Recent Progress in the Synthesis of MoS₂ Thin Films for Sensing, Photovoltaic and Plasmonic Applications: A Review

Abstract

In the surge of recent successes of 2D materials following the rise of graphene, molybdenum disulfide (2D-MoS₂) has been attracting growing attention from both fundamental and applications viewpoints, owing to the combination of its unique nanoscale properties. For instance, the bandgap of 2D-MoS₂, which changes from direct (in the bulk form) to indirect for ultrathin films (few layers), offers new prospects for various applications in optoelectronics. In this review, we present the latest scientific advances in the field of synthesis and characterization of 2D-MoS₂ films while highlighting some of their applications in energy harvesting, gas sensing, and plasmonic devices. A survey of the physical and chemical processing routes of 2D-MoS₂ is presented first, followed by a detailed description and listing of the most relevant characterization techniques used to study the MoS₂ nanomaterial as well as theoretical simulations of its interesting optical properties. Finally, the challenges related to the synthesis of high quality and fairly controllable MoS₂ thin films are discussed along with their integration into novel functional devices.

1. Introduction

Two-dimensional (2D) materials are generally defined as crystalline substances with a few atoms thickness [1]. Graphene was the first 2D crystal to be ever isolated in 2004 and has since been extensively investigated by many groups around the world [2,3,4,5,6]. In fact, graphene became known as the material of superlatives showing a mechanical strength hundreds of times larger than steel [7] while maintaining a high mechanical flexibility [8] and superior electrical and thermal conductivities [9]. Following the discovery of grapheme [10], a very large spectrum of 2D materials possessing a wide range of highly attractive properties have emerged [8,10]. For instance, two-dimensional transition metal dichalcogenide (2D-TMDs) semiconducting (SC) materials have exhibited unique optical and electrical properties [11,12], resulting from the quantum confinement effect attributed to their shapes and sizes with respect to the Bohr radius [13,14,15,16,17], in addition to their surface effects, which is due to the transition from an indirect bandgap in the “bulk form” to a direct bandgap for the “mono- to few-layer” ultrathin film form [18]. The layered configuration of the 2D-TMDs materials is at the origin of their strong interaction with light [19] and the relatively high mobility of their charge carriers [20], which in turn prompted their use in many optoelectronic applications, such as ultra-thin field-effect transistors [21], photo-detectors [22], light emitting diode [23], and solar-cells [24]. Generally, 2D-TMDs form a family of graphite-like layered thin semiconducting structures with the chemical formula of MX₂, where M refers to a transition metal atom (Mo, W, etc.) and X is a chalcogen atom (Se, S, etc.). The layered nature of this class of 2D materials induces a strong anisotropy in their electrical, chemical, mechanical, and thermal properties. In particular, molybdenum disulfide (MoS₂) is the most studied layered 2D-TMD [25,26,27,28,29,30]. From a crystalline point of view, layered MoS₂ exists in three polymorphic crystalline structures: 1T (tetragonal) [31], 2H (hexagonal) [32], and 3R (rhombohedral) [33] (Figure 1). The crystallographic parameters associated to these crystalline forms are summarized in

Table 1. Crystal parameters and the nature of polymorphic structures of 2D-MoS₂.

Polymorphic Structure	Lattice Parameter	Point Group	Electronic Behavior	Ref
1T	a = 5.60 Å, c = 5.99 Å	D6d	Metal	[31]
2H	a = 3.15 Å, c = 12.30 Å	D6h	Semiconductor	[32]
3R	a = 3.17 Å, c = 18.38 Å.	C3v	Semiconductor	[33]

. In the case of mono- to few-layer structures, 2H-MoS₂ is the most thermodynamically stable phase and thus the most commonly encountered. When the MoS₂ is in the monolayer form, it takes an octahedral or a trigonal prismatic coordination phase.

Furthermore, MoS₂ layered materials were observed to exhibit various shapes and morphologies, such as planar [34,35,36] and vertically aligned nanosheets (NSs) [37], nanoflowers [38], nanotubes [39], nanowires [40], and nanoplatelets [41,42]. This variety of forms could be controlled by choosing suitable synthesis routes with optimized operating parameters [38,39,40,41,43,44,45,46,47]. Thus, it is possible to adjust the 2D-MoS₂ properties to develop high performance devices i energy storage [47], electronics [46], photonics [45], sensing [48], and field emission [49] applications. Recently, up to few-layer MoS₂ nanosheets have been shown to be highly efficient for electronic, optoelectronic, and solar energy harvesting devices [50,51,52] because of their tunable direct bandgap [53], strong light-absorption, and prominent photoluminescence with energies lying in the visible range (1.8–1.9 eV) [54].

Although Mo and S are strongly covalently bonded within an individual layer, adjacent sheets are linked together only by the very weak van der Waals interaction. This weak bonding provides a facile processing route such as mechanical or chemical exfoliation to form few- to monolayer MoS₂ films. Unlike graphene, 2D-MoS₂ is much less prone to surface contaminations, which offers a superior chemical stability to 2D-MoS2, making it more attractive for the above-mentioned applications [55,56,57].

This review is timely to report on the state of the art of 2D-MoS₂ from synthesis, properties, and applications viewpoints. It also intends to provide insights on the remaining challenges to widen the applications range of this fantastic 2D-MoS₂ material. It is organized as follows. In Section 2, various fabrication routes are highlighted with a special focus on physical vapor deposition (PVD) methods. Key processing parameters are pinpointed and their influence on the material characteristics, i.e., thickness, crystallinity, morphology, etc., and properties are underlined. In Section 3, relevant techniques used to investigate the complex structure and morphology of 2D-MoS₂ are presented and discussed. In particular, its unique and outstanding optical properties are put forward through theoretical simulations based on the complex permittivity of the MoS₂ monolayer. In Section 4, density functional theory (DFT) calculations were carried out on both the bulk and the monolayer MoS₂ using Quantum Expresso™ code and one-dimensional solar cell capacitance simulator SCAPS-1D™. These calculations were used to determine, respectively, the optoelectronic properties and photovoltaic performances in solar cell configuration. Then, interesting applications in three selected fields where 2D-MoS₂ has shown promising outcomes, namely solar energy conversion, gas sensing, and plasmonics, are presented in Section 5. In the last section, we discuss the reported works and point towards new directions and applications in which 2D-MoS₂ would potentially play a key technological role.

2. Fabrication Techniques of 2D-MoS₂

Tremendous efforts have been devoted to the synthesis of 2D-MoS₂ with controllable large-area growth and uniform atomic layers using both top-down and bottom-up approaches. The most commonly used processing routes are detailed in the following sub-sections along with their advantages and limitations.

