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Showing papers on "Heterojunction published in 2014"


Journal Article
TL;DR: In this paper, transient absorption and photoluminescence-quenching measurements were performed to determine the electron-hole diffusion lengths, diffusion constants, and lifetimes in mixed halide and triiodide perovskite absorbers.
Abstract: Organic-inorganic perovskites have shown promise as high-performance absorbers in solar cells, first as a coating on a mesoporous metal oxide scaffold and more recently as a solid layer in planar heterojunction architectures. Here, we report transient absorption and photoluminescence-quenching measurements to determine the electron-hole diffusion lengths, diffusion constants, and lifetimes in mixed halide (CH3NH3PbI(3-x)Cl(x)) and triiodide (CH3NH3PbI3) perovskite absorbers. We found that the diffusion lengths are greater than 1 micrometer in the mixed halide perovskite, which is an order of magnitude greater than the absorption depth. In contrast, the triiodide absorber has electron-hole diffusion lengths of ~100 nanometers. These results justify the high efficiency of planar heterojunction perovskite solar cells and identify a critical parameter to optimize for future perovskite absorber development.

6,454 citations


Journal ArticleDOI
TL;DR: The trap states on the surface and grain boundaries of the perovskite materials are demonstrated to be the origin of photocurrent hysteresis and that the fullerene layers deposited onperovskites can effectively passivate these charge trap states and eliminate the notorious photocurrent Hysteresi.
Abstract: The large photocurrent hysteresis observed in many organometal trihalide perovskite solar cells has become a major hindrance impairing the ultimate performance and stability of these devices, while its origin was unknown. Here we demonstrate the trap states on the surface and grain boundaries of the perovskite materials to be the origin of photocurrent hysteresis and that the fullerene layers deposited on perovskites can effectively passivate these charge trap states and eliminate the notorious photocurrent hysteresis. Fullerenes deposited on the top of the perovskites reduce the trap density by two orders of magnitude and double the power conversion efficiency of CH(3)NH(3)PbI(3) solar cells. The elucidation of the origin of photocurrent hysteresis and its elimination by trap passivation in perovskite solar cells provides important directions for future enhancements to device efficiency.

2,440 citations


Journal ArticleDOI
TL;DR: The use of a thin layer of zinc oxide nanoparticles as an electron-transport layer allows flexible perovskite solar cells to be fabricated with a power conversion efficiency as high as 15.7% as mentioned in this paper.
Abstract: The use of a thin layer of zinc oxide nanoparticles as an electron-transport layer allows flexible perovskite solar cells to be fabricated with a power conversion efficiency as high as 15.7%.

2,402 citations


Journal ArticleDOI
TL;DR: A low-temperature vapor-assisted solution process is demonstrated to construct polycrystalline perovskite thin films with full surface coverage, small surface roughness, and grain size up to microscale, paving the way for high reproducibility of films and devices.
Abstract: Hybrid organic/inorganic perovskites (e.g., CH3NH3PbI3) as light absorbers are promising players in the field of third-generation photovoltaics. Here we demonstrate a low-temperature vapor-assisted solution process to construct polycrystalline perovskite thin films with full surface coverage, small surface roughness, and grain size up to microscale. Solar cells based on the as-prepared films achieve high power conversion efficiency of 12.1%, so far the highest efficiency based on CH3NH3PbI3 with the planar heterojunction configuration. This method provides a simple approach to perovskite film preparation and paves the way for high reproducibility of films and devices. The underlying kinetic and thermodynamic parameters regarding the perovskite film growth are discussed as well.

2,136 citations


Journal ArticleDOI
TL;DR: In this paper, a planar heterojunction CH3NH3PbI3-xCl x solar cells with thin solid films of a perovskite absorber was shown to achieve power conversion efficiencies of up to 11.4% with optimized solution-based film formation.
Abstract: Organometal trihalide perovskite based solar cells have exhibited the highest efficiencies to-date when incorporated into mesostructured composites. However, thin solid films of a perovskite absorber should be capable of operating at the highest efficiency in a simple planar heterojunction configuration. Here, it is shown that film morphology is a critical issue in planar heterojunction CH3NH3PbI3-xCl x solar cells. The morphology is carefully controlled by varying processing conditions, and it is demonstrated that the highest photocurrents are attainable only with the highest perovskite surface coverages. With optimized solution based film formation, power conversion efficiencies of up to 11.4% are achieved, the first report of efficiencies above 10% in fully thin-film solution processed perovskite solar cells with no mesoporous layer. © 2013 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim.

