@article{PangerlMuellerRuecketal., author = {Pangerl, Jonas and M{\"u}ller, Max and R{\"u}ck, Thomas and Weigl, Stefan and Bierl, Rudolf}, title = {Characterizing a sensitive compact mid-infrared photoacoustic sensor for methane, ethane and acetylene detection considering changing ambient parameters and bulk composition (N2, O2 and H2O)}, series = {Sensors and Actuators B: Chemical}, volume = {352,1}, journal = {Sensors and Actuators B: Chemical}, publisher = {Elsevier}, doi = {10.1016/j.snb.2021.130962}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:898-opus4-25868}, pages = {1 -- 12}, abstract = {We present a sensitive and compact interband cascade laser (ICL) based photoacoustic setup for the detection of gaseous hydrocarbons and discuss its applicability towards trace gas analysis. We investigated the performance of the sensor for trace concentrations of methane, ethane and acetylene diluted in nitrogen. The excitation of methane and ethane was accomplished using one tunable diode laser, covering a range from 3360 to 3372 nm, which was replaced by a separate ICL at 3025 nm for acetylene detection. The influence of ambient parameters such as temperature, flow rate and pressure as well as potential cross-sensitivities towards O2 and H2O have been examined in terms of methane and acetylene detection. A series of simulations proved several of these influences to be attributed to relaxation effects. With a 3σ limit of detection (LoD) of 6.8 parts per billion (ppbV) in case of methane, 2.3 ppbV regarding ethane and 3.6 ppbV in terms of acetylene, the sensor demonstrates a great potential for applications in the field of trace gas analysis.}, language = {en} } @article{MuellerRueckJobstetal., author = {M{\"u}ller, Max and R{\"u}ck, Thomas and Jobst, Simon and Pangerl, Jonas and Weigl, Stefan and Bierl, Rudolf and Matysik, Frank-Michael}, title = {An Algorithmic Approach to Compute the Effect of Non-Radiative Relaxation Processes in Photoacoustic Spectroscopy}, series = {Photoacoustics}, volume = {26}, journal = {Photoacoustics}, publisher = {Elsevier}, doi = {10.1016/j.pacs.2022.100371}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:898-opus4-39935}, abstract = {Successful transfer of photoacoustic gas sensors from laboratory to real-life applications requires knowledge about potential cross-sensitivities towards environmental and gas matrix changes. Multi-dimensional calibration in case of cross-sensitivities can become very complex or even unfeasible. To address this challenge, we present a novel algorithm to compute the collision based non-radiative efficiency and phase lag of energy relaxation on a molecular level (CoNRad) for photoacoustic signal calculation. This algorithmic approach allows to calculate the entire elaxation cascade of arbitrarily complex systems, yielding a theoretical photoacoustic signal. In this work the influence of varying bulk compositions, i.e. nitrogen (N2), oxygen (O2) and water (H2O) on the photoacoustic signal during methane (CH4) detection is demonstrated. The applicability of the algorithm to other photoacoustic setups is shown exemplary by applying it to the relaxational system investigated in [1]. Hayden et al. examined the effect of water on photoacoustic carbon monoxide (CO) detection.}, language = {en} } @article{PangerlSukulRuecketal., author = {Pangerl, Jonas and Sukul, Pritam and R{\"u}ck, Thomas and Fuchs, Patricia and Weigl, Stefan and Miekisch, Wolfram and Bierl, Rudolf and Matysik, Frank-Michael}, title = {An inexpensive UV-LED photoacoustic based real-time sensor-system detecting exhaled trace-acetone}, series = {Photoacoustics}, volume = {38}, journal = {Photoacoustics}, publisher = {Elsevier}, issn = {2213-5979}, doi = {10.1016/j.pacs.2024.100604}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:898-opus4-71279}, pages = {12}, abstract = {n this research we present a low-cost system for breath acetone analysis based on UV-LED photoacoustic spectroscopy. We considered the end-tidal phase of exhalation, which represents the systemic concentrations of volatile organic compounds (VOCs) - providing clinically relevant information about the human health. This is achieved via the development of a CO2-triggered breath sampling system, which collected alveolar breath over several minutes in sterile and inert containers. A real-time mass spectrometer is coupled to serve as a reference device for calibration measurements and subsequent breath analysis. The new sensor system provided a 3σ detection limit of 8.3 ppbV and an NNEA of 1.4E-9 Wcm 1Hz 0.5. In terms of the performed breath analysis measurements, 12 out of 13 fell within the error margin of the photoacoustic measurement system, demonstrating the reliability of the measurements in the field.