Quantum information processing based on magnetic ions are considered potential candidates for applications because they can be modified and scaled up by a variety of chemical methods. For these systems to achieve individual spin addressability and high energy efficiency, we exploited the electric field as a tool to manipulate their quantum behaviours, functioning via spin-orbit coupling. A Ce:YAG single crystal was employed due to that rare-earth ions have strong spin-orbit coupling and with considerations regarding the dynamics and the symmetry requirements. The Stark effect of the Ce3+ ion was observed and measured. When demonstrated as a quantum phase gate, the electric field manipulation exhibited high efficiency which allowed up to 57 π/2 operations before decoherence with optimized field directions. It was also utilized to carry out quantum bang-bang control, as a method of dynamic decoupling, and the refined Deutsch-Jozsa algorithm. Our experiments highlighted rare-earth ions as potentially applicable qubits since they offer enhanced spin-electric coupling which enables high-efficiency quantum manipulation.
Fluoride crystals doped with rare-earth ions (REI) and pair centers in diamond for fast ($10^{-9}\rm{s}$) quantum computers (FQC) are proposed. As specific systems for REI doping, we propose $Ca_{1-x}Sr_{x}F_{2}$ crystals and their analogues. The $^{4}f$-states with different total orbital angular moments of these ions serve as two-level systems (qubits). Suitable REIs are proposed as well. It is established that the pair $SiV$ and $GeV$ centers in diamond are promising systems for fast optical quantum computers operating at elevated temperatures.
We report a study of magnetic dynamics in multiferroic hexagonal manganite HoMnO3 by far-infrared spectroscopy. Low-temperature magnetic excitation spectrum of HoMnO3 consists of magnetic-dipole transitions of Ho ions within the crystal-field split J=8 manifold and of the triangular antiferromagnetic resonance of Mn ions. We determine the effective spin Hamiltonian for the Ho ion ground state. The magnetic-field splitting of the Mn antiferromagnetic resonance allows us to measure the magnetic exchange coupling between the rare-earth and Mn ions.
Absorption, excitation and emission spectra of cadmium fluoride crystals doped with rare-earth ions were investigated. In contrast to alkaline-earth fluorides the absorption spectra due to 4f - 5d transitions of Ce$^{3+}$, Pr$^{3+}$ and Tb$^{3+}$ ions are broadened. No 5d-4f emissions were observed. These prove that 5d(e$_g$) levels of rare earth ions lie in conduction band of CdF$_2$ crystal. Emission spectra of Tb$^{3+}$ show the group of 4f-4f $^5$D$_4$-$^7$F$_j$ lines in contrast to other alkaline-earth fluorides where emission due to $^5$D$_3$-$^7$F$_j$ transitions is also observed. The a…
We present a quantum repeater scheme that is based on individual erbium and europium ions. Erbium ions are attractive because they emit photons at telecommunication wavelength, while europium ions offer exceptional spin coherence for long-term storage. Entanglement between distant erbium ions is created by photon detection. The photon emission rate of each erbium ion is enhanced by a microcavity with high Purcell factor, as has recently been demonstrated. Entanglement is then transferred to nearby europium ions for storage. Gate operations between nearby ions are performed using dynamically co…
The possibility of using mixed crystals highly doped with rare earth ions (REIs) as physical systems for creating fast quantum computers with a sampling time of nanoseconds is discussed. The electronic 4f states of rare earth ions with small values of the diagonal elements of the Judd-Ofelt matrix U(2) are proposed as optical frequency qubit levels. CNOT and other conditional gate operations are performed by exciting the rare earth ion into the 4f state with a large diagonal element of U(2), causing a Stark blockade. It is found that the main interaction responsible for this blockade is the qu…
We have demonstrated electron-electron and electron-nuclear spin manipulations of Gd3+ ion in CaWO4 crystal. The results suggest that the studied system is perspective for multiqubit implementation in quantum computing.
We have studied the absorption spectra of x-ray irradiation-induced Ce2+ and Pr2+ ions in crystals of alkaline-earth fluorides. We have calculated absorption spectra of divalent praseodymium ions in SrF2 crystals doped with Pr2+ for the first time. The calculated spectra agree rather well with the experimental data. In crystals containing induced Ce2+ ions we have found strong electron-phonon coupling. In BaF2, we do not observe bands corresponded to divalent Ce or Pr ions.
