Quantum spin dynamics

Abstract:

The photoexcited triplet states of porphyrins show great promise for applications in the fields of opto-electronics, photonics, molecular wires, and spintronics. The magnetic properties of porphyrin triplet states are most conveniently studied by time-resolved continuous wave and pulse electron spin resonance (ESR). This family of techniques is singularly able to probe small yet essential details of triplet states: zero-field splittings, g-anisotropy, spin polarisation, and hyperfine interactions. These characteristics are linked to spin–orbit coupling (SOC) which is known to have a strong influence on photophysical properties such as intersystem crossing rates. The present study explores SOC effects induced by the presence of Pd2+ in various porphyrin architectures. In particular, the impact of this relativistic interaction on triplet state fine-structure and spin polarisation is investigated. These properties are probed using time-resolved ESR complemented by electron-nuclear double resonance. The findings of this study could influence the future design of molecular spintronic devices. The Pd2+ ion may be incorporated into porphyrin molecular wires as a way of controlling spin polarisation.

Abstract:

Inside Front Cover
In article number 2300095, Hesjedal and co-workers demonstrate that the substitution of Co2+ ions into the halide perovskite imparts magnetic behavior to the material while maintaining photovoltaic performance. We utilize the Co2+ ions (shown as robots) themselves as probes to sense the local electronic environment of lead in the perovskite, thereby opening the substitution gateway for developing novel functional perovskite materials and devices for future technologies.

Abstract:

Scanning tunneling microscopy (STM) enables the bottom-up fabrication of tailored spin systems on a surface that are engineered with atomic precision. When combining STM with electron spin resonance (ESR), these single atomic and molecular spins can be controlled quantum-coherently and utilized as electron-spin qubits. Here we demonstrate universal quantum control of such a spin qubit on a surface by employing coherent control along two distinct directions, achieved with two consecutive radio-frequency (RF) pulses with a well-defined phase difference. We first show transformations of each Cartesian component of a Bloch vector on the quantization axis, followed by ESR-STM detection. Then we demonstrate the ability to generate an arbitrary superposition state of a single spin qubit by using two-axis control schemes, in which experimental data show excellent agreement with simulations. Finally, we present an implementation of two-axis control in dynamical decoupling. Our work extends the scope of STM-based pulsed ESR, highlighting the potential of this technique for quantum gate operations of electron-spin qubits on a surface.