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Matthew Mecklenburg

Publications and source records attributed to Matthew Mecklenburg.

16 recordsLinked to original sources

An Improved Paralyzable Detector Model

Certain radiation detectors are 'paralyzed' with high input count rates. When applied to count rates close to the event discriminator working rate the one-parameter dead time model fails. Here we present a corrected paralyzable detector model accounting for the event discriminator's finite response time. This two-parameter analytical model, when compared to the experimental data from a commercial x-ray detector, gives an improved description of the input and output count rate relations. Furthermore, it can independently determine the discriminator response time and the pulse shaper dead time, critical parameters for understanding a detector's performance. Finally, this model also provides a post-acquisition pile-up correction that greatly reduces artifacts in high-throughput spectra. In some situations, applying this model to optimize the acquisition and post-acquisition correction allows a user to acquire data an order of magnitude faster without compromising accuracy.

physics.ins-det

Mapping Temperature Using Transmission Kikuchi Diffraction

Electronic devices are engineered at increasingly smaller length scales; new metrologies to understand nanoscale thermodynamics are needed. Temperature and pressure are fundamental thermodynamic quantities whose nanoscale measurement is challenging as physical contact inevitably perturbs the system. Here we demonstrate Kikuchi diffraction thermometry (KDTh), a non-contact scanning electron microscope (SEM) technique capable of mapping nanoscale temperatures and pressures. KDTh detects local volumetric lattice changes in crystalline samples by precisely fitting Kikuchi patterns. Temperature changes are deduced using the coefficient of thermal expansion (CTE). We map lattice parameters and temperatures on Joule-heated graphite by rastering a 5.5-nm electron probe across the sample. Our parameter precision is ~0.01% and our temperature sensitivity is 2.2 K/$\sqrt{Hz}$. KDTh offers advanced sensitivity by fitting the entire Kikuchi pattern, even beyond the precision measured in transmission electron microscopy. KDTh can operate in both transmission (transmission Kikuchi diffraction, TKD) and reflection (electron backscatter diffraction, EBSD) modes.

cond-mat.mes-hall

Modification of the scattering mechanisms in bilayer graphene in proximity to a molecular thin film probed in the mesoscopic regime

Quantum coherent effects can be probed in multilayer graphene through electronic transport measurements at low temperatures. In particular, bilayer graphene is known to be susceptible to quantum interference corrections of the conductivity, presenting weak localization at all electronic densities, and dependent on different scattering mechanisms as well as on the trigonal warping of the electron dispersion near the K and K' valleys. Proximity effects with a molecular thin film influence these scattering mechanisms, which can be quantified through the known theory of magnetoconductance for bilayer graphene. Here, we present weak localization measurements in a copper-phthalocyanine / bilayer graphene / h-BN heterostructure that suggest an important suppression of trigonal warping effects in bilayer graphene (BLG), restoring the manifestation of the chirality of the charge carriers in the localization properties of BLG. Additionally, we observe a charge transfer of 3.6$\times$10$^{12}$cm$^{-2}$ from the BLG to the molecules, as well as a very small degradation of the mobility of the BLG/h-BN heterostructure upon the deposition of copper phthalocyanine (CuPc). The molecular arrangement of the CuPc thin film is characterized in a control sample through transmission electron microscopy, that we relate to the electronic transport results.

cond-mat.mes-hall

Measuring Chemical Shifts with Energy-Dispersive X-ray Spectroscopy

Electron microscopy prevalently uses energy-dispersive x-ray spectroscopy (EDS) and electron energy loss spectroscopy (EELS) for elemental analysis. EDS and EELS energy resolutions are commonly between 30-100 eV or 0.01-1 eV, respectively. Large solid angle EDS detector technology has increased collection efficiency to enable precision spectroscopy via averaging of 0.02-0.1 eV. This improved precision gives access to chemical shifts; examples are shown in compounds of Al, Ti, and W. EDS can now detect chemical information in a complementary parameter space (accelerating voltage, thickness, atomic number) to that covered by EELS.