2.1. Mechanical and Chemical Exfoliations

Mechanical exfoliation, also known as micromechanical cleavage, is a straightforward technique that takes advantage of the weak bonding between layers, for the production of high-quality mono- to few-layer MoS₂ [58,59,60]. It consists of exfoliating thin films of 2D-MoS₂ from a bulk MoS₂ crystal by using a low surface tension tape to break the weak interlayer bonds in a similar way as for grapheme [61]. Additional exfoliation of the extracted films may be needed to obtain few- to monolayer MoS₂. Tapes could be attached to glass slides to achieve planar exfoliation and slow peeling. The obtained monolayers are usually transferred to an appropriate substrate for further analysis and testing.

The advantage of the mechanical exfoliation process lies in its simplicity that requires the sole use of a confocal microscope to localize the 2D-MoS₂ layers deposited on the substrate. Conveniently, this technique can produce high crystalline quality mono- to few layers with a lateral size up to few tens of micrometers, making them highly suitable for sensing applications. However, this approach suffers from a lack of a consistent control in producing the 2D monolayers as it is heavily user-dependent and does not permit the control of the size and/or thickness uniformity of the exfoliated 2D-MoS₂ layers [62]. Therefore, the mechanical exfoliation technique is not necessarily suitable for the production of 2D-MoS₂ layers intended for large-area and high-throughput applications.

Chemical exfoliation, on the other hand, appears as a promising approach to produce large quantities of mono- and few-layer MoS₂ nanosheets [60,63,64,65]. Eda et al. [54] reported a high yield of monolayer crystal synthesis using chemical exfoliation of bulk MoS₂ via Li intercalation. However, this approach may induce an alteration in the quality of the produced 2D-MoS₂. For instance, the chemically exfoliated MoS₂ layers can lose their semiconducting properties because of the structural changes resulting from the Li intercalation process. However, this fabrication route stands by its ease of processing, low production costs, and suitability for catalysis and/or sensing applications [66].

2.2. Chemical Vapor Deposition

Chemical vapor deposition (CVD) is one of the most popular routes for large-scale, high-quality, and low-cost 2D-MoS₂ material production [49,67,68,69]. CVD is a bottom-up fabrication method at the equilibrium state, which enables the processing of layered 2D-MoS₂ with controlled morphology and good crystallinity while minimizing structural defects. The control of the CVD process is ensured by tuning the deposition parameters such as temperature, pressure, gas flow rate, precursor’s quantities, and substrate types. The 2D-MoS₂ synthesis via the CVD technique can be achieved by means of thermal vapor sulfurization (TVS), thermal vapor deposition (TVD), and thermal decomposition (TD). Deokar et al. [43] used TVS for high quality and vertically-aligned luminescent MoS₂ nanosheets. A similar process could be used to grow 2D-MoS₂ layers [36,70] by employing two sources, such as molybdenum thin film (below 20 nm) or molybdenum oxide (MoO₃) powder deposited on a SiO₂/Si substrate as a first precursor and the sulfur powder or gaseous sulfur source (H₂S, etc.) as the second precursor [49,67,68,69,71,72]. A typical CVD sulfurization process (Figure 2a) is usually performed in a tubular furnace reactor, where a continuous argon flow (typical flow rate 100 sccm) is used as a carrier gas to stream the evaporated sulfur into the Mo source materials.

One of the critical aspects to be controlled in such a CVD tubular reactor is the temperature gradient between the S powder and the substrate. In fact, while the S powder is at 150–200 °C, the substrate’s temperature—with or without Mo thin film—should be maintained in the 700–900 °C range to obtain the 2D-MoS₂ phase. This technique offers sufficient latitude to fairly control the thickness and the homogeneity of the grown 2D-MoS₂. The typical average lateral crystal size obtained by CVD is usually in the 10–30 nm range.

Table 2. Examples of CVD-TVS grown MoS₂ nanostructures.

Substrate	Precursors	Growth Conditions	Morphology	Ref
Si	MoO3 and S powders dispersed on substrate	MoO3 and S powders dispersed on substrate at 850 °C; S powder at 400 °C; Ar-0.725 L/min; time reaction = 30 min	MoS2 nanosheets	[43]
Si [001]	S powder and Mo film deposited on substrate	Mo deposited on Silicon at 850 °C, S at 400 °C; Ar-0.725 L/min; time reaction = 30 min	MoS2 nanosheets	[44]
Si/SiO2	S powder and Mo film deposited on substrate	Mo deposited on Silicon at 850 °C, S at 400 °C; Ar-0.725 L/min; time reaction = 30 min	MoS2 nanosheets	[49]
Diamond substrate	S powder and Mo deposited on substrate	Mo deposited on Silicon with S powder at 800 °C; N2; ambient pressure; time reaction = 30 min	Horizontally and vertically MoS2	[73]
Si/SiO2	S powder and MoO3 deposited on substrate	MoO3 film deposited on Silicon at 750–850 °C, 600 mg of S powder at 100 °C; Ar-0.01 L/min; time reaction = 10 min	Mono-to few-layers of MoS2	[74]

shows few examples of CVD-TVS grown MoS₂ nanostructures along with their associated processing conditions.

Table 2 shows the typical morphologies obtained for MoS₂, which seem to depend on the carrier gas and the type of the substrate used. The reaction time and the spatial position of the substrate strongly affect the number of resulting layers.

The TVD based MoS₂ growth (Figure 2b) involves the concomitant evaporation of both MoO₃ and S powders. This approach consists of a stepwise sulfurization of MoO₃ to form the MoS₂ phase. It has been shown that, by increasing the S vapor flux, the sulfurization proceeds through several phase changes before reaching the final product. First, MoO₃ is formed, then MoO₂ followed by MoOS₂, and finally MoS₂. This approach is very useful to obtain 2D MoS₂ layers with a lateral size of few tens of microns. The TVD growth conditions of MoS₂ under various conditions and with different characteristics are summarized in

Table 3. Examples of TVD grown MoS₂ along with their relevant processing conditions (* D is the distance between the MoO₃ and $S$ powders inside the tubular furnace).

Substrate/Setup	MoO3 (mg)	S (mg)	D * (cm)	Gas, Flow (sccm)	T (°C), Time (min)	Morphology	Ref
Si face-down	15	80	18	Ar 10 to 500	700, 30	Flake size between 5.1–47.9 µm	[75]
SiO2/Si face-up	10	200	30	Ar, 100	850, 20	Monolayer, bilayer and trilayer MoS2	[76]
SiO2/Si face-down	10	100	–	N2, 20	650, 20	MoS2 monolayer	[77]
SiO2/Si face-down	10-30	–	25	Ar, 150	800, 10	MoS2 triangular flakes	[78]
SiO2/Si face-up	50	175	–	N2, 300	750, 15	MoS2 monolayer with lateral size of 50 µm	[79]

.

