Conduction Band Of MoS2 Research Articles

Fundamental Understanding of Interface Chemistry and Electrical Contact Properties of Bi and MoS2.

The interface properties and thermal stability of bismuth (Bi) contacts on molybdenum disulfide (MoS2) shed light on their behavior under various deposition conditions and temperatures. The examination involves extensive techniques including X-ray photoelectron spectroscopy, scanning tunneling microscopy (STM), and scanning tunneling spectroscopy (STS). Bi contacts formed a van der Waals interface on MoS2 regardless of deposition conditions, such as ultrahigh vacuum (UHV, 3 × 10-11 mbar) and high vacuum (HV, 4 × 10-6 mbar), while the oxidation on MoS2 has been observed. However, the semimetallic properties of Bi suppress the impact of defect states, including oxidized-MoS2 and vacancies. Notably, the n-type characteristic of Bi/MoS2 remains unaffected, and no significant changes in the local density of states near the conduction band minimum are observed despite the presence of defects detected by STM and STS. As a result, the Fermi level (EF) resides below the conduction band of MoS2. The study also examines the impact of annealing on the contact interface, revealing no interface reaction between Bi and MoS2 up to 300 °C. These findings enhance our understanding of semimetal (Bi) contacts on MoS2, with implications for improving the performance and reliability of electronic devices.

Promoting the optoelectronic and nonlinear optics properties of MoS2 nanosheets via metal Al anchoring

Molybdenum disulfide (MoS2) has attracted much attention in the field of optoelectronic materials due to its stability and adjustable bandgap structure. However, improving the optoelectronic properties of MoS2 is still a challenging research. Herein, Al doped MoS2 (AMS) films were prepared by a simple single-step magnetron sputtering method. The bonding modes of Al implantation and auxiliary MoS2 were investigated by adjusting metal Al anchoring. The successful synthesis of AMS films was confirmed by the analysis of X-ray diffraction and X-ray photoelectron spectroscopy measurements to investigate the diffraction peaks of Al and Al2S3 and the valence electron structures of Al3+. Compared to MoS2, the A1g Raman peaks of AMS films are slightly blue-shifted, and the peak positions of both Mo3d and S2p are slightly shifted towards higher binding energies. This is attributed to the surface plasmon resonance effect produced by Al doping resulting in a large amount of electron transfer to the conduction band (CB) of MoS2. In addition, the density functional theory calculations reveal that Al doping of MoS2 results in a higher concentration of electrons in CB of MoS2, the band gap of MoS2 can be adjusted by changing the doping concentration of Al. The Z-scan results illustrated that MoS2 was converted from saturable absorption to reverse saturable absorption (RSA) by adjusting the sputtering power of Al. This is attributed to the fact that Al doping increases the electron concentration in the CB of MoS2, which promotes the RSA of the excited states and doping energy levels of AMS films. The values of the nonlinear absorption coefficients of AMS films are 2–5 times higher than those of MoS2, which significantly improves the nonlinear absorption performance of MoS2. The carrier relaxation process and kinetic mechanism of AMS films were investigated by transient absorption spectroscopy, moderate doping of Al can effectively improve the carrier lifetime. This implies that AMS films have good optoelectronic properties and have a wide application potential in optoelectronic devices.

Two-Channel Indirect-Gap Photoluminescence and Competition between the Conduction Band Valleys in Few-Layer MoS2.

MoS2 is a two-dimensional layered transition metal dichalcogenide with unique electronic and optical properties. The fabrication of ultrathin MoS2 is vitally important, since interlayer interactions in its ultrathin varieties will become thickness-dependent, providing thickness-governed tunability and diverse applications of those properties. Unlike with a number of studies that have reported detailed information on direct bandgap emission from MoS2 monolayers, reliable experimental evidence for thickness-induced evolution or transformation of the indirect bandgap remains scarce. Here, the sulfurization of MoO3 thin films with nominal thicknesses of 30 nm, 5 nm and 3 nm was performed. All sulfurized samples were examined at room temperature with spectroscopic ellipsometry and photoluminescence spectroscopy to obtain information about their dielectric function and edge emission spectra. This investigation unveiled an indirect-to-indirect crossover between the transitions, associated with two different Λ and K valleys of the MoS2 conduction band, by thinning its thickness down to a few layers.

