Publications

In medical infections such as blood sepsis and in food quality control, fast and accurate bacteria analysis is required. Using magnetic nanoparticles (MNPs) for bacterial capture and concentration is very promising for rapid analysis. When MNPs are functionalized with the proper surface chemistry, they have the ability to bind to bacteria and aid in the removal and concentration of bacteria from a sample for further analysis. This study introduces a novel approach for bacterial concentration using polydopamine (pDA), a highly adhesive polymer often purported to create antibacterial and antibiofouling coatings on medical devices. Although pDA has been generally studied for its ability to coat surfaces and reduce biofilm growth, we have found that when coated on magnetic nanoclusters (MNCs), more specifically iron oxide nanoclusters, it effectively binds to and can remove from suspension some types of bacteria. This study investigated the binding of pDA-coated MNCs (pDA-MNCs) to various Gram-negative and Gram-positive bacteria, including Staphylococcus aureus, Staphylococcus epidermidis, Pseudomonas aeruginosa, and several E. coli strains. MNCs were successfully coated with pDA, and these functionalized MNCs bound a wide variety of bacterial strains. The efficiency of removing bacteria from a suspension can range from 0.99 for S. aureus to 0.01 for an E. coli strain. Such strong capture and differential capture have important applications in collecting bacteria from dilute samples found in medical diagnostics, food and water quality monitoring, and other industries.

Tabletop extreme ultraviolet (EUV) sources based on high harmonic generation (HHG) have been used as a powerful tool for probing magnetism. Obtaining magnetic information via magneto-optical contrast often requires the energy of the light to be tuned to magnetic resonance energies of the magnetic element present in the material; therefore, it is essential to calibrate the HHG spectrum to well defined absorption energies of materials. We have designed and assembled a HHG based EUV source for studying transition metal magnetic materials at their resonant M-absorption edges (35-75 eV of photon energy). One material of interest is iron, for which the iron M2,3 edge is 52.7 eV (23.5 nm wavelength) according to CXRO. We prepared and characterized a thin sample of iron for absorption spectroscopy and calibration of the absorption edge with beamline 6.3.2 at the Advance Light Source (ALS) in Lawrence Berkeley National Laboratory. This well characterized sample was capped with gold to prevent oxidation. From these measurements we extracted the absorption part of the index of refraction β spectrally and confirmed that the absorption edge of iron is 52.7 eV. With this information, we can better calibrate the HHG spectrum of our tabletop EUV source. Calibration of the HHG spectrum was achieved using model fitting the HHG spectrum using the grating equation and law of cosines while taking account into the results of the ALS data. We have determined that driving wavelength of the HHG process to be 773 nm. We also conclude that the chirp of the driving laser pulse can cause an energy shift to a HHG spectrum.

We report on magnetic orderings of nanospins in self-assemblies of Fe₃O₄ nanoparticles (NPs), occurring at various stages of the magnetization process throughout the superparamagnetic (SPM)-blocking transition. Essentially driven by magnetic dipole couplings and by Zeeman interaction with a magnetic field applied out-of-plane, these magnetic orderings include a mix of long-range parallel and antiparallel alignments of nanospins, with the antiparallel correlation being the strongest near the coercive point below the blocking temperature. The magnetic ordering is probed via x-ray resonant magnetic scattering (XRMS), with the x-ray energy tuned to the Fe−L₃ edge and using circular polarized light. By exploiting dichroic effects, a magnetic scattering signal is isolated from the charge scattering signal. We measured the nanospin ordering for two different sizes of NPs, 5 and 11 nm, with blocking temperatures TB of 28 and 170 K, respectively. At 300 K, while the magnetometry data essentially show SPM and absence of hysteresis for both particle sizes, the XRMS data reveal the presence of nonzero (up to 9%) antiparallel ordering when the applied field is released to zero for the 11 nm NPs. These antiparallel correlations are drastically amplified when the NPs are cooled down below TB and reach up to 12% for the 5 nm NPs and 48% for the 11 nm NPs, near the coercive point. The data suggest that the particle size affects the prevalence of the antiparallel correlations over the parallel correlations by a factor ∼1.6 to 3.8 higher when the NP size increases from 5 to 11 nm.

