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At least 199 records · Page 11

Membrane potential sensing: Material design and method development for single particle optical electrophysiology

We review the development of “single” nanoparticle-based inorganic and organic voltage sensors, which can eventually become a viable tool for “non-genetic optogenetics.” The voltage sensing is accomplished with optical imaging at the fast temporal response and high spatial resolutions in a large field of view. Inorganic voltage nanosensors utilize the Quantum Confined Stark Effect (QCSE) to sense local electric fields. Engineered nanoparticles achieve substantial single-particle voltage sensitivity (~2% Δλ spectral Stark shift up to ~30% ΔF/F per 160 mV) at room temperature due to enhanced charge separation. A dedicated home-built fluorescence microscope records spectrally resolved images to measure the QCSE induced spectral shift at the single-particle level. Biomaterial based surface ligands are designed and developed based on theoretical simulations. The hybrid nanobiomaterials satisfy anisotropic facet-selective coating, enabling effective compartmentalization beyond non-specific staining. Self-spiking- and patched-HEK293 cells and cortical neurons, when stained with hybrid nanobiomaterials, show clear photoluminescence intensity changes in response to membrane potential (MP) changes. Organic voltage nanosensors based on polystyrene beads and nanodisk technology utilize Fluorescence (Förster) Resonance Energy Transfer (FRET) to sense local electric fields. Voltage sensing FRET pairs achieve voltage sensitivity up to ~35% ΔF/F per 120 mV in cultures. Non-invasive MP recording from individual targeted sites (synapses and spines) with nanodisks has been realized. However, both of these QCSE- and FRET-based voltage nanosensors yet need to reach the milestone of recording individual action potentials from individual targeted sites.

59 BASIC BIOLOGICAL SCIENCES↗

Injection current dependences of electroluminescence transition energy in InGaN/GaN multiple quantum wells light emitting diodes under pulsed current conditions

Injection current dependences of electroluminescence transition energy in blue InGaN/GaN multiple quantum wells light emitting diodes (LEDs) with different quantum barrier thicknesses under pulsed current conditions have been analyzed taking into account the related effects including deformation caused by lattice strain, quantum confined Stark effects due to polarization field partly screened by carriers, band gap renormalization, Stokes-like shift due to compositional fluctuations which are supposed to be random alloy fluctuations in the sub-nanometer scale, band filling effect (Burstein-Moss shift), and quantum levels in finite triangular wells. The bandgap renormalization and band filling effect occurring at high concentrations oppose one another, however, the renormalization effect dominates in the concentration range studied, since the band filling effect arising from the filling in the tail states in the valence band of quantum wells is much smaller than the case in the bulk materials. In order to correlate the carrier densities with current densities, the nonradiative recombination rates were deduced experimentally by curve-fitting to the external quantum efficiencies. The transition energies in LEDs both with 15 nm quantum barriers and 5 nm quantum barriers, calculated using full strengths of theoretical macroscopic polarization given by Barnardini and Fiorentini [Phys. Status Solidi B 216, 391 (1999)] are in excellent accordance with experimental results. The LED with 5 nm barriers has been shown to exhibit a higher transition energy and a smaller blue shift than those of LED with 15 nm barriers, which is mainly caused by the smaller internal polarization field in the quantum wells.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Effects of the Stark Shift on the Evolution of the Field Entropy and Entanglement in the Two-Photon Jaynes-Cummings Model

The evolution of the field entropy in the two-photon JCM in the presence of the Stark shift is investigated, and the effects of the dynamic Stark shift on the evolution of the field entropy and entanglement between the atom and field, are examined. The results show that the dynamic Stark shift plays an important role in the evolution of the field entropy in two-photon processes.

Fang, Mao Fa↗

Electric Field Analysis in a Cold-Ion Source Using Stark Spectroscopy of Rydberg Atoms

Here, we analyze electric fields in ion sources generated by quasicontinuous photoionization of cold Rb atoms trapped in the focal spot of a near-concentric, in-vacuum cavity for 1064-nm laser light. Ion streams are extracted with an external electric field, F. Stark effects of Rb 57F and of nearby high-angular-momentum Rydberg levels, which exhibit large, linear Stark shifts, are employed to study the net electric-field probability distribution within the ion-source region over an extraction-field range of 0 < F < 0.35 V/cm. For F = 0, we also investigate ion-field-induced Stark spectra of the 60P 1/2 state, which exhibits a (lesser) quadratic electric-field response that affords a simplified electric-field analysis. Experimental Rydberg spectra are compared with theoretical Stark spectra, which are weighted with net electric-field distributions obtained from classical ion-trajectory simulations that include Coulomb interactions. Experiments and models are in good agreement. At small F and high ion-source rates, the field approximately follows a Holtsmark distribution, and the ion streams are degraded by the Coulomb microfields. With increasing F and at lower ion-source rates, the fields become narrowly distributed around F, resulting in directional ion streams that are less degraded by microfields. Our results are of interest for monitoring cold-ion sources for focused-ion-beam applications, where Coulomb interactions are of concern, and for studies of electric fields in cold plasmas.

