Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:2007.11900 · New Journal of Physics

A spectrally bright wavelength-switchable vacuum ultraviolet source driven by quantum coherence in strong-field-ionized molecules

Yuexin Wan, Zhaoxiang Liu, Jinping Yao, Bo Xu, Jinming Chen, Fangbo Zhang, Zhihao Zhang, Lingling Qiao, Ya Cheng

Published Jan 21, 2021• 6 citations
arXivHTMLPDF

Abstract

Abstract We report generation of spectrally bright vacuum ultraviolet (VUV) and deep UV (DUV) coherent radiations at the wavelengths of 192 nm, 198 nm and 204 nm. These DUV/VUV radiations originate from resonant four-wave mixing assisted by quantum coherence in tunnel-ionized CO molecules. The electronic coherence is created when the pump pulses resonantly excite electronic transitions of CO+. The technique allows for the selective switch of DUV/VUV wavelengths provided by the abundant energy levels of molecular ions. The developed source can have arbitrary polarization states by manipulating the polarization of the pump pulse. It also exhibits a spectral bandwidth of 5∼7 cm−1, a divergence angle of 3∼5 mrad, a pulse duration of ∼10 ps, and a photon flux of ∼1010 photons/s. The superior temporal and spectral properties give rise to a broadband Raman comb in the DUV/VUV region.

DOI
10.1088/1367-2630/abde6e

Related papers

Ultraviolet supercontinuum generation driven by ionic coherence in a strong laser field

Hongbin Lei, Jinping Yao, Jing Zhao +11 more

Supercontinuum (SC) light sources hold versatile applications in many fields ranging from imaging microscopic structural dynamics to achieving frequency comb metrology. Although such broadband light sources are readily accessible in the visible and near infrared regime, the ultraviolet (UV) extension of SC spectrum is still challenging. Here, we demonstrate that the joint contribution of strong field ionization and quantum resonance leads to the unexpected UV continuum radiation spanning the 100 nm bandwidth in molecular nitrogen ions. Quantum coherences in a bunch of ionic levels are found to be created by dynamic Stark-assisted multiphoton resonances following tunneling ionization. We show that the dynamical evolution of the coherence-enhanced polarization wave gives rise to laser-assisted continuum emission inside the laser field and free-induction decay after the laser field, which jointly contribute to the SC generation together with fifth harmonics. As proof of principle, we also show the application of the SC radiation in the absorption spectroscopy. This work offers an alternative scheme for constructing exotic SC sources, and opens up the territory of ionic quantum optics in the strong-field regime.

Nature Communications•Jul 14, 2022•55 citations

Generation of high-brightness coherent radiation in the vacuum ultraviolet by four-wave parametric oscillation in mercury vapor

Jeffrey Bokor A, Richard R. Freeman, R. L. Panock +1 more

Coherent radiation at several wavelengths in the vacuum ultraviolet (VUV) has been generated by four-wave parametric oscillation in mercury vapor. When a powerful ultraviolet pump laser of frequency omega(p) is tuned to a two-photon resonance, VUV signal photons at frequency omega(s), as well as idler photons at frequency omega(i), are generated such that omega(s) + omega(i) = 2omega(p). A frequency-doubled dye laser tuned to two-photon resonance with the 6s6d(1)D(2) level near 280.3 nm produced output at 184.9 and 143.5 nm. A tunable krypton fluoride excimer laser tuned to two-photon resonance with the 6s10s (1)S(0) level near 248.7 nm produced output at 140.1, 130.7, 130.1, 125.9, and 125.0 nm. Approximately 1-microJ, 200-W pulses were observed at 143.5 and 125.9 nm.

Optics Letters•Apr 1, 1981•60 citations

Attosecond pulse formation via switching of resonant interaction by tunnel ionization

