Obafemi Otelaja

Highly Conductive Cu2–xS Nanoparticle Films through Room-Temperature Processing and an Order of Magnitude Enhancement of Conductivity via Electrophoretic Deposition

A facile room-temperature method for assembling colloidal copper sulfide (Cu2-xS) nanoparticles into highly electrically conducting films is presented. Ammonium sulfide is utilized for connecting the nanoparticles via ligand removal, which transforms the as-deposited insulating films into highly conducting films. Electronic properties of the treated films are characterized with a combination of Hall effect measurements, field-effect transistor measurements, temperature-dependent conductivity measurements, and capacitance-voltage measurements, revealing their highly doped p-type semiconducting nature. The spin-cast nanoparticle films have carrier concentration of ∼ 10(19) cm(-3), Hall mobilities of ∼ 3 to 4 cm(2) V(-1) s(-1), and electrical conductivities of ∼ 5 to 6 S · cm(-1). Our films have hole mobilities that are 1-4 orders of magnitude higher than hole mobilities previously reported for heat-treated nanoparticle films of HgTe, InSb, PbS, PbTe, and PbSe. We show that electrophoretic deposition (EPD) as a method for nanoparticle film assembly leads to an order of magnitude enhancement in film conductivity (∼ 75 S · cm(-1)) over conventional spin-casting, creating copper sulfide nanoparticle films with conductivities comparable to bulk films formed through physical deposition methods. The X-ray diffraction patterns of the Cu2-xS films, with and without ligand removal, match the Djurleite phase (Cu(1.94)S) of copper sulfide and show that the nanoparticles maintain finite size after the ammonium sulfide processing. The high conductivities reported are attributed to better interparticle coupling through the ammonium sulfide treatment. This approach presents a scalable room-temperature route for fabricating highly conducting nanoparticle assemblies for large-area electronic and optoelectronic applications.

Non-equilibrium phonon generation and detection in microstructure devices

We demonstrate a method to excite locally a controllable, non-thermal distribution of acoustic phonon modes ranging from 0 to ~200 GHz in a silicon microstructure, by decay of excited quasiparticle states in an attached superconducting tunnel junction (STJ). The phonons transiting the structure ballistically are detected by a second STJ, allowing comparison of direct with indirect transport pathways. This method may be applied to study how different phonon modes contribute to the thermal conductivity of nanostructures.

Design and operation of a microfabricated phonon spectrometer utilizing superconducting tunnel junctions as phonon transducers

In order to fully understand nanoscale heat transport it is necessary to spectrally characterize phonon transmission in nanostructures. Toward this goal we have developed a microfabricated phonon spectrometer. We utilize microfabricated superconducting tunnel junction (STJ)-based phonon transducers for the emission and detection of tunable, non-thermal and spectrally resolved acoustic phonons, with frequencies ranging from ?100 to ?870?GHz, in silicon microstructures. We show that phonon spectroscopy with STJs offers a spectral resolution of ?15?20?GHz, which is ?20 times better than thermal conductance measurements, for probing nanoscale phonon transport. The STJs are Al?AlxOy?Al tunnel junctions and phonon emission and detection occurs via quasiparticle excitation and decay transitions that occur in the superconducting films. We elaborate on the design geometry and constraints of the spectrometer, the fabrication techniques and the low-noise instrumentation that are essential for successful application of this technique for nanoscale phonon studies. We discuss the spectral distribution of phonons emitted by an STJ emitter and the efficiency of their detection by an STJ detector. We demonstrate that the phonons propagate ballistically through a silicon microstructure, and that submicron spatial resolution is realizable in a design such as ours. Spectrally resolved measurements of phonon transport in nanoscale structures and nanomaterials will further the engineering and exploitation of phonons, and thus have important ramifications for nanoscale thermal transport as well as the burgeoning field of nanophononics.

Enhancement of phonon backscattering due to confinement of ballistic phonon pathways in silicon as studied with a microfabricated phonon spectrometer

In this work, the mechanism for enhanced phonon backscattering in silicon is investigated. An understanding of phonon propagation through substrates has implications for engineering heat flow at the nanoscale, for understanding sources of decoherence in quantum systems, and for realizing efficient phonon-mediated particle detectors. In these systems, phonons that backscatter from the bottom of substrates, within the crystal or from interfaces, often contribute to the overall detector signal. We utilize a microscale phonon spectrometer, comprising superconducting tunnel junction emitters and detectors, to specifically probe phonon backscattering in silicon substrates (∼500 μm thick). By etching phonon “enhancers” or deep trenches (∼90 μm) around the detectors, we show that the backscattered signal level increases by a factor of ∼2 for two enhancers versus one enhancer. Using a geometric analysis of the phonon pathways, we show that the mechanism of the backscattered phonon enhancement is due to confinement of the ballistic phonon pathways and increased scattering off the enhancer walls. Our result is applicable to the geometric design and patterning of substrates that are employed in phonon-mediated detection devices.