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At least 19 records

Identification of Auger mechanisms responsible for low energy electron emission from graphene on copper using Auger-gamma coincidence spectroscopy

We have applied positron annihilation induced Auger-gamma coincidence spectroscopy to identify important mechanisms responsible for the emission of low energy electrons following the sudden creation of holes in bilayer graphene on copper substrate. The novel surface spectroscopic method measures the energy of the Doppler shifted annihilation gamma photon in coincidence with the Auger electron emitted following the relaxation of the hole created by the annihilation of a surface electron with a surface trapped positron. By extracting and theoretically modelling the annihilation gamma spectra coincident with low energy electrons, we associate majority of the intensity in the low energy (7 eV–25 eV) region of the Auger spectrum to electron emission following Auger decays of 2s holes in adsorbed oxygen and deep valence holes in graphene. We provide additional support to this conclusion by showing that most of the Auger electrons with energy less than ~ 25 eV are coincident with gamma photons with small Doppler shift (511 keV–512 keV) indicating that the primary electron whose annihilation resulted in low energy Auger electron emission had small momentum parallel to the gamma emission direction. On the other hand, majority of the Auger electrons measured in coincidence with the photons having maximum Doppler shift (515 keV–521 keV) were emitted following the decay of core holes (C 1s and O 1s). Furthermore, by selecting annihilation gamma photons coincident only with the O KVV (from surface adsorbed oxygen), C KVV (graphene), and Cu MVV (copper substrate) Auger electrons, we have also experimentally derived the energy spectrum of Doppler shifted gamma photons resulting from the annihilation of positrons with 1s electrons of O, 1s electrons of C and 3p electrons of Cu respectively. Model Doppler broadened gamma spectra produced using ab-initio calculations agree well with the experimentally derived line shapes. This demonstrates the ability of Auger-gamma coincidence method to experimentally resolve the Doppler broadened annihilation gamma spectrum from surfaces into its veiled electronic level constituents which has, heretofore, relied solely on theoretical analysis. Our results also demonstrate that the line shape of the Doppler broadened annihilation gamma peak reflect the chemical composition of the topmost atomic layer and can thus be used to characterize both external and inaccessible surfaces of porous materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The Auger Radioisotope Microscope: an instrument for characterization of Auger electron multiplicities and energy distributions

We describe a new instrument, the Argonne Auger Radioisotope Microscope (ARM), capable of characterizing the Auger electron (AE) emission of radionuclides, including candidates relevant in nuclear medicine. Our approach relies on event-by-event ion–electron coincidence, time-of-flight, and spatial readout measurement to determine correlated electron multiplicity and energy distributions of Auger decays. We present a proof-of-principle measurement with the ARM using x-ray photoionization of stable krypton beyond the K-edge and identify a bifurcation in the electron multiplicity distribution depending on the emission of K-LX electrons. Extension of the ARM to the characterization of radioactive sources of AE emissions is enabled by the combination of two recent developments: (1) cryogenic buffer gas beam technology to introduce Auger emitters into the detection region with well-defined initial conditions, and (2) large-area micro-channel plate detectors with multi-hit detection capabilities to simultaneously detect multiple electrons emitted in a single decay.

Auger emitters↗

Suppressing Auger Recombination in Multiply Excited Colloidal Silicon Nanocrystals with Ligand-Induced Hole Traps

Nonradiative Auger recombination in multiply excited nanocrystals is a dominant efficiency loss pathway for nanocrystal-containing optoelectronic devices that rely on high-rate emission and absorption operating conditions. Overcoming Auger recombination in these quantum-confined systems is therefore a longstanding challenge to the synthetic nanocrystal as well as device manufacturing communities. Several successful strategies have been realized to reduce Auger recombination, but they rely on complex and time-consuming nanocrystal core/shell synthesis. Alternatively, controlling Auger rates by varying the nanocrystal–ligand-binding chemistry is a promising route to obtain functional tunability, which reduces the barrier to large-scale manufacturing. The covalent surface chemistry and the extremely long-lived photoexcited lifetimes of silicon nanocrystals (Si NCs) make them a unique system among colloidal semiconductor NCs to study the intersection between surface chemistry and photoexcited carrier dynamics. Here, we show that changing the functional group that binds a saturated dodecyl ligand to the surface of nonthermal plasma-synthesized Si NCs from alkyl to thiolate slows Auger recombination rates within multiply excited Si NCs. This reduction in Auger rate persists across Si NC sizes ranging from 3.5 to 8 nm in diameter, but the expected linear dependence of Auger rates on the NC volume is retained for both alkyl and alkylthiolate surface terminations. To understand the origin behind this elongation, we carry out steady-state and time-resolved photoluminescence measurements as well as time-resolved terahertz spectroscopy measurements. These measurements reveal that thiolate groups introduce mid-gap surface states, which, we argue, reduces the photoexcited electron–hole overlap and elongates Auger recombination times. These results highlight how a typically detrimental chemical species—mid-band gap NC surface states—can be beneficial under high-rate absorption/emission conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Auger electron angular distributions following excitation or ionization from the Xe 3d and F 1s levels in xenon difluoride

