Entangling remote nuclear spins linked by a chromophore

TL;DR

This paper proposes a method to entangle remote nuclear spins via their interaction with an optically excited electron spin, combining theoretical calculations and experimental validation to enable quantum information processing in molecular nanostructures.

Contribution

It introduces a novel approach for entangling nuclear spins using optical excitation and identifies molecular properties that facilitate high-fidelity quantum gates.

Findings

Density functional theory supports feasibility of entanglement.

Experimental validation on a test molecule confirms theoretical predictions.

Identified molecular features enable efficient optical control of nuclear spins.

Abstract

Molecular nanostructures may constitute the fabric of future quantum technologies, if their degrees of freedom can be fully harnessed. Ideally one might use nuclear spins as low-decoherence qubits and optical excitations for fast controllable interactions. Here, we present a method for entangling two nuclear spins through their mutual coupling to a transient optically-excited electron spin, and investigate its feasibility through density functional theory and experiments on a test molecule. From our calculations we identify the specific molecular properties that permit high entangling power gates under simple optical and microwave pulses; synthesis of such molecules is possible with established techniques.