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At least 37 records · Page 2

Parametric and Robustness Studies of Qudit Mediated Quantum State Transfer and Entanglement Creation

The large number of available states participating in quantum state evolution in a system of qudits translates into better thermal resilience, for quantum state transfer (QST) and distributed entangled states, than a system of 2-level qubits. In this report we study the dependence of fidelities of the above processes on various system parameters. Sensitivity to modes of dissipation and errors is also studied. An alternative and potentially more efficient scheme to create Bell states is used.

Chao, Yu-Chiu [Fermilab] (ORCID:000900039584159X)↗

Evolution of an Asteroid Family under YORP, Yarkovsky, and Collisions

Any population of asteroids, like asteroid families, will disperse in semimajor axis due to the Yarkovsky effect. The amount of drift is modulated by the asteroid spin state evolution, which determines the balance between the diurnal and seasonal Yarkovsky forces. The asteroid’s spin state is, in turn, controlled in part by the Yarkovsky–O’Keefe–Radzievskii–Paddack (YORP) effect. The otherwise smooth evolution of an asteroid can be abruptly altered by collisions, which can cause impulsive changes in the spin state and can move the asteroid onto a different YORP track. In addition, collisions may also alter the YORP parameters by changing the superficial features and overall shape of the asteroid. Thus, the coupling between YORP and Yarkovsky is also strongly affected by the impact history of each body. To investigate this coupling, we developed a statistical code modeling the time evolution of semimajor axis under YORP–Yarkovsky coupling. It includes the contributions of NYORP (normal YORP), TYORP (tangential YORP), and collisions whose effects are deterministically calculated and not added in a statistical way. We find that both collisions and TYORP increase the dispersion of a family in semimajor axis by making the spin axis evolution less smooth and regular. We show that the evolution of a family’s structure with time is complex and collisions randomize the YORP evolution. In our test families, we do not observe the formation of a “YORP-eye” in the semimajor axis versus diameter distribution, even after a long period of time. If present, the “YORP-eye” might be a relic of an initial ejection velocity pattern of the collisional fragments.

79 ASTRONOMY AND ASTROPHYSICS↗

A time-parallel multiple-shooting method for large-scale quantum optimal control

Quantum optimal control plays a crucial role in quantum computing by providing the interface between compiler and hardware. Solving the optimal control problem is particularly challenging for multi-qubit gates, due to the exponential growth in computational complexity with the system's dimensionality and the deterioration of optimization convergence. To ameliorate the computational complexity of time-integration, this paper introduces a multiple-shooting approach in which the time domain is divided into multiple windows and the intermediate states at window boundaries are treated as additional optimization variables. Further, this enables parallel computation of state evolution across time-windows, significantly accelerating objective function and gradient evaluations. Since the initial state matrix in each window is only guaranteed to be unitary upon convergence of the optimization algorithm, the conventional gate trace infidelity is replaced by a generalized infidelity that is convex for non-unitary state matrices. Continuity of the state across window boundaries is enforced by equality constraints. A quadratic penalty optimization method is used to solve the constrained optimal control problem, and an efficient adjoint technique is employed to calculate the gradients in each iteration. We demonstrate the effectiveness of the proposed method through numerical experiments on quantum Fourier transform gates in systems with 2, 3, and 4 qubits, noting a speedup of 80x for evaluating the gradient in the 4-qubit case, highlighting the method's potential for optimizing control pulses in multi-qubit quantum systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Unraveling the Surface Termination and Evolution of Surface States for Electrocatalyst PtSn 4 in Alkaline HER

