Dephasing by optical phonons in GaN defect single-photon emitters.

Single-photon defect emitters (SPEs), especially those with magnetically and optically addressable spin states, in technologically mature wide bandgap semiconductors are attractive for realizing integrated platforms for quantum applications. Broadening of the zero phonon line (ZPL) caused by dephasing in solid state SPEs limits the indistinguishability of the emitted photons. Dephasing also limits the use of defect states in quantum information processing, sensing, and metrology. In most defect emitters, such as those in SiC and diamond, interaction with low-energy acoustic phonons determines the temperature dependence of the dephasing rate and the resulting broadening of the ZPL with the temperature obeys a power law. GaN hosts bright and stable single-photon emitters in the 600-700 nm wavelength range with strong ZPLs even at room temperature. In this work, we study the temperature dependence of the ZPL spectra of GaN SPEs integrated with solid immersion lenses with the goal of understanding the relevant dephasing mechanisms. At temperatures below ~ 50 K, the ZPL lineshape is found to be Gaussian and the ZPL linewidth is temperature independent and dominated by spectral diffusion. Above ~ 50 K, the linewidth increases monotonically with the temperature and the lineshape evolves into a Lorentzian. Quite remarkably, the temperature dependence of the linewidth does not follow a power law. We propose a model in which dephasing caused by absorption/emission of optical phonons in an elastic Raman process determines the temperature dependence of the lineshape and the linewidth. Our model explains the temperature dependence of the ZPL linewidth and lineshape in the entire 10-270 K temperature range explored in this work. The ~ 19 meV optical phonon energy extracted by fitting the model to the data matches remarkably well the ~ 18 meV zone center energy of the lowest optical phonon band ([Formula: see text]) in GaN. Our work sheds light on the mechanisms responsible for linewidth broadening in GaN SPEs. Since a low energy optical phonon band ([Formula: see text]) is a feature of most group III-V nitrides with a wurtzite crystal structure, including hBN and AlN, we expect our proposed mechanism to play an important role in defect emitters in these materials as well.

Molecular beam homoepitaxy of N-polar AlN: Enabling role of aluminum-assisted surface cleaning.

N-polar aluminum nitride (AlN) is an important building block for next-generation high-power radio frequency electronics. We report successful homoepitaxial growth of N-polar AlN by molecular beam epitaxy (MBE) on large-area, cost-effective N-polar AlN templates. Direct growth without any in situ surface cleaning leads to films with inverted Al polarity. It is found that Al-assisted cleaning before growth enables the epitaxial film to maintain N-polarity. The grown N-polar AlN epilayer with its smooth, pit-free surface duplicates the structural quality of the substrate, as evidenced by a clean and smooth growth interface with no noticeable extended defects generation. Near band-edge photoluminescence peaks are observed at room temperature on samples with MBE-grown layers but not on the bare AlN templates, implying the suppression of nonradiative recombination centers in the epitaxial N-polar AlN.

Properties for Thermally Conductive Interfaces with Wide Band Gap Materials.

The goal of this study is to determine how bulk vibrational properties and interfacial structure affect thermal transport at interfaces in wide band gap semiconductor systems. Time-domain thermoreflectance measurements of thermal conductance G are reported for interfaces between nitride metals and group IV (diamond, SiC, Si, and Ge) and group III-V (AlN, GaN, and cubic BN) materials. Group IV and group III-V semiconductors have systematic differences in vibrational properties. Similarly, HfN and TiN are also vibrationally distinct from each other. Therefore, comparing G of interfaces formed from these materials provides a systematic test of how vibrational similarity between two materials affects interfacial transport. For HfN interfaces, we observe conductances between 140 and 300 MW m-2 K-1, whereas conductances between 200 and 800 MW m-2 K-1 are observed for TiN interfaces. TiN forms exceptionally conductive interfaces with GaN, AlN, and diamond, that is, G > 400 MW m-2 K-1. Surprisingly, interfaces formed between vibrationally similar and dissimilar materials are similarly conductive. Thus, vibrational similarity between two materials is not a necessary requirement for high G. Instead, the time-domain thermoreflectance experiment (TDTR) data, an analysis of bulk vibrational properties, and transmission electron microscopy (TEM) suggest that G depends on two other material properties, namely, the bulk phonon properties of the vibrationally softer of the two materials and the interfacial structure. To determine how G depends on interfacial structure, TDTR and TEM measurements were conducted on a series of TiN/AlN samples prepared in different ways. Interfacial disorder at a TiN/AlN interface adds a thermal resistance equivalent to ∼1 nm of amorphous material. Our findings improve fundamental understanding of what material properties are most important for thermally conductive interfaces. They also provide benchmarks for the thermal conductance of interfaces with wide band gap semiconductors.