In comparison to the results obtained by CVD-TVS summarized in Table 2, TVD exhibits high-yield fabrication of 2D-MoS₂ monolayers generally exhibiting a triangular flakes shape. Besides, one can notice the two possible configurations of the substrate of interest in TVD face-up and face-down compared to CVD-TVS [75,76,77,78,79].

Moreover, the TD-based CVD method presents an alternative approach to produce highly crystalline MoS₂ thin layers with superior electrical properties on insulating substrates [34]. Typically, the TD-CVD is based on the high-temperature annealing of a thermally decomposed ammonium thiomolybdate layer (NH₄)₂MoS₄ in the presence of S, as illustrated in Figure 2c. It is worth noting that the excess in sulfur introduces changes in the shape, size, and morphology of fabricated MoS₂. It also leads to a p-type MoS₂ semiconductor by increasing the electrons deficiency. In contrast, the presence of sulfur vacancies in MoS₂ was reported to have a direct impact on the catalytic properties of MoS₂, suggesting a carriers’ mobility alteration [80]

Besides, the addition of S during the high-temperature annealing drastically enhances the crystallinity of MoS₂. Relatively, centimeter-sized MoS₂ crystals could be formed on Al₂O₃ substrates compared to SiO₂ ones [35]. The fully covered Al₂O₃ substrate with an epitaxial monolayer of MoS₂ was achieved at 930 °C. The MoS₂ crystals nucleate in a single domain to pursue by domain-to-domain stitching process occurring during annealing at 1000 °C mediated by the oxygen flow. The difference in the self-limited monolayer growth observed between the SiO₂ and Al₂O₃ substrates is related to the absorption energy barrier on MoS₂ [37]. In particular, the growth of MoS₂ on Al₂O₃ obeys the surface-limited epitaxial growth mode, which is not the case for the SiO₂ due to lattice mismatch. Moreover, the patterning of the as-grown MoS₂ layers has been reported by means of the polydimethylsiloxane (PDMS) stamps and the reuse of the substrate after transferring the MoS₂ layers [35]. Recently, the epitaxial growth of centimeter wafer-scale single-crystal MoS₂ monolayers on vicinal Au (111) thin films were also obtained at a processing temperature of 720 °C, by melting and re-solidifying commercial Au foils [36]. This allows overcoming the evolution of antiparallel domains and twin boundaries, leading to the formation of polycrystalline films. It has been proposed that the step edge of Au (111) induced the unidirectional nucleation, growth, and subsequent merging of MoS₂ monolayer domains into single-crystalline films.

2.3. Atomic Layer Deposition

The atomic layer deposition (ALD) technique is known to produce high-quality thin films even at low temperatures, typically between 150 and 350 °C. Since ALD is an atom stepwise growth process, where the reactants are alternately injected into the growth area, it allows the purging of excess species and by-products after each reaction. As a result, high-quality films are obtained by sequential surface reactions. A schematic representation of the ALD synthesis of 2D-MoS₂ can be found elsewhere [81].

Despite the challenges related to its synthesis conditions, ALD makes it possible to deposit crystalline MoS₂ thin films at a relatively low temperature (<350 °C) followed by annealing. For instance, L.K. Tan et al. [82] reported the possibility to use ALD for the synthesis of highly crystallized MoS₂ films on sapphire substrates at 300 °C. They prepared MoS₂ films by alternating exposure of the substrate to Mo(V) chlorides (MoCl₅) and hydrogen disulfide (H₂S) vapors. Similarly, Mattinen et al. [83] proposed the use of a Mo based precursor, namely Mo(thd)₃ (thd = 2,2,6,6 tetramethylheptane 3,5-dionato), with H₂S as a sulfur source. They have been able to achieve a self-limiting growth and a linear film thickness control (with a very low growth rate of ≈0.025 Å per cycle). While the crystallinity of these MoS₂ films was found to be particularly good (taking into account that the deposition was done at a low temperature), their surface was rather rough, consisting of flake-like grains with a size of ≈10–30 nm. One of the advantages of this process is the possibility to deposit layered MoS₂ films on various substrates.

Table 4. Summary of the ALD deposition conditions and achieved MoS₂ film thicknesses.

Substrate	Precursors	P (Torr)	T (°C)	Cycles	Thickness	Ref
SiO2/Si	Mo hexacarbonyl and dimethyldisulfide	1.4–3.3	100	100	≈11 nm	[84]
SiO2/n-Si	MoCl5 and H2S	0.75	350–450	100	≈9 nm	[85]
Al2O3	Mo(NMe2)4 and H2S	–	60	100	≈12 nm	[81]
Al2O3 2-inch wafer	MoCl5 and H2S	0.001	300	50	≈9 nm	[82]
SiO2/Si	Mo(thd)3 (thd = 2,2,6,6 tetramethylheptane 3,5-dionato) and H2S	3.75	300	100	≈25 nm	[83]
Al2O3 c-plane	MoCl5 and hexamethyldisilathiane	3.75	350	250	≈22 nm	[86]
Carbon nanotubes, Si-wafers and glass	bis(tbutylimino)bis(dimethylamino) Mo (VI) and H2S	300	100–250	100	≈11 nm	[87]
Si, SiO2, Al2O3	MoCl5 and H2S	3.75	430–480	1	1 layer	[88]
Si	MoCl5 and H2S	–	390–480	100	≈21.5 nm	[89]
SiO2	Mo hexacarbonyl and H2S	–	175	100	≈5 nm	[90]

summarizes the main processing conditions used by different groups along with the achieved MoS₂ film thicknesses.

The ALD appears as a potentially interesting technique for the production of high-quality MoS₂ ultrathin films at relatively low temperatures and with the ability to achieve excellent step coverage onto different substrates. However, the very low throughput of the ALD might hinder its scalability and competitiveness in comparison with other physical and/or chemical deposition methods.

2.4. Pulsed Laser Deposition

Pulsed laser deposition (PLD) has emerged as one of the most promising physical vapor deposition (PVD) techniques for the deposition of MoS₂ thin films. The PLD approach consists of shining a focused high-power laser beam onto the surface of a solid target to be ablated and deposited as a film on a substrate. PLD is a non-equilibrium process that leads to the absorption of very-short (15–20 ns) and highly-energetic laser pulses by the target and to the formation of a directive plasma plume. The laser-ablated species that form the plasma plume condense onto the substrate, leading to the growth of a thin film. The PLD is well known for its large process latitude, high-flexibility, and excellent process controllability. For instance, by controlling the number of laser ablation pulses and/or the background gas pressure, nanoparticles, and/or films with thicknesses varying from few nm to few microns can be synthesized. Figure 3 shows a schematic representation of a PLD system.

