Hyoyoung Lee

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Organization: Institute for Basic Science (IBS)
Department: Centre for Integrated Nanostructure Physics (CINAP)
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Co-reporter:Dr. Sohyeon Seo;Dr. Eunhee Hwang;Yunhee Cho;Dr. Junghyun Lee; Dr. Hyoyoung Lee
Angewandte Chemie International Edition 2017 Volume 56(Issue 40) pp:12122-12126
Publication Date(Web):2017/09/25
DOI:10.1002/anie.201705518
AbstractInformation processing using molecular junctions is becoming more important as devices are miniaturized to the nanoscale. Herein, we report functional molecular junctions derived from double self-assembled monolayers (SAMs) intercalated between soft graphene electrodes. Newly assembled molecular junctions are fabricated by placing a molecular SAM/(top) electrode on another molecular SAM/(bottom) electrode by using a contact-assembly technique. Double SAMs can provide tunneling conjugation across the van der Waals gap between the terminals of each monolayer and exhibit new electrical functions. Robust contact-assembled molecular junctions can act as platforms for the development of equivalent contact molecular junctions between top and bottom electrodes, which can be applied independently to different kinds of molecules to enhance either the structural complexity or the assembly properties of molecules.
Co-reporter:Dr. Sohyeon Seo;Dr. Eunhee Hwang;Yunhee Cho;Dr. Junghyun Lee; Dr. Hyoyoung Lee
Angewandte Chemie 2017 Volume 129(Issue 40) pp:12290-12294
Publication Date(Web):2017/09/25
DOI:10.1002/ange.201705518
AbstractInformation processing using molecular junctions is becoming more important as devices are miniaturized to the nanoscale. Herein, we report functional molecular junctions derived from double self-assembled monolayers (SAMs) intercalated between soft graphene electrodes. Newly assembled molecular junctions are fabricated by placing a molecular SAM/(top) electrode on another molecular SAM/(bottom) electrode by using a contact-assembly technique. Double SAMs can provide tunneling conjugation across the van der Waals gap between the terminals of each monolayer and exhibit new electrical functions. Robust contact-assembled molecular junctions can act as platforms for the development of equivalent contact molecular junctions between top and bottom electrodes, which can be applied independently to different kinds of molecules to enhance either the structural complexity or the assembly properties of molecules.
Co-reporter:An P. Tiwari;Doyoung Kim;Yongshin Kim
Advanced Energy Materials 2017 Volume 7(Issue 14) pp:
Publication Date(Web):2017/07/01
DOI:10.1002/aenm.201602217
Improving the electrochemical performance of both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) has been of great interest in emerging renewable energy technologies. This study reports an advanced bifunctional hybrid electrocatalyst for both ORR and OER, which is composed of tungsten disulphide (WS2) and carbon nanotube (CNT) connected via tungsten carbide (WC) bonding. WS2 sheets on the surface of CNTs provide catalytic active sites for electrocatalytic activity while the CNTs act as conduction channels and provide a large surface area. Moreover, the newly formed WC crystalline structure provides an easy path for electron transfer by spin coupling and helps to solve stability issues to enable excellent electrocatalytic activity. In addition, it is found that four to five layers of WS2 sheets on the surface of CNTs produce excellent catalytic activity toward both ORR and OER, which is comparable to noble metals (Pt, RuO2, etc.). These findings show the many advantages enabled by designing highly active, durable, and cost-effective ORR and OER electrocatalysts.
Co-reporter:Meeree Kim, Hee Min Hwang, G. Hwan Park, Hyoyoung Lee
FlatChem 2017 Volume 6(Volume 6) pp:
Publication Date(Web):1 December 2017
DOI:10.1016/j.flatc.2017.08.002
•Issues and challenges of graphene-based electrodes in EESDs are demonstrated.•Various nano-structured graphene-based electrodes in EESDs are summarized.•Chemical methods for each device to overcome the current limitations are discussed.As the importance of applications depending on electrical energy storage devices (EESDs), including portable electronics, electric vehicles, and devices for renewable energy storage, has gradually increased, research has focused more and more on innovative energy systems for advanced EESDs in order to achieve enhanced performance. Over the past two decades, graphene-based materials have been considered as ideal electrode materials for lithium-ion, sodium-ion, and lithium/sulfur batteries, as well as supercapacitors, due to their promising applications for advanced electrodes. In this review, we will demonstrate the issues and challenges of each type of EESD, with an emphasis placed on the use of graphene-based electrodes. Recent trends related to research into graphene-based composite materials as electrodes in Korea will also be shown and a summary of the overall strategies and future perspectives will be given.Download high-res image (326KB)Download full-size image
Co-reporter:Sohyeon Seo;Keunsik Lee;Misook Min;Yunhee Cho;Meeree Kim
Nanoscale (2009-Present) 2017 vol. 9(Issue 11) pp:3969-3979
Publication Date(Web):2017/03/17
DOI:10.1039/C6NR09428G
A major challenge in the development of electrocatalysts is to determine a detailed catalysis mechanism on a molecular level for enhancing catalytic activity. Here, we present bottom-up studies for an electrocatalytic hydrogen evolution reaction (HER) process through molecular activation to systematically control surface catalytic activity corresponding to an interfacial charge transfer in a porphyrin monolayer on inactive graphene. The two-dimensional (2D) assembly of porphyrins that create homogeneous active sites (e.g., electronegative tetrapyrroles (N4)) on graphene showed structural stability against electrocatalytic reactions and enhanced charge transfer at the graphene-liquid interface. Performance operations of the graphene field effect transistor (FET) were an effective method to analyse the interfacial charge transfer process associated with information about the chemical nature of the catalytic components. Electronegative pristine porphyrin or Pt-porphyrin networks, where intermolecular hydrogen bonding functioned, showed larger interfacial charge transfers and higher HER performance than Ni-, or Zn-porphyrin. A process to create surface electronegativity by either central N4 or metal (M)–N4 played an important role in the electrocatalytic reaction. These findings will contribute to an in-depth understanding at the molecular level for the synergetic effects of molecular structures on the active sites of electrocatalysts toward HER.
Co-reporter:Kan Zhang, Luyang Wang, Jung Kyu Kim, Ming Ma, Ganapathy Veerappan, Chang-Lyoul Lee, Ki-jeong Kong, Hyoyoung Lee and Jong Hyeok Park  
Energy & Environmental Science 2016 vol. 9(Issue 2) pp:499-503
Publication Date(Web):18 Nov 2015
DOI:10.1039/C5EE03100A
Surface engineering of TiO2 is faced with the challenge of high solar-to-hydrogen conversion efficiency. Recently, surface-disordered TiO2, referred to as black TiO2, which can absorb both visible and near-infrared solar light, has triggered an explosion of interest in many important applications. Unfortunately, the mechanism underlying the improved photocatalytic effect from an amorphous surface layer remains unclear and seems to contradict conventional wisdom. Here, we demonstrate selectively “disorder engineered” Degussa P-25 TiO2 nanoparticles using simple room-temperature solution processing, which maintain the unique three-phase interfaces composed of ordered white-anatase and disordered black-rutile with open structures for easy electrolyte access. The strong reducing agent in a superbase, which consists of lithium in ethylenediamine (Li-EDA), can disorder only the white-rutile phase of P-25, leaving behind blue coloured TiO2 nanoparticles. The order/disorder/water junction created by the blue P-25 can not only efficiently internally separate electrons/holes through type-II bandgap alignment but can also induce a strong hydrogen (H2) evolution surface reaction in the sacrificial agent containing electrolyte. As a result, the blue P-25 exhibited outstanding H2 production rates of 13.89 mmol h−1 g−1 using 0.5 wt% Pt (co-catalyst) and 3.46 mmol h−1 g−1 without using any co-catalyst.
Co-reporter:Hanleem Lee;Meeree Kim;Ikjoon Kim
Advanced Materials 2016 Volume 28( Issue 22) pp:4541-4548
Publication Date(Web):
DOI:10.1002/adma.201505559

Many studies have accompanied the emergence of a great interest in flexible or/and stretchable devices for new applications in wearable and futuristic technology, including human-interface devices, robotic skin, and biometric devices, and in optoelectronic devices. Especially, new nanodimensional materials enable flexibility or stretchability to be brought based on their dimensionality. Here, the emerging field of flexible devices is briefly introduced using silver nanowires and graphene, which are famous nanomaterials for the use of transparent conductive electrodes, as examples, and their unique functions originating from the intrinsic property of these nanomaterials are highlighted. It is thought that this work will evoke more interest and idea exchanges in this emerging field and hopefully can trigger a breakthrough on a new type of optoelectronics and optogenetic devices in the near future.

Co-reporter:Hanleem Lee, Ikjoon Kim, Meeree Kim and Hyoyoung Lee  
Nanoscale 2016 vol. 8(Issue 4) pp:1789-1822
Publication Date(Web):08 Dec 2015
DOI:10.1039/C5NR06851G
Stretchable and/or flexible electrodes and their associated electronic devices have attracted great interest because of their possible applications in high-end technologies such as lightweight, large area, wearable, and biointegrated devices. In particular, metal nanowires and graphene derivatives are chosen for electrodes because they show low resistance and high mechanical stability. Here, we review stretchable and flexible soft electrodes by discussing in depth the intrinsic properties of metal NWs and graphenes that are driven by their dimensionality. We investigate these properties with respect to electronics, optics, and mechanics from a chemistry perspective and discuss currently unsolved issues, such as how to maintain high conductivity and simultaneous high mechanical stability. Possible applications of stretchable and/or flexible electrodes using these nanodimensional materials are summarized at the end of this review.
