United States

Abstract Body: Phonon polaritons are collective oscillations resulting from the coupling of photons with optical phonons in polar materials and are supported within a material-specific spectral region called the reststrahlen band, which is bounded by the transverse and longitudinal optical phonons. In this region, the material behaves optically like a metal; it is highly reflective and has a negative real part of the permittivity. When polar materials are nanostructured, phonon polaritons can enable a variety of near-field optical effects such as sub-diffraction light confinement. Polar materials that support phonon polaritons can also have anisotropic optical properties, such that the optical constants depend on the propagation direction and polarization of the incoming light. When the principal components of the permittivity tensor have opposite signs, the material is referred to as hyperbolic. Hyperbolic materials are somewhat unusual as they behave optically like a dielectric and metal along different crystal axes, and this anisotropy of the metal-like response has important implications for the physics of its supported modes. Here, we report on the first experimental observation of hyperbolic phonon polaritons (HPs) in calcite nanopillar arrays, demonstrate the aspect ratio dependence of the HP resonance frequencies, discuss fabrication challenges, observe a new, possibly higher order mode as the pitch is reduced, and compare our results to both numerical simulations and an analytical model. We also found that the simulated electric field distributions for the HP modes are not localized to the pillars but extend appreciably into the calcite substrate. In addition, we have fabricated nanohole arrays in calcite, which also support HPs. However, the HP resonances appear to exhibit a slight aspect ratio dependence but opposite in trend to what was observed for the nanopillars. Additionally, the nanohole arrays have fewer HP modes and these modes are blueshifted in comparison to the nanopillars. We are currently using finite difference time domain simulations to characterize the HP modes supported in the nanohole arrays and to understand the differences between these modes and the HP modes confined within the nanopillars. Calcite is an ideal low-loss material for studying HPs that could find applications in mid-IR nanophotonic devices, and so these results are an important step toward creating a library of materials with the appropriate phonon properties to span the infrared.

EMC 2021

Hyperbolic Phonon Polaritons in Calcite Nanopillar and Nanohole Arrays for Nanoscale Infrared Confinement

nanophotonics

dielectric materials

inorganic crystalline materials

infrared spectroscopy

phonon polaritons

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technical paper

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Abstract Body: The integration of plasmonic materials with emitters and optoelectronic devices allows for remarkable enhancement and improved understanding of light-matter interaction. Previous approaches to plasmonic integration rely on the noble metals to achieve a plasmonic response near the metal’s plasma frequency, limiting plasmonic devices to the near-infrared and visible wavelength range. The noble metals offer strong confinement but with the possibly of greater loss.[1] Since emitters in the near-infrared and visible wavelength ranges already have high optical efficiencies, it is difficult to increase that efficiency with the introduction of a plasmonic material. However, the mid-infrared has few highly efficient light emitting materials.[2] Emission from mid-infrared materials can be significantly enhanced when coupled with a plasmonic material and thus have a strongly enhanced efficiency. The integration of a noble metal in the near-field of an emitter is often incompatible with the electronic requirements of the active device, compromising the device architecture and significantly limiting possible emission enhancement.[3] Each of these drawbacks conspire to limit the design flexibility and potential performance of polylithically-integrated metal-based optoelectronic devices. Molecular beam epitaxy allows for the engineering of so-called “designed metals” for a monolithic all-epitaxial integration of a plasmonic material and active device in the mid-infrared.[4] Previously we have shown the first all-epitaxial integration of a plasmonic “designer metal” and emitter to produce a cavity-enhanced light-emitting diode (LED).[5] Experimental electroluminescence showed a strong enhancement of emission at the peak wavelength, increasing by a factor of 5.6x when compared to a control LED. The device with the plasmonic virtual substrate showed upper hemisphere powers of 1.45 μW at 300 K, comparable to state-of-the-art mid-infrared LEDs at the same wavelength.[6] In order to increase the efficiency of the cavity-enhanced LEDs, we are integrating our emitters into an AlInAsSb/InAs/AlInAsSb double heterostructure design with a tunnel junction to increase efficiency.[7] The cavity-enhanced LED design was optimized using rigorous coupled-wave analysis. Further simulations and characterization of the double heterostructure cavity-enhanced LED are underway and will be presented at the conference. This work was supported by the National Science Foundation (NSF) under grant EECS-1926187 and performed at the Texas Nanofabrication Facility, supported by NSF grant NNCI-2025227. [1] J. B. Khurgin and A. Boltasseva, MRS Bulletin, 37, 768, (2012). [2] D. Jung, et al., J. Opt., 19, 123001 (2017). [3] J. B. Khurgin and G. Sun, Nat. Photonics, 8, 468 (2014) [4] S. Law, et al., Opt. Express (2012). [5] A.F. Briggs, et al., Optica, 7, 1355 (2020). [6] Boston Electronics, IoffeLED, Optically immersed 7.0 µm optically pumped LED in heatsink optimized housing, OPLED70Sr datasheet. [7] A. J. Muhowski et al., 2020 IEEE Research and Applications of Photonics in Defense Conference (RAPID), (2020).

