TY - JOUR A1 - van Wasen, S. A1 - You, Yi A1 - Beck, S. A1 - Riedel, Jens A1 - Volmer, D. A. T1 - Miniaturized Protein Digestion Using Acoustic Levitation with Online High Resolution Mass Spectrometry N2 - The combination of acoustically levitated droplets, mid-IR laser evaporation, and subsequent post-ionization by secondary electrospray ionization was applied for monitoring the enzymatic digestion of various proteins. Acoustically levitated droplets are an ideal, wall-free model reactor, readily allowing compartmentalized microfluidic trypsin digestions. Time-resolved interrogation of the droplets yielded real-time information on the progress of the reaction and thus provided insights into reaction kinetics. After 30 min of digestion in the acoustic levitator, the obtained protein sequence coverages were identical to the reference overnight digestions. Importantly, our results clearly demonstrate that the applied experimental setup can be used for the real-time investigation of chemical reactions. Furthermore, the described methodology only uses a fraction of the typically applied amounts of solvent, analyte, and trypsin. Thus, the results exemplify the use of acoustic levitation as a green analytical chemistry alternative to the currently used batch reactions. KW - Acoustic levitation KW - Protein analysis KW - Mass spectrometry PY - 2023 DO - https://doi.org/10.1021/acs.analchem.2c05334 VL - 95 SP - 4190 EP - 4195 PB - ACS Publications AN - OPUS4-57053 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Alcalde-Vasquez, R. A1 - Moreno-Pedraza, A. A1 - Rosas-Román, I. A1 - Guillén-Alonso, H. A1 - Riedel, Jens A1 - Partida-Martínez, L. P. A1 - Winkler, R. T1 - MoBiMS: A Modular Miniature Mass Analyzer for the Real-Time 2 Monitoring of Gases and Volatile Compounds in Biological Systems N2 - Living organisms constantly interact with their environment, including through the exchange of gases. Respiration and the release and uptake of volatile organic compounds (VOCs) create dynamic microenvironments in biological systems. Studying the kinetics of volatiles in biological systems requires expensive instruments, and data analysis is challenging. Therefore, we aimed to design a minimal analytical device for measuring the composition of gaseous mixtures in realtime. We built the ‘Modular Biological Mass Spectrometer’ (MoBiMS) from 3D-printed parts and custom sensors to fit a wide array of experimental set-ups. We tested the chemical detection range and temporal resolution of the MoBiMS employing pure compounds and complex biological samples. Compounds with a higher than 0.4 mmHg vapor pressure and a molecular weight up to 154 g/mol were reliably sensed within seconds. The generated electron impact (EI) spectra were directly comparable with standard databases like the NIST EI library. Under a direct analysis approach, the MoBiMS identified the characteristic odor of banana (Musa sp.), that is, isoamyl acetate; tracked the dynamics of CO2 release while the Alka-Seltzer® reaction occurred showed the kinetics of the transient production and consumption of carbon dioxide during photosynthesis. MoBiMS also discriminated between volatile compounds ions coming from tobacco (Nicotiana benthamiana) leaves and the surrounding air through untargeted analysis. The small footprint of the MoBiMS and its relatively low energy consumption facilitate in situ analyses, as an additional gas supply is not necessary with EI ionization. The MoBiMS is easy to assemble, and its construction and operation are very cost-efficient compared to commercial devices. The analytical performance of the MoBiMS is suitable for real-time studies of biological systems, environmental monitoring, and medical diagnostics. KW - Mass spectrometry KW - Instrumentation KW - Miniaturization KW - Volatiles PY - 2022 DO - https://doi.org/10.1016/j.microc.2021.107090 SN - 0026-265X VL - 175 PB - Elsevier B.V. CY - Amsterdam AN - OPUS4-56528 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Zöllner, Moritz T. A1 - Dariz, Petra A1 - Riedel, Jens A1 - Schmid, Thomas T1 - Dolomite and Mg Calcite as Mineral Thermometers in Mortar Binders. A High Resolution Raman Spectroscopic Study N2 - This paper suggests the use of high‐resolution Raman scattering bands of MgCa carbonates as posteriori thermometer minerals in archaeometric studies. Therefore, the thermal behavior of two dolomite samples and the hydration and carbonation reaction in air of the decomposition products were investigated by Raman microspectroscopy. The increase in the calcination temperature resulted in the formation