Co-reporter:Keunsik Lee, Hanleem Lee, Yonghun Shin, Yeoheung Yoon, Doyoung Kim, Hyoyoung Lee
Nano Energy 2016 Volume 26() pp:746-754
Publication Date(Web):August 2016
DOI:10.1016/j.nanoen.2016.06.030
•Transparent and flexible micro-supercapacitors based on graphene and GQDs have been successfully developed using a simple electrophoretic deposition method.•GQDs play an essential role to contribute the rough surfaces and high conductivity allowing fast diffusion of electrolyte ions and capacitive effects.•ipG-GQDs-MSC exhibit outstanding performances as high capacitance, transparency and stable retention at severe bending.Nowadays, transparent and flexible energy storage devices are attracting a great deal of research interest due to their great potential as integrated power sources. In order to take full advantage of transparent and flexible devices, however, their power sources also need to be transparent and flexible. In the present work we fabricated new transparent and flexible micro-supercapacitors using chelated graphene and graphene quantum dots (GQDs) by a simple electrophoretic deposition (EPD) method. Through a chelate formation between graphene and GQDs with metal ions, the GQD materials were strongly adhered on an interdigitated pattern of graphene (ipG-GQDs) and its resulting porous ipG-GQDs film was used as the active material in the micro-supercapacitors. Amazingly, these supercapacitor devices showed high transparency (92.97% at 550 nm), high energy storage (9.09 μF cm−2), short relaxation time (8.55 ms), stable cycle retention (around 100% for 10,000 cycles), and high stability even under severe bending angle 45° with 10,000 cycles.Graphene quantum dots on interdigitated graphene for microsupercapacitor (ipG-GQDs-MSC) show high transparency and stable flexibility performance as well as superior capacitive effect, which will be applicable for flexible, bendable, foldable, and even stretchable devices.
Co-reporter:Keunsik Lee, Yeoheung Yoon, Yunhee Cho, Sae Mi Lee, Yonghun Shin, Hanleem Lee, and Hyoyoung Lee
ACS Nano 2016 Volume 10(Issue 7) pp:6799
Publication Date(Web):June 16, 2016
DOI:10.1021/acsnano.6b02415
Although there are numerous reports of high performance supercapacitors with porous graphene, there are few reports to control the interlayer gap between graphene sheets with conductive molecular linkers (or molecular pillars) through a π-conjugated chemical carbon–carbon bond that can maintain high conductivity, which can explain the enhanced capacitive effect of supercapacitor mechanism about accessibility of electrolyte ions. For this, we designed molecularly gap-controlled reduced graphene oxides (rGOs) via diazotization of three different phenyl, biphenyl, and para-terphenyl bis-diazonium salts (BD1–3). The graphene interlayer sub-nanopores of rGO–BD1–3 are 0.49, 0.7, and 0.96 nm, respectively. Surprisingly, the rGO–BD2 0.7 nm gap shows the highest capacitance in 1 M TEABF4 having 0.68 nm size of cation and 6 M KOH having 0.6 nm size of hydrated cation. The maximum energy density and power density of the rGO–BD2 were 129.67 W h kg–1 and 30.3 kW kg–1, respectively, demonstrating clearly that the optimized sub-nanopore of the rGO–BDs corresponding to the electrolyte ion size resulted in the best capacitive performance.Keywords: bis-diazonium salt; diazotization; graphene; sub-nanopore; supercapacitor
Co-reporter:Anand P. Tiwari, Doyoung Kim, Yongshin Kim, Om Prakash, Hyoyoung Lee
Nano Energy 2016 Volume 28() pp:366-372
Publication Date(Web):October 2016
DOI:10.1016/j.nanoen.2016.08.065
•Single layered ternary transition metal chalcogenides have been synthesized for highly active and stable electrocatalyst.•Se-doping plays an essential role to exfoliate Cu2Mo(S1-ySey)4 for high electrochemical active surface.•Se-doping strategy can be implemented to exfoliate and enhance electrocatalytic activity of transition metals chalcogens.Layered ternary transition metal chalcogenides (TTMCs) material has great potentials that can overcome to the limitation of active sites which is challenging in binary transition metal chalcogenides (BTMC), such as MoS2, towards electrochemical hydrogen production. Here, we demonstrate TTMC material which contains two transition metals Cu and Mo with chalcogen S. The TTMC, Cu2MoS4 has been successfully synthesized by a facile solution-processed method. Moreover, by anion doping such as Se in as the synthesized Cu2MoS4, it has been found that TTMC can be exfoliated into single layer nanosheets. Furthermore, by controlling the number of layers, single layers TTMC exhibit the highest electrocatalytic activity towards hydrogen evolution reaction (HER) because the single layers can provide more catalytic active sites than multilayers and bulk. The onset potential for hydrogen generation is −96 mV for single layer TTMC electrode material with corresponding Tafel slope 52 mV/decade. After 1000 cycles with continuous electrolysis in acid electrolyte for 15 h, the electrode material preserves its structure and robust catalytic activity perfectly. Our new TTMC materials show highly active electrocatalytic performance and high stability which overcome the intrinsic limitation of BTMC. As a result, our work can guide new strategy for the developments of real applications of TMCs in HER.Effective approaches to synthesis of single layered ternary transition metal chalcogenide (TTMC) have been developed to produce highly active and stable electrocatalyst towards hydrogen evolution reaction. The single layered TTMC are achieved by Se-doping in Cu2MoS4 which can be applicable for other transition metal chalcogenide (TMC).
Co-reporter:Hanleem Lee;Guebum Han;Meeree Kim;Hyo-sok Ahn
Advanced Materials 2015 Volume 27( Issue 13) pp:2252-2259
Publication Date(Web):
DOI:10.1002/adma.201405326
Co-reporter:Anand P. Tiwari, HeeJoun Yoo, JeongTaik Lee, Doyoung Kim, Jong Hyeok Park and Hyoyoung Lee  
Nanoscale 2015 vol. 7(Issue 28) pp:11928-11933
Publication Date(Web):15 Jun 2015
DOI:10.1039/C5NR03111G
We report new three-dimensional (3D)-nanostructured MoS2-carbonaceous materials in which MoS2 sheets are intercalated between the graphite layers that possess a multiply repeated graphite/MoS2/graphite structure which prevents the aggregation of MoS2 and diffusion of sulfur from carbonaceous materials, enhancing the cycling stability of Li-ion batteries. We developed an efficient and scalable process applicable to mass production for synthesizing non-aggregated MoS2-intercalated 3D hybrid-nanostructured graphite based on stress induced and microwave irradiation. X-ray diffraction, X-ray photospectroscopy, Raman spectroscopy, field emission scanning electron microscopy, and high-resolution transmission electron microscopy analyses demonstrated that the as-synthesized materials consisted of MoS2-intercalated 3D hybrid-nanostructured graphite platelets that had a multiply repeated graphite/MoS2/graphite structure. The obtained MoS2–graphite powder surpasses MoS2 as an anode material in terms of specific capacity, cyclic stability, and rate performances at high current densities for Li-ion batteries. The electrochemical impedance spectroscopy demonstrated that the graphite sheets not only reduced the contact resistance in the electrode but also facilitated electron transfer in the lithiation/delithiation processes. The superior electrochemical performances especially for the cycling stability of the Li-ion battery originate from prevention of the sulfur diffusion of the MoS2-intercalated 3D-nanostructured graphite.
Co-reporter:Yonghun Shin, Jintaek Park, Daesun Hyun, Junghee Yang, Jae-Hyeok Lee, Jae-Ho Kim and Hyoyoung Lee  
Nanoscale 2015 vol. 7(Issue 13) pp:5633-5637
Publication Date(Web):03 Mar 2015
DOI:10.1039/C5NR00814J
To prepare carbon-based fluorescent materials such as graphene quantum dots (GQDs), new and effective methods are needed to convert one-dimensional (1D) or two-dimensional (2D) carbon materials to 0D GQDs. Here, we report a novel acid-free and oxone oxidant-assisted solvothermal synthesis of GQDs using various natural carbon resources including graphite (G), multiwall carbon nanotubes (M), carbon fibers (CF), and charcoal (C). This acid-free method, not requiring the neutralization process of strong acids, exhibits a simple and eco-friendly purification process and also represents a recycling production process, together with mass production and high yield. Newly synthesized GQDs exhibited a strong blue photoluminescence (PL) under 365 nm UV light illumination. The PL emission peaks of all the recycled GQDs did not change.