It was shown that the divalent rare earth ions (La, Ce, Gd, Tb, Lu, and Y) in cubic sites in alkaline earth fluorides are unstable with respect to electron autodetachment since its d1(eg) ground state is located in the conduction band which is consistent with the general tendency of these ions in various compounds. The localization of doubly degenerate d1(eg) level in the conduction band creates a configuration instability around the divalent rare earth ion that leading to the formation of anion vacancy in the nearest neighborhood, as was reported in the previous paper [Journal of Physics and …
The effect of rare-earth ions (R = Er^{3+}, Tb^{3+}) with strong spin-orbit coupling on the dielectric properties and the electric polarization induced by local polar phase separation domains in RMn_2O_5 multiferroics has been studied. These parameters were found to be qualitatively distinguished from those studied before in GdMn_2O_5, in which Gd^{3+} ion in the ground ^8S_{7/2} state is weakly bounded with the lattice. It is shown that the properties of the polar phase separation domains, which form in the subsystem of Mn^{3+} and Mn^{4+} ions, are substantially dependent on the values of cr…
Results of absolute light output measurements on strontium and barium fluoride doped with PrF$_3$ and CeF$_3$ are presented and compared with scintillators having well-known light output (NaI-Tl, CsI-Tl, BGO). For pure SrF$_2$ crystal we obtain a value of about 28600 photons/MeV.
The present work reports results of the electron paramagnetic resonance (EPR), optical absorption, radio- and photoluminescence (RL and PL) complex study of the Lu2Si2O7:Pr and Lu2Si2O7:Ce pyrosilicate crystals. In both crystals, the EPR spectra demonstrate the presence of characteristic signals originating from the Yb3+, Er3+, Nd3+, Dy3+, Gd3+ and V3+ ions existing in the material as uncontrolled impurities. The corresponding spectra (except for Gd3+) have been analysed in detail and g- and hyperfine tensors are determined for all these ions in the lutetium pyrosilicate for the first time. Op…
We investigate the prospect of achieving negative permittivity and permeability at optical frequencies in a dielectric crystal containing stoichiometric rare-earth ions. We derive the necessary transition linewidth, ion density and electric and magnetic oscillator strengths using a simplified model of non-interacting dipoles. We identify Erbium crystals in a magnetically ordered phase as the most promising material to meet these conditions, and describe initial optical measurements of two potential candidates, \ercl{} and ${}^7$\lierf{}, which display linewidths of 3~GHz and 250~MHz, respectiv…
Zeeman spectroscopy is used to demonstrate that phenomenological crystal-field parameters determined for the two $C_1$ point-group sites in Er$^{3+}$:Y$_2$SiO$_5$ may be transferred to other ions. The two crystallographic six- and seven-coordinate substitutional sites may be distinguished by comparing the spectra with crystal-field calculations.
The $4f-5d$ transition rates for rare-earth ions in crystals can be calculated with an effective transition operator acting between model $4f^N$ and $4f^{N-1}5d$ states calculated with effective Hamiltonian, such as semi-empirical crystal Hamiltonian. The difference of the effective transition operator from the original transition operator is the corrections due to mixing in transition initial and final states of excited configurations from both the center ion and the ligand ions. These corrections are calculated using many-body perturbation theory. For free ions, there are important one-body …
Thermally induced spin control is one of the main directions for future spin devices. In this study, we synthesized single-phase polycrystalline ErFe1-xCrxO3 and combined the magnetization curves and Mössbauer spectra to determine the macroscopic magnetism at room temperature. The magnetization of the system at various temperatures is well simulated by molecular field theory. And it is found that under the DM interaction, not only the B-site ions undergo a reorientation process, but the spins of the A-site ions also change at the same time. The effective spin is defined as the projection of Er…
We describe an experimental technique for associating the satellite lines in a rare earth optical spectrum caused by a defect with the rare earth ions in crystal sites around that defect. This method involves measuring the hyperfine splitting caused by a magnetic dipole-dipole interaction between host ions and a magnetic defect. The method was applied to Ce3+:EuCl3.6H2O to assign 13 of the outermost 22 satellite lines to sites. The assignments show that the optical shift of a satellite line is loosely dependent on the distance to the dopant. The interaction between host and dopant ions is pure…
