Terahertz radiation from propagating acoustic phonons based on deformation potential coupling.

We report on new THz electromagnetic emission mechanism from deformational coupling of acoustic (AC) phonons with electrons in the propagation medium of non-polar Si. The epicenters of the AC phonon pulses are the surface and interface of a GaP transducer layer whose thickness (d) is varied in nanoscale from 16 to 45 nm. The propagating AC pulses locally modulate the bandgap, which in turn generates a train of electric field pulses, inducing an abrupt drift motion at the depletion edge of Si. The fairly time-delayed THz bursts, centered at different times (t1T H z, t2T H z, and t3T H z), are concurrently emitted only when a series of AC pulses reach the point of the depletion edge of Si, even without any piezoelectricity. The analysis on the observed peak emission amplitudes is consistent with calculations based on the combined effects of mobile charge carrier density and AC-phonon-induced local deformation, which recapitulates the role of deformational potential coupling in THz wave emission in a formulatively distinct manner from piezoelectric counterpart.

Nanoscale mapping of surface strain in tapered nanorods using confocal photoluminescence spectroscopy.

The strain occurs spontaneously at the heterogeneous interfaces of virtually all crystalline materials. Consequently, the analysis across multiple interfaces requires a complementary characterization scheme with a resolution that fits the deformation scale. By implementing two-photon confocal laser scanning nanoscopy with an axial resolution of 10 nm, we extract the surface strain from the photoluminescence (PL) spectra, epitomized by a 2-fold enhancement at the tapered tips in comparison to the substrate of ZnO nanorods. We firstly traced the well-established contribution from quantum confinement (QC) to PL shift in three geometrically classified regions: (I) a strongly tapered region where the diameter increases from 3 to 20 nm; (II) a weakly tapered region with a gradually increasing diameter from 20 to 58 nm; (III) round cylindrical region interfacing the sapphire substrate. The measured PL shift influenced by the deformation is significantly stronger than the attained QC effect. Particularly, surface strain at the strongly tapered region turned out to drastically increase the PL shift which matches well with the analysis based on the surface to volume ratio incorporating mechanical parameters such as the compliance tensor component, strain dislocation constant, and surface stress. The surface strain increased at a lower temperature, further disclosing its inherent dependence on the thermal expansion coefficients in clear contrast to the temperature-invariant characteristics of QC.

Broadband tuning of ring-type cavity-dumped femtosecond optical parametric oscillator in the near-infrared.

We report a cavity-dumped optical parametric oscillator (OPO) with a ring-type cavity configuration, which is based on periodically poled lithium niobate gain synchronously pumped by a mode-locked Ti:sapphire laser. Because of reduced cavity loss and group velocity dispersion inherent to ring-cavity employment, a wide wavelength tuning capability from 1.02 to 1.65 µm was achieved by the simple displacement of a cavity mirror. At a wavelength of 1.28 µm, the cavity-dumped system provides femtosecond pulses with 42 nJ energy and 50% dumping efficiency. The group delay dispersion (GDD) of the OPO cavity could be characterized through the wavelength tuning behavior with cavity displacement, and its validity was confirmed by the numerical GDD calculation of each optical component within the cavity.

Emission analysis of Tb3+ -and Sm3+ -ion-doped (Li2 O/Na2 O/K2 O) and (Li2 O + Na2 O/Li2 O + K2 O/K2 O + Na2 O)-modified borosilicate glasses.

Four series of borosilicate glasses modified by alkali oxides and doped with Tb3+ and Sm3+ ions were prepared using the conventional melt quenching technique, with the chemical composition 74.5B2 O3 + 10SiO2 + 5MgO + R + 0.5(Tb2 O3 /Sm2 O3 ) [where R = 10(Li2 O /Na2 O/K2 O) for series A and C, and R = 5(Li2 O + Na2 O/Li2 O + K2 O/K2 O + Na2 O) for series B and D]. The X-ray diffraction (XRD) patterns of all the prepared glasses indicate their amorphous nature. The spectroscopic properties of the prepared glasses were studied by optical absorption analysis, photoluminescence excitation (PLE) and photoluminescence (PL) analysis. A green emission corresponding to the 5 D4 → 7 F5 (543 nm) transition of the Tb3+ ions was registered under excitation at 379 nm for series A and B glasses. The emission spectra of the Sm3+ ions with the series C and D glasses showed strong reddish-orange emission at 600 nm (4 G5/2 →6 H7/2 ) with an excitation wavelength λexci = 404 nm (6 H5/2 →4 F7/2 ). Furthermore, the change in the luminescence intensity with the addition of an alkali oxide and combinations of these alkali oxides to borosilicate glasses doped with Tb3+ and Sm3+ ions was studied to optimize the potential alkali-oxide-modified borosilicate glass.