Momentum-resolved electronic structure and band offsets in an epitaxial NbN/GaN superconductor/semiconductor heterojunction.

The electronic structure of heterointerfaces is a pivotal factor for their device functionality. We use soft x-ray angle-resolved photoelectron spectroscopy to directly measure the momentum-resolved electronic band structures on both sides of the Schottky heterointerface formed by epitaxial films of the superconducting NbN on semiconducting GaN, and determine their momentum-dependent interfacial band offset as well as the band-bending profile. We find, in particular, that the Fermi states in NbN are well separated in energy and momentum from the states in GaN, excluding any notable electronic cross-talk of the superconducting states in NbN to GaN. We support the experimental findings with first-principles calculations for bulk NbN and GaN. The Schottky barrier height obtained from photoemission is corroborated by electronic transport and optical measurements. The momentum-resolved understanding of electronic properties of interfaces elucidated in our work opens up new frontiers for the quantum materials where interfacial states play a defining role.

An all-epitaxial nitride heterostructure with concurrent quantum Hall effect and superconductivity.

Creating seamless heterostructures that exhibit the quantum Hall effect and superconductivity is highly desirable for future electronics based on topological quantum computing. However, the two topologically robust electronic phases are typically incompatible owing to conflicting magnetic field requirements. Combined advances in the epitaxial growth of a nitride superconductor with a high critical temperature and a subsequent nitride semiconductor heterostructure of metal polarity enable the observation of clean integer quantum Hall effect in the polarization-induced two-dimensional (2D) electron gas of the high-electron mobility transistor. Through individual magnetotransport measurements of the spatially separated GaN 2D electron gas and superconducting NbN layers, we find a small window of magnetic fields and temperatures in which the epitaxial layers retain their respective quantum Hall and superconducting properties. Its analysis indicates that in epitaxial nitride superconductor/semiconductor heterostructures, this window can be significantly expanded, creating an industrially viable platform for robust quantum devices that exploit topologically protected transport.

Crystal orientation dictated epitaxy of ultrawide-bandgap 5.4- to 8.6-eV α-(AlGa)2O3 on m-plane sapphire.

Ultrawide-bandgap semiconductors are ushering in the next generation of high-power electronics. The correct crystal orientation can make or break successful epitaxy of such semiconductors. Here, it is found that single-crystalline layers of α-(AlGa)2O3 alloys spanning bandgaps of 5.4 to 8.6 eV can be grown by molecular beam epitaxy. The key step is found to be the use of m-plane sapphire crystal. The phase transition of the epitaxial layers from the α- to the narrower bandgap ß-phase is catalyzed by the c-plane of the crystal. Because the c-plane is orthogonal to the growth front of the m-plane surface of the crystal, the narrower bandgap pathways are eliminated, revealing a route to much wider bandgap materials with structural purity. The resulting energy bandgaps of the epitaxial layers span a broad range, heralding the successful epitaxial stabilization of the largest bandgap materials family to date.

Engineering the Berreman mode in mid-infrared polar materials.

We demonstrate coupling to and control over the broadening and dispersion of a mid-infrared leaky mode, known as the Berreman mode, in samples with different dielectric environments. We fabricate subwavelength films of AlN, a mid-infrared epsilon-near-zero material that supports the Berreman mode, on materials with a weakly negative permittivity, strongly negative permittivity, and positive permittivity. Additionally, we incorporate ultra-thin AlN layers into a GaN/AlN heterostructure, engineering the dielectric environment above and below the AlN. In each of the samples, coupling to the Berreman mode is observed in angle-dependent reflection measurements at wavelengths near the longitudinal optical phonon energy. The measured dispersion of the Berreman mode agrees well with numerical modes. Differences in the dispersion and broadening for the different materials is quantified, including a 13 cm-1 red-shift in the energy of the Berreman mode for the heterostructure sample.

Enhanced injection efficiency and light output in bottom tunnel-junction light-emitting diodes.

