Triplet-radical spin entanglement: potential of molecular materials for high-temperature quantum information processing

TL;DR: In this article , a theoretical model based on the theory of open quantum systems for spin dynamics in a molecule containing one radical, which can interact with the triplet state arising from another part of the molecule owing to optical excitation and intersystem crossing was proposed.

Abstract: Abstract Recently, spin-bearing molecules have been experimentally demonstrated to have great potential as building blocks for quantum information processing due to their substantial advantages including tunability, portability, and scalability. Here, we propose a theoretical model based on the theory of open quantum systems for spin dynamics in a molecule containing one radical, which can interact with the triplet state arising from another part of the molecule owing to optical excitation and intersystem crossing. With the initial state being a classical mixture of a radical $$\frac{1}{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mfrac> <mml:mrow> <mml:mn>1</mml:mn> </mml:mrow> <mml:mrow> <mml:mn>2</mml:mn> </mml:mrow> </mml:mfrac> </mml:math> -spin, the exchange interaction between the radical and the triplet produces a spin coherent state, which could potentially be used for a qubit-qutrit quantum entangling gate. Our calculations for the time-resolved electron paramagnetic resonance spectra showed good qualitative agreement with the related experimental results for radical-bearing molecules at high temperature (~77 K, the boiling point of liquid nitrogen). This work therefore lays a solid theoretical cornerstone for optically driven quantum gate operations in radical-bearing molecular materials, aiming toward high-temperature quantum information processing.