Measuring biological samples by atom probe tomography (APT) in their natural environment, i.e. aqueous solution, would take this analytical method, which is currently well established for metals, semi-conductive materials and non-metals, to a new level. It would give information about the 3D chemical structure of biological systems, which could enable unprecedented insights into biological systems and processes, such as virus protein interactions. For this future aim, we present as a first essential step the APT analysis of pure water (Milli-Q) which is the main component of biological systems. After Cryo-preparation, nanometric water tips are field evaporated with assistance by short laser pulses. The obtained data sets of several tens of millions of atoms reveal a complex evaporation behavior. Understanding the field evaporation process of water is fundamental for the measurement of more complex biological systems. For the identification of the individual signals in the mass spectrum, DFT calculations were performed to prove the stability of the detected molecules.
Atom Probe Tomography (APT) is currently a well-established technique to analyse the composition of solid materials including metals, semiconductors and ceramics with up to near-atomic resolution. Using an aqueous glucose solution, we now extended the technique to frozen solutions. While the mass signals of the common glucose fragments CxHy and CxOyHz overlap with (H2O)nH from water, we achieved stoichiometrically correct values via signal deconvolution. Density functional theory (DFT) calculations were performed to investigate the stability of the detected pyranose fragments. This paper demonstrates APT’s capabilities to achieve sub-nanometre resolution in tracing whole glucose molecules in a frozen solution by using cryogenic workflows. We use a solution of defined concentration to investigate the chemical resolution capabilities as a step toward the measurement of biological molecules. Due to the evaporation of nearly intact glucose molecules, their position within the measured 3D volume of the solution can be determined with sub-nanometre resolution. Our analyses take analytical techniques to a new level, since chemical characterization methods for cryogenically-frozen solutions or biological materials are limited.
Atom probe tomography (APT) has been established in the microscopic chemical and spatial analysis of metallic or semiconductors nanostructures. In recent years, and especially with the development of a transfer shuttle system and adapted preparation protocols, the field of frozen liquids has been opened up. Still, very limited knowledge is available about the evaporation and fragmentation behavior of frozen liquids in APT. In this work, efforts were made to extend the method toward organic and biological soft matter, which are mostly built from hydrocarbon chains, the evaporation and fragmentation behavior of simple alkane chains (n-tetradecanes). Tetradecane shows a very complex evaporation behavior whereby peaks of C1–C15 can be observed. Based on multihit events and the representation of these in correlation plots, more detailed information about the evaporation behavior and the decay of molecules into smaller fragments in the region near the tip can be studied. A variety of different dissociation tracks of larger molecules in their excited state and their subsequent decay in low-field regions, on the way to the detector, could be observed and the dissociation zone in the low-field region was calculated.
Atom Probe Tomography (APT) is currently a well-established technique to analyse the composition of solid materials including metals, semiconductors and ceramics with up to near-atomic resolution. Using an aqueous glucose solution, we now extended the technique to frozen solutions. While the mass signals of the common glucose fragments CxHy and CxOyHz overlap with (H2O)nH from water, we achieved stoichiometrically correct values via signal deconvolution. Density functional theory (DFT) calculations were performed to investigate the stability of the detected pyranose fragments. This paper demonstrates APT’s capabilities to achieve sub-nanometre resolution in tracing whole glucose molecules in a frozen solution by using cryogenic workflows. We use a solution of defined concentration to investigate the chemical and spatial resolution capabilities as a step toward the measurement of biological molecules in solution in 3D with sub-nanometre resolution by using cryo-APT. Our analyses take analytical techniques to a new level, since chemical characterization methods for cryogenically-frozen solutions or biological materials are limited.
The photoluminescence intensity of a light emitter embedded in an atom probe needle-shaped specimen varies with the morphological evolution of the latter during field evaporation. Light absorption and emission patterns within such an evolving system were calculated considering the increase in the reflectivity induced by the high electrostatic field present at the apex surface. A good agreement is obtained between the experimental and calculated photoluminescence intensity as a function of the evaporation progress. These methods could be applied to more general situations in which the properties of nanoscale objects are modulated by surface chemistry or morphology changes.
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