Linearly polarized synchrotron radiation has been used to record polarization dependent, non-resonant Auger electron spectra of XeF 2 , encompassing the bands due to the xenon M 45 N 1 N 45 , M 45 N 23 N 45 , M 45 N 45 N 45 and M 45 N 45 V and fluorine KVV transitions. Resonantly excited Auger spectra have been measured at photon energies coinciding with the Xe 3d 5/2 → σ* and the overlapped Xe 3d 3/2 /F 1s → σ* excitations in XeF 2 . The non-resonant and resonantly excited spectra have enabled the Auger electron angular distributions, as characterized by the β A parameter, to be determined for the M 45 N 45 N 45 transitions. In the photon energy range over which the Auger electron angular distributions were measured, theoretical results indicate that transitions into the εf continuum channel dominate the Xe 3d photoionization in XeF 2 . In this limit, the theoretical value of the atomic alignment parameter (A 20 ) characterizing the core ionized state becomes constant. This theoretical value has been used to obtain the Auger electron intrinsic anisotropy parameters (α 2 ) from the β A parameters extracted from our non-resonant Auger spectra. For a particular Auger transition, the electron kinetic energy measured in the resonantly excited spectrum is higher than that in the directly ionized spectrum, due to the screening provided by the electron promoted into the σ* orbital. The interpretation of the F KVV Auger band in XeF 2 has been discussed in relation to previously published one-site populations of the doubly charged ions (XeF 2 2+ ). Here, the experimental results show that the ionization energies of the doubly charged states predominantly populated in the decay of a vacancy in the F 1s orbital in XeF 2 tend to be higher than those populated in the decay of a vacancy in the Xe 4d level in XeF 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Anomalous Auger Recombination in PbSe

Using first-principles approaches we find that the Auger recombination in PbSe is anomalous in three distinct ways. First, the direct Auger coefficient is 4 orders of magnitude lower than that of other semiconductors with similar band gaps, a result that can be attributed to the lack of involvement of a heavy-hole band. Second, phonon-assisted indirect Auger recombination prevails, contrary to the common belief that direct Auger is dominant in narrow-gap semiconductors. Third, an unexpectedly weak temperature dependence of the Auger coefficient is observed, which we can now attribute to the indirect nature of the Auger process. The widely accepted explanation of this behavior in terms of an unusual temperature dependence of the band gap is only a secondary effect. Furthermore, our results elucidate the mechanisms underlying the anomalous Auger recombination in IV-VI semiconductors in general, which is critical for understanding and engineering carrier transport.

36 MATERIALS SCIENCE↗

Auger@TA: In-situ Cross-Calibration of the World's Largest Cosmic Ray Observatories

The Pierre Auger Observatory (Auger) and the Telescope Array (TA) are the world's two largest ultra-high-energy cosmic ray (UHECR) observatories. They operate in the Southern and Northern hemispheres, respectively, at similar latitudes but with distinct surface detector (SD) designs. A significant challenge in studying UHECR physics across the full sky is the apparent discrepancy in flux measurements between the two experiments. This discrepancy could arise from astrophysical differences and/or systematic effects related to their detector designs and sensitivities to extensive air shower components. To address this, the Auger@TA working group aims to cross-calibrate the two observatories with a self-triggering micro-Auger array within the TA array. This micro-array consists of eight Auger Surface Detector (SD) stations equipped with Water Cherenkov Detectors (WCDs) and AugerPrime Surface Scintillator Detectors. Seven SD stations, configured with a centered-1-PMT design, are arranged in a hexagonal pattern with one station in the center, with 1.5 km spacing, mirroring the Auger layout. The eighth station, which features a standard 3-PMT Auger station, is located in conjunction with a TA detector at the center of the hexagon, forming a triplet for high-statistics and low-uncertainty cross-calibration. A custom communication system that uses readily available components enables seamless communication between stations and remote access to each station through a central computer. The micro-array is now fully deployed, and initial data-taking is about to start. This presentation will detail the instrumentation, communication systems, central data acquisition system, expected performance of the micro-array, and preliminary results as appropriate.