MoS2-TiO2 Nanocomposites for Enhanced Photo-electrocatalytic Hydrogen Evolution

The investigation on the designing and fabrication of highly efficient electrocatalysts for hydrogen evolution reaction (HER) is critical for future applications in renewable sustainable energy. The present work reports the hydrothermal synthesis of two-dimensional MoS2 and MoS2-TiO2 nanostructures. The as-prepared nanostructures were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Raman analysis, UV–vis-NIR, and photoluminescence spectrophotometry and vibrating sample magnetometer (VSM). Systematic electrochemical measurements for HER were performed and MoS2-TiO2 nanocomposites demonstrated the lowest onset potential in comparison with MoS2. The results suggest that the nanofusion interface between MoS2 nanoflakes and TiO2 nanoparticles induced an efficient charge transfer from the conduction band of MoS2 to TiO2 and favored the reduction of H+ at active sites. We believe the present work can open up new possibilities that would provide deep insights for the rational design of 2D materials-based catalysts for energy storage and conversion applications.

Strong Photocurrent from Solution‐Processed Ruddlesden–Popper 2D Perovskite–MoS2 Hybrid Heterojunctions

AbstractThis study reports overall improvement in structural, morphological, and optoelectronic properties of Ruddlesden–Popper (RP) perovskites of type (BA)2(MA)n−1PbnI3n+1 by forming their bulk heterojunction hybrids with few‐layer MoS2 nanoflakes. RP perovskite–MoS2 hybrid thin films have shown significantly improved packing and crystallinity compared to pristine perovskites. The presence of MoS2 at RP perovskite interface has improved the quantum confinement effects and transport of photogenerated charge carriers from perovskite to MoS2, due to suitable conduction band of MoS2 and more number of decay channels. The optoelectronic properties of RP perovskite–MoS2 hybrids are studied for various MoS2 concentrations (4.2–25.6 × 10−3 m) and at optimum concentration (12.8 × 10−3 m) the photodetectors (n = 2, 4) have shown strong, sharp, and highly stable photocurrent response. At 0.0 V bias, the RP perovskite (n = 4) and MoS2 (12.8 × 10−3 m) hybrid‐based photodetectors, prepared without any encapsulation, have shown strong photocurrent density of ≈9.8 µA cm−2 under 1 sun illumination, which is ≈17 times higher compared to the pristine RP perovskites‐based photodetector (0.6 µA cm−2). Further transient photocurrent, performed over 200 cycles for hybrid (n = 4+MoS2) thin film photodetector under laser (λex ≈ 405 nm, ≈630 mW cm−2) illumination and ambient air conditions has shown highly stable photocurrent with only ≈9.6% reduction in the peak photocurrent density.

Simultaneous removal of Cr(VI) and phenol in a dual-chamber photocatalytic microbial fuel with NiCo2O4/MoS2/GF photocathode

Efficient treatment and resource utilization of sewage are of great value for global sustainability. In this study, a composite photocathode was prepared by loading NiCo2O4 nanosheets and MoS2 nanoflowers to a graphite felt (GF)-based electrode through a two-step hydrothermal and calcination method. A photocatalytic microbial fuel cell (PMFC) was constructed using the NiCo2O4/MoS2/GF photocathode and carbon felt (CF) anode in a dual-chamber H-type battery. Cr(VI) and phenol were employed as target pollutants in the cathode chamber. The photoelectric performance of the NiCo2O4/MoS2/GF photocathode and the removal efficiency of the battery system were studied systematically. When a mixed solution of Cr(VI) and phenol was used, the removal rates of Cr(VI) and phenol after 24 h of light exposure were 8.13 % and 12.65 % higher than those when Cr(VI) or phenol was used alone, respectively. At the same time, the output power density of the battery in the mixed pollutants was 362.7 mW/m3, which was 45.78 % higher than that in the single Cr(VI) solution (248.8 mW/m3). The excellent performance of the PMFC was attributed to three reasons: (1) NiCo2O4 and MoS2 were simultaneously excited as two narrow-bandgap semiconductors, and the utilization rate of light energy was increased; (2) The Z-scheme heterojunction between NiCo2O4 and MoS2 improved the separation efficiency of the photoelectric carriers and retained the high valence band of NiCo2O4 and low conduction band of MoS2 to the greatest extent, which is crucial for the PMFC to achieve electronic export and double contaminant removal; and (3) the NiCo2O4 nanosheet and MoS2 nanoflower structures enhanced the contact between the catalysts and the pollutants.

Charge transfer dynamics and interlayer exciton formation in MoS2/VOPc mixed dimensional heterojunction.