V. A. Antonov, T. R. Akhmedzhanov, Yevgeny V. Radeonychev +1 more

We derive an analytical solution uncovering the origin of few-cycle attosecond pulse formation from vacuum-ultraviolet (VUV) radiation in an atomic gas simultaneously irradiated by a moderately strong infrared (IR) laser field, which does not perturb atoms in the ground state, but induces rapid quasistatic ionization from the excited states [Polovinkin et al., Opt. Lett. 36, 2296 (2011)]. The derived solution shows that the pulses are produced due to periodic switching of the resonant interaction between the incident VUV radiation and the atoms: turning it off near the crests of the IR-field strength and switching it back on near the IR-field zero crossings. We extend the method originally proposed by Polovinkin et al. [Opt. Lett. 36, 2296 (2011)] to non-hydrogen-like media and show that the pulses can be produced from resonant VUV radiation in a variety of atomic gases. The pulses are nearly bandwidth limited without external adjustment of phases of the generated sidebands. Proximity of the carrier frequency of the produced pulses to intra-atomic resonances may allow their efficient utilization for nondestructive steering of ultrafast dynamics of the bound electrons. The experimental possibilities for attosecond pulse formation from 58.4 nm VUV radiation in helium and from 73.6 nm VUV radiation in neon dressed by the 3.9 \ensuremath{\mu}m laser field, as well as from 122 nm VUV radiation in atomic hydrogen dressed by $\mathrm{C}{\mathrm{O}}_{2}$-laser field are discussed.

Physical Review A•Feb 24, 2015•8 citations

Generation of continuously tunable coherent vacuum-ultraviolet radiation in Cd vapor

Kenzo Miyazaki, Hirofumi Sakai, Takuzo Sato

Continuously tunable coherent vacuum-ultraviolet (VUV) radiation has been generated in the 128.7-135.3-nm region by two-photon resonant four-wave mixing in Cd vapor. The generated VUV has no spectral structure over the tuning range and indicates that Cd vapor is an efficient nonlinear medium for frequency conversion.

Optics Letters•Oct 1, 1984•14 citations

Theory of deep ultraviolet generation at maximum coherence assisted by Stark-chirped two-photon resonance

S. A. Myslivets, A. K. Popov, Victor Kimberg +1 more

A scheme is analyzed for effcient generation of vacuum ultraviolet radiation through four-wave mixing processes assisted by the technique of Stark-chirped rapid adiabatic passage. These opportunities are associated with pulse excitation of laddertype short-wavelength two-photon atomic or molecular transitions so that relaxation processes can be neglected. In this three-laser technique, a delayed-pulse of strong oR-resonant infrared radiation sweeps the laser-induced Stark-shift of a two-photon transition in a such way that facilitates robust maximum two-photon coherence induced by the first ultraviolet laser. A judiciously delayed third pulse scatters at this coherence and generates short-wavelength radiation. A theoretical analysis of these problems based on the density matrix is performed. A numerical model is developed to carry out simulations of a typical experiment. The results illustrate a behavior of populations, coherence and generated radiation along the medium as well as opportunities of effcient generation of deep (vacuum) ultraviolet radiation.

arXiv:quant-ph/0301158•Jan 29, 2003•0 citations

High-efficiency, energy-scalable, coherent 130-nm source by four-wave mixing in Hg vapor

C. H. Muller, Arlee V. Smith, Dennis D. Lowenthal +1 more

Coherent vacuum-ultraviolet (VUV) pulses with energy of 1.1 mJ, 2.2-nsec pulse length (2 MW cm−2 unfocused), and measured bandwidth ≤0.1 cm−1 have been achieved at 130 nm from four-wave mixing in Hg vapor. Conversion efficiencies of 5% have been demonstrated in a collimated beam geometry over 1-m interaction lengths. These high efficiencies are made possible by using two-photon-resonant sum-frequency mixing through the Hg 71S level. The experimental facility assembled to produce this efficient VUV source is described, and a comparison between experimental measurements and theory is provided.

