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Massive 9 GHz Hyperfine Clock Transition in a Molecular Spin Qubit

ORAL

Abstract

Spins in molecules have been proposed as potential qubits in quantum computers, enabling chemical tunability of their quantum nature and potential for scaleup via self-assembly. We demonstrate chemical control on the degree of s-orbital mixing into the spin-bearing d-orbital associated with a series of spin-\textonehalf La(II) and Lu(II) molecules. Increased s-orbital character reduces spin-orbit coupling and enhances the electron-nuclear Fermi contact interaction. In one particular Lu(II) complex, we have observed an enormous hyperfine interaction for a molecular system, Aiso $=$ 3467 MHz (more than 1200 G), which, in turn, generates a 9 GHz clock transition. The large magnitude of this hyperfine interaction necessitated high-field W-band EPR in order to fully characterize the electron-nuclear spin Hamiltonian parameters. Meanwhile, pulsed X-band EPR studies reveal an order of magnitude increase in phase memory time, Tm, at the 9 GHz clock transition. These findings suggest new strategies for the development of molecular quantum technologies, akin to trapped ion systems.

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Authors

  • Krishnendu Kundu

    Post-doctor

  • Jessica White

    Student

  • Robert Grzywacz

    Moscow Institute of Physics and Technology, University of Virginia, California Institute of Technology, National High Magnetic Field Laboratory, University and Student Affairs; Oak Ridge Laboratory, Brookhaven National Laboratory, Physicist, Brookhaven National Laboratory, Oak Ridge National Laboratory, USA, Center for Nuclear Study, University of Tokyo, Advanced Science Research Center, Japan Atomic Energy Agency, Florida State University, Presidency University, Kolkata, INDIA, VECC,Kolkata, INDIA, SINP,Kolkata, INDIA, UGC-DAE CSR (Kolkata), INDIA, IFIN-HH, ELI-NP, Romania, Variable Energy Cyclotron Centre,Kolkata, INDIA, IEM, Kolkata, India, Victoria Institution (College), Kolkata, INDIA, Variable Energy Cyclotron Centre, Kolkata, INDIA, NHMFL; Florida State University, FAMU-FSU College of Engineering, Florida State University, Physics Department, Florida State University, Mississippi State University, NHMFL-FSU, U. Colorado at Boulder, NHMFL, University of Alabama at Birmingham, Oak Ridge National Laboratory, Argonne National Laboratory, Alabama School of Math and Science, University of South Alabama, University of Florida, University of Notre Dame, University of Texas at Dallas, Bob Jones University, University of Tennessee at Chattanooga, The Autonomous University of San Luis Potosí, Northern Arizona University, Flagstaff, AZ, Harvard-Smithsonian Center for Astrophysics, Cambridge, National Institute of Standards and Technology, Clemson University, University of South Florida, Phenikaa University, University of Ulsan, Ohio University, University of Hawaii, University of California, Davis, University of California, Davis., Saleh Research Centre, Department of Physics, Florida State university, Tallahassee, FL32306, USA, WestCHEM, School of Chemistry, University of Glasgow, Glasgow, G12 8QQ, UK, Professor, facility manager, Student, Florida State University(Former), Hebrew University, Israel \& Ioffe Institute, St.\ Petersburg, Russia, University of Tennessee, Knoxville

