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Published work

34 published item(s)

preprint2026arXiv

PRTS: A Primitive Reasoning and Tasking System via Contrastive Representations

Vision-Language-Action (VLA) models advance robotic control via strong visual-linguistic priors. However, existing VLAs predominantly frame pretraining as supervised behavior cloning, overlooking the fundamental nature of robot learning as a goal-reaching process that requires understanding temporal task progress. We present \textbf{PRTS} (\textbf{P}rimitive \textbf{R}easoning and \textbf{T}asking \textbf{S}ystem), a VLA foundation model that reformulates pretraining through Goal-Conditioned Reinforcement Learning. By treating language instructions as goals and employing contrastive reinforcement learning, PRTS learns a unified embedding space where the inner product of state-action and goal embeddings approximates the log-discounted goal occupancy, the probability of reaching the language-specified goal from the current state-action, quantitatively assessing physical feasibility beyond static semantic matching. PRTS draws this dense goal-reachability supervision directly from offline trajectories without reward annotations, and folds it into the VLM backbone via a role-aware causal mask, incurring negligible overhead over vanilla behavior cloning. This paradigm endows the high-level reasoning system with intrinsic goal reachability awareness, bridging semantic reasoning and temporal task progress, and further benefits goal-conditioned action prediction. Pretrained on 167B tokens of diverse manipulation and embodied-reasoning data, PRTS reaches state-of-the-art performance on LIBERO, LIBERO-Pro, LIBERO-Plus, SimplerEnv, and a real-world suite of 14 complex tasks, with particularly substantial gains on long-horizon, contact-rich, and zero-shot novel-instruction settings, confirming that injecting goal-reachability awareness significantly improves both execution success and long-horizon planning of general-purpose robotic foundation policies.

preprint2022arXiv

Automatic Meta-Path Discovery for Effective Graph-Based Recommendation

Heterogeneous Information Networks (HINs) are labeled graphs that depict relationships among different types of entities (e.g., users, movies and directors). For HINs, meta-path-based recommenders (MPRs) utilize meta-paths (i.e., abstract paths consisting of node and link types) to predict user preference, and have attracted a lot of attention due to their explainability and performance. We observe that the performance of MPRs is highly sensitive to the meta-paths they use, but existing works manually select the meta-paths from many possible ones. Thus, to discover effective meta-paths automatically, we propose the Reinforcement learning-based Meta-path Selection (RMS) framework. Specifically, we define a vector encoding for meta-paths and design a policy network to extend meta-paths. The policy network is trained based on the results of downstream recommendation tasks and an early stopping approximation strategy is proposed to speed up training. RMS is a general model, and it can work with all existing MPRs. We also propose a new MPR called RMS-HRec, which uses an attention mechanism to aggregate information from the meta-paths. We conduct extensive experiments on real datasets. Compared with the manually selected meta-paths, the meta-paths identified by RMS consistently improve recommendation quality. Moreover, RMS-HRec outperforms state-of-the-art recommender systems by an average of 7% in hit ratio. The codes and datasets are available on https://github.com/Stevenn9981/RMS-HRec.

preprint2022arXiv

Domain-Adaptive Text Classification with Structured Knowledge from Unlabeled Data

Domain adaptive text classification is a challenging problem for the large-scale pretrained language models because they often require expensive additional labeled data to adapt to new domains. Existing works usually fails to leverage the implicit relationships among words across domains. In this paper, we propose a novel method, called Domain Adaptation with Structured Knowledge (DASK), to enhance domain adaptation by exploiting word-level semantic relationships. DASK first builds a knowledge graph to capture the relationship between pivot terms (domain-independent words) and non-pivot terms in the target domain. Then during training, DASK injects pivot-related knowledge graph information into source domain texts. For the downstream task, these knowledge-injected texts are fed into a BERT variant capable of processing knowledge-injected textual data. Thanks to the knowledge injection, our model learns domain-invariant features for non-pivots according to their relationships with pivots. DASK ensures the pivots to have domain-invariant behaviors by dynamically inferring via the polarity scores of candidate pivots during training with pseudo-labels. We validate DASK on a wide range of cross-domain sentiment classification tasks and observe up to 2.9% absolute performance improvement over baselines for 20 different domain pairs. Code will be made available at https://github.com/hikaru-nara/DASK.

