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Similar to how carbon can be sculpted into low-dimensional allotropes such as fullerenes, nanotubes, and graphene, the major premise of our research program is that the framework connectivity of atoms for any crystalline solid can be constrained along specific axes to produce stable, single atom or polyhedron thick (<1 nm) dimensionally-reduced derivatives with transformative physical phenomena. Using a combination of synthesis, electronic, optical, and thermal measurements and theoretical simulations we aim to establish a predictive understanding on how the electronic and phonon structure of the parent materials can be altered in this reduced framework and tuned via a surface bound ligand. Bestowing these novel properties onto existing materials is truly only possible on the atomic-scale, and is expected to lead to novel competitive optoelectronics, thermoelectrics, and spintronics. \u00a0Our research is focused along numerous thrusts.<\/p>\n
Current Directions<\/strong><\/h2>\n\u00a0<\/p>\n
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1) 2D Materials Beyond Graphene<\/span><\/strong>\u00a0–\u00a0Since the discovery of single-layer graphene\u2019s unique electronic properties, there has been great interest in the synthesis, properties, and application of single layers of graphene and other inorganic two-dimensional layered sheets. \u00a0We are creating\u00a0new single-\/few-atom thick layered materials that have novel optical, electronic, and magnetic properties and phenomena. \u00a0Major directions in our lab involve creating and understanding\u00a0the properties of new 2D\u00a0topological insulators, and 2D magnets. \u00a0These systems show great potential for\u00a0next generation electronic materials, spintronics, and thermoelectrics.<\/p>\nExample Publications;<\/p>\n
W. L. B. Huey, J. E. Goldberger, \u201cCovalent Functionalization of Two-Dimensional Group 14 Graphane Analogues<\/strong><\/a>\u201c, Chem. Soc. Rev., 47, 2601-2623, 2018. DOI: 10.1039\/C8CS00291F<\/p>\nD. Weber, A. Trout, D. W. McComb, and J. E. Goldberger, \u201cDecomposition-Induced Room Temperature Magnetism of the Na-intercalated Layered Ferromagnet<\/a>\u201d<\/strong> Nano Letters.\u00a019, 5031-5035. (2019)<\/p>\nM.Q. Arguilla,\u00a0J. Katoch,\u00a0K. Krymowski,\u00a0N.\u00a0Cultrara,\u00a0J. Xu,\u00a0X.\u00a0Xi,\u00a0A.\u00a0Hanks,\u00a0S.\u00a0Jiang,\u00a0R.D. Ross,\u00a0R.J. Koch,\u00a0S. Ulstrup,\u00a0A. Bostwick,\u00a0C. Jozwiak,\u00a0E. Rotenberg,\u00a0D. McComb,\u00a0J.\u00a0Shan,\u00a0W.\u00a0Windl,\u00a0R. K. Kawakami\u00a0and J.E. Goldberger, \u201cNaSn2As2: An Exfoliatable Layered van der Waals Zintl Phase<\/a><\/strong>\u201d ACS Nano,\u00a010<\/span>, 9500\u20139508 (2016) \u00a0DOI:\u00a0<\/strong>10.1021\/acsnano.6b04609<\/p>\nE. Bianco, S. Butler, S. Jiang, O. Restrepo, W. Windl, J. Goldberger, “Stability and Exfoliation of Germanane: A Germanium Graphane Analogue<\/a>“<\/strong> ACS Nano, 7, 4414-4421, (2013).<\/p>\nS. Jiang, S. Butler, E. Bianco, O. Restrepo, W. Windl, J.E. Goldberger “Improving\u00a0the stability and optoelectronic properties of germanane via one-step covalent methyl-termination<\/a><\/strong>” Nature Communications 5, 3389 (2014).<\/p>\n\u00a0<\/p>\n