}, language = {en} } @article{EscherRueckJobstetal., author = {Escher, Lukas and R{\"u}ck, Thomas and Jobst, Simon and Pangerl, Jonas and Bierl, Rudolf and Matysik, Frank-Michael}, title = {Photodissociation-Driven Photoacoustic Spectroscopy with UV-LEDs for Ozone Detection}, series = {Photoacoustics}, volume = {43}, journal = {Photoacoustics}, publisher = {Elsevier BV}, issn = {2213-5979}, doi = {10.1016/j.pacs.2025.100718}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:898-opus4-80076}, pages = {16}, abstract = {This study presents the development and evaluation of a UV-LED based photoacoustic (PA) measurement system for ozone (O3) detection to demonstrate its potential for low-cost and accurate sensing while for the first time addressing the importance of photodissociation for PA signal generation for O3 in the UV range. With a detection limit of 7.9 ppbV, the system exhibits a significant advancement over state-of-the-art UV-PA O3 detection and is on par with laser-based setups. Following a novel discussion of the PA signal arising from photodissociation and its products, cross-sensitivity effects due to environmental factors such as temperature and gas composition were systematically analyzed. A digital twin driven compensation for these influences was implemented and evaluated. Despite the challenges associated with modeling the effects of H2O and CO2, the PA system shows considerable potential, though further studies in real world applications must be conducted.}, language = {en} } @unpublished{PangerlSukulRuecketal., author = {Pangerl, Jonas and Sukul, Pritam and R{\"u}ck, Thomas and Fuchs, Patricia and Weigl, Stefan and Miekisch, Wolfram and Bierl, Rudolf and Matysik, Frank-Michael}, title = {An Inexpensive Uv-Led Photoacoustic Based Real-Time Sensor-System Detecting Exhaled Trace-Acetone}, publisher = {Elsevier}, doi = {10.2139/ssrn.4724198}, abstract = {In this research we present a low-cost system for breath acetone analysis based on UV-LED photoacoustic spectroscopy. We considered the end-tidal phase of exhalation, which represents the systemic concentrations of volatile organic compounds (VOCs) - providing clinically relevant information about the human health. This is achieved via the development of a CO2-triggered breath sampling system, which collected alveolar breath over several minutes in sterile and inert containers. A real-time mass spectrometer is coupled to serve as a reference device for calibration measurements and subsequent breath analysis. The new sensor system provided a 3σ detection limit of 6.4 ppbV and an NNEA of 1.1E-9 Wcm-1Hz-0.5. In terms of the performed breath analysis measurements, 12 out of 13 fell within the error margin of the photoacoustic measurement system, demonstrating the reliability of the measurements in the field.}, language = {en} } @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} } @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} } @incollection{WeiglMuellerPangerletal., author = {Weigl, Stefan and M{\"u}ller, Max and Pangerl, Jonas and R{\"u}ck, Thomas}, title = {Scopes and Limits of Photoacoustic Spectroscopy in Modern Breath Analysis}, series = {Breath Analysis}, booktitle = {Breath Analysis}, publisher = {Springer nature}, isbn = {978-3-031-18526-7}, doi = {10.1007/11663_2022_22}, pages = {101 -- 159}, abstract = {Photoacoustic spectroscopy is a viable tool for trace gas detection in various application fields. In recent years, this technique has been exploited more and more for modern breath analysis as well. Within this chapter, a holistic overview of photoacoustic spectroscopy is presented, while maintaining the relationship to breath analysis. Therefore, a concise description of the fundamentals of photoacoustic spectroscopy is provided. This is essential for understanding the scopes and limits of this outstanding measurement technique being described within this chapter. In the past several different types of photoacoustic measurement setups for trace gas detection have emerged, including different light sources, modulation techniques, and detection schemes. These are described shortly and advantages as well as disadvantages, especially in relation to breath analysis, are highlighted. Though being a promising sensor principle, measurement devices based on photoacoustic spectroscopy are still rare on the sensor market, especially when it comes to trace gas detection in complex gas matrices, e.g., human breath exhale. One main reason is due to possible molecular interactions influencing the relaxational behavior of the analyte altering the sensor signal. Recent results shedding light on the intricate relaxational processes within complex gas matrices are discussed in detail, providing approaches to overcome this issue. Finally, various applications of photoacoustic spectroscopy in breath analysis are described demonstrating the great potential of this technology.}, language = {en} } @inproceedings{MoserPangerlJobstetal., author = {Moser, Elisabeth and Pangerl, Jonas and Jobst, Simon and Weigl, Stefan and Bierl, Rudolf}, title = {Modeling the Photoacoustic Spectrum of a Quantum Cascade Laser for Human Breath}, series = {Optical Sensors and Sensing Congress 2022 (AIS, LACSEA, Sensors, ES): July 11 - 15, 2022, Vancouver, British Columbia Canada}, booktitle = {Optical Sensors and Sensing Congress 2022 (AIS, LACSEA, Sensors, ES): July 11 - 15, 2022, Vancouver, British Columbia Canada}, publisher = {Optica Publishing Group}, isbn = {978-1-957171-10-4}, doi = {10.1364/AIS.2022.ATu3G.2}, abstract = {A modeling approach to create a photoacoustic spectrum from synthetic data is presented and evaluated. The resulting model reaches a MAPE score of 2.7\% and can be used to enable data-driven development in future work.}, subject = {Quantenkaskadenlaser}, 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} }