Submicron Length Scales Research Articles

Near-field coupling of gold plasmonic antennas for sub-100 nm magneto-thermal microscopy

The development of spintronic technology with increasingly dense, high-speed, and complex devices will be accelerated by accessible microscopy techniques capable of probing magnetic phenomena on picosecond time scales and at deeply sub-micron length scales. A recently developed time-resolved magneto-thermal microscope provides a path towards this goal if it is augmented with a picosecond, nanoscale heat source. We theoretically study adiabatic nanofocusing and near-field heat induction using conical gold plasmonic antennas to generate sub-100 nm thermal gradients for time-resolved magneto-thermal imaging. Finite element calculations of antenna-sample interactions reveal focused electromagnetic loss profiles that are either peaked directly under the antenna or are annular, depending on the sample’s conductivity, the antenna’s apex radius, and the tip-sample separation. We find that the thermal gradient is confined to 40 nm to 60 nm full width at half maximum for realistic ranges of sample conductivity and apex radius. To mitigate this variation, which is undesirable for microscopy, we investigate the use of a platinum capping layer on top of the sample as a thermal transduction layer to produce heat uniformly across different sample materials. After determining the optimal capping layer thickness, we simulate the evolution of the thermal gradient in the underlying sample layer and find that the temporal width is below 10 ps. These results lay a theoretical foundation for nanoscale, time-resolved magneto-thermal imaging.

High-order multipole radiation from quantum Hall states in Dirac materials

We investigate the optical response of strongly disordered quantum Hall states in two-dimensional Dirac materials and find qualitatively different effects in the radiation properties of the bulk versus the edge. We show that the far-field radiation from the edge is characterized by large multipole moments (> 50) due to the efficient transfer of angular momentum from the electrons into the scattered light. The maximum multipole transition moment is a direct measure of the coherence length of the edge states. Accessing these multipole transitions would provide new tools for optical spectroscopy and control of quantum Hall edge states. On the other hand, the far-field radiation from the bulk appears as random dipole emission with spectral properties that vary with the local disorder potential. We determine the conditions under which this bulk radiation can be used to image the disorder landscape. Such optical measurements can probe sub-micron length scales over large areas and provide complementary information to scanning probe techniques. Spatially resolving this bulk radiation would serve as a novel probe of the percolation transition near half-filling.

Solving Nongray Boltzmann Transport Equation in Gallium Nitride

Several studies have validated that diffusive Fourier model is inadequate to model thermal transport at submicron length scales. Hence, Boltzmann transport equation (BTE) is being utilized to improve thermal predictions in electronic devices, where ballistic effects dominate. In this work, we investigated the steady-state thermal transport in a gallium nitride (GaN) film using the BTE. The phonon properties of GaN for BTE simulations are calculated from first principles—density functional theory (DFT). Despite parallelization, solving the BTE is quite expensive and requires significant computational resources. Here, we propose two methods to accelerate the process of solving the BTE without significant loss of accuracy in temperature prediction. The first one is to use the Fourier model away from the hot-spot in the device where ballistic effects can be neglected and then couple it with a BTE model for the region close to hot-spot. The second method is to accelerate the BTE model itself by using an adaptive model which is faster to solve as BTE for phonon modes with low Knudsen number is replaced with a Fourier like equation. Both these methods involve choosing a cutoff parameter based on the phonon mean free path (mfp). For a GaN-based device considered in the present work, the first method decreases the computational time by about 70%, whereas the adaptive method reduces it by 60% compared to the case where full BTE is solved across the entire domain. Using both the methods together reduces the overall computational time by more than 85%. The methods proposed here are general and can be used for any material. These approaches are quite valuable for multiscale thermal modeling in solving device level problems at a faster pace without a significant loss of accuracy.

Preliminary Study on Tensile Properties of Electrospun Silica Fibers/Polypropylene Composites

Composites based on silica and glass fibers conventionally contain fibers with dimension in the range of a few micrometers to millimeters. Electrospinning technique allows fabrication of fibers in the submicron length scale. With smaller dimension, these fibers when applied as reinforcement in composites may yield interesting composite properties. In this paper, silica fibers fabricated via electrospinning were utilized as reinforcement in polypropylene-matrixed composites. The silica precursor was prepared by sol-gel reaction of tetraethyl orthosilicate, ethyl alcohol, de-ionized water and hydrochloric acid. Viscous silica precursor was made into fibers by electrospinning with electric field of 1 kV/cm. Electrospun non-woven fiber mats were stabilized at 200°C and calcined at 800°C to remove remaining organic residues. The fiber diameter average was 279±40 nm. In the process of making composites, the silica fiber mats were sandwiched between polypropylene sheets, and the layers were compression-molded together. The composite samples with varied silica fiber contents up to 2 wt% were mechanically tested. Tensile tests demonstrate slight increases in tensile modulus, tensile strength with increasing silica fiber content. However, silica fiber content within the experimental range does not have prominent effects on yield strength and strain at break.

