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  1. Abstract

    Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single-photon emitters or spin qubits, the uncontrolled, and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here, we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect–exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which competes together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single-photon emitters such as SiVVand spin qubits such as TiVVand MoVVin hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.

  2. Abstract

    The quantum simulation of quantum chemistry is a promising application of quantum computers. However, forNmolecular orbitals, the$${\mathcal{O}}({N}^{4})$$O(N4)gate complexity of performing Hamiltonian and unitary Coupled Cluster Trotter steps makes simulation based on such primitives challenging. We substantially reduce the gate complexity of such primitives through a two-step low-rank factorization of the Hamiltonian and cluster operator, accompanied by truncation of small terms. Using truncations that incur errors below chemical accuracy allow one to perform Trotter steps of the arbitrary basis electronic structure Hamiltonian with$${\mathcal{O}}({N}^{3})$$O(N3)gate complexity in small simulations, which reduces to$${\mathcal{O}}({N}^{2})$$O(N2)gate complexity in the asymptotic regime; and unitary Coupled Cluster Trotter steps with$${\mathcal{O}}({N}^{3})$$O(N3)gate complexity as a function of increasing basis size for a given molecule. In the case of the Hamiltonian Trotter step, these circuits have$${\mathcal{O}}({N}^{2})$$O(N2)depth on a linearly connected array, an improvement over the$${\mathcal{O}}({N}^{3})$$O(N3)scaling assuming no truncation. As a practical example, we show that a chemically accurate Hamiltonian Trotter step for a 50 qubit molecular simulation can be carried out in the molecular orbital basis with as few as 4000 layers of parallel nearest-neighbor two-qubit gates, consisting of fewer than 105non-Clifford rotations. We also apply our algorithm to iron–sulfur clusters relevant for elucidating the mode of action of metalloenzymes.

  3. Abstract

    Leakage is a particularly damaging error that occurs when a qubit state falls out of its two-level computational subspace. Compared to independent depolarizing noise, leaked qubits may produce many more configurations of harmful correlated errors during error-correction. In this work, we investigate different local codes in the low-error regime of a leakage gate error model. When restricting to bare-ancilla extraction, we observe that subsystem codes are good candidates for handling leakage, as their locality can limit damaging correlated errors. As a case study, we compare subspace surface codes to the subsystem surface codes introduced by Bravyiet al. In contrast to depolarizing noise, subsystem surface codes outperform same-distance subspace surface codes below error rates as high as ⪅ 7.5 × 10−4while offering better per-qubit distance protection. Furthermore, we show that at low to intermediate distances, Bacon–Shor codes offer better per-qubit error protection against leakage in an ion-trap motivated error model below error rates as high as ⪅ 1.2 × 10−3. For restricted leakage models, this advantage can be extended to higher distances by relaxing to unverified two-qubit cat state extraction in the surface code. These results highlight an intrinsic benefit of subsystem code locality to error-corrective performance.

  4. Abstract

    Understanding the near-field electromagnetic interactions that produce optical orbital angular momentum (OAM) is crucial for integrating twisted light into nanotechnology. Here, we examine the cathodoluminescence (CL) of plasmonic vortices carrying OAM generated in spiral nanostructures. The nanospiral geometry defines a photonic local density of states that is sampled by the electron probe in a scanning transmission electron microscope (STEM), thus accessing the optical response of the plasmonic vortex with high spatial and spectral resolution. We map the full spectral dispersion of the plasmonic vortex in spiral structures designed to yield increasing topological charge. Additionally, we fabricate nested nanospirals and demonstrate that OAM from one nanospiral can be coupled to the nested nanospiral, resulting in enhanced luminescence in concentric spirals of like handedness with respect to concentric spirals of opposite handedness. The results illustrate the potential for generating and coupling plasmonic vortices in chiral nanostructures for sensitive detection and manipulation of optical OAM.

  5. null (Ed.)
  6. Solid-state single-photon emitters (SPEs) such as the bright, stable, room-temperature defects within hexagonal boron nitride (hBN) are of increasing interest for quantum information science. To date, the atomic and electronic origins of SPEs within hBN have not been well understood, and no studies have reported photochromism or explored cross correlations between hBN SPEs. Here, we combine irradiation time-dependent microphotoluminescence spectroscopy with two-color Hanbury Brown–Twiss interferometry in an investigation of the electronic structure of hBN defects. We identify evidence of photochromism in an hBN SPE that exhibits single-photon cross correlations and correlated changes in the intensity of its two zero-phonon lines.