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DOE OSTI2025

End-to-end protocol for high-quality quantum approximate optimization algorithm parameters with few shots

The quantum approximate optimization algorithm (QAOA) is a quantum heuristic for combinatorial optimization that has been demonstrated to scale better than state-of-the-art classical solvers for some problems. For a given problem instance, QAOA performance depends crucially on the choice of the parameters. While average-case optimal parameters are available in many cases, meaningful performance gains can be obtained by fine-tuning these parameters for a given instance. This task is especially challenging, however, when the number of circuit executions (shots) is limited. In this work, we develop an end-to-end protocol that combines multiple parameter settings and fine-tuning techniques. We use large-scale numerical experiments to optimize the protocol for the shot-limited setting and observe that optimizers with the simplest internal model (linear) perform best. We implement the optimized pipeline on a trapped-ion processor using up to 32 qubits and 5 QAOA layers, and we demonstrate that the pipeline is robust to small amounts of hardware noise. To the best of our knowledge, these are the largest demonstrations of QAOA parameter fine-tuning on a trapped-ion processor in terms of two-qubit gate count.

quantum algorithms & computation↗

DOE OSTI2020

Single-ion addressing via trap potential modulation in global optical fields

To date, individual addressing of ion qubits has relied primarily on local Rabi or transition frequency differences between ions created via electromagnetic field spatial gradients or via ion transport operations. Alternatively, it is possible to synthesize arbitrary local one-qubit gates by leveraging local phase differences in a global driving field. Here we report individual addressing of 40 Ca + ions in a two-ion crystal using axial potential modulation in a global gate laser field. We characterize the resulting gate performance via one-qubit randomized benchmarking, applying different random sequences to each co-trapped ion. We identify the primary error sources and compare the results with single-ion experiments to better understand our experimental limitations. These experiments form a foundation for the universal control of two ions, confined in the same potential well, with a single gate laser beam.

quantum computing↗

DOE OSTI2021

Practical verification protocols for analog quantum simulators

Abstract Analog quantum simulation is expected to be a significant application of near-term quantum devices. Verification of these devices without comparison to known simulation results will be an important task as the system size grows beyond the regime that can be simulated classically. We introduce a set of experimentally-motivated verification protocols for analog quantum simulators, discussing their sensitivity to a variety of error sources and their scalability to larger system sizes. We demonstrate these protocols experimentally using a two-qubit trapped-ion analog quantum simulator and numerically using models of up to five qubits.

Physics↗

DOE OSTI2026

Spectroscopy and dynamics of the v = 1 levels derived from the OH(D) stretching modes in the I‾∙HDO complex using CW and time-resolved, resonant two-photon infrared excitation of the cryogenically cooled ions

The vibrational energy levels of the two isotopomers adopted by the I‾∙HDO ion-molecule complex occur such that the OH(D) stretching fundamentals span its dissociation energy, thus enabling a spectroscopic investigation of the dynamics displayed by a system prepared in the vicinity of the dissociation threshold. This regime is explored using infrared photoexcitation of the mass-selected complexes cooled in a cryogenic radiofrequency (Paul) ion trap. Survey spectra are obtained at modest resolution using two-color, IR-IR photodissociation with nanosecond lasers to establish the level structure and unimolecular decay dynamics of the v = 1 and 2 levels of the bound OH(D) oscillator. The v = 1 levels are prepared by fixed frequency excitation in the trap and the absorption spectra arising from this excited state are probed by photofragmentation of the complex with a second pulsed IR laser after a variable delay time (0 to 20 ms). The transitions to levels above the dissociation threshold for I‾ + HDO formation are observed to be sharp (~5 cm -1 FWHM). At low pressure, the bound OD (v = 1) population relaxes very slowly (~3 ms), consistent with resonant fluorescence in the IR. The collisional quenching rate constants of this level by the He buffer gas were estimated to be on the order 3 x 10 -12 cm 3 /s based on a crude Stern-Volmer analysis. Here, the rotational fine structure and linewidths (≲0.01 cm -1 FWHM) arising from transitions of the non-bonded OH stretch fundamental of the OD-bound isotopomer that lies just above the dissociation energy are determined using single photon photodissociation by excitation of the 10 K ions with a single-frequency, CW IR laser in the ion trap.