cond-mat.mtrl-sci

Mapping electron beam-induced radiolytic damage in molecular crystals

Every electron crystallography experiment is fundamentally limited by radiation damage. Nevertheless, little is known about the onset and progression of radiolysis in beam-sensitive molecular crystals. Here we apply ambient-temperature scanning nanobeam electron diffraction to record simultaneous dual-space snapshots of organic and organometallic nanocrystals at sequential stages of beam-induced radiolytic decay. We show that the underlying mosaic of coherently diffracting zones (CDZs) continuously undergoes spatial reorientation as a function of accumulating electron exposure, causing the intensities of many Bragg reflections to fade nonmonotonically. Furthermore, we demonstrate that repeated irradiation at a single probe position leads to the concentric propagation of delocalized radiolytic damage well beyond the initial point of impact. These results sharpen our understanding of molecular crystals as conglomerates of CDZs whose complex lattice structure deteriorates through a series of dynamic internal changes during exposure to ionizing radiation.

cond-mat.mtrl-sci

Mapping Charge Recombination and the Effect of Point Defect Insertion in Gallium Arsenide Nanowire Heterojunctions

Electronic devices are extremely sensitive to defects in their constituent semiconductors, but locating electronic point defects in bulk semiconductors has previously been impossible. Here we apply scanning transmission electron microscopy (STEM) electron beam-induced current (EBIC) imaging to map electronic defects in a GaAs nanowire Schottky diode. Imaging with a non-damaging 80 or 200 kV STEM acceleration potential reveals a minority-carrier diffusion length that decreases near the surface of the hexagonal nanowire, thereby demonstrating that the device's charge collection efficiency (CCE) is limited by surface defects. Imaging with a 300 keV STEM beam introduces vacancy-interstitial (VI, or Frenkel) defects in the GaAs that increase carrier recombination and reduce the CCE of the diode. We create, locate, and characterize a single insertion event, determining that a defect inserted 7 nm from the Schottky interface broadly reduces the CCE by 10% across the entire nanowire device. Variable-energy STEM EBIC imaging thus allows both benign mapping and pinpoint modification of a device's e-h recombination landscape, enabling controlled experiments that illuminate the impact of both extended (1D and 2D) and point (0D) defects on semiconductor device performance.

cond-mat.mes-hall

Tunable Thermal Energy Transport across Diamond Membranes and Diamond-Si Interfaces by Nanoscale Graphoepitaxy

The development of electronic devices, especially those that involve heterogeneous integration of materials, has led to increased challenges in addressing their thermal operational-temperature demands. The heat flow in these systems is significantly influenced or even dominated by thermal boundary resistance at interface between dissimilar materials. However, controlling and tuning heat transport across an interface and in the adjacent materials has so far drawn limited attention. In this work, we grow chemical-vapor-deposited (CVD) diamond on silicon substrates by graphoepitaxy and experimentally demonstrate tunable thermal transport across diamond membranes and diamond-silicon interfaces. We observed the highest diamond-silicon thermal boundary conductance (TBC) measured to date and increased diamond thermal conductivity due to strong grain texturing in the diamond near the interface. Additionally, non-equilibrium molecular-dynamics (NEMD) simulations and a Landauer approach are used to understand the diamond-silicon TBC. These findings pave the way for tuning or increasing thermal conductance in heterogeneously integrated electronics that involve polycrystalline materials and will impact applications including electronics thermal management and diamond growth.

