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DOE OSTI2019

Microbial electron uptake in microbial electrosynthesis: a mini-review

Abstract Microbial electron uptake (EU) is the biological capacity of microbes to accept electrons from electroconductive solid materials. EU has been leveraged for sustainable bioproduction strategies via microbial electrosynthesis (MES). MES often involves the reduction of carbon dioxide to multi-carbon molecules, with electrons derived from electrodes in a bioelectrochemical system. EU can be indirect or direct. Indirect EU-based MES uses electron mediators to transfer electrons to microbes. Although an excellent initial strategy, indirect EU requires higher electrical energy. In contrast, the direct supply of cathodic electrons to microbes (direct EU) is more sustainable and energy efficient. Nonetheless, low product formation due to low electron transfer rates during direct EU remains a major challenge. Compared to indirect EU, direct EU is less well-studied perhaps due to the more recent discovery of this microbial capability. This mini-review focuses on the recent advances and challenges of direct EU in relation to MES.

Biotechnology & Applied Microbiology↗

DOE OSTI2018

A flavin-based extracellular electron transfer mechanism in diverse Gram-positive bacteria

Extracellular electron transfer (EET) describes microbial bioelectrochemical processes in which electrons are transferred from the cytosol to the exterior of the cell. Mineral-respiring bacteria use elaborate haem-based electron transfer mechanisms but the existence and mechanistic basis of other EETs remain largely unknown. Here we show that the food-borne pathogen Listeria monocytogenes uses a distinctive flavin-based EET mechanism to deliver electrons to iron or an electrode. By performing a forward genetic screen to identify L. monocytogenes mutants with diminished extracellular ferric iron reductase activity, we identified an eight-gene locus that is responsible for EET. This locus encodes a specialized NADH dehydrogenase that segregates EET from aerobic respiration by channelling electrons to a discrete membrane-localized quinone pool. Other proteins facilitate the assembly of an abundant extracellular flavoprotein that, in conjunction with free-molecule flavin shuttles, mediates electron transfer to extracellular acceptors. This system thus establishes a simple electron conduit that is compatible with the single-membrane structure of the Gram-positive cell. Activation of EET supports growth on non-fermentable carbon sources, and an EET mutant exhibited a competitive defect within the mouse gastrointestinal tract. Orthologues of the genes responsible for EET are present in hundreds of species across the Firmicutes phylum, including multiple pathogens and commensal members of the intestinal microbiota, and correlate with EET activity in assayed strains. These findings suggest a greater prevalence of EET-based growth capabilities and establish a previously underappreciated relevance for electrogenic bacteria across diverse environments, including host-associated microbial communities and infectious disease.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2018

Extended Electronic Structure Inhomogeneity Created by Double Chain Layer Defects Surrounding Columnar Tracks in Heavy-Ion Irradiated YBa{sub 2}Cu{sub 3}O{sub 7-{delta}}.

In YBa2Cu3O7-delta (YBCO), heavy-ion irradiation creates continuous amorphous tracks that are highly effective for vortex pinning. However, the electronic structure landscape of defects and consequently their vortex pinning roles are unclear. Here, we show double chain layer (DCL) defects which intersect the columnar tracks are additionally produced by high energy Pb ion irradiation in YBCO. The DCL defects are similar to 29 nm long, about three times the columnar defect diameter. The electronic structures of the DCL and columnar track defects were determined using atomic-resolution scanning transmission electron microscopy (STEM) and high resolution electron energy loss spectroscopy (EELS). Results show a decrease in the oxygen and copper content at the interface between the track and the YBCO matrix, resulting in interfacial strain. For the DCL defects, the STEM/EELS study revealed a localized electron doped CuO2 plane next to the DCL defect. The DCL defects thus further extend the electronic inhomogeneity into YBCO.

critical current↗

DOE OSTI2018

Measurements of the effective electron density in an electron beam ion trap using extreme ultraviolet spectra and optical imaging