1,856 citations


Journal ArticleDOI
TL;DR: It is shown that hole transfer from the MoS2 layer to the WS2 layer takes place within 50 fs after optical excitation, a remarkable rate for van der Waals coupled two-dimensional layers, which can enable novel two- dimensional devices for optoelectronics and light harvesting.
Abstract: The charge transfer between two layers of different two-dimensional materials occurs at a much faster speed than expected, holding promise for efficient optoelectronic devices. Van der Waals heterostructures have recently emerged as a new class of materials, where quantum coupling between stacked atomically thin two-dimensional layers, including graphene, hexagonal-boron nitride and transition-metal dichalcogenides (MX2), give rise to fascinating new phenomena1,2,3,4,5,6,7,8,9,10. MX2 heterostructures are particularly exciting for novel optoelectronic and photovoltaic applications, because two-dimensional MX2 monolayers can have an optical bandgap in the near-infrared to visible spectral range and exhibit extremely strong light–matter interactions2,3,11. Theory predicts that many stacked MX2 heterostructures form type II semiconductor heterojunctions that facilitate efficient electron–hole separation for light detection and harvesting12,13,14,15,16. Here, we report the first experimental observation of ultrafast charge transfer in photoexcited MoS2/WS2 heterostructures using both photoluminescence mapping and femtosecond pump–probe spectroscopy. We show that hole transfer from the MoS2 layer to the WS2 layer takes place within 50 fs after optical excitation, a remarkable rate for van der Waals coupled two-dimensional layers. Such ultrafast charge transfer in van der Waals heterostructures can enable novel two-dimensional devices for optoelectronics and light harvesting.

1,804 citations


Journal ArticleDOI
TL;DR: It is reported that flat, uniform thin films of this material can be deposited by a one-step, solvent-induced, fast crystallization method involving spin-coating of a DMF solution of CH3NH3PbI3 followed immediately by exposure to chlorobenzene to induce crystallization.
Abstract: Thin-film photovoltaics based on alkylammonium lead iodide perovskite light absorbers have recently emerged as a promising low-cost solar energy harvesting technology. To date, the perovskite layer in these efficient solar cells has generally been fabricated by either vapor deposition or a two-step sequential deposition process. We report that flat, uniform thin films of this material can be deposited by a one-step, solvent-induced, fast crystallization method involving spin-coating of a DMF solution of CH3NH3PbI3 followed immediately by exposure to chlorobenzene to induce crystallization. Analysis of the devices and films revealed that the perovskite films consist of large crystalline grains with sizes up to microns. Planar heterojunction solar cells constructed with these solution-processed thin films yielded an average power conversion efficiency of 13.9±0.7% and a steady state efficiency of 13% under standard AM 1.5 conditions.

1,554 citations


Journal ArticleDOI
TL;DR: The status of understanding of the operation of bulk heterojunction (BHJ) solar cells is reviewed and a summary of the problems to be solved to achieve the predicted power conversion efficiencies of >20% for a single cell is concluded.
Abstract: The status of understanding of the operation of bulk heterojunction (BHJ) solar cells is reviewed. Because the carrier photoexcitation recombination lengths are typically 10 nm in these disordered materials, the length scale for self-assembly must be of order 10–20 nm. Experiments have verified the existence of the BHJ nanostructure, but the morphology remains complex and a limiting factor. Three steps are required for generation of electrical power: i) absorption of photons from the sun; ii) photoinduced charge separation and the generation of mobile carriers; iii) collection of electrons and holes at opposite electrodes. The ultrafast charge transfer process arises from fundamental quantum uncertainty; mobile carriers are directly generated (electrons in the acceptor domains and holes in the donor domains) by the ultrafast charge transfer (≈70%) with ≈30% generated by exciton diffusion to a charge separating heterojunction. Sweep-out of the mobile carriers by the internal field prior to recombination is essential for high performance. Bimolecular recombination dominates in materials where the donor and acceptor phases are pure. Impurities degrade performance by introducing Shockly–Read–Hall decay. The review concludes with a summary of the problems to be solved to achieve the predicted power conversion efficiencies of >20% for a single cell.

