Force–conductance spectroscopy of a single-molecule reaction

Mejía, Leopoldo; Franco, Ignacio

doi:10.1039/c8sc04830d

Cited by 14 publications

(20 citation statements)

References 75 publications

(82 reference statements)

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“…Exploring chemical reactions at the nanoscale, and ultimately at the single-molecule level, is a topic of significant interest among researchers trying to develop unconventional reactions. [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19] Recently, single-molecule junctions (SMJs), which trap molecules inside a nanogap, have attracted attention as testbeds for probing chemical reactions. [3][4][5][6][7][8][9][10][11][12][13][14][15][16][17] The character-Water splitting is an essential process for converting light energy into easily storable energy in the form of hydrogen.…”

Section: Introductionmentioning

confidence: 99%

“…[+] Present address: Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China istic electronic states of the molecules of interest in the SMJs provide the opportunity to induce unconventional chemical reactions. The unique electronic states of the adsorbed molecule trigger unconventional reactions by ions, [3][4][5] tunnel electrons, [6][7][8] electrostatic effects, [9][10][11][12] mechanical force, [13,14] and light irradiation, [15][16][17][18] Some effectors should be marked as illustrators that induce unique reactions at SMJs, e.g., an external electric field oriented along the reaction axis catalytically promotes chemical reactions at the SMJs. [9][10][11][12] Another example includes localized surface plasmon resonance (LSPR) induced reactions.…”

Section: Introductionmentioning

confidence: 99%

“…Exploring chemical reactions at the nanoscale, and ultimately at the single‐molecule level, is a topic of significant interest among researchers trying to develop unconventional reactions. [ 1–19 ] Recently, single‐molecule junctions (SMJs), which trap molecules inside a nanogap, have attracted attention as testbeds for probing chemical reactions. [ 3–17 ] The characteristic electronic states of the molecules of interest in the SMJs provide the opportunity to induce unconventional chemical reactions.…”

Section: Introductionmentioning

confidence: 99%

“…[ 1–19 ] Recently, single‐molecule junctions (SMJs), which trap molecules inside a nanogap, have attracted attention as testbeds for probing chemical reactions. [ 3–17 ] The characteristic electronic states of the molecules of interest in the SMJs provide the opportunity to induce unconventional chemical reactions. The unique electronic states of the adsorbed molecule trigger unconventional reactions by ions, [ 3–5 ] tunnel electrons, [ 6–8 ] electrostatic effects, [ 9–12 ] mechanical force, [ 13,14 ] and light irradiation, [ 15–18 ] Some effectors should be marked as illustrators that induce unique reactions at SMJs, e.g., an external electric field oriented along the reaction axis catalytically promotes chemical reactions at the SMJs.…”

Section: Introductionmentioning

confidence: 99%

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Water Splitting Induced by Visible Light at a Copper‐Based Single‐Molecule Junction

Fukuzumi

Buerkle

Liu

et al. 2021

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Water splitting is an essential process for converting light energy into easily storable energy in the form of hydrogen. As environmentally preferable catalysts, Cu‐based materials have attracted attention as water‐splitting catalysts. To enhance the efficiency of water splitting, a reaction process should be developed. Single‐molecule junctions (SMJs) are attractive structures for developing these reactions because the molecule electronic state is significantly modulated, and characteristic electromagnetic effects can be expected. Here, water splitting is induced at Cu‐based SMJ and the produced hydrogen is characterized at a single‐molecule scale by employing electron transport measurements. After visible light irradiation, the conductance states originate from Cu/hydrogen molecule/Cu junctions, while before irradiation, only Cu/water molecule/Cu junctions were observed. The vibration spectra obtained from inelastic electron tunneling spectroscopy combined with the first‐principles calculations reveal that the water molecule trapped between the Cu electrodes is decomposed and that hydrogen is produced. Time‐dependent and wavelength‐dependent measurements show that localized‐surface plasmon decomposes the water molecule in the vicinity of the junction. These findings indicate the potential ability of Cu‐based materials for photocatalysis.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Water Splitting Induced by Visible Light at a Copper‐Based Single‐Molecule Junction

Fukuzumi

Buerkle

Liu

et al. 2021

Small

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“…In this case, the complexity in the histograms is of structural origin, such as the heterogeneity in the orientation of the molecule at the junction. The histogram of currents takes a particular form in the presence of external mechanical forces [23][24][25] , with the structural fluctuations affecting both force and conductance. In the offa) Electronic mail: mpz@nist.gov resonance regime and under elastic conditions, the conductance histogram is an indirect map of the values taken by the transmission function.…”

Section: Introductionmentioning

confidence: 99%

Optimal in situ electromechanical sensing of molecular species

Ochoa

Zwolak

2020

The Journal of Chemical Physics

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We investigate protocols for optimal molecular detection with electromechanical nanoscale sensors in ambient conditions. Our models are representative of suspended graphene nanoribbons, which due to their piezoelectric and electronic properties, provide responsive and versatile sensors. In particular, we analytically account for the corrections in the electronic transmission function and signal-to-noise ratio originating in environmental perturbations, such as thermal fluctuations and solvation effects. We also investigate the role of the sampling time in the current statistics. As a result, we formulate a protocol for optimal sensing based on the modulation of the Fermi level at fixed bias, and provide approximate forms for the current, linear susceptibility, and current fluctuations. We show how the algebraic tails in the thermally broadened transmission function affect the behavior of the signal-to-noise ratio and optimal sensing. These results provide further insights into the operation of graphene deflectometers and other techniques for electromechanical sensing.

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Mechano‐Nanoarchitectonics: Design and Function

Ariga

2022

Small Methods

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Mechanical stimuli have rather ambiguous and less‐specific features among various physical stimuli, but most materials exhibit a certain level of responses upon mechanical inputs. Unexplored sciences remain in mechanical responding systems as one of the frontiers of materials science. Nanoarchitectonics approaches for mechanically responding materials are discussed as mechano‐nanoarchitectonics in this review article. Recent approaches on molecular and materials systems with mechanical response capabilities are first exemplified with two viewpoints: i) mechanical control of supramolecular assemblies and materials and ii) mechanical control and evaluation of atom/molecular level structures. In the following sections, special attentions on interfacial environments for mechano‐nanoarchitectonics are emphasized. The section entitled iii) Mechanical Control of Molecular System at Dynamic Interface describes coupling of macroscopic mechanical forces and molecular‐level phenomena. Delicate mechanical forces can be applied to functional molecules embedded at the air–water interface where operation of molecular machines and tuning of molecular receptors upon macroscopic mechanical actions are discussed. Finally, the important role of the interfacial media are further extended to the control of living cells as described in the section entitled iv) Mechanical Control of Biosystems. Pioneering approaches on cell fate regulations at liquid–liquid interfaces are discussed in addition to well‐known mechanobiology.

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Force–conductance spectroscopy of a single-molecule reaction

Abstract: We demonstrate how simultaneous measurements of conductance and force can be used to monitor the step-by-step progress of a mechanically activated cis-to-trans isomerization single-molecule reaction, including events that cannot be distinguished using force or conductance alone.

Cited by 14 publications

References 75 publications

Water Splitting Induced by Visible Light at a Copper‐Based Single‐Molecule Junction

Water Splitting Induced by Visible Light at a Copper‐Based Single‐Molecule Junction

Optimal in situ electromechanical sensing of molecular species

Mechano‐Nanoarchitectonics: Design and Function

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