Development of a sensor system for human breath acetone analysis based on photoacoustic spectroscopy

The breath analysis section of this thesis outlines the potentials but also emphasises the concomitant challenges of human breath analysis. The section further describes the usefulness of a point-of-care (POC) device for breath acetone detection. In addition, it covers various breath analysis related subjects, which can be useful considering further developments of breath analysers. This includes an extensive summary involving the high abundant endogenous as well as the exogenous breath species present in a clinical environment. Subsequently, a detailed discussion about the theoretical aspects of absorption spectra is provided, forming the basis for the spectral interference chapter. Classical absorption spectroscopy (AS) is compared with photoacoustic spectroscopy (PAS) in view of trace gas analysis. Different modulation schemes for signal generation, i.e. amplitude modulation (AM) and wavelength modulation (WM) are part of the comparison, while the advantages and disadvantages of each technique are highlighted. As a result, PAS is considered superior to AS and hence is selected as the method of choice regarding the development of a sensor for breath acetone detection. A detailed mathematical derivation of the photoacoustic signal generation as well as the signal enhancement by means of acoustic resonance amplification is provided. Moreover, several phenomena causing signal attenuation are outlined, including vibrational-translational (VT) relaxation, vibrational-vibrational (VV) energy transfer mechanism, acoustic detuning and photodissociation. Various simulations regarding spectral interferences in the infra-red (IR) and ultraviolet (UV) region are presented, demonstrating the susceptibility towards spectral cross-sensitivities in the IR region, hence, rather suggesting the UV region for acetone detection. However, this simulation can be easily adopted to other target analytes and serves as a basis for multicomponent analysis approaches in the IR region using tuneable light sources. Ultra sensitive acetone detection employing a high power UV LED is presented and a detailed analysis considering the effects of environmental parameters onto the photoacoustic signal, including temperature, pressure, LED duty cycle and flow rate, is provided. In addition, general cross-sensitivities of the photoacoustic signal towards the high abundant species O2, CO2 and H2O have been investigated and discussed. Moreover, several LED and photoacoustic cell (PAC) combinations have been compared in order to evaluate improvement approaches regarding an enhancement of the system’s sensitivity. Finally, photoacoustic sensor setups employing an interband cascade laser (ICL) or a quantum cascade laser (QCL) have been studied and compared to various UV setups in view of different key performance parameters, including the limits of detection (LOD) and the normalised noise equivalent absorption (NNEA) coefficients. The juxtaposition of the different approaches once more emphasises the extraordinary sensitivity of photoacoustic spectroscopy. To the best of the author’s knowledge, the LODs (3σ) of the UV LED based photoacoustic measurement in typical breath conditions (12.5 ppbV) and the LOD of the QCL measurement (0.79 ppbV) provide two world records. First, regarding photoacoustic acetone detection using an UV LED and second, in view of other published results for photoacoustic acetone detection in general