Thermoelectric Phenomena in Quantum Dots

Thermoelectricity is being intensively researched as it is believed to hold great promise for applications in power generation and cooling. One way to quantify the electrical power output of a thermoelectric material is the power factor, a function of electrical conductivity and thermopower. There are relationships between these relevant material properties that make efficient thermoelectric materials challenging to produce. The development of methods for creating nanostructured materials has allowed such trade-offs in material properties to be circumvented. Quantum dots are useful as model systems in this context since they have tunable energy filtering effects that are straightforward to characterize. The work described in this thesis explores thermoelectric phenomena in quantum dots. The aim of this work was to gain a better understanding of the most basic thermoelectric behavior of quantum dots. This knowledge can provide deeper insight into which mechanisms may be of interest in increasing the efficiency of a thermoelectric material. A deeper understanding also allows the measurement method itself to be used as a tool for characterization. A thermoelectric measurement can complement the more commonly used electrical conductance measurements, by both confirming and supplementing data. This could be of great importance for the investigation of physical phenomena in nanostructures. The quantum dots used in this work were defined in semiconductor nanowires. They were formed either by heterostructure growth or afterwards during fabrication of devices. The thermoelectric properties of the quantum dots were thoroughly investigated in the Coulomb blockade regime, and both linear and nonlinear responses as a function of the applied thermal gradient were observed and explained. Thermoelectric measurements were also successfully used to characterize different InAs nanowire devices, either with the nanowire as is or covered by a polymer electrolyte. Closer investigations of these devices revealed physical properties of the nanowires that could be used to improve thermoelectric efficiency. In fact, this thesis presents the first measurements demonstrating an increase in thermoelectric power factor at low temperatures

Nonlinear thermoelectric response due to energy-dependent transport properties of a quantum dot

Quantum dots are useful model systems for studying quantum thermoelectric behavior because of their highly energy-dependent electron transport properties, which are tunable by electrostatic gating. As a result of this strong energy dependence, the thermoelectric response of quantum dots is expected to be nonlinear with respect to an applied thermal bias. However, until now this effect has been challenging to observe because, first, it is experimentally difficult to apply a sufficiently large thermal bias at the nanoscale and, second, it is difficult to distinguish thermal bias effects from purely temperature-dependent effects due to overall heating of a device. Here we take advantage of a novel thermal biasing technique and demonstrate a nonlinear thermoelectric response in a quantum dot which is defined in a heterostructured semiconductor nanowire. We also show that a theoretical model based on the Master equations fully explains the observed nonlinear thermoelectric response given the energy-dependent transport properties of the quantum dot.Comment: Cite as: A. Svilans, et al., Physica E (2015), http://dx.doi.org/10.1016/j.physe.2015.10.00

Using polymer electrolyte gates to set-and-freeze threshold voltage and local potential in nanowire-based devices and thermoelectrics

We use the strongly temperature-dependent ionic mobility in polymer electrolytes to 'freeze in' specific ionic charge environments around a nanowire using a local wrap-gate geometry. This enables us to set both the threshold voltage for a conventional doped substrate gate and the local disorder potential at temperatures below 200 Kelvin, which we characterize in detail by combining conductance and thermovoltage measurements with modeling. Our results demonstrate that local polymer electrolyte gates are compatible with nanowire thermoelectrics, where they offer the advantage of a very low thermal conductivity, and hold great potential towards setting the optimal operating point for solid-state cooling applications.Comment: Published in Advanced Functional Materials. Includes colour versions of figures and supplementary informatio

Fully tunable, non-invasive thermal biasing of gated nanostructures suitable for low-temperature studies.

There is much recent interest in the thermoelectric (TE) characterization of single nanostructures at low temperatures, because such measurements yield information that is complementary to traditional conductance measurements, and because they may lead to novel paradigms for TE energy conversion. However, previously reported techniques for thermal biasing of nanostructures are difficult to use at low temperatures because of unintended global device heating, the lack of ability to continuously tune the thermal bias, or limited compatibility with gating techniques. By placing a heater directly on top of the electrical contact to a single InAs nanowire, we demonstrate fully tunable thermal biases of up to several tens of Kelvin, combined with negligible overall heating of the device, and with full functionality of a back gate, in the temperature range between 4 K and 300 K

Control and understanding of kink formation in InAs-InP heterostructure nanowires.

Nanowire heterostructures are of special interest for band structure engineering due to an expanded range of defect-free material combinations. However, the higher degree of freedom in nanowire heterostructure growth comes at the expense of challenges related to nanowire-seed particle interactions, such as undesired composition, grading and kink formation. To better understand the mechanisms of kink formation in nanowires, we here present a detailed study of the dependence of heterostructure nanowire morphology on indium pressure, nanowire diameter, and nanowire density. We investigate InAs-InP-InAs heterostructure nanowires grown with chemical beam epitaxy, which is a material system that allows for very abrupt heterointerfaces. Our observations indicate that the critical parameter for kink formation is the availability of indium, and that the resulting morphology is also highly dependent on the length of the InP segment. It is shown that kinking is associated with the formation of an inclined facet at the interface between InP and InAs, which destabilizes the growth and leads to a change in growth direction. By careful tuning of the growth parameters, it is possible to entirely suppress the formation of this inclined facet and thereby kinking at the heterointerface. Our results also indicate the possibility of producing controllably kinked nanowires with a high yield