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- 저자 : Malliakas, Christos D. (검색결과 4 건)
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Biswas, Kanishka,Chung, In,Song, Jung-Hwan,Malliakas, Christos D.,Freeman, Arthur J.,Kanatzidis, Mercouri G. American Chemical Society 2013 Inorganic chemistry Vol.52 No.10
<P>Lewis acidic organic ionic liquids provide a novel synthetic medium to prepare new semiconducting chalcogenides, [(Bi<SUB>4</SUB>Te<SUB>4</SUB>Br<SUB>2</SUB>)(Al<SUB>2</SUB>Cl<SUB>5.46</SUB>Br<SUB>0.54</SUB>)]Cl<SUB>2</SUB> (<B>1</B>) and [Bi<SUB>2</SUB>Se<SUB>2</SUB>Br](AlCl<SUB>4</SUB>) (<B>2</B>). Compound <B>1</B> features a cationic [(Bi<SUB>4</SUB>Te<SUB>4</SUB>Br<SUB>2</SUB>)(Al<SUB>2</SUB>Cl<SUB>5.46</SUB>Br<SUB>0.54</SUB>)]<SUP>2+</SUP> three-dimensional framework, while compound <B>2</B> consists of cationic layers of [Bi<SUB>2</SUB>Se<SUB>2</SUB>Br]<SUP>2+</SUP>. Spectroscopically measured band gaps of <B>1</B> and <B>2</B> are ∼0.6 and ∼1.2 eV, respectively. Thermoelectric power measurements of single crystals of <B>1</B> indicate an n-type semiconductor.</P><P>Cationic chalcogenide frameworks are rare, but they can be synthesized in organic ionic liquids containing strong Lewis acids such as AlCl<SUB>3</SUB>. The Lewis acidic nature of the medium is believed to favor the assembly of the cationic chalcogenide [Bi<SUB>2</SUB>Q<SUB>2</SUB>Br]<SUP>+</SUP> frameworks.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/inocaj/2013/inocaj.2013.52.issue-10/ic400782c/production/images/medium/ic-2013-00782c_0005.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ic400782c'>ACS Electronic Supporting Info</A></P>
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Tunneling Electrical Connection to the Interior of Metal–Organic Frameworks
Han, Shuangbing,Warren, Scott C.,Yoon, Seok Min,Malliakas, Christos D.,Hou, Xianliang,Wei, Yanhu,Kanatzidis, Mercouri G.,Grzybowski, Bartosz A. American Chemical Society 2015 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.137 No.25
<P>Metal–organic frameworks (MOFs) are typically poor electrical conductors, which limits their uses in sensors, fuel cells, batteries, and other applications that require electrically conductive, high surface area materials. Although metal nanoclusters (NCs) are often added to MOFs, the electrical properties of these hybrid materials have not yet been explored. Here, we show that adding NCs to a MOF not only imparts moderate electrical conductivity to an otherwise insulating material but also renders it photoconductive, with conductivity increasing by up to 4 orders of magnitude upon light irradiation. Because charge transport occurs via tunneling between spatially separated NCs that occupy a small percent of the MOF’s volume, the pores remain largely open and accessible. While these phenomena are more pronounced in single-MOF crystals (here, Rb-CD-MOFs), they are also observed in films of smaller MOF crystallites (MIL-53). Additionally, we show that in the photoconductive MOFs, the effective diffusion coefficients of electrons can match the typical values of small molecules diffusing through MOFs; this property can open new vistas for the development of MOF electrodes and, in a wider context, of electroactive and light-harvesting MOFs.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2015/jacsat.2015.137.issue-25/jacs.5b03263/production/images/medium/ja-2015-03263s_0007.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja5b03263'>ACS Electronic Supporting Info</A></P>
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Mao, Lingling,Tsai, Hsinhan,Nie, Wanyi,Ma, Lin,Im, Jino,Stoumpos, Constantinos C.,Malliakas, Christos D.,Hao, Feng,Wasielewski, Michael R.,Mohite, Aditya D.,Kanatzidis, Mercouri G. American Chemical Society 2016 Chemistry of materials Vol.28 No.21
