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  Quantitative sampling of atomic-scale electromagnetic waveforms

Peller, D., Roelcke, C., Kastner, L. Z., Buchner, T., Neef, A., Hayes, J., et al. (2020). Quantitative sampling of atomic-scale electromagnetic waveforms. Nature Photonics, xx(xx), xx-xx. doi:10.1038/s41566-020-00720-8.

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Item Permalink: https://hdl.handle.net/21.11116/0000-0007-66A4-D Version Permalink: https://hdl.handle.net/21.11116/0000-0007-90FB-B
Genre: Journal Article

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Supplementary Information (pdf): Supplementary Note 1 and Figs. 1 and 2. | Supplementary Video 1 (mp4): Simulated temporal evolution of the Hartree potential comparing the set-up with molecule in the junction and the free junction. Video showing the vertical cross-section of the Hartree potential, similar to Fig. 4a,b, as it evolves over time when driven by an external waveform. Locally, the calculated Hartree potential without the molecule (left panel) and including the molecule in the junction (right panel) vary strongly. Every frame corresponds to a time step of 215 as. The colour scale indicates the Hartree potential in electronvolts. | Supplementary Video 2 (mp4): Simulated temporal evolution of the Hartree potential comparing two different tip orientations. Video showing the vertical cross-section of the Hartree potential as in Supplementary Video 1 (same time step per frame). Comparing a tilted tip configuration (left panel) with a symmetric geometry (right panel), we obtain very similar spatial distributions of the potential in the vicinity of the molecule, causing similar near-field profiles. Hence the near-field is not strongly dependent on the tip symmetry or orientation. The colour scale indicates the Hartree potential in electronvolts.
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 Creators:
Peller, D.1, Author
Roelcke, C.1, Author
Kastner, L. Z.1, Author
Buchner, T.1, Author
Neef, A.1, Author
Hayes, J.1, Author
Bonafé, F.2, Author           
Sidler, D.2, Author           
Ruggenthaler, M.2, Author           
Rubio, A.2, 3, 4, Author           
Huber, R.1, Author
Repp, J.1, Author
Affiliations:
1Department of Physics, University of Regensburg, ou_persistent22              
2Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
3Center for Computational Quantum Physics, Simons Foundation Flatiron Institute, ou_persistent22              
4Universidad del País Vasco, UPV/EHU, San Sebastián, ou_persistent22              

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 Abstract: Tailored nanostructures can confine electromagnetic waveforms in extremely sub-wavelength volumes, opening new avenues in lightwave sensing and control down to sub-molecular resolution. Atomic light–matter interaction depends critically on the absolute strength and the precise time evolution of the near field, which may be strongly influenced by quantum-mechanical effects. However, measuring atom-scale field transients has remained out of reach. Here we introduce quantitative atomic-scale waveform sampling in lightwave scanning tunnelling microscopy to resolve a tip-confined near-field transient. Our parameter-free calibration employs a single-molecule switch as an atomic-scale voltage standard. Although salient features of the far-to-near-field transfer follow classical electrodynamics, we develop a comprehensive understanding of the atomic-scale waveforms with time-dependent density functional theory. The simulations validate our calibration and confirm that single-electron tunnelling ensures minimal back-action of the measurement process on the electromagnetic fields. Our observations access an uncharted domain of nano-opto-electronics where local quantum dynamics determine femtosecond atomic near fields.

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Language(s): eng - English
 Dates: 2020-04-012020-10-152020-11-162020
 Publication Status: Issued
 Pages: -
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 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41566-020-00720-8
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Grant ID : 895747
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: Nature Photonics
Source Genre: Journal
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Publ. Info: London [u.a.] : Nature Publ. Group
Pages: - Volume / Issue: xx (xx) Sequence Number: - Start / End Page: xx - xx Identifier: Other: 1749-4885
Other: 1749-4893
CoNE: https://pure.mpg.de/cone/journals/resource/1000000000240270