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Autores principales: Fuerst, Lukas, Eber, Alexander, Pal, Mithun, Hruska, Emily, Hofmann, Clemens, Gordon, Iouli, Schultze, Martin, Breinbauer, Rolf, Bernhardt, Birgitta
Formato: Preprint
Publicado: 2025
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Acceso en línea:https://arxiv.org/abs/2501.07350
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author Fuerst, Lukas
Eber, Alexander
Pal, Mithun
Hruska, Emily
Hofmann, Clemens
Gordon, Iouli
Schultze, Martin
Breinbauer, Rolf
Bernhardt, Birgitta
author_facet Fuerst, Lukas
Eber, Alexander
Pal, Mithun
Hruska, Emily
Hofmann, Clemens
Gordon, Iouli
Schultze, Martin
Breinbauer, Rolf
Bernhardt, Birgitta
contents Photochemistry in the earth's atmosphere is driven by the sun, continuously altering the concentration and spatial distribution of pollutants. Precisely monitoring their atmospheric abundance relies predominantly on optical sensing, which requires the knowledge of exact absorption cross sections. One key pollutant which impacts many photochemical reaction-pathways is formaldehyde. Agreement on formaldehyde absolute absorption cross section remains elusive in the photochemically-relevant ultraviolet spectral region, hampering sensitive concentration tracking. Here, we introduce free-running ultraviolet dual comb spectroscopy, combining high spectral resolution (1 GHz), broad spectral coverage (12 THz), and fast acquisition speed (500 ms), as a novel method for absolute absorption cross section determination with unprecedented fidelity. Within this bandwidth, our method uncovers almost one order of magnitude more rovibrational transitions than detected before which leads to refined rotational constants for high-level quantum simulations of molecular eigenstates. This ultra-resolution method can be generalized to provide a universal tool for fast electronic fingerprinting of atmospherically-relevant species, both for sensing applications and to benchmark improvements of ab-initio quantum theory.
format Preprint
id arxiv_https___arxiv_org_abs_2501_07350
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Ultra-resolution photochemical sensing
Fuerst, Lukas
Eber, Alexander
Pal, Mithun
Hruska, Emily
Hofmann, Clemens
Gordon, Iouli
Schultze, Martin
Breinbauer, Rolf
Bernhardt, Birgitta
Optics
Photochemistry in the earth's atmosphere is driven by the sun, continuously altering the concentration and spatial distribution of pollutants. Precisely monitoring their atmospheric abundance relies predominantly on optical sensing, which requires the knowledge of exact absorption cross sections. One key pollutant which impacts many photochemical reaction-pathways is formaldehyde. Agreement on formaldehyde absolute absorption cross section remains elusive in the photochemically-relevant ultraviolet spectral region, hampering sensitive concentration tracking. Here, we introduce free-running ultraviolet dual comb spectroscopy, combining high spectral resolution (1 GHz), broad spectral coverage (12 THz), and fast acquisition speed (500 ms), as a novel method for absolute absorption cross section determination with unprecedented fidelity. Within this bandwidth, our method uncovers almost one order of magnitude more rovibrational transitions than detected before which leads to refined rotational constants for high-level quantum simulations of molecular eigenstates. This ultra-resolution method can be generalized to provide a universal tool for fast electronic fingerprinting of atmospherically-relevant species, both for sensing applications and to benchmark improvements of ab-initio quantum theory.
title Ultra-resolution photochemical sensing
topic Optics
url https://arxiv.org/abs/2501.07350