2) “Goniopolar” Materials\u00a0<\/u><\/strong>\u00a0– <\/em><\/strong>The textbook understanding of the electronic properties materials is that a single material gives rise to a single kind of electronic behavior.\u00a0 A material can either be a metal, or a semiconductor which is doped with other elements to produce either p-type or n-type behavior.\u00a0 Then, in almost all modern electronic devices these p-type and n-type regions are connected together for functionality.\u00a0 In characterizing the in-plane and cross-plane electronic properties of NaSn2As2, \u00a0we have discovered a new class of materials that simultaneously behave n-type along one crystallographic axis, and p-type along an orthogonal axis, and established the fundamental mechanism behind this phenomena. \u00a0This opens up the opportunity to potentially fabricate new electronic devices (photovoltaics, thermoelectrics, transistors) in a single crystal simply by changing its shape and contacting different crystal facets. \u00a0Through a combination of computational predictions, single-crystal growth, and measurements, we are continuing to expand the scope of goniopolar materials, developing general solid-state chemistry design principles for these materials, and exploring their applications in new technologies.<\/p>\nExample Publications.<\/p>\n
B. He, Y. Wang, M.Q. Arguilla, N.D. Cultrara, M.R. Scudder, J.E. Goldberger, W. Windl, J. Heremans,\u201d\u00a0The Fermi surface geometrical origin of axis-dependent conduction polar<\/strong><\/a>ity in layered materials<\/strong><\/a>\u00a0Nature Materials.\u00a018<\/strong>,\u00a0568\u2013572 (2019).<\/p>\nY. Wang, K. Koster, A. Ochs, M. R. Scudder, J. P. Heremans, W. Windl, J. E. Goldberger, \u201cThe Chemical Design Principles for Axis-dependent Conduction Polarity<\/strong><\/a>,<\/strong>\u201d J. Am. Chem. Soc.\u00a0142<\/strong>, 2812\u22122822, (2020).<\/p>\n\u00a0A.M. Ochs, P. Gorai, Y. Wang, M.R. Scudder, K. Koster, C. E. Moore, J. P. Heremans, W. Windl, E. Toberer, J.E. Goldberger, \u201cComputationally Guided Discovery of Axis-Dependent Conduction Polarity in NaSnAs Crystals\u201d<\/a> <\/strong>Chemistry of Materials, 33, 3, 946\u2013951 (2021).<\/p>\nM.R. Scudder, B. He, Y. Wang, A. Rai, D. G. Cahill, W. Windl, J. P. Heremans, J. E. Goldberger, accepted.<\/p>\n
3.\u00a0 New Solid-State Heterogeneous Catalysts<\/strong> –\u00a0 <\/strong>There remains a need for new catalysts and electrocatalysts that utilize less energy (i.e. operation at lower temperatures, lower overpotentials), that replace noble metals with earth-abundant elements, and that enable fundamentally new pathways to transform specific reactants into products. Our lab is focused on discovering new heterogeneous catalysts in previously unexplored families of solid-state compounds.\u00a0 As a recent example, we have recently established that BaGa2<\/sub>, a transition metal-free layered intermetallic compounds that reacts with H2<\/sub>\u00a0under moderate conditions to form BaGa2<\/sub>H2<\/sub>, is an excellent alkyne hydrogenation catalyst.<\/p>\nK. Hodge, J. E. Goldberger, \u201cTransition Metal-Free Alkyne Hydrogenation Catalysis with BaGa2, a Hydrogen Absorbing Layered Zintl Phase<\/a><\/strong>.\u201d Journal of the American Chemical Society,\u00a0\u00a0141<\/span>, 51<\/span>, 19969-19972 (2019).<\/span><\/span><\/p>\n\u00a0<\/h2>\nPrevious Directions<\/strong><\/h2>\n\u00a0<\/p>\n
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4) \u00a0Dimensionally-Reduced Metal Chalcogenides<\/span><\/strong> –\u00a0\u00a0 Metal chalcogenides\u00a0are some of the most well-studied classes of materials in the condensed matter research community due to the wealth of interesting physical phenomena and applications. \u00a0We are rationally designing dimensionally reduced variants of these crystalline materials in order to create novel optoelectronic and battery materials.<\/p>\n\u00a0<\/p>\n