In an electron beam ion trap (EBIT), the ions are not confined to the electron beam, but rather oscillate in and out of the beam. As a result, the ions do not continuously experience the full density of the electron beam. To determine the effective electron density, n e,eff , experienced by the ions, the electron beam size, the nominal electron density n e , and the ion distribution around the beam, i.e., the so-called ion cloud, must be measured. We use imaging techniques in the extreme ultraviolet (EUV) and optical to determine these. The electron beam width is measured using 3 d → 3 p emission from Fe xii and xiii between 185 and 205 Å. These transitions are fast and the EUV emission occurs only within the electron beam. The measured spatial emission profile and variable electron current yield a nominal electron density range of n e ~ 10 11 –10 13 cm –3 . We determine the size of the ion cloud using optical emission from metastable levels of ions with radiative lifetimes longer than the ion orbital periods. Here, the resulting emission maps out the spatial distribution of the ion cloud. We find a typical electron beam radius of ~60 μm and an ion cloud radius of ~300 μ m. These yield a spatially averaged effective electron density, ne,eff, experienced by the ions in EBIT spanning ~ 5 × 10 9 –5 × 10 11 cm –3 .

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Experimental determination of electron attenuation lengths in complex materials by means of epitaxial film growth: advantages and challenges

Accurate electron attenuation lengths are of critical importance in using electron spectroscopic methods to quantitatively characterize complex materials. Here we show that analysis of core-level and valence-band x-ray photoelectron spectra excited with monochromatic AlK? x-rays from the substrate and measured as a function of film thickness can be used to determine electron attenuation lengths in epitaxial SrTiO3 films on Ge(001). Closely lattice-matched epitaxial heterojunctions are ideal systems for determining attenuation lengths provided the films grow in a layer-by-layer fashion, leading to atomically flat surfaces, and the buried interfaces are atomically abrupt. In principle, either the rate of attenuation of substrate peak intensities or the rate of increase of film peak intensities can be used for this purpose. However, we find that structural nonuniformities in the films reduce the accuracy of electron attenuation lengths determined from photoelectrons that originate within the films. A more reliable source of information is found in photoelectrons from the substrate which traverse the film. By using the energy dependence of calculated electron attenuation lengths from the NIST database in combination with Ge 3d core and Ge-derived valence band intensities, we determine electron attenuation length as a function of kinetic energy for SrTiO3.

Chambers, Scott A.↗

DOE OSTI2019

Effect of electron–electron interactions on optical properties of GaN/AlN quantum wells: a nonlinear Schrödinger equation approach

Researchers usually neglect the electron–electron interaction effect when they study the optical properties of semiconducting nanostructures through the compact density matrix approach. In the existing papers, this work has also been done through self-consistent solution of the Schrödinger and Poisson equations. For the first time, we have investigated the electronic and optical properties of wurtzite GaN/AlN quantum wells in the presence of electron–electron interactions assuming weak electron–electron scattering through a numerical solution of a nonlinear Schrödinger equation. It is shown that the electron–electron interaction effect leads to the removal of the N-fold degeneracy in the energy levels of N-well multiple quantum well systems. Effects of different parameters such as electric field, the strength of the electron–electron interaction, a total length of the system and also two different numbers of wells (1 and 2) on the mentioned optical properties have been investigated. Also, we observed redshifts in the optical rectification coefficient peak positions when the nonlinear parameter increased. Finite difference self-consistent method was employed to solve the nonlinear Schrödinger equation and we demonstrated the method convergence. Finally, we illustrated the accuracy of the method by comparing our energy values with those of the Sinc method.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2019

Measurement of the full electron spectrum associated with the Ag N 3 VV Auger transitions: Evidence for the contribution of multi-electron Auger processes

