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Träfflista för sökning "L773:0002 7863 ;pers:(Björk Jonas)"

Sökning: L773:0002 7863 > Björk Jonas

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1.
  • Björk, Jonas, et al. (författare)
  • Mechanisms of halogen-based covalent self-assembly on metal surfaces
  • 2013
  • Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 135:15, s. 5768-5775
  • Tidskriftsartikel (refereegranskat)abstract
    • We computationally study the reaction mechanisms of halogen-based covalent self-assembly, a major route for synthesizing molecular nanostructures and nanographenes on surfaces. Focusing on biphenyl as a small model system, we describe the dehalogenation, recombination, and diffusion processes. The kinetics of the different processes are also investigated, in particular how diffusion and coupling barriers affect recombination rates. Trends across the periodic table are derived from three commonly used close-packed (111) surfaces (Cu, Ag, and Au) and two halogens (Br and I). We show that the halogen atoms can poison the surface, thus hindering long-range ordering of the self-assembled structures. Finally, we present core-level shifts of the relevant carbon and halogen atoms, to provide reference data for reliably detecting self-assembly without the need for atomic-resolution scanning tunneling microscopy.
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2.
  • Björk, Jonas, et al. (författare)
  • Zipping Up: Cooperativity Drives the Synthesis of Graphene Nanoribbons
  • 2011
  • Ingår i: Journal of the American Chemical Society. - : American Chemical Society. - 0002-7863 .- 1520-5126. ; 133:38, s. 14884-14887
  • Tidskriftsartikel (refereegranskat)abstract
    • We investigate the cooperative effects controlling the synthesis of a graphene nanoribbon on the Au(111) surface starting from an anthracene polymer using density functional calculations including van der Waals interactions. We focus on the high-temperature cyclodehydrogenation step of the reaction and find that the reaction proceeds by simultaneously transferring two H-atoms from the anthracene units to the Au surface, leaving behind a C C bond in the process. This step is significantly more favorable than the three other potential reaction paths. Moreover, we find that successive dehydrogenations proceed from one end of the polyanthracene and propagate step-by-step through the polymer in a domino-like fashion.
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3.
  • Cirera, Borja, et al. (författare)
  • Long-Range Orientational Self-Assembly, Spatially Controlled Deprotonation, and Off-Centered Metalation of an Expanded Porphyrin
  • 2017
  • Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 139:40, s. 14129-14136
  • Tidskriftsartikel (refereegranskat)abstract
    • Expanded porphyrins are large-cavity macro cycles with enormous potential in coordination chemistry, anion sensing, photodynamic therapy, and optoelectronics. In the last two decades, the surface science community has assessed the physicochemical properties of tetrapyrrolic-like macrocydes. However, to date, the sublimation, self-assembly and atomistic insights of expanded porphyrins on surfaces have remained elusive. Here, we show the self-assembly on Au(111) of an expanded aza-porphyrin, namely, an "expanded hemi-spatially-controlled porphyrazine", through a unique growth mechanism based on deprotonation long-range orientational self-assembly. Furthermore, a spatially controlled "writing" protocol on such self-assembled architecture is presented based on the STM tip-induced deprotonation of the inner protons of individual macrocydes. Finally, the capability of these surface-confined macrocydes to host lanthanide elements is assessed, introducing a novel off-centered coordination motif. The presented findings represent a milestone in the fields of porphyrinoid chemistry and surface science, revealing a great potential for novel surface patterning, opening new avenues for molecular level information storage, and boosting the emerging field of surface-confined coordination chemistry involving f-block elements.
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4.
