Fangze Liu

Tunable Graphene–Silicon Heterojunctions for Ultrasensitive Photodetection

We present the photodetection properties of graphene/Si heterojunctions both in the photocurrent and photovoltage modes. Monolayer graphene/Si junctions were found to be excellent weak-signal detectors with photovoltage responsivity exceeding 10(7) V/W and with noise-equivalent-power reaching ∼1 pW/Hz(1/2), potentially capable of distinguishing materials with transmittance, T = 0.9995 in a 0.5 s integration time. In the photocurrent mode, the response was found to remain linear over at least six decades of incident power (P), with tunable responsivity up to 435 mA/W (corresponding to incident photon conversion efficiency (IPCE) > 65%) obtained by layer thickening and doping. With millisecond-scale responses and ON/OFF ratios exceeding 10(4), these photodiodes are highly suitable for tunable and scalable broadband (400 < λ < 900 nm) photodetectors, photometers, and millisecond-response switching, spectroscopic and imaging devices, and further, and are architecturally compatible with on-chip low-power optoelectronics.

Quantum Carrier Reinvestment-induced ultrahigh and broadband photocurrent responses in graphene-silicon junctions.

In an earlier work, we had reported a method that enables graphene-silicon junctions to display exceptionally high photovoltaic responses, exceeding 10(7) V/W. Using a completely different method that has recently been reported to result in ultrahigh gain, we now show that these junctions can also demonstrate giant photocurrent responsivities that can approach ∼ 10(7) A/W. Together, these mechanisms enable graphene-silicon junctions to be a dual-mode, broad-band, scalable, CMOS-compatible, and tunable photodetector that can operate either in photovoltage or photocurrent modes with ultrahigh responsivity values. We present detailed validation of the underlying mechanism (which we call Quantum Carrier Reinvestment, or QCR) in graphene-silicon junctions. In addition to ultrasensitive photodetection, we present QCR photocurrent spectroscopy as a tool for investigating spectral recombination dynamics at extremely low incident powers, a topic of significant importance for optoelectronic applications. We show that such spectroscopic studies can also provide a direct measure of photon energy values associated with various allowed optical transitions in silicon, again an extremely useful technique that can in principle be extended to characterize electronic levels in arbitrary semiconductors or nanomaterials. We further show the significant impact that underlying substrates can have on photocurrents, using QCR-photocurrent mapping. Contrary to expectations, QCR-photocurrents in graphene on insulating SiO2 substrates can be much higher than its intrinsic photocurrents, and even larger than QCR-photocurrents obtained in graphene overlaying semiconducting or metallic substrates. These results showcase the vital role of substrates in photocurrent measurements in graphene or potentially in other similar materials which have relatively high carrier mobility values.

Chemical Vapor Deposition Synthesized Atomically Thin Molybdenum Disulfide with Optoelectronic-Grade Crystalline Quality

The ability to synthesize high-quality samples over large areas and at low cost is one of the biggest challenges during the developmental stage of any novel material. While chemical vapor deposition (CVD) methods provide a promising low-cost route for CMOS compatible, large-scale growth of materials, it often falls short of the high-quality demands in nanoelectronics and optoelectronics. We present large-scale CVD synthesis of single- and few-layered MoS2 using direct vapor-phase sulfurization of MoO2, which enables us to obtain extremely high-quality single-crystal monolayer MoS2 samples with field-effect mobility exceeding 30 cm(2)/(V s) in monolayers. These samples can be readily synthesized on a variety of substrates, and demonstrate a high-degree of optoelectronic uniformity in Raman and photoluminescence mapping over entire crystals with areas exceeding hundreds of square micrometers. Because of their high crystalline quality, Raman spectroscopy on these samples reveal a range of multiphonon processes through peaks with equal or better clarity compared to past reports on mechanically exfoliated samples. This enables us to investigate the layer thickness and substrate dependence of the extremely weak phonon processes at 285 and 487 cm(-1) in 2D-MoS2. The ultrahigh, optoelectronic-grade crystalline quality of these samples could be further established through photocurrent spectroscopy, which clearly reveal excitonic states at room temperature, a feat that has been previously demonstrated only on samples which were fabricated by micro-mechanical exfoliation and then artificially suspended across trenches. Our method reflects a big step in the development of atomically thin, 2D-MoS2 for scalable, high-quality optoelectronics.