74 ATOMIC AND MOLECULAR PHYSICS↗

Electrical Tuning of Tin-Vacancy Centers in Diamond

Group-IV color centers in diamond have attracted significant attention as solid-state spin qubits because of their excellent optical and spin properties. Among these color centers, the tin-vacancy (Sn-V - ) center is of particular interest because its large ground-state splitting enables long spin coherence times at temperatures above 1 K. However, color centers typically suffer from inhomogeneous broadening, which can be exacerbated by nanofabrication-induced strain, hindering the implementation of quantum nodes emitting indistinguishable photons. Although strain and Raman tuning have been investigated as promising tuning techniques to overcome the spectral mismatch between distinct group-IV color centers, other approaches need to be explored to find methods that can offer more localized control without sacrificing emission intensity. Here, we study the electrical tuning of Sn-V - centers in diamond via the direct-current Stark effect. We demonstrate a tuning range beyond 1.7 GHz. We observe both quadratic and linear dependence on the applied electric field. Further, we also confirm that the tuning effect we observe is a result of the applied electric field and is distinct from thermal tuning due to Joule heating. Stark tuning is a promising avenue toward overcoming detunings between emitters and enabling the realization of multiple identical quantum nodes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Dynamics of superconducting qubit relaxation times

Superconducting qubits are a leading candidate for quantum computing but display temporal fluctuations in their energy relaxation times T 1 . This introduces instabilities in multi-qubit device performance. Furthermore, autocorrelation in these time fluctuations introduces challenges for obtaining representative measures of T 1 for process optimization and device screening. These T 1 fluctuations are often attributed to time varying coupling of the qubit to defects, putative two level systems (TLSs). In this work, we develop a technique to probe the spectral and temporal dynamics of T 1 in single junction transmons by repeated T 1 measurements in the frequency vicinity of the bare qubit transition, via the AC-Stark effect. Across 10 qubits, we observe strong correlations between the mean T 1 averaged over approximately nine months and a snapshot of an equally weighted T 1 average over the Stark shifted frequency range. These observations are suggestive of an ergodic-like spectral diffusion of TLSs dominating T 1 , and offer a promising path to more rapid T 1 characterization for device screening and process optimization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Implementation of a real-time MSE system

Motional Stark effect polarimetry is a key diagnostic for plasma fusion research since its usage on PBX-M. The MSE diagnostic measures the radial magnetic pitch angle profile in a plasma from a neutral beam by observation of Stark split D-alpha emission from atoms excited by collision with ions and electrons in the plasma. The pitch angle measurement is used with equilibrium reconstruction codes to determine the q-profile for studies of plasma stability, confinement, and transport. Historically, the algorithm was used in a post-processing fashion. The goal of our work was to apply this method in real time and pass the results to the plasma control system computer for real-time equilibrium reconstruction and control.

Instruments & Instrumentation↗

Full-wave model for the lower hybrid wave electric field vector with synthetic turbulence on Alcator C-Mod

The effects of synthetic turbulence on lower hybrid (LH) wave field magnitude and polarization are studied on Alcator C-Mod. Three synthetic turbulence models are evaluated to assess the impact of filaments, holes, and periodic fluctuations on the LH wave electric fields. For all three cases, the synthetic turbulence can greatly impact the LH wave magnitude and polarization. Back scattering, interference and edge/SOL absorption of the LH wave is observed. This impact is shown to depend on the wavelength and amplitude of the fluctuations. The strongest effect appears for fluctuations at high amplitudes and wavelengths comparable to the LH wavelength. This synthetic turbulence model can be used as inputs into a synthetic diagnostic to calculate the lower hybrid wave field magnitude and direction measured by dynamic Stark effect spectroscopy. It will be shown that fluctuations at these high amplitudes and wavelengths may explain the experimentally measured results. Here, the effect of fluctuations on modifying LH polarization are also shown to be anti-correlated with SOL power losses, similar to recently observed experimental trends on Alcator C-Mod. These SOL losses may have detrimental impact on LHCD efficiency.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Spatial heterodyne spectroscopy for fast local magnetic field measurements of magnetized fusion plasmas

