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Effects of strong interactions in ultracold Rydberg gases

Jovica Stanojevic

Published Jan 1, 2007• 1 citation
OpenAlex

Abstract

In this thesis I present several theoretical methods to explore the excitation dynamics of Ultracold Rydberg systems in various regimes. For some applications the details of interactions between Rydberg atoms have to be carefully examined, while for others, the many-body aspect of Rydberg excitation may be crucial. In both cases, the basic prerequisite is to know the interactions sufficiently well. I will review the basic concepts how to evaluate molecular potentials in various Hund's cases and approximations. Long-range Rydberg-Rydberg interactions between Rydberg atoms induce ℓ-mixing which in certain situations gives rise to molecular resonances. For these resonances, we calculate long-range potentials in Hund's case (c) by diagonalization of an interaction matrix. The excitation dynamics of the resonances is always modeled as pair excitation. At high principal quantum number n, the interactions between Rydberg atoms can blockade the excitation of many surrounding atoms in the range of few μm. The atoms within this range are strongly correlated so that many-body treatments are, in general, needed. To describe this blockading effect and other manifestations of the collective behavior of Rydberg excitation, such as the many-body Rabi oscillations, spatial correlations between atoms and the fluctuations of the number of excited atoms, I have used three different approaches. In the mean-field approach the interactions between different atoms is modeled by a distribution of mean-field shifts for which a distribution of probabilities is calculated, A good agreement between the theoretical model and experimental measurements is found. To study the correlations between atoms the many-body wavefunction is numerically computed. The possibility of observing the many-body Rabi oscillations of Rydberg excitation and other aspects of many-body dynamics is analyzed. Although strong interactions cannot be treated perturbatively other expansions may be feasible. I will show that the expansion in powers of the single atom Rabi frequency can be evaluated in the interaction and Heisenberg picture. The expansion is expected to behave well for arbitrary strong interactions. ^

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Many-body dynamics of Rydberg excitation using the Ω expansion

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We investigate the excitation dynamics of Rydberg atoms in ultracold atomic samples by expanding the excitation probability and the correlation function between excited atoms in powers of the isolated atom Rabi frequency $\ensuremath{\Omega}$. In the Heisenberg picture, we give recurrence relations to calculate any order of these expansions, which are expected to be well behaved for arbitrarily strong interactions. For large homogeneous samples, the explicit terms of the expansions, up to ${\ensuremath{\Omega}}^{4}$, are given and then averaged over all possible random spatial distributions of atoms for the most important cases of excitation pulses and interactions.

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During this thesis, the Physics of interacting systems has been investigated experimentally using Cold Rydberg gases. Rydberg atoms are very excited atoms and have the particularity to interact strongly together through long-range electrostatic interaction. A first highlight of the thesis is a direct experimental observation of a 4-body process. This process consists in internal exchanges of excitations between 4 Rydberg atoms due to their mutual interactions. In addition to its experimental observation, the process has been succefully described theoretically at a quantum level. A second highlight of this thesis has concerns the study of the laser excitation of strongly interacting Rydberg gases. In this regime, many-body quantum correlations play a central role leading to fascinating many-body behavior. In addition to fundamental interests, such systems could be used to implement quantum simulator or non-classical light sources. The system has been investigated during this thesis through the counting statistics of the Rydberg excitation. A highly sub-poisonian, i.e correlated, statistics has been observed in the regim of strong interactions proving the many-body nature of the system. A third highlight of this thesis is the development of an original theoretical model to describe the laser excitation of strongly interacting Rydberg gases. Using the so-called Dicke collective states, it has been possible to catch several interesting features of this many-body problem.

