@unpublished{RueckMuellerJobstetal., author = {R{\"u}ck, Thomas and M{\"u}ller, Max and Jobst, Simon and Weigl, Stefan and Pangerl, Jonas and Bierl, Rudolf and Matysik, Frank-Michael}, title = {Digital Twin of a Photoacoustic Trace Gas Sensor for Monitoring Methane in Complex Gas Compositions}, publisher = {Elsevier / SSRN}, doi = {10.2139/ssrn.4215170}, pages = {22}, abstract = {The digitalization of industrial processes requires smart sensor systems. Photoacoustic spectroscopy is well suited for this purpose as it allows for small-sized and low-cost trace gas analysis. However, the method is susceptible to changes in measurement conditions and standard calibration routines often fail to correct for all changes. We therefore created a Digital Twin (DT) of a photoacoustic trace gas sensor for methane and evaluated it regarding variations in gas composition (CH4, N2, O2, CO2, H2O), temperature and pressure. With a mean absolute percentage error of 0.8 \% the accuracy of the sensor after DT compensation significantly exceeds the 24 \% achieved based on standard calibration in nitrogen. For the first time, we can fully analytically compute the photoacoustic signal under moderate ambient conditions with an error in the ppbV range by taking a holistic approach. Assuming knowledge of the underlying energy transfer processes, the model of this Digital Twin can be adapted to any microphone based photoacoustic sensor for monitoring any analyte species.}, language = {en} } @inproceedings{MuellerRueckJobstetal., author = {M{\"u}ller, Max and R{\"u}ck, Thomas and Jobst, Simon and Pangerl, Jonas and Bierl, Rudolf and Matysik, Frank-Michael}, title = {Creating a Digital Twin of a Photoacoustic Gas Sensor for Methane Detection in Complex Gas Matrices}, series = {Proceedings Optical Sensors and Sensing Congress 2022 (AIS, LACSEA, Sensors, ES): 11-15 July 2022, Vancouver, British Columbia, Canada}, booktitle = {Proceedings Optical Sensors and Sensing Congress 2022 (AIS, LACSEA, Sensors, ES): 11-15 July 2022, Vancouver, British Columbia, Canada}, publisher = {Optica Publishing Group}, isbn = {978-1-957171-10-4}, doi = {10.1364/LACSEA.2022.LW4D.2}, abstract = {We present the calculation results from a digital twin (DT) of our photoacoustic (PA) sensor for methane detection, regarding gas composition, temperature and pressure variations.}, language = {en} } @unpublished{MuellerWeiglMuellerWilliamsetal., author = {M{\"u}ller, Max and Weigl, Stefan and M{\"u}ller-Williams, Jennifer and Lindauer, Matthias and R{\"u}ck, Thomas and Jobst, Simon and Bierl, Rudolf and Matysik, Frank-Michael}, title = {Ambient methane monitoring at Hohenpeißenberg utilizing photoacoustic spectroscopy and cavity ring down spectroscopy}, doi = {10.5194/egusphere-2023-1010}, abstract = {With an atmospheric concentration of approximately 2000 parts per billion (ppbV, 10-9) methane (CH4) is the second most abundant greenhouse gas (GHG) in the atmosphere after carbon dioxide (CO2). The task of long-term and spatially resolved GHG monitoring to verify whether climate policy actions are effective, is becoming more crucial as climate change progresses. In this paper we report the CH4 concentration readings of our photoacoustic (PA) sensor over a five day period at Hohenpeißenberg, Germany. As a reference device a calibrated cavity ringdown spectrometer Picarro G2301 from the meteorological observatory was employed. Trace gas measurements with photoacoustic instruments promise to provide low detection limits at comparably low costs. However, PA devices are often susceptible to cross-sensitivities related to environmental influences. The obtained results show that relaxation effects due to fluctuating environmental conditions, e.g. ambient humidity, are a non-negligible factor in PA sensor systems. Applying algorithm compensation techniques, which are capable of calculating the influence of relaxational effects on the photoacoustic signal, increase the accuracy of the photoacoustic sensor significantly. With an average relative deviation of 1.11 \% from the G2301, the photoacoustic sensor shows good agreement with the reference instrument.