Co-reporter:HeeJoun Yoo, Anand P. Tiwari, JeongTaik Lee, Doyoung Kim, Jong Hyeok Park and Hyoyoung Lee  
Nanoscale 2015 vol. 7(Issue 8) pp:3404-3409
Publication Date(Web):12 Jan 2015
DOI:10.1039/C4NR06348A
Direct attachment of MoS2 to materials with carbonaceous architecture remains a major challenge because of non-intimate contact between the carbonaceous materials and active MoS2 material. In this study, we report a new unique synthetic method to produce a new type of hybrid nanostructure of MoS2-CNTs composites. We developed a novel strategy for the synthesis of cylindrical MoS2 directly grown on CNT composites without the use of any other additives, exhibiting superior electrochemical performance as the anode material of lithium-ion batteries via a microwave irradiation technique. We adopted a simple step-by-step method: coating sulfur on CNTs and then reaction with a Mo source to synthesize hybrid cylindrical nanostructures of the MoS2-CNT composite. X-ray diffraction, field emission scanning electron microscopy, and high-resolution transmission electron microscopy analyses demonstrated that the as-synthesized MoS2-CNTs possessed a hybrid nanostructure, in which MoS2 sheets were well attached to the CNTs. The directly attached MoS2 sheets on the CNTs showed superior electrochemical performance as anode materials in a lithium-ion battery.
Co-reporter:Hongyue Jing, Misook Min, Sohyeon Seo, Benzheng Lu, Yeoheung Yoon, Sae Mi Lee, Eunhee Hwang, Hyoyoung Lee
Carbon 2015 Volume 86() pp:272-278
Publication Date(Web):May 2015
DOI:10.1016/j.carbon.2015.01.044
Direct synthesis of graphene without metal catalysts on a dielectric substrate is a major goal in graphene-based electronics and is an increasingly popular nanotechnology alternative to metal oxide semiconductor technology. However, current methods for the synthesis of these graphenes have many limitations, including the use of metal catalyst. Herein, we report a facile approach to the direct synthesis of graphene sheets based on the self-assembled monolayers (SAMs) technique. The new method for metal catalyst-free direct synthesis of a graphene sheet is through a solution-processable, inexpensive, easy, and reproducible cross-linked polythiophene self-assembled monolayer (SAM) that is formed via the [4 + 2] π cycloaddition reaction of π-electron conjugated thiophene layer self-assembled on the dielectric silicon dioxide substrate. The bifunctional molecules were carefully designed to create an SAM via silanization of alkoxy silane groups on the SiO2 substrate, and at the other end, a thin cross-linked polythiophene layer via a [4 + 2] π-electron cycloaddition reaction of π-electron conjugated thiophene SAM. By heating the cross-linked polythiophene SAM up to 1000 °C under a high vacuum, single-layered or few-layered graphene sheets were successfully prepared on the dielectric silicon oxide substrate.
Co-reporter:Keunsik Lee, Doyoung Kim, Yeoheung Yoon, Junghee Yang, Ho-Gyeong Yun, In-Kyu You and Hyoyoung Lee  
RSC Advances 2015 vol. 5(Issue 75) pp:60914-60919
Publication Date(Web):06 Jul 2015
DOI:10.1039/C5RA10246D
In order to obtain a high performance supercapacitor, there are several factors that must be achieved including a high specific surface area (SSA), high electrical conductivity, and a high diffusion rate of the electrolyte due to an appropriate pore volume. Herein, we report a high performance supercapacitor using activated non-stacked reduced graphene oxide (a-NSrGO) that has a high SSA (up to 999.75 m2 g−1) with intrinsic high graphene conductivity (1202 S m−1) and fast diffusion of the electrolyte. Due to a high total pore volume (5.03 cm3 g−1) and a wide pore size distribution from macro- to micropores (main pore width: 0.61 – 0.71 nm) in the a-NSrGO sheets, the as-prepared a-NSrGO electrode shows high specific capacitance (105.26 F g−1) and a short relaxation time (τ0 = 1.5 s) in a propylene carbonate (PC)-based organic electrolyte. A maximum energy density of 91.13 W h kg−1 and a power density of 66684.73 W kg−1 were estimated in a fully packaged coin cell. The high performance of the a-NSrGO supercapacitors is attributed to their specific appearance and enlarged pore distribution with high SSA.
Co-reporter:Yonghun Shin, Jintaek Park, Daesun Hyun, Junghee Yang and Hyoyoung Lee  
New Journal of Chemistry 2015 vol. 39(Issue 4) pp:2425-2428
Publication Date(Web):05 Feb 2015
DOI:10.1039/C4NJ02299H
A novel and facile method to synthesize graphene quantum dots (GQDs) from graphene oxide (GO) via sonication or UV-irradiation reaction using an acid-free oxone oxidant (potassium monopersulfate) that does not require a neutralization process with a strong base was developed. Our novel sono- and photo-oxidation approach yielded high quality GQDs after simple purification. GO sheets treated by sono- and photo-oxidation with the oxone oxidant as the free radical source broke in multiple places for efficient generation of GQDs. Sono-oxidation is a simpler and more facile method than photo-oxidation in terms of mass production and the strong fluorescence properties of the resulting GQDs. Facile synthesis by sono- and photo-oxidation represents a new route to prepare GQDs from GO in organic solvent.
Co-reporter:Shahbaz Khan, Shahzada Qamar Hussain, Doyeon Hwang, S. Velumani, Hyoyoung Lee
Materials Science in Semiconductor Processing 2015 Volume 37() pp:51-56
Publication Date(Web):September 2015
DOI:10.1016/j.mssp.2015.01.019
Surface morphology of the front transparent conductive oxide film is critical to achieve high short circuit current density in amorphous silicon (a-Si) thin film solar cells due to its high electrical conductivity and transparency accompanying excellent light scattering. Here, we present a low cost hydrothermal route to deposit zinc oxide nanoflowers and nanoflakes exhibiting low sheet resistance and high haze ratio for a-Si thin film solar cells. Zinc oxide nanoflowers and nanoflakes with various aspect ratios were grown on standard fluorine doped tin oxide glass by modulating growth time and hydrogen doping. Zinc oxide nanoflowers and nanoflakes exhibited superior light scattering compared to conventional zinc oxide nanostructures due to a higher surface area and displayed a higher haze ratio compared to the commercially available fluorine doped tin oxide films. Moreover, electrical conductivity and crystallinity of zinc oxide nanoflowers and nanoflakes could be enhanced by annealing in hydrogen atmosphere at 350 °C. We also observed that zinc oxide nanoflowers with high aspect ratio showed high transmittance spectra for a wider wavelength range. Therefore, we propose a low cost scale up synthesis of high haze ratio zinc oxide nanoflowers and nanoflakes for the enhanced performance of thin film solar cells.
Co-reporter:Sae Mi Lee;Ji Hun Lee;Sora Bak;Keunsik Lee;Yang Li
Nano Research 2015 Volume 8( Issue 6) pp:1882-1892
Publication Date(Web):2015 June
DOI:10.1007/s12274-014-0696-4
We introduce a transparent windshield-glass heater produced via transparent electrodes using silver nanowire (AgNW) networks for conventional use in the automobile industry. A high-quality conducting hybrid film is deposited on a plasma-treated glass substrate by spraying AgNWs, immersing the sprayed product in positively charged adhesive polymer solution, and then spraying negatively charged graphene oxide (GO) and a silane layer as an over-coating layer (OCL).The results of heating tests conducted after adhesion tests show that the sheet resistance changes with the application of polymer glue. Surprisingly, the transmittance of the film with the GO OCL is higher than that of the film without the GO OCL. Heating and defrosting tests are carefully conducted via infrared (IR) monitoring. Adhesive-polymer-treated and GO-protected AgNW transparent glass heaters exhibit the best performance with low sheet resistance; thus, through strong electrostatic interaction among the substrate, adhesive layer, and OCL, our AgNW hybrid glass heater can reach the target temperature with a standard vehicle voltage of 12 V in a short period of time.
Co-reporter:Eunhee Hwang;Sohyeon Seo;Sora Bak;Hanleem Lee;Misook Min
Advanced Materials 2014 Volume 26( Issue 30) pp:5129-5136
Publication Date(Web):
DOI:10.1002/adma.201401201
Co-reporter:Hanleem Lee;Keunsik Lee;Jin Taek Park;Woon Chun Kim
Advanced Functional Materials 2014 Volume 24( Issue 21) pp:3276-3283
Publication Date(Web):
DOI:10.1002/adfm.201303276

Recently, Ag nanowires (AgNWs) has had a great interest as a conducting material for flexible and transparent devices, but it still shows several problems such as the ultimate detachment of AgNWs from substrate and a high contact resistance on AgNW junctions. Therefore, the novel concept to enhance permanent and closed attachment of AgNWs by silane modification to polydimethylsilaoxane (PDMS) substrate well known as high stretchable film with extremly low adhesive is suggested. According to this experiment, higher sigma (σ)-donating ability and hydrophilicity indicate better electrical and mechanical properties in real device. Especially, densely amine self-assembled PDMS surface exhibits the strongest contact force to the AgNWs, especially for junction side, and the longest maintenance of hydrophilicity by coordination-type bonding. In addition, AgNWs adhere permanently to stretchable substrates while simultaneously maintaining high transparency (87%) and high conductivity (27 Ω sq–1). Consequently, the resulting AgNW film shows excellent mechanical durability which includes enhanced performance of both flexibility and stretchability.

