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DOE OSTI2020

Quandary

Quandary numerically simulates and optimizes the time-evolution of open quantum systems. The underlying dynamics are modelled by Lindblad's master equation, a linear ordinary differential equation (ODE) describing quantum systems interacting with the environment. Quandary solves this ODE numerically by applying a time-stepping integration scheme, and utilizes a gradient-based optimization approach to determine optimal control pulses that drive the quantum system to a desired target state. Two optimization objectives are considered: (a) Unitary gate optimization that finds controls to realize a unitary gate transformation, and (b) optimal reset that aims to drive the quantum system to the ground states. Gradient-based optimization schemes utilizing Petsc's Tao optimization package are applied to generate control pulses that minimize the respective measure. To evaluate the gradient of the objective function, the discrete adjoint method is used while leveraging techniques from Algorithmic Differentiation to produce exact and consistent gradients. To mitigate excessive execution run times, the software can be build together with the XBraid software library which provides a parallelization strategy to distribute the time-evolution of the underlying dynamics onto multiple processor.

Petersson, NilsA.↗

DOE OSTI2026

Purcell enhancement of directional edge photocurrent in a van der Waals self-cavity

Cavities provide a means to manipulate the optical and electronic responses of quantum materials by selectively enhancing light-matter interaction at specific frequencies and momenta. While cavities typically involve external structures, exfoliated flakes of van der Waals (vdW) materials can form intrinsic self-cavities due to their small finite dimensions, confining electromagnetic fields into plasmonic cavity modes, characterized by standing-wave current distributions. While cavity-enhanced phenomena are well-studied at optical frequencies, the impact of self-cavities on nonlinear electronic responses—such as directional photocurrent—remains largely unexplored, particularly in the terahertz regime, critical for emerging ultrafast optoelectronic technologies. Here, we report a self-cavity-induced Purcell enhancement of directional photocurrents in the vdW semimetal WTe 2 . Using ultrafast optoelectronic circuitry, we measured coherent near-field THz emission resulting from nonlinear photocurrents excited at the sample edges. We observed enhanced emission at finite frequencies, tunable via excitation fluence and sample geometry, which we attribute to plasmonic interference effects controlled by the cavity boundaries. We developed an analytical theory that captures the cavity resonance conditions and spectral response across multiple devices. Our findings establish WTe 2 as a bias-free, geometry-tunable THz emitter and demonstrate the potential of self-cavity engineering for controlling nonlinear, nonequilibrium dynamics in quantum materials.

condensed-matter physics↗

DOE OSTI2023

Frequency combs in optically injected terahertz ring quantum cascade lasers

Quantum cascade lasers (QCLs) have emerged as promising candidates for generating chip-scale frequency combs in mid-infrared and terahertz wavelengths. In this work, we demonstrate frequency comb formation in ring terahertz QCLs using the injection of light from a distributed feedback (DFB) laser. The DFB design frequency is chosen to match the modes of the ring cavity (near 3.3 THz), and light from the DFB is injected into the ring QCL via a bus waveguide. By controlling the power and frequency of the optical injection, we show that combs can be selectively formed and controlled in the ring cavity. Numerical modeling suggests that this comb is primarily frequency-modulated in character, with the injection serving to trigger comb formation. We also show that the ring can be used as a filter to control the output of the DFB QCL, potentially being of interest in terahertz photonic integrated circuits. Our work demonstrates that waveguide couplers are a compelling approach for injecting and extracting radiation from ring terahertz combs and offer exciting possibilities for the generation of new comb states in terahertz, such as frequency-modulated waves, solitons, and more.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Direct Observation of 2DEG States in Shallow Si:Sb δ-Layers

We investigate the electronic structure of high-density layers of Sb dopants in a silicon host, so-called Si:Sb δ-layers. We show that, in spite of the known challenges in producing highly confined Sb δ-layers, sufficient confinement is created such that the lowest conduction band states (Γ states, studied in depth in other silicon δ-layers), become occupied and can be observed using angle-resolved photoemission spectroscopy. The electronic structure of the Si:Sb δ-layers closely resembles that of Si:P systems, where the observed conduction band is near-parabolic and slightly anisotropic in the k ∥ plane. The observed Γ state extends ∼1 nm in the out-of-plane direction, which is slightly wider than the 1/3 monolayer thick dopant distribution. This is caused by a small segregation of the dopant layer, which is nevertheless minimal when comparing with earlier published attempts. Our results serve to demonstrate that Sb is still a feasible dopant alternative for use in the semiconductor δ-layer platform, providing similar electronic functionality to Si:P systems. Additionally, it has the advantages of being less expensive, more controllable, safer to handle, and more compatible with industrial patterning techniques. Si:Sb is therefore a viable platform for emerging quantum device applications.