1,492 citations


Journal ArticleDOI
15 Sep 2014-ACS Nano
TL;DR: It is proposed that this is due to the electronic passivation of under-coordinated Pb atoms within the crystal, and power conversion efficiencies for solution-processed planar heterojunction solar cells enhanced from 13% for the untreated solar cells to 15.3% and 16.5% for thiophene and pyridine-treated solar cells, respectively.
Abstract: Organic-inorganic metal halide perovskites have recently emerged as a top contender to be used as an absorber material in highly efficient, low-cost photovoltaic devices. Solution-processed semiconductors tend to have a high density of defect states and exhibit a large degree of electronic disorder. Perovskites appear to go against this trend, and despite relatively little knowledge of the impact of electronic defects, certified solar-to-electrical power conversion efficiencies of up to 17.9% have been achieved. Here, through treatment of the crystal surfaces with the Lewis bases thiophene and pyridine, we demonstrate significantly reduced nonradiative electron-hole recombination within the CH(3)NH(3)PbI(3-x)Cl(x) perovskite, achieving photoluminescence lifetimes which are enhanced by nearly an order of magnitude, up to 2 μs. We propose that this is due to the electronic passivation of under-coordinated Pb atoms within the crystal. Through this method of Lewis base passivation, we achieve power conversion efficiencies for solution-processed planar heterojunction solar cells enhanced from 13% for the untreated solar cells to 15.3% and 16.5% for the thiophene and pyridine-treated solar cells, respectively.

1,389 citations


Journal ArticleDOI
TL;DR: This work presents a probabilistic analysis of the chiral stationary phase transition of Na6(CO3)(SO4)2, a mixture of Na2CO3 and Na2SO4 which has shown promise as a raw material for high-performance liquid chromatography.
Abstract: P.-W. Liang, C.-Y. Liao, Dr. C.-C. Chueh, Dr. F. Zuo, S. T. Williams, Dr. X.-K. Xin, Prof. A. K.-Y. Jen Department of Materials Science and Engineering University of Washington Seattle , WA 98195 , USA E-mail: ajen@u.washington.edu Prof. A. K.-Y. Jen Department of Chemistry University of Washington Seattle , WA 98195 , USA C.-Y. Liao, Prof. J. J. Lin Institute of Polymer Science and Engineering National Taiwan University Taipei 106 , Taiwan

1,360 citations


Journal ArticleDOI
TL;DR: It is shown that light-emitting diodes made by stacking metallic graphene, insulating hexagonal boron nitride and various semiconducting monolayers into complex but carefully designed sequences can also provide the basis for flexible and semi-transparent electronics.
Abstract: The advent of graphene and related 2D materials has recently led to a new technology: heterostructures based on these atomically thin crystals. The paradigm proved itself extremely versatile and led to rapid demonstration of tunnelling diodes with negative differential resistance, tunnelling transistors5, photovoltaic devices, etc. Here we take the complexity and functionality of such van der Waals heterostructures to the next level by introducing quantum wells (QWs) engineered with one atomic plane precision. We describe light emitting diodes (LEDs) made by stacking up metallic graphene, insulating hexagonal boron nitride (hBN) and various semiconducting monolayers into complex but carefully designed sequences. Our first devices already exhibit extrinsic quantum efficiency of nearly 10% and the emission can be tuned over a wide range of frequencies by appropriately choosing and combining 2D semiconductors (monolayers of transition metal dichalcogenides). By preparing the heterostructures on elastic and transparent substrates, we show that they can also provide the basis for flexible and semi-transparent electronics. The range of functionalities for the demonstrated heterostructures is expected to grow further with increasing the number of available 2D crystals and improving their electronic quality.

Journal ArticleDOI
25 Jul 2014-ACS Nano
TL;DR: The demonstrated results of monolayer MoS2/Si-based solar cells hold the promise for integration of 2D materials with commercially available Si-based electronics in highly efficient devices.
Abstract: We realized photovoltaic operation in large-scale MoS2 monolayers by the formation of a type-II heterojunction with p-Si. The MoS2 monolayer introduces a built-in electric field near the interface between MoS2 and p-Si to help photogenerated carrier separation. Such a heterojunction photovoltaic device achieves a power conversion efficiency of 5.23%, which is the highest efficiency among all monolayer transition-metal dichalcogenide-based solar cells. The demonstrated results of monolayer MoS2/Si-based solar cells hold the promise for integration of 2D materials with commercially available Si-based electronics in highly efficient devices.