Co-reporter:Surajit Some, Sungjin Kim, Khokan Samanta, Youngmin Kim, Yeoheung Yoon, Younghun Park, Sae Mi Lee, Keunsik Lee and Hyoyoung Lee  
Nanoscale 2014 vol. 6(Issue 19) pp:11322-11327
Publication Date(Web):25 Jul 2014
DOI:10.1039/C4NR03009E
An approach of presenting new reducing reagents, sodium–benzophenone (Na–B) or Na–B in the presence of the hydrazine (Na–B–H) system under light exposure could produce rGOs with/without N-doping at room temperature in both the solution phase and on a solid substrate. Benzophenone activated those solutions acting as a photosensitizer under light. It was assumed that the newly generated radical anions with electrons from Na–B under light can reduce GO to rGO sheets (rGONa–B1). In addition, the Na–B–H system can allow a higher degree of reduction with the doping of nitrogen atoms by the introduction of hydrazine to produce radical anions and electrons with a sodium hydrazide complex, which helps decrease the sheet resistance of the as-made rGONa–B–H2. The excellent properties (very low oxygen content (C/O ∼16.2), and low sheet resistance (∼130 Ω square−1)) of the rGOs were confirmed by XPS, XRD, IR, Raman spectroscopy, TGA, wettability, and sheet resistance measurements. High-quality rGO films on flexible substrates could be prepared by directly immersing the GO films in these solutions for several minutes.
Co-reporter:Heejoun Yoo, Misook Min, Sora Bak, Yeoheung Yoon and Hyoyoung Lee  
Journal of Materials Chemistry A 2014 vol. 2(Issue 18) pp:6663-6668
Publication Date(Web):18 Feb 2014
DOI:10.1039/C4TA00158C
A hydrophilic surface modified carbon electrode shows a good electrolyte affinity with homogeneous dispersibility in water, resulting in low ion-transfer resistance and a uniform and dense electrode to give a high volumetric capacitor. The hydrophilic carbon electrode exhibits a superior capacitance (58 F cm−3, 99.3 mF cm−2) and is stable up to 5000 cycles.
Co-reporter:Luyang Wang, Younghun Park, Peng Cui, Sora Bak, Hanleem Lee, Sae Mi Lee and Hyoyoung Lee  
Chemical Communications 2014 vol. 50(Issue 10) pp:1224-1226
Publication Date(Web):30 Oct 2013
DOI:10.1039/C3CC47224H
We introduce a facile method to prepare an n-type reduced graphene oxide field effect transistor at room temperature via a typical Benkeser reduction using lithium and ethylenediamine.
Co-reporter:Yeoheung Yoon, Keunsik Lee, Soongeun Kwon, Sohyeon Seo, Heejoun Yoo, Sungjin Kim, Yonghun Shin, Younghun Park, Doyoung Kim, Jae-Young Choi, and Hyoyoung Lee
ACS Nano 2014 Volume 8(Issue 5) pp:4580
Publication Date(Web):March 30, 2014
DOI:10.1021/nn500150j
Supercapacitors with porous carbon structures have high energy storage capacity. However, the porous nature of the carbon electrode, composed mainly of carbon nanotubes (CNTs) and graphene oxide (GO) derivatives, negatively impacts the volumetric electrochemical characteristics of the supercapacitors because of poor packing density (<0.5 g cm–3). Herein, we report a simple method to fabricate highly dense and vertically aligned reduced graphene oxide (VArGO) electrodes involving simple hand-rolling and cutting processes. Because of their vertically aligned and opened-edge graphene structure, VArGO electrodes displayed high packing density and highly efficient volumetric and areal electrochemical characteristics, very fast electrolyte ion diffusion with rectangular CV curves even at a high scan rate (20 V/s), and the highest volumetric capacitance among known rGO electrodes. Surprisingly, even when the film thickness of the VArGO electrode was increased, its volumetric and areal capacitances were maintained.Keywords: electrochemistry; reduced graphene oxide; supercapacitor; vertically aligned
Co-reporter:Yeoheung Yoon;Keunsik Lee;Chul Baik;Heejoun Yoo;Misook Min;Younghun Park;Sae Mi Lee
Advanced Materials 2013 Volume 25( Issue 32) pp:4437-4444
Publication Date(Web):
DOI:10.1002/adma.201301230
Co-reporter:Misook Min;Sohyeon Seo;Sae Mi Lee
Advanced Materials 2013 Volume 25( Issue 48) pp:7045-7050
Publication Date(Web):
DOI:10.1002/adma.201303335
Co-reporter:Khokan Samanta, Surajit Some, Youngmin Kim, Yeoheung Yoon, Misook Min, Sae Mi Lee, Younghun Park and Hyoyoung Lee  
Chemical Communications 2013 vol. 49(Issue 79) pp:8991-8993
Publication Date(Web):05 Aug 2013
DOI:10.1039/C3CC45376F
A facile method for the synthesis of highly fluorinated reduced graphene oxide from graphene oxide using BF3-OEt2 solution and alkylthiol/alkylamine on the Gram scale has been described using a detailed mechanism. The maximum fluorination was as high as 38 wt% and the fluorinated reduced graphene oxide produced has great wettability and high insulating properties.
Co-reporter:Misook Min, Sohyeon Seo, Junghyun Lee, Sae Mi Lee, Eunhee Hwang and Hyoyoung Lee  
Chemical Communications 2013 vol. 49(Issue 56) pp:6289-6291
Publication Date(Web):22 May 2013
DOI:10.1039/C3CC42591F
Changes in major charge transport of graphene channel transistors in terms of the spatial orientation of adsorbed functional molecules were demonstrated. In contrast to the horizontally (physically) bound molecules, the vertically (chemically) bound molecules did not change major charge carriers of graphene channels, revealing the molecular orientation-dependent doping effects.
Co-reporter:Youngmin Kim, Surajit Some and Hyoyoung Lee  
Chemical Communications 2013 vol. 49(Issue 50) pp:5702-5704
Publication Date(Web):09 May 2013
DOI:10.1039/C3CC42787K
We demonstrated a simple and green chemical method to obtain Michael adducts and their derivatives by using GO as a phase transfer catalyst with different kinds of bases in water and dichloromethane, and we also used GO multiple cycles almost without reduction in reaction yields.
Co-reporter:Yang Li, Peng Cui, Luyang Wang, Hanleem Lee, Keunsik Lee, and Hyoyoung Lee
ACS Applied Materials & Interfaces 2013 Volume 5(Issue 18) pp:9155
Publication Date(Web):August 22, 2013
DOI:10.1021/am402578d
Recently, silver nanowires (AgNWs) have attracted considerable interest for their potential application in flexible transparent conductive films (TCFs). One challenge for the commercialization of AgNW-based TCFs is the low conductivity and stability caused by the weak adhesion forces between the AgNWs and the substrate. Here, we report a highly bendable, conductive, and transparent AgNW film, which consists of an underlying poly(diallyldimethyl-ammonium chloride) (PDDA) and AgNW composite bottom layer and a top layer-by-layer (LbL) assembled graphene oxide (GO) and PDDA overcoating layer (OCL). We demonstrated that PDDA could increase the adhesion between the AgNW and the substrate to form a uniform AgNW network and could also serve to improve the stability of the GO OCL. Hence, a highly bendable, conductive, and transparent AgNW–PDDA–GO composite TCF on a poly(ethylene terephthalate) (PET) substrate with Rs ≈ 10 Ω/sq and T ≈ 91% could be made by an all-solution processable method at room temperature. In addition, our AgNW–PDDA–GO composite TCF is stable without degradation after exposure to H2S gas or sonication.Keywords: materials science; polymers; silver nanowires; transparent conductors;
Co-reporter:Sohyeon Seo, Yeoheung Yoon, Junghyun Lee, Younghun Park, and Hyoyoung Lee
ACS Nano 2013 Volume 7(Issue 4) pp:3607
Publication Date(Web):March 23, 2013
DOI:10.1021/nn400588u
As memory materials, two-dimensional (2D) carbon materials such as graphene oxide (GO)-based materials have attracted attention due to a variety of advantageous attributes, including their solution-processability and their potential for highly scalable device fabrication for transistor-based memory and cross-bar memory arrays. In spite of this, the use of GO-based materials has been limited, primarily due to uncontrollable oxygen functional groups. To induce the stable memory effect by ionic charges of a negatively charged carboxylic acid group of partially reduced graphene oxide (PrGO), a positively charged pyridinium N that served as a counterion to the negatively charged carboxylic acid was carefully introduced on the PrGO framework. Partially reduced N-doped graphene oxide (PrGODMF) in dimethylformamide (DMF) behaved as a semiconducting nonvolatile memory material. Its optical energy band gap was 1.7–2.1 eV and contained a sp2 C═C framework with 45–50% oxygen-functionalized carbon density and 3% doped nitrogen atoms. In particular, rewritable nonvolatile memory characteristics were dependent on the proportion of pyridinum N, and as the proportion of pyridinium N atom decreased, the PrGODMF film lost memory behavior. Polarization of charged PrGODMF containing pyridinium N and carboxylic acid under an electric field produced N-doped PrGODMF memory effects that followed voltage-driven rewrite-read-erase-read processes.Keywords: nitrogen doping; nonvolatile memory; optical band gap; partially reduced graphene oxide; polarization
Co-reporter:Sohyeon Seo, Junghyun Lee, Sung-Yool Choi and Hyoyoung Lee  
Journal of Materials Chemistry A 2012 vol. 22(Issue 5) pp:1868-1875
Publication Date(Web):01 Dec 2011
DOI:10.1039/C1JM14715C
Redox-active metal complexes (e.g., FeII, RuII, and CoII biphenylterpyridine) exhibiting multiple electroreduction behaviors show multilevel conductance switching through various metallic contacts, including Au, Pt/Ir, and reduced graphene oxide (rGO), in solid-state molecular junctions (e.g., a metal–molecule–metal junction). At Pt/Ir and Au contacts in the scanning tunneling microscopy (STM)-based junctions or Au/rGO film contacts in monolayer-based devices, current–voltage (I/V) characteristics have different energy distributions depending on the level of injection into the three electron affinity levels of the redox-active metal complexes. These metal complexes can be negatively charged when the energy levels between the Fermi levels of the metal contacts and the molecular reduction states are aligned, which strongly depends upon the molecular conductance states of conjugated ligands coordinated to central metal atoms. Multiple reduction states of redox-active metal complexes measured with solution-phase electrochemistry correspond to the multiple electron affinity levels of the solid-state molecular junctions, which suggests the possibility of multilevel molecular memory components.
