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Abstract Silicon is the ideal material for building electronic and photonic circuits at scale. Integrated photonic quantum technologies in silicon offer a promising path to scaling by leveraging advanced semiconductor manufacturing and integration capabilities. However, the lack of deterministic quantum light sources and strong photon-photon interactions in silicon poses a challenge to scalability. In this work, we demonstrate an indistinguishable photon source in silicon photonics based on an artificial atom. We show that a G center in a silicon waveguide can generate high-purity telecom-band single photons. We perform high-resolution spectroscopy and time-delayed two-photon interference to demonstrate the indistinguishability of single photons emitted from a G center in a silicon waveguide. Our results show that artificial atoms in silicon photonics can source single photons suitable for photonic quantum networks and processors. 

Rare-earth-free permanent magnet materials based on Mn show great promise for applications in electric motors and devices. The metastable ferromagnetic τ phase of the Mn-Al system has magnetic properties between those of the high-performance Nd-Fe-B magnets and the lower-performance ferrite magnets. However, the hybrid displacive-diffusional pathway of τ formation, from the parent ε phase through the intermediary ε’ phase, is still not fully understood. This phase transformation progression was studied in-situ using diffractive, calorimetric, and magnetometric techniques to show that the progression from ε to τ in Mn54Al46 at <450 ◦C involves the ordering of ε into ε’. Density functional theory calculations were performed on each phase and confirmed the experimental observation that the ε to ε’ to τ pathway is energetically favorable. Isothermal annealing of quenched-in ε at 350 ◦C demonstrated that ε’ is ferromagnetic, also in agreement with theoretical results, with a moderate coercivity of at least 50 kA/m. The τ phase was observed to nucleate along the prior ε phase grain boundaries and grow into the ε’ phase regions. A boundary front of ε’ was observed between the τ and ε phases. Both Kissinger and Flynn-Wall-Ozawa methods were used to determine the activation energies for the ε’ and τ phase transformations with values of ~140 kJ/mol obtained for both phases. Therefore, the ordering transformation to ε’ and the hybrid displacive-diffusional transformation to τ were shown to overcome the same magnitude energy barrier. Both activation energies were less than previous τ phase activation energies measured on Mn55Al45 in the absence of a significant ε’ ordering exotherm, providing a kinetic benefit to the ε to ε’ to τ pathway at 350 ◦C. The results of this study give insight into the phase transformation of L10 binary materials as well as materials that undergo a disorder–order transformation followed by displacive shear. 

Abstract There is tremendous interest in employing collective excitations of the lattice, spin, charge, and orbitals to tune strongly correlated electronic phenomena. We report such an effect in a ruthenate, Ca₃Ru₂O₇, where two phonons with strong electron-phonon coupling modulate the electronic pseudogap as well as mediate charge and spin density wave fluctuations. Combining temperature-dependent Raman spectroscopy with density functional theory reveals two phonons,B₂^PandB₂^M, that are strongly coupled to electrons and whose scattering intensities respectively dominate in the pseudogap versus the metallic phases. TheB₂^Psqueezes the octahedra along the out of planec-axis, while theB₂^Melongates it, thus modulating the Ru 4d orbital splitting and the bandwidth of the in-plane electron hopping; Thus,B₂^Popens the pseudogap, whileB₂^Mcloses it. Moreover, theB₂phonons mediate incoherent charge and spin density wave fluctuations, as evidenced by changes in the background electronic Raman scattering that exhibit unique symmetry signatures. The polar order breaks inversion symmetry, enabling infrared activity of these phonons, paving the way for coherent light-driven control of electronic transport. 

Abstract Point defects in two-dimensional materials are of key interest for quantum information science. However, the parameter space of possible defects is immense, making the identification of high-performance quantum defects very challenging. Here, we perform high-throughput (HT) first-principles computational screening to search for promising quantum defects within WS₂, which present localized levels in the band gap that can lead to bright optical transitions in the visible or telecom regime. Our computed database spans more than 700 charged defects formed through substitution on the tungsten or sulfur site. We found that sulfur substitutions enable the most promising quantum defects. We computationally identify the neutral cobalt substitution to sulfur (Co$${}_{{{{{{{{\rm{S}}}}}}}}}^{0}$$ ${}_S^0$) and fabricate it with scanning tunneling microscopy (STM). The Co$${}_{{{{{{{{\rm{S}}}}}}}}}^{0}$$ ${}_S^0$electronic structure measured by STM agrees with first principles and showcases an attractive quantum defect. Our work shows how HT computational screening and nanoscale synthesis routes can be combined to design promising quantum defects. 

Nonlinear optical (NLO) crystals with superior properties are significant for advancing laser technologies and applications. Introducing rare earth metals to borates is a promising and effective way to modify the electronic structure of a crystal to improve its optical properties in the visible and ultraviolet range. In this work, we computationally discover inversion symmetry breaking in EuBa₃(B₃O₆)₃, which was previously identified as centric, and demonstrate noncentrosymmetry via synthesizing single crystals for the first time by the floating zone method. We determine the correct space group to beP6¯. The material has a large direct bandgap of 5.56 eV and is transparent down to 250 nm. The complete anisotropic linear and nonlinear optical properties were also investigated with ad₁₁of ∼0.52 pm/V for optical second harmonic generation. Further, it is Type I and Type II phase matchable. This work suggests that rare earth metal borates are an excellent crystal family for exploring future deep ultraviolet (DUV) NLO crystals. It also highlights how first principles computations combined with experiments can be used to identify noncentrosymmetric materials that have been wrongly assigned to be centrosymmetric. 

The interplay of synthesis, experiments, and theory in broadening the landscape of thermoelectric materials is reported. 

Abstract Nonaqueous sodium-based batteries are ideal candidates for the next generation of electrochemical energy storage devices. However, despite the promising performance at ambient temperature, their low-temperature (e.g., < 0 °C) operation is detrimentally affected by the increase in the electrolyte resistance and solid electrolyte interphase (SEI) instability. Here, to circumvent these issues, we propose specific electrolyte formulations comprising linear and cyclic ether-based solvents and sodium trifluoromethanesulfonate salt that are thermally stable down to −150 °C and enable the formation of a stable SEI at low temperatures. When tested in the Na||Na coin cell configuration, the low-temperature electrolytes enable long-term cycling down to −80 °C. Via ex situ physicochemical (e.g., X-ray photoelectron spectroscopy, cryogenic transmission electron microscopy and atomic force microscopy) electrode measurements and density functional theory calculations, we investigate the mechanisms responsible for efficient low-temperature electrochemical performance. We also report the assembly and testing between −20 °C and −60 °C of full Na||Na 3 V 2 (PO 4 ) 3 coin cells. The cell tested at −40 °C shows an initial discharge capacity of 68 mAh g −1 with a capacity retention of approximately 94% after 100 cycles at 22 mA g −1 .