www.sciencemag.org/cgi/content/full/science.aam7424/DC1

Supplementary Materials for

Dual-comb spectroscopy of water vapor with a free-running semiconductor disk laser

S. M. Link,* D. J. H. C. Maas, D. Waldburger, U. Keller

*Corresponding author. Email: slink@phys.ethz.ch

Published 11 May 2017 on Science First Release

DOI: 10.1126/science.aam7424

This PDF file includes:

Materials and Methods Figs. S1 to S3 Caption for Movie S1 References

Other Supplementary Materials for this manuscript includes the following: (available at www.sciencemag.org/cgi/content/full/science.aam7424/DC1)

Movie S1

Title: Dual-comb spectroscopy of water vapor with a free-running

semiconductor disk laser

S1 Materials and methods

S1.1 Experimental setup

The dual-comb MIXSEL benefits from the simple straight linear cavity. The linear cavity is

defined by the MIXSEL chip and an output coupler (radius of curvature 100 mm,

transmission 0.5%) as the two end mirrors (Fig. 2A). It is straightforward with this cavity design

to apply the concept of polarization duplexing by inserting a 2-mm thick, wedged birefringent

CaCO3 crystal into the cavity to split the one cavity beam into two cross-polarized and spatially

separated beams (13). Both cavity spots on the MIXSEL chip are pumped under an angle of 45°

with a commercial multimode pump diode at 808 nm, which is split with a 50:50 beam splitter

(BS). Both optical spectra are tuned with an intracavity etalon to a center wavelength of

968.3 nm to match an absorption line of water vapor. The pulse duration is 17.6 ps and 18.6 ps

and the average output power is 60 mW and 78 mW for the p- and s-polarized beam, respectively

(Fig S1). The temperature of the MIXSEL chip is kept constant with a Peltier element at 14 °C.

S1.2 Absorption calculation

The time-dependent interferograms (Fig S2) of the reference arm and the multi-pass cell arm are

recorded simultaneously with two photodetectors (PD1 and PD2) with a 5-GHz bandwidth and a

high-speed oscilloscope with a 1-GHz bandwidth. (Fig. 3A). The Fourier transformations of the

two time-dependent interferograms result in the two microwave combs (Fig. 3B) from which the

area below each peak is calculated with numeric integration. The absorption at each peak

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position Ai is then calculated by subtracting the area of the ith peak of the reference spectrum ai,ref

from the area of the corresponding peak in the spectrum measured with the multi-pass gas cell

ai,MPC. Dividing this value by ai,ref gives the absorption:

Ai =ai,ref − ai,MPC

ai,ref (S1)

The wavelength axis can be calibrated using the optical mode spacing and Δfrep. For the absolute

wavelength position one could take a single frequency laser with known frequency or an atomic

transition. Here we directly use the absorption line of water to calibrate the absolute wavelength,

which is a commonly used method for dual-comb spectroscopy. The microwave axis (Fig. 3B)

has to be inverted compared to the wavelength axis (Fig 3 C and D) in this case. This depends on

which of the two combs between DC and the pulse repetition rates (comb1 or comb2 in Fig. 2A)

have been used for the measurement because they mirror each other. Measuring the comb at

lower microwave frequencies is preferred, since less bandwidth is required for the PDs and the

oscilloscope. The HITRAN simulation is calculate with the HITRAN database taking the

temperature, pressure, relative humidity and path length as input parameters (Fig. 3C and D).

S1.3 Full stabilization of the microwave comb

Stabilizing only a single line of the microwave comb is not sufficient to stabilize the full comb

since it depends on two parameters: the difference in repetition rate Δfrep and the difference in

carrier envelope offset (CEO) frequency ΔfCEO. Therefore two feedback loops are required. The

comb lines are a result of the beating of the optical modes of the two combined collinear OFCs.

