Advanced quantum cascade laser infrared attenuated total reflection spectroscopy
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Date
2024-12-20
Authors
Teuber, Andrea
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Dissertation
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Abstract
The overarching topic of this cumulative thesis is the development and application of next-generation quantum cascade laser (QCL) based infrared attenuated total reflection (IR-ATR) infrared spectroscopy.
Cascade lasers (i.e., interband and quantum cascade lasers; ICLs, QCLs) are considered the most advanced mid-infrared light sources, as discussed and exemplified in the introduction section of this dissertation. The characteristic properties of quantum cascade lasers include a broad spectral coverage and tunability in the mid-infrared range (MIR; 3 – 12 µm), well-defined spectral properties, and a high energy density within the emitted spectral band. As a result, spectroscopic information can be obtained based on differentiating molecular signatures. Consequently, the remainder of this cumulative thesis focuses on a variety of analytical applications capitalizing on the unique properties of cascade lasers presented as a series of peer-reviewed research articles.
If laser light sources are combined with appropriate transducers, numerous application opportunities arise in a variety of scenarios ranging from environmental monitoring to bioanalytics. Hence, the development of innovative sensor technologies is an important yet challenging topic. The main purpose of the transducer in optical sensors is to ensure reproducible interaction between the sample and the photons, i.e., herein, light emitted by the laser light source. This is of particular interest if optical sensing technologies aim at taking advantage of inherent molecular specificity without additional chem/bio recognition architectures, as is the case for mid-infrared spectroscopic concepts. While the aforementioned scenarios – environmental vs. life science applications – clearly have their specific needs and requirements, both may capitalize on similar fundamental photonic concepts and building blocks, which are at the core of the present thesis, i.e., mid-infrared laser and mid-infrared waveguide technology.
Analyzing molecular constituents in real-world environmental scenarios requires measurement techniques that may particularly withstand harsh external conditions while providing robust and reliable analytical data. Only a few infrared spectroscopic systems have been developed for harsh environments with most devices in routine practice being deployed in appropriate research facilities providing for a constant measurement environment without the need for portable or mobile devices. Among the most robust sensing concepts in mid-infrared photonics are transducers/sampling interfaces based on single or multiple reflection waveguides facilitating IR-ATR (i.e., evanescent field absorption) spectroscopy, which are readily adaptable to harsh conditions as shown in the present thesis. To this end, conventional multi-reflection ATR concepts were augmented with substrate-integrated hollow waveguide (iHWG) technology pioneered by our research team yielding an exceedingly robust modular transducer platform. This was achieved by developing an iHWG-based invariant light coupling concept for coupling IR photons to an ATR waveguide without the need for any additional optics in a robust and compact arrangement. This innovative assembly was proven useful for conventional broadband IR spectroscopy using Fourier transform infrared spectrometers, as well as QCLs. In the course of this thesis, a robust MIR sensor system was developed for mobile measurement applications at harsh environmental or process analytical conditions. The versatility of the developed sensor technology was demonstrated by coupling to a variety of light sources, the optional use of MIR fiberoptics, and by investigating a series of relevant analytes.
Bioanalytical sensing technologies frequently require addressing exceedingly small sample volumes/quantities or directly addressing live biological specimens or systems. This requires biocompatible and chemically inert transducers when probing samples in life science applications. To this end, diamond is an ideal waveguide material that next to its inertness and biocompatibility provides a broad spectral transmission window that extends well into the MIR regime, which is of particular interest for the present thesis. While conventional diamond ATR crystals with only a few internal reflections readily exist, the present thesis was focused on optimizing frequency-matched thin-film diamond waveguide technology ideally combining with QCL light sources. Using nanocrystalline diamond layers with a thickness of around 20 µm, near single-mode waveguiding behavior has been achieved yielding a homogeneous evanescent field at the waveguide surface rather than hotspots, as encountered via discrete internal reflections using macroscopic ATR waveguides. Thereby, highly miniaturized sensing concepts are facilitated without trading off size against sensitivity. The performance and quantitative analytical capabilities of QCL-based MIR sensors combined with thin-film diamond waveguides were compared to conventional IR-ATR technology for the exemplary analyte caffeine, which is among the most commonly ingested psychoactive substances found in simulating beverages such as tea, coffee, or energy drinks.
The utility of the developed sensing concepts was also shown for the analysis of live biological specimens, i.e., model bacteria, whereby biofilm formation processes were studied in molecular detail using QCLs combined with diamond thin-film waveguide technology for the first time. Different growth phases of bacteria were analyzed and compared with conventional IR spectroscopic data confirming the feasibility of IR laser spectroscopy for complex bioanalytical application scenarios.
Finally, even though QCLs combined with diamond thin-film waveguide technology gave rise to adequately sensitive measurement concepts, there are analytical scenarios where even more sensitivity is required. Hence, it was shown that the strategy of surface-enhanced infrared absorption (SEIRA) spectroscopy may be readily adapted for harnessing the MIR sensing technologies developed in this thesis, especially by using graphene for amplifying selected infrared signatures.
