Chan Wook Jang

High photoresponsivity in an all-graphene p – n vertical junction photodetector

Intensive studies have recently been performed on graphene-based photodetectors, but most of them are based on field effect transistor structures containing mechanically exfoliated graphene, not suitable for practical large-scale device applications. Here we report high-efficient photodetector behaviours of chemical vapor deposition grown all-graphene p-n vertical-type tunnelling diodes. The observed photodetector characteristics well follow what are expected from its band structure and the tunnelling of current through the interlayer between the metallic p- and n-graphene layers. High detectivity (~10(12) cm Hz(1/2) W(-1)) and responsivity (0.4~1.0 A W(-1)) are achieved in the broad spectral range from ultraviolet to near-infrared and the photoresponse is almost consistent under 6-month operations. The high photodetector performance of the graphene p-n vertical diodes can be understood by the high photocurrent gain and the carrier multiplication arising from impact ionization in graphene.

High-performance graphene-quantum-dot photodetectors

Graphene quantum dots (GQDs) have received much attention due to their novel phenomena of charge transport and light absorption/emission. The optical transitions are known to be available up to ~6 eV in GQDs, especially useful for ultraviolet (UV) photodetectors (PDs). Thus, the demonstration of photodetection gain with GQDs would be the basis for a plenty of applications not only as a single-function device in detecting optical signals but also a key component in the optoelectronic integrated circuits. Here, we firstly report high-efficient photocurrent (PC) behaviors of PDs consisting of multiple-layer GQDs sandwiched between graphene sheets. High detectivity (>1011 cm Hz1/2/W) and responsivity (0.2 ~ 0.5 A/W) are achieved in the broad spectral range from UV to near infrared. The observed unique PD characteristics prove to be dominated by the tunneling of charge carriers through the energy states in GQDs, based on bias-dependent variations of the band profiles, resulting in novel dark current and PC behaviors.

Rapid-thermal-annealing surface treatment for restoring the intrinsic properties of graphene field-effect transistors

Graphene field-effect transistors (GFETs) were fabricated by photolithography and lift-off processes, and subsequently heated in a rapid-thermal-annealing (RTA) apparatus at temperatures (T(A)) from 200 to 400 °C for 10 min under nitrogen to eliminate the residues adsorbed on the graphene during the GFET fabrication processes. Raman-scattering, current-voltage (I-V), and sheet resistance measurements showed that, after annealing at 250 °C, graphene in GFETs regained its intrinsic properties, such as very small intensity ratios of D to G and G to 2D Raman bands, a symmetric I-V curve with respect to ~0 V, and very low sheet resistance. Atomic force microscopy images and height profiles also showed that the surface roughness of graphene was almost minimized at T(A) = 250 °C. By annealing at 250 °C, the electron and hole mobilities reached their maxima of 4587 and 4605 cm(2) V(-1) s(-1), respectively, the highest ever reported for chemical-vapor-deposition-grown graphene. Annealing was also performed under vacuum or hydrogen, but this was not so effective as under nitrogen. These results suggest that the RTA technique is very useful for eliminating the surface residues of graphene in GFETs, in that it employs a relatively low thermal budget of 250 °C and 10 min.

Graphene p-n vertical tunneling diodes.

Formation and characterization of graphene p-n junctions are of particular interest because the p-n junctions are used in a wide variety of electronic/photonic systems as building blocks. Graphene p-n junctions have been previously formed by using several techniques, but most of the studies are based on lateral-type p-n junctions, showing no rectification behaviors. Here, we report a new type of graphene p-n junction. We first fabricate and characterize vertical-type graphene p-n junctions with two terminals. One of the most important characteristics of the vertical junctions is the asymmetric rectifying behavior showing an on/off ratio of ~10(3) under bias voltages below ±10 V without gating at higher n doping concentrations, which may be useful for practical device applications. In contrast, at lower n doping concentrations, the p-n junctions are ohmic, consistent with the Klein-tunneling effect. The observed rectification results possibly from the formation of strongly corrugated insulating or semiconducting interlayers between the metallic p- and n-graphene sheets at higher n doping concentrations, which is actually a structure like a metal-insulator-metal or metal-semiconductor-metal tunneling diode. The properties of the diodes are almost invariant even 6 months after fabrication.

Graphene/Si‐Quantum‐Dot Heterojunction Diodes Showing High Photosensitivity Compatible with Quantum Confinement Effect

Graphene/Si quantum dot (QD) heterojunction diodes are reported for the first time. The photoresponse, very sensitive to variations in the size of the QDs as well as in the doping concentration of graphene and consistent with the quantum-confinement effect, is remarkably enhanced in the near-ultraviolet range compared to commercially available bulk-Si photodetectors. The photoresponse proves to be dominated by the carriertunneling mechanism.

Annealing effects on the characteristics of AuCl3-doped graphene

Single-layer graphene sheets grown on Cu foils by chemical vapor deposition were transferred on 300 nm SiO2/n-type Si wafers and subsequently doped with 10 mM AuCl3 solution. The doped graphene sheets were annealed at various temperatures (TA) under vacuum below 10−3 Torr for 10 min and characterized by atomic force microscopy, Raman spectroscopy, x-ray photoelectron spectroscopy (XPS), and 4-probe van der Pauw method. The XPS studies show that the compositions of Cl and Au3+ ions in doped graphene sheets increase slightly by annealing at 50 °C, but by further increase of TA above 50 °C, they monotonically decrease and become almost negligible at TA = 500 °C. These XPS results are consistent with the corresponding TA-dependent behaviors of the Raman scattering and the sheet resistance, implying that the doping efficiency is maximized at TA = 50 °C and the Cl and Au3+ ions play a major role in the doping/dedoping processes that are very reversible, different from the case of carbon nanotubes. These results...