preprint2022arXiv

PreTraM: Self-Supervised Pre-training via Connecting Trajectory and Map

Deep learning has recently achieved significant progress in trajectory forecasting. However, the scarcity of trajectory data inhibits the data-hungry deep-learning models from learning good representations. While mature representation learning methods exist in computer vision and natural language processing, these pre-training methods require large-scale data. It is hard to replicate these approaches in trajectory forecasting due to the lack of adequate trajectory data (e.g., 34K samples in the nuScenes dataset). To work around the scarcity of trajectory data, we resort to another data modality closely related to trajectories-HD-maps, which is abundantly provided in existing datasets. In this paper, we propose PreTraM, a self-supervised pre-training scheme via connecting trajectories and maps for trajectory forecasting. Specifically, PreTraM consists of two parts: 1) Trajectory-Map Contrastive Learning, where we project trajectories and maps to a shared embedding space with cross-modal contrastive learning, and 2) Map Contrastive Learning, where we enhance map representation with contrastive learning on large quantities of HD-maps. On top of popular baselines such as AgentFormer and Trajectron++, PreTraM boosts their performance by 5.5% and 6.9% relatively in FDE-10 on the challenging nuScenes dataset. We show that PreTraM improves data efficiency and scales well with model size.

preprint2022arXiv

Private Adaptive Optimization with Side Information

Adaptive optimization methods have become the default solvers for many machine learning tasks. Unfortunately, the benefits of adaptivity may degrade when training with differential privacy, as the noise added to ensure privacy reduces the effectiveness of the adaptive preconditioner. To this end, we propose AdaDPS, a general framework that uses non-sensitive side information to precondition the gradients, allowing the effective use of adaptive methods in private settings. We formally show AdaDPS reduces the amount of noise needed to achieve similar privacy guarantees, thereby improving optimization performance. Empirically, we leverage simple and readily available side information to explore the performance of AdaDPS in practice, comparing to strong baselines in both centralized and federated settings. Our results show that AdaDPS improves accuracy by 7.7% (absolute) on average -- yielding state-of-the-art privacy-utility trade-offs on large-scale text and image benchmarks.

preprint2021arXiv

CoDeNet: Efficient Deployment of Input-Adaptive Object Detection on Embedded FPGAs

Deploying deep learning models on embedded systems has been challenging due to limited computing resources. The majority of existing work focuses on accelerating image classification, while other fundamental vision problems, such as object detection, have not been adequately addressed. Compared with image classification, detection problems are more sensitive to the spatial variance of objects, and therefore, require specialized convolutions to aggregate spatial information. To address this need, recent work introduces dynamic deformable convolution to augment regular convolutions. However, this will lead to inefficient memory accesses of inputs with existing hardware. In this work, we harness the flexibility of FPGAs to develop a novel object detection pipeline with deformable convolutions. We show the speed-accuracy tradeoffs for a set of algorithm modifications including irregular-access versus limited-range and fixed-shape. We then Co-Design a Network CoDeNet with the modified deformable convolution and quantize it to 4-bit weights and 8-bit activations. With our high-efficiency implementation, our solution reaches 26.9 frames per second with a tiny model size of 0.76 MB while achieving 61.7 AP50 on the standard object detection dataset, Pascal VOC. With our higher accuracy implementation, our model gets to 67.1 AP50 on Pascal VOC with only 2.9 MB of parameters-20.9x smaller but 10% more accurate than Tiny-YOLO.

preprint2021arXiv

Efficient all-optical helicity dependent switching of spins in a Pt/Co/Pt film by a dual-pulse excitation

All-optical helicity dependent switching (AO-HDS), deterministic control of magnetization by circularly polarized laser pulses, allows to efficiently manipulate spins without the need of a magnetic field. However, AO-HDS in ferromagnetic metals so far requires many laser pulses for fully switching their magnetic states. Using a combination of a short, 90-fs linearly polarized pulse and a subsequent longer, 3-ps circularly polarized pulse, we demonstrate that the number of pulses for full magnetization reversal can be reduced to 4 pulse pairs in a single stack of Pt/Co/Pt. The obtained results suggest that the dual-pulse approach is a potential route towards realizing efficient AO-HDS in ferromagnetic metals.

