Laser-induzierte Messverfahren zur in-situ-Charakterisierung nicht-Kohlenstoff-basierter Nanopartikel

• Antragsteller: Professor Dr. Christof Schulz
• Fachliche Zuordnung: Chemische und Thermische Verfahrenstechnik ; Energieverfahrenstechnik
• Förderung: Förderung von 2013 bis 2021
• Projektkennung: Deutsche Forschungsgemeinschaft (DFG) - Projektnummer 222540104

• Erstellungsjahr: 2021

Zusammenfassung der Projektergebnisse

In this project, non-perturbative optical techniques for the in situ particle diagnostics of gasborne nanoparticle synthesis of non-soot materials has been performed. The intention is on the one hand to develop suitable spectroscopic methods and on the other hand to use these methods to further characterize the optical properties of these materials. The main accomplishments in this proposal period was the in situ characterization of Si and Ge nanoparticles, mainly in terms of their optical properties. The particles are synthesized in an optically accessible microwave plasma reactor using silane and/or germane as precursor gases. Extinction/emission measurements were performed with a broadband laser-driven light source (LDLS), a spectrometer, and an EMCCD camera. The optical properties of liquid Si and Ge were modeled based on line-of-sight attenuation (LOSA) spectra using Drude and Mie theory. The uncertainties in the properties for Ge also were determined by Bayesian analysis. From the significantly different extinction spectral signatures, it was possible to determine the particle phase (liquid/solid) in the probe volume – which is a novel and previously not expected possibility. Furthermore, the gas-phase temperature and the particle volume fraction of liquid silicon and germanium nanoparticles were retrieved using tomographic reconstruction of lineof-sight emission and extinction spectroscopy. The experiments were performed by either using a focused beam through different locations of the particle stream or with a diffuse light beam of the LDLS source. Furthermore, the line-of-sight averaged gas-phase temperature was determined from the wavelength-dependent incandescence of hot particles. For gas-phase temperature measurements, some oxygen was introduced into the reaction zone to produce SiO, and the measured absorption spectra allowed us to determine the gas-phase temperature by spectral fitting. The measurements were also performed for silane/germane precursor mixtures for the synthesis of nanoparticle composites to later determine their optical properties. Along with the in situ characterization, ex situ TEM analysis of the particle was performed by collecting the samples using a pneumatically-driven thermophoretic sampler at the same measurement location as for LOSA measurements. An EDX analysis shows the composition of mixture of Si and Ge nanoparticles. Moreover, the purity of the Si nanoparticles was validated by recording the Raman spectrum of Si powder in a different experiment.

Projektbezogene Publikationen (Auswahl)

• Determination of optical properties of non-soot nanoparticles generated by microwave plasma via line-of-sight attenuation (LOSA)” 8th International Workshop on Laser-Induced Incandescence (2018)
  M. Asif, J. Menser, K. Daun, T. Dreier, C. Schulz
  
• Transition from laser-induced incandescence (LII) to laser-induced breakdown spectroscopy (LIBS) on elemental nanoparticles. 8th International Workshop on Laser-Induced Incandescence; 2018; Tutzing
  J. Menser, K.J. Daun, T. Dreier, C. Schulz
  
• Detector calibration and measurement issues in multi-color time-resolved laser-induced incandescence, Appl. Phys. B 125 (2019) 126
  R. Mansmann, T.A. Sipkens, J. Menser, K.J. Daun, T. Dreier, C. Schulz
  
• Evalution of Drude parameters for liquid Germanium nanoparticles through aerosol-based line-ofsight attenuation measurements, J. Quant. Spectrosc. Radiat. Transf. 226, 146-156 (2019)
  K. Daun, J. Menser, M. Asif, S. Musikhin, T. Dreier, C. Schulz
  
• “Phase-sensitive detection of silicon and germanium nanoparticle aerosols via line-of-sight attenuation and emission measurements” Gordon Research Seminar on Laser Diagnostics in Energy and Combustion Science (GRS) (2019)
  M. Asif, J. Menser, K. Daun, T. Dreier, C. Schulz
  
• Interrogating gas-borne nanoparticles using laserbased diagnostics and Bayesian data fusion, J. Phys. Chem., (2021)
  J. Menser, K. Daun, C. Schulz
  
• Phase-sensitive detection of gas-borne Si nanoparticles via line-of-sight UV/VIS attenuation
  M. Asif, J. Menser, T. Endres, T. Dreier, K. Daun, C. Schulz
  
• Spatial distribution of gas-phase synthesized germanium nanoparticle volume-fraction and temperature using combined in situ line-of-sight emission and extinction spectroscopy, Opt. Expr. 29 (2021) 8387-8257
  G. Liu, M. Asif, J. Menser, T. Dreier, K. Mohri, C. Schulz, T. Endres