arXiv subjects

Jan Dreiser

Publications and source records attributed to Jan Dreiser.

14 recordsLinked to original sources

arXiv2025

Coherent microwave control of coupled electron-muon centers

Coherent control by means of tailored excitation is a key to versatile experimental schemes for spectroscopic investigation and technological utilization of quantum systems. Here we study a quantum system which consists of a coupled electron-moun spin state, i.e., muonium, a light isotope of hydrogen. We demonstrate the most fundamental coherent control techniques by microwave excitation of spin transitions, namely driven Rabi oscillations and Ramsey fringes upon free evolution. Unprecedented performance is achieved by the microwave hardware devised for these experiments, which enables coherent spin manipulation of individual, isolated, muonium centers. For muonium formed in SiO$_2$ with strong electron-muon hyperfine interaction, a virtually undamped free precession signal is observed up to a 3.5 $\mu$s time window. For muonium formed in Si with weak and anisotropic hyperfine interaction, a strong drive at the multi-quantum transition decouples the muonium center from its magnetic environment formed by the bath of $^{29}$Si nuclear spins at natural abundance. We expect that these capabilities will provide a powerful tool to investigate the effect of the environment on isolated coupled spins, uncover the details of coupled electron-muon systems in matter and validate quantum electrodynamics in the context of muonium spectroscopy.

quant-ph↗

arXiv2024

Orientation-Driven Large Magnetic Hysteresis of Er(III) Cyclooctatetraenide-Based Single-Ion Magnets Adsorbed on Ag(100)

The molecular self-assembly and the magnetic properties of two cyclooctatetraenide (COT) - based single-ion magnets (SIM) adsorbed on Ag(100) in the sub-monolayer range are reported. Our study combines scanning-tunneling microscopy, X-ray photoemission spectroscopy and polarized X-ray absorption spectroscopy to show that Cp*ErCOT (Cp* = 1,2,3,4,5-pentamethylcyclopentadienide anion) SIMs self-assemble as alternating compact parallel rows including standing-up and lying-down conformations, following the main crystallographic directions of the substrate. Conversely, K[Er(COT)$_2$], obtained from subliming the [K(18-c-6)][Er(COT)$_2$]$\cdot$ 2THF salt, forms uniaxially ordered domains with the (COT)$^{2-}$ rings perpendicular to the substrate plane. The polarization-dependent X-ray absorption spectra reproduced by the multiX simulations suggest that the strong in-plane magnetic anisotropy of K[Er(COT)$_2$]/Ag(100) and the weak out-of-plane anisotropy of Cp*ErCOT/Ag(100) can be attributed to the strikingly different surface ordering of these two complexes. Compared to the bulk phase, surface-supported K[Er(COT)$_2$] exhibits a similarly large hysteresis opening, while the Cp*ErCOT shows a rather small opening. This result reveals that despite structural similarities, the two organometallic SMMs have strongly different magnetic properties when adsorbed on the metal substrate, attributed to the different orientations and the resulting interactions of the ligand rings with the surface.

cond-mat.mtrl-sci↗

arXiv2024

In-plane Antiferromagnetism in Ferromagnetic Kagome Semimetal Co3Sn2S2

Co3Sn2S2 has been reported to be a Weyl semimetal with broken time-reversal symmetry with c axis ferromagnetism (FM) below a Curie temperature of 177 K. Despite the large interest in Co3Sn2S2, the magnetic structure is still under debate and recent studies have challenged our understanding of the magnetic phase diagram of Co3Sn2S2 by reporting unusual magnetic phases including the presence of exchange bias. Understanding the magnetism of Co3Sn2S2 is important since its electronic band structure including the much-celebrated flat bands and Weyl nodes depend on the magnetic phase. In this work, using X-ray Magnetic Circular Dichroism (XMCD), we establish that the magnetic moment in Co arises from the spin, with negligible orbital moment. In addition, we detect an in-plane AFM minority phase in the sea of a FM phase using spatially-resolved angle-resolved photoemission spectroscopy ({\mu}-ARPES) combined with density functional theory (DFT) calculation. Separately, we detect a sharp flat band precisely at the Fermi level (EF) at some regions in the sample, which we attribute to a surface state. The AFM phase survives even to the low temperature of 6 K. This example of entirely different magnetic ground states in a stoichiometric intermetallic invites further efforts to explore the observed AFM phase and understand the origin and nature of the magnetic and electronic inhomogeneity on the mesoscale and the interface between the AFM and FM phases.

