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DOE OSTI2025

Correlating Superconducting Qubit Performance Losses to Sidewall Near-Field Scattering via Terahertz Nanophotonics

Elucidating dielectric losses, structural heterogeneity, and interface imperfections is critical for improving coherence in superconducting qubits. However, most diagnostics rely on destructive electron microscopy or low-throughput millikelvin quantum measurements. Here, we demonstrate noninvasive terahertz (THz) nano-imaging/-spectroscopy of encapsulated niobium transmon qubits, revealing sidewall near-field scattering that correlates with qubit coherence. We further employ a THz hyperspectral line scan to probe dielectric responses and field participation at Al junction interfaces. These findings highlight the promise of THz near-field methods as a high-throughput proxy characterization tool for guiding material selection and optimizing processing protocols to improve qubit and quantum circuit performance.

Kim, Richard H.J. [Ames Lab]↗

DOE OSTI2025

Analysis methodology of coherent oscillations in time- and angle-resolved photoemission spectroscopy

Oscillatory signals from coherently excited phonons are regularly observed in ultrafast pump–probe experiments on condensed matter samples. Electron–phonon coupling implies that coherent phonons also modulate the electronic band structure. These oscillations can be probed with energy and momentum resolution using time- and angle-resolved photoemission spectroscopy (trARPES), which reveals the orbital dependence of the electron–phonon coupling for a specific phonon mode. However, a comprehensive analysis remains challenging when multiple coherent phonon modes couple to multiple electronic bands. Complex spectral line shapes due to strong correlations in quantum materials add to this challenge. In this work, we examine how the frequency domain representation of trARPES data facilitates a quantitative analysis of coherent oscillations of the electronic bands. Here, we investigate the frequency domain representation of the photoemission intensity and the first moment of the energy distribution curves. Both quantities provide complementary information and are able to distinguish oscillations of binding energy, linewidth, and intensity. We analyze a representative trARPES dataset of the transition metal dichalcogenide WTe 2 and construct composite spectra, which intuitively illustrate how much each electronic band is affected by a specific phonon mode. We also show how a linearly chirped probe pulse can generate extrinsic artifacts that are distinct from the intrinsic coherent phonon signal.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Telecom-Luminescent and Room Temperature Coherent Tetrathiafulvalene-Based Qubits in Spin-Rich Solids

One of the main challenges facing quantum information science (QIS) is the development of robust qubits that can be op-erated under ambient conditions. Current state-of-the-art anionic nitrogen vacancy center (NV–) defect qubits are robust enough to be operated at room temperature but lack scalability and tunability. These are areas where molecular qubits excel, although they typically suffer from poor air stability and fast decoherence at elevated temperatures and in magneti-cally noisy environments. Organic-based systems offer advantages to this end, although examples retaining room tem-perature coherence are still rare. Furthermore, most organic-based systems lack optical transitions similar to NV– centers that could allow for optical initialization and readout. Here we report two new organic-based qubit candidates that demonstrate room temperature coherence in nuclear and electron spin-rich environments. These qubits luminesce far into the near-infrared (NIR, 700-1700 nm) and telecom (~1260-1625 nm) regions, ideal for biological sensing and com-munications applications, respectively.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

QuDPy: A Python-based tool for computing ultrafast non-linear optical responses

Nonlinear Optical Spectroscopy is a well-developed field with theoretical and experimental advances that have benefited multiple disciplines, including chemistry, biology, and physics. However, for the accurate interpretation of the corresponding multi-dimensional spectra, there is a need for precise quantum dynamical simulations based on model Hamiltonians. In this article, we present the initial release of our code, QuDPy (Quantum Dynamics in Python), which provides a robust numerical platform for performing quantum dynamics simulations based on model systems, including open quantum systems. Furthermore, a distinguishing feature of our approach is the ability to specify various high-order optical response pathways in the form of double-sided Feynman diagrams through a straightforward input syntax. This syntax outlines the time-ordering of ket-sided or bra-sided optical interactions acting on the time-evolving density matrix of the system. We utilize the quantum dynamics capabilities of QuTip to simulate the spectral response of complex systems, allowing us to compute virtually any $n$-th order optical response of the model system. To illustrate the utility of our approach, we provide a series of example calculations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Absolute contrast estimation for soft X-ray photon fluctuation spectroscopy using a variational droplet model

