Binding energies determined from kinetic energy release measurements following the evaporation of single molecules from the molecular clusters H+(H2O)n, H+(NH3)n and H+(CH3OH)n

Bruzzi, E.; Parajuli, Rajendra Prasad; Stace, A. J.

doi:10.1016/j.ijms.2012.08.003

Cited by 12 publications

(36 citation statements)

References 66 publications

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“…To emphasize the decline in terms of the influence a 2+ charge has on water molecules in the larger complexes, figure 3 compares the binding energy data presented here with those recorded in earlier experiments on H + (H 2 O) n clusters [35], where it was found that, as n increased, the results rapidly converged to a value that was approximately equal to the strength of a single hydrogen bond. As can be seen from figure 3, the data for [Ca(H 2 O) n ] 2+ complexes show binding energies that, even for n = 20, remain high and will probably not converge close to those recorded for H + (H 2 O) n clusters (or the value for a hydrogen bond) until n is approximately 25 or more.…”

Section: Resultsmentioning

confidence: 73%

“…It is instructive to compare figure 5 with data recorded previously for the series (H 2 O) n H + , (CH 3 OH) n H + and (NH 3 ) n H + [35], some of which are shown in figure 3. In the latter, the binding energies dropped abruptly until n = 6/7 and then exhibited no further decline, having reached values that match approximately hydrogen bond strengths found in neutral molecular pairs.…”

Section: Resultsmentioning

confidence: 81%

“…As can be seen from figure 3, the data for [Ca(H 2 O) n ] 2+ complexes show binding energies that, even for n = 20, remain high and will probably not converge close to those recorded for H + (H 2 O) n clusters (or the value for a hydrogen bond) until n is approximately 25 or more. In earlier discussions of the results derived from kinetic energy measurements, it has been argued that the nature of the experiment is such that only the lowest energy process available to a cluster will contribute to reaction (2.1) above [26,35]. A simple kinetic argument has also been presented in support of such a conclusion.…”

Section: Resultsmentioning

confidence: 99%

“…

Figure 3.Comparison between experimental binding energies determined for [Ca(H 2 O) n ] 2+ and for H + (H 2 O) n plotted as a function of n . The data for H + (H 2 O) n have been adapted from [35]. …”

Section: Resultsmentioning

confidence: 99%

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Experimental measurements of water molecule binding energies for the second and third solvation shells of [Ca(H ₂ O) _n ] ²⁺ complexes

Bruzzi¹,

Stace²

2017

R. Soc. open sci.

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Further understanding of the biological role of the Ca2+ ion in an aqueous environment requires quantitative measurements of both the short- and long-range interactions experienced by the ion in an aqueous medium. Here, we present experimental measurements of binding energies for water molecules occupying the second and, quite possibly, the third solvation shell surrounding a central Ca2+ ion in [Ca(H2O)n]2+ complexes. Results for these large, previously inaccessible, complexes have come from the application of finite heat bath theory to kinetic energy measurements following unimolecular decay. Even at n = 20, the results show water molecules to be more strongly bound to Ca2+ than would be expected just from the presence of an extended network of hydrogen bonds. For n > 10, there is very good agreement between the experimental binding energies and recently published density functional theory calculations. Comparisons are made with similar data recorded for [Ca(NH3)n]2+ and [Ca(CH3OH)n]2+ complexes.

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Section: Resultsmentioning

confidence: 73%

Section: Resultsmentioning

confidence: 81%

Section: Resultsmentioning

confidence: 99%

“…

Section: Resultsmentioning

confidence: 99%

See 2 more Smart Citations

Experimental measurements of water molecule binding energies for the second and third solvation shells of [Ca(H ₂ O) _n ] ²⁺ complexes

Bruzzi¹,

Stace²

2017

R. Soc. open sci.

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“…Thet otal kinetic energy released (KER) during the dissociation is partitioned because of momentum conservation, that is,t he evaporated molecule acquires an additional velocity randomly oriented in the center-of-mass reference frame (CMF) of the parent droplet. Differently from previous mass spectrometric measurements of the average kinetic energy release in decaying metastable water cluster ions, [13] the present experiment combines velocity map imaging with the correlated ion and neutral time-of-flight mass spectrometry technique on an event-by-event basis [14][15][16] (COINTOF MS). Measurements are performed on alarge number of individual droplets (typically 10 6 )t hereby obtaining the velocity distribution.…”

