M. R. Wagner

Reduction of the thermal conductivity in free-standing silicon nano-membranes investigated by non-invasive Raman thermometry

We report on the reduction of the thermal conductivity in ultra-thin suspended Si membranes with high crystalline quality. A series of membranes with thicknesses ranging from 9 nm to 1.5 μm was investigated using Raman thermometry, a novel contactless technique for thermal conductivity determination. A systematic decrease in the thermal conductivity was observed as reducing the thickness, which is explained using the Fuchs-Sondheimer model through the influence of phonon boundary scattering at the surfaces. The thermal conductivity of the thinnest membrane with d = 9 nm resulted in (9 ± 2) W/mK, thus approaching the amorphous limit but still maintaining a high crystalline quality.

Lithium related deep and shallow acceptors in Li-doped ZnO nanocrystals

We study the existence of Li-related shallow and deep acceptor levels in Li-doped ZnO nanocrystals using electron paramagnetic resonance (EPR) and photoluminescence (PL) spectroscopy. ZnO nanocrystals with adjustable Li concentrations between 0% and 12% have been prepared using organometallic precursors and show a significant lowering of the Fermi energy upon doping. The deep Li acceptor with an acceptor energy of 800 meV could be identified in both EPR and PL measurements and is responsible for the yellow luminescence at 2.2 eV. Additionally, a shallow acceptor state at 150 meV above the valence band maximum is made responsible for the observed donor-acceptor pair and free electron-acceptor transitions at 3.235 and 3.301 eV, possibly stemming from the formation of Li-related defect complexes acting as acceptors.

Tuning thermal transport in ultrathin silicon membranes by surface nanoscale engineering

A detailed understanding of the connections of fabrication and processing to structural and thermal properties of low-dimensional nanostructures is essential to design materials and devices for phononics, nanoscale thermal management, and thermoelectric applications. Silicon provides an ideal platform to study the relations between structure and heat transport since its thermal conductivity can be tuned over 2 orders of magnitude by nanostructuring. Combining realistic atomistic modeling and experiments, we unravel the origin of the thermal conductivity reduction in ultrathin suspended silicon membranes, down to a thickness of 4 nm. Heat transport is mostly controlled by surface scattering: rough layers of native oxide at surfaces limit the mean free path of thermal phonons below 100 nm. Removing the oxide layers by chemical processing allows us to tune the thermal conductivity over 1 order of magnitude. Our results guide materials design for future phononic applications, setting the length scale at which nanostructuring affects thermal phonons most effectively.

A novel contactless technique for thermal field mapping and thermal conductivity determination: two-laser Raman thermometry.

We present a novel contactless technique for thermal conductivity determination and thermal field mapping based on creating a thermal distribution of phonons using a heating laser, while a second laser probes the local temperature through the spectral position of a Raman active mode. The spatial resolution can be as small as 300 nm, whereas its temperature accuracy is ±2 K. We validate this technique investigating the thermal properties of three free-standing single crystalline Si membranes with thickness of 250, 1000, and 2000 nm. We show that for two-dimensional materials such as free-standing membranes or thin films, and for small temperature gradients, the thermal field decays as T(r) ∝ ln(r) in the diffusive limit. The case of large temperature gradients within the membranes leads to an exponential decay of the thermal field, T ∝ exp[ - A·ln(r)]. The results demonstrate the full potential of this new contactless method for quantitative determination of thermal properties. The range of materials to which this method is applicable reaches far beyond the here demonstrated case of Si, as the only requirement is the presence of a Raman active mode.

Phonon deformation potentials in wurtzite GaN and ZnO determined by uniaxial pressure dependent Raman measurements

We report the phonon deformation potentials of wurtzite GaN and ZnO for all zone center optical phonon modes determined by Raman measurements as a function of uniaxial pressure. Despite all the structural and optical similarities between these two material systems, the pressure dependency of their vibrational spectra exhibits fundamental distinctions, which is attributed to their different bond ionicities. In addition, the LO-TO splitting of the A1 and E1 phonon modes is analyzed which yields insight into the uniaxial pressure dependency of Born’s transverse effective charge eT∗.

Temperature dependent photoluminescence of lateral polarity junctions of metal organic chemical vapor deposition grown GaN

We report on fundamental structural and optical properties of lateral polarity junctions in GaN. GaN with Ga- to N-polar junctions was grown on sapphire using an AlN buffer layer. Results from scanning electron microscopy and Raman spectroscopy measurements indicate a superior quality of the Ga-polar GaN. An extremely strong luminescence signal is observed at the inversion domain boundary (IDB). Temperature dependent micro photoluminescence measurements are used to reveal the recombination processes underlying this strong emission. At 5 K the emission mainly arises from a stripe along the inversion domain boundary with a thickness of 4-5 μm. An increase of the temperature initially leads to a narrowing to below 2 μm emission area width followed by a broadening at temperatures above 70 K. The relatively broad emission area at low temperatures is explained by a diagonal IDB. It is shown that all further changes in the emission area width are related to thermalization effects of carriers and defects attracte...

Two-Dimensional Phononic Crystals: Disorder Matters

The design and fabrication of phononic crystals (PnCs) hold the key to control the propagation of heat and sound at the nanoscale. However, there is a lack of experimental studies addressing the impact of order/disorder on the phononic properties of PnCs. Here, we present a comparative investigation of the influence of disorder on the hypersonic and thermal properties of two-dimensional PnCs. PnCs of ordered and disordered lattices are fabricated of circular holes with equal filling fractions in free-standing Si membranes. Ultrafast pump and probe spectroscopy (asynchronous optical sampling) and Raman thermometry based on a novel two-laser approach are used to study the phononic properties in the gigahertz (GHz) and terahertz (THz) regime, respectively. Finite element method simulations of the phonon dispersion relation and three-dimensional displacement fields furthermore enable the unique identification of the different hypersonic vibrations. The increase of surface roughness and the introduction of short-range disorder are shown to modify the phonon dispersion and phonon coherence in the hypersonic (GHz) range without affecting the room-temperature thermal conductivity. On the basis of these findings, we suggest a criteria for predicting phonon coherence as a function of roughness and disorder.

Nanoscale imaging of InN segregation and polymorphism in single vertically aligned InGaN/GaN multi quantum well nanorods by tip-enhanced Raman scattering

Vertically aligned GaN nanorod arrays with nonpolar InGaN/GaN multi quantum wells (MQW) were grown by MOVPE on c-plane GaN-on-sapphire templates. The chemical and structural properties of single nanorods are optically investigated with a spatial resolution beyond the diffraction limit using tip-enhanced Raman spectroscopy (TERS). This enables the local mapping of variations in the chemical composition, charge distribution, and strain in the MQW region of the nanorods. Nanoscale fluctuations of the In content in the InGaN layer of a few percent can be identified and visualized with a lateral resolution below 35 nm. We obtain evidence for the presence of indium clustering and the formation of cubic inclusions in the wurtzite matrix near the QW layers. These results are directly confirmed by high-resolution TEM images, revealing the presence of stacking faults and different polymorphs close to the surface near the MQW region. The combination of TERS and HRTEM demonstrates the potential of this nanoscale near-field imaging technique, establishing TERS as a very potent, comprehensive, and nondestructive tool for the characterization and optimization of technologically relevant semiconductor nanostructures.

Reduction of the transverse effective charge of optical phonons in ZnO under pressure

From Raman scattering on a-plane wurtzite ZnO crystals we obtained a decreasing splitting between longitudinal and transversal optical phonons with A1 and E1 symmetry as a function of hydrostatic pressure up to 5.5 GPa. Consequently, the transverse effective charge (eT∗) exhibits a strong reduction with increasing pressure, yielding 2.17–14.6×10−3 P/GPa and 2.04–13.7×10−3 P/GPa (in units of the elementary charge) for the A1 and E1 phonons, respectively. We find a clear systematic in the linear pressure coefficient of eT∗ with bond polarity for the series of wide-band gap semiconductors SiC, AlN, GaN, and ZnO.

Structural and optical investigation of non-polar (1-100) GaN grown by the ammonothermal method

We studied the structural and optical properties of state-of-the-art non-polar bulk GaN grown by the ammonothermal method. The investigated samples have an extremely low dislocation density (DD) of less than 5 × 104 cm−2, which results in very narrow high-resolution x-ray rocking curves. The a and c lattice parameters of these stress-free GaN samples were precisely determined by using an x-ray diffraction technique based on the modified Bond method. The obtained values are compared to the lattice parameters of free-standing GaN from different methods and sources. The observed differences are discussed in terms of free-electron concentrations, point defects, and DD. Micro Raman spectroscopy revealed a very narrow phonon linewidth and negligible built-in strain in accordance with the high-resolution x-ray diffraction data. The optical transitions were investigated by cathodoluminescence measurements. The analysis of the experimental data clearly demonstrates the excellent crystalline perfection of ammonothe...