Ece Aytan

Variable-temperature inelastic light scattering spectroscopy of nickel oxide: Disentangling phonons and magnons

We report the results of an investigation of the temperature dependence of the magnon and phonon frequencies in NiO. A combination of Brillouin-Mandelstam and Raman spectroscopies allowed us to elucidate the evolution of the phonon and magnon spectral signatures from the Brillouin zone center (GHz range) to the second-order peaks from the zone boundary (THz range). The temperature-dependent behavior of the magnon and phonon bands in the NiO spectrum indicates the presence of antiferromagnetic (AF) order fluctuation or a persistent AF state at temperatures substantially above the Neel temperature (TN=523 K). Tuning the intensity of the excitation laser provides a method for disentangling the features of magnons from acoustic phonons in AF materials without the application of a magnetic field. Our results are useful for the interpretation of the inelastic-light scattering spectrum of NiO and add to the knowledge of its magnon properties important for THz spintronic devices.We report results of an investigation of the temperature dependence of the magnon and phonon frequencies in NiO. A combination of Brillouin - Mandelstam and Raman spectroscopies allowed us to elucidate the evolution of the phonon and magnon spectral signatures from the Brillouin zone center (GHz range) to the second-order peaks from the zone boundary (THz range). The temperature-dependent behavior of the magnon and phonon bands in the NiO spectrum indicates the presence of antiferromagnetic (AF) order fluctuation or a persistent AF state at temperatures above the Neel temperature (T=523 K). Tuning the intensity of the excitation laser provides a method for disentangling the features of magnons from acoustic phonons without the application of a magnetic field. Our results are useful for interpretation of the inelastic-light scattering spectrum of NiO, and add to the knowledge of its magnon properties important for THz spintronic devices.

Chelant Enhanced Solution Processing for Wafer Scale Synthesis of Transition Metal Dichalcogenide Thin Films

It is of paramount importance to improve the control over large area growth of high quality molybdenum disulfide (MoS2) and other types of 2D dichalcogenides. Such atomically thin materials have great potential for use in electronics, and are thought to make possible the first real applications of spintronics. Here in, a facile and reproducible method of producing wafer scale atomically thin MoS2 layers has been developed using the incorporation of a chelating agent in a common organic solvent, dimethyl sulfoxide (DMSO). Previously, solution processing of a MoS2 precursor, ammonium tetrathiomolybdate ((NH4)2MoS4), and subsequent thermolysis was used to produce large area MoS2 layers. Our work here shows that the use of ethylenediaminetetraacetic acid (EDTA) in DMSO exerts superior control over wafer coverage and film thickness, and the results demonstrate that the chelating action and dispersing effect of EDTA is critical in growing uniform films. Raman spectroscopy, photoluminescence (PL), x-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), atomic force microscopy (AFM) and high-resolution scanning transmission electron microscopy (HR-STEM) indicate the formation of homogenous few layer MoS2 films at the wafer scale, resulting from the novel chelant-in-solution method.

Spin-phonon coupling in antiferromagnetic nickel oxide

We report the results of ultraviolet Raman spectroscopy of NiO, which allowed us to determine the spin-phonon coupling coefficients in this important antiferromagnetic material. The use of the second-order phonon scattering and ultraviolet laser excitation (λ = 325 nm) was essential for overcoming the problem of the optical selection rules and dominance of the two-magnon band in the visible Raman spectrum of NiO. We established that the spins of Ni atoms interact more strongly with the longitudinal than transverse optical phonons and produce opposite effects on the phonon energies. The peculiarities of the spin-phonon coupling are consistent with the trends given by density functional theory. The obtained results shed light on the nature of the spin-phonon coupling in antiferromagnetic insulators and can help in developing spintronic devices.

