arXiv subjects

Aaron Himmler

Publications and source records attributed to Aaron Himmler.

4 recordsLinked to original sources

arXiv2024

Temperature-dependent dynamic nuclear polarization of diamond

Dynamic nuclear polarization (DNP) can increase nuclear magnetic resonance (NMR) signals by orders of magnitude. DNP in diamond proceeds through different DNP mechanisms with a possible temperature-dependence. We report on 13C dynamic nuclear polarization (DNP) experiments in diamonds at 3.4 T and 7 T between 300 K and 1.7 K. Nuclear polarization enhancements between 100 and 600 were measured for all temperatures, corresponding to polarizations at 7 T between 0.1% (300 K) and 38% (1.7 K). A strong temperature dependence of the DNP profiles was observed. Longitudinal-detected (LOD) electron paramagnetic resonance (EPR) experiments revealed an additional broad temperature-dependent electron line centered around the mI = 0 line of the P1 triplet transitions. Our results suggest that nuclei are preferentially polarized via a direct hyperfine mediated polarization transfer while spin diffusion in the sample plays a minor role.

cond-mat.mtrl-sci↗

arXiv2024

The role of nuclear spin diffusion in dynamic nuclear polarization of crystalline nanoscale silicon particles

Hyperpolarized nanoparticles (NPs) offer high polarization levels with room temperature relaxation times exceeding half an hour. In this work, we demonstrate that the achievable hyperpolarization enhancement and relaxation (decay) time at room temperature are largely independent of the particle size contrary to previous assumptions. This is explained through first-principles spin-diffusion coefficient calculations and finite-element polarization simulations. The simulated zero-quantum (flip-flop) line width governing the spin diffusion is found to agree with the experimentally accessible single-quantum (single spin flip, e.g. radio-frequency pulse) line width. The transport of hyperpolarization from strongly hyperfine-coupled spins towards the bulk is most likelybelieved to be responsible for the slow polarization dynamics including long room temperature decay time. The line width and spin-diffusion simulations are extended to other cubic crystal structures and analytical expressions, which only require insertion of the gyromagnetic ratio, lattice constant, isotope abundance and measured spectral density distribution (nuclear line width), are fitted. The presented simulations can be adjusted to study spin diffusion in other materials.

quant-ph↗

arXiv2024

Controlled synthesis and characterization of porous silicon nanoparticles for dynamic nuclear polarization

Si nanoparticles (NPs) have been actively developed as a hyperpolarized magnetic resonance imaging (MRI) contrast agent with an imaging window close to one hour. However, the progress in the development of NPs has been hampered by the incomplete understanding of their structural properties that correspond to efficient hyperpolarization buildup and long polarization decays. In this work we study dynamic nuclear polarization (DNP) of single crystal porous Si (PSi) NPs with defined doping densities ranging from nominally undoped to highly doped with boron or phosphorus. To develop such PSi NPs we perform low-load metal-assisted catalytic etching for electronic grade Si powder followed by thermal oxidation to form the dangling bonds in the Si/SiO$_2$ interface, the $P_b$ centers. $P_b$ centers are the endogenous source of the unpaired electron spins necessary for DNP. The controlled fabrication and oxidation procedures allow us to thoroughly investigate the impact of the magnetic field, temperature and doping on the DNP process. We argue that the buildup and decay rate constants are independent of size of Si crystals between approximately 10 and 60 nm. Instead, the rates are limited by the polarization transfer across the nuclear spin diffusion barrier determined by the large hyperfine shift of the central $^{29}$Si nuclei of the $P_b$ centers. The size-independent rates are then weakly affected by the doping degree for low and moderately doped Si although slight doping is required to achieve the highest polarization. Thus, we find the room temperature relaxation of low boron doped PSi NPs reaching $75 \pm 3$ minutes and nuclear polarization levels exceeding $\sim 6$ % when polarized at 6.7 T and 1.4 K. Our study thus establishes solid grounds for further development of Si NPs as hyperpolarized contrast agents.

cond-mat.mtrl-sci↗

arXiv2023

Relaxation enhancement by microwave irradiation may limit dynamic nuclear polarization

Dynamic nuclear polarization enables the hyperpolarization of nuclear spins beyond the thermal-equilibrium Boltzmann distribution. However, it is often unclear why the experimentally measured hyperpolarization is below the theoretical achievable maximum polarization. We report a (near-) resonant relaxation enhancement by microwave (MW) irradiation, leading to a significant increase in the nuclear polarization decay compared to measurements without MW irradiation. For example, the increased nuclear relaxation limits the achievable polarization levels to around 35% instead of hypothetical 60%, measured in the DNP material TEMPO in 1H glassy matrices at 3.3 K and 7 T. Applying rate-equation models to published build-up and decay data indicates that such relaxation enhancement is a common issue in many samples when using different radicals at low sample temperatures and high Boltzmann polarizations of the electrons. Accordingly, quantification and a better understanding of the relaxation processes under MW irradiation might help to design samples and processes towards achieving higher nuclear hyperpolarization levels.better understanding of the relaxation processes under MW irradiation might help to design samples and processes towards achieving higher nuclear hyperpolarization levels.

physics.chem-ph↗