Optical grating technique, where optical gratings are generated via light inference, has been widely used to measure charge carrier and phonon transport in semiconductors. In this paper, compared are three types of transient optical grating techniques: transient grating diffraction, transient grating heterodyne, and grating imaging, by utilizing them to measure carrier diffusion coefficient in a GaAs/AlAs superlattice. Theoretical models are constructed for each technique to extract the carrier diffusion coefficient, and the results from all three techniques are consistent. Our main findings are: (1) the transient transmission change obtained from transient grating heterodyne and grating imaging techniques are identical, even these two techniques originate from different detection principles; and (2) By adopting detection of transmission change (heterodyne amplification) instead of pure diffraction, the grating imaging technique (transient grating heterodyne) has overwhelming advantage in signal intensity than the transient grating diffraction, with a signal intensity ratio of 315:1 (157:1).
Silicon‐organic hybrid integrated devices show great potential in high‐speed optical interconnects and sensors. In this paper, a high‐speed modulator based on an electro‐optic (EO) polymer (SEO125) infiltrated sub‐wavelength grating (SWG) waveguide ring resonator is presented. The core of the SWG waveguide consists of periodically arranged silicon pillars along the light propagation direction, which provides large mode volume overlap with EO polymer. The optimized SWG shows a mode volume overlap of 36.2% with a silicon duty cycle of 0.7. The 3‐dB modulation bandwidth of the fabricated modulator is measured to be larger than 40 GHz occupying an area of 70 μm x 29 μm, which is the largest bandwidth and the most compact footprint that has been demonstrated for ring resonators on the silicon‐organic hybrid platform.
The intensity‐scan (I‐scan) technique to study the polarization‐dependent, nonlinear processes in exfoliated bulk ReS2 is utilized. The polarization‐dependent reflection and transmission of ReS2, from which the absorption coefficients are extracted using the transfer matrix method, are measured. Absorption coefficients under high laser peak power show a transition from saturable absorption (SA) to reverse saturable absorption when rotating the laser polarization with respect to the b‐axis. It is found that SA and excited‐state absorption (ESA) contribute to the nonlinear optical processes. Both the SA and ESA show strong dependence on the polarization angle, which is attributed to the anisotropic optical transition probability and electronic band structure in ReS2. The anisotropic nonlinear optical properties of ReS2 may find applications as saturable absorbers in lasers and optical modulators.
Defect-carrier interaction in transition metal dichalcogenides (TMDs) plays important roles in carrier relaxation dynamics and carrier transport, which determines the per- formance of electronic devices. With femtosecond laser time-resolved spectroscopy, we investigated the effect of grain boundary/edge defects on the ultrafast dynamics of photoexcited carrier in molecular beam epitaxy (MBE)-grown MoTe2 and MoSe2. We found that, comparing with exfoliated samples, the carrier recombination rate in MBE- grown samples accelerates by about 50 times. We attribute this striking difference to the existence of abundant grain boundary/edge defects in MBE-grown samples, which can serve as effective recombination centers for the photoexcited carriers. We also observed coherent acoustic phonons in both exfoliated and MBE-grown MoTe2, indi- cating strong electron-phonon coupling in this materials. Our measured sound velocity agrees well with the previously reported result of theoretical calculation. Our findings provide a useful reference for the fundamental parameters: carrier lifetime and sound velocity and reveal the undiscovered carrier recombination effect of grain boundary/edge defects, both of which will facilitate the defect engineering in TMD materials for high speed opto-electronics.
We develop a nanosecond grating imaging (NGI) technique to measure in-plane thermal transport properties in bulk and thin-film samples. Based on nanosecond time-domain thermoreflectance (ns-TDTR), NGI incorporates a photomask with periodic metal strips patterned on a transparent dielectric substrate to generate grating images of pump and probe lasers on the sample surface, which induces heat conduction along both cross- and in-plane directions. Analytical and numerical models have been developed to extract thermal conductivities in both bulk and thin-film samples from NGI measurements. This newly developed technique is used to determine thickness-dependent in-plane thermal conductivities (κx) in Cu nano-films, which agree well with the electron thermal conductivity values converted from four-point electrical conductivity measurements using the Wiedemamn–Franz law, as well as previously reported experimental values. The κx measured with NGI in an 8 nm x 8 nm GaAs/AlAs superlattice (SL) is about 10.2 W/m⋅K, larger than the cross-plane thermal conductivity (8.8 W/m⋅K), indicating the anisotropic thermal transport in the SL structure. The uncertainty of the measured κx is about 25% in the Cu film and less than 5% in SL. Sensitivity analysis suggests that, with the careful selection of proper substrate and interface resistance, the uncertainty of κx in Cu nano-films can be as low as 5%, showing the potential of the NGI technique to determine κx in thin films with improved accuracy. By simply installing a photomask into ns-TDTR, NGI provides a convenient, fast, and cost-effective method to measure the in-plane thermal conductivities in a wide range of structures and materials.
