Effects of Static Electric Fields on the Excitations of Silver Nanowire Dimers
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Chemistry↗
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Flexoelectricity and New Phenomena
It is easy to miss the scientific implications of our recent work on Triboelectricity. Everyone knows that rubbing and contact can produce static electricity; less appreciated is that the thermodynamic driver has been an open question since static electricity was first observed by Thales of Miletus around 585 BC. People think they understand it, for instance one common explanation that can still be found in the current literature is that differences in the work function drives charge transfer, often called the Volta-Helmholtz hypothesis. As summarized in 1967 by Harper, this fails to explain many experimental observations, for instance that charging can occur when two pieces of the same material are rubbed against each other. We are the first to place triboelectricity on a solid foundation rooted in quantum mechanics – the flexoelectric effect. We were able to explain a significant number of previously unexplained phenomena: 1) Bipolar tribocurrents associated with stick-slip, due to the change in sign of the strain gradients. 2) A one-third power scaling of tribocurrents with indentation force. 3) Tribocharging when two identical materials are used, these being due to local variations in the asperities so there are usually local potential differences. 4) Inhomogeneous charging of insulators, related to the statistical nature of asperities. 5) An experimentally observed reversal in the sign of charge transfer for negative and positive curvature, which is related to a change in the sign of the strain gradient. Exploiting our DOE prior funded work on flexoelectricity, we obtained semi-quantitative matching to existing experimental measurements of the surface charge in triboelectric experiments. The work has been well received in the literature. The work has been the focus of a number of popular science press articles, and also formed the basis for a Podcast for children 6-10 “The Rise and Fall of Static Man” posted in December 2019 by NPR as part of their “Wow in the World” series. I was also briefly interviewed by the Chicago PBS station in January 2020. This work are significant for a wide range of energy applications; to quote from an independent source: "Triboelectric power has plenty of potential, says Wenzhuo Wu, an assistant professor of engineering at Purdue. If the basics of static electricity are better understood, we could maximize the efficiency of wind or wave power generators, Wu says. The body's own movement could be used to power internal medical devices. Imagine being able to create a roof shaped to harness the power of a raindrop — the friction of the rain passing over the surface — to generate triboelectricity, powering the building below it." This is the start of new science, some of which we already partially understand such as the role of band bending in charge transfer. We need to understand charge transfer combining elasticity, quantum mechanics, band bending and defect states. These directly involve several of the DOE Grand Challenges: "How do we control material processes at the level of electrons? How do remarkable properties of matter emerge from complex correlations of the atomic or electronic constituents and how can we control these properties? How do we characterize and control matter away—especially very far away— from equilibrium?" I will argue that this work truly falls into the class of disruptive science; it is not just a simple extension, linear science. Not everyone will accept the approach. Since we explain far more about triboelectricity than anyone before, the preponderance of evidence supports the model. The feedback I have received is that many agree with the work, to quote: "The model makes sense, says Michael McAlpine, a professor of engineering at the University of Minnesota. "It's such a simple explanation, I was surprised I didn't put my finger on that," McAlpine says." The proposal received strong reviews. It was also publicized on the Department of Energy Web Site.
16 TIDAL AND WAVE POWER↗
New electric force and charge exchange modules in discrete element model enables particle dynamics simulation in electric field
Discrete element modeling (DEM) is an important technique for particle dynamics simulation. The field of metal additive manufacturing often utilizes DEM to simulate the rheological behaviors of powder. Standard contact and short-range interactions are sufficient in most cases but insufficient to describe the particle dynamics with the influence of an electric field. Modeling such a system requires additional physics to describe the particle–field interactions. The relevant physics has been experimentally understood but is not yet available in DEM. Here, we develop a charge exchange and an electric force module. The electric force module governs particle response to the electric field, while the charge exchange module enables particles to acquire proper charge during contact with charged geometries. We validate the modules against analytical calculations and high-speed videos of electrostatic powder deposition experiments. Notably, the model struggles to capture the initial particle levitation. We later deploy a modified electric field, as supported by static electric field simulation, to better approximate the electric field penetration into the powder layer. This modification improves the model’s capability of simulating realistic particle levitation. The results highlight the challenges of modeling particle behaviors in the electric field while demonstrating the feasibility of obtaining quantitative results, which are difficult to measure experimentally.
