More Like this

1. Tuning Electrical and Thermal Transport in AlGaN/GaN Heterostructures via Buffer Layer Engineering

   https://doi.org/10.1002/adfm.201705823  

   Yalamarthy, Ananth Saran ; So, Hongyun ; Muñoz Rojo, Miguel ; Suria, Ateeq J. ; Xu, Xiaoqing ; Pop, Eric ; Senesky, Debbie G. ( March 2018 , Advanced Functional Materials)

   Progress in wide bandgap, III–V material systems based on gallium nitride (GaN) has enabled the realization of high‐power and high‐frequency electronics. Since the highly conductive, 2D electron gas (2DEG) at the aluminum gallium nitride (AlGaN)/GaN interface is based on built‐in polarization fields and is confined to nanoscale thicknesses, its charge carriers exhibit much higher mobilities compared to their doped counterparts. This study shows that such 2DEGs also offer the unique ability to manipulate electrical transport separately from thermal transport, through the examination of fully suspended AlGaN/GaN diaphragms of varied GaN buffer layer thickness. Notably, ≈100 nm thin GaN layers can considerably impede heat flow without electrical transport degradation. These achieve 4× improvement in the thermoelectric figure of merit (zT) over externally doped GaN, with state‐of‐the‐art power factors of 4–7 mW m^‐1K^‐2. The remarkable tuning behavior and thermoelectric enhancement, elucidated here for the first time in a polarization‐based heterostructure, are achieved because electrons are at the heterostructured interface, while phonons are within the material system. These results highlight the potential for using 2DEGs in III–V materials for on‐chip thermal sensing and energy harvesting.

    

   more » « less
2. Nanoscale imaging of phonon dynamics by electron microscopy

   https://doi.org/10.1038/s41586-022-04736-8  

   Gadre, Chaitanya A. ; Yan, Xingxu ; Song, Qichen ; Li, Jie ; Gu, Lei ; Huyan, Huaixun ; Aoki, Toshihiro ; Lee, Sheng-Wei ; Chen, Gang ; Wu, Ruqian ; et al ( June 2022 , Nature)

   Abstract Spatially resolved vibrational mapping of nanostructures is indispensable to the development and understanding of thermal nanodevices 1 , modulation of thermal transport 2 and novel nanostructured thermoelectric materials 3–5 . Through the engineering of complex structures, such as alloys, nanostructures and superlattice interfaces, one can significantly alter the propagation of phonons and suppress material thermal conductivity while maintaining electrical conductivity 2 . There have been no correlative experiments that spatially track the modulation of phonon properties in and around nanostructures due to spatial resolution limitations of conventional optical phonon detection techniques. Here we demonstrate two-dimensional spatial mapping of phonons in a single silicon–germanium (SiGe) quantum dot (QD) using monochromated electron energy loss spectroscopy in the transmission electron microscope. Tracking the variation of the Si optical mode in and around the QD, we observe the nanoscale modification of the composition-induced red shift. We observe non-equilibrium phonons that only exist near the interface and, furthermore, develop a novel technique to differentially map phonon momenta, providing direct evidence that the interplay between diffuse and specular reflection largely depends on the detailed atomistic structure: a major advancement in the field. Our work unveils the non-equilibrium phonon dynamics at nanoscale interfaces and can be used to study actual nanodevices and aid in the understanding of heat dissipation near nanoscale hotspots, which is crucial for future high-performance nanoelectronics. 

   more » « less
3. Materials selection rules for optimum power factor in two-dimensional thermoelectrics

   https://doi.org/10.1088/2515-7639/ab4600  

   Kommini, Adithya ; Aksamija, Zlatan ( November 2019 , Journal of Physics: Materials)

   Two-dimensional (2D) materials have emerged as the ideal candidates for many applications, including nanoelectronics, low-power devices, and sensors. Several 2D materials have been shown to possess large Seebeck coefficients, thus making them suitable for thermoelectric (TE) energy conversion. Whether even higher TE power factors can be discovered among the ≈2000 possible 2D materials (Mounetet al2018Nat. Nanotechnol.13246–52) is an open question. This study aims at formulating selection rules to guide the search for superior 2D TE materials without the need for expensive atomistic simulations. We show that a 2D material having a combination of low effective mass, higher separation in the height of the step-like density of states, and valley splitting, which is the energy difference between the bottom of conduction band and the satellite valley, equal to 5k_BTwill lead to a higher TE power factor. Further, we find that inelastic scattering with optical phonons plays a significant role: if inelastic scattering is the dominant mechanism and the energy of the optical phonon equals 5k_BT, then the TE power factor is maximized. Starting from a model for carrier transport in MoS₂and progressively introducing the aforementioned features results in a two-orders-of-magnitude improvement in the power factor. Compared to the existing selection rules or material descriptors, features identified in this study provide the ability to comprehensively evaluate TE capability of a material and helps in identifying future TE materials suitable for applications in waste-heat scavenging, thermal sensors, and nanoelectronics cooling.

    

   more » « less
4. Size‐ and Temperature‐Dependent Suppression of Phonon Thermal Conductivity in Carbon Nanotube Thermoelectric Films

   https://doi.org/10.1002/aelm.202000746  

   Wesenberg, Devin J. ; Roos, Michael J. ; Avery, Azure D. ; Blackburn, Jeffrey L. ; Ferguson, Andrew J. ; Zink, Barry L. ( October 2020 , Advanced Electronic Materials)

   Heat transport in nanoscale carbon materials such as carbon nanotubes and graphene is normally dominated by phonons. Here, measurements of in‐plane thermal conductivity, electrical conductivity, and thermopower are presented from 77–350 K on two films with thickness <100 nm formed from semiconducting single‐walled carbon nanotubes. These measurements are made with silicon–nitride membrane thermal isolation platforms. The two films, formed from disordered networks of tubes with differing tube and bundle size, have very different thermal conductivity. One film matches a simple model of heat conduction assuming constant phonon velocity and mean free path, and 3D Debye heat capacity with a Debye temperature of 770 K. The second film shows a more complicated temperature dependence, with a dramatic drop in a relatively narrow window near 200 K where phonon contributions to thermal conductivity essentially vanish. This causes a corresponding large increase in thermoelectric figure‐of‐merit at the same temperature. A better understanding of this behavior can allow significant improvement in thermoelectric efficiency of these low‐cost earth‐abundant, organic electronic materials. Heat and charge conductivity near room temperature is also presented as a function of doping, which provides further information on the interaction of dopant molecules and phonon transport in disordered nanotube films.

    

   more » « less
5. Energy transfer and thermoelectricity in molecular junctions in non-equilibrated solvents

   https://doi.org/10.1063/5.0086319  

   Kirchberg, Henning ; Nitzan, Abraham ( March 2022 , The Journal of Chemical Physics)

   We consider a molecular junction immersed in a solvent where the electron transfer is dominated by Marcus-type steps. However, the successive nature of the charge transfer through the junction does not imply that the solvent reaches thermal equilibrium throughout the transport. In our previous work [Kirchberg et al., J. Phys. Chem. Lett. 11, 1729 (2020)], we have determined the nonequilibrium distribution of the solvent where its dynamics, expressed by a friction, is considered in two limiting regimes of fast and slow solvent relaxation. In dependence of the nonequilibrium solvent dynamics, we investigate now the electrical, thermal, and thermoelectric properties of the molecular junction. We show that by suitable tuning of the friction, we can reduce the heat dissipation into the solvent and enhance the heat transfer between the electrodes. Interestingly, we find that the Seebeck coefficient grows significantly by adapting the solvent friction in both regimes.

    

   more » « less