Controlling molecular spin quantum bits optically offers the potential to effectively reduce decoherence and raise the working temperature of quantum computers. Here, exchange interactions and spin dynamics, as mediated by an optically driven triplet state, are calculated for a molecule that consists of a pair of radicals and represents a potential quantum-circuit building block. Consistent with the previous experimental observation of spin coherence induced by the triplet state, our work demonstrates an optically driven quantum gate operation scheme in a molecule. A technological blueprint combining a two-dimensional molecular network and programmable nanophotonics, both of which are sufficiently developed, is proposed. We thus realize computational exploration of chemical databases to identify suitable candidates for molecular spin quantum bits and couplers to be hybridized with nanophotonic devices. The work presented here is proposed to realize a new approach for exploring molecular excited states and click chemistry, toward advancing molecular quantum technology.

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 1/2 -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.

Optically connecting quantum bits can effectively reduce decoherence and facilitate long-distance communication. Optically addressable spin-bearing molecules have been demonstrated to have a good potential for quantum computing. In this report optically induced exchange interactions and spin dynamics, which are inherently important for spin-based quantum computing, have been calculated for a bi-radical - a potential quantum computing circuit unit. Consistent with the previous experimental observation of spin coherence induced by optical excitation, our work demonstrated an optically driven quantum gate operation scheme, implying a great potential of molecular quantum-circuit network. A blueprint of quantum circuit, integrating two-dimensional molecular network and programmable nano-photonics, both of which have been under extensive investigations and rather mature, was proposed. We thus envisage computational exploration of chemical database to identify suitable candidates for molecular spin quantum bit and coupler, which could be optimally integrated with nano-photonic devices to realize quantum circuit. The work presented here would therefore open up a new direction to explore 'Click Chemistry' for quantum technology.

Recently the perovskite oxide CaCrO3 has raised concerns for its ground-state electronic structure and magnetic properties. In this report, the hybrid-exchange density functional, PBE0, is used to calculate the electronic structure and magnetic properties of CaCrO3. The ferromagnetic, A-type anti-ferromagnetic, C-type anti-ferromagnetic, and G-type anti-ferromagnetic states (defined in the text) have been investigated carefully. The computed magnetic ground state has a G-type anti-ferromagnetic configuration (the Néel state). The calculation result is that the nearest-neighboring exchange interactions in the ab-plane and along the c-axis are antiferromagnetic. The next-nearest-neighboring exchange interaction in the ab-plane is much weak but ferromagnetic. We hope this work would shed some light on the controversial ground state of CaCrO3.

Studying optical properties of organic materials is important due to the rapid development of organic light-emitting diodes, solar cells, and photon detectors. Here, for the first time, we have performed tight-binding calculations for singlet excitons, in combination with first-principles calculations of the excited states in molecular dimers, to describe the optical properties of a zinc-phthalocyanine one-dimensional molecular chain. We have included the intra-molecule and charge-transfer excitations and the coupling between them. Our calculations have successfully interpreted a body of experimental UV–visible optical spectra of transition-metal phthalocyanines. Compared with the previous ab initio calculations for a molecular dimer, the optical absorptions at the split peaks of the Q-bands can be comparable, which indicates the importance of the coupling between the intra-molecular and charge-transfer excitons.