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Title: Super-octave longwave mid-infrared coherent transients produced by optical rectification of few-cycle 25-μm pulses

Abstract

Femtosecond laser sources and optical frequency combs in the molecular fingerprint region of the electromagnetic spectrum are crucial for a plethora of applications in natural and life sciences. Here we introduce Cr2+-based lasers as a convenient means for producing super-octave mid-IR electromagnetic transients via optical rectification (or intra-pulse difference frequency generation, IDFG). We demonstrate that a relatively long, 2.5 μm, central wavelength of a few-cycle Cr2+:ZnS driving source (20 fs pulse duration, 6 W average power, 78 MHz repetition rate) enabled the use of highly nonlinear ZnGeP2 crystal for IDFG with exceptionally high conversion efficiency (>3%) and output power of 0.15 W, with the spectral span of 5.8–12.5 μm. Even broader spectrum was achieved in GaSe crystal: 4.3–16.6 μm for type I and 5.8–17.6 μm for type II phase matching. The results highlight the potential of this architecture for ultrafast spectroscopy and generation of broadband frequency combs in the longwave infrared.

Authors:
; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Univ. of Alabama, Birmingham, AL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); US Department of the Navy, Office of Naval Research (ONR); Defense Advanced Research Projects Agency (DARPA)
OSTI Identifier:
1490922
Alternate Identifier(s):
OSTI ID: 1612965
Grant/Contract Number:  
SC0018378
Resource Type:
Published Article
Journal Name:
Optica
Additional Journal Information:
Journal Name: Optica Journal Volume: 6 Journal Issue: 1; 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; Optics

Citation Formats

Vasilyev, Sergey, Moskalev, Igor S., Smolski, Viktor O., Peppers, Jeremy M., Mirov, Mike, Muraviev, Andrey V., Zawilski, Kevin, Schunemann, Peter G., Mirov, Sergey B., Vodopyanov, Konstantin L., and Gapontsev, Valentin P. Super-octave longwave mid-infrared coherent transients produced by optical rectification of few-cycle 25-μm pulses. United States: N. p., 2019. Web. https://doi.org/10.1364/OPTICA.6.000111.
Vasilyev, Sergey, Moskalev, Igor S., Smolski, Viktor O., Peppers, Jeremy M., Mirov, Mike, Muraviev, Andrey V., Zawilski, Kevin, Schunemann, Peter G., Mirov, Sergey B., Vodopyanov, Konstantin L., & Gapontsev, Valentin P. Super-octave longwave mid-infrared coherent transients produced by optical rectification of few-cycle 25-μm pulses. United States. https://doi.org/10.1364/OPTICA.6.000111
Vasilyev, Sergey, Moskalev, Igor S., Smolski, Viktor O., Peppers, Jeremy M., Mirov, Mike, Muraviev, Andrey V., Zawilski, Kevin, Schunemann, Peter G., Mirov, Sergey B., Vodopyanov, Konstantin L., and Gapontsev, Valentin P. Thu . "Super-octave longwave mid-infrared coherent transients produced by optical rectification of few-cycle 25-μm pulses". United States. https://doi.org/10.1364/OPTICA.6.000111.
@article{osti_1490922,
title = {Super-octave longwave mid-infrared coherent transients produced by optical rectification of few-cycle 25-μm pulses},
author = {Vasilyev, Sergey and Moskalev, Igor S. and Smolski, Viktor O. and Peppers, Jeremy M. and Mirov, Mike and Muraviev, Andrey V. and Zawilski, Kevin and Schunemann, Peter G. and Mirov, Sergey B. and Vodopyanov, Konstantin L. and Gapontsev, Valentin P.},
abstractNote = {Femtosecond laser sources and optical frequency combs in the molecular fingerprint region of the electromagnetic spectrum are crucial for a plethora of applications in natural and life sciences. Here we introduce Cr2+-based lasers as a convenient means for producing super-octave mid-IR electromagnetic transients via optical rectification (or intra-pulse difference frequency generation, IDFG). We demonstrate that a relatively long, 2.5 μm, central wavelength of a few-cycle Cr2+:ZnS driving source (20 fs pulse duration, 6 W average power, 78 MHz repetition rate) enabled the use of highly nonlinear ZnGeP2 crystal for IDFG with exceptionally high conversion efficiency (>3%) and output power of 0.15 W, with the spectral span of 5.8–12.5 μm. Even broader spectrum was achieved in GaSe crystal: 4.3–16.6 μm for type I and 5.8–17.6 μm for type II phase matching. The results highlight the potential of this architecture for ultrafast spectroscopy and generation of broadband frequency combs in the longwave infrared.},
doi = {10.1364/OPTICA.6.000111},
journal = {Optica},
number = 1,
volume = 6,
place = {United States},
year = {2019},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1364/OPTICA.6.000111

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Cited by: 15 works
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Works referenced in this record:

Mid-Infrared Time-Resolved Frequency Comb Spectroscopy of Transient Free Radicals
journal, June 2014

  • Fleisher, Adam J.; Bjork, Bryce J.; Bui, Thinh Q.
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 13
  • DOI: 10.1021/jz5008559

Ultrafast Dynamics of Surface Plasmons in InAs by Time-Resolved Infrared Nanospectroscopy
journal, July 2014

  • Wagner, Martin; McLeod, Alexander S.; Maddox, Scott J.
  • Nano Letters, Vol. 14, Issue 8
  • DOI: 10.1021/nl501558t

47-fs Kerr-lens mode-locked Cr:ZnSe laser with high spectral purity
journal, January 2017

  • Wang, Yuchen; Fernandez, Toney T.; Coluccelli, Nicola
  • Optics Express, Vol. 25, Issue 21
  • DOI: 10.1364/OE.25.025193

Frontiers of Mid-IR Lasers Based on Transition Metal Doped Chalcogenides
journal, September 2018

  • Mirov, Sergey B.; Moskalev, Igor S.; Vasilyev, Sergey
  • IEEE Journal of Selected Topics in Quantum Electronics, Vol. 24, Issue 5
  • DOI: 10.1109/JSTQE.2018.2808284

Multi-watt, multi-octave, mid-infrared femtosecond source
journal, April 2018


Generation of ultrabroadband femtosecond pulses in the mid‐infrared by optical rectification of 15 fs light pulses at 100 MHz repetition rate
journal, November 1995

  • Bonvalet, A.; Joffre, M.; Martin, J. L.
  • Applied Physics Letters, Vol. 67, Issue 20
  • DOI: 10.1063/1.114838

Mid-infrared supercontinuum covering the 1.4–13.3 μm molecular fingerprint region using ultra-high NA chalcogenide step-index fibre
journal, September 2014

  • Petersen, Christian Rosenberg; Møller, Uffe; Kubat, Irnis
  • Nature Photonics, Vol. 8, Issue 11
  • DOI: 10.1038/nphoton.2014.213

Molecular fingerprinting with bright, broadband infrared frequency combs
journal, January 2018


High-brightness table-top hard X-ray source driven by sub-100-femtosecond mid-infrared pulses
journal, November 2014


Characterization of high-harmonic emission from ZnO up to 11  eV pumped with a Cr:ZnS high-repetition-rate source
journal, January 2019

  • Vampa, Giulio; Vasilyev, Sergey; Liu, Hanzhe
  • Optics Letters, Vol. 44, Issue 2
  • DOI: 10.1364/OL.44.000259

Generation and field-resolved detection of femtosecond electromagnetic pulses tunable up to 41 THz
journal, May 2000

  • Huber, R.; Brodschelm, A.; Tauser, F.
  • Applied Physics Letters, Vol. 76, Issue 22
  • DOI: 10.1063/1.126625

Coherence properties of a 26–75  μm frequency comb produced as a subharmonic of a Tm-fiber laser
journal, January 2016

  • Smolski, V. O.; Yang, H.; Gorelov, S. D.
  • Optics Letters, Vol. 41, Issue 7
  • DOI: 10.1364/OL.41.001388

Multi-mW, few-cycle mid-infrared continuum spanning from 500 to 2250 cm−1
journal, December 2017

  • Zhang, Jinwei; Fai Mak, Ka; Nagl, Nathalie
  • Light: Science & Applications, Vol. 7, Issue 2
  • DOI: 10.1038/lsa.2017.180

Cascaded half-harmonic generation of femtosecond frequency combs in the mid-infrared
journal, January 2016


Watt-scale super-octave mid-infrared intrapulse difference frequency generation
journal, November 2018

  • Gaida, Christian; Gebhardt, Martin; Heuermann, Tobias
  • Light: Science & Applications, Vol. 7, Issue 1
  • DOI: 10.1038/s41377-018-0099-5

Midinfrared frequency comb from self-stable degenerate GaAs optical parametric oscillator
journal, January 2015


Parametric generation of tunable infrared radiation in ZnGeP_2 and GaSe pumped at 3 μm
journal, January 1993


Nano-FTIR Absorption Spectroscopy of Molecular Fingerprints at 20 nm Spatial Resolution
journal, July 2012

  • Huth, Florian; Govyadinov, Alexander; Amarie, Sergiu
  • Nano Letters, Vol. 12, Issue 8
  • DOI: 10.1021/nl301159v

Characterization of the noise in continuously operating mode-locked lasers
journal, April 1986


Massively parallel sensing of trace molecules and their isotopologues with broadband subharmonic mid-infrared frequency combs
journal, March 2018


Gate-tuning of graphene plasmons revealed by infrared nano-imaging
journal, June 2012


Three optical cycle mid-IR Kerr-lens mode-locked polycrystalline Cr^2+:ZnS laser
journal, January 2015

  • Vasilyev, Sergey; Moskalev, Igor; Mirov, Mike
  • Optics Letters, Vol. 40, Issue 21
  • DOI: 10.1364/OL.40.005054