cond-mat.mes-hall

Thermometry of Silicon Nanoparticles

Current thermometry techniques lack the spatial resolution required to see the temperature gradients in typical, highly-scaled modern transistors. As a step toward addressing this problem, we have measured the temperature dependence of the volume plasmon energy in silicon nanoparticles from room temperature to 1250$^\circ$C, using a chip-style heating sample holder in a scanning transmission electron microscope (STEM) equipped with electron energy loss spectroscopy (EELS). The plasmon energy changes as expected for an electron gas subject to the thermal expansion of silicon. Reversing this reasoning, we find that measurements of the plasmon energy provide an independent measure of the nanoparticle temperature consistent with that of the heater chip's macroscopic heater/thermometer to within the 5\% accuracy of the chip thermometer's calibration. Thus silicon has the potential to provide its own, high-spatial-resolution thermometric readout signal via measurements of its volume plasmon energy. Furthermore, nanoparticles in general can serve as convenient nanothermometers for \emph{in situ} electron microscopy experiments.

cond-mat.mes-hall

Impedance matching of inverted conductors: Two-dimensional beam splitters with divergent gain

A thin conducting sheet - graphene, for example - transmits, absorbs, and reflects radiation. A sheet that is very thin, even vanishingly so, can still produce 50% absorption at normal incidence if it has conductivity corresponding to half the impedance of free space. We find that, regardless of the sheet conductivity, there exists a combination of polarization and angle of incidence that achieves this impedance half-matching condition. If the conducting medium can be inverted, the conductivity is formally negative and the sheet amplifies the incident radiation. To the extent that a negative half-match in a thin sheet can be maintained, enormous single-pass gain in both transmission and reflection is possible. Known semiconductors (e.g., gallium nitride) have the optical properties necessary to give large amplification in a structure that is, remarkably, both thin and nonresonant.

cond-mat.mes-hall

Single-color pyrometry of individual incandescent multiwalled carbon nanotubes

Objects that are small compared to their thermal photon wavelengths violate the assumptions underlying optical pyrometry and can show unusual coherence effects. To investigate this regime we measure the absolute light intensity from individual, incandescent multiwalled carbon nanotubes. The nanotube filaments' physical dimensions and composition are determined using transmission electron microscopy and their emissivities are calculated in terms of bulk conductivities. A single-color pyrometric analysis then returns a temperature value for each wavelength, polarization, and applied bias measured. Compared to the more common multiwavelength analysis, single-color pyrometry supports a more consistent and complete picture of the carbon nanotube lamps, one that describes their emissivity, optical conductivity, and thermal conductivity in the range 1600-2400 K.

cond-mat.mes-hall

Dark-field transmission electron microscopy and the Debye-Waller factor of graphene

Graphene's structure bears on both the material's electronic properties and fundamental questions about long range order in two-dimensional crystals. We present an analytic calculation of selected area electron diffraction from multi-layer graphene and compare it with data from samples prepared by chemical vapor deposition and mechanical exfoliation. A single layer scatters only 0.5% of the incident electrons, so this kinematical calculation can be considered reliable for five or fewer layers. Dark-field transmission electron micrographs of multi-layer graphene illustrate how knowledge of the diffraction peak intensities can be applied for rapid mapping of thickness, stacking, and grain boundaries. The diffraction peak intensities also depend on the mean-square displacement of atoms from their ideal lattice locations, which is parameterized by a Debye-Waller factor. We measure the Debye-Waller factor of a suspended monolayer of exfoliated graphene and find a result consistent with an estimate based on the Debye model. For laboratory-scale graphene samples, finite size effects are sufficient to stabilize the graphene lattice against melting, indicating that ripples in the third dimension are not necessary.