  • Robert Grzywacz

    Moscow Institute of Physics and Technology, University of Virginia, California Institute of Technology, National High Magnetic Field Laboratory, University and Student Affairs; Oak Ridge Laboratory, Brookhaven National Laboratory, Physicist, Brookhaven National Laboratory, Oak Ridge National Laboratory, USA, Center for Nuclear Study, University of Tokyo, Advanced Science Research Center, Japan Atomic Energy Agency, Florida State University, Presidency University, Kolkata, INDIA, VECC,Kolkata, INDIA, SINP,Kolkata, INDIA, UGC-DAE CSR (Kolkata), INDIA, IFIN-HH, ELI-NP, Romania, Variable Energy Cyclotron Centre,Kolkata, INDIA, IEM, Kolkata, India, Victoria Institution (College), Kolkata, INDIA, Variable Energy Cyclotron Centre, Kolkata, INDIA, NHMFL; Florida State University, FAMU-FSU College of Engineering, Florida State University, Physics Department, Florida State University, Mississippi State University, NHMFL-FSU, U. Colorado at Boulder, NHMFL, University of Alabama at Birmingham, Oak Ridge National Laboratory, Argonne National Laboratory, Alabama School of Math and Science, University of South Alabama, University of Florida, University of Notre Dame, University of Texas at Dallas, Bob Jones University, University of Tennessee at Chattanooga, The Autonomous University of San Luis Potosí, Northern Arizona University, Flagstaff, AZ, Harvard-Smithsonian Center for Astrophysics, Cambridge, National Institute of Standards and Technology, Clemson University, University of South Florida, Phenikaa University, University of Ulsan, Ohio University, University of Hawaii, University of California, Davis, University of California, Davis., Saleh Research Centre, Department of Physics, Florida State university, Tallahassee, FL32306, USA, WestCHEM, School of Chemistry, University of Glasgow, Glasgow, G12 8QQ, UK, Professor, facility manager, Student, Florida State University(Former), Hebrew University, Israel \& Ioffe Institute, St.\ Petersburg, Russia, University of Tennessee, Knoxville

  • Robert Grzywacz

    Moscow Institute of Physics and Technology, University of Virginia, California Institute of Technology, National High Magnetic Field Laboratory, University and Student Affairs; Oak Ridge Laboratory, Brookhaven National Laboratory, Physicist, Brookhaven National Laboratory, Oak Ridge National Laboratory, USA, Center for Nuclear Study, University of Tokyo, Advanced Science Research Center, Japan Atomic Energy Agency, Florida State University, Presidency University, Kolkata, INDIA, VECC,Kolkata, INDIA, SINP,Kolkata, INDIA, UGC-DAE CSR (Kolkata), INDIA, IFIN-HH, ELI-NP, Romania, Variable Energy Cyclotron Centre,Kolkata, INDIA, IEM, Kolkata, India, Victoria Institution (College), Kolkata, INDIA, Variable Energy Cyclotron Centre, Kolkata, INDIA, NHMFL; Florida State University, FAMU-FSU College of Engineering, Florida State University, Physics Department, Florida State University, Mississippi State University, NHMFL-FSU, U. Colorado at Boulder, NHMFL, University of Alabama at Birmingham, Oak Ridge National Laboratory, Argonne National Laboratory, Alabama School of Math and Science, University of South Alabama, University of Florida, University of Notre Dame, University of Texas at Dallas, Bob Jones University, University of Tennessee at Chattanooga, The Autonomous University of San Luis Potosí, Northern Arizona University, Flagstaff, AZ, Harvard-Smithsonian Center for Astrophysics, Cambridge, National Institute of Standards and Technology, Clemson University, University of South Florida, Phenikaa University, University of Ulsan, Ohio University, University of Hawaii, University of California, Davis, University of California, Davis., Saleh Research Centre, Department of Physics, Florida State university, Tallahassee, FL32306, USA, WestCHEM, School of Chemistry, University of Glasgow, Glasgow, G12 8QQ, UK, Professor, facility manager, Student, Florida State University(Former), Hebrew University, Israel \& Ioffe Institute, St.\ Petersburg, Russia, University of Tennessee, Knoxville