The red line (Fig. 4b) fred is given by

fred = N2 ⋅ frep,2 + fCEO,2( )− N1 ⋅ frep,1 + fCEO,1( ) ≈ const , (S2)

3

where N1 and N2 are integers. This beat frequency is kept constant within the limits of the

feedback loop. The expression can be re-written as

fred = ΔfCEO + N2 − N1( ) ⋅ frep,1 + N2 ⋅ Δfrep ≈ const . (S3)

with Δfrep given by

Δfrep = frep,2 − frep,1 (S4)

and ΔfCEO described by

ΔfCEO = fCEO,2 − fCEO,1 . (S5)

The green line (Fig. 4b) fgreen of the comb is given by

fgreen = N2 +m( ) ⋅ frep,2 + fCEO,2( )− N1 +m( ) ⋅ frep,1 + fCEO,1( ) , (S6)

where m is an integer counting the number of lines between the red and the green line. We can

re-write fgreen and express it as a function of fred,

fgreen = ΔfCEO + N2 − N1( ) ⋅ frep,1 + N2 ⋅ Δfrep +m ⋅ Δfrep = fred +m ⋅ Δfrep ≈ const +m ⋅ Δfrep (S7)

from which we can conclude that in order to stabilize the green line, we need to stabilize both

Δfrep and one comb line, which are directly detected with PD3 and PD4 (Fig. 4A). We use PD3

and PD4 to obtain a better signal-to-noise ratio, but in principle it would also be sufficient to take

the signal from PD1 for the stabilization and therefore only use two detectors in total. Since Eq.

(S7) is true for any integer m, it is true for all microwave comb lines and therefore the full comb

is stabilized simultaneously when both feedback loops are applied.

Even though the microwave comb is fully stabilized, both optical spectra could fluctuate the

same amount in the same direction, e.g. if the two CEO frequencies are changing by the exact

4

same amount, which would not be visible in the microwave spectrum and accordingly could not

be prevented by the two feedback loops. Therefore, we characterize the absolute stability of the

modes of the optical frequency combs as well (Fig. S3) (Fig 4D).

Fig. S1 Second-harmonic autocorrelation of the two cross-polarized laser beams.

Fig. S2 Signal from optical interference of the two combined OFCs recorded with the PD in the

time domain showing time-dependent interferograms over a time span of 1 ms and 0.8 µs.

Whenever one pulse of each OFC hits the detector at the same time a strong burst peak is

recorded. The bursts are repeated every 0.25 µs, corresponding to the inverse of the difference in

pulse repetition rate Δfrep of 4 MHz.

1.0

0.8

0.6

0.4

0.2

0.050-50

delay [ps]

!p= 18.6 ps

1.0

0.8

0.6

0.4

0.2

0.0

auto

corre

latio

n [a

rb. u

.]

50-50delay [ps]

meas. sech2 fit

!p=17.6 ps

1.0

0.8

0.6

0.4

0.2

0.0

auto

corre

latio

n [a

rb. u

.]

-50 0 50delay [ps]

meas. sech2 fit

0.80.60.40.20.0time [us]

!T= 0.24 !s

8004000time [us]

60

40

20

0

-20

-40

volta

ge [m

V]

5

Fig. S3 Measurement setup for the absolute stability of the optical modes of one of the two

optical frequency combs (OFCs). A commercial highly stable single frequency laser (Toptica DL

pro) is used to generate a beat frequency with one of the modes of one OFC on the photo

detector (PD). This beat frequency is measured with a microwave spectrum analyzer (MSA) and

a frequency counter. To make sure that the measurement is not limited by the fluctuations of the

single frequency laser, its frequency is characterized with a wavelength meter. PBS polarizing

beam splitter (polarizer axis turned such that the OFCs are spatially separated), FC fiber

coupling.

Movie S1 Dual-comb spectroscopy demonstration of water vapor with the free-running dual-

comb MIXSEL in the laboratory. The laser cavity is shown during operation.

PBS

pumpdiode

MSA / frequencycounter PD

single frequency laser wavelength

meter

FCdual-combMIXSEL

6

7

References and Notes 1. L.-S. Ma, Z. Bi, A. Bartels, L. Robertsson, M. Zucco, R. S. Windeler, G. Wilpers, C. Oates, L.