cond-mat.mtrl-sci↗

arXiv2023

Robust room temperature ferromagnetism in an itinerant van der Waals antiferromagnet

The coexistence of antiferromagnetic and ferromagnetic order at room temperature in single-phase van der Waals materials, particularly within the two-dimensional limit, has attracted significant research interest. Nonetheless, such materials are rare. In this work, we introduce an itinerant van der Waals antiferromagnet (Fe0.56Co0.44)5GeTe2, where the ferromagnetic order of its exfoliated flakes remains discernible up to room temperature, extending down to the monolayer limit. A notable phenomenon observed is the evident odd-even layer-number effect at high temperature (e.g., T = 150 K). Such behaviour can be expounded by a linear-chain model. Of particular interest is the robust ferromagnetic order observed in even-layer flakes at low temperature (e.g., T = 2 K), which could potentially be attributed to spin-polarized defects. The intricate interplay among magnetic field strength, layer number, and temperature gives rise to a diverse array of phenomena, holding promise not only for new physics but also for practical applications.

cond-mat.str-el↗

arXiv2022

Precise measurement of angles between two magnetic moments and their configurational stability in single-molecule magnets

A key parameter for the low-temperature magnetic coupling of in dinuclear lanthanide single-molecule magnets (SMMs) is the barrier $U_{FA}$ resulting from the exchange and dipole interactions between the two $4f$ moments. Here we extend the pseudospin model previously used to describe the ground state of dinuclear endofullerenes to account for variations in the orientation of the single-ion anisotropy axes and apply it to the two SMMs Dy$_2$ScN@C$_{80}$ and Dy$_2$TiC@C$_{80}$. While x-ray magnetic circular dichroism (XMCD) indicates the same $J_z=15/2$ Dy groundstate in both molecules, the Dy-Dy coupling strength and the stability of magnetization is distinct. We demonstrate that both the magnitude of the barrier $U_{FA}$ and the angle between the two $4f$ moments are determined directly from precise temperature-dependent magnetization data to an accuracy better than $1^{\circ}$. The experimentally found angles between the $4f$ moments are in excellent agreement with calculated angles between the quantisation axes of the two Dy ions. Theory indicates a larger deviation of the orientation of the Dy magnetic moments from the Dy bond axes to the central ion in Dy$_2$TiC@C$_{80}$. This may explain the lower stability of the magnetisation in Dy$_2$TiC@C$_{80}$, although it exhibits a $\sim 49\%$ stronger exchange coupling than in Dy$_2$ScN@C$_{80}$.

cond-mat.mtrl-sci↗

arXiv2020

Gadolinium as a single atom catalyst in a single molecule magnet

Endohedral fullerenes are perfect nanolaboratories for the study of magnetism. The substitution of a diamagnetic scandium atom in Dy2ScN@C80 with gadolinium decreases the stability of a given magnetization and demonstrates Gd to act as a single atom catalyst that accelerates the reaching of thermal equilibrium. X-ray magnetic circular dichroism at the M4,5 edges of Gd and Dy shows that the Gd magnetic moment follows the sum of the external and the dipolar magnetic field of the two Dy ions and compared to Dy2ScN@C80 a lower exchange barrier is found between the ferromagnetic and the antiferromagnetic Dy configuration. The Arrhenius equilibration barrier as obtained from superconducting quantum interference device magnetometry is more than one order of magnitude larger, though a much smaller prefactor imposes faster equilibration in Dy2GdN@C80. This sheds light on the importance of the angular momentum balance in magnetic relaxation.

cond-mat.mtrl-sci↗

arXiv2019

Large effect of the metal substrate on the magnetic anisotropy of Co on hexagonal Boron Nitride

We combine x-ray absorption spectroscopy (XAS), x-ray magnetic circular dichroism (XMCD) and x-ray magnetic linear dichroism (XMLD) data with first principles density functional theory (DFT) calculations and a multiorbital many body Hamiltonian approach to understand the electronic and magnetic properties of Co atoms adsorbed on h-BN/Ru(0001) and h-BN/Ir(111). The XAS line shape reveals, for both substrates, an electronic configuration close to $3d^8$, corresponding to a spin $S = 1$. Magnetic field dependent XMCD data show large (14 meV) out-of-plane anisotropy on h-BN/Ru(0001), while it is almost isotropic (tens of $\mu$eV) on h-BN/Ir(111). XMLD data together with both DFT calculations and the results of the multiorbital Hubbard model suggest that the dissimilar magnetic anisotropy originates from different Co adsorption sites, namely atop N on h-BN/Ru(0001) and 6-fold hollow on h-BN/Ir(111).