Temperature-Dependent Mean Free Path Spectra of Thermal Phonons Along the c-Axis of Graphite.

Heat conduction in graphite has been studied for decades because of its exceptionally large thermal anisotropy. While the bulk thermal conductivities along the in-plane and cross-plane directions are well-known, less understood are the microscopic properties of the thermal phonons responsible for heat conduction. In particular, recent experimental and computational works indicate that the average phonon mean free path (MFP) along the c-axis is considerably larger than that estimated by kinetic theory, but the distribution of MFPs remains unknown. Here, we report the first quantitative measurements of c-axis phonon MFP spectra in graphite at a variety of temperatures using time-domain thermoreflectance measurements of graphite flakes with variable thickness. Our results indicate that c-axis phonon MFPs have values of a few hundred nanometers at room temperature and a much narrower distribution than in isotropic crystals. At low temperatures, phonon scattering is dominated by grain boundaries separating crystalline regions of different rotational orientation. Our study provides important new insights into heat transport and phonon scattering mechanisms in graphite and other anisotropic van der Waals solids.

Electron and phonon coupling dynamics in low-gap semiconductor: quantum versus classical scale.

We have studied the characteristics of longitudinal-optical-phonon-plasmon coupled (LOPC) mode by using the ultrashort pulsed laser with 45 THz bandwidth as a function of thickness in InAs epilayers, ranging from 10 to 900 nm. We have observed the LOPC modes split into the upper (L(+) mode) and the lower (L(-) mode) branches only in the classical scale, but the longitudinal-optical (LO) phonon peak was persistently observed. The shorter decay time of the plasmon-like L(+) modes rather than the phonon-like L(-) modes should be associated with carrier-carrier scattering which is further considered with diffusion properties in the low-gap semiconductors. This result leads to that the absence of the LOPC modes in a scale less than exciton Bohr radius manifests the role of electron diffusion rather than the carrier screening via drift motion in surface depletion region.

Propagation effects of THz waves in InAs-based heterostructures.

We have investigated THz radiation characteristics along different directions, either reflective or along lateral by using InAs-based heterostructures. Firstly, we demonstrate the phase shift with InAs layer thickness, revealing the change of dominant THz wave generation mechanism along both directions. Along the lateral direction, the time-domain signals in thin InAs epilayers showed an abrupt phase and amplitude change at certain time delays which suggest the interference between two rays at the photoconductive switch. This behavior was further substantiated by the multiple cavity modes in Fourier-transformed spectra and by the amplitude variation with excitation spot displacement.

Directional terahertz emission from corrugated InAs structures.

The terahertz (THz) radiation from transient dipoles, formed by distinct diffusion coefficients between oppositely charged carriers as often observed in low band gap semiconductors, propagates with an anisotropic amplitude distribution perpendicular to the dipole axis along the diffusive motion. By directionally adjusting the electronic diffusion, we conceptualize groove-patterned THz emitters based on (100) InAs thin films and demonstrate the unidirectional radiation. Line-of-sight emission along the surface-normal direction is greatly enhanced in a distributed asymmetric trapezoid with its period similar to the electronic diffusion length of InAs. This directional enhancement is in clear contrast to the constant emission amplitude along the lateral direction, regardless of pattern scale, which manifests the role of groove patterns as microscale reflectors in laterally corrugating the carrier density. In contrast to the rather limited nonlinearity in (100) plane, the azimuthal angle dependence of the THz field amplitude in corrugated samples shows a combined effect of diffusive transport and second-order nonlinearity, whose compositional contributions varies in different structures.