Synchrotron-based X-ray fluorescence microscopy enables multiscale spatial visualization of ions involved in fungal lignocellulose deconstruction

The role of ions in the fungal decay process of lignocellulose biomaterials, and more broadly fungal metabolism, has implications for diverse research disciplines ranging from plant pathology and forest ecology, to carbon sequestration. Despite the importance of ions in fungal decay mechanisms, the spatial distribution and quantification of ions in lignocellulosic cell walls and fungal hyphae during decay is not known. Here we employ synchrotron-based X-ray fluorescence microscopy (XFM) to map and quantify physiologically relevant ions, such as K, Ca, Mn, Fe, and Zn, in wood being decayed by the model brown rot fungus Serpula lacrymans. Two-dimensional XFM maps were obtained to study the ion spatial distributions from mm to submicron length scales in wood, fungal hyphae with the dried extracellular matrix (ECM) from the fungus, and Ca oxalate crystals. Three-dimensional ion volume reconstructions were also acquired of wood cell walls and hyphae with ECM. Results show that the fungus actively transports some ions, such as Fe, into the wood and controls the distribution of ions at both the bulk wood and cell wall length scales. These measurements provide new insights into the movement of ions during decay and illustrate how synchrotron-based XFM is uniquely suited study these ions.

In situ observation of strain and phase transformation in plastically deformed 301 austenitic stainless steel

To inform the design of superior transformation-induced plasticity (TRIP) steels, it is important to understand what happens at the microstructural length scales. In this study, strain-induced martensitic transformation is studied by in situ digital image correlation (DIC) in a scanning electron microscope. Digital image correlation at submicron length scales enables mapping of transformation strains with high confidence. These are correlated with electron backscatter diffraction (EBSD) prior to and post deformation process to get a comprehensive understanding of the strain-induced transformation mechanism. The results are compared with mathematical models for enhanced prediction of strain-induced martensitic phase transformation.

Microscopic Investigation of Degradation Processes in a Polyfluorene Blend by Near-Field Scanning Optical Microscopy

We have studied the degradation of the photoluminescence (PL) of a phase-separated film of a polyfluorene blend, F8BT/PFO, on the submicron length scale using near-field scanning optical microscopy, visualizing the PL of blend compositions that do not exist macroscopically in equilibrium. In the initial scans, the topography and the PL were anticorrelated, as the emission was dominated by the PFO-rich phase. This behavior changed at longer illumination times, where the emission was dominated by the F8BT-rich phase; i.e., the topography and PL were correlated. Using macroscopic investigation of the mechanisms that govern the PL, we could explain the time dependence of the PL spatial distribution: while the degradation of F8BT was driven by photobleaching, both faster absorption degradation and photobleaching processes dominate the degradation of PFO. In addition, we found that energy transfer does not protect the PFO from degradation and does not improve its resistance to oxidation.

Mesoscale simulation of clay aggregate formation and mechanical properties

This paper proposes a novel methodology for understanding the meso-scale aggregation of clay platelets in water. We use Molecular Dynamics simulations using the CLAYFF force fields to represent the interactions between two layers of Wyoming montmorillonite (Na-smectite) in bulk water. The analyses are used to establish the potential of mean force at different spacings between the layers for edge-to-edge and face-to-face interactions. This is accomplished by finding the change in free energy as a function of the separation distance between the platelets using thermodynamic perturbation theory with a simple overlap sampling method. These nanoscale results are then used to calibrate the Gay–Berne (GB) potential that represents each platelet as a single-site ellipsoidal body. A coarse-graining upscaling approach then uses the GB potentials and molecular dynamics to represent the meso-scale aggregation of clay platelets (at submicron length scale). Results from meso-scale simulations obtain the equilibrium/jamming configurations for mono-disperse clay platelets. The results show aggregation for a range of clay platelets dimensions and pressures with mean stack size ranging from 3 to 8 platelets. The particle assemblies become more ordered and exhibit more pronounced elastic anisotropy at higher confining pressures. The results are in good agreement with previously measured nano-indentation moduli over a wide range of clay packing densities.

Uncovering three-dimensional gradients in fibrillar orientation in an impact-resistant biological armour.

