Collision-Induced 
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 Rovibrational Relaxation Probed by State-Resolved Nonlinear Spectroscopy

Liu, Lee R.; Changala, P. Bryan; Weichman, Marissa L.; Liang, Qizhong; Toscano, Jutta; Kłos, Jacek; Kotochigova, Svetlana; Nesbitt, David J.; Ye, Jun

doi:10.1103/prxquantum.3.030332

Cited by 7 publications

(6 citation statements)

References 40 publications

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“…We apply our methodology to study transitions between the different nuclear spin sublevels of 13 C 16 O in cold collisions with 4 He buffer atoms. This system is experimentally relevant as buffer-gas-cooled diatomic and polyatomic molecules have been probed spectroscopically in a number of recent experiments. − We perform rigorous coupled-channel quantum scattering calculations based on an accurate ab initio potential energy surface of He-CO, focusing on transitions between the nuclear spin sublevels of the ground ( N = 0) and the first excited ( N = 1) rotational states.…”

Section: Discussionmentioning

confidence: 99%

“…Nuclear spin-flipping collisions are responsible for the stability of the nuclear spin states of molecules immersed in a cold inert buffer gas (such as He or Ne). These systems can be realized experimentally using cryogenic buffer gas cooling, ,− and they are interesting for a variety of reasons. First, preparing molecules in a single nuclear spin (or hyperfine) state enhances the sensitivity of spectroscopic measurements − and is essential for the initialization steps of molecule-based quantum information processing protocols.…”

Section: Introductionmentioning

confidence: 99%

“…These systems can be realized experimentally using cryogenic buffer gas cooling, ,− and they are interesting for a variety of reasons. First, preparing molecules in a single nuclear spin (or hyperfine) state enhances the sensitivity of spectroscopic measurements − and is essential for the initialization steps of molecule-based quantum information processing protocols. One example is hyperpolarized nuclear magnetic resonance (NMR), which relies on driving populations of nuclear spin states out of thermal equilibrium as a means to enhance the sensitivity of conventional (thermal) NMR. − Because nuclear spins interact weakly with their environment, they could be an ideal platform for long-term quantum information storage. , Our ability to use buffer-gas-cooled molecules for these applications is currently hindered by the lack of knowledge of collisional nuclear spin relaxation rates.…”

Section: Introductionmentioning

confidence: 99%

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Nuclear Spin Relaxation in Cold Atom–Molecule Collisions

2023

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We explore the quantum dynamics of nuclear spin relaxation in cold collisions of 1Σ+ 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 1Σ+ 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 13CO molecules immersed in a cold buffer gas of 4He atoms. We find that nuclear spin relaxation in the ground rotational manifold (N = 0) of 13CO 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 13CO 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 13CO(N = 0) immersed in a cold buffer gas of 4He. 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 ≪ 2B e ), where B e is the rotational constant.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Nuclear Spin Relaxation in Cold Atom–Molecule Collisions

2023

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“…There remain pairs of molecular states, which have not been explored for qubit encoding, such as the hyperfine components of different electronic and rovibrational states. It would also be interesting to extend our scheme to classify qubit encodings in polyatomic molecules, , which have recently been cooled and trapped in several laboratories. − It may also be fruitful to explore the electric dipole–quadrupole interaction, which is activated only when the molecules are prepared in different types of rotational encodings (e.g., one half in a coherent superposition of the N = 0 and 1 rotational states and the other half in that of the N = 0 and 2 states). These cross-encoding interactions could prove useful for engineering interactions in ultracold two-component mixtures of polar and nonpolar molecular gases.…”

Section: Discussionmentioning

confidence: 99%

General Classification of Qubit Encodings in Ultracold Diatomic Molecules

2023

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Owing to their rich internal structure and significant long-range interactions, ultracold molecules have been widely explored as carriers of quantum information. Several different schemes for encoding qubits into molecular states, both bare and field-dressed, have been proposed. At the same time, the rich internal structure of molecules leaves many unexplored possibilities for qubit encodings. We show that all molecular qubit encodings can be classified into four classes by the type of the effective interaction between the qubits. In the case of polar molecules, the four classes are determined by the relative magnitudes of matrix elements of the dipole moment operator in the single-molecule basis. We exemplify our classification scheme by considering the encoding of the effective spin-1/2 system into nonadjacent rotational states (e.g., N = 0 and 2) of polar and nonpolar molecules with the same nuclear spin projection. Our classification scheme is designed to inform the optimal choice of molecular qubit encoding for quantum information storage and processing applications, as well as for dynamical generation of many-body entangled states and for quantum annealing.

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“…Among polyatomic molecules, buckminsterfullerene ( 12 C 60 ) is notable for its structural rigidity and high degree of symmetry, which suppress IVR and allow for spectroscopic resolution ( 13 ) and optical pumping ( 14 ) of individual rovibrational states—an unusual and fortuitous situation for a molecule with 174 vibrational modes. Its small rotational constant and stiff, cage-like structure ensure that hundreds of rotational states are populated even when vibrational excitations are largely frozen out, which can be achieved with modest buffer gas cooling to ~120 K. Thus, a thermal ensemble of 12 C 60 can reveal extensive, state-resolved rotational perturbations spanning hundreds of rotational quanta by eliminating vibrational “hot bands.”…”

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confidence: 99%

Ergodicity breaking in rapidly rotating C ₆₀ fullerenes

Liu,

Rosenberg,

Changala

et al. 2023

Science

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Ergodicity, the central tenet of statistical mechanics, requires an isolated system to explore all available phase space constrained by energy and symmetry. Mechanisms for violating ergodicity are of interest for probing nonequilibrium matter and protecting quantum coherence in complex systems. Polyatomic molecules have long served as a platform for probing ergodicity breaking in vibrational energy transport. Here, we report the observation of rotational ergodicity breaking in an unprecedentedly large molecule, 12 C 60 , determined from its icosahedral rovibrational fine structure. The ergodicity breaking occurs well below the vibrational ergodicity threshold and exhibits multiple transitions between ergodic and nonergodic regimes with increasing angular momentum. These peculiar dynamics result from the molecule’s distinctive combination of symmetry, size, and rigidity, highlighting its relevance to emergent phenomena in mesoscopic quantum systems.

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Collision-Induced C60 Rovibrational Relaxation Probed by State-Resolved Nonlinear Spectroscopy

Cited by 7 publications

References 40 publications

Nuclear Spin Relaxation in Cold Atom–Molecule Collisions

Nuclear Spin Relaxation in Cold Atom–Molecule Collisions

General Classification of Qubit Encodings in Ultracold Diatomic Molecules

Ergodicity breaking in rapidly rotating C ₆₀ fullerenes

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Collision-Induced C60 Rovibrational Relaxation Probed by State-Resolved Nonlinear Spectroscopy

Cited by 7 publications

References 40 publications

Nuclear Spin Relaxation in Cold Atom–Molecule Collisions

Nuclear Spin Relaxation in Cold Atom–Molecule Collisions

General Classification of Qubit Encodings in Ultracold Diatomic Molecules

Ergodicity breaking in rapidly rotating C 60 fullerenes

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Ergodicity breaking in rapidly rotating C ₆₀ fullerenes