}, language = {en} } @article{RueckMuellerJobstetal., author = {R{\"u}ck, Thomas and M{\"u}ller, Max and Jobst, Simon and Weigl, Stefan and Pangerl, Jonas and Bierl, Rudolf and Matysik, Frank-Michael}, title = {Digital Twin of a Photoacoustic Trace Gas Sensor for Monitoring Methane in Complex Gas Compositions}, series = {Sensors and Actuators B: Chemical}, journal = {Sensors and Actuators B: Chemical}, number = {378}, doi = {10.1016/j.snb.2022.133119}, abstract = {The digitalization of industrial processes requires smart sensor systems. Photoacoustic spectroscopy is well suited for this purpose as it allows for small-sized and low-cost trace gas analysis. However, the method is susceptible to changes in measurement conditions and standard calibration routines often fail to correct for all changes. We therefore created a Digital Twin (DT) of a photoacoustic trace gas sensor for methane and evaluated it regarding variations in gas composition (CH4, N2, O2, CO2, H2O), temperature and pressure. With a mean absolute percentage error of 0.8 \% the accuracy of the sensor after DT compensation significantly exceeds the 24 \% achieved based on standard calibration in nitrogen. For the first time, we can fully analytically compute the photoacoustic signal under moderate ambient conditions with an error in the ppbV range by taking a holistic approach. Assuming knowledge of the underlying energy transfer processes, the model of this Digital Twin can be adapted to any microphone based photoacoustic sensor for monitoring any analyte species.}, language = {en} } @inproceedings{PangerlWittmannWeigletal., author = {Pangerl, Jonas and Wittmann, Elisabeth and Weigl, Stefan and M{\"u}ller, Max and Bierl, Rudolf and Matysik, Frank-Michael}, title = {Using a Modulated Quantum Cascade Laser for Photoacoustic Spectra Recording of Exhaled Acetone and Main Breath Components}, series = {Optical Sensors and Sensing Congress 2022 (AIS, LACSEA, Sensors, ES)}, booktitle = {Optical Sensors and Sensing Congress 2022 (AIS, LACSEA, Sensors, ES)}, publisher = {Optica Publishing Group}, doi = {10.1364/AIS.2022.ATu3G.1}, abstract = {Photoacoustic spectra of main breath components together with acetone are presented demonstrating spectral linearity towards different concentrations and compositions. The acetone 3σ detection limit at 1209 cm-1 is 0.28 ppbV}, language = {en} } @unpublished{PangerlSukulRuecketal., author = {Pangerl, Jonas and Sukul, Pritam and R{\"u}ck, Thomas and Escher, Lukas and Miekisch, Wolfram and Bierl, Rudolf and Matysik, Frank-Michael}, title = {Photoacoustic Trace-Analysis of Breath Isoprene and Acetone Via Interband- and Quantum Cascade Lasers}, publisher = {Elsevier / SSRN}, doi = {10.2139/ssrn.4834735}, abstract = {This research presents two laser-based photoacoustic approaches for analyzing exhaled breath isoprene and acetone. The integration of a PTR-ToF-MS as a reference device ensured the reliability and accuracy of the PAS systems that is based on an ICL for isoprene and a QCL for acetone detection. The calibration yielded limits of detection of 26.9 ppbV and 1.7 ppbV, respectively, and corresponding normalized noise equivalent absorption coefficients (NNEAs) of 5.0E-9 Wcm-1Hz-0.5 and 4.9E-9 Wcm-1Hz-0.5. Laboratory as well as real breath sample measurements from alveolar breath revealed a robust system performance, with only one outlier within the static isoprene measurements. However, discrepancies emerged under dynamic breath sampling conditions, emphasizing the need for further optimization. Especially by knowing the dynamic nature and endogenous origin of exhaled isoprene our findings highlight the potential of breath analysis for non-invasive physio-metabolic and pathophysiological monitoring towards point-of-care devices.