Understanding defect effect on carrier dynamics is essential for both fundamental physics and potential applications of transition metal dichalcogenides (TMDs). Here, the phenomenon of oxygen impurities trapping photoexcited carriers has been studied with ultrafast pump-probe spectroscopy. Oxygen impurities are intentionally created in exfoliated multilayer MoSe2 with Ar+plasma irradiation and air exposure. After plasma treatment, the signal of transient absorption first increases and then decreases, which is a signature of defect-capturing carriers. With larger density of oxygen defects, the trapping effect becomes more prominent. The trapping defect densities are estimated from the transient absorption signal, and its increasing trend in the longer-irradiated sample agrees with the results from X-ray photoelectron spectroscopy. First-principle calculations with density functional theory reveal that oxygen atoms occupying Mo vacancies create mid-gap defect states, which are responsible for carrier trapping. Our findings shed light on the important role of oxygen defects as carrier trappers in TMDs, and facilitate defect engineering in relevant materials and device applications.
A high electrical and thermal conductivity coupled with low costs make copper (Cu) an enticing alternative to aluminum for fabrication of interconnects in packaging applications. To tap into the benefits of the ever-reducing size of transistors, it is required to increase the input/output (I/O) pin count on electronic chips and thus minimize the size of chip to board interconnects. Laser sintering of Cu nanoparticle (NP) inks can serve as a promising process for developing these micron sized, 3D interconnect structures. However, the exact processing windows for Cu NP sintering are not well known. Therefore, this paper presents an extensive experimental investigation of the sintering processing window with different lasers including femtosecond (fs), nanosecond (ns) and continuous-wave (CW) lasers. The dependence of the processing window on Cu layer thicknesses and laser exposure durations has also been investigated. A simplified model to estimate optimum laser sintering windows for Cu NPs using pulsed lasers is presented and the predicted estimates are compared against the experimental results. Given the simplicity of the model, it is shown to provide good estimates for fluence required for the onset of sintering and the processing window for good sintering of Cu NPs.
Metallic nanoparticles have unique optical properties such as localized surface plasmon resonance (LSPR) effect, which can be used to improve the energy absorption and photocatalytic properties of semiconductor bases. In this paper, we construct a model to study the influence of Ag or Au nanoparticles (cubes or spheres) on the solar energy absorption and photocatalytic properties of nitrogen doped TiO2 (or N-TiO2). Effects of specific nanoparticle coupling parameters, such as particle shape, size, doping period (metal–metal distance) and separation distance (metal–semiconductor distance), on the properties of N-TiO2 are studied in detail. We show that the photocurrent improvement can be optimized by setting suitable geometric parameters. In particular, the separation distance between metallic nanoparticles and N-TiO2D should be around 6–7 nm, and the period of doping P should be around 360 nm. The silver cubes with edge length show the best performance. The results can help the design of solar energy materials, in which metallic nanoparticles may play an important role.
All-optical switches have been considered as a promising solution to overcome the fundamental speed limit of the current electronic switches. However, the lack of a suitable third-order nonlinear material greatly hinders the development of this technology. Here we report the observation of ultrahigh third-order nonlinearity about 0.45 cm2/GW in graphene oxide thin films at the telecommunication wavelength region, which is four orders of magnitude higher than that of single crystalline silicon. Besides, graphene oxide is water soluble and thus easy to process due to the existence of oxygen containing groups. These unique properties can potentially significantly advance the performance of all-optical switches.