Recently, the use of bottom-TJ geometry in LEDs, which achieves N-polar-like alignment of polarization fields in conventional metal-polar orientations, has enabled enhancements in LED performance due to improved injection efficiency. Here, we elucidate the root causes behind the enhanced injection efficiency by employing mature laser diode structures with optimized heterojunction GaN/In0.17Ga0.83N/GaN TJs and UID GaN spacers to separate the optical mode from the heavily doped absorbing p-cladding regions. In such laser structures, polarization offsets at the electron blocking layer, spacer, and quantum barrier interfaces play discernable roles in carrier transport. By comparing a top-TJ structure to a bottom-TJ structure, and correlating features in the electroluminescence, capacitance-voltage, and current-voltage characteristics to unique signatures of the N- and Ga-polar polarization heterointerfaces in energy band diagram simulations, we identify that improved hole injection at low currents, and improved electron blocking at high currents, leads to higher injection efficiency and higher output power for the bottom-TJ device throughout 5 orders of current density (0.015-1000 A/cm2). Moreover, even with the addition of a UID GaN spacer, differential resistances are state-of-the-art, below 7 × 10-4 Ωcm2. These results highlight the virtues of the bottom-TJ geometry for use in high-efficiency laser diodes.

A polarization-induced 2D hole gas in undoped gallium nitride quantum wells.

A high-conductivity two-dimensional (2D) hole gas, analogous to the ubiquitous 2D electron gas, is desirable in nitride semiconductors for wide-bandgap p-channel transistors. We report the observation of a polarization-induced high-density 2D hole gas in epitaxially grown gallium nitride on aluminium nitride and show that such hole gases can form without acceptor dopants. The measured high 2D hole gas densities of about 5 × 1013 per square centimeters remain unchanged down to cryogenic temperatures and allow some of the lowest p-type sheet resistances among all wide-bandgap semiconductors. The observed results provide a probe for studying the valence band structure and transport properties of wide-bandgap nitride interfaces.

Route to High Hole Mobility in GaN via Reversal of Crystal-Field Splitting.

A fundamental obstacle toward the realization of GaN p-channel transistors is its low hole mobility. Here we investigate the intrinsic phonon-limited mobility of electrons and holes in wurtzite GaN using the ab initio Boltzmann transport formalism, including all electron-phonon scattering processes and many-body quasiparticle band structures. We predict that the hole mobility can be increased by reversing the sign of the crystal-field splitting in such a way as to lift the split-off hole states above the light and heavy holes. We find that a 2% biaxial tensile strain can increase the hole mobility by 230%, up to a theoretical Hall mobility of 120 cm^{2}/V s at room temperature and 620 cm^{2}/V s at 100 K.

GaN/NbN epitaxial semiconductor/superconductor heterostructures.

Epitaxy is a process by which a thin layer of one crystal is deposited in an ordered fashion onto a substrate crystal. The direct epitaxial growth of semiconductor heterostructures on top of crystalline superconductors has proved challenging. Here, however, we report the successful use of molecular beam epitaxy to grow and integrate niobium nitride (NbN)-based superconductors with the wide-bandgap family of semiconductors-silicon carbide, gallium nitride (GaN) and aluminium gallium nitride (AlGaN). We apply molecular beam epitaxy to grow an AlGaN/GaN quantum-well heterostructure directly on top of an ultrathin crystalline NbN superconductor. The resulting high-mobility, two-dimensional electron gas in the semiconductor exhibits quantum oscillations, and thus enables a semiconductor transistor-an electronic gain element-to be grown and fabricated directly on a crystalline superconductor. Using the epitaxial superconductor as the source load of the transistor, we observe in the transistor output characteristics a negative differential resistance-a feature often used in amplifiers and oscillators. Our demonstration of the direct epitaxial growth of high-quality semiconductor heterostructures and devices on crystalline nitride superconductors opens up the possibility of combining the macroscopic quantum effects of superconductors with the electronic, photonic and piezoelectric properties of the group III/nitride semiconductor family.

Hot Electron Transistor with van der Waals Base-Collector Heterojunction and High-Performance GaN Emitter.

