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arXiv:1307.2913 · Physical Review A

Collective effects in linear spectroscopy of dipole-coupled molecular arrays

Aleksey A. Kocherzhenko, Jahan M. Dawlaty, B. P. Abolins, Felipe Herrera, Douglas B. Abraham, K. Birgitta Whaley

Published Dec 2, 2014• 3 citations
arXivHTMLPDF

Abstract

We present a consistent analysis of linear spectroscopy for arrays of nearest-neighbor dipole-coupled two-level molecules that reveals distinct signatures of weak- and strong-coupling regimes separated for infinite-size arrays by a quantum critical point. In the weak-coupling regime, the ground state of the molecular array is disordered, but in the strong-coupling regime, it has (anti)ferroelectric ordering. We show that multiple molecular excitations [odd (even) in the weak- (strong-) coupling regime] can be accessed directly from the ground state. We analyze the scaling of absorption and emission with system size and find that the oscillator strengths show enhanced superradiant behavior in both ordered and disordered phases. As the coupling increases, the single-excitation oscillator strength rapidly exceeds the well-known Heitler-London value. In the strong-coupling regime we show the existence of a unique spectral transition with excitation energy that can be tuned by varying the system size and that asymptotically approaches zero for large systems. The oscillator strength for this transition scales quadratically with system size, showing an anomalous one-photon superradiance. For systems of infinite size, we find a novel singular spectroscopic signature of the quantum phase transition between disordered and ordered ground states. We outline how arrays of ultracold dipolar molecules trapped in an optical lattice can be used to access the strong-coupling regime and observe the anomalous superradiant effects associated with this regime.

DOI
10.1103/physreva.90.062502

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We present a consistent analysis of linear spectroscopy for arrays of nearest-neighbor dipole-coupled two-level molecules that reveals distinct signatures of weak- and strong-coupling regimes separated for infinite-size arrays by a quantum critical point. In the weak-coupling regime, the ground state of the molecular array is disordered, but in the strong-coupling regime, it has (anti)ferroelectric ordering. We show that multiple molecular excitations [odd (even) in the weak- (strong-) coupling regime] can be accessed directly from the ground state. We analyze the scaling of absorption and emission with system size and find that the oscillator strengths show enhanced superradiant behavior in both ordered and disordered phases. As the coupling increases, the single-excitation oscillator strength rapidly exceeds the well-known Heitler-London value. In the strong-coupling regime we show the existence of a unique spectral transition with excitation energy that can be tuned by varying the system size and that asymptotically approaches zero for large systems. The oscillator strength for this transition scales quadratically with system size, showing an anomalous one-photon superradiance. For systems of infinite size, we find a novel singular spectroscopic signature of the quantum phase transition between disordered and ordered ground states. We outline how arrays of ultracold dipolar molecules trapped in an optical lattice can be used to access the strong-coupling regime and observe the anomalous superradiant effects associated with this regime.
A consistent analysis of linear spectroscopy for arrays of dipole-coupled two-level molecules reveals distinct signatures of weak and strong coupling regimes separated by a critical point. Multiple molecular excitations (odd(even) in weak(strong) coupling) are accessed from the ground state. As the coupling increases, the single excitation oscillator strength rapidly exceeds the Heitler-London value and diverges at the critical point, returning to a quadratic size scaling in strong coupling, where also the photon frequency decreases with size. The lowest accessible excitation is found to show a one-photon hyperradiance.
Ultracold atomic systems are among the most promising platforms that have the potential to shed light on the complex behavior of many-body quantum systems. One prominent example is the case of a dense ensemble illuminated by a strong coherent drive while interacting via dipole-dipole interactions. Despite being subjected to intense investigations, this system retains many open questions. A recent experiment carried out in a pencil-shaped geometry [Ferioli Nat. Phys. 19, 1345 (2023)] has reported measurements that have seemed consistent with the emergence of strong collective effects in the form of a “superradiant” phase transition in free space, when looking at the light-emission properties in the forward direction. Motivated by the experimental observations, we carry out a systematic theoretical analysis of the steady-state properties of the system as a function of the driving strength and atom number N . We observe signatures of collective effects in the weak-driving regime, which disappear with increasing drive strength as the system evolves into a single-particle-like mixed state comprised of randomly aligned dipoles. Although the steady state features some similarities to the reported superradiant-to-normal nonequilibrium transition, also known as cooperative resonance fluorescence, we observe significant qualitative and quantitative differences, including a different scaling of the critical drive parameter (from N to N ). We validate the applicability of a mean-field treatment to capture the steady-state dynamics under currently accessible conditions. Furthermore, we develop a simple theoretical model that explains the scaling properties by accounting for