Mid-IR Kerr-lens mode-locked polycrystalline Cr:ZnS and Cr:ZnSe lasers with intracavity frequency conversion via random quasi-phase-matching
conference, March 2016

  • Vasilyev, Sergey; Moskalev, Igor; Mirov, Mike
  • SPIE LASE, SPIE Proceedings
  • DOI: 10.1117/12.2218356

Half-Watt average power femtosecond source spanning 3–8 µm based on subharmonic generation in GaAs
journal, May 2018


Ultrafast middle-IR lasers and amplifiers based on polycrystalline Cr:ZnS and Cr:ZnSe
journal, January 2017

  • Vasilyev, Sergey; Moskalev, Igor; Mirov, Mike
  • Optical Materials Express, Vol. 7, Issue 7
  • DOI: 10.1364/OME.7.002636

Broadband phase-matched difference frequency mixing of femtosecond pulses in GaSe: Experiment and theory
journal, August 1999

  • Kaindl, R. A.; Eickemeyer, F.; Woerner, M.
  • Applied Physics Letters, Vol. 75, Issue 8
  • DOI: 10.1063/1.124596

High-power sub-two-cycle mid-infrared pulses at 100 MHz repetition rate
journal, September 2015


    Works referencing / citing this record:

    Complementary vibrational spectroscopy
    journal, September 2019

    • Hashimoto, Kazuki; Badarla, Venkata Ramaiah; Kawai, Akira
    • Nature Communications, Vol. 10, Issue 1
    • DOI: 10.1038/s41467-019-12442-9

    Multi-octave spanning, Watt-level ultrafast mid-infrared source
    journal, October 2019


    Multi-octave visible to long-wave IR femtosecond continuum generated in Cr:ZnS-GaSe tandem
    journal, January 2019

    • Vasilyev, Sergey; Moskalev, Igor; Smolski, Viktor
    • Optics Express, Vol. 27, Issue 11
    • DOI: 10.1364/oe.27.016405

    Octave-spanning single-cycle middle-infrared generation through optical parametric amplification in LiGaS 2
    journal, January 2019

    • Chen, Bo-Han; Wittmann, Emanuel; Morimoto, Yuya
    • Optics Express, Vol. 27, Issue 15
    • DOI: 10.1364/oe.27.021306

    Directly diode-pumped, Kerr-lens mode-locked, few-cycle Cr:ZnSe oscillator
    journal, January 2019

    • Nagl, Nathalie; Gröbmeyer, Sebastian; Pervak, Vladimir
    • Optics Express, Vol. 27, Issue 17
    • DOI: 10.1364/oe.27.024445

    Middle-IR frequency comb based on Cr:ZnS laser
    journal, January 2019

    • Vasilyev, Sergey; Smolski, Viktor; Peppers, Jeremy
    • Optics Express, Vol. 27, Issue 24
    • DOI: 10.1364/oe.27.035079

    Towards high power longwave mid-IR frequency combs: power scalability of high repetition-rate difference-frequency generation
    journal, January 2020

    • Cao, Qian; Kärtner, Franz X.; Chang, Guoqing
    • Optics Express, Vol. 28, Issue 2
    • DOI: 10.1364/oe.28.001369

    Mid-infrared frequency comb with 67 W average power based on difference frequency generation
    journal, January 2020

    • Catanese, Anthony; Rutledge, Jay; Silfies, Myles C.
    • Optics Letters, Vol. 45, Issue 5
    • DOI: 10.1364/ol.385294

    Broadband mid-infrared coverage (2–17  μm) with few-cycle pulses via cascaded parametric processes
    journal, January 2019

    • Wang, Qing; Zhang, Jinwei; Kessel, Alexander
    • Optics Letters, Vol. 44, Issue 10
    • DOI: 10.1364/ol.44.002566

    Intra-pulse difference-frequency generation of mid-infrared (27–20  μm) by random quasi-phase-matching
    journal, January 2019

    • Zhang, Jinwei; Fritsch, Kilian; Wang, Qing
    • Optics Letters, Vol. 44, Issue 12
    • DOI: 10.1364/ol.44.002986

    Table-top high-energy 7  μm OPCPA and 260  mJ Ho:YLF pump laser
    journal, January 2019


    Broadband dispersive Ge/YbF 3 mirrors for mid-infrared spectral range
    journal, January 2019

    • Amotchkina, Tatiana; Trubetskov, Michael; Hussain, Syed Ali
    • Optics Letters, Vol. 44, Issue 21
    • DOI: 10.1364/ol.44.005210

    Dioxin and Related Compound Detection: Perspectives for Optical Monitoring
    journal, May 2019

    • Patrizi, Barbara; Siciliani de Cumis, Mario; Viciani, Silvia
    • International Journal of Molecular Sciences, Vol. 20, Issue 11
    • DOI: 10.3390/ijms20112671