Section: Methodsmentioning

confidence: 99%

Velocity of a Molecule Evaporated from a Water Nanodroplet: Maxwell–Boltzmann Statistics versus Non‐Ergodic Events

et al. 2015

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The velocity of amolecule evaporated from amassselected protonated water nanodroplet is measured by velocity map imaging in combination with ar ecently developed mass spectrometry technique.T he measured velocity distributions allowp robing statistical energy redistribution in ultimately small water nanodroplets after ultrafast electronic excitation. As the droplet sizei ncreases,t he velocity distribution rapidly approaches the behavior expected for macroscopic droplets. However,adistinct high-velocity contribution provides evidence of molecular evaporation before complete energy redistribution, corresponding to non-ergodic events.The evaporation of water occurs through the breaking of one or several hydrogen bonds.T hese hydrogen bonds are responsible for many of the remarkable features of water [1] that are essential to life.W ater is known for its exceptional ability to absorb and hold heat at the macroscopic level, whereas at the sub-microscopic level, the intermolecular transfer of vibrational energy is known to be ultrafast because of the strong interactions between OÀHo scillators. [2,3] Thequantitative description of energy transfer in hydrogen-bonded compounds after electronic excitation is particularly challenging. Foralarge water droplet, the evaporation of water manifests itself as av elocity distribution of the evaporated molecules obeying Maxwell-Boltzmann (MB) statistics as ar esult of energy equipartitioning in athermalized system. In the present letter we address the thermalizing ability of even as mall water droplet following the sudden excitation of one of its molecules.Protonated water nanodroplets,H + (H 2 O) n=2-8 ,a re produced by supersonic expansion followed by electron impact ionization and acceleration at 8keV energy.T hey are then mass-and velocity-selected more than 1 msa fter being formed.[4] As ingle high-velocity collision (with V i in the laboratory frame ranging from 10 5 to 2.10 5 ms À1)w ith an Ar atom leads to energy deposition in the droplet by electronic excitation [5] of one of the molecules on atypical time scale of af raction of af emtosecond.[6] High-velocity collisions [7,8] probe ab road range of energy deposition, in contrast to Figure 1. Velocity map imaging of molecules evaporated from water nanodroplets. Evaporation is induced by asingle collision between amass-selectedprotonated water nanodropleta nd an argon atom. The nanodroplet has aselected laboratoryframe velocity V i before the collision. The evaporated H 2 Omolecule acquires an additionalt ransverse velocity, V t, (with respect to the original flight direction of the droplet) and reaches the detectorplaced at adistance D = 250 mm from the collision point. The impact position, R,o fthe evaporated molecule on the detector is related to the velocity, V,o fthe evaporated molecule in the center-of-mass reference frame of the nanodroplet.

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Velocity of a Molecule Evaporated from a Water Nanodroplet: Maxwell–Boltzmann Statistics versus Non‐Ergodic Events

et al. 2015

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The velocity of a molecule evaporated from a mass-selected protonated water nanodroplet is measured by velocity map imaging in combination with a recently developed mass spectrometry technique. The measured velocity distributions allow probing statistical energy redistribution in ultimately small water nanodroplets after ultrafast electronic excitation. As the droplet size increases, the velocity distribution rapidly approaches the behavior expected for macroscopic droplets. However, a distinct high-velocity contribution provides evidence of molecular evaporation before complete energy redistribution, corresponding to non-ergodic events.

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Binding energies determined from kinetic energy release measurements following the evaporation of single molecules from the molecular clusters H+(H2O)n, H+(NH3)n and H+(CH3OH)n

Cited by 12 publications

References 66 publications

Experimental measurements of water molecule binding energies for the second and third solvation shells of [Ca(H ₂ O) _n ] ²⁺ complexes

Experimental measurements of water molecule binding energies for the second and third solvation shells of [Ca(H ₂ O) _n ] ²⁺ complexes

Velocity of a Molecule Evaporated from a Water Nanodroplet: Maxwell–Boltzmann Statistics versus Non‐Ergodic Events

Velocity of a Molecule Evaporated from a Water Nanodroplet: Maxwell–Boltzmann Statistics versus Non‐Ergodic Events

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Binding energies determined from kinetic energy release measurements following the evaporation of single molecules from the molecular clusters H+(H2O)n, H+(NH3)n and H+(CH3OH)n

Cited by 12 publications

References 66 publications

Experimental measurements of water molecule binding energies for the second and third solvation shells of [Ca(H 2 O) n ] 2+ complexes

Experimental measurements of water molecule binding energies for the second and third solvation shells of [Ca(H 2 O) n ] 2+ complexes

Velocity of a Molecule Evaporated from a Water Nanodroplet: Maxwell–Boltzmann Statistics versus Non‐Ergodic Events

Velocity of a Molecule Evaporated from a Water Nanodroplet: Maxwell–Boltzmann Statistics versus Non‐Ergodic Events

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Experimental measurements of water molecule binding energies for the second and third solvation shells of [Ca(H ₂ O) _n ] ²⁺ complexes

Experimental measurements of water molecule binding energies for the second and third solvation shells of [Ca(H ₂ O) _n ] ²⁺ complexes