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DOE OSTI2022

Apex hydrogen bonds in dendron assemblies modulate close-packed mesocrystal structures

The close-packed mesocrystal structures from soft-matter assemblies have recently received attention due to their structural similarity to atomic crystals, displaying various sphere-packing Frank–Kasper (FK) and quasicrystal structures. Herein, diverse mesocrystal structures are explored in second-generation dendrons (G2-X) designed with identical wedges, in which the terminal functionalities X = CONH 2 and CH 2 NH 2 represent two levels of the strong and weak hydrogen-bonding apexes, respectively. The cohesive interactions at the core apex, referred to as the core interactions, are effectively modulated by forming heterogeneous hydrogen bonds between these two functional units. For the dendron assemblies compositionally close to each pure component of G2-CONH 2 and G2-CH 2 NH 2 , their own FK A15 and C14 phases dominate other phases, respectively. We show the existence of the wide-range FK σ including the dodecagonal quasicrystal (DDQC) phases from the dendron mixtures between G2-CONH 2 and G2-CH 2 NH 2 , providing an experimental phase sequence of A15–σ–DDQC–C14 as the core interactions are alleviated. Intriguingly, the temperature dependence of particle sizes shows that the high plateau values of particle sizes are maintained equivalently until each threshold temperature (T th ), followed by a prompt decrease above the T th . A decrease in T th by alleviating the core interactions and its composition dependence suggest that the more size-dispersed particles, the more susceptibility to chain exchange with increasing temperature. Here our results on the formation of supramolecular dendron assemblies provide a guide to understand the core-interaction-dependent mesocrystal structures toward the fundamental principle underlying the temperature dependence of their particle sizes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Time evolution of a pumped molecular magnet—A time-resolved inelastic neutron scattering study

Introducing an experimental technique of time-resolved inelastic neutron scattering (TRINS), we explore the time-dependent effects of resonant pulsed microwaves on the molecular magnet Cr 8 F 8 Piv 16 . The octagonal rings of magnetic Cr 3+ atoms with antiferromagnetic interactions form a singlet ground state with a weakly split triplet of excitations at 0.8 meV. A 4.6 tesla field was applied to tune the splitting between two members of the triplet excited level |1$\rangle$ ↔ |2$\rangle$ to resonance with 105 GHz (0.434 meV) microwaves. The time-dependent occupations of the ground state |0$\rangle$, lower lying levels |1$\rangle$ and |2$\rangle$, and higher energy states |λ ≥ 3$\rangle$ were extracted during and after 20 s long microwave pulses incident along the (101) direction of a Cr 8 F 8 Piv 16 crystal held at 1.9 K. At significantly elevated spin temperatures, we found underpopulation relative to thermal equilibrium of |2$\rangle$ and spin-lattice thermalization time scales ranging from 1.6(2) s to 5.7(2) s depending on the power level. This contrasts with the relaxation time τ 1 (T → 0) = 27(5) 𝛍 s inferred for |2$\rangle$ from in situ Electron Spin Resonance measurements. By probing a broad range of excited states during intense microwave pumping, TRINS thus provides a first view of long lived excited states in a molecular antiferromagnet.

Science & Technology - Other Topics↗

DOE OSTI2025

Quantum simulation of Lindbladian dynamics via repeated interactions

The Lindblad equation generalizes the Schrödinger equation to quantum systems that undergo dissipative dynamics. The quantum simulation of Lindbladian dynamics is therefore non-unitary, preventing a naive application of state-of-the-art quantum algorithms. Here, we make use of an approximate correspondence between Lindbladian dynamics and evolution based on repeated interaction (RI) CPTP maps to write down a Hamiltonian formulation of the Lindblad dynamics and derive a rigorous error bound on the master equation. Specifically, we show that the number of interactions needed to simulate the Liouvillian within error e scales in most physical scenarios as . This is significant because the error in the Lindbladian approximation to the dynamics is not explicitly bounded in existing quantum algorithms for open system simulations. We then provide quantum algorithms to simulate RI maps using an iterative qubitization approach and Trotter–Suzuki formulas, and specifically show that for iterative qubitization the number of operations needed to simulate the dynamics (for a fixed value of ?) scales as in the limit where a0 (the coefficient 1-norm for the system and bath Hamiltonians) asymptotically dominates over the corresponding factor for the interaction Hamiltonian, which is often the case in weak coupling. This scaling would appear to be optimal if the complexity of ? is not considered, which underscores the importance of considering the error in the Liouvillian that we reveal in this work.