In this paper, we report the first measurement of the full energy spectrum (down to 0 eV) of electrons emitted from the surface of Ag(100) as a result of the N 3 VV Auger transition. A comparison with a Monte-Carlo model was used to obtain an estimate of the contribution of multi-electron Auger processes to the low energy part of the Auger spectrum. The experimental Auger spectrum was obtained in time coincidence with photo-emitted 4p 3/2 core electrons from Ag using Auger-Photoelectron coincidence spectroscopy (APECS). The coincidence condition in APECS can remove most, but not all, spectral contributions from events unrelated to the Auger transition. The remaining contributions to the APECS spectrum from Auger-unrelated events, which are significant, were determined from a series of coincidence measurements of inelastically scattered valence band photoelectrons. The contribution from Auger-unrelated events was subtracted from the APECS Auger spectrum of Ag(100) to obtain the full Auger spectrum down to 0 eV. The resulting spectrum includes, in addition to Auger electrons emitted without energy loss, inelastically scattered Auger electrons. We observe that the spectral weight of the low energy tail (LET) in the APECS spectrum is reduced by more than a factor of two after subtracting the Auger-unrelated contributions. However, the intensity of the LET after this subtraction is still two times the integrated intensity in the Auger peak. A Monte Carlo model that includes the inelastic transport of the N 3 VV Auger electrons through the surface showed that LET produced by the inelastic scattering of the Auger electrons has the same intensity as the integrated intensity in the Auger peak. The excess intensity in the experimental LET provides strong evidence that the Auger related spectrum also includes contribution from multiple electron emissions that are intrinsic to the creation and/or the Auger decay of the core hole. In conclusion, our estimate shows that as low as 20% to as high as 60% of the core hole decay events result in the emission of more than one Auger electron from Ag (100). This result demonstrates the need for a better understanding of the contribution of valence-electron correlations to the entire CVV Auger spectrum down to 0 eV.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Electronic Structures and Magnetism of Zr-, Th-, and U-based Metal-Organic Frameworks (MOFs) by Density Functional Theory

Metal-organic frameworks (MOFs) have recently gained wide interest as candidate materials for nuclear waste immobilization. While the fundamental thermodynamic properties, such as the substitution energies determine the favorability of radionuclide sequestration by utilization of a MOF matrix, the studies of MOF electronic structure reveal the role of d-, and/or f-electrons on changes in physical properties of actinide-containing materials. We use density functional theory (DFT) calculations to investigate the electronic structures of Zr-, Th-, and U-MOFs, including their electronic band structures and, where appropriate, their magnetic properties. We employ various DFT methods including DFT+U, collinear spin-polarization, spin-orbit coupling, and different flavors of exchange-correlation functionals to assess the robustness to the specific exchange-correlation functional. Unlike the Zr-, and Th-MOFs, the U-MOF is found to be sensitive to electron localization and spin; hence we explore the magnetic structure of the U-MOF in further detail.

Metal-Organic Framework, MOF, Actinides, DFT↗

DOE OSTI2020

Thermal transport in compensated semimetals: Effect of electron-electron scattering on Lorenz ratio

It is well known that the electronic thermal conductivity of clean compensated semimetals can be greatly enhanced over the electric conductivity by the availability of an ambipolar mechanism of conduction, whereby electrons and holes flow in the same direction experiencing negligible Coulomb scattering as well as negligible impurity scattering. This enhancement—resulting in a breakdown of the Wiedemann-Franz law with an anomalously large Lorenz ratio—has been recently observed in two-dimensional monolayer and bilayer graphene near the charge neutrality point. In contrast to this, three-dimensional compensated semimetals such as WP 2 and Sb are typically found to show a reduced Lorenz ratio. Here, we investigate the reasons for this difference, focusing on the low-temperature regime where the electron-electron scattering is expected to dominate over other scattering mechanisms. We show that the different regimes of Fermi statistics (nondegenerate electron-hole liquid in graphene versus degenerate electron-hole liquid in compensated semimetals) are not sufficient to explain the reduction of the Lorenz ratio in the latter. We propose that the solution of the puzzle lies in the large separation of electron and hole pockets in momentum space, which allows compensated semimetals to sustain sizable regions of electron-hole accumulation near the contacts. These accumulations suppress the ambipolar conduction mechanism and effectively split the system into two independent electron and hole conductors. We present a quantitative theory of the crossover from ambipolar to unipolar conduction as a function of the size of the electron-hole accumulation regions, and show that it naturally leads to a sample-size-dependent thermal conductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Modulating the Electron Affinity of Small Bipyridyl Molecules on Single Gold Nanoparticles for Plasmon-Driven Electron Transfer