In summary, the results of this cumulative thesis were published within ten peer-reviewed contributions in leading international journals, including seven of them as a first author. A review contribution introduces the fundamentals of cascade lasers and their applications providing selected highlight examples published as a book chapter. The obtained research results address two main areas – environmental/process analytical scenarios and bioanalytics – demonstrating the versatility of waveguide-based laser spectroscopy in the mid-infrared contributing three publications each to robust IR-ATR concepts suitable for harsh environments, and to advanced thin-film diamond waveguide technology for bioanalytical scenarios.
Description
Faculties
Fakultät für Naturwissenschaften
Institutions
Institut für Analytische und Bioanalytische Chemie
Institut für Chemieingenieurwesen
Institut für Chemieingenieurwesen
Citation
DFG Project uulm
EU Project THU
Other projects THU
GRA//DIA / Graphen-auf-bor-dotiertem-Diamant / BMBF / #03XP0206B
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Teuber, A. and Mizaikoff, B. (2023). Cascade Laser Infrared Spectroscopy. In Encyclopedia of Analytical Chemistry, R.A. Meyers (Ed.). https://doi.org/10.1002/9780470027318.a9751
Teuber A, Stach R, Haas J, Mizaikoff B., Innovative Substrate-Integrated Hollow Waveguide Coupled Attenuated Total Reflection Sensors for Quantum Cascade Laser Based Infrared Spectroscopy in Harsh Environments. Applied Spectroscopy. 2022; 76(1):132-140. doi:10.1177/00037028211064331
Teuber, A.; Mizaikoff, B., RobustATR: Substrate-Integrated Hollow Waveguide Coupled Infrared Attenuated Total Reflectance Sensors. Appl. Sci. 2022, 12, 10019. https://doi.org/10.3390/app121910019
A. Teuber and B. Mizaikoff, "Robust Attenuated Total Reflection Infrared Spectroscopic Sensors Based on Quantum Cascade Lasers for Harsh Environments," in IEEE Sensors Journal, vol. 24, no. 1, pp. 814-821, 1 Jan.1, 2024, doi: 10.1109/JSEN.2023.3330525
A. Teuber, G. Caniglia, M. Wild, M. Godejohann, C. Kranz, and B. Mizaikoff, Espresso Science: Laser-Based Diamond Thin-Film Waveguide Sensors for the Quantification of Caffeine, Vol. 8(5):1871-1881; 10.1021/acssensors.2c01841
A. Teuber, G. Caniglia, H. Barth, C. Kranz and B. Mizaikoff, Thin-Film Waveguide Laser Spectroscopy: A Novel Platform for Bacterial Analysis, Vol. 95, 45, 16600–16608, 2023, 10.1021/acs.analchem.3c02782
Andrea Teuber, Giada Caniglia, Christine Kranz, Boris Mizaikoff, Graphene enhanced Quantum Cascade Laser Infrared Absorbance Spectroscopy based on Diamond Thin Film Waveguides, Analyst (2023), 10.1039/d3an00824j
Teuber A, Stach R, Haas J, Mizaikoff B., Innovative Substrate-Integrated Hollow Waveguide Coupled Attenuated Total Reflection Sensors for Quantum Cascade Laser Based Infrared Spectroscopy in Harsh Environments. Applied Spectroscopy. 2022; 76(1):132-140. doi:10.1177/00037028211064331
Teuber, A.; Mizaikoff, B., RobustATR: Substrate-Integrated Hollow Waveguide Coupled Infrared Attenuated Total Reflectance Sensors. Appl. Sci. 2022, 12, 10019. https://doi.org/10.3390/app121910019
A. Teuber and B. Mizaikoff, "Robust Attenuated Total Reflection Infrared Spectroscopic Sensors Based on Quantum Cascade Lasers for Harsh Environments," in IEEE Sensors Journal, vol. 24, no. 1, pp. 814-821, 1 Jan.1, 2024, doi: 10.1109/JSEN.2023.3330525
A. Teuber, G. Caniglia, M. Wild, M. Godejohann, C. Kranz, and B. Mizaikoff, Espresso Science: Laser-Based Diamond Thin-Film Waveguide Sensors for the Quantification of Caffeine, Vol. 8(5):1871-1881; 10.1021/acssensors.2c01841
A. Teuber, G. Caniglia, H. Barth, C. Kranz and B. Mizaikoff, Thin-Film Waveguide Laser Spectroscopy: A Novel Platform for Bacterial Analysis, Vol. 95, 45, 16600–16608, 2023, 10.1021/acs.analchem.3c02782
Andrea Teuber, Giada Caniglia, Christine Kranz, Boris Mizaikoff, Graphene enhanced Quantum Cascade Laser Infrared Absorbance Spectroscopy based on Diamond Thin Film Waveguides, Analyst (2023), 10.1039/d3an00824j
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Keywords
Dünnschichtlichtwellenleiter, Sensordesign, Bioanalytik, Quantum cascade laser, chemical sensor, Thin-film waveguide, Infrarotspektroskopie, Photonik, Chemischer Sensor, Biochemische Analyse, Umweltanalytik, Laser, Quantenkaskadenlaser, Infrared spectroscopy, Photonics, Chemical detectors, Analytical biochemistry, Lasers, DDC 570 / Life sciences, DDC 540 / Chemistry & allied sciences