Electron and nuclear spin polarization in Rb-Xe spin-exchange optical hyperpolarization

Hanni, Matti; Lantto, Perttu; Repiský, Michal; Mareš, Jiřı́ J.; Saam, B.; Vaara, Juha

doi:10.1103/physreva.95.032509

Cited by 8 publications

(11 citation statements)

References 66 publications

(113 reference statements)

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“… 20 , 26 DFT potential energy and NMR shielding calculations were performed with the Turbomole 27 code, whereas the Amsterdam Density Functional 28 program package was used for relativistic calculations of the Xe NMR shielding at the zeroth-order regular approximation level of theory including scalar (SR-ZORA) or both scalar and spin–orbit (SO) relativistic effects (SO-ZORA) 28 (see details in the ESI † ). All-electron co-r 20 , 29 /def2-SVP 30 (NR) and jpcl/TZP 31 (ZORA) basis sets were used for Xe/other atoms.…”

Section: Resultsmentioning

confidence: 99%

Inside information on xenon adsorption in porous organic cages by NMR

et al. 2017

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Section: Resultsmentioning

confidence: 99%

Inside information on xenon adsorption in porous organic cages by NMR

et al. 2017

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“…The approach relies on an iterative approach where new basis functions are added one by one, until the property has converged. Completeness‐optimization has been demonstrated so far for electric and magnetic properties, electron momentum densities, as well as NAO simulations of nanoplasmonics …”

Section: Lcao Approachesmentioning

confidence: 99%

A review on non‐relativistic, fully numerical electronic structure calculations on atoms and diatomic molecules

Lehtola

2019

Int J of Quantum Chemistry

102

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The need for accurate calculations on atoms and diatomic molecules is motivated by the opportunities and challenges of such studies. The most commonly used approach for all-electron electronic structure calculations in general-the linear combination of atomic orbitals (LCAO) method-is discussed in combination with Gaussian, Slater a.k.a. exponential, and numerical radial functions. Even though LCAO calculations have major benefits, their shortcomings motivate the need for fully numerical approaches based on, for example, finite differences, finite elements, or the discrete variable representation, which are also briefly introduced. Applications of fully numerical approaches for general molecules are briefly reviewed, and their challenges are discussed. It is pointed out that the high level of symmetry present in atoms and diatomic molecules can be exploited to fashion more efficient fully numerical approaches for these special cases, after which it is possible to routinely perform allelectron Hartree-Fock and density functional calculations directly at the basis set limit on such systems. Applications of fully numerical approaches to calculations on atoms as well as diatomic molecules are reviewed. Finally, a summary and outlook is given.atomic calculations, density functional theory, diatomic calculations, fully numerical electronic structure theory, Hartree-Fock | INTRODUCTIONThanks to decades of development in approximate density functionals and numerical algorithms, density functional theory [1,2] (DFT) is now one of the cornerstones of computational chemistry and solid-state physics. [3][4][5] Since atoms are the basic building block of molecules, a number of popular density functionals [6][7][8][9][10] have been parametrized using ab initio data on noble gas atoms; these functionals have been used in turn as the starting point for the development of other functionals. A comparison of the results of density-functional calculations to accurate ab initio data on atoms has, however, recently sparked controversy on the accuracy of a number of recently published, commonly used density functionals. [11][12][13][14][15][16][17][18][19][20][21] This underlines that there is still room for improvement in DFT even for the relatively simple case of atomic studies.The development and characterization of new density functionals require the ability to perform accurate atomic calculations. Because atoms are the simplest chemical systems, atomic calculations may seem simple; however, they are in fact sometimes surprisingly challenging. For instance, a long-standing discrepancy between the theoretical and experimental electron affinity and ionization potential of gold has been resolved only very recently with high-level ab initio calculations. [22] Atomic calculations can also be used to formulate efficient starting guesses for molecular electronic structure calculations via either the atomic density [23,24] or the atomic potential as discussed in Ref. [25].

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“…The ab initio Rb-Xe potential energy function of Ref. [12] was used. Events (labeled ) of interacting Rb-Xe pairs were extracted from evenly spaced (τ = 50 fs) MD snapshots.…”

Section: A Molecular Dynamics Simulationsmentioning

confidence: 99%

“…The hybrid exchange-correlation functional PBE0 [30] was employed. The completenessoptimized 27s25p21d1f basis [12] was used for the largecomponent wave function, for both Rb and Xe. A common gauge origin at the center of mass of the Rb-Xe complex was employed for the g tensor.…”

Section: B Spin Hamiltonianmentioning

confidence: 99%

“…Depending on the efficiency of such collisions, the very large degree of electron spin polarization (see, e.g., Ref. [12]) can be converted to nuclear polarization that greatly exceeds the level attainable by thermal polarization in standard NMR magnets [10,13]. Continuous-flow SEOP is powerful in producing large quantities of hyperpolarized noble gases [14].…”

Section: Introductionmentioning

confidence: 99%

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Polarization transfer in a spin-exchange optical-pumping experiment

2020

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Spin-exchange optical pumping (SEOP) enables hyperpolarization of magnetic noble gas nuclei and allows enormously enhanced signal in nuclear magnetic resonance studies in materials, biosciences, and medicine. We model the dynamics of the SEOP process taking place in a Rb-129 Xe gas mixture and shed light on how the different microscopic processes influence the macroscopic polarization transfer. For each Rb-Xe collision taking place in simulated molecular dynamics trajectory, we sample a time series of quantum-chemically preparametrized Hamiltonians. Combined electron and nuclear spin dynamics of each event is propagated by solving the corresponding Liouville-von Neumann equation. The rarely occurring, long-lived van der Waals molecules are seen to give the most significant contribution to polarization transfer under the simulated conditions (T = 300 K, p = 2.4 bar), in agreement with earlier findings. Besides the lifetime of the collision complex, the average and minimum Rb-Xe interatomic distances characterize the efficiency of the polarization transfer events. We obtain insight into magnetization transfer in both individual binary collisions and van der Waals complexes and demonstrate a stepwise buildup of 129 Xe spin polarization upon bond-length oscillations in the latter.

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Electron and nuclear spin polarization in Rb-Xe spin-exchange optical hyperpolarization

Cited by 8 publications

References 66 publications

Inside information on xenon adsorption in porous organic cages by NMR

Inside information on xenon adsorption in porous organic cages by NMR

A review on non‐relativistic, fully numerical electronic structure calculations on atoms and diatomic molecules

Polarization transfer in a spin-exchange optical-pumping experiment

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