Abstract X-ray photon fluctuation spectroscopy using a two-pulse mode at the Linac Coherent Light Source has great potential for the study of quantum fluctuations in materials as it allows for exploration of low-energy physics. However, the complexity of the data analysis and interpretation still prevent recovering real-time results during an experiment, and can even complicate post-analysis processes. This is particularly true for high-spatial resolution applications using CCDs with small pixels, which can decrease the photon mapping accuracy resulting from the large electron cloud generation at the detector. Droplet algorithms endeavor to restore accurate photon maps, but the results can be altered by their hyper-parameters. We present numerical modeling tools through extensive simulations that mimic previous x-ray photon fluctuation spectroscopy experiments. By modification of a fast droplet algorithm, our results demonstrate how to optimize the precise parameters that lift the intrinsic counting degeneracy impeding accuracy in extracting the speckle contrast. These results allow for an absolute determination of the summed contrast from multi-pulse x-ray speckle diffraction, the modus operandi by which the correlation time for spontaneous fluctuations can be measured.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Strong-Field Bloch Electron Interferometry for Band-Structure Retrieval

When Bloch electrons in a solid are exposed to a strong optical field, they are coherently driven in their respective bands where they acquire a quantum phase as the imprint of the band shape. If an electron approaches an avoided crossing formed by two bands, it may be split by undergoing a Landau-Zener transition. We here employ subsequent Landau-Zener transitions to realize strong-field Bloch electron interferometry (SFBEI), allowing us to reveal band structure information. In particular, we measure the Fermi velocity (band slope) of graphene in the vicinity of the K points as 1.07±0.04 nm fs –1 . As a result, we expect SFBEI for band structure retrieval to apply to a wide range of material systems and experimental conditions, making it suitable for studying transient changes in band structure with femtosecond temporal resolution at ambient conditions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Intermolecular vibrations mediate ultrafast singlet fission

Singlet fission is a spin-allowed exciton multiplication process in organic semiconductors that converts one spin-singlet exciton to two triplet excitons. It offers the potential to enhance solar energy conversion by circumventing the Shockley-Queisser limit on efficiency. We study the primary steps of singlet fission in a pentacene film by using a combination of TG and 2D electronic spectroscopy complemented by quantum chemical and nonadiabatic dynamics calculations. We show that the coherent vibrational dynamics induces the ultrafast transition from the singlet excited electronic state to the triplet-pair state via a degeneracy of potential energy surfaces, i.e., a multidimensional conical intersection. Significant vibronic coupling of the electronic wave packet to a few key intermolecular rocking modes in the low-frequency region connect the excited singlet and triplet-pair states. Along with high-frequency local vibrations acting as tuning modes, they open a new channel for the ultrafast exciton transfer through the resulting conical intersection.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Vibration Studies for the CLARA Interferometer

The purpose of the CLARA experiment is to study the nature of undulator radiation emitted by single electrons circulating in the IOTA storage ring. The classical and quantum properties of the radiation are investigated by measuring its coherence length, intensity fluctuations and time correlations. The experiment took data in IOTA Run 4 (2022-2023). The key component of the apparatus is a Mach-Zehnder interferometer (MZI), in which the optical length of one of the arms can be precisely controlled. For some measurements, the fine regulation of the arm length must be smaller than the radiation wavelength. For this reason, the apparatus is particularly sensitive to mechanical vibrations. In this note, we model and measure the effect of vibrations on the performance of the MZI under various conditions. Several improvements of the setup were implemented to minimize systematic distortions of the observed interference patterns. In this report, we present a mathematical model of the effect of mechanical vibrations on observed detector and coincidence rates. We also describe the measurements that were made to estimate the magnitude and spectra of rate fluctuations and their sources in the CLARA MZI under various conditions. Finally, we estimate the magnitude of arm length fluctuations and we deduce the sensitivity to coincidence-rate variations in our apparatus.

43 PARTICLE ACCELERATORS↗

NASA NTRS1994

Measurement of very small phase fluctuations by means of the operational approach

Recently Noh, Fourgeres and Mandel (NFM) have improved the operational approach to the quantum phase problem substantially and measured the phase dispersion of coherent light down to very small means photon numbers of the order of 10(exp -2). This has prompted many other investigations and clarified some important questions in relation to what is actually measured. Although their treatment is rather general, we confine ourselves here to the case of a strong local oscillator (LO) and reproduce their measurement scheme. Surprisingly enough, this simultaneous measurement of the sine and the cosine of the phase difference is completely equivalent to an old proposal to measure the phase after strong linear amplification realized experimentally by the Welling group. The reason for this rests on the fact, that in both cases the results are determined by the Q function of the signal. This was shown for amplification in and for the measurement after beam splitting by Lai and Haus.

