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Number of bits returned by a quantum estimation

We give two upper bounds to the mutual information in arbitrary quantum estimation strategies. The first is based on some simple Fourier properties of the estimation apparatus. The second is derived using the first, but, interestingly, depends only on the Fisher information of the parameter, so it is valid even beyond quantum estimation. We illustrate the usefulness of these bounds by characterizing the quantum phase estimation algorithm in the presence of noise. In addition, for the noiseless case, we extend the analysis beyond applying the bound and we discuss the optimal entangled and adaptive strategies, clarifying inaccuracies appearing on this topic in the literature.

97 MATHEMATICS AND COMPUTING↗

Lifetime renormalization of weakly anharmonic superconducting qubits. I. Role of number nonconserving terms

The dynamics of a weakly anharmonic superconducting qubit in a complex electromagnetic environment is generally well described by an effective multimode Kerr Hamiltonian at sufficiently weak excitation. This Hamiltonian can be embedded in a master equation with losses determined by the details of the electromagnetic environment. Recent experiments indicate, however, that when a superconducting circuit is driven with microwave signals populating the system with sufficiently high excitations, the observed relaxation rates appear to be substantially different from expectations based on the electromagnetic environment of the qubit alone. This issue is a limiting factor in the optimization of superconducting qubit readout schemes. We claim here that an effective master equation with drive-power-dependent parameters is an efficient approach to model such quantum dynamics. In this sequence of papers, we derive effective master equations, whose parameters exhibit nonlinear dependence on the excitation level of the circuit as well as the electromagnetic environment of the qubit. Further, we show that the number nonconserving terms in the qubit nonlinearity generally lead to a renormalization of dissipative parameters of the effective master equation, while the number conserving terms give rise to a renormalization of the system frequencies. Here, in Paper I, we consider the excitation-relaxation dynamics of a transmon qubit that is prepared in a certain initial state, but is not driven otherwise. A unitary transformation technique is introduced to study the renormalization of (i) qubit relaxation due to coupling to a generic bath and (ii) Purcell decay. Analytic expressions are provided for the dependence of the nonlinear dissipative terms on the details of the electromagnetic environment of the qubit. The perturbation technique based on unitary transformations developed here is generalized to the continuously driven case in Paper II.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ge:Be infrared photoconductors

Ge:Be photoconductors were optimized for the 30 to 50 micron wavelength range. Crystal growth of detector quality material requires good control of both the Be and residual impurity doping. Detective quantum efficiencies of n sub d = 46% at 5 A/W were achieved at a photon background of 10 to the 8th power p/s. The responsivity of Ge:Be detectors can be strongly temperature-dependent when the residual shallow levels in the material are closely compensated. Transient responses on the order of approximately 1 second were observed in some materials. The role of residual shallow impurities on the performance of photoconductors doped with semi-deep and deep impurities is discussed.

Haegel, N. M.↗

LED Device Illuminates New Path to Healing

Among NASA s research goals is increased understanding of factors affecting plant growth, including the effects of microgravity. Impeding such studies, traditional light sources used to grow plants on Earth are difficult to adapt to space flight, as they require considerable amounts of power and produce relatively large amounts of heat. As such, an optimized experimental system requires much less energy and reduces temperature variance without negatively affecting plant growth results. Ronald W. Ignatius, founder and chairman of the board at Quantum Devices Inc. (QDI), of Barneveld, Wisconsin, proposed using light-emitting diodes (LEDs) as the photon source for plant growth experiments in space. This proposition was made at a meeting held by the Wisconsin Center for Space Automation and Robotics, a NASA-sponsored research center that facilitates the commercialization of robotics, automation, and other advanced technologies. The Wisconsin group teamed with QDI to determine whether an LED system could provide the necessary wavelengths and intensities for photosynthesis, and the resultant system proved successful. The center then produced the Astroculture3, a plant growth chamber that successfully incorporated this LED light source, which has now flown on several space shuttle missions. NASA subsequently identified another need that could be addressed with the use of LEDs: astronaut health. A central concern in astronaut health is maintaining healthy growth of cells, including preventing bone and muscle loss and boosting the body s ability to heal wounds all adversely affected by prolonged weightlessness. Thus, having determined that LEDs can be used to grow plants in space, NASA decided to investigate whether LEDs might be used for photobiomodulation therapy (PBMT).