Example publications;<\/p>\n
Y.H. Liu, S. H. Porter, J. Goldberger, “Dimensional Reduction of a Layered Metal Chalcogenide into a 1D Near-IR Direct Band Gap Semiconductor<\/a><\/strong>” \u00a0J. Am. Chem. Soc., 134, 5044-7 (2012).<\/p>\nT. Li*, Y.H. Liu*, B. Chitara, J. E. Goldberger “Li Intercalation into 1D TiS2(en) Chains<\/strong><\/a>” (*=co-authors)\u00a0 J. Am. Chem. Soc. 136, 2986-2989 (2014).<\/p>\nT. Li, Z. J. Baum, J. E. Goldberger,\u00a0\u201cA Vanadium Chalcogenide Dicubane\u201d<\/strong><\/a>\u00a0European Journal of Inorganic Chemistry. 2016, 28-32. DOI: 10.1002\/ejic.201501189<\/p>\nR. Morasse, T. Li, Z. Baum, J. E. Goldberger \u00a0“The Rational Synthesis of Dimensionally Reduced TiS2 phases<\/strong><\/a>” Chem. Mater., 26<\/strong> 4776\u20134780 (2014).<\/p>\nT. Li, J. E. Goldberger, “Atomic Scale Derivatives of Solid-State Materials<\/a><\/strong>” Chemistry of Materials.\u00a0\u00a027,<\/span><\/strong>\u00a03549\u20133559, (2015).<\/p>\n\u00a0<\/p>\n
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5) Dynamic Self-assembling 0D\/1D Materials fo<\/span>r Medical Imaging<\/span><\/strong> We are learning how to exploit the superior properties of inorganic and peptide nanomaterials to improve upon the state-of-the-art medical diagnostic and therapeutics.\u00a0 For example, one of\u00a0our long-term goals is to develop clinically translatable agents for detecting cancer using self-assembling peptide materials that contain different metals for imaging (MRI, PET, etc.). \u00a0 We are developing dynamic materials that respond to the chemistry of the tumor microvasculature to enhance the sensitivity of traditional diagnostic and therapeutic agents.<\/p>\n\u00a0<\/p>\n
Example Publications;<\/p>\n
A. Ghosh, M. Haverick, K. Stump, X. Yang, M. Tweedle, and J. Goldberger, \u00a0“Fine-tuning the pH trigger of self-assembly<\/a><\/strong>” \u00a0J. Am. Chem. Soc., 134, 3647-50 (2012).<\/p>\nA. Ghosh, E. T. Dobson, C. Buettner, M. Nicholl, J.E. Goldberger, “Programming pH-Triggered Self-Assembly Transitions via Isomerization of Peptide Sequences.<\/strong><\/a>” Langmuir, 30<\/strong>, 15383\u201315387, (2014).<\/p>\n
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1) 2D Materials Beyond Graphene<\/span><\/strong>\u00a0–\u00a0Since the discovery of single-layer graphene\u2019s unique electronic properties, there has been great interest in the synthesis, properties, and application of single layers of graphene and other inorganic two-dimensional layered sheets. \u00a0We are creating\u00a0new single-\/few-atom thick layered materials that have novel optical, electronic, and magnetic properties and phenomena. \u00a0Major directions in our lab involve creating and understanding\u00a0the properties of new 2D\u00a0topological insulators, and 2D magnets. \u00a0These systems show great potential for\u00a0next generation electronic materials, spintronics, and thermoelectrics.<\/p>\n Example Publications;<\/p>\n W. L. B. Huey, J. E. Goldberger, \u201cCovalent Functionalization of Two-Dimensional Group 14 Graphane Analogues<\/strong><\/a>\u201c, Chem. Soc. Rev., 47, 2601-2623, 2018. DOI: 10.1039\/C8CS00291F<\/p>\n D. Weber, A. Trout, D. W. McComb, and J. E. Goldberger, \u201cDecomposition-Induced Room Temperature Magnetism of the Na-intercalated Layered Ferromagnet<\/a>\u201d<\/strong> Nano Letters.\u00a019, 5031-5035. (2019)<\/p>\n M.Q. Arguilla,\u00a0J. Katoch,\u00a0K. Krymowski,\u00a0N.