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Register a new userAlternating-Gradient Focusing of the Benzonitrile-Argon Van der Waals Complex
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We report on the focusing and guiding of the van der Waals complex formed between benzonitrile molecules (C$_6$H$_5$CN) and argon atoms in a cold molecular beam using an ac electric quadrupole guide. The distribution of quantum states in the guided beam is non-thermal, because the transmission efficiency depends on the state-dependent effective dipole moment in the applied electric fields. At a specific ac frequency, however, the excitation spectrum can be described by a thermal distribution at a rotational temperature of 0.8 K. From the observed transmission characteristics and a combination of trajectory and Stark-energy calculations we conclude that the permanent electric dipole moment of benzonitrile remains unchanged upon the attachment of the argon atom to within pm5%. By exploiting the different dipole-moment-to-mass (mu/m) ratios of the complex and the benzonitrile monomer, transmission can be selectively suppressed for or, in the limit of 0 K rotational temperature, restricted to the complex.
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The non-local van der Waals density functional (vdW-DF) has had tremendous success since its inception in 2004 due to its constraint-based formalism that is rigorously derived from a many-body starting point. However, while vdW-DF can describe binding energies and structures for van der Waals complexes and mixed systems with good accuracy, one long-standing criticism---also since its inception---has been that the $C_6$ coefficients that derive from the vdW-DF framework are largely inaccurate and can be wrong by more than a factor of two. It has long been thought that this failure to describe the $C_6$ coefficients is a conceptual flaw of the underlying plasmon framework used to derive vdW-DF. We prove here that this is not the case and that accurate $C_6$ coefficient can be obtained without sacrificing the accuracy at binding separations from a modified framework that is fully consistent with the constraints and design philosophy of the original vdW-DF formulation. Our design exploits a degree of freedom in the plasmon-dispersion model $omega_{mathbf{q}}$, modifying the strength of the long-range van der Waals interaction and the cross-over from long to short separations, with additional parameters tuned_ to reference systems. Testing the new formulation for a range of different systems, we not only confirm the greatly improved description of $C_6$ coefficients, but we also find excellent performance for molecular dimers and other systems. The importance of this development is not necessarily that particular aspects such as $C_6$ coefficients or binding energies are improved, but rather that our finding opens the door for further conceptual developments of an entirely unexplored direction within the exact same constrained-based non-local framework that made vdW-DF so successful in the first place.
We have focused and decelerated benzonitrile (C$_7$H$_5$N) molecules from a molecular beam, using an array of time-varying inhomogeneous electric fields in alternating gradient configuration. Benzonitrile is prototypical for large asymmetric top molecules that exhibit rich rotational structure and a high density of states. At the rotational temperature of 3.5 K in the pulsed molecular beam, many rotational states are populated. Benzonitrile molecules in their absolute ground state are decelerated from 320 m/s to 289 m/s, and similar changes in velocity are obtained for excited rotational states. All measurements agree well with the outcome of trajectory calculations. These experiments demonstrate that such large polyatomic molecules are amenable to the powerful method of Stark deceleration.
We report on the direct measurement in real space of the effect of the van der Waals forces between individual Rydberg atoms on their external degrees of freedom. Clusters of Rydberg atoms with inter-particle distances of around 5 {mu}m are created by first generating a small number of seed excitations in a magneto-optical trap, followed by off-resonant excitation that leads to a chain of facilitated excitation events. After a variable expansion time the Rydberg atoms are field ionized, and from the arrival time distributions the size of the Rydberg cluster after expansion is calculated. Our experimental results agree well with a numerical simulation of the van der Waals explosion.
In inhomogeneous dielectric media the divergence of the electromagnetic stress is related to the gradients of varepsilon and mu, which is a consequence of Maxwells equations. Investigating spherically symmetric media we show that this seemingly universal relationship is violated for electromagnetic vacuum forces such as the generalized van der Waals and Casimir forces. The stress needs to acquire an additional anomalous pressure. The anomaly is a result of renormalization, the need to subtract infinities in the stress for getting a finite, physical force. The anomalous pressure appears in the stress in media like dark energy appears in the energy-momentum tensor in general relativity. We propose and analyse an experiment to probe the van der Waals anomaly with ultracold atoms. The experiment may not only test an unusual phenomenon of quantum forces, but also an analogue of dark energy, shedding light where nothing is known empirically.
We study the repulsive van der Waals interaction of cold rubidium $70S_{1/2}$ Rydberg atoms by analysis of time-delayed pair correlation functions. After excitation, Rydberg atoms are allowed to accelerate under the influence of the van der Waals force. Their positions are then measured using a single-atom imaging technique. From the average pair correlation function of the atom positions we obtain the initial atom-pair separation and the terminal velocity, which yield the van der Waals interaction coefficient $C_{6}$. The measured $C_{6}$ value agrees well with calculations. The experimental method has been validated by simulations. The data hint at anisotropy in the overall expansion, caused by the shape of the excitation volume. Our measurement implies that the interacting entities are individual Rydberg atoms, not groups of atoms that coherently share a Rydberg excitation.
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