Cryogenic ion infrared spectroscopy↗

DOE OSTI2021

Bound state dynamics in the long-range spin- 1 2 XXZ model

Experimental platforms based on trapped ions, cold molecules, and Rydberg atoms have made possible the investigation of highly nonlocal spin-1 / 2 Hamiltonians with long-range couplings. Here, we study the effects of such nonlocal couplings in the long-range spin-1 / 2 XXZ Heisenberg Hamiltonian. Here, we calculate explicitly the two-spin energy spectrum, which describes all possible energetic configurations of two spins pointing in a specific direction embedded in a background of spins with opposite orientation. For fast decay of the spin-spin couplings, we find that the two-spin energy spectrum is characterized by well-defined discrete values, corresponding to bound states, separated by a set of continuum states describing the scattering region. In the deep long-range regime instead, the bound states disappear as they get incorporated by the scattering region. The presence of two-spin bound states results to be crucial to determine both two- and many-spin dynamics. On one hand, radically different two-spin spreadings can be observed by tuning the decay of the spin couplings. On the other hand, two-spin bound states enable the dynamical stabilization of effective antiferromagnetic states in the presence of ferromagnetic couplings. Finally, we propose a novel scheme based on a trapped-ion quantum simulator to experimentally realize the long-range XXZ model and to study its out-of-equilibrium properties.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2020

Mapping the Temperature-dependent and network site-specific onset of spectral diffusion at the surface of a water cluster cage

We explore the kinetic processes that sustain equilibrium in a microscopic, finite system. This is accomplished by monitoring the spontaneous, time-dependent frequency evolution (the frequency autocorrelation) of a single OH oscillator, embedded in a water cluster held in a temperature-controlled ion trap. The measurements are carried out by applying two-color, IR-IR photodissociation mass spectrometry to the D3O+?(HDO)(D2O)19 isotopologue of the “magic number” protonated water cluster, H+?(H2O)21. The OH group can occupy any one of the five spectroscopically distinct sites in the distorted pentagonal dodecahedron cage structure. The OH frequency is observed to evolve over tens of milliseconds in the temperature range (90-120 K). Starting at 100 K, large “jumps” are observed between two OH frequencies separated by ~300 cm-1 indicating migration of the OH group from the bound OH site at 3350 cm-1 to the free position at 3686 cm-1. Increasing the temperature to 110 K leads to partial interconversion among many sites. All sites are observed to interconvert at 120 K such that the distribution of the unique OH group among them adopts the form one would expect for a canonical ensemble. The spectral dynamics displayed by the clusters thus offer an unprecedented view into the molecular-level processes that drive spectral diffusion in an extended network of water molecules.

Yang, Nan↗

DOE OSTI2022

Effects of Molecular Size on Resolution in Charge Detection Mass Spectrometry

Instrumental resolution of Fourier transform-charge detection mass spectrometry instruments with electrostatic ion trap detection of individual ions depends on the precision with which ion energy is determined. Energy can be selected using ion optic filters or from harmonic amplitude ratios (HARs) that provide Fellgett’s advantage and eliminate the necessity of ion transmission loss to improve resolution. Unlike the ion energy-filtering method, the resolution of the HAR method increases with charge (improved S/N) and thus with mass. An analysis of the HAR method with current instrumentation indicates that higher resolution can be obtained with the HAR method than the best resolution demonstrated for instruments with energy-selective optics for ions in the low MDa range and above. However, this gain is typically unrealized because the resolution obtainable with molecular systems in this mass range is limited by sample heterogeneity. Here, this phenomenon is illustrated with both tobacco mosaic virus (0.6–2.7 MDa) and AAV9 (3.7–4.7 MDa) samples where mass spectral resolution is limited by the sample, including salt adducts, and not by instrument resolution. Nevertheless, the ratio of full to empty AAV9 capsids and the included genome mass can be accurately obtained in a few minutes from 1× PBS buffer solution and an elution buffer containing 300+ mM nonvolatile content despite extensive adduction and lower resolution. Empty and full capsids adduct similarly indicating that salts encrust the complexes during late stages of droplet evaporation and that mass shifts can be calibrated in order to obtain accurate analyte masses even from highly salty solutions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Electron Trapping and Ion Leaching at the Li-Modified Quartz–Water Interface

