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Electronic and Magnetic Materials From Two-dimensional Honeycomb Tin Lattices

Arguilla, Maxx Que
http://rave.ohiolink.edu/etdc/view?acc_num=osu1500481320103395

Abstract Details

2017, Doctor of Philosophy, Ohio State University, Chemistry.
The discovery of new families of layered 2D crystals that have diverse sets of electronic, optical, and spin-orbit coupling properties, enable the realization of unique electronic and magnetic phenomena in the single-layer regime. Herein, we present the synthesis and characterization of three classes of exfoliatable and non-exfoliatable 2D-honeycomb Sn and main group-based layered materials with diverse properties ranging from topological insulators to anisotropic magnets. In Chapter 2, we present the growth and electronic, optical and Raman properties of an array of layered Zintl phases which feature flat or puckered anionic sheets of group 14 (CaSi2, CaGe2, EuGe2 and BaSn2) and group 14/15 elements (NaSnP, KSnAs and KSnSb). We show that the Raman-active modes in these phases strongly depend on the reduced mass and the in-plane bond lengths in the 2D sheets. We have also experimentally determined that CaSi2 (6R), CaGe2 (6R) and EuGe2 are metallic while NaSnP, KSnAs and KSnSb are semiconducting. In addition, we have shown via DFT calculations that BaSn2 possesses topologically-protected surface states and is a strong 3D Z2-type topological insulator. In Chapters 3 and 4, we discuss the structural, electronic and magnetic properties and exfoliation of a family of vdW layered Zintl phases with the ASn2As2 (A= Na, Sr and Eu) stoichiometry which exhibit unique electronic and magnetic properties such as: anisotropic two-carrier transport in NaSn2As2 and tunable anisotropic magnetism, with anti-ferromagnetic coupling out-of-plane and ferromagnetic coupling in-plane, in EuSn2As2/Eu1-xNaxSn2As2 (x = 0.25, 0.50 and 0.75). Lastly, in Chapter 5, we have shown two routes towards the realization of sp3-hybridized 2D vdW Tin phases. First, we alloy Sn into the 2D germanane (GeH) lattice via the low temperature topochemical deintercalation of CaGe2-2xSn2x in HCl to produce sheets of Ge1-xSnxH1-x(OH)x held by van der Waals forces (x = 0, 0.04, 0.07, 0.09). This enabled the tuning of the optoelectronic properties of GeH from a band gap of 1.59 eV down to 1.38 eV with just 9% of Sn, which we have demonstrated through the combination of absorbance and single crystal wavelength-dependent photoconductivity measurements. Second, we impart synthetic insights on the creation of highly unstable crystalline 2D van der Waals phases with high Sn content (=50%). We show that the deintercalation of Sn-based layered Zintl phases (NaSnP, KSnAs and KSnSb) into 2D organic-functionalized materials is limited by an underlying electrochemical process, wherein the Zintl phase precursor reduces the alkyl halide (organic ligand source and deintercalant) via a one-electron reduction process which produces organic radicals that further amorphize the crystalline framework. By choosing the correct alkyl halide/Zintl phase pair, where the alkyl halide’s reduction process is more negative in potential than the oxidation process of the Zintl phase, we have observed evidence of formation of 2D Sn(CH2CH3)Pn (Pn = P, As and Sb) phases that have absorption edges from 1.3 eV (P) down to 0.2 eV (Sb). Overall, the creation and discovery of these classes of electronic and magnetic materials beyond graphene will allow for the experimental demonstration and realization of novel physical phenomena, properties and applications in 2D.
Joshua Goldberger, PhD (Advisor)
McGrier Psaras, PhD (Committee Member)
Wu Yiying, PhD (Committee Member)
305 p.
Chemistry; Inorganic Chemistry

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Citations

  • Arguilla, M. Q. (2017). Electronic and Magnetic Materials From Two-dimensional Honeycomb Tin Lattices [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1500481320103395

    APA Style (7th edition)

  • Arguilla, Maxx. Electronic and Magnetic Materials From Two-dimensional Honeycomb Tin Lattices. 2017. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1500481320103395.

    MLA Style (8th edition)

  • Arguilla, Maxx. "Electronic and Magnetic Materials From Two-dimensional Honeycomb Tin Lattices." Doctoral dissertation, Ohio State University, 2017. http://rave.ohiolink.edu/etdc/view?acc_num=osu1500481320103395

    Chicago Manual of Style (17th edition)

osu1500481320103395
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This open access ETD is published by The Ohio State University and OhioLINK.