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arXiv:2501.16470 · Physica Scripta

Optical nuclear electric resonance in LiNa: selective addressing of nuclear spins through pulsed lasers

Johannes K. Krondorfer, Matthias Diez, Andreas W Hauser

Published May 31, 2024• 3 citations
arXivHTMLPDF

Abstract

Abstract Optical nuclear electric resonance (ONER), a recently proposed protocol for nuclear spin manipulation in atomic systems via short laser pulses with MHz repetition rate, exploits the coupling between the nuclear quadrupole moment of a suitable atom and the periodic modulations of the electric field gradient generated by an optically stimulated electronic excitation. In this theory paper, we extend the scope of ONER from atomic to molecular systems and show that molecular vibrations do not interfere with our protocol. Exploring the diatomic molecule LiNa as a first benchmark system, our investigation showcases the robustness with respect to molecular vibration, and the ability to address and manipulate each of the two nuclear spins independently, simply by adjusting the repetition rate of a pulsed laser. Our findings suggest that it might be possible to shift complicated spin manipulation tasks required for quantum computing into the time domain by pulse-duration encoded laser signals.

DOI
10.1088/1402-4896/ad52fe

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The realization of rovibrationally stable dense samples of ultracold diatomic molecules remains one of the main stepping stones to achieve the next slate of major goals in the field of atomic and molecular physics. Though obtaining diatomic alkali molecules was seen as a logical next step following the optical cooling of atoms, many of the possible applications currently under investigation extend beyond atomic and molecular physics. For example, spectroscopy of ultracold molecules can help in testing extensions of the Standard Model via the search for a permanent electric dipole moment of the electron (1; 2), or the energy difference between enantiomers of chiral molecules (3). Various molecular transitions can be utilized to track the time dependence of fundamental constants, including the fine structure constant and the proton to electron mass ratio (4). They also open the way for cold and ultracold chemistry, where the interacting species and products are in a coherent quantum superposition state (5) and reactions can happen via quantum tunneling. Dipolar ultracold quantum gases promise to show a plethora of new phenomena due to anisotropic long-range dipole-dipole interactions (6). Dipolar molecules in optical lattices can be employed as a quantum simulator of condensed matter systems, and they are predicted to demonstrate new quantum phases such as a dipolar crystal, supersolid, checkerboard and collapse phases (7; 8). Ultracold polar molecules also represent an attractive platform for quantum computation (9). They offer a variety of long-lived states for qubit encoding, including rotational, spin and hyperfine (if electronic and nuclear spins are non-zero), Λ and Ω-doublet states (10) and scalability to a large number of qubits. Polar molecules can be easily controlled by DC electric and magnetic fields, as well as bymicrowave and optical fields, allowing the design of various traps (11; 12). The main appeal of polar molecules for quantum information processing, however, comes from their permanent electric dipole moment, permitting them to interact via a long-range dipole-dipole interaction. The dipole-dipole interaction offers a tool to construct two-qubit gates, required for universal quantum computation (9; 13). Ultracold molecules in their ground vibrational state v = 0 (and even in specific rotational, hyperfine or Zeeman states) are required formany of these applications since they have a large permanent electric dipole moment and are stable with respect to collisions and spontaneous emission. Currently translationally ultracold (100 nK 1 mK) molecules are produced by magneto(14) and photo-association (15) techniques. In a typical photoassociation scheme, 3

