Polarization Dynamics of Solid-State Quantum Emitters

ACS Nano. 2024 Feb 9;18(7):5270-5281. doi: 10.1021/acsnano.3c08940. Online ahead of print.

Abstract

Quantum emitters in solid-state crystals have recently attracted a great deal of attention due to their simple applicability in optical quantum technologies. The polarization of single photons generated by quantum emitters is one of the key parameters that plays a crucial role in various applications, such as quantum computation, which uses the indistinguishability of photons. However, the degree of single-photon polarization is typically quantified using the time-averaged photoluminescence intensity of single emitters, which provides limited information about the dipole properties in solids. In this work, we use single defects in hexagonal boron nitride and nanodiamond as efficient room-temperature single-photon sources to reveal the origin and temporal evolution of the dipole orientation in solid-state quantum emitters. The angles of the excitation and emission dipoles relative to the crystal axes were determined experimentally and then calculated using density functional theory, which resulted in characteristic angles for every specific defect that can be used as an efficient tool for defect identification and understanding their atomic structure. Moreover, the temporal polarization dynamics revealed a strongly modified linear polarization visibility that depends on the excited-state decay time of the individual excitation. This effect can potentially be traced back to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further improve the performance of polarization-sensitive experiments, particularly that for quantum communication with single-photon emitters.

Keywords: defect identification; density functional theory; electron irradiation; hexagonal boron nitride; nanodiamond NV centers; quantum emitters array; temporal polarization dynamics.