Deposition↗

DOE OSTI2024

Isotope engineering for spin defects in van der Waals materials

Abstract Spin defects in van der Waals materials offer a promising platform for advancing quantum technologies. Here, we propose and demonstrate a powerful technique based on isotope engineering of host materials to significantly enhance the coherence properties of embedded spin defects. Focusing on the recently-discovered negatively charged boron vacancy center ($${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − ) in hexagonal boron nitride (hBN), we grow isotopically purified h 10 B 15 N crystals. Compared to$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − in hBN with the natural distribution of isotopes, we observe substantially narrower and less crowded$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − spin transitions as well as extended coherence timeT 2 and relaxation timeT 1 . For quantum sensing,$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − centers in our h 10 B 15 N samples exhibit a factor of 4 (2) enhancement in DC (AC) magnetic field sensitivity. For additional quantum resources, the individual addressability of the$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − hyperfine levels enables the dynamical polarization and coherent control of the three nearest-neighbor 15 N nuclear spins. Our results demonstrate the power of isotope engineering for enhancing the properties of quantum spin defects in hBN, and can be readily extended to improving spin qubits in a broad family of van der Waals materials.

Science & Technology - Other Topics↗

DOE OSTI2026

Measurement of the QE Map

113 MHz SRF gun utilized CsK 2 Sb and Na 2 KSb cathodes, which were irradiated with a pulsed green laser with a wavelength of 0.53 microns. The drive laser generated 78 kHz pulses with an acousto-optic modulator selecting the desired number of pulses reaching the cathode. The operator can select the aperture size, defining the laser spot diameter on the cathode, and the power level, which is controlled by a rotating polarizer. The laser power reaching the cathode can be measured with a meter based on a photodiode. The quantum efficiency (QE) of a photocathode serves as a primary indicator of its state. Small QE renders the cathode unusable when the desired bunch charge cannot be achieved. Strong variations in the quantum efficiency on the cathode surface might lead to the growth of the beam emittance due to the space charge effects. We have created a routine to measure the distribution of the QE on the cathode. The operator selects the aperture size, the central spot location, and the scan ranges for both planes. The scan starts from the central spots and proceeds along a spiral-like trajectory, making N rounds. The number of rounds can be chosen, and the total number of measured points is (2N+1) 2 . The laser spot movement is shown in Fig. 1.

43 PARTICLE ACCELERATORS↗

DOE OSTI2025

Quantum Enhanced Dark-Matter Search with Entangled Fock States in High-Quality Cavities

We present a quantum-enhanced protocol for detecting wave-like dark matter using an array of $N$ entangled superconducting cavities initialized in an $m$-photon Fock state. By distributing and recollecting the quantum state with an entanglement-distribution operation, the scan rate scales as $N^2(m+1)$ while thermal excitation is the dominant background, significantly outperforming classical single-cavity methods under matched conditions. We evaluate the robustness of our scheme against additional noise sources, including decoherence and beamsplitter infidelity, through theoretical analysis and numerical simulations. In practice, the key requirements, namely high-Q superconducting radio-frequency cavities that support long integration times, high-fidelity microwave beamsplitters, and universal cavity control, are already available on current experimental platforms, making the protocol experimentally feasible.

Freiman, Benjamin [Fermilab]↗

DOE OSTI2021

Effect of surface disorder on the chiral surface states of a three-dimensional quantum Hall system