Among the advantages and the unique features of the PLD method, we can cite: (i) its ability to achieve a congruent transfer to the films when a multi-element target is used [91]; (ii) its highest instantaneous deposition rate along with the highly-energetic aspect of the ablated species (~10 times higher than in sputtering) enables the growth of metastable phases and/or crystalline phases even at room temperature; and (iii) its process latitude, which makes it easy to control almost independently each of the deposition parameters (laser intensity, number of laser ablation pulses, background gas pressure, and substrate temperature), and hence the properties of the deposited materials [92,93,94]. While the early studies on the PLD of MoS₂ date back to the 1990s [95,96,97,98,99,100], it is only recently that important advancements have been made in PLD synthesis of 2D-MoS₂ films onto various substrates opening thereby the way to their use for different optoelectronic applications. In 2014, PLD was successfully used to grow one to several layers of MoS₂ onto different metal, semiconducting, and sapphire substrates [101,102]. Siegel et al. [103] were the first to report, in 2015, the growth of MoS₂ films (from 1 to a few 10s of monolayers thick) on centimeter-sized areas. Other attempts were made to deposit ultrathin (≤3 nm) films of nearly-stoichiometric amorphous MoS₂ onto irregular surfaces such as silicon and tungsten tips and to study their field electron emission (FEE) properties [95]. The authors stated that the addition of the MoS₂ coating is beneficial to the FEE process since lower electric fields were required to extract an electron current density of 10 μA/cm² (namely, 2.8 V/μm for MoS₂-coated Si and ~5.5 V/μm for MoS₂-coated W tips). More recently, PLD has been used to fabricate high-quality MoS₂ films (monolayer to few layers) and integrated them into functional ultraviolet (UV) photodetectors [104]. The developed photodetectors were found to exhibit a very low dark current (~10 × 10⁻¹⁰ A), low operating voltage (2 V), and good response time (32 ms). Their performance surpassed that previously reported for 2D-MoS₂ synthesized by other routes [105,106,107,108,109]. Indeed, under UV irradiation, their detectivity, photoresponse (I_on/I_off ratio), and responsivity were found to be as high as 1.81 × 10¹⁴ Jones, 1.37 × 10⁵, and 3 × 10⁴ A/W, respectively.

Table 5. Summary of the PLD conditions of MoS₂ films along with their thickness and some of their properties.

Substrate	Target	P(Pa)	T(°C)	Laser Energy	Thickness	Properties	Ref
Stainless steel	MoS2	2.66 × 10−6	RT/200/300/450	5 mJ	≈400 nm	Granular structure stoichiometric, crystalline MoS2	[110]
Stainless steel	MoS2	10−6	RT/300	100 mJ	≈70 nm	Stoichiometric single crystal MoS2	[111]
c-Al2O3 (0001) and Si/SiO2	2H-MoS2	9.33 × 10−4	600	500 mJ/cm2	≈1.4 nm	Stoichiometric 2H phase Flake size ≈ 10 µm	[112]
GaN/c-Al2O3 (0001)	2H-MoS2	8 × 10−4	700	50 mJ	Few layers	Mixed phase Roughness ≈0.11 nm	[102]
Titanium foil	p-MoS2	1.33 × 10−2	RT	–	0.65 nm	1T phase MoS2	[113]
SiO2 on Si [100]	MoS2	1.33 × 10−2	800	200 mJ/cm2	≈20–60 nm	2H phase MoS2	[104]
Gold-coated carbon cloth	Amorphous MoS2	1.33 × 10−2	RT	220 mJ/cm2	≈200 nm	2H phase MoS2	[97]
Quartz	MoS2	9 × 10−5	300	8500 mJ/cm2	30 layers	Mixed phase	[114]
Al2O3 (0001)	MoS2+S Powder	1.33 × 10−2	700	50 mJ	1–15 Layers of MoS2	p-MoS2 2H phase MoS2 Roughness of 0.27 nm	[101]
Si	MoS2	4 × 10−4	RT	5/10/100/400 mJ/cm2	≈100–200 nm	Various compositions of MoSx (x ≤ 2.2)	[115]
SiO2	MoS2	3 × 10−5	700	200 mJ	1–5 layers	2H phase MoS2	[116]
W (100)-tip	MoS2+poly(vinl)	5 × ${10}^{-3}$	700	2000 mJ/cm2	≈20–60 nm	nearly stoichiometric 2H phase MoS2	[95]
n-Si and p-Si	MoS2+poly(vinl)	5 × ${10}^{-3}$	700	500 mJ/cm2	≈20–60 nm	nearly stoichiometric 2H phase MoS2	[95]
Al, Ag, Ni, Cu	MoS2	2.6 × 10−5	500	50 mJ	≈5 nm	Epitaxial growth of 2H phase MoS2	[98]
Sapphire Quartz SiO2 HfO2	MoS2 +S powder	1.33 × 10−2	700	30 mJ	1 monolayer—2.8 nm	large-area growth of stoichiometric layered 2H phase MoS2	[117]
SiO2/Si	MoS2	10−5	700	200 mJ	few-layer	2H phase MoS2	[118]
SiO2/Si	MoS2 powder	5 × 10−4	600	2200 mJ/cm2	13 nm	Epitaxial growth of 2H phase MoS2	[119]
Si	MoS2	10−4	RT	100 mJ	129–1900 nm	Stoichiometric films	[120]
c-plane sapphire	MoS2	10−3	800	2000–3000 mJ/cm2	1–5 layers	Epitaxial growth of 2H phase MoS2	[121]
Quartz glass	Polycrystalline MoS2 powder	5 × 10−4	300	8500 mJ/cm2	9–10 monolayers	nearly stoichiometric 2H phase MoS2	[122]
Quartz	MoS2	8.9 × 10−5		600 mJ	≈5.8 nm	2H phase MoS2	[123]
SiO2/Si	MoS2@Ag	1.33 × 10−7	500	1000–2000 mJ/cm2	≈1.3–12.8 nm	2H phase MoS2	[124]
fluorophlogopite mica	MoS2	10−5	700	4000 mJ/cm2	≈3.3 nm	2H phase MoS2	[125]
Al2O3 (0001)	MoS2	10−3	650	100 mJ	≈400 nm	2H phase MoS2	[126]

summarizes most of the papers reported so far on the PLD of MoS₂ films. More specifically, it compares the main PLD growth conditions of 2D-MoS₂ films along with the obtained crystallographic phase and some of the reported optoelectronic properties.

