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This work describes the engineering and characterization methods required to control all four principle axis systems (P.A.S.) of NV ensembles in a single crystal diamond without an applied static magnetic field. Circularly polarized microwaves enable arbitrary simultaneous control with spin-locking experiments and collective control using optimal control theory (OCT) in a (100) diamond. These techniques may be further improved and integrated to realize high-sensitivity NV-based quantum sensing devices using all four P.A.S. systems.<\/jats:p>","DOI":"10.1007\/s11128-023-04106-x","type":"journal-article","created":{"date-parts":[[2023,9,27]],"date-time":"2023-09-27T18:02:28Z","timestamp":1695837748000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Optimal control theory techniques for nitrogen vacancy ensembles in single crystal diamond"],"prefix":"10.1007","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5694-2318","authenticated-orcid":false,"given":"Madelaine S. 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