Semimetal PtSn 4 has been experimentally demonstrated as a promising topological electrocatalyst for the hydrogen evolution reaction (HER) under both acidic and alkaline conditions. While two possible mechanisms have been proposed to explain its activity, the role of its surface states in HER remains unclear. It is indeed in question how the surface states of this alloy evolve as HER proceeds. In this study, we investigate the surface termination that sustains conducting surface states on PtSn 4 , and we track their evolution during HER catalysis. We show that a reconstructed surface with a Sn-poor termination reproduces the scanning tunneling microscopy pattern observed in experiments and sustains a conducting surface. Through phase diagram and geometric structure analysis, we outline the HER profile following the Volmer–Heyrovsky mechanism. As hydrogen atoms adsorb onto the surface, the structure undergoes further reconstruction to an equilibrium phase with a coverage of two hydrides per unit cell. Meanwhile, the surface electronic bands evolve in response to interactions with the adsorbed hydrogen atoms. A hybridization diagram is further proposed for understanding the surface state evolution based on wave function and chemical bonding analyses. While the Pt atoms serve as conventional sites for hydrogen binding, the surface states of PtSn 4 are essential for stabilizing the hydrogen antibonding states via in-phase electronic interactions with the Sn components. This stabilization results in frontier surface bands that are responsible for driving the HER catalysis. Here, our findings provide a detailed description for the direct involvement of surface states on PtSn4 when employed as a catalyst for HER.

catalysts↗

Dissociative electron recombination and rotational cooling of the deuterated triatomic hydrogen ions H 2 ⁡D + and D 2 ⁢H +

We have measured the dissociative recombination (DR) of the deuterated triatomic hydrogen ions H 2 ⁡D + and D 2 ⁢H + as a function of storage time at the Cryogenic Storage Ring (CSR). Both molecular ions were stored for up to 1000 s inside the cryogenic vacuum of the CSR prior to the electron recombination measurements, allowing them to cool to their lowest rotational states. We implement a comprehensive model for all relevant processes to predict the internal state evolution of the ions during storage inside the CSR, employing calculated radiative transition strengths and state-selective rate coefficients for electron collisions. Our DR rate coefficient measurements with deuterated triatomic hydrogen ions in defined quantum states allow for meaningful comparisons with state-of-the-art theoretical calculations, paving the way for a better understanding of the complex DR process for polyatomic molecular ions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Best of both worlds: Enforcing detailed balance in machine learning models of transition rates

The slow microstructural evolution of materials often plays a key role in determining material properties. When the unit steps of the evolution process are slow, direct simulation approaches such as molecular dynamics become prohibitive and Kinetic Monte-Carlo (kMC) algorithms, where the state-to-state evolution of the system is represented in terms of a continuous-time Markov chain, are instead frequently relied upon to efficiently predict long-time evolution. The accuracy of kMC simulations however relies on the complete and accurate knowledge of reaction pathways and corresponding kinetics. This requirement becomes extremely stringent in complex systems such as concentrated alloys where the astronomical number of local atomic configurations makes the a priori tabulation of all possible transitions impractical. Machine learning models of transition kinetics have been used to mitigate this problem by enabling the efficient on-the-fly prediction of kinetic parameters. While conventional KMC methods based on transition state theory naturally yield reversible dynamics that exactly obey the detailed balance criterion, providing strong guarantees on the properties of the stationary distribution, many recently-proposed ML-based approaches to barrier predictions provide no such guarantees. In this study, we derive conditions under which physics-informed ML architectures exactly enforce the detailed balance condition by construction, even when relying on non-extensive descriptions of states in terms of local environments around mobile defects. In conclusion, using the diffusion of a vacancy in a concentrated alloy as an example, we show that such ML architectures also exhibit superior performance in terms of prediction accuracy, demonstrating that the imposition of physical constraints can facilitate the accurate learning of barriers at no increase in computational cost.

36 MATERIALS SCIENCE↗

Advancing Multiscale Simulation of Plasma-Surface Interfaces

We report the development of an atomistic-informed, surface-state-dependent predictive model for particle exchange in a carbon-tungsten plasma-surface interface. The predictive model uses machine learning (ML) techniques to learn the energy and angular distributions for particle exchange and rate functions for surface state evolution from molecular dynamics simulations of cumulative bombardment of tungsten by energetic carbon ions. Each predictive component is sensitive to the energy and trajectory of incident plasma species and the surface state. The surface state is represented by a set of surface state descriptors, which were derived from the atomistic surface state for each independent carbon bombardment event. These descriptors are representative of the composition and degree of amorphization of the outermost angstrom of surface material and were chosen to optimize predictive performance for particle exchange at the interface. The distributions for particle exchange (reflection/sputtering) are demonstrated to vary with each surface state descriptor, motivating the development of surface-state-dependent particle exchange models for plasma simulations. The performance of various ML methods was compared, including polynomial quantile regression, artificial neural networks, k-nearest neighbors, and random forest algorithms, with polynomial regression performing the best for interpolation and extrapolation of learned relationships. In addition to the particle exchange model, a neutral network was developed and used to identify data sufficiency throughout surface descriptor space, which will enable real-time feedback during future data production to ensure data is produced where it is most needed, and we provide commentary on improvements to the data production workflow for future endeavors.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Stability and Control of Burning Tokamak Plasmas with Resistive Walls (Second Year Report/ Final Report)