cond-mat.mes-hall↗

arXiv2018

Engineering on-surface spin crossover: spin-state switching in a self-assembled film of vacuum sublimable functional molecule

Realization of spin crossover (SCO) based applications requires studying of spin state switching characteristics of SCO complex molecules at nanostructured environments especially on-surface. Except for a very few cases, the SCO of a surface bound thin molecular film is either quenched or heavily altered due to (i) strong molecule-surface interactions and (ii) differing intermolecular interactions in films relative to the bulk. By fabricating SCO complexes on a weakly interacting surface such as highly oriented pyrolytic graphite (HOPG) and copper nitride (CuN), the interfacial quenching problem has been tackled. However, engineering intermolecular interactions in thin SCO active films is rather difficult. This work proposes a molecular self-assembly strategy to fabricate thin spin switchable surface bound films with programmable intermolecular interactions. Molecular engineering of the parent complex system [Fe(H$_{2}$B(pz)$_{2}$)$_{2}$(bpy)] (pz = pyrazole, bpy = 2,2'-bipyridine) with a dodecyl (C$_{12}$) alkyl chain yielded a classical amphiphile-like functional and vacuum sublimable charge neutral Fe$^{\rm II}$ complex, [Fe(H$_{2}$B(pz)$_{2}$)$_{2}$(C$_{12}$-bpy)] (C$_{12}$-bpy = dodecyl[2,2'-bipyridine]-5-carboxylate). The bulk powder and 10 nm thin film, on quartz glass/SiO$_{\rm x}$ surface, of the complex showed comparable spin state switching characteristics mediated by similar lamellar bilayer like self-assembly/molecular interactions in both bulk and thin film states. This unprecedented observation augurs well for the development of SCO based applications, especially in molecular spintronics.

physics.app-ph↗

arXiv2017

Nanoscale X-ray investigation of magnetic metallofullerene peapods

Endohedral lanthanide ions packed inside carbon nanotubes (CNTs) in a one-dimensional assembly have been studied with a combination of high resolution transmission electron microscopy (HRTEM), scanning transmission X-ray microscopy (STXM), and X-ray magnetic circular dichroism (XMCD). By correlating HRTEM and STXM images we show that structures down to 30 nm are resolved with chemical contrast and record X-ray absorption spectra from endohedral lanthanide ions embedded in individual nanoscale CNT bundles. XMCD measurements of an Er$_3$N@C$_{80}$ bulk sample and a macroscopic assembly of filled CNTs indicates that the magnetic properties of the endohedral Er3+ ions are unchanged when encapsulated in CNTs. This study demonstrates the feasibility of local magnetic X-ray characterization of low concentrations of lanthanide ions embedded in molecular nanostructures.

cond-mat.mtrl-sci↗

arXiv2015

Surface aligned magnetic moments and hysteresis of an endohedral single-molecule magnet on a metal

The interaction between the endohedral unit in the single-molecule magnet Dy$_2$ScN@C$_{80}$ and a rhodium (111) substrate leads to alignment of the Dy 4$f$ orbitals. The resulting orientation of the Dy$_2$ScN plane parallel to the surface is inferred from comparison of the angular anisotropy of x-ray absorption spectra and multiplet calculations in the corresponding ligand field. The x-ray magnetic circular dichroism (XMCD) is also angle dependent and signals strong magnetocrystalline anisotropy. This directly relates geometric and magnetic structure. Element specific magnetization curves from different coverages exhibit hysteresis at a sample temperature of $\sim4$ K. From the measured hysteresis curves we estimate the zero field remanence life-time during x-ray exposure of a sub-monolayer to be about 30 seconds.

cond-mat.mtrl-sci↗

arXiv2013

Tunneling, Remanence, and Frustration in Dysprosium based Endohedral Single Molecule Magnets