  • Fritton, Massimo, et al. (författare)
  • The Role of Kinetics versus Thermodynamics in Surface-Assisted Ullmann Coupling on Gold and Silver Surfaces
  • 2019
  • Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 141:12, s. 4824-4832
  • Tidskriftsartikel (refereegranskat)abstract
    • Surface-assisted Ullmann coupling is the workhorse of on-surface synthesis. Despite its obvious relevance, many fundamental and mechanistic aspects remain elusive. To shed light on individual reaction steps and their progression with temperature, temperature-programmed X-ray photoelectron spectroscopy (TP-XPS) experiments are performed for a prototypical model system. The activation of the coupling by initial dehalogenation is tracked by monitoring Br 3d core levels, whereas the C 1s signature is used to follow the emergence of metastable organometallic intermediates and their conversion to the final covalent products upon heating in real time. The employed 1,3,5-tris(4-bromophenyl)benzene precursor is comparatively studied on Ag(111) versus Au(111), whereby intermolecular bonds and network topologies are additionally characterized by scanning tunneling microscopy (STM). Besides the well-comprehended differences in activation temperatures for debromination, the thermal progression shows marked differences between the two surfaces. Debromination proceeds rapidly on Ag(111), but is relatively gradual on Au(111). While on Ag(111) debromination is well explained by first-order reaction kinetics, thermodynamics prevail on Au(111), underpinned by a close agreement between experimentally deduced and density functional theory (DFT) calculated reaction enthalpies. Thermodynamically controlled debromination on Au(111) over a large temperature range implies an unexpectedly long lifetime of surface-stabilized radicals prior to covalent coupling, as corroborated by TP-XPS of C is core levels. These insights are anticipated to play an important role regarding our ability to rationally synthesize atomically precise low-dimensional covalent nanostructures on surfaces.
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5.
  • Li, Qing, et al. (författare)
  • Hierarchical Dehydrogenation Reactions on a Copper Surface
  • 2018
  • Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 140:19, s. 6076-6082
  • Tidskriftsartikel (refereegranskat)abstract
    • Hierarchical control of chemical reactions is being considered as one of the most ambitious and challenging topics in modern organic chemistry. In this study, we have realized the one-by-one scission of the X-H bonds (X = N and C) of aromatic amines in a controlled fashion on the Cu(lll) surface. Each dehydrogenation reaction leads to certain metal-organic supramolecular structures, which were monitored in single-bond resolution via scanning tunneling microscopy and noncontact atomic force microscopy. Moreover, the reaction pathways were elucidated from X-ray photoelectron spectroscopy measurements and density functional theory calculations. Our insights pave the way for connecting molecules into complex structures in a more reliable and predictable manner, utilizing carefully tuned stepwise on-surface synthesis protocols.
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6.
  • Li, Xuechao, et al. (författare)
  • Pyridinic Nitrogen Modification for Selective Acetylenic Homocoupling on Au(111)
  • 2023
  • Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 145:8, s. 4545-4552
  • Tidskriftsartikel (refereegranskat)abstract
    • On-surface acetylenic homocoupling has been proposed to construct carbon nanostructures featuring sp hybrid-ization. However, the efficiency of linear acetylenic coupling is far from satisfactory, often resulting in undesired enyne products or cyclotrimerization products due to the lack of strategies to enhance chemical selectivity. Herein, we inspect the acetylenic homocou-pling reaction of polarized terminal alkynes (TAs) on Au(111) with bond-resolved scanning probe microscopy. The replacement of benzene with pyridine moieties significantly prohibits the cyclotrimerization pathway and facilitates the linear coupling to produce well-aligned N-doped graphdiyne nanowires. Combined with density functional theory calculations, we reveal that the pyridinic nitrogen modification substantially differentiates the coupling motifs at the initial C-C coupling stage (head-to-head vs head-to-tail), which is decisive for the preference of linear coupling over cyclotrimerization.
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7.
  • Palma, Carlos-Andres, et al. (författare)
  • Photo-induced C-C reactions on insulators towards photolithography of graphene nanoarchitectures
  • 2014
  • Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 136, s. 4651-4658
  • Tidskriftsartikel (refereegranskat)abstract
    • On-surface chemistry for atomically precise sp2 macromolecules requires top-down lithographic methods on insulating surfaces in order to pattern the long-range complex architectures needed by the semiconductor industry. Here, we fabricate sp2-carbon nm-thin films on insulators and under ultra-high vacuum (UHV) conditions from photo-coupled brominated precursors. We reveal that covalent coupling is initiated by C-Br bond cleavage through photon energies exceeding 4.4 eV, as monitored by laser desorption ionization (LDI) mass spectrometry (MS) and X-ray photoelectron spectroscopy (XPS). Density functional theory (DFT) gives insight into the mechanisms of C-Br scission and C-C coupling processes. Further, unreacted material can be sublimed and the coupled sp2-carbon precursors can be graphitized by e-beam treatment at 500°C, demonstrating promising applications in photolithography of graphene nanoarchitectures. Our results present UV-induced reactions on insulators for the formation of all sp2-carbon architectures, thereby converging top-down lithography and bottom-up on-surface chemistry into technology.