This research will focus on quantitative prediction of the stability, control, and equilibrium state evolution in toroidal burning plasmas. The stability of long pulse burning plasmas is highly sensitive to the physics of resonant layers in the plasma, sources of momentum and ow, kinetic effects of energetic particles, and boundary conditions at the wall, including feedback control and error fields. In ITER in particular, the low toroidal ow equilibrium state, sustained primarily by energetic alpha particles from fusion reactions, will require the consideration of all of these key elements to predict quantitatively the stability and evolution. The principal investigators on this proposal are leading experts in the relevant theoretical and computational areas, and aim to perform computations guided by analytic modeling, to address this physics in realistic configurations. The overall goal is to understand the key physics mechanisms that describe resistive toroidal burning plasmas, surrounded by a resistive wall, under active feedback control. With the physics of the energetic ions, resonant layers, resistive wall, and toroidal momentum transport included, this study will extend from recent publications in theory and simulation of individual effects and move toward predictive modeling for burning plasmas.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Stability and Control of Burning Tokamak Plasmas with Resistive Walls (Final Report)

This research has focused on quantitative prediction of the stability, control, and equilibrium state evolution in toroidal burning plasmas. The stability of long pulse burning plasmas is highly sensitive to the physics of resonant layers in the plasma, sources of momentum and flow, kinetic effects of energetic particles, and boundary conditions at the wall, including feedback control and error fields. In ITER in particular, the low toroidal flow equilibrium state, sustained primarily by energetic alpha particles from fusion reactions, will require the consideration of all of these key elements to predict quantitatively the stability and evolution. The principal investigators on this proposal are leading experts in the relevant theoretical and computational areas, and aimed to perform computations guided by analytic modeling, to address this physics in realistic configurations. The overall goal is to understand the key physics mechanisms that describe resistive toroidal burning plasmas, surrounded by a resistive wall, under active feedback control. With the physics of the energetic ions, resonant layers, resistive wall, and toroidal momentum transport included, this study will extend from recent publications in theory and simulation of individual effects and move toward predictive modeling for burning plasmas.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Initial energy-momentum to final flow: A general framework for heavy-ion collisions

The evolution of a relativistic heavy-ion collision is typically understood as a process that transmutes the initial geometry of the system into the final momentum distribution of observed hadrons, which can be described via a cumulant expansion of the initial distribution of energy density and is represented at leading order as the well-known eccentricity scaling of anisotropic flow. We extend this framework to include the contribution from initial momentum-space properties, as encoded in other components of the energy-momentum tensor. Furthermore, we confirm the validity of the framework in state-of-the-art hydrodynamic simulations of large and small systems. With this framework, it is possible to separate the effects of early time dynamics from those of final-state evolution, even in the case when the distribution of energy does not fully determine subsequent evolution, as for example, in small systems. Specifically, we answer the question of when and how azimuthal correlations from the initial state survive to the final state. In very small systems such as 𝑝−𝑝, for example, initial momentum degrees of freedom dominate over energy. Thus, even if the system forms a quark-gluon plasma that is well described by hydrodynamics, the usual hydrodynamic picture of the transmutation of initial geometry to final momentum anisotropy is broken. Nevertheless, we show that the hydrodynamic response to the full energy-momentum tensor can be well understood in a similar manner as larger systems. Additionally, this framework elucidates the generic features of the system's evolution that are responsible for the impressive success of hydrodynamic simulations, but which may still hold even in cases where hydrodynamics is not applicable.

