Ultrafast optical control of orbital and spin dynamics in a solid-state defect

Abstract

Atom-scale defects in semiconductors are promising building blocks for quantum devices, but our understanding of their material-dependent electronic structure, optical interactions, and dissipation mechanisms is lacking. Using picosecond resonant pulses of light, we study the coherent orbital and spin dynamics of a single nitrogen-vacancy center in diamond over time scales spanning six orders of magnitude. We develop a time-domain quantum tomography technique to precisely map the defect's excited-state Hamiltonian and exploit the excited-state dynamics to control its ground-state spin with optical pulses alone. These techniques generalize to other optically addressable nanoscale spin systems and serve as powerful tools to characterize and control spin qubits for future applications in quantum technology.

State-selective intersystem crossing in nitrogen-vacancy centers

“…The axial SO coupling rate λ = 5.33 ± 0.03 GHz has been measured precisely through spectroscopy of the 3 E manifold [32], but λ ⊥ cannot be determined through similar methods. An approximate theoretical argument implies that λ ⊥ ∼ λ .…”

Optical Coherence in Atomic-Monolayer Transition-Metal Dichalcogenides Limited by Electron-Phonon Interactions

“…The ability to obtain two-dimensional materials with variable band gaps has been very attractive for transistors, photodiodes, sensors [1][2][3][4][5][6][7][8][9][10][11], and more recently as single photon sources [12][13][14][15]. Furthermore, the preservation of the optical coherence is of importance to quantum computation devices [16,17]. Therefore, understanding the fundamental many-body interactions and how these interactions influence the optical properties of these materials is crucially important.…”

All-optical control of a single electron spin in diamond

“…The complex level structure and selection rules of the NV center's optical transitions offer a rich and flexible set of possibilities for coherent all-optical control of all three spin sublevels. Past experiments have demonstrated optical spin manipulation under a large magnetic field or two-photon Rabi oscillations and stimulated Raman adiabatic passage (STIRAP) on microsecond timescales [13][14][15].In this Letter, we demonstrate complete all-optical coherent manipulation of the NV spin states. Importantly, initialization and readout of the spin states are also performed all-optically, providing a full set of experimental techniques that eliminates the need for microwave addressing.…”