The complex hierarchical structure in biological and synthetic fibrous nanocomposites entails considerable difficulties in the interpretation of the crystallographic texture from diffraction data. Here, we present a novel reconstruction method to obtain the 3D distribution of fibres in such systems. An analytical expression is derived for the diffraction intensity from fibres, explaining the azimuthal intensity distribution in terms of the angles of the three dimensional fibre orientation distributions. The telson of stomatopod (mantis shrimp) serves as an example of natural biological armour whose high impact resistance property is believed to arise from the hierarchical organization of alpha chitin nanofibrils into fibres and twisted plywood (Bouligand) structures at the sub-micron and micron scale. Synchrotron microfocus scanning X-ray diffraction data on stomatopod telson were used as a test case to map the 3D fibre orientation across the entire tissue section. The method is applicable to a range of biological and biomimetic structures with graded 3D fibre texture at the sub-micron and micron length scales.

Hydrogen behavior in Al[sbnd]Cr alloys: Synchrotron-based photoelectron microscopy of the rapidly solidified structure

This work reports recent advances in characterization of the composition at submicron length scales of Al-based rapidly solidified alloys, which are correlated to their interactions with hydrogen. The hydrogen desorption kinetics and the evolution of the surface and subsurface structure and chemical state of high-purity Al and Al-3.0 at.% Cr alloy have been studied by thermal desorption analysis and scanning photoelectron microscopy. The alloy foil structure consisted of Cr-rich and Cr-depleted surface regions exhibits Cr segregation beneath the surface. The obtained results reveal how inclusions of aluminum oxide species can become very strong hydrogen traps at the highest temperatures of 600–630 °C, representing irreversible trapping in Al and its alloy. The effect of strong reversible and irreversible hydrogen traps on hydrogen desorption from aluminum alloys is discussed, suggesting that their direct identification in the microstructure provides further insights into hydrogen embrittlement mechanisms for aluminum materials in energy technologies.

Influences of Substrate Adhesion and Particle Size on the Shape Memory Effect of Polystyrene Particles.

Formulations and applications of micro- and nanoscale polymer particles have proliferated rapidly in recent years, yet knowledge of their mechanical behavior has not grown accordingly. In this study, we examine the ways that compressive strain, substrate surface energy, and particle size influence the shape memory cycle of polystyrene particles. Using nanoimprint lithography, differently sized particles are programmed into highly deformed, temporary shapes in contact with substrates of differing surface energies. Atomic force microscopy is used to obtain in situ measurements of particle shape recovery kinetics, and scanning electron microscopy is employed to assess differences in the profiles of particles at the conclusion of the shape memory cycle. Finally, finite element models are used to investigate the growing impact of surface energies at smaller length scales. Results reveal that the influence of substrate adhesion on particle recovery is size-dependent and can become dominating at submicron length scales.

Gating mechanism of mechanosensitive channel of large conductance: a coupled continuum mechanical-continuum solvation approach.

Gating transition of the mechanosensitive channel of large conductance (MscL) represents a good example of important biological processes that are difficult to describe using atomistic simulations due to the large (submicron) length scale and long (millisecond) time scale. Here we develop a novel computational framework that tightly couples continuum mechanics with continuum solvation models to study the detailed gating behavior of E. coli-MscL. The components of protein molecules are modeled by continuum elements that properly describe their shape, material properties and physicochemical features (e.g., charge distribution). The lipid membrane is modeled as a three-layer material in which the lipid head group and tail regions are treated separately, taking into account the fact that fluidic lipid bilayers do not bear shear stress. Coupling between mechanical and chemical responses of the channel is realized by an iterative integration of continuum mechanics (CM) modeling and continuum solvation (CS) computation. Compared to previous continuum mechanics studies, the present model is capable of capturing the most essential features of the gating process in a much more realistic fashion: due mainly to the apolar solvation contribution, the membrane tension for full opening of MscL is reduced substantially to the experimental measured range. Moreover, the pore size stabilizes constantly during gating because of the intricate interactions of the multiple components of the system, implying the mechanism for sub-conducting states of MscL gating. A significant fraction ([Formula: see text]2/3) of the gating membrane strain is required to reach the first sub-conducting state of our model, which is featured with a relative conductance of 0.115 to the fully opened state. These trends agree well with experimental observations. We anticipate that the coupled CM/CS modeling framework is uniquely suited for the analysis of many biomolecules and their assemblies under external mechanical stimuli.

Femtosecond few- to single-electron point-projection microscopy for nanoscale dynamic imaging.

