Communication: Where does the first water molecule go in imidazole?

Zischang, Julia; Lee, Juhyon J.; Suhm, Martin A.

doi:10.1063/1.3624841

Cited by 43 publications

(55 citation statements)

References 25 publications

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“…Note that the problem is not unique to the supersonic jet synthesis; it is also the case for other approaches such as the matrix isolation method and the spectroscopy of clusters generated in helium nanodroplets (see, e.g., the discussion in Ref. 3 …”

Section: Introductionmentioning

confidence: 98%

The temperature and size distribution of large water clusters from a non-equilibrium model

Gimelshein¹,

Gimelshein

Pradzynski

et al. 2015

The Journal of Chemical Physics

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A hybrid Lagrangian-Eulerian approach is used to examine the properties of water clusters formed in neon-water vapor mixtures expanding through microscale conical nozzles. Experimental size distributions were reliably determined by the sodium doping technique in a molecular beam machine. The comparison of computed size distributions and experimental data shows satisfactory agreement, especially for (H2O)n clusters with n larger than 50. Thus validated simulations provide size selected cluster temperature profiles in and outside the nozzle. This information is used for an in-depth analysis of the crystallization and water cluster aggregation dynamics of recently reported supersonic jet expansion experiments.

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Section: Introductionmentioning

confidence: 98%

The temperature and size distribution of large water clusters from a non-equilibrium model

Gimelshein¹,

Gimelshein

Pradzynski

et al. 2015

The Journal of Chemical Physics

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“…One might also consider an alternative mechanism, which is occasionally discussed46, 47 and profits from a relatively high diol concentration in the supersonic jet expansions. Collision of a metastable and thus reactive CC‐homochiral dimer with an enantiomeric monomer could result in the more stable CC‐heterochiral dimer and a surplus monomer carrying away the excess energy (and chirality) via a transient trimer.…”

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confidence: 99%

A Symmetric Recognition Motif between Vicinal Diols: The Fourfold Grip in Ethylene Glycol Dimer

2016

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“…One might also consider an alternative mechanism, which is occasionally discussed and profits from a relatively high diol concentration in the supersonic jet expansions. Collision of a metastable and thus reactive CC‐homochiral dimer with an enantiomeric monomer could result in the more stable CC‐heterochiral dimer and a surplus monomer carrying away the excess energy (and chirality) via a transient trimer.…”

Section: Figurementioning

confidence: 99%

A Symmetric Recognition Motif between Vicinal Diols: The Fourfold Grip in Ethylene Glycol Dimer

2016

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Ethylene glycol has atransiently chiral, asymmetric global minimum structure,b ut it favors ah ighly symmetric, achiral dimer arrangement which has not been considered or found in previous quantum-chemical studies.C omplementary FTIR and Raman spectroscopyinsupersonic jets allows for the detection and straightforwarda ssignment of this four-fold hydrogen-bonded dimer,w hich introduces an interesting supramolecular binding motif for vicinal diols and provides astrong case for transient chirality synchronization.Carbohydrates are among the most versatile molecules employed by nature in molecular recognition processes and their biomimetic detection is challenging.[1] When reducing their molecular complexity to am inimum, one naturally arrives at vicinal diols.A mong them, the simplest representative ethylene glycol has even been detected in interstellar space.[2] Ethylene glycol or 1,2-ethanediol is ap articularly valuable model system for the study of multiple hydrogenbonded dimers and carbohydrate interactions, [3] because it allows for av ast range of quantum-chemical options to be explored. Indeed, the question of its preferred dimer structure has been addressed repeatedly by theory, [4][5][6] but not by experimental techniques.B ecause of the torsional flexibility of ethylene glycol, there are several possibilities how the four OH groups of the dimer can engage in hydrogen bonds.None of the previously proposed structures involves more than three hydrogen bonds among these OH groups. [4][5][6][7][8][9][10][11] We present unambiguous combined IR and Raman spectroscopic evidence that ethylene glycol in fact forms an S 4 -symmetric and thus non-polar and achiral dimer with four equivalent hydrogen bonds.U sing Gaussian 09, [12] an extensive search of the intermolecular potential-energy hypersurface at B3LYP-D3(BJ)/6-311 + G(2d,p) level (in short B3LYP) confirms that this structure wins over all triply hydrogen-bonded dimer structures by as ubstantial energy margin.Thet wo lowest monomer structures found at the harmonically zero-point energy-corrected B3LYP level are depicted in Figure 1. They have in common a gauche OCCO backbone,aweakly hydrogen-bonded OH group, and af ree OH group pointing in trans (M) or gauche (M') direction relative to the CÀCb ackbone.T hese monomer conformations are chiral and differ only by 1.4 kJ mol À1 at B3LYP level, making both of them potentially observable in aseeded adiabatic jet expansion. They have been investigated previously in much detail, [13][14][15][16][17][18][19][20][21][22][23][24][25] mostly by microwave spectroscopy, [13][14][15][16][17][18][19][20] and experimental estimates for their energy difference are rather close to our theoretical prediction, with 1.4(4) and 2.5(5) kJ mol À1 . [16,20] In jet experiments,t ypically only Mi so bserved in substantial abundance because of efficient conformational relaxation, [18] whereas at room temperature,M ' is also populated. Donor-acceptor OH torsional tunneling splits the levels by 0.2 and 0.05 cm À1 , respectively. ...

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Communication: Where does the first water molecule go in imidazole?

Cited by 43 publications

References 25 publications

The temperature and size distribution of large water clusters from a non-equilibrium model

The temperature and size distribution of large water clusters from a non-equilibrium model

A Symmetric Recognition Motif between Vicinal Diols: The Fourfold Grip in Ethylene Glycol Dimer

A Symmetric Recognition Motif between Vicinal Diols: The Fourfold Grip in Ethylene Glycol Dimer

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