Point defects in solid-state quantum systems are vital for enabling single-photon emission at specific wavelengths,making their precise identification essential for advancing applications in quantum technologies.Howev...Point defects in solid-state quantum systems are vital for enabling single-photon emission at specific wavelengths,making their precise identification essential for advancing applications in quantum technologies.However,pinpointing the microscopic origins of these defects remains a challenge.In this work,we propose Raman spectroscopy as a robust strategy for defect identification.Using density functional theory,we characterize the Raman signatures of 100 defects in hexagonal boron nitride(hBN)spanning periodic groups III to VI,encompassing around 30,000 phonon modes.Our findings reveal that the local atomic environment plays a pivotal role in shaping the Raman lineshape.Furthermore,we demonstrate that Raman spectroscopy can differentiate defects based on their spin and charge states as well as strain-induced variations.The ability to resolve spin configurations offers a pathway to identifying defects with spins suitable for quantum sensing.Finally,an experimental concept using tip-enhanced Raman spectroscopy has been proposed in this work.Therefore,this study not only provides a comprehensive theoretical database of Raman spectra for hBN defects but also establishes a novel experimental framework to identify point defects.More broadly,our approach offers a universal method for defect identification in any quantum materials with spin configurations specific to any quantum application.展开更多
基金funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - Projektnummer 445275953under Germany’s Excellence Strategy - EXC-2111 - 390814868, and as part of the CRC 1375 NOA project C2 (Projektnummer 398816777)+2 种基金The authors acknowledge support from the Federal Ministry of Research, Technology and Space (BMFTR) under grant number 13N16292 (ATOMIQS). The authors acknowledge support by the German Space Agency DLR with funds provided by the Federal Ministry for Economic Affairs and Climate Action BMWK under grant numbers 50WM2165 (QUICK3) and 50RP2200 (QuVeKS)S.S. acknowledges research funding by Mahidol University (Fundamental Fund FF-111/2568: fiscal year 2025 by the National Science Research and Innovation Fund (NSRF))V.D. acknowledges the SFB-1375 NOA–Project C02 (Projektnummer 398816777). The authors gratefully acknowledge the Gauss Centre for Supercomputing e.V.\ (www.gauss-centre.eu) for funding this project by providing computing time on the GCS Supercomputer SuperMUC-NG at Leibniz Supercomputing Centre (www.lrz.de) and on its Linux-Cluster.
文摘Point defects in solid-state quantum systems are vital for enabling single-photon emission at specific wavelengths,making their precise identification essential for advancing applications in quantum technologies.However,pinpointing the microscopic origins of these defects remains a challenge.In this work,we propose Raman spectroscopy as a robust strategy for defect identification.Using density functional theory,we characterize the Raman signatures of 100 defects in hexagonal boron nitride(hBN)spanning periodic groups III to VI,encompassing around 30,000 phonon modes.Our findings reveal that the local atomic environment plays a pivotal role in shaping the Raman lineshape.Furthermore,we demonstrate that Raman spectroscopy can differentiate defects based on their spin and charge states as well as strain-induced variations.The ability to resolve spin configurations offers a pathway to identifying defects with spins suitable for quantum sensing.Finally,an experimental concept using tip-enhanced Raman spectroscopy has been proposed in this work.Therefore,this study not only provides a comprehensive theoretical database of Raman spectra for hBN defects but also establishes a novel experimental framework to identify point defects.More broadly,our approach offers a universal method for defect identification in any quantum materials with spin configurations specific to any quantum application.