\u00a0Cultrara,\u00a0J. Xu,\u00a0X.\u00a0Xi,\u00a0A.\u00a0Hanks,\u00a0S.\u00a0Jiang,\u00a0R.D. Ross,\u00a0R.J. Koch,\u00a0S. Ulstrup,\u00a0A. Bostwick,\u00a0C. Jozwiak,\u00a0E. Rotenberg,\u00a0D. McComb,\u00a0J.\u00a0Shan,\u00a0W.\u00a0Windl,\u00a0R. K. Kawakami\u00a0and J.E. Goldberger, \u201cNaSn2As2: An Exfoliatable Layered van der Waals Zintl Phase<\/a><\/strong>\u201d ACS Nano,\u00a010<\/span>, 9500\u20139508 (2016) \u00a0DOI:\u00a0<\/strong>10.1021\/acsnano.6b04609<\/p>\n E. Bianco, S. Butler, S. Jiang, O. Restrepo, W. Windl, J. Goldberger, “Stability and Exfoliation of Germanane: A Germanium Graphane Analogue<\/a>“<\/strong> ACS Nano, 7, 4414-4421, (2013).<\/p>\n S. Jiang, S. Butler, E. Bianco, O. Restrepo, W. Windl, J.E. Goldberger “Improving\u00a0the stability and optoelectronic properties of germanane via one-step covalent methyl-termination<\/a><\/strong>” Nature Communications 5, 3389 (2014).<\/p>\n \u00a0<\/p>\n 2) “Goniopolar” Materials\u00a0<\/u><\/strong>\u00a0– <\/em><\/strong>The textbook understanding of the electronic properties materials is that a single material gives rise to a single kind of electronic behavior.\u00a0 A material can either be a metal, or a semiconductor which is doped with other elements to produce either p-type or n-type behavior.\u00a0 Then, in almost all modern electronic devices these p-type and n-type regions are connected together for functionality.\u00a0 In characterizing the in-plane and cross-plane electronic properties of NaSn2As2, \u00a0we have discovered a new class of materials that simultaneously behave n-type along one crystallographic axis, and p-type along an orthogonal axis, and established the fundamental mechanism behind this phenomena. \u00a0This opens up the opportunity to potentially fabricate new electronic devices (photovoltaics, thermoelectrics, transistors) in a single crystal simply by changing its shape and contacting different crystal facets. \u00a0Through a combination of computational predictions, single-crystal growth, and measurements, we are continuing to expand the scope of goniopolar materials, developing general solid-state chemistry design principles for these materials, and exploring their applications in new technologies.<\/p>\n Example Publications.<\/p>\n B. He, Y. Wang, M.Q. Arguilla, N.D. Cultrara, M.R. Scudder, J.E. Goldberger, W. Windl, J. Heremans,\u201d\u00a0The Fermi surface geometrical origin of axis-dependent conduction polar<\/strong><\/a>ity in layered materials<\/strong><\/a>\u00a0Nature Materials.\u00a018<\/strong>,\u00a0568\u2013572 (2019).<\/p>\n Y. Wang, K. Koster, A. Ochs, M. R. Scudder, J. P. Heremans, W. Windl, J. E. Goldberger, \u201cThe Chemical Design Principles for Axis-dependent Conduction Polarity<\/strong><\/a>,<\/strong>\u201d J. Am. Chem. Soc.\u00a0142<\/strong>, 2812\u22122822, (2020).<\/p>\n \u00a0A.M. Ochs, P. Gorai, Y. Wang, M.R. Scudder, K. Koster, C. E. Moore, J. P. Heremans, W. Windl, E. Toberer, J.E. Goldberger, \u201cComputationally Guided Discovery of Axis-Dependent Conduction Polarity in NaSnAs Crystals\u201d<\/a> <\/strong>Chemistry of Materials, 33, 3, 946\u2013951 (2021).<\/p>\n M.R. Scudder, B. He, Y. Wang, A. Rai, D. G. Cahill, W. Windl, J. P. Heremans, J. E. Goldberger, accepted.<\/p>\n 3.