Relativistic heavy-ion collisions↗

Latent-space time evolution of non-intrusive reduced-order models using Gaussian process emulation

Non-intrusive reduced-order models (ROMs) have recently generated considerable interest for constructing computationally efficient counterparts of nonlinear dynamical systems emerging from various domain sciences. They provide a low-dimensional emulation framework for systems that may be intrinsically high-dimensional. This is accomplished by utilizing a construction algorithm that is purely data-driven. It is no surprise, therefore, that the algorithmic advances of machine learning have led to non-intrusive ROMs with greater accuracy and computational gains. However, in bypassing the utilization of an equation-based evolution, it is often seen that the interpretability of the ROM framework suffers. This becomes more problematic when black-box deep learning methods are used which are notorious for lacking robustness outside the physical regime of the observed data. In this article, we propose the use of a novel latent-space interpolation algorithm based on Gaussian process regression. Notably, this reduced-order evolution of the system is parameterized by control parameters to allow for interpolation in space. The use of this procedure also allows for a continuous interpretation of time which allows for temporal interpolation. The latter aspect provides information, with quantified uncertainty, about full-state evolution at a finer resolution than that utilized for training the ROMs. This research assesses the viability of this algorithm for an advection-dominated system given by the inviscid shallow water equations.

97 MATHEMATICS AND COMPUTING↗

Clifford orbits from cayley graph quotients

We describe the structure of the $n$-qubit Clifford group $\mathcal{C}_n$ via Cayley graphs, whose vertices represent group elements and edges represent generators. In order to obtain the action of Clifford gates on a given quantum state, we introduce a quotient procedure. Quotienting the Cayley graph by the stabilizer subgroup of a state gives a reduced graph which depicts the state's Clifford orbit. Using this protocol for $\mathcal{C}_2$, we reproduce and generalize the reachability graphs. Since the procedure is state-independent, we extend our study to non-stabilizer states, including the W and Dicke states. Furthermore, our new construction provides a more precise understanding of state evolution under Clifford circuit action.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Magnetism and quantum melting in moiré-material Wigner crystals

Recent experiments have established that semiconductor-based moir´e materials can host incompressible states at a series of fractional moir´e-miniband fillings. These states have been identified as generalized Wigner crystals in which electrons localize on a subset of the available triangular-lattice moir´e superlattice sites. In this article, we use momentum-space exact diagonalization to investigate the many-body ground state evolution at rational fillings from the weak-hopping classical lattice gas limit, in which only spin degrees-of-freedom are active at low energies, to the strong-hopping metallic regime where the Wigner crystals melt. We specifically address the nature of the magnetic ground states of the generalized Wigner crystals at fillings ν = 1/3 and ν = 2/3.

36 MATERIALS SCIENCE↗

Quantum state preparation by adiabatic evolution with custom gates

Quantum state preparation by adiabatic evolution is currently rendered ineffective by the long implementation times of the underlying quantum circuits, comparable to the decoherence time of present and near-term quantum devices. These implementation times can be significantly reduced by realizing these circuits with custom gates. Using classical computing, we model the output of a realistic two-qubit processor implementing the adiabatic evolution of a two-spin system by means of custom gates. This modeled output is then compared with the results of quantum simulations solving the same problem on IBM Quantum (IBMQ) systems. Additionally, when used to emulate the behavior of the IBMQ quantum circuit, our realistic model yields state fidelities ranging from 65% to 85%, similar to the actual performance of a diverse set of IBMQ devices. When we reduced the implementation time by using custom gates, however, the loss of fidelity was reduced by at least a factor of 4, allowing us to accurately extract the energy of the target state. This improvement is enough to render adiabatic evolution useful for quantum state preparation for small systems or as a preconditioner for other state preparation methods.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

In situ catalyst activation and regeneration enable energy-efficient high-current CO 2 reduction to ethanol-rich C 2+ mixtures

