Radiative recombination processes can occur in solid-state systems through the pairing of donor and acceptor defects of the lattice. Recently, donor-acceptor pairs (DAP) have been proposed as promising candidates for quantum applications, and their signature has been observed in emerging low-dimensional materials. Therefore, the identification of such processes is gaining interest and requires methods to efficiently and reliably characterize them. Here, we introduce a general algorithm to identify DAP processes starting from the experimental photoluminescence (PL) emission spectrum and basic material parameters, including the lattice structure and dielectric constant. The algorithm recognizes possible DAP transitions from the emission pattern in the spectrum and returns the characteristic energy of the DAP transition and the separation between the donor and acceptor sites. By testing the algorithm on the photoluminescence spectrum of hexagonal boron nitride (hBN), we show that our method is robust against experimental errors and adds new capabilities to the investigation toolbox of semiconductors and their optical properties.
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Single-photon emitters serve as building blocks for many emerging concepts in quantum photonics. The recent identification of bright, tunable and stable emitters in hexagonal boron nitride (hBN) has opened the door to quantum platforms operating across the infrared to ultraviolet spectrum. Although it is widely acknowledged that defects are responsible for single-photon emitters in hBN, crucial details regarding their origin, electronic levels and orbital involvement remain unknown. Here we employ a combination of resonant inelastic X-ray scattering and photoluminescence spectroscopy in defective hBN, unveiling an elementary excitation at 285 meV that gives rise to a plethora of harmonics correlated with single-photon emitters. We discuss the importance of N π* anti-bonding orbitals in shaping the electronic states of the emitters. The discovery of elementary excitations in hBN provides fundamental insights into quantum emission in low-dimensional materials, paving the way for future investigations in other platforms.more » « lessFree, publicly-accessible full text available April 23, 2025
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Most resonant inelastic x-ray scattering (RIXS) studies of dynamic charge order correlations in the cuprates have focused on the high-symmetry directions of the copper oxide plane. However, scattering along other in-plane directions should not be ignored as it may help understand, for example, the origin of charge order correlations or the isotropic scattering resulting in strange metal behavior. Our RIXS experiments reveal dynamic charge correlations over the
qx-qy scattering plane in underdoped Bi2Sr2CaCu2O8+δ. Tracking the softening of the RIXS-measured bond-stretching phonon, we show that these dynamic correlations exist at energies below approximately 70 meV and are centered around a quasi-circular manifold in theqx-qy scattering plane with radius equal to the magnitude of the charge order wave vector,q CO. This phonon-tracking procedure also allows us to rule out fluctuations of short-range directional charge order (i.e., centered around [qx = ±q CO,qy = 0] and [qx = 0,qy = ±q CO]) as the origin of the observed correlations. -
Abstract The sustained interest in investigating magnetism in the 2D limit of insulating antiferromagnets is driven by the possibilities of discovering, or engineering, novel magnetic phases through layer stacking. However, due to the difficulty of directly measuring magnetic interactions in 2D antiferromagnets, it is not yet understood how
intra layer magnetic interactions ininsulating , strongly correlated, materials can be modified through layer proximity. Herein, the impact of reduced dimensionality in the model van der Waals antiferromagnet NiPS3is explored by measuring electronic excitations in exfoliated samples using Resonant Inelastic X‐ray Scattering (RIXS). The resulting spectra shows systematic broadening of NiS6multiplet excitations with decreasing layer count from bulk down to three atomic layers (3L). It is shown that these trends originate from a decrease in transition metal‐ligand and ligand–ligand hopping integrals, and by charge‐transfer energy evolving from Δ = 0.83 eV in the bulk to 0.37 eV in 3L NiPS3. Relevant intralayer magnetic exchange integrals computed from the electronic parameters exhibit a decrease in the average interaction strength with thickness. This study underscores the influence ofinter layer electronic interactions onintra layer ones in insulating magnets, indicating that magnetic Hamiltonians in few‐layer insulating magnets can greatly deviate from their bulk counterparts. -
Abstract The omnipresence of charge density waves (CDWs) across almost all cuprate families underpins a common organizing principle. However, a longstanding debate of whether its spatial symmetry is stripe or checkerboard remains unresolved. While CDWs in lanthanum‐ and yttrium‐based cuprates possess a stripe symmetry, distinguishing these two scenarios is challenging for the short‐range CDW in bismuth‐based cuprates. Here, high‐resolution resonant inelastic x‐ray scattering is employed to uncover the spatial symmetry of the CDW in Bi2Sr2 −
x Lax CuO6 + δ. Across a wide range of doping and temperature, anisotropic CDW peaks with elliptical shapes are found in reciprocal space. Based on Fourier transform analysis of real‐space models, the results are interpreted as evidence of unidirectional charge stripes, hosted by mutually 90°‐rotated anisotropic domains. This work paves the way for a unified symmetry and microscopic description of CDW order in cuprates. -
Abstract Complex oxide films stabilized by epitaxial growth can exhibit large populations of point defects which have important effects on their properties. The site occupancy of pulsed laser‐deposited epitaxial terbium iron garnet (TbIG) films with excess terbium (Tb) is analyzed, in which the terbium:iron (Tb:Fe)ratio is 0.86 compared to the stoichiometric value of 0.6. The magnetic properties of the TbIG are sensitive to site occupancy, exhibiting a higher compensation temperature (by 90 K) and a lower Curie temperature (by 40 K) than the bulk Tb3Fe5O12garnet. Data derived from X‐ray core‐level spectroscopy, magnetometry, and molecular field coefficient modeling are consistent with occupancy of the dodecahedral sites by Tb3+, the octahedral sites by Fe3+, Tb3+and vacancies, and the tetrahedral sites by Fe3+and vacancies. Energy dispersive X‐ray spectroscopy in a scanning transmission electron microscope provides direct evidence of TbFeantisites. A small fraction of Fe2+is present, and oxygen vacancies are inferred to be present to maintain charge neutrality. Variation of the site occupancies provides a path to considerable manipulation of the magnetic properties of epitaxial iron garnet films and other complex oxides, which readily accommodate stoichiometries not found in their bulk counterparts.