Jeong Won Kim

Graphene Oxide Thin Films for Flexible Nonvolatile Memory Applications

There has been strong demand for novel nonvolatile memory technology for low-cost, large-area, and low-power flexible electronics applications. Resistive memories based on metal oxide thin films have been extensively studied for application as next-generation nonvolatile memory devices. However, although the metal oxide based resistive memories have several advantages, such as good scalability, low-power consumption, and fast switching speed, their application to large-area flexible substrates has been limited due to their material characteristics and necessity of a high-temperature fabrication process. As a promising nonvolatile memory technology for large-area flexible applications, we present a graphene oxide based memory that can be easily fabricated using a room temperature spin-casting method on flexible substrates and has reliable memory performance in terms of retention and endurance. The microscopic origin of the bipolar resistive switching behavior was elucidated and is attributed to rupture and formation of conducting filaments at the top amorphous interface layer formed between the graphene oxide film and the top Al metal electrode, via high-resolution transmission electron microscopy and in situ X-ray photoemission spectroscopy. This work provides an important step for developing understanding of the fundamental physics of bipolar resistive switching in graphene oxide films, for the application to future flexible electronics.

Energy level alignment at a charge generation interface between 4,4′-bis(N-phenyl-1-naphthylamino)biphenyl and 1,4,5,8,9,11-hexaazatriphenylene-hexacarbonitrile

We have determined the electronic energy level alignment at the interface between 4,4′-bis(N-phenyl-1-naphthylamino)biphenyl (NPB) and 1,4,5,8,9,11-hexaazatriphenylene-hexacarbonitrile (HAT-CN) using ultraviolet photoelectron spectroscopy. The highest occupied molecular orbital (HOMO) of 20 nm thick HAT-CN film was located at 3.8 eV below the Fermi level. Thus the lowest unoccupied molecular orbital (LUMO) is very close to the Fermi level. The HOMO position of NPB was only about 0.3 eV below Fermi level at NPB/HAT-CN interface. This enables an easy excitation of electrons from the NPB HOMO to the HAT-CN LUMO, creating electron-hole pairs across this organic-organic interface.

Microscopic origin of bipolar resistive switching of nanoscale titanium oxide thin films

We report a direct observation of the microscopic origin of the bipolar resistive switching behavior in nanoscale titanium oxide films. Through a high-resolution transmission electron microscopy, an analytical transmission electron microscopy technique using energy-filtering transmission electron microscopy, and an in situ x-ray photoelectron spectroscopy, we demonstrated that the oxygen ions piled up at the top interface by an oxidation-reduction between the titanium oxide layer and the top Al metal electrode. We also found that the drift of oxygen ions during the on/off switching induced the bipolar resistive switching in the titanium oxide thin films.

Insertion of an organic interlayer for hole current enhancement in inverted organic light emitting devices

We report the enhancement of hole current density in the hole transport part of an inverted top-emission organic light emitted diode by applying an organic insertion layer of 1,4,5,8,9,11-hexaazatriphenylene-hexacarbonitrile (HAT-CN). Poor hole transporting performance of Al/4,4′-bis(N-phenyl-1-naphthylamino)biphenyl (NPB)/indium tin oxide is greatly improved by the HAT-CN insertion between Al and NPB layer. The highest occupied molecular orbital level onset of the NPB bends toward Fermi level at the HAT-CN/NPB interface. This extra charge generation layer made of pure organic molecules substantially enhances hole injection from Al anode as revealed by the results of ultraviolet photoelectron spectroscopy and J-V measurement data.

Effective work function lowering of multilayer graphene films by subnanometer thick AlOx overlayers

A simple method for controlling the effective work function (WF) of conductive multilayer graphene (MLG) film, synthesized by using chemical vapor deposition and transferred to a dielectric substrate, was developed. The WFs of the MLG during the step-by-step deposition of aluminum (Al) were measured using in situ ultraviolet photoelectron spectroscopy. Core-level spectra were also collected to investigate the chemical reaction that occurred when a small amount of Al was deposited onto MLG in a stepwise manner. The measurements revealed that the effective WF of the conductive MLG film could be controlled from 3.77 to 4.40 eV by the deposition of an Al layer less than 0.6 nm thick.

