Recent Submissions

  • Carrier dynamics of InxGa1-xN/GaN multiple quantum wells grown on (−201) β-Ga2O3 for bright vertical light emitting diodes

    Mumthaz Muhammed, Mufasila; Xu, Jian; Wehbe, Nimer; Roqan, Iman S. (The Optical Society, 2018-05-30)
    High-quality InxGa1-xN/GaN multi-quantum well (MQW) structures (0.05≤x≤0.13), are successfully grown on transparent and conductive (−201)-oriented β-Ga2O3 substrate. Scanning-transmission electron microscopy and secondary ion mass spectrometry (SIMS) show well-defined high quality MQWs, while the In and Ga compositions in the wells and the barriers are estimated by SIMS. Temperature-dependant Photoluminescence (PL) confirms high optical quality with a strong bandedge emission and negligble yellow band. time-resolved PL measurements (via above/below-GaN bandgap excitations) explain carrier dynamics, showing that the radiative recombination is predominant. Our results demonstrate that (−201)-oriented β-Ga2O3 is a strong candidate as a substrate for III-nitride-based vertical- emitting devices.
  • Efficient Photon Recycling and Radiation Trapping in Cesium Lead Halide Perovskite Waveguides

    Dursun, Ibrahim; Zheng, Yangzi; Guo, Tianle; de Bastiani, Michele; Turedi, Bekir; Sinatra, Lutfan; Haque, Mohammed; Sun, Bin; Zhumekenov, Ayan A.; Saidaminov, Makhsud I.; Garcia de Arquer, F. Pelayo; Sargent, Edward H.; Wu, Tao; Gartstein, Yuri N; Bakr, Osman; Mohammed, Omar F.; Malko, Anton V. (American Chemical Society (ACS), 2018-05-26)
    Cesium lead halide perovskite materials have attracted considerable attention for potential applications in lasers, light emitting diodes and photodetectors. Here, we provide the experimental and theoretical evidence for photon recycling in CsPbBr3 perovskite microwires. Using two-photon excitation, we recorded photoluminescence (PL) lifetimes and emission spectra as a function of the lateral distance between PL excitation and collection positions along the microwire, with separations exceeding 100 µm. At longer separations, the PL spectrum develops a red-shifted emission peak accompanied by an appearance of well-resolved rise times in the PL kinetics. We developed quantitative modeling that accounts for bimolecular recombination and photon recycling within the microwire waveguide and is sufficient to account for the observed decay modifications. It relies on a high radiative efficiency in CsPbBr3 perovskite microwires and provides crucial information about the potential impact of photon recycling and waveguide trapping on optoelectronic properties of cesium lead halide perovskite materials.
  • Inherent Electrochemistry and Charge Transfer Properties of Few-Layer Two Dimensional Ti3C2Tx MXene

    Nayak, Pranati; Jiang, Qiu; Mohanraman, Rajeshkumar; Anjum, Dalaver H.; Hedhili, Mohamed N.; Alshareef, Husam N. (Royal Society of Chemistry (RSC), 2018-05-25)
    We report the effect of Ti3C2Tx MXene flake thickness on its inherent electrochemistry and heterogeneous charge transfer characteristics. It is shown that the Ti3C2Tx undergoes irreversible oxidation in the positive potential window, which strongly depends on the flake thickness and pH of the electrolyte. Few-layer Ti3C2Tx exhibits faster electron transfer kinetics (k0=0.09533 cm/s) with Fe(CN)64−/3− redox mediator compared to multi-layer Ti3C2Tx (k0= 0.00503 cm/s). In addition, few-layer free standing Ti3C2Tx film electrode remains intact after enduring irreversible oxidation.
  • Quantification of Ionic Diffusion in Lead Halide Perovskite Single Crystals

    Peng, Wei; Aranda, Clara; Bakr, Osman; Garcia-Belmonte, Germà; Bisquert, Juan; Guerrero, Antonio (American Chemical Society (ACS), 2018-05-25)
    Lead halide perovskites are mixed electronic/ionic semiconductors that have recently revolutionized the photovoltaics field. The physical characterization of the ionic conductivity has been rather elusive due to the highly intermixing of ionic and electronic current. In this work the synthesis of low defect density monocrystalline MAPbBr3 (MA=Methyl ammonium) solar cells free of hole transport layer (HTL) suppresses the effect of electronic current. Impedance spectroscopy reveals the characteristic signature of ionic diffusion (the Warburg element and transmission line equivalent circuit) and ion accumulation at the MAPbBr3/Au interface. Diffusion coefficients are calculated based on a good correlation between thickness of MAPbBr3 and characteristic diffusion transition frequency. In addition, reactive external interfaces are studied by comparison of polycrystalline MAPbBr3 devices prepared either with or without a HTL. The low frequency response in IS measurements is correlated with the chemical reactivity of moving ions with the external interfaces and diffusion into the HTL.
  • Robust nonfullerene solar cells approaching unity external quantum efficiency enabled by suppression of geminate recombination