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8.
  • Palma, Carlos-Andres, et al. (författare)
  • Tailoring Bicomponent Supramolecular Nanoporous Networks : Phase Segregation, Polymorphism, and Glasses at the Solid−Liquid Interface
  • 2009
  • Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 131:36, s. 13062-13071
  • Tidskriftsartikel (refereegranskat)abstract
    • We study the formation of four supramolecular bicomponent networks based on four linear modules (linkers) bridging melamine via triple hydrogen-bonds. We explore at the nanoscale level the phenomena of polymorphism and phase segregation which rule the generation of highly crystalline nanoporous patterns self-assembled at the solid-liquid interface. The investigated linkers include two systems exposing diuracil groups in the R and ω position, naphthalene tetracarboxylic diimide and pyromellitic diimide. In situ scanning tunneling microscopy (STM) investigations revealed that, when blended with melamine, out of the four systems, three are able to form two-dimensional (2D) porous architectures, two of which exhibit highly ordered hexagonal structures, while pyromellitic diimide assembles only into one- dimensional (1D) supramolecular arrays. These bicomponent self-assembled monolayers are used as a test bed to gain detailed insight into phase segregation and polymorphism in 2D supramolecular systems by exploring the contribution of hydrogen-bond energy and periodicity, molecular flexibility, concentration and ratio of the components in solution as well as the effect of annealing via time-dependent and temperature-modulated experiments. These comparative studies, obtained through a joint experimental and computational analysis, offer new insights into strategies toward the bottom-up fabrication of highly ordered tunable nanopatterning at interfaces mediated by hydrogen bonds.
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9.
  • Shchyrba, Aneliia, et al. (författare)
  • Controlling the dimensionality of on-surface coordination polymers via endo- or exoligation
  • 2014
  • Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 136:26, s. 9355-9363
  • Tidskriftsartikel (refereegranskat)abstract
    • The formation of on-surface coordination polymers is controlled by the interplay of chemical reactivity and structure of the building blocks, as well as by the orientating role of the substrate registry. Beyond the predetermined patterns of structural assembly, the chemical reactivity of the reactants involved may provide alternative pathways in their aggregation. Organic molecules, which are transformed in a surface reaction, may be subsequently trapped via coordination of homo- or heterometal adatoms, which may also play a role in the molecular transformation. The amino-functionalized perylene derivative, 4,9-diaminoperylene quinone-3,10-diimine (DPDI), undergoes specific levels of dehydrogenation (-1 H-2 or -3 H-2) depending on the nature of the present adatoms (Fe, Co, Ni or Cu). In this way, the molecule is converted to an endo- or an exoligand, possessing a concave or convex arrangement of ligating atoms, which is decisive for the formation of either ID or 2D coordination polymers.
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10.
  • Wang, Junbo, et al. (författare)
  • Influence of Molecular Configurations on the Desulfonylation Reactions on Metal Surfaces
  • 2022
  • Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 144:47, s. 21596-21605
  • Tidskriftsartikel (refereegranskat)abstract
    • On-surface synthesis is a powerful methodology for the fabrication of low-dimensional functional materials. The precursor molecules usually anchor on different metal surfaces via similar configurations. The activation energies are therefore solely determined by the chemical activity of the respective metal surfaces. Here, we studied the influence of the detailed adsorption configuration on the activation energy on different metal surfaces. We systematically studied the desulfonylation homocoupling for a molecular precursor on Au(111) and Ag(111) and found that the activation energy is lower on inert Au(111) than on Ag(111). Combining scanning tunneling microscopy observations, synchrotron radiation photoemission spectroscopy measurements, and density functional theory calculations, we elucidate that the phenomenon arises from different molecule-substrate interactions. The molecular precursors anchor on Au(111) via Au-S interactions, which lead to weakening of the phenyl-S bonds. On the other hand, the molecular precursors anchor on Ag(111) via Ag-O interactions, resulting in the lifting of the S atoms. As a consequence, the activation barrier of the desulfonylation reactions is higher on Ag(111), although silver is generally more chemically active than gold. Our study not only reports a new type of on-surface chemical reaction but also clarifies the influence of detailed adsorption configurations on specific on-surface chemical reactions.
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