Large arrays of multifunctional rolled-up semiconductors can be mass produced with precisely controlled size and composition, making them of great technological interest for micro- and nano-scale device fabrication. The microtube behavior at different temperatures is a key factor towards further engineering their functionality, as well as for characterizing strain, defects, and temperature-dependent properties of the structures. For this purpose, we probe optical phonons of GaAs/InGaAs rolled-up microtubes using Raman spectroscopy on defect-rich (faulty) and defect-free microtubes. The microtubes are fabricated by selectively etching an AlAs sacrificial layer in order to release the strained InGaAs/GaAs bilayer, all grown by molecular beam epitaxy. Pristine microtubes show homogeneity of the GaAs and InGaAs peak positions and intensities along the tube, which indicates a defect-free rolling up process, while for a cone-like microtube, a downward shift of the GaAs LO phonon peak along the cone is observed. Formation of other type of defects, including partially unfolded microtubes, can also be related to a high Raman intensity of the TO phonon in GaAs. We argue that the appearance of the TO phonon mode is a consequence of further relaxation of the selection rules due to the defects on the tubes, which makes this phonon useful for failure detection/prediction in such rolled up systems. In order to systematically characterize the temperature stability of the rolled up microtubes, Raman spectra were acquired as a function of sample temperature up to 300[degree sign]C. The reversibility of the changes in the Raman spectra of the tubes within this temperature range is demonstrated.
In this study, we investigate the effect of annealing and nitrogen amount on electronic transport properties in n- and p-type-doped Ga0.68In0.32NyAs1 - y/GaAs quantum well (QW) structures with y = 0%, 0.9%, 1.2%, 1.7%. The samples are thermal annealed at 700°C for 60 and 600 s, and Hall effect measurements have been performed between 10 and 300 K. Drastic decrease is observed in the electron mobility of n-type N-containing samples due to the possible N-induced scattering mechanisms and increasing effect mass of the alloy. The temperature dependence of electron mobility has an almost temperature insensitive characteristic, whereas for p-type samples hole mobility is decreased drastically at T > 120 K. As N concentration is increased, the hole mobility also increased as a reason of decreasing lattice mismatch. Screening effect of N-related alloy scattering over phonon scattering in n-type samples may be the reason of the temperature-insensitive electron mobility. At low temperature regime, hole mobility is higher than electron mobility by a factor of 3 to 4. However, at high temperatures (T > 120 K), the mobility of p-type samples is restricted by the scattering of the optical phonons. Because the valance band discontinuity is smaller compared to the conduction band, thermionic transport of holes from QW to the barrier material, GaAs, also contributes to the mobility at high temperatures that results in a decrease in mobility. The hole mobility results of as-grown samples do not show a systematic behavior, while annealed samples do, depending on N concentration. Thermal annealing does not show a significant improvement of electron mobility.
The main goal of the present work is to study the coherent phonon in strongly confined CdSe quantum dots (QDs) under varied pump fluences. The main characteristics of coherent phonons (amplitude, frequency, phase, spectrogram) of CdSe QDs under the red-edge pump of the excitonic band [1S(e)-1S3/2(h)] are reported. We demonstrate for the first time that the amplitude of the coherent optical longitudinal-optical (LO) phonon at 6.16 THz excited in CdSe nanoparticles by a femtosecond unchirped pulse shows a non-monotone dependence on the pump fluence. This dependence exhibits the maximum at pump fluence ~0.8 mJ/cm². At the same time, the amplitudes of the longitudinal acoustic (LA) phonon mode at 0.55 THz and of the coherent wave packet of toluene at 15.6, 23.6 THz show a monotonic rise with the increase of pump fluence. The time frequency representation of an oscillating signal corresponding to LO phonons revealed by continuous wavelet transform (CWT) shows a profound destructive quantum interference close to the origin of distinct (optical phonon) and continuum-like (exciton) quasiparticles. The CWT spectrogram demonstrates a nonlinear chirp at short time delays, where the chirp sign depends on the pump pulse fluence. The CWT spectrogram reveals an anharmonic coupling between optical and acoustic phonons.
With about two-thirds of all used energy being lost as waste heat, there is a compelling need for high-performance thermoelectric materials that can directly and reversibly convert heat to electrical energy. However, the practical realization of thermoelectric materials is limited by their hitherto low figure of merit, ZT, which governs the Carnot efficiency according to the second law of thermodynamics. The recent successful strategy of nanostructuring to reduce thermal conductivity has achieved record-high ZT values in the range 1.5-1.8 at 750-900 kelvin, but still falls short of the generally desired threshold value of 2. Nanostructures in bulk thermoelectrics allow effective phonon scattering of a significant portion of the phonon spectrum, but phonons with long mean free paths remain largely unaffected. Here we show that heat-carrying phonons with long mean free paths can be scattered by controlling and fine-tuning the mesoscale architecture of nanostructured thermoelectric materials. Thus, by considering sources of scattering on all relevant length scales in a hierarchical fashion–from atomic-scale lattice disorder and nanoscale endotaxial precipitates to mesoscale grain boundaries–we achieve the maximum reduction in lattice thermal conductivity and a large enhancement in the thermoelectric performance of PbTe. By taking such a panoscopic approach to the scattering of heat-carrying phonons across integrated length scales, we go beyond nanostructuring and demonstrate a ZT value of ∼2.2 at 915 kelvin in p-type PbTe endotaxially nanostructured with SrTe at a concentration of 4 mole per cent and mesostructured with powder processing and spark plasma sintering. This increase in ZT beyond the threshold of 2 highlights the role of, and need for, multiscale hierarchical architecture in controlling phonon scattering in bulk thermoelectrics, and offers a realistic prospect of the recovery of a significant portion of waste heat.
