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Application of Graphene and Two-Dimensional Materials in Thin Films

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A special issue of Coatings (ISSN 2079-6412). This special issue belongs to the section "Thin Films".

Deadline for manuscript submissions: closed (10 September 2024) | Viewed by 28681

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Prof. Dr. Vera Marinova

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Institute of Optical Materials and Technologies, Bulgarian Academy of Sciences, Sofia, Bulgaria
Interests: graphene and 2D materials: synthesis, characterization, and applications; organic–inorganic hybrid structures; holography; liquid crystal displays; spatial light modulators

Special Issue Information

Dear Colleagues,

We would like to invite you to submit your work to this Special Issue on "Application of Graphene and Two-Dimensional Materials in Thin Films". Graphene and two-dimensional (2D) materials are expected to revolutionize next-generation technologies. Their superior physical and chemical properties provide them with a range of potential applications in the fields of optoelectronics, spintronics, electrochemistry, energy storage conversion, catalysis, supercapacitors, and solar cells. Their versatility creates a diverse range of possibilities for biomedicine, sensing, and diagnostics. Moreover, they can be stacked using van der Waals forces to form Van der Waals heterostructures with desirable properties for high-end electronics and flexible optoelectronic devices.

Topics of interest for this Special Issue include (but are not limited to):

graphene and 2D materials in thin films: synthesis, properties, and applications;
graphene and 2D materials in thin films for solar cells, energy harvesting, and energy conversion;
graphene and 2D materials in thin films for biomedicine, sensing, and diagnostics;
novel 2D-based Van der Waals heterostructures;
graphene and 2D materials as flexible thin films;
graphene and 2D materials: new concepts in optoelectronics and spintronics.

The aim of this Special Issue is to publish a collection of original research papers and review articles related to recent advances in the synthesis and characterization of 2D materials and their application as flexible conductor layers in supercapacitors, solar cells, sensors, and other optoelectronic devices. Contributions that present new concepts or mechanisms and describe their potential impacts are also welcome.

Prof. Dr. Vera Marinova
Guest Editor

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Published Papers (11 papers)

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Research

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14 pages, 1720 KiB

Open AccessArticle

The Role of the Manganese Content on the Properties of Mn₃O₄ and Reduced Graphene Oxide Nanocomposites for Supercapacitor Electrodes

by Víctor Fernández-Jiménez, Santiago de Bernardi-Martín, Alejandra García-Gómez, David López-Díaz, M. Jesús Sánchez-Montero, M. Mercedes Velázquez and M. Dolores Merchán

Coatings 2024, 14(9), 1136; https://doi.org/10.3390/coatings14091136 - 4 Sep 2024

Viewed by 740

Abstract

Increasing the energy density and power of supercapacitors through hybrids of carbonaceous materials and metal oxides continues to be the subject of numerous research works. The correlation between specific capacitance and the properties of materials used as electrodes attracts great interest. In the present study, we investigated composites (GO/Mn₃O₄) prepared by the hydrothermal method with a variable ratio of GO/Mn₃O₄ and tested them as supercapacitor electrode materials in three- and two-electrode cells. The chemical characterization carried out by X-ray photoelectron spectroscopy and the adsorption techniques used allowed the determination of the surface carbon and oxygen content, as well as its textural properties. In this work, we analyzed the contribution of the double layer and the Faradaic reactions to the value of the final capacitance of the synthesized materials. Beyond empirically obtaining the electrochemical properties, these have been related to the physicochemical characteristics of the hybrids to help design materials with the best performance for supercapacitor electrodes. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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13 pages, 6063 KiB

Open AccessArticle

Atomic Layer Deposition Growth and Characterization of Al₂O₃ Layers on Cu-Supported CVD Graphene

by Peter Rafailov, Vladimir Mehandzhiev, Peter Sveshtarov, Blagoy Blagoev, Penka Terziyska, Ivalina Avramova, Kiril Kirilov, Bogdan Ranguelov, Georgi Avdeev, Stefan Petrov and Shiuan Huei Lin