charge exchange↗
Electrical Manipulation of Quantum Coherence in a Two-Level Molecular System
We report the manipulation of ultrafast quantum coherence of a two-level single hydrogen molecular system by employing static electric field from the sample bias in a femtosecond terahertz scanning tunneling microscope. A H 2 molecule adsorbed on the polar Cu 2 N surface develops an electric dipole and exhibits a giant Stark effect. An avoided crossing of the quantum state energy levels is derived from the resonant frequency of the single H 2 two levels in a double-well potential. The dephasing time of the initial wave packet can also be changed by applying the electric field. The electrical manipulation for different tunneling gaps in three dimensions allows quantification of the surface electrostatic fields at the atomic scale. Further, our work demonstrated the potential application of molecules as controllable two-level molecular systems.
36 MATERIALS SCIENCE↗
Efficient on-chip terahertz generation and detection with GaN photoconductive emitters
Photoconductive emitters for terahertz generation hold promise for highly efficient down-conversion of optical photons because it is not constrained by the Manley-Rowe relation. Existing terahertz photoconductive devices, however, faces limits in efficiency due to the semiconductor properties of commonly used GaAs materials. Here, we demonstrate that large bandgap semiconductor GaN, characterized by its high breakdown electric field, facilitates the highly efficient generation of terahertz waves in a coplanar stripline waveguide. Towards this goal, we investigated the excitonic contribution to the electro-optic response of GaN under static electric field both through experiments and first-principles calculations, revealing a robust excitonic Stark shift. Using this electro-optic effect, we developed a novel ultraviolet pump-probe spectroscopy for in-situ characterization of the terahertz electric field strength generated by the GaN photoconductive emitter. Our findings show that terahertz power scales quadratically with optical excitation power and applied electric field over a broad parameter range. We achieved an optical-to-terahertz conversion efficiency approaching 100% within the 0.03–1 THz bandwidth at the highest bias field (116 kV/cm) in our experiment. Further optimization of GaN-based terahertz generation devices could achieve even greater optical-to-terahertz conversion efficiencies.
Uzundal, Can B↗
Bias-Modulated ALD of ZnO: Insights into Precursor-Surface Interactions for ZnO Films
Atomic layer deposition (ALD) is widely used to deposit conformal thin films but is often limited in the tunability of the resulting material’s properties. Substrate bias and electric fields alter precursor-surface interactions and provide means to tune material properties. To explore this, we performed zinc oxide (ZnO) ALD using diethylzinc (DEZ) and water on silicon native oxide substrates at 150 °C in a sample holder designed to create a static electrical field by biasing one plate of a parallel plate capacitor-style sample holder during deposition. ZnO films prepared in an electric field/on a biased sample holder were thinner, changed relative crystalline composition, and contained more carbon compared to samples grown in identical sample holders without bias. The thickness was independent of the magnitude of the eletric field between plates, indicating that the primary driver for the change was substrate biasing not the electric field between plates of the parallel plate capacitor-style sample holder. Density functional theory calculations showed enhanced electron migration between dissociatively adsorbed DEZ molecules and the ZnO (002) facet with increasing force from an electric field at the substrate surface, which strengthens the electronic interactions between the surface and the adsorbate. These models offer a compelling explanation for the inhibited growth, changes in the crystallinity, and increase in carbon content of films grown in an electric field/on biased plates.