Electrons and ions at metal oxide-water interfaces have a critical role in many phenomena and applications, thus making their properties of considerable interest. We here investigate the behavior of a lithium impurity at the water interface with Li-doped SiO 2 using hybrid density functional based ab initio molecular dynamics simulations. We find that the excess electron donated by the lithium dopant localizes on a surface silicon atom and is partially solvated at the aqueous interface. While the position of the excess electron does not change during our ~60 ps simulation, the lithium cation diffuses from its initial position in the SiO 2 subsurface toward the interface and eventually leaches out of the oxide surface and becomes solvated by four water molecules, forming an aqueous Li+- electron complex at the interface. The degree of interaction between the localized electron and the lithium ion controls not only the energy level of the excess electron but also the extent of structural distortion and hydrogen-bonding at the interface. The results of our study can be relevant for understanding the initial stages of glass corrosion, where alkali ions are leached from the surface region by interactions with water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Cross-beam energy transfer in direct-drive ICF. I. Nonlinear and kinetic effects

Results are presented from a series of simulations examining the susceptibility of the cross-beam energy transfer (CBET) instability to nonlinear processes in the context of direct-drive inertial confinement fusion experiments on the OMEGA laser facility. These form the basis for the second paper of this series [A. G. Seaton, L. Yin, R. Follett, B. J. Albright, and A. Le, “Cross-beam energy transfer in direct-drive ICF. II. Theory and simulation of mitigation through increased laser bandwidth,” Phys. Plasmas 29, 042707 (2022)], where we examine the efficacy of increases in laser bandwidth at suppressing CBET. We choose laser and plasma conditions for the simulations that are favorable to CBET and promote nonlinearity. Through a comparison of outputs from the particle-in-cell code vector particle in cell (VPIC) and the linearized fluid code laser-plasma simulation environment (LPSE), a series of nonlinear effects have been identified in the kinetic simulations that include particle trapping, the two-ion wave decay, and ion-acoustic wave self-focusing. These effects produce time-dependent energy transfer, in contrast to the linearized fluid simulations in which a steady state is reached after an initial transient. Ion trapping is shown to allow for increased energy transfer relative to fluid simulations, with the remaining nonlinear processes acting to reduce the energy transfer. Nonlinear dynamics is contrasted for low- and high-intensity beams as well as between speckled and planar beams. For the parameters under consideration, beam profile has a significant effect on nonlinear dynamics, though the greatest sensitivity is to beam intensity.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Cross-Beam Energy Transfer Saturation by Ion Heating

Cross-beam energy transfer (CBET) saturation by ion heating was measured in a gas-jet plasma characterized using Thomson scattering. Here, a wavelength-tunable ultraviolet (UV) probe laser beam was interacted with four intense UV pump beams to drive large-amplitude ion-acoustic waves. For the highest-intensity interactions, the power transferred to the probe laser dropped, demonstrating ion-acoustic wave saturation. Over this time, the ion temperature was measured to increase by a factor of 7 during the 500-ps interaction. Particle-in-cell simulations show ion trapping and a subsequent ion heating consistent with measurements. Linear kinetic CBET models were found to agree well with the observed energy transfer when the measured plasma conditions were used.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Evaluating Ion Accumulation and Storage in Traveling Wave Based Structures for Lossless Ion Manipulations

Structures for lossless ion manipulations (SLIM) technology has demonstrated high resolving power ion mobility separation and flexibility to integrate complex ion manipulations into a single experimental platform. To enable IMS separations, trapping/accumulating ions inside SLIM (or in-SLIM) prior to injection of a packet for separations provides ease of operation and reduces the need for dedicated ion traps external to SLIM. To fully characterize the ion accumulation process, we have evaluated the effect of TW amplitudes, ion collection times, and storage times on the “in-SLIM” accumulation process. The study utilized a SLIM module comprising 5 distinct tracks, each with a specific ion accumulation configuration. The effect of the TW conditions on the accumulation process was investigated for a 3-peptide mixture: kemptide, angiotensin II, and neurotensin at a TW speed of 106 m/s. The effect of ion accumulation time/collection time and storage time was investigated, in addition to TW amplitude. Overall, the signal of the analyte ions increased when the ion collection time increased from 49 to 163 ms but decreased when the ion collection time increased further to 652 ms due to the space charge effects. Ion losses were observed at high TW amplitudes (e.g., 15 V p–p and 20 V p–p ). In addition, under space charge conditions (e.g., collection times of 163 and 652 ms), the signal of the analyte ions decreased with an increase in storage times for all TW amplitudes applied to the trapping region. For ion accumulation, the data indicate that gentler TW conditions must be utilized to minimize ion losses and fragments to benefit from the “in-SLIM” accumulation process. Finally, wider SLIM tracks provided better performance than those with narrower tracks.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Sheath transitions in a cylindrical filament discharge: Axisymmetric 1D3V PIC-MCC simulations