Co-reporter:Prasenjit Bhunia, Eunhee Hwang, Misook Min, Junghyun Lee, Sohyeon Seo, Surajit Some and Hyoyoung Lee  
Chemical Communications 2012 vol. 48(Issue 6) pp:913-915
Publication Date(Web):21 Nov 2011
DOI:10.1039/C1CC16225J
We introduce non-volatile resistive crossbar memory based on ionic liquid covalently functionalized on a partially reduced graphene oxide (PrGO). The write–read–erase–read (WRER) cycles were very stable after several hundred cycles and the retention time of both the ON and OFF states was stable for over 1000 s, indicating that the device we developed can function as a non-volatile memory device.
Co-reporter:Changhua Jin, Junghyun Lee, Eunkyo Lee, Eunhee Hwang and Hyoyoung Lee  
Chemical Communications 2012 vol. 48(Issue 35) pp:4235-4237
Publication Date(Web):07 Mar 2012
DOI:10.1039/C2CC30973D
Recently, the number of studies concerning organic memory devices has grown rapidly due to increase in the demand for electronic devices. Among the organic memory devices, the development of organic nonvolatile memory materials and devices is becoming an important research topic due to their low power consumption.
Co-reporter:Luyang Wang, Jie Lian, Peng Cui, Yang Xu, Sohyeon Seo, Junghyun Lee, Yinthai Chan and Hyoyoung Lee  
Chemical Communications 2012 vol. 48(Issue 34) pp:4052-4054
Publication Date(Web):12 Jan 2012
DOI:10.1039/C2CC17543F
Here, we demonstrate a rapid and simple method for doping a reduced graphene oxide (rGO) field effect transistor (FET) with nanocrystals to produce dual n-type behavior with light and bias voltage. This convenient method promises industrial level doping of graphene transistors.
Co-reporter:Prasenjit Bhunia, Giyoun Kim, Chul Baik and Hyoyoung Lee  
Chemical Communications 2012 vol. 48(Issue 79) pp:9888-9890
Publication Date(Web):15 Aug 2012
DOI:10.1039/C2CC35120J
The iron oxide nanoparticles were transformed to a matrix of iron–iron oxide on the graphene surface at an elevated temperature in a H2/Ar atmosphere. The resultant iron–iron oxide dispersed graphene was highly porous, robust and attractive for a variety of potential applications.
Co-reporter:Surajit Some, Youngmin Kim, EunHee Hwang, HeeJoun Yoo and Hyoyoung Lee  
Chemical Communications 2012 vol. 48(Issue 62) pp:7732-7734
Publication Date(Web):13 Jun 2012
DOI:10.1039/C2CC33916A
For the first time, stable aqueous dispersions of graphene sheets can be prepared via exfoliation/in situ reduction of graphene oxide in the presence of binol salt, a stabilizing surfactant that can be completely removed without affecting the properties of graphene sheets.
Co-reporter:Surajit Some, Seok-Man Ho, Pooja Dua, Eunhee Hwang, Young Hun Shin, HeeJoun Yoo, Jong-Sun Kang, Dong-ki Lee, and Hyoyoung Lee
ACS Nano 2012 Volume 6(Issue 8) pp:7151
Publication Date(Web):July 30, 2012
DOI:10.1021/nn302215y
Dual-function poly(l-lysine) (PLL) composites that function as antibacterial agents and promote the growth of human cell culture have been sought by researchers for a long period. In this paper, we report the preparation of new graphene derivative–PLL composites via electrostatic interactions and covalent bonding between graphene derivatives and PLL. The resulting composites were characterized by infrared spectroscopy, scanning electron microscopy, and X-ray photoelectron spectroscopy. The novel dual function of PLL composites, specifically antibacterial activity and biocompatibility with human cells [human adipose-derived stem cells and non-small-cell lung carcinoma cells (A549)], was carefully investigated. Graphene–DS–PLL composites composed of 4-carboxylic acid benzene diazonium salt (DS) generated more anionic carboxylic acid groups to bind to cationic PLLs, forming the most potent antibacterial agent among PLL and PLL composites with high biocompatibility with human cell culture. This dual functionality can be used to inhibit bacterial growth while enhancing human cell growth.Keywords: bacterial inhibition; electrostatic interactions; graphene oxide; noncytotoxic effect; PLL−graphene composite
Co-reporter:Dr. Prasenjit Bhunia;Eunhee Hwang;Yeoheung Yoon;Eunkyo Lee;Dr. Sohyeon Seo ; Hyoyoung Lee
Chemistry - A European Journal 2012 Volume 18( Issue 39) pp:12207-12212
Publication Date(Web):
DOI:10.1002/chem.201201593
Co-reporter:Dr. Surajit Some;Dr. Prasenjit Bhunia;EunHee Hwang;Keunsik Lee;Yeoheung Yoon;Dr. Sohyeon Seo ; Hyoyoung Lee
Chemistry - A European Journal 2012 Volume 18( Issue 25) pp:7665-7670
Publication Date(Web):
DOI:10.1002/chem.201200104
Co-reporter:Yeoheung Yoon;Dr. Sohyeon Seo;Giyoun Kim;Dr. Hyoyoung Lee
Chemistry - A European Journal 2012 Volume 18( Issue 42) pp:13466-13472
Publication Date(Web):
DOI:10.1002/chem.201201901

Abstract

Thermally doped nitrogen atoms on the sp2-carbon network of reduced graphene oxide (rGO) enhance its electrical conductivity. Atomic structural information of thermally annealed graphene oxide (GO) provides an understanding on how the heteroatomic doping could affect electronic property of rGO. Herein, the spectroscopic and microscopic variations during thermal graphitization from 573 to 1 373 K are reported in two different rGO sheets, prepared by thermal annealing of GO (rGOtherm) and post-thermal annealing of chemically nitrogen-doped rGO (post-therm-rGO). The spectroscopic transitions of rGO in thermal annealing ultimately showed new oxygen-functional groups, such as cyclic edge ethers and new graphitized nitrogen atoms at 1 373 K. During the graphitization process, the microscopic evolution resolved by scanning tunneling microscopy (STM) produced more wrinkled surface morphology with graphitized nanocrystalline domains due to atomic doping of nitrogen on a post-therm-rGO sheet. As a result, the post-therm-rGO-containing nitrogen showed a less defected sp2-carbon network, resulting in enhanced conductivity, whereas the rGOtherm sheet containing no nitrogen had large topological defects on the basal plane of the sp2-carbon network. Thus, our investigation of the structural evolution of original wrinkles on a GO sheet incorporated into the graphitized N-doped rGO helps to explain how the atomic doping can enhance the electrical conductivity.

Co-reporter:Heejoun Yoo;Youngmin Kim;Dr. Junghyun Lee;Hyemi Lee;Yeoheung Yoon;Giyoun Kim ; Hyoyoung Lee
Chemistry - A European Journal 2012 Volume 18( Issue 16) pp:4923-4929
Publication Date(Web):
DOI:10.1002/chem.201103967

Abstract

Graphene is of considerable interest as a next-generation semiconductor material to serve as a possible substitute for silicon. For real device applications with complete circuits, effective n-type graphene field effect transistors (FETs) capable of operating even under atmospheric conditions are necessary. In this study, we investigated n-type reduced graphene oxide (rGO) FETs of photoactive metal oxides, such as TiO2 and ZnO. These metal oxide doped FETs showed slight n-type electric properties without irradiation. Under UV light these photoactive materials readily generated electrons and holes, and the generated electrons easily transferred to graphene channels. As a result, the graphene FET showed strong n-type electric behavior and its drain current was increased. These n-doping effects showed saturation curves and slowly returned back to their original state in darkness. Finally, the n-type rGO FET was also highly stable in air due to the use of highly resistant metal oxides and robust graphene as a channel.