Enhanced Double Heterostructure Infrared LEDs Using Monolithically Integrated Plasmonic Materials

Abstract Body: Silicon photonics require a reliable integrated light source to be a viable technology. While heterogeneous integration techniques such as wafer bonding III-V on silicon has proven successful, dramatic cost reductions can be achieved through direct growth of III-V on silicon. This presents numerous challenges to material quality due to mismatches in lattice constant, coefficient of thermal expansion, and crystal symmetry. Even so, decades of work developing defect filtering buffers paired with defect-tolerant quantum dot (QD) active regions have yielded lasers with satisfactory reliability at room temperature, however laser lifetimes at elevated temperatures remain insufficient for commercial applications. We have recently uncovered a source for lagging performance in InAs QD lasers on silicon, namely misfit dislocations (MDs) that lie along the upper and lower boundaries of the active region and act as potent non-radiative recombination centers. We have proposed that these MDs form not due to lattice mismatch in the active region, but instead form by an alternative mechanism based on (1) tensile thermal strain that builds in the AlGaAs cladding layers during cooldown after growth and (2) pinning of threading dislocations (TDs) in the InAs QD active region. TDs, which are mobile in the cladding layers above ~300 °C, glide to relieve the thermal tensile strain in these layers. The TD segment passing through the active region would ideally glide with the segment in the cladding, but as QDs act as powerful pinning sites, glide is prohibited under these low stress conditions. It follows then that MDs will form at both the upper and lower boundaries between the cladding and active region if both cladding layers are above critical thickness due to thermal strain. To solve this, we insert strained indium-alloyed “trapping layers” (TLs) to displace formation of these MDs away from the active region. Unlike the active region, these layers do not contain QDs, but they can still pin TDs in the low stress environment encountered during cooldown because natural compositional fluctuations in the indium-alloyed TLs generate sufficiently large in-layer stress fluctuations. In lasers with TLs, MDs are no longer adjacent to the active region, so their supply of minority carriers is sharply reduced, benefiting not only initial laser performance but also laser reliability since this reduces recombination-enhanced dislocation climb, which we have observed to be a significant source of laser degradation. Initial performance improvements over baseline include median threshold current reduced by half, median slope efficiency increased by over 50%, and median output power increased by over 3×. Thermal performance is also greatly improved with the threshold characteristic temperature, T0, increased from 70 K in baseline lasers to 100 K in TL lasers, indicating their lasing threshold is less sensitive to temperature. Initial laser aging experiments reveal that TLs dramatically enhance the reliability of InAs QD lasers on silicon. After aging for 1200 h at 60 °C at approximately 2× initial 60 °C threshold current, TL lasers have a median threshold current increase of just 3%, far lower than the 56% increase for baseline lasers, lower than the 19% increase of our previous record lifetime InAs QD lasers on silicon under comparable conditions, and even lower than the 11% median threshold increase of QD lasers on GaAs substrates. We suspect that the TL lasers’ lower degradation rate compared to lasers on GaAs, despite their much lower TD density, is due to the higher thermal conductivity of the silicon substrate which reduces the active region temperature during operation. Overall, these reliability results provide a clear path forward toward reliable monolithically integrated light sources for silicon photonics.