Coatings 2024, 14(6), 662; https://doi.org/10.3390/coatings14060662 - 24 May 2024

Cited by 2 | Viewed by 1475

Abstract

The deposition of thin uniform dielectric layers on graphene is important for its successful integration into electronic devices. We report on the atomic layer deposition (ALD) of Al₂O₃ nanofilms onto graphene grown by chemical vapor deposition onto copper foil. A pretreatment with deionized water (DI H₂O) for graphene functionalization was carried out, and, subsequently, trimethylaluminum and DI H₂O were used as precursors for the Al₂O₃ deposition process. The proper temperature regime for this process was adjusted by means of the ALD temperature window for Al₂O₃ deposition onto a Si substrate. The obtained Al₂O₃/graphene heterostructures were characterized by Raman and X-ray photoelectron spectroscopy, ellipsometry and atomic force and scanning electron microscopy. Samples of these heterostructures were transferred onto glass substrates by standard methods, with the Al₂O₃ coating serving as a protective layer during the transfer. Raman monitoring at every stage of the sample preparation and after the transfer enabled us to characterize the influence of the Al₂O₃ coating on the graphene film. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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9 pages, 4520 KiB

Open AccessArticle

NbSe₂ Crystals Growth by Bromine Transport

by Dimitre Dimitrov, Peter Rafailov, Vera Marinova, Ivalina Avramova, Daniela Kovacheva, Irnik Dionisiev, Nikolay Minev and Marin Gospodinov

Coatings 2023, 13(5), 947; https://doi.org/10.3390/coatings13050947 - 18 May 2023

Viewed by 2702

Abstract

Recently, low-dimensional structures in the form of bulk crystals and nanoflakes have received considerable interest due to their 2D unique functionality and promising applications in electronics, photonics, sensing devices and photovoltaic solar cells. As a result, remarkable efforts and modifications have been made for the synthesis process of crystalline material by the vapor transport technique. Here, an alternative concept of NbSe₂ crystal growth by the chemical vapor transport (CVT) technique using bromine as a vapor transport agent is presented and subsequently analyzed by X-ray diffraction (XRD), Raman and X-ray photoelectron spectroscopy (XPS) spectroscopy. X-ray powder diffraction analysis revealed hexagonal 2H-NbSe₂ and 4H-NbSe₂ phases, and characteristic Raman and XPS spectra typical for crystalline NbSe₂ were obtained. The environmental sensitivity of the grown crystals is manifested by luminescence attributed to oxidized Nb at the samples’ surface. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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16 pages, 4463 KiB

Open AccessArticle

MXenes as Alternative Plasmonic Coatings on 1D Photonic Crystals Platforms for Tamm Plasmon Polaritons

by Marko Obradov, Zoran Jakšić, Ivana Mladenović, Anja Bartula and Olga Jakšić

Coatings 2023, 13(1), 198; https://doi.org/10.3390/coatings13010198 - 16 Jan 2023

Cited by 1 | Viewed by 2088

Abstract

New materials are of essential importance for the advancement of nanophotonics and nanoplasmonics. Numerous electromagnetic modes, especially various evanescent surface waves, prove themselves useful in multitudinous practical applications. Here we investigate the use of MXenes as alternative plasmonic materials in freestanding (substrateless) planar nanocomposites that support the existence of Tamm plasmon polaritons (TPP). We use finite element simulations to consider the influence of using MXenes on the propagation and distribution of TPP and the difference in their electromagnetic behavior compared to that of commonly used noble metals. While MXenes allow for somewhat weaker coupling between incident light and TPP, even the thinnest MXene layers practically completely screen the structure behind them. Our diffraction grating-enhanced stacks achieved incident light direction-dependent improvement of the coupling strength and polarization-dependent hybridization of electromagnetic states. MXene ensures improvements in functionality, especially spectral, directional, and polarization selectivity, by imparting rich modal behavior. Importantly, we observed high optical asymmetry of reflectance when illuminating the structures from opposite directions and obtained large high-to-low reflection ratios with a very small number of dielectric layers in the capping 1D photonic crystal. We conclude that MXenes represent a viable alternative for TPP-supporting structures, offering many advantages. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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12 pages, 7338 KiB