Source record↗

Bi-alkali antimonide photocathode growth: An X-ray diffraction study

Bi-alkali antimonide photocathodes are one of the best known sources of electrons for high current and/or high bunch charge applications like Energy Recovery Linacs or Free Electron Lasers. Despite their high quantum efficiency in visible light and low intrinsic emittance, the surface roughness of these photocathodes prohibits their use as low emittance cathodes in high accelerating gradient superconducting and normal conducting radio frequency photoguns and limits the minimum possible intrinsic emittance near the threshold. Also, the growth process for these materials is largely based on recipes obtained by trial and error and is very unreliable. In this paper, using X-ray diffraction, we investigate the different structural and chemical changes that take place during the growth process of the bi-alkali antimonide material K{sub 2}CsSb. Our measurements give us a deeper understanding of the growth process of alkali-antimonide photocathodes allowing us to optimize it with the goal of minimizing the surface roughness to preserve the intrinsic emittance at high electric fields and increasing its reproducibility.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Phase stability and interlayer interaction of blue phosphorene

In this work, we study the interlayer interactions between sheets of blue phosphorus with quantum Monte Carlo (QMC) methods. Here, we find that as previously observed in black phosphorus, interlayer binding of blue phosphorus cannot be described by van der Waals (vdW) interactions alone within the density functional theory framework. Specifically, while some vdW density functionals produced reasonable binding curves, none of them could provide a correct, even qualitatively, description of charge redistribution due to interlayer binding. We also show that small systematic errors in common practice QMC calculations, such as the choice of optimized geometry and finite-size corrections, are non-negligible given the energy and length scales of this problem. We mitigate some of the major sources of error and report QMC-optimized lattice constant, stacking, and interlayer binding energy for blue phosphorus. Finally, it is strongly suggested that these considerations are important and quite general in the modeling of two-dimensional phosphorus allotropes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Wildfire Segmentation From Remotely Sensed Data Using Quantum-Compatible Conditional Vector Quantized-Variational Autoencoders