We present a comparative study of the gain achievement in a waveguide whose active layer is constituted by a silica matrix containing silicon nanograins acting as sensitizer of either neodymium ions (Nd3+) or erbium ions (Er3+). By means of an auxiliary differential equation and finite difference time domain (ADE-FDTD) approach that we developed, we investigate the steady states regime of both rare earths ions and silicon nanograins levels populations as well as the electromagnetic field for different pumping powers ranging from 1 to 104 mW/mm2. Moreover, the achievable gain has been estimated…
Atomic and atom-like defects in the solid-state are widely explored for quantum computers, networks and sensors. Rare earth ions are an attractive class of atomic defects that feature narrow spin and optical transitions that are isolated from the host crystal, allowing incorporation into a wide range of materials. However, the realization of long electronic spin coherence times is hampered by magnetic noise from abundant nuclear spins in the most widely studied host crystals. Here, we demonstrate that Er$^{3+}$ ions can be introduced via ion implantation into TiO$_2$, a host crystal that has n…
An influence of high magnetic fields on hyperfine interaction in the rare-earth ions with non-magnetic ground state (Van Vleck ions) is theoretically investigated for the case of $Tm^{3+}$ ion in axial symmetrical crystal electric field (ethylsulphate crystal). It is shown that magnetic-field induced distortions of $4f$-electron shell lead to essential changes in hyperfine magnetic field at the nucleus. The proposed theoretical model is in agreement with recent experimental data.
Structural and Optical Characteristics of $β-Ga_2O_3$ Implanted with Rare Earth Ions
National Centre for Nuclear Research（国家核研究中心）；Helmholtz-Zentrum Dresden-Rossendorf（德累斯顿-罗斯多夫亥姆霍兹中心）；Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所）；Universite Paris-Saclay（巴黎萨克雷大学）
Exchange bias effect is an important attribute in several device applications. Traditionally, it is discussed as a form of exchange anisotropy at the interface between the ferromagnetic/antiferromagnetic layers of two distinct systems. We report here on the magnetically ordered alloys possessing the feature of unidirectional anisotropy, which reverses its sign across a characteristic temperature. These are admixed rare earth intermetallics, comprising two dissimilar rare earth (RE) ions, belonging to the two different halves of the 4f-series and imbibing the notion of ferromagnetic coupling be…
The electronic structure and magnetic coupling properties of rare-earth metals (Gd, Nd) doped ZnO have been investigated using first-principles methods. We show that the magnetic coupling between Gd or Nd ions in the nearest neighbor sites is ferromagnetic. The stability of the ferromagnetic coupling between Gd ions can be enhanced by appropriate electron doping into ZnO:Gd system and the room-temperature ferromagnetism can be achieved. However, for ZnO:Nd system, the ferromagnetism between Nd ions can be enhanced by appropriate holes doping into the sample. The room-temperature ferromagnetism…
Exploration of rare-earth (RE)-based Kagome lattice magnets with spin-orbital entangled jeff=1/2 moments will provide new platform for investigating the exotic magnetic phases. Here, we report a new family of RE3BWO9 (RE=Pr,Nd,Gd-Ho) boratotungstates with magnetic RE3+ ions arranged on Kagome lattice, and perform its structure and magnetic characterizations. This serial compounds crystallize in hexagonal coordinated structure with space group P63 (No.173), where magnetic RE3+ ions have distorted Kagomé lattice connections within the ab plane and stacked in a AB-type fashion along c axis. The i…
A comparative study of the gain achievement is performed in a waveguide optical amplifier whose active layer is constituted by a silica matrix containing silicon nanograins acting as sensitizer of either neodymium ions (Nd 3+) or erbium ions (Er 3+). Due to the large difference between population levels characteristic times (ms) and finite-difference time step (10 --17 s), the conventional auxiliary differential equation and finite-difference time-domain (ADE-FDTD) method is not appropriate to treat such systems. Consequently, a new two loops algorithm based on ADE-FDTD method is presented in …
Rare-earth (RE) based frustrated magnets as typical systems of combining strong spin-orbit coupling, geometric frustration and anisotropic exchange interactions, can give rise to diverse exotic magnetic ground states such as quantum spin liquid (QSL). The discovery of new RE-based frustrated materials is crucial for exploring the exotic magnetic phases. Herein, we report the synthesis, structure and magnetic properties of a family of melilite-type RE2Be2GeO7 (RE = Pr, Nd, Gd-Yb) compounds crystallized in a tetragonal structure, where magnetic RE3+ ions lay out on Shastry-Sutherland lattice (SS…
