scholarly journals In Situ Formation of N-Heterocyclic Carbene-Bound Single-Molecule Junctions

2018 ◽  
Vol 140 (28) ◽  
pp. 8944-8949 ◽  
Author(s):  
Evan A. Doud ◽  
Michael S. Inkpen ◽  
Giacomo Lovat ◽  
Enrique Montes ◽  
Daniel W. Paley ◽  
...  
2011 ◽  
Vol 6 (6) ◽  
pp. 353-357 ◽  
Author(s):  
Z.-L. Cheng ◽  
R. Skouta ◽  
H. Vazquez ◽  
J. R. Widawsky ◽  
S. Schneebeli ◽  
...  

2021 ◽  
Vol 11 (8) ◽  
pp. 3317
Author(s):  
C.S. Quintans ◽  
Denis Andrienko ◽  
Katrin F. Domke ◽  
Daniel Aravena ◽  
Sangho Koo ◽  
...  

External electric fields (EEFs) have proven to be very efficient in catalysing chemical reactions, even those inaccessible via wet-chemical synthesis. At the single-molecule level, oriented EEFs have been successfully used to promote in situ single-molecule reactions in the absence of chemical catalysts. Here, we elucidate the effect of an EEFs on the structure and conductance of a molecular junction. Employing scanning tunnelling microscopy break junction (STM-BJ) experiments, we form and electrically characterize single-molecule junctions of two tetramethyl carotene isomers. Two discrete conductance signatures show up more prominently at low and high applied voltages which are univocally ascribed to the trans and cis isomers of the carotenoid, respectively. The difference in conductance between both cis-/trans- isomers is in concordance with previous predictions considering π-quantum interference due to the presence of a single gauche defect in the trans isomer. Electronic structure calculations suggest that the electric field polarizes the molecule and mixes the excited states. The mixed states have a (spectroscopically) allowed transition and, therefore, can both promote the cis-isomerization of the molecule and participate in electron transport. Our work opens new routes for the in situ control of isomerisation reactions in single-molecule contacts.


2021 ◽  
Vol 7 (10) ◽  
pp. eabe4365
Author(s):  
Zihao Liu ◽  
Xingxing Li ◽  
Hiroshi Masai ◽  
Xinyi Huang ◽  
Susumu Tsuda ◽  
...  

One of the ultimate goals of analytic chemistry is to efficiently discriminate between amino acids. Here we demonstrate this ability using a single-molecule electrical methodology based on molecular nanocircuits formed from stable graphene-molecule-graphene single-molecule junctions. These molecular junctions are fabricated by covalently bonding a molecular machine featuring a permethylated-β-cyclodextrin between a pair of graphene point contacts. Using pH to vary the type and charge of the amino acids, we find distinct multimodal current fluctuations originating from the different host-guest interactions, consistent with theoretical calculations. These conductance data produce characteristic dwell times and shuttling rates for each amino acid, and allow accurate, statistical real-time, in situ measurements. Testing four amino acids and their enantiomers shows the ability to distinguish between them within a few microseconds, thus paving a facile and precise way to amino acid identification and even single-molecule protein sequencing.


Author(s):  
Shi Li ◽  
Yuxuan Jiang ◽  
Yongfeng Wang ◽  
Stefano Sanvito ◽  
Shimin Hou

2020 ◽  
Author(s):  
María Camarasa-Gómez ◽  
Daniel Hernangómez-Pérez ◽  
Michael S. Inkpen ◽  
Giacomo Lovat ◽  
E-Dean Fung ◽  
...  

Ferrocenes are ubiquitous organometallic building blocks that comprise a Fe atom sandwiched between two cyclopentadienyl (Cp) rings that rotate freely at room temperature. Of widespread interest in fundamental studies and real-world applications, they have also attracted<br>some interest as functional elements of molecular-scale devices. Here we investigate the impact of<br>the configurational degrees of freedom of a ferrocene derivative on its single-molecule junction<br>conductance. Measurements indicate that the conductance of the ferrocene derivative, which is<br>suppressed by two orders of magnitude as compared to a fully conjugated analog, can be modulated<br>by altering the junction configuration. Ab initio transport calculations show that the low conductance is a consequence of destructive quantum interference effects that arise from the hybridization of metal-based d-orbitals and the ligand-based π-system. By rotating the Cp rings, the hybridization, and thus the quantum interference, can be mechanically controlled, resulting in a conductance modulation that is seen experimentally.<br>


2018 ◽  
Author(s):  
Kun Wang ◽  
Andrea Vezzoli ◽  
Iain Grace ◽  
Maeve McLaughlin ◽  
Richard Nichols ◽  
...  

We have used scanning tunneling microscopy to create and study single molecule junctions with thioether-terminated oligothiophene molecules. We find that the conductance of these junctions increases upon formation of charge transfer complexes of the molecules with tetracyanoethene, and that the extent of the conductance increase is greater the longer is the oligothiophene, i.e. the lower is the conductance of the uncomplexed molecule in the junction. We use non-equilibrium Green's function transport calculations to explore the reasons for this theoretically, and find that new resonances appear in the transmission function, pinned close to the Fermi energy of the contacts, as a consequence of the charge transfer interaction. This is an example of a room temperature quantum interference effect, which in this case boosts junction conductance in contrast to earlier observations of QI that result in diminished conductance.<br>


2019 ◽  
Vol 491 (4) ◽  
pp. 5595-5620 ◽  
Author(s):  
Sanson T S Poon ◽  
Richard P Nelson ◽  
Seth A Jacobson ◽  
Alessandro Morbidelli

ABSTRACT The NASA’s Kepler mission discovered ∼700 planets in multiplanet systems containing three or more transiting bodies, many of which are super-Earths and mini-Neptunes in compact configurations. Using N-body simulations, we examine the in situ, final stage assembly of multiplanet systems via the collisional accretion of protoplanets. Our initial conditions are constructed using a subset of the Kepler five-planet systems as templates. Two different prescriptions for treating planetary collisions are adopted. The simulations address numerous questions: Do the results depend on the accretion prescription?; do the resulting systems resemble the Kepler systems, and do they reproduce the observed distribution of planetary multiplicities when synthetically observed?; do collisions lead to significant modification of protoplanet compositions, or to stripping of gaseous envelopes?; do the eccentricity distributions agree with those inferred for the Kepler planets? We find that the accretion prescription is unimportant in determining the outcomes. The final planetary systems look broadly similar to the Kepler templates adopted, but the observed distributions of planetary multiplicities or eccentricities are not reproduced, because scattering does not excite the systems sufficiently. In addition, we find that ∼1 per cent of our final systems contain a co-orbital planet pair in horseshoe or tadpole orbits. Post-processing the collision outcomes suggests that they would not significantly change the ice fractions of initially ice-rich protoplanets, but significant stripping of gaseous envelopes appears likely. Hence, it may be difficult to reconcile the observation that many low-mass Kepler planets have H/He envelopes with an in situ formation scenario that involves giant impacts after dispersal of the gas disc.


Nano Letters ◽  
2012 ◽  
Vol 12 (3) ◽  
pp. 1643-1647 ◽  
Author(s):  
Sriharsha V. Aradhya ◽  
Jeffrey S. Meisner ◽  
Markrete Krikorian ◽  
Seokhoon Ahn ◽  
Radha Parameswaran ◽  
...  

AIP Advances ◽  
2021 ◽  
Vol 11 (6) ◽  
pp. 065015
Author(s):  
Fu Yi ◽  
Xupeng Qi ◽  
Xuexin Zheng ◽  
Huize Yu ◽  
Wenming Bai ◽  
...  

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