Developing controlled platforms for plasmon-driven chemistry is of great importance in catalytic reactions at the nanoscale. We report anion radical formation for five bipyridyl complexes of varying degrees of electron affinity utilizing optically fo-cused intraband (594 nm) and interband (532 nm) pump excitation of single gold nanoparticles. The surface-enhanced Raman scattering (SERS) of anion radicals for the five non-resonant adsorbed molecules 2,2’-bipyridine (22BPY), 4,4’-bipyridine (44BPY), trans-1,2-bis(4-pyridyl)ethylene (BPE), 1,2-bis(4-pyridyl)acetylene (BPA), and 1,2-bis(4-pyridyl)ethane (BPEt) were detected using localized surface-plasmon resonance (LSPR) excitation with 785 nm. The electron affinity of the five bipyridyl complexes were determined using electrochemistry. Molecules with low electron affinity experienced high-er instances of radical anion formation under a plasmon-coupled intraband electron transfer excitation (594 nm) whereas molecules with high electron affinity showed a preference for anion radical formation under direct interband electron trans-fer excitation (532 nm). The lowest unoccupied molecular orbital (LUMO) energy levels for low electron affinity surface-bound molecules (22BPY, BPEt) are on average ~0.43 eV higher for high electron affinity surface-bound molecules (BPA, BPE, 44BPY) as calculated using time-dependent density functional theory, elucidating the importance of plasmon coupling to energy levels that facilitate charge transfer pathways. We also show the ability to ‘activate’ high vs low electron affinity single nanoparticles with the choice of pump excitation wavelength. The findings show the complex interplay between molecular electron affinity, orbital overlap with the density of states of the plasmonic metal, and excitation energetics of the pump laser wavelength. Potential applications of this work include enhanced control over molecular scale catalysis, biosensor design, and solar energy capture.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Electronic–Vibrational Coupling and Electron Transfer

This Feature Article describes our recent work on implementing pump-degenerate four-wave mixing for studying electronic vibrational coupling in solid-state systems and in particular in interfacial electron transfer systems. Interfacial electron transfer (ET) reactions constitute key physical phenomena central to a variety of light-induced energy transport and conversion processes such as vision, photocatalysis, photovoltaics, energy storage, molecular electronics, etc. Heterogeneous material systems like organic/inorganic interfaces are of particular interest due to the variety of possible modifications to their properties. Although ET dynamics has been studied intensively in heterogeneous systems, many questions remain unanswered. The significance of electronic–vibrational coupling and coherence is one aspect that has yet to be fully explored. It is well-known that ET between a molecule and a semiconductor can be accompanied by vibrational excitation due to Franck–Condon overlap of the excited state and cation. The energy necessary for exciting these high-energy vibrational modes is taken from the excess energy of the transferred electron and leads to an ET spectrum. This spectrum carries information that is associated with the vibrational wavepacket that is involved in the ET process, including the coherent beating that results from periodic attempts to overcome the transition state. The dynamics of the wavepacket, and in particular its coherence time, provides insight into the strength of the coupling between electron donor and acceptor states and the adiabaticity of the process. This information is important but not readily available for interfacial ET systems comprising a large number of possible electron acceptor states because neither the rate of the reaction nor the electronic spectrum allows unambiguous assignment. These recent studies give access to vibrational wave packet dynamics triggered by ET reaction and have the potential to allow direct measurement of Huang–Rys parameters and study fundamental properties of interfacial ET like the adiabaticity and the amount of coherence—electronic and vibrational—in the system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Structural origins of the electronic properties of materials via time-resolved infrared spectroscopy

