Dynamic breaking of a single gold bond

Pobelov, Ilya V.; Lauritzen, Kasper Primdal; Yoshida, Kōji; Jensen, Annie Aarup; Mészáros, Gábor; Jacobsen, Karsten Wedel; Strange, Mikkel; Wandlowski, Thomas; Solomon, Gemma C.

doi:10.1038/ncomms15931

Cited by 33 publications

(68 citation statements)

References 31 publications

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“…We hypothesized that the formation of the interconnects of NPs at ambient condition (e.g., room temperature and in air) that starts from the NCs via surface‐mediated mobility of the atoms controlled by atom–substrate interactions creates an SMI pathway toward a conductive network of the atomically connected NPs. The choice of AuCu NCs and NPs, on the one hand, exploits the bimetallic difference, e.g., Au atoms having larger binding strength than Cu atoms, [ 15 ] and the surface mobility difference of the two atoms, and on the other hand, takes advantage of the difference of surface‐mediated Ostwald Ripening (OR) propensity of the two differently sized particles, e.g., NCs having great solubility (involving detachment, diffusion, and reattachment processes) than larger NPs on the surface. The concept of SMI could also be expanded to other types of bimetallic NCs/NPs on surfaces.…”

Section: Figurementioning

confidence: 99%

Surface‐Mediated Interconnections of Nanoparticles in Cellulosic Fibrous Materials toward 3D Sensors

et al. 2020

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Fibrous materials serve as an intriguing class of 3D materials to meet the growing demands for flexible, foldable, biocompatible, biodegradable, disposable, inexpensive, and wearable sensors and the rising desires for higher sensitivity, greater miniaturization, lower cost, and better wearability. The use of such materials for the creation of a fibrous sensor substrate that interfaces with a sensing film in 3D with the transducing electronics is however difficult by conventional photolithographic methods. Here, a highly effective pathway featuring surface‐mediated interconnection (SMI) of metal nanoclusters (NCs) and nanoparticles (NPs) in fibrous materials at ambient conditions is demonstrated for fabricating fibrous sensor substrates or platforms. Bimodally distributed gold–copper alloy NCs and NPs are used as a model system to demonstrate the semiconductive‐to‐metallic conductivity transition, quantized capacitive charging, and anisotropic conductivity characteristics. Upon coupling SMI of NCs/NPs as electrically conductive microelectrodes and surface‐mediated assembly (SMA) of the NCs/NPs as chemically sensitive interfaces, the resulting fibrous chemiresistors function as sensitive and selective sensors for gaseous and vaporous analytes. This new SMI–SMA strategy has significant implications for manufacturing high‐performance fibrous platforms to meet the growing demands of the advanced multifunctional sensors and biosensors.

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Section: Figurementioning

confidence: 99%

Surface‐Mediated Interconnections of Nanoparticles in Cellulosic Fibrous Materials toward 3D Sensors

et al. 2020

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“…[16] Such data provide new insight into the nature of the molecule-electrode bonding and intermolecular interactions. [21][22][23][24] However, the binding structural evolution at the atomic level during the stretching processes of a metal-molecule-metal junction is still a key experimental and theoretical challenge.…”

Section: Introductionmentioning

confidence: 99%

Adsorption, Stretching, and Breaking Processes in Single‐Molecule Conductance of para‐Benzenedimethanethiol in Gold Nanogaps: A DFT‐NEGF Theoretical Study**

et al. 2021

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An invited contribution to a Special Collection in memory of Prof. Jingdong Zhang Electrical and mechanical properties of gold-para-benzenedimethanethiol (BDMT)-gold molecular junctions with different binding configurations have been investigated using density functional theory (DFT) combined with a non-equilibrium Green's function (NEGF) approach. We first determined the most stable structure in total electronic energy by geometry optimization of the molecular junction. We then studied how different stretching processes affect the conductance and the stretching forces. Particularly, two stretching modes can bring about different conductance behavior. When only a single-end molecular contact in interfacial configurations at the top and bridge sites is stretched, the molecular conductance first decreases exponentially. This is followed by a flat platform, and finally produced an abrupt conductance drop from the fracture of interfacial chemical bond AuÀ Au. In the junction with a doubleend stretching mode, the fracture of AuÀ S bond occurs either between the sulfur-bonded gold atom and the underlying Au surfaces, or at either of the two AuÀ S bonds in the double-end stretching mode at the top-pyramidal site. The latter interfacial structure consists of a four-Au-atom pyramidal structure adsorbed on gold surface, resulting in a sharp conductance increase just before complete fracture. This is closely associated with resonance tunneling of beta spin electrons in the critical fracture state of interfacial AuÀ S bonds in gold-BDMT-gold molecular junction.