We investigate the effect of surface disorder on the chiral surface states of a three-dimensional quantum Hall system. Utilizing a transfer-matrix method, we find that the localization length of the surface state along the magnetic field decreases with the surface disorder strength in the weak disorder regime but increases anomalously in the strong disorder regime. In the strong disorder regime, the surface states mainly locate at the first inward layer to avoid the strong disorder in the outmost layer. The anomalous increase of the localization length can be explained by an effective model, which maps the strong disorder on the surface layer to the weak disorder on the first inward layer. Our work demonstrates that surface disorder can be an effective way to control the transport behavior of the surface states along the magnetic field. We also investigate the effect of surface disorder on the full distribution of conductances P(g) of the surface states in the quasi-one-dimensional (1D) regime for various surface disorder strengths. In particular, we find that P(g) is Gaussian in the quasi-1D metal regime and log-normal in the quasi-1D insulator regime. In the crossover regime, P(g) exhibits highly nontrivial forms, whose shapes coincide with the results obtained from the Dorokhov-Mello-Pereyra-Kumar equation of a weakly disordered quasi-1D wire in the absence of time-reversal symmetry. Our results suggest that P(g) is fully determined by the average conductance, independent of the details of the system, in agreement with the single-parameter scaling hypothesis.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Stroboscopic x-ray diffraction microscopy of dynamic strain in diamond thin-film bulk acoustic resonators for quantum control of nitrogen-vacancy centers

Bulk-mode acoustic waves in a crystalline material exert lattice strain through the thickness of the sample, which couples to the spin Hamiltonian of defect-based qubits such as the nitrogen-vacancy (N-V) center defect in diamond. This mechanism has previously been harnessed for unconventional quantum spin control, spin decoherence protection, and quantum sensing. Bulk-mode acoustic wave devices are also important in the microelectronics industry as microwave filters. A key challenge in both applications is a lack of appropriate operando microscopy tools for quantifying and visualizing gigahertz-frequency dynamic strain. Here, in this work, we directly image acoustic strain within N-V center-coupled diamond thin-film bulk acoustic wave resonators using stroboscopic scanning hard x-ray diffraction microscopy at the Advanced Photon Source. The far-field scattering patterns of the nanofocused x-ray diffraction encode strain information entirely through the illuminated thickness of the resonator. These patterns have a real-space spatial variation that is consistent with the bulk strain’s expected modal distribution and a momentum-space angular variation from which the strain amplitude can be quantitatively deduced. We also perform optical measurements of strain-driven Rabi precession of of the N-V center spin ensemble, providing an additional quantitative measurement of the strain amplitude. As a result, we directly measure one of the six N-V spin-stress coupling parameters, 𝑏 =2.73⁢(2) MHz/GPa, by correlating these measurements at the same spatial position and applied microwave power. Our results demonstrate a unique technique for directly imaging ac lattice strain in micromechanical structures and provide a direct measurement of a fundamental constant for the N-V center defect spin Hamiltonian.

acoustic techniques↗

DOE OSTI2021

Intrinsic donor-bound excitons in ultraclean monolayer semiconductors

The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability. Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe 2 . These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping. They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (>6 µs) and polarization lifetimes (>100 ns). Resonant excitation of the free inter- and intravalley bright trions leads to opposite optical orientation of the satellites, while excitation of the free dark trion resonance suppresses the satellites' photoluminescence. Defect-controlled crystal synthesis and scanning tunneling microscopy measurements provide corroboration that these features are dark excitons bound to dilute donors, along with associated phonon replicas. Our work opens opportunities to engineer homogenous single emitters and explore collective quantum optical phenomena using intrinsic donor-bound excitons in ultraclean 2D semiconductors.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Defects go green: using defects in nanomaterials for renewable energy and environmental sustainability

Induction of point defects in nanomaterials can bestow upon them entirely new physics or augment their pre-existing physical properties, thereby expanding their potential use in green energy technology. Predicting structure-property relationships for defects a priori is challenging, and developing methods for precise control of defect type, density, or structural distribution during synthesis is an even more formidable task. Hence, tuning the defect structure to tailor nanomaterials for enhanced device performance remains an underutilized tool in materials design. We review here the state of nanomaterial design through the lens of computational prediction of defect properties for green energy technology, and synthesis methods to control defect formation for optimal performance. We illustrate the efficacy of defect-focused approaches for refining nanomaterial physics by describing several specific applications where these techniques hold potential. Most notably, we focus on quantum dots for reabsorption-free solar windows and net-zero emission buildings, oxide cathodes for high energy density lithium-ion batteries and electric vehicles, and transition metal dichalcogenides for electrocatalytic green hydrogen production and carbon-free fuels.

