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arXiv:1606.08791 · Physical Review X

Phase Diagram and Self-Organizing Dynamics in a Thermal Ensemble of Strongly Interacting Rydberg Atoms

Dong-Sheng Ding, Hannes Busche, Bao-Sen Shi, Guang-Can Guo, Charles S. Adams

Published Apr 29, 2020• 68 citations
arXivHTMLPDF

Abstract

Far-from-equilibrium dynamics that lead to self-organization are highly relevant to complex dynamical systems not only in physics but also in life, earth, and social sciences.However, it is challenging to find systems with sufficiently controllable parameters that allow quantitatively modeling of emergent properties.Here, we study a nonequilibrium phase transition and observe signatures of self-organized criticality in a dilute thermal vapor of atoms optically excited to strongly interacting Rydberg states.Electromagnetically induced transparency provides excellent control over the population dynamics and enables highresolution probing of the driven-dissipative dynamics, which also exhibits phase bistability.Increased sensitivity compared to previous work allows us to reconstruct the complete phase diagram, including in the vicinity of the critical point.We observe that interaction-induced energy shifts and enhanced decay only occur in one of the phases above a critical Rydberg population.This case limits the application of generic mean-field models; however, a modified, threshold-dependent approach is in qualitative agreement with experimental data.Near threshold, we observe self-organized dynamics in the form of population jumps that return the density to a critical value.

DOI
10.1103/physrevx.10.021023

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Far-from-equilibrium dynamics that lead to self-organization are highly relevant to complex dynamical systems not only in physics but also in life, earth, and social sciences.However, it is challenging to find systems with sufficiently controllable parameters that allow quantitatively modeling of emergent properties.Here, we study a nonequilibrium phase transition and observe signatures of self-organized criticality in a dilute thermal vapor of atoms optically excited to strongly interacting Rydberg states.Electromagnetically induced transparency provides excellent control over the population dynamics and enables highresolution probing of the driven-dissipative dynamics, which also exhibits phase bistability.Increased sensitivity compared to previous work allows us to reconstruct the complete phase diagram, including in the vicinity of the critical point.We observe that interaction-induced energy shifts and enhanced decay only occur in one of the phases above a critical Rydberg population.This case limits the application of generic mean-field models; however, a modified, threshold-dependent approach is in qualitative agreement with experimental data.Near threshold, we observe self-organized dynamics in the form of population jumps that return the density to a critical value.
Abstract Far-from equilibrium dynamics that lead to self-organization are highly relevant to complex dynamical systems not only in physics, but also in life-, earth-, and social sciences. It is challenging however to find systems with sufficiently controllable parameters that allow quantitatively modelling of emergent properties. Here, we study a non-equilibrium phase transition and observe signatures of self-organized criticality in a dilute thermal vapour of atoms optically excited to strongly interacting Rydberg states. Electromagnetically induced transparency (EIT) provides excellent control over the population dynamics and enables high-resolution probing of the driven-dissipative dynamics, which also exhibits phase bistability. Increased sensitivity compared to previous work allows us to reconstruct the complete phase diagram including in the vicinity of the critical point. We observe that interaction-induced energy shifts and enhanced decay only occur in one of the phases above a critical Rydberg population. This limits the application of generic mean-field models, however a modified, threshold-dependent approach is in qualitative agreement with experimental data. Near threshold, we observe self-organized dynamics in the form of population jumps that return the density to a critical value.
We observe and characterize intrinsic optical bistability in a dilute Rydberg vapor. The bistability is characterized by sharp jumps between states of low and high Rydberg occupancy with jump-up and -down positions displaying hysteresis depending on the direction in which the control parameter is changed. We find that the shift in frequency of the jump point scales with the fourth power of the principal quantum number. Also, the width of the hysteresis window increases with increasing principal quantum number, before reaching a peak and then closing again. The experimental results are consistent with predictions from a simple theoretical model based on semiclassical Maxwell--Bloch equations including the effects of interaction-induced broadening and level shifts. These results provide insight into the dynamics of driven dissipative systems.
We demonstrate a nonequilibrium phase transition in a dilute thermal atomic gas. The phase transition, between states of low and high Rydberg occupancy, is induced by resonant dipole-dipole interactions between Rydberg atoms. The gas can be considered as dilute as the atoms are separated by distances much greater than the wavelength of the optical transitions used to excite them. In the frequency domain, we observe a mean-field shift of the Rydberg state which results in intrinsic optical bistability above a critical Rydberg number density. In the time domain, we observe critical slowing down where the recovery time to system perturbations diverges with critical exponent α=-0.53±0.10. The atomic emission spectrum of the phase with high Rydberg occupancy provides evidence for a superradiant cascade.
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.
Due to the variety of tools available to control atomic, molecular, and optical (AMO) systems, they provide a versatile platform for studying many-body physics, quantum simulation, and quantum computation. Although extensive efforts are employed to reduce coupling between the system and the environment, the effects of the environment can never fully be avoided, so it is important to develop a comprehensive understanding of open quantum systems. The system-environment coupling often leads to loss via dissipation, which can be countered by a coherent drive. Open quantum systems subject to dissipation and drive are known as driven-dissipative systems, and they provide an excellent platform for studying many-body nonequilibrium physics. The first part of this dissertation will focus on driven-dissipative phase transitions. Despite the nonequilibrium nature of these systems, the corresponding phase transitions tend to exhibit emergent equilibrium behavior. However, we will show that in the vicinity of a multicritical point where multiple phase transitions intersect, genuinely nonequilibrium criticality can emerge, even though the individual phase transitions on their own exhibit equilibrium criticality. These nonequilibrium multicritical points can exhibit a variety of exotic phenomena not possible for their equilibrium counterparts, including the emergence of complex critical exponents, which lead to discrete scale invariance and spiraling phase boundaries. Furthermore, the Liouvillian gap can take on complex values, and the fluctuation-dissipation theorem is violated, corresponding to an effective temperature which gets "hotter" and "hotter" at longer and longer wavelengths. The second part of this dissertation will focus on Rydberg atoms. In particular, we study how the spontaneous generation of contaminant Rydberg states drastically modifies the behavior of a driven-dissipative Rydberg system due to the resultant dipole-dipole interactions. These interactions lead to a complicated competition of both blockade and anti-blockade effects, leading to strongly enhanced Rydberg populations for far-detuned drive and reduced Rydberg populations for resonant drive.
We investigate the out-of-equilibrium behavior of a dissipative gas of Rydberg atoms that features a dynamical transition between two stationary states characterized by different excitation densities. We determine the structure and properties of the phase diagram and identify the universality class of the transition, both for the statics and the dynamics. We show that the proper dynamical order parameter is in fact not the excitation density and find evidence that the dynamical transition is in the "model A" universality class; i.e., it features a nontrivial Z2 symmetry and a dynamics with nonconserved order parameter. This sheds light on some relevant and observable aspects of dynamical transitions in Rydberg gases. In particular it permits a quantitative understanding of a recent experiment [C. Carr, Phys. Rev. Lett. 111, 113901 (2013)] which observed bistable behavior as well as power-law scaling of the relaxation time. The latter emerges not due to critical slowing down in the vicinity of a second order transition, but from the nonequilibrium dynamics near a so-called spinodal line.