  • Robert Grzywacz

    Moscow Institute of Physics and Technology, University of Virginia, California Institute of Technology, National High Magnetic Field Laboratory, University and Student Affairs; Oak Ridge Laboratory, Brookhaven National Laboratory, Physicist, Brookhaven National Laboratory, Oak Ridge National Laboratory, USA, Center for Nuclear Study, University of Tokyo, Advanced Science Research Center, Japan Atomic Energy Agency, Florida State University, Presidency University, Kolkata, INDIA, VECC,Kolkata, INDIA, SINP,Kolkata, INDIA, UGC-DAE CSR (Kolkata), INDIA, IFIN-HH, ELI-NP, Romania, Variable Energy Cyclotron Centre,Kolkata, INDIA, IEM, Kolkata, India, Victoria Institution (College), Kolkata, INDIA, Variable Energy Cyclotron Centre, Kolkata, INDIA, NHMFL; Florida State University, FAMU-FSU College of Engineering, Florida State University, Physics Department, Florida State University, Mississippi State University, NHMFL-FSU, U. Colorado at Boulder, NHMFL, University of Alabama at Birmingham, Oak Ridge National Laboratory, Argonne National Laboratory, Alabama School of Math and Science, University of South Alabama, University of Florida, University of Notre Dame, University of Texas at Dallas, Bob Jones University, University of Tennessee at Chattanooga, The Autonomous University of San Luis Potosí, Northern Arizona University, Flagstaff, AZ, Harvard-Smithsonian Center for Astrophysics, Cambridge, National Institute of Standards and Technology, Clemson University, University of South Florida, Phenikaa University, University of Ulsan, Ohio University, University of Hawaii, University of California, Davis, University of California, Davis., Saleh Research Centre, Department of Physics, Florida State university, Tallahassee, FL32306, USA, WestCHEM, School of Chemistry, University of Glasgow, Glasgow, G12 8QQ, UK, Professor, facility manager, Student, Florida State University(Former), Hebrew University, Israel \& Ioffe Institute, St.\ Petersburg, Russia, University of Tennessee, Knoxville

  • Robert Grzywacz

    Moscow Institute of Physics and Technology, University of Virginia, California Institute of Technology, National High Magnetic Field Laboratory, University and Student Affairs; Oak Ridge Laboratory, Brookhaven National Laboratory, Physicist, Brookhaven National Laboratory, Oak Ridge National Laboratory, USA, Center for Nuclear Study, University of Tokyo, Advanced Science Research Center, Japan Atomic Energy Agency, Florida State University, Presidency University, Kolkata, INDIA, VECC,Kolkata, INDIA, SINP,Kolkata, INDIA, UGC-DAE CSR (Kolkata), INDIA, IFIN-HH, ELI-NP, Romania, Variable Energy Cyclotron Centre,Kolkata, INDIA, IEM, Kolkata, India, Victoria Institution (College), Kolkata, INDIA, Variable Energy Cyclotron Centre, Kolkata, INDIA, NHMFL; Florida State University, FAMU-FSU College of Engineering, Florida State University, Physics Department, Florida State University, Mississippi State University, NHMFL-FSU, U. Colorado at Boulder, NHMFL, University of Alabama at Birmingham, Oak Ridge National Laboratory, Argonne National Laboratory, Alabama School of Math and Science, University of South Alabama, University of Florida, University of Notre Dame, University of Texas at Dallas, Bob Jones University, University of Tennessee at Chattanooga, The Autonomous University of San Luis Potosí, Northern Arizona University, Flagstaff, AZ, Harvard-Smithsonian Center for Astrophysics, Cambridge, National Institute of Standards and Technology, Clemson University, University of South Florida, Phenikaa University, University of Ulsan, Ohio University, University of Hawaii, University of California, Davis, University of California, Davis., Saleh Research Centre, Department of Physics, Florida State university, Tallahassee, FL32306, USA, WestCHEM, School of Chemistry, University of Glasgow, Glasgow, G12 8QQ, UK, Professor, facility manager, Student, Florida State University(Former), Hebrew University, Israel \& Ioffe Institute, St.\ Petersburg, Russia, University of Tennessee, Knoxville

  • Steve Hill

    Florida State University; National High Magnetic Field Laboratory, Professor, FSU