The rare-earth (RE) elements [Holmium (Ho) and Ytterbium (Yb)] doped vanadium pentoxide (V2O5) with a series of doping concentrations (1 mol.%, 3 mol.%, and 5 mol.%) have been successfully synthesized using environment-friendly facile hydrothermal method. The effect of RE ions on the photocatalytic efficiency of doped V2O5 has also been analyzed. The stable orthorhombic crystal structure of doped V2O5 confirms by the X-ray diffraction with no secondary phase, and high-stressed conditions are generated for the 3 mol.%. The crystallite size, strain, and dislocation density are calculated to perc…
The magnetic interaction between rare-earth and Fe ions in hexagonal rare-earth ferrites (h-REFeO3), may amplify the weak ferromagnetic moment on Fe, making these materials more appealing as multiferroics. To elucidate the interaction strength between the rare-earth and Fe ions as well as the magnetic moment of the rare-earth ions, element specific magnetic characterization is needed. Using X-ray magnetic circular dichroism, we have studied the ferrimagnetism in h-YbFeO3 by measuring the magnetization of Fe and Yb separately. The results directly show anti-alignment of magnetization of Yb and …
Optically addressable spins are actively investigated in quantum communication, processing and sensing. Optical and spin coherence lifetimes, which determine quantum operation fidelity and storage time, are often limited by spin-spin interactions, which can be decreased by polarizing spins in their lower energy state using large magnetic fields and/or mK range temperatures. Here, we show that optical pumping of a small fraction of ions with a fixed frequency laser, coupled with spin-spin interactions and spin diffusion, leads to substantial spin polarization in a paramagnetic rare earth doped …
A combination of density functional and dynamical mean field theory calculations are used to show that the remarkable metal-insulator transition in the rare earth nickelate perovskites arise from a site-selective Mott phase, in which the $d$-electrons on a half of the Ni ions are localized to form a fluctuating moment while the $d$-electrons on other Ni ions form a singlet with holes on the surrounding oxygen ions. The calculation reproduces key features observed in the nickelate materials, including an insulating gap in the paramagnetic state, a strong variation of static magnetic moments amo…
We theoretically and numerically investigate metal enhanced fluorescence of plasmonic core-shell nanoparticles doped with rare earth (RE) ions. Particle shape and size are engineered to maximize the average enhancement factor (AEF) of the overall doped shell. We show that the highest enhancement (11 in the visible and 7 in the near-infrared) are achieved by tuning either the dipolar or quadrupolar particle resonance to the rare earth ions excitation wavelength. Additionally, the calculated AEFs are compared to experimental data reported in the literature, obtained in similar conditions (plasmo…
We used Raman scattering to study the lattice and magnetic excitations in the hexagonal HoMnO3 single crystals. The E2 phonon mode at 237 cm-1 is affected by the magnetic order. This mode is related to the displacement of Mn and O ions in a-b plane and modulates the Mn-O-Mn bond angles in a-b plane and the in-plane Mn-Mn superexchange interaction. The mode at 269 cm-1 associated to the displacement of the apical Ho3+ ions along the c direction presents an abrupt change of slope at TN showing that the role of the rare earth ions can not be neglected in the magnetic transition. We have identifie…
We present a theoretical study on the relation between the size of the rare earth ions, often known as chemical pressure, and the stability of the coherent Jahn-Teller distortions in undoped perovskite manganites. Using a Keating model expressed in terms of atomic scale symmetry modes, we show that there exists a coupling between the uniform shear distortion and the staggered buckling distortion within the Jahn-Teller energy term. It is found that this coupling provides a mechanism by which the coherent Jahn-Teller distortion is more stabilized by smaller rare earth ions. We analyze the appear…
Electro-optical control of on-chip photonic devices is an essential tool for efficient integrated photonics. Lithium niobate on insulator (LNOI) is an emerging platform for on-chip photonics due to its large electro-optic coefficient and high nonlinearity [1]. Integrating quantum emitters into LNOI would extend their versatile use in classic photonics to quantum computing and communication [2, 3]. Here, we incorporate single rare-earth ions (REI) quantum emitters in electro-optical tunable lithium niobite (LN) thin films and demonstrate control of LN microcavities coupled to REI over a frequen…
The damping due to rare earth impurities in transition metals is discussed in the low concentration limit. It is shown that the increase in damping is mainly due to the coupling of the orbital moments of the rare earth impurities and the conduction $p$-electrons. It is shown that an itinerant picture for the host transition ions is needed to reproduce the observed dependence of the damping on the total angular moment of the rare earths.