preprint2020arXiv

Fair Resource Allocation in Federated Learning

Federated learning involves training statistical models in massive, heterogeneous networks. Naively minimizing an aggregate loss function in such a network may disproportionately advantage or disadvantage some of the devices. In this work, we propose q-Fair Federated Learning (q-FFL), a novel optimization objective inspired by fair resource allocation in wireless networks that encourages a more fair (specifically, a more uniform) accuracy distribution across devices in federated networks. To solve q-FFL, we devise a communication-efficient method, q-FedAvg, that is suited to federated networks. We validate both the effectiveness of q-FFL and the efficiency of q-FedAvg on a suite of federated datasets with both convex and non-convex models, and show that q-FFL (along with q-FedAvg) outperforms existing baselines in terms of the resulting fairness, flexibility, and efficiency.

preprint2020arXiv

FedDANE: A Federated Newton-Type Method

Federated learning aims to jointly learn statistical models over massively distributed remote devices. In this work, we propose FedDANE, an optimization method that we adapt from DANE, a method for classical distributed optimization, to handle the practical constraints of federated learning. We provide convergence guarantees for this method when learning over both convex and non-convex functions. Despite encouraging theoretical results, we find that the method has underwhelming performance empirically. In particular, through empirical simulations on both synthetic and real-world datasets, FedDANE consistently underperforms baselines of FedAvg and FedProx in realistic federated settings. We identify low device participation and statistical device heterogeneity as two underlying causes of this underwhelming performance, and conclude by suggesting several directions of future work.

preprint2020arXiv

Federated Optimization in Heterogeneous Networks

Federated Learning is a distributed learning paradigm with two key challenges that differentiate it from traditional distributed optimization: (1) significant variability in terms of the systems characteristics on each device in the network (systems heterogeneity), and (2) non-identically distributed data across the network (statistical heterogeneity). In this work, we introduce a framework, FedProx, to tackle heterogeneity in federated networks. FedProx can be viewed as a generalization and re-parametrization of FedAvg, the current state-of-the-art method for federated learning. While this re-parameterization makes only minor modifications to the method itself, these modifications have important ramifications both in theory and in practice. Theoretically, we provide convergence guarantees for our framework when learning over data from non-identical distributions (statistical heterogeneity), and while adhering to device-level systems constraints by allowing each participating device to perform a variable amount of work (systems heterogeneity). Practically, we demonstrate that FedProx allows for more robust convergence than FedAvg across a suite of realistic federated datasets. In particular, in highly heterogeneous settings, FedProx demonstrates significantly more stable and accurate convergence behavior relative to FedAvg---improving absolute test accuracy by 22% on average.

preprint2020arXiv

Outage Behaviors of NOMA-based Satellite Network over Shadowed-Rician Fading Channels

This paper investigates the application of non-orthogonal multiple access (NOMA) to satellite communication network over Shadowed-Rician fading channels. The impact of imperfect successive interference cancellation (ipSIC) on NOMA-based satellite network is taken into consideration from the perspective of practical scenarios. We first derive new exact expressions of outage probability for the p-th terrestrial user and provide the corresponding asymptotic analysis results. The diversity order of zero and p are achieved by the p-th terrestrial user with ipSIC and perfect successive interference cancellation (pSIC), respectively. Finally, the presented simulation results show that: 1) On the condition of pSIC, the outage behaviors of NOMA-based satellite network are superior to that of orthogonal multiple access; 2) With the value of residual interference increasing, the outage performance of terrestrial users with ipSIC is becoming worse seriously; and 3) Infrequent light shadowing of Shadowed-Rician fading brings the better outage probability compared to frequent heavy and average shadowing.

preprint2020arXiv

Squeezed Light Induced Two-photon Absorption Fluorescence of Fluorescein Biomarkers

