• Solution-Processed Smart Window Platforms Based on Plasmonic Electrochromics

      Abbas, Sara (2018-04-30) [Dissertation]
      Advisor: Amassian, Aram
      Committee members: Baran, Derya; Nunes, Suzana Pereira; Li, Lain-Jong
      Electrochromic smart windows offer a viable route to reducing the consumption of buildings energy, which represents about 30% of the worldwide energy consumption. Smart windows are far more compelling than current static windows in that they can dynamically modulate the solar spectrum depending on climate and lighting conditions or simply to meet personal preferences. The latest generation of smart windows relies on nominally transparent metal oxide nanocrystal materials whose chromism can be electrochemically controlled using the plasmonic effect. Plasmonic electrochromic materials selectively control the near infrared (NIR) region of the solar spectrum, responsible for solar heat, without affecting the visible transparency. This is in contrast to conventional electrochromic materials which block both the visible and NIR and thus enables electrochromic devices to reduce the energy consumption of a building or a greenhouse in warm climate regions due to enhancements of both visible lighting and heat blocking. Despite this edge, this technology can benefit from important developments, including low-cost solution-based manufacturing on flexible substrates while maintaining durability and coloration efficiency, demonstration of independent control in the NIR and visible spectra, and demonstration of self-powering capabilities. This thesis is focused on developing low-temperature and all-solution processed plasmonic electrochromic devices and dual-band electrochromic devices. We demonstrate new device fabrication approaches in terms of materials and processes which enhance electrochromic performance all the while maintaining low processing temperatures. Scalable fabrication methods are used to highlight compatibility with high throughput, continuous roll-to-roll fabrication on flexible substrates. In addition, a dualband plasmonic electrochromic device was developed by combining the plasmonic layer with a conventional electrochromic ion storage layer. This enables independent control of the transmittance of NIR and visible spectra and is done without time- and energyintensive synthesis and processing methods. We have fabricated self-powered smart windows by integrating the plasmonic and dual-band devices with organic photovoltaic mini-modules and introduced static color bias with the help of photonic crystals to explore a few possibilities of multi-platform building integration.
    • 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 (Advanced Functional Materials, Wiley, 2018-04-30) [Article]
      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. (Advanced Materials Interfaces, Wiley, 2018-04-27) [Article]
      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 (Chemical Society Reviews, Royal Society of Chemistry (RSC), 2018-04-26) [Article]
      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. (Applied Sciences, MDPI AG, 2018-04-26) [Article]
      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 (ACS Applied Energy Materials, American Chemical Society (ACS), 2018-04-26) [Article]
      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.
    • Solution-Processed In2O3/ZnO Heterojunction Electron Transport Layers for Efficient Organic Bulk Heterojunction and Inorganic Colloidal Quantum-Dot Solar Cells

      Eisner, Flurin; Seitkhan, Akmaral; Han, Yang; Khim, Dongyoon; Yengel, Emre; Kirmani, Ahmad R.; Xu, Jixian; García de Arquer, F. Pelayo; Sargent, Edward H.; Amassian, Aram; Fei, Zhuping; Heeney, Martin; Anthopoulos, Thomas D. (Solar RRL, Wiley, 2018-04-25) [Article]
      We report the development of a solution-processed In2O3/ZnO heterojunction electron transport layer (ETL) and its application in high efficiency organic bulk-heterojunction (BHJ) and inorganic colloidal quantum dot (CQD) solar cells. Study of the electrical properties of this low-dimensional oxide heterostructure via field-effect measurements reveals that electron transport along the heterointerface is enhanced by more than a tenfold when compared to the individual single-layer oxides. Use of the heterojunction as the ETL in organic BHJ photovoltaics is found to consistently improve the cell's performance due to the smoothening of the ZnO surface, increased electron mobility and a noticeable reduction in the cathode's work function, leading to a decrease in the cells’ series resistance and a higher fill factor (FF). Specifically, non-fullerene based organic BHJ solar cells based on In2O3/ZnO ETLs exhibit very high power conversion efficiencies (PCE) of up to 12.8%, and high FFs of over 70%. The bilayer ETL concept is further extended to inorganic lead-sulphide CQD solar cells. Resulting devices exhibit excellent performance with a maximum PCE of 8.2% and a FF of 56.8%. The present results highlight the potential of multilayer oxides as novel ETL systems and lay the foundation for future developments.
    • Multidirection Piezoelectricity in Mono- and Multilayered Hexagonal α-In2Se3