Optimizing magnetic thin films for nanotechnologies often requires imaging nanoscale magnetic domain patterns via magnetic microscopy. The finite size of the image may however significantly affect the characterization of the observed magnetic states. We evaluated finite image size effects on the characterization of a variety of stripe and bubble domain patterns exhibited by ferromagnetic Co/Pt multilayers with perpendicular magnetic anisotropy, where the domain size (stripe width and bubble diameter) is around 100 nm. If the image size is too small, below ∼5 μm, it may cause a significant underestimation of average domain size and overestimation of domain density by up to a factor 5 when reducing the image size from about 20 μm to about a 1 μm. Using a criterion based on how the excess density evolves with image size, we found that to obtain reliable statistical estimates of domain density and average domain size, the image needs to be large enough, and include at least about 100 stripes or about 2500 bubbles.

Thermoelectric materials hold tremendous promise for energy applications, but developing economically and environmentally viable high-performance thermoelectrics remains challenging. Recently, the paramagnon drag effect was discovered, in which local thermal fluctuations of the magnetization known as paramagnons drag charge carriers and impart to them a magnetic contribution to thermopower. This is significant because it opens a new avenue for optimizing thermoelectric properties in magnetic semiconductors. In this work, neutron scattering is used to visualize the nanoscale magnetism responsible for paramagnon drag in the antiferromagnetic semiconductor MnTe. First-principles calculations quantitatively reproduce the short-range magnetic correlations observed above the ordering temperature. These results shed light on how magnetism enhances thermoelectricity and provide a template for studies of other magnetic semiconductors as potential high-performance thermoelectrics.

We measured the local magneto-transport (MT) signal with an out-of-plane magnetic field, including magneto-resistance (MR) and Extraordinary Hall effect (EHE), in exchange-biased [Co/Pd]IrMn thin multilayers that are micro-structured with a 100 μm window. We found that when measured locally around the window, the MT signal deviate from the expected behavior. We studied possible causes, including film micro-structuration, electrical contact geometry as well as magnetic field angular tilt. We found that tilting the magnetic field direction with respect to the normal direction does not significantly affect the MT signal, whereas the positioning and geometry of the contacts seem to highly affect the MT signal. For comparison purposes, we carried these MT measurements using the Van-der-Pauw method on a set of four microscopic contacts directly surrounding the window, and on another set of micro-contacts located outside the window, as well as a set of four contacts positioned several millimeters away of each other at the corners of the wafer. If the contacts are sufficiently far apart, the EHE and MR signals have the expected shape and are not significantly affected by the presence of the window. If, on the other hand, the contacts are micro-positioned, the shape of the EHE signal is drastically deformed, and may be modeled as a mix of the standard EHE and MR signals measured on the outer contacts. Furthermore, if the micro-contacts are located directly around the window, the deformation is amplified, and the weight of the MR signal in the mix is further increased by about 40 %. This suggests that the electron path in the Hall geometry is disturbed by both the proximity of the electrodes and by the presence of the window, which both contribute to the deformation for about two-third and one third, respectively.

Magnetic nanoparticles offer unique potential for various technological, biomedical, or environmental applications thanks to the size-, shape- and material-dependent tunability of their magnetic properties. To optimize particles for a specific application, it is crucial to interrelate their performance with their structural and magnetic properties. This review presents the advantages of small-angle X-ray and neutron scattering techniques for achieving a detailed multiscale characterization of magnetic nanoparticles and their ensembles in a mesoscopic size range from 1 to a few hundred nanometers with nanometer resolution. Both X-rays and neutrons allow the ensemble-averaged determination of structural properties, such as particle morphology or particle arrangement in multilayers and 3D assemblies. Additionally, the magnetic scattering contributions enable retrieving the internal magnetization profile of the nanoparticles as well as the inter-particle moment correlations caused by interactions within dense assemblies. Most measurements are used to determine the time-averaged ensemble properties, in addition advanced small-angle scattering techniques exist that allow accessing particle and spin dynamics on various timescales. In this review, we focus on conventional small-angle X-ray and neutron scattering (SAXS and SANS), X-ray and neutron reflectometry, gracing-incidence SAXS and SANS, X-ray resonant magnetic scattering, and neutron spin-echo spectroscopy techniques. For each technique, we provide a general overview, present the latest scientific results, and discuss its strengths as well as sample requirements. Finally, we give our perspectives on how future small-angle scattering experiments, especially in combination with micromagnetic simulations, could help to optimize the performance of magnetic nanoparticles for specific applications.