Femtosecond electron microscopy produces real-space images of matter in a series of ultrafast snapshots. Pulses of electrons self-disperse under space-charge broadening, so without compression, the ideal operation mode is a single electron per pulse. Here, we demonstrate femtosecond single-electron point projection microscopy (fs-ePPM) in a laser-pump fs-e-probe configuration. The electrons have an energy of only 150 eV and take tens of picoseconds to propagate to the object under study. Nonetheless, we achieve a temporal resolution with a standard deviation of 114 fs (equivalent to a full-width at half-maximum of 269 ± 40 fs) combined with a spatial resolution of 100 nm, applied to a localized region of charge at the apex of a nanoscale metal tip induced by 30 fs 800 nm laser pulses at 50 kHz. These observations demonstrate real-space imaging of reversible processes, such as tracking charge distributions, is feasible whilst maintaining femtosecond resolution. Our findings could find application as a characterization method, which, depending on geometry, could resolve tens of femtoseconds and tens of nanometres. Dynamically imaging electric and magnetic fields and charge distributions on sub-micron length scales opens new avenues of ultrafast dynamics. Furthermore, through the use of active compression, such pulses are an ideal seed for few-femtosecond to attosecond imaging applications which will access sub-optical cycle processes in nanoplasmonics.

Thermomechanical discrete dislocation–transformation model of single-crystal shape memory alloy

The interaction between martensitic phase transformation and plastic deformation affects the response of shape memory alloys (SMAs) during cyclic loading, in particular in terms of their pseudoelasticity characteristics and the shape memory effect. This interaction, which occurs at a sub-micron length scale inside single crystal grains, influences the reversibility and the actuation capacity of SMAs. In order to capture the sub-grain interactions while keeping the simulations tractable, a suitable modeling compromise between length scale resolution and computational effort is required. To this end, a model originally developed for multiphase steels assisted by transformation-induced plasticity is extended for shape memory alloys. Two new features, relevant for shape memory alloys, are introduced in the model, namely (i) the modeling of crystallographically reversible transformations and (ii) the thermal contribution in the free energy and the thermal effects on the transformation driving force. The two-dimensional model uses discrete dislocations to simulate plastic deformation due to slip and discrete regions to explicitly take into account the evolution of the martensitic phase. Through representative numerical simulations, the microscale coupling between phase transformation and plasticity is investigated with a view of elucidating (i) the effect of dislocations on the martensitic transformation, (ii) the effect of the phase transformation on dislocation slip and (iii) the interaction of both phenomena on the total reversibility of SMAs during cyclic loading. The results provide valuable information for the understanding of the interaction mechanism in shape memory alloys at the level of single crystals, which may be extended to an aggregate of grains.

All-electrical detection of spin dynamics in magnetic antidot lattices by the inverse spin Hall effect

The understanding of spin dynamics in laterally confined structures on sub-micron length scales has become a significant aspect of the development of novel magnetic storage technologies. Numerous ferromagnetic resonance measurements, optical characterization by Kerr microscopy and Brillouin light scattering spectroscopy and x-ray studies were carried out to detect the dynamics in patterned magnetic antidot lattices. Here, we investigate Oersted-field driven spin dynamics in rectangular Ni80Fe20/Pt antidot lattices with different lattice parameters by electrical means and compare them to micromagnetic simulations. When the system is driven to resonance, a dc voltage across the length of the sample is detected that changes its sign upon field reversal, which is in agreement with a rectification mechanism based on the inverse spin Hall effect. Furthermore, we show that the voltage output scales linearly with the applied microwave drive in the investigated range of powers. Our findings have direct implications on the development of engineered magnonics applications and devices.

Nanochemo-mechanical signature of organic-rich shales: a coupled indentation–EDX analysis

The organic–inorganic nature of organic-rich source rocks poses several challenges for the development of functional relations that link mechanical properties with geochemical composition. With this focus in mind, we herein propose a method that enables chemo-mechanical characterization of this highly heterogeneous source rock at the micron and submicron length scale through a statistical analysis of a large array of energy-dispersive X-ray spectroscopy (EDX) data coupled with nanoindentation data. The ability to include elemental composition to the indentation probe via EDX is shown to provide a means to identify pure material phases, mixture phases, and interfaces between different phases. Employed over a large array, the statistical clustering of this set of chemo-mechanical data provides access to the properties of the fundamental building blocks of clay-dominated organic-rich source rocks. The versatility of the approach is illustrated through the application to a large number of source rocks of different origin, chemical composition, and organic content. We find that the identified properties exhibit a unique scaling relation between stiffness and hardness. This suggests that organic-rich shale properties can be reduced to their elementary constituents, with several implications for the development of predictive functional relations between chemical composition and mechanical properties of organic-rich source rocks such as the intimate interplay between clay-packing, organic maturity, and mechanical properties of porous clay/organic phase.