High-Reliability InAs QD Lasers on Silicon Through Misfit Dislocation Trapping Layers

Abstract Body: InGaAs is an ideal material for near-infrared (near-IR) photodetection at telecommunications wavelengths. Its direct band gap offers strong absorption and is tunable by varying the alloy composition, making InGaAs versatile for such applications. However, most commercial devices based on this material require InP substrates, which are costly and difficult to process. Moreover, the In content of the InGaAs layer is limited by the requirement for lattice matching.[1] Nanowires are a promising avenue for heteroepitaxy of InGaAs and InAs on common substrates like Si and GaAs, and offer several performance advantages over bulk devices.[2] For example, their thin, anisotropic geometry enables devices to benefit from fast carrier collection and polarization-dependent absorption, making them suitable for fast and efficient multiplexed applications.[3] Nanowires also allow for a significant reduction in the amount of scarce materials, such as In, required to make a device. Typically, nanowires are grown vertically, perpendicular to the substrate, but vertical nanowires are notoriously difficult to incorporate into devices, and a horizontal configuration is often preferred. Recently, horizontal networks of high-quality In(Ga)As nanowires have been demonstrated by growing them on top of GaAs nanomembrane buffers using selective-area epitaxy on III-V substrates.[4,5] In this work we investigate the growth of horizontal In(Ga)As nanowire networks on GaAs substrates by molecular beam epitaxy. An epitaxial GaAs buffer nanomembrane is grown on the substrate to ensure high crystal quality In(Ga)As. Different crystallographic orientations are investigated. For growth on (111)B GaAs substrates, we demonstrate InGaAs nanowire networks positioned atop high aspect ratio GaAs nanomembranes. We show that the In content of the nanowires can be tuned up to 50% of the group III component by controlling growth conditions, but that pure InAs nanowires are not achievable.[6] Next, we demonstrate InAs nanowires grown on low-aspect ratio GaAs nanomembrane on (100) GaAs substrates. The nanowires grow conformally on the nanomembranes, which are dominated by (111) facets, and pure InAs can be achieved with just a narrow intermixed region near the interface. We compare the nanowires on each of these crystallographic orientations, highlighting their advantages for different applications. Finally, we present preliminary electrical characterization data from basic photodetector devices based on these nanowires. We compare nanowires of different lengths and widths and characterize the photoconductive response for both single nanowires and ensembles in an array. Insights from these preliminary results will guide design choices for future photodetector architectures based on these nanowires. 1 R. LaPierre et al., J. Phys. D: Appl. Phys. 50 (2017) 2 C. L. Tan et al., Nanophotonics. 7 (2018) 3 A. Dorodnyy et al., IEEE J. Sel. Top. Quant. Electr. 24 (2018) 4 M. Friedl et al., Nano Lett. 18 (2018) 5 F. Krizek et al., Phys. Rev. Mat. 2 (2018) 6 M. Friedl et al., Nano Lett. 20 (2020) Funding from Swiss National Science Foundation, NCCR QSIT

