Surface nanostructuring enables the manipulation of many essential surface properties. With the recent rapid advancements in laser technology, a contactless large-area processing at rates of up to m 2 s −1 becomes feasible that allows new industrial applications in medicine, optics, tribology, biology, etc. On the other hand, the last two decades enable extremely successful and intense research in the field of so-called laser-induced periodic surface structures (LIPSS, ripples). Different types of these structures featuring periods of hundreds of nanometers only-far beyond the optical diffraction limit-up to several micrometers are easily manufactured in a single-step process and can be widely controlled by a proper choice of the laser processing conditions. From a theoretical point of view, however, a vivid and very controversial debate emerges, whether LIPSS originate from electromagnetic effects or are caused by matter reorganization. This article aims to close a gap in the available literature on LIPSS by reviewing the currently existent theories of LIPSS along with their numerical implementations and by providing a comparison and critical assessment of these approaches.
The Rosetta Orbiter Spectrometer for Ion and Neutral Analysis (ROSINA) will answer important questions posed by the mission's main objectives. After Giotto, this will be the first time the volatile part of a comet will be analyzed in situ. This is a very important investigation, as comets, in contrast to meteorites, have maintained most of the volatiles of the solar nebula. To accomplish the very demanding objectives through all the different phases of the comet's activity, ROSINA has unprecedented capabilities including very wide mass range (1 to >300 amu), very high mass resolution (m/Δ m > 3000, i.e. the ability to resolve CO from N2 and 13C from 12CH), very wide dynamic range and high sensitivity, as well as the ability to determine cometary gas velocities, and temperature. ROSINA consists of two mass spectrometers for neutrals and primary ions with complementary capabilities and a pressure sensor. To ensure that absolute gas densities can be determined, each mass spectrometer carries a reservoir of a calibrated gas mixture allowing in-flight calibration. Furthermore, identical flight-spares of all three sensors will serve for detailed analysis of all relevant parameters, in particular the sensitivities for complex organic molecules and their fragmentation patterns in our electron bombardment ion sources
Lipidomics is a particularly difficult analytical challenge due to the number and importance of isomeric species that are known or postulated in biological samples. Current separation and identification techniques are too often insufficiently powerful, slow or ambiguous. High resolution, low field ion mobility coupled to mass spectrometry is shown here to have sufficient performance to represent a new alternative for lipidomics. For the first time, drift-tube ion mobility separation of lipid isomers that differ only in position of the acyl chain, position of the double bond or double bond geometry is demonstrated. Differences in collision cross sections of less than 1% are sufficient for baseline separation. The same level of performance is maintained in complex biological mixtures. More than 130 high-precision reduced mobility and collision cross section values were also determined for a range of lipids. Such data can be the basis of a new lipidomics workflow, as the appropriate libraries are developed.
Highly oxygenated multifunctional organic compounds (HOMs) originating from biogenic emissions constitute a widespread source of organic aerosols in the pristine atmosphere. However, the molecular forms in which HOMs are present in the condensed phase upon gas-particle partitioning remain unclear. In this study, we show that highly oxygenated molecules that contain multiple peroxide functionalities are readily cationized by the attachment of Na during electrospray ionization operated in the positive ion mode. With this method, we present the first identification of HOMs characterized as CHO monomers and CHO dimers in α-pinene derived secondary organic aerosol (SOA). Simultaneous detection of these molecules in the gas phase provides direct evidence for their gas-to-particle conversion. Molecular properties of particulate HOMs generated from ozonolysis and OH oxidation of unsubstituted (CH) and deuterated (CHD) α-pinene are investigated using coupled ion mobility spectrometry with mass spectrometry. The systematic shift in the mass of monomers in the deuterated system is consistent with the decomposition of isomeric vinylhydroperoxides to release vinoxy radical isotopologues, the precursors to a sequence of autoxidation reactions that ultimately yield HOMs in the gas phase. The remarkable difference observed in the dimer abundance under O- versus OH-dominant environments underlines the competition between intramolecular hydrogen migration of peroxy radicals and their bimolecular termination reactions. Our results provide new and direct molecular-level information for a key component needed for achieving carbon mass closure of α-pinene SOA.
Abstract. Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS–MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS–MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI–IMS–MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS) ambient field campaign in the forested SE US. The ambient IMS–MS signals are consistent with laboratory IMS–MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS–MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS–MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. Controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of oligomers, and confirm the presence of the organosulfate functional group.
Nuclear Magnetic Resonance (NMR) spectroscopy is a non-invasive analytical technique which allows for the study of intact samples. Comprehensive Multiphase NMR (CMP-NMR) combines techniques and hardware from solution state and solid state NMR to allow for the holistic analysis of all phases (i.e. solutions, gels and solids) in unaltered samples. This study is the first to apply CMP-NMR to deceased, intact organisms and uses 13 C enriched Daphnia magna (water fleas) as an example. D. magna are commonly used model organisms for environmental toxicology studies. As primary consumers, they are responsible for the transfer of nutrients across trophic levels, and a decline in their population can potentially impact the entire freshwater aquatic ecosystem. Though in vivo research is the ultimate tool to understand an organism’s most biologically relevant state, studies are limited by conditions (i.e. oxygen requirements, limited experiment time and reduced spinning speed) required to keep the organisms alive, which can negatively impact the quality of the data collected. In comparison, ex vivo CMP-NMR is beneficial in that; organisms do not need oxygen (eliminating air holes in rotor caps and subsequent evaporation); samples can be spun faster, leading to improved spectral resolution; more biomass per sample can be analyzed; and experiments can be run for longer. In turn, higher quality ex vivo NMR, can provide more comprehensive NMR assignments, which in many cases could be transferred to better understand less resolved in vivo signals. This manuscript is divided into three sections: 1) multiphase spectral editing techniques, 2) detailed metabolic assignments of 2D NMR of 13 C enriched D. magna and 3) multiphase biological changes over different life stages, ages and generations of D. magna . In summary, ex vivo CMP-NMR proves to be a very powerful approach to study whole organisms in a comprehensive manner and should provide very complementary information to in vivo based research.
The formation and properties of laser-induced periodic surface structures (LIPSS) was investigated on different technically relevant glasses including fused silica, borosilicate glass, and soda-lime-silicate glass under irradiation of fs-laser pulses characterized by a pulse duration τ = 300 fs and a laser wavelength λ = 1025 nm. For this purpose, LIPSS were fabricated in an air environment at normal incidence with different laser peak fluence, pulse number, and repetition frequency. The generated structures were characterized by using optical microscopy, scanning electron microscopy, focused ion beam preparation and Fast-Fourier transformation. The results reveal the formation of LIPSS on all investigated glasses. LIPSS formation on soda-lime-silicate glass is determined by remarkable melt-formation as an intra-pulse effect. Differences between the different glasses concerning the appearing structures, their spatial period and their morphology were discussed based on the non-linear absorption behavior and the temperature-dependent viscosity. The findings facilitate the fabrication of tailored LIPSS-based surface structures on different technically relevant glasses that could be of particular interest for various applications.
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