We explore the quantum dynamics of nuclear spin relaxation in cold collisions of 1 Σ + molecules with structureless atoms in an external magnetic field. To this end, we develop a rigorous coupled-channel methodology, which accounts for rotational and nuclear spin degrees of freedom of 1 Σ + molecules and their interaction with an external magnetic field as well as anisotropic atom–molecule interactions. We apply the methodology to study the collisional relaxation of the nuclear spin sublevels of 13 CO molecules immersed in a cold buffer gas of 4 He atoms. We find that nuclear spin relaxation in the ground rotational manifold ( N = 0) of 13 CO occurs extremely slowly due to the absence of direct couplings between the nuclear spin sublevels. The rates of collisional transitions between the rotationally excited ( N = 1) nuclear spin states of 13 CO are generally much higher due to the direct nuclear spin–rotation coupling between the states. These transitions obey selection rules, which depend on the values of space-fixed projections of rotational and nuclear spin angular momenta ( M N and M I ) for the initial and final molecular states. For some initial states, we also observe a strong magnetic field dependence, which can be understood by using the first Born approximation. We use our calculated nuclear spin relaxation rates to investigate the thermalization of a single nuclear spin state of 13 CO( N = 0) immersed in a cold buffer gas of 4 He. The calculated nuclear spin relaxation times ( T 1 ≃ 1 s at T = 1 K at a He density of 10 –14 cm –3 ) display a steep temperature dependence decreasing rapidly at elevated temperatures due to the increased population of rotationally excited states, which undergo nuclear spin relaxation at a much faster rate. Thus, long relaxation times of N = 0 nuclear spin states in cold collisions with buffer gas atoms can be maintained only at sufficiently low temperatures ( k B T ≪ 2 B e ), where B e is the rotational constant.We explore the quantum dynamics of nuclear spin relaxation in cold collisions of 1 Σ + molecules with structureless atoms in an external magnetic field. To this end, we develop a rigorous coupled-channel methodology, which accounts for rotational and nuclear spin degrees of freedom of 1 Σ + molecules and their interaction with an external magnetic field as well as anisotropic atom–molecule interactions. We apply the methodology to study the collisional relaxation of the nuclear spin sublevels of 13 CO molecules immersed in a cold buffer gas of 4 He atoms. We find that nuclear spin relaxation in the ground rotational manifold ( N = 0) of 13 CO occurs extremely slowly due to the absence of direct couplings between the nuclear spin sublevels. The rates of collisional transitions between the rotationally excited ( N = 1) nuclear spin states of 13 CO are generally much higher due to the direct nuclear spin–rotation coupling between the states. These transitions obey selection rules, which depend on the values of space-fixed projections of rotational and nuclear spin angular momenta ( M N and M I ) for the initial and final molecular states. For some initial states, we also observe a strong magnetic field dependence, which can be understood by using the first Born approximation. We use our calculated nuclear spin relaxation rates to investigate the thermalization of a single nuclear spin state of 13 CO( N = 0) immersed in a cold buffer gas of 4 He. The calculated nuclear spin relaxation times ( T 1 ≃ 1 s at T = 1 K at a He density of 10 –14 cm –3 ) display a steep temperature dependence decreasing rapidly at elevated temperatures due to the increased population of rotationally excited states, which undergo nuclear spin relaxation at a much faster rate. Thus, long relaxation times of N = 0 nuclear spin states in cold collisions with buffer gas atoms can be maintained only at sufficiently low temperatures ( k B T ≪ 2 B e ), where B e is the rotational constant.

arXiv:2212.05363The Journal of Physical Chemistry AMay 16, 20236 citations

All-optical measurement of nuclear-spin relaxation

Robert Klieber, Andreas Michalowski, Rudolf Neuhaus +1 more

Nuclear-spin relaxation rates are usually measured by pulsed radio frequency excitation of nuclear-spin transitions. When the number of spins is too small for direct detection with conventional nuclear-magnetic-resonance spectrometers, pulsed excitation may be combined with optical detection of the nuclear spins for increased sensitivity. Here we demonstrate that such measurements can also be done purely optically, without radio frequency fields. This is achieved by preparing nonthermal populations by optical hole-burning and time-resolved probing of the populations as a function of the decay time. Measurements of the nuclear-spin relaxation of ${}^{141}\mathrm{Pr}$ in the electronic ground state of ${\mathrm{Pr}}^{3+}:{\mathrm{YAlO}}_{3}$ show that the relaxation rates for the three transitions differ by a factor of 3.Nuclear-spin relaxation rates are usually measured by pulsed radio frequency excitation of nuclear-spin transitions. When the number of spins is too small for direct detection with conventional nuclear-magnetic-resonance spectrometers, pulsed excitation may be combined with optical detection of the nuclear spins for increased sensitivity. Here we demonstrate that such measurements can also be done purely optically, without radio frequency fields. This is achieved by preparing nonthermal populations by optical hole-burning and time-resolved probing of the populations as a function of the decay time. Measurements of the nuclear-spin relaxation of ${}^{141}\mathrm{Pr}$ in the electronic ground state of ${\mathrm{Pr}}^{3+}:{\mathrm{YAlO}}_{3}$ show that the relaxation rates for the three transitions differ by a factor of 3.

Physical review. B, Condensed matterAug 26, 20035 citations

Relaxation transitions in spin systems

Lieven van Gerven

PhysicaJan 1, 19671 citation

{}^{141}\mathrm{Pr}

in the electronic ground state of

{\mathrm{Pr}}^{3+}:{\mathrm{YAlO}}_{3}

show that the relaxation rates for the three transitions differ by a factor of 3.