Energy transfer from an individual silica nanoparticle to graphene quantum dots and resulting enhancement of photodetector responsivity

Förster resonance energy transfer (FRET), referred to as the transfer of the photon energy absorbed in donor to acceptor, has received much attention as an important physical phenomenon for its potential applications in optoelectronic devices as well as for the understanding of some biological systems. If one-atom-thick graphene is used for donor or acceptor, it can minimize the separation between donor and acceptor, thereby maximizing the FRET efficiency (EFRET). Here, we report first fabrication of a FRET system composed of silica nanoparticles (SNPs) and graphene quantum dots (GQDs) as donors and acceptors, respectively. The FRET from SNPs to GQDs with an EFRET of ∼78% is demonstrated from excitation-dependent photoluminescence spectra and decay curves. The photodetector (PD) responsivity (R) of the FRET system at 532 nm is enhanced by 100∼101/102∼103 times under forward/reverse biases, respectively, compared to the PD containing solely GQDs. This remarkable enhancement is understood by network-like current paths formed by the GQDs on the SNPs and easy transfer of the carriers generated from the SNPs into the GQDs due to their close attachment. The R is 2∼3 times further enhanced at 325 nm by the FRET effect.

Structural and optical characteristics of graphene quantum dots size-controlled and well-aligned on a large scale by polystyrene-nanosphere lithography

Graphene quantum dots (GQDs) are one of the most attractive graphene nanostructures due to their potential optoelectronic device applications, but it is a challenge to accurately control the size and arrangement of GQDs. In this report, we fabricate well-aligned GQDs on a large area by polystyrene (PS)-nanosphere (NS) lithography and study their structural and optical properties. Single-layer graphene grown on a Cu foil by chemical vapour deposition is patterned by reactive ion etching employing aligned PS-NS arrays as an etching mask. The size (d) of the GQDs is controlled from 75 to 23 nm by varying the etching time, as proved by scanning electron microscopy and atomic force microscopy. This method is well valid for both rigid/flexible target substrates and even for multilayer graphene formed by piling up single layers. The absorption peak of the GQDs is blue-shifted with respect to that of a graphene sheet, and is sequentially shifted to higher energies by reducing d, consistent with the quantum confinement effect (QCE). The Raman D-to-G band intensity ratio shows an almost monotonic increase with decreasing d, resulting from the dominant contribution of the edge states at the periphery of smaller GQDs. The G-band frequency shows a three-step size-dependence: initial increase, interim saturation, and final decrease with decreasing d, thought to be caused by the competition between the QCE and edge-induced strain effect.

Light-induced negative differential resistance in graphene/Si-quantum-dot tunneling diodes

One of the interesing tunneling phenomena is negative differential resistance (NDR), the basic principle of resonant-tunneling diodes. NDR has been utilized in various semiconductor devices such as frequency multipliers, oscillators, relfection amplifiers, logic switches, and memories. The NDR in graphene has been also reported theoretically as well as experimentally, but should be further studied to fully understand its mechanism, useful for practical device applications. Especially, there has been no observation about light-induced NDR (LNDR) in graphene-related structures despite very few reports on the LNDR in GaAs-based heterostructures. Here, we report first observation of LNDR in graphene/Si quantum dots-embedded SiO2 (SQDs:SiO2) multilayers (MLs) tunneling diodes. The LNDR strongly depends on temperature (T) as well as on SQD size, and the T dependence is consistent with photocurrent (PC)-decay behaviors. With increasing light power, the PC-voltage curves are more structured with peak-to-valley ratios over 2 at room temperature. The physical mechanism of the LNDR, governed by resonant tunneling of charge carriers through the minibands formed across the graphene/SQDs:SiO2 MLs and by their nonresonant phonon-assisted tunneling, is discussed based on theoretical considerations.

Enhancement of efficiency and long-term stability in graphene/Si-quantum-dot heterojunction photodetectors by employing bis(trifluoromethanesulfonyl)-amide as a dopant for graphene

We for the first time employ bis(trifluoromethanesulfonyl)-amide as a dopant for graphene to enhance the efficiency and the stability of graphene/Si quantum dot (SQDs)-embedded SiO2 (SQDs:SiO2) multilayer (ML) heterojunction photodetectors (PDs). With increasing the doping concentration (nD) to 30 mM, the sheet resistance of the doped-graphene transparent conductive electrode (TCE) sharply decreases to ∼155 ohm sq−1 with only 1% reduction in its transmittance at 550 nm, whilst the work function gradually increases to ∼4.95 eV, indicating p-type doping, useful for the graphene/SQDs:SiO2 MLs interface. The DC conductivity/optical conductivity ratio saturates to ∼75 at nD = 20 mM, much larger than the minimum industry standard (= 35) for the optoelectronic applications of TCEs. The PDs optimized at nD = 20 mM exhibit 0.413 A W−1 responsivity (R), 92 dB linear dynamic range, 1.09 × 1010 cm Hz1/2 W−1 detectivity, and 81.33% external quantum efficiency at a peak wavelength of 630 nm, and the loss of R is almost negligible while the PDs are kept for 700 h in air. These characteristics are comparable to those of commercially-available Si PDs and better than those of previously-reported graphene/Si PDs.