Jones, Jessica C. (ORCID:0000000174754620)↗
Electrical Control of the Nuclear Spin States of Rare-Earth Adatoms
Rare-earth adatoms on surfaces have been studied for potential atomic-scale magnetic storage, quantum sensing, and quantum computing applications. Despite accumulating experimental efforts, a comprehensive description of the electronic configurations of the adatoms remains elusive. Here, we investigate two charge states and several electronic configurations, including 5d and 6s valence shells, for a Sm adatom on a MgO substrate using multiconfigurational ab initio methods, for the possibility of using the Sm nuclear spin levels as qubits. For the configurations in a neutral charge state, we find that the electronic ground state is a singlet, and thus the hyperfine interaction associated with the 147 Sm nucleus is absent, which may greatly enhance nuclear spin coherence time. The degeneracy of the nuclear levels is lifted by the nuclear quadrupole interaction. We show that the splitting of the nuclear levels can be controlled by a static electric field, and that Rabi oscillations between the nuclear levels can be induced by a time-dependent electric field. For the configurations in a singly charged state, electronic Kramers doublets are formed. The electronic configurations including an unpaired 6s orbital exhibit a strong hyperfine Stark effect due to a large Fermi contact contribution to the hyperfine interaction. In these configurations, electric-field-induced Rabi oscillations between the electronic-nuclear levels can occur at frequencies up to 3 orders of magnitude higher than those for the neutral charge state. The proposed system may be experimentally observed within scanning tunneling microscopy.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Direct Simulations of H–He Mixtures at Planetary Interior Conditions: Demixing, Insulator–Metal Transition and Miscibility Boundaries
Accurate knowledge of the electrical and thermal conductivities and structural properties of hydrogen–helium mixtures under thermodynamic conditions within and beyond the immiscibility range is very important to predict the thermal evolution and internal structure of gas giant planets like Jupiter and Saturn. Here, we propose a novel method to determine the immiscibility boundary accurately without the need for free energy calculations, while providing consistent insights into structural and transport properties of mixtures. We show with direct large-scale ab initio simulations that the insulator–metal transition (IMT) of the hydrogen subsystem is strongly affected by an admixture with a small fraction of helium and occurs at temperatures significantly higher than those of pure hydrogen. At pressures below 150 GPa, the IMT boundary is not related anymore to the H 2 subsystem dissociation, the system remains insulating even after the full dissociation of H 2 molecules and its transition to an H–He mixture. The offset of the IMT in the H–He mixture relative to the dissociation region in the hydrogen subsystem and the significant reduction of static electrical and thermal conductivity by a factor between two and a few thousand relative to pure hydrogen found in mixtures have consequences for Jupiter and Saturn’s thermal evolution, internal structure, and dynamo action, affecting a large fraction of the interior of both planets.
Helium↗
Transition from Vehicular to Structural Ionic Transport in Electrified Alkali Aqueous Solutions
A molecular understanding of the solvation and dynamics of ions under static electric fields is crucial for modelling a wide range of natural and technological processes. Yet, traditional simulation methods suffer from a trade-off that has to be made between accuracy and statistical convergence. To bridge this gap, herein we extend our recently introduced Perturbed Neural Network Potential Molecular Dynamics (PNNP MD) approach to investigate the solvation structures and ionic transport mechanisms of electrified alkali cationic solutions. We obtain ionic conductivities for Li+, Na+ and Cs+ from the field dependence of the ionic current density in good agreement with experiment. Surprisingly, the migration mechanism is found to be strikingly different for the three ions despite their similar ionic conductivities. While Li+ conducts predominantly through vehicular migration of a stable 4-fold coordinated ion at all field strengths, Cs+ conducts strictly through a structural diffusion mechanism, where 9-12 transient first shell water coordination bonds are broken and renewed. Notably, aqueous Na+ emerges as a “Goldilocks” ion: its ion-water interactions are strong enough to maintain distinct 5-6 fold coordination shells at zero field (unlike Cs+) yet labile enough to be strongly perturbed by electric fields (unlike Li+). As a consequence, we observe an electric field-induced transition from vehicular to structural ionic transport for Na+ that is accompanied by a marked increase in the ionic current density. Our results imply that the conductance mechanism of ions with moderate ion-solvent interactions can be effectively tuned by external electric fields.