Quantum Computing↗

DOE OSTI2020

Anisotropic superconductivity mediated by ferroelectric fluctuations in cubic systems with spin-orbit coupling

Motivated by the experimental observation that superconductivity in bulk doped SrTiO 3 is enhanced as a putative ferroelectric quantum critical point (FE-QCP) is approached, we study the pairing instability of a cubic system in which electrons exchange low-energy ferroelectric fluctuations. Instead of the gradient coupling to the lattice distortion associated with ferroelectricity, we consider direct coupling between the electrons and the bosonic ferroelectric field that appears in the presence of spin-orbit coupling. Working in the weak-coupling regime, we find that the pairing interaction is dominated by the soft transverse optical (TO) mode, resulting in a Tc enhancement upon approaching the FE-QCP. Focusing on even-parity states, we find that although the s-wave state always wins, states with higher Cooper-pair angular momentum become close competitors as the TO mode softens. We show that the cubic anisotropy of the FE fluctuations mixes the s-wave and g-wave states, resulting in a characteristic anisotropy of the gap function. Here, the gap anisotropy behaves nonmonotonically as the FE-QCP is approached: upon decreasing the TO mode frequency, the gap anisotropy first changes sign and then increases in magnitude. We discuss the possible applications of our results to the superconducting state of SrTiO 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Area-selective atomic layer deposition enabled by competitive adsorption

In this work, we investigate the atomic layer deposition (ALD) of ZrO2 thin films on Cu and SiO2 substrates, using Zr[N(C2H5CH3)]4 as the thin-film precursor, and H2O or O2 as the coreactants. Here, we introduce 3-hexyne as a coadsorbate molecule during the thin-film precursor half-cycle and examine its effect on the selectivity of growth. We find that 3-hexyne strongly inhibits growth on Cu, while having essentially no effect on the growth on SiO2. Calculations using dispersion-inclusive density functional theory verify that 3-hexyne undergoes sp → sp2 rehybridization on Cu, which results in strong chemisorption on the metal surface, while only binding weakly to SiO2 via nonbonded van der Waals/dispersion interactions. After 10 cycles of ALD using 3-hexyne as the coadsorbate, we observed the deposition of ∼1.5 nm of ZrO2 on SiO2. On a Cu substrate, we only detected <0.15 nm of ZrO2 after the same number of cycles of ALD. At this point in the process, we find evidence of the formation of cuprous oxide (Cu2O) from in situ x-ray photoelectron spectroscopy and a significant increase in the roughness of the Cu substrate. We conclude that both factors likely contribute to the loss of selectivity due to the formation of sites (e.g., Cu2O) that bind 3-hexyne less strongly and/or an increase in the density of highly reactive sites (e.g., steps, kinks) that promote dissociative chemisorption of the thin-film precursor.

Suh, Taewon (ORCID:0000000163823811)↗

DOE OSTI2022

Braneworld cosmological effect on freeze-in dark matter density and lifetime frontier

In the 5-dimensional braneworld cosmology, the Friedmann equation of our 4-dimensional universe on a brane is modified at high temperatures while the standard Big Bang cosmology is reproduced at low temperatures. Based on two well-known scenarios, the Randall–Sundrum and Gauss–Bonnet braneworld cosmologies, we investigate the braneworld cosmological effect on the relic density of a non-thermal dark matter particle whose interactions with the Standard Model particles are so weak that its relic density is determined by the freeze-in mechanism. For dark matter production processes in the early universe, we assume a simple scenario with a light vector-boson mediator for the dark matter particle to communicate with the Standard Model particles. We find that the braneworld cosmological effect can dramatically alters the resultant dark matter relic density from the one in the standard Big Bang cosmology. As an application, we consider a right-handed neutrino dark matter in the minimal B – L extended Standard Model with a light B – L gauge boson (Z') as a mediator. We find an impact of the braneworld cosmological effect on the search for the long-lived Z' boson at the planned/proposed Lifetime Frontier experiments.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