Time-resolved mid-infrared (TRIR) spectroscopy offers new opportunities to investigate how the molecular and structural properties of optoelectronic materials influence their electronic and transport states. This capability emerges from the ability to measure low energy electronic transitions in the mid-infrared that are related to delocalized states in materials and to simultaneously detect the vibrational properties of the materials that influence those states. Furthermore, the ability to simultaneously measure electronic and vibrational transitions in materials offers unprecedented opportunities to correlate structural dynamics of materials with their electronic and transport properties. Here, these capabilities are introduced by first describing the basic principles of TRIR spectroscopy used to examine electronic processes in materials. Then, several applications of TRIR spectroscopy are described in which measurements of the vibrational spectra of electronic excited states are probed as a means to correlate the structural properties of materials with the delocalization of their electronic states. In one example, exciton localization mechanisms in organic semiconductors are probed through vibrational spectra of the molecules in their excited states and correlated with their crystalline packing arrangements. Another example highlights the use of TRIR spectroscopy to examine singlet fission reaction dynamics through a combination of low energy electronic transitions and the vibrational spectra that are unique to the electronic states involved in the reaction. Finally, the use of TRIR spectroscopy to investigate charge carrier localization mechanisms in lead-halide perovskites is described, followed by an outlook of future applications of the technique in optoelectronic materials research.

36 MATERIALS SCIENCE↗

DOE OSTI2019

A benchmark photoelectron spectroscopic and theoretical study of the electronic stability of [B12H12]2-

We report a joint benchmark study on the electronic stability of closo-dodecaborate [B12H12]2- employing negative ion photoelectron spectroscopy and high level electronic structure methods. The photoelectron spectra of [B12H12]2-, measured at 266, 193 and 157 nm, yield the Adiabatic and Vertical Detachment Energies (ADE and VDE) of this dianion at 0.93 ± 0.05 eV and 1.15 ± 0.05 eV, respectively, along with a ~ 3 eV Repulsive Coulomb Barrier (RCB) against electron detachment. Theoretical calculations at various levels of electronic structure theory confirm the high stability of this dianion. The ADE and VDE values calculated at the CCSD(T)/aug-cc-PVQZ level are 0.92, and 1.16 eV, in excellent agreement with the experimental benchmark values. The comparison between the experimental and the theoretical values obtained at different levels of theory indicate that the PBE0 density functional represents a cost-effective method of sufficient accuracy to describe the molecular properties of this dianion and associated compounds. The theoretical RCB was modelled after the electrostatic potential (ESP) and point charge method (PCM) along three different detachment pathways, viz. along the B-H bond, perpendicular to a B-B bond, and normal to a B-B-B triangle. It was found that detachment of the electron along the B-H bond is preferred, as this pathway is associated with RCBs between 2.3 eV (PCM) and 3.3 eV (ESP), values that bracket the experimental estimate of ~ 3 eV.

Apra, Edoardo↗

DOE OSTI2019

The electron canonical battery effect in magnetic reconnection: Completion of the electron canonical vorticity framework

A widespread practice in studying magnetic reconnection is to examine the electron momentum equation. Here, we present an alternative, ab initio framework that examines the motion of the electron canonical vorticity, which is the curl of the electron canonical momentum. The competition between just two terms—the convective term and the electron canonical battery term—determines the dynamics of electron canonical vorticity and equivalently the electron physics down to first principles. To demonstrate the power of this approach, the growth, saturation, stability, and morphology of the electron diffusion region are explained within the electron canonical vorticity framework. The framework provides a clear distinction between reconnection models where the frozen-in property of the magnetic field is violated by electron inertia and by pressure tensor effects such as electron viscosity.

25 ENERGY STORAGE↗

DOE OSTI2020

Neutralization of ion beam by electron injection: Accumulation of cold electrons

Ion beam charge neutralization by electron injection is a complex kinetic process. Recent experiments show that the resulting self-potential of the ion beam after neutralization by plasma is much lower than the temperature of plasma electrons [Stepanov et al., Phys. Plasmas 23, 043113 (2016)], indicating that kinetic effects are important and may affect the neutralization of the ion beam. We performed a numerical study of the charge neutralization process of an ion beam making use of a two-dimensional electrostatic particle-in-cell code. The results show that the process of charge neutralization by electron injection is composed of two stages. During the first stage, the self-potential of the beam is higher than the temperature of injected electrons (T e /e) and all injected electrons are captured by the ion beam. During the second stage, hot electrons escape from the ion beam and the beam self-potential (φ) decreases because cold electrons slowly accumulate resulting in the beam self-potential φ to become much lower than Te/e in agreement with previous experimental observations at Princeton Advanced Teststand. We also determined that the resulting φ scales as φ~√T e , in agreement with previous experimental observations from Gabovich's group. In addition, the results show that the transverse position of the electron source has a great impact on ion beam neutralization. A slight shift of the electron source as relevant to the ion thrusters leads to a large increase in the beam self-potential because of an increase in potential energy of injected electrons.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