    Baran, Derya; Gasparini, Nicola; Wadsworth, Andrew; Tan, Ching Hong; Wehbe, Nimer; Song, Xin; Hamid, Zeinab; Zhang, Weimin; Neophytou, Marios; Kirchartz, Thomas; Brabec, Christoph J.; Durrant, James R.; McCulloch, Iain (Springer Nature, 2018-05-21)
    Nonfullerene solar cells have increased their efficiencies up to 13%, yet quantum efficiencies are still limited to 80%. Here we report efficient nonfullerene solar cells with quantum efficiencies approaching unity. This is achieved with overlapping absorption bands of donor and acceptor that increases the photon absorption strength in the range from about 570 to 700 nm, thus, almost all incident photons are absorbed in the active layer. The charges generated are found to dissociate with negligible geminate recombination losses resulting in a short-circuit current density of 20 mA cm-2 along with open-circuit voltages >1 V, which is remarkable for a 1.6 eV bandgap system. Most importantly, the unique nano-morphology of the donor:acceptor blend results in a substantially improved stability under illumination. Understanding the efficient charge separation in nonfullerene acceptors can pave the way to robust and recombination-free organic solar cells.
  • Plasmonic Nanowires for Wide Wavelength Range Molecular Sensing

    Marinaro, Giovanni; Das, Gobind; Giugni, Andrea; Allione, Marco; Torre, Bruno; Candeloro, Patrizio; Kosel, Jürgen; Di Fabrizio, Enzo M. (MDPI AG, 2018-05-17)
    In this paper, we propose the use of a standing nanowires array, constituted by plasmonic active gold wires grown on iron disks, and partially immersed in a supporting alumina matrix, for surface-enhanced Raman spectroscopy applications. The galvanic process was used to fabricate nanowires in pores of anodized alumina template, making this device cost-effective. This fabrication method allows for the selection of size, diameter, and spatial arrangement of nanowires. The proposed device, thanks to a detailed design analysis, demonstrates a broadband plasmonic enhancement effect useful for many standard excitation wavelengths in the visible and NIR. The trigonal pores arrangement gives an efficiency weakly dependent on polarization. The devices, tested with 633 and 830 nm laser lines, show a significant Raman enhancement factor, up to around 6 × 10⁴, with respect to the flat gold surface, used as a reference for the measurements of the investigated molecules.
  • Efficient Long - Range Electron Transfer Processes in Polyfluorene – Perylene Diimide Blends

    Isakova, Anna; Karuthedath, Safakath; Arnold, Thomas; Howse, Jonathan; Topham, Paul D.; Toolan, Daniel Thomas William; Laquai, Frédéric; Lüer, Larry (Royal Society of Chemistry (RSC), 2018-05-17)
    In bulk heterojunction donor-acceptor (D-A) blends, high photovoltaic yields require charge carrier separation to outcompete geminate recombination. Recently, evidence for long-range electron transfer mechanisms has been presented, avoiding strongly-bound interfacial charge transfer (CT) states. However, due to the lack of specific optical probes at the D-A interface, a detailed quantification of the long-range processes has not been feasible, until now. Here, we present a transient absorption study of long-range processes in a unique phase consisting of perylene diimide (PDI) crystals intercalated with polyfluorene (PFO), as widely used non-fullerene electron acceptor and donor, respectively. The intercalated PDI:PFO phase possesses specific well-separated spectral features for the excited states at the D-A interface. By use of femtosecond spectroscopy we reveal the excitation dynamics in this blend. PDI excitons undergo a clear symmetry-breaking charge separation in the PDI bulk, which occurs within several hundred femtoseconds, thus outcompeting excimer formation, known to limit charge separation yields when PDI is used as an acceptor. In contrast, PFO excitons are dissociated with very high yields in a one-step long-range process, enabled by large delocalization of the PFO exciton wavefunction. Moreover, both scenarios circumvent the formation of strongly-bound interfacial CT states and enable a targeted interfacial design for bulk heterojunction blends with near unity charge separation yields.
  • Using Mosaicity to Tune Thermal Transport in Polycrystalline AlN Thin Films