Mixed-dimensional van der Waals heterojunctions involve interfacing materials with different dimensionalities, such as a 2D transition metal dichalcogenide and a 0D organic semiconductor. These heterojunctions have shown unique interfacial properties not found in either individual component. Here, we use femtosecond transient absorption to reveal photoinduced charge transfer and interlayer exciton formation in a mixed-dimensional type-II heterojunction between monolayer MoS2 and vanadyl phthalocyanine (VOPc). Selective excitation of the MoS2 exciton leads to hole transfer from the MoS2 valence band to VOPc highest occupied molecular orbit in ∼710fs. On the contrary, selective photoexcitation of the VOPc layer leads to instantaneous electron transfer from its excited state to the conduction band of MoS2 in less than 100fs. This light-initiated ultrafast separation of electrons and holes across the heterojunction interface leads to the formation of an interlayer exciton. These interlayer excitons formed across the interface lead to longer-lived charge-separated states of up to 2.5ns, longer than in each individual layer of this heterojunction. Thus, the longer charge-separated state along with ultrafast charge transfer times provide promising results for photovoltaic and optoelectronic device applications.

Plasmon-Induced Enhanced Light Emission and Ultrafast Carrier Dynamics in a Tunable Molybdenum Disulfide-Gallium Nitride Heterostructure.

The effect of localized plasmon on the photoemission and absorption in hybrid molybdenum disulfide-Gallium nitride (MoS2-GaN) heterostructure has been studied. Localized plasmon induced by platinum nanoparticles was resonantly coupled to the bandedge states of GaN to enhance the UV emission from the hybrid semiconductor system. The presence of the platinum nanoparticles also increases the effective absorption and the transient gain of the excitonic absorption in MoS2. Localized plasmons were also resonantly coupled to the defect states of GaN and the exciton states using gold nanoparticles. The transfer of hot carriers from Au plasmons to the conduction band of MoS2 and the trapping of excited carriers in MoS2 within GaN defects results in transient plasmon-induced transparency at ~1.28 ps. Selective optical excitation of the specific resonances in the presence of the localized plasmons can be used to tune the absorption or emission properties of this layered 2D-3D semiconductor material system.

Dry and hydrated defective molybdenum Disulfide/Graphene bilayer heterojunction under strain for hydrogen evolution from water Splitting: A First-principle study

In search of exploiting cost-effective, highly stable, efficient, and greatly active electrocatalysts for hydrogen evolution reaction (HER), molybdenum disulfide-graphene heterostructures (MoS2/graphene) are promising, in contrast to noble metals. We used density functional theory (DFT) to examine the changes in the electronic structure of MoS2/graphene under compressive strain for structural defects in the MoS2 and graphene layers, as well as from hydration of the MoS2 layer. In the pristine MoS2/graphene heterostructure, a small bandgap (minigap) is opened at the graphene Dirac point, which is located above the Fermi energy, for dry and hydrated configurations. The presence of sulfur and carbon vacancies in the MoS2/graphene upshifts the Dirac point and widens the minigap. However, additional sulfur vacancies further widen or shrink the minigap depending on the location of the MoS2 conduction band bottom and the presence of defect bands at the Dirac point. The minigap tunability in the MoS2/graphene heterostructure could be engineered for producing efficient HER electrocatalysts and beyond. The Quantum Theory of Atoms in Molecules (QTAIM) reveals SC bond critical points, which correspond to van der Waals forces interactions in agreement with the Non-covalent Interaction (NCI) analysis. A correlation is drawn between the minigap and the electron density at the SC bond critical points.

Efficient modulation of MoS2/WSe2 interlayer excitons via uniaxial strain

Artificially stacked van der Waals heterostructures (vdWH) of two-dimensional (2D) atomic layers have attracted considerable attention due to substantial interactions between different layers. In particular, the strongly bound interlayer exciton (IX) within vdWH offers a platform for exploring fundamental physics as well as innovative device applications. However, to date, it remains a critical challenge to modulate the IX emission energy, limiting the achievement of high-performance spin-valleytronics and excitonic devices. Here, we report a simple strain engineering approach to efficiently modulate the MoS2/WSe2 IX via uniaxial strain. By encapsulating the vdWH within a flexible substrate, the applied mechanical strain could be effectively transferred to the lattice of vdWH during the mechanical bending process, leading to an unprecedent IX modulation range of 144 meV with a linear fitted gauge factor of 121.8 meV per 1% strain. Furthermore, we found that the gauge factor of IX in vdWH is larger than that of individual MoS2 and WSe2 intralayer excitons, further confirming that the observed IX originates from the momentum-indirect exciton between the K point of the MoS2 conduction band and the Γ point of the WSe2 valence band. Our study not only achieves a high vdWH IX modulation value using efficient strain engineering but also provides a route to investigate the evolution of band energy for various two-dimensional (2D) materials as well as their vertical vdWH.