Co-reporter:Dr. Junghyun Lee;Eunhee Hwang;Eunkyo Lee;Dr. Sohyeon Seo ; Hyoyoung Lee
Chemistry - A European Journal 2012 Volume 18( Issue 17) pp:5155-5159
Publication Date(Web):
DOI:10.1002/chem.201103554
Co-reporter:Dr. Sohyeon Seo;Misook Min;Dr. Junghyun Lee;Dr. Takhee Lee;Dr. Sung-Yool Choi;Dr. Hyoyoung Lee
Angewandte Chemie International Edition 2012 Volume 51( Issue 1) pp:108-112
Publication Date(Web):
DOI:10.1002/anie.201105895
Co-reporter:Dr. Sohyeon Seo;Misook Min;Dr. Junghyun Lee;Dr. Takhee Lee;Dr. Sung-Yool Choi;Dr. Hyoyoung Lee
Angewandte Chemie 2012 Volume 124( Issue 1) pp:112-116
Publication Date(Web):
DOI:10.1002/ange.201105895
Co-reporter:Sohyeon Seo, Changhua Jin, Young Rae Jang, Junghyun Lee, Seong Kyu Kim and Hyoyoung Lee  
Journal of Materials Chemistry A 2011 vol. 21(Issue 15) pp:5805-5811
Publication Date(Web):02 Mar 2011
DOI:10.1039/C0JM03939J
Electric field-induced (EFI) reduction of graphene oxide (GO) was performed by conductive atomic force microscopy (C-AFM) in order to create a reduced GO (rGO) p–n nanopattern diode in a dry and non-destructive single-pot process. Single GO sheets were deposited by the Langmuir–Blodgett (LB) method onto semiconducting (n- and p-doping Si) substrates that control charge transfer at the rGO interface. EFI nanolithography resulted in locally reduced GO nanopatterns on GO sheets corresponding to the application of a negative bias voltage on an n-doping Si substrate. EFI nanolithography was performed as a function of applied voltage, and the rGO nanopatterned at −10.0 Vsub showed high conductivity, comparable with that of the chemically reduced GO. In addition, transport of rGO sheets, which were efficiently reduced under a local electric field, showed a uniform conductivity at sheet edges and the basal plane. Current–voltage (I–V) characteristics of rGO on n- and p-doping Si substrates indicated that EFI reduction nanolithography produced p-type rGO nanopatterns on the Si substrates. In conclusion, we successfully fabricated a p–n diode junction of p-type rGO/n-doping Si into nanopatterns. This junction is an indispensable electronic component that rectifies charge transport and prevents interference between neighboring electronic components in high density integrated crossbar devices.
Co-reporter:Peng Cui, Junghyun Lee, Eunhee Hwang and Hyoyoung Lee  
Chemical Communications 2011 vol. 47(Issue 45) pp:12370-12372
Publication Date(Web):20 Oct 2011
DOI:10.1039/C1CC15569E
We report a new reducing agent system: hydriodic acid with trifluoroacetic acid, which can chemically convert graphene oxide into reduced graphene oxide at temperatures below 0 °C in solution. This is the first achievement to produce reduced graphene oxide at subzero temperature with a mass production.
Co-reporter:In Kyu Moon, Junghyun Lee and Hyoyoung Lee  
Chemical Communications 2011 vol. 47(Issue 34) pp:9681-9683
Publication Date(Web):22 Jul 2011
DOI:10.1039/C1CC13312H
We report new step-by-step reduction methods by alternating two different reducing reagents with the order of hydrazine with NH3 (NH)/HI in acetic acid (HI) and the reverse order (HI/NH) to understand nitrogen incorporation and removal or reduction for providing highly qualified reduced graphene oxides (rGOs).
Co-reporter:Joowon Lee, Won G. Hong, Hyoyoung Lee
Organic Electronics 2011 Volume 12(Issue 6) pp:988-992
Publication Date(Web):June 2011
DOI:10.1016/j.orgel.2011.03.021
An organic, electrically bistable device with a novel charge trap system (CTS, LiF/Al/LiF) in the crossbar structure of Al/Alq3/(LiF/Al/LiF)/Alq3/Al was fabricated to develop a vertically oriented crossbar array memory device. The novel concept of CTS with thickness control (2, 4, and 6 nm) of an insulating LiF layer was introduced. The CTS with a 4.0 nm-thick LiF layer displayed non-volatile memory behavior with a hysteresis having large ON/OFF ratio (more than three orders of magnitude) and had the ability of writing–reading–erasing–reading cycles. No significant degradation of the device was observed in either the ON or OFF state after continuous stress testing (>2000 s).Graphical abstractCharge-trap organic memoryHighlights► The crossbar structure of Al/Alq3/(LiF/Al/LiF)/Alq3/Al was fabricated. ► A charge trap system (CTS, LiF/Al/LiF) showed bistability. ► The CTS with a 4.0 nm-thick LiF layer displayed non-volatile memory behavior. ► No significant degradation of writing–reading–erasing–reading cycles was not observed.
Co-reporter:Peng Cui, Sohyeon Seo, Junghyun Lee, Luyang Wang, Eunkyo Lee, Misook Min, and Hyoyoung Lee
ACS Nano 2011 Volume 5(Issue 9) pp:6826
Publication Date(Web):August 15, 2011
DOI:10.1021/nn2021875
Nonvolatile memory devices using gold nanoparticles (AuNPs) and reduced graphene oxide (rGO) sheets were fabricated in both horizontal and vertical structures. The horizontal memory device, in which a singly and doubly overlayered semiconducting rGO channel was formed by simply using a spin-casting technique to connect two gold electrodes, was designed for understanding the origin of charging effects. AuNPs were chemically bound to the rGO channel through a π-conjugated molecular linker. The π-conjugated bifunctional molecular linker, 4-mercapto-benzenediazonium tetrafluoroborate (MBDT) salt, was newly synthesized and used as a molecular bridge to connect the AuNPs and rGOs. By using a self-assembly technique, the diazonium functional group of the MBDT molecular linker was spontaneously immobilized on the rGOs. Then, the monolayered AuNPs working as capacitors were covalently connected to the thiol groups of the MBDT molecules, which were attached to rGOs (AuNP-frGO). These covalent bonds were confirmed by XPS analyses. The current–voltage characteristics of both the horizontal and vertical AuNP-frGO memory devices showed noticeable nonlinear hysteresis, stable write–multiple read–erase–multiple read cycles over 1000 s, and a long retention time over 700 s. In addition, the vertical AuNP-frGO memory device showed a large current ON/OFF ratio and high stability.Keywords: gold nanoparticle; nanotechnology; nonvolatile memory; reduced graphene oxide; self-assembled monolayer
Co-reporter:Sohyeon Seo and Hyoyoung Lee
The Journal of Physical Chemistry C 2011 Volume 115(Issue 31) pp:15480-15486
Publication Date(Web):July 5, 2011
DOI:10.1021/jp203919w
Using ultrahigh vacuum scanning tunneling microscopy (UHV-STM), we studied the thermal-processing-induced structural changes that occur during formation of a 1-octanethiol (OT) self-assembled monolayer (SAM) on Au(111) near melting temperature in an OT solution. A favorable ordered phase of a c(4√3 × 2√3) structure was achieved at high temperature (e.g., 343 K) below the melting temperature of (e.g., 353 K) alkanethiol SAMs, while a favorably ordered phase of a (√3 × √3) structure was achieved at the melting temperature. The high resolution STM observation indicated the following: (1) the growth process of OT SAMs in an OT solution induced a change in the structural phase via diffusion of OT molecules on gold by thermal energy at a high temperature below the melting temperature; (2) application of the melting temperature resulted in partial desorption of OT molecules from the surface due to melting of OT SAMs, showing a striped phase and a disordered phase; and (3) after melting of the SAM, time-dependent rearrangement of OT molecules adsorbed on Au(111) occurred through relaxation of surface Au atoms, which caused thiolate–gold complexes to diffuse and reform a (√3 × √3) phase. Furthermore, the ultimate structural transition to a c(4√3 × 2√3) structure at 343 K revealed the translational transition of molecular adsorption sites induced by lateral movements of OT–Au complexes at a high temperature in a solution. Also, the absence of domain boundaries among the three mobile phases (i.e., disordered, striped, and ordered (√3 × √3)) at 353 K revealed that there is no transition of molecular adsorption sites after melting of the SAM.
Co-reporter:Dr. Junghyun Lee;Eunkyo Lee;Sangkwan Kim;Dr. Gyeong Sook Bang; David A. Shultz;Dr. Robert D. Schmidt; Malcolm D. E. Forbes; Hyoyoung Lee
Angewandte Chemie International Edition 2011 Volume 50( Issue 19) pp:4414-4418
Publication Date(Web):
DOI:10.1002/anie.201004899
Co-reporter:Mi-Hee Jung, Kyu Ho Song, Kyoung Chul Ko, Jin Yong Lee and Hyoyoung Lee  
Journal of Materials Chemistry A 2010 vol. 20(Issue 37) pp:8016-8020
Publication Date(Web):10 Aug 2010
DOI:10.1039/C0JM00854K
We report a nonvolatile memory organic field effect transistor (OFET) using ambipolar organic molecules as nano-interfaced semiconductor materials. Newly synthesized push-pull organic molecules (PPOMs) containing triarylamine as an electron donating group, thiophene as a spacer, and malononitrile as an electron withdrawing group are proposed. The tilted PPOMs with side chains could control the charge trapping of the conducting channel formed between pentacene and PPOMs. Quantum chemical calculations were carried out to estimate the dihedral angle at the neutral and electron charged anion molecules and to explain the charging effects for the memory OFET performance (write-read-erase-read cycles). The charge mobilities of OFETs comprising the nano-interfaced PPOMs were affected by the dihedral angles derived from the steric hindrance of the bulky side chain of the spacer. The memory OTFT with higher dihedral angle material exhibited a wider memory window as well as reduced current flow. The memory OFET devices showed a memory window of −40 to +40 V, a memory ratio of 100 for “ON” to “OFF” currents, and long retention time for the nonvolatile memory.