Scalable III-V Nanowire Networks for IR Photodetection

Abstract Body: Ga-assisted self-catalyzed epitaxial growth and demonstration of Te-doped axial GaAsSbN NW-based Schottky barrier photodetector on p-Si (111) in the near-infrared region is reported. The successful growth of improved dilute nitride quaternary GaAsSbN (Te) NWs in axial configuration was achieved by stringent control on NW nucleation conditions, NW stem growth, and exposure of N-plasma on NW growth. Planar defect-free structures were realized with room temperature photoluminescence (PL) characteristics, revealing reduced N-induced point defects and non-radiative recombination centers. N incorporation in the dilute nitride NWs was ascertained from PL and Raman spectral mode shifts and shapes and weak temperature-dependent PL peak energy. The advantage of Te-doping in dilute nitride NW using a GaTe captive source in the compensation of point defects is demonstrated, as evidenced by a significant improvement in PL characteristics, Raman mode shifts, and spectral shape with improved photodetector device performance relative to intrinsic dilute nitride NWs. Te-doped GaAsSbN NW Schottky based photodetectors have been demonstrated on both single and ensemble configurations yielding responsivity of 5 A/W at 860 nm and 3800 A/W at 1100, respectively. Detectivity of 3.2x1010 Jones was achieved on the Te-doped ensemble NW device. This work showcases rich prospects for engineering bandgap in the near-infrared region for telecommunication wavelength applications using GaAsSb alloy system.

Epitaxial GaAsSbN (Te) NWs for Near-Infrared Region Photodetection Application

Abstract Body: We report on a systematic investigation of the effect of tellurium (Te)-doping on the morphological, optical, and electrical properties of the GaAsSb nanowires (NWs) grown by self-catalyzed molecular beam epitaxy and realization of the ensemble NW photodetector (PD). Qualitative assessment of Te-incorporation in the NWs was made from the structural, optical, and electrical properties, whereas the quantitative assessment was made based on the dark I-V simulations. The single nanowire I-V characterization demonstrated a significant reduction in turn-on voltage with doping. High-resolution transmission electron microscopy image and the selected area electron diffraction patterns of n-GaAsSb NWs revealed the defect-free single-crystal zinc-blende crystal structure. The compositional homogeneity of the NWs is attested by the extended plateau in the energy-dispersive X-ray spectroscopy line scan. An ensemble PD fabricated using n-GaAsSb NWs demonstrated a wide spectral range with the longer wavelength cutoff at ~1.2 µm, with the figure of merits namely, responsivity in the range of 580- 620 A/W and detectivity of 3x 1012 Jones. Low-frequency noise (LFN) spectroscopy revealed the generation-recombination noise being the dominant noise source in the Te doped GaAsSb NWs.