Two-photon absorption (TPA) fluorescence of biomarkers has been decisive in advancing the fields of biosensing and deep-tissue in vivo imaging of live specimens. However, due to the extremely small TPA cross section and the quadratic dependence on the input photon flux, extremely high peak-intensity pulsed lasers are imperative, which can result in significant photo- and thermal-damage. Previous works on entangled TPA (ETPA) with spontaneous parametric down-conversion (SPDC) light sources found a linear dependence on the input photon-pair flux, but are limited by low optical powers, along with a very broad spectrum. We report that by using a high-flux squeezed light source for TPA, a fluorescence enhancement of 47 is achieved in fluorescein biomarkers as compared to classical TPA. Moreover, a polynomial behavior of the TPA rate is observed in the DCM laser dye.

preprint2019arXiv

Federated Learning: Challenges, Methods, and Future Directions

Federated learning involves training statistical models over remote devices or siloed data centers, such as mobile phones or hospitals, while keeping data localized. Training in heterogeneous and potentially massive networks introduces novel challenges that require a fundamental departure from standard approaches for large-scale machine learning, distributed optimization, and privacy-preserving data analysis. In this article, we discuss the unique characteristics and challenges of federated learning, provide a broad overview of current approaches, and outline several directions of future work that are relevant to a wide range of research communities.

preprint2018arXiv

Magnetotransport in phase-separated (Ga,Fe)N with $γ$'-Ga$_y$Fe$_{4-y}$N nanocrystals

The magnetotransport in phase-separated (Ga,Fe)N containing $γ$'-Ga$_y$Fe$_{4-y}$N (0\,$<$\,y\,$<$1) nanocrystals (NCs) is studied in the temperature range between 2\,K and 300\,K. The evolution of the resistivity and of the magnetoresistance (MR) as a function of temperature points at two conduction mechanisms: namely a conventional Arrhenius-type one down to 50\,K, and Mott variable range hopping at lower temperatures, where the spin-polarized current is transported between NCs in a regime in which phonon-scattering effects are not dominant. Below 25\,K, the MR shows a hysteretic contribution at magnetic fields $<$1\,T and proportional to the coercive field. Anisotropic magnetoresistance with values one order of magnitude greater than those previously reported for $γ$'-Fe$_4$N thin films over the whole considered temperature range, confirms that the observed MR in these layers is determined by the embedded nanocrystals.

preprint2016arXiv

Stretching magnetism with an electric field in a nitride semiconductor

By direct magnetization measurements, performed employing a new detection scheme, we demonstrate an electrical control of magnetization in wurtzite (Ga,Mn)N. In this dilute magnetic insulator the Fermi energy is pinned by Mn ions in the mid-gap region, and the Mn3+ ions show strong single-ion anisotropy. We establish that (Ga,Mn)N sustains an electric field up to at least 5 MV/cm, indicating that Mn doping turns GaN into a worthwhile semi-insulating material. Under these conditions, the magnetoelectric coupling may be driven by the inverse piezoelectric effect that stretches the elementary cell along the c axis and, thus, affects the magnitude of magnetic anisotropy. We develop a corresponding theory and show that it describes the experimentally determined dependence of magnetization on the electric field quantitatively with no adjustable parameters as a function of the magnetic field and temperature. In this way, our work bridges two research domains developed so far independently: piezoelectricity of wurtzite semiconductors and electrical control of magnetization in hybrid and composite magnetic structures containing piezoelectric components.

preprint2016arXiv

The effect of input phase modulation to a phase-sensitive optical amplifier

Many optical applications depend on amplitude modulating optical beams using devices such as acousto-optical modulators (AOMs) or optical choppers. Methods to add amplitude modulation (AM) often inadvertently impart phase modulation (PM) onto the light as well. While this PM is of no consequence to many phase-insensitive applications, phase-sensitive processes can be affected. Here we study the effects of input phase and amplitude modulation on the output of a quantum-noise limited phase-sensitive optical amplifier (PSA) realized in hot $^{85}$Rb vapor. We investigate the dependence of PM on AOM alignment and demonstrate a novel approach to quantifying PM by using the PSA as a diagnostic tool. We then use this method to measure the alignment-dependent PM of an optical chopper which arises due to diffraction effects as the chopper blade passes through the optical beam.

