Materials chemistry of triplet dynamic nuclear polarization

Nishimura, Koki; Kouno, Hironori; Kawashima, Yusuke; Orihashi, Kana; Fujiwara, Saiya; Tateishi, Kenichiro; Uesaka, T.; Kimizuka, Nobuo; Yanai, Nobuhiro

doi:10.1039/d0cc02258f

Cited by 41 publications

(38 citation statements)

References 119 publications

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“…Since the populations of each sublevel follow a Boltzmann distribution in thermal equilibrium, the electron spin polarization is very small under ambient conditions. Therefore, cryogenic conditions are required to obtain a large electron polarization in a thermal equilibrium state. − As one of the solutions to this problem, the nonequilibrium and temperature-independent spin polarization of triplet electrons is widely used for applications such as quantum computing, , room-temperature masers, − and triplet dynamic nuclear polarization (triplet-DNP). − The large polarization of a triplet state can be generated even at room temperature by sublevel-selective intersystem crossing from the photoexcited singlet state.…”

Section: Introductionmentioning

confidence: 99%

Design Guidelines to Elongate Spin–Lattice Relaxation Times of Porphyrins with Large Triplet Electron Polarization

et al. 2021

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The spin-polarized triplet state generated by light irradiation has potential for applications such as triplet dynamic nuclear polarization (triplet-DNP). Recently, we have reported free-base porphyrins as versatile and biocompatible polarizing agents for triplet-DNP. However, the electron polarization of free-base porphyrins is not very high, and the dilemma is that the high polarization of metalloporphyrins is accompanied by a too short spin–lattice relaxation time to be used for triplet-DNP. We report here that the introduction of electron-withdrawing fluorine groups into Zn porphyrins enables a long enough spin–lattice relaxation time (>1 μs) while maintaining a high polarization (P x:P y:P z = 0:0:1.0) at room temperature. Interestingly, the spin–lattice relaxation time of Zn porphyrin becomes much longer by introducing fluorine substituents, whereas the spin–lattice relaxation time of free-base porphyrin becomes shorter by the fluorine substitution. Theoretical calculations suggest that this is because the introduction of the electron-withdrawing fluorine substituents reduces the spin density on Zn atoms and weakens the spin–orbit interaction.

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Section: Introductionmentioning

confidence: 99%

Design Guidelines to Elongate Spin–Lattice Relaxation Times of Porphyrins with Large Triplet Electron Polarization

et al. 2021

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“…However, the poor sensitivity remains the Achilles heel to all magnetic resonance experiments. Dynamic nuclear polarization (DNP), a technique to transfer spin polarization from electrons to nuclei, has been extensively studied since its early discovery (Overhauser, 1953) and has seen an impressive revival in the current century (Ardenkjaer-Larsen et al, 2003;Maly et al, 2008;Lesage et al, 2010;Nelson et al, 2013). In DNP using unpaired electrons as the sources of polarization, the polarization enhancement factor is limited to γ e /γ n , where γ e(n) are the gyromagnetic ratios of the electron (nuclear) spins.…”

Section: Introductionmentioning

confidence: 99%

Room-temperature hyperpolarization of polycrystalline samples with optically polarized triplet electrons: pentacene or nitrogen-vacancy center in diamond?

et al. 2021

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Abstract. We demonstrate room-temperature 13C hyperpolarization by dynamic nuclear polarization (DNP) using optically polarized triplet electron spins in two polycrystalline systems: pentacene-doped [carboxyl-13C] benzoic acid and microdiamonds containing nitrogen-vacancy (NV−) centers. For both samples, the integrated solid effect (ISE) is used to polarize the 13C spin system in magnetic fields of 350–400 mT. In the benzoic acid sample, the 13C spin polarization is enhanced by up to 0.12 % through direct electron-to-13C polarization transfer without performing dynamic 1H polarization followed by 1H−13C cross-polarization. In addition, the ISE has been successfully applied to polarize naturally abundant 13C spins in a microdiamond sample to 0.01 %. To characterize the buildup of the 13C polarization, we discuss the efficiencies of direct polarization transfer between the electron and 13C spins as well as that of 13C−13C spin diffusion, examining various parameters which are beneficial or detrimental for successful bulk dynamic 13C polarization.