A novel spectroscopy diagnostic for measuring internal magnetic fields in high temperature magnetized plasmas has been developed. It involves spectrally resolving the Balmer- α (656 nm) neutral beam radiation split by the motional Stark effect with a spatial heterodyne spectrometer (SHS). The unique combination of high optical throughput (3.7 mm 2 sr) and spectral resolution (δλ ~ 0.1 nm) allows these measurements to be made with time resolution $\ll$1 ms. The high throughput is effectively utilized by incorporating a novel geometric Doppler broadening compensation technique in the spectrometer. The technique significantly reduces the spectral resolution penalty inherent to using large area, high-throughput optics while still collecting the large photon flux provided by such optics. In this work, fluxes of order 10 10 s –1 support the measurement of deviations of <5 mT (Δ λ Stark ~ 10 –4 nm) in the local magnetic field with 50 µs time resolution. Example high time resolution measurements of the pedestal magnetic field throughout the ELM cycle of a DIII-D tokamak plasma are presented. Local magnetic field measurements give access to the dynamics of the edge current density, which is essential to understanding stability limits, edge localized mode generation and suppression, and predicting performance of H-mode tokamaks.

47 OTHER INSTRUMENTATION↗

MHD stability trends and improved performance of LHD inward-shifted configurations: The role of the neutral beam current drive and thermal plasma density

The aim of the present study is to analyze the effect of the neutral beam current drive (NBCD), thermal plasma density, and NBI operational regime on the stability of pressure gradient-driven modes (PGDM) and Alfvén eigenmodes (AE) in LHD inward-shifted configurations. The stabilization of n/m = 1/2 PGDM (n toroidal mode and m poloidal mode) is observed in the discharge 167 800 during the co-NBCD phase. The iota profile evolution measured by motional stark effect diagnostic may indicate the iota profile up-shift caused by the co-NBCD can induce a non-resonant transition of the rational surface 1/2 before the mode stabilization. The evolution of the iota profile and continuum gaps in the discharge 167 805 during the ctr-NBCD phase leads to the stabilization of the AE, caused by the narrowing of the continuum gap as the iota profile down-shift. Opposite stability trends are identified for PGDM and AE stability with respect to the thermal plasma density. A larger thermal plasma density (larger thermal β) further enhances PGDM although the continuum gaps are narrower leading to configurations with stable AEs. The linear stability of AEs is analyzed using the gyro-fluid FAR3d code to reproduce the AE stability trends observed in the experiments with respect to the NBCD and thermal plasma density. The analysis of hypothetical scenarios dedicated to study different NBI operational regimes with respect to EP energy, and β and radial density profiles indicate off-axis NBI operation shows a higher EP β threshold to destabilize AEs compared to on-axis configuration. This is explained by the presence of a TAE gap in the inner plasma region, easily destabilized by an on-axis NBI injection. The control of the NBCD and thermal plasma in the discharge 167 800 shows a transitory stabilization of PGDM and AEs, as well as an improved discharge performance identified by an increment of the neutron fluxes.

Varela, Jacobo↗

Kinetic equilibrium reconstructions of plasmas in the MAST database and preparation for reconstruction of the first plasmas in MAST upgrade

Reconstructions of plasma equilibria using magnetic sensors were routine during operation of the Mega Ampere Spherical Tokamak (MAST) device, but reconstructions using kinetic profiles were not. These are necessary for stability and disruption analysis of the MAST database, as well as for operation in the upgrade to the device, MAST-U. The three-dimensional (3D) code VALEN is used to determine eddy currents in the 3D vessel structures for vacuum coil test shots, which are then mapped to effective resistances in the two-dimensional vessel groupings in the EFIT equilibrium reconstruction code to be used in conjunction with nearby loop voltage measurements for estimated currents in the structures during reconstruction. Kinetic equilibrium reconstructions with EFIT, using all available magnetic sensors as well as Thomson scattering measurements of electron temperature and density, charge exchange recombination spectroscopy measurements of ion temperature, and internal magnetic field pitch angle measurements from a motional Stark effect (MSE) diagnostic are performed for a large database of MAST discharges. Excellent convergence errors are obtained for the portions of the discharges where the stored energy was not too low, and it is found that reconstructions performed with temperature and density measurements but without MSE data usually already match the pitch angle measurements well. A database of 275 kinetic equilibria is used to test the ideal MHD stability calculation capability for MAST. In conclusion, the necessary changes to conducting structure in VALEN, and diagnostic setup in EFIT have been completed for the upgrade from MAST to MAST-U, enabling kinetic reconstructions to commence from the first plasma discharges of the upgraded device.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Electric-field-tuned topological phase transition in ultrathin Na 3 Bi