Preliminary searches for spin-dependent interactions using sidebands of nuclear spin-precession signals

Various theories beyond the Standard Model predict new particles with masses in the sub-eV range with very weak couplings to ordinary matter. A new P-odd and T-odd interaction between polarized and unpolarized nucleons proportional to s⃗⋅r̂ is one such possibility, where r⃗=rr̂ is the spatial vector connecting the nucleons, and s⃗ is the spin of the polarized nucleon. Such an interaction involving a scalar coupling gsN at one vertex and a pseudoscalar coupling gpn at the polarized nucleon vertex can be induced by the exchange of spin-0 pseudoscalar bosons. We describe a new technique to search for interactions of this form and present the first measurements of this type. We show that future improvements to this technique can improve the laboratory upper bound on the product gsNgpn by two orders of magnitude for interaction ranges at the 100 micron scale.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Ab initio calculation of the β-decay spectrum of 6 He

Here, we calculate the β spectrum in the decay of 6 He using quantum Monte Carlo methods with nuclear interactions derived from chiral effective field theory and consistent weak vector and axial currents. We work at second order in the multipole expansion, retaining terms suppressed by O(q 2 /m$^{2}_{π}$), where q denotes low-energy scales such as the reaction’s Q value or the electron energy, and m π is the pion mass. We go beyond the impulse approximation by including the effects of two-body vector and axial currents. We estimate the theoretical error on the spectrum by using four potential models in the Norfolk family of local two- and three-nucleon interactions, which have different cutoffs, fit two-nucleon data up to different energies, and use different observables to determine the couplings in the three-body force. We find the theoretical uncertainty on the β spectrum, normalized by the total rate, to be well below the permille level, and to receive contributions of comparable size from first- and second-order corrections in the multipole expansion. We consider corrections to the β decay spectrum induced by beyond-standard-model charged-current interactions in the standard model effective field theory, with and without sterile neutrinos, and discuss the sensitivity of the next generation of experiments to these interactions.

6 ≤ A ≤ 19↗

DOE OSTI2021

Interacting fermions in narrow-gap semiconductors with band inversion

Abstract Highly unconventional behavior of the thermodynamic response functions has been experimentally observed in a narrow gap semiconductor samarium hexaboride. Motivated by these observations, we use renormalization group technique to investigate many-body instabilities in the f -orbital narrow gap semiconductors with band inversion in the limit of weak coupling. By projecting out the double occupancy of the f -states we formulate a low-energy theory describing the interacting particles in two hybridized electron- and hole-like bands. The interactions are assumed to be weak and short-ranged. We take into account the difference between the effective masses of the quasiparticles in each band. Upon carrying out the renormalization group analysis we find that there is only one stable fixed point corresponding to the excitonic instability with time-reversal symmetry breaking for small enough mismatch between the effective masses.

Physics↗

DOE OSTI2022

Pressure–strain interaction. III. Particle-in-cell simulations of magnetic reconnection

How energy is converted into thermal energy in weakly collisional and collisionless plasma processes, such as magnetic reconnection and plasma turbulence, has recently been the subject of intense scrutiny. The pressure–strain interaction has emerged as an important piece, as it describes the rate of conversion between bulk flow and thermal energy density. In two companion studies, we presented an alternate decomposition of the pressure–strain interaction to isolate the effects of converging/diverging flow and flow shear instead of compressible and incompressible flow, and we derived the pressure–strain interaction in magnetic field-aligned coordinates. Here, we use these results to study pressure–strain interaction during two-dimensional anti-parallel magnetic reconnection. We perform particle-in-cell simulations and plot the decompositions in both Cartesian and magnetic field-aligned coordinates. We identify the mechanisms contributing to positive and negative pressure–strain interaction during reconnection. Furthermore, this study provides a roadmap for interpreting numerical and observational data of the pressure–strain interaction, which should be important for studies of reconnection, turbulence, and collisionless shocks.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Chiral effective field theory calculations of weak transitions in light nuclei