    Singh, Shivkant; Shervin, Shahab; Sun, Haiding; Yarali, Milad; Chen, Jie; Lin, Ronghui; Li, Kuang-Hui; Li, Xiaohang; Ryou, Jae-Hyun; Mavrokefalos, Anastassios (American Chemical Society (ACS), 2018-05-17)
    The effect of controlling the c-axis alignment (mosaicity) to the cross-plane thermal transport in textured polycrystalline aluminum nitride (AlN) thin films is experimentally and theoretically investigated. We show that by controlling the sputtering conditions we are able to deposit AlN thin films with varying c-axis grain tilt (mosaicity) from 10° to 0°. Microstructural characterization shows that the films are nearly identical in thickness and grain size, and the difference in mosaicity alters the grain interface quality. This has a significant effect to thermal transport where a thermal conductivity of 4.22 W/mK vs. 8.09 W/mK are measured for samples with tilt angles of 10° vs. 0° respectively. The modified Callaway model was used to fit the theoretical curves to the experimental results using various phonon scattering mechanisms at the grain interface. It was found that using a non-gray model gives an overview of the phonon scattering at the grain boundaries, whereas treating the grain boundary as an array of dislocation lines with varying angle relative to the heat flow, best describes the mechanism of the thermal transport. Lastly, our results show that controlling the quality of the grain interface provides a tuning knob to control thermal transport in polycrystalline materials.
  • Molecular dynamics of Middle East Respiratory Syndrome Coronavirus (MERS CoV) fusion heptad repeat trimers

    Kandeel, Mahmoud; Al-Taher, Abdulla; Li, Huifang; Schwingenschlögl, Udo; Alnazawi, Mohamed (Elsevier BV, 2018-05-17)
    Structural studies related to Middle East Respiratory Syndrome Coronavirus (MERS CoV) infection process are so limited. In this study, molecular dynamics (MD) simulation was carried out to unravel changes in the MERS CoV heptad repeat domains (HRs) and factors affecting fusion state HR stability. Results indicated that HR trimer is more rapidly stabilized, having stable system energy and lowest root mean square deviations (RMSDs). While trimers were the predominant active form of CoVs HR, monomers were also discovered in both of viral and cellular membranes. In order to find the differences between S2 monomer and trimer molecular dynamics, S2 monomer were modelled and subjected to MD simulation. In contrast to S2 trimer, S2 monomer was unstable, having high RMSDs with major drifts above 8 Å. Fluctuation of HR residue positions revealed major changes in the C-terminal of HR2 and the linker coil between HR1 and HR2 in both monomer and trimer. Hydrophobic residues at the “a” and “d” positions of HR helices stabilize the whole system, having minimal changes in RMSD. The global distance test and contact area difference scores support instability of MERS CoV S2 monomer. Analysis of HR1-HR2 inter-residue contacts and interaction energy revealed three different energy scales along HR helices. Two strong interaction energies were identified at the start of the HR2 helix and at the C-terminal of HR2. The identified critical residues by MD simulation and residues at a and d position of HR helix were strong stabilizers of HRs recognition.
  • Atomic-Layer-Deposited AZO Outperforms ITO in High-Efficiency Polymer Solar Cells

    Kan, Zhipeng; Wang, Zhenwei; Firdaus, Yuliar; Babics, Maxime; Alshareef, Husam N.; Beaujuge, Pierre (Royal Society of Chemistry (RSC), 2018-05-11)
    Tin-doped indium oxide (ITO) transparent conducting electrodes are widely used across the display industry, and are currently the cornerstone of photovoltaic device developments, taking a substantial share in the manufacturing cost of large-area modules. However, cost and supply considerations are set to limit the extensive use of indium for optoelectronic device applications and, in turn, alternative transparent conducting oxide (TCO) materials are required. In this report, we show that aluminum-doped zinc oxide (AZO) thin films grown by atomic layer deposition (ALD) are sufficiently conductive and transparent to outperform ITO as the cathode in inverted polymer solar cells. Reference polymer solar cells made with atomic-layer-deposited AZO cathodes, PCE10 as the polymer donor and PC71BM as the fullerene acceptor (model systems), reach power conversion efficiencies of ca. 10% (compared to ca. 9% with ITO-coated glass), without compromising other figures of merit. These ALD-grown AZO electrodes are promising for a wide range of optoelectronic device applications relying on TCOs.
  • Phase Transition Control for High-Performance Blade-Coated Perovskite Solar Cells