The Role of the Graphene Oxide (GO) and Reduced Graphene Oxide (RGO) Intermediate Layer in CZTSSe Thin-Film Solar Cells.

Cu2ZnSn(S,Se)4 (CZTSSe) solar cells with low cost and eco-friendly characteristics are attractive as future sources of electricity generation, but low conversion efficiency remains an issue. To improve conversion efficiency, a method of inserting intermediate layers between the CZTSSe absorber film and the Mo back contact is used to suppress the formation of MoSe2 and decomposition of CZTSSe. Among the candidates for the intermediate layer, graphene oxide (GO) and reduced GO have excellent properties, including high-charge mobility and low processing cost. Depending on the type of GO, the solar cell parameters, such as fill factor (FF), were enhanced. Thus, the conversion efficiency of 6.3% was achieved using the chemically reduced GO intermediate layer with significantly improved FF.

Terahertz waves emitted from an optical fiber.

We report a simple method of creating terahertz waves by applying the photo-Dember effect in a (100)-oriented InAs film coated onto the 45-degree wedged-end facet of an optical fiber. The terahertz waves are generated by infrared pulses guided through the optical fiber which is nearly in contact with a sample and then measured by a conventional photo-conductive antenna detector. Using this alignment-free terahertz source, we performed proof-of-principle experiments of terahertz time-domain spectroscopy and near-field terahertz microscopy. We obtained a bandwidth of 2 THz and 180-microm spatial resolution. Using this method, the THz imaging resolution is expected to be reduced to the size of the optical fiber core. Applications of this device can be extended to sub-wavelength terahertz spectroscopic imaging, miniaturized terahertz system design, and remote sensing.

High frequency atomic tunneling yields ultralow and glass-like thermal conductivity in chalcogenide single crystals.

Crystalline solids exhibiting glass-like thermal conductivity have attracted substantial attention both for fundamental interest and applications such as thermoelectrics. In most crystals, the competition of phonon scattering by anharmonic interactions and crystalline imperfections leads to a non-monotonic trend of thermal conductivity with temperature. Defect-free crystals that exhibit the glassy trend of low thermal conductivity with a monotonic increase with temperature are desirable because they are intrinsically thermally insulating while retaining useful properties of perfect crystals. However, this behavior is rare, and its microscopic origin remains unclear. Here, we report the observation of ultralow and glass-like thermal conductivity in a hexagonal perovskite chalcogenide single crystal, BaTiS3, despite its highly symmetric and simple primitive cell. Elastic and inelastic scattering measurements reveal the quantum mechanical origin of this unusual trend. A two-level atomic tunneling system exists in a shallow double-well potential of the Ti atom and is of sufficiently high frequency to scatter heat-carrying phonons up to room temperature. While atomic tunneling has been invoked to explain the low-temperature thermal conductivity of solids for decades, our study establishes the presence of sub-THz frequency tunneling systems even in high-quality, electrically insulating single crystals, leading to anomalous transport properties well above cryogenic temperatures.

Two-Step Energy Transfer Dynamics in Conjugated Polymer and Dye-Labeled Aptamer-Based Potassium Ion Detection Assay.

We recently implemented highly sensitive detection systems for photo-sensitizing potassium ions (K+) based on two-step Förster resonance energy transfer (FRET). As a successive study for quantitative understanding of energy transfer processes in terms of the exciton population, we investigated the fluorescence decay dynamics in conjugated polymers and an aptamer-based 6-carboxyfluorescein (6-FAM)/6-carboxytetramethylrhodamine (TAMRA) complex. In the presence of K+ ions, the Guanine-rich aptamer enabled efficient two-step resonance energy transfer from conjugated polymers to dyed pairs of 6-FAM and TAMRA through the G-quadruplex phase. Although the fluorescence decay time of TAMRA barely changed, the fluorescence intensity was significantly increased. We also found that 6-FAM showed a decreased exciton population due the compensation of energy transfer to TAMRA by FRET from conjugated polymers, but a fluorescence quenching also occurred concomitantly. Consequently, the fluorescence intensity of TAMRA showed a 4-fold enhancement, where the initial transfer efficiency (~300%) rapidly saturated within ~0.5 ns and the plateau of transfer efficiency (~230%) remained afterward.