Atomically thin layers of B-N-C-O with tunable composition

Atomically thin quaternary alloy of boron, nitrogen, carbon and oxygen, 2D-BNCO with tunable composition. In recent times, atomically thin alloys of boron, nitrogen, and carbon have generated significant excitement as a composition-tunable two-dimensional (2D) material that demonstrates rich physics as well as application potentials. The possibility of tunably incorporating oxygen, a group VI element, into the honeycomb sp2-type 2D-BNC lattice is an intriguing idea from both fundamental and applied perspectives. We present the first report on an atomically thin quaternary alloy of boron, nitrogen, carbon, and oxygen (2D-BNCO). Our experiments suggest, and density functional theory (DFT) calculations corroborate, stable configurations of a honeycomb 2D-BNCO lattice. We observe micrometer-scale 2D-BNCO domains within a graphene-rich 2D-BNC matrix, and are able to control the area coverage and relative composition of these domains by varying the oxygen content in the growth setup. Macroscopic samples comprising 2D-BNCO domains in a graphene-rich 2D-BNC matrix show graphene-like gate-modulated electronic transport with mobility exceeding 500 cm2 V−1 s−1, and Arrhenius-like activated temperature dependence. Spin-polarized DFT calculations for nanoscale 2D-BNCO patches predict magnetic ground states originating from the B atoms closest to the O atoms and sizable (0.6 eV < Eg < 0.8 eV) band gaps in their density of states. These results suggest that 2D-BNCO with novel electronic and magnetic properties have great potential for nanoelectronics and spintronic applications in an atomically thin platform.

Graphene–aluminum nitride NEMS resonant infrared detector

The use of micro-/nanoelectromechanical resonators for the room temperature detection of electromagnetic radiation at infrared frequencies has recently been investigated, showing thermal detection capabilities that could potentially outperform conventional microbolometers. The scaling of the device thickness in the nanometer range and the achievement of high infrared absorption in such a subwavelength thickness, without sacrificing the electromechanical performance, are the two key challenges for the implementation of fast, high-resolution micro-/nanoelectromechanical resonant infrared detectors. In this paper, we show that by using a virtually massless, high-electrical-conductivity, and transparent graphene electrode, floating at the van der Waals separation of a few angstroms from a piezoelectric aluminum nitride nanoplate, it is possible to implement ultrathin (460 nm) piezoelectric nanomechanical resonant structures with improved electromechanical performance (>50% improved frequency×quality factor) and infrared detection capabilities (>100× improved infrared absorptance) compared with metal-electrode counterparts, despite their reduced volumes. The intrinsic infrared absorption capabilities of a submicron thin graphene–aluminum nitride plate backed with a metal electrode are investigated for the first time and exploited for the first experimental demonstration of a piezoelectric nanoelectromechanical resonant thermal detector with enhanced infrared absorptance in a reduced volume. Moreover, the combination of electromagnetic and piezoelectric resonances provided by the same graphene–aluminum nitride-metal stack allows the proposed device to selectively detect short-wavelength infrared radiation (by tailoring the thickness of aluminum nitride) with unprecedented electromechanical performance and thermal capabilities. These attributes potentially lead to the development of uncooled infrared detectors suitable for the implementation of high performance, miniaturized and power-efficient multispectral infrared imaging systems.

The Changing Colors of a Quantum- Confined Topological Insulator

Bismuth selenide (Bi2Se3) is a 3D topological insulator, its strong spin-orbit coupling resulting in the well-known topologically protected coexistence of gapless metallic surface states and semiconducting bulk states with a band gap, Eg ≃ 300 meV. A fundamental question of considerable importance is how the electronic properties of this material evolve under nanoscale confinement. We report on catalyst-free, high-quality single-crystalline Bi2Se3 with controlled lateral sizes and layer thicknesses that could be tailored down to a few nanometers and a few quintuple layers (QLs), respectively. Energy-resolved photoabsorption spectroscopy (1.5 eV < E(photon) < 6 eV) of these samples reveals a dramatic evolution of the photon absorption spectra as a function of size, transitioning from a featureless metal-like spectrum in the bulk (corresponding to a visually gray color), to one with a remarkably large band gap (Eg ≥ 2.5 eV) and a spectral shape that correspond to orange-red colorations in the smallest samples, similar to those seen in semiconductor nanostructures. We analyze this colorful transition using ab initio density functional theory and tight-binding calculations which corroborate our experimental findings and further suggest that while purely 2D sheets of few QL-thick Bi2Se3 do exhibit small band gaps that are consistent with previous ARPES results, the presently observed large gaps of a few electronvolts can only result from a combined effect of confinement in all three directions.