    Li, Jianbo; Munir, Rahim; Fan, Yuanyuan; Niu, Tianqi; Liu, Yucheng; Zhong, Yufei; Yang, Zhou; Tian, Yuansi; Liu, Bo; Sun, Jie; Smilgies, Detlef-M.; Thoroddsen, Sigurdur T; Amassian, Aram; Zhao, Kui; Liu, Shengzhong (Frank) (Elsevier BV, 2018-05-07)
    Summary Here, we have identified that the key issue for rational transitioning from spin-coating to blade-coating processes of perovskite films arises from whether intermediate phases participate in the phase transition. In situ characterizations were carried out to provide a comprehensive picture of structural evolution and crystal growth mechanisms. These findings present opportunities for designing an effective process for blade-coating perovskite film: a large-grained dense perovskite film with high crystal quality and photophysical properties can be obtained only via direct crystallization for both spin-coating and blade-coating processes. As a result, the blade-coated MAPbI3 films deliver excellent charge-collection efficiency at both short circuit and open circuit, and photovoltaic properties with efficiencies of 18.74% (0.09 cm2) and 17.06% (1 cm2) in planar solar cells. The significant advances in understanding how the phase transition links spin-coating and blade-coating processes should provide a path toward high-performance printed perovskite devices.
  • Electronic Reconstruction in (LaVO3 ) m /SrVO3 ( m = 5, 6) Superlattices

    Dai, Qingqing; Lüders, Ulrike; Frésard, Raymond; Eckern, Ulrich; Schwingenschlögl, Udo (Wiley, 2018-05-04)
    The (LaV3+O3)m/SrV4+O3 (m = 5, 6) superlattices are investigated by first principles calculations. While bulk LaVO3 is a C‐type antiferromagnetic semiconductor and bulk SrVO3 is a paramagnetic metal, semiconducting A‐type antiferromagnetic states for both superlattices are found due to epitaxial strain. At the interfaces, however, the V spins couple antiferromagnetically for m = 5 and ferromagnetically for m = 6 (m‐dependence of the magnetization). Electronic reconstruction in form of charge ordering is predicted to occur with V3+ and V4+ states arranged in a checkerboard pattern on both sides of the SrO layer. As compared to bulk LaVO3, the presence of V4+ ions introduces in‐gap states that strongly reduce the bandgap and influence the orbital occupation and ordering.
  • Hybrid Tandem Quantum Dot/Organic Solar Cells with Enhanced Photocurrent and Efficiency via Ink and Interlayer Engineering

    Kim, Taesoo; Firdaus, Yuliar; Kirmani, Ahmad R.; Liang, Ru-Ze; Hu, Hanlin; Liu, Mengxia; El Labban, Abdulrahman; Hoogland, Sjoerd; Beaujuge, Pierre; Sargent, Edward H.; Amassian, Aram (American Chemical Society (ACS), 2018-05-03)
    Realization of colloidal quantum dot (CQD)/organic photovoltaic (OPV) tandem solar cells that integrate the strong infrared absorption of CQDs with large photovoltages of OPVs is an attractive option toward high-performing, low-cost thin film solar cells. To date, monolithic hybrid tandem integration of CQD/OPV solar cells has been restricted due to the CQD ink’s catastrophic damage to the organic subcell, thus forcing the low bandgap CQD to be used as front cell. This sub-optimal configuration limits the maximum achievable photocurrent in CQD/OPV hybrid tandem solar cells. In this work, we demonstrate hybrid tandem solar cells employing a low-bandgap CQD back cell on top of an organic front cell thanks to a modified CQD ink formulation and a robust interconnection layer (ICL) which together overcome the long-standing integration challenges for CQD and organic subcells. The resulting tandem architecture surpasses previously reported current densities by ~20-25% and yields a state-of-the-art power conversion efficiency (PCE) of 9.4%.
  • Charge Photogeneration and Recombination in Mesostructured CuSCN-Nanowire/PC70 BM Solar Cells

