Manipulating phonons at the nanoscale: Impurities and boundaries

Efficiently controlling phonon propagation is important in many applications, ranging from the design of thermoelectric materials to thermal budget engineering. Phonon manipulation, nonetheless, has proved to be an elusive task. Here, we review some basic strategies to alter vibrational modes throughout the entire phonon spectrum by means of point and extended defects, boundaries, and design of periodic superstructures. These individual scattering mechanisms allow altering the phononic properties in specific spectral regions; combining two or more can lead to a modification of the full-spectrum

Phonon Transport in GaAs and InAs Twinning Superlattices

Crystal phase engineering gives access to new types of periodic nanostructures, such as the so-called twinning superlattices, where the motif of the superlattice is determined by a periodic rotation of the crystal. Here, by means of atomistic nonequilibrium molecular dynamics calculations, we study to what extent these periodic systems can be used to alter phonon transport in a controlled way, similar to what has been predicted and observed in conventional superlattices based on heterointerfaces. We focus on twinning superlattices in GaAs and InAs and highlight the existence of two different transport regimes: in one, each interface behaves like an independent scatterer; in the other, a segment with a sufficiently large number of closely spaced interfaces is seen by propagating phonons as a metamaterial with its own thermal properties. In this second scenario, we distinguish the case where the phonon mean free path is smaller or larger than the superlattice segment, pointing out a different dependence of the thermal resistance with the number of interfaces

Effects of Dielectric Stoichiometry on the Photoluminescence Properties of Encapsulated WSe2 Monolayers

Two-dimensional transition-metal-dichalcogenide semiconductors have emerged as promising candidates for optoelectronic devices with unprecedented properties and ultra-compact performances. However atomically thin materials are highly sensitive to surrounding dielectric media, which imposes severe limitations to their practical applicability. Hence for their suitable integration into devices, the development of reliable encapsulation procedures that preserve their physical properties are required. Here, the excitonic photoluminescence of WSe2 monolayer flakes is assessed, at room temperature and 10 K, on mechanically exfoliated flakes encapsulated with SiOx and AlxOy layers employing chemical and physical deposition techniques. Conformal flakes coating on untreated - non-functionalized - flakes is successfully demonstrated by all the techniques except for atomic layer deposition, where a cluster-like oxide coating is observed. No significant compositional or strain state changes in the flakes are detected upon encapsulation by any of the techniques. Remarkably, our results evidence that the flakes' optical emission is strongly influenced by the quality of the encapsulating oxide - stoichiometry -. When the encapsulation is carried out with slightly sub-stoichiometric oxides two remarkable phenomena are observed. First, there is a clear electrical doping of the monolayers that is revealed through a dominant trion - charged exciton - room-temperature photoluminescence. Second, a strong decrease of the monolayers optical emission is measured attributed to non-radiative recombination processes and/or carriers transfer from the flake to the oxide. Power- and temperature-dependent photoluminescence measurements further confirm that stoichiometric oxides obtained by physical deposition lead to a successful encapsulation.Comment: 30 pages, 6 figure

Single-step Au-catalysed synthesis and microstructural characterization of core-shell Ge/In-Te nanowires by MOCVD

We report on the self-assembly of core-shell Ge/In-Te nanowires (NWs) on single crystal Si substrates by Metalorganic Chemical Vapour Deposition (MOCVD), coupled to the Vapour-Liquid-Solid (VLS) mechanism, catalysed by Au nanoparticles (NPs). The NWs are formed by a crystalline Ge core and an InTe (II) shell, have diameters down to 15 nm and show <110> oriented growth direction. The role of the MOCVD process parameters and of the NPs size in determining the NWs core-shell microstructure and their alignment was investigated by high-resolution TEM, EDX, XRD and Raman spectroscopy

Spatially mapping thermal transport in graphene by an opto-thermal method

Mapping the thermal transport properties of materials at the nanoscale is of critical importance for optimizing heat conduction in nanoscale devices. Several methods to determine the thermal conductivity of materials have been developed, most of them yielding an average value across the sample, thereby disregarding the role of local variations. Here, we present a method for the spatially resolved assessment of the thermal conductivity of suspended graphene by using a combination of confocal Raman thermometry and a finite-element calculations-based fitting procedure. We demonstrate the working principle of our method by extracting the two-dimensional thermal conductivity map of one pristine suspended single-layer graphene sheet and one irradiated using helium ions. Our method paves the way for spatially resolving the thermal conductivity of other types of layered materials. This is particularly relevant for the design and engineering of nanoscale thermal circuits (e.g. thermal diodes)

In-plane thermal diffusivity determination using beam-offset frequency-domain thermoreflectance with a one-dimensional optical heat source

We present an innovative contactless method suitable to study in-plane thermal transport based on beam-offset frequency-domain thermoreflectance using a one-dimensional heat source with uniform power distribution. Using a one-dimensional heat source provides a number of advantages as compared to point-like heat sources, as typically used in time- and frequency-domain thermoreflectance experi- ments, just to name a few: (i) it leads to a slower spatial decay of the temperature field in the direction perpendicular to the line-shaped heat source, allowing to probe the temperature field at larger distances from the heater, hence, enhancing the sensitivity to in-plane thermal transport; (ii) the frequency range of interest is typically < 100 kHz. This rather low frequency range is convenient regarding the cost of the required excitation laser system but, most importantly, it allows the study of materials without the presence of a metallic transducer with almost no influence of the finite optical penetration depth of the pump and probe beams on the thermal phase lag, which arises from the large thermal penetration depth imposed by the used frequency range. We also show that for the case of a harmonic thermal excitation source, the phase lag between the thermal excitation and thermal response of the sample exhibits a lin- ear dependence with their spatial offset, where the slope is proportional to the inverse of the thermal diffusivity of the material. We demonstrate the applicability of this method to the cases of: (i) suspended thin films of Si and PDPP4T, (ii) Bi bulk samples, and (iii) Si, glass, and highly-oriented pyrollitic graphite (HOPG) bulk samples with a thin metallic transducer. Finally, we also show that it is possible to study in-plane heat transport on substrates with rather low thermal diffusivity, e.g., glass, even using a metallic transducer. We achieve this by an original approach based on patterning the transducer using focused ion beam, with the key purpose of limiting in-plane heat transport through the thin metallic transducer

Low-Charge-Noise Nitrogen-Vacancy Centers in Diamond Created Using Laser Writing with a Solid-Immersion Lens

We report on pulsed-laser-induced generation of nitrogen-vacancy (NV) centers in diamond facilitated by a solid-immersion lens (SIL). The SIL enables laser writing at energies as low as 5.8 nJ per pulse and allows vacancies to be formed close to a diamond surface without inducing surface graphitization. We operate in the previously unexplored regime, where lattice vacancies are created following tunneling breakdown rather than multiphoton ionization. We present three samples in which NV center arrays were laser-written at distances between similar to 1 and 40 mu m from a diamond surface, all presenting narrow distributions of optical linewidths with means between 62.1 and 74.5 MHz. The linewidths include the effect of long-term spectral diffusion induced by a 532 nm repump laser for charge-state stabilization, thereby emphasizing the particularly low-charge-noise environment of the created color centers. Such high-quality NV centers are excellent candidates for practical applications employing two-photon quantum interference with separate NV centers. Finally, we propose a model for disentangling power broadening from inhomogeneous broadening in the NV center optical linewidth