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Physical Review Letters•Oct 7, 2014•25 citations
Abstract Optical nuclear electric resonance (ONER), a recently proposed protocol for nuclear spin manipulation in atomic systems via short laser pulses with MHz repetition rate, exploits the coupling between the nuclear quadrupole moment of a suitable atom and the periodic modulations of the electric field gradient generated by an optically stimulated electronic excitation. In this theory paper, we extend the scope of ONER from atomic to molecular systems and show that molecular vibrations do not interfere with our protocol. Exploring the diatomic molecule LiNa as a first benchmark system, our investigation showcases the robustness with respect to molecular vibration, and the ability to address and manipulate each of the two nuclear spins independently, simply by adjusting the repetition rate of a pulsed laser. Our findings suggest that it might be possible to shift complicated spin manipulation tasks required for quantum computing into the time domain by pulse-duration encoded laser signals.
Optical nuclear electric resonance (ONER) was recently proposed as a fast and robust single-qubit gate mechanism in Sr 87 . Here, we demonstrate through numerical simulations that ONER can be extended to single-qudit control, addressing multiple one-level hyperfine transitions within the ten-dimensional nuclear-spin manifold. We identify suitable operating regimes and show that ONER enables high-fidelity spin manipulations, with simulated π-gate fidelities exceeding 99.9%, while maintaining coherence under realistic parameter fluctuations. These results establish a proof of principle for optical qudit control in Sr 87 and delineate practical parameter ranges for future experiments, highlighting ONER as a promising pathway toward high-dimensional quantum information processing.
Abstract The precise control of nuclear spin states is crucial for a wide range of quantum technology applications. Here, we propose a fast and robust single-qubit gate in 87 Sr utilizing the concept of optical nuclear electric resonance (ONER). ONER exploits the interaction between the quadrupole moment of a nucleus and the electric field gradient generated by its electronic environment, enabling spin level transitions via amplitude-modulated laser light. We investigate the hyperfine structure of the 5s 2 1 S 0 → 5s5p 3 P 1 optical transition in neutral 87 Sr and identify the magnetic field strengths and laser parameters necessary to drive spin transitions between the m I = − 9 / 2 and m I = − 5 / 2 hyperfine levels in the ground state. Our simulations show that ONER could enable faster spin operations compared to the state-of-the-art oscillations in this ‘atomic qubit’. Moreover, we show that spin-flip operations exceeding 99.9% fidelity can be performed even in the presence of typical noise sources. These results pave the way for significant advances in nuclear spin control, opening new possibilities for quantum memories and other quantum technologies.
The nuclear spin of a phosphorus atom in silicon is considered as a promising quantum information carrier for quantum computing due to its long coherence time. Coherent control of the nuclear spin is typically realized using nuclear magnetic resonance (NMR). In this work, we theoretically propose that with the aid of hyperfine interactions and magnetic field gradients, fast electric-dipole-induced nuclear electric resonance (EDNER) can be achieved. The stronger EDNER (compared with NMR) arises from the combined effects of hyperfine interaction between the nuclear and electron spins and coupling between the electron spin and charge degrees of freedom mediated by magnetic field gradients in this scheme. By operating at specific working points, the nuclear-spin splitting becomes less sensitive to electrical noise, enabling long coherence times and high-fidelity quantum operations. All elctrical, addressable control of nuclear spins paves the way for scalable silicon-based quantum computing.
The realization of rovibrationally stable dense samples of ultracold diatomic molecules remains one of the main stepping stones to achieve the next slate of major goals in the field of atomic and molecular physics. Though obtaining diatomic alkali molecules was seen as a logical next step following the optical cooling of atoms, many of the possible applications currently under investigation extend beyond atomic and molecular physics. For example, spectroscopy of ultracold molecules can help in testing extensions of the Standard Model via the search for a permanent electric dipole moment of the electron (1; 2), or the energy difference between enantiomers of chiral molecules (3). Various molecular transitions can be utilized to track the time dependence of fundamental constants, including the fine structure constant and the proton to electron mass ratio (4). They also open the way for cold and ultracold chemistry, where the interacting species and products are in a coherent quantum superposition state (5) and reactions can happen via quantum tunneling. Dipolar ultracold quantum gases promise to show a plethora of new phenomena due to anisotropic long-range dipole-dipole interactions (6). Dipolar molecules in optical lattices can be employed as a quantum simulator of condensed matter systems, and they are predicted to demonstrate new quantum phases such as a dipolar crystal, supersolid, checkerboard and collapse phases (7; 8). Ultracold polar molecules also represent an attractive platform for quantum computation (9). They offer a variety of long-lived states for qubit encoding, including rotational, spin and hyperfine (if electronic and nuclear spins are non-zero), Λ and Ω-doublet states (10) and scalability to a large number of qubits. Polar molecules can be easily controlled by DC electric and magnetic fields, as well as bymicrowave and optical fields, allowing the design of various traps (11; 12). The main appeal of polar molecules for quantum information processing, however, comes from their permanent electric dipole moment, permitting them to interact via a long-range dipole-dipole interaction. The dipole-dipole interaction offers a tool to construct two-qubit gates, required for universal quantum computation (9; 13). Ultracold molecules in their ground vibrational state v = 0 (and even in specific rotational, hyperfine or Zeeman states) are required formany of these applications since they have a large permanent electric dipole moment and are stable with respect to collisions and spontaneous emission. Currently translationally ultracold (100 nK 1 mK) molecules are produced by magneto(14) and photo-association (15) techniques. In a typical photoassociation scheme, 3
In the absence of experimental data for molecular spectra in strong magnetic fields, high resolution and reliable computational spectra are required for the interpretation of spectra collected from highly magnetic astrophysical objects. In this paper, we extend the Wilson-Hamiltonian framework, recently implemented and benchmarked by us (\textit{J. Chem. Theory Comput.}, \textbf{21}, 9753 (2025) ), to a general three-dimensional framework suitable for computing the rovibrational spectra of diatomic molecules in strong uniform magnetic fields. The field-dependent electronic and nuclear Hamiltonians capture full non-perturbative coupling between particle motion and the field making the method applicable to all field strengths. The electric quadrupole transition moment integrals for rovibrational transitions in external static magnetic fields are formulated, implemented, and computed to yield spectra which respect the selection rules of the molecule-field system. The spectral changes with increasing field strength such as shifting, splitting, merging, appearance and disappearance of peaks are noted. Contributions from electrons and nuclei are studied individually, as well as in unison to reveal the underlying physics such as stiffening of the bond, emergence of a rotational barrier, field-induced coupling/decoupling of states, and symmetry-breaking in rotational and vibrational states. These results provide the first fully quantum mechanical computational results for the rovibrational signature of 1H2^1\mathrm{H}_{2}1H2​ in extreme magnetic field environments with accuracy suitable for experimental interpretation. The methodology developed herein has direct relevance for high-field spectroscopy and astrochemical modeling, both for providing computational data as well as for understanding the spectral impact of strong magnetic fields on electronic structure and nuclear motion in molecules.
We show that the coherence properties of the nuclear spin states of rare-earth ions in solids can be manipulated by small applied electric fields. This was done by measuring the Stark effect on the nuclear quadrupole transitions of 151Eu^{151}\mathrm{Eu}151Eu in Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ (YSO) using a combination of Raman heterodyne optical detection and Stark modulated quadrupole echoes to achieve high sensitivity. The measured Stark coefficients were 0.42 and 1.0  Hz cm/V1.0\text{ }\text{ }\mathrm{Hz}\text{ }\mathrm{cm}/\mathrm{V}1.0  Hz cm/V for the two quadrupole transitions at 34.54 and 46.20 MHz, respectively. The long decoherence time of the nuclear spin states (25 ms) allowed us to make the measurements in very low electric fields of $\ensuremath{\sim}10\text{ }\text{ }\mathrm{V}/\mathrm{cm}$, which produced 100% modulation of the nuclear spin echo, and to measure Stark shifts of $\ensuremath{\sim}1\text{ }\text{ }\mathrm{Hz}$ or 20 ppm of the inhomogeneous linewidth.