Open AccessArticle

Evolution of WSe₂ Flakes Synthesized by Thermally Assisted Conversion Method

by Vera Marinova, Krastyo Buchkov, Vladimira Videva, Irnik Dionisiev, Nikolay Minev, Velichka Strijkova, Deyan Dimov, Hristosko Dikov, Ivalina Avramova, Peter Rafailov and Dimitre Dimitrov

Coatings 2022, 12(3), 353; https://doi.org/10.3390/coatings12030353 - 7 Mar 2022

Cited by 5 | Viewed by 2969

Abstract

We report the synthesis of tungsten diselenide (WSe₂) flakes and continuous layers using an atmospheric pressure thermally assisted conversion (TAC) method, where the tungsten (W) layers were pre-deposited by a magnetron sputtering system onto fused silica substrates. Optical microscopy (OM) and atomic force microscopy (AFM) mapping predominantly revealed the formation of isolated flakes with different shapes, mainly concentrated near the substrate’s edges, which tended to form clusters and to further overlap to continuous layers, moving to the central part of the fused silica substrates. Raman spectroscopy and photoluminescence measurements confirmed the existence of atomically thin flakes and 2H-WSe₂ continuous layers. The measured current–voltage characteristics indicated Ohmic behavior under dark conditions and photo illumination. Finally, the demonstrated resistor-like behavior suggested unlimited prospects for WSe₂ integration into a variety of heterostructures. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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12 pages, 2518 KiB

Open AccessArticle

Electronic Structure of Graphene on the Hexagonal Boron Nitride Surface: A Density Functional Theory Study

by Gladys Casiano-Jiménez, César Ortega-López, Jairo Arbey Rodríguez-Martínez, María Guadalupe Moreno-Armenta and Miguel J. Espitia-Rico

Coatings 2022, 12(2), 237; https://doi.org/10.3390/coatings12020237 - 12 Feb 2022

Cited by 9 | Viewed by 3187

Abstract

Poor electron-related cutting current in graphene-based field-effect transistors (FETs) can be solved by placing a graphene layer over a hexagonal boron nitride (BN) substrate, as established by Giovannetti et al. and other researchers. In order to produce high-quality results, this investigation uses 2 × 2 cells (~2.27% mismatch), given that larger cells lead to more favourable considerations regarding interactions on cell edges. In this case, the substrate-induced band gap is close to 138 meV. In addition, we propose a new material based on graphene on BN in order to take advantage of the wonderful physical properties of both graphene and BN. In this new material, graphene is rotated with respect to BN, and it exhibits a better mismatch, only ~1.34%, than the 1 × 1-graphene/1 × 1-BN; furthermore, it has a very small bandgap, which is almost zero. Therefore, in the bands, there are electronic states in cone form that are like the Dirac cones, which maintain the same characteristics as isolated graphene. In the first case (2 × 2-graphene/2 × 2-BN), for example, the resulting band gap of 138 meV is greater than Giovannetti’s value by a factor of ~2.6. The 2 × 2-graphene/2 × 2-BN cell is better than the 1 × 1-graphene/BN one because a greater bandgap is an improvement in the cutting current of graphene-based FETs, since the barrier created by the bandgap is larger. The calculations in this investigation are performed within the density functional theory (DFT) theory framework, by using 2 × 2-graphene/2 × 2-BN and

\sqrt{13}

\sqrt{13}

-graphene/

2 \sqrt{3}

2 \sqrt{3}

-(0001) BN cells. Pseudopotentials and the generalized gradient approximation (GGA), combined with the Perdew–Burke–Ernzerhof parametrization, were used. Relaxation is allowed for all atoms, except for the last layer of the BN substrate, which serves as a reference for all movements and simulates the bulk BN. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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11 pages, 3000 KiB

