Enhanced Thermal Boundary Conductance across GaN/SiC Interfaces with AlN Transition Layers.

Heat dissipation plays a crucial role in the performance and reliability of high-power GaN-based electronics. While AlN transition layers are commonly employed in the heteroepitaxial growth of GaN-on-SiC substrates, concerns have been raised about their impact on thermal transport across GaN/SiC interfaces. In this study, we present experimental measurements of the thermal boundary conductance (TBC) across GaN/SiC interfaces with varying thicknesses of the AlN transition layer (ranging from 0 to 73 nm) at different temperatures. Our findings reveal that the addition of an AlN transition layer leads to a notable increase in the TBC of the GaN/SiC interface, particularly at elevated temperatures. Structural characterization techniques are employed to understand the influence of the AlN transition layer on the crystalline quality of the GaN layer and its potential effects on interfacial thermal transport. To gain further insights into the trend of TBC, we conduct molecular dynamics simulations using high-fidelity deep learning-based interatomic potentials, which reproduce the experimentally observed enhancement in TBC even for atomically perfect interfaces. These results suggest that the enhanced TBC facilitated by the AlN intermediate layer could result from a combination of improved crystalline quality at the interface and the "phonon bridge" effect provided by AlN that enhances the overlap between the vibrational spectra of GaN and SiC.

Borazine Promoted Growth of Highly Oriented Thin Films.

We report on a phenomenon, where thin films sputter-deposited on single-crystalline Al2O3(0001) substrates exposed to borazine─a precursor commonly used for the synthesis of hexagonal boron nitride layers─are more highly oriented than those grown on bare Al2O3(0001) under the same conditions. We observed this phenomenon in face-centered cubic Pd, body-centered cubic Mo, and trigonal Ta2C thin films grown on Al2O3(0001). Interestingly, intermittent exposure to borazine during the growth of Ta2C thin films on Ta2C yields better crystallinity than direct deposition of monolithic Ta2C. We attribute these rather unusual results to a combination of both enhanced adatom mobilities on, and epitaxial registry with, surfaces exposed to borazine during the deposition. We expect that our approach can potentially help improve the crystalline quality of thin films deposited on a variety of substrates.

Experimental evidence of auxeticity in ion implanted single crystal calcite.

We report initial experimental evidence of auxeticity in calcite by ion implanting (1010) oriented single crystalline calcite with Ar+ at room temperature using an ion energy of 400 keV and a dose of 1 × 1014 cm-2. Lattice compression normal to the substrate surface was observed, which is an atypical result for ion implanted materials. The auxetic behavior is consistent with predictions that indicate auxeticity had been predicted along two crystallographic directions including [1010]. Materials with a positive Poisson's ratio experience lattice expansion normal to the substrate surface when ion implanted, whereas lattice contraction normal to the surface is evidence of auxetic behavior. Triple-axis X-ray diffraction measurements confirmed the auxetic strain state of the implanted calcite substrates. Reciprocal space maps for the symmetric 3030 and asymmetric 1450 reflections revealed that the implanted region was fully strained (pseudomorphic) to the bulk of the substrate, as is typical with implanted single crystals. A symmetric (3030) ω:2θ line scan was used with X-ray dynamical diffraction simulations to model the strain profile and extract the variation of compressive strain as a function of depth normal to the substrate surface. SRIM calculations were performed to obtain a displacement-per-atom profile and implanted Ar+ concentration profile. It was found that the strain profile matches the displacement-per-atom profile. This study demonstrated the use of ion implantation and X-ray diffraction methods to probe mechanical properties of materials and to test predictions such as the auxeticity.

Experimental observation of localized interfacial phonon modes.

Interfaces impede heat flow in micro/nanostructured systems. Conventional theories for interfacial thermal transport were derived based on bulk phonon properties of the materials making up the interface without explicitly considering the atomistic interfacial details, which are found critical to correctly describing thermal boundary conductance. Recent theoretical studies predicted the existence of localized phonon modes at the interface which can play an important role in understanding interfacial thermal transport. However, experimental validation is still lacking. Through a combination of Raman spectroscopy and high-energy-resolution electron energy-loss spectroscopy in a scanning transmission electron microscope, we report the experimental observation of localized interfacial phonon modes at ~12 THz at a high-quality epitaxial Si-Ge interface. These modes are further confirmed using molecular dynamics simulations with a high-fidelity neural network interatomic potential, which also yield thermal boundary conductance agreeing well with that measured in time-domain thermoreflectance experiments. Simulations find that the interfacial phonon modes have an obvious contribution to the total thermal boundary conductance. Our findings significantly contribute to the understanding of interfacial thermal transport physics and have impact on engineering thermal boundary conductance at interfaces in applications such as electronics thermal management and thermoelectric energy conversion.

Surface Reconstruction of Halide Perovskites During Post-treatment.

Postfabrication surface treatment strategies have been instrumental to the stability and performance improvements of halide perovskite photovoltaics in recent years. However, a consensus understanding of the complex reconstruction processes occurring at the surface is still lacking. Here, we combined complementary surface-sensitive and depth-resolved techniques to investigate the mechanistic reconstruction of the perovskite surface at the microscale level. We observed a reconstruction toward a more PbI2-rich top surface induced by the commonly used solvent isopropyl alcohol (IPA). We discuss several implications of this reconstruction on the surface thermodynamics and energetics. Particularly, our observations suggest that IPA assists in the adsorption process of organic ammonium salts to the surface to enhance their defect passivation effects.

High In-Plane Thermal Conductivity of Aluminum Nitride Thin Films.

High thermal conductivity materials show promise for thermal mitigation and heat removal in devices. However, shrinking the length scales of these materials often leads to significant reductions in thermal conductivities, thus invalidating their applicability to functional devices. In this work, we report on high in-plane thermal conductivities of 3.05, 3.75, and 6 µm thick aluminum nitride (AlN) films measured via steady-state thermoreflectance. At room temperature, the AlN films possess an in-plane thermal conductivity of ∼260 ± 40 W m-1 K-1, one of the highest reported to date for any thin film material of equivalent thickness. At low temperatures, the in-plane thermal conductivities of the AlN films surpass even those of diamond thin films. Phonon-phonon scattering drives the in-plane thermal transport of these AlN thin films, leading to an increase in thermal conductivity as temperature decreases. This is opposite of what is observed in traditional high thermal conductivity thin films, where boundaries and defects that arise from film growth cause a thermal conductivity reduction with decreasing temperature. This study provides insight into the interplay among boundary, defect, and phonon-phonon scattering that drives the high in-plane thermal conductivity of the AlN thin films and demonstrates that these AlN films are promising materials for heat spreaders in electronic devices.

Author Correction: Solid-phase hetero epitaxial growth of α-phase formamidinium perovskite.

A Correction to this paper has been published: https://doi.org/10.1038/s41467-020-19846-y .

Solid-phase hetero epitaxial growth of α-phase formamidinium perovskite.

Conventional epitaxy of semiconductor films requires a compatible single crystalline substrate and precisely controlled growth conditions, which limit the price competitiveness and versatility of the process. We demonstrate substrate-tolerant nano-heteroepitaxy (NHE) of high-quality formamidinium-lead-tri-iodide (FAPbI3) perovskite films. The layered perovskite templates the solid-state phase conversion of FAPbI3 from its hexagonal non-perovskite phase to the cubic perovskite polymorph, where the growth kinetics are controlled by a synergistic effect between strain and entropy. The slow heteroepitaxial crystal growth enlarged the perovskite crystals by 10-fold with a reduced defect density and strong preferred orientation. This NHE is readily applicable to various substrates used for devices. The proof-of-concept solar cell and light-emitting diode devices based on the NHE-FAPbI3 showed efficiencies and stabilities superior to those of devices fabricated without NHE.

Thermal Transport across Ion-Cut Monocrystalline ß-Ga2O3 Thin Films and Bonded ß-Ga2O3-SiC Interfaces.

The ultrawide band gap, high breakdown electric field, and large-area affordable substrates make ß-Ga2O3 promising for applications of next-generation power electronics, while its thermal conductivity is at least 1 order of magnitude lower than other wide/ultrawide band gap semiconductors. To avoid the degradation of device performance and reliability induced by the localized Joule-heating, proper thermal management strategies are essential, especially for high-power high-frequency applications. This work reports a scalable thermal management strategy to heterogeneously integrate wafer-scale monocrystalline ß-Ga2O3 thin films on high thermal conductivity SiC substrates by the ion-cutting technique and room-temperature surface-activated bonding technique. The thermal boundary conductance (TBC) of the ß-Ga2O3-SiC interfaces and thermal conductivity of the ß-Ga2O3 thin films were measured by time-domain thermoreflectance to evaluate the effects of interlayer thickness and thermal annealing. Materials characterizations were performed to understand the mechanisms of thermal transport in these structures. The results show that the ß-Ga2O3-SiC TBC values are reasonably high and increase with decreasing interlayer thickness. The ß-Ga2O3 thermal conductivity increases more than twice after annealing at 800 °C because of the removal of implantation-induced strain in the films. A Callaway model is built to understand the measured thermal conductivity. Small spot-to-spot variations of both TBC and Ga2O3 thermal conductivity confirm the uniformity and high quality of the bonding and exfoliation. Our work paves the way for thermal management of power electronics and provides a platform for ß-Ga2O3-related semiconductor devices with excellent thermal dissipation.

Bulk-like Intrinsic Phonon Thermal Conductivity of Micrometer-Thick AlN Films.

Aluminum nitride (AlN) has garnered much attention due to its intrinsically high thermal conductivity. However, engineering thin films of AlN with these high thermal conductivities can be challenging due to vacancies and defects that can form during the synthesis. In this work, we report on the cross-plane thermal conductivity of ultra-high-purity single-crystal AlN films with different thicknesses (∼3-22 µm) via time-domain thermoreflectance (TDTR) and steady-state thermoreflectance (SSTR) from 80 to 500 K. At room temperature, we report a thermal conductivity of ∼320 ± 42 W m-1 K-1, surpassing the values of prior measurements on AlN thin films and one of the highest cross-plane thermal conductivities of any material for films with equivalent thicknesses, surpassed only by diamond. By conducting first-principles calculations, we show that the thermal conductivity measurements on our thin films in the 250-500 K temperature range agree well with the predicted values for the bulk thermal conductivity of pure single-crystal AlN. Thus, our results demonstrate the viability of high-quality AlN films as promising candidates for the high-thermal-conductivity layers in high-power microelectronic devices. Our results also provide insight into the intrinsic thermal conductivity of thin films and the nature of phonon-boundary scattering in single-crystal epitaxially grown AlN thin films. The measured thermal conductivities in high-quality AlN thin films are found to be constant and similar to bulk AlN, regardless of the thermal penetration depth, film thickness, or laser spot size, even when these characteristic length scales are less than the mean free paths of a considerable portion of thermal phonons. Collectively, our data suggest that the intrinsic thermal conductivity of thin films with thicknesses less than the thermal phonon mean free paths is the same as bulk so long as the thermal conductivity of the film is sampled independent of the film/substrate interface.

Ultra-high vacuum dc magnetron sputter-deposition of 0001-textured trigonal α-Ta2C/Al2O3(0001) thin films.

We report on the effects of substrate temperature (1073 K ≤ T s ≤ 1373 K) and deposition time t (= 3 ~ 30 min.) on the crystallinity of Ta2C/Al2O3(0001) thin films grown via ultra-high vacuum direct current magnetron sputtering of TaC target in 20 mTorr (2.7 Pa) pure Ar atmospheres. Using X-ray diffraction and transmission electron microscopy, we determine that the layers are 0001-oriented, trigonal-structured α-Ta2C at all T s. With increasing T s, we obtain smoother and thinner layers with enhanced out-of-plane coherency and decreasing unit cell volume. Interestingly, the Ta2C 0001 texture improves with increasing T s up to 1273 K above which the layers are relatively more polycrystalline. At T s = 1373 K, during early stages of deposition, the Ta2C layers grow heteroepitaxially on Al2O3(0001) with ( 0001 ) Ta 2 C ‖ ( 0001 ) Al 2 O 3 and [ 10 1 ¯ 0 ] Ta 2 C ‖ [ 11 2 ¯ 0 ] Al 2 O 3 . With increasing t, we observe the formation of anti-phase domains and misoriented grains resulting in polycrystalline layers. We attribute the observed enhancement in 0001 texture to increased surface adatom mobilities and the development of polycrystallinity to reduced incorporation of C in the lattice with increasing T s. We expect that our results help develop methods for the synthesis of high-quality Ta2C thin films.