Todays timeresolved spectroscopy FTIR Typical stepscan FTIR measurement

Single-shot sub-microsecond mid-infrared spectroscopy with quantum cascade laser frequency combs Markus Mangold Jessica Klocke,

IRsweep products IRcell IRis-F 1 10 cm Markus Mangold| info@irsweep. com | 21/05/2021 |

IRis-F 1 High-Speed Observe fast processes Single-shot IRis-F 1 Easier measurements / sample low

Available time-resolved methods: step-scan, rapid scan, tunable laser spectroscopy Step-scan FTIR Rapid-scan FTIR Tunable

IRis-F 1: Dual-comb spectrometer using quantum cascade lasers § Quantum cascade laser frequency combs

IRis-F 1: Dual-comb spectrometer using quantum cascade lasers Two frequency combs superimposed Direct optical

Quantum cascade laser frequency comb emission High power lasers • Up to 1 W

IRis-F 1: Dual-comb spectrometer using quantum cascade lasers • Large repetition rate • Large

IRis-F 1: Signal-to-noise ratio µOD absorbance noise levels with µs time resolution Markus Mangold

Bacteriorhodopsin: IRis-F 1 experimental setup Schematic setup Instrument setup Markus Mangold | info@irsweep. com

Bacteriorhodopsin: FTIR step-scan reference measurement Markus Mangold | info@irsweep. com | 21/05/2021 | 13

Comparison: FTIR vs. IRis. F 1 Step-scan FT-IR ~ 20’ 000 repetitions IRis. F

Study fast reaction kinetics: Sub µs time resolution feasible Sub-microsecond time resolution reveals transition

Bacteriorhodopsin single shot spectra IRis-F 1 500 repetitions IRis-F 1 10 repetitions Markus Mangold

Bacteriorhodopsin single shot spectra IRis-F 1 500 repetitions IRis-F 1 single shot Markus Mangold

Conclusion Dual-comb spectrometer with § Up to 100 cm-1 coverage § Sub-microsecond time resolution

IRsweep Pitt Allmendinger Markus Geiser Andreas Hugi Michael Baumann Quentin Saudan Pawel Walkiewicz Balinth

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Today’s time-resolved spectroscopy: FT-IR Typical step-scan FTIR measurement § 450 mirror positions § 44 averages § ~ 20’ 000 repetitions Markus Mangold | info@irsweep. com | 21/05/2021 | 2

Single-shot sub-microsecond mid-infrared spectroscopy with quantum cascade laser frequency combs Markus Mangold Jessica Klocke, Pierre Jouy, Andreas Hugi, Pitt Allmendinger, Markus Geiser, Jerome Faist, Tilman Kottke 19. 6. 2018, International Symposium on Molecular Spectroscopy Urbana-Champaign Andreas Hugi | info@irsweep. com | 21/05/2021 | 3

IRsweep products IRcell IRis-F 1 10 cm Markus Mangold| info@irsweep. com | 21/05/2021 | 4

IRis-F 1 High-Speed Observe fast processes Single-shot IRis-F 1 Easier measurements / sample low sample preparation and consumption high SNR Parallel Multi-wavelength High Brightness Markus Mangold| info@irsweep. com | 21/05/2021 | 5

Available time-resolved methods: step-scan, rapid scan, tunable laser spectroscopy Step-scan FTIR Rapid-scan FTIR Tunable laser spectroscopy x x + Single shot + High time-resolution - Low time-resolution (ms) - Low brightness - Many repetitions λ + High brightness + High time-resolution - Single wavelength per measurement Not applicable to non-repetitive processes requiring high time resolution Markus Mangold | info@irsweep. com | 21. 05. 2021 | 6

IRis-F 1: Dual-comb spectrometer using quantum cascade lasers § Quantum cascade laser frequency combs § Mid-infrared operation § Multi-color operation § High emission power § Hugi et al. Nature 492, 229 -233, (2012) § Villares, Hugi et al. , Nature Communications 5: 5192 (2014) Markus Mangold | info@irsweep. com | 21/05/2021 | 7

IRis-F 1: Dual-comb spectrometer using quantum cascade lasers Two frequency combs superimposed Direct optical – radio frequency link Markus Mangold | info@irsweep. com | 21. 05. 2021 | 8

Quantum cascade laser frequency comb emission High power lasers • Up to 1 W power at – 10°C • > 600 m. W at room temperature • > 1 m. W per mode P. Jouy, M. Mangold et al. , Applied Physics Letter 111, 141102 (2017). QCL emission spectrum • 60 -100 cm-1 coverage ~ Equivalent of 30 DFBS • Center wavelengths between 1000 and 2000 cm-1 • 10 GHz rep. rate = 1/3 cm-1 line spacing Markus Mangold | info@irsweep. com | 21/05/2021 | 9

IRis-F 1: Dual-comb spectrometer using quantum cascade lasers • Large repetition rate • Large Δfrep • High time-resolution info@irsweep. com | 21/05/2021 | 10

IRis-F 1: Signal-to-noise ratio µOD absorbance noise levels with µs time resolution Markus Mangold | info@irsweep. com | 21/05/2021 | 11

Bacteriorhodopsin: IRis-F 1 experimental setup Schematic setup Instrument setup Markus Mangold | info@irsweep. com | 21/05/2021 | 12

Bacteriorhodopsin: FTIR step-scan reference measurement Markus Mangold | info@irsweep. com | 21/05/2021 | 13

Comparison: FTIR vs. IRis. F 1 Step-scan FT-IR ~ 20’ 000 repetitions IRis. F 1 500 repetitions Markus Mangold | info@irsweep. com | 21/05/2021 | 14

Study fast reaction kinetics: Sub µs time resolution feasible Sub-microsecond time resolution reveals transition from K L state of b. R cycle. Sub-microsecond information with low repetition numbers Markus Mangold | info@irsweep. com | 21. 05. 2021 | 15

Bacteriorhodopsin single shot spectra IRis-F 1 500 repetitions IRis-F 1 10 repetitions Markus Mangold | info@irsweep. com | 21/05/2021 | 16

Bacteriorhodopsin single shot spectra IRis-F 1 500 repetitions IRis-F 1 single shot Markus Mangold | info@irsweep. com | 21/05/2021 | 17

Conclusion Dual-comb spectrometer with § Up to 100 cm-1 coverage § Sub-microsecond time resolution § m. OD noise in a single-shot § µOD noise in 100’s of shots Time-resolved studies of non-repetitive processes are now possible! Markus Mangold | info@irsweep. com | 21. 05. 2021 | 18

IRsweep Pitt Allmendinger Markus Geiser Andreas Hugi Michael Baumann Quentin Saudan Pawel Walkiewicz Balinth Horvath Uni Bielefeld Jessica Klocke Tilman Kottke ETH Zurich Pierre Jouy Fillippos Kapsalidis Jerome Faist IRsweep AG Auguste-Piccard-Hof 1 8093 Zürich Switzerland www. irsweep. com info@irsweep. com +41 (0)44 586 79 79 info@irsweep. com | 21/05/2021 | 19