Hollberg, S. A. Diddams, Optical frequency synthesis and comparison with uncertainty at the 10–19 level. Science 303, 1843–1845 (2004). doi:10.1126/science.1095092 Medline

2. H. R. Telle, G. Steinmeyer, A. E. Dunlop, J. Stenger, D. H. Sutter, U. Keller, Carrier-envelope offset phase control: A novel concept for absolute optical frequency measurement and ultrashort pulse generation. Appl. Phys. B 69, 327–332 (1999). doi:10.1007/s003400050813

3. D. J. Jones, S. A. Diddams, J. K. Ranka, A. Stentz, R. S. Windeler, J. L. Hall, S. T. Cundiff, Carrier-envelope phase control of femtosecond mode-locked lasers and direct optical frequency synthesis. Science 288, 635–640 (2000). doi:10.1126/science.288.5466.635 Medline

4. A. Apolonski, A. Poppe, G. Tempea, C. Spielmann, T. Udem, R. Holzwarth, T. W. Hänsch, F. Krausz, Controlling the phase evolution of few-cycle light pulses. Phys. Rev. Lett. 85, 740–743 (2000). doi:10.1103/PhysRevLett.85.740 Medline

5. P. Del’Haye, A. Schliesser, O. Arcizet, T. Wilken, R. Holzwarth, T. J. Kippenberg, Optical frequency comb generation from a monolithic microresonator. Nature 450, 1214–1217 (2007). doi:10.1038/nature06401 Medline

6. J. Li, H. Lee, T. Chen, K. J. Vahala, Low-pump-power, low-phase-noise, and microwave to millimeter-wave repetition rate operation in microcombs. Phys. Rev. Lett. 109, 233901 (2012). doi:10.1103/PhysRevLett.109.233901 Medline

D. Cotter, “Technique for highly stable active mode-locking,” in Ultrafast Phenomena IV, D. H. Auston, K. B. Eisenthal, Eds. (Springer Series in Chemical Physics, Springer, 1984), vol. 38, pp. 78–80.

8. M. J. W. Rodwell, D. M. Bloom, K. J. Weingarten, Subpicosecond laser timing stabilization. IEEE J. Quantum Electron. 25, 817–827 (1989). doi:10.1109/3.17346

9. A. Klenner, S. Schilt, T. Südmeyer, U. Keller, Gigahertz frequency comb from a diode-pumped solid-state laser. Opt. Express 22, 31008–31019 (2014). doi:10.1364/OE.22.031008 Medline

10. I. Hartl, H. A. McKay, R. Thapa, B. K. Thomas, J. Dong, M. E. Ferman, “GHz Yb-femtosecond-fiber laser frequency comb,” paper presented at the Conference on Lasers and Electro-Optics (CLEO), CMN1, San Jose, CA, 2009.

11. A. Bartels, D. Heinecke, S. A. Diddams, 10-GHz self-referenced optical frequency comb. Science 326, 681 (2009). doi:10.1126/science.1179112 Medline

12. D. J. H. C. Maas, A.-R. Bellancourt, B. Rudin, M. Golling, H. J. Unold, T. Südmeyer, U. Keller, Vertical integration of ultrafast semiconductor lasers. Appl. Phys. B 88, 493–497 (2007). doi:10.1007/s00340-007-2760-1

13. S. M. Link, A. Klenner, M. Mangold, C. A. Zaugg, M. Golling, B. W. Tilma, U. Keller, Dual-comb modelocked laser. Opt. Express 23, 5521–5531 (2015). doi:10.1364/OE.23.005521 Medline

8

14. U. Keller, A. C. Tropper, Passively modelocked surface-emitting semiconductor lasers. Phys. Rep. 429, 67–120 (2006). doi:10.1016/j.physrep.2006.03.004

15. N. Schulz, J. M. Hopkins, M. Rattunde, D. Burns, J. Wagner, High-brightness longwavelength semiconductor disk lasers. Laser Photonics Rev. 2, 160–181 (2008). doi:10.1002/lpor.200710037