2.5. Other Processing Routes

In addition to the main fabrication methods presented above, other PVD techniques have been used to deposit 2D-MoS₂ films. Among these methods, magnetron sputtering has been used to deposit both MoS₂ and WS₂ films onto polydimethylsiloxane (PDMS) polymer substrates [37,127,128,129,130] with controllable defect densities. The PDMS substrate was chosen to fabricate flexible devices based on 2D-semiconducting materials. Interestingly, very smooth MoS₂ surfaces, with a roughness of less than 2 nm, were achieved by casting the polymer on a polished silicon wafer. It has also been shown that it is possible to induce subsequent crystallization of MoS₂ by exposing it to a pulsed 532 nm laser [127].

Finally, the use of any of the above-discussed techniques to fabricate 2D-MoS₂ films is mostly dictated by the availability of the equipment, expertise, and requirements of targeted application. In a general context, the physical-chemical and optoelectronic properties of the final MoS₂ films will be determined to select the appropriate synthesis route. Nevertheless, the level of complexity, throughput, and fabrication costs have to be considered to choose the appropriate synthesis technique particularly when a technology has to be adopted.

Table 6. Comparison of the advantages and limitations of different preparation techniques of MoS₂.

Techniques	Advantages	Limitations
Mechanical exfoliation	- High-quality and good crystallinity. - Mono- to few-layer MoS2 - Simple process	- Long processing time (8–84 h) - Tedious and no controllability - Difficult integration with micro/optoelectronic processing
Chemical exfoliation	- Large-scale growth - Synthesis of MoS2 monolayer	- Loss of semiconducting properties of MoS2 during Li intercalation.
Chemical vapor deposition	- High-quality and crystallinity - Centimeter-scale area growth - Good control of morphologies	- Caution due to the use of toxic precursors - High synthesis temperatures requirement - No lateral uniformity - Mixed phases of 1T, 2H, etc.
Atomic layer deposition	- Low-temperature deposition - Uniformity of MoS2 films - High quality of uniformity - Excellent step coverage	- Very low throughput - Long processing time - High cost
Pulsed laser deposition	- High-quality and faithful transfer of film stoichiometry - Nanometer-level control of the film thickness - Uniformity onto a large surface (up to 3” or 4” diameter wafers) - Quasi-independent control of the growth parameters. - Room-temperature deposition of crystallized MoS2 - Compatibility with electronic and optoelectronic device processing	- Relatively costly - Presence of ablated particulates on the surface
Sputtering	- High quality and uniformity onto large surface - Compatibility with electronic and optoelectronic device processing. - Fair thickness control	- Relatively costly - Preferential sputtering - Less control on the stoichiometry

provides a general comparison of the preparation techniques of MoS₂ described in this review by listing their main advantages and limitations.

3. Characterizations of MoS₂ Thin Films

To assess the crystalline quality, microstructure, and optoelectronic properties of the synthesized 2D-MoS₂, a variety of characterization techniques have been employed and reported in the literature. These include optical microscopy (OM), scanning electron microscopy (SEM), high-resolution transmission and Scanning transmission electron microscopy (HRTEM and HRSTEM), atomic force microscopy (AFM), energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and photoluminescence (PL). These methods are often used to investigate the overall 2D-MoS₂ surface topography and to qualify the nature of the synthesized material and the shapes of its building blocks (i.e., triangle, nanosheets, and nanoplates) (Figure 4). The observations made by imaging methods are also essential to envision a possible growth mechanism of the micro/nanostructures with respect to the used processing parameters. For instance, Figure 4d shows a schematic representation of the nucleation process of some morphologies of 2D-MoS₂.

Subsequently, HRTEM investigations could be carried out to precisely characterize the MoS₂ crystalline structure and examine locally its lattice parameters and the presence of defects. In particular, the HRTEM image depicted in Figure 4e is of great importance, as it was recorded in cross-region containing the two possible crystal configurations of MoS₂. As it can be seen in Figure 4e–g, the identified phase mixture of 1T@2H-MoS₂ could coexist simultaneously in the same fabricated MoS₂ thin film [131].

AFM and its variant methods constitute key characterization tools for the investigation of 2D crystals, mainly due to the atomically thin nature of this layered class of materials. Both vertical and lateral resolutions are fundamentally required to properly investigate the intrinsic properties of 2D materials. AFM is among the few techniques that allow the characterization of 2D-MoS₂ in ambient and controlled environments at the nanometer scale. In addition to measuring the local thickness and surface topography, AFM-based electrical methods provide access to additional interesting properties such as the local variations in surface potential of 2D-MoS₂. For instance, the Kelvin probe force microscopy (KPFM) method allows the characterization of the sample’s surface work function variations. The work function is an extreme surface property, which depends on the energy differences between the Fermi and vacuum levels at the surface. This renders the use of KPFM for the characterization of 2D-MoS₂ fundamentally important to investigate band alignments in nanostructures and to study the dependencies of local electronic properties on the number of 2D-MoS₂ layers. It also provides key insights into the environmental effects on the state of the sample surface both electronically and morphologically. The KPFM technique was used (Figure 5a) to determine the surface potential variations in mono- and multilayer MoS₂, under different humidity conditions.

X-ray photoelectron spectroscopy (XPS) is another relevant surface characterization technique that is widely used to achieve the elemental surface composition of MoS₂ films as well as their chemical bonding states. Figure 5b shows typical high-resolution XPS spectra of the Mo_3d and S_2p core levels. The Mo_3d region exhibits two characteristic emission peaks at 232.5 (Mo 3d_3/2) and 229.4 (Mo 3d_5/2) eV. These binding energy values are consistent with electrons of Mo⁴⁺⁺ corresponding to MoS₂. Likewise, the S 2p_3/2 and S 2p_1/2 doublet appearing at binding energies of 162.3 and 163.5 eV is typical for S^2- in MoS₂ structure. Nan et al. [132] used XPS to show the PL enhancement of monolayer MoS₂ through defect engineering and oxygen bonding. The chemical adsorption of oxygen created a heavy p-type doping and the conversion of the Trion into Excitons. Moreover, it caused the suppression of the non-radiative recombination of the excitons at the defect sites. Their results were verified by PL measurements at low temperature, as shown in Figure 5c,d.

Unlike bulk MoS₂, the ultrathin 2D-MoS₂ (i.e., one to few layers) exhibits a strong PL intensity which increases with reducing the number of layers [136], which has been attributed to quantum confinement effects [53,137]. The PL response can be tuned via several mechanisms including doping [134], plasmonic effect, and defects engineering [132]. For instance, Mouri et al. [134] studied the influence of the thickness on the PL response of MoS₂ by using mono-, bi-, and trilayer MoS₂ and the PL modulation using doping. They demonstrated that p-type doping with high electron affinity seems to enhance the PL intensity, while the n-type doping tends to reduce it, as illustrated in Figure 5c,d.

