Spectroscopy and microscopy of transition metal chalcogenide nanomaterials

King, Martin O. (2013) Spectroscopy and microscopy of transition metal chalcogenide nanomaterials. PhD thesis, University of Glasgow.

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Abstract

This thesis details the physical and electronic structure of several technologically important transition metal chalcogenides (TMCs) using a combination of transmission electron microscopy (TEM) and surface science experimental techniques. The materials studied include CuxTe and CdTe, which find application in high efficiency, low weight photovoltaic devices. CuxTe alloys are frequently used as an electrical back contact in high efficiency CdTe photovoltaics. Here, we examine the alloying of Te on the Cu(111), polycrystalline Cu and Cu(643) surfaces. Chapter 3 of this thesis shows that the alloying of Te and Cu(111) is facile at room temperature, contrary to previous reports. Two distinct surface phases exist, depending on Te surface concentration. Below a coverage of 0.33 monolayers (MLs) of Te a surface substitutional alloy (SSA) is found to exist, where a Te adatom substituted for a surface Cu atom. For Te coverages greater than 0.66 ML, an unusual Cu3Te2 alloy continually grows on the surface, stabilised by a good lattice match to the Cu(111) substrate. The surface alloying of the Cu-Te system displays an intriguing dependence on the surface termination of the Cu substrate. Of the three Cu substrates studied here, Cu(111), Cu(643)R and polycrystalline Cu, a 1 ML film of Te gave ordered alloy structures with stoichiometries of Cu3Te2, CuTe and Cu2Te, respectively. In chapter 4, the study of thin film photovoltaics is extended to the deposition of CdTe onto Cu and CuxTe substrates. CdTe is observed to grow three dimensionally on Cu(111), Cu3Te2 and Cu2Te. Cu+ diffusion, crucial for photovoltaic performance, is detected for CdTe thicknesses greater than 2 ML and is assigned, predominately, to Cu2Te crystallites forming within the CdTe layer, with a minor amount of Cu residing in interstitial sites in the host CdTe structure. Chapter 5 describes the alloying of Te with a intrinsically chiral surface, Cu(643)R, the first study of its kind. The results of this study reveal that step mediated alloying occurs between Cu and Te with significant faceting of the surface. Two ordered CuTe alloy phases were observed for sub-monolayer Te coverages. The low coverage alloy exists for Te coverages between 0.18 ML and 0.45 ML and has a chiral unit cell. The high coverage alloy exists for Te coverages between 0.45 ML and 1.5 ML and has an achiral unit cell. The atomic positions of these surface alloys are tentatively interpreted from the scanning tunnelling microscopy (STM) images. In contrast to the thin film experiments in chapters 3-5, chapter 6 describes a study of TaS3 nanoribbons. These studies reveal that the nanoribbons have a distinct core-shell type structure. Characterisation with surface science techniques shows that the shell is nonstoichiometric and amorphous while TEM shows a crystalline core to the material. Interestingly, the TaS3 are observed to be unstable when interfaced on a Au substrate, with the shell persistently losing S to the substrate, which have potential implications in device integration.

Item Type: Thesis (PhD)
Qualification Level: Doctoral
Keywords: Surface Science, Electron Microscopy, Photovoltaic, Nanomaterials, Cadmium Telluride, Copper Telluride
Subjects: Q Science > QD Chemistry
Colleges/Schools: College of Science and Engineering > School of Chemistry
Funder's Name: UNSPECIFIED
Supervisor's Name: Kadodwala, Dr. Malcolm and MacLaren, Dr. Donald
Date of Award: 2013
Depositing User: Mr Martin King
Unique ID: glathesis:2013-4506
Copyright: Copyright of this thesis is held by the author.
Date Deposited: 07 Aug 2013 07:18
Last Modified: 07 Aug 2013 07:20
URI: http://theses.gla.ac.uk/id/eprint/4506

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