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Title: Femtosecond covariance spectroscopy

Abstract

The success of nonlinear optics relies largely on pulse-to-pulse consistency. In contrast, covariance-based techniques used in photoionization electron spectroscopy and mass spectrometry have shown that a wealth of information can be extracted from noise that is lost when averaging multiple measurements. Here, we apply covariance-based detection to nonlinear optical spectroscopy, and show that noise in a femtosecond laser is not necessarily a liability to be mitigated, but can act as a unique and powerful asset. As a proof of principle we apply this approach to the process of stimulated Raman scattering in α-quartz. Our results demonstrate how nonlinear processes in the sample can encode correlations between the spectral components of ultrashort pulses with uncorrelated stochastic fluctuations. This in turn provides richer information compared with the standard nonlinear optics techniques that are based on averages over many repetitions with well-behaved laser pulses. Finally, these proof-of-principle results suggest that covariance-based nonlinear spectroscopy will improve the applicability of fs nonlinear spectroscopy in wavelength ranges where stable, transform-limited pulses are not available, such as X-ray free-electron lasers which naturally have spectrally noisy pulses ideally suited for this approach.

Authors:
; ; ; ; ; ; ; ; ; ; ORCiD logo;
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; European Research Council (ERC); National Science Foundation (NSF)
OSTI Identifier:
1497259
Alternate Identifier(s):
OSTI ID: 1609515
Grant/Contract Number:  
FG02-04ER15571; SC0019484; 677488; CHE-1663822
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 116 Journal Issue: 12; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; impulsive stimulated scattering; ultrafast spectroscopy; stochastic light

Citation Formats

Tollerud, Jonathan Owen, Sparapassi, Giorgia, Montanaro, Angela, Asban, Shahaf, Glerean, Filippo, Giusti, Francesca, Marciniak, Alexandre, Kourousias, George, Billè, Fulvio, Cilento, Federico, Mukamel, Shaul, and Fausti, Daniele. Femtosecond covariance spectroscopy. United States: N. p., 2019. Web. doi:10.1073/pnas.1821048116.
Tollerud, Jonathan Owen, Sparapassi, Giorgia, Montanaro, Angela, Asban, Shahaf, Glerean, Filippo, Giusti, Francesca, Marciniak, Alexandre, Kourousias, George, Billè, Fulvio, Cilento, Federico, Mukamel, Shaul, & Fausti, Daniele. Femtosecond covariance spectroscopy. United States. doi:https://doi.org/10.1073/pnas.1821048116
Tollerud, Jonathan Owen, Sparapassi, Giorgia, Montanaro, Angela, Asban, Shahaf, Glerean, Filippo, Giusti, Francesca, Marciniak, Alexandre, Kourousias, George, Billè, Fulvio, Cilento, Federico, Mukamel, Shaul, and Fausti, Daniele. Thu . "Femtosecond covariance spectroscopy". United States. doi:https://doi.org/10.1073/pnas.1821048116.
@article{osti_1497259,
title = {Femtosecond covariance spectroscopy},
author = {Tollerud, Jonathan Owen and Sparapassi, Giorgia and Montanaro, Angela and Asban, Shahaf and Glerean, Filippo and Giusti, Francesca and Marciniak, Alexandre and Kourousias, George and Billè, Fulvio and Cilento, Federico and Mukamel, Shaul and Fausti, Daniele},
abstractNote = {The success of nonlinear optics relies largely on pulse-to-pulse consistency. In contrast, covariance-based techniques used in photoionization electron spectroscopy and mass spectrometry have shown that a wealth of information can be extracted from noise that is lost when averaging multiple measurements. Here, we apply covariance-based detection to nonlinear optical spectroscopy, and show that noise in a femtosecond laser is not necessarily a liability to be mitigated, but can act as a unique and powerful asset. As a proof of principle we apply this approach to the process of stimulated Raman scattering in α-quartz. Our results demonstrate how nonlinear processes in the sample can encode correlations between the spectral components of ultrashort pulses with uncorrelated stochastic fluctuations. This in turn provides richer information compared with the standard nonlinear optics techniques that are based on averages over many repetitions with well-behaved laser pulses. Finally, these proof-of-principle results suggest that covariance-based nonlinear spectroscopy will improve the applicability of fs nonlinear spectroscopy in wavelength ranges where stable, transform-limited pulses are not available, such as X-ray free-electron lasers which naturally have spectrally noisy pulses ideally suited for this approach.},
doi = {10.1073/pnas.1821048116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 12,
volume = 116,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: https://doi.org/10.1073/pnas.1821048116

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