Excited state absorption induced optical limiting action of MoS2-rGO nanocomposites

Molybdenum sulphide-reduced graphene oxide nanocomposite made of microsphere MoS2 with varying concentration of layered (15, 30, 45 wt%) rGO was prepared by hydrothermal method. XRD confirms the molecular formation of mixed phase MoS2 having rich semiconducting hexagonal phase with traces of metallic tetragonal phase (1T@2H MoS2) and reduced graphene oxide (2θ = 25.7°, (002)). Further EDS also ascertains the reduction of Mo and S with increase in C content with respect to rGO concentration. As the rGO concentration increases (15–45 wt%), strengthening of characteristic Raman peaks of rGO (G and D band) and weakening of MoS2 (E1g, E2g1 and A1g modes) in composite was observed. Estimated ID/IG (1.04) and I2D/IG (0.62) ratio suggest the formation of 2–3 layers of graphene. SEM depicts layered morphology of rGO, floret like microstructure of MoS2 and floret microspheres MoS2 decorated rGO layers of MoS2 – rGO nanocomposite. Optical studies show absorption peaks at 266 nm (π-π* transition of the CC aromatic bonds of graphene), 370 nm (and n-π* transition of the CO bond of graphene) and 330 nm (direct transitions in valence to conduction band of MoS2). Liquid dispersion of both pristine and composite depicted strong absorption in UV–Visible region and available electronic state favours the opportunity for two-photon absorption. Intensity dependent Z-Scan with nano-pulsed green laser excitation shows the existence of excited state absorption involved two-photon absorption. Variation of saturation intensity and nonlinear absorption coefficient with on-axis peak intensity (620 –2160 GW/cm2) confirms the involvement of sequential 2PA process (1PA + ESA). MoS2-(30 wt%)rGO nanocomposite exhibited higher 2PA coefficient (9.42 × 10−10 m/W) and lower onset optical limiting threshold (3.15 × 1012 W/m2) than its pristine counterparts and other well-known TMDC’s and graphene derivatives. Enhanced NLO response is due to synergistic effects of rGO (higher defect induced states, extended conjugation for charge transfer) and MoS2 (floret morphology, uniform decoration and strong visible absorption). Observed excited state absorption induced energy absorbing optical limiting action of MoS2-rGO nanocomposite with augmented NLO coefficients open up potential horizon for developing laser goggles against most sensitive and widely used nanopulsed green laser.

Origins of genuine Ohmic van der Waals contact between indium and MoS2

The achievement of ultraclean Ohmic van der Waals (vdW) contacts at metal/transition-metal dichalcogenide (TMDC) interfaces would represent a critical step for the development of high-performance electronic and optoelectronic devices based on two-dimensional (2D) semiconductors. Herein, we report the fabrication of ultraclean vdW contacts between indium (In) and molybdenum disulfide (MoS2) and the clarification of the atomistic origins of its Ohmic-like transport properties. Atomically clean In/MoS2 vdW contacts are achieved by evaporating In with a relatively low thermal energy and subsequently cooling the substrate holder down to ~100 K by liquid nitrogen. We reveal that the high-quality In/MoS2 vdW contacts are characterized by a small interfacial charge transfer and the Ohmic-like transport based on the field-emission mechanism over a wide temperature range from 2.4 to 300 K. Accordingly, the contact resistance reaches ~600 Ω μm and ~1000 Ω μm at cryogenic temperatures for the few-layer and monolayer MoS2 cases, respectively. Density functional calculations show that the formation of large in-gap states due to the hybridization between In and MoS2 conduction band edge states is the microscopic origins of the Ohmic charge injection. We suggest that seeking a mechanism to generate strong density of in-gap states while maintaining the pristine contact geometry with marginal interfacial charge transfer could be a general strategy to simultaneously avoid Fermi-level pinning and minimize contact resistance for 2D vdW materials.