of – Raman silent MgO and – inert Mg calcite at 700°C–750°C. In contrast, the decarbonation, hydration, and recarbonation of sample material exposed to 750°C–900°C in a muffle furnace led to the appearance of Mg‐free calcite. High spectral resolution Raman spectroscopy enabled a spectral distinction between these two groups due to differences in the band parameters (peak position, bandwidth) of the vibrational (v1, v4, L) modes of calcite. In combination with Raman microspectroscopic mapping, this spectral information represents a new approach for the estimation of burning temperatures of medieval high‐fired gypsum mortars via natural dolomite impurities. Thus, the results of this work highlight the importance and potential of Raman microspectroscopy as a thermometric tool for elucidating the thermal history of anthropogenic fired materials, with potential applications for archaeometry and art technology, as well as for quality controls in the frame of the production of mineral mortar binders and ceramics or bricks, respectively. KW - Mineral thermometry KW - Raman spectroscopy KW - Dolomite KW - High-fired gypsum mortar PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-630270 DO - https://doi.org/10.1002/jrs.6810 SN - 1097-4555 SP - 1 EP - 13 PB - Wiley AN - OPUS4-63027 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Winckelmann, Alexander A1 - Morcillo Garcia-Morato, Dalia A1 - Richter, Silke A1 - Recknagel, Sebastian A1 - Riedel, Jens A1 - Vogl, Jochen A1 - Panne, Ulrich A1 - Abad Andrade, Carlos Enrique T1 - Determination of lithium in human serum by isotope dilution atomic absorption spectrometry N2 - The therapeutic dose of lithium (Li) compounds, which are widely used for the treatment of psychiatric and hematologic disorders, is close to its toxic level; therefore, drug monitoring protocols are mandatory. Herein, we propose a fast, simple, and low-cost analytical procedure for the traceable determination of Li concentration in human serum, based on the monitoring of the Li isotope dilution through the partially resolved isotope shift in its electronic transition around 670.80 nm using a commercially available high-resolution continuum source graphite furnace atomic absorption spectrometer. With this technique, serum samples only require acidic digestion before analysis. The procedure requires three measurements—an enriched 6Li spike, a mixture of a certified standard solution and spike, and a mixture of the sample and spike with a nominal 7Li/6Li ratio of 0.82. Lanthanum has been used as an internal spectral standard for wavelength correction. The spectra are described as the linear superposition of the contributions of the respective isotopes, each consisting of a spin-orbit doublet, which can be expressed as Gaussian components with constant spectral position and width and different relative intensity, reflecting the isotope ratio in the sample. Both the spectral constants and the correlation between isotope ratio and relative band intensity have been experimentally obtained using commercially available materials enriched with Li isotopes. The Li characteristic mass (mc) obtained corresponds to 0.6 pg. The procedure has been validated using five human serum certified reference materials. The results are metrologically comparable and compatible to the certified values. The measurement uncertainties are comparable to those obtained by the more complex and expensive technique, isotope dilution mass spectrometry. KW - Lithium KW - Human serum KW - Isotope dilution KW - Atomic absorption spectrometry KW - High-resolution continuum source graphite furnace atomic absorption spectrometry PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-532446 DO - https://doi.org/10.1007/s00216-021-03636-6 VL - 414 IS - 1 SP - 251 EP - 256 PB - Springer CY - Berlin AN - OPUS4-53244 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Winckelmann, Alexander A1 - Nowak, S. A1 - Richter, Silke A1 - Recknagel, Sebastian A1 - Riedel, Jens A1 - Vogl, Jochen A1 - Panne, Ulrich A1 - Abad Andrade, Carlos Enrique T1 - High-Resolution Atomic Absorption Spectrometry Combined With Machine Learning Data Processing for Isotope Amount Ratio Analysis of Lithium N2 - An alternative method for lithium isotope amount ratio analysis based on a combination of high-resolution atomic absorption spectrometry and spectral data analysis by machine learning (ML) is proposed herein. It is based on the well-known isotope shift of approximately 15 pm for the electronic transition 22P←22S at around the wavelength of 670.8 nm, which can be measured by