Journal ArticleDOI
17 Jul 2014-ACS Nano
TL;DR: A gate-tunable p–n diode based on a p-type black phosphorus/n-type monolayer MoS2 van der Waals p-n heterojunction is demonstrated, showing promise for broad-band photodetection and solar energy harvesting.
Abstract: Phosphorene, a elemental 2D material, which is the monolayer of black phosphorus, has been mechanically exfoliated recently. In its bulk form, black phosphorus shows high carrier mobility (∼10 000 cm2/V·s) and a ∼0.3 eV direct band gap. Well-behaved p-type field-effect transistors with mobilities of up to 1000 cm2/V·s, as well as phototransistors, have been demonstrated on few-layer black phosphorus, showing its promise for electronics and optoelectronics applications due to its high hole mobility and thickness-dependent direct band gap. However, p–n junctions, the basic building blocks of modern electronic and optoelectronic devices, have not yet been realized based on black phosphorus. In this paper, we demonstrate a gate-tunable p–n diode based on a p-type black phosphorus/n-type monolayer MoS2 van der Waals p–n heterojunction. Upon illumination, these ultrathin p–n diodes show a maximum photodetection responsivity of 418 mA/W at the wavelength of 633 nm and photovoltaic energy conversion with an exter...

Journal ArticleDOI
TL;DR: In this article, the structure of an interdigitated back contact was adopted with crystalline silicon heterojunction solar cells to reduce optical loss from a front grid electrode, a transparent conducting oxide (TCO) layer, and a-Si:H layers as an approach for exceeding the conversion efficiency of 25%.
Abstract: The crystalline silicon heterojunction structure adopted in photovoltaic modules commercialized as Panasonic's HIT has significantly reduced recombination loss, resulting in greater conversion efficiency. The structure of an interdigitated back contact was adopted with our crystalline silicon heterojunction solar cells to reduce optical loss from a front grid electrode, a transparent conducting oxide (TCO) layer, and a-Si:H layers as an approach for exceeding the conversion efficiency of 25%. As a result of the improved short-circuit current (J sc ), we achieved the world's highest efficiency of 25.6% for crystalline silicon-based solar cells under 1-sun illumination (designated area: 143.7 cm 2 ).

Journal ArticleDOI
TL;DR: An important advance in the development of layered semiconductor heterostructures, an essential step towards achieving functional electronics and optoelectronics.
Abstract: Two-dimensional layered semiconductors such as MoS₂ and WSe₂ have attracted considerable interest in recent times. Exploring the full potential of these layered materials requires precise spatial modulation of their chemical composition and electronic properties to create well-defined heterostructures. Here, we report the growth of compositionally modulated MoS₂-MoSe₂ and WS₂-WSe₂ lateral heterostructures by in situ modulation of the vapour-phase reactants during growth of these two-dimensional crystals. Raman and photoluminescence mapping studies demonstrate that the resulting heterostructure nanosheets exhibit clear structural and optical modulation. Transmission electron microscopy and elemental mapping studies reveal a single crystalline structure with opposite modulation of sulphur and selenium distributions across the heterostructure interface. Electrical transport studies demonstrate that the WSe₂-WS₂ heterojunctions form lateral p-n diodes and photodiodes, and can be used to create complementary inverters with high voltage gain. Our study is an important advance in the development of layered semiconductor heterostructures, an essential step towards achieving functional electronics and optoelectronics.