Optics Letters•Aug 1, 1988•35 citations
Abstract We report generation of spectrally bright vacuum ultraviolet (VUV) and deep UV (DUV) coherent radiations at the wavelengths of 192 nm, 198 nm and 204 nm. These DUV/VUV radiations originate from resonant four-wave mixing assisted by quantum coherence in tunnel-ionized CO molecules. The electronic coherence is created when the pump pulses resonantly excite electronic transitions of CO+. The technique allows for the selective switch of DUV/VUV wavelengths provided by the abundant energy levels of molecular ions. The developed source can have arbitrary polarization states by manipulating the polarization of the pump pulse. It also exhibits a spectral bandwidth of 5∼7 cm−1, a divergence angle of 3∼5 mrad, a pulse duration of ∼10 ps, and a photon flux of ∼1010 photons/s. The superior temporal and spectral properties give rise to a broadband Raman comb in the DUV/VUV region.
Supercontinuum (SC) light sources hold versatile applications in many fields ranging from imaging microscopic structural dynamics to achieving frequency comb metrology. Although such broadband light sources are readily accessible in the visible and near infrared regime, the ultraviolet (UV) extension of SC spectrum is still challenging. Here, we demonstrate that the joint contribution of strong field ionization and quantum resonance leads to the unexpected UV continuum radiation spanning the 100 nm bandwidth in molecular nitrogen ions. Quantum coherences in a bunch of ionic levels are found to be created by dynamic Stark-assisted multiphoton resonances following tunneling ionization. We show that the dynamical evolution of the coherence-enhanced polarization wave gives rise to laser-assisted continuum emission inside the laser field and free-induction decay after the laser field, which jointly contribute to the SC generation together with fifth harmonics. As proof of principle, we also show the application of the SC radiation in the absorption spectroscopy. This work offers an alternative scheme for constructing exotic SC sources, and opens up the territory of ionic quantum optics in the strong-field regime.
Coherent radiation at several wavelengths in the vacuum ultraviolet (VUV) has been generated by four-wave parametric oscillation in mercury vapor. When a powerful ultraviolet pump laser of frequency omega(p) is tuned to a two-photon resonance, VUV signal photons at frequency omega(s), as well as idler photons at frequency omega(i), are generated such that omega(s) + omega(i) = 2omega(p). A frequency-doubled dye laser tuned to two-photon resonance with the 6s6d(1)D(2) level near 280.3 nm produced output at 184.9 and 143.5 nm. A tunable krypton fluoride excimer laser tuned to two-photon resonance with the 6s10s (1)S(0) level near 248.7 nm produced output at 140.1, 130.7, 130.1, 125.9, and 125.0 nm. Approximately 1-microJ, 200-W pulses were observed at 143.5 and 125.9 nm.
We derive an analytical solution uncovering the origin of few-cycle attosecond pulse formation from vacuum-ultraviolet (VUV) radiation in an atomic gas simultaneously irradiated by a moderately strong infrared (IR) laser field, which does not perturb atoms in the ground state, but induces rapid quasistatic ionization from the excited states [Polovinkin et al., Opt. Lett. 36, 2296 (2011)]. The derived solution shows that the pulses are produced due to periodic switching of the resonant interaction between the incident VUV radiation and the atoms: turning it off near the crests of the IR-field strength and switching it back on near the IR-field zero crossings. We extend the method originally proposed by Polovinkin et al. [Opt. Lett. 36, 2296 (2011)] to non-hydrogen-like media and show that the pulses can be produced from resonant VUV radiation in a variety of atomic gases. The pulses are nearly bandwidth limited without external adjustment of phases of the generated sidebands. Proximity of the carrier frequency of the produced pulses to intra-atomic resonances may allow their efficient utilization for nondestructive steering of ultrafast dynamics of the bound electrons. The experimental possibilities for attosecond pulse formation from 58.4 nm VUV radiation in helium and from 73.6 nm VUV radiation in neon dressed by the 3.9 \ensuremath{\mu}m laser field, as well as from 122 nm VUV radiation in atomic hydrogen dressed by CO2\mathrm{C}{\mathrm{O}}_{2}CO2​-laser field are discussed.
A scheme is analyzed for effcient generation of vacuum ultraviolet radiation through four-wave mixing processes assisted by the technique of Stark-chirped rapid adiabatic passage. These opportunities are associated with pulse excitation of laddertype short-wavelength two-photon atomic or molecular transitions so that relaxation processes can be neglected. In this three-laser technique, a delayed-pulse of strong oR-resonant infrared radiation sweeps the laser-induced Stark-shift of a two-photon transition in a such way that facilitates robust maximum two-photon coherence induced by the first ultraviolet laser. A judiciously delayed third pulse scatters at this coherence and generates short-wavelength radiation. A theoretical analysis of these problems based on the density matrix is performed. A numerical model is developed to carry out simulations of a typical experiment. The results illustrate a behavior of populations, coherence and generated radiation along the medium as well as opportunities of effcient generation of deep (vacuum) ultraviolet radiation.
Coherent vacuum-ultraviolet (VUV) pulses with energy of 1.1 mJ, 2.2-nsec pulse length (2 MW cm−2 unfocused), and measured bandwidth ≤0.1 cm−1 have been achieved at 130 nm from four-wave mixing in Hg vapor. Conversion efficiencies of 5% have been demonstrated in a collimated beam geometry over 1-m interaction lengths. These high efficiencies are made possible by using two-photon-resonant sum-frequency mixing through the Hg 71S level. The experimental facility assembled to produce this efficient VUV source is described, and a comparison between experimental measurements and theory is provided.