Single layer graphene is an ideal material for the base layer of hot electron transistors (HETs) for potential terahertz (THz) applications. The ultrathin body and exceptionally long mean free path maximizes the probability for ballistic transport across the base of the HET. We demonstrate for the first time the operation of a high-performance HET using a graphene/WSe2 van der Waals (vdW) heterostructure as a base-collector barrier. The resulting device with a GaN/AlN heterojunction as emitter, exhibits a current density of 50 A/cm2, direct current gain above 3 and 75% injection efficiency, which are record values among graphene-base HETs. These results not only provide a scheme to overcome the limitations of graphene-base HETs toward THz operation but are also the first demonstration of a GaN/vdW heterostructure in HETs, revealing the potential for novel electronic and optoelectronic applications.

Layered transition metal dichalcogenides: promising near-lattice-matched substrates for GaN growth.

Most III-nitride semiconductors are grown on non-lattice-matched substrates like sapphire or silicon due to the extreme difficulty of obtaining a native GaN substrate. We show that several layered transition-metal dichalcogenides are closely lattice-matched to GaN and report the growth of GaN on a range of such layered materials. We report detailed studies of the growth of GaN on mechanically-exfoliated flakes WS2 and MoS2 by metalorganic vapour phase epitaxy. Structural and optical characterization show that strain-free, single-crystal islands of GaN are obtained on the underlying chalcogenide flakes. We obtain strong near-band-edge emission from these layers, and analyse their temperature-dependent photoluminescence properties. We also report a proof-of-concept demonstration of large-area growth of GaN on CVD MoS2. Our results show that the transition-metal dichalcogenides can serve as novel near-lattice-matched substrates for nitride growth.

Scanning Tunneling Microscopy and Spectroscopy of Air Exposure Effects on Molecular Beam Epitaxy Grown WSe2 Monolayers and Bilayers.

The effect of air exposure on 2H-WSe2/HOPG is determined via scanning tunneling microscopy (STM). WSe2 was grown by molecular beam epitaxy on highly oriented pyrolytic graphite (HOPG), and afterward, a Se adlayer was deposited in situ on WSe2/HOPG to prevent unintentional oxidation during transferring from the growth chamber to the STM chamber. After annealing at 773 K to remove the Se adlayer, STM images show that WSe2 layers nucleate at both step edges and terraces of the HOPG. Exposure to air for 1 week and 9 weeks caused air-induced adsorbates to be deposited on the WSe2 surface; however, the band gap of the terraces remained unaffected and nearly identical to those on decapped WSe2. The air-induced adsorbates can be removed by annealing at 523 K. In contrast to WSe2 terraces, air exposure caused the edges of the WSe2 to oxidize and form protrusions, resulting in a larger band gap in the scanning tunneling spectra compared to the terraces of air-exposed WSe2 monolayers. The preferential oxidation at the WSe2 edges compared to the terraces is likely the result of dangling edge bonds. In the absence of air exposure, the dangling edge bonds had a smaller band gap compared to the terraces and a shift of about 0.73 eV in the Fermi level toward the valence band. However, after air exposure, the band gap of the oxidized WSe2 edges became about 1.08 eV larger than that of the WSe2 terraces, resulting in the electronic passivation of the WSe2.

Esaki Diodes in van der Waals Heterojunctions with Broken-Gap Energy Band Alignment.

van der Waals (vdW) heterojunctions composed of two-dimensional (2D) layered materials are emerging as a solid-state materials family that exhibits novel physics phenomena that can power a range of electronic and photonic applications. Here, we present the first demonstration of an important building block in vdW solids: room temperature Esaki tunnel diodes. The Esaki diodes were realized in vdW heterostructures made of black phosphorus (BP) and tin diselenide (SnSe2), two layered semiconductors that possess a broken-gap energy band offset. The presence of a thin insulating barrier between BP and SnSe2 enabled the observation of a prominent negative differential resistance (NDR) region in the forward-bias current-voltage characteristics, with a peak to valley ratio of 1.8 at 300 K and 2.8 at 80 K. A weak temperature dependence of the NDR indicates electron tunneling being the dominant transport mechanism, and a theoretical model shows excellent agreement with the experimental results. Furthermore, the broken-gap band alignment is confirmed by the junction photoresponse, and the phosphorus double planes in a single layer of BP are resolved in transmission electron microscopy (TEM) for the first time. Our results represent a significant advance in the fundamental understanding of vdW heterojunctions and broaden the potential applications of 2D layered materials.

High-performance, highly bendable MoS2 transistors with high-k dielectrics for flexible low-power systems.

