Many-body kinetics of dynamic nuclear polarization by the cross effect

Dynamic nuclear polarization (DNP) is an out-of-equilibrium method for generating nonthermal spin polarization which provides large signal enhancements in modern diagnostic methods based on nuclear magnetic resonance. A particular instance is cross-effect DNP, which involves the interaction of two c...

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Main Authors: Karabanov, Alexander, Wiśniewski, Daniel, Raimondi, F., Lesanovsky, Igor, Köckenberger, Walter
Format: Article
Language:English
Published: American Physical Society 2018
Online Access:https://eprints.nottingham.ac.uk/51498/
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author Karabanov, Alexander
Wiśniewski, Daniel
Raimondi, F.
Lesanovsky, Igor
Köckenberger, Walter
author_facet Karabanov, Alexander
Wiśniewski, Daniel
Raimondi, F.
Lesanovsky, Igor
Köckenberger, Walter
author_sort Karabanov, Alexander
building Nottingham Research Data Repository
collection Online Access
description Dynamic nuclear polarization (DNP) is an out-of-equilibrium method for generating nonthermal spin polarization which provides large signal enhancements in modern diagnostic methods based on nuclear magnetic resonance. A particular instance is cross-effect DNP, which involves the interaction of two coupled electrons with the nuclear spin ensemble. Here we develop a theory for this important DNP mechanism and show that the nonequilibrium nuclear polarization buildup is effectively driven by three-body incoherent Markovian dissipative processes involving simultaneous state changes of two electrons and one nucleus. We identify different parameter regimes for effective polarization transfer and discuss under which conditions the polarization dynamics can be simulated by classical kinetic Monte Carlo methods. Our theoretical approach allows simulations of the polarization dynamics on an individual spin level for ensembles consisting of hundreds of nuclear spins. The insight obtained by these simulations can be used to find optimal experimental conditions for cross-effect DNP and to design tailored radical systems that provide optimal DNP efficiency.
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spelling nottingham-514982018-05-05T00:15:58Z https://eprints.nottingham.ac.uk/51498/ Many-body kinetics of dynamic nuclear polarization by the cross effect Karabanov, Alexander Wiśniewski, Daniel Raimondi, F. Lesanovsky, Igor Köckenberger, Walter Dynamic nuclear polarization (DNP) is an out-of-equilibrium method for generating nonthermal spin polarization which provides large signal enhancements in modern diagnostic methods based on nuclear magnetic resonance. A particular instance is cross-effect DNP, which involves the interaction of two coupled electrons with the nuclear spin ensemble. Here we develop a theory for this important DNP mechanism and show that the nonequilibrium nuclear polarization buildup is effectively driven by three-body incoherent Markovian dissipative processes involving simultaneous state changes of two electrons and one nucleus. We identify different parameter regimes for effective polarization transfer and discuss under which conditions the polarization dynamics can be simulated by classical kinetic Monte Carlo methods. Our theoretical approach allows simulations of the polarization dynamics on an individual spin level for ensembles consisting of hundreds of nuclear spins. The insight obtained by these simulations can be used to find optimal experimental conditions for cross-effect DNP and to design tailored radical systems that provide optimal DNP efficiency. American Physical Society 2018-03-26 Article PeerReviewed application/pdf en https://eprints.nottingham.ac.uk/51498/1/Karabanov_et_al_PhysRevA2018.pdf Karabanov, Alexander, Wiśniewski, Daniel, Raimondi, F., Lesanovsky, Igor and Köckenberger, Walter (2018) Many-body kinetics of dynamic nuclear polarization by the cross effect. Physical Review A, 97 (3). 031404-1. ISSN 2469-9934 https://journals.aps.org/pra/abstract/10.1103/PhysRevA.97.031404 doi:10.1103/PhysRevA.97.031404 doi:10.1103/PhysRevA.97.031404
spellingShingle Karabanov, Alexander
Wiśniewski, Daniel
Raimondi, F.
Lesanovsky, Igor
Köckenberger, Walter
Many-body kinetics of dynamic nuclear polarization by the cross effect
title Many-body kinetics of dynamic nuclear polarization by the cross effect
title_full Many-body kinetics of dynamic nuclear polarization by the cross effect
title_fullStr Many-body kinetics of dynamic nuclear polarization by the cross effect
title_full_unstemmed Many-body kinetics of dynamic nuclear polarization by the cross effect
title_short Many-body kinetics of dynamic nuclear polarization by the cross effect
title_sort many-body kinetics of dynamic nuclear polarization by the cross effect
url https://eprints.nottingham.ac.uk/51498/
https://eprints.nottingham.ac.uk/51498/
https://eprints.nottingham.ac.uk/51498/