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“…To further corroborate this assumption and get more insight into the uncommon mechanochromic behavior of the SP copolymer, density functional theory (DFT) calculations were performed. Bond breaking under the action of an external force F ext mostly is a stochastic process as it is initiated by thermal fluctuations . Only in case of extremely rapid pulling, thermal effects are overcome and the force corresponding to the maximal derivative of the potential gets visible.…”

Section: Methodsmentioning

confidence: 99%

“…Bond breaking under the action of an external force F ext mostly is as tochastic process as it is initiated by thermal fluctuations. [19][20][21][22] Only in case of extremely rapid pulling,t hermal effects are overcome and the force corresponding to the maximal derivative of the potential gets visible.T he force needed to break abond thus depends on the loading rate a = dF ext /dt. We modeled two SP derivatives,o ne having the SP substitution pattern as in PmmpPand "para,para-pulling direction", and one with the commonly used 6-nitro group (SP-NO 2 )a nd "para, orthopulling direction".…”

Section: Angewandte Chemiementioning

confidence: 99%

“…[19][20][21][22] Only in case of extremely rapid pulling,t hermal effects are overcome and the force corresponding to the maximal derivative of the potential gets visible.T he force needed to break abond thus depends on the loading rate a = dF ext /dt. Bond breaking under the action of an external force F ext mostly is as tochastic process as it is initiated by thermal fluctuations.…”

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confidence: 99%

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A Simply Synthesized, Tough Polyarylene with Transient Mechanochromic Response

Kempe

Brügner²,

Buchheit

et al. 2017

Angew Chem Int Ed

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As imple and high-yielding route to tough polyarylenes of the type poly(meta,meta,para-phenylene) (PmmpP) is developed. PmmpP is tough even in its as-synthesized state which has an intermediate molar mass of M w % 60 kg mol À1 and exhibits outstanding mechanical properties at further optimized molecular weight of M w = 96 kg mol À1 ,E= 0.9 GPa, e = 300 %. Statistical copolymers with para,para-spiropyran (SP) are mechanochromic, and the toughness allows mechanochromism to be investigated. Strained samples instantaneously lose color upon force release.D FT calculations showt his phenomenon to be caused by the PmmpP matrix that allows build-up of sufficiently large forces to be transduced to SP,and the relatively unstable corresponding merocyanine (MC) form arising from the aromatic co-monomer.M Cu nits covalently incorporated into PmmpP show adrastically reduced half life time of 3.1 scompared to 4.5 hobtained for SP derivatives with common 6-nitro substitution.Polyarylenes have intrigued material scientists since the invention of transition-metal-catalyzed cross-coupling reactions. [1,2] In 2007, Schlüter et al. introduced ah igh molecular weight (MW) poly(meta,para-phenylene) (PmpP) by careful selection of catalyst, solvent mixture,c oncentration, and temperature. [3] In their pioneering work ac rude polymer of M w = 83 kg mol À1 was synthesized and the molecular weight further increased to M w = 255 kg mol À1 by fractionation. After fractionation, this material showed at oughness close to that of aromatic polycarbonates (E = 1GPa, e = 122 %). This was aremarkable feat both from asynthetic as well as amaterials science point of view,b ecause polyarylenes are inherently chemically more stable than polycarbonates as aresult of the exclusive presence of aryl-aryl bonds in the backbone. Subsequently,S chlüter et al. investigated various kinked polyarylenes,w ith some of them exhibiting toughness at high molecular weight after fractionation. [3][4][5][6][7] Our interest in tough polyarylenes stems from their potentially ideal use as stable,tough yet amorphous matrices for covalent incorporation of mechanochromic dyes,s uch as spiropyrans (SPs). [8][9][10] SPs isomerize to their colored merocyanine (MC) form under an umber of external stimuli, including force,and can therefore be used as mechanical force sensors. [11][12][13][14][15] Compared to matrix polymers used so far in combination with covalently linked SPs,t ough polyarylenes have several distinct advantages.T heir toughness allows drawing samples and thus to transduce mechanical force to SP.A lso,t hey are typically amorphous,h ence mechanochromism can be investigated within an isotropic matrix which is not possible with semi-crystalline polymers.H erein we show that the nature and high strength of polyarylenes is of striking additional advantage in that high forces can be transduced to SP co-monomers.We found existing methods for kinked polyarylene synthesis to be cumbersome,expensive,and inefficient owing to significant loss of polymer during fractionation. ...

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Dynamic breaking of a single gold bond

Cited by 33 publications

References 31 publications

Surface‐Mediated Interconnections of Nanoparticles in Cellulosic Fibrous Materials toward 3D Sensors

Surface‐Mediated Interconnections of Nanoparticles in Cellulosic Fibrous Materials toward 3D Sensors

Adsorption, Stretching, and Breaking Processes in Single‐Molecule Conductance of para‐Benzenedimethanethiol in Gold Nanogaps: A DFT‐NEGF Theoretical Study**

A Simply Synthesized, Tough Polyarylene with Transient Mechanochromic Response

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