preprint2015arXiv

Controlling a three dimensional electron slab of graded Al$_{x}$Ga$_{1-x}$N

Polarization induced degenerate $n$-type doping with electron concentrations up to $\sim$10$^{20}$\,cm$^{-3}$ is achieved in graded Al$_{x}$Ga$_{1-x}$N layers ($x$: 0\%$\rightarrow$37\%) grown on unintentionally doped and on $n$-doped GaN:Si buffer/reservoir layers by metal organic vapor phase epitaxy. High resolution x-ray diffraction, transmission electron microscopy and electron energy loss spectroscopy confirm the gradient in the composition of the Al$_{x}$Ga$_{1-x}$N layers, while magnetotransport studies reveal the formation of a three dimensional electron slab, whose conductivity can be adjusted through the GaN(:Si) buffer/reservoir.

preprint2015arXiv

Incorporation of Mn in Al$_{x}$Ga$_{1-x}$N probed by x-ray absorption and emission spectroscopy, high-resolution microscopy, x-ray diffraction and first-principles calculations

Synchrotron radiation x-ray absorption and emission spectroscopy techniques, complemented by high-resolution transmission electron microscopy methods and density functional theory calculations are employed to investigate the effect of Mn in Al$_{x}$Ga$_{1-x}$N:Mn samples with an Al content up to 100%. The atomic and electronic structure of Mn is established together with its local environment and valence state. A dilute alloy without precipitation is obtained for Al$_{x}$Ga$_{1-x}$N:Mn with Al concentrations up to 82%, and the surfactant role of Mn in the epitaxial process is confirmed.

preprint2015arXiv

Non-Resonant Below-Bandgap Two-Photon Absorption in Quantum Dot Solar Cells

We are the first to show with clear experimental results that photons that have energy lower than the transition energy between quantum dots states and valance band can still contribute greatly to the photocurrent via both one-photon absorption process (1PA) and two-photon absorption process (2PA). The tailing states function as both the energy states for low energy photon absorption and the photocarriers extraction pathway. One of the biggest advantages of our method is that it can clearly differentiate the photocurrent due to 1PA process and 2PA process. Both 1PA and 2PA photocurrent generation efficiency in an InAs/GaAs QD device with photon excitation at 1550 nm have been quantitatively evaluated.

preprint2014arXiv

Planar array of self-assembled Ga$_{x}$Fe$_{4-x}$N nanocrystals in GaN: Magnetic anisotropy determined via ferromagnetic resonance

The magnetic anisotropy of a planar array of Ga$_{x}$Fe$_{4-x}$N nanocrystals (NCs) embedded in a GaN host is studied by ferromagnetic resonance. X-ray diffraction and transmission electron microscopy are employed to determine the phase and distribution of the nanocrystals. The magnetic anisotropy is found to be primarily uniaxial with the hard axis normal to the NCs plane and to have a comparably weak in-plane hexagonal symmetry. The origin of the magnetic anisotropy is discussed taking into consideration the morphology of the nanocrystals, the epitaxial relations, strain effects and magnetic coupling between the NCs.

preprint2014arXiv

Quantum mutual information of an entangled state propagating through a fast-light medium

Although it is widely accepted that classical information cannot travel faster than the speed of light in vacuum, the behavior of quantum correlations and quantum information propagating through actively-pumped fast-light media has not been studied in detail. To investigate this behavior, we send one half of an entangled state of light through a gain-assisted fast-light medium and detect the remaining quantum correlations. We show that the quantum correlations can be advanced by a small fraction of the correlation time while the entanglement is preserved even in the presence of noise added by phase-insensitive gain. Additionally, although we observe an advance of the peak of the quantum mutual information between the modes, we find that the degradation of the mutual information due to the added noise appears to prevent an advancement of the leading edge. In contrast, we show that both the leading and trailing edges of the mutual information in a slow-light system can be significantly delayed.

preprint2013arXiv

Advanced Quantum Noise

We use the quantum correlations of twin-beams of light to probe the added noise when one of the beams propagates through a medium with anomalous dispersion. The experiment is based on two successive four-wave mixing processes in rubidium vapor, which allow for the generation of bright two-mode-squeezed twin-beams followed by a controlled advancement while maintaining the shared quantum-correlations between the beams. The demonstrated effect allows the study of irreversible decoherence in a medium exhibiting anomalous dispersion, and for the first time shows the advancement of a bright nonclassical state of light. The advancement and corresponding degradation of the quantum correlations are found to be operating near the fundamental quantum limit imposed by using a phase-insensitive amplifier.