Journal ArticleDOI
TL;DR: Artificial semiconductor heterostructures built from single-layer WSe2 and MoS2 observe a large Stokes-like shift of ∼100 meV between the photoluminescence peak and the lowest absorption peak that is consistent with a type II band alignment having spatially direct absorption but spatially indirect emission.
Abstract: Semiconductor heterostructures are the fundamental platform for many important device applications such as lasers, light-emitting diodes, solar cells, and high-electron-mobility transistors. Analogous to traditional heterostructures, layered transition metal dichalcogenide heterostructures can be designed and built by assembling individual single layers into functional multilayer structures, but in principle with atomically sharp interfaces, no interdiffusion of atoms, digitally controlled layered components, and no lattice parameter constraints. Nonetheless, the optoelectronic behavior of this new type of van der Waals (vdW) semiconductor heterostructure is unknown at the single-layer limit. Specifically, it is experimentally unknown whether the optical transitions will be spatially direct or indirect in such hetero-bilayers. Here, we investigate artificial semiconductor heterostructures built from single-layer WSe2 and MoS2. We observe a large Stokes-like shift of ∼100 meV between the photoluminescence peak and the lowest absorption peak that is consistent with a type II band alignment having spatially direct absorption but spatially indirect emission. Notably, the photoluminescence intensity of this spatially indirect transition is strong, suggesting strong interlayer coupling of charge carriers. This coupling at the hetero-interface can be readily tuned by inserting dielectric layers into the vdW gap, consisting of hexagonal BN. Consequently, the generic nature of this interlayer coupling provides a new degree of freedom in band engineering and is expected to yield a new family of semiconductor heterostructures having tunable optoelectronic properties with customized composite layers.

Journal ArticleDOI
TL;DR: A type-II van der Waals heterojunction made of molybdenum disulfide and tungsten diselenide monolayers and under appropriate gate bias an atomically thin diode is realized, which exhibits a photovoltaic effect.
Abstract: Semiconductor heterostructures form the cornerstone of many electronic and optoelectronic devices and are traditionally fabricated using epitaxial growth techniques. More recently, heterostructures have also been obtained by vertical stacking of two-dimensional crystals, such as graphene and related two-dimensional materials. These layered designer materials are held together by van der Waals forces and contain atomically sharp interfaces. Here, we report on a type-II van der Waals heterojunction made of molybdenum disulfide and tungsten diselenide monolayers. The junction is electrically tunable, and under appropriate gate bias an atomically thin diode is realized. Upon optical illumination, charge transfer occurs across the planar interface and the device exhibits a photovoltaic effect. Advances in large-scale production of two-dimensional crystals could thus lead to a new photovoltaic solar technology.

Journal ArticleDOI
TL;DR: It is demonstrated that seamless high-quality in-plane heterojunctions can be grown between the 2D monolayer semiconductors MoSe2 and WSe2, and their structure is an undistorted honeycomb lattice in which substitution of one transition metal by another occurs across the interface.
Abstract: Heterojunctions between three-dimensional (3D) semiconductors with different bandgaps are the basis of modern light-emitting diodes, diode lasers and high-speed transistors. Creating analogous heterojunctions between different 2D semiconductors would enable band engineering within the 2D plane and open up new realms in materials science, device physics and engineering. Here we demonstrate that seamless high-quality in-plane heterojunctions can be grown between the 2D monolayer semiconductors MoSe2 and WSe2. The junctions, grown by lateral heteroepitaxy using physical vapour transport, are visible in an optical microscope and show enhanced photoluminescence. Atomically resolved transmission electron microscopy reveals that their structure is an undistorted honeycomb lattice in which substitution of one transition metal by another occurs across the interface. The growth of such lateral junctions will allow new device functionalities, such as in-plane transistors and diodes, to be integrated within a single atomically thin layer.

Journal ArticleDOI
TL;DR: In this article, an atomically thin and sharp heterojunction p-n diode can be created by vertically stacking p-type monolayer tungsten diselenide (WSe2) and n-type few-layer molybdenum disulfide (MoS2).
Abstract: The p-n diodes represent the most fundamental device building blocks for diverse optoelectronic functions, but are difficult to achieve in atomically thin transition metal dichalcogenides (TMDs) due to the challenges in selectively doping them into p- or n-type semiconductors. Here, we demonstrate that an atomically thin and sharp heterojunction p-n diode can be created by vertically stacking p-type monolayer tungsten diselenide (WSe2) and n-type few-layer molybdenum disulfide (MoS2). Electrical measurements of the vertically staked WSe2/MoS2 heterojunctions reveal excellent current rectification behavior with an ideality factor of 1.2. Photocurrent mapping shows rapid photoresponse over the entire overlapping region with a highest external quantum efficiency up to 12%. Electroluminescence studies show prominent band edge excitonic emission and strikingly enhanced hot-electron luminescence. A systematic investigation shows distinct layer-number dependent emission characteristics and reveals important insight about the origin of hot-electron luminescence and the nature of electron-orbital interaction in TMDs. We believe that these atomically thin heterojunction p-n diodes represent an interesting system for probing the fundamental electro-optical properties in TMDs and can open up a new pathway to novel optoelectronic devices such as atomically thin photodetectors, photovoltaics, as well as spin- and valley-polarized light emitting diodes, on-chip lasers.