Ultrathin and Flat Layer Black Phosphorus Fabricated by Reactive Oxygen and Water Rinse

Ultrathin black phosphorus (BP) is one of the promising two-dimensional (2D) materials for future optoelectronic devices. Its chemical instability in ambient conditions and lack of a bottom-up approach for its synthesis necessitate efficient etching methods that generate BP films of designed thickness with stable and high-quality surfaces. Herein, reporting a photochemical etching method, we demonstrate a controlled layer-by-layer thinning of thick BP films down to a few layers or a single layer and confirm their Raman and photoluminescence characteristics. Ozone molecules generated by O2 photolysis oxidize BP, forming P2O5-like oxides. When the resulting phosphorus oxides are removed by water, the surface of BP with preset thickness is highly flat and self-protective by surface oxygen functional groups. This method provides a fabrication strategy of BP and possibly other 2D semiconductors with band gaps tuned by their thickness.

Direct evidence of n-type doping in organic light-emitting devices: N free Cs doping from CsN3

Cesium azide (CsN3) is confirmed to be decomposed during thermal evaporation. Only Cs could be deposited on tris(8-hydroxyquinolinato)aluminum (Alq3) and n-type doping is easily achieved. Organic light-emitting devices with CsN3 show highly improved current density-luminance-voltage characteristics compared to the control device without CsN3. To understand the origin of the improvements, in situ x-ray and UV photoemission spectroscopy measurements were carried out and a remarkable reduction in electron injection barrier is verified with successive deposition of Al on CsN3 on Alq3. CsN3 has a potential as alternative to doping the electron transport layer by replacing the direct deposition of alkali metals.

Low-temperature growth of layered molybdenum disulphide with controlled clusters

Layered molybdenum disulphide was grown at a low-temperature of 350 °C using chemical vapour deposition by elaborately controlling the cluster size. The molybdenum disulphide grown under various sulphur-reaction-gas to molybdenum-precursor partial-pressure ratios were examined. Using spectroscopy and microscopy, the effect of the cluster size on the layered growth was investigated in terms of the morphology, grain size, and impurity incorporation. Triangular single-crystal domains were grown at an optimized sulphur-reaction-gas to molybdenum-precursor partial-pressure ratio. Furthermore, it is proved that the nucleation sites on the silicon-dioxide substrate were related with the grain size. A polycrystalline monolayer with the 100-nm grain size was grown on a nucleation site confined substrate by high-vacuum annealing. In addition, a field-effect transistor was fabricated with a MoS2 monolayer and exhibited a mobility and on/off ratio of 0.15 cm2 V−1 s−1 and 105, respectively.

Photovoltaic Performance and Interface Behaviors of Cu(In,Ga)Se2 Solar Cells with a Sputtered-Zn(O,S) Buffer Layer by High-Temperature Annealing

We selected a sputtered-Zn(O,S) film as a buffer material and fabricated a Cu(In,Ga)Se2 (CIGS) solar cell for use in monolithic tandem solar cells. A thermally stable buffer layer was required because it should withstand heat treatment during processing of top cell. Postannealing treatment was performed on a CIGS solar cell in vacuum at temperatures from 300-500 °C to examine its thermal stability. Serious device degradation particularly in VOC was observed, which was due to the diffusion of thermally activated constituent elements. The elements In and Ga tend to out-diffuse to the top surface of the CIGS, while Zn diffuses into the interface of Zn(O,S)/CIGS. Such rearrangement of atomic fractions modifies the local energy band gap and band alignment at the interface. The notch-shape induced at the interface after postannealing could function as an electrical trap during electron transport, which would result in the reduction of solar cell efficiency.

Effects of UV/ozone treatment of a polymer dielectric surface on the properties of pentacene thin films for organic transistors

Ultraviolet photoelectron spectroscopy and atomic force microscopy (AFM) were used to investigate the energy level alignment and growth morphology of pentacene (Pn) films deposited on a PMMA derivative-based dielectric surface with and without ultraviolet/ozone treatment. The treated surface exhibited higher offset values for the highest occupied molecular orbital levels between Pn and the polymer, which would result in higher threshold voltages for the device. However, aligned vacuum levels of the treated surface and the Pn at the interface were observed, suggesting that the dipole field would be reduced in the Pn film on the treated surface. The hydrophilic nature of the treated surface, observed by water contact angle measurement, allowed for a larger grain size of the Pn film, as confirmed by the AFM measurements, which will also favorably contribute to device mobility.