      Xue, Fei; Zhang, Junwei; Hu, Weijin; Hsu, Wei-Ting; Han, Ali; Leung, Siu; Huang, Jing-Kai; Wan, Yi; Liu, Shuhai; Zhang, Junli; He, Jr-Hau; Chang, Wen-Hao; Wang, Zhong Lin; Zhang, Xixiang; Li, Lain-Jong (ACS Nano, American Chemical Society (ACS), 2018-04-25) [Article]
      Piezoelectric materials have been widely used for sensors, actuators, electronics, and energy conversion. Two-dimensional (2D) ultrathin semiconductors, such as monolayer h-BN and MoS2 with their atom-level geometry, are currently emerging as new and attractive members of the piezoelectric family. However, their piezoelectric polarization is commonly limited to the in-plane direction of odd-number ultrathin layers, largely restricting their application in integrated nanoelectromechanical systems. Recently, theoretical calculations have predicted the existence of out-of-plane and in-plane piezoelectricity in monolayer α-In2Se3. Here, we experimentally report the coexistence of out-of-plane and in-plane piezoelectricity in monolayer to bulk α-In2Se3, attributed to their noncentrosymmetry originating from the hexagonal stacking. Specifically, the corresponding d33 piezoelectric coefficient of α-In2Se3 increases from 0.34 pm/V (monolayer) to 5.6 pm/V (bulk) without any odd-even effect. In addition, we also demonstrate a type of α-In2Se3-based flexible piezoelectric nanogenerator as an energy-harvesting cell and electronic skin. The out-of-plane and in-plane piezoelectricity in α-In2Se3 flakes offers an opportunity to enable both directional and nondirectional piezoelectric devices to be applicable for self-powered systems and adaptive and strain-tunable electronics/optoelectronics.
    • A triphenylamine-based push-pull – σ – C60 dyad as photoactive molecular material for single-component organic solar cells: synthesis, characterizations and photophysical properties

      Labrunie, Antoine; Gorenflot, Julien; Babics, Maxime; Aleveque, Olivier; Dabos-Seignon, Sylvie; Balawi, Ahmed H.; Kan, Zhipeng; Wohlfahrt, Markus; Levillain, Eric; Hudhomme, Pietrick; Beaujuge, Pierre; Laquai, Frédéric; Cabanetos, Clément; Blanchard, Philippe (Chemistry of Materials, American Chemical Society (ACS), 2018-04-23) [Article]
      A push-pull – σ – C60 molecular dyad was synthesized via Huisgen-type click-chemistry and used as photoactive material for single-component organic solar cells. Steady-state photoluminescence (PL) experiments of the dyad in solution show a significant quenching of the emission of the push-pull moiety. Spin-casting of a solution of the dyad results in homogenous and smooth thin-films, which exhibit complete PL quenching in line with ultrafast photo-induced electron-transfer in the solid-state. Spectro-electrochemistry reveals the optical signatures of radical cations and radical anions. Evaluation of the charge carrier mobility by space-charge limited current measurements gives an electron-mobility of μe = 4.3 × 10-4 cm2 V-1 s-1, ca. 50 times higher than the hole-mobility. Single-component organic solar cells yield an open-circuit voltage Voc of 0.73 V and a short-circuit current density of 2.1 mA cm-2 however, a poor fill-factor FF (29%) is obtained, resulting in low power conversion efficiency of only 0.4%. Combined TA and time-delayed collection field (TDCF) experiments show mostly ultrafast photon-to-charge conversion and a small component of diffusion-limited exciton dissociation, revealing the presence of pure fullerene domains. Furthermore, a strong field dependence of charge generation is observed, governing the device fill factor, which is further reduced by a competition between extraction and fast recombination of separated charges.
    • Plasmonic nanospherical dimers for color pixels