- Journal of physics. Condensed matter : an Institute of Physics journal
- Published over 6 years ago
A theoretical investigation of the possible existence of chiral polaron formation in graphene is reported. We present an analytical method to calculate the ground-state of the electron-phonon system within the framework of the Lee-Low-Pines theory. On the basis of our model, the influence of electron-optical phonon interaction on the graphene electronic spectrum is investigated. We considered only the doubly degenerate optical phonon modes of E(2g) symmetry near the zone center Γ. It is analytically shown that the energy dispersions of both valence and conduction bands of the pristine graphene differ significantly from those obtained through the standard electron self-energy calculations arising from the electron-optical phonon interactions. In this paper, we also show for the first time that the degenerate band structure of the graphene promotes the chiral polaron formation. Furthermore, due to the k-dependent nature of the polaronic self-energy, in analogy with quantum chromodynamics, we also propose a running electron-phonon coupling constant as a function of energy.
Heat transport across interfaces is often discussed in terms of the transmission probability of the heat-carrying phonons through the contact zone. Although interface roughness influences the true contact area and affects phonon scattering within the contact zone, its effect on nanoscale heat transport remains poorly understood. Here, we report experimental data on the pressure dependence of thermal transport across polished nanoscale contacts. The data can be quantitatively explained by a model of thermal conductance across interfaces that incorporates the effect of nanoscale roughness through the quantized thermal conductance across individual atomic-scale contacts within the contact zone.
- Spectrochimica acta. Part A, Molecular and biomolecular spectroscopy
- Published over 5 years ago
The novel crystalline alloys CdTe-CuInTe2 were synthesized. The photoinduced spectral changes of the anharmonic phonon modes were explored by cw CO2 laser at power about 2 kW in the vicinity of the 1650 cm(-1) mode. The changes of the intensities for principal phonon modes were found. These modes were assigned both to harmonic as well as anharmonic modes. All the measurements are studied after the Ir illumination. The performed quantum chemical calculations with application of the norm-conserving pseudopotential method and Green functions allow to identify the origin of the content dependent anharmonic phonon modes. Some correlation between the intensities of the corresponding phonon modes at about 1600-1700 cm(-1) and the corresponding IR induced changes were found.
- Journal of physics. Condensed matter : an Institute of Physics journal
- Published about 6 years ago
We report an experimental study of the phonon dispersion in BiFeO(3) single crystals at ambient conditions by inelastic x-ray scattering (IXS). The phonon dispersions were recorded along several symmetry directions up to 35 meV. Our results compare favorably with first-principles calculations performed using density functional theory (DFT) within the local-density approximation (LDA). We resolve a discrepancy concerning the symmetry of the optical phonon branches observed by Raman spectroscopy, determine the energy of the lowest Raman and infrared silent mode, and derive a subset of the elastic moduli of BiFeO(3).
GaAs metal-oxide-semiconductor devices historically suffer from Fermi-level pinning, which is mainly due to the high trap density of states at the oxide/GaAs interface. In this work, we present a new way of passivating the interface trap states by growing an epitaxial layer of high-k dielectric oxide, La(2-x)Y(x)O(3), on GaAs(111)A. High-quality epitaxial La(2-x)Y(x)O(3) thin films are achieved by an ex situ atomic layer deposition (ALD) process, and GaAs MOS capacitors made from this epitaxial structure show very good interface quality with small frequency dispersion and low interface trap densities (D(it)). In particular, the La(2)O(3)/GaAs interface, which has a lattice mismatch of only 0.04%, shows very low D(it) in the GaAs bandgap, below 3 × 10(11) cm(-2) eV(-1) near the conduction band edge. The La(2)O(3)/GaAs capacitors also show the lowest frequency dispersion of any dielectric on GaAs. This is the first achievement of such low trap densities for oxides on GaAs.
We present femtosecond broadband transient absorption experiments for the investigation of the carrier dynamics in the organolead trihalide perovskite CH3NH3PbI3. The perovskite was prepared on a mesoporous TiO2 scaffold either by 1-step deposition from solution or by 2-step methods employing deposition of lead iodide followed by an on-surface reaction with methylammonium iodide. The thin films were characterized by XRD and FTIR chemical mapping. After pumping with an ultrashort laser pulse at 400 or 500 nm, the dynamics were monitored by a broadband supercontinuum reaching from the near IR (920 nm) into the UV. Specifically, the usage of quartz substrates and thin perovskite/TiO2 films enabled us to cover the spectral development down to 320 nm. The charge carrier dynamics were largely independent from the specific route of perovskite preparation: initial ultrafast carrier relaxation steps with time constants τCC and τCOP of <0.08, 0.2 and 2.6 ps were assigned to carrier-carrier and carrier-optical phonon scattering. Pronounced sub-band-gap absorption was found in the near IR at early times. Transient carrier temperatures were extracted from a Boltzmann fit to the blue wing of the photobleach band in the time range 0.2-700 ps, allowing us to distinguish between the decay of acoustic phonons (τAP = 50 and >1000 ps) and Auger recombination (τAR = 9, 75 and 450 ps). Carrier relaxation was accompanied by formation of an absorption band around 550 nm, with a characteristic structure assignable to a transient Stark effect, i.e. a red-shift of the perovskite spectrum due to the appearance of a directed electric field in the material and possibly additional influence of lattice heating. We observed a substantial Stokes shift between the relaxed photobleach and photoluminescence bands. Contributions of unreacted PbI2 to the transient absorption features appear to be negligible.