Mocellin, Adriel G.B. [Colorado School of Mines]↗

Monolayer Semiconductor Auger Detector

Auger recombination in semiconductors is a many-body phenomenon in which the recombination of electrons and holes is accompanied by excitation of other charge carriers. The excess energy of the excited carriers is normally rapidly converted to heat, making Auger processes difficult to probe directly. In this paper, we employ a technique in which the Auger-excited carriers are detected by their ability to tunnel out of the semiconductor through a thin barrier, generating a current. We use vertical van der Waals heterostructures with monolayer WSe 2 as the semiconductor, with hexagonal boron nitride as the tunnel barrier, and a graphite collector electrode. The Auger processes combined with resonant absorption produce characteristic negative photoconductance. We detect holes Auger-excited by both neutral and charged excitons and find that the Auger scattering is surprisingly strong under weak excitation. Our work expands the range of techniques available for probing relaxation processes in 2D materials.

47 OTHER INSTRUMENTATION↗

Clocking Auger electrons

Intense X-ray free-electron lasers (XFELs) can rapidly excite matter, leaving it in inherently unstable states that decay on femtosecond timescales. The relaxation occurs primarily via Auger emission, so excited-state observations are constrained by Auger decay. In situ measurement of this process is therefore crucial, yet it has thus far remained elusive in XFELs owing to inherent timing and phase jitter, which can be orders of magnitude larger than the timescale of Auger decay. Here we develop an approach termed ‘self-referenced attosecond streaking’ that provides subfemtosecond resolution in spite of jitter, enabling time-domain measurement of the delay between photoemission and Auger emission in atomic neon excited by intense, femtosecond pulses from an XFEL. FUrthermore, using a fully quantum-mechanical description that treats the ionization, core-hole formation and Auger emission as a single process, the observed delay yields an Auger decay lifetime of \(2.2_{ - 0.3}^{ + 0.2}\) fs for the KLL decay channel.

47 OTHER INSTRUMENTATION↗

New methods for image collection and analysis in scanning Auger microscopy

While scanning Auger micrographs are used extensively for illustrating the stoichiometry of complex surfaces and for indicating areas of interest for fine point Auger spectroscopy, there are many problems in the quantification and analysis of Auger images. These problems include multiple contrast mechanisms and the lack of meaningful relationships with other Auger data. Collection of multielemental Auger images allows some new approaches to image analysis and presentation. Information about the distribution and quantity of elemental combinations at a surface are retrievable, and particular combinations of elements can be imaged, such as alloy phases. Results from the precipitate hardened alloy Al-2124 illustrate multispectral Auger imaging.

Browning, R.↗

Binary collision model for neon Auger spectra from neon ion bombardment of the aluminum surface

A model is developed to account for the angle-resolved Auger spectra from neon ion bombardment of the aluminum surface recently obtained by Pepper and Aron. The neon is assumed to be excited in a single asymmetric neon-aluminum-collision and scattered back into the vacuum where it emits an Auger electron. The velocity of the Auger electron acquires a Doppler shift by virtue of the emission from a moving source. The dependence of the Auger peak shape and energy on the incident ion energy, angle of incidence and on the angle of Auger electron emission with respect to the surface is presented. Satisfactory agreement with the angle resolved experimental observations is obtained. The dependence of the angle-integrated Auger yield on the incident ion energy and angle of incidence is also obtained and shown to be in satisfactory agreement with available experimental evidence.

Pepper, S. V.↗

Design of a rotary stepped auger for a lunar environment

A lunar outpost will have need for deep drilling operations for both explorative and practical purposes. As in any drilling operation, the cuttings must be cleared from the hole. The hard vacuum of the lunar environment renders conventional flushing methods of cutting removal unfeasible, and requires a new system of removal. A rotary stepped auger (RSA) is a simple mechanical method of removing dry cuttings from a deep hole, and is ideally suited to the lunar environment. The RSA consists of a helical auger with stepped ramps which allow cuttings to slide up the helix, but will prevent them from sliding back down. The auger is driven in a pulsed manner by applying a periodic function of acceleration to the auger shaft. These pulses will compel the cuttings to slide up the auger's helix while the stepped ramps prevent the cuttings from backsliding while the auger accelerates. A mathematical model of the RSA was developed and experimentally evaluated. The math model produced a good baseline design, but the experimental model required some tuning to account for the approximations made in the math model. This design is suited for lunar drilling because it is mechanically simple, integral to the drill string, requires no fluids, is suited to the dry soil, and has relatively low weight and power requirements.

Dardet, Eduardo↗

Auger electron intensity variations in oxygen-charged silver

Auger intensity variations over an oxygen-charged polycrystalline silver surface have been observed by studies of Auger images and line scans of selected adjacent grains which were determined to be the (421) and (221) orientations. The observed contrast (M4.5VV transition) between the grains is produced by the variation in the detected Auger electrons caused by the different directions (interatomic direction) of forward focusing in each grain. The contrast produced by the Ag Auger electrons was found to be strongly dependent on the surface order of the grains, but that of the O Auger electrons was not, presumably because the atoms were randomly distributed throughout the Ag surface or subsurface. The contrast observed between the grains at the lower Auger energies (N1VV and N1N2.3V transitions) appeared to be produced by constructive interference from multiple scattering. The N1N2.3V electrons at 29 eV, for example, gave higher contrast than that of the N1VV transition at 78 eV.

