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Nonthermalizing Dynamics of Interacting Rydberg Atoms

Chlanda, Nicolaus A.

Published May 7, 2025• 0 citations
OpenAlex

Abstract

An isolated system of ultracold Rydberg atoms can come to equilibrium by exchanging energy through dipole-dipole interactions. In our experiment, a static electric field of a few V/cm shifts the energy levels of the atoms, so that the energy levels are nearly degenerate at zero field and fan out with increasing field to form a manifold. We excite atoms to energy levels near the center of the manifold, where the spacing is nearly harmonic. We allow them to interact for a few microseconds, by which time the population of each energy level has reached a steady state. The population is then measured at various densities and compared to simulation results. We use the notion of dynamical typicality to predict the equilibrium configuration and show that the system fails to thermalize.

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•Jan 1, 2013•1 citation
An isolated system of ultracold Rydberg atoms can come to equilibrium by exchanging energy through dipole-dipole interactions. In our experiment, a static electric field of a few V/cm shifts the energy levels of the atoms, so that the energy levels are nearly degenerate at zero field and fan out with increasing field to form a manifold. We excite atoms to energy levels near the center of the manifold, where the spacing is nearly harmonic. We allow them to interact for a few microseconds, by which time the population of each energy level has reached a steady state. The population is then measured at various densities and compared to simulation results. We use the notion of dynamical typicality to predict the equilibrium configuration and show that the system fails to thermalize.
We use dynamical quantum typicality to predict the thermal equilibrium state of ultracold Rydberg atoms exchanging energy via long-range dipole-dipole interactions. We excite atoms to the center of a manifold of nearly-harmonically spaced clusters of Stark energy levels and then allow them to equilibrate. Comparing the equilibrium state to our thermal prediction across a range of Rydberg densities, we find that this system generally fails to thermalize, though it approaches the thermal state at the highest tested density. This is the first direct comparison of a dynamical quantum typicality calculation to experiment.
We measure the transport of energy among the internal states of ultracold rubidium Rydberg atoms coupled by dipole-dipole exchange. In a magneto-optical trap, a static electric field of a few V/cm shifts the energy levels of the atoms. For a particular principal quantum number, nnn, the angular momentum eigenstates ℓ>4\ell > 4ℓ>4 are nearly degenerate at zero electric field. At nonzero field, a manifold of equally spaced clusters form a ladder with each rung consisting of a set of closely spaced mmm energy eigenstates. We excite Rydberg atoms to energy levels near the center of the manifold and allow them to exchange energy via resonant dipole-dipole interactions. We measure the time evolution as energy spreads away from the center of the manifold, which reveals that the system may fail to thermalize for long interaction times. A computational model that includes only a few essential features of the system qualitatively agrees with this result.
Isolated quantum systems are typically observed to come to thermal equilibrium. The weak Eigenstate Thermalization Hypothesis (wETH) states that the vast majority of eigenvectors are thermal. This implies that most initial states should thermalize. Studying the rare cases in which they fail to thermalize could reveal insight into quantum dynamics. In our experiment, we excite Rydberg atoms and allow them to exchange energy via dipole-dipole interactions. We find that they do not thermalize. We present numerical and theoretical results that show that our experimental initial state is not typical.
The dipole-dipole interaction strongly couples ultracold highly excited atoms, known as Rydberg atoms, and is the dominant mechanism for energy exchange among such atoms on microsecond time scales. I present the results of experiments that investigate this interaction using rubidium atoms excited to Rydberg states with an all-diode laser system. In the first of these, high resolution dipole-dipole interaction spectra for different magnetic sublevels of the 32d5/2 state are collected and analyzed. In the second experiment, ultracold rubidium atoms are implusively excited to coherent superpositions of three closely spaced |mj|sublevels of the 32d5/2 state in a weak electric field. The magnitude of the field sets the energy level spacing between these states, and hence the frequency of the phase dependent oscillations resulting from interference in resonant energy exchange processes. In the third experiment, the dipole-dipole interaction induced resonant energy exchange between columns of ultracold rubidium Rydberg atoms is imaged using a new technique involving selective field ionization with a spatially sensitive ion detector.
Systems are known to thermalize, or reach equilibrium, with the passing of time. However, when this does not occur, the quantum states of the system may be localized. Localized states carry information of the system’s initial state that is typically lost during the process of thermalization. We aim to study thermalization and localization in systems of rubidium Rydberg atoms, and to further understand these phenomena via simulation while we are developing a more refined experiment. These atoms exchange energy via tuned resonances while contained within a magneto optical trap. This process can be categorized as either a two, three, or four body interaction; localization is only expected to occur in the latter two. As the atoms transfer energy via dipole-dipole interactions, the population of atoms occupying different states shifts. Some atoms are shifted to a measurable state, and each trial of the experiment lasts for only several microseconds as data is collected. The energy transport within the system is simulated on a supercomputer in order to produce a model for the experimental data, while also allowing us to closely analyze parameters that are not accessible through experiment. From the model, we hope to learn whether the system thermalizes or localizes. We present initial simulation results exploring the energy exchange dynamics in a Rubidium many-body system.
This thesis reports the investigation of cooperative non-equilibrium dynamics in a thermal Rydberg ensemble. Cooperative behaviour arises due to resonant dipole-dipole interactions between highly excited Rydberg atoms. In order to transfer atomic population from the ground state to the Rydberg state in a caesium vapour, a three-photon excitation scheme is developed. This scheme has a number of benefits over traditional two-photon Rydberg excitation as each transition utilises in- expensive high-power diode lasers. The process of developing the excitation scheme produces a number of important results, including an excited-state polarisation spectroscopy technique and the observation of coherent three-photon electromagnetically induced transparency. The optical response and atomic dynamics of the interacting ensemble can be separated into two distinct phases. When the Rydberg number density is low and the interactions are negligible, the system can be described by the behaviour of a single atom. However, when the Rydberg number density is high, resonant dipole-dipole interactions result in a significant modification of the ensemble properties. This cooperative many-body phase cannot be described by the behaviour of a single atom. In the frequency domain, the interactions produce an excitation-dependent cooperative energy shift that is observed using probe transmission spectroscopy. In the time domain, the interactions result in a cooperative enhancement of the atomic decay rate that is analysed using fluorescence spectroscopy. At the transition between the single-body and many-body phase, a first-order non-equilibrium phase transition occurs. This is observed spatially along the length of the excitation region as a sharp switch in the emitted fluorescence. The first-order phase transition is also observed in the temporal response of the ensemble through critical slowing down. The divergence of the switching time to steady state follows a universal scaling law for phase transitions and the determined critical exponent is in excellent agreement with previous work on non-equilibrium phase transitions.