The magnetic properties of Fe₃O₄ nanoparticle assemblies have been investigated in detail through a combination of vibrating sample magnetometry (VSM) and muon spin relaxation (μSR) techniques. Two samples with average particle sizes of 5 and 20 nm, respectively, were studied. For both samples, the VSM and μSR results exhibit clear signatures of superparamagnetism at high temperature and magnetic blocking at low temperature. The μSR data demonstrate that the transition from the superparamagnetic to the blocked state occurs gradually throughout the sample volume over an extended temperature range due to the finite particle size distribution of each nanoparticle batch. The transition occurs between approximately 3 and 45 K for the 5-nm nanoparticles and 150 and 300 K for the 20-nm nanoparticles. The VSM and μSR data are further analyzed to yield estimates of microscopic magnetic parameters including the nanoparticle spin-flip activation energy EA, magnetic anisotropy K, and intrinsic nanoparticle spin reversal attempt time τ₀. These results highlight the complementary information about magnetic nanoparticles that can be obtained by bulk magnetic probes such as magnetometry and local magnetic probes such as μSR.

65th Annual Conference on Magnetism and Magnetic Materials, (Online, November 2020).

Due to their non-toxicity and their ability to be functionalized, magnetite (Fe3O4) nanoparticles (NP) are good candidates for a variety of biomedical applications. To better implement their applications, it is crucial to well understand the basic structural and magnetic properties of the NPs in correlation with their synthesis method. Here, we show interesting properties of Fe3O4 NPs of various sizes ranging from 5 to 100 nm and the dependence of these properties on particle size and preparation method. One synthetic method based on heating Fe(acac)3 with oleic acid consistently gives 5 ± 1 nm NPs. A second method using the thermal decomposition of Fe(oleate)3 in oleic acid led to larger NPs, greater than 8 nm in size. Increasing the amount of oleic acid caused the average NP size to slightly increase, from 8 to 10 nm. Increasing both the reaction temperature and the reaction time caused the NP size to drastically increase from 10 to 100 nm. Powder x-ray diffraction and electron-microscopy imaging show a pure single crystalline Fe3O4 phase for all NPs smaller than 50 nm and spherical in shape. When the NPs get larger than 50 nm, they notably tend to form faceted, FeO core-Fe3O4 shell structures. Magnetometry data collected in various field-cooling conditions show a pure superparamagnetic (SPM) behavior for all NPs smaller than 20 nm. The observed blocking temperature, TB, gradually increases with NP size from about 25 K to 150 K. In addition, the Verwey transition is observed with the emergence of a strong narrow peak at 125 K in the magnetization curves when larger NPs are present. Our data confirm the vanishing of the Verwey transition in smaller NPs. Magnetization loops indicate that the saturating field drastically decreases with NP size. While larger NPs show some coercivity (Hc ) up to 30 mT at 400 K, NPs smaller than 20 nm show no coercivity (Hc =0), confirming their pure SPM behavior at high temperature. Upon cooling below TB, some of the SPM NPs gradually show some coercivity, with Hc reaching 50 mT at 5 K for the 10 nm NPs, indicating emergent interparticle couplings in the blocked state.

The occurrence of memory effects in the formation of magnetic domains is both of fundamental and technological interest. We have probed the amount of domain memory in ferromagnetic thin films by using soft x-ray speckle cross-correlation metrology. We have found that a very strong domain memory (over 90%) can be induced in the ferromagnetic layer when subjected to exchange couplings with an antiferromagnetic layer. We show here the variation of the degree of memory as function of magnetic field through magnetization loop and the persistence of this memory through repeated field cycling.