We report a systematic study on the crystal growth of the rare-earth titanates $R_2$Ti$_2$O$_7$ ($R$ = Gd, Tb, Dy, Ho, Y, Er, Yb and Lu) and Y-doped Tb$_{2-x}$Y$_x$Ti$_2$O$_7$ ($x$ = 0.2 and 1) using an optical floating-zone method. High-quality single crystals were successfully obtained and the growth conditions were carefully optimized. The oxygen pressure was found to be the most important parameter and the appropriate ones are 0.1--0.4 MPa, depending on the radius of rare-earth ions. The growth rate is another parameter and was found to be 2.5--4 mm/h for different rare-earth ions. X-ray d…
Sub-oxides with the anti-perovskite structure constitute a large part of the interstitial stabilized compounds with novel chemical and physical properties, especially in the systems containing rare earth elements and/or early transition metal elements. A new sub-oxide compound, (Ce$_{0.85}$Ti$_{0.15}$)Ge$_3$O$_{0.5}$, is synthesized by flux growth. The compound crystallizes in a cubic structure which can be considered as an ordered vacancy variant of anti-perovskite-structure or an ordered interstitial variant of the Cu$_3$Au type, with a space group of Fm-3m (225). The structure is refined fr…
The role of rare-earth (R) ions on the magnetodielectric (MD) coupling is always intriguing and markedly different for different systems. Although many reports are available concerning this aspect in frustrated 3d-transition metal oxides, no such reports exist on higher d (4d/5d)-orbital based systems due to the rare availability of highly insulating 4d/5d-systems. Here, we systematically investigated the magnetic, dielectric, ferroelectric and magnetodielectric behavior of the 6H-perovskites Ba3RRu2O9 for different R-ions, namely, R= Sm, Tb and Ho, which magnetically order at 12, 9.5 and 10.2…
The delafossite family of compounds with a triangular lattice of rare earth ions has been recently proposed as a candidate host for quantum spin liquid (QSL) states. To realize QSLs, the crystal-electric-field (CEF) ground state of the rare earth ions should be composed of a doublet that allows sizable quantum tunneling, but till now the knowledge on CEF states in the delafossite compounds is still limited. Here we employ inelastic neutron scattering (INS) to study the CEF transitions in a powder sample of the delafossite NaErS$_2$, where the large total angular momentum $J = 15/2$ of the Er$^…
We provide accurate projected augmented wave (PAW) datasets for rare-earth (RE) elements with some suggested Hubbard U values allowing efficient plane-wave calculations. Solid state tests of generated datasets were performed on rare-earth nitrides. Through density of state (DOS) and equation of state (EoS) comparisons, generated datasets were shown to yield excellent results comparable to highly accurate all-electron full-potential linearized augmented plane-wave plus local orbital (FLAPW+LO) calculations. Hubbard U values for trivalent RE ions are determined according to hybrid functional cal…
Rare earth Manganite Nickelite double perovskites are prepared by solgel assisted combustion route, where, R varies from La, Pr, Nd, Sm, Gd, Tb, Dy, Y, and Ho. The samples have been systematically investigated using powder xray diffraction, Raman spectroscopy, ultraviolet visible spectroscopy, magnetization, and synchrotron based xray absorption spectroscopy measurements. All compounds in the family crystallize in the monoclinic structure and the monoclinic distortion enhances with decreasing trivalent rare earth radii. The magnetic ordering temperature, Tc, decreases from 270 K for La to 80 K…
On the basis of the point charge model, we formulate the crystalline electronic field (CEF) Hamiltonian $H_{\rm CEF}$ in the rare-earth based quasicrystal (QC) and approximant crystal (AC) with ligand ions located at pseudo 5-fold configurations by using the operator equivalent method. By setting the total angular momentum $J=7/2$, the CEF in the quantum critical QC Au$_{51}$Al$_{34}$Yb$_{15}$ and the 1/1 AC Au$_{51}$Al$_{35}$Yb$_{14}$ is analyzed with consideration for the effect of Al/Au mixed sites. We find that the ratio of the valences of ligand ions $x=Z_{\rm Al}/Z_{\rm Au}$ plays an imp…
The location of the energy levels of rare-earth (RE) elements in the energy band diagram of BaF2 and CdF2 crystals is determined. The role of RE3+ and RE2+ ions in the capture of charge carriers, luminescence, and the formation of radiation defects is evaluated. It is shown that the substantial difference in the luminescence properties of BaF2:RE and CdF2:RE is associated with the location of the excited energy levels in the band diagram of the crystals.