    Firdaus, Yuliar; Seitkhan, Akmaral; Eisner, Flurin; Sit, Wai-Yu; Kan, Zhipeng; Wehbe, Nimer; Balawi, Ahmed H.; Yengel, Emre; Karuthedath, Safakath; Laquai, Frédéric; Anthopoulos, Thomas D. (Wiley, 2018-05-02)
    Fullerene‐based materials are widely used as electron acceptors in organic bulk‐heterojunction solar cells; yet, they have rarely been used as the only photoactive component due to their low absorbance and limited charge generation efficiency. However, blending the wide‐bandgap p‐type material copper (I) thiocyanate (CuSCN) with [6,6]‐phenyl‐C71‐butyric acid methyl ester (PC70BM) leads to the formation of a unique mesostructured p‐n like heterointerface between CuSCN and PC70BM and solar cells with a power conversion efficiency (PCE) of up to 5.4%. Here, we examine in detail the reasons for the surprisingly good device performance and elucidate the charge photogeneration and recombination mechanisms in CuSCN‐based devices with PC70BM as the exclusive light‐absorbing material. Our studies clearly demonstrate that a substantial fraction of the photocurrent in the CuSCN‐based devices results from improved dissociation of fullerene excitons and efficient charge transfer at the CuSCN:PC70BM interface combined with reduced geminate and nongeminate charge recombination losses. Our results have implications beyond the fullerene‐based devices studied here, as they demonstrate that careful selection of a mesostructured p‐type transparent semiconductor paves the path to a new type of efficient single photoactive material solar cells.
  • Inversion symmetry and bulk Rashba effect in methylammonium lead iodide perovskite single crystals

    Frohna, Kyle; Deshpande, Tejas; Harter, John; Peng, Wei; Barker, Bradford A.; Neaton, Jeffrey B.; Louie, Steven G.; Bakr, Osman; Hsieh, David; Bernardi, Marco (Springer Nature, 2018-05-02)
    Methylammonium lead iodide perovskite (MAPbI3) exhibits long charge carrier lifetimes that are linked to its high efficiency in solar cells. Yet, the mechanisms governing these unusual carrier dynamics are not completely understood. A leading hypothesis-disproved in this work-is that a large, static bulk Rashba effect slows down carrier recombination. Here, using second harmonic generation rotational anisotropy measurements on MAPbI3 crystals, we demonstrate that the bulk structure of tetragonal MAPbI3 is centrosymmetric with I4/mcm space group. Our calculations show that a significant Rashba splitting in the bandstructure requires a non-centrosymmetric lead iodide framework, and that incorrect structural relaxations are responsible for the previously predicted large Rashba effect. The small Rashba splitting allows us to compute effective masses in excellent agreement with experiment. Our findings rule out the presence of a large static Rashba effect in bulk MAPbI3, and our measurements find no evidence of dynamic Rashba effects.
  • Accurate Extraction of Charge Carrier Mobility in 4-Probe Field-Effect Transistors

    Choi, Hyun Ho; Rodionov, Yaroslav I.; Paterson, Alexandra F.; Panidi, Julianna; Saranin, Danila; Kharlamov, Nikolai; Didenko, Sergei I.; Anthopoulos, Thomas D.; Cho, Kilwon; Podzorov, Vitaly (Wiley, 2018-04-30)
    Charge carrier mobility is an important characteristic of organic field-effect transistors (OFETs) and other semiconductor devices. However, accurate mobility determination in FETs is frequently compromised by issues related to Schottky-barrier contact resistance, that can be efficiently addressed by measurements in 4-probe/Hall-bar contact geometry. Here, it is shown that this technique, widely used in materials science, can still lead to significant mobility overestimation due to longitudinal channel shunting caused by voltage probes in 4-probe structures. This effect is investigated numerically and experimentally in specially designed multiterminal OFETs based on optimized novel organic-semiconductor blends and bulk single crystals. Numerical simulations reveal that 4-probe FETs with long but narrow channels and wide voltage probes are especially prone to channel shunting, that can lead to mobilities overestimated by as much as 350%. In addition, the first Hall effect measurements in blended OFETs are reported and how Hall mobility can be affected by channel shunting is shown. As a solution to this problem, a numerical correction factor is introduced that can be used to obtain much more accurate experimental mobilities. This methodology is relevant to characterization of a variety of materials, including organic semiconductors, inorganic oxides, monolayer materials, as well as carbon nanotube and semiconductor nanocrystal arrays.
  • Low-Temperature Deposition of Layered SnSe2 for Heterojunction Diodes

