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P. Maddaloni National Institute for Applied Optics, Naples (Italy)

High-resolution and high-sensitivity spectroscopy of methane by means of a mW-power DFG spectrometer around 3.3 m m. P. Maddaloni National Institute for Applied Optics, Naples (Italy). CLEO Europe – EQEC Munich, 12-17 June 2005. Outline. INTRODUCTION The experimental apparatus

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P. Maddaloni National Institute for Applied Optics, Naples (Italy)

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  1. High-resolution and high-sensitivity spectroscopy of methane by means of amW-power DFG spectrometer around 3.3 mm P. Maddaloni National Institute for Applied Optics, Naples (Italy) CLEO Europe – EQEC Munich, 12-17 June 2005

  2. Outline INTRODUCTION The experimental apparatus Characterization of the source • METHANE SPECTROSCOPY • High resolution • Saturated absorption spectroscopy • High sensitivity • ICOS with a high-finesse cavity in off-axis configuration

  3. Motivations BS Laser 1 Crystal Laser 2 M • Most molecular species exhibit very strong ro-vibrational transitions between 2.9 and 3.5 mm  • high sensitivity • lower saturation intensities (frequency-reference grid) Wide tunability Mode-hop-free operation Narrow linewidth periodically poled crystals  much more efficient conversion

  4. The main ingredients • PUMP SOURCE • ECDL (few mW) + Yb fiber amplifier: 1026-1070 nm; up to 700mW; <1 MHz linewidth • Coarse tuning by diffraction grating • Temperature tuning: 0.3 nm/K • PZT: 300 MHz/V • SIGNAL SOURCE • Erbium fiber laser: 1545-1605 nm; up to 5W; <1 MHz linewidth • Coarse tuning: 0.8 nm step MULTIPLE CHANNEL PPLN L=29.6–30.6 mm; T=50-68 °C l=5 cm; h=w=1 mm IDLER RADIATION2.9-3.5 mm

  5. InSb detector InSb array 320*256 30-mm pixel The DFG set-up idler beam

  6. Characterization of the spectrometer • Control of the spatial beam profile  • efficient coupling to high-finesse cavities • excitation of very narrow transitions

  7. Sub-Doppler spectroscopy of methane pump beam 2.5 mW probe beam 1.4 mW dia. = 1 mm G = 1 MHz d = 2.86E-31 C·m  Is = 1 mW/mm2 P = 30 mTorr (L = 50 cm)

  8. Results n3 stretching mode phase-sensitive detection Fm = 3.5 kHz, Am = 5 MHz det. BW = 40 Hz R(4) E 3067.2344 cm-1 R(4) F1(2) 3067.2610 cm-1 S = 4% FWHM = 2.5  0.5 MHz det. BW = 1 kHz DFG emission linewidth pressure broad.  200 kHz transit-time broad.  500 kHz

  9. High-sensitivity spectroscopy RESONANT-COUPLING METHODS (ON-AXIS ALIGNMENT) lock the laser to a single resonance mode of the cavity decrease in FSR (extremely dense-mode spectrum)  cavity transmission very effectively averaged OFF-AXIS ALIGNMENT “transmission is frequency independent (solely determined by the round-trip cavity loss)” • Advantages • no need for complex components and sub-ms time-resolved measurement • lower sensitivity to vibration and misalignment •  in-situ trace-gas monitoring Drawbacks lower power transmission  a higher power is required

  10. ICOS set-up R = 99.95% (r = 6 m) Leff = d/(1-R) = 2 km

  11. FSRoff = FSRon/nre nre = 11.07 Off-axis cavity transmission scan interval=400 ms transmission exhibits large peak-to-peak intensity fluctuations FSR=15 MHz • reduce scan interval (4 ms) • modulate laser frequency (Am = 25 MHz, Fm = 10 kHz) • modulate cavity length (Am = 4.5 GHz, Fm = 410 Hz) intensity fluctuations are dramatically reduced by time-integration (det. BW = 6 Hz)

  12. CH3D CH4 Absorption spectra isotope detection in pure methane 2960.617586 cm-1; 2960.655300 cm-1 a(CH4) = 3.410-5 cm-1torr-1 P = 0.1 torr det. BW = 6 Hz acquisition time = 4 s

  13. P=1 atm P=50 Torr det. BW = 6 Hz acquisition time = 4 s nmin = 1 ppb/Hz Absorption spectra methane detection in ambient-air (n = 2 ppm) n = 2943.107924 cm-1 ; S = 8.410-20 cm/mol

  14. Conclusions and perspectives Sub-Doppler spectroscopy of methane Absolute frequency measurements (phase-lock to “Comb”) Cavity enhanced spectroscopy isotope detection in pure methane detection of methane in ambient-air WM and/or two-tone FM spectroscopy Portable all-fiber MIRTuS Sensing in liquid samples by fiber-loop ring-down spectroscopy

  15. National Institute for Applied Optics Laboratory team G. Gagliardi research scientist P. Malara PhD student P. De Natale research director P. Maddaloni research scientist

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