Bandilla, Arno↗

DOE OSTI2025

Quantum description of wave dark matter

We outline a fundamentally quantum description of bosonic dark matter (DM) from which the conventional classical-wave picture emerges in the limit 𝑚 ≪10 eV. As appropriate for a quantum system, we start from the density matrix, which encodes the full information regarding the possible measurements we could make of DM and their fluctuations. Following fundamental results in quantum optics, we argue that for DM it is most likely that the density matrix takes the explicitly mixed form of a Gaussian over the basis of coherent states. Deviations from this would generate non-Gaussian fluctuations in DM observables, allowing a direct probe of the quantum state of DM. Our quantum optics–inspired approach allows us to rigorously define and interpret various quantities that are often only described heuristically, such as the coherence time or length. The formalism further provides a continuous description of DM through the wave-particle transition, which we exploit to study how density fluctuations over various physical scales evolve between the two limits and to reveal the unique behavior of DM near the boundary of the wave and particle descriptions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Substrate-controlled dynamics of spin qubits in low dimensional van der Waals materials

We report a theoretical study of the coherence dynamics of spin qubits in two-dimensional materials (2DMs) and van der Waals heterostructures, as a function of the host thickness and the composition of the surrounding environment. We focus on MoS2 and WS2, two promising systems for quantum technology applications, and we consider the decoherence arising from the interaction of the spin qubit with nuclear spins. We show that the Hahn-echo coherence time is determined by a complex interplay between the source of decoherence in the qubit host and in the environment, which in turn determines whether the noise evolution is in a classical or quantum mechanical regime. We suggest that the composition and thickness of van der Waals heterostructures encapsulating a qubit host can be engineered to maximize coherence times. Finally, we discuss how quantum sensors may be able to probe the dynamics of the nuclear bath in 2DMs.

Onizhuk, Mykyta (ORCID:0000000304344575)↗

DOE OSTI2022

Quantum Fluctuations and Lineshape Anomaly in a High‐ β Silver‐Coated InP‐Based Metallic Nanolaser

Abstract Metallic nanocavity lasers provide important technological advancement toward even smaller integrable light sources. They give access to widely unexplored lasing physics in which the distinction between different operational regimes, like those of thermal or coherent light emission, becomes increasingly challenging upon approaching a device with a near‐perfect spontaneous‐emission coupling factor . In fact, quantum‐optical studies have to be employed to reveal a transition to coherent emission in the intensity fluctuation behavior of nanolasers when the input–output characteristic appears thresholdless for nanolasers. Here, a new indicator for lasing operation in high‐ lasers is identified by showing that stimulated emission can give rise to a lineshape anomaly manifested as a transition from a Lorentzian to a Gaussian component in the emission linewidth that dominates the spectrum above the lasing threshold.

Koulas‐Simos, Aris↗

DOE OSTI2026

Creating and Interfacing Designer Chemical Qubits (Final Technical Report)

The Final Technical Report describes a multi‑institution effort to develop programmable molecular qubits as precision quantum sensors for probing quantum materials. The team created chemically tunable qubits with optical addressability and practical coherence, integrated them into thin films and frameworks while preserving functionality, and established new magnetic and electric sensing methods suited to two‑dimensional magnets, ferroelectrics, and multiferroics. They also built computational models and spectroscopic tools that connect molecular design to material behavior, enabling access to quantum phenomena that previously could not be measured. The project produced more than 40 publications and trained a large cohort of graduate students and postdocs, strengthening the workforce and infrastructure needed for DOE's quantum information science mission.

