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Register a new userIntermolecular Casimir-Polder Forces in Water and near Surfaces
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The Casimir-Polder force is an important long range interaction involved in adsorption and desorption of molecules in fluids. We explore Casimir-Polder interactions between methane molecules in water, and between a molecule in water near SiO2 and hexane surfaces. Inclusion of the finite molecular size in the expression for the Casimir-Polder energy leads to estimates of the dispersion contribution to the binding energies between molecules and between one molecule and a planar surface.
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Casimir and Casimir-Polder repulsion have been known for more than 50 years. The general Lifshitz configuration of parallel semi-infinite dielectric slabs permits repulsion if they are separated by a dielectric fluid that has a value of permittivity that is intermediate between those of the dielectric slabs. This was indirectly confirmed in the 1970s, and more directly by Capassos group recently. It has also been known for many years that electrically and magnetically polarizable bodies can experience a repulsive quantum vacuum force. More amenable to practical application are situations where repulsion could be achieved between ordinary conducting and dielectric bodies in vacuum. The status of the field of Casimir repulsion with emphasis on recent developments will be surveyed. Here, stress will be placed on analytic developments, especially of Casimir-Polder (CP) interactions between anisotropically polarizable atoms, and CP interactions between anisotropic atoms and bodies that also exhibit anisotropy, either because of anisotropic constituents, or because of geometry. Repulsion occurs for wedge-shaped and cylindrical conductors, provided the geometry is sufficiently asymmetric, that is, either the wedge is sufficiently sharp or the atom is sufficiently far from the cylinder.
Here we present a fundamental study on how the ground-state chemical reactivity of a molecule can be modified in a QED scenario, i.e., when it is placed inside a cavity and there is strong coupling between the cavity field and vibrational modes within the molecule. We work with a model system for the molecule (Shin-Metiu model) in which nuclear, electronic and photonic degrees of freedom are treated on the same footing. This simplified model allows the comparison of exact quantum reaction rate calculations with predictions emerging from transition state theory based on the cavity Born-Oppenheimer approach. We demonstrate that QED effects are indeed able to significantly modify activation barriers in chemical reactions and, as a consequence, reaction rates. The critical physical parameter controlling this effect is the permanent dipole of the molecule and how this magnitude changes along the reaction coordinate. We show that the effective coupling can lead to significant single-molecule energy shifts in an experimentally available nanoparticle-on-mirror cavity. We then apply the validated theory to a realistic case (internal rotation in the 1,2-dichloroethane molecule), showing how reactions can be inhibited or catalyzed depending on the profile of the molecular dipole. Furthermore, we discuss the absence of resonance effects in this process, which can be understood through its connection to Casimir-Polder forces. Finally, we treat the case of many-molecule strong coupling, and find collective modifications of reaction rates if the molecular permanent dipole moments are oriented with respected to the cavity field. This demonstrates that collective coupling can also provide a mechanism for modifying ground-state chemical reactivity of an ensemble of molecules coupled to a cavity mode.
Polarisable atoms and molecules experience the Casimir-Polder force near magnetoelectric bodies, a force that is induced by quantum fluctuations of the electromagnetic field and the matter. Atoms and molecules in relative motion to a magnetoelectric surface experience an additional, velocity-dependent force. We present a full quantum-mechanical treatment of this force and identify a generalised Doppler effect, the time delay between photon emission and reabsorption, and the Roentgen interaction as its three sources. For ground-state atoms, the force is very small and always decelerating, hence commonly known as quantum friction. For atom and molecules in electronically excited states, on the contrary, both decelerating and accelerating forces can occur depending on the magnitude of the atomic transition frequency relative to the surface plasmon frequency.
We take a closer look at the fundamental Casimir-Polder interaction between quantum particles and dispersive dielectric surfaces with surface polariton or plasmon resonances. Linear response theory shows that in the near field, van der Waals, regime the free energy shift of a particle contains a thermal component that depends exclusively on the population/excitation of the evanescent surface polariton/plasmon modes. Our work makes evident the link between particle surface interaction and near field thermal emission and demonstrates how this can be used to engineer Casimir-Polder forces. We also examine how the exotic effects of surface waves are washed out as the distance from the surface increases. In the case of molecules or excited state atoms, far field approximations result in a classical dipole-dipole interaction which depends on the surface reflectivity and the mean number of photons at the frequency of the atomic/molecular transition. Finally we present numerical results for the CP interaction between Cs atoms and various dielectric surfaces with a single polariton resonance and discuss the implications of temperature and retardation effects for specific spectroscopic experiments.
It has always been conventionally understood that, in the dilute limit, the Casimir energy of interaction between bodies or the Casimir self-energy of a dielectric body could be identified with the sum of the van der Waals or Casimir-Polder energies of the constituents of the bodies. Recently, this proposition for self-energies has been challenged by Avni and Leonhardt [Ann. Phys. {bf 395}, 326 (2018)], who find that the energy or self-stress of a homogeneous dielectric ball with permittivity $varepsilon$ begins with a term of order $varepsilon-1$. Here we demonstrate that this cannot be correct. The only possible origin of a term linear in $varepsilon-1$ lies in the bulk energy, that energy which would be present if either the material of the body, or of its surroundings, filled all space. Since Avni and Leonhardt correctly subtract the bulk terms, the linear term they find likely arises from their omission of an integral over the transverse stress tensor.
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