      Alrasheed, Salma; Di Fabrizio, Enzo M. (Nanomaterials and Nanotechnology, SAGE Publications, 2018-04-20) [Article]
      Display technologies are evolving more toward higher resolution and miniaturization. Plasmonic color pixels can offer solutions to realize such technologies due to their sharp resonances and selective scattering and absorption at particular wavelengths. Metal nanosphere dimers are capable of supporting plasmon resonances that can be tuned to span the entire visible spectrum. In this article, we demonstrate numerically bright color pixels that are highly polarized and broadly tuned using periodic arrays of metal nanosphere dimers on a glass substrate. We show that it is possible to obtain RGB pixels in the reflection mode. The longitudinal plasmon resonance of nanosphere dimers along the axis of the dimer is the main contributor to the color of the pixel, while far-field diffractive coupling further enhances and tunes the plasmon resonance. The computational method used is the finite-difference time-domain method. The advantages of this approach include simplicity of the design, bright coloration, and highly polarized function. In addition, we show that it is possible to obtain different colors by varying the angle of incidence, the periodicity, the size of the dimer, the gap, and the substrate thickness.
    • 2D matrix engineering for homogeneous quantum dot coupling in photovoltaic solids

      Xu, Jixian; Voznyy, Oleksandr; Liu, Mengxia; Kirmani, Ahmad R.; Walters, Grant; Munir, Rahim; Abdelsamie, Maged; Proppe, Andrew H.; Sarkar, Amrita; García de Arquer, F. Pelayo; Wei, Mingyang; Sun, Bin; Liu, Min; Ouellette, Olivier; Quintero-Bermudez, Rafael; Li, Jie; Fan, James; Quan, Li Na; Todorovic, Petar; Tan, Hairen; Hoogland, Sjoerd; Kelley, Shana O.; Stefik, Morgan; Amassian, Aram; Sargent, Edward H. (Nature Nanotechnology, Springer Nature, 2018-04-20) [Article]
      Colloidal quantum dots (CQDs) are promising photovoltaic (PV) materials because of their widely tunable absorption spectrum controlled by nanocrystal size1,2. Their bandgap tunability allows not only the optimization of single-junction cells, but also the fabrication of multijunction cells that complement perovskites and silicon 3 . Advances in surface passivation2,4-7, combined with advances in device structures 8 , have contributed to certified power conversion efficiencies (PCEs) that rose to 11% in 2016 9 . Further gains in performance are available if the thickness of the devices can be increased to maximize the light harvesting at a high fill factor (FF). However, at present the active layer thickness is limited to ~300 nm by the concomitant photocarrier diffusion length. To date, CQD devices thicker than this typically exhibit decreases in short-circuit current (JSC) and open-circuit voltage (VOC), as seen in previous reports3,9-11. Here, we report a matrix engineering strategy for CQD solids that significantly enhances the photocarrier diffusion length. We find that a hybrid inorganic-amine coordinating complex enables us to generate a high-quality two-dimensionally (2D) confined inorganic matrix that programmes internanoparticle spacing at the atomic scale. This strategy enables the reduction of structural and energetic disorder in the solid and concurrent improvements in the CQD packing density and uniformity. Consequently, planar devices with a nearly doubled active layer thicknesses (~600 nm) and record values of JSC (32 mA cm-2) are fabricated. The VOC improved as the current was increased. We demonstrate CQD solar cells with a certified record efficiency of 12%.
    • Two-Dimensional Tellurene as Excellent Thermoelectric Material