    Serna, Martha I.; Hasan, Syed M. N.; Nam, S.; El Bouanani, Lidia; Moreno, Salvador; Choi, Hyunjoo; Alshareef, Husam N.; Minary-Jolandan, Majid; Quevedo-Lopez, Manuel A. (Wiley, 2018-04-27)
    Tin diselenide (SnSe) has been recently investigated as an alternative layered metal dichalcogenide due to its unique electrical and optoelectronics properties. Although there are several reports on the deposition of layered crystalline SnSe films by chemical and physical methods, synthesis methods like pulsed laser deposition (PLD) are not reported. An attractive feature of PLD is that it can be used to grow 2D films over large areas. In this report, a deposition process to grow stoichiometric SnSe on different substrates such as single crystals (Sapphire) and amorphous oxides (SiO and HfO) is reported. A detailed process flow for the growth of 2D SnSe at temperatures of 300 °C is presented, which is substantially lower than temperatures used in chemical vapor deposition and molecular beam epitaxy. The 2D SnSe films exhibit a mobility of ≈4.0 cm V s, and are successfully used to demonstrate SnSe/p-Si heterojunction diodes. The diodes show I /I ratios of 10-10 with a turn on voltage of <0.5 V, and ideality factors of 1.2-1.4, depending on the SnSe film growth conditions.
  • Critical review of the molecular design progress in non-fullerene electron acceptors towards commercially viable organic solar cells

    Wadsworth, Andrew; Moser, Maximilian; Marks, Adam; Little, Mark S.; Gasparini, Nicola; Brabec, Christoph J.; Baran, Derya; McCulloch, Iain (Royal Society of Chemistry (RSC), 2018-04-26)
    Fullerenes have formed an integral part of high performance organic solar cells over the last 20 years, however their inherent limitations in terms of synthetic flexibility, cost and stability have acted as a motivation to develop replacements; the so-called non-fullerene electron acceptors. A rapid evolution of such materials has taken place over the last few years, yielding a number of promising candidates that can exceed the device performance of fullerenes and provide opportunities to improve upon the stability and processability of organic solar cells. In this review we explore the structure-property relationships of a library of non-fullerene acceptors, highlighting the important chemical modifications that have led to progress in the field and provide an outlook for future innovations in electron acceptors for use in organic photovoltaics.
  • Nature Inspired Plasmonic Structures: Influence of Structural Characteristics on Sensing Capability

    Perozziello, Gerardo; Candeloro, Patrizio; Coluccio, Maria; Das, Godind; Rocca, Loredana; Pullano, Salvatore; Fiorillo, Antonino; De Stefano, Mario; Di Fabrizio, Enzo M. (MDPI AG, 2018-04-26)
    Surface enhanced Raman scattering (SERS) is a powerful analytical technique that allows the enhancement of a Raman signal in a molecule or molecular assemblies placed in the proximity of nanostructured metallic surfaces, due to plasmonic effects. However, laboratory methods to obtain of these prototypes are time-consuming, expensive and they do not always lead to the desired result. In this work, we analyse structures existing in nature that show, on a nanoscale, characteristic conformations of photonic crystals. We demonstrate that these structures, if covered with gold, change into plasmonic nanostructures and are able to sustain the SERS effect. We study three different structures with this property: opal, a hydrated amorphous form of silica (SiO·nHO); diatoms, a kind of unicellular alga; and peacock tail feather. Rhodamine 6G (down to 10 M) is used to evaluate their capability to increase the Raman signal. These results allow us to define an alternative way to obtain a high sensitivity in Raman spectroscopy, currently achieved by a long and expensive technique, and to fabricate inexpensive nanoplasmonic structures which could be integrated into optical sensors.
  • Alloying as a Route to Monolayer Transition Metal Dichalcogenides with Improved Optoelectronic Performance: Mo(S1–xSex)2 and Mo1–yWyS2

    Shi, Zhiming; Zhang, Qingyun; Schwingenschlögl, Udo (American Chemical Society (ACS), 2018-04-26)
    On the basis of first-principles and cluster expansion calculations, we propose an effective approach to realize monolayer transition metal dichalcogenides with sizable band gaps and improved optoelectronic performance. We show that monolayer Mo(S1–xSex)2 and Mo1–yWyS2 with x = 1/3, 2/3 and y = 1/3, 1/2, 2/3 are stable according to phonon calculations and realize 1T′ or 1T″ phases. The transition barriers from the 2H phase are lower than for monolayer MoS2, implying that the 1T′ or 1T″ phases can be achieved experimentally. Furthermore, it turns out that the 1T″ monolayer alloys with x = 1/3, 2/3 and y = 1/3, 2/3 are semiconductors with band gaps larger than 1 eV, due to trimerization. The visible light absorption and carrier mobility are strongly improved as compared to 2H monolayer MoS2, MoSe2, and WS2. Thus, the 1T″ monolayer alloys have the potential to expand the applications of transition metal dichalcogenides, for example, in solar cells.

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