RESUMEN
We present qPeaks (quality peaks), a novel, user-parameter-free algorithm for peak detection and peak characterization applicable to chromatographic data. The algorithm is based on a linearizable regression model that analyzes asymmetric peaks and estimates the specific uncertainties associated with the peak regression parameters. The uncertainties of the parameters are used to derive a data quality score DQSpeak, rendering low reliability results more transparent during processing and allowing for the prioritization of generated features. High DQSpeak chromatographic peaks have a lower chance of being classified as false-positive and show higher repeatability over multiple measurements. The high efficiency of the algorithm makes it particularly useful for application within processing routines of nontarget screening through chromatography coupled with high-resolution mass spectrometry. qPeaks is integrated into the qAlgorithms nontarget screening processing toolbox and appends a parameter-free chromatographic peak detection and characterization step to it. With qAlgorithms, now high-resolution mass spectra are centroided using the qCentroids algorithms, centroids are clustered to form extracted ion chromatograms (EICs) with the qBinning algorithm, and chromatographic peaks are found on the generated EICs with qPeaks. However, all tools from qAlgorithms can also be used independently.
RESUMEN
Due to the complexity and volume of data generated through non-target screening (NTS) using chromatographic couplings with high-resolution mass spectrometry, automized processing routines are necessary. The processing routines usually consist of many individual steps that are user-parameter-dependent and, thus, require labor-intensive optimization. Additionally, the effect of variations in raw data quality on the processing results is unclear and not fully understood. Within this work, we present qBinning, a novel algorithm for constructing extracted ion chromatograms (EICs) based on statistical principles and, thus, without the need to set user parameters. Furthermore, we give the user feedback on the specific qualities of the generated EICs using a scoring system (DQSbin). The DQSbin measures reliability as it correlates with the probability of correct classification of masses into EICs and the degree of overlap between different EIC construction algorithms. This work is a big step forward in understanding the behavior of NTS data and increasing the overall transparency in the results of NTS.
RESUMEN
Non-target screening (NTS) is a powerful environmental and analytical chemistry approach for detecting and identifying unknown compounds in complex samples. High-resolution mass spectrometry has enhanced NTS capabilities but created challenges in data analysis, including data preprocessing, peak detection, and feature extraction. This review provides an in-depth understanding of NTS data processing methods, focusing on centroiding, extracted ion chromatogram (XIC) building, chromatographic peak characterization, alignment, componentization, and prioritization of features. We discuss the strengths and weaknesses of various algorithms, the influence of user input parameters on the results, and the need for automated parameter optimization. We address uncertainty and data quality issues, emphasizing the importance of incorporating confidence intervals and raw data quality assessment in data processing workflows. Furthermore, we highlight the need for cross-study comparability and propose potential solutions, such as utilizing standardized statistics and open-access data exchange platforms. In conclusion, we offer future perspectives and recommendations for developers and users of NTS data processing algorithms and workflows. By addressing these challenges and capitalizing on the opportunities presented, the NTS community can advance the field, improve the reliability of results, and enhance data comparability across different studies.
RESUMEN
High-resolution mass spectrometry is widely used in many research fields allowing for accurate mass determinations. In this context, it is pretty standard that high-resolution profile mode mass spectra are reduced to centroided data, which many data processing routines rely on for further evaluation. Yet information on the peak profile quality is not conserved in those approaches; i.e., describing results reliability is almost impossible. Therefore, we overcome this limitation by developing a new statistical parameter called data quality score (DQS). For the DQS calculations, we performed a very fast and robust regression analysis of the individual high-resolution peak profiles and considered error propagation to estimate the uncertainties of the regression coefficients. We successfully validated the new algorithm with the vendor-specific algorithm implemented in Proteowizard's msConvert. Moreover, we show that the DQS is a sum parameter associated with centroid accuracy and precision. We also demonstrate the benefit of the new algorithm in nontarget screenings as the DQS prioritizes signals that are not influenced by non-resolved isobaric ions or isotopic fine structures. The algorithm is implemented in Python, R, and Julia programming languages and supports multi- and cross-platform downstream data handling.