16. M. Guina, A. Härkönen, V.-M. Korpijärvi, T. Leinonen, S. Suomalainen, Semiconductor disk lasers: Recent advances in generation of yellow-orange and mid-IR radiation. Adv. Opt. Technol. 2012, 265010 (2012). doi:10.1155/2012/265010

17. B. W. Tilma, M. Mangold, C. A. Zaugg, S. M. Link, D. Waldburger, A. Klenner, A. S. Mayer, E. Gini, M. Golling, U. Keller, Recent advances in ultrafast semiconductor disk lasers. Light Sci. Appl. 4, e310 (2015). doi:10.1038/lsa.2015.83

18. A. Rahimi-Iman, Recent advances in VECSELs. J. Opt. 18, 093003 (2016). doi:10.1088/2040-8978/18/9/093003

19. M. A. Gaafar, A. Rahimi-Iman, K. A. Fedorova, W. Stolz, E. U. Rafailov, M. Koch, Mode-locked semiconductor disk lasers. Adv. Opt. Photonics 8, 370–400 (2016). doi:10.1364/AOP.8.000370

20. S. Schiller, Spectrometry with frequency combs. Opt. Lett. 27, 766–768 (2002). doi:10.1364/OL.27.000766 Medline

21. I. Coddington, N. Newbury, W. Swann, Dual-comb spectroscopy. Optica 3, 414–426 (2016). doi:10.1364/OPTICA.3.000414

22. A. Bartels, R. Cerna, C. Kistner, A. Thoma, F. Hudert, C. Janke, T. Dekorsy, Ultrafast time-domain spectroscopy based on high-speed asynchronous optical sampling. Rev. Sci. Instrum. 78, 035107 (2007). doi:10.1063/1.2714048 Medline

23. I. Coddington, W. C. Swann, L. Nenadovic, N. R. Newbury, Rapid and precise absolute distance measurements at long range. Nat. Photonics 3, 351–356 (2009). doi:10.1038/nphoton.2009.94

24. K. O. Hill, Y. Fujii, D. C. Johnson, B. S. Kawasaki, Photosensitivity in optical fiber waveguides: Application to reflection filter fabrication. Appl. Phys. Lett. 32, 647–649 (1978). doi:10.1063/1.89881

25. T. Ideguchi, A. Poisson, G. Guelachvili, N. Picqué, T. W. Hänsch, Adaptive real-time dual-comb spectroscopy. Nat. Commun. 5, 3375 (2014). doi:10.1038/ncomms4375 Medline

26. Y. Liu, X. Zhao, G. Hu, C. Li, B. Zhao, Z. Zheng, Unidirectional, dual-comb lasing under multiple pulse formation mechanisms in a passively mode-locked fiber ring laser. Opt. Express 24, 21392–21398 (2016). doi:10.1364/OE.24.021392 Medline

27. M.-G. Suh, Q.-F. Yang, K. Y. Yang, X. Yi, K. J. Vahala, Microresonator soliton dual-comb spectroscopy. Science 354, 600–603 (2016). doi:10.1126/science.aah6516 Medline

28. T. Yasui, R. Ichikawa, Y.-D. Hsieh, K. Hayashi, H. Cahyadi, F. Hindle, Y. Sakaguchi, T. Iwata, Y. Mizutani, H. Yamamoto, K. Minoshima, H. Inaba, Adaptive sampling dual terahertz comb spectroscopy using dual free-running femtosecond lasers. Sci. Rep. 5, 10786 (2015). doi:10.1038/srep10786 Medline

9

29. C. E. Shannon, Communication in the presence of noise. Proc. IEEE 86, 447–457 (1998) [reprinted from Proc. IRE 37, 10–21 (1949)]. doi:10.1109/JPROC.1998.659497

30. M. Mangold, C. A. Zaugg, S. M. Link, M. Golling, B. W. Tilma, U. Keller, Pulse repetition rate scaling from 5 to 100 GHz with a high-power semiconductor disk laser. Opt. Express 22, 6099–6107 (2014). doi:10.1364/OE.22.006099 Medline

