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Title: Spectroscopic probe of the van der Waals interaction between polar molecules and a curved surface

Authors:
; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1297271
Grant/Contract Number:
DF-FC02-94ER40818
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Physical Review A
Additional Journal Information:
Journal Volume: 94; Journal Issue: 2; Related Information: CHORUS Timestamp: 2016-08-17 18:10:04; Journal ID: ISSN 2469-9926
Publisher:
American Physical Society
Country of Publication:
United States
Language:
English

Citation Formats

Bimonte, Giuseppe, Emig, Thorsten, Jaffe, R. L., and Kardar, Mehran. Spectroscopic probe of the van der Waals interaction between polar molecules and a curved surface. United States: N. p., 2016. Web. doi:10.1103/PhysRevA.94.022509.
Bimonte, Giuseppe, Emig, Thorsten, Jaffe, R. L., & Kardar, Mehran. Spectroscopic probe of the van der Waals interaction between polar molecules and a curved surface. United States. doi:10.1103/PhysRevA.94.022509.
Bimonte, Giuseppe, Emig, Thorsten, Jaffe, R. L., and Kardar, Mehran. 2016. "Spectroscopic probe of the van der Waals interaction between polar molecules and a curved surface". United States. doi:10.1103/PhysRevA.94.022509.
@article{osti_1297271,
title = {Spectroscopic probe of the van der Waals interaction between polar molecules and a curved surface},
author = {Bimonte, Giuseppe and Emig, Thorsten and Jaffe, R. L. and Kardar, Mehran},
abstractNote = {},
doi = {10.1103/PhysRevA.94.022509},
journal = {Physical Review A},
number = 2,
volume = 94,
place = {United States},
year = 2016,
month = 8
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1103/PhysRevA.94.022509

Citation Metrics:
Cited by: 2works
Citation information provided by
Web of Science

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  • The van der Waals potential between a neutral atom (no permanent dipole) and a metallic surface is presented. The treatment, based on the normal modes of the system, allows a deeper understanding of the nature of van der Waals forces and makes it practically possible to calculate for complex geometries. To show this we derive theoretical expressions for the interactions of atoms with cylinders and spheres, besides the well-known plane-geometry formula. These formulas are new in some aspects and constitute the theoretical counterpart of many experimental situations. In the same vein we allow a stochastic surface roughness to be presentmore » in the plane geometry and show how the problem can be solved analytically in the electrostatic approximation. Numerical calculations and comparison with experiments are presented in paper II.« less
  • The scattering of nonpolarized atoms by a macroscopic metallic cylinder is studied in detail. The interaction potential for such a system has been presented in a previous paper. Applying it to the Cs-Au system we find that the disagreement between theory and experiment can actually be explained in terms of surface roughness only, while dynamical corrections and geometrical effects are negligible. Our result differs somewhat from the Mehl and Schaich analysis, but it does not conflict with their findings, since the two models for the surface are different. In addition we present an analytical solution for the intensity that canmore » be advantageously employed to within 3% of accuracy and can be retained exact for a z/sup -n/-type potential. This allows us to show how the averaged potential remains, a good quantity to work with even if the fluctuations are large.« less
  • Calculations are presented of the coefficient C/sub 3/ of the z/sup -3/ dispersion interaction between Ir and Ta atoms and a W surface. The results depend sensitively on the assumed value of the atomic polarizability. If experimental values are used, the results for C/sub 3/ are consistent with determinations based on the atomic deflection by a field-emission tip.
  • The copper paddle-wheel is the building unit of many metal organic frameworks. Because of the ability of the copper cations to attract polar molecules, copper paddle-wheels are promising for carbon dioxide adsorption and separation. They have therefore been studied extensively, both experimentally and computationally. In this work we investigate the copper–CO 2 interaction in HKUST-1 and in two different cluster models of HKUST-1: monocopper Cu(formate) 2 and dicopper Cu 2(formate) 4. We show that density functional theory methods severely underestimate the interaction energy between copper paddle-wheels and CO 2, even including corrections for the dispersion forces. In contrast, a multireferencemore » wave function followed by perturbation theory to second order using the CASPT2 method correctly describes this interaction. The restricted open-shell Møller–Plesset 2 method (ROS-MP2, equivalent to (2,2) CASPT2) was also found to be adequate in describing the system and used to develop a novel force field. Our parametrization is able to predict the experimental CO 2 adsorption isotherms in HKUST-1, and it is shown to be transferable to other copper paddle-wheel systems.« less
  • The copper paddle-wheel is the building unit of many metal organic frameworks. Because of the ability of the copper cations to attract polar molecules, copper paddle-wheels are promising for carbon dioxide adsorption and separation. They have therefore been studied extensively, both experimentally and computationally. In this work we investigate the copper–CO 2 interaction in HKUST-1 and in two different cluster models of HKUST-1: monocopper Cu(formate) 2 and dicopper Cu 2(formate) 4. We show that density functional theory methods severely underestimate the interaction energy between copper paddle-wheels and CO 2, even including corrections for the dispersion forces. In contrast, a multireferencemore » wave function followed by perturbation theory to second order using the CASPT2 method correctly describes this interaction. The restricted open-shell Møller–Plesset 2 method (ROS-MP2, equivalent to (2,2) CASPT2) was also found to be adequate in describing the system and used to develop a novel force field. Our parametrization is able to predict the experimental CO 2 adsorption isotherms in HKUST-1, and it is shown to be transferable to other copper paddle-wheel systems.« less