Joll, Kit↗
A Conjugated Oligoelectrolyte Exhibiting Room Temperature Spin-Correlated Radical Pair Character for Biological Sensing
We report a water-soluble conjugated oligoelectrolyte (COE) composed of carbazole-benzophenone, COE-CbzBP, that exhibits photogenerated spin-correlated radical pair (SCRP) behavior sensitive to static electric fields from DNA but not from lipid bilayers. The SCRP forms from a thermally activated, spin-polarized state enabled by partial π-conjugation disruption at the donor–acceptor (carbazole-benzophenone) nitrogen–carbon (N–C) junction, which facilitates a twisted intramolecular charge-transfer (TICT) geometry. This state minimizes the singlet–triplet energy gap (ΔE ST = 0.12 eV), radical–pair exchange coupling (J RP ∼ ΔE ST /2), and charge separation free energy (ΔG CS ) in both DNA (−0.19 eV) and lipid bilayers (−0.55 eV). Room-temperature continuous-wave electron paramagnetic resonance (CW-EPR) reveals a photogenerated spin-polarized singlet for COE-CbzBP that splits upon DNA association, consistent with modulation of J RP and hyperfine coupling (A x ), presumably via electric field-spin coupling. No spin-polarized signal was observed under dark, cryogenic conditions, or in liposomes, but was quenched by the spin trap 4-POBN. Transient absorption and spectroelectrochemistry confirmed magnetic-field sensitive long-lived excited-state absorption features attributed to charge-separated states 3 [Cbz •+ -BP •– ]*, which were lengthened by DNA, and quenched in lipid bilayers and 4-POBN. Quantum chemical simulations show that planar geometries (lipid-like) increase ΔE ST by 0.31 eV compared to TICT-optimized structures. This geometry-dependent modulation explains the absence of SCRP signatures in rigid environments, underscoring the importance of TICT states, minimized ΔE ST , and favorable ΔG CS for achieving room-temperature SCRP generation. These findings establish design principles for TICT-enabled molecules exhibiting qubit-like behavior that operate under ambient and biologically relevant conditions, with direct implications for quantum information science (QIS).
Aromatic compounds↗
Thermodynamic driving forces in contact electrification between polymeric materials
Abstract Contact electrification, or contact charging, refers to the process of static charge accumulation after rubbing, or even simple touching, of two materials. Despite its relevance in static electricity, various natural phenomena, and numerous technologies, contact charging remains poorly understood. For insulating materials, even the species of charge carrier may be unknown, and the direction of charge-transfer lacks firm molecular-level explanation. Here, we use all-atom molecular dynamics simulations to investigate whether thermodynamics can explain contact charging between insulating polymers. Based on prior work suggesting that water-ions, such as hydronium and hydroxide ions, are potential charge carriers, we predict preferred directions of charge-transfer between polymer surfaces according to the free energy of water-ions within water droplets on such surfaces. Broad agreement between our predictions and experimental triboelectric series indicate that thermodynamically driven ion-transfer likely influences contact charging of polymers. Furthermore, simulation analyses reveal how specific interactions of water and water-ions proximate to the polymer-water interface explain observed trends. This study establishes relevance of thermodynamic driving forces in contact charging of insulators with new evidence informed by molecular-level interactions. These insights have direct implications for future mechanistic studies and applications of contact charging involving polymeric materials.
36 MATERIALS SCIENCE↗
High resolution electronic spectroscopy of uranium mononitride, UN