A Te Doped GaAsSb Ensemble Nanowire Photodetector for Near-Infrared Application

Abstract Body: Background. β-Ga2O3 has been actively studied for power electronics, RF devices, etc. Among various device topologies, fin-structures are particularly attractive since they enable the RESURF effect, which is key in designing high-field electronics and enhancement-mode transistor operation1,2. Fin-structures have been successfully employed in demonstrating record-setting devices in β-Ga2O33,4. However, we also observed in these devices that a “waist” tends to develop in the middle of a fin thus current flow can be severely pinched by “narrowed waist”. Here, we report what has been learned to date on fin-waist formation during ICP reactive ion etching (RIE). Experiments. The fin/trench arrays were fabricated on single-crystal β-Ga2O3 substrates with 2 orientations: (010) and (001). Hard masks of Pt were patterned by EBL for fin/trench widths less than 1 μm and optical lithography for wider ones. Definitions of dimensional parameters for fin, trench, fin waist and waist narrowing are illustrated in Fig.1. The dry etch parameters were fixed at 350 W ICP power, 20 W RIE power, 5 mTorr, 20C with 35 sccm BCl3 and 5 sccm Ar. Prior to SEM, the etched samples were soaked in HCl and/or HF to remove etch damage/residue. This dry+wet etch condition has rendered consistently rectangular-shaped single fins on (001) β-Ga2O3 with a fin height/width aspect ratio (AR) up to 9 and used in our reported devices3. Fin-waist dependence on the fin orientation and AR of fins/trenches. Arrays of fins were etched on (001) β-Ga2O3 with fin orientation varied. The fin width was varied from 0.15 to 8 μm, the trench width was varied from 1 to 8 μm, and the fin/trench depth was varied from 1.1 to 2 μm, which corresponds to a fin AR of 0.2-9 and a trench AR of 0.5-1.3. Upon examining cross-sections of these fins/trenches under SEM (Figs. 2-4), we discover following trends: 1) all outermost sidewalls of fin arrays and single fins appear to be vertical, while inner sidewalls all show waist; 2) there is no noticeable dependence on fin orientation; 3) waist narrowing increases from 50±10 nm for a trench AR of 0.5 to 200±10 nm for a trench AR up to 1.3, while appears nearly independent of fin width; and 4) wet etch worsens waist narrowing. Fin-waist dependence on the substrate orientation. Similar trench etching experiments were applied to (010) substrates, given their popular use in device development. Example cross-section SEM images are shown in Fig. 5. Though the ranges of fin/trench geometric parameters are slightly different from the ones explored on the (001) β-Ga2O3, the trends observed are largely consistent across different substrate orientations. Discussions. To advance fin-based device performance, it is essential to increase filling factor of fins with respect to entire area occupied by devices on wafer; the preferred trench AR is >1. Under the present ICP-RIE etch condition, waist narrowing is minimal for a low trench AR; but low trench AR implies a low filling factor of current-carrying fins. Waist narrowing is tolerable for fat fins, but the resultant fins can suffer from severe waist narrowing for large-AR trenches and narrow fins (Fig.6) thus detrimental to realizing smooth current flow in devices. Based on our observations, we hypothesize that in trenches with a high AR, a combination of poor sidewall passivation and ion/electron redistribution can result in appreciable lateral etching thus forming waist in fins or bowing of sidewalls. Similar effects were widely observed in other material systems, and improved passivation of sidewalls and neutralization of charges on sidewalls are common tactics to suppress bowing. Ongoing studies are undertaken to curb this undesirable waist narrowing. 1Hu, et al, EDL, 39, 869(2018). 2Li, et al, TED, 67, 3954(2020). 3Li, et al, IEDM, 270(2019). 4Li, et al, EDL, 41, 107(2020). * This work is in part supported by AFOSR Center of Excellence: ACCESS (FA9550-18-1-0529). CNF uses are partly supported by NSF NNCI-2025233.

