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Vibrational pooling and constrained ...

Boney, E. T. D.

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Vibrational pooling and constrained equilibration on surfaces.

紀錄類型:	書目-語言資料,印刷品 : Monograph/item
正題名/作者:	Vibrational pooling and constrained equilibration on surfaces./
作者:	Boney, E. T. D.
面頁冊數:	78 p.
附註:	Source: Dissertation Abstracts International, Volume: 75-02(E), Section: B.
Contained By:	Dissertation Abstracts International75-02B(E).
標題:	Chemistry, Physical. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3600019
ISBN:	9781303499104

Vibrational pooling and constrained equilibration on surfaces.
Boney, E. T. D.

Vibrational pooling and constrained equilibration on surfaces. - 78 p.

Source: Dissertation Abstracts International, Volume: 75-02(E), Section: B.

Thesis (Ph.D.)--California Institute of Technology, 2014.

In this thesis, we provide a statistical theory for the vibrational pooling and fluorescence time dependence observed in infrared laser excitation of CO on an NaCl surface. The pooling is seen in experiment and in computer simulations. In the theory, we assume a rapid equilibration of the quanta in the substrate and minimize the free energy subject to the constraint at any time t of a fixed number of vibrational quanta N(t). At low incident intensity, the distribution is limited to one-quantum exchanges with the solid and so the Debye frequency of the solid plays a key role in limiting the range of this one-quantum domain. The resulting inverted vibrational equilibrium population depends only on fundamental parameters of the oscillator (oe and oe&khgr;e) and the surface (oD and T). Possible applications and relation to the Treanor gas phase treatment are discussed. Unlike the solid phase system, the gas phase system has no Debye-constraining maximum. We discuss the possible distributions for arbitrary N-conserving diatom-surface pairs, and include application to H:Si(111) as an example.

ISBN: 9781303499104Subjects--Topical Terms:

560527
Chemistry, Physical.

Vibrational pooling and constrained equilibration on surfaces.
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245 1 0 $a Vibrational pooling and constrained equilibration on surfaces.
300 $a 78 p.
500 $a Source: Dissertation Abstracts International, Volume: 75-02(E), Section: B.
500 $a Adviser: Rudolph A. Marcus.
502 $a Thesis (Ph.D.)--California Institute of Technology, 2014.
520 $a In this thesis, we provide a statistical theory for the vibrational pooling and fluorescence time dependence observed in infrared laser excitation of CO on an NaCl surface. The pooling is seen in experiment and in computer simulations. In the theory, we assume a rapid equilibration of the quanta in the substrate and minimize the free energy subject to the constraint at any time t of a fixed number of vibrational quanta N(t). At low incident intensity, the distribution is limited to one-quantum exchanges with the solid and so the Debye frequency of the solid plays a key role in limiting the range of this one-quantum domain. The resulting inverted vibrational equilibrium population depends only on fundamental parameters of the oscillator (oe and oe&khgr;e) and the surface (oD and T). Possible applications and relation to the Treanor gas phase treatment are discussed. Unlike the solid phase system, the gas phase system has no Debye-constraining maximum. We discuss the possible distributions for arbitrary N-conserving diatom-surface pairs, and include application to H:Si(111) as an example.
520 $a Computations are presented to describe and analyze the high levels of infrared laser induced vibrational excitation of a monolayer of absorbed 13CO on a NaCl(100) surface. The calculations confirm that, for situations where the Debye frequency limited n domain restriction approximately holds, the vibrational state population deviates from a Boltzmann population linearly in n, a result that we have derived earlier theoretically for a domain of n restricted to one-phonon transfers. This theoretically understood term, linear in n, dominates the Boltzmann term and is responsible for the inversion of the population of vibrational states, Pn.
520 $a We discuss the one-to-one relationship between N and gamma and the examine the state space of the new distribution function for varied gamma. We derive the Free Energy and effective chemical potential for the vibrational pool. We also find the anti correlation of neighbor vibrations leads to an emergent correlation that appears to extend further than nearest neighbor.
590 $a School code: 0037.
650 4 $a Chemistry, Physical. $3 560527
650 4 $a Physics, Condensed Matter. $3 1018743
650 4 $a Chemistry, General. $3 1021807
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710 2 $a California Institute of Technology. $b Chemistry. $3 2096080
773 0 $t Dissertation Abstracts International $g 75-02B(E).
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791 $a Ph.D.
792 $a 2014
793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3600019