The isoelectronic molecules UN and UO + are known to have Ω = 3.5 and Ω = 4.5 ground states, respectively (where Ω is the unsigned projection of the electronic angular momentum along the internuclear axis). A ligand field theory model has been proposed to account for the difference [Matthew and Morse, J. Chem. Phys. 138, 184303 (2013)]. The ground state of UO + arises from the U 3+ (5f 3 ( 4 I 4.5 ))O 2− configuration. Owing to the higher nominal charge of the N 3− ligand, the U 3+ ion in UN is stabilized by promoting one of the 5f electrons to the more polarizable 7s orbital, reducing the repulsive interaction with the ligand and rendering U 3+ (5f 2 7s( 4 H 3.5 ))N 3− the lowest energy configuration. In the present work, we have advanced the characterization of the UN ground state through studies of two electronic transitions, [18.35]4.5-X(1)3.5 and [18.63]4.5-X(1)3.5, using sub-Doppler laser excitation techniques with fluorescence detection. Further, spectra were recorded under field-free conditions and in the presence of static electric or magnetic fields. The ground state electric dipole moment [μ = 4.30(2) D] and magnetic g e -factor [2.160(9)] were determined from these data. These values were both consistent with the 5f 2 7s configurational assignment. Dispersed fluorescence measurements were used to determine vibrational constants for the ground and first electronically excited states. Electric dipole moments and magnetic g e -factors are also reported for the higher-energy electronically excited states.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Quantum Geometric Oscillations in Two-Dimensional Flat-Band Solids
Two-dimensional van der Waals heterostructures can be engineered into artificial superlattices that host flat bands with significant Berry curvature and provide a favorable environment for the emergence of novel electron dynamics. In particular, the Berry curvature can induce an oscillating trajectory of an electron wave packet transverse to an applied static electric field. Though analogous to Bloch oscillations, this novel oscillatory behavior is driven entirely by quantum geometry in momentum space instead of band dispersion. While the current from Bloch oscillations can be localized by increasing field strength, the current from the geometric orbits saturates to a nonzero plateau in the strong-field limit. Finally, in nonmagnetic materials, the geometric oscillations are even under inversion of the applied field, whereas the Bloch oscillations are odd, a property that can be used to distinguish these two coexisting effects.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Influence of substituents on the vectorial difference static dipole upon excitation in synthetic bacteriochlorins
Organic dye aggregates have been shown to exhibit exciton delocalization in natural and synthetic systems. Such dye aggregates show promise in the emerging area of quantum information science (QIS). We believe that the difference static dipole (Δd) is an essential dye parameter in the development of molecular QIS systems. However, a foundational understanding of the structural factors influencing Δd remains elusive. Bacteriochlorins play a vital role in photosynthesis due to their exceptional photophysical properties. Therefore, bacteriochlorins are particularly suitable dyes for the construction of aggregate systems for QIS. Synthetic bacteriochlorins further offer stability and tunability via chemical modifications. Here, the influence of substituents on the Δd of monomeric (non-aggregated) dyes was investigated via density functional theory (DFT) and time-dependent (TD-)DFT in a set of 5-methoxybacteriochlorins progressively substituted with ethynyl, phenyl, and phenylethynyl substituents at the 3,13- and 3,13,15-positions of the macrocycle. Symmetrically substituted 5-methoxybacteriochlorins were shown to have the largest Δd. The increase in Δd in the series of dyes was largely due to changes in orientation of the static dipole upon excitation rather than large changes in magnitude. In addition, the transition dipole (μ) and the angle between Δd and μ (ζ) were calculated. Three 5-methoxybacteriochlorins with high predicted Δd and μ were synthesized and characterized spectroscopically. The trend in Δd values empirically determined using the solvatochromic Stokes shift method was comparable with the DFT calculations.
36 MATERIALS SCIENCE↗
Additively manufacturing fluorine-containing polymers
A system and method of additively manufacturing a part including electrically conductive or static dissipating fluorine-containing polymers. The method includes depositing fluorine-containing polymer additive manufacturing material onto a build platform, selectively cross-linking portions of the deposited additive manufacturing material, and curing the selectively cross-linked portions such that the part is at least one of electrically conductive and static dissipating.
