Hans-Martin Vieth | Searcharxiv

arXiv2021

Hyperpolarization of cis-15N,15N'-azobenzene by parahydrogen at ultralow magnetic fields

Development of the methods to exploit nuclear hyperpolarization and search for molecules whose nuclear spins can be efficiently hyperpolarized is an active area in nuclear magnetic resonance. Of particular interest are those molecules that have long nuclear relaxation times, making them to be suitable candidates as contrast agents in magnetic resonance imaging. In this work, we present a detailed study of SABRE SHEATH (Signal Amplification By Reversible Exchange in Shield Enabled Alignment Transfer to Heteronuclei) experiments of 15N,15N' azobenzene. In SABRE SHEATH experiments nuclear spins of the target are hyperpolarized by transfer of spin polarization from parahydrogen at ultralow fields during a reversible chemical process. The studied system is complicated, and we are concerned only about a subset of the data, presenting details for the molecules that experience fast chemical exchange at the catalytic complex and thus are involved in polarizing the free azobenzene. Azobenzene exists in two isomers trans- and cis-. We show that all nuclear spins in cis-azobenzene can be efficiently hyperpolarized by SABRE at suitable magnetic fields. Enhancement factors (relative to 9.4 T) reach several thousands of times for 15N spins and a few tens of times for the 1H spins. There are two approaches to observe either hyperpolarized magnetization of 15N/1H spins or hyperpolarized singlet order of the 15N spin pair. We compare these approaches and present the field dependencies of SABRE experiments for them. No hyperpolarization of trans 15N,15N' azobenzene was observed. The results presented here will be useful for further experiments where hyperpolarized cis-15N,15N' azobenzene is switched by light to trans 15N,15N' azobenzene for storing the produced hyperpolarization in the long-lived spin state of the 15N pair of trans-15N,15N' azobenzene.

physics.chem-ph↗

arXiv2016

Robust conversion of singlet spin order in coupled spin-1/2 pairs by adiabatically switched RF-fields

We propose a robust and highly efficient NMR technique to create singlet spin order from longitudinal spin magnetization in coupled spin-1/2 pairs and to perform backward conversion (singlet order)$\to$magnetization. In this method we exploit adiabatic switching of an RF-field in order to drive transitions between the singlet state and the $T_\pm$ triplet states of a spin pair under study. We demonstrate that the method works perfectly for both strongly and weakly coupled spin pairs, providing a conversion efficiency between the singlet spin order and magnetization, which is equal to the theoretical maximum. We anticipate that the proposed technique is useful for generating long-lived singlet order, for preserving spin hyperpolarization and for assessing singlet spin order in nearly equivalent spin pairs in specially designed molecules and in low-field NMR studies.

physics.chem-ph↗

arXiv2001

Non-thermal nuclear magnetic resonance quantum computing using hyperpolarized Xenon

Current experiments in liquid-state nuclear magnetic resonance quantum computing are limited by low initial polarization. To address this problem, we have investigated the use of optical pumping techniques to enhance the polarization of a 2-qubit NMR quantum computer (13C and 1H in 13CHCl3). To efficiently use the increased polarization, we have generalized the procedure for effective pure state preparation. With this new, more flexible scheme, an effective pure state was prepared with polarization-enhancement of a factor of 10 compared to the thermal state. An implementation of Grover's quantum search algorithm was demonstrated using this new technique.

quant-ph↗