The electric-field-induced quantum phase transition from topological to conventional insulator has been proposed as the basis of a topological field effect transistor. In this scheme, 'on' is the ballistic flow of charge and spin along dissipationless edges of a two-dimensional quantum spin Hall insulator, and 'off' is produced by applying an electric field that converts the exotic insulator to a conventional insulator with no conductive channels. Such a topological transistor is promising for low-energy logic circuits, which would necessitate electric-field-switched materials with conventional and topological bandgaps much greater than the thermal energy at room temperature, substantially greater than proposed so far. Topological Dirac semimetals are promising systems in which to look for topological field-effect switching, as they lie at the boundary between conventional and topological phases. Here we use scanning tunnelling microscopy and spectroscopy and angle-resolved photoelectron spectroscopy to show that mono- and bilayer films of the topological Dirac semimetal Na 3 Bi are two-dimensional topological insulators with bulk bandgaps greater than 300 millielectronvolts owing to quantum confinement in the absence of electric field. On application of electric field by doping with potassium or by close approach of the scanning tunnelling microscope tip, the Stark effect completely closes the bandgap and re-opens it as a conventional gap of 90 millielectronvolts. The large bandgaps in both the conventional and quantum spin Hall phases, much greater than the thermal energy at room temperature (25 millielectronvolts), suggest that ultrathin Na 3 Bi is suitable for room-temperature topological transistor operation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Modeling Competing Line-broadening Mechanisms in Neutron Star Atmospheres: Interference between Motional Stark and Ion Broadening

Neutron star surfaces have extremely high magnetic fields. In the atmosphere, the broadening of spectral lines will be substantial from the dense plasma as well as from the magnetic field. One broadening mechanism of note is due to the motional Stark effect (MSE)—an additional electric field that arises from the motion of the atom in the magnetic field. However, approximate formulae are often used to construct atmosphere models, and the MSE is assumed to be the dominant line-broadening mechanism even in ions. Detailed pressure-broadening models in these extreme magnetic fields are now currently being developed. In these more detailed models, it was suggested that the MSE may not be as large as previously predicted. If correct, this hypothesis implies that neutron star line widths might be dominated by pressure broadening rather than by motional Stark broadening. We find that, in the absence of plasma perturbations, for typical magnetic fields (B = 10 12 G), mid-Z elements, such as oxygen, have motional Stark widths of order 1 eV for transitions between dipole-allowed transitions from the ground state, though higher temperatures and transitions to higher-energy states are expected to have more broadening. The MSE also breaks down selection rules, giving rise to forbidden transitions, which have much larger widths. When plasma perturbations are included, we find that the plasma perturbation and motional Stark processes are not independent and, as a result, the spectral lines become narrow in a nontrivial way and display harmonics of the ion cyclotron frequency.

74 ATOMIC AND MOLECULAR PHYSICS↗

Excitonic Effects in Methylammonium Lead Halide Perovskites

The exciton binding energy in methylammonium lead iodide (MAPbI3) is about 10 meV, around 1/3 of the available thermal energy (k B T ~ 26 meV) at room temperature. Thus, exciton populations are not stable at room temperature at moderate photoexcited carrier densities. However, excitonic resonances dominate the absorption onset. Furthermore, these resonances determine the transient absorbance and transient reflectance spectra. The exciton binding energy is a reflection of the Coulomb interaction energy between photoexcited electrons and holes. As such, it serves as a marker for the strength of electron/hole interactions and impacts a variety of phenomena, such as, absorption, radiative recombination, and Auger recombination. In this Perspective, we discuss the role of excitons and excitonic resonances in the optical properties of lead-halide perovskite semiconductors. Finally, we discuss how the strong light-matter interactions induce an optical stark effect splitting the doubly spin degenerate ground exciton states and are easily observed at room temperature.

36 MATERIALS SCIENCE↗

Comprehensive analysis of the optical Kerr coefficient of graphene

We present a comprehensive analysis of the nonlinear optical Kerr effect in graphene. We directly solve the S-matrix element to calculate the absorption rate, utilizing the Volkov-Keldysh-type crystal wave functions. We then convert to the nonlinear refractive index coefficients through the Kramers-Kronig relation. In this formalism, the source of Kerr nonlinearity is the interplay of optical fields that cooperatively drive the transition from valence to conduction band. This formalism makes it possible to identify and compute the rates of distinct nonlinear processes that contribute to the Kerr nonlinear refractive index coefficient. The four identified mechanisms are two-photon absorption, Raman transition, self-coupling, and quadratic ac Stark effect. As a result, we present a comparison of our theory with recent experimental and theoretical results.