We present the first nonplanar hot cathode discharge simulations that capture the role of the trapped-ions plasma, elucidating new phenomena unobservable in planar geometric discharges. A discharge struck between a single emitting wire filament cathode and a bounding anode is simulated in cylindrical geometry using an axisymmetric (radial) particle-in-cell Monte-Carlo collisions code. Operating the discharge near its ionization energy threshold can lead to the formation of a two plasma mode (TPM). One plasma forms in the conventional upstream region through electron impact ionization of background neutrals. A second plasma, whose global effect on the discharge was not previously well understood, forms downstream through the trapping of cold ions in the potential well of the filament’s virtual cathode, a process enabled by ion-neutral charge exchange collisions. Three space charge regions intersperse the electrode gap—an emissive sheath between the cathode filament and trapped-ions plasma, a double layer between the two plasmas, and a classical sheath between the upstream plasma and the outer anode. Simulations exhibit mode transitions and quenching instabilities that transform the discharge between the TPM and other single-plasma sheath modes that include classical (temperature-limited), space charge limited, and inverse (anode glow) modes. The transitions are explained via “aid-and-compete” dynamics wherein the growth of one plasma enhances growth in the other while concurrently exhibiting expansion dynamics antagonistic to each other. The system exhibits strong hysteresis memory during the mode transitions. Improved understanding and control of these sheath mode transitions are expected to benefit plasma applications with hot cathodes.

Electrical hysteresis↗

DOE OSTI2023

The competing effects of wave amplitude and collisions on multi-ion species suppression of stimulated Brillouin scattering in inertial confinement fusion Hohlraums

Reduction in stimulated Brillouin scattering (SBS) from National Ignition Facility Hohlraums has been predicted through the use of multi-ion species materials on Hohlraum walls. This approach to controlling SBS is based upon introducing a lighter ion species to the heavier ion species Hohlraum wall in order to greatly increase the ion Landau damping of ion acoustic waves (IAWs). In a collisionless plasma, if the IAWs driven by SBS reach sufficient amplitudes, this increased damping is reduced or even eliminated by ion trapping in the IAWs. Here, the nonlinear behavior of IAWs is simulated with a multi-ion species Vlasov code, including interspecies ion–ion collisions, self-collisions, and electron–ion pitch-angle collisions. The effect of collisions on the trapping of ions and electrons in a large-amplitude IAW is studied in a regime of relevance to current Inertial Confinement Fusion experiments. Our simulations show that collisions can scatter trapped particles out of resonance with the IAW, suppressing trapping and helping to maintain an effective Landau damping of the IAW. The IAW amplitude required to trap particles in the presence of strong collisions is estimated analytically. These estimates are tested for strongly damped IAWs in tantalum oxide and pure helium plasmas. Here our simulations show that, above a threshold amplitude, the damping is reduced by an amount inversely proportional to the wave amplitude. Thus, the success of controlling SBS using a multispecies plasma may depend sensitively on laser power and pulse length.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Coupling Two Laser-Cooled Ions via a Room-Temperature Conductor

We demonstrate coupling between the motions of two independently trapped ions with a separation distance of 620 μm. Here, the ion-ion interaction is enhanced via a room-temperature electrically floating metallic wire which connects two surface traps. Tuning the motion of both ions into resonance, we show flow of energy with a coupling rate of 11 Hz. Quantum-coherent coupling is hindered by strong surface electric-field noise in our device. Our ion-wire-ion system demonstrates that room-temperature conductors can be used to mediate and tune interactions between independently trapped charges over distances beyond those achievable with free-space dipole-dipole coupling. This technology may be used to sympathetically cool or entangle remotely trapped charges and enable coupling between disparate physical systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Energetic particle transport and loss induced by helically-trapped energetic-ion-driven resistive interchange modes in the Large Helical Device