2D Quantum Materials↗

DOE OSTI2022

Demonstration of long-range correlations via susceptibility measurements in a one-dimensional superconducting Josephson spin chain

Abstract Spin chains have long been considered an effective medium for long-range interactions, entanglement generation, and quantum state transfer. In this work, we explore the properties of a spin chain implemented with superconducting flux circuits, designed to act as a connectivity medium between two superconducting qubits. The susceptibility of the chain is probed and shown to support long-range, cross-chain correlations. In addition, interactions between the two end qubits, mediated by the coupler chain, are demonstrated. This work has direct applicability in near term quantum annealing processors as a means of generating long-range, coherent coupling between qubits.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Quantum computer-enabled receivers for optical communication

Abstract Optical communication is the standard for high-bandwidth information transfer in today’s digital age. The increasing demand for bandwidth has led to the maturation of coherent transceivers that use phase- and amplitude-modulated optical signals to encode more bits of information per transmitted pulse. Such encoding schemes achieve higher information density, but also require more complicated receivers to discriminate the signaling states. In fact, achieving the ultimate limit of optical communication capacity, especially in the low light regime, requires coherent joint detection of multiple pulses. Despite their superiority, such joint detection receivers are not in widespread use because of the difficulty of constructing them in the optical domain. In this work we describe how optomechanical transduction of phase information from coherent optical pulses to superconducting qubit states followed by the execution of trained short-depth variational quantum circuits can perform joint detection of communication codewords with error probabilities that surpass all classical, individual pulse detection receivers. Importantly, we utilize a model of optomechanical transduction that captures non-idealities such as thermal noise and loss in order to understand the transduction performance necessary to achieve a quantum advantage with such a scheme. We also execute the trained variational circuits on an IBM-Q device with the modeled transduced states as input to demonstrate that a quantum advantage is possible even with current levels of quantum computing hardware noise.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2024

Single phonon detection for dark matter via quantum evaporation and sensing of He 3

Dark matter is five times more abundant than ordinary visible matter in our Universe. While laboratory searches hunting for dark matter have traditionally focused on the electroweak scale, theories of low mass hidden sectors motivate new detection techniques. Extending these searches to lower mass ranges, well below 1 GeV / c 2 , poses new challenges as rare interactions with standard model matter transfer progressively less energy to electrons and nuclei in detectors. Here, we propose an approach based on phonon-assisted quantum evaporation combined with quantum sensors for detection of desorption events via tracking of spin coherence. The intent of our proposed dark matter sensors is to extend the parameter space to energy transfers in rare interactions to as low as a few meV for detection of dark matter particles in the keV / c 2 mass range. Published by the American Physical Society 2024

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Geometry-driven modeling of electron localization in InAs/GaAs double quantum dots

The coupled electronic states in two-dimensional (2D) and three-dimensional (3D) double quantum dot (DQD) systems are investigated using a phenomenological model applied to InAs/GaAs heterostructures. The single-band k • p effective potential approach previously proposed by our group is employed to numerically calculate the energy spectrum and spatial localization of a single electron, serving as an indicator of the coupling strength within the binary system. For identical quantum dots (QDs) in a DQD, the electronic states exhibit ideal coherence. We systematically vary the DQD geometry and the strength of the confinement potential (via an applied electric field) to examine the effects of symmetry breaking and the sensitivity of electron localization in both identical and nearly identical DQDs. Our results show that coherence in DQDs is highly sensitive to these subtle variations. This sensitivity can be harnessed to detect changes in the surrounding environment, such as fluctuations in chemical or electrical properties that affect the DQD system.

electron localization↗

DOE OSTI2024

Ultrathin Magnesium-Based Coating as an Efficient Oxygen Barrier for Superconducting Circuit Materials

Scaling up superconducting quantum circuits based on transmon qubits necessitates substantial enhancements in qubit coherence time. Over recent years, tantalum (Ta) has emerged as a promising candidate for transmon qubits, surpassing conventional counterparts in terms of coherence time. However, amorphous surface Ta oxide layer may introduce dielectric loss, ultimately placing a limit on the coherence time. In this study, a novel approach for suppressing the formation of tantalum oxide using an ultrathin magnesium (Mg) capping layer is presented. Synchrotron-based X-ray photoelectron spectroscopy studies demonstrate that oxide is confined to an extremely thin region directly beneath the Mg/Ta interface. Additionally, it is demonstrated that the superconducting properties of thin Ta films are improved following the Mg capping, exhibiting sharper and higher-temperature transitions to superconductive and magnetically ordered states. Moreover, an atomic-scale mechanistic understanding of the role of the capping layer in protecting Ta from oxidation is established based on computational modeling. Further, this work provides valuable insights into the formation mechanism and functionality of surface tantalum oxide, as well as a new materials design principle with the potential to reduce dielectric loss in superconducting quantum materials. Ultimately, the findings pave the way for the realization of large-scale, high-performance quantum computing systems.

36 MATERIALS SCIENCE↗