Single-atom vibrational spectroscopy in the scanning transmission electron microscope
Single-atom impurities and other atomic-scale defects can notably alter the local vibrational responses of solids and, ultimately, their macroscopic properties. Using high-resolution electron energy-loss spectroscopy in the electron microscope, we show that a single substitutional silicon impurity i...
Main Authors: | , , , , |
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Format: | Journal article |
Language: | English |
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American Association for the Advancement of Science
2020
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_version_ | 1797068475070414848 |
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author | Hage, FS Radtke, G Kepaptsoglou, DM Lazzeri, M Ramasse, QM |
author_facet | Hage, FS Radtke, G Kepaptsoglou, DM Lazzeri, M Ramasse, QM |
author_sort | Hage, FS |
collection | OXFORD |
description | Single-atom impurities and other atomic-scale defects can notably alter the local vibrational responses of solids and, ultimately, their macroscopic properties. Using high-resolution electron energy-loss spectroscopy in the electron microscope, we show that a single substitutional silicon impurity in graphene induces a characteristic, localized modification of the vibrational response. Extensive ab initio calculations reveal that the measured spectroscopic signature arises from defect-induced pseudo-localized phonon modes—that is, resonant states resulting from the hybridization of the defect modes and the bulk continuum—with energies that can be directly matched to the experiments. This finding realizes the promise of vibrational spectroscopy in the electron microscope with single-atom sensitivity and has broad implications across the fields of physics, chemistry, and materials science. |
first_indexed | 2024-03-06T22:11:15Z |
format | Journal article |
id | oxford-uuid:51e0f98d-277c-4813-ba92-b5d5c2fd725b |
institution | University of Oxford |
language | English |
last_indexed | 2024-03-06T22:11:15Z |
publishDate | 2020 |
publisher | American Association for the Advancement of Science |
record_format | dspace |
spelling | oxford-uuid:51e0f98d-277c-4813-ba92-b5d5c2fd725b2022-03-26T16:22:19ZSingle-atom vibrational spectroscopy in the scanning transmission electron microscopeJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:51e0f98d-277c-4813-ba92-b5d5c2fd725bEnglishSymplectic ElementsAmerican Association for the Advancement of Science2020Hage, FSRadtke, GKepaptsoglou, DMLazzeri, MRamasse, QMSingle-atom impurities and other atomic-scale defects can notably alter the local vibrational responses of solids and, ultimately, their macroscopic properties. Using high-resolution electron energy-loss spectroscopy in the electron microscope, we show that a single substitutional silicon impurity in graphene induces a characteristic, localized modification of the vibrational response. Extensive ab initio calculations reveal that the measured spectroscopic signature arises from defect-induced pseudo-localized phonon modes—that is, resonant states resulting from the hybridization of the defect modes and the bulk continuum—with energies that can be directly matched to the experiments. This finding realizes the promise of vibrational spectroscopy in the electron microscope with single-atom sensitivity and has broad implications across the fields of physics, chemistry, and materials science. |
spellingShingle | Hage, FS Radtke, G Kepaptsoglou, DM Lazzeri, M Ramasse, QM Single-atom vibrational spectroscopy in the scanning transmission electron microscope |
title | Single-atom vibrational spectroscopy in the scanning transmission electron microscope |
title_full | Single-atom vibrational spectroscopy in the scanning transmission electron microscope |
title_fullStr | Single-atom vibrational spectroscopy in the scanning transmission electron microscope |
title_full_unstemmed | Single-atom vibrational spectroscopy in the scanning transmission electron microscope |
title_short | Single-atom vibrational spectroscopy in the scanning transmission electron microscope |
title_sort | single atom vibrational spectroscopy in the scanning transmission electron microscope |
work_keys_str_mv | AT hagefs singleatomvibrationalspectroscopyinthescanningtransmissionelectronmicroscope AT radtkeg singleatomvibrationalspectroscopyinthescanningtransmissionelectronmicroscope AT kepaptsogloudm singleatomvibrationalspectroscopyinthescanningtransmissionelectronmicroscope AT lazzerim singleatomvibrationalspectroscopyinthescanningtransmissionelectronmicroscope AT ramasseqm singleatomvibrationalspectroscopyinthescanningtransmissionelectronmicroscope |