Here, energetic-ion confinement and loss due to energetic-ion driven magnetohydrodynamic modes are studied using comprehensive neutron diagnostics and orbit-following numerical simulations for the Large Helical Device (LHD). The neutron flux monitor is employed in order to obtain global confinement of energetic ions and two installed vertical neutron cameras (VNCs) viewing different poloidal cross-sections are utilized in order to measure the radial profile of energetic ions. A strong helically-trapped energetic-ion-driven resistive interchange mode (EIC) excited in relatively low-density plasma terminated high-temperature state in LHD. Changes in the neutron emission profile due to the EIC excitation are clearly visualized by the VNCs. The reduction in the neutron signal for the helical ripple valley increases with EIC amplitude, which reaches approximately 50%. In addition to the EIC experiment, orbit-following simulations using the DELTA5D code with EIC fluctuations were performed to assess the energetic-ion transport and loss. Two-dimensional temporal evolution results show that the neutron emissivity at the helical ripple decreases significantly due to the EIC. The rapid reduction in neutron emissivity shows that the helically-trapped beam ions immediately escape from the plasma. The reduction in the VNC signals for the helical ripple valley and the total neutron emission rate increase with increasing EIC amplitude, as observed in the experiment. Calculated line-integrated neutron emission results show that the profile measured by VNC1 has one peak, whereas the profile measured by VNC2 has two peaks, as observed in the experiment. Although the neutron emission profile for VNC2 has a relatively wide peak compared with the experimental results, the significant decrease in neutron signal corresponding to the helical ripple valley was successfully reproduced.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Lithium-like O 5+ Emission near 19 Å

Using a high-resolution grating spectrometer on the Livermore EBIT-I electron beam ion trap, we have measured three n = 3,4 → n = 1 K-shell emission lines in lithiumlike O 5+ , which are situated near the O VIII Lyman-α lines at 19 Å. Two of the resulting wavelengths agree well with the wavelengths of these lines we reported earlier, but the wavelength of the third line does not. In contrast, our new wavelengths now fully agree with those from resonant photo-absorption experiments on the PETRA III synchrotron facility.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2023

Time-dependent saturation and physics-based nonlinear model of cross-beam energy transfer

The nonlinear physics of cross-beam energy transfer (CBET) for multi-speckled laser beams is examined using large-scale particle-in-cell simulations for a range of laser and plasma conditions relevant to indirect-drive inertial confinement fusion (ICF) experiments. The time-dependent growth and saturation of CBET involve complex, nonlinear ion and electron dynamics, including ion trapping-induced enhancement and detuning, ion acoustic wave (IAW) nonlinearity, oblique forward stimulated Raman scattering (FSRS), and backward stimulated Brillouin scattering (BSBS) in a CBET-amplified seed beam. Ion-trapping-induced detuning of CBET is captured in the kinetic linear response by a new δf-Gaussian-mixture algorithm, enabling an accurate characterization of trapping-induced non-Maxwellian distributions. Ion trapping induces nonlinear processes, such as changes to the IAW dispersion and nonlinearities (e.g., bowing and self-focusing), which, together with pump depletion, FSRS, and BSBS, determine the time-dependent nature and level of CBET gain as the system approaches a steady state. Using VPIC simulations at intensities at and above the onset threshold for ion trapping and the insight from the time-dependent saturation analyses, we construct a nonlinear CBET model from local laser and plasma conditions that predicts the CBET gain and the energy deposition into the plasma. This model is intended to provide a more accurate, physics-based description of CBET saturation over a wide range of conditions encountered in ICF hohlraums compared with linear CBET gain models with ad hoc saturation clamps often used in laser ray-based methods in multi-physics codes.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Floquet Gauge Pumps as Sensors for Spectral Degeneracies Protected by Symmetry or Topology

We introduce the concept of a Floquet gauge pump whereby a dynamically engineered Floquet Hamiltonian is employed to reveal the inherent degeneracy of the ground state in interacting systems. We demonstrate this concept in a one-dimensional XY model with periodically driven couplings and transverse field. In the high-frequency limit, we obtain the Floquet Hamiltonian consisting of the static XY and dynamically generated Dzyaloshinsky-Moriya interaction (DMI) terms. The dynamically generated magnetization current depends on the phases of complex coupling terms, with the XY interaction as the real and DMI as the imaginary part. As these phases are cycled, the current reveals the ground-state degeneracies that distinguish the ordered and disordered phases. In conclusion, we discuss experimental requirements needed to realize the Floquet gauge pump in a synthetic quantum spin system of interacting trapped ions.

74 ATOMIC AND MOLECULAR PHYSICS↗