preprint2013arXiv

Magnetooptical properties of (Ga,Fe)N layers

Magnetooptical properties of (Ga,Mn)N layers containing various concentrations of Fe-rich nanocrystals embedded in paramagnetic (Ga,Fe)N layers are reported. Previous studies of such samples demonstrated that magnetization consists of a paramagnetic contribution due to substitutional diluted Fe ions as well as of ferromagnetic and antiferromagnetic components originating from Fe-rich nanocrystals, whose relative abundance can be controlled by the grow conditions. The nanocrystals are found to broaden and to reduce the magnitude of the excitonic features. However, the ferromagnetic contribution, clearly seen in SQUID magnetometry, is not revealed by magnetic circular dichroism (MCD). Possible reasons for differences in magnetic response determined by MCD and SQUID measurements are discussed.

preprint2013arXiv

Manipulating Mn--Mg$_k$ cation complexes to control the charge- and spin-state of Mn in GaN

Owing to the variety of possible charge and spin states and to the different ways of coupling to the environment, paramagnetic centres in wide band-gap semiconductors and insulators exhibit a strikingly rich spectrum of properties and functionalities, exploited in commercial light emitters and proposed for applications in quantum information. Here we demonstrate, by combining synchrotron techniques with magnetic, optical and \emph{ab initio} studies, that the codoping of GaN:Mn with Mg allows to control the Mn$^{n+}$ charge and spin state in the range $3\le n\le 5$ and $2\ge S\ge 1$. According to our results, this outstanding degree of tunability arises from the formation of hitherto concealed cation complexes Mn-Mg$_k$, where the number of ligands $k$ is pre-defined by fabrication conditions. The properties of these complexes allow to extend towards the infrared the already remarkable optical capabilities of nitrides, open to solotronics functionalities, and generally represent a fresh perspective for magnetic semiconductors.

preprint2013arXiv

Method for traveling-wave deceleration of buffer-gas beams of CH

Cryogenic buffer-gas beams are a promising method for producing bright sources of cold molecular radicals for cold collision and chemical reaction experiments. In order to use these beams in studies of reactions with controlled collision energies, or in trapping experiments, one needs a method of controlling the forward velocity of the beam. A Stark decelerator can be an effective tool for controlling the mean speed of molecules produced by supersonic jets, but efficient deceleration of buffer-gas beams presents new challenges due to longer pulse lengths. Traveling-wave decelerators are uniquely suited to meet these challenges because of their ability to confine molecules in three dimensions during deceleration and the versatility afforded by the analog control of the electrodes. We have created ground state CH($X^2Π$) radicals in a cryogenic buffer-gas cell with the potential to produce a cold molecular beam of $10^{11}$ mol./pulse. We present a general protocol for Stark deceleration of beams with large position and velocity spreads for use with a traveling-wave decelerator. Our method involves confining molecules transversely with a hexapole for an optimized distance before deceleration. This rotates the phase-space distribution of the molecular packet so that the packet is matched to the time varying phase-space acceptance of the decelerator. We demonstrate with simulations that this method can decelerate a significant fraction of the molecules in successive wells of a traveling-wave decelerator to produce energy-tuned beams for cold and controlled molecule experiments.

preprint2013arXiv

Phase diagram and critical behavior of the random ferromagnet $Ga_{1-x}Mn_xN$

Molecular beam epitaxy has been employed to obtain Ga1-xMnxN films with x up to 10% and Curie temperatures T_C up to 13 K. The magnitudes of T_C and their dependence on x, T_C(x) ~ x^m, where m = 2.2 +/- 0.2 are quantitatively described by a tight binding model of superexchange interactions and Monte Carlo simulations of T_C. The critical behavior of this dilute magnetic insulator shows strong deviations from the magnetically clean case (x = 1), in particular, (i) an apparent breakdown of the Harris criterion; (ii) a non-monotonic crossover in the values of the susceptibility critical exponent gamma_eff between the high temperature and critical regimes, and (iii) a smearing of the critical region, which can be explained either by the Griffiths effects or by macroscopic inhomogeneities in the spin distribution with a variance Delta x = (0.2 +/- 0.1)%.

