Here we describe a new high frequency/high field continuous wave and pulsed electrically detected magnetic resonance (CW EDMR and pEDMR) setup, operating at 263 GHz and resonance fields between 0 and 12 T. Spin dependent transport in illuminated hydrogenated amorphous silicon p-i-n solar cells at 5 K and 90 K was studied by in operando 263 GHz CW and pEDMR alongside with complementary X-band CW EDMR. Benefiting from the superior resolution at 263 GHz, we were able to better resolve EDMR signals originating from spin dependent hopping and recombination processes. 5 K EDMR spectra were found to be dominated by conduction and valence band tale states involved in spin dependent hopping, with additional contributions from triplet exciton states. 90 K EDMR spectra could be assigned to spin pair recombination involving conduction band tail states and dangling bonds as dominating spin dependent transport process, with additional contributions from valence band tail and triplet exciton states.
Abstract The results of intense pulsed ion beam (IPIB) treatment of the soft magnetic amorphous alloy of a FINEMET-type are presented. Foil produced from the alloy was irradiated with short (about 100 ns) pulses of carbon ions and protons with energy of up to 300 keV and an energy density of up to 7 J/cm2. X-ray diffraction, Mössbauer spectroscopy and magnetic measurements were used to investigate structural and magnetic properties of irradiated foils. It is shown that the foil remains intact after the treatment, and the crystal structure still amorphous. Spontaneous magnetization vector is fo…
The investigation of paramagnetic species (such as point defects, dopants, and impurities) in solid-state electronic devices is significant because of their effect on device performance. Conventionally, these species are detected and imaged using the electron spin resonance (ESR) technique. In many instances, ESR is not sensitive enough to deal with miniature devices having small numbers of paramagnetic species and high spatial heterogeneity. This limitation can in principle be overcome by employing a more sensitive method called electrically-detected magnetic resonance, which is based on meas…
We show that in pulsed electrically detected magnetic resonance (pEDMR) signal modulation in combination with a lock-in detection scheme can reduce the low-frequency noise level by one order of magnitude and in addition removes the microwave-induced non-resonant background. This is exemplarily demonstrated for spin-echo measurements in phosphorus-doped Silicon. The modulation of the signal is achieved by cycling the phase of the projection pulse used in pEDMR for the read-out of the spin state.
We deposit intrinsic hydrogenated amorphous silicon (a-Si:H) thin films by reactive pulsed laser deposition, for various hydrogen pressures in the 0-20 Pa range, at a low deposition temperature of 120C, and investigate the hydrogen incorporation, structural, optical, and electrical properties of the films, as a function of the ambient hydrogen pressure. The film thickness decreases linearly as the hydrogen pressure increases. The hydrogen content of the films is determined by infrared spectroscopy and the optical bandgap from UV-Vis-NIR transmittance and reflectance measurements. Electric meas…
Pulsed Laser Deposition allows to obtain W and W-Ta alloy coatings with different nanostructures, monitored by X-ray diffraction. The correlation between such structures and the elastic properties is investigated for amorphous-like, ultra-nano- and nano-crystalline coatings obtained by tuning the gas pressure during deposition, annealing temperature and Ta concentration. The full elastic characterization is achieved by surface Brillouin spectroscopy, interpreted by isotropic and anisotropic film models. Amorphous like coatings are obtained with He pressures of tens of Pa. In comparison with bu…
We investigate the spin species relevant for the spin-dependent recombination used for the electrical readout of coherent spin manipulation in phosphorus-doped silicon. Via a multi-frequency pump-probe experiment in pulsed electrically detected magnetic resonance, we demonstrate that the dominant spin-dependent recombination transition occurs between phosphorus donors and Si/SiO2 interface states. Combining pulses at different microwave frequencies allows us to selectively address the two spin subsystems participating in the recombination process and to coherently manipulate and detect the rel…
In situ optical absorption spectroscopy was used to study the generation of E' centres in amorphous SiO_2 occurring by photo-induced breaking of Si-H groups under 4.7eV pulsed laser radiation. The dependence from laser intensity of the defect generation rate is consistent with a two-photon mechanism for Si-H rupture, while the growth and the saturation of the defects are conditioned by their concurrent annealing due to reaction with mobile hydrogen arising from the same precursor. A rate equation is proposed to model the kinetics of the defects and tested on experimental data.