Fin-Waist Formation in β-Ga2O3 Fin Arrays Defined by ICP-RIE

Abstract Body: β-Ga2O3 is an emerging ultra-wide bandgap (UWBG) semiconductor that holds promise to enable advances in power, RF and opto-electronic devices. With the introduction of β-(Al,Ga)2O3, UWBG heterostructures are possible that increase the range of viable devices. In fact, two-dimensional electron gases (2DEG) in modulation-doped β-(Al,Ga)2O3/Ga2O3heterojunctions [1, 2] have already been reported. However, while there are numerous studies on defect spectroscopies and electrical properties of β-Ga2O3, comparatively little information on electrically active defects and their impact on material properties in β-(Al,Ga)2O3 is available. An understanding of traps in β-(Al,Ga)2O3 will be important to identify and mitigate sources for device degradation, as well as to optimize epitaxial growth. Presented here are deep level transient and optical spectroscopy (DLTS/DLOS) results obtained from β-(Al0.1Ga0.9)2O3 epitaxial layers grown by metal organic chemical vapor deposition (MOCVD). These are discussed in the context of our prior β-Ga2O3 results, to provide a baseline from which trends and conclusions can be provided. MOCVD was used to grow b-(Al0.1Ga0.9)2O3 layers in an Agnitron Agilis R&D system, using TEGa, TMAl and O2 precursors on β-Ga2O3 (010) Sn-doped EFG-grown substrates with a growth temperature of 880 °C. To enable useful comparisons with our β-Ga2O3 results, an Al cation mole fraction of 0.10 was targeted for our initial studies, which should yield a bandgap of approximately 5.0 eV. Ni Schottky diodes were fabricated on the sample using conventional photolithography methods. Capacitance-voltage, current-voltage and internal photoemission measurements (IPE) revealed the Schottky diodes were suitable for defect spectroscopy measurements and characterize the Ni/b-(Al0.1Ga0.9)2O3 Schottky properties themselves. Comparisons are made to previously characterized Schottky diodes fabricated on a β-Ga2O3 epitaxial film grown by MOCVD in the same reactor under the same growth conditions [3]. The net doping concentration in the initial layers under study was measured by CV to be 1.8 x 1018 cm-3. Good Schottky behavior was observed, even at this high doping value, with strong rectification, ideality factor of ~1.5, and IPE-determined Schottky barrier heights of ~1.4 V. Preliminary deep level defect characterization using admittance spectroscopy (AS) along with DLTS and DLOS revealed the presence of five trap states within the b-(Al0.1Ga0.9)2O3 bandgap. A state with an activation energy of ~EC-0.2 eV as observed by AS; three trap levels were revealed by DLTS with approximate trap energies of ~EC-0.3 eV, ~EC-0.4 eV and EC-0.8 eV; and two trap levels were observed in the steady-state photo-capacitance (SSPC) spectra having onset energies of ~EC-2.0 eV and ~EC-4.6 eV. Overall, a similar energy distribution of trap states is observed compared with MOCVD grown b-Ga2O3 is suggestive of similar physical sources of traps between these the two materials, accounting for the small bandgap differences. A notable difference is the EC-0.8 eV trap, which is absent in the MOCVD b-Ga2O3, but matches the signature in b-Ga2O3 grown by other techniques suggesting it may be related to Fe [4]. Much more work is needed to confirm the meaning of these observations, which is ongoing. However, total trap concentrations are markedly different, being ~ 100x larger in the b-(Al0.1Ga0.9)2O3 epitaxial films, which is indicative of the very early stage of β-(Al,Ga)2O3 epitaxial growth development. Complete discussion of the nature of the traps seen in b-(Al0.1Ga0.9)2O3 and an expanded range of alloy compositions and growth conditions will be presented, including further comparisons to prior data obtained from high quality b-Ga2O3[3]. [1] N. Kalarickal, et al, J. Appl. Phys. 127, 215706 (2020) [2] Y. Zhang, et al, Appl. Phys. Lett. 112, 233503 (2018) [3] H. Ghadi, et al, Appl. Phys. Lett. 117, 172106 (2020) [4] J. F. McGlone, et al, Electron Dev. Lett. 39, 1042 (2018)

Quantitative Defect Characterization of MOCVD-Grown β-(Al,Ga)2O3 and Comparison with β-Ga2O3

