Self‐Cooling Molecular Spin Qudits

The need of operating molecular spin qubits at very low temperatures constitutes a technological limitation. This challenge is addressed by integrating, in the same material and at the molecular scale, quantum processing and magnetic refrigeration capabilities. The molecular unit is a [GdEr] heterolanthanide coordination complex, where Er(III) encodes a qubit while Gd(III) provides a large magnetocaloric effect. The properties of each component are separately studied in isostructural [LaEr] and [GdLu] complexes, where each functional ion lies next to a diamagnetic metal. All complexes are characterized by magnetic, heat capacity, and EPR measurements. The results show that the presence of both ions in the same molecule has a synergic effect on both functionalities. Thus, the coupling between Er(III) and Gd(III) spins lifts any level degeneracies even close to zero magnetic field, leading to a d = 16 set of spin states that, as revealed by pulse EPR measurements, can be coherently manipulated. In turn, Er(III) enhances the magnetocaloric effect compared to [GdLu], extending it to lower temperatures. This is corroborated by direct magnetocaloric measurements, which show the ability of this material to cool itself, and a device, down to temperatures as low as 0.4 K.