We demonstrate the electrical detection of pulsed X-band Electron Nuclear Double Resonance (ENDOR) in phosphorus-doped silicon at 5\,K. A pulse sequence analogous to Davies ENDOR in conventional electron spin resonance is used to measure the nuclear spin transition frequencies of the $^{31}$P nuclear spins, where the $^{31}$P electron spins are detected electrically via spin-dependent transitions through Si/SiO$_2$ interface states, thus not relying on a polarization of the electron spin system. In addition, the electrical detection of coherent nuclear spin oscillations is shown, demonstrating…
We present pulsed electrically detected magnetic resonance (EDMR) measurements at low magnetic fields using posphorus-doped silicon with natural isotope composition as a model system. Our measurements show that pulsed EDMR experiments, well established at X-band frequencies (10 GHz), such as coherent spin rotations, Hahn echoes, and measurements of parallel and antiparallel spin pair life times are also feasible at frequencies in the MHz regime. We find that the Rabi frequency of the coupled 31P electron-nuclear spin system scales with the magnetic field as predicted by the spin Hamiltonian, w…
Several microscopic pathways have been proposed to explain the large magnetic effects observed in organic semiconductors, but identifying and characterising which microscopic process actually influences the overall magnetic field response is challenging. Pulsed electrically-detected magnetic resonance provides an ideal platform for this task as it intrinsically monitors the charge carriers of interest and provides dynamical information which is inaccessible through conventional magnetoconductance measurements. Here we develop a general time domain theory to describe the spin-dependent reaction…
The magnetization dynamics for ferrimagnets at the angular momentum compensation temperature T_A is believed to be analogous to that for antiferromagnets. We investigated the pulsed-laser-induced magnetization dynamics in amorphous rare-earth transition-metal ferrimagnet films with a T_A just above room temperature. For a low pulse fluence, the magnetization precession frequency decreases as the applied magnetic field increases, whereas for a higher pulse fluence, it increases as the applied field increases. The result was well explained by the left-handed and right-handed precession modes of …
Monatomic antimony thin films have recently attracted attention for applications in phase change memory, nanophotonics, and 2D materials. Although some promising results have been reported, the true potential of Sb thin films is still hindered by the scalability issue and the lack of reliable bottom-up production. Here we demonstrate the growth of Sb thin films on a lattice-matching and amorphous substrates using pulsed laser deposition (PLD). C-axis out-of-plane textured Sb thin films were successfully deposited on Sb$_2$Te$_3$ and SiO$_2$\Si$_3$N$_4$ substrates. In the case of growth on Sb$_…
Additive solid immersion lenses for enhanced collection efficiency of shallow NV centers by pulsed laser deposition and structurization of high-k amorphous oxides
Leipzig University（莱比锡大学）；Felix Bloch Institute, Leipzig University（莱比锡大学费利克斯·布洛赫研究所）；SaxonQ GmbH（萨克森量子有限公司）；Department of Prosthetic Dentistry and Dental Material Science, Leipzig University（莱比锡大学假肢牙科与牙科材料科学系）
Spin-dependent relaxation and recombination processes in $γ$-irradiated $n$-type Czochralski-grown silicon are studied using continuous wave (cw) and pulsed electrically detected magnetic resonance (EDMR). Two processes involving the SL1 center, the neutral excited triplet state of the oxygen-vacancy complex, are observed which can be separated by their different dynamics. One of the processes is the relaxation of the excited SL1 state to the ground state of the oxygen-vacancy complex, the other a charge transfer between $^{31}$P donors and SL1 centers forming close pairs, as indicated by elec…
Thin films consisting of Ag and Au nanoparticles embedded in amorphous ZrO2 matrix were grown by pulsed laser deposition in a wide range of metal volume concentrations in the dielectric regime (0.08<x(Ag)<0.28 and 0.08<x(Au)<0.52). High resolution transmission electron microscopy (TEM) showed regular distribution of spherical Au and Ag nanoparticles having very sharp interfaces with the amorphous matrix. Mean particle size determined from X-ray diffraction agreed with direct TEM observation. The silver mean diameter increases more abruptly with metal volume content than that corresponding to g…
We present the design and implementation of a scanning probe microscope, which combines electrically detected magnetic resonance (EDMR) and (photo-)conductive atomic force microscopy ((p)cAFM). The integration of a 3-loop 2-gap X-band microwave resonator into an AFM allows the use of conductive AFM tips as a movable contact for EDMR experiments. The optical readout of the AFM cantilever is based on an infrared laser to avoid disturbances of current measurements by absorption of straylight of the detection laser. Using amorphous silicon thin film samples with varying defect densities, the capab…