In this work, we report quantum Monte Carlo calculations of weak transitions in A≤10 nuclei, based on the Norfolk two- and three-nucleon chiral interactions, and associated one- and two-body axial currents. Furthermore, we find that the contribution from two-body currents is at the 2–3% level, with the exception of matrix elements entering the rates of 8Li, 8B, and 8He β decay. These matrix elements are suppressed in impulse approximation based on the (leading order) Gamow Teller transition operator alone; two-body currents provide a 20–30% correction, which is, however, insufficient to bring theory in agreement with experimental data. For the other transitions, the agreement with the data is satisfactory, and the results exhibit a negligible to mild model dependence when different combinations of Norfolk interactions are utilized to construct the nuclear wave functions. We report a complete study of two-body weak transition densities which reveals the expected universal behavior of two-body currents at short distances throughout the range of A=3 to A=10 systems considered here.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Evolution of 1 / f Flux Noise in Superconducting Qubits with Weak Magnetic Fields

The microscopic description of 1/f magnetic flux noise in superconducting circuits has remained an open question for several decades despite extensive experimental and theoretical investigation. Recent progress in superconducting devices for quantum information has highlighted the need to mitigate sources of qubit decoherence, driving a renewed interest in understanding the underlying noise mechanism(s). Though a consensus has emerged attributing flux noise to surface spins, their identity and interaction mechanisms remain unclear, prompting further study. Here, we apply weak in-plane magnetic fields to a capacitively shunted flux qubit (where the Zeeman splitting of surface spins lies below the device temperature) and study the flux-noise-limited qubit dephasing, revealing previously unexplored trends that may shed light on the dynamics behind the emergent 1/f noise. Notably, we observe an enhancement (suppression) of the spin-echo (Ramsey) pure-dephasing time in fields up to B = 100 G. With direct noise spectroscopy, we further observe a transition from a 1/f to approximately Lorentzian frequency dependence below 10 Hz and a reduction of the noise above 1 MHz with increasing magnetic field. Here, we suggest that these trends are qualitatively consistent with an increase of spin cluster sizes with magnetic field. These results should help to inform a complete microscopic theory of 1/f flux noise in superconducting circuits.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2026

Design Rules for Open-Shell Molecular Wires: Insights from Correlated Many-Body Transport

Open-shell π-conjugated systems have emerged as promising molecular wires that can sustain unusually high low-bias conductance over tens of nanometers. However, predictive design rules remain limited because near-degeneracy and spin polarization give rise to correlated electronic states that are not reliably captured by standard density functional theory and Landauer transport descriptions. Here, we establish physically transparent design rules for long-range, weakly length-dependent charge transport based on the interplay between bond-length alternation and electron–electron interactions. Using a fully correlated transport framework that combines density matrix renormalization group calculations with nonequilibrium Green’s function embedding, we show that weak dimerization maintains spatially extended edge states, while moderate on-site interaction stabilizes open-shell character without excessively separating transport-relevant resonances. This balance yields zero-bias transmission that is largely insensitive to molecular length, providing a route to connect chemically tunable structure to correlated transport beyond mean-field descriptions.

Charge transport↗

DOE OSTI2022

TOLERANCES OF CRAB DISPERSION AT THE INTERACTION POINT IN THE HADRON STORAGE RING OF THE ELECTRON-ION COLLIDER

The Electron Ion Collider (EIC) presently under construction at Brookhaven National Laboratory will collide polarized high energy electron beams with hadron beams with luminosities up to 10^34 cm^?2 s^?1 in the center mass energy range of 20-140 GeV. Due to the detector solenoid in the interaction region, the design horizontal crabbing angle will be coupled to the vertical plane if uncompensated. In this article, we study the tolerances of crab dispersion at the interaction point in the EIC Hadron Storage Ring (HSR). Both strong-strong and weak-strong simulations are used. We found that there is a tight tolerance of vertical crabbing angle at the interaction point in the HSR.