      Sharma, Sitansh; Singh, Nirpendra; Schwingenschlögl, Udo (ACS Applied Energy Materials, American Chemical Society (ACS), 2018-04-20) [Article]
      We study the thermoelectric properties of two-dimensional tellurene by first-principles calculations and semiclassical Boltzmann transport theory. The HSE06 hybrid functional results in a moderate direct band gap of 1.48 eV at the Γ point. A high room temperature Seebeck coefficient (Sxx = 0.38 mV/K, Syy = 0.36 mV/K) is combined with anisotropic lattice thermal conductivity (κxxl = 0.43 W/m K, κyyl = 1.29 W/m K). Phonon band structures demonstrate a key role of optical phonons in the record low thermal conductivity that leads to excellent thermoelectric performance of tellurene. At room temperature and moderate hole doping of 1.2 × 10–11 cm–2, for example, a figure of merit of ZTxx = 0.8 is achieved.
    • Correlation of the Dzyaloshinskii–Moriya interaction with Heisenberg exchange and orbital asphericity

      Kim, Sanghoon; Ueda, Kohei; Go, Gyungchoon; Jang, Peong-Hwa; Lee, Kyung-Jin; Belabbes, Abderrezak; Manchon, Aurelien; Suzuki, Motohiro; Kotani, Yoshinori; Nakamura, Tetsuya; Nakamura, Kohji; Koyama, Tomohiro; Chiba, Daichi; Yamada, Kihiro. T.; Kim, Duck-Ho; Moriyama, Takahiro; Kim, Kab-Jin; Ono, Teruo (Nature Communications, Springer Nature, 2018-04-19) [Article]
      Chiral spin textures of a ferromagnetic layer in contact to a heavy non-magnetic metal, such as Néel-type domain walls and skyrmions, have been studied intensively because of their potential for future nanomagnetic devices. The Dyzaloshinskii–Moriya interaction (DMI) is an essential phenomenon for the formation of such chiral spin textures. In spite of recent theoretical progress aiming at understanding the microscopic origin of the DMI, an experimental investigation unravelling the physics at stake is still required. Here we experimentally demonstrate the close correlation of the DMI with the anisotropy of the orbital magnetic moment and with the magnetic dipole moment of the ferromagnetic metal in addition to Heisenberg exchange. The density functional theory and the tight-binding model calculations reveal that inversion symmetry breaking with spin–orbit coupling gives rise to the orbital-related correlation. Our study provides the experimental connection between the orbital physics and the spin–orbit-related phenomena, such as DMI.
    • Silica diatom shells tailored with Au nanoparticles enable sensitive analysis of molecules for biological, safety and environment applications

      Onesto, V.; Villani, M.; Coluccio, M. L.; Majewska, R.; Alabastri, A.; Battista, E.; Schirato, A.; Calestani, D.; Coppedé, N.; Cesarelli, M.; Amato, F.; Di Fabrizio, Enzo M.; Gentile, F. (Nanoscale Research Letters, Springer Nature, 2018-04-19) [Article]
      Diatom shells are a natural, theoretically unlimited material composed of silicon dioxide, with regular patterns of pores penetrating through their surface. For their characteristics, diatom shells show promise to be used as low cost, highly efficient drug carriers, sensor devices or other micro-devices. Here, we demonstrate diatom shells functionalized with gold nanoparticles for the harvesting and detection of biological analytes (bovine serum albumin—BSA) and chemical pollutants (mineral oil) in low abundance ranges, for applications in bioengineering, medicine, safety, and pollution monitoring.
    • Tantalum Nitride Electron-Selective Contact for Crystalline Silicon Solar Cells

