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arXiv:1302.6621 · Physical Review Letters

Nonequilibrium Phase Transition in a Dilute Rydberg Ensemble

C. Carr, Ralf Ritter, Christopher G. Wade, Charles S. Adams, Kevin J. Weatherill

Published Sep 10, 2013• 248 citations
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Abstract

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.

DOI
10.1103/physrevlett.111.113901

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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.
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.
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.
The possibility of experimental creation of a system of Rydberg atoms with an arbitrary probability distribution of their dipole moments is shown. The equation of state is calculated by the Monte Carlo method in the NVT ensemble for two options of the distribution: isotropic distribution and distribution for the system of identical dipoles. Critical parameters of the phase transition and the binodal are determined in both cases. Critical temperatures for both options virtually coincide. However, critical density for isotropic distribution is 20 times higher. It is shown that the absence of spatial separation in the region of coexistence of dense and dilute phases is a specific feature of the phase transition in dipole systems, and such absence of separation is due to the topological features of clusters of the dense phase. Areas of parameters for the experimental observation of the self-organisation of ultracold Rydberg atoms on the existing experimental stands are determined.
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 study a driven-dissipative system of atoms in the presence of laser excitation to a Rydberg state and spontaneous emission. The atoms interact via the blockade effect, whereby an atom in the Rydberg state shifts the Rydberg level of neighboring atoms. We use mean-field theory to study how the Rydberg population varies in space. As the laser frequency changes, there is a continuous transition between the uniform and antiferromagnetic phases. The nonequilibrium nature also leads to a novel oscillatory phase and bistability between the uniform and antiferromagnetic phases.