Wildfires represent a critical environmental hazard with multifaceted implications for ecosystems, communities, and public health [1]. The escalating frequency and intensity of wildfires globally have intensified the urgency for robust segmentation methodologies to facilitate effective mitigation, response, and recovery strategies [2]. Accurate wildfire segmentation is pivotal for delineating fire boundaries, assessing progression patterns, and prioritizing resource allocation during emergency scenarios. Furthermore, precise segmentation enables stakeholders, including policymakers, environmental scientists, and emergency responders, to formulate evidence-based strategies, thereby minimizing socio-economic disruptions and ecological degradation. Consequently, advancing wildfire segmentation techniques through innovative technological interventions remains a paramount research imperative. Although foundational in wildfire segmentation, traditional deterministic models exhibit inherent limitations that compromise their efficacy in dynamic and uncertain environments. These models often operate on rigid algorithms prioritizing deterministic classifications, thereby overlooking the inherent complexities and uncertainties associated with wildfire behavior and satellite data variability. Such deterministic frameworks tend to produce oversimplified representations that fail to capture the intricate nuances of evolving fire dynamics, spatial heterogeneity, and environmental interactions [1]. Consequently, the deterministic approach’s propensity for uncertainty collapsing [1, 3] hampers the accuracy, reliability, and applicability of segmentation outcomes in real-world scenarios. Contrastingly, stochastic models offer a more nuanced and adaptable framework for wildfire segmentation. By integrating probabilistic elements into the modeling paradigm, stochastic approaches, particularly probabilistic approaches such as variational auto encoders (VAEs) [4], facilitate comprehensive uncertainty assessment, enabling researchers to quantify and incorporate uncertainties into segmentation outcomes effectively. This probabilistic nature empowers stochastic models to encapsulate variability, account for data inconsistencies, and adapt to evolving environmental conditions, enhancing segmentation accuracy, reliability, and robustness. Embracing stochastic methodologies thus catalyzes advancements in wildfire science by fostering a more holistic, adaptive, and resilient segmentation framework. Despite VAEs demonstrating significant promise in various applications, they come with inherent limitations that have garnered attention within the machine learning community. One of the primary drawbacks lies in their reliance on static priors, which essentially assume a fixed distribution for latent variables, thereby limiting the model’s flexibility to capture complex data structures effectively [5]. This static nature leads to suboptimal representations, especially when dealing with complex and high-dimensional data. Additionally, VAEs often struggle with generating sharp and realistic samples, a phenomenon commonly referred to as mode collapse [5, 7, 6]. Furthermore, the optimization process in VAEs, which involves balancing the reconstruction loss and the regularization term, can sometimes be challenging to fine-tune [7]. In recent efforts to address these shortcomings, alternative approaches like Vector Quantized Variational Auto encoders(VQ-VAEs) [7], address the challenges by incorporating discrete latent variables and leveraging techniques that enhance the quality and diversity of generated samples while maintaining efficient training dynamics. VQ-VAEs propose a dynamic prior distribution generation mechanism that diverges from the static priors commonly associated with traditional VAEs. This dynamic approach allows for more adaptive and context-aware latent variable representations, thereby potentially capturing complex data structures more effectively. Unlike autoregressive prior models such as PixelCNN, which, despite their ability to model dependencies across data dimensions, suffer from significant computational inefficiencies and lack flexibility in handling diverse datasets. In our work, we propose to use a generative quantum-compatible approach to help alleviate the shortcomings of autoregressive prior model in VQ-VAEs. Restricted Boltzmann Machines (RBMs) are a viable alternative prior model that can learn prior distributions in a faster and more flexible manner. In this research endeavor, we meticulously curate a state-of-the-art dataset leveraging satellite MODIS data in conjunction with VIIRS fire masks, derived from Fire Radiative Power (FRP), thereby encapsulating diverse wildfire scenarios and environmental contexts. We developed a conditional VQ-VAE architecture with the RBM prior model that is trained in a supervised manner for segmenting wildfire masks. This innovative approach synergistically harnesses deep learning capabilities, enabling the generation of segmentation maps characterized by heightened precision, granularity, and contextual relevance. Furthermore, replacing the autoregressive prior learning method proposed by the original VQ-VAE with a prior density approximation via quantum-compatible RBM facilitates expedited inference processes, augments flexibility in prior sampling, optimizes computational efficiency and establishes a groundbreaking benchmark in wildfire segmentation methodologies.

quantum machine learning↗

Field emission from optimized structure of carbon nanotube field emitter array

The authors report a detail study on the emission properties of field emitter array (FEA) of micro-circular emitters of multiwall carbon nanotubes (CNTs). The FEAs were fabricated on patterned substrates prepared with an array of circular titanium (Ti) islands on titanium nitride coated tantalum substrates. CNTs were rooted into these Ti islands to prepare an array of circular emitters. The circular emitters were prepared in different diameters and pitches in order to optimize their structure for acquiring a high emission current. The pitch was varied from 0 to 600 μm, while a diameter of circular emitters was kept constant to be 50 μm in order to optimize a pitch. For diameter optimization, a diameter was changed from 50 to 200 μm while keeping a constant edge-to-edge distance of 150 μm between the circular emitters. The FEA with a diameter of 50 μm and a pitch of 120 μm was found to be the best to achieve an emission current of 47 mA corresponding to an effective current density of 30.5 A/cm{sup 2} at 7 V/μm. The excellent emission current was attributed to good quality of CNT rooting into the substrate and optimized FEA structure, which provided a high electric field on a whole circular emitter of 50 μm and the best combination of the strong edge effect and CNT coverage. The experimental results were confirmed with computer simulation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Full-Scale Ab Initio Simulation of Magic-Angle-Spinning Dynamic Nuclear Polarization

Theoretical models aimed at describing magic-angle-spinning (MAS) dynamic nuclear polarization (DNP) NMR have great potential in facilitating the in silico design of DNP polarizing agents and formulations. These models must typically face a trade-off between the accuracy of a strict quantum mechanical description and the need for using realistically large spin systems, for instance, using phenomenological models. In this paper, we show that the use of aggressive state-space restrictions and an optimization strategy allows full-scale ab initio MAS-DNP simulations of spin systems containing thousands of nuclei. Our simulations are shown to reproduce experimental DNP enhancements quantitatively, including their MAS rate dependence, for both frozen solutions and solid materials. They also reveal the importance of a previously unrecognized structural feature found in some polarizing agents that helps minimize the sensitivity losses imposed by the spin diffusion barrier.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tree tensor network hierarchical equations of motion based on time-dependent variational principle for efficient open quantum dynamics in structured thermal environments