•Mar 12, 2013•0 citations
In this thesis I present several theoretical methods to explore the excitation dynamics of Ultracold Rydberg systems in various regimes. For some applications the details of interactions between Rydberg atoms have to be carefully examined, while for others, the many-body aspect of Rydberg excitation may be crucial. In both cases, the basic prerequisite is to know the interactions sufficiently well. I will review the basic concepts how to evaluate molecular potentials in various Hund's cases and approximations. Long-range Rydberg-Rydberg interactions between Rydberg atoms induce ℓ-mixing which in certain situations gives rise to molecular resonances. For these resonances, we calculate long-range potentials in Hund's case (c) by diagonalization of an interaction matrix. The excitation dynamics of the resonances is always modeled as pair excitation. At high principal quantum number n, the interactions between Rydberg atoms can blockade the excitation of many surrounding atoms in the range of few μm. The atoms within this range are strongly correlated so that many-body treatments are, in general, needed. To describe this blockading effect and other manifestations of the collective behavior of Rydberg excitation, such as the many-body Rabi oscillations, spatial correlations between atoms and the fluctuations of the number of excited atoms, I have used three different approaches. In the mean-field approach the interactions between different atoms is modeled by a distribution of mean-field shifts for which a distribution of probabilities is calculated, A good agreement between the theoretical model and experimental measurements is found. To study the correlations between atoms the many-body wavefunction is numerically computed. The possibility of observing the many-body Rabi oscillations of Rydberg excitation and other aspects of many-body dynamics is analyzed. Although strong interactions cannot be treated perturbatively other expansions may be feasible. I will show that the expansion in powers of the single atom Rabi frequency can be evaluated in the interaction and Heisenberg picture. The expansion is expected to behave well for arbitrary strong interactions. ^
We investigate the excitation dynamics of Rydberg atoms in ultracold atomic samples by expanding the excitation probability and the correlation function between excited atoms in powers of the isolated atom Rabi frequency $\ensuremath{\Omega}$. In the Heisenberg picture, we give recurrence relations to calculate any order of these expansions, which are expected to be well behaved for arbitrarily strong interactions. For large homogeneous samples, the explicit terms of the expansions, up to ${\ensuremath{\Omega}}^{4}$, are given and then averaged over all possible random spatial distributions of atoms for the most important cases of excitation pulses and interactions.
We investigate the excitation dynamics of Rydberg atoms in ultracold atomic samples by expanding the excitation probability and the correlation function between excited atoms in powers of the isolated atom Rabi frequency ΩΩΩ. In the Heisenberg picture, we give recurrence relations to calculate any order of the expansions, which ere expected to be well-behaved for arbitrarily strong interactions. For homogeneous large samples, we give the explicit form of the expansions, up to Ω4Ω^4Ω4, averaged over all possible random spatial distributions of atoms, for the most important cases of excitation pulses and interactions.
We investigate collective aspects of Rydberg excitations in ultracold mesoscopic samples. Strong interactions between Rydberg atoms influence the excitation process and impose correlations between excited atoms. The manifestations of the collective behavior of Rydberg excitations are many-body Rabi oscillations, spatial correlations between atoms, as well as fluctuations in the number of excited atoms. We study these phenomena in detail by numerically solving the many-body Schr\"odinger equation, using a ``superatom'' approach. We find that, under certain conditions, these many-body behaviors could be observed experimentally.
Pulsed laser excitation of a dense ultracold Cs vapor has been used to study the pairwise interactions between Cs atoms excited to np3/2n{p}_{3/2}np3/2​ Rydberg states of principal quantum numbers in the range n=22−−36n=22--36n=22−−36. Molecular resonances were observed that correspond to excitation of Rydberg-atom-pair states correlated not only to the np3/2+np3/2n{p}_{3/2}+n{p}_{3/2}np3/2​+np3/2​ dissociation asymptotes, but also to $n{s}_{1/2}+(n+1){s}_{1/2}, n{s}_{1/2}+{n}^{\ensuremath{'}}{f}_{j}$, and $(n\ensuremath{-}4){f}_{j}+(n\ensuremath{-}3){f}_{j}\phantom{\rule{4pt}{0ex}}(j=5/2,7/2)$ dissociation asymptotes. These pair resonances are interpreted as arising from dipole-dipole and higher-order long-range-interaction terms between the Rydberg atoms on the basis of (i) their spectral positions, (ii) their response to static and pulsed electric fields, and (iii) millimeter-wave spectra between pair states correlated to different pair-dissociation asymptotes. The Rydberg-atom-pair states were found to spontaneously decay by Penning ionization and the dynamics of the ionization process were investigated during the first 15 $\ensuremath{\mu}\mathrm{s}$ following initial photoexcitation. To interpret the experimental observations, a potential model was derived that is based on the numerical determination of the eigenvalues and eigenfunctions of the long-range interaction Hamiltonian. With this potential model, which does not include adjustable parameters, all experimental observations could be accounted for, and the results demonstrate that long-range-interaction models provide a global and accurate description of interactions in ultracold Rydberg gases and that they correctly account for, and enable the analysis of, phenomena as diverse as the formation of Rydberg macrodimers, Penning ionization in dense Rydberg gases, and Rydberg-excitation-blockade effects.
Systems of cold, interacting Rydberg atoms are of interest because they exhibit a wide range of collective quantum phenomena. This thesis describes experimental and theoretical work related to these systems with an emphasis on two phenomena: Rydberg excitation blockades and quantum-state-changing collisions. I begin by presenting a detailed calculation of the interaction energies of two Rydberg atoms for a variety of orientations, quantum states, and applied electric fields. The calculated energies are used to interpret the experimental results that follow. I then describe measurements showing that the widths of the distributions of Rydberg excitation number are related to the effectiveness of a Rydberg excitation blockade. These distributions are investigated as a function of principal quantum number, n, and applied electric field. In the presence of a Forster resonant field, sub-Poissonian distributions are measured. I next present a spectroscopic measurement of the energy level shift of a system of atoms which collectively shares two Rydberg excitations. The qualitative nature of the shift depends sensitively on the type of interactions between the atoms (van der Waals or dipole-dipole) and may be changed by changing the quantum state or applied electric field. This measurement provides the first spectroscopic proof that Rydberg excitation blockades are operative. Finally, I describe measurements of the probability for quantum state-changing and Penning-ionizing collisions to provide evidence for intrinsic, electric field-free-interaction resonances and complex many-body interactions in systems of cold Rydberg atoms.
During this thesis, the Physics of interacting systems has been investigated experimentally using Cold Rydberg gases. Rydberg atoms are very excited atoms and have the particularity to interact strongly together through long-range electrostatic interaction. A first highlight of the thesis is a direct experimental observation of a 4-body process. This process consists in internal exchanges of excitations between 4 Rydberg atoms due to their mutual interactions. In addition to its experimental observation, the process has been succefully described theoretically at a quantum level. A second highlight of this thesis has concerns the study of the laser excitation of strongly interacting Rydberg gases. In this regime, many-body quantum correlations play a central role leading to fascinating many-body behavior. In addition to fundamental interests, such systems could be used to implement quantum simulator or non-classical light sources. The system has been investigated during this thesis through the counting statistics of the Rydberg excitation. A highly sub-poisonian, i.e correlated, statistics has been observed in the regim of strong interactions proving the many-body nature of the system. A third highlight of this thesis is the development of an original theoretical model to describe the laser excitation of strongly interacting Rydberg gases. Using the so-called Dicke collective states, it has been possible to catch several interesting features of this many-body problem.