Selter, Thomas Matthew↗
Connectivity between Static Field and Continuous Wave Field Effects on Excitation-Induced H 2 Activation
Due to the tremendous applications of the plasmon resonance excitation process, such as improvements in catalytic efficiency due to plasmonic enhancement and/or hot-electron processes, understanding the mechanism behind these processes has become a popular topic in recent years. In this work, we focus on unraveling the mechanism of excitation-induced H 2 activation using a simplified triangular Au 6 /Ag 6 cluster to investigate the effects of the electric field on electron redistribution and bond activation. We applied both static and continuous wave fields to investigate how these fields affect the systems. Geometrical changes (such as bond lengthening), molecular orbital reordering (affecting the relative energies of orbitals corresponding to hot-electron and charge-transfer excited states), and electronic charge redistribution between the cluster and the adsorbate occur upon application of a static electric field. To study H 2 activation, we apply Ehrenfest dynamics with real-time time-dependent density functional theory and examine how different excitation frequencies and polarizations affect bond activation. Moreover, electron-only dynamics are examined with real-time time-dependent density functional theory, and the time-dependent variations in the orbital populations and electronic transitions provide information about the excitation and relaxation processes of hot electrons with applied electric fields. Here, the static field results represent structures that can be accessed during the evolution of the systems when applying continuous wave fields. Through these studies, the effects of static and continuous wave field effects on plasmon-induced H 2 activation can be understood.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Langevin Dynamics modeling of gas-phase ion-ion recombination (Final Technical Report)
A self-consistent trajectory simulation approach to model MN reactions (Fig. 1) which incorporates the probability of electron transfer as a Monte Carlo operator (Fig. 2) was developed and published as Liu et al. J. Chem. Phys. 159, 114111 (2023). The electron transfer probability p ET estimated using the two-state Landau-Zener (LZ) theory was incorporated into classical trajectory simulations to elicit predictions of MN reaction cross-section σ (vacuum) or rate constant β (finite pressure). Electronic structure calculations with multireference configuration interaction (MRCI) and large correlation consistent basis sets were used to derive inputs to the LZ theory. The key advance of our trajectory simulation approach is the incorporation of electron transfer probability and the inclusion of the effect of ion-neutral interactions on MN using a Langevin representation of the effect of neutral gas on ions. For H + – H - and Li + – H(D) - pairs, our approach quantitatively agrees with measured speed-dependent cross-sections for up to ~10 5 m/s. For the ion pair Ne + – Cl - , our predictions of the MN rate constant at ~1 torr are a factor of ~2 – 3 higher than the experimentally measured value. Similarly, for Xe + – F - in the pressure range of ~20000 – 80000 Pa, our predictions of the MN rate constant are ~20% lower but are in excellent qualitative agreement with experimental data. The paradigm of using trajectory simulations to self-consistently model MN reactions is the basis for inclusion of additional non-classical, and static magnetic and electric field effects. Subsequent work, published as Roy et al. focused on modeling recombination rate constant for three ion pairs (rare gas Ar + cation and halide anions): Ar + – Cl - , Ar + – Br - , Ar + – I - , 2) considering spin-orbit couplings in the electronic structure calculations to obtain high-fidelity estimates of the electron transfer probability and incorporated within the classical trajectory simulations to elicit predictions. In addition to calculations of ion-ion recombination rate constants, a classical trajectory simulation technique (published as Roy et al. J. Chem. Phys. 162(9), 094104 (2023)) that uses quaternions to represent orientation of non-spherical particles (ions or aerosol particles) was developed to simulate the recombination of diatomic or more generally, polyatomic molecules. Finally, several other ion pairs such as Ne + – Cl - , Kr + – Cl - , were explored using the developed semi-classical trajectory simulations to understand various challenges in tackling electronic structure calculations. Using empirical approaches to parameterize the electron transfer radius, trajectory simulations were also used to probe the effect of ion number density on MN rate constant.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Enhanced energy gain through higher-order resonances during direct laser acceleration with superluminal phase velocity
Ultra-high intensity laser–plasma interactions can produce ultra-relativistic electrons via direct laser acceleration, assisted by quasi-static plasma magnetic and electric fields. These fields transversely confine electron motion and induce betatron oscillations. The net energy gain is strongly influenced by the interplay between two frequencies: the betatron frequency and the frequency of laser field oscillations experienced by the electron. Prior work has shown that energy gain is enabled by a resonance between the betatron oscillations and the oscillations of the laser field. In particular, higher-order resonances occur when the laser field completes multiple cycles during one betatron oscillation, allowing additional regimes of energy transfer beyond the fundamental (betatron) resonance. In this work, we demonstrate that such resonances become particularly effective when the laser's phase velocity is superluminal. Although the two frequencies generally evolve differently with increasing electron energy—leading to detuning—a superluminal phase velocity introduces a non-monotonic frequency ratio with a global minimum. This minimum allows sustained frequency matching over a broad energy range, thereby enabling enhanced energy gain. As the phase velocity increases, the betatron resonance becomes ineffective due to premature frequency detuning. At the same time, higher-order resonances become increasingly effective, emerging as the dominant mechanisms for enhanced energy gain in this regime of direct laser acceleration.
Laser plasma interactions↗