Two-dimensional phase cartography for high-harmonic spectroscopy
Abstract
Extremely nonlinear spectroscopy based on high-order-harmonic generation has become a powerful investigation method for attosecond dynamics in gas and solid targets. In particular, the phase of harmonic emission was shown to carry profound insight into atomic and molecular structure and dynamics. However, current techniques offer phase measurements only along specific directions, thus providing partial characterization. Here we report on a new approach combining optical and quantum interferometers measuring along two dimensions the intensity and phase of harmonic emission from aligned molecules in the exact same experimental conditions. This two-dimensional cartography technique measures the phase with no arbitrary offset and no uncertainty on its sign. Measurements along different dimensions can be combined in two ways: either a single mapping or a redundant mapping allowing high-precision phase recovery using a Shack–Hartmann-like algorithm. We demonstrate both methods in a nitrogen test case, which allows disentangling structural and dynamical effects. Two-dimensional phase cartography paves the way to high-resolution high-harmonic spectroscopy for applications such as quantum orbital tomography and attosecond charge migration in molecules.
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES), Chemical Sciences, Geosciences & Biosciences; Agence Nationale de la Recherche; Marie Curie Intra European Fellowship; Marie Curie Initial Training Network; COST; Laserlab-Europe Division (SC-22.1)
- OSTI Identifier:
- 1768667
- Alternate Identifier(s):
- OSTI ID: 1785257
- Grant/Contract Number:
- AC02-05CH11231; ANR-10-LABX-0039-PALM; ANR-11-EQPX0005-ATTOLAB; ANR-15-CE30-0001-CIMBAAD; 238362-ATTOFEL; CA18222-AttoChem Action; EU-H2020 871124
- Resource Type:
- Published Article
- Journal Name:
- Optica
- Additional Journal Information:
- Journal Name: Optica Journal Volume: 8 Journal Issue: 3; Journal ID: ISSN 2334-2536
- Publisher:
- Optical Society of America
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Camper, Antoine, Skantzakis, Emmanouil, Géneaux, Romain, Risoud, François, English, Elizabeth, Diveki, Zsolt, Lin, Nan, Gruson, Vincent, Auguste, Thierry, Carré, Bertrand, Lucchese, Robert R., Maquet, Alfred, Taïeb, Richard, Caillat, Jérémie, Ruchon, Thierry, and Salières, Pascal. Two-dimensional phase cartography for high-harmonic spectroscopy. United States: N. p., 2021.
Web. doi:10.1364/OPTICA.403859.
Camper, Antoine, Skantzakis, Emmanouil, Géneaux, Romain, Risoud, François, English, Elizabeth, Diveki, Zsolt, Lin, Nan, Gruson, Vincent, Auguste, Thierry, Carré, Bertrand, Lucchese, Robert R., Maquet, Alfred, Taïeb, Richard, Caillat, Jérémie, Ruchon, Thierry, & Salières, Pascal. Two-dimensional phase cartography for high-harmonic spectroscopy. United States. https://doi.org/10.1364/OPTICA.403859
Camper, Antoine, Skantzakis, Emmanouil, Géneaux, Romain, Risoud, François, English, Elizabeth, Diveki, Zsolt, Lin, Nan, Gruson, Vincent, Auguste, Thierry, Carré, Bertrand, Lucchese, Robert R., Maquet, Alfred, Taïeb, Richard, Caillat, Jérémie, Ruchon, Thierry, and Salières, Pascal. Tue .
"Two-dimensional phase cartography for high-harmonic spectroscopy". United States. https://doi.org/10.1364/OPTICA.403859.
@article{osti_1768667,
title = {Two-dimensional phase cartography for high-harmonic spectroscopy},
author = {Camper, Antoine and Skantzakis, Emmanouil and Géneaux, Romain and Risoud, François and English, Elizabeth and Diveki, Zsolt and Lin, Nan and Gruson, Vincent and Auguste, Thierry and Carré, Bertrand and Lucchese, Robert R. and Maquet, Alfred and Taïeb, Richard and Caillat, Jérémie and Ruchon, Thierry and Salières, Pascal},
abstractNote = {Extremely nonlinear spectroscopy based on high-order-harmonic generation has become a powerful investigation method for attosecond dynamics in gas and solid targets. In particular, the phase of harmonic emission was shown to carry profound insight into atomic and molecular structure and dynamics. However, current techniques offer phase measurements only along specific directions, thus providing partial characterization. Here we report on a new approach combining optical and quantum interferometers measuring along two dimensions the intensity and phase of harmonic emission from aligned molecules in the exact same experimental conditions. This two-dimensional cartography technique measures the phase with no arbitrary offset and no uncertainty on its sign. Measurements along different dimensions can be combined in two ways: either a single mapping or a redundant mapping allowing high-precision phase recovery using a Shack–Hartmann-like algorithm. We demonstrate both methods in a nitrogen test case, which allows disentangling structural and dynamical effects. Two-dimensional phase cartography paves the way to high-resolution high-harmonic spectroscopy for applications such as quantum orbital tomography and attosecond charge migration in molecules.},
doi = {10.1364/OPTICA.403859},
journal = {Optica},
number = 3,
volume = 8,
place = {United States},
year = {Tue Mar 02 00:00:00 EST 2021},
month = {Tue Mar 02 00:00:00 EST 2021}
}
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