Creation of Polar and Nonpolar Ultra-Long-Range Rydberg Molecules

Abstract

We predict the existence of a ubiquitous class of long-range molecular Rydberg states, whose Born-Oppenheimer potential curves are oscillatory in nature. These oscillations reflect the nodal structure of the atomic Rydberg state wave functions. The temperature and density of atoms in a Bose-Einstein condensate are particularly favorable for the laser excitation of ultra-long-range vibrational bound states localized at internuclear distances in the range 10(3)- 10(5) a.u. A surprising trilobitelike class of polar homonuclear diatomics should exhibit electric dipole moments in the kilodebye range.

Ultralong-range Rydberg molecules in combined electric and magnetic fields

“…For the considered quantum numbers n ≈ 30-50 the vibrational binding energies are in the MHz and GHz regime depending on the type of states. More specifically, low-angular momentum non-polar states and large angular momentum polar states, so-called trilobites, have been predicted [10]. They possess electric dipole moments in the range of 1 Debye (low-) up to 1 kDebye (high-) in the polar case.…”

“…A prominent new species are the weakly bound ultralong-range diatomic molecules composed of a ground state and a Rydberg atom. Theoretically predicted more than a decade ago [10] they have been recently discovered experimentally [11]. The molecular Born-Oppenheimer potential energy surfaces, which are responsible for the diatomic binding, show for these species an unusual strong oscillatory behavior providing a large number of local potential minima.…”

Ultralong-Range Rydberg Cs2 Molecules Investigated at the Ab Initio Level of Theory

“…In the first case, a macrodimer Rydberg molecule [6][7][8][9] associated by two Rydberg atoms (A*+B*) has a size larger than 1 µm and in the second case a butterfly or trilobite like Rydberg molecule [10][11][12][13] associated by a Rydberg atom and a ground state one (A*+B) has a typical size of about 10 3 a 0 (Bohr radius). Since the first calculation of Rydberg molecular potential curves in 2000 by Greene and coworkers [10], Rydberg molecules have been extensively investigated both theoretically and experimentally [14][15][16][17] due to their extraordinary properties such as huge size, large dipole moment, weak bounding energy and long lifetime. In particular, in some fast developing area of quantum physics, Rydberg molecules are more suitable than Rydberg atoms for quantum manipulation with electric field [18,19].…”

“…[7] and [10] respectively. Soon experimental evidence [20][21][22] has been found for the A*+B* type of Rydberg molecules.…”

“…For A*+B type of Rydberg molecules, in general the available theoretical investigations [10,11] have adopted s wave scattering or perturbation treatment based on Rydberg states from certain empirical electron-core potential for the Rydberg atom. Therefore accurate description of the Rydberg atom is essential for the accuracy of the Rydberg molecular potential curve no matter by scattering or perturbation treatments, in particular when pursuing quantitative agreement with experiments.…”