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Quantum information processing and quantum sensing is a central topic for researchers who are part of the Materials Research Society and the Quantum Staging Group is providing leadership and guidance in this context. We convened a workshop before the 2022 MRS Spring Meeting and covered four topics to explore challenges that need to be addressed to further promote and accelerate the development of materials with applications in quantum technologies. This article captures the discussions at this workshop and refers to the pertinent literature.

 

The molecule-based ferrimagnetic semiconductor vanadium tetracyanoethylene (V[TCNE] x , x [Formula: see text] 2) has garnered interest from the quantum information community due to its excellent coherent magnonic properties and ease of on-chip integration. Despite these attractive properties, a detailed understanding of the electronic structure and mechanism for long-range magnetic ordering have remained elusive due to a lack of detailed atomic and electronic structural information. Previous studies via x-ray absorption near edge spectroscopy and the extended x-ray absorption fine structure have led to various proposed structures, and in general, V[TCNE] x is believed to be a three-dimensional network of octahedrally coordinated V 2+ , each bonded to six TCNE molecules. Here, we elucidate the electronic structure, structural ordering, and degradation pathways of V[TCNE] x films by correlating calculations of density functional theory (DFT) with scanning transmission electron microscopy and electron energy-loss spectroscopy (EELS) of V[TCNE] x films. Low-loss EELS measurements reveal a bandgap and an excited state structure that agree quantitatively with DFT modeling, including an energy splitting between apical and equatorial TCNE ligands within the structure, providing experimental results directly backed by theoretical descriptions of the electronic structure driving the robust magnetic ordering in these films. Core-loss EELS confirms the presence of octahedrally coordinated V +2 atoms. Upon oxidation, changes in the C1s- π* peak indicate that C=C of TCNE is preferentially attacked. Furthermore, we identify a relaxation of the structural ordering as the films age. These results lay the foundation for a more comprehensive and fundamental understanding of magnetic ordering and dynamics in these classes of metal–ligand compounds. 

In this work, we investigate multiphoton and optical field tunneling emission from metallic surfaces with nanoscale vacuum gaps. Using time-dependent Schrödinger equation (TDSE) simulations, we find that the properties of the emitted photocurrent in such systems can be greatly altered by the application of only a few-volt direct current (DC) bias. We find that when coupled with expected plasmonic enhancements within the nanometer-scale metallic gaps, the application of this DC bias significantly reduces the threshold for the transition to optical-field-driven tunneling from the metal surface, and could sufficiently enhance the emitted photocurrents, to make it feasible to electronically tag fJ ultrafast pulses at room temperature. Given the petahertz-scale instantaneous response of the photocurrents, and the low effective capacitance of thin-film nanoantenna devices that enables$<<\#comment/>1\mathrm{f}\mathrm{s}$response time, detectors that exploit this bias-enhanced surface emission from nanoscale vacuum gaps could prove to be useful for communication, petahertz electronics, and ultrafast optical-field-resolved metrology.