Electrochemical conversion of dissolved CO 2 in bicarbonate electrolytes, i.e., bicarbonate electrolysis, offers distinct advantages over gas diffusion electrode systems by enabling direct utilization of the CO 2 capture electrolyte while bypassing the energy-intensive CO 2 release step. However, bicarbonate electrolysis faces challenges such as CO 2 mass-transfer limitation, local pH-driven CO 2 depletion, and high cathodic potentials. The higher potential often causes catalyst surface reorganization, leading to a gradual loss of active sites and variations in selectivity during CO 2 reduction. Here, we report a directed, in situ activation and regeneration method that allows precatalysts to equilibrate under dynamic (pulsed) electrolysis conditions. We demonstrate in situ activation of a scalable Cu 2 O/Cu mesh that, under short-width (t = 4 s) pulsed electrolysis, provides stable mixed oxidation states of Cu, favoring the formation of an ethanol-rich crude mixture. The pulsed electrolysis waveform, consisting of six distinct segments, is tuned to form Cu + oxides, which are then reduced to generate local alkaline conditions favoring C–C coupling. This synergistic effect results in FEs of 73% for C2+ products and 39% for ethanol at an applied current density of −150 mA cm −2 and a cathodic potential of −1.45 V (vs. RHE). The overall half-cell energy efficiency is ∼30% for C 2+ products. The in situ Raman experiments confirm the role of pCO 2 R in dynamically regenerating Cu+-containing surface species during pulsed operation, thereby steering selectivity towards C 2+ products. A comprehensive multiscale, multiphysics model is developed to investigate the dynamic behavior of copper surface species (Cu, Cu + , and Cu 2+ ) and local microenvironmental conditions during the pCO 2 R. The results reveal that the coexistence of different copper oxidation states, especially the Cu+ intermediate, is critical in steering selectivity towards multicarbon (C 2+ ) products. The dynamic modulation of surface redox states via tailored pulsing strategies favors C–C coupling pathways by inducing localized alkaline conditions and stabilizing reactive intermediates. This work establishes a predictive modeling platform that links pulse waveform design with mechanistic insights into catalyst state evolution and product selectivity. Overall, this study provides valuable insights into the synergistic effect of in situ activation of pre-catalysts and pulsed electrolysis for higher selectivity towards C 2+ products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Cycling Performance and Structure Evolution of Co-Free Lithium- and Manganese-Rich Layered Oxides in Lithium-Ion Batteries

Lithium- and manganese-rich (LMR) layered oxides are high-capacity cathode materials that are being considered for electric vehicle (EV) lithium-ion batteries (LIBs). Here, we investigate the electrochemical cycling behavior of cells containing a cobalt-free LMR oxide, 0.3Li 2 MnO 3 ·0.7LiMn 0.5 Ni 0.5 O 2 , paired with either Li or graphite anodes. Two- and three-electrode cells are cycled under varying conditions to examine the effects of oxide activation, upper cutoff voltage, separator type, and electrolyte composition. Post-cycling characterization of harvested electrodes, with electrochemical, X-ray absorption spectroscopy, and solid-state 6 Li nuclear magnetic resonance spectroscopy techniques, are used to correlate cell performance changes with redox state evolution in the oxide and Li inventory shifts in the cell. Our results show that capacity fade and impedance rise primarily originate at the graphite anode and LMR cathode, respectively. Notably, while Ni undergoes reversible redox, Mn shows no evidence of bulk redox activity even in highly-aged electrodes: only relithiated LMR electrodes show some reduction of Mn. Graphite electrodes degrade due to particle isolation and SEI growth, exacerbated by Mn dissolution and deposition on graphite anodes. These findings highlight the coupled structural and electrochemical degradation mechanisms in LMR/graphite cells and underscore lithium inventory retention and electrode interfacial stability as critical factors for enhancing long-term performance.