High-resolution planar electron beam induced current in bulk diodes using high-energy electrons

Understanding the impact of high-energy electron radiation on device characteristics remains critical for the expanding use of semiconductor electronics in space-borne applications and other radiation harsh environments. Here in this paper, we report on in situ measurements of high-energy electron radiation effects on the hole diffusion length in low threading dislocation density homoepitaxial bulk n-GaN Schottky diodes using electron beam induced current (EBIC) in high-voltage scanning electron microscopy mode. Despite the large interaction volume in this system, quantitative EBIC imaging is possible due to the sustained collimation of the incident electron beam. This approach enables direct measurement of electron radiation effects without having to thin the specimen. Using a combination of experimental EBIC measurements and Monte Carlo simulations of electron trajectories, we determine a hole diffusion length of 264 ± 11 nm for n-GaN. Irradiation with 200 kV electron beam with an accumulated dose of 24 × 10 16 electrons cm -2 led to an approximate 35% decrease in the minority carrier diffusion length.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2026

Near-infrared noise in intense electron bunches

This article investigates electron bunch density fluctuations in the 1 −10 μ⁢m wavelength range, focusing on their impact on coherent electron cooling (CEC) in hadron storage rings. In this study, we compare the shot-noise model with experimental observations using bandwidth-filtered near-infrared optical transition radiation (OTR) photodiode signals, where the transverse bunch size is much larger than the OTR wavelength of interest. The relativistic electron bunch (𝛾 ≈ 50) parameters are close to those proposed for the coherent electron cooler in the electron-ion collider (EIC) project. Preliminary feasibility experiments were conducted, and the noise factors are presented, supported by particle tracking. No major density fluctuations or effective cooling rate decrease were revealed for EIC CEC design parameters. Additionally, longitudinal-space-charge-induced microbunching for the chicane-compressed bunch was observed with coherent OTR enhancements up to 100 times, providing further calibration of the measurement method.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2019

Photoferrotrophs Produce a PioAB Electron Conduit for Extracellular Electron Uptake

Photoferrotrophy is a form of anoxygenic photosynthesis whereby bacteria utilize soluble or insoluble forms of ferrous iron as an electron donor to fix carbon dioxide using light energy. They can also use poised electrodes as their electron donor via phototrophic extracellular electron uptake (phototrophic EEU). The electron uptake mechanisms underlying these processes are not well understood. Using Rhodopseudomonas palustris TIE-1 as a model, we show that a single periplasmic decaheme cytochrome c , PioA, and an outer membrane porin, PioB, form a complex allowing extracellular electron uptake across the outer membrane from both soluble iron and poised electrodes. We observe that PioA undergoes postsecretory proteolysis of its N terminus to produce a shorter heme-attached PioA (holo-PioA C , where PioA C represents the C terminus of PioA), which can exist both freely in the periplasm and in a complex with PioB. The extended N-terminal peptide controls heme attachment, and its processing is required to produce wild-type levels of holo-PioA C and holo-PioA C B complex. It is also conserved in PioA homologs from other phototrophs. The presence of PioAB in these organisms correlate with their ability to perform photoferrotrophy and phototrophic EEU. IMPORTANCE Some anoxygenic phototrophs use soluble iron, insoluble iron minerals (such as rust), or their proxies (poised electrodes) as electron donors for photosynthesis. However, the underlying electron uptake mechanisms are not well established. Here, we show that these phototrophs use a protein complex made of an outer membrane porin and a periplasmic decaheme cytochrome (electron transfer protein) to harvest electrons from both soluble iron and poised electrodes. This complex has two unique characteristics: (i) it lacks an extracellular cytochrome c , and (ii) the periplasmic decaheme cytochrome c undergoes proteolytic cleavage to produce a functional electron transfer protein. These characteristics are conserved in phototrophs harboring homologous proteins.

Microbiology↗