the state-of-the-art high-resolution continuum source graphite furnace atomic absorption spectrometry. For isotope amount ratio analysis, a scalable tree boosting ML algorithm (XGBoost) was employed and calibrated using a set of samples with 6Li isotope amount fractions, ranging from 0.06 to 0.99 mol mol–1, previously determined by a multicollector inductively coupled plasma mass spectrometer (MC-ICP-MS). The calibration ML model was validated with two certified reference materials (LSVEC and IRMM-016). The procedure was applied toward the isotope amount ratio determination of a set of stock chemicals (Li2CO3, LiNO3, LiCl, and LiOH) and a BAM candidate reference material NMC111 (LiNi1/3Mn1/3Co1/3O2), a Li-battery cathode material. The results of these determinations were compared with those obtained by MC-ICP-MS and found to be metrologically comparable and compatible. The residual bias was −1.8‰, and the precision obtained ranged from 1.9 to 6.2‰. This precision was sufficient to resolve naturally occurring variations, as demonstrated for samples ranging from approximately −3 to +15‰. To assess its suitability to technical applications, the NMC111 cathode candidate reference material was analyzed using high-resolution continuum source atomic absorption spectrometry with and without matrix purification. The results obtained were metrologically compatible with each other. KW - Lithium KW - Isotope KW - Machine learning KW - Algorithms KW - Reference material KW - AAS KW - Atomic Absorption Spectrometry PY - 2021 DO - https://doi.org/10.1021/acs.analchem.1c00206 SN - 1520-6882 VL - 93 IS - 29 SP - 10022 EP - 10030 PB - American Chemical Society CY - Washington, DC, USA AN - OPUS4-53028 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Li, Xunyu A1 - Riedel, Jens A1 - You, Yi T1 - Practical high-resolution spectroscopy with a spatial heterodyne spectrometer: Determination of instrumental function for lineshape recovery N2 - The spatial heterodyne spectrometer (SHS) is a well-recognized platform for its high resolving power in various use cases of spectroscopy. Same as other spectrometer topologies, the SHS, unfortunately, also suffers from classical challenges such as distorted lineshape due to the instrumental function. The goal of this work is to tackle this persisting issue through a simple numerical approach. With the inherent characteristics of an SHS interferogram, we report the direct extraction and determination of the instrumental function in its numerical representation from an SHS interferogram; this instrumental function was further used for spectral data processing that enables significant improvements in spectral resolution through deconvolution algorithms.Here, we systematically discuss the recognition of the embedded instrumental function among various ingredients within an interferogram. To verify the numerical approach, lithium was chosen as the model sample, resembling the use of SHS in an isotopic analysis application. Specifically, the resonance transition of lithium D-lines (2P1/2,3/2 ← 2S1/2) was selected to assess the performance of the spectral processing. With the spectral deconvolution, the spectral features that represent the 6Li and 7Li were nearly baseline-separated, allowing for the accurate measure of the isotopic abundance without external references or algorithm adjustments (e.g., curve fitting). KW - SHS KW - Isotopic analysis KW - High Resolution PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-613401 DO - https://doi.org/10.1016/j.sab.2024.107053 SN - 0584-8547 VL - 221 SP - 1 EP - 5 PB - Elsevier AN - OPUS4-61340 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Steinbeck, Christoph A1 - Jung, Nicole A1 - Bach, Felix A1 - Neumann, Steffen A1 - Herres-Pawlis, Sonja A1 - Liermann, Johannes A1 - Koepler, Oliver A1 - Bannwarth, Christoph A1 - Bender, Theo A1 - Bocklitz, Thomas A1 - Boehm, Franziska A1 - Bonatto Minella, Christian A1 - Biedermann, Frank A1 - Brack, Werner A1 - Cunha, Ricardo A1 - Czodrowski, Paul A1 - Eberl, Franziska A1 - Engel, Thomas A1 - Engstfeld, Albert A1 - Fischer, Tillmann G. A1 - Friedrich, Pascal A1 - Glorious, Frank A1 - Golub, Benjamin A1 - Grathwol, Christoph A1 - Haag, Rainer A1 - Hunold, Johannes A1 - Jacob, Christoph A1 - Johannsen, Jochen A1 - Jollife, John A1 - Kast, Stefan A1 - Kettner, Carsten A1 - Kuhn, Stefan A1 - Lanza, Giacomo A1 - Lisec, Jan A1 - Manolikakes, Georg A1 - Mata, Ricardo A1 - Meiler, Jens A1 - Müller, Matthias A1 - Müller-Pfefferkorn, Ralph A1 - Ortmeyer, Jochen A1 - Patterson, Wendy A1 - Pleiss, Jürgen A1 - Riedel, Annalisa A1 - Riedel, Jens A1 - Schatzschneider, Ulrich A1 - Schuster, Leonie A1 - Seeberger, Peter A1 - Seibert, Johann-Nikolaus A1 - Stadler, Peter A1 - Zeitler, Kirsten T1 - Proposal NFDI4Chem 2025-2030 In the National Research Data Infrastructure (NFDI) — Our Vision: All Chemists Publish FAIR Data N2 - The first funding period of NFDI4Chem established a robust foundation for research data management (RDM) in chemistry by promoting FAIR data principles and creating a cohesive infrastructure to capture well-annotated data early in the lab through electronic lab notebooks (ELNs) and making this data available in public repositories. Key achievements include standardised data formats and metadata, a federated repository environment, and improved data visibility and accessibility. Training programs and outreach have significantly increased awareness and adoption of best RDM practices. In the second funding period, the consortium aims to advance these achievements by consolidating this infrastructure, developing a model for its sustainable maintenance and operation, and fostering cultural change for its widespread adoption. Goals include ensuring seamless data workflows from laboratories to open repositories, enhancing interoperability, and supporting innovative research through AI-ready data. The work plan is organised into six task areas (TAs). TA1 (Management) provides leadership and supports all other TAs in achieving their objectives. TA2 (Smart Lab) aims to develop a fully digital research environment, including an ELN as a modular platform. This environment will support data collection, management, storage, analysis, and sharing. Integrating devices and external resources will enable seamless data transfer to repositories. TA3 (Repositories) will consolidate the repository ecosystem. The goal is to integrate repositories into a federated system for better accessibility and interoperability, ensuring long-term data availability and sustainability. TA4 (Metadata, Data Standards, and Publication Standards) focuses on developing and promoting new data and metadata standards in an international community process. This includes applying ontologies to create a semantic foundation for linking research data, making it machine-readable and enabling knowledge graphs. TA5 (Community and Training) is dedicated to fostering a cultural shift towards digital chemistry through continuous engagement, collecting requirements, and providing extensive training and support through workshops and open education resources. It will promote FAIR-compliant machine learning applications, embedding RDM into academic curricula to ensure future scientists are well-versed in these practices. TA6 (Synergies and Cross-Cutting Topics) aims to enhance collaboration across NFDI consortia and beyond. This includes developing ontologies, terminology services, the search service, and other cross-cutting solutions, integrating these developments into existing infrastructure, enabling interdisciplinary data harmonisation and fostering machine learning applications. KW - Research Data Management KW - FAIR KW - Chemistry PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-648540 DO - https://doi.org/10.3897/rio.11.e177037 SN - 2367-7163 VL - 11 SP - 1 EP - 100 PB - Pensoft Publishers AN - OPUS4-64854 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Riedel, Jens T1 - Current Transformations and Challenges through the Eyes of a Scientist at a German Federal Research Agency N2 - Innovative research, harmonized standards, certification of reference products, policy advice and regulatory action. To most researchers, federal research agencies (FRAs) are abstract chimeras as these tasks appear cryptic and unrelated or even entirely incompatible with each other. Instead of one body, they are pictured as a loose conglomerate of individual institutes, agencies, and offices. The German federal institute for materials research and testing (BAM), is currently undergoing a change process to tear down the walls between these disjunct facilities. Apart from an organizational streamlining, such an infrastructure ideally allows for a holistic approach to tackle complex problems. This presentation will shed some light onto the challenges and opportunities arising. Recent years have been dominated by pivotal changes, crises, and challenges. Many scientists see an increasing circularity in material flows and a fossil fuel phase out to be the only feasible way to proceed. By all this, the material world is faced with a plethora of the above mentioned complicate and complex problems. Parallel