Tunable Cr Molecular Color Centers.

The inherent atomistic precision of synthetic chemistry enables bottom-up structural control over quantum bits, or qubits, for quantum technologies. Tuning paramagnetic molecular qubits that feature optical-spin initialization and readout is a crucial step toward designing bespoke qubits for applications in quantum sensing, networking, and computing. Here, we demonstrate that the electronic structure that enables optical-spin initialization and readout for = 1, Cr(aryl), where aryl = 2,4-dimethylphenyl (), -tolyl (), and 2,3-dimethylphenyl (), is readily translated into Cr(alkyl) compounds, where alkyl = 2,2,2-triphenylethyl (), (trimethylsilyl)methyl (), and cyclohexyl ().

Trigonal Bipyramidal V Complex as an Optically Addressable Molecular Qubit Candidate.

Synthetic chemistry enables a bottom-up approach to quantum information science, where atoms can be deterministically positioned in a quantum bit or qubit. Two key requirements to realize quantum technologies are qubit initialization and read-out. By imbuing molecular spins with optical initialization and readout mechanisms, analogous to solid-state defects, molecules could be integrated into existing quantum infrastructure.

Optically addressable molecular spins for quantum information processing.

Spin-bearing molecules are promising building blocks for quantum technologies as they can be chemically tuned, assembled into scalable arrays, and readily incorporated into diverse device architectures. In molecular systems, optically addressing ground-state spins would enable a wide range of applications in quantum information science, as has been demonstrated for solid-state defects. However, this important functionality has remained elusive for molecules.

Electrical and optical control of single spins integrated in scalable semiconductor devices.

Spin defects in silicon carbide have the advantage of exceptional electron spin coherence combined with a near-infrared spin-photon interface, all in a material amenable to modern semiconductor fabrication. Leveraging these advantages, we integrated highly coherent single neutral divacancy spins in commercially available p-i-n structures and fabricated diodes to modulate the local electrical environment of the defects. These devices enable deterministic charge-state control and broad Stark-shift tuning exceeding 850 gigahertz.

Local optical control of ferromagnetism and chemical potential in a topological insulator.

Many proposed experiments involving topological insulators (TIs) require spatial control over time-reversal symmetry and chemical potential. We demonstrate reconfigurable micron-scale optical control of both magnetization (which breaks time-reversal symmetry) and chemical potential in ferromagnetic thin films of Cr-(Bi,Sb)Te grown on SrTiO By optically modulating the coercivity of the films, we write and erase arbitrary patterns in their remanent magnetization, which we then image with Kerr microscopy. Additionally, by optically manipulating a space charge layer in the underlying SrTiO substrates, we control the local chemical potential of the films.

Persistent optical gating of a topological insulator.

The spin-polarized surface states of topological insulators (TIs) are attractive for applications in spintronics and quantum computing. A central challenge with these materials is to reliably tune the chemical potential of their electrons with respect to the Dirac point and the bulk bands. We demonstrate persistent, bidirectional optical control of the chemical potential of (Bi,Sb)2Te3 thin films grown on SrTiO3.

Spin-transfer torque generated by a topological insulator.

Magnetic devices are a leading contender for the implementation of memory and logic technologies that are non-volatile, that can scale to high density and high speed, and that do not wear out. However, widespread application of magnetic memory and logic devices will require the development of efficient mechanisms for reorienting their magnetization using the least possible current and power. There has been considerable recent progress in this effort; in particular, it has been discovered that spin-orbit interactions in heavy-metal/ferromagnet bilayers can produce strong current-driven torques on the magnetic layer, via the spin Hall effect in the heavy metal or the Rashba-Edelstein effect in the ferromagnet.