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Title: Time-resolved Chemical Imaging of Molecules by High-order Harmonics and Ultrashort Rescattering Electrons

Directly monitoring atomic motion during a molecular transformation with atomic-scale spatio-temporal resolution is a frontier of ultrafast optical science and physical chemistry. Here we provide the foundation for a new imaging method, fixed-angle broadband laser-induced electron scattering, based on structural retrieval by direct one-dimensional Fourier transform of a photoelectron energy distribution observed along the polarization direction of an intense ultrafast light pulse. The approach exploits the scattering of a broadband wave packet created by strong-field tunnel ionization to self-interrogate the molecular structure with picometre spatial resolution and bond specificity. With its inherent femtosecond resolution, combining our technique with molecular alignment can, in principle, provide the basis for time-resolved tomography for multi-dimensional transient structural determination.
Authors:
 [1]
  1. Kansas State Univ., Manhattan, KS (United States)
Publication Date:
OSTI Identifier:
1242403
Report Number(s):
DOE-KSU--15832-1
TRN: US1600913
DOE Contract Number:
FG02-06ER15832
Resource Type:
Technical Report
Resource Relation:
Related Information: DOI: 10.1103/PhysRevLett.109.133202
Research Org:
Kansas State University, Manhattan, KS (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; TIME RESOLUTION; FOURIER TRANSFORMATION; RESCATTERING; SPATIAL RESOLUTION; ELECTRONS; ENERGY SPECTRA; HARMONICS; VISIBLE RADIATION; TOMOGRAPHY; MOLECULAR STRUCTURE; ONE-DIMENSIONAL CALCULATIONS; IONIZATION; LASER RADIATION; WAVE PACKETS; POLARIZATION; PULSES; CHEMICAL BONDS; SPECIFICITY; TRANSIENTS; PHOTOELECTRON SPECTROSCOPY imaging; ultrafast