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        Temperature-Dependent Hall and Field-Effect Mobility in Strongly Coupled All-Inorganic Nanocrystal Arrays

        Jang, Jaeyoung,Liu, Wenyong,Son, Jae Sung,Talapin, Dmitri V. American Chemical Society 2014 NANO LETTERS Vol.14 No.2

        <P>We report on the temperature-dependent Hall effect characteristics of nanocrystal (NC) arrays prepared from colloidal InAs NCs capped with metal chalcogenide complex (MCC) ligands (In<SUB>2</SUB>Se<SUB>4</SUB><SUP>2–</SUP> and Cu<SUB>7</SUB>S<SUB>4</SUB><SUP>–</SUP>). Our study demonstrates that Hall effect measurements are a powerful way of exploring the fundamental properties of NC solids. We found that solution-cast 5.3 nm InAs NC films capped with copper sulfide MCC ligands exhibited high Hall mobility values over 16 cm<SUP>2</SUP>/(V s). We also showed that the nature of MCC ligands can control doping in NC solids. The comparative study of the temperature-dependent Hall and field-effect mobility values provides valuable insights concerning the charge transport mechanism and points to the transition from a weak to a strong coupling regime in all-inorganic InAs NC solids.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/nalefd/2014/nalefd.2014.14.issue-2/nl403889u/production/images/medium/nl-2013-03889u_0007.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/nl403889u'>ACS Electronic Supporting Info</A></P>

      • Prospects of Nanoscience with Nanocrystals

        Kovalenko, Maksym V.,Manna, Liberato,Cabot, Andreu,Hens, Zeger,Talapin, Dmitri V.,Kagan, Cherie R.,Klimov, Victor I.,Rogach, Andrey L.,Reiss, Peter,Milliron, Delia J.,Guyot-Sionnnest, Philippe,Konstan American Chemical Society 2015 ACS NANO Vol.9 No.2

        <P>Colloidal nanocrystals (NCs, <I>i.e.</I>, crystalline nanoparticles) have become an important class of materials with great potential for applications ranging from medicine to electronic and optoelectronic devices. Today’s strong research focus on NCs has been prompted by the tremendous progress in their synthesis. Impressively narrow size distributions of just a few percent, rational shape-engineering, compositional modulation, electronic doping, and tailored surface chemistries are now feasible for a broad range of inorganic compounds. The performance of inorganic NC-based photovoltaic and light-emitting devices has become competitive to other state-of-the-art materials. Semiconductor NCs hold unique promise for near- and mid-infrared technologies, where very few semiconductor materials are available. On a purely fundamental side, new insights into NC growth, chemical transformations, and self-organization can be gained from rapidly progressing <I>in situ</I> characterization and direct imaging techniques. New phenomena are constantly being discovered in the photophysics of NCs and in the electronic properties of NC solids. In this Nano Focus, we review the state of the art in research on colloidal NCs focusing on the most recent works published in the last 2 years.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/ancac3/2015/ancac3.2015.9.issue-2/nn506223h/production/images/medium/nn-2014-06223h_0020.gif'></P>

      • Solution-Processed, Ultrathin Solar Cells from CdCl<sub>3</sub><sup>–</sup>-Capped CdTe Nanocrystals: The Multiple Roles of CdCl<sub>3</sub><sup>–</sup> Ligands

        Zhang, Hao,Kurley, J. Matthew,Russell, Jake C.,Jang, Jaeyoung,Talapin, Dmitri V. American Chemical Society 2016 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.138 No.24

        <P>Solution-processed CdTe solar cells using CdTe nanocrystal (NC) ink may offer an economically viable route for large-scale manufacturing. Here we design a new CdCl3--capped CdTe NC ink by taking advantage of novel surface chemistry. In this ink, CdCl3- ligands act as surface ligands, sintering promoters, and dopants. Our solution chemistry allows obtaining very thin continuous layers of high-quality CdTe which is challenging for traditional vapor transport methods. Using benign solvents, in air, and without additional CdCl2 treatment, we obtain a well-sintered CdTe absorber layer from the new ink and demonstrate thin-film solar cells with power conversion efficiency over 10%, a record efficiency for sub 400 nm thick CdTe absorber layer.</P>

      • New Forms of CdSe: Molecular Wires, Gels, and Ordered Mesoporous Assemblies

        Hudson, Margaret H.,Dolzhnikov, Dmitriy S.,Filatov, Alexander S.,Janke, Eric M.,Jang, Jaeyoung,Lee, Byeongdu,Sun, Chengjun,Talapin, Dmitri V. American Chemical Society 2017 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.139 No.9

        <P>This work investigates the structure and properties of soluble chalcogenidocadmates, a molecular form of cadmium chalcogenides with unprecedented one-dimensional bonding motifs. The single crystal X-ray structure reveals that sodium selenocadmate consists of infinite one-dimensional wires of (Cd2Se3)(n)2(n-) charge balanced by Na+ and stabilized by coordinating solvent molecules. Exchanging the sodium cation with tetraethylammonium or didodecyldimethylammonium expands the versatility of selenocadmate by improving its solubility in a variety of polar and nonpolar solvents without changing the anion structure and properties. The introduction of a micelle-forming cationic surfactant allows for the templating of selenocadmate, or the analogous telluride species, to create ordered organic-inorganic hybrid CdSe or CdTe mesostructures. Finally, the interaction of selenocadmate 'wires' with Cd2+ ions creates an unprecedented gel-like form of stoichiometric CdSe. We also demonstrate that these low-dimensional CdSe species show characteristic semiconductor behavior, and can be used in photodetectors and field-effect transistors.</P>

      • Tandem Solar Cells from Solution-Processed CdTe and PbS Quantum Dots Using a ZnTe–ZnO Tunnel Junction

        Crisp, Ryan W.,Pach, Gregory F.,Kurley, J. Matthew,France, Ryan M.,Reese, Matthew O.,Nanayakkara, Sanjini U.,MacLeod, Bradley A.,Talapin, Dmitri V.,Beard, Matthew C.,Luther, Joseph M. American Chemical Society 2017 Nano letters Vol.17 No.2

        <P>We developed a monolithic CdTe–PbS tandem solar cell architecture in which both the CdTe and PbS absorber layers are solution-processed from nanocrystal inks. Due to their tunable nature, PbS quantum dots (QDs), with a controllable band gap between 0.4 and ∼1.6 eV, are a promising candidate for a bottom absorber layer in tandem photovoltaics. In the detailed balance limit, the ideal configuration of a CdTe (<I>E</I><SUB>g</SUB> = 1.5 eV)–PbS tandem structure assumes infinite thickness of the absorber layers and requires the PbS band gap to be 0.75 eV to theoretically achieve a power conversion efficiency (PCE) of 45%. However, modeling shows that by allowing the thickness of the CdTe layer to vary, a tandem with efficiency over 40% is achievable using bottom cell band gaps ranging from 0.68 and 1.16 eV. In a first step toward developing this technology, we explore CdTe–PbS tandem devices by developing a ZnTe–ZnO tunnel junction, which appropriately combines the two subcells in series. We examine the basic characteristics of the solar cells as a function of layer thickness and bottom-cell band gap and demonstrate open-circuit voltages in excess of 1.1 V with matched short circuit current density of 10 mA/cm<SUP>2</SUP> in prototype devices.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/nalefd/2017/nalefd.2017.17.issue-2/acs.nanolett.6b04423/production/images/medium/nl-2016-04423k_0006.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/nl6b04423'>ACS Electronic Supporting Info</A></P>

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