31. T. J. Kippenberg, R. Holzwarth, S. A. Diddams, Microresonator-based optical frequency combs. Science 332, 555–559 (2011). doi:10.1126/science.1193968 Medline

32. G. Villares, A. Hugi, S. Blaser, J. Faist, Dual-comb spectroscopy based on quantum-cascade-laser frequency combs. Nat. Commun. 5, 5192 (2014). doi:10.1038/ncomms6192 Medline

33. G. Villares, J. Wolf, D. Kazakov, M. J. Süess, A. Hugi, M. Beck, J. Faist, On-chip dual-comb based on quantum cascade laser frequency combs. Appl. Phys. Lett. 107, 251104 (2015). doi:10.1063/1.4938213

34. M. Mangold, S. M. Link, A. Klenner, C. A. Zaugg, M. Golling, B. W. Tilma, U. Keller, Amplitude noise and timing jitter characterization of a high-power mode-locked integrated external-cavity surface emitting laser. IEEE Photonics J. 6, 1–9 (2014). doi:10.1109/JPHOT.2013.2295464

35. S. M. Link, A. Klenner, U. Keller, Dual-comb modelocked lasers: Semiconductor saturable absorber mirror decouples noise stabilization. Opt. Express 24, 1889–1902 (2016). doi:10.1364/OE.24.001889 Medline

36. Materials and methods are available as supplementary materials.

37. L. S. Rothman, I. E. Gordon, Y. Babikov, A. Barbe, D. Chris Benner, P. F. Bernath, M. Birk, L. Bizzocchi, V. Boudon, L. R. Brown, A. Campargue, K. Chance, E. A. Cohen, L. H. Coudert, V. M. Devi, B. J. Drouin, A. Fayt, J.-M. Flaud, R. R. Gamache, J. J. Harrison, J.-M. Hartmann, C. Hill, J. T. Hodges, D. Jacquemart, A. Jolly, J. Lamouroux, R. J. Le Roy, G. Li, D. A. Long, O. M. Lyulin, C. J. Mackie, S. T. Massie, S. Mikhailenko, H. S. P. Müller, O. V. Naumenko, A. V. Nikitin, J. Orphal, V. Perevalov, A. Perrin, E. R. Polovtseva, C. Richard, M. A. H. Smith, E. Starikova, K. Sung, S. Tashkun, J. Tennyson, G. C. Toon, V. G. Tyuterev, G. Wagner, The HITRAN2012 molecular spectroscopic database. J. Quant. Spectrosc. Radiat. Transf. 130, 4–50 (2013). doi:10.1016/j.jqsrt.2013.07.002

38. P. J. Schroeder, R. J. Wright, S. Coburn, B. Sodergren, K. C. Cossel, S. Droste, G. W. Truong, E. Baumann, F. R. Giorgetta, I. Coddington, N. R. Newbury, G. B. Rieker, Dual frequency comb laser absorption spectroscopy in a 16 MW gas turbine exhaust. Proc. Combust. Inst. 36, 4565–4573 (2017). doi:10.1016/j.proci.2016.06.032

39. G. Vicidomini, G. Moneron, K. Y. Han, V. Westphal, H. Ta, M. Reuss, J. Engelhardt, C. Eggeling, S. W. Hell, Sharper low-power STED nanoscopy by time gating. Nat. Methods 8, 571–573 (2011). doi:10.1038/nmeth.1624 Medline

40. C. A. Zaugg, S. Gronenborn, H. Moench, M. Mangold, M. Miller, U. Weichmann, W. P. Pallmann, M. Golling, B. W. Tilma, U. Keller, Absorber and gain chip optimization to improve performance from a passively modelocked electrically pumped vertical external

10

cavity surface emitting laser. Appl. Phys. Lett. 104, 121115 (2014). doi:10.1063/1.4870048

41. D. Waldburger, S. M. Link, M. Mangold, C. G. E. Alfieri, E. Gini, M. Golling, B. W. Tilma, U. Keller, High-power 100 fs semiconductor disk lasers. Optica 3, 844–852 (2016). doi:10.1364/OPTICA.3.000844