From megahertz to terahertz qubits encoded in molecular ions: theoretical analysis of dipole-forbidden spectroscopic transitions in N$\mathbf{_2^+}$

TL;DR

This paper theoretically explores the use of molecular nitrogen ions for quantum computing, identifying magnetically insensitive qubits, analyzing spectroscopic transitions across a wide frequency range, and proposing methods for coherent control of nuclear spins.

Contribution

It introduces new magnetically insensitive qubits in N₂⁺ and analyzes their spectroscopic properties, including previously overlooked vibrational transitions, for quantum information applications.

Findings

Identification of magnetically insensitive qubits with long coherence times.

Prediction of magnetic-dipole allowed vibrational transitions in N₂⁺.

Feasibility of coherent nuclear-spin control in molecular ions.

Abstract

Recent advances in quantum technologies have enabled the precise control of single trapped molecules on the quantum level. Exploring the scope of these new technologies, we studied theoretically the implementation of qubits and clock transitions in the spin, rotational, and vibrational degrees of freedom of molecular nitrogen ions including the effects of magnetic fields. The relevant spectroscopic transitions span six orders of magnitude in frequency illustrating the versatility of the molecular spectrum for encoding quantum information. We identified two types of magnetically insensitive qubits with very low ("stretched"-state qubits) or even zero ("magic" magnetic-field qubits) linear Zeeman shifts. The corresponding spectroscopic transitions are predicted to shift by as little as a few mHz for an amplitude of magnetic-field fluctuations on the order of a few mG translating into Zeeman-limited coherence times of tens of minutes encoded in the rotations and vibrations of the molecule. We also found that the Q(0) line of the fundamental vibrational transition is magnetic-dipole allowed by interaction with the first excited electronic state of the molecule. The Q(0) transitions, which benefit from small systematic shifts for clock operation and high sensitivity to a possible variation in the proton-to-electron mass ratio, were so far not considered in single-photon spectra. Finally, we explored possibilities to coherently control the nuclear-spin configuration of N$_2^+$ through the magnetically enhanced mixing of nuclear-spin states.