Moreover, Raman spectroscopy presents a very sensitive, fast, and non-destructive technique to access valuable information on the chemical structure, phase and polymorphs, crystallinity, and chemical bonding states of 2D-MoS₂ materials. It allows the monitoring of the two characteristic peaks of MoS₂, namely the in-plane and out-of-plane vibration modes E¹_2g and A¹_g appearing for 514 nm excitation energy at the respective positions of 384.5 and 404.6 cm⁻¹ for 2D-MoS₂ monolayer [135] (Figure 5e). More interestingly, the difference between the peak positions of E¹_2g, A¹_g (Δω) can be used as a robust and effective diagnostic to determine the number of MoS₂ layers (up to four layers) or to simply estimate the MoS₂ film thickness (Figure 5f). Usually, Δω is less than 20 cm⁻¹ in the presence of a single layer of MoS₂, but it increases with increasing MoS₂ thickness to reach 25 cm⁻¹ for the bulk MoS₂ [135]. In fact, a thorough study on the dependence of the characteristic Raman peak positions, width, and intensity of MoS₂ films on their thickness have been investigated [103,135,138]. Furthermore, H. Li et al. [138] reported that the frequency of the characteristic peaks is strongly dependent on the excitation energy due to the resonance effect. They showed a red shift of the E¹_2g mode of about 2.2 cm⁻¹ and blue shift of the A¹_g mode of about 4.1 cm⁻¹. Thus, to effectively determine the exact MoS₂ number of layers using Raman spectroscopy, one has to consider the excitation energy and the thickness limit at which the Raman vibrations frequency is reaching a plateau, indicating that it is less sensitive to MoS₂ thickness variation above four layers.

4. Band Structures and Electronic Properties

We employed density functional theory (DFT) to determine the optoelectronic properties in particular the bandgap energy of both bulk and monolayer MoS₂. Perdew–Burke–Ernzerhof (PBE) approach was applied to describe the electronic states of MoS₂ using band structure and the density of states (DOS). DFT calculations were implemented in Quantum Espresso™ code [139,140]. The considered 2H-MoS₂ has a hexagonal crystal form with the space group P63/mmc (No. 194). The equivalent positions for this structure employed in the calculations are Mo (1/3, 2/3, and 2/8) and S (1/3, 2/3, and 0.621). The valence electron configuration selected for Mo and S atoms are 4p⁵ 5s¹ and 3s² 3p⁴, respectively. The cutoff wave function and the cutoff charge densities are 70 and 700 Ryd, respectively [140]. The cell parameters and atomic positions were fully relaxed by the process of the total energy minimization. The values of the relaxed lattice constants for bulk MoS₂ are a = 3.15 Å and c = 12.3 Å, respectively. The optimized structure was used to perform calculations for band structures and the total density of states for both MoS₂ bulk and monolayer. For bulk MoS₂ (top left panel of Figure 6a), 9 × 9 ×2 k-points were used to obtain the band structure along the path Γ-K-M-Γ in the Brillouin zone. For MoS₂ monolayer (top right panel of Figure 6a), 9 × 9 × 1 k-points were used. A 15 Å vacuum along the z-axis above the monolayer was added to isolate the MoS₂ and prevent any interaction between the adjacent layers [141]. The top view of the MoS₂ monolayer is shown in the bottom panel of Figure 6a, where sulfur atoms are represented in yellow and molybdenum atoms are shown in purple.

To obtain the electronic properties, the MoS₂ bulk was considered as a set of two hexagonal planes linked together by weak Van Der Waals bonds. The MoS₂ monolayer was considered as a single hexagonal plane with covalent bonds between atoms S-Mo-S [142]. The left panel of Figure 6b shows the total DOS calculation results of the bulk MoS₂ while the right panel of Figure 6b shows the calculation of its band structure. The energy range is between −8 and 4 eV versus the directions of the highest symmetries in the first Brillouin zone Γ, M, K, and Γ. As observed from the band structure calculations, the MoS₂ bulk has an indirect bandgap of 0.9 eV. The minimum of the conduction band is located between K and G and the maximum of valence band at point G. This indirect bandgap obtained for the MoS₂ bulk was attributed to the presence of interlayer interactions in the bulk structure [143]. In contrast, Figure 6c shows that the monolayer MoS₂ has a direct bandgap of 1.89 eV at the K point. The DOS results are compatible with the results of the band structure. Similar conclusions have been stated in other investigations [141,142].

5. MoS₂ Applications

Because of their attractive optoelectronic properties, possibly tunable by for example controlling the number of monolayers, MoS₂ thin films were tested and validated for a variety of applications including electronics, photonics, solar energy, and energy storage. Here, we give a few examples of some specific successful and promising applications of MoS₂ films for solar energy conversion [144,145], gas sensing [44,48,146,147], and plasmonics [148,149,150,151,152].

5.1. MoS₂ for Solar Energy Harvesting

As demonstrated by DFT calculations, 2D-MoS₂ exhibits interesting optoelectronic properties attributed to its direct bandgap ranging from 1.2 to 1.9 eV and an absorption coefficient greater than 105 cm⁻¹ throughout the solar spectrum. These key properties are very promising for the use of MoS₂ in photovoltaic (PV) applications. Indeed, it has been shown that, when a monolayer of n-type MoS₂ is deposited onto a p-type silicon substrate, the resulting p-n junction based PV device is able to yield a power conversion efficiency (PCE) as high as 5.23%, as recorded elsewhere [153]. Such a PV performance is most likely a consequence of the excellent ability of MoS₂ to efficiently separate the generated photo-charges at the n-MoS2/p-Si interface of the heterojunction.

To highlight the electrical performance of thin films MoS₂-based solar cells in a homojunction form, we used the one-dimensional solar cell capacitance simulator SCAPS-1D™ software 3.3.08 interface [154], developed by M. Burgelman – Department of Electronics and Information Systems at the University of Ghent, Belgium [155,156], to calculate the different PV parameters, i.e., open circuit voltage V_OC, short-circuit current density J_SC, fill factor FF, and PCE (η). In this sense, a solar cell made of Ag/p-Si/MoS₂/Al structure, as the one represented by a schematic in Figure 7, was implemented in the SCAPS-3308™ environment.

The simulations were made under AM1.5 illumination conditions at an operating temperature of 300 K. The physical parameters related to the electronic properties of the layers used in the simulation are shown in

Table 7. Physical parameters of n-MoS₂ monolayer and p-Si substrate used in the SCAPS-1D™ simulations.