While there has been increasing studies of MoS2 and other two-dimensional (2D) semiconducting dichalcogenides on hard conventional substrates, experimental or analytical studies on flexible substrates has been very limited so far, even though these 2D crystals are understood to have greater prospects for flexible smart systems. In this article, we report detailed studies of MoS2 transistors on industrial plastic sheets. Transistor characteristics afford more than 100x improvement in the ON/OFF current ratio and 4x enhancement in mobility compared to previous flexible MoS2 devices. Mechanical studies reveal robust electronic properties down to a bending radius of 1 mm which is comparable to previous reports for flexible graphene transistors. Experimental investigation identifies that crack formation in the dielectric is the responsible failure mechanism demonstrating that the mechanical properties of the dielectric layer is critical for realizing flexible electronics that can accommodate high strain. Our uniaxial tensile tests have revealed that atomic-layer-deposited HfO2 and Al2O3 films have very similar crack onset strain. However, crack propagation is slower in HfO2 dielectric compared to Al2O3 dielectric, suggesting a subcritical fracture mechanism in the thin oxide films. Rigorous mechanics modeling provides guidance for achieving flexible MoS2 transistors that are reliable at sub-mm bending radius.

Role of metal contacts in designing high-performance monolayer n-type WSe2 field effect transistors.

This work presents a systematic study toward the design and first demonstration of high-performance n-type monolayer tungsten diselenide (WSe2) field effect transistors (FET) by selecting the contact metal based on understanding the physics of contact between metal and monolayer WSe2. Device measurements supported by ab initio density functional theory (DFT) calculations indicate that the d-orbitals of the contact metal play a key role in forming low resistance ohmic contacts with monolayer WSe2. On the basis of this understanding, indium (In) leads to small ohmic contact resistance with WSe2 and consequently, back-gated In-WSe2 FETs attained a record ON-current of 210 µA/µm, which is the highest value achieved in any monolayer transition-metal dichalcogenide- (TMD) based FET to date. An electron mobility of 142 cm(2)/V·s (with an ON/OFF current ratio exceeding 10(6)) is also achieved with In-WSe2 FETs at room temperature. This is the highest electron mobility reported for any back gated monolayer TMD material till date. The performance of n-type monolayer WSe2 FET was further improved by Al2O3 deposition on top of WSe2 to suppress the Coulomb scattering. Under the high-κ dielectric environment, electron mobility of Ag-WSe2 FET reached ~202 cm(2)/V·s with an ON/OFF ratio of over 10(6) and a high ON-current of 205 µA/µm. In tandem with a recent report of p-type monolayer WSe2 FET ( Fang , H . et al. Nano Lett. 2012 , 12 , ( 7 ), 3788 - 3792 ), this demonstration of a high-performance n-type monolayer WSe2 FET corroborates the superb potential of WSe2 for complementary digital logic applications.

Terahertz imaging employing graphene modulator arrays.

In this paper we propose and experimentally demonstrate arrays of graphene electro-absorption modulators as electrically reconfigurable patterns for terahertz cameras. The active element of these modulators consists of only single-atom-thick graphene, achieving a modulation of the THz wave reflectance > 50% with a potential modulation depth approaching 100%. Although the prototype presented here only contains 4x4 pixels, it reveals the possibility of developing reliable low-cost video-rate THz imaging systems employing single detector.

Exciton dynamics in suspended monolayer and few-layer MoS2 2D crystals.

Femtosecond transient absorption spectroscopy and microscopy were employed to study exciton dynamics in suspended and Si3N4 substrate-supported monolayer and few-layer MoS2 2D crystals. Exciton dynamics for the monolayer and few-layer structures were found to be remarkably different from those of thick crystals when probed at energies near that of the lowest energy direct exciton (A exciton). The intraband relaxation rate was enhanced by more than 40 fold in the monolayer in comparison to that observed in the thick crystals, which we attributed to defect assisted scattering. Faster electron-hole recombination was found in monolayer and few-layer structures due to quantum confinement effects that lead to an indirect-direct band gap crossover. Nonradiative rather than radiative relaxation pathways dominate the dynamics in the monolayer and few-layer MoS2. Fast trapping of excitons by surface trap states was observed in monolayer and few-layer structures, pointing to the importance of controlling surface properties in atomically thin crystals such as MoS2 along with controlling their dimensions.