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Main Authors: Chacon, Ignacio, Echeverri, Andrea, Cardenas, Carlos, Munoz, Francisco
Format: Preprint
Published: 2024
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Online Access:https://arxiv.org/abs/2412.17457
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author Chacon, Ignacio
Echeverri, Andrea
Cardenas, Carlos
Munoz, Francisco
author_facet Chacon, Ignacio
Echeverri, Andrea
Cardenas, Carlos
Munoz, Francisco
contents Substitutional carbon defects in hexagonal boron nitride (hBN) are prominent single photon emitters (SPEs), and their potential for spin activity ($S\geq1$) is particularly intriguing. While studies have largely focused on intra-layer defects, we employ density functional theory (DFT) to investigate inter-layer dimers of identical carbon species (C$_X$C$_X$). We demonstrate that these C$_X$C$_X$ pairs can exhibit a stable triplet spin state at room temperature when closely spaced (e.g., within 3.5-7.1 Å) across hBN layers. As their separation increases beyond this range (e.g., $>7$ Å), they transition into weakly interacting $S=1/2$ pairs, characterized by singlet-triplet degeneracy. This regime is predicted to result in a very small zero-field splitting for the triplet manifold, offering a potential explanation for certain optically detected magnetic resonance (ODMR) signals. The zero-phonon line (ZPL) energy of these inter-layer C$_X$C$_X$ pairs is found to be practically monochromatic and within the visible range. Furthermore, we identify specific C$_B$C$_B$ inter-layer configurations exhibiting atypical low-energy phonon replicas due to out-of-plane vibrational coupling, a finding that may clarify the vibronic structure of other hBN emitters, such as the 'yellow emitters'.
format Preprint
id arxiv_https___arxiv_org_abs_2412_17457
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Optical Properties and Spin States of Inter-layer Carbon Defect Pairs in Hexagonal Boron Nitride: A First-Principles Study
Chacon, Ignacio
Echeverri, Andrea
Cardenas, Carlos
Munoz, Francisco
Materials Science
Mesoscale and Nanoscale Physics
Quantum Physics
Substitutional carbon defects in hexagonal boron nitride (hBN) are prominent single photon emitters (SPEs), and their potential for spin activity ($S\geq1$) is particularly intriguing. While studies have largely focused on intra-layer defects, we employ density functional theory (DFT) to investigate inter-layer dimers of identical carbon species (C$_X$C$_X$). We demonstrate that these C$_X$C$_X$ pairs can exhibit a stable triplet spin state at room temperature when closely spaced (e.g., within 3.5-7.1 Å) across hBN layers. As their separation increases beyond this range (e.g., $>7$ Å), they transition into weakly interacting $S=1/2$ pairs, characterized by singlet-triplet degeneracy. This regime is predicted to result in a very small zero-field splitting for the triplet manifold, offering a potential explanation for certain optically detected magnetic resonance (ODMR) signals. The zero-phonon line (ZPL) energy of these inter-layer C$_X$C$_X$ pairs is found to be practically monochromatic and within the visible range. Furthermore, we identify specific C$_B$C$_B$ inter-layer configurations exhibiting atypical low-energy phonon replicas due to out-of-plane vibrational coupling, a finding that may clarify the vibronic structure of other hBN emitters, such as the 'yellow emitters'.
title Optical Properties and Spin States of Inter-layer Carbon Defect Pairs in Hexagonal Boron Nitride: A First-Principles Study
topic Materials Science
Mesoscale and Nanoscale Physics
Quantum Physics
url https://arxiv.org/abs/2412.17457