Luo, Y.↗

DOE OSTI2022

TOLERANCES OF CRAB DISPERSION AT THE INTERACTION POINT IN THE HADRON STORAGE RING OF THE ELECTRON-ION COLLIDER

Luo, Y.↗

DOE OSTI2020

Signatures of self-interacting dark matter on cluster density profile and subhalo distributions

Non-gravitational interactions between dark matter particles with strong scattering, but relatively small annihilation and dissipation, has been proposed to match various observables on cluster and group scales. In this paper, we present the results from large cosmological simulations which include the effects of different self-interaction scenarios. In particular we explore a model with the differential cross section that can depend on both the relative velocity of the interacting particles and the angle of scattering. We focus on how quantities, such as the stacked density profiles, subhalo counts and the splashback radius change as a function of different forms of self-interaction. We find that self-interactions not only affect the central region of the cluster, the effect well known from previous studies, but also significantly alter the distribution of subhalos and the density of particles out to the splashback radius. Therefore, our results suggest that current weak lensing data can already put constraints on the self-interaction cross-section that are only slightly weaker than the Bullet Cluster constraints (σ/m ≲ 2 cm 2 /g), and future lensing surveys should be able to tighten them even further making halo profiles on cluster scales a competitive probe for DM physics.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Building Cybersecurity Educational Materials for Students: The Windfarm Capture-The-Flag Exercise

Securing and protecting critical infrastructure in an increasingly digital world is vital but it is all too often an afterthought. It is especially important that students become aware of internet safety and security at an early age. However, the availability of interactive and educational cybersecurity material targeted toward students is minimal in the United States. Here we show an example of interactive cyber security educational material that an educator can use in their classroom to encourage students to think about the interaction between real-world physical objects, cyber security, and information security. By putting together a “capture-the-flag” exercise, students can see in real time how hackers and cybercriminals exploit vulnerabilities and gain access information. The students try to “capture” the “flag” (i.e., information) in the wind farm by looking for oddities in the code or by taking advantage of weaknesses in everyday protocols. Students can also see how cybersecurity interacts with the power grid through the wind farm project scenario and how a hacker could cause serious problems to a critical infrastructure sector. Our goal for the project is getting students interested in cybersecurity and help them develop an awareness of how important having robust security systems is. We also hope that this project demonstrates the importance of introducing these concepts early and inspires others to create similar projects geared toward students.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2020

Role of weak interlayer coupling in ultrafast exciton-exciton annihilation in two-dimensional rhenium dichalcogenides

Strong interactions between excitons are a characteristic feature of two-dimensional (2D) semiconductors, determining important excitonic properties, such as exciton lifetime, coherence, and photon-emission efficiency. Rhenium disulfide (ReS 2 ), a member of the 2D transition-metal dichalcogenide (TMD) family, has recently attracted great attention due to its unique excitons that exhibit excellent polarization selectivity and coherence features. However, an in-depth understanding of exciton-exciton interactions in ReS 2 is still lacking. In this work, we used ultrafast pump-probe spectroscopy to study exciton-exciton interactions in monolayer (1L), bilayer (2L), and triple layer ReS 2 . Additionally, we directly measure the rate of exciton-exciton annihilation, a representative Auger-type interaction between excitons. It decreases with increasing layer number, as observed in other 2D TMDs. However, while other TMDs exhibit a sharp weakening of exciton-exciton annihilation between 1L and 2L, such behavior was not observed in ReS 2 . We attribute this distinct feature in ReS 2 to the relatively weak interlayer coupling, which prohibits a substantial change in the electronic structure when the thickness varies. This work not only highlights the unique excitonic properties of ReS 2 but also provides novel insight into the thickness dependence of exciton-exciton interactions in 2D systems.

36 MATERIALS SCIENCE↗