      Yang, Xinbo; Aydin, Erkan; Xu, Hang; Kang, Jingxuan; Hedhili, Mohamed N.; Liu, Wenzhu; Wan, Yimao; Peng, Jun; Samundsett, Christian; Cuevas, Andres; De Wolf, Stefaan (Advanced Energy Materials, Wiley, 2018-04-19) [Article]
      Minimizing carrier recombination at contact regions by using carrier-selective contact materials, instead of heavily doping the silicon, has attracted considerable attention for high-efficiency, low-cost crystalline silicon (c-Si) solar cells. A novel electron-selective, passivating contact for c-Si solar cells is presented. Tantalum nitride (TaN x ) thin films deposited by atomic layer deposition are demonstrated to provide excellent electron-transporting and hole-blocking properties to the silicon surface, due to their small conduction band offset and large valence band offset. Thin TaNx interlayers provide moderate passivation of the silicon surfaces while simultaneously allowing a low contact resistivity to n-type silicon. A power conversion efficiency (PCE) of over 20% is demonstrated with c-Si solar cells featuring a simple full-area electron-selective TaNx contact, which significantly improves the fill factor and the open circuit voltage (Voc) and hence provides the higher PCE. The work opens up the possibility of using metal nitrides, instead of metal oxides, as carrier-selective contacts or electron transport layers for photovoltaic devices.
    • Current Controlled Magnetization Switching in Cylindrical Nanowires for High-Density 3D Memory Applications

      Mohammed, Hanan; Corte-León, Hector; Ivanov, Yurii P.; Lopatin, Sergei; Moreno, Julian A.; Chuvilin, Andrey; Salimath, Akshaykumar; Manchon, Aurelien; Kazakova, Olga; Kosel, Jürgen (arXiv, 2018-04-18) [Preprint]
      A next-generation memory device utilizing a three-dimensional nanowire system requires the reliable control of domain wall motion. In this letter, domain walls are studied in cylindrical nanowires consisting of alternating segments of cobalt and nickel. The material interfaces acting as domain wall pinning sites, are utilized in combination with current pulses, to control the position of the domain wall, which is monitored using magnetoresistance measurements. Magnetic force microscopy results further confirm the occurrence of current assisted domain wall depinning. Data bits are therefore shifted along the nanowire by sequentially pinning and depinning a domain wall between successive interfaces, a requirement necessary for race-track type memory devices. We demonstrate that the direction, amplitude and duration of the applied current pulses determine the propagation of the domain wall across pinning sites. These results demonstrate a multi-bit cylindrical nanowire device, utilizing current assisted data manipulation. The prospect of sequential pinning and depinning in these nanowires allows the bit density to increase by several Tbs, depending on the number of segments within these nanowires.
    • Device Strategies Directed to Improving the Efficiency of Solution-Processed Organic Solar Cells

      Liang, Ru-Ze (2018-04-18) [Dissertation]
      Advisor: Beaujuge, Pierre
      Committee members: Alshareef, Husam N.; He, Jr-Hau; Jones, David J.
      In the last decade, organic photovoltaics (OPVs) have been attracting much attention for their low cost, and feasibility of mass production in large-area modules. Reported power conversion efficiencies (PCE) of organic solar cells have reached more than 10%. These promising PCEs can be realized by uncovering important principles: (1) rational molecular design, (2) matching of the material energy level, (3) favorable morphology of donor-acceptor (D/A) network, (4) higher carrier mobilities, and (5) suppression of charge recombination within the bulk heterojunction (BHJ). Though these key properties are frequently stated, the relationships between these principles remain unclear, which motivates us to fill these gaps. In the beginning, we show that changing the sequence of donor and acceptor units of the benzodithiophene-core (BDT) SM donors critically impacts molecular packing and charge transport in BHJ solar cells. Moreover, we find out that by adding small amount of the external solvent additive, the domain size of the SMFQ1 become relatively smaller, resulting in the FF enhancement of ~70% and thus pushing PCE to >6.5%. To further improve the device performance, we utilize another technique of device optimization: Solvent Vapor Annealing (SVA). Compared with solvent additive, the SVA creates a solvent-saturated environment for SMs to re-arrange and crystalize, leading to PCE of >8%, with nearly-free bimolecular recombination. When the systems are shifted from fullerene acceptors to nonfullerene acceptors, using solvent additives in indacenodithiophene-core (IDT) systems significantly reduces the domain size from >500nm to <50nm and also allows the SM donors to orderly packed, rising the PCE from <1% to 4.5%. Furthermore in a similar IDT-based system, it shows unexpectedly high VOC and low energy loss, and high PCE > 6% can be reached by employing the dimethyl disulfide (DMDS) as the SVA solvent to re-organize the morphology from excessive mixing to ordered phase-separated D/A network. Lastly, taking advantage of the distinct and complementary absorption of fullerene and nonfullerene acceptors, we show that the SM ternary system successfully realizes the high PCE of 11%, good air stability, and scalable property.
    • Highly Sensitive Sensing of NO and NO2 Gases by Monolayer C3 N

