Coherent Manipulation and Decoherence of S=10 Single-Molecule Magnets

TL;DR

This study demonstrates coherent control of S=10 Fe8 single-molecule magnets, showing that spin decoherence is mainly caused by spin bath fluctuations and can be reduced by bath polarization and isotopic substitution.

Contribution

It provides the first detailed analysis of spin decoherence mechanisms in S=10 single-molecule magnets and shows how to extend coherence times using bath polarization.

Findings

Spin decoherence time T2 reaches 712 ns with bath polarization.

Decoherence mainly caused by Fe8 spin bath fluctuations.

Nuclear spin bath fluctuations also contribute to decoherence.

Abstract

We report coherent manipulation of S=10 Fe$_{8}$ single-molecule magnets. The temperature dependence of the spin decoherence time $T_2$ measured by high frequency pulsed electron paramagnetic resonance indicates that strong spin decoherence is dominated by Fe$_{8}$ spin bath fluctuations. By polarizing the spin bath in Fe$_{8}$ single-molecule magnets at magnetic field $B$ = 4.6 T and temperature $T$ = 1.3 K, spin decoherence is significantly suppressed and extends the spin decoherence time $T_2$ to as long as 712 ns. A second decoherence source is likely due to fluctuations of the nuclear spin bath. This hints that the spin decoherence time can be further extended via isotopic substitution to smaller magnetic moments.