preprint2012arXiv

GaMnN epitaxial films with high magnetization

We report on the fabrication of pseudomorphic wurtzite GaMnN grown on GaN with Mn concentrations up to 10% using molecular beam epitaxy. According to Rutherford backscattering the Mn ions are mainly at the Ga-substitutional positions, and they are homogeneously distributed according to depth-resolved Auger-electron spectroscopy and secondary-ion mass-spectroscopy measurements. A random Mn distribution is indicated by transmission electron microscopy, no Mn-rich clusters are present for optimized growth conditions. A linear increase of the c-lattice parameter with increasing Mn concentration is found using x-ray diffraction. The ferromagnetic behavior is confirmed by superconducting quantum-interference measurements showing saturation magnetizations of up to 150 emu/cm^3.

preprint2012arXiv

Planar arrays of magnetic nanocrystals embedded in GaN

Single planar arrays of Ga(x)Fe(4-x)N magnetic nanocrystals embedded in GaN have been fabricated in an epitaxial process. The phase of the nanocrystals and their epitaxial relationship with the host matrix are studied $via$ high-resolution transmission electron microscopy and high-resolution x-ray diffraction. By changing the growth parameters and mode, the crystallographic phase and chemical composition of the nanocrystals can be varied on demand. In view of the different magnetic properties of the various phases, applications in room-temperature ferromagnetic as well as antiferromagnetic spintronic devices are envisaged.

preprint2011arXiv

Experimental probing of exchange interactions between localized spins in the dilute magnetic insulator (Ga,Mn)N

The sign, magnitude, and range of the exchange couplings between pairs of Mn ions is determined for (Ga,Mn)N and (Ga,Mn)N:Si with x < 3%. The samples have been grown by metalorganic vapor phase epitaxy and characterized by secondary-ion mass spectroscopy; high-resolution transmission electron microscopy with capabilities allowing for chemical analysis, including the annular dark-field mode and electron energy loss spectroscopy; high-resolution and synchrotron x-ray diffraction; synchrotron extended x-ray absorption fine-structure; synchrotron x-ray absorption near-edge structure; infra-red optics and electron spin resonance. The results of high resolution magnetic measurements and their quantitative interpretation have allowed to verify a series of ab initio predictions on the possibility of ferromagnetism in dilute magnetic insulators and to demonstrate that the interaction changes from ferromagnetic to antiferromagnetic when the charge state of the Mn ions is reduced from 3+ to 2+.

preprint2011arXiv

Structural and paramagnetic properties of dilute Ga1-xMnxN

Systematic investigations of the structural and magnetic properties of single crystal (Ga,Mn)N films grown by metal organic vapor phase epitaxy are presented. High resolution transmission electron microscopy, synchrotron x-ray diffraction, and extended x-ray absorption fine structure studies do not reveal any crystallographic phase separation and indicate that Mn occupies Ga-substitutional sites in the Mn concentration range up to 1%. The magnetic properties as a function of temperature, magnetic field and its orientation with respect to the c-axis of the wurtzite structure can be quantitatively described by the paramagnetic theory of an ensemble of non-interacting Mn$^{3+}$ ions in the relevant crystal field, a conclusion consistent with the x-ray absorption near edge structure analysis. A negligible contribution of Mn in the 2+ charge state points to a low concentration of residual donors in the studied films. Studies on modulation doped p-type (Ga,Mn)N/(Ga,Al)N:Mg heterostructures do not reproduce the high temperature robust ferromagnetism reported recently for this system.

