Single-atom vibrational spectroscopy in the scanning transmission electron microscope

Science
F S HageQ M Ramasse

Abstract

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.

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Citations

Sep 2, 2020·Microscopy and Microanalysis : the Official Journal of Microscopy Society of America, Microbeam Analysis Society, Microscopical Society of Canada·Ray F EgertonPeter A Crozier
Mar 27, 2021·Science·Xiaoyan LiMathieu Kociak
Mar 29, 2021·Ultramicroscopy·Jacob MadsenToma Susi
May 20, 2021·ACS Nano·Andrea KonečnáF Javier García de Abajo
May 23, 2021·Nature Communications·Yong WangYe Tian
Jun 8, 2021·Chemical Science·Weiwei WuShaojun Dong
Jun 27, 2021·Microscopy and Microanalysis : the Official Journal of Microscopy Society of America, Microbeam Analysis Society, Microscopical Society of Canada·Kartik Venkatraman, Peter A Crozier
Nov 15, 2020·Ultramicroscopy·Peter Rez, Arunima Singh
Jul 27, 2021·ACS Nano·Fadil IyikanatF Javier García de Abajo
Aug 21, 2021·Microscopy and Microanalysis : the Official Journal of Microscopy Society of America, Microbeam Analysis Society, Microscopical Society of Canada·Jingyue Jimmy Liu

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