Journal ArticleDOI
31 Jan 2014-Science
TL;DR: The time dependence of the separation of photogenerated electron hole pairs across the donor-acceptor heterojunction in OPV model systems is reported, consistent with charge separation through access to delocalized π-electron states in ordered regions of the fullerene acceptor material.
Abstract: Understanding the charge-separation mechanism in organic photovoltaic cells (OPVs) could facilitate optimization of their overall efficiency. Here we report the time dependence of the separation of photogenerated electron hole pairs across the donor-acceptor heterojunction in OPV model systems. By tracking the modulation of the optical absorption due to the electric field generated between the charges, we measure ~200 millielectron volts of electrostatic energy arising from electron-hole separation within 40 femtoseconds of excitation, corresponding to a charge separation distance of at least 4 nanometers. At this separation, the residual Coulomb attraction between charges is at or below thermal energies, so that electron and hole separate freely. This early time behavior is consistent with charge separation through access to delocalized π-electron states in ordered regions of the fullerene acceptor material.

Journal ArticleDOI
TL;DR: In this paper, the authors investigated the electronic properties of bilayer phosphorene with different stacking orders and found that the direct bandgap of the bilayers can vary from 0.78 to 1.04 eV.
Abstract: Phosphorene, a monolayer of black phosphorus, is promising for nanoelectronic applications not only because it is a natural p-type semiconductor but also because it possesses a layer-number-dependent direct bandgap (in the range of 0.3 to 1.5 eV). On basis of the density functional theory calculations, we investigate electronic properties of the bilayer phosphorene with different stacking orders. We find that the direct bandgap of the bilayers can vary from 0.78 to 1.04 eV with three different stacking orders. In addition, a vertical electric field can further reduce the bandgap to 0.56 eV (at the field strength 0.5 V/A). More importantly, we find that when a monolayer of MoS2 is superimposed with the p-type AA- or AB-stacked bilayer phosphorene, the combined trilayer can be an effective solar-cell material with type-II heterojunction alignment. The power conversion efficiency is predicted to be ∼18 or 16% with AA- or AB-stacked bilayer phosphorene, higher than reported efficiencies of the state-of-the-ar...

Journal ArticleDOI
TL;DR: This work demonstrates large-area (>tens of micrometers) heterostructures of CVD-grown WS2 and MoS2 monolayers, where the interlayer interaction is externally tuned from noncoupling to strong coupling, which opens up venues to creating new material systems with rich functionalities and novel physical effects.
Abstract: Band offsets between different monolayer transition metal dichalcogenides are expected to efficiently separate charge carriers or rectify charge flow, offering a mechanism for designing atomically thin devices and probing exotic two-dimensional physics. However, developing such large-area heterostructures has been hampered by challenges in synthesis of monolayers and effectively coupling neighboring layers. Here, we demonstrate large-area (>tens of micrometers) heterostructures of CVD-grown WS2 and MoS2 monolayers, where the interlayer interaction is externally tuned from noncoupling to strong coupling. Following this trend, the luminescence spectrum of the heterostructures evolves from an additive line profile where each layer contributes independently to a new profile that is dictated by charge transfer and band normalization between the WS2 and MoS2 layers. These results and findings open up venues to creating new material systems with rich functionalities and novel physical effects.

Journal ArticleDOI
TL;DR: In this article, the authors used spray-coating under ambient conditions as a deposition technique for the fabrication of planar heterojunction CH3NH3PbI3−xClx perovskite solar cells.
Abstract: We report the use of ultra-sonic spray-coating under ambient conditions as a deposition technique for the fabrication of planar heterojunction CH3NH3PbI3−xClx perovskite solar cells. We make a first optimization of processing parameter space using this deposition technique, and explore the role of the temperature of the substrate during spray-casting, the volatility of the casting solvent and the post deposition anneal on determining the efficiency of the resultant solar cells. We find that maximum device efficiency is correlated with the creation of dense films having a surface coverage above 85%. When such films are incorporated into a solar cell device, power conversion efficiencies of up to 11% are realized. These results demonstrate that spray-coating can be used in the large-area, low-cost manufacture of high efficiency solution-processed perovskite solar cells.

