TY - JOUR
T1 - High-Throughput Search for Triplet Point Defects with Narrow Emission Lines in 2D Materials
AU - Ali, Sajid
AU - Nilsson, Fredrik Andreas
AU - Manti, Simone
AU - Bertoldo, Fabian
AU - Mortensen, Jens Jørgen
AU - Thygesen, Kristian Sommer
PY - 2023
Y1 - 2023
N2 - We employ a first-principles computational workflow to screen for optically accessible, high-spin point defects in wide band gap, two-dimensional (2D) crystals. Starting from an initial set of 5388 point defects, comprising both native and extrinsic, single and double defects in ten previously synthesized 2D host materials, we identify 596 defects with a triplet ground state. For these defects, we calculate the defect formation energy, hyperfine (HF) coupling, and zero-field splitting (ZFS) tensors. For 39 triplet transitions exhibiting particularly low Huang-Rhys factors, we calculate the full photoluminescence (PL) spectrum. Our approach reveals many spin defects with narrow PL line shapes and emission frequencies covering a broad spectral range. Most of the defects are hosted in hexagonal BN (hBN), which we ascribe to its high stiffness, but some are also found in MgI2, MoS2, MgBr2 and CaI2. As specific examples, we propose the defects vSMoS0 and NiSMoS0 in MoS2 as interesting candidates with potential applications to magnetic field sensors and quantum information technology.
AB - We employ a first-principles computational workflow to screen for optically accessible, high-spin point defects in wide band gap, two-dimensional (2D) crystals. Starting from an initial set of 5388 point defects, comprising both native and extrinsic, single and double defects in ten previously synthesized 2D host materials, we identify 596 defects with a triplet ground state. For these defects, we calculate the defect formation energy, hyperfine (HF) coupling, and zero-field splitting (ZFS) tensors. For 39 triplet transitions exhibiting particularly low Huang-Rhys factors, we calculate the full photoluminescence (PL) spectrum. Our approach reveals many spin defects with narrow PL line shapes and emission frequencies covering a broad spectral range. Most of the defects are hosted in hexagonal BN (hBN), which we ascribe to its high stiffness, but some are also found in MgI2, MoS2, MgBr2 and CaI2. As specific examples, we propose the defects vSMoS0 and NiSMoS0 in MoS2 as interesting candidates with potential applications to magnetic field sensors and quantum information technology.
KW - 2D Materials
KW - Databases
KW - High-Throughput
KW - Point Defects
KW - Quantum Technology
KW - Single Photon Emission
KW - Triplets
U2 - 10.1021/acsnano.3c04774
DO - 10.1021/acsnano.3c04774
M3 - Journal article
C2 - 37889165
SN - 1936-0851
VL - 17
SP - 21105
EP - 21115
JO - ACS Nano
JF - ACS Nano
IS - 21
ER -