}, language = {en} } @article{PangerlSukulRuecketal., author = {Pangerl, Jonas and Sukul, Pritam and R{\"u}ck, Thomas and Escher, Lukas and Miekisch, Wolfram and Bierl, Rudolf and Matysik, Frank-Michael}, title = {Photoacoustic trace-analysis of breath isoprene and acetone via interband- and Quantum Cascade Lasers}, series = {Sensors and Actuators: B. Chemical}, volume = {424}, journal = {Sensors and Actuators: B. Chemical}, publisher = {Elsevier}, doi = {10.1016/j.snb.2024.136886}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:898-opus4-77024}, pages = {12}, abstract = {This research presents two laser-based photoacoustic approaches for analyzing exhaled breath isoprene and acetone. The integration of a PTR-ToF-MS as a reference device ensured the reliability and accuracy of the photoacoustic systems that is based on an ICL for isoprene and a QCL for acetone detection. The calibration yielded limits of detection of 26.9 ppbV and 1.7 ppbV, respectively, and corresponding normalized noise equivalent absorption coefficients (NNEAs) of 5.0E-9 Wcm 1Hz 0.5 and 4.9E-9 Wcm 1Hz 0.5. Laboratory as well as real breath sample measurements from alveolar breath revealed a robust system performance, with only one outlier within the static isoprene measurements. However, discrepancies emerged under dynamic breath sampling conditions, emphasizing the need for further optimization. Especially by knowing the dynamic nature and endogenous origin of exhaled isoprene our findings highlight the potential of breath analysis for non-invasive physio-metabolic and pathophysiological monitoring towards point-of-care devices}, language = {en} } @article{RueckPangerlEscheretal., author = {R{\"u}ck, Thomas and Pangerl, Jonas and Escher, Lukas and Jobst, Simon and M{\"u}ller, Max and Bierl, Rudolf and Matysik, Frank-Michael}, title = {Kinetic cooling in mid-infrared methane photoacoustic spectroscopy: A quantitative analysis via digital twin verification}, series = {Photoacoustics}, volume = {40}, journal = {Photoacoustics}, publisher = {Elsevier}, doi = {10.1016/j.pacs.2024.100652}, abstract = {This study presents a detailed quantitative analysis of kinetic cooling in methane photoacoustic spectroscopy, leveraging the capabilities of a digital twin model. Using a quantum cascade laser tuned to 1210.01 cm⁻¹, we investigated the effects of varying nitrogen-oxygen matrix compositions on the photoacoustic signals of 15 ppmV methane. Notably, the photoacoustic signal amplitude decreased with increasing oxygen concentration, even falling below the background signal at oxygen levels higher than approximately 6 \%V. This phenomenon was attributed to kinetic cooling, where thermal energy is extracted from the surrounding gas molecules rather than added, as validated by complex vector analysis using a previously published digital twin model. The model accurately reproduced complex signal patterns through simulations, providing insights into the underlying molecular mechanisms by quantifying individual collision contributions. These findings underscore the importance of digital twins in understanding the fundamentals of photoacoustic signal generation at the molecular level.}, language = {en} } @article{PangerlMoserMuelleretal., author = {Pangerl, Jonas and Moser, Elisabeth and M{\"u}ller, Max and Weigl, Stefan and Jobst, Simon and R{\"u}ck, Thomas and Bierl, Rudolf and Matysik, Frank-Michael}, title = {A sub-ppbv-level Acetone and Ethanol Quantum Cascade Laser Based Photoacoustic Sensor- Characterization and Multi-Component Spectra Recording in Synthetic Breath}, series = {Photoacoustics}, volume = {30}, journal = {Photoacoustics}, publisher = {Elsevier}, issn = {2213-5979}, doi = {10.1016/j.pacs.2023.100473}, pages = {1 -- 12}, abstract = {Trace gas analysis in breath is challenging due to the vast number of different components. We present a highly sensitive quantum cascade laser based photoacoustic setup for breath analysis. Scanning the range between 8263 and 8270 nm with a spectral resolution of 48 pm, we are able to quantify acetone and ethanol within a typical breath matrix containing water and CO2. We photoacoustically acquired spectra within this region of mid-infra-red light and prove that those spectra do not suffer from non-spectral interferences. The purely additive behavior of a breath sample spectrum was verified by comparing it with the independently acquired single component spectra using Pearson and Spearman correlation coefficients. A previously presented simulation approach is improved and an error attribution study is presented. With a 3σ detection limit of 6.5 ppbv in terms of ethanol and 250 pptv regarding acetone, our system is among the best performing presented so far.