Natural and Intrinsic Vacancies in two-dimensional g-C$_3$N$_4$ for Trapping Isolated B and C Atoms as Color Centers

TL;DR

This paper explores natural vacancies in 2D g-C₃N₄ as stable, tunable hosts for B and C atoms to form color centers suitable for quantum information processing, with detailed analysis of their electronic and optical properties.

Contribution

It demonstrates that intrinsic vacancies in g-C₃N₄ can effectively trap B and C atoms, creating stable, optically active color centers with tunable spin and charge states for quantum applications.

Findings

Vacancy sites are the most stable adsorption positions for B and C atoms.

Charge states of the defect centers can be tuned to modify electronic and optical properties.

Zero-phonon lines indicate fluorescence in the mid-infrared, suitable for qubit operations.

Abstract

Color centers are vital for quantum information processing, but traditional ones often suffer from instability, difficulty in realization, and precise control of locations. In contrast, natural intrinsic vacancy-based color centers in two-dimensional systems offer enhanced stability and tunability. In this work, we demonstrate that g-C$_3$N$_4$ with natural intrinsic vacancies is highly suitable for trapping B/C atoms to form stable color centers as qubits. With easily identifiable vacancies, B/C atoms are expectable to be placed at the vacancy sites in g-C$_3$N$_4$ through STM manipulation. The vacancy sites are confirmed as the most stable adsorption positions, and once atoms are adsorbed, they are protected by diffusion barriers from thermal diffusions. The most stable charge states are C$_V^{+2}$/B$_V^{+2}$, C$_V^{+1}$/B$_V^{+1}$, and C$_V^0$/B$_V^0$ in turn, with charge transition levels of 0.39 eV and 2.49 eV, respectively. Specifically, the defect levels and net spin of C$_V$/B$_V$ can be adjusted by charge states. C$_V$, C$_V^{+1}$, C$_V^{+2}$, B$_V^{+1}$, and B$_V^{+2}$ exhibit optically allowable defect transition levels. The zero-phonon lines suggest fluorescence wavelengths fall within the mid-infrared band, ideal for qubit operations of stable initialization and readout. Furthermore, the Zero-field splitting (ZFS) parameter and the characteristic hyperfine tensor are provided as potential fingerprints for electron paramagnetic resonance (EPR) experiments.