to these analog challenges, paradigm-changing advancements in robotics, semantic-data technology, and artificial intelligence, currently empower the digital world with unprecedented speed. Using the example of lithium-ion batteries, the talk will showcase modern FRAs as nutritious ecosystem for a holistic approach towards accelerating all future research and development processes. It will give a glimpse of the complex interplay of different stakeholders like industry, politics, researchers, and end-users but also a simultaneous work on simulation, research and development, characterization, standardization, and regularization. After a brief introduction into these different facets of our institute, a deep dive will be given into the development of novel spectroscopic techniques (e.g. laser induced breakdown spectroscopy (LIBS), glow discharge optical emission spectroscopy, and Raman scattering), directly addressing the demands identified by the above stakeholders. Since by design, a future applicability is already included into this chemical characterization methodologies, all the presented techniques all share the same characteristics to be relatively inexpensive, fast, robust and do not need laborious sample preparation. T2 - Institute Seminar CY - Troy, NY, USA DA - 29.10.2024 KW - Federal research KW - Transformation KW - Analytical Chemistry KW - Instrumentation PY - 2024 AN - OPUS4-61971 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Riedel, Jens T1 - Is LIBS ready for the future? N2 - Recent years have brought up many challenges for an analytical tracing of material flows. While planetary boundaries force end of life material into circular recycling pathways, geopolitical tension creates demands regarding the origin of raw materials. The analytical demands on any instrumentation to tackle the arising challenges of this scenario are straight forward: No sample preparation, precision in the percentage region, and high throughput at comparably low cost. All these demands make LIBS a perfect candidate, why it is time for a re-evaluation of how it exploits the potential possibilities arising from todays’ technology. While being a relatively young technique, the vast majority of conducted LIBS experiments still relies on well established instrumentation, sometimes ignoring the innovations and breakthroughs in the development of its empowering technology sectors such as battery powered compact high repetition rate lasers with tuneable pulse rate and length, low priced cameras with millions of small sized pixels and extremely fast shutter and readout times, optical modulators, galvonometer scanners, and simple robotics. In this talk we will showcase some examples on how the implantation of all these new tools can lead to extremely affordable and compact instrumentation with unprecedented acquisition speed and a spectral resolution sufficient to resolve atomic isotope lines. T2 - FACCS SCiX CY - Raleigh, NC, USA DA - 20.10.2024 KW - LIBS KW - Isotopes KW - Instrumentation PY - 2024 AN - OPUS4-61970 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - You, Yi A1 - Danischewski, Julia A1 - Molnar, Brian A1 - Riedel, Jens A1 - Shelley, Jacob T1 - Manipulation of Gaseous Ions with Acoustic Fields at Atmospheric Pressure N2 - The ability to controllably move gaseous ions is an essential aspect of ion-based spectrometry (e.g., mass spectrometry and ion mobility spectrometry) as well as materials processing. At higher pressures, ion motion is largely governed by diffusion and multiple collisions with neutral gas molecules. Thus, high-pressure ion optics based on electrostatics require large fields, radio frequency drives, complicated geometries, and/or partially transmissive grids that become contaminated. Here, we demonstrate that low-power standing acoustic waves can be used to guide, block, focus, and separate beams of ions akin to electrostatic ion optics. Ions preferentially travel through the static-pressure regions (“nodes”) while neutral gas does not appear to be impacted by the acoustic field structure and continues along a straight trajectory. This acoustic ion manipulation (AIM) approach has broad implications for ion manipulation techniques at high pressure, while expanding our fundamental understanding of the behavior of ions in gases. KW - Ion mobility spectrometry KW - Acoustic KW - Mass spectrometry PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-600704 DO - https://doi.org/10.1021/jacs.4c01224 SP - 1 EP - 6 PB - ACS Publications AN - OPUS4-60070 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -