Colloidal semiconductor nanocrystals are promising luminophores for creating a new generation of electroluminescence devices. Research on semiconductor nanocrystal based light-emitting diodes (LEDs) has made remarkable advances in just one decade: the external quantum efficiency has improved by over two orders of magnitude and highly saturated color emission is now the norm. Although the device efficiencies are still more than an order of magnitude lower than those of the purely organic LEDs there are potential advantages associated with nanocrystal-based devices, such as a spectrally pure emission color, which will certainly merit future research. Further developments of nanocrystal-based LEDs will be improving material stability, understanding and controlling chemical and physical phenomena at the interfaces, and optimizing charge injection and charge transport.
Knowledge of the mean-free-path distribution of heat-carrying phonons is key to understanding phononmediated thermal transport. We demonstrate that thermal conductivity measurements of thin membranes spanning a wide thickness range can be used to characterize how bulk thermal conductivity is distributed over phonon mean free paths. A noncontact transient thermal grating technique was used to measure the thermal conductivity of suspended Si membranes ranging from 15-1500 nm in thickness. A decrease in the thermal conductivity from 74-13% of the bulk value is observed over this thickness range, which is attributed to diffuse phonon boundary scattering. Due to the well-defined relation between the membrane thickness and phonon mean-free-path suppression, combined with the range and accuracy of the measurements, we can reconstruct the bulk thermal conductivity accumulation vs. phonon mean free path, and compare with theoretical models.
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.
We present a multiscale ab initio study of electronic and transport properties of two-dimensional graphene after epoxide functionalization via ozone treatment. The orbital rehybridization induced by the epoxide groups triggers a strong intervalley scattering and changes dramatically the conduction properties of graphene. By varying the coverage density of epoxide defects from 0.1 to 4%, charge conduction can be tuned from a diffusive to a strongly localized regime, with localization lengths down to a few nanometers long. Experimental results supporting the interpretation as a metal-insulator transition are also provided.
We present a magnetotransport study of graphene samples into which a mild disorder was introduced by exposure to ozone. Unlike the conductivity of pristine graphene, the conductivity of graphene samples exposed to ozone becomes very sensitive to temperature: it decreases by more than three orders of magnitude between 100 and 1 K. By varying either an external gate voltage or temperature, we continuously tune the transport properties from the weak to the strong localization regime. We show that the transition occurs as the phase coherence length becomes comparable to the localization length. We also highlight the important role of disorder-enhanced electron-electron interaction on the resistivity.
We study the relaxation of coherent acoustic phonon modes with frequencies up to 500 GHz in ultra-thin free-standing silicon membranes. Using an ultrafast pump-probe technique of asynchronous optical sampling, we observe that the decay time of the first-order dilatational mode decreases significantly from ∼ 4.7 ns to 5 ps with decreasing membrane thickness from ∼ 194 to 8 nm. The experimental results are compared with theories considering both intrinsic phonon-phonon interactions and extrinsic surface roughness scattering including a wavelength-dependent specularity. Our results provide insight to understand some of the limits of nanomechanical resonators and thermal transport in nanostructures.Mechanical and acoustic properties in the nanoscale are receiving increasing attention as they are key properties affecting the limits of ultrasensitive detectors of force [1], mass [2,3], charge [4,5] and spin [6], influencing platforms for biosensing [7] and the investigation of quantum behaviour in extended objects [8]. In particular, phonon lifetimes influence the achievable mechanical quality (Q) -factors in nanomechanical resonators, which often limit device performance [9]. Moreover, they are necessary input parameters for accurate calculations of nanoscale thermal transport, with high-impact applications such as heat management in nanoelectronics [10] and the engineering of novel thermoelectric materials [11]. Despite their importance, phonon lifetimes are perhaps the least well known of all phonon properties due to the challenges associated with their quantitative determination and theoretical modelling. Even though silicon is the most important material for nanoelectronics, MEMS and NEMS, there are few experimental reports of direct measurements of phonon lifetimes in the gigahertz to terahertz range [12] and for all materials open questions remain about the relative contributions of intrinsic and extrinsic scattering processes at high frequencies in both bulk and nanoscale structures [9,[13][14][15][16]. Recent experimental investigations of phonons in superlattice cavities with frequencies of around 1 THz have suggested that lifetimes of high-frequency phonons could be limited by an average interface roughness of just 0.06 nm [17]. On the other hand, phonon wavepackets experiments in bulk silicon with frequencies up to approximately 100 GHz were analysed with a simplified Akhiezer relaxation damping model [12,18] of intrinsic scattering, using an average lifetime of high-frequency thermal phonons of 17 ps. Other intrinsic damping models include clamping losses [19], thermoelastic dissipation [20] and three-phonon interactions [21], which predict a different behaviour depending on the frequency and temperature regimes. In this context, generation and detection of coherent acoustic phonons at high frequencies in different materials and nanostructures is an ideal method to obtain quantitative information on phonon lifetimes and compare with the main theoretical models.Here we use free-standing single-crystalline ...
Recent years have witnessed the boom of cavity optomechanics, which exploits the confinement and coupling of optical and mechanical waves at the nanoscale. Among their physical implementations, optomechanical (OM) crystals built on semiconductor slabs enable the integration and manipulation of multiple OM elements in a single chip and provide gigahertz phonons suitable for coherent phonon manipulation. Different demonstrations of coupling of infrared photons and gigahertz phonons in cavities created by inserting defects on OM crystals have been performed. However, the considered structures do not show a complete phononic bandgap, which should enable longer lifetimes, as acoustic leakage is minimized. Here we demonstrate the excitation of acoustic modes in a one-dimensional OM crystal properly designed to display a full phononic bandgap for acoustic modes at 4 GHz. The modes inside the complete bandgap are designed to have high-mechanical Q-factors, limit clamping losses and be invariant to fabrication imperfections.
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