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research article

Ultrafast Photon-Induced Tunneling Microscopy

Garg, Manish
•
Martin-Jimenez, Alberto
•
Luo, Yang
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November 23, 2021
Acs Nano

Unification of the techniques of ultrafast science and scanning tunneling microscopy (STM) has the potential of tracking electronic motion in molecules simultaneously in real space and real time. Laser pulses can couple to an STM junction either in the weak-field or in the strong-field interaction regime. The strong-field regime entails significant modification (dressing) of the tunneling barrier of the STM junction, whereas the weak-field or the photon-driven regime entails perturbative interaction. Here, we describe how photons carried in an ultrashort pulse interact with an STM junction, defining the basic fundamental framework of ultrafast photon-induced tunneling microscopy. Selective dipole coupling of electronic states by photons is shown to be controllable by adjusting the DC bias at the STM junction. An ultrafast tunneling microscopy involving photons is established. Consolidation of the technique calls for innovative approaches to detect photon-induced tunneling currents at the STM junction. We introduce and characterize here three techniques involving dispersion, polarization, and frequency modulation of the laser pulses to lock-in detect the laser-induced tunneling current. We show that photon-induced tunneling currents can simultaneously achieve angstrom scale spatial resolution and sub-femtosecond temporal resolution. Ultrafast photon-induced tunneling microscopy will be able to directly probe electron dynamics in complex molecular systems, without the need of reconstruction techniques.

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Type
research article
DOI
10.1021/acsnano.1c06716
Web of Science ID

WOS:000747115200084

Author(s)
Garg, Manish
Martin-Jimenez, Alberto
Luo, Yang
Kern, Klaus  
Date Issued

2021-11-23

Publisher

AMER CHEMICAL SOC

Published in
Acs Nano
Volume

15

Issue

11

Start page

18071

End page

18084

Subjects

Chemistry, Multidisciplinary

•

Chemistry, Physical

•

Nanoscience & Nanotechnology

•

Materials Science, Multidisciplinary

•

Chemistry

•

Science & Technology - Other Topics

•

Materials Science

•

ultrashort pulses

•

atomic space-time resolution

•

angstrom-femtosecond resolution

•

4d tunneling microscopy

•

ultrafast optical stm techniques

•

dynamics

•

motion

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LSEN  
Available on Infoscience
February 28, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/185813
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