In this work, we introduce an efficient method, TTN-HEOM, for exactly calculating the open quantum dynamics for driven quantum systems interacting with highly structured bosonic baths by combining the tree tensor network (TTN) decomposition scheme with the bexcitonic generalization of the numerically exact hierarchical equations of motion (HEOM). The method yields a series of quantum master equations for all core tensors in the TTN that efficiently and accurately capture the open quantum dynamics for non-Markovian environments to all orders in the system–bath interaction. These master equations are constructed based on the time-dependent Dirac–Frenkel variational principle, which isolates the optimal dynamics for the core tensors given the TTN ansatz. The dynamics converges to the HEOM when increasing the rank of the core tensors, a limit in which the TTN ansatz becomes exact. We introduce TENSO, tensor equations for non-Markovian structured open systems, as a general-purpose Python code to propagate the TTN-HEOM dynamics. We implement three general propagators for the coupled master equations: two fixed-rank methods that require a constant memory footprint during the dynamics and one adaptive-rank method with a variable memory footprint controlled by the target level of computational error. We exemplify the utility of these methods by simulating a two-level system coupled to a structured bath containing one Drude–Lorentz component and eight Brownian oscillators, which is beyond what can presently be computed using the standard HEOM. Our results show that the TTN-HEOM is capable of simulating both dephasing and relaxation dynamics of driven quantum systems interacting with structured baths, even those of chemical complexity, with an affordable computational cost.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-Performance Computing Optimization for Aladyn – Adaptive Neural Network Molecular Dynamics Mini-Application

This report provides a description and performance evaluation of the optimization techniques for high performance computing (HPC) implementation of the open source Computational Materials mini-application Aladyn (https://github.com/nasa/aladyn). Aladyn is a basic molecular dynamics code written in FORTRAN 2003, which is designed to demonstrate the use of adaptive neural networks (ANNs) in atomistic simulations. The role of ANNs is to efficiently reproduce the very complex energy landscape resulting from the atomic interactions in materials with the accuracy of the more expensive quantum mechanics-based calculations. The ANN is trained on a large set of atomic structures calculated using the density functional theory (DFT) method. While achieving orders of magnitude faster computational performance than DFT, the ANN-based approach was still very computationally demanding compared to the conventional approach of using empirically fitted energy functions. After its initial development, Aladyn was evaluated and optimized by experts at the NASA Advanced Supercomputing (NAS) division to exploit modern supercomputer architectures. The code has been optimized for execution on multicore central processing units (CPUs), including Intel® Skylake microarchitecture, and on graphic accelerators, such as Nvidia® V100 graphic processing units (GPUs), using Open Multi-Processing (OpenMP) and Open Accelerators (OpenACC) programming interfaces. The optimization achieved a speedup of 4.7 times the baseline version on CPU performance and an additional 2.4 times on CPU+GPU performance. Atomistic computer simulations are a fundamental tool in materials research to model material properties form physics-based first principles. Atomic interaction, governed by Quantum Mechanics (QM) require sophisticated and highly computationally demanding mathematical models to calculate [1]. Classical methods use approximate functional forms, empirically fitted through a set of variable parameters to emulate atomic energies as direct functions of atomic coordinates [2]. While empirical potentials are computationally much simpler, allowing simulations of large-scale systems of up to a trillion (1012) atoms [3], they are substantially less accurate compared to quantum calculations and applicable only to very specific atomic configurations or predefined crystallographic phases. A recently suggested approach is to use heuristic machine learning methods [4], such as those based on Adaptive Neural Networks (ANNs) to predict atomic energies, after being trained on a sufficiently large database of QM-calculated structures [5,6]. This approach reduces significantly the computational complexity, allowing for simulations of orders of magnitude larger systems compared to QM-based methods without compromising accuracy. Still, compared to classical methods using empirical energy functions, ANN methods remain two- to three orders of magnitude more computationally demanding. Hence, the computational cost of simulations, together with the need for extensive training of ANNs, still makes the practical implementation of ANN-based methods quite challenging. The purpose of the Aladyn mini-application software [7], available as open source at https://github.com/nasa/aladyn, is to be a testbed for exploring possible optimization strategies to develop highly scalable parallel algorithms for ANN-based atomistic simulations. Aladyn is aimed at utilizing the architecture of the high-end modern highperformance computing (HPC) hardware based on multicore central processing units (CPUs) equipped with graphic processing unit (GPU) accelerators. Specifically, the goal is to optimize the performance on a single HPC compute node, before implementing scaling to multi-node parallelization using message passing interface (MPI). At the same time, the open source code of Aladyn can serve as a training model for students and professors in academia.

