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Nuclear singlet multimers (NUSIMERs) with long-lived singlet states.

ABSTRACT: Magnetic resonance (NMR) is a powerful tool in chemical analysis, structure determination and in medical diagnostics. Developing novel biological sensors for this field holds promise to better investigate protein structures or target diseases more efficiently. Herein, we explore nuclear spin singlet states in dendritic macromolecules as a platform molecule to develop stimuli responsive probes. We have developed a nuclear singlet multimer (NUSIMER) based on a generation 5 poly(amidoamine) dendrimer (PAMAM) which contains on average about 90 accessible nuclear spin singlet states with lifetimes up to 10-fold longer than the T ₁ relaxation times (up to 10 seconds T _s vs. T ₁ < 0.5 seconds) in a single molecule. We demonstrate little influence on the singlet lifetime in phosphate buffer (H₂O) and a high viscosity gel environment in the presence of paramagnetic oxygen. Additionally, we demonstrate an increase in singlet lifetime upon the release of a protective chemical moiety from the NUSIMER following a stimulus, whereby no change in longitudinal relaxation time is observed. The robustness and change in singlet lifetime of the NUSIMER holds promise for the development of a novel type of biosensors.

SUBMITTER: Saul P

PROVIDER: S-EPMC6334717 | biostudies-literature | 2019 Jan

REPOSITORIES: biostudies-literature

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Nuclear singlet multimers (NUSIMERs) with long-lived singlet states.

Saul Philip P Mamone Salvatore S Glöggler Stefan S

Chemical science 20181025 2

Magnetic resonance (NMR) is a powerful tool in chemical analysis, structure determination and in medical diagnostics. Developing novel biological sensors for this field holds promise to better investigate protein structures or target diseases more efficiently. Herein, we explore nuclear spin singlet states in dendritic macromolecules as a platform molecule to develop stimuli responsive probes. We have developed a nuclear singlet multimer (NUSIMER) based on a generation 5 poly(amidoamine) dendrim ...[more]

PMID: 30746089

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Project description:We report a systematic study of relaxation dynamics of hyperpolarized (HP) propane and HP propane-d6 prepared by heterogeneous pairwise parahydrogen addition to propylene and propylene-d6 respectively. Long-lived spin states (LLS) created for these molecules at the low magnetic field of 0.0475 T were employed for this study. The parahydrogen-induced overpopulation of a HP propane LLS decays exponentially with time constant (TLLS) approximately 3-fold greater than the corresponding T1 values. Both TLLS and T1 increase linearly with propane pressure in the range from 1 atm (the most biomedically relevant conditions for pulmonary MRI) to 5 atm. The TLLS value of HP propane gas at 1 atm is ~3 s. Deuteration of the substrate (propylene-d6) yields hyperpolarized propane-d6 gas with TLLS values approximately 20% shorter than those of hyperpolarized fully protonated propane gas, indicating that deuteration does not benefit the lifetime of the LLS HP state. The use of pH2 or Xe/N2 buffering gas during heterogeneous hydrogenation reaction (leading to production of 100% HP propane (no buffering gas) versus 43% HP propane gas (with 57% buffering gas) composition mixtures) results in (i) no significant changes in T1, (ii) decrease of TLLS values (by 35±7% and 8±7% respectively); and (iii) an increase of the polarization levels of HP propane gas with a propane concentration decrease (by 1.6±0.1-fold and 1.4±0.1-fold respectively despite the decrease in TLLS, which leads to disproportionately greater polarization losses during HP gas transport). Moreover, we demonstrate the feasibility of HP propane cryo-collection (which can be potentially useful for preparing larger amounts of concentrated HP propane, when buffering gas is employed), and TLLS of liquefied HP propane reaches 14.7 seconds, which is greater than the TLLS value of HP propane gas at any pressure studied. Finally, we have explored the utility of using a partial Spin-Lock Induced Crossing (SLIC) radio frequency (RF) pulse sequence for converting the overpopulated LLS into observable 1H nuclear magnetization at low magnetic field. We find that (i) the bulk of the overpopulated LLS is retained even when the optimal or near-optimal values of SLIC pulse duration are employed, and (ii) the overpopulated LLS of propane is also relatively immune to strong RF pulses-thereby, indicating that LLS is highly suitable as a spin-polarization reservoir in the context of NMR/MRI detection applications. The presented findings may be useful for improving the levels of polarization of HP propane produced by HET-PHIP via the use of an inert buffer gas; increasing the lifetime of the HP state during preparation and storage; and developing efficient approaches for ultrafast MR imaging of HP propane in the context of biomedical applications of HP propane gas, including its potential use as an inhalable contrast agent.

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Nuclear singlet multimers (NUSIMERs) with long-lived singlet states.

Publications

Nuclear singlet multimers (NUSIMERs) with long-lived singlet states.

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