Single transistor oscillator based on a Graphene-Aluminum Nitride nano plate resonator

This paper reports on the first demonstration of a high frequency (245 MHz) single transistor oscillator based on Graphene-Aluminum Nitride (G-AlN) nano-plate resonator (NPR). For the first time, a 2-dimensional (2D) electrically conductive graphene layer was integrated on top of an ultra-thin (500 nm) AlN nano-plate and excited into a high frequency contour-extensional mode of vibration by piezoelectric transduction. The resulting ultra-thin, low mass and high frequency G-AlN nanomechanical resonator showed high values of electromechanical coupling coefficient (kt2≈1.8%) and quality factor (Qm≈1000) which enabled the implementation of a low phase noise (-87 dBc/Hz @ 1kHz offset and -125 dBc/Hz floor) single transistor oscillator. The experimental results also demonstrate the great potential of the proposed technology for the implementation of a new class of ultra-sensitive and low noise G-AlN resonant sensors.

Giant enhancement of light emission from nanoscale Bi2Se3

Bi2Se3 is a well-known room temperature topological insulator with a gapless surface state and ∼300 meV bulk band-gap, and as such has never been proposed to possess light-emitting properties. Here, we report prominent light emission in the visible region via photoluminescence (PL) measurements of chemical vapor deposition grown Bi2Se3 nanoplates with an average thickness and effective diameter of tens of nanometers. When excited using 488 nm (2.54 eV) laser light, these nanoscale Bi2Se3 platelets show a strong photoluminescence response in the Eph ∼ 2.1–2.3 eV region, with significant enhancement of light emission compared to bulk level emission. After annealing samples at 200 °C for 4 h, PL intensity increased by a factor of 2.4 to 3 for nanoscale Bi2Se3.

Tunable and laser-reconfigurable 2D heterocrystals obtained by epitaxial stacking of crystallographically incommensurate Bi2Se3 and MoS2 atomic layers

Heterocrystals: rotationally oriented stacks of incommensurate 2D materials with tunable and laser-reconfigurable properties. Vertical stacking is widely viewed as a promising approach for designing advanced functionalities using two-dimensional (2D) materials. Combining crystallographically commensurate materials in these 2D stacks has been shown to result in rich new electronic structure, magnetotransport, and optical properties. In this context, vertical stacks of crystallographically incommensurate 2D materials with well-defined crystallographic order are a counterintuitive concept and, hence, fundamentally intriguing. We show that crystallographically dissimilar and incommensurate atomically thin MoS2 and Bi2Se3 layers can form rotationally aligned stacks with long-range crystallographic order. Our first-principles theoretical modeling predicts heterocrystal electronic band structures, which are quite distinct from those of the parent crystals, characterized with an indirect bandgap. Experiments reveal striking optical changes when Bi2Se3 is stacked layer by layer on monolayer MoS2, including 100% photoluminescence (PL) suppression, tunable transmittance edge (1.1→0.75 eV), suppressed Raman, and wide-band evolution of spectral transmittance. Disrupting the interface using a focused laser results in a marked the reversal of PL, Raman, and transmittance, demonstrating for the first time that in situ manipulation of interfaces can enable “reconfigurable” 2D materials. We demonstrate submicrometer resolution, “laser-drawing” and “bit-writing,” and novel laser-induced broadband light emission in these heterocrystal sheets.

1.27 GHz Graphene-Aluminum Nitride nano plate resonant infrared detector

This paper reports on the Infrared (IR) detection capabilities of a 1.27 GHz Graphene-Aluminum Nitride (G-AlN) nano-plate resonator. For the first time we demonstrate that by using a virtually massless graphene electrode, floating at the van der Waals separation of a few angstroms from a piezoelectric nano-plate (zero interfacial strain), it is possible to implement ultra-thin (460 nm) piezoelectric nanomechanical resonant structures operating in the GHz range with improved electromechanical performance (2X improved f·Q) and IR detection capabilities (>100X improved IR absorptance) compared to conventional devices employing metal electrodes. The demonstrated achievement of low damping, efficient electromechanical transduction and high IR responsivity, in nanomechanical resonant structures with reduced volume and higher vibration frequency, addresses one of the most fundamental challenges in the NEMS field opening exciting new directions in nanotechnology.