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“…Since optical fields can routinely be detected at the shot-noise limit, the sensitivity of magnetic resonance spectroscopy and the fidelity of spin state readout can be significantly increased while spin initialization and readout can be achieved with a much higher spatial resolution set by the optical wavelength. Finally, these advantages can be translated to nuclear spin spectroscopy through the use of hyperfine coupling 18 . Together, these features are placing ODMR at the core of many emerging spin-based quantum technologies.…”

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confidence: 99%

Optically detected magnetic resonance with an open source platform

Babashah¹,

Shirzad²,

Losero³

et al. 2022

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Localized electronic spins in solid-state environments form versatile and robust platforms for quantum sensing, metrology and quantum information processing. With optically detected magnetic resonance (ODMR), it is possible to prepare and readout highly coherent spin systems, up to room temperature, with orders of magnitude enhanced sensitivities and spatial resolutions compared to induction-based techniques, allowing single spin manipulations. While ODMR was first observed in organic molecules, many other systems are nowadays intensively being searched for, discovered and studied. Among them is the nitrogen-vacany (NV) center in diamond. Beyond ODMR it is notably already widely and successfully used both as a high-resolution high-sensitivity quantum sensors for external fields and as a qubit. Others are rare earth ions used as quantum memories and many other color centers trapped in bulk or 2-dimensional materials. In order to allow the broadest possible community of researchers and engineers to investigate and develop novel ODMR-based materials and applications, we overview here the setting up of ODMR experiments using commercially available hardware. We also present in detail a dedicated collaborative open-source interface named Qudi and describe the original features we have added to speed-up data acquisition, relax instrumental requirements and widen its applicability to individual and ensemble ODMR systems. Associating hardware and software discussions, this article aims to steepen the learning curve of newcomers in ODMR from a variety of scientific backgrounds, to optimize the experimental development time, preempt the common measurement pitfalls, and to provide an efficient, portable and collaborative interface to explore innovative experiments.

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Materials chemistry of triplet dynamic nuclear polarization

Abstract:
This Feature Article overviews the recently-emerged materials chemistry of triplet dynamic nuclear polarization (triplet-DNP) towards biological and medical applications.

Cited by 41 publications

References 119 publications

Design Guidelines to Elongate Spin–Lattice Relaxation Times of Porphyrins with Large Triplet Electron Polarization

Design Guidelines to Elongate Spin–Lattice Relaxation Times of Porphyrins with Large Triplet Electron Polarization

Room-temperature hyperpolarization of polycrystalline samples with optically polarized triplet electrons: pentacene or nitrogen-vacancy center in diamond?

Optically detected magnetic resonance with an open source platform

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Materials chemistry of triplet dynamic nuclear polarization

Abstract: This Feature Article overviews the recently-emerged materials chemistry of triplet dynamic nuclear polarization (triplet-DNP) towards biological and medical applications.

Cited by 41 publications

References 119 publications

Design Guidelines to Elongate Spin–Lattice Relaxation Times of Porphyrins with Large Triplet Electron Polarization

Design Guidelines to Elongate Spin–Lattice Relaxation Times of Porphyrins with Large Triplet Electron Polarization

Room-temperature hyperpolarization of polycrystalline samples with optically polarized triplet electrons: pentacene or nitrogen-vacancy center in diamond?

Optically detected magnetic resonance with an open source platform

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Resources

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Abstract:
This Feature Article overviews the recently-emerged materials chemistry of triplet dynamic nuclear polarization (triplet-DNP) towards biological and medical applications.