Free-standing Ag nanoparticle-decorated MoS2 microflowers grown on carbon cloth for photocatalytic oxidation of Rhodamine B

MoS2 microflowers were grown on the surface of a carbon cloth (CC) via a one-step hydrothermal method. Sodium borohydride was used to chemically reduce Ag nanoparticles on the surface of the as-grown MoS2 microflowers. The Ag nanoparticle-decorated MoS2 microflowers grown on the CC (Ag@MoS2/CC) were used for the photocatalytic degradation of rhodamine B (RB) via visible light absorption. The Ag nanoparticles significantly affected the reactivity of the photocatalyst by generating a large number of oxidative radical species. The catalytic reaction followed first-order kinetics and the rate of degradation improved by about 3.3 times upon the deposition of Ag nanoparticles on the surface. Scavenger experiments showed that the hydroxyl radicals generated by the photogenerated electrons were the main contributing species in the degradation of RB. The catalytic mechanism involved efficient electron transfer from the conduction band of MoS2 to Ag through a space charge region, making the surface of the photocatalyst highly electron populated. The fabricated catalyst was highly stable for multiple experiments.

Local photodoping in monolayer MoS2

Inducing electrostatic doping in 2D materials by laser exposure (photodoping effect) is an exciting route to tune optoelectronic phenomena. However, there is a lack of investigation concerning in what respect the action of photodoping in optoelectronic devices is local. Here, we employ scanning photocurrent microscopy (SPCM) techniques to investigate how a permanent photodoping modulates the photocurrent generation in MoS2 transistors locally. We claim that the photodoping fills the electronic states in MoS2 conduction band, preventing the photon-absorption and the photocurrent generation by the MoS2 sheet. Moreover, by comparing the persistent photocurrent (PPC) generation of MoS2 on top of different substrates, we elucidate that the interface between the material used for the gate and the insulator (gate-insulator interface) is essential for the photodoping generation. Our work gives a step forward to the understanding of the photodoping effect in MoS2 transistors and the implementation of such an effect in integrated devices.

Quantum mechanical analysis of 2D transition metal dichalcogenide material based vertical heterojunction tunnel FET

In this work, a single layer n-doped MoS2 and p-doped WTe2 based vertical heterojunction tunnel FET has been investigated through a well-organized quantum mechanical approach. The key outcome is the design criteria of the device for low subthreshold swing keeping its length as short as possible. Inter-coupled real space model Hamiltonian of the device is formed by introducing the coupling energy of the WTe2 valence band and the MoS2 conduction band in the overlap region. Here, MATLAB based self-consistent analysis is used to numerically solve the device by coupling Schrödinger and Poisson equations taking into account the plane dependence of permittivity in 2D transition metal dichalcogenide materials. For 15 nm channel overlap length and 15 nm gate extension length, a subthreshold slope of as low as 10 mV/decade has been obtained. For 20 nm channel overlap length, an ON current of 18 µA/μm has been obtained as well. The effect of the top gate extension, overlap length, and dielectric layer thickness over the ON and OFF state currents has been explained from the viewpoint of device physics. Thus, the framework presented will help designers to optimize the device for improved performance.

Modulating the Optical Band Gap of Small Semiconducting Two-Dimensional Materials by Conjugated Polymers.

Ultra-high-resolution optical microscopic techniques are used to measure the reflectance and photoluminescence (PL) spectrum of individual monolayered MoS2 of dimensions below 200 × 200 nm, while placed on top of a thin film conjugated polymer (CP). p-type and n-type CPs such as poly(3-hexylthiophene-2,5-diyl) (P3HT) and [6,6]-phenyl C61 butyric acid methyl ester (PCBM), respectively, modified the optical band gap of the MoS2 sheet differently. However, the optical band gap is decreased after integration with P3HT, while it is increased after being combined with PCBM. The acceptable reason for the modification of the band gap of MoS2 by CPs is the generation of interlayer excitons (ILE) at their interface. The optical band gap of MoS2 is further changed by introducing an inert polymer spacer of different thickness to separate MoS2 from the CP. This is attributed to the reduction of the efficiency of excitonic interactions and lowering the exciton binding energy, which is induced by the increase of the dielectric function at the CP-MoS2 interface. No sign of electron injection to the conduction band of MoS2 after integration with P3HT or PCBM, as no significant shift of the A1' Raman band of MoS2 was measured on top of CPs, which is sensitive to the electron injection.