Abstract Body: Ultra-wide-bandgap semiconductors (UWBG's) are a very promising material for the next-generation power semiconductors devices due to the rapid developments and requirements of highly efficient power electronics. The beta phase of Ga2O3 (β-Ga2O3) is considered in a family of UWBG semiconductors, which provides a new opportunity in myriad applications in electronics, optoelectronics, and photonics, with a superior performance matrix than conventional WBG materials. It exhibits some remarkable properties such as ultra-wide bandgap (>4.8 eV) at room temperature, thermally and chemically stability, high carrier mobility (>300 cm2/v.s), critical electric breakdown filed (~8 MV/cm), highest electron-Baliga’s Figure of Merit (BFoM). All of these properties could lead β-Ga2O3, a potential candidate for high-frequency devices, deep-ultraviolet optoelectronics, and high-power applications. However, the monoclinic and anisotropic crystal structure of β-Ga2O3 (a= 12.214 Å, b= 3.037 Å, and c=5.798 Å) exhibits larger lattice constant on the a-axis other than b-axes and c-axes. These benefits could open up a new direction of creating a nanoscale freestanding form of sub-micron thick β-Ga2O3 flake (typically known as nanomembranes, NMs), Recently several research groups have demonstrated creating NMs using the “Scotch tape” method. Thus, β-Ga2O3 provides a new opportunity to realize the use of UWBG’s in flexible devices that have the advantages of high breakdown electric field, transparency and solar blind photodetection while maintaining good mechanical stability. In fact, our group demonstrated the first flexible electronics (Schottky barrier diode and Solar blind photodetector) based on β-Ga2O3 NMs. However, structural-property relationship investigation of β-Ga2O3 NMs under mechanical strain conditions has not been well studied yet. Here in this presentation, we will first discuss the formation of nanogaps β-Ga2O3 NMs under uniaxial strain conditions, and the impact of randomly generated nanogaps on the electrical and optical properties using the β-Ga2O3 NMs fabricated on a plastic substrate. The scanning electron microscope (SEM) and the atomic force microscope (AFM) was used to identify the strain-induced nano-cracks, which also provided direct evidence of layer delamination and fracture in the β-Ga2O3 NMs. It was noticed that the electrical properties of β-Ga2O3 NM, such as the sheet resistance and capacitance were changed under uniaxial strain conditions. In order to investigate the change in sheet resistance and capacitance, a transmission line measurement (TLM) pattern was used. The results uncovered a significant degradation in the electrical properties and uneven distribution of the charges in the β-Ga2O3 NMs. The sheet resistance increased, and the total capacitance decreased due to substantial degradation of β-Ga2O3 NM’s under bending conditions. The optical properties of flexible β-Ga2O3 NMs were also investigated as a solar-blind photodetector. Interestingly, the degraded performance in β-Ga2O3 NM was recovered by employing a water vapor treatment. The presence of OH bonds in β-Ga2O3 NM confirmed by X-ray photoelectron spectroscopy (XPS) indicated that a water vapor treatment chemically bonds the nano-cracks effectively. Hence it was possible to recover up to 90 % of the original electrical properties. In addition, the water vapor treatment prevented further performance degradation in β-Ga2O3 NM from multiple bending cycles, thus providing good reliability. This result provides a viable route in realizing high-performance flexible devices, which is one of the crucial components in the upcoming internet of things era.

Nanogaps Formation and Recovery Process of Flexible β-Ga2O3 Nanomembranes Under Uniaxial Strain

Abstract Body: Light–matter interactions that induce charge and energy transfer across interfaces form the foundation for photocatalysis, energy harvesting and photodetection, among other technologies. One of the most common mechanisms associated with these processes relies on carrier injection. However, the exact role of the energy transport associated with this hot-electron injection remains unclear. Plasmon-assisted photocatalytic efficiencies can improve when intermediate insulation layers are used to inhibit the charge transfer or when off-resonance excitations are employed, which suggests that additional energy transport and thermal effects could play an explicit role even if the charge transfer is inhibited. This provides an additional interfacial mechanism for the catalytic and plasmonic enhancement at interfaces that moves beyond the traditionally assumed physical charge injection. In this work, we report on a series of ultrafast plasmonic measurements that provide a direct measure of electronic distributions, both spatially and temporally, after the optical excitation of a metal/semiconductor heterostructure. We explicitly demonstrate that in cases of strong non-equilibrium, a novel energy transduction mechanism arises at the metal/semiconductor interface. We find that hot electrons in the metal contact transfer their energy to pre-existing free electrons in the semiconductor, without an equivalent spatiotemporal transfer of charge. Further, we demonstrate that this ballistic thermal injection mechanism can be utilized as a unique means to modulate plasmonic interactions. These experimental results are well-supported by both rigorous multilayer optical modelling and first-principle ab initio calculations.