preprint2011arXiv

The Fe-Mg interplay and the effect of deposition mode in (Ga,Fe)N doped with Mg

The effect of Mg codoping and its deposition mode on the Fe distribution in (Ga,Fe)N layers grown by metalorganic vapor phase epitaxy is investigated. Both homogeneously- and digitally-Mg codoped samples are considered and contrasted to the case of (Ga,Fe)N layers obtained without any codoping by shallow impurities. The structural analysis of the layers by high-resolution transmission electron microscopy and by high-resolution- and synchrotron x-ray diffraction gives evidence of the fact that in the case of homogenous-Mg doping, Mg and Fe competitively occupy the Ga-substitutional cation sites, reducing the efficiency of Fe incorporation. Accordingly, the character of the magnetization is modified from ferromagnetic-like in the non-codoped films to paramagnetic in the case of homogeneous Mg codoping. The findings are discussed vis-`a-vis theoretical results obtained by ab initio computations, showing only a weak effect of codoping on the pairing energy of two Fe cations in bulk GaN. However, according to these computations, codoping reverses the sign of the paring energy of Fe cations at the Ga-rich surface, substantiating the view that the Fe aggregation occurs at the growth surface. In contrast to the homogenous deposition mode, the digital one is found to remarkably promote the aggregation of the magnetic ions. The Fe-rich nanocrystals formed in this way are distributed non-uniformly, giving reason for the observed deviation from a standard superparamagnetic behavior.

preprint2010arXiv

Compensation-dependence of magnetic and electrical properties in Ga1-xMnxP

We demonstrate the control of the hole concentration in Ga1-xMnxP over a wide range by introducing compensating vacancies. The resulting evolution of the Curie temperature from 51 K to 7.5 K is remarkably similar to that observed in Ga1-xMnxAs despite the dramatically different character of hole transport between the two material systems. The highly localized nature of holes in Ga1-xMnxP is reflected in the accompanying increase in resistivity by many orders of magnitude. Based on variable-temperature resistivity data we present a general picture for hole conduction in which variable-range hopping is the dominant transport mechanism in the presence of compensation.

preprint2010arXiv

Embedded magnetic phases in (Ga,Fe)N: the key role of growth temperature

The local chemistry, structure, and magnetism of (Ga,Fe)N nanocomposites grown by metal organic vapor phase epitaxy is studied by high resolution synchrotron x-ray diffraction and absorption, transmission electron microscopy, and superconducting quantum interference device magnetometry as a function of the growth temperature $T_{\mathrm{g}}$. Three contributions to the magnetization are identified: i) paramagnetic -- originating from dilute and non-interacting Fe$^{3+}$ ions substitutional of Ga, and dominating in layers obtained at the lowest considered $T_{\mathrm{g}}$ (800$^{\circ}$C); ii) superparamagnetic-like -- brought about mainly by ferromagnetic nanocrystals of $ε-$Fe$_3$N but also by $γ'$-Fe$_4$N and by inclusions of elemental $α$- and $γ$-Fe, and prevalent in films obtained in the intermediate $T_{\mathrm{g}}$ range; iii) component linear in the magnetic field and associated with antiferromagnetic interactions -- found to originate from highly nitridated Fe$_x$N ($x \leq$ 2) phases, like $ζ$-Fe$_2$N, and detected in samples deposited at the highest employed temperature, $T_{\mathrm{g}}$ = 950$^{\circ}$C. Furthermore, depending on $T_{\mathrm{g}}$, the Fe-rich nanocrystals segregate towards the sample surface or occupy two-dimensional planes perpendicular to the growth direction.

preprint2009arXiv

Local structure of (Ga,Fe)N and (Ga,Fe)N:Si investigated by x-ray absorption fine structure spectroscopy

X-ray absorption fine-structure (XAFS) measurements supported by {\em ab initio} computations within the density functional theory (DFT) are employed to systematically characterize Fe-doped as well as Fe and Si-co-doped films grown by metalorganic vapour phase epitaxy. The analysis of extended-XAFS data shows that depending on the growth conditions, Fe atoms either occupy Ga substitutional sites in GaN or precipitate in the form of $ε$-Fe$_3$N nanocrystals, which are ferromagnetic and metallic according to the DFT results. Precipitation can be hampered by reducing the Fe content, or by increasing the growth rate or by co-doping with Si. The near-edge region of the XAFS spectra provides information on the Fe charge state and shows its partial reduction from Fe$^{+3}$ to Fe$^{+2}$ upon Si co-doping, in agreement with the Fe electronic configurations expected within various implementations of DFT.