Multilayer MoS2 possesses highly anisotropic thermal conductivities along in-plane and cross-plane directions that could hamper heat dissipation in electronics. With about 9% cross-plane compressive strain created by hydrostatic pressure in a diamond anvil cell, we observed about 12 times increase in the cross-plane thermal conductivity of multilayer MoS2. Our experimental and theoretical studies reveal that this drastic change arises from the greatly strengthened interlayer interaction and heavily modified phonon dispersions along cross-plane direction, with negligible contribution from electronic thermal conductivity, despite its enhancement of 4 orders of magnitude. The anisotropic thermal conductivity in the multilayer MoS2 at ambient environment becomes almost isotropic under highly compressive strain, effectively transitioning from 2D to 3D heat dissipation. This strain tuning approach also makes possible parallel tuning of structural, thermal and electrical properties, and can be extended to the whole family of 2D Van der Waals solids, down to two layer systems.
In two dimensional (2D) transition metal dichalcogenides, defect-related processes can significantly affect carrier dynamics and transport properties. Using femtosecond degenerate pump-probe spectroscopy, exciton capture, and release by mid-gap defects have been observed in chemical vapor deposition (CVD) grown monolayer MoSe2. The observed defect state filling shows a clear saturation at high exciton densities, from which the defect density is estimated to be around 0.5 × 1012/cm2. The exciton capture time extracted from experimental data is around ~ 1 ps, while the average fast and slow release times are 52 and 700 ps, respectively. The process of defect trapping excitons is found to exist uniquely in CVD grown samples, regardless of substrate and sample thickness. X-ray photoelectron spectroscopy measurements on CVD and exfoliated samples suggest that the oxygen-associated impurities could be responsible for the exciton trapping. Our results bring new insights to understand the role of defects in capturing and releasing excitons in 2D materials, and demonstrate an approach to estimate the defect density nondestructively, both of which will facilitate the design and application of optoelectronics devices based on CVD grown 2D transition metal dichalcogenides.
A novel ultrafast reflective grating-imaging technique has been developed to measure ambipolar carrier diffusion in GaAs/AlAs quantum wells and bulk GaAs. By integrating a transmission grating and an imaging system into the traditional pump–probe setup, this technique can acquire carrier diffusion properties conveniently and accurately. The fitted results of the diffusion coefficient and diffusion length in bulk GaAs agree well with the literature values obtained by other techniques. The diffusion coefficient and diffusion length of GaAs/AlAs quantum wells are found to increase with the well layer thickness, which suggests that interface roughness scattering dominates carrier diffusion in GaAs/AlAs quantum wells. With the advantages of simple operation, sensitive detection, rapid and nondestructive measurement, and extensive applicability, the ultrafast reflective grating-imaging technique has great potential in experimental study of carrier diffusion in various materials.
Size and pump-fluence dependent ultrafast carrier dynamics of CdSeTe QDs are investigated using femtosecond pump-probe techniques operating at two different repetition rates: 1 kHz (low-repetition rate), and 76 MHz (high-repetition rate). With a low-repetition rate laser and 3.1 eV excitation photon energy, multiple exciton generation (MEG) is observed and the optical responses of alloyed QDs clearly show three components: a fast decay ascribed to carrier recombination, an intermediate component associated with MEG decay, and a slow decay associated with radiative Auger recombination. With a high-repetition rate laser and excitation photon energy resonant with band-edge energy, obvious coherent phonon oscillations are observed in 4 nm CdSeTe QDs due to impulsive stimulated Raman scattering. Open-aperture Z-scan measurement is used to clarify the size and pump-fluence dependence of optical nonlinearity under femtosecond laser excitation. With increasing laser power, an evolution from saturable absorption to reverse saturable absorption in CdSeTe QDs is observed. The transition process is analyzed using a phenomenological model based on nonlinear absorption coefficient and saturation intensity. These results indicate that CdSeTe QDs in a glass matrix are a class of materials for potential application in all-optical switching devices.
Subwavelength grating (SWG) waveguide is an intriguing alternative to conventional optical waveguides due to the extra degree of freedom it offers in tuning a few important waveguide properties, such as dispersion and refractive index. Devices based on SWG waveguides have demonstrated impressive performances compared to conventional waveguides. However, the high loss of SWG waveguide bends jeopardizes their applications in integrated photonic circuits. In this work, we propose a geometrical tuning art, which realizes a pre-distorted refractive index profile in SWG waveguide bends. The pre-distorted refractive index profile can effectively reduce the mode mismatch and radiation loss simultaneously, thus significantly reduce the bend loss. This geometry tuning art has been numerically optimized and experimentally demonstrated in present study. Through such tuning, the average insertion loss of a 5 μm SWG waveguide bend is reduced drastically from 5.43 dB to 1.10 dB per 90° bend for quasi-TE polarization. In the future, the proposed scheme will be utilized to enhance performance of a wide range of SWG waveguide based photonics devices.