Fabrication of ZnO@MoS2 Nanocomposite Heterojunction Arrays and Their Photoelectric Properties

In this paper, ZnO@MoS2 core-shell heterojunction arrays were successfully prepared by the two-step hydrothermal method, and the growth mechanism was systematically studied. We found that the growth process of molybdenum disulfide (MoS2) was sensitively dependent on the reaction temperature and time. Through an X-ray diffractometry (XRD) component test, we determined that we prepared a 2H phase MoS2 with a direct bandgap semiconductor of 1.2 eV. Then, the photoelectric properties of the samples were studied on the electrochemical workstation. The results show that the ZnO@MoS2 heterojunction acts as a photoanode, and the photocurrent reaches 2.566 mA under the conditions of 1000 W/m2 sunshine and 0.6 V bias. The i-t curve also illustrates the perfect cycle stability. Under the condition of illumination and external bias, the electrons flow to the conduction band of MoS2 and flow out through the external electrode of MoS2. The holes migrate from the MoS2 to the zinc oxide (ZnO) valence band. It is transferred to the external circuit through the glass with fluorine-doped tin oxide (FTO) together with the holes on the ZnO valence band. The ZnO@MoS2 nanocomposite heterostructure provides a reference for the development of ultra-high-speed photoelectric switching devices, photodetector(PD) devices, and photoelectrocatalytic technologies.

Fabrication of ultrathin-MoS2/Ag/AgBr composite with enhanced photocatalytic activity

The MoS2/Ag/AgBr composite with ultrathin-MoS2 layers was prepared by the methods of ultrasonic liquid exfoliation and ion exchange. The composition and micromorphology of ultrathin-MoS2/Ag/AgBr were detected by XRD, EDS, SEM and TEM in detail. The element mapping showed that the samples were well-distributed. The MoS2 in samples and the number of plies were detected by Raman spectra specifically. The results indicated that the photocatalytic performance of the as-prepared samples would increase by 50% when the average thickness of MoS2 was about 4 nm. The enhanced photocatalytic performance of ultrathin-MoS2/Ag/AgBr composite is attributed to the modified conduction band of MoS2 by reducing the layers of MoS2 to fit the potential of O2/O2·−. In particular, this work would expand the scope of application of MoS2 in photodegradation.

Detection of cyclotron resonance using photo-induced thermionic emission at graphene/MoS2 van der Waals interface

We demonstrate the detection of cyclotron resonance in graphene by a photo-induced thermionic emission mechanism at the graphene/MoS2 van der Waals (vdW) Schottky junction. At cyclotron resonance in Landau-quantized graphene, the infrared light is absorbed, and an electron–hole pair is generated. When the energy of a photoexcited electron exceeds the band offset energy at the graphene/MoS2 interface, the electron transfer occurs from graphene to the conduction band of MoS2, and the hole remains in graphene. This creates an electron–hole separation at the graphene/MoS2 interface at cyclotron resonance, and a photovoltage is generated. The proposed method is an infrared photodetection technique through out-of-plane transport at the vdW junction, which is distinct from the previously reported methods that use in-plane transport in graphene for electronic detection of the cyclotron resonance. Despite the simple structure of our device with a single-vdW junction, our method exhibits a very high sensitivity of ∼106 V/W, which shows an improvement of three orders of magnitude over the previously reported values. Therefore, the proposed method displays a high potential for cyclotron resonance-based infrared photodetector applications.

Photoinduced Carrier Dynamics at the Interface of Pentacene and Molybdenum Disulfide.

Understanding of photoinduced interfacial carrier dynamics in organic-transition metal dichalcogenides heterostructures is very important for the enhancement of their potential photoelectronic conversion efficiencies. In this work we have used density functional theory (DFT) calculations and DFT-based fewest-switches surface-hopping dynamics simulations to explore the photoinduced hole transfer and subsequent nonadiabatic electron-hole recombination dynamics taking place at the interface of pentacene and MoS2 in pentacene@MoS2. Upon photoexcitation the electronic transition mainly occurs on the MoS2 monolayer, which corresponds to moving an electron to the MoS2 conduction band. As a result, a hole is left in the valence band. This hole state is energetically lower than certain occupied states of the pentacene molecule; thus, the interfacial hole transfer from MoS2 to pentacene is favorable in energy. In terms of nonadiabatic dynamics simulations, the hole transfer time to the HOMO-1 state of the pentacene is estimated to be about 600 fs; however, the following hole relaxation process from HOMO-1 to HOMO takes much longer time of ca. 15 ps due to the large energy gap between HOMO-1 and HOMO. Moreover, our results also show that the subsequent radiationless recombination process between the hole transferred to the pentacene molecule and the remaining electron on the MoS2 CBM needs about 10.2 ns. The computational results shed important mechanistic insights on the interfacial carrier dynamics of mixed-dimensional pentacene@MoS2. These insights could help to design excellent interfaces for organic-TMDs heterostructures.