRACT

An experimental and theoretical study of phosphorus electronic structure based on high energy resolution X-ray emission spectroscopy was performed. The Kα and Kß emission spectra of several phosphorus compounds were recorded using monochromatic synchrotron radiation and megaelectronvolt (MeV) proton beam for target excitation. Measured spectra are compared to the results of ab initio quantum chemical calculations based on density functional theory (DFT). Clear correlation between energy position of the Kα emission line and the phosphorus formal oxidation state as well as DFT-calculated number of valence electrons is obtained; measured energy shifts are reproduced by the calculations. Chemical sensitivity is increased further by looking at the Kß emission spectra probing directly the structure of occupied molecular orbitals. Energies and relative intensities of main components are given together with the calculated average atomic character of the corresponding molecular orbitals involved in transitions.


Subject(s)
Chemistry Techniques, Analytical/methods , Phosphorus/chemistry , Quantum Theory , Spectrometry, X-Ray Emission , Limit of Detection , Phosphorus/analysis
8.
J Chem Phys ; 141(14): 144301, 2014 Oct 14.
Article in English | MEDLINE | ID: mdl-25318716

ABSTRACT

We report a theoretical and experimental study of the high resolution resonant K(α) X-ray emission lines around the chlorine K-edge in gas phase 1,1-dichloroethylene. With the help of ab initio electronic structure calculations and cross section evaluation, we interpret the lowest lying peak in the X-ray absorption and emission spectra. The behavior of the K(α) emission lines with respect to frequency detuning highlights the existence of femtosecond nuclear dynamics on the dissociative Potential Energy Surface of the first K-shell core-excited state.

9.
Phys Rev Lett ; 98(24): 243002, 2007 Jun 15.
Article in English | MEDLINE | ID: mdl-17677962

ABSTRACT

We study the Stark effect on doubly excited states of the helium atom below N=2. We present the ab initio photoionization and total inelastic photon scattering cross sections calculated with the method of complex scaling for field strengths F

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