The thermal conductivity of amorphous TaOx memristive films having variable oxygen content is measured using time domain thermoreflectance. Thermal transport is described by a two-part model where the electrical contribution is quantified via the Wiedemann-Franz relation and the vibrational contribution by the minimum thermal conductivity limit for amorphous solids. The vibrational contribution remains constant near 0.9 W/mK regardless of oxygen concentration, while the electrical contribution varies from 0 to 3.3 W/mK. Thus, the dominant thermal carrier in TaOx switches between vibrations and charge carriers and is controllable either by oxygen content during deposition, or dynamically by field-induced charge state migration.
The transport properties of ceramic materials strongly depend on oxygen activity, which is tuned by changing the partial oxygen pressure (pO2) prior to and during measurement. Within, we describe an instrument for highly stable measurements of Seebeck coefficient and electrical resistivity at temperatures up to 1300 K with controlled oxygen partial pressure. An all platinum construction is used to avoid potential materials instabilities that can cause measurement drift. Two independent heaters are employed to establish a small temperature gradient for Seebeck measurements, while keeping the average temperature constant and avoiding errors associated with pO2-induced drifts in thermocouple readings. Oxygen equilibrium is monitored using both an O2 sensor and the transient behavior of the resistance as a proxy. A pO2 range of 10−25–100 atm can be established with appropriate gas mixtures. Seebeck measurements were calibrated against a high purity platinum wire, Pt/Pt–Rh thermocouple wire, and a Bi2Te3 Seebeck coefficient Standard Reference Material. To demonstrate the utility of this instrument for oxide materials we present measurements as a function of pO2 on a 1 % Nb-doped SrTiO3 single crystal, and show systematic changes in properties consistent with oxygen vacancy defect chemistry. An approximately 11 % increase in power factor over a pO2 range of 10−19–10−8 atm at 973 K for the donor-doped single crystals is observed.
Dynamic control of thermal transport in solid-state systems is a transformative capability with the promise to propel technologies including phononic logic, thermal management, and energy harvesting. A solid-state solution to rapidly manipulate phonons has escaped the scientific community. We demonstrate active and reversible tuning of thermal conductivity by manipulating the nanoscale ferroelastic domain structure of a Pb(Zr0.3Ti0.7)O3 film with applied electric fields. With subsecond response times, the room-temperature thermal conductivity was modulated by 11%.
We study the interplay between the contributions of electron thermal flux and interface scattering to the Kapitza conductance across metal-metal interfaces through measurements of thermal conductivity of copper-niobium multilayers. Thermal conductivities of copper-niobium multilayer films of period thicknesses ranging from 5.4 to 96.2 nm and sample thicknesses ranging from 962 to 2677 nm are measured by time-domain thermoreflectance over a range of temperatures from 78 to 500 K. The Kapitza conductances between the Cu and Nb interfaces in multilayer films are determined from the thermal conductivities using a series resistor model and are in good agreement with the electron diffuse mismatch model. Our results for the thermal boundary conductance between Cu and Nb are compared to literature values for the thermal boundary conductance across Al-Cu and Pd-Ir interfaces, and demonstrate that the interface conductance in metallic systems is dictated by the temperature derivative of the electron energy flux in the metallic layers, rather than electron mean free path or scattering processes at the interface.
Sachet, Edward; Shelton, Christopher T.; Harris, Joshua S.; Gaddy, Benjamin E.; Irving, Douglas L.; Curtarolo, Stefano; Donovan, Brian F.; Hopkins, Patrick E.; Sharma, Peter A.; Sharma, Ana L.; Ihlefeld, Jon I.; Franzen, Stefan; Maria, Jon P.
The interest in plasmonic technologies surrounds many emergent optoelectronic applications, such as plasmon lasers, transistors, sensors and information storage. Although plasmonic materials for ultraviolet-visible and near-infrared wavelengths have been found, the mid-infrared range remains a challenge to address: few known systems can achieve subwavelength optical confinement with low loss in this range. With a combination of experiments and ab initio modelling, here we demonstrate an extreme peak of electron mobility in Dy-doped CdO that is achieved through accurate 'defect equilibrium engineering'. In so doing, we create a tunable plasmon host that satisfies the criteria for mid-infrared spectrum plasmonics, and overcomes the losses seen in conventional plasmonic materials. In particular, extrinsic doping pins the CdO Fermi level above the conduction band minimum and it increases the formation energy of native oxygen vacancies, thus reducing their populations by several orders of magnitude. The substitutional lattice strain induced by Dy doping is sufficiently small, allowing mobility values around 500 cm2 V-1 s-1 for carrier densities above 1020 cm-3. Our work shows that CdO:Dy is a model system for intrinsic and extrinsic manipulation of defects affecting electrical, optical and thermal properties, that oxide conductors are ideal candidates for plasmonic devices and that the defect engineering approach for property optimization is generally applicable to other conducting metal oxides.
We have measured the cross-plane thermal conductivity (κ) of (010)-textured, undoped, and lanthanum-doped strontium niobate (Sr2-xLaxNb2O7-δ) thin films via time-domain thermoreflectance. The thin films were deposited on (001)-oriented SrTiO3 substrates via the highly-scalable technique of chemical solution deposition. We find that both film thickness and lanthanum doping have little effect on κ, suggesting that there is a more dominant phonon scattering mechanism present in the system; namely the weak interlayer-bonding along the b-axis in the Sr2Nb2O7 parent structure. Furthermore, we compare our experimental results with two variations of the minimum-limit model for κ and discuss the nature of transport in material systems with weakly-bonded layers. The low cross-plane κ of these scalably-fabricated films is comparable to that of similarly layered niobate structures grown epitaxially.
Henriques, Alexandra; Graham, Joseph T.; Landsberger, Sheldon; Ihlefeld, Jon I.; Brennecka, Geoffrey L.; Brown, Donald W.; Forrester, Jennifer S.; Jones, Jacob L.
Piezoelectric and ferroelectric materials are useful as the active element in non-destructive monitoring devices for high-radiation areas. Here, crystallographic structural refinement (i.e., the Rietveld method) is used to quantify the type and extent of structural changes in PbZr0.5Ti0.5O3 after exposure to a 1 MeV equivalent neutron fluence of 1.7×1015 neutrons/cm2. The results showa measurable decrease in the occupancy of Pb and O due to irradiation, with O vacancies in the tetragonal phase being created preferentially on one of the two Osites. The results demonstrate a method by which the effects of radiation on crystallographic structure may be investigated.