Journal ArticleDOI
09 Dec 2014-ACS Nano
TL;DR: Through spectroscopic measurements, it is found that electron transfer from the perovskite to the TiO2 in the standard planar junction cells is very slow, so fullerene-modified devices achieve up to 17.3% power conversion efficiency with significantly reduced hysteresis, and stabilized power output reaching 15.7% in the planar p-i-n heterojunction solar cells measured under simulated AM 1.5 sunlight.
Abstract: Organic–inorganic perovskites, such as CH3NH3PbX3 (X = I, Br, Cl), have emerged as attractive absorber materials for the fabrication of low cost high efficiency solar cells. Over the last 3 years, there has been an exceptional rise in power conversion efficiencies (PCEs), demonstrating the outstanding potential of these perovskite materials. However, in most device architectures, including the simplest thin-film planar structure, a current–voltage response displays an “anomalous hysteresis”, whereby the power output of the cell varies with measurement time, direction and light exposure or bias history. Here we provide insight into the physical processes occurring at the interface between the n-type charge collection layer and the perovskite absorber. Through spectroscopic measurements, we find that electron transfer from the perovskite to the TiO2 in the standard planar junction cells is very slow. By modifying the n-type contact with a self-assembled fullerene monolayer, electron transfer is “switched on...

Journal ArticleDOI
24 Nov 2014-ACS Nano
TL;DR: It is proved that ultrafast transfer of electrons from MoSe2 to MoS2 layers, despite the strong Coulomb attraction from the holes in the resonantly excited excitons, can be accomplished on an ultrafast time scale, as observed by measuring the differential reflection of a probe tuned to theMoSe2 resonance.
Abstract: We observe subpicosecond charge separation and formation of indirect excitons a van der Waals heterostructure formed by molybdenum disulfide and molybdenum diselenide monolayers. The sample is fabricated by manually stacking monolayer MoS2 and MoSe2 flakes prepared by mechanical exfoliation. Photoluminescence measurements confirm the formation of an effective heterojunction. In the transient absorption measurements, an ultrafast laser pulse resonantly injects excitons in the MoSe2 layer of the heterostructure. Differential reflection of a probe pulse tuned to the MoS2 exciton resonance is immediately observed following the pump excitation. This proves ultrafast transfer of electrons from MoSe2 to MoS2 layers, despite the strong Coulomb attraction from the holes in the resonantly excited excitons. Conversely, when excitons are selectively injected in MoS2, holes transfer to MoSe2 on an ultrafast time scale, too, as observed by measuring the differential reflection of a probe tuned to the MoSe2 resonance. T...

Journal ArticleDOI
TL;DR: This paper demonstrates a novel technology for constructing large-scale electronic systems based on graphene/molybdenum disulfide (MoS2) heterostructures grown by chemical vapor deposition, and provides a systematic comparison of the graphene/MoS 2 heterojunction contact to more traditional MoS2-metal junctions.
Abstract: Two-dimensional (2D) materials have generated great interest in the past few years as a new toolbox for electronics. This family of materials includes, among others, metallic graphene, semiconducting transition metal dichalcogenides (such as MoS2), and insulating boron nitride. These materials and their heterostructures offer excellent mechanical flexibility, optical transparency, and favorable transport properties for realizing electronic, sensing, and optical systems on arbitrary surfaces. In this paper, we demonstrate a novel technology for constructing large-scale electronic systems based on graphene/molybdenum disulfide (MoS2) heterostructures grown by chemical vapor deposition. We have fabricated high-performance devices and circuits based on this heterostructure, where MoS2 is used as the transistor channel and graphene as contact electrodes and circuit interconnects. We provide a systematic comparison of the graphene/MoS2 heterojunction contact to more traditional MoS2-metal junctions, as well as ...