Parameters	p-Si [SCAPS]	n-MoS2
Thickness (nm)	200	0.32
Bandgap (eV)	1.12	1.9 [153]
Electron affinity (eV)	4.5	4.2 [153]
Dielectric permittivity (relative)	11.9	10.5 [157]
CB effective density of states (1/cm3)	2.8 × 1019	2.2 × 1018 [158]
VB effective density of states (1/cm3)	1.04 × 1019	1.8 × 1019 [158]
Electron thermal velocity (cm/s)	1 × 107	1 × 107 [159]
Hole thermal velocity (cm/s)	1 × 107	1 × 107 [159]
Electron mobility (cm2/Vs)	1500	150 [20]
Hole mobility (cm2/Vs)	4500	86 [159]
Shallow uniform donor density (1/cm3)	0	1 × 1017 [159]
Shallow uniform acceptor density NA (1/cm3)	1 × 1016	0

. For the considered junction, the thermal speed of the electrons and the holes were fixed at 10⁷ cm/s, the type of defect is neutral, and the capture cross section is 10⁻¹⁴ cm².

Beyond, the input parameters used in our SCAPS simulations, we provide hereinafter a survey of commonly used physical parameters of MoS₂ reported in the literature to simulate the performance of MoS₂ in PV applications. As can be seen in

Table 8. A survey of the physical parameters of MoS₂ used for the simulation of photovoltaic applications.

PV Parameters	Reported Values and References
Bandgap	1.29 eV [158,160,161]	1.2–1.8 eV [159]	1.23 eV [162]	1.8 eV [163]
Electron affinity	4.2 eV [158,160,161,162,163]	4–4.7 eV [159]	4.22 eV [163]	–
Relative dielectric permittivity	3 [164]	4 [160,161,162]	7 [159]	13.6 [158]
Effective density of states in conduction band	1016 cm−3 [163]	7.5 × 1017 cm−3 [160,162]	2.2 × 1018 cm−3 [158,161]	1019, 2.5 × 1020 cm−3 [159,164]
Effective density of states in valance band	1017 cm−3 [163]	1.8 × 1018 cm [160,162]	~1019 cm−3 [158,161,164]	2.5 × 1020 cm−3 [159]
Electron thermal velocity	105 cm/s [162]	2.12 × 107 cm/s	–	–
Hole thermal velocity	107 cm/s [162]	1.18 × 107 cm/s [161]	–	–
Electron mobility	44 cm2/Vs [159]	50 cm2/Vs [161]	100 cm2/Vs [158,160,162]	–
Hole mobility	30 cm2/Vs [161]	86 cm2/Vs [159]	150 cm2/Vs [158,160,162]
Shallow uniform donor density	1016 [161]	1017 [164]	1018 [162]	–
Shallow uniform acceptor density	10 cm−3 [161]	1017 cm−3 (MoS2 type P) [158]	1021 cm−3 (MoS2 type P) [160]	–

, several combinations are possible which may yield different results.

The outcome of our simulations shows that the p-Si/n-MoS₂ structure in Figure 7 can yield a PCE value as high as 19.82% when considering 2D-MoS₂ with the highest bandgap of 1.9 eV. Figure 8 shows the simulated J-V curve of the p-Si/n-MoS₂ cell along with its associated PV parameters. The rather high V_oc value of 0.64 V reflects the strong built-in electrical field at the interface between the n-MoS₂ layer and p-Si substrate.

The high PCE obtained is comparable to the one obtained for well-proven solar cell materials. This is an outstanding yield for an only 0.33 nm thick material used in conjunction with p-Si in the solar cell set up as compared to 250 µm thickness used for conventional Si technology. Moreover, sulfur and molybdenum are abundant and cheaper raw materials as compared to the technologies achieving similar performances such as III-V materials.

Nevertheless, although the simulated PCE performance underlines the great potential of 2D-MoS₂ films for PV devices, other challenging issues still need to be addressed or mitigated to develop such devices. For instance, the controlled deposition of MoS₂ monolayer, the achievement of a reliable metal contact on MoS₂ monolayer free of leakage current or a shortcut with the underlying Si substrate, and the scalability of 2D-MoS2 ultrathin films to the well-established large-size Si wafer technology are among the challenging issues to be addressed in future works.

5.2. MoS₂ for Gas Sensing Applications

MoS₂ nanosheets (NS) have been reported to exhibit enhanced gas sensing performances for a variety of gases, including toxic and hazardous gases such as ammonia (NH₃) and nitrogen dioxide (NO₂) [43,48,146,165,166,167]. Thus, MoS₂ NS act as a simple chemiresistor that changes its electrical resistance when in contact with reactive gases. The sensing response or sensitivity (S) towards a target gas, at a given operating temperature, is determined from the measured values of resistances of the MoS₂-NS sensing element in the presence of atmospheric air resistance (R_a) and target gas (R_g). Usually, the target gas molecules adsorb onto the MoS₂ NS exposed edges and changes its conductivity through the donor/acceptor exchanges process. The sensitivity (S) is defined as follows:

$$S=\frac{R_a-R_g}{R_g}$$

To design an effective 2D-MoS₂ gas sensor, care must be taken to the optimization of its operating temperature, response/recovery times, and selectivity. 2D-MoS₂-based gas sensors were found to offer certain advantages, such as high-temperature stability, high resistance to a corrosive environment, and high sensitivity [26,146,165,166]. In addition, 2D-MoS₂ thin film-based sensors were reported to detect NH₃ triethylamine (TEA) molecules at the sub-ppm level, at an operating temperature as low as 30 °C [147].

MoS₂ thin films obtained by mechanical exfoliation were used for highly sensitive field-effect transistor (FET) sensors [147]. By varying the number of MoS₂ layers, the MoS₂-based FET sensor exhibited high nitrogen monoxide (NO) sensitivity with a detection limit of 0.8 ppm. Moreover, DFT calculations indicated that NO and NO₂ seemed to strongly bind to MoS₂ nanosheets in contrast to other molecules such as carbon monoxide (CO), carbon dioxide (CO₂), NH₃, NO, NO₂, and CH₄. In addition, the exfoliated MoS₂ monolayer showed high response to triethylamine (TEA) at concentrations ranging from 1 to 100 ppm at room temperature (Figure 9a). Due to the strong response and excellent signal-to-noise ratio, a detection limit of TEA as low as 10 ppb was achieved.

Furthermore, exfoliated few-layer MoS₂ nanosheets deposited on a substrate with interdigitated electrodes demonstrated good NO₂ detection performances at room temperature [168]. The reported device shows a quick and complete recovery time of 2 s at a rate greater than 97%. Similarly (Figure 9b), DFT calculations indicated that the fairly fast recovery of MoS₂ arises from the weak van der Waals interactions between NO₂ and the MoS₂ surface.