\u00a0 New Solid-State Heterogeneous Catalysts<\/strong> –\u00a0 <\/strong>There remains a need for new catalysts and electrocatalysts that utilize less energy (i.e. operation at lower temperatures, lower overpotentials), that replace noble metals with earth-abundant elements, and that enable fundamentally new pathways to transform specific reactants into products. Our lab is focused on discovering new heterogeneous catalysts in previously unexplored families of solid-state compounds.\u00a0 As a recent example, we have recently established that BaGa2<\/sub>, a transition metal-free layered intermetallic compounds that reacts with H2<\/sub>\u00a0under moderate conditions to form BaGa2<\/sub>H2<\/sub>, is an excellent alkyne hydrogenation catalyst.<\/p>\n K. Hodge, J. E. Goldberger, \u201cTransition Metal-Free Alkyne Hydrogenation Catalysis with BaGa2, a Hydrogen Absorbing Layered Zintl Phase<\/a><\/strong>.\u201d Journal of the American Chemical Society,\u00a0\u00a0141<\/span>, 51<\/span>, 19969-19972 (2019).<\/span><\/span><\/p>\n \u00a0<\/p>\n \u00a0<\/p>\n 4) \u00a0Dimensionally-Reduced Metal Chalcogenides<\/span><\/strong> –\u00a0\u00a0 Metal chalcogenides\u00a0are some of the most well-studied classes of materials in the condensed matter research community due to the wealth of interesting physical phenomena and applications. \u00a0We are rationally designing dimensionally reduced variants of these crystalline materials in order to create novel optoelectronic and battery materials.<\/p>\n \u00a0<\/p>\n Example publications;<\/p>\n Y.H. Liu, S. H. Porter, J. Goldberger, “Dimensional Reduction of a Layered Metal Chalcogenide into a 1D Near-IR Direct Band Gap Semiconductor<\/a><\/strong>” \u00a0J. Am. Chem. Soc., 134, 5044-7 (2012).<\/p>\n T. Li*, Y.H. Liu*, B. Chitara, J. E. Goldberger “Li Intercalation into 1D TiS2(en) Chains<\/strong><\/a>” (*=co-authors)\u00a0 J. Am. Chem. Soc. 136, 2986-2989 (2014).<\/p>\n T. Li, Z. J. Baum, J. E. Goldberger,\u00a0\u201cA Vanadium Chalcogenide Dicubane\u201d<\/strong><\/a>\u00a0European Journal of Inorganic Chemistry. 2016, 28-32. DOI: 10.1002\/ejic.201501189<\/p>\n R. Morasse, T. Li, Z. Baum, J. E. Goldberger \u00a0“The Rational Synthesis of Dimensionally Reduced TiS2 phases<\/strong><\/a>” Chem. Mater., 26<\/strong> 4776\u20134780 (2014).<\/p>\n T. Li, J. E. Goldberger, “Atomic Scale Derivatives of Solid-State Materials<\/a><\/strong>” Chemistry of Materials.\u00a0\u00a027,<\/span><\/strong>\u00a03549\u20133559, (2015).<\/p>\n \u00a0<\/p>\n \u00a0<\/p>\n \u00a0<\/p>\n 5) Dynamic Self-assembling 0D\/1D Materials fo<\/span>r Medical Imaging<\/span><\/strong> We are learning how to exploit the superior properties of inorganic and peptide nanomaterials to improve upon the state-of-the-art medical diagnostic and therapeutics.\u00a0 For example, one of\u00a0our long-term goals is to develop clinically translatable agents for detecting cancer using self-assembling peptide materials that contain different metals for imaging (MRI, PET, etc.). \u00a0 We are developing dynamic materials that respond to the chemistry of the tumor microvasculature to enhance the sensitivity of traditional diagnostic and therapeutic agents.<\/p>\n \u00a0<\/p>\n Example Publications;<\/p>\n A. Ghosh, M. Haverick, K. Stump, X. Yang, M. Tweedle, and J. Goldberger, \u00a0“Fine-tuning the pH trigger of self-assembly<\/a><\/strong>” \u00a0J. Am. Chem. Soc., 134, 3647-50 (2012).<\/p>\n A. Ghosh, E. T. Dobson, C. Buettner, M. Nicholl, J.E. Goldberger, “Programming pH-Triggered Self-Assembly Transitions via Isomerization of Peptide Sequences.<\/strong><\/a>” Langmuir, 30<\/strong>, 15383\u201315387, (2014).<\/p>\n\u00a0<\/h2>\n
Previous Directions<\/strong><\/h2>\n
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