EAGER: Quantum Dynamics of Spin in Single-Molecule Magnets

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Non-technical abstract:This proposal seeks to consolidate an integrated experimental and educational framework for the study, understanding, and dissemination of knowledge that details the quantum magnetic properties of single-molecule magnets. The control of quantum properties of nanoscale materials has led to the appearance of new emerging technologies, such as quantum information and computation processes. Nanoscale molecular systems have great potential for ultra-high density integration and quantum information processing, which are technologies that base on the fundamental properties studied in this project. Along these lines, this project will advance a conjunction of experimental realizations to study the coupling between photons and ensembles of molecular magnets, in view of application in quantum information, molecular spintronics and related emerging quantum technologies. This high risk/high reward project will open the door to explore the quantum dynamics of spin in an energy and temperature range never explored before. The proposed research is strongly integrated with a series of educational activities ongoing in the group of the principal investigator. Graduate and undergraduate students will be trained at the interface between inorganic chemistry and fundamental and applied physics, and exposed to a large, interdisciplinary and international net of collaborations that the principal investigator has established over many years.Technical abstract:This project seeks to consolidate an integrated experimental and educational framework for the study, understanding, and dissemination of knowledge that details the magnetic properties of single-molecule magnets under a broad range of experimental conditions. The main scientific goal of this project is to study the nature of light-matter interaction in single-molecule and single-ion magnets and achieve quantum coherent control over the molecular spin. The main scientific goal of this proposal is to study the nature of light-matter interaction in molecular nanomagnets and achieve quantum coherent control over the molecular spin. In particular, the objective is to coherently control the time evolution of the spin of molecules upon application of fast pulsed microwave irradiation in the weak coupling regime at sub-Kelvin temperatures (50 mK) for which dipolar dephasing will be suppressed due to polarization of the spin bath without the need of large magnetic fields. This will open a window into the fundamental sources of decoherence in single crystals of SMMs in an energy range (frequencies 10GHz, and magnetic fields 1T) never before explored. The technique has already been demonstrated by the PI under prior NSF-DMR support. This milli-Kelvin time-resolved EPR capability is unique worldwide and will allow exploring dynamical effects in SMMs and SIMs directly associated to the intrinsic anisotropy of the system, placing the PI’s group in a leading position within the field. This is a high risk-high reward project in that proof-of-concept experimental results have only been obtained in standard spectroscopic spin markers. The challenge resides in expanding these studies into single crystals of molecular nanomagnets, which will require identification of viable candidate samples and will rely on weak effects of dephasing sources other than the one that can be eliminated with the PI’s new technique (dipolar dephasing). However, if the technique works with molecular magnets, it will open an exciting door to explore the quantum dynamics of spin in an energy and temperature range never explored before (high reward), allowing exploring a realm of low magnetic fields when the systems respond to the intrinsic and complex anisotropy symmetries that make molecular nanomagnets unique.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.