      Babar, Vasudeo Pandurang; Sharma, Sitansh; Schwingenschlögl, Udo (Advanced Theory and Simulations, Wiley, 2018-04-17) [Article]
      Using density functional theory with van der Waals dispersion correction, the adsorption behavior of common gaseous pollutants (CO, NO, NO2, and NH3) on monolayer C3N is investigated. The adsorption sites and energies, binding distances, charge transfers, and electronic band structures are calculated to understand the influence of the adsorbed molecules on the transport properties of monolayer C3N. The current–voltage characteristics are calculated using the nonequilibrium Green's function formalism. It turns out that all investigated molecules are physisorbed on monolayer C3N and that NO and NO2 gases can be sensed with high sensitivity. The recovery time of the sensor is found to be outstanding in the case of NO sensing (2.4 μs at room temperature) and competitive to other materials in the case of NO2 sensing.
    • Rashba effect and enriched spin-valley coupling in GaX / MX2 ( M = Mo, W; X = S, Se, Te) heterostructures

      Zhang, Qingyun; Schwingenschlögl, Udo (Physical Review B, American Physical Society (APS), 2018-04-16) [Article]
      Using first-principles calculations, we investigate the electronic properties of the two-dimensional GaX/MX2 (M = Mo, W; X = S, Se, Te) heterostructures. Orbital hybridization between GaX and MX2 is found to result in Rashba splitting at the valence-band edge around the Γ point, which grows for increasing strength of the spin-orbit coupling in the p orbitals of the chalcogenide atoms. The location of the valence-band maximum in the Brillouin zone can be tuned by strain and application of an out-of-plane electric field. The coexistence of Rashba splitting (in-plane spin direction) and band splitting at the K and K′ valleys (out-of-plane spin direction) makes GaX/MX2 heterostructures interesting for spintronics and valleytronics. They are promising candidates for two-dimensional spin-field-effect transistors and spin-valley Hall effect devices. Our findings shed light on the spin-valley coupling in van der Waals heterostructures.
    • Temperature stability and electrical properties in La-doped KNN-based ceramics

      Lv, Xiang; Wu, Jiagang; Zhu, Jianguo; Xiao, Dingquan; Zhang, Xixiang (Journal of the American Ceramic Society, Wiley, 2018-04-16) [Article]
      To improve the temperature stability and electrical properties of KNN-based ceramics, we simultaneously consider the phase boundary and the addition of rare earth element (La), 0.96K0.5Na0.5Nb0.96Sb0.04O3-0.04(Bi1-xLax)0.5Na0.5ZrO3 (0 ≤ x ≤ 1.0) ceramics. More specifically, we investigate how the phase boundary and the addition of La3+ affect the phase structure, electrical properties, and temperature stability of the ceramic. We show that increasing the La3+ content leads to a change in phase structure, from a rhombohedral-tetragonal (R-T) phase coexistence to a cubic phase. More importantly, we show that the appropriate addition of La3+ (x = 0.2) can simultaneously improve the unipolar strain (from 0.127% to 0.147%) and the temperature stability (i.e., the unipolar strain of 0.147% remains unchanged when T is increased from 25 to 80°C). In addition, we find that the ceramics with x = 0.2 exhibit a large piezoelectric constant (d33) of ~430 pC/N, a high Curie temperature (TC) of ~240°C and a fatigue-free behavior (after 106 electric cycles). The enhanced electrical properties mostly originate from the easy domain switching, whereas the improved temperature stability can be attributed to the R-T phase boundary and the appropriate addition of La3+.