The structural relaxation of amorphous materials is described as arising from the superposition of elementary processes with varying activation energies. We show that it is possible to obtain the kinetic parameters of these processes from differential scanning calorimetry experiments. The transformation rate is predicted for the transient decay when an isotherm is reached and for the relaxation threshold detected in partially relaxed samples. Good agreement is obtained with experiment if the individual components transform through first-order kinetics, but inconsistencies arise for second-orde…
We demonstrate that the bandwidth of pulsed electrically detected magnetic resonance can be increased to at least 80 MHz using a radio frequency-reflectometry detection scheme. Using this technique, we measure coherent spin oscillations in real time during a resonant microwave pulse. We find that the observed signal is in quantitative agreement with simulations based on rate equations modeling the recombination dynamics of the spin system under study. The increased bandwidth opens the way to electrically study faster spin-dependent recombination processes, e.g., in direct semiconductors which …
This study focuses on the synthesis of FeRh nanoparticles via pulsed laser ablation in liquid and on controlling the oxidation of the synthesized nanoparticles. Formation of monomodal γ-FeRh nanoparticles was confirmed by transmission electron microscopy (TEM) and their composition confirmed by atom probe tomography (APT). On these particles, three major contributors to oxidation were analysed: 1) dissolved oxygen in the organic solvents, 2) the bound oxygen in the solvent and 3) oxygen in the atmosphere above the solvent. The decrease of oxidation for optimized ablation conditions was confirm…
Micron-thick boron films have been deposited by Pulsed Laser Deposition in vacuum on several substrates at room temperature. The use of high energy pulses (>700 mJ) results in the deposition of smooth coatings with low oxygen uptake even at base pressures of 10$^{-4}$ - 10$^{-3}$ Pa. A detailed structural analysis, by X-Ray Diffraction and Raman, allowed to assess the amorphous nature of the deposited films as well as to determine the base pressure that prevents boron oxide formation. In addition the crystallization dynamics has been characterized showing that film crystallinity already improv…
Room-temperature (RT) Pulsed Cathodoluminescence (PCL) spectra of a set of pure synthetic (both crystalline and amorphous) silicon dioxide materials were studied. It is shown, that the PCL spectra of all samples (both amorphous and crystalline) possess a separate band at 495 nm (2.5 eV). This band is the most intensive one in PCL spectra of disordered materials. The RT PCL band at 495 nm (2.5 eV) of α-quartz single crystal is polarized in XY crystalline plane (perpendicular to the $3^{rd}$ order symmetry axis). The structure of this band was detected. It consists of three peaks: at 480$\pm$2 n…
The electron spins of semiconductor defects can have complex interactions with their host, particularly in polar materials like SiC where electrical and mechanical variables are intertwined. By combining pulsed spin resonance with ab-initio simulations, we show that spin-spin interactions within SiC neutral divacancies give rise to spin states with an enhanced Stark effect, sub-10**-6 strain sensitivity, and highly spin-dependent photoluminescence with intensity contrasts of 15-36%. These results establish SiC color centers as compelling systems for sensing nanoscale fields.
Herein we demonstrate the ability to optically tune the mobility of electrically powered Janus particles (JP) that are half coated with various Zinc Oxide (ZnO) semiconducting layers, i.e. polycrystalline, amorphous and amorphous with a SiO2 passivation layer. The ZnO semiconductor photo-response enables increase in its electrical conductivity with light having wavelengths of sufficient photon energy with respect to the semiconductor bandgap. This effect, termed optically modulated electrokinetic propulsion (OMEP), can be harnessed to increase the contrast in polarizability between the dielect…
We studied the optical absorption induced by 4.7eV pulsed laser radiation on Ge-doped a-SiO2 synthesized by a sol-gel technique. The absorption spectra in the ultraviolet spectral range were measured during and after the end of irradiation with an in situ technique, evidencing the growth of an absorption signal whose profile is characterized by two main peaks near 4.5eV and 5.7eV and whose shape depends on time. Electron spin resonance measurements performed ex situ a few hours after the end of exposure permit to complete the information acquired by optical absorption by detection of the param…
