Efficient generation of few-cycle pulses beyond 10 μm from an optical parametric amplifier pumped by a 1-µm laser system

Abstract Nonlinear vibrational spectroscopy profits from broadband sources emitting in the molecular fingerprint region. Yet, broadband lasers operating at wavelengths above 7 μm have been lacking, while traditional cascaded parametric frequency down-conversion schemes suffer from exceedingly low co...

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Main Authors: Zsuzsanna Heiner, Valentin Petrov, Vladimir L. Panyutin, Valeriy V. Badikov, Kiyoshi Kato, Kentaro Miyata, Mark Mero
Format: Article
Language:English
Published: Nature Portfolio 2022-03-01
Series:Scientific Reports
Online Access:https://doi.org/10.1038/s41598-022-08964-w
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author Zsuzsanna Heiner
Valentin Petrov
Vladimir L. Panyutin
Valeriy V. Badikov
Kiyoshi Kato
Kentaro Miyata
Mark Mero
author_facet Zsuzsanna Heiner
Valentin Petrov
Vladimir L. Panyutin
Valeriy V. Badikov
Kiyoshi Kato
Kentaro Miyata
Mark Mero
author_sort Zsuzsanna Heiner
collection DOAJ
description Abstract Nonlinear vibrational spectroscopy profits from broadband sources emitting in the molecular fingerprint region. Yet, broadband lasers operating at wavelengths above 7 μm have been lacking, while traditional cascaded parametric frequency down-conversion schemes suffer from exceedingly low conversion efficiencies. Here we present efficient, direct frequency down-conversion of femtosecond 100-kHz, 1.03-μm pulses to the mid-infrared from 7.5 to 13.3 μm in a supercontinuum-seeded, tunable, single-stage optical parametric amplifier based on the wide-bandgap material Cd0.65Hg0.35Ga2S4. The amplifier delivers near transform-limited, few-cycle pulses with an average power > 30 mW at center wavelengths between 8.8 and 10.6 μm, at conversion efficiencies far surpassing that of optical parametric amplification followed by difference-frequency generation or intrapulse difference-frequency generation. The pulse duration at 10.6 μm is 101 fs corresponding to 2.9 optical cycles with a spectral coverage of 760–1160 cm−1. CdxHg1−xGa2S4 is an attractive alternative to LiGaS2 and BaGa4S7 in small-scale, Yb-laser-pumped, few-cycle mid-infrared optical parametric amplifiers and offers a much higher nonlinear figure of merit compared to those materials. Leveraging the inherent spatial variation of composition in CdxHg1−xGa2S4, an approach is proposed to give access to a significant fraction of the molecular fingerprint region using a single crystal at a fixed phase matching angle.
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spelling doaj.art-a9bf73f36b6d40088892b58eddf02cff2022-12-22T02:37:51ZengNature PortfolioScientific Reports2045-23222022-03-011211710.1038/s41598-022-08964-wEfficient generation of few-cycle pulses beyond 10 μm from an optical parametric amplifier pumped by a 1-µm laser systemZsuzsanna Heiner0Valentin Petrov1Vladimir L. Panyutin2Valeriy V. Badikov3Kiyoshi Kato4Kentaro Miyata5Mark Mero6School of Analytical Sciences Adlershof, Humboldt-Universität zu BerlinMax Born Institute for Nonlinear Optics and Short Pulse SpectroscopyMax Born Institute for Nonlinear Optics and Short Pulse SpectroscopyHigh Technologies Laboratory, Kuban State UniversityChitose Institute of Science and TechnologyRIKEN Center for Advanced Photonics, RIKENMax Born Institute for Nonlinear Optics and Short Pulse SpectroscopyAbstract Nonlinear vibrational spectroscopy profits from broadband sources emitting in the molecular fingerprint region. Yet, broadband lasers operating at wavelengths above 7 μm have been lacking, while traditional cascaded parametric frequency down-conversion schemes suffer from exceedingly low conversion efficiencies. Here we present efficient, direct frequency down-conversion of femtosecond 100-kHz, 1.03-μm pulses to the mid-infrared from 7.5 to 13.3 μm in a supercontinuum-seeded, tunable, single-stage optical parametric amplifier based on the wide-bandgap material Cd0.65Hg0.35Ga2S4. The amplifier delivers near transform-limited, few-cycle pulses with an average power > 30 mW at center wavelengths between 8.8 and 10.6 μm, at conversion efficiencies far surpassing that of optical parametric amplification followed by difference-frequency generation or intrapulse difference-frequency generation. The pulse duration at 10.6 μm is 101 fs corresponding to 2.9 optical cycles with a spectral coverage of 760–1160 cm−1. CdxHg1−xGa2S4 is an attractive alternative to LiGaS2 and BaGa4S7 in small-scale, Yb-laser-pumped, few-cycle mid-infrared optical parametric amplifiers and offers a much higher nonlinear figure of merit compared to those materials. Leveraging the inherent spatial variation of composition in CdxHg1−xGa2S4, an approach is proposed to give access to a significant fraction of the molecular fingerprint region using a single crystal at a fixed phase matching angle.https://doi.org/10.1038/s41598-022-08964-w
spellingShingle Zsuzsanna Heiner
Valentin Petrov
Vladimir L. Panyutin
Valeriy V. Badikov
Kiyoshi Kato
Kentaro Miyata
Mark Mero
Efficient generation of few-cycle pulses beyond 10 μm from an optical parametric amplifier pumped by a 1-µm laser system
Scientific Reports
title Efficient generation of few-cycle pulses beyond 10 μm from an optical parametric amplifier pumped by a 1-µm laser system
title_full Efficient generation of few-cycle pulses beyond 10 μm from an optical parametric amplifier pumped by a 1-µm laser system
title_fullStr Efficient generation of few-cycle pulses beyond 10 μm from an optical parametric amplifier pumped by a 1-µm laser system
title_full_unstemmed Efficient generation of few-cycle pulses beyond 10 μm from an optical parametric amplifier pumped by a 1-µm laser system
title_short Efficient generation of few-cycle pulses beyond 10 μm from an optical parametric amplifier pumped by a 1-µm laser system
title_sort efficient generation of few cycle pulses beyond 10 μm from an optical parametric amplifier pumped by a 1 µm laser system
url https://doi.org/10.1038/s41598-022-08964-w
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