Open AccessArticle

Effect of Ultrafast Broadband Nonlinear Optical Responses by Doping Silver into Ti₃C₂ Nanosheets at Visible Spectra

by Yabin Shao, Chen Chen, Qing He, Lingling Xiang and Xianjing Lai

Coatings 2022, 12(2), 189; https://doi.org/10.3390/coatings12020189 - 1 Feb 2022

Cited by 5 | Viewed by 1961

Abstract

Ti₃C₂ nanosheet is a newly discovered two-dimensional (2D) clan. It turns out to have encouraging applications for electromagnetic shielding and energy storage. Here, Ag@ Ti₃C₂ hybrids are precisely synthesized by using the one-step solution processing method. Also, their ultrafast broadband nonlinear optical responses in the visible region are studied systematically through nanosecond open-aperture Z-scan and transient absorption techniques. The mechanism of two-photon absorption (TPA) is disclosed in the visible region (409–532 nm). When the laser energy is low and the wavelength is longer than 400 nm, nonlinear absorption cannot happen. Meanwhile, as the laser energy increases, two photons will be absorbed by the electrons in the valence band and the electrons will jump to the conduction band. The process is named as two-photon absorption which will make the specimen show reverse saturable absorption (RSA) properties. What is more, the ultrafast carrier dynamics of the specimen are studied by using the transient absorption. The result shows that the decay contains two phases: the fast and then the slow one. The two phases first come from electron–phonon and then from phonon–phonon interactions, respectively. The electron transfer and charge carrier trapping processes are further verified by the outcomes of similar measurements on Ag@ Ti₃C₂ hybrids. Besides, the two decay processes increase together with the pump fluence. These results show that Ti₃C₂ nanosheet has potential applications in broadband optical limiter. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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16 pages, 2320 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Pseudo-Planar Organic Heterojunctions by Sequential Printing of Quasi-Miscible Inks

by Ana-Gianina Gereanu, Camillo Sartorio, Aurelio Bonasera, Giuliana Giuliano, Sebastiano Cataldo, Michelangelo Scopelliti, Giuseppe Arrabito and Bruno Pignataro

Coatings 2021, 11(5), 586; https://doi.org/10.3390/coatings11050586 - 17 May 2021

Cited by 5 | Viewed by 3534

Abstract

This work deals with the interfacial mixing mechanism of picoliter (pL)-scale droplets produced by sequential inkjet printing of organic-based inks onto ITO/PET surfaces at a moderately high Weber number (~10¹). Differently from solution dispensing processes at a high Bond number such as spin coating, the deposition by inkjet printing is strictly controlled by droplet velocity, ink viscosity, and surface tension. In particular, this study considers the interfacial mixing of droplets containing the most investigated donor/acceptor couple for organic solar cells, i.e., poly(3-hexylthiophene) (P3HT) and (6,6)-phenyl-C₆₁-butyric acid methyl ester (PCBM), showing how low-viscosity and low-surface energy inks can be leveraged for the fabrication of an interface suitable for a pseudo-planar heterojunction (pseudo-PHJ) organic solar cell (OSC) that is a convenient alternative to a bulk heterojunction (BHJ) OSC. The resulting thin-film morphology and molecular organization at the P3HT/PCBM interface are investigated, highlighting the roles of dissolution-driven molecular recirculation. This report represents a first step toward the sequential inkjet printing fabrication of pseudo-PHJ OSCs at low consumption of solvents/chemicals. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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15 pages, 6118 KiB

Open AccessArticle

Tuning Electronic Structure and Magnetic Properties of Flat Stanene by Hydrogenation and Al/P Doping: A First Principle DFT Study

by Mauludi Ariesto Pamungkas, Vinsa Kharisma Rofiqo Sari, Irwansyah, Setiawan Ade Putra, Abdurrouf and Muhammad Nurhuda