Journal ArticleDOI
TL;DR: This work addresses the fundamental issue of how these cells work by applying a scanning electron microscopy-based technique to cell cross-sections, and shows the presence of two prime high efficiency locations, one at/near the absorber/hole-blocking-layer, and the second at/ near the absorbers/electron- blocking-layer interfaces, with the former more pronounced.
Abstract: Developments in organic-inorganic lead halide-based perovskite solar cells have been meteoric over the last 2 years, with small-area efficiencies surpassing 15%. We address the fundamental issue of how these cells work by applying a scanning electron microscopy-based technique to cell cross-sections. By mapping the variation in efficiency of charge separation and collection in the cross-sections, we show the presence of two prime high efficiency locations, one at/near the absorber/hole-blocking-layer, and the second at/near the absorber/electron-blocking-layer interfaces, with the former more pronounced. This 'twin-peaks' profile is characteristic of a p-i-n solar cell, with a layer of low-doped, high electronic quality semiconductor, between a p- and an n-layer. If the electron blocker is replaced by a gold contact, only a heterojunction at the absorber/hole-blocking interface remains.

Journal ArticleDOI
TL;DR: Based on ab initio density functional calculations, γ-P and δ-P are proposed as two additional stable structural phases of layered phosphorus besides the layered α-P (black) and β- P (blue) phosphorus allotropes.
Abstract: Based on ab initio density functional calculations, we propose γ-P and δ-P as two additional stable structural phases of layered phosphorus besides the layered α-P (black) and β-P (blue) phosphorus allotropes. Monolayers of some of these allotropes have a wide band gap, whereas others, including γ-P, show a metal-insulator transition caused by in-layer strain or changing the number of layers. An unforeseen benefit is the possibility to connect different structural phases at no energy cost. This becomes particularly valuable in assembling heterostructures with well-defined metallic and semiconducting regions in one contiguous layer.

Journal ArticleDOI
TL;DR: The fabrication of graphene nanoribbon heterojunctions and heterostructures by combining pristine hydrocarbon precursors with their nitrogen-substituted equivalents are reported, and it is shown that these materials bear a high potential for applications in photovoltaics and electronics.
Abstract: p–n junctions are formed in heterostructures made of pristine and nitrogen-doped graphene nanoribbons. Despite graphene's remarkable electronic properties1,2, the lack of an electronic bandgap severely limits its potential for applications in digital electronics3,4. In contrast to extended films, narrow strips of graphene (called graphene nanoribbons) are semiconductors through quantum confinement5,6, with a bandgap that can be tuned as a function of the nanoribbon width and edge structure7,8,9,10. Atomically precise graphene nanoribbons can be obtained via a bottom-up approach based on the surface-assisted assembly of molecular precursors11. Here we report the fabrication of graphene nanoribbon heterojunctions and heterostructures by combining pristine hydrocarbon precursors with their nitrogen-substituted equivalents. Using scanning probe methods, we show that the resulting heterostructures consist of seamlessly assembled segments of pristine (undoped) graphene nanoribbons (p-GNRs) and deterministically nitrogen-doped graphene nanoribbons (N-GNRs), and behave similarly to traditional p–n junctions12. With a band shift of 0.5 eV and an electric field of 2 × 108 V m–1 at the heterojunction, these materials bear a high potential for applications in photovoltaics and electronics.

Journal ArticleDOI
TL;DR: This work demonstrates the use of nm-thick transition metal oxides as a simple and versatile pathway for dopant-free contacts to inorganic semiconductors and has important implications toward enabling a novel class of junctionless devices with applications for solar cells, light-emitting diodes, photodetectors, and transistors.
Abstract: Using an ultrathin (∼15 nm in thickness) molybdenum oxide (MoOx, x < 3) layer as a transparent hole selective contact to n-type silicon, we demonstrate a room-temperature processed oxide/silicon solar cell with a power conversion efficiency of 14.3%. While MoOx is commonly considered to be a semiconductor with a band gap of 3.3 eV, from X-ray photoelectron spectroscopy we show that MoOx may be considered to behave as a high workfunction metal with a low density of states at the Fermi level originating from the tail of an oxygen vacancy derived defect band located inside the band gap. Specifically, in the absence of carbon contamination, we measure a work function potential of ∼6.6 eV, which is significantly higher than that of all elemental metals. Our results on the archetypical semiconductor silicon demonstrate the use of nm-thick transition metal oxides as a simple and versatile pathway for dopant-free contacts to inorganic semiconductors. This work has important implications toward enabling a novel cl...