It is worth mentioning that, regardless of their form or morphology, MoS₂ thin films remain as robust gas sensors. Indeed, atomic layered MoS₂ fabricated by CVD showed excellent sensitivity and high selectivity once exposed to NH₃ and NO₂ [169]. The resistance of the MoS₂ films increases in the case of NO₂ adsorption, while it decreases for the NH₃ adsorption. The recovery rate of NO₂ is higher at 100 °C than at room temperature, while the NH₃ sensing signal is negligible at 100 °C. To further exploit the large affinity of NO₂ with MoS₂ thin films, MoS₂ hexagonal-shaped nanoplates (HNPs), with exposed edges allowing significant charge transfer, were grown on the top 20 nm of carbon nanotubes (CNTs). This configuration is advantageous to increase both the surface area and the number of sites for gas adsorption. The hybridization of MoS₂ by deposition on CNTs showed an enhanced room-temperature gas-sensing performance [42], attaining a detection limit of a few ppb of NO₂ concentration.

5.3. MoS₂ for Plasmonic Applications

Because of their optical bandgap spread, MoS₂ thin films offer interesting opportunities to be coupled with noble metal nanoparticles (NPs) in order to exacerbate the plasmonic properties. Indeed, the coupling effects between the excitons from MoS₂ with the plasmons generated within the metal NPs open various prospects for tunable light emitters and absorbers over a wide spectrum. Various MoS₂-related plasmonic structures have been developed for different optoelectronic applications, including photodetection [152], photoluminescence modulation [150], photocatalysis [170,171], and photovoltaics [172].

To better understand the origin of the enhancement in light emission/absorption properties of MoS₂/metal-NPs hybrid structures, it is necessary to comprehend and estimate the variation of 2D-MoS₂ complex permittivity. A mathematical approach based on hybrid Lorentz–Drude–Gaussian (HLDG) model was proposed by Mukherjee et al. [173] to describe the complex permittivity of MoS₂ monolayer based on its absorption spectrum (Figure 10a).

The HLDG model can be presented as follows:

$${\mathsf{\epsilon }}_c={\mathsf{\epsilon }}_c^{LD}+{\mathsf{\epsilon }}_c^G,$$

where the superscripts LD and G correspond to Lorentz–Drude and Gaussian permittivity terms, respectively, as described elsewhere [173].

Chen et al. [176] used the HLDG model to design and simulate a perfect absorber based on the local surface plasmon resonance (LSPR) and the coupling properties between Ag patterns and a MoS₂ monolayer. Their results show that MoS₂ could increase the optical absorption dramatically. In another work, Jiang et al. [174] integrated the generalized interference theory in the HLDG model to investigate the optical properties of a broadband absorber utilizing a MoS₂ monolayer. A more rigorous approach, consisting in the use of a coupled-wave analysis algorithm with the HLDG model, has been proposed to study the optical absorption of a composite photonic structure made of MoS₂ Au grating [175]. The authors showed that the optical absorption of Au grating can be strongly modified by altering the number of MoS₂ layers (Figure 10b), changing the layout of the MoS₂ layer (e.g., to a MoS₂ nanoribbon array), or inserting a hafnium dioxide spacer. Furthermore, they showed an enhancement of the localized electromagnetic field due to surface plasmon polaritons triggered by Au grating in the presence of few layers of MoS₂. The observed enhancement of the MoS₂ optical absorption was mainly attributed to the exciton transition. Additionally, the HLDG model was used by Xiaoyong et al. [149] to investigate the tunability of wave propagation in MoS₂ supported hybrid surface plasmons waveguides based on dielectric fiber-gap metal substrate structures. By using the finite element method, these authors examined the influence of the structural parameters, the dielectric fiber shape and carrier concentration of the MoS₂ layer on the hybrid modes. Their results allow identifying the tunable parameters of the hybrid modes of waveguide structures that could lead to the design of novel surface plasmon devices in the future.

On the other hand, the association of MoS₂ with plasmonic NPs was also exploited by Yang et al. [151]. The authors reported on the fabrication of a hybrid nanostructure where a MoS₂ monolayer is transferred onto the surface of 10-nm-wide Au nanogap arrays. Interestingly, by adjusting the length of the Au nanogaps, the authors achieved a photoluminescence enhancement as high as ~20 folds. In a more recent work, Mawlong et al. [150] also reported a much higher enhancement factor ~463 folds compared to pristine MoS₂ monolayer at ambient of the PL intensity in the case of TiO₂/Au/MoS₂ ternary core–shell hetero-nanostructures. Such a strong PL enhancement was attributed to the heavy p-doping of the MoS₂ lattice along with LSPR initiated exciton–plasmon coupling at the MoS₂/Au interface [148]. These results suggest that the hybridization of MoS₂ with appropriate metal nanostructures enhances the photoresponse. Indeed, Rahmati et al. [152] also reported an enhancement in the photocurrent generated by vertically aligned MoS₂ nanosheets decorated with Au NPs.

6. Summary and Outlook

Based on the ever-increasing number of published works on 2D-TMDs materials, there is no doubt that MoS₂ will continue to be one of the materials of the choice for the development of innovative and potentially scalable optoelectronic devices.

In term of fabrication, the CVD technique remains a comfortable and affordable route for continuous developments of a variety of shapes and morphologies of 2D-MoS₂. By gaining more control of the deposition process itself, it is possible to further tune the optical and electrical properties of MoS₂ nanostructures while increasing the size of the sample and the lateral uniformity. Of particular concern is the need to improve the reproducibility of defect-free structures. On the other hand, PLD appears as a highly promising alternative for the production of high-quality MoS₂ thin films with a fairly high-level of homogeneity. It also allows tuning the MoS₂ strain level during the elaboration, which may lead to exotic physical properties. PLD also offers an additional possibility to optimize, almost quasi-independently, different deposition parameters of MoS₂ films, and hence tune at will their properties of interest. Finally, PLD also has the advantage of growing crystalline 2D-TMDS at room temperature, which opens the way to deposit MoS₂ films onto flexible and thermo-sensitive substrates, thereby leading to a variety of new applications.

Regarding the applications, apart from those described in this review, 2D-MoS₂ exhibits very appealing performances in infrared domains especially in combination with metamaterials such as passive radiative cooling. There are some emerging works [177,178,179,180] related to this aspect such as developing hybrid MoS₂ thin films with new structures, including metamaterials, metasurfaces, photonic crystals, plasmonics, etc. Similarly, the development of 2D material-based antennas remains unsatisfactory as most of the known achievements on MoS₂ in this domain are developed theoretically. Especially, the recent works [181] on terahertz (THz) plasmonics have shown the potential of MoS₂ for their application in antenna research. Precisely, the use of MoS₂ as a conductive medium in THz antenna appears as a potential direction of recent developments.