Coatings 2021, 11(1), 47; https://doi.org/10.3390/coatings11010047 - 5 Jan 2021

Cited by 10 | Viewed by 2888

Abstract

A Stanene, is a two-dimensional material composed of tin atoms arranged in a single hexagonal layer, in a manner similar to graphene. First principle studies based on density functional theory were performed to investigate the effects of hydrogenation and Al/P doping on electronic structure and magnetic properties of stanene. Hydrogenation opens the bandgap of stanene and changes it from nonmagnetic to the ferromagnetic material through H 1s states and Sn 5p states hybridization. Al/P atom at hollow site prevent electrons of adjacent Sn atoms to connect so that inducing unpaired electrons. The combination of hydrogenation and Al/P doping increases its magnetization. The sequence based on its magnetic moment from small to large is as follows: pure stanene, Al-doped stanene, P-doped stanene, hydrogenated stanene, Al-doped hydrogenated stanene, and P-doped hydrogenated stanene. The controllable transformation from nonmagnetic metallic to a magnetic semiconductor is a key requirement for materials to be used as spintronic materials. Thus, these results may shed light on designing the stanene-based electronic and spintronics materials. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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Review

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19 pages, 4697 KiB

Open AccessReview

Influence of Defects and Heteroatoms on the Chemical Properties of Supported Graphene Layers

by Giovanni Carraro, Letizia Savio and Luca Vattuone

Coatings 2022, 12(3), 397; https://doi.org/10.3390/coatings12030397 - 17 Mar 2022

Cited by 11 | Viewed by 2420

Abstract

A large and growing number of theoretical papers report the possible role of defects and heteroatoms on the chemical properties of single-layer graphene. Indeed, they are expected to modify the electronic structure of the graphene film, allow for chemisorption of different species, and enable more effective functionalisation. Therefore, from theoretical studies, we get the suggestion that single and double vacancies, Stone–Wales defects and heteroatoms are suitable candidates to turn nearly chemically inert graphene into an active player in chemistry, catalysis, and sensoristics. Despite these encouraging premises, experimental proofs of an enhanced reactivity of defected/doped graphene are limited because experimental studies addressing adsorption on well-defined defects and heteroatoms in graphene layers are much less abundant than theoretical ones. In this paper, we review the state of the art of experimental findings on adsorption on graphene defects and heteroatoms, covering different topics such as the role of vacancies on adsorption of oxygen and carbon monoxide, the effect of the presence of N heteroatoms on adsorption and intercalation underneath graphene monolayers, and the role of defects in covalent functionalisation and defect-induced gas adsorption on graphene transistors. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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23 pages, 2735 KiB

Open AccessReview

Two-Dimensional Nanomaterials for Boosting the Performance of Organic Solar Cells

by Zhenbang Wei, Langkun Chen, Kunzhu Liu, Shenghua Liu, Xiangguo Li, Qian Zhang and Jing Shuai

Coatings 2021, 11(12), 1530; https://doi.org/10.3390/coatings11121530 - 13 Dec 2021

Cited by 6 | Viewed by 2836

Abstract

The thin-film organic solar cells (OSCs) are currently one of the most promising photovoltaic technologies to effectively harvest the solar energy due to their attractive features of mechanical flexibility, light weight, low-cost manufacturing, and solution-processed large-scale fabrication, etc. However, the relative insufficient light absorption, short exciton diffusion distance, and low carrier mobility of the OSCs determine the power conversion efficiency (PCE) of the devices are relatively lower than their inorganic photovoltaic counterparts. To conquer the challenges, the two-dimensional (2D) nanomaterials, which have excellent photoelectric properties, tunable energy band structure, and solvent compatibility etc., exhibit the great potential to enhance the performance of the OSCs. In this review, we summarize the most recent successful applications of the 2D materials, including graphene, black phosphorus, transition metal dichalcogenides, and g-C₃N₄, etc., adapted in the charge transporting layer, the active layer, and the electrode of the OSCs, respectively, for boosting the PCE and stability of the devices. The strengths and weaknesses of the 2D materials in the application of OSCs are also reviewed in details. Additionally, the challenges, commercialization potentials, and prospects for the further development of 2D materials-based OSCs are outlined in the end. Full article

(This article belongs to the Special Issue Application of Graphene and Two-Dimensional Materials in Thin Films)

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