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Updated: Jun 9, 2026
11:33
All-electronic Nanosecond-resolved Scanning Tunneling Microscopy: Facilitating the Investigation of Single Dopant Charge Dynamics
Published on: January 19, 2018
Real-time mapping of electronic structure with single-shot two-dimensional electronic spectroscopy
Elad Harel1, Andrew F Fidler, Gregory S Engel
1The James Franck Institute and Department of Chemistry, University of Chicago, Chicago, IL 60637, USA.
Summary
GRAPE spectroscopy maps electronic Hamiltonian evolution in real-time using a single laser shot. This technique dramatically reduces acquisition time and eliminates phase errors for studying ultrafast electronic dynamics.
Area of Science:
- Physical Chemistry
- Spectroscopy
- Materials Science
Background:
- Electronic structure and dynamics govern material properties.
- Ultrafast electronic dynamics occur on attosecond to millisecond timescales.
- Conventional 2D optical spectroscopy is limited to fast dynamics due to long acquisition times.
Purpose of the Study:
- To develop a novel spectroscopic method for mapping electronic Hamiltonian evolution.
- To enable real-time observation of electronic coupling dynamics.
- To overcome the temporal limitations of existing 2D optical spectroscopy techniques.
Main Methods:
- Introduced GRadient-Assisted Photon Echo (GRAPE) spectroscopy.
- Employs spatial encoding of temporally encoded information within a homogeneous sample.
- Utilizes conventional optical components for femtosecond temporal resolution in a single laser shot.
Main Results:
- GRAPE spectroscopy provides real-time maps of electronic coupling.
- Acquisition time is reduced by orders of magnitude compared to traditional methods.
- Eliminates phase errors common in Fourier transform spectroscopies.
- Spatial encoding enhances signal-to-noise ratio without signal loss.
Conclusions:
- GRAPE spectroscopy offers a powerful new tool for studying ultrafast electronic dynamics.
- Enables correlation of fast energy transfer events with slow dynamics.
- Applications span photobiology, solar energy, nonlinear spectroscopy, and optoelectronics.
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