Inelastic neutron scattering was employed to study the crystal-field interaction in the strontium-doped rare-earth compounds R(x)Sr(1-x)CoO(3-z) (R=Pr, Nd, Ho, and Er). Particular emphasis is laid on the effect of oxygen deficiencies which naturally occur in the synthesis of these compounds. The observed energy spectra are found to be the result of a superposition of crystal fields with different nearest-neighbor oxygen coordination at the R sites. The experimental data are interpreted in terms of crystal-field parameters which behave in a consistent manner through the rare-earth series, there…
Absolute Primary Nanothermometry Using Individual Stark Sublevels of Rare-Earth-doped Crystals
Universidade Federal de Pernambuco（伯南布哥联邦大学）；Instituto Federal de Educação, Ciência e Tecnologia de Pernambuco（伯南布哥联邦教育、科学和技术学院）；Ludwig-Maximilians-Universität München（慕尼黑路德维希-马克西米利安大学）；Faculdade de Filosofia, Ciências e Letras de Ribeirão Preto, Universidade de São Paulo（圣保罗大学里贝朗普雷图哲学、文学与人类科学学院）
Frustrated quantum magnets are expected to host many exotic quantum spin states like quantum spin liquid (QSL), and have attracted numerous interest in modern condensed matter physics. The discovery of the triangular lattice spin liquid candidate YbMgGaO$_4$ stimulated an increasing attention on the rare-earth-based frustrated magnets with strong spin-orbit coupling. Here we report the synthesis and characterization of a large family of rare-earth chalcogenides AReCh$_2$ (A = alkali or monovalent ions, Re = rare earth, Ch = O, S, Se). The family compounds share the same structure (R$\bar{3}$m)…
We review recent studies of spin dynamics in rare-earth orthorhombic perovskite oxides of the type $RM$O$_3$, where $R$ is a rare-earth ion and $M$ is a transition-metal ion, using single-crystal inelastic neutron scattering (INS). After a short introduction to the magnetic INS technique in general, the results of INS experiments on both transition-metal and rare-earth subsystems for four selected compounds (YbFeO$_3$, TmFeO$_3$, YFeO$_3$, YbAlO$_3$) are presented. We show that the spectrum of magnetic excitations consists of two types of collective modes that are well separated in energy: gap…
A principal possibility of formation the nanostructures on the surfaces of 50PbO-25Bi$_2$O$_3$-20Ga$_2$O$_3$-5BaO (doped by Eu3+, Er3+, Dy3+) is demonstrated by using multi-coherent beams. As a sources of the photoinducing coherent light we have used nanosecond Nd:YAG and Er:Yb lasers generating at 1064 nm and 1540 nm, respectively. The morphology of the photoinduced surfaces is sensitive to the type of rare earth ions. The thickness of the layer was about 20-30 nm. Possible mechanisms are explained by coherent photoinduction of the valence electrons.
We consider the spin correlation functions for rare-earth compounds in their paramagnetic state with the aim to understand the temperature dependence of the quasi-elastic and crystal-field linewidths and the spin-lattice relaxation rates measured by the muon-spin-relaxation technique. Both the conduction electron and phonon relaxation mechanisms are treated. First the single-ion dynamics is described using an iterative method introduced by P. M. Richards. Then the case of a regular lattice of rare-earth ions is studied using the random-phase approximation (RPA). Applications to simple crystal-…