cond-mat.mes-hall

Electron tomography at 2.4 Å resolution

Transmission electron microscopy (TEM) is a powerful imaging tool that has found broad application in materials science, nanoscience and biology(1-3). With the introduction of aberration-corrected electron lenses, both the spatial resolution and image quality in TEM have been significantly improved(4,5) and resolution below 0.5 Å has been demonstrated(6). To reveal the 3D structure of thin samples, electron tomography is the method of choice(7-11), with resolutions of ~1 nm^3 currently achievable(10,11). Recently, discrete tomography has been used to generate a 3D atomic reconstruction of a silver nanoparticle 2-3 nm in diameter(12), but this statistical method assumes prior knowledge of the particle's lattice structure and requires that the atoms fit rigidly on that lattice. Here we report the experimental demonstration of a general electron tomography method that achieves atomic scale resolution without initial assumptions about the sample structure. By combining a novel projection alignment and tomographic reconstruction method with scanning transmission electron microscopy, we have determined the 3D structure of a ~10 nm gold nanoparticle at 2.4 Å resolution. While we cannot definitively locate all of the atoms inside the nanoparticle, individual atoms are observed in some regions of the particle and several grains are identified at three dimensions. The 3D surface morphology and internal lattice structure revealed are consistent with a distorted icosahedral multiply-twinned particle. We anticipate that this general method can be applied not only to determine the 3D structure of nanomaterials at atomic scale resolution(13-15), but also to improve the spatial resolution and image quality in other tomography fields(7,9,16-20).

cond-mat.mtrl-sci

Polarized light emission from individual incandescent carbon nanotubes

We fabricate nanoscale lamps which have a filament consisting of a single multiwalled carbon nanotube. After determining the nanotube geometry with a transmission electron microscope, we use Joule heating to bring the filament to incandescence, with peak temperatures in excess of 2000 K. We image the thermal light in both polarizations simultaneously as a function of wavelength and input electrical power. The observed degree of polarization is typically of the order of 75%, a magnitude predicted by a Mie model of the filament that assigns graphene's optical conductance $πe^2/2 h$ to each nanotube wall.

cond-mat.mes-hall

Spin and the Honeycomb Lattice: Lessons from Graphene

Spin-1/2 particles such as the electron are described by the Dirac equation, which allows for two spin eigenvalues (up or down) and two types of energy eigenvalues (positive or negative, corresponding to the electron and the positron). A model of electrons hopping from atom to atom in graphene's honeycomb lattice gives low-energy electronic excitations that obey a relation formally identical to a 2+1 dimensional Dirac equation. Graphene's spin equivalent, "pseudospin", arises from the degeneracy introduced by the honeycomb lattice's two inequivalent atomic sites per unit cell. Previously it has been thought that the usual electron spin and the pseudospin indexing the graphene sublattice state are merely analogues. Here we show that the pseudospin is also a real angular momentum. This identification explains the suppression of electron backscattering in carbon nanotubes and the angular dependence of light absorption by graphene. Furthermore, it demonstrates that half-integer spin like that carried by the quarks and leptons can derive from hidden substructure, not of the particles themselves, but rather of the space in which these particles live.

cond-mat.mes-hall

Tree-level electron-photon interactions in graphene

Graphene's low-energy electronic excitations obey a 2+1 dimensional Dirac Hamiltonian. After extending this Hamiltonian to include interactions with a quantized electromagnetic field, we calculate the amplitude associated with the simplest, tree-level Feynman diagram: the vertex connecting a photon with two electrons. This amplitude leads to analytic expressions for the 3D angular dependence of photon emission, the photon-mediated electron-hole recombination rate, and corrections to graphene's opacity $πα$ and dynamic conductivity $πe^2/2 h$ for situations away from thermal equilibrium, as would occur in a graphene laser. We find that Ohmic dissipation in perfect graphene can be attributed to spontaneous emission.

cond-mat.mes-hall

Electron Transport Driven by Nonequilibrium Magnetic Textures

Spin-polarized electron transport driven by inhomogeneous magnetic dynamics is discussed in the limit of a large exchange coupling. Electron spins rigidly following the time-dependent magnetic profile experience spin-dependent fictitious electric and magnetic fields. We show that the electric field acquires important corrections due to spin dephasing, when one relaxes the spin-projection approximation. Furthermore, spin-flip scattering between the spin bands needs to be taken into account in order to calculate voltages and spin accumulations induced by the magnetic dynamics. A phenomenological approach based on the Onsager reciprocity principle is developed, which allows us to capture the effect of spin dephasing and make a connection to the well studied problem of current-driven magnetic dynamics. A number of results that recently appeared in the literature are related and generalized.

cond-mat.mes-hall