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Metal phthalocyanines, a highly versatile class of aromatic, planar, macrocyclic molecules with a chelated central metal ion, are topical objects of ongoing research and particularly interesting due to their magnetic properties. However, while current focus lies almost exclusively on spin-Zeeman-related effects, the high symmetry of the molecule and its circular shape suggests the exploitation of light-induced excitation of twofold degenerate vibrational states in order to generate, switch and manipulate magnetic fields at the nanoscale. The underlying mechanism is a molecular pseudorotation that can be triggered by infrared pulses and gives rise to a quantized, small but controllable magnetic dipole moment. We investigate the optical stimulation of vibrationally-induced molecular magnetism and estimate changes in the magnetic shielding constants for confirmation by future experiments., Comment: This is the final published version of the article, available Open Access under a CC-BY license. The supplementary information is The article was published in the Journal of the American Chemical Society on May 2024. DOI: https://doi.org/10.1021/jacs.4c01915 . The supplementary information is included at the end of the article

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., Comment: This is the final published version of the article, available Open Access under a CC-BY license. The article was published in *Physica Scripta* by IOP Publishing in June 2024. DOI: https://dx.doi.org/10.1088/1402-4896/ad52fe

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$^2$ $^1S_{0}\rightarrow{}$ 5s5p $^3P_1$ 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 the threshold for fault-tolerant quantum computing can be surpassed 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.

Particle production through ultra-strong electric fields is a well-studied research field. Nevertheless, despite repeated attempts to relate the production rate within the field to the formation time of a particle, the latter is still shrouded in mystery. We provide an interpretation of a particle distribution at finite times enabling us to isolate and, therefore, identify the relevant time scales regarding particle formation in quantum physics within and beyond perturbation theory., Comment: 6 pages, 3 figures

Spin defects in solid-state materials are strong candidate systems for quantum information technology and sensing applications. Here we explore in details the recently discovered negatively charged boron vacancies ($V_B^-$) in hexagonal boron nitride (hBN) and demonstrate their use as atomic scale sensors for temperature, magnetic fields and externally applied pressure. These applications are possible due to the high-spin triplet ground state and bright spin-dependent photoluminescence (PL) of the $V_B^-$. Specifically, we find that the frequency shift in optically detected magnetic resonance (ODMR) measurements is not only sensitive to static magnetic fields, but also to temperature and pressure changes which we relate to crystal lattice parameters. Our work is important for the future use of spin-rich hBN layers as intrinsic sensors in heterostructures of functionalized 2D materials., Comment: 9 pages, 4 figures, 2 tables

Optically active defects in solids with accessible spin states are promising candidates for solid state quantum information and sensing applications. To employ these defects as quantum building blocks, coherent manipulation of their spin state is required. Here we realize coherent control of ensembles of boron vacancy (V$_B^-$) centers in hexagonal boron nitride (hBN). Specifically, by applying pulsed spin resonance protocols, we measure spin-lattice relaxation time ($T_1$) of 18 $\mu$s and spin coherence time ($T_2$) of 2 $\mu$s at room temperature. The spin-lattice relaxation time increases by three orders of magnitude at cryogenic temperature. Furthermore, employing a two- and three-pulse electron spin-echo envelope modulation (ESEEM) we separate the quadrupole and hyperfine interactions with the surrounding nuclei. Finally, by applying a method to decouple the spin state from its inhomogeneous nuclear environment - a "hole-burning" - the spectral optically detected magnetic resonance linewidth is significantly reduced to several tens of kHz, thus extending the spin coherence time by a factor of three. Our results are important for employment of van der Waals materials for quantum technologies, specifically in the context of using hBN as a high-resolution quantum sensor for hybrid quantum systems including 2D heterostructures, nanoscale devices and emerging atomically thin magnets.