Acoustic phonon spectrum engineering in bulk crystals via incorporation of dopant atoms

We report results of Brillouin—Mandelstam spectroscopy of transparent Al2O3 crystals with Nd dopants. The ionic radius and atomic mass of Nd atoms are distinctively different from those of the host Al atoms. Our results show that even a small concentration of Nd atoms incorporated into the Al2O3 samples produces a profound change in the acoustic phonon spectrum. The velocity of the transverse acoustic phonons decreases by ∼600 m/s at the Nd density of only ∼0.1%. Interestingly, the decrease in the phonon frequency and velocity with the doping concentration is non-monotonic. The obtained results, demonstrating that modification of the acoustic phonon spectrum can be achieved not only by traditional nanostructuring but also by low-concentration doping, have important implications for thermal management as well as thermoelectric and optoelectronic devices.

Monoclinic structures of niobium trisulfide

Two new polymorphs of niobium trisulfide are established by single crystal x-ray diffraction. NbS3-iv crystallizes in the monoclinic space group P21/c with lattice parameters a = 6.7515(5) A, b = 4.9736(4) A, c = 18.1315(13) A, and β = 90.116(2)°. Its structure is based on chains of [NbS6] trigonal prisms containing Nb–Nb pairs with a bond length of 3.0448(8) A; this pairing causes the chains to corrugate slightly along their axis, a feature also present in triclinic NbS3-i that leads to semiconductor properties. The stacking arrangement of chains is different in these polymorphs, however, with NbS3-i having an ABCDE repeating sequence of chain bilayers and NbS3-iv having an AB repeating sequence. HRTEM studies show the presence of topotactically-oriented intergrown zones and numerous dislocations, which result in mosaic structuring. A second new polymorph, NbS3-v, crystallizes in the monoclinic space group P21/m with lattice parameters a = 4.950(5) A, b = 3.358(4) A, c = 9.079(10) A, β = 97.35(2)°. In co...

Thermal Percolation Threshold and Thermal Properties of Composites with High Loading of Graphene and Boron Nitride Fillers

We investigated thermal properties of the epoxy-based composites with the high loading fraction-up to f ≈ 45 vol %-of the randomly oriented electrically conductive graphene fillers and electrically insulating boron nitride fillers. It was found that both types of the composites revealed a distinctive thermal percolation threshold at the loading fraction fT > 20 vol %. The graphene loading required for achieving thermal percolation, fT, was substantially higher than the loading, fE, for electrical percolation. Graphene fillers outperformed boron nitride fillers in the thermal conductivity enhancement. It was established that thermal transport in composites with high filler loadings, f ≥ fT, is dominated by heat conduction via the network of percolating fillers. Unexpectedly, we determined that the thermal transport properties of the high loading composites were influenced strongly by the cross-plane thermal conductivity of the quasi-two-dimensional fillers. The obtained results shed light on the debated mechanism of the thermal percolation, and facilitate the development of the next generation of the efficient thermal interface materials for electronic applications.

Quasi-1D van der Waals materials as high current-density local interconnects (Conference Presentation)

The continuous downscaling of interconnect dimensions in combination with the introduction of low-k dielectrics has increased the number of heat dissipation, integration and reliability challenges in modern electronics. As a result, there is a strong need for new materials that have high current-carrying capacity for applications as nanoscale interconnects. In this presentation, we show that quasi-one-dimensional (1D) van der Waals metals such as TaSe3 have excellent breakdown current density exceeding that of 5 MA/cm2. This value is above that currently achievable in conventional copper or aluminum wires. The quasi-1D van der Waals materials are characterized by strong bonds along one dimension and weak van der Waals bonds along two other dimensions. The material for this study was grown by the chemical vapor transport (CVT) method. Both mechanical and chemical exfoliation methods were used to fabricate nanowires with lateral dimensions below 100 nm. The dimensions of the quasi-1D nanowires were verified with scanning electron microscopy (SEM) and atomic force microscopy (AFM). The metal (Ti/Au) contacts for the electrical characterization were deposited using electron beam evaporation (EBE). The measurements were conducted on a number of prototype interconnects with multiple electric contacts to ensure reproducibility. The obtained results suggest that quasi-1D van der Waals metals present a feasible alternative to conventional copper interconnects in terms of the current-carrying capacity and the breakdown current-density. This work was supported, in part, by the SRC and DARPA through STARnet Center for Function Accelerated nanoMaterial Engineering (FAME).