Yamakov, Vesselin I.↗

Predicting radiative transport properties of plasma sprayed porous ceramics

The typical yttria-stabilized zirconia material for making the thermal barrier coatings (TBCs) is intrinsically semitransparent to thermal radiation, and the unique disordered microstructures in TBCs make them surprisingly highly scattering. To quantitatively understand the influence of disordered microstructures, this paper presents a quantitative prediction on the radiative properties, especially the transport scattering coefficient of plasma sprayed TBC based on microstructure analysis and rigorous electromagnetic theory. The impact of the porosity, shape, size, and orientation of different types of voids on transport scattering coefficient is comprehensively investigated under the discrete dipole approximation. An inverse model integrating these factors together is then proposed to quantitatively connect transport scattering coefficient with microstructural information, which is also validated by available experimental data. Afterwards, an optimization procedure is carried out based on this model to obtain the optimal size and orientation distribution of the microscale voids to achieve the maximal radiation insulation performance at different operating temperatures, providing guidelines for practical coating design and fabrication. This work suggests that the current model is effective and also efficient for connecting scattering properties to microstructures and can be implemented as a quantitative tool for further studies like non-destructive infrared imaging as well as micro/nanoscale thermal design of TBCs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Photovoltaic Properties of Selenized CuGa/In Films with Varied Compositions

Thin CuGa/In films with varied compositions were deposited by co-evaporation and then selenized in situ with evaporated selenium. The selenized Cu(In, Ga)Se2 absorbers were used to fabricate 390 solar cells. Cu/(Ga+In) and Ga/(Ga+In) (Cu/III and Ga/III) were independently varied, and photovoltaic performance was optimal at Cu/III of 77-92% for all Ga/III compositions studied (Ga/III ~ 30, 50, and 70%). The best absorbers at each Ga/III composition were characterized with time-resolved photoluminescence, scanning electron microscopy, and secondary ion mass spectrometry, and devices were studied with temperature-dependent current density-voltage, light and electrical biased quantum efficiency, and capacitance-voltage. The best cells with Ga/III ~ 30, 50, and 70% had efficiencies of 14.5, 14.4, and 12.2% and maximum power temperature coefficients of -0.496, -0.452, and -0.413%/degrees C, respectively. This resulted in the Ga/III ~ 50% champion having the highest efficiency at temperatures greater than 40 degrees C, making it the optimal composition for practical purposes. This optimum is understood as a result of the absorber's band gap grading- where minimum band gap dominates short-circuit current density, maximum space charge region band gap dominates open-circuit voltage, and average absorber band gap dominates maximum power temperature coefficient.

14 SOLAR ENERGY↗

Enhancement of flow measurements using fluid-dynamic constraints

Novel experimental modalities acquire spatially resolved velocity measurements for steady state and transient flows which are of interest for engineering and biological applications. One of the drawbacks of such high resolution velocity data is their susceptibility to measurement errors. In this paper, we propose a novel filtering strategy that allows enhancement of the noisy measurements to obtain reconstruction of smooth divergence free velocity and corresponding pressure fields which together approximately comply to a prescribed flow model. The main step in our approach consists of the appropriate use of the velocity measurements in the design of a linearized flow model which can be shown to be well-posed and consistent with the true velocity and pressure fields up to measurement and modeling errors. The reconstruction procedure is then formulated as an optimal control problem for this linearized flow model. The resulting filter has analyzable smoothing and approximation properties. We briefly discuss the discretization of the approach by finite element methods and comment on the efficient solution by iterative methods. The capability of the proposed filter to significantly reduce data noise is demonstrated by numerical tests including the application to experimental data. In addition, we compare with other methods like smoothing and solenoidal filtering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Synergy between Fe and Ni in the optimal performance of (Ni,Fe)OOH catalysts for the oxygen evolution reaction