Co-reporter:Misook Min, Gyeong Sook Bang, Hyoyoung Lee and Byung-Chan Yu  
Chemical Communications 2010 vol. 46(Issue 29) pp:5232-5234
Publication Date(Web):26 May 2010
DOI:10.1039/C0CC00521E
Aryldiazonium-terminated methylene-spaced trifluoromethylazobenzene derivatives have been synthesized. Their self-assembled monolayers (SAMs) on a silicon surface allow for a stable and reversible molecular photoswitch.
Co-reporter:Kyoungja Seo, Alexander V. Konchenko, Junghyun Lee, Gyeong Sook Bang and Hyoyoung Lee  
Journal of Materials Chemistry A 2009 vol. 19(Issue 41) pp:7617-7624
Publication Date(Web):10 Sep 2009
DOI:10.1039/B912563A
Voltammograms and current–voltage (I–V) characteristics are measured to elucidate electron transport processes in the bistable conducting states of single molecular junctions of a molecular switch, alkyl-tailed RuII terpyridine complexes. (1) On the basis of the Ru-centered electrochemical reaction data, the electron transport rate increases in the mixed self-assembled monolayer (SAM) of RuII terpyridine complexes, indicating strong electronic coupling between the redox center and the substrate, along the molecules. (2) In a low-conducting state before switch-on, I–V characteristics are fitted to a direct tunneling model, and the estimated tunneling decay constant across the RuII terpyridine complex is found to be smaller than that of alkanethiol. (3) The threshold voltages for the switch-on from low- to high-conducting states are identical, corresponding to the electron affinity of the molecules. (4) A high-conducting state after switch-on remains in the reverse voltage sweep, and a linear relationship of the current to the voltage is obtained. These results reveal electron transport paths via the redox centers of the alkyl-tailed RuII terpyridine complexes, a molecular switch.
Co-reporter:Junghyun Lee Dr.;Hojong Chang;Sangkwan Kim;GyeongSook Bang Dr.
Angewandte Chemie International Edition 2009 Volume 48( Issue 45) pp:8501-8504
Publication Date(Web):
DOI:10.1002/anie.200902990
Co-reporter:Junghyun Lee Dr.;Hojong Chang;Sangkwan Kim;GyeongSook Bang Dr.
Angewandte Chemie 2009 Volume 121( Issue 45) pp:8653-8656
Publication Date(Web):
DOI:10.1002/ange.200902990
Co-reporter:Gyeong Sook Bang, Junghyun Lee, Hee Yoel Baek, Hyoyoung Lee, Kun Jun and Seung Rim Shin
Langmuir 2009 Volume 25(Issue 18) pp:10788-10793
Publication Date(Web):July 15, 2009
DOI:10.1021/la901323d
The novel azothiophene derivatives [AT-di(CnSAc) (n = 6 and 12)], an azo linkage (N═N) that bridges one phenyl ring with an N-bridging dialkylthioacetate tail and one thiophene ring, are synthesized and characterized. The azothiophene derivatives substituted with electron-withdrawing groups are blue in color, exhibit a bathochromic shift of a longer wavelength, and are electrochemically active. The formation and characterization of AT-di(CnSAc) SAMs with a bidentate tail group of the N-bridging dialkylthioacetate have been studied by surface sensitive techniques such as grazing angle Fourier transform infrared (FT-IR), a quartz crystal microbalance (QCM), spectroscopic ellipsometry, X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry (CV). It has been shown that the adsorption reaction of the thioacetate group is almost spontaneous and the N-bridging dialkylthioacetate SAMs with longer methylene length have a packing density higher than that with a shorter methylene length. However, the sulfur tethers of the N-bridging dialkylthioacetate show incomplete binding of sulfur atoms in AT-di(CnSAc) SAMs.
Co-reporter:Kyoungja Seo and Hyoyoung Lee
ACS Nano 2009 Volume 3(Issue 9) pp:2469
Publication Date(Web):August 11, 2009
DOI:10.1021/nn8008917
We demonstrated structural phase dependency of conductance across thiolate self-assembled monolayers (SAMs) in different junctions. A structural phase transition from a hexagonal closed phase to a striped phase in 1-octanethiol (OT) and 1,8-octanedithiol (ODT) SAMs was revealed by high resolution scanning tunneling microscopy (STM) images. Electron tunneling characteristics were measured through STM-based individual molecular junctions and micropore-based large molecular junctions. The tunneling barrier height and the tunneling decay constant of the molecular junctions were used as measures of the intermolecular coupling for different structural phases of the thiolate SAMs. Electron transport through ODT SAMs was found to be more sensitive than that through OT SAMs, according to the structural phase transition. These results suggest that (1) the structural phase transition in the SAM induces a change in the electron tunneling distance through the pathway of through-bond tunneling and through-space tunneling, leading to a change in the tunneling barrier of molecular junctions, and (2) integrated intermolecular coupling in a large molecular junction leads to a significant change of the electron transport between two structural phases.Keywords: electron transport; molecular electronics; molecular junction; self-assembled monolayer; structural phase transition
Co-reporter:Kyoungja Seo, Alexander V. Konchenko, Junghyun Lee, Gyeong Sook Bang and Hyoyoung Lee
Journal of Materials Chemistry A 2009 - vol. 19(Issue 41) pp:NaN7624-7624
Publication Date(Web):2009/09/10
DOI:10.1039/B912563A
Voltammograms and current–voltage (I–V) characteristics are measured to elucidate electron transport processes in the bistable conducting states of single molecular junctions of a molecular switch, alkyl-tailed RuII terpyridine complexes. (1) On the basis of the Ru-centered electrochemical reaction data, the electron transport rate increases in the mixed self-assembled monolayer (SAM) of RuII terpyridine complexes, indicating strong electronic coupling between the redox center and the substrate, along the molecules. (2) In a low-conducting state before switch-on, I–V characteristics are fitted to a direct tunneling model, and the estimated tunneling decay constant across the RuII terpyridine complex is found to be smaller than that of alkanethiol. (3) The threshold voltages for the switch-on from low- to high-conducting states are identical, corresponding to the electron affinity of the molecules. (4) A high-conducting state after switch-on remains in the reverse voltage sweep, and a linear relationship of the current to the voltage is obtained. These results reveal electron transport paths via the redox centers of the alkyl-tailed RuII terpyridine complexes, a molecular switch.
Co-reporter:Mi-Hee Jung, Kyu Ho Song, Kyoung Chul Ko, Jin Yong Lee and Hyoyoung Lee
Journal of Materials Chemistry A 2010 - vol. 20(Issue 37) pp:NaN8020-8020
Publication Date(Web):2010/08/10
DOI:10.1039/C0JM00854K
We report a nonvolatile memory organic field effect transistor (OFET) using ambipolar organic molecules as nano-interfaced semiconductor materials. Newly synthesized push-pull organic molecules (PPOMs) containing triarylamine as an electron donating group, thiophene as a spacer, and malononitrile as an electron withdrawing group are proposed. The tilted PPOMs with side chains could control the charge trapping of the conducting channel formed between pentacene and PPOMs. Quantum chemical calculations were carried out to estimate the dihedral angle at the neutral and electron charged anion molecules and to explain the charging effects for the memory OFET performance (write-read-erase-read cycles). The charge mobilities of OFETs comprising the nano-interfaced PPOMs were affected by the dihedral angles derived from the steric hindrance of the bulky side chain of the spacer. The memory OTFT with higher dihedral angle material exhibited a wider memory window as well as reduced current flow. The memory OFET devices showed a memory window of −40 to +40 V, a memory ratio of 100 for “ON” to “OFF” currents, and long retention time for the nonvolatile memory.
Co-reporter:Sohyeon Seo, Junghyun Lee, Sung-Yool Choi and Hyoyoung Lee
Journal of Materials Chemistry A 2012 - vol. 22(Issue 5) pp:NaN1875-1875
Publication Date(Web):2011/12/01
DOI:10.1039/C1JM14715C
Redox-active metal complexes (e.g., FeII, RuII, and CoII biphenylterpyridine) exhibiting multiple electroreduction behaviors show multilevel conductance switching through various metallic contacts, including Au, Pt/Ir, and reduced graphene oxide (rGO), in solid-state molecular junctions (e.g., a metal–molecule–metal junction). At Pt/Ir and Au contacts in the scanning tunneling microscopy (STM)-based junctions or Au/rGO film contacts in monolayer-based devices, current–voltage (I/V) characteristics have different energy distributions depending on the level of injection into the three electron affinity levels of the redox-active metal complexes. These metal complexes can be negatively charged when the energy levels between the Fermi levels of the metal contacts and the molecular reduction states are aligned, which strongly depends upon the molecular conductance states of conjugated ligands coordinated to central metal atoms. Multiple reduction states of redox-active metal complexes measured with solution-phase electrochemistry correspond to the multiple electron affinity levels of the solid-state molecular junctions, which suggests the possibility of multilevel molecular memory components.