A single molecule magnet (SMM) can maintain its magnetization direction over a long period of time [1,2]. It consists in a low number of atoms that facilitates the understanding and control of the ground state, which is essential in future applications such as high-density information storage or quantum computers [3,4]. Endohedral fullerenes realize robust, nanometer sized, and chemically protected magnetic clusters that are not found as free species in nature. Here we demonstrate how adding one, two, or three dysprosium atoms to the carbon cage results in three distinct magnetic ground states. The significantly different hysteresis curves demonstrate the decisive influence of the number of magnetic moments and their interactions. At zero field the comparison relates tunneling of the magnetization, with remanence, and frustration. The ground state of the tridysprosium species turns out to be one of the simplest realizations of a frustrated, ferromagnetically coupled magnetic system.

cond-mat.mtrl-sci↗

arXiv2010

High-Frequency Electron-Spin-Resonance Study of the Octanuclear Ferric Wheel CsFe$_8$

High-frequency ($f$ = 190 GHz) electron paramagnetic resonance (EPR) at magnetic fields up to 12 T as well as Q-band ($f$ = 34.1 GHz) EPR were performed on single crystals of the molecular wheel CsFe$_8$. In this molecule, eight Fe(III) ions, which are coupled by nearest-neighbor antiferromagnetic (AF) Heisenberg exchange interactions, form a nearly perfect ring. The angle-dependent EPR data allow for the accurate determination of the spin Hamiltonian parameters of the lowest spin multiplets with $S \leq$ 4. Furthermore, the data can well be reproduced by a dimer model with a uniaxial anisotropy term, with only two free parameters $J$ and $D$. A fit to the dimer model yields $J$ = -15(2) cm$^{-1}$ and $D$ = -0.3940(8) cm$^{-1}$. A rhombic anisotropy term is found to be negligibly small, $E$ = 0.000(2) cm$^{-1}$. The results are in excellent agreement with previous inelastic neutron scattering (INS) and high-field torque measurements. They confirm that the CsFe$_8$ molecule is an excellent experimental model of an AF Heisenberg ring. These findings are also important within the scope of further investigations on this molecule such as the exploration of recently observed magnetoelastic instabilities.

cond-mat.mes-hall↗

arXiv2007

Optical investigations of quantum-dot spin dynamics

We have performed all-optical measurements of spin relaxation in single self-assembled InAs/GaAs quantum dots (QD) as a function of static external electric and magnetic fields. To study QD spin dynamics we measure the degree of resonant absorption which results from a competition between optical spin pumping induced by the resonant laser field and spin relaxation induced by reservoirs. Fundamental interactions that determine spin dynamics in QDs are hyperfine coupling to QD nuclear spin ensembles, spin-phonon coupling and exchange-type interactions with a nearby Fermi sea of electrons. We show that the strength of spin relaxation generated by the three fundamental interactions can be changed by up to five orders of magnitude upon varying the applied electric and magnetic fields. We find that the strength of optical spin pumping that we use to study the spin relaxation is determined predominantly by hyperfine-induced mixing of single-electron spin states at low magnetic fields and heavy-light hole mixing at high magnetic fields. Our measurements allow us to determine the rms value of the hyperfine (Overhauser) field to be ~15 mTesla with an electron g-factor of g_e=0.6 and a hole mixing strength of |epsilon|^2 = 0.0005.

cond-mat.mes-hall↗

arXiv2006

Observation of Faraday rotation from a single confined spin

Ability to read-out the state of a single confined spin lies at the heart of solid-state quantum information processing. While all-optical spin measurements using Faraday rotation has been successfully implemented in ensembles of semiconductor spins, read-out of a single semiconductor spin has only been achieved using transport measurements based on spin-charge conversion. Here, we demonstrate an all-optical dispersive measurement of the spin-state of a single electron trapped in a semiconductor quantum dot. We obtain information on the spin state through conditional Faraday rotation of a spectrally detuned optical field, induced by the polarization- and spin-selective trion (charged quantum dot) transitions. To assess the sensitivity of the technique, we use an independent resonant laser for spin-state preparation. An all-optical dispersive measurement on single spins has the important advantage of channeling the measurement back-action onto a conjugate observable, thereby allowing for repetitive or continuous quantum nondemolition (QND) read-out of the spin-state. We infer from our results that there are of order unity back-action induced spin-flip Raman scattering events within our measurement timescale. Therefore, straightforward improvements such as the use of a solid-immersion lens and higher efficiency detectors would allow for back-action evading spin measurements, without the need for a cavity.

quant-ph↗