14 SOLAR ENERGY↗

DOE OSTI2022

Nanoscale interplay of native point defects near Sr-deficient SrxTiO 3 /SrTiO 3 interfaces

SrTiO 3 has many applications involving interfaces with other materials, but defects that affect the properties of SrTiO 3 films can also play a significant role at its heterointerfaces and even at junctions with nonstoichiometric SrTiO 3 . Depth-resolved cathodoluminescence spectroscopy (DRCLS) combined with systematic cation Sr content reduction in SrxTiO 3 ultrathin films grown on SrTiO 3 showed an interplay of native point defects and electronic structure within the Sr-deficient film and how interplay extends tens of nanometers into the substrate below. Understanding how defects form and affect interface electronic structure during epitaxial growth is central to improving complex oxide devices. Controlling the balance of oxygen vacancy defects with strontium vacancies and other acceptor-like defects can improve control over free carrier densities. Likewise, control over nanoscale defect charge distributions can advance new device features such as two-dimensional hole gases and the performance of existing devices such as ferroelectric tunnel junctions. This study shows how DRCLS directly measures the relative densities and spatial distributions of multiple native defects within and extending away from nanoscale SrxTiO 3 /SrTiO 3 junctions and how their interplay varies with controlled epitaxial growth. In turn, these growth-dependent defect variations can help guide SrTiO 3 epitaxial growth with other complex oxides.

36 MATERIALS SCIENCE↗

DOE OSTI2025

A Review of Quantum Computing Technologies in Power System Optimization

As modern power grids increasingly integrate variable renewable generation, distributed energy resources, and energy storage systems, classical optimization techniques are facing unprecedented challenges. This review examines the emerging application of quantum computing to overcome these challenges in power system optimization, including optimal power flow (OPF), unit commitment (UC), economic dispatch (ED), and intelligent switching and topology optimization (IS-TO). Recent research has introduced various quantum methodologies—such as gate-based, annealing-based, variational algorithms, and quantum-inspired algorithms—to address the combinatorial complexity inherent in grid reconfiguration and energy management. The review summaries the quantum algorithms, quantum devices and the power system test cases, highlighting hybrid quantum–classical strategies that leverage the complementary strengths of both paradigms. Some quantum advantages have been observed, including theoretical speedup, accurate simulation results, scalable qubit usage, efficient QUBO mapping. In particular, the review emphasizes the importance of integrating quantum optimization techniques with classical control frameworks, these hybrid approaches demonstrate the potential to improve real-time grid management and operational reliability. A significant portion of the analysis is devoted to the practical limitations of current quantum devices. Present-day quantum hardware, operating in the noisy intermediate-scale quantum (NISQ) era, remains highly sensitive to noise and limited in qubit connectivity, which constrains the scale and accuracy of implemented algorithms. The review delves into specific challenges such as the need for qubit-efficient encoding techniques and error mitigation strategies that are critical for handling real-world grid optimization problems. In addition, the work draws attention to the performance discrepancies between theoretical quantum speedups and experimental validations, underscoring the importance of rigorous benchmark studies using representative power grid test cases. In summary, this review highlights both the promise and limitations of quantum computing for power system optimization. It provides a comprehensive overview of the state-of-the-art technologies, categorizes recent advancements in algorithm design, and discusses practical considerations for implementation, and serves as an informative resource on current research. Future research directions include developing robust hybrid frameworks, advancing qubit-efficient formulations, and scaling up experimental demonstrations to confirm the theoretical advantages of quantum methods in large-scale power system operations.

24 POWER TRANSMISSION AND DISTRIBUTION↗

DOE OSTI2020

Effects of lithium intercalation in twisted bilayer graphene

In this work, we investigate the effects of lithium intercalation in twisted bilayers of graphene, using first-principles electronic structure calculations. To model this system we employ commensurate supercells that correspond to twist angles of 7.34° and 2.45°. From the energetics of lithium absorption we demonstrate that for low Li concentration the intercalants cluster in the AA regions with double the density of a uniform distribution. The charge donated by the Li atoms to the graphene layers results in modifications to the band structure that can be qualitatively captured using a continuum model with modified interlayer couplings in a region of parameter space that has yet to be explored either experimentally or theoretically. Thus, the combination of intercalation and twisted layers simultaneously provides the means for spatial control over material properties and an additional knob with which to tune moiré physics in twisted bilayers of graphene, with potential applications ranging from energy storage and conversion to quantum information.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Does Carrier Envelope Phase Affect the Ionization Site in a Neutral Diatomic Molecule?