}, language = {en} } @article{MuellerWeiglMuellerWilliamsetal., author = {M{\"u}ller, Max and Weigl, Stefan and M{\"u}ller-Williams, Jennifer and Lindauer, Matthias and R{\"u}ck, Thomas and Jobst, Simon and Bierl, Rudolf and Matysik, Frank-Michael}, title = {Comparison of photoacoustic spectroscopy and cavity ring-down spectroscopy for ambient methane monitoring at Hohenpeißenberg}, series = {Atmospheric Measurement Techniques}, volume = {16}, journal = {Atmospheric Measurement Techniques}, number = {18}, publisher = {Copernicus Publications}, issn = {1867-8548}, doi = {10.5194/amt-16-4263-2023}, pages = {4263 -- 4270}, abstract = {With an atmospheric concentration of approximately 2000 parts per billion (ppbV, 10-9), methane (CH4) is the second most abundant greenhouse gas (GHG) in the atmosphere after carbon dioxide (CO2). The task of long-term and spatially resolved GHG monitoring to verify whether climate policy actions are effective is becoming more crucial as climate change progresses. In this paper we report the CH4 concentration readings of our photoacoustic (PA) sensor over a 5 d period at Hohenpeißenberg, Germany. As a reference device, a calibrated cavity ring-down spectrometer, Picarro G2301, from the meteorological observatory of the German Weather Service (DWD) was employed. Trace gas measurements with photoacoustic instruments promise to provide low detection limits at comparably low costs. However, PA devices are often susceptible to cross-sensitivities related to fluctuating environmental conditions, e.g. ambient humidity. The obtained results show that for PA sensor systems non-radiative relaxation effects induced by varying humidity are a non-negligible factor. Applying algorithm compensation techniques, which are capable of calculating the influence of non-radiative relaxation effects on the photoacoustic signal, increase the accuracy of the photoacoustic sensor significantly. With an average relative deviation of 1.11 \% from the G2301, the photoacoustic sensor shows good agreement with the reference instrument.}, language = {en} } @unpublished{PangerlMoserMuelleretal., author = {Pangerl, Jonas and Moser, Elisabeth and M{\"u}ller, Max and Weigl, Stefan and Jobst, Simon and R{\"u}ck, Thomas and Bierl, Rudolf and Matysik, Frank-Michael}, title = {A Highly Sensitive Acetone and Ethanol Quantum Cascade Laser Based Photoacoustic Sensor: Characterization and Multi-Component Spectra Recording in Synthetic Breath}, series = {SSRN Electronic Journal}, journal = {SSRN Electronic Journal}, publisher = {Elsevier}, doi = {10.2139/ssrn.4305376}, abstract = {Trace gas analysis in breath is challenging due to the vast number of different components. We present a highly sensitive quantum cascade laser based photoacoustic setup for breath analysis. Scanning the range between 8260 and 8270 nm with a spectral resolution of 48 pm, we are able to quantify acetone and ethanol within a typical breath matrix containing water and CO2. We photoacoustically acquired spectra within this region of mid-infra-red light and prove that those spectra do not suffer from non-spectral interferences. The purely additive behavior of a breath sample spectrum was verified by comparing it with the independently acquired single component spectra using Pearson and Spearman correlation coefficients. A previously presented simulation approach is improved and an error attribution study is presented. With a 3σ detection limit of 6.5 ppbV in terms of ethanol and 250 pptV regarding acetone, our system is among the best performing presented so far.}, language = {en} }