1363 56 18505 2 73133 document 18505 bRatioSourceData.xlsx application/vnd.openxmlformats-officedocument.spreadsheetml.sheet c2862fbd7af4e45a096fdb6749df787d MD5 221931 2024-10-28 13:32:09 https://researchdata.bath.ac.uk/1363/2/bRatioSourceData.xlsx 1363 2 2 application/vnd.openxmlformats-officedocument.spreadsheetml.sheet other en public cc_by

bRatioSourceData.xlsx

data 18506 2 73138 document 18506 tolueneBRatioAnalysis.py text/x-python 2e3c4962264b9e23182184212a309b24 MD5 94009 2024-10-28 13:38:26 https://researchdata.bath.ac.uk/1363/3/tolueneBRatioAnalysis.py 1363 3 3 text/x-python other en public cc_gnu_gpl

tolueneBRatioAnalysis.py

code archive 3587 disk0/00/00/13/63 2024-11-29 09:09:17 2024-11-30 05:52:06 2024-11-29 09:09:17 data_collection show Sloan Peter P.Sloan@bath.ac.uk 0000-0002-0810-8468 University of Bath FALSE Keenan Pieter pk530@bath.ac.uk 0000-0002-9346-7982 University of Bath FALSE Purkiss Rebecca R.M.Purkiss@bath.ac.uk University of Bath FALSE Rusimova Kristina K.R.Rusimova@bath.ac.uk 0000-0002-3679-9948 University of Bath TRUE CA0040 dept_physics Nanoscience, Excited state, Surface science, Atomic manipulation The data used to plot each figure in the paper is provided on a separate sheet in the Excel workbook. The raw experimental data is also included on separate sheets. This dataset contains data supporting the results presented in the paper "Measuring competing outcomes of a single-molecule reaction reveals classical Arrhenius chemical kinetics". It contains the analysed data of single toluene molecule manipulation experiments carried out on the Si(111)-7x7 surface in Excel spreadsheet format. The experiments span the injection bias voltage range of +1.4 eV to +2.2 eV, the injection current range of 25 pA to 900 pA, and three separate injection locations: on top of an adatoms, a molecule, and a restaom. The dataset contains the extracted manipulation probabilities and branching ratios as well as spectroscopy data above faulted corner and toluene faulted middel sites. The atomic resolution of scanning probe microscopy and its ability to excite a molecule locally can give control over the probability of inducing a single-outcome single-molecule reaction. The paper shows our control over the branching ratio between a single-molecule reaction that exhibits two reaction outcomes. Toluene molecules chemisorbed on the Si(111)-7x7 surface at room temperature are induced to react, one at a time, by the tunnelling current of a scanning tunnelling microscope: the molecule either desorbs, or switches to an adjacent surface site. Above a voltage threshold set by the electronics structure of the molecule, we see that the branching ratio between these two outcomes is dependent on the excess energy the exciting electron carries. Using known values and ab inito DFT calculations support our findings, a simple Arrhenius model is developed to describe the intermediate physisorbed state that leads to either desorption or site-switching. We conclude that the excess energy of the exciting electron leads to a heating of the intermediate physisorbed state and hence, via their energy barrier and pre-factors, gives control over the two reaction outcomes. 2024-11-28 University of Bath public RightsHolder University of Bath Engineering and Physical Sciences Research Council (EPSRC) https://doi.org/10.13039/501100000266 EP/X031934/1 Shining light on single molecule dynamics: a pathway to digital chemistry Engineering and Physical Sciences Research Council (EPSRC) https://doi.org/10.13039/501100000266 EP/L015544/1 EPSRC Centre for Doctoral Training in Condensed Matter Physics Royal Society https://doi.org/10.13039/501100000288 RGS\R1\231369 Steering the dynamics of a single electron through atomic-scale surface engineering cent_photon Experiments were performed with an Omicron STM1 microscope operating at room temperature and a base pressure of approximately 1×10⁻¹⁰ mbar. Si(111)-7×7 samples, tungsten tips and toluene molecules were prepared following the procedures outlined in reference 16 of the associated paper. The Si(111)-7×7 surface reconstruction was obtained from pre-cut Si(111) samples (n-type, phosphorus doped, 0.001–0.002 Ω cm) by repeated resistive heating to 1250°C. Tungsten tips were etched in a 2 M NaOH solution and out-gassed in vacuum to remove any tungsten-oxide. Toluene was purified by the freeze-pump-thaw technique with liquid nitrogen and checked for purity with a quadrupole mass spectrometer. We chose toluene for this study because of its thermal stability at room temperature, its ease of STM-induced molecular desorption, and its lack of STM current induced intramolecular bond breaking. To prepare a partially toluene covered surface (approximately 3 molecules per unit cell) the Si(111)−7×7 surface was dosed through a computer-controlled leak valve. Stability during the injection was ensured by a drift-compensation software which limited sample drift to between 100 fm/s and 10 pm/s in each of the x, y and z directions. All voltages are applied to the sample with the tip grounded through a Femto pre-amplifier. Full details of how the data were processed may be found in the supplementary text of the paper. The dataset is in Excel (Office Open XML) spreadsheet format. en 1 10.15125/BATH-01363 https://doi.org/10.1038/s41467-024-54677-1 pub Omicron Scanning Tunnelling Microscope f5d4cd7b-b67d-464c-9d6f-7e400f13dcde open Dataset