Lee, W. S.↗

Auger Dynamics in InP/ZnSe/ZnS Quantum Dots Having Pure and Doped Shells

In this study, we report the negative trion and biexciton Auger dynamics in very high-quality InP/ZnSe/ZnS quantum dots (QDs) having varying amounts of indium-based traps in the ZnSe shell. Negative trion times are determined by time-correlated photon-counting measurements on QDs that have been photoreduced with lithium triethylborohydride. We find that the Auger times vary from 280 to 425 ps and scale linearly with the total particle volume. Excess indium in the ZnSe shell gives rise to hole traps that are transiently populated following photoexcitation. Comparing stoichiometric and nonstoichiometric particles, we find that the negative trion lifetimes are independent of the presence of indium in the ZnSe shell. Biexciton dynamics are determined from transient absorption (TA) bleach recovery measurements. Absorption of two photons results in the formation of two types of biexcitons: those having both holes in the InP core (XX state) and those having one hole trapped in the ZnSe shell (XT state). XX state Auger times are measured in stoichiometric QDs, and for these particles, the Auger times are ~80 ps. Nonstoichiometric QDs show an additional long TA decay component, assigned to Auger recombination of the XT state. Here, a previous study (J. Phys. Chem. C 2021, 125, 4110–4118) found that hole trapping at indium-based shell traps results in a slow photoluminescence (PL) rise component. We find that the fraction of the XT state formed by the absorption of two photons correlates with the product of the fraction of slow PL rise and the rise time constant following one-photon excitation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Self-Trapped-Exciton Radiative Recombination in β–Ga 2 O 3 : Impact of Two Concurrent Nonradiative Auger Processes

The peculiarities of radiative and nonradiative processes associated with self-trapped intrinsic eXcitons in the excited β-Ga 2 O 3 crystals are studied via time-resolved techniques of induced absorption, transient grating, and photoluminescence (PL) at room temperature. The excitation above the bandgap is produced by laser pulses with linear light polarization parallel and orthogonal in the (–201) and (001) planes. We elucidate that the nonradiative recombination rate occurring in the eXciton prevails over its radiative emission rate in a wide range of free carrier concentration composed of excited and equilibrium electrons. Hence, the nonradiative recombination has no effect on the strong anisotropy and the shape of the eXciton emission band. However, we find out that the conventional ABC model of electron effective lifetime is insufficient for explanation of the excitation dependences. Inclusion of two nonradiative Auger mechanisms in a modified ABC formula provides excellent agreement of these dependences. We conclude that the trap-assisted Auger process is in proportion to the free electron density with coefficient B = 1.1 × 10 –11 cm 3 /s and appears at low/intermediate excitation, while the triple-particle Auger process is in proportion to Δn 2 with coefficient C = 8 × 10 –30 cm 6 /s and appears at high excitation conditions. The transition between two Auger mechanisms is accompanied by a rise of the eXciton diffusivity in preferred crystallographic directions where the radiative PL intensity is maximal. The diffusion length LD in these directions can reach values ~300 nm, but, at high excitations, LD becomes limited by Auger lifetimes. These findings pave the way for the implementation of self-trapped eXcitons into specific optoelectronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influence of trap-assisted and intrinsic Auger–Meitner recombination on efficiency droop in green InGaN/GaN LEDs

Here, we study the impact of deep-level defects on trap-assisted Auger–Meitner recombination in c-plane InGaN/GaN LEDs using a small-signal electroluminescence (SSEL) method and deep-level optical spectroscopy (DLOS). Carrier dynamics information, including carrier lifetime, recombination rate, and carrier density, is obtained from SSEL, while DLOS is used to obtain the deep-level defect density. Through fitting the nonradiative recombination rates of wafers with different deep-level defect densities, we obtain the Shockley–Read–Hall (SRH) and trap-assisted Auger–Meitner recombination (TAAR) coefficients. We show that defect-related nonradiative recombination, including both SRH and TAAR, accounts for a relatively small fraction of the total nonradiative recombination, which is dominated by intrinsic Auger–Meitner recombination. The interplay between carrier localization and Coulomb enhancement has a different impact on radiative and intrinsic Auger–Meitner recombination. Evidence is presented that the imbalance between the change of radiative and intrinsic Auger–Meitner recombination is the primary cause of the efficiency droop at high carrier densities in the samples studied.

36 MATERIALS SCIENCE↗