The oxygen evolution reaction (OER) is critical to solar production of fuels, but the reaction mechanism underlying the performance for a best OER catalyst, Fe-doped NiOOH [(Ni,Fe)OOH], remains highly controversial. We used grand canonical quantum mechanics to predict the OER mechanisms including kinetics and thus overpotentials as a function of Fe content in (Ni,Fe)OOH catalysts. We find that density functional theory (DFT) without exact exchange predicts that addition of Fe does not reduce the overpotential much. However, DFT with exact exchange predicts dramatic improvement in performance for (Ni,Fe)OOH, leading to an overpotential of 0.42 V and a Tafel slope of 23 mV/decade (dec), in good agreement with experiments, 0.3–0.4 V and 30 mV/dec. We reveal that the high spin d 4 Fe(IV) leads to efficient formation of an active O radical intermediate, while the closed shell d 6 Ni(IV) catalyzes the subsequent O–O coupling, and thus it is the synergy between Fe and Ni that delivers the optimal performance for OER.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

ARQUIN: Architectures for Multinode Superconducting Quantum Computers

Many proposals to scale quantum technology rely on modular or distributed designs wherein individual quantum processors, called nodes, are linked together to form one large multinode quantum computer (MNQC). One scalable method to construct an MNQC is using superconducting quantum systems with optical interconnects. However, internode gates in these systems may be two to three orders of magnitude noisier and slower than local operations. Surmounting the limitations of internode gates will require improvements in entanglement generation, use of entanglement distillation, and optimized software and compilers. Still, it remains unclear what performance is possible with current hardware and what performance algorithms require. In this article, we employ a systems analysis approach to quantify overall MNQC performance in terms of hardware models of internode links, entanglement distillation, and local architecture. We show how to navigate tradeoffs in entanglement generation and distillation in the context of algorithm performance, lay out how compilers and software should balance between local and internode gates, and discuss when noisy quantum internode links have an advantage over purely classical links. Here, we find that a factor of 10–100× better link performance is required and introduce a research roadmap for the co-design of hardware and software towards the realization of early MNQCs. While we focus on superconducting devices with optical interconnects, our approach is general across MNQC implementations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Erbium-doped optical fibre with enhanced radiation resistance for superluminescent fibre sources

This paper presents a study of the properties of erbium-doped optical fibres with enhanced gamma-ray resistance at a high dose rate. The fibres have a silica core containing different dopants. The gamma-ray resistance of the fibres is due to additional doping of their core with cerium and germanium ions, as well as to aluminium concentration optimisation. We assess the effect of fibre composition on the radiation-induced loss at a wavelength of 1310 nm and the output power and weighted average wavelength of superluminescent fibre sources based on erbium-doped fibre under pulsed gamma irradiation (dose per pulse, ∼ 20 Gy). The fibre doped with aluminium, germanium and cerium oxides is shown to be optimal for use in gamma-ray-resistant broadband superluminescent fibre sources. (optical fibres)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Noisy Intermediate-Scale Quantum Applications on a Pathfinder System

Work performed under this one-year LDRD was concerned with estimating resource requirements for small quantum test beds that are expected to be available in the near future. This work represents a preliminary demonstration of our ability to leverage quantum hardware for solving small quantum simulation problems in areas of interest to the DOE. The algorithms enabling such studies are hybrid quantum-classical variational algorithms, in particular the widely-used variational quantum eigensolver (VQE). Employing this hybrid algorithm, in which the quantum computer complements the classical one, we implemented an end-to-end application-level toolchain that allows the user to specify a molecule of interest and compute the ground state energy using the VQE approach. We found significant limitations attributable to the classical portion of the hybrid system, including a greater than greater-than-quartic power scaling of the classical memory requirements with the system size. Current VQE approaches would require an exascale machine for solving any molecule with size greater than 150 nuclei. Our findings include several improvements that we implemented into the VQE toolchain, including a new classical optimizer that is decades old but hadn't been considered before in the VQE ecosystem. Our findings suggest limitations to variational hybrid approaches to simulation that further motivate the need for a gate-based fault-tolerant quantum processor that can implement larger problems using the fully digital quantum phase estimation algorithm.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