Identification of an X-Band Clock Transition in Cp' 3 Pr - Enabled by a 4f 2 5d 1 Configuration

• Published in: Journal of the American Chemical Society Vol. 146; no. 9; pp. 5781 - 5785
• Main Authors: Smith, Patrick W, Hrubý, Jakub, Evans, William J, Hill, Stephen, Minasian, Stefan G
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 06.03.2024
• ISSN: 0002-7863; 1520-5126
• DOI: 10.1021/jacs.3c12725

Molecular qubits offer an attractive basis for quantum information processing, but challenges remain with regard to sustained coherence. Qubits based on clock transitions offer a method to improve the coherence times. We propose a general strategy for identifying molecules with high-frequency clock transitions in systems where a d electron is coupled to a crystal-field singlet state of an f configuration, resulting in an = ±1/2 ground state with strong hyperfine coupling. Using this approach, a 9.834 GHz clock transition was identified in a molecular Pr complex, [K(crypt)][Cp' Pr ], leading to 3-fold enhancements in relative to other transitions in the spectrum. This result indicates the promise of the design principles outlined here for the further development of f-element systems for quantum information applications.