Solvated Electrons in Very Small Clusters of Polar Molecules: (HF)(3)(-): art. no. 143001

Gutowski, Maciej S; Hall, C; Adamowicz, L; Hendricks, J H; De Clercq, Helen; Lyapustina, S A; Nilles, J M; Xu, S J; Bowen, Jr, K H

Title: Solvated Electrons in Very Small Clusters of Polar Molecules: (HF)(3)(-): art. no. 143001

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Abstract

A cluster of polar molecules can host an excess electron in at least two ways. First, the excess electron can be tethered to the cluster by its interaction with the cluster?s dipole moment. , Second, the electron can localize inside the cluster, bulk analogs being the hydrated and ammoniated electrons. - While the structural reorganization of the cluster, due to attachment of an excess electron, is typically small for dipole-bound electrons (dbe), it is usually quite significant for''solvated electrons'' (se), since the solvation occurs at the expense of breaking of pre-existing hydrogen bonds. The se structures, however, provide more contact interactions between the polar molecules and the excess electron. For these reasons, it is often assumed that dbe's dominate for small polar clusters, whereas large clusters form se's. Here we show that dbe's and se's coexist in as small a cluster as (HF)3-. The stability of these anions with respect to the neutral cluster results not only from the excess electron binding energy but also from favorable entropic effects, which reflect the greater ''floppiness'' of the anionic structures.

Authors:

Gutowski, Maciej S ^[1]; Hall, C ^[2]; Adamowicz, L ^[2]; Hendricks, J H ^[3]; De Clercq, Helen ^[4]; Lyapustina, S A ^[3]; Nilles, J M ^[3]; Xu, S J ^[3]; Bowen, Jr, K H ^[3]

BATTELLE (PACIFIC NW LAB)
Arizona, University Of
Johns Hopkins Univ
Howard University

Publication Date:: Sat Dec 01 00:00:00 EST 2001

Research Org.:: Pacific Northwest National Lab., Richland, WA (US)

Sponsoring Org.:: US Department of Energy (US)

OSTI Identifier:: 15001004

Report Number(s):: PNNL-SA-35589
KC0302010; TRN: US200401%%377

DOE Contract Number:: AC06-76RL01830

Resource Type:: Journal Article

Journal Name:: Physical Review Letters

Additional Journal Information:: Journal Volume: 88; Journal Issue: 14; Other Information: PBD: 1 Dec 2001

Country of Publication:: United States

Language:: English

Subject:: 08 HYDROGEN; ANIONS; BINDING ENERGY; DIPOLE MOMENTS; ELECTRONS; HYDROGEN; SOLVATED ELECTRONS; SOLVATION; STABILITY

Citation Formats


                    Gutowski, Maciej S, Hall, C, Adamowicz, L, Hendricks, J H, De Clercq, Helen, Lyapustina, S A, Nilles, J M, Xu, S J, and Bowen, Jr, K H. Solvated Electrons in Very Small Clusters of Polar Molecules: (HF)(3)(-): art. no. 143001.  United States: N. p., 2001. 
        Web.

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                    Gutowski, Maciej S, Hall, C, Adamowicz, L, Hendricks, J H, De Clercq, Helen, Lyapustina, S A, Nilles, J M, Xu, S J, & Bowen, Jr, K H. Solvated Electrons in Very Small Clusters of Polar Molecules: (HF)(3)(-): art. no. 143001.  United States.

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                    Gutowski, Maciej S, Hall, C, Adamowicz, L, Hendricks, J H, De Clercq, Helen, Lyapustina, S A, Nilles, J M, Xu, S J, and Bowen, Jr, K H. 2001.  
        "Solvated Electrons in Very Small Clusters of Polar Molecules: (HF)(3)(-): art. no. 143001".  United States.

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@article{osti_15001004,

  title        = {Solvated Electrons in Very Small Clusters of Polar Molecules: (HF)(3)(-): art. no. 143001},

  author       = {Gutowski, Maciej S and Hall, C and Adamowicz, L and Hendricks, J H and De Clercq, Helen and Lyapustina, S A and Nilles, J M and Xu, S J and Bowen, Jr, K H},

  abstractNote = {A cluster of polar molecules can host an excess electron in at least two ways. First, the excess electron can be tethered to the cluster by its interaction with the cluster?s dipole moment. , Second, the electron can localize inside the cluster, bulk analogs being the hydrated and ammoniated electrons. - While the structural reorganization of the cluster, due to attachment of an excess electron, is typically small for dipole-bound electrons (dbe), it is usually quite significant for''solvated electrons'' (se), since the solvation occurs at the expense of breaking of pre-existing hydrogen bonds. The se structures, however, provide more contact interactions between the polar molecules and the excess electron. For these reasons, it is often assumed that dbe's dominate for small polar clusters, whereas large clusters form se's. Here we show that dbe's and se's coexist in as small a cluster as (HF)3-. The stability of these anions with respect to the neutral cluster results not only from the excess electron binding energy but also from favorable entropic effects, which reflect the greater ''floppiness'' of the anionic structures.},

  doi          = {},

  url          = {https://www.osti.gov/biblio/15001004},
  journal      = {Physical Review Letters},
number       = 14,

  volume       = 88,

  place        = {United States},

  year         = {Sat Dec 01 00:00:00 EST 2001},

  month        = {Sat Dec 01 00:00:00 EST 2001}

}

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