Co-reporter:Heejoun Yoo, Misook Min, Sora Bak, Yeoheung Yoon and Hyoyoung Lee
Journal of Materials Chemistry A 2014 - vol. 2(Issue 18) pp:NaN6668-6668
Publication Date(Web):2014/02/18
DOI:10.1039/C4TA00158C
A hydrophilic surface modified carbon electrode shows a good electrolyte affinity with homogeneous dispersibility in water, resulting in low ion-transfer resistance and a uniform and dense electrode to give a high volumetric capacitor. The hydrophilic carbon electrode exhibits a superior capacitance (58 F cm−3, 99.3 mF cm−2) and is stable up to 5000 cycles.
Co-reporter:Peng Cui, Junghyun Lee, Eunhee Hwang and Hyoyoung Lee
Chemical Communications 2011 - vol. 47(Issue 45) pp:NaN12372-12372
Publication Date(Web):2011/10/20
DOI:10.1039/C1CC15569E
We report a new reducing agent system: hydriodic acid with trifluoroacetic acid, which can chemically convert graphene oxide into reduced graphene oxide at temperatures below 0 °C in solution. This is the first achievement to produce reduced graphene oxide at subzero temperature with a mass production.
Co-reporter:Surajit Some, Youngmin Kim, EunHee Hwang, HeeJoun Yoo and Hyoyoung Lee
Chemical Communications 2012 - vol. 48(Issue 62) pp:NaN7734-7734
Publication Date(Web):2012/06/13
DOI:10.1039/C2CC33916A
For the first time, stable aqueous dispersions of graphene sheets can be prepared via exfoliation/in situ reduction of graphene oxide in the presence of binol salt, a stabilizing surfactant that can be completely removed without affecting the properties of graphene sheets.
Co-reporter:Changhua Jin, Junghyun Lee, Eunkyo Lee, Eunhee Hwang and Hyoyoung Lee
Chemical Communications 2012 - vol. 48(Issue 35) pp:NaN4237-4237
Publication Date(Web):2012/03/07
DOI:10.1039/C2CC30973D
Recently, the number of studies concerning organic memory devices has grown rapidly due to increase in the demand for electronic devices. Among the organic memory devices, the development of organic nonvolatile memory materials and devices is becoming an important research topic due to their low power consumption.
Co-reporter:Luyang Wang, Jie Lian, Peng Cui, Yang Xu, Sohyeon Seo, Junghyun Lee, Yinthai Chan and Hyoyoung Lee
Chemical Communications 2012 - vol. 48(Issue 34) pp:NaN4054-4054
Publication Date(Web):2012/01/12
DOI:10.1039/C2CC17543F
Here, we demonstrate a rapid and simple method for doping a reduced graphene oxide (rGO) field effect transistor (FET) with nanocrystals to produce dual n-type behavior with light and bias voltage. This convenient method promises industrial level doping of graphene transistors.
Co-reporter:Khokan Samanta, Surajit Some, Youngmin Kim, Yeoheung Yoon, Misook Min, Sae Mi Lee, Younghun Park and Hyoyoung Lee
Chemical Communications 2013 - vol. 49(Issue 79) pp:NaN8993-8993
Publication Date(Web):2013/08/05
DOI:10.1039/C3CC45376F
A facile method for the synthesis of highly fluorinated reduced graphene oxide from graphene oxide using BF3-OEt2 solution and alkylthiol/alkylamine on the Gram scale has been described using a detailed mechanism. The maximum fluorination was as high as 38 wt% and the fluorinated reduced graphene oxide produced has great wettability and high insulating properties.
Co-reporter:Luyang Wang, Younghun Park, Peng Cui, Sora Bak, Hanleem Lee, Sae Mi Lee and Hyoyoung Lee
Chemical Communications 2014 - vol. 50(Issue 10) pp:NaN1226-1226
Publication Date(Web):2013/10/30
DOI:10.1039/C3CC47224H
We introduce a facile method to prepare an n-type reduced graphene oxide field effect transistor at room temperature via a typical Benkeser reduction using lithium and ethylenediamine.
Co-reporter:Youngmin Kim, Surajit Some and Hyoyoung Lee
Chemical Communications 2013 - vol. 49(Issue 50) pp:NaN5704-5704
Publication Date(Web):2013/05/09
DOI:10.1039/C3CC42787K
We demonstrated a simple and green chemical method to obtain Michael adducts and their derivatives by using GO as a phase transfer catalyst with different kinds of bases in water and dichloromethane, and we also used GO multiple cycles almost without reduction in reaction yields.
Co-reporter:Misook Min, Sohyeon Seo, Junghyun Lee, Sae Mi Lee, Eunhee Hwang and Hyoyoung Lee
Chemical Communications 2013 - vol. 49(Issue 56) pp:NaN6291-6291
Publication Date(Web):2013/05/22
DOI:10.1039/C3CC42591F
Changes in major charge transport of graphene channel transistors in terms of the spatial orientation of adsorbed functional molecules were demonstrated. In contrast to the horizontally (physically) bound molecules, the vertically (chemically) bound molecules did not change major charge carriers of graphene channels, revealing the molecular orientation-dependent doping effects.
Co-reporter:Prasenjit Bhunia, Eunhee Hwang, Misook Min, Junghyun Lee, Sohyeon Seo, Surajit Some and Hyoyoung Lee
Chemical Communications 2012 - vol. 48(Issue 6) pp:NaN915-915
Publication Date(Web):2011/11/21
DOI:10.1039/C1CC16225J
We introduce non-volatile resistive crossbar memory based on ionic liquid covalently functionalized on a partially reduced graphene oxide (PrGO). The write–read–erase–read (WRER) cycles were very stable after several hundred cycles and the retention time of both the ON and OFF states was stable for over 1000 s, indicating that the device we developed can function as a non-volatile memory device.
Co-reporter:Prasenjit Bhunia, Giyoun Kim, Chul Baik and Hyoyoung Lee
Chemical Communications 2012 - vol. 48(Issue 79) pp:NaN9890-9890
Publication Date(Web):2012/08/15
DOI:10.1039/C2CC35120J
The iron oxide nanoparticles were transformed to a matrix of iron–iron oxide on the graphene surface at an elevated temperature in a H2/Ar atmosphere. The resultant iron–iron oxide dispersed graphene was highly porous, robust and attractive for a variety of potential applications.
Co-reporter:In Kyu Moon, Junghyun Lee and Hyoyoung Lee
Chemical Communications 2011 - vol. 47(Issue 34) pp:NaN9683-9683
Publication Date(Web):2011/07/22
DOI:10.1039/C1CC13312H
We report new step-by-step reduction methods by alternating two different reducing reagents with the order of hydrazine with NH3 (NH)/HI in acetic acid (HI) and the reverse order (HI/NH) to understand nitrogen incorporation and removal or reduction for providing highly qualified reduced graphene oxides (rGOs).
Co-reporter:Misook Min, Gyeong Sook Bang, Hyoyoung Lee and Byung-Chan Yu
Chemical Communications 2010 - vol. 46(Issue 29) pp:NaN5234-5234
Publication Date(Web):2010/05/26
DOI:10.1039/C0CC00521E
Aryldiazonium-terminated methylene-spaced trifluoromethylazobenzene derivatives have been synthesized. Their self-assembled monolayers (SAMs) on a silicon surface allow for a stable and reversible molecular photoswitch.
Co-reporter:Sohyeon Seo, Changhua Jin, Young Rae Jang, Junghyun Lee, Seong Kyu Kim and Hyoyoung Lee
Journal of Materials Chemistry A 2011 - vol. 21(Issue 15) pp:NaN5811-5811
Publication Date(Web):2011/03/02
DOI:10.1039/C0JM03939J
Electric field-induced (EFI) reduction of graphene oxide (GO) was performed by conductive atomic force microscopy (C-AFM) in order to create a reduced GO (rGO) p–n nanopattern diode in a dry and non-destructive single-pot process. Single GO sheets were deposited by the Langmuir–Blodgett (LB) method onto semiconducting (n- and p-doping Si) substrates that control charge transfer at the rGO interface. EFI nanolithography resulted in locally reduced GO nanopatterns on GO sheets corresponding to the application of a negative bias voltage on an n-doping Si substrate. EFI nanolithography was performed as a function of applied voltage, and the rGO nanopatterned at −10.0 Vsub showed high conductivity, comparable with that of the chemically reduced GO. In addition, transport of rGO sheets, which were efficiently reduced under a local electric field, showed a uniform conductivity at sheet edges and the basal plane. Current–voltage (I–V) characteristics of rGO on n- and p-doping Si substrates indicated that EFI reduction nanolithography produced p-type rGO nanopatterns on the Si substrates. In conclusion, we successfully fabricated a p–n diode junction of p-type rGO/n-doping Si into nanopatterns. This junction is an indispensable electronic component that rectifies charge transport and prevents interference between neighboring electronic components in high density integrated crossbar devices.
(1,1-Biphenyl)-4,4-bis(diazonium), bis(tetrafluoroborate(1-))
Benzenediazonium, 4-sulfo-, inner salt