Coherent thermal phonons (CTPs) play an important role in thermal transport in superlattice (SL) structures. To have a profound understanding of CTP transport in SL, direct measurement of CTP properties is necessary. In this study, coherent phonon spectroscopy has been utilized to generate and detect CTP in Bi2Te3/Sb2Te3 SL. Phonon lifetimes have been extracted from experimental data, with which mode-wise thermal conductivities have been calculated. Comparing with bulk Bi2Te3, the estimated mode-wise thermal conductivity of longitudinal acoustic phonons shifts to higher frequencies, due to constructive coherent phonon interference. Our results suggest that it is possible to use SL structure to manipulate coherent phonon propagation and to tailor thermal conductivity.
Subwavelength grating waveguide-based micro-ring resonators (SWGMRs) are a promising platform for research in light–matter interaction. However, it is extremely difficult to achieve small radius SWGMR devices (e.g., 5 μm) with satisfying quality factors (e.g., ∼10,000). One major issue is the large bend loss of small radius SWGMRs. In this work, we report the use of trapezoidal silicon pillars instead of conventional rectangular silicon pillars as building blocks of SWGMRs. We found that an asymmetric effective refractive index profile created by trapezoidal silicon pillars can significantly reduce the bend loss and therefore increase the quality factors of SWGMRs. For the first time to the best of our knowledge, we have experimentally demonstrated a 5 μm radius SWGMR made of trapezoidal silicon pillars (T-SWGMR) with an applicable quality factor as high as 11,500, 4.6 times of that (∼2800) offered by a conventional SWGMR made of rectangular silicon pillars, which indicates an 81.4% reduction of the propagation loss. This approach can also be readily employed to enhance SWGMRs with larger radii. We have also experimentally demonstrated a 10 μm radius T-SWGMR with a quality factor as high as 45,000, which indicates a propagation loss as low as 6.07 dB/cm.
Graphene has great potential for fabrication of ultrafast opto-electronics, in which relaxation and transport of photoexcited carriers determine device performance. Even though ultrafast carrier relaxation in graphene has been studied vigorously, transport properties of photoexcited carriers in graphene are largely unknown. In this work, we utilize an ultrafast grating imaging technique to measure lifetime (τr), diffusion coefficient (D), diffusion length (L) and mobility (μ) of photoexcited carriers in mono- and multi-layer graphene non-invasively. In monolayer graphene, D∼10,000 cm2/s and μ∼120,000 cm2/V have been observed, both of which decrease drastically in multilayer graphene, indicating that the remarkable transport properties in monolayer graphene originate from its unique Dirac-Cone energy structure. Mobilities of photoexcited carriers measured here are several times larger than the Hall and Field-Effect mobilities reported in literature (<15,000 cm2/V), due to the high energy of photoexcited carriers. Our results indicate the importance of obtaining monolayer graphene to realize high-performance graphene devices, as well as the necessity to use transport properties of photoexcited carriers for predicting the performance of graphene-based opto-electronics.
In this work, transient reflectivity changes in bulk CdSe have been measured with two-color femtosecond pump-probe spectroscopy under a wide range of pump fluences. Three regions of reflectivity change with pump fluences have been consistently revealed for excited carrier density, coherent phonon amplitude, and lattice temperature. For laser fluences from 13 to 19.3 mJ/cm2, ultrafast melting happens in first several picoseconds. This melting process is purely thermal and reversible. A complete phase transformation in bulk CdSe may be reached when the absorbed laser energy is localized long enough, as observed in nanocrystallineCdSe.
The femtosecond pump-probe technique is used to study the dynamics of photoexcited carriers and coherent acoustic phonons in bulk CdSe semiconductor. A turning point from fast to slow decay is observed, whose amplitude decreases with pump fluences and eventually flips the sign of differential reflectivity. The maximum change of differential reflectivity shows a saturation at high pump fluences, which is attributed to the optical energy gap dependent on carrier density. Long-lasting coherent oscillations of acoustic phonons have also been detected, and their amplitude and lifetime have a strong dependence on pump fluences. Our results can facilitate the understanding of ultrafast carrier and phonon dynamics in CdSe nanocrystals.