1. High-speed ultrasensitive measurements of trace atmospheric species 250 spectra in 0.7 s David A. Long A. J. Fleisher, D. F. Plusquellic, J. T. Hodges ISMS 16 June 2014

2. Measurements with frequency-stabilized cavity ring-down spectroscopy (FS-CRDS) Hyperfine structure Measured CO 2, CO, H 2 O, O 2, CH 4 Line positions linked to OFC O 2 A-band line list for HITRAN Very powerful. But very slow. SNR=1,800,000:1

3. The problem frequency To record a spectrum you need to tune the laser frequency This generally requires thermal or mechanical tuning This is usually non-linear and very slow Things are even more difficult with cavity-enhanced spectroscopy (discrete frequencies)

4. One solution Stabilize the cavity’s length (actively or passively) This ensures we know exactly where the cavity mode are located Use an electro-optic modulator (EOM) to program the laser frequency We can do this with microwave-level accuracy These waveguide based devices are amazing: Very high bandwidth (up to 300 GHz!) Ultra-low insertion loss Very low V π (i.e. required microwave power) Very high efficiencies Fiber coupled

5. Frequency-agile, rapid scanning (FARS) spectroscopy Advantages: Overcomes slow mechanical and thermal scanning Links optical detuning axis link to radio-frequency (RF) standards Wide frequency tuning range (> 130 GHz = 4.3 cm -1 ) Method: Use waveguide electro-optic phase-modulator (EOM) to generate tunable sidebands Drive PM with a rapidly-switchable microwave (MW) source Fix carrier and use ring-down cavity to filter out all but one selected side band G.-W. Truong et al., Nature Photonics, (2013) MW source EOM cw laser ring-down cavity side-band spectrum Detector gas analyte

6. Very high acquisition rates: scanning No dead time due to tuning Rates as high as 8 kHz limited by cavity response time D. A. Long et al., Appl. Phys. B, (2013)

7. Lower finesse = faster rates D. A. Long et al., Appl. Phys. B, (2013) t = 30.85 ns  1.2 ns Finesse = 60 RD acq. rate = 5 MHz   /  = 4 % NEA = 1.9×10 -8 cm -1 Hz -1/2 Finesse = 20,000 RD acq. rate = 8 kHz   /  = 0.008 % NEA = 1.7×10 -12 cm -1 Hz -1/2 K. O. Douglass, JOSA B, (2013)

8. Even faster rates Use recently developed W-band modulators (bandwidth up to 300 GHz!) Image from Phase Sensitive Innovations

9. Even faster rates: single grating position Allows for a 130 GHz (4.3 cm -1) to be recorded in 3 s.

10. Even faster rates: grating tuning

11. Improving the sensitivity: Heterodyne measurements J. Ye and J. Hall., Phys. Rev. A, (2000) To do this we adapted the approach of Ye and Hall

12. Heterodyne measurements: Our approach D. A. Long, et al., Appl. Phys. B, (2014) Replace their two AOMs with a single EOM This enables rapid scanning Our approach also allows for a continuous lock (greatly reduces complexity)

13. Heterodyne measurements: Reaching the quantum-noise limit Utilized both a traditional InGaAs detector and an APD Able to reach the quantum-noise limit with the APD The traditional InGaAs allows for an NEA of 6E-14 cm -1 Hz -1/2 APDPIN D. A. Long, et al., Appl. Phys. B, (2014)

14. Most sensitive spectrometers TechniqueRef.Sensitivity (cm -1 Hz -1/2 ) Laser Tuning range (nm) NICE-OHMSYe et al.1E-14cw-Nd:YAG0.1 HD-CRDSLong et al.6E-14ECDL60 HD-CRDSYe and Hall3E-13cw-Yb:YAG~0.5 CRDSSpence et al.1E-12cw-Nd:YAG0.14 FARS-CRDSLong et al.2E-12ECDL60 NICE-OHMS Ehlers et al. 6E-12 Fiber laser1 D. A. Long et al., Appl. Phys. B, (2013) D. A. Long, et al., Appl. Phys. B, (2014)

15. Heterodyne measurements: Rapid scanning Able to record a 26 GHz-wide spectrum in 17 ms with 50 GS/s AWG Observed a weak CO 2 hot band transition in an air sample D. A. Long, et al., Appl. Phys. B, (2014)

16. Conclusions Presented two new techniques for rapid, ultrasensitive detection – Frequency-agile, rapid scanning (FARS) spectroscopy Use an EOM to step scan the laser frequency Scanning rates limited only by the cavity response time – Heterodyne-detected cavity ring-down spectroscopy (HD-CRDS) Make the measurement well above DC Leads to quantum-noise-limited sensitivity Does not compromise scanning rate

17. Acknowledgements Joseph Hodges, David Plusquellic, Adam Fleisher, Gar-Wing Truong, Szymon Wojtewicz, Katarzyna Bielska, Hong Lin, Zachary Reed, Kevin Douglass, Stephen Maxwell, Roger van Zee – NIST A NIST Innovations in Measurement Science (IMS) award The NIST Greenhouse Gas Measurements and Climate Research Program Always looking for good post-docs Email: David.Long@nist.gov

19. High accuracy of frequency axis-linked to OFC cavity dispersion g DD  40 fs 2 Absolute accuracy of 4 kHz Two measurements agree to within 4 Hz