<P>Hybrid halide perovskites are emerging semiconducting materials, with a diverse set of remarkable optoelectronic properties. Besides the widely studied three-dimensional (3D) perovskites, two-dimensional (2D) perovskites show significant potential as photovoltaic (PV) active layers while exhibiting high moisture resistance. Here, we report two series of new 2D halide perovskite solid solutions: (HA)Pb1-xSnxI4 and (BZA)(2)Pb1-xSnxI4 (x = 1, 0.75, 0.5, 0.25, 0), where HA stands for the organic spacer histammonium and BZA stands for benzylammonium cations. These compounds are assembled by corner-sharing octahedral [MI6](4-) units stabilizing single-layered, anionic, inorganic perovskite sheets with organic cations filled in between. The optical band gaps are heavily affected by the M-I-M perovksite angles with the band gap steadily decreasing when the angle approaches 180 degrees, ranging from 2.18 eV for (BZA)(2)PbI4 to 2.05 eV for (HA)PbI4. We find an anomalous trend in electronic band gap in the mixed compositions (HA)Pb1-xSnxI4 and (BZA)(2)Pb1-xSnxI4. When Sn substitutes for Pb to form a solid solution, the band gap further decreases to 1.67 eV for (HA)SnI4. The minimum band gap is at x = 0.75 at 1.74 eV. For BZA, the irregular trend is more intense, as all the intermediate compounds (BZA)(2)Pb(1-x)SnxI(4) (x = 0.75, 0.5, 0.25) have even slightly lower band gaps than (BZA)(2)SnI4 (1.89 eV). DFT calculations confirm the pure Pb and Sn compounds are direct band gap semiconductors. Relatively shorter photoluminescence (PL) lifetime in (BZA)2PbI4 than (HA)PbI4 is observed, suggesting faster recombination rates of the carriers. Solution deposited thin films of (HA)PbI4 and (BZA)2PbI4 show drastically different orientations with (HA)PbI4 displaying a perpendicular rather than parallel growth orientation with respect to the substrate, which is more favorable for PV devices. The higher potential in PV applications of the HA system is indicated by device performance, as the champion air stable planar device with the structure ITO/PEDOT:PSS/2D-perovskite/PCBM/Al of (HA)PbI4 achieves a preliminary power conversion efficiency (PCE) of 1.13%, featuring an open-circuit voltage (VOC) of 0.91 V.</P>
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Mercouri G. Kanatzidis: Excellence and Innovations in Inorganic and Solid-State Chemistry
Arachchige, Indika U.,Armatas, Gerasimos S.,Biswas, Kanishka,Subrahmanyam, Kota S.,Latturner, Susan,Malliakas, Christos D.,Manos, Manolis J.,Oh, Youngtak,Polychronopoulou, Kyriaki,P. Poudeu, Pierre. F ACS AMERICAN CHEMICAL SOCIETY 2017 Inorganic Chemistry Vol.56 No.14
<P>Over the last 3-4 decades, solid-state chemistry has emerged as the forefront of materials design and development. The field has revolutionized into a multidisciplinary subject and matured with a scope of new synthetic strategies, new challenges, and opportunities. Understanding the structure is very crucial in the design of appropriate materials for desired applications. Professor Mercouri G. Kanatzidis has encountered both challenges and opportunities during the course of the discovery of many novel materials. Throughout his scientific career, Mercouri and his group discovered several inorganic compounds and pioneered structure-property relationships. We, a few Ph.D. and postdoctoral students, celebrate his 60th birthday by providing a Viewpoint summarizing his contributions to inorganic solid-state chemistry. The topics discussed here are of significant interest to various scientific communities ranging from condensed matter to green energy production.</P>
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