Surface Plasmon Polariton Graphene Photodetectors.

The combination of plasmonic nanoparticles and graphene enhances the responsivity and spectral selectivity of graphene-based photodetectors. However, the small area of the metal-graphene junction, where the induced electron-hole pairs separate, limits the photoactive region to submicron length scales. Here, we couple graphene with a plasmonic grating and exploit the resulting surface plasmon polaritons to deliver the collected photons to the junction region of a metal-graphene-metal photodetector. This gives a 400% enhancement of responsivity and a 1000% increase in photoactive length, combined with tunable spectral selectivity. The interference between surface plasmon polaritons and the incident wave introduces new functionalities, such as light flux attraction or repulsion from the contact edges, enabling the tailored design of the photodetector's spectral response. This architecture can also be used for surface plasmon biosensing with direct-electric-redout, eliminating the need of bulky optics.

Fractal Characterization of Chromatin Decompaction in Live Cells

Chromatin organization has a fundamental impact on the whole spectrum of genomic functions. Quantitative characterization of the chromatin structure, particularly at submicron length scales where chromatin fractal globules are formed, is critical to understanding this structure-function relationship. Such analysis is currently challenging due to the diffraction-limited resolution of conventional light microscopy. We herein present an optical approach termed inverse spectroscopic optical coherence tomography to characterize the mass density fractality of chromatin, and we apply the technique to observe chromatin decompaction in live cells. The technique makes it possible for the first time, to our knowledge, to sense intracellular morphology with length-scale sensitivity from ∼30 to 450 nm, thus primarily probing the higher-order chromatin structure, without resolving the actual structures. We used chromatin decompaction due to inhibition of histone deacytelases and measured the subsequent changes in the fractal dimension of the intracellular structure. The results were confirmed by transmission electron microscopy and confocal fluorescence microscopy.

In Situ TEM Nanoindentation Studies on Stress-Induced Phase Transformations in Metallic Materials

Although abundant phase transformations are in general thermally driven processes, there are many examples wherein stresses can induce phase transformations. Numerous in situ techniques, such as in situ x-ray diffraction and neutron diffraction, have been applied to reveal phase transformations. Recently, an in situ nanoindentation technique coupled with transmission electron microscopy demonstrated the capability to directly correlating stresses with phase transformations and microstructural evolutions at a submicron length scale. Here we briefly review in situ studies on stress-induced diffusional and diffusionless phase transformations in amorphous CuZrAl alloy and NiFeGa shape memory alloy. In the amorphous CuZrAl, in situ nanoindentation studies show that the nucleation of nanocrystals (a diffusional process) occurs at ultra-low stresses manifested by a prominent stress drop. In the NiFeGa shape memory alloy, two distinctive types of martensitic (diffusionless) phase transformations accompanied by stress plateaus are observed, including a reversible gradual phase transformation at low stress levels, and an irreversible abrupt phase transition at higher stress levels.

Age-related changes in the fracture resistance of male Fischer F344 rat bone

In addition to the loss in bone volume that occurs with age, there is a decline in material properties. To test new therapies or diagnostic tools that target such properties as material strength and toughness, a pre-clinical model of aging would be useful in which changes in bone are similar to those that occur with aging in humans. Toward that end, we hypothesized that similar to human bone, the estimated toughness and material strength of cortical bone at the apparent-level decreases with age in the male Fischer F344 rat. In addition, we tested whether the known decline in trabecular architecture in rats translated to an age-related decrease in vertebra (VB) strength and whether non-X-ray techniques could quantify tissue changes at micron and sub-micron length scales. Bones were harvested from 6-, 12-, and 24-month (mo.) old rats (n=12 per age). Despite a loss in trabecular bone with age, VB compressive strength was similar among the age groups. Similarly, whole-bone strength (peak force) in bending was maintained (femur) or increased (radius) with aging. There was though an age-related decrease in post-yield toughness (radius) and bending strength (femur). The ability to resist crack initiation was actually higher for the 12-mo. and 24-mo. than for 6-mo. rats (notch femur), but the estimated work to propagate the crack was less for the aged bone. For the femur diaphysis region, porosity increased while bound water decreased with age. For the radius diaphysis, there was an age-related increase in non-enzymatic and mature enzymatic collagen crosslinks. Raman spectroscopy analysis of embedded cross-sections of the tibia mid-shaft detected an increase in carbonate subsitution with advanced aging for both inner and outer tissue.