Coherent spin-control of S = 1 vanadium and molybdenum complexes
The burgeoning field of quantum sensing hinges on the creation and control of quantum bits. To date, the most well-studied quantum sensors are optically active, paramagnetic defects residing in crystalline hosts. We previously developed analogous optically addressable molecules featuring a ground-st...
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Veröffentlicht in: | Chemical science (Cambridge) 2024-08, Vol.15 (34), p.14016-14026 |
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Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | The burgeoning field of quantum sensing hinges on the creation and control of quantum bits. To date, the most well-studied quantum sensors are optically active, paramagnetic defects residing in crystalline hosts. We previously developed analogous optically addressable molecules featuring a ground-state spin-triplet centered on a Cr
ion with an optical-spin interface. In this work, we evaluate isovalent V
and Mo
congeners, which offer unique advantages, such as an intrinsic nuclear spin for V
or larger spin-orbit coupling for Mo
, as optically addressable spin systems. We assess the ground-state spin structure and dynamics for each complex, illustrating that all of these spin-triplet species can be coherently controlled. However, unlike the Cr
derivatives, these pseudo-tetrahedral V
and Mo
complexes exhibit no measurable emission. Coupling absorption spectroscopy with computational predictions, we investigate why these complexes exhibit no detectable photoluminescence. These cumulative results suggest that design of future V
complexes should target pseudo-tetrahedral symmetries using bidentate or tridentate ligand scaffolds, ideally with deuterated or fluorinated ligand environments. We also suggest that spin-triplet Mo
, and by extension W
, complexes may not be suitable candidate optically addressable qubit systems due to their low energy spin-singlet states. By understanding the failures and successes of these systems, we outline additional design features for optically addressable V- or Mo-based molecules to expand the library of tailor-made quantum sensors. |
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ISSN: | 2041-6520 2041-6539 |
DOI: | 10.1039/d4sc03107e |