Badami, Pavan P. [Argonne National Laboratory (ANL↗

Fe-single atom catalysts facilitate fast electron transfer with MoS 2 /SnS 2 cathodes in lithium–sulfur batteries

Lithium–sulfur batteries (LSBs) emerge as promising next-generation energy storage systems offering cost-effectiveness, environmental friendliness, and high theoretical energy density. The practical implementation of LSBs faces significant hindrances due to the shuttle effect and sluggish redox reactions. To address these challenges, single-atom catalyst (SAC) based combination materials from d-block elements can offer increased active catalytic sites, rapid charge transfer, accelerated electron migration, and fast sulfur redox conversion kinetics of lithium polysulfides (LiPSs). In this study, we fabricated three different LSB cathodes: pure S, S@MoS 2 /SnS 2 , and S@Fe–MoS 2 /SnS 2 . These cathodes were then used to explore the cycle life, capacity, rate capability, and redox kinetic reactions of LiPSs while assessing the influence of Fe-SACs on their performance. As a result, LSBs with S@Fe–MoS 2 /SnS 2 cathodes demonstrate an extended cycle life of 1000 cycles at a C-rate of 0.2C, maintaining a capacity close to 500 mA h g −1 , the highest initial discharge capacity of 1622 mA h g −1 and 1066 mA h g −1 at 0.05C and 0.2C, and excellent rate capabilities of 708 mA h g −1 and 558 mA h g −1 at 1C and 2C, respectively. The synergistic effect of the Fe-SAC-based combination cathode (S@Fe–MoS 2 /SnS 2 ) creates plentiful adsorptive and highly active catalytic sites, resulting in substantially enhanced capacity for adsorbing soluble long-chain LiPSs. This facilitates ultra-fast redox kinetics, surpassing the performance of the S@MoS 2 /SnS 2 and pure S cathodes. In the ex situ analysis, results from powder X-ray diffraction (XRD) to observe the new phase, soft X-ray absorption spectroscopy (XAS) to investigate the electronic structure, and hard X-ray photoelectron microscopy (HAXPES) with different energies (900 eV, 2000 eV, and 6000 eV) to track the chemical-state evolution of Fe-SACs in MoS 2 /SnS 2 cathodes displayed notable electrochemical reversibility involving S 8 ⇄ LiPSs ⇄ Li 2 S conversion even after 1000 cycles. Additionally, in situ, operando Raman analysis can unveil a novel catalytic mechanism of Fe-SACs in MoS 2 /SnS 2 “facilitating rapid electron transfer” during the discharge and charge processes of LSBs involving the conversion of S 8 ⇄ long-chain LiPSs ⇄ Li 2 S 2 /Li 2 S. This study elucidates the working mechanism of Fe-SAC cathodes, offering insights into overcoming the shuttle effect and facilitating sulfur redox kinetics to advance commercial LSBs.

36 MATERIALS SCIENCE↗

Comparison of the Forward and Reverse Photocycle Dynamics of Two Highly Similar Canonical Red/Green Cyanobacteriochromes Reveals Unexpected Differences

Cyanobacteriochromes (CBCRs) are cyanobacterial photoreceptors that exhibit photochromism between two states: a thermally stable dark-adapted state and a metastable light-adapted state with bound linear tetrapyrrole (bilin) chromophores possessing 15Z and 15E configurations, respectively. The photodynamics of canonical red/green CBCRs have been extensively studied; however, the time scales of their excited-state lifetimes and subsequent ground-state evolution rates widely differ and, at present, remain difficult to predict. Here, we compare the photodynamics of two closely related red/green CBCRs that have substantial sequence identity (~68%) and similar chromophore environments: AnPixJg2 from Anabaena sp. PCC 7120 and NpR6012g4 from Nostoc punctiforme. Using broadband transient absorption spectroscopy on the primary (125 fs to 7 ns) and secondary (7 ns to 10 ms) time scales together with global analysis modeling, our studies revealed that AnPixJg2 and NpR6012g4 have comparable quantum yields for initiating the forward ( 15Z P r → 15E P g ) and reverse ( 15E P g → 15Z P r ) reactions, which proceed through monotonic and nonmonotonic mechanisms, respectively. In addition to small discrepancies in the kinetics, the secondary reverse dynamics resolved unique features for each domain: intermediate shunts in NpR6012g4 and a Meta-Gf intermediate red-shifted from the 15Z P r photoproduct in AnPixJg2. Altogether, this study supports the conclusion that sequence similarity is a useful criterion for predicting pathways of the light-induced evolution and quantum yield of generating primary intermediate Φ p within subfamilies of CBCRs, but more studies are still needed to develop a comprehensive molecular level understanding of these processes.

59 BASIC BIOLOGICAL SCIENCES↗