Long-Lived Modulation of Plasmonic Absorption by Ballistic Thermal Injection

Abstract Body: Surface plasmon polariton (SPP), which result from the strong coupling of bound electromagnetic (EM) waves and collective charge oscillations, enable subwavelength manipulation of light and matter interaction. Conventional noble metals-based SPP excited in the visible and near-Infrared spectra ranges suffer from large energy losses and cannot be dynamically tuned. Thanks to its 2D nature, graphene has emerged as a promising alternative plasmonic material with well- confined SPPs in the mid-infrared (MIR) and terahertz (THz) ranges and remarkable tunability. On the other hand, polar dielectric materials support low optical losses and sub-wavelength mode in the MIR and THz regions via surface phonon polariton (SPhP)mode' stimulation within the Reststrahlen band, a narrow spectral range between transverse optical (TO) and longitudinal optical (LO) frequencies. Due to the excellent polaritonic responses in both graphene and silicon carbide in the MIR and THz regions, devices combining the two materials are inferred to greatly advance photonics and THz technologies. We have recently theoretically demonstrated the strong confinement and large propagation figures of merit (FOM) for hybrid surface plasmon and surface phonon polariton in the epitaxial graphene on silicon carbide. The ability to confine such MIR light into small volume through excitation of SPP and SPhP has many implications for optoelectronic technologies such as the MIR photodetection[2], sensing[3], and solar cells[4]. Epitaxial graphene(EG) grown on silicon carbide(SiC) on silicon(Si) has been investigated as a suitable platform for graphene growth on semiconductors to meet the prospective technologies [5]. Despite this platform being very advantageous, experimental and theoretical works demonstrating the potentials properties/applications of EG on SiC on Si are still missing. Here we combine electromagnetic simulations based on finite elements method (FEM) with attenuated total reflectance Fourier transformed infrared (ATR-FTIR) spectroscopy to indicate improved MIR absorption, E field enhancement, and tunability for graphene-coated SiC nanowires (NWs). As anticipated, low absorption was confirmed from both simulations and measurements on bare SiC NWs, further supported by the calculated weak electric field due to the thin size of SiC NWs being incapable of absorbing sufficient light. On the other hand, enhanced absorption for the SiC NWs was measured by ATR-FTIR after a conformal graphitization of NWs[6]. Our previous study of this material system revealed a low-density oxide layer formed between graphene and SiC NWs[6]. This oxide layer between EG and SiC NW has been implemented in the FEM model, leading to field enhancement of incident EM field and strongly confined in the thin oxide. This substantial absorption and field enhancement originates from the coupling between the incident MIR photon and the plasmon/ phonon in graphene and SiC, respectively, with the oxide layer acting as a coupling medium. Furthermore, we demonstrate the modes' tunability whereby tuning the graphene's Fermi energy, the modes' resonance frequencies can be shifted to ~ 100 cm-1. Lastly, we realize substantial field enhancement, which is achieved by carefully tuning the graphene's Fermi energy and adjusting the spectra position of mode 1(mode on the left of LO frequency) closer to TO frequency. These results hold promise for various photonic applications such as perfect absorber to improve solar cell, MIR photodetectors, and other tunable photonics. [1]P. Rufangura, et al., J. Phys. Mater., vol. 3, no. 3, p. 032005, 2020. [2]T. Low and P. Avouris, ACS nano, vol. 8, no. 2, pp. 1086-1101, 2014. [3]A. G. Brolo, Nat. Photon., vol. 6, no. 11, p. 709, 2012. [4]H. A. Atwater and A. Polman, Nat. Mater., vol. 9, no. 3, p. 205, 2010. [5] N. Mishra et al., Phys. Status Solidi (a), vol. 213, no. 9, pp. 2277-2289, 2016. [6]N. Mishra et al., J. Appl. Phys., vol. 126, no. 6, p. 065304, 2019.

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Imaging the dynamics of 2D polariton wavepackets

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