A recent work shows how to extract the ionization site of a neutral diatomic molecule by comparing Quantum Trajectory Monte Carlo (QTMC) simulations with experimental measurements of the final electron momenta distribution. This method was applied to an experiment using a 40-femtosecond infrared pulse, finding that a downfield atom is roughly twice as likely to be ionized as an upfield atom in a neutral nitrogen molecule. However, an open question remains as to whether an assumption of the zero carrier envelope phase (CEP) used in the above work is still valid for short, few-cycle pulses where the CEP can play a large role. Given experimentalists’ limited control over the CEP and its dramatic effect on electron momenta after ionization, it is desirable to see what influence the CEP may have in determining the ionization site. In this paper, we employ QTMC techniques to simulate strong-field ionization and electron propagation from neutral N2 using an intense 6-cycle laser pulse with various CEP values. Comparing simulated electron momenta to experimental data indicates that the ratio of down-to-upfield ions remains roughly 2:1 regardless of the CEP. This confirms that the ionization site of a neutral molecule is determined predominantly by the laser frequency and intensity, as well as the ground-state molecular wavefunction, and is largely independent of the CEP.

Schimmoller, Alex↗

DOE OSTI2023

Fabricating Single Crystal Quantum Dot Solids

The central goal of this research program was to establish fundamental synthesis and processing principles to enable the fabrication of single crystal quantum dot solids (QDS) with programmable structure (i.e., hexagonal and square) and composition. Our approach towards that goal leveraged access to and experience with unique in-situ, multi-probe characterization techniques to understand and ultimately control the fundamental relationship between processing conditions and nucleation and growth of QDS. The program integrated synthesis and fabrication (Hanrath) with in-situ TEM analysis (Kourkoutis) and computational modeling (Clancy) to gain atomic-level insights into the underlying physical phenomena governing assembly and attachment and to guide the development of optimized processing methods. We have established a foundational understanding of physicochemical interactions of self-assembly at a fluid interface, superlattice structure transformation pathways, the critical role of disorder during the initial dimerization of colloidal quantum dot monomers, and the residual strain distribution within the inter-dot epitaxial bridge which hampers the formation of novel electronics states of the quantum dot solids. Collectively, these insights have contributed towards advancing the mechanistic understanding of the complex choreography of assembly and attachment as well as understanding what currently limits further advances in high-fidelity quantum dot solids and tiles.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Dynamically controlled random lasing with colloidal titanium carbide MXene

Control of lasing properties through tailorable and dynamically tunable materials and reconfigurable compositions can augment the performance of random lasers for a wide range of applications. Here, a colloid of randomly dispersed weakly scattering single-layer titanium carbide (Ti 3 C 2 T x ) MXene flakes embedded within rhodamine 101 gain medium is experimentally shown to provide feedback for random lasing. Additionally, in contrast to previously reported random laser systems where the optical properties of scatterers are static, the relative permittivity of Ti 3 C 2 T x MXene flakes can be varied under optical pumping due to the saturable absorption properties. Numerical simulations indicate that the observed nonlinear response of Ti 3 C 2 T x MXene flakes enables dynamically tunable random lasing. Thus, pumping the Ti 3 C 2 T x MXene flakes with a second optical source decreases the gain threshold required to obtain random lasing. Also, using numerical simulations, it is shown that the control over the intensity of the second pump enables tuning the field distribution of the random lasing modes. Considering the diversity of the MXenes family, the proposed MXene colloidal metamaterial design opens up a new avenue to advanced control of lasing properties for photonic applications.

36 MATERIALS SCIENCE↗

NASA NTRS1984

Comparative lifetesting results for microchannel plates in windowless EUV photon detectors

Microchannel plates (MCPs) from seven manufacturers were subjected to a series of tests to determine their suitability for the Extreme Ultraviolet Explorer satellite. Comparative data are presented for sixteen MCP tandem pairs with channel length to diameter ratios (l/d) ranging from 40:1 to 60:1 and for two saturable (curved channel) MCPs with l/d's of 80:1. Results for MCPs with funnelled channel throats are also discussed. Properties of the MCPs which were monitored include: background count rate, output charge pulse height distribution (PHD), modal gain, PHD full width half maximum (FWHM), and extreme ultraviolet (EUV) photon quantum efficiency. Five detectors were chosen for further lifetime testing consisting of a mild bake to 100 C, and charge extraction to 0.01 coulombs, repeated high voltage cycling and reexposure to one atmosphere conditions. The results of these tests and their implications for the flight detectors are discussed. Erratic events in the detector background were recorded, probably due to field emission from high voltage surfaces or the absorption of water vapor into the electrode following exposure to air. The steps taken to control the detector background are discussed.

Malina, R. F.↗