Coherent control of thermal phonon transport in van der Waals superlattices.

van der Waals (vdW) heterostructures are a central focus of materials science and condensed matter physics due to the novel physical phenomena and properties obtained by precisely stacking heterogeneous atomically thin layers. vdW heterostructures are expected to allow for the coherent manipulation of THz lattice vibrations and hence heat conduction due to the ability to precisely control chemical composition at the atomic scale, but little work has focused on thermal transport in these materials. Here, we report an ab initio study of thermal transport in vdW superlattices consisting of alternating transition metal dichalcogenide atomic layers. Our calculations show that the lattice vibrational spectrum and scattering rates can be precisely manipulated by the choice of each atomically thin layer, resulting in materials with novel properties such as large thermal anisotropies approaching 200 and ultralow cross-plane thermal conductivities comparable to those of amorphous materials. Our work demonstrates how coherent manipulation of phonons in vdW superlattices can expand the property space beyond that occupied by natural materials and suggests an experimental route to realize these properties.

III-nitride core-shell nanorod array on quartz substrates.

We report the fabrication of near-vertically elongated GaN nanorods on quartz substrates. To control the preferred orientation and length of individual GaN nanorods, we combined molecular beam epitaxy (MBE) with pulsed-mode metal-organic chemical vapor deposition (MOCVD). The MBE-grown buffer layer was composed of GaN nanograins exhibiting an ordered surface and preferred orientation along the surface normal direction. Position-controlled growth of the GaN nanorods was achieved by selective-area growth using MOCVD. Simultaneously, the GaN nanorods were elongated by the pulsed-mode growth. The microstructural and optical properties of both GaN nanorods and InGaN/GaN core-shell nanorods were then investigated. The nanorods were highly crystalline and the core-shell structures exhibited optical emission properties, indicating the feasibility of fabricating III-nitride nano-optoelectronic devices on amorphous substrates.

Combined Effect of Carrier Localization and Polarity in InxGa1-xN/GaN Quantum Wells.

The influence of carrier localization and polarization-induced electric fields on the spectral variation of photoluminescence was comparatively studied in polar and semipolar InxGa1-x N/GaN strained quantum wells embedded in p-i-n diodes. Two representative structures with x = 0.16 for polar (0001) diodes and potential fluctuations for semipolar diodes grown along (1122) direction have been investigated with a reverse bias up to -4 V. From the s-shaped spectral shift as a function of temperature, the existence of single and triple localization traps was confirmed in polar and semipolar diodes. Within our bias range, we observed the monotonic blueshift with reverse bias in the polar sample, indicating that the carriers are laterally localized and thus influenced by the vertical piezoelectric fields. In clear contrast, the semipolar sample showed the blueshift of localized states only at low temperatures, while the deepest localization features were found at the highest available temperatures, overriding the influence of thermal activation and polarization fields.

Directional Terahertz Radiation from GalnP Lateral Superlattice.

We devised directionally controllable THz emission sources based on lateral composition modulation (LCM) structures. LCM structures were composed of In-rich Ga0.47In0.53P and Ga-rich Ga0.51In0.49P layers whose period was in quantum scale of ~`5 nm. The inherent type II band alignment in these structures leads to electron-hole (e-h) separation and plays a key role in generating later- ally polarized dipole ensembles, thus concomitantly emitting enhanced transmissive THz waves as compared to bulk sample. On the other hand, in lateral geometry, changes in THz fields between LCM and bulk structures turned out to negligible since the vertical electronic diffusion was allowed in both samples.

Polarized Terahertz Waves Emitted from In0.2Ga0.8As Nanowires.

We investigate the polarizability of terahertz (THz) waves emitted from undoped In0.2Ga0.8As nanowires (NWs). THz emission amplitude shows strong enhancement in vertically aligned NWs compared to less-aligned NWs. In particular, polarized THz waves are clearly demonstrated in aligned NWs via a drastic variation of amplitudes as a function of the axis angle in polarization-sensitive photoconductive antenna. In addition, phase reversal between aligned and less-aligned NWs substantiates the geometrical dependence of electronic diffusion in generating the transient THz electric fields.