36 MATERIALS SCIENCE↗

Space-Time Quantum Information from the Entangled States of Magnetic Molecule (STI Product)

This collaborative project combines synthesis, measurement, and theory by three faculty members at the Eddleman Quantum Institute of UC Irvine to effectively investigate the quantum properties of molecules in the space, time, and frequency domains. Through synthetic chemistry, molecules are tailored for their magnetic and coherent properties. By combining femtosecond (fs) terahertz (THz) light and a continuous wave (cw) THz laser with a low temperature scanning tunneling microscope (STM), quantum phenomena are probed with simultaneous femtosecond temporal and atomic-scale spatial resolution. In particular, the invention of the quantum superposition microscope (QSM) advances quantum sensing for enhanced spectroscopy and imaging capabilities. Coupling theory to the experimental efforts offers a deeper understanding and predictive power for the molecular systems. The phenomena of superposition, entanglement, and coherence is central to quantum information science and can be realized in qubit states. Many systems can be modeled by a double-well potential in which two levels are formed in the two lowest energy states interacting with the environment and external radiation. In focusing on molecules as two-level systems, the underlying expectation is that their tunable composition and structure allows an effective parameter space to optimize their use as qubits for quantum sensing and computing. The THz radiation induces the superposition between the two states, appearing as temporal oscillations that damp in amplitude. Enhanced spectroscopy and imaging in the time and frequency domains is achieved through the extreme sensitivity of the frequency and damping of coherence of two-level systems to its environment. A single hydrogen molecule trapped in the STM tunneling gap experiences a double-well potential and absorption of THz femtosecond pulses of light creates the superposition of its two levels, appearing as damped oscillations in the light induced direct current (DC). The oscillation frequency depends sensitively on the electric field distribution of the copper nitride (Cu 2 N) surface, through the Stark effect, and associated with the different charge distributions at the copper and nitrogen sites and in between. This QSM can resolve variation in the surface electric field with 0.02 nanometer resolution. In addition, the single hydrogen molecule entaes with nearby hydrogen molecules as seen in the avoided level crossings of energy (oscillation frequency) versus the voltage across the tunneling gap. Thus, the first application of the QSM senses and images the surface electric field at the atomic scale. Results from this project advance fundamental understanding of quantum phenomena, develop novel synthesis, measurement, and theory, provide the knowledge foundation for molecule-based qubits and sensing that enable the development of the QSM and emergent technologies. This project trained researchers in quantum information science, extended knowledge in classrooms, and outreached to the community.

47 OTHER INSTRUMENTATION↗

Relativistic Douglas–Kroll–Hess calculations of hyperfine interactions within first-principles multireference methods

A relativistic magnetic hyperfine interaction Hamiltonian based on the Douglas–Kroll–Hess (DKH) theory up to the second order is implemented within the ab initio multireference methods, including spin–orbit coupling in the Molcas/OpenMolcas package. This implementation is applied to calculate relativistic hyperfine coupling (HFC) parameters for atomic systems and diatomic radicals with valence s or d orbitals by systematically varying active space size in the restricted active space self-consistent field formalism with restricted active space state interaction for spin–orbit coupling. The DKH relativistic treatment of the hyperfine interaction reduces the Fermi contact contribution to the HFC due to the presence of kinetic factors that regularize the singularity of the Dirac delta function in the nonrelativistic Fermi contact operator. This effect is more prominent for heavier nuclei. As the active space size increases, the relativistic correction of the Fermi contact contribution converges well to the experimental data for light and moderately heavy nuclei. The relativistic correction, however, does not significantly affect the spin-dipole contribution to the hyperfine interaction. In addition to the atomic and molecular systems, the implementation is applied to calculate the relativistic HFC parameters for large trivalent and divalent Tb-based single-molecule magnets (SMMs), such as Tb(III)Pc2 and Tb(II)(CpiPr5)2 without ligand truncation using well-converged basis sets. In particular, for the divalent SMM, which has an unpaired valence 6s/5d hybrid orbital, the relativistic treatment of HFC is crucial for a proper description of the Fermi contact contribution. Even with the relativistic hyperfine Hamiltonian, the divalent SMM is shown to exhibit strong tunability of HFC via an external electric field (i.e., strong hyperfine Stark effect).

Chemistry↗