We have investigated recrystallization of amorphous Yttrium Iron Garnet (YIG) by annealing in oxygen atmosphere. Our findings show that well below the melting temperature the material transforms into a fully epitaxial layer with exceptional quality, both structural and magnetic.\\ In ferromagnetic resonance (FMR) ultra low damping and extremely narrow linewidth can be observed. For a 56 nm thick layer a damping constant of $α$=(6.63$\pm$1.50)$\cdot$10$^{-5}$ is found and the linewidth at 9.6 GHz is as small as 1.30$\pm$0.05 Oe which are the lowest values for PLD grown thin films reported so fa…
Electrically driven single-photon emitting devices have immediate applications in quantum cryptography, quantum computation and single-photon metrology. Mature device fabrication protocols and the recent observations of single defect systems with quantum functionalities make silicon carbide (SiC) an ideal material to build such devices. Here, we demonstrate the fabrication of bright single photon emitting diodes. The electrically driven emitters display fully polarized output, superior photon statistics (with a count rate of $>$300 kHz), and stability in both continuous and pulsed modes, all a…
We report on Boron diffusion and subsequent crystallization of Co$_{40}$Fe$_{40}$B$_{20}$ (CoFeB) thin films on SiO$_2$/Si(001) substrate using pulsed laser deposition. Secondary ion mass spectroscopy reveals Boron diffusion at the interface in both amorphous and crystalline phase of CoFeB. High-resolution transmission electron microscopy reveals a small fraction of nano-crystallites embedded in the amorphous matrix of CoFeB. However, annealing at 400$^\circ$C results in crystallization of CoFe with \textit{bcc} structure along (110) orientation. As-deposited films are non-metallic in nature w…
A study of donor electron spins and spin--dependent electronic transitions involving phosphorous ($^{31}$P) atoms in proximity of the (111) oriented crystalline silicon (c-Si) to silicon dioxide (SiO$_{2}$) interface is presented for [$^{31}$P] = 10$^{15}$ $\mathrm{cm}^{-3}$ and [$^{31}$P] = 10$^{16}$ $\mathrm{cm}^{-3}$ at about liquid $^4$He temperatures ($T = 5$ $\mathrm{K} - 15$ $\mathrm{K}$). Using pulsed electrically detected magnetic resonance (pEDMR), spin--dependent transitions between the \Phos donor state and two distinguishable interface states are observed, namely (i) \Pb centers w…
Thermally conductive polymers are of fundamental interest and can also be exploited in thermal management applications. Recent studies have shown stretched polymers can achieve high thermal conductivity. However, the transport mechanisms of heat in thermally conductive polymers have yet to be elucidated. Here we report a method for scalable fabrication of polyethylene films with a high thermal conductivity of 62 W/m-K. The achieved thermal conductivity is over two orders-of-magnitude greater than that of typical polymers (~0.1 W/m-K), and exceeds those of many metals and ceramics used as tradi…
Pulsed electrically-detected magnetic resonance of phosphorous (31P) in bulk crystalline silicon at very high magnetic fields (B > 8.5 T) and low temperatures (T = 2.8 K) is presented. We find that the spin-dependent capture and reemission of highly polarized (>95%) conduction electrons by equally highly polarized 31P donor electrons introduces less decoherence than other mechanisms for spin-to-charge conversion. This allows the electrical detection of spin coherence times in excess of 100 microseconds: 50 times longer than the previous maximum for electrically-detected spin readout experiment…
Study of amorphous alumina coatings for next-generation nuclear reactors: hightemperature in-situ and post-mortem Raman spectroscopy and X-ray diffraction
Explosive crystallization (EC) is often observed when using nanosecond-pulsed melt laser annealing (MLA) in amorphous silicon (Si) and germanium (Ge). The solidification velocity in EC is so fast that a diffusion-less crystallization can be expected. In the contacts of advanced transistors, the active level at the metal/semiconductor Schottky interface must be very high to achieve a sub-10^{-9} ohm.cm2 contact resistivity, which has been already demonstrated by using the dopant surface segregation induced by MLA. However, the beneficial layer of a few nanometers at the surface may be easily co…
We have performed continuous wave and pulsed electron spin resonance measurements of implanted bismuth donors in isotopically enriched silicon-28. Donors are electrically activated via thermal annealing with minimal diffusion. Damage from bismuth ion implantation is repaired during thermal annealing as evidenced by narrow spin resonance linewidths (B_pp=12uT and long spin coherence times T_2=0.7ms, at temperature T=8K). The results qualify ion implanted bismuth as a promising candidate for spin qubit integration in silicon.
We present experiments to systematically study the time constants of spin-dependent recombination processes in semiconductors using pulsed electrically detected magnetic resonance (EDMR). The combination of time-programmed optical excitation and pulsed spin manipulation allows us to directly measure the recombination time constants of electrons via localized spin pairs and the time constant of spin pair formation as a function of the optical excitation intensity. Using electron nuclear double resonance, we show that the time constant of spin pair formation is determined by an electron capture …
High-speed electrical switching of Ge2Sb2Te5 (GST) remains a challenging task due to the large impedance mismatch between the low-conductivity amorphous state and the high-conductivity crystalline state. In this letter, we demonstrate an effective doping scheme using nickel to reduce the resistivity contrast between the amorphous and crystalline states by nearly three orders of magnitude. Most importantly, our results show that doping produces the desired electrical performance without adversely affecting the film's optical properties. The nickel doping level is approximately 2% and the lattic…
We have studied the role of spin-dependent processes on conductivity in polyfluorene (PFO) thin films by conducting continuous wave (c.w.) electrically detected magnetic resonance (EDMR) spectroscopy at temperatures between 10 K and 293 K using microwave frequencies between about 100 MHz and 20 GHz as well as pulsed EDMR at X-band. Variable frequency EDMR allows us to establish the role of spin-orbit coupling in spin-dependent processes, pulsed EDMR probes coherent spin motion effects. We used PFO for this study in order to allow for the investigation of the effects of microscopic morphologica…
We have studied the nature and dynamics of spin-dependent charge carrier recombination in Tris(8-hydroxyquinolinato) aluminum (Alq$_3$) films in light emitting diodes at room temperature using continuous wave and pulsed electrically detected magnetic resonance (EDMR) spectroscopy. We found that the EDMR signal is dominated by an electron-hole recombination process, and another, weaker EDMR signal whose fundamental nature was investigated. From the pulsed EDMR measurements we obtained a carrier spin relaxation time, $T_2 = 45\pm 25$ ns which is much shorter than $T_2$ in conjugated polymers, bu…
We demonstrate the coherent control and electrical readout of the nuclear spins of ionized phosphorus donors in natural silicon. By combining pulsed illumination with coherent electron spin manipulation, we selectively ionize the donor depending on its nuclear spin state, exploiting a spin-dependent recombination process via a spin pair at the Si/SiO2 interface. The nuclear-spin coherence time of the ionized donor is 18 ms, two orders of magnitude longer than in the neutral donor state, rendering the ionized donor a potential resource as a quantum memory. The presented experimental techniques …
The manganese induced magnetic, electrical and structural modification in InMnP epilayers, prepared by Mn ion implantation and pulsed laser annealing, are investigated in the following work. All samples exhibit clear hysteresis loops and strong spin polarization at the Fermi level. The degree of magnetization, the Curie temperature and the spin polarization depend on the Mn concentration. The bright-field transmission electron micrographs show that InP samples become almost amorphous after Mn implantation but recrystallize after pulsed laser annealing. We did not observe an insulator-metal tra…
The effect of dipolar and exchange interactions within pairs of paramagnetic electronic states on Pauli-blockade-controlled spin-dependent transport and recombination rates during magnetic resonant spin excitation is studied numerically using the superoperator Liouville-space formalism. The simulations reveal that spin-Rabi nutation induced by magnetic resonance can control transition rates which can be observed experimentally by pulsed electrically (pEDMR) and pulsed optically (pODMR) detected magnetic resonance spectroscopies. When the dipolar coupling exceeds the difference of the pair part…
Magnetotransport is investigated in thin films of the half-metallic ferrimagnet Mn$_2$Ru$_x$Ga in pulsed magnetic fields of up to 58 T. A non-vanishing Hall signal is observed over a broad temperature range, spanning the compensation temperature 155 K, where the net magnetic moment is strictly zero, the anomalous Hall conductivity is 6673 $Ω^{-1}.m^{-1}$ and the coercivity exceeds 9 T. Molecular field modelling is used to determine the intra- and inter-sublattice exchange constants and from the spin-flop transition we infer the anisotropy of the electrically active sublattice to be 216 kJ/m$^3…
TmFeO$_3$ (TFO) is a canted antiferromagnet that undergoes a spin reorientation transition (SRT) with temperature between 82 K and 94 K in single crystals. In this temperature region, the Néel vector continuously rotates from the crystallographic $c$-axis (below 82 K) to the $a$-axis (above 94 K). The SRT allows for a temperature control of distinct antiferromagnetic states without the need for a magnetic field, making it apt for applications working at THz frequencies. For device applications, thin films of TFO are required as well as an electrical technique for reading out the magnetic state…
Modulation of donor electron wavefunction via electric fields is vital to quantum computing architectures based on donor spins in silicon. For practical and scalable applications, the donor-based qubits must retain sufficiently long coherence times in any realistic experimental conditions. Here, we present pulsed electron spin resonance studies on the longitudinal $(T_1)$ and transverse $(T_2)$ relaxation times of phosphorus donors in bulk silicon with various electric field strengths up to near avalanche breakdown in high magnetic fields of about 1.2 T and low temperatures of about 8 K. We fi…
