Markus Mangold

Compact multipass optical cell for laser spectroscopy

A multipass cell (MPC) design for laser absorption spectroscopy is presented. The development of this new type of optical cell was driven by stringent criteria for compactness, robustness, low volume, and ease of use in optical systems. A single piece of reflective toroidal surface forms a near-concentric cavity with a volume of merely 40 cm(3). Contrary to traditional MPCs, this design allows for flexible path-length adjustments by simply changing the aiming angle of the laser beam at the entrance window. Two effective optical path lengths of 2.2 and 4.1 m were chosen to demonstrate the cells suitability for high-precision isotope ratio measurements of CO(2) at 1% and ambient mixing ratio levels.

Dual-wavelength quantum cascade laser for trace gas spectroscopy

We demonstrate a sequentially operating dual-wavelength quantum cascade laser with electrically separated laser sections, emitting single-mode at 5.25 and 6.25 μm. Based on a single waveguide ridge, this laser represents a considerable asset to optical sensing and trace gas spectroscopy, as it allows probing multiple gas species with spectrally distant absorption features using conventional optical setups without any beam combining optics. The laser capability was demonstrated in simultaneous NO and NO2 detection, reaching sub-ppb detection limits and selectivity comparable to conventional high-end spectroscopic systems.

Simultaneous measurement of NO and NO(2) by dual-wavelength quantum cascade laser spectroscopy.

The concept of a multi-wavelength quantum cascade laser emitting at two or more spectrally well-separated wavelengths is highly appealing for applied spectroscopy, as it allows detecting several species with compact and cost-efficient optical setups. Here we present a practical realization of such a dual-wavelength setup, which is based on a room-temperature quantum cascade laser emitting single-mode at 1600 cm-1 and 1900 cm-1 and is thus well-suited for simultaneous NO and NO2 detection. Operated in a time-division multiplexed mode, our spectrometer reaches detection limits of 0.5 and 1.5 ppb for NO2 and NO, respectively. The performance of the system is validated against the well-established chemiluminescence detection while measuring the NOx emissions on an automotive test-bench, as well as upon monitoring the pollution at a suburban site.

Dual comb operation of λ ∼ 8.2 μm quantum cascade laser frequency comb with 1 W optical power

In this work, we report the characterization of a quantum cascade laser frequency comb with an optical power of 1.05 W at λ∼8.2 μm. A 4.5 mm long device has a high reflectivity coating on the back facet as well as a top cladding designed to lower the group velocity dispersion and is operated at 258 K. Very strong (more than 60 dB) narrow beatnotes are shown, and frequency comb operation is obtained on a bandwidth of 85 cm−1 in a very large range of light-versus current characteristics. A bandwidth of 82 cm−1 has a power per mode of more than 1 mW and an average power per mode of 4.1 mW. Finally, a multi-heterodyne spectrum with 215 lines covering an optical bandwidth of more than 70 cm−1 measured with lasers showing similar performances is presented with very good line separation.

Circular paraboloid reflection cell for laser spectroscopic trace gas analysis

Absorption cells with circular geometry are a class of multipass reflection cells consisting of a single, circular mirror. They can be particularly favorable for trace gas measurements because of their mechanical robustness, simplicity, and their optical versatility. In this article, we present detailed theoretical considerations and ray tracing simulations for the optimization of the optical design of circular multipass reflection cells. A parabolic mirror shape in a confocal arrangement is found to be most suitable for long optical paths in a small volume. We experimentally demonstrate more than 12 m optical path in a 14.5 cm diameter gas cell and NO2 concentration measurements in ambient air with a measurement precision better than 0.1 ppb.

Standoff detection from diffusely scattering surfaces using dual quantum cascade laser comb spectroscopy

Using dual optical frequency comb (OFC) spectroscopy in the longwave infrared (LWIR), we demonstrate standoff detection of trace amounts of target compounds on diffusely scattering surfaces. The OFC is based on quantum cascade lasers (QCL) that emit ~1 Watt of optical power under cw operation at room temperature over coherent comb bandwidths approaching 100 cm-1. We overlap two nearly identical 1250 cm-1 QCL OFC sources so that the two interfering optical combs create via heterodyne a single comb in the radio frequency (rf) that represents the entire optical spectrum in a single acquisition. In a laboratory scale demonstration we show detection of two spectrally distinct fluorinated silicone oils, poly(methyl-3,3,3-trifluoropropylsiloxane) and Krytox™, that act as LWIR simulants for security relevant compounds whose room temperature vapor pressure is too low to be detected in the gas phase. These target compounds are applied at mass loadings of 0.3 to 90 μg/cm2 to sanded aluminum surfaces. Only the diffusely scattered light is collected by a primary collection optic and focused onto a high speed (0.5 GHz bandwidth) thermoelectrically cooled mercury cadmium telluride (MCT) detector. At standoff distances of both 0.3 and 1 meter, we demonstrate 3 μg/cm2 and 1 μg/cm2 detection limits against poly(methyl-3,3,3-trifluoropropylsiloxane) and Krytox™, respectively.

Multi-wavelength QCL based MIR spectroscopy for fluids and gases

We demonstrate multi-color DFB QCLs with separated electrical pumping for independent single-mode emission of several wavelengths from the same ridge. This will be implemented in our mid-infrared spectroscopy sensors for gases (CO2) and liquids (cocaine).

Single-Shot Sub-microsecond Mid-infrared Spectroscopy on Protein Reactions with Quantum Cascade Laser Frequency Combs.

The kinetic analysis of irreversible protein reactions requires an analytical technique that provides access to time-dependent infrared spectra in a single shot. Here, we present a spectrometer based on dual-frequency-comb spectroscopy using mid-infrared frequency combs generated by quantum cascade lasers. Attenuation of the intensity of the combs by molecular vibrational resonances results in absorption spectra covering 55 cm-1 in the fingerprint region. The setup has a native resolution of 0.3 cm-1, noise levels in the μOD range, and achieves sub-microsecond time resolution. We demonstrate the simultaneous recording of both spectra and transients of the photoactivated proton pump bacteriorhodopsin. More importantly, a single shot, i.e., a single visible light excitation, is sufficient to extract spectral and kinetic characteristics of several intermediates in the bacteriorhodopsin photocycle. This development paves the way for the noninvasive analysis of enzymatic conversions with high time resolution, broad spectral coverage, and minimal sample consumption.

Mid-Infrared spectrometer featuring μ-second time resolution based on dual-comb quantum cascade laser frequency combs

We present a dual-comb spectrometer based on QCL frequency combs. It features a large optical bandwidth and high-resolution. One key benefit of this instrument is the ability to measure broadband μs time-resolved mid-IR spectra.

MIR Spectroscopy: trace-level detection for environmental and industrial applications

Direct absorption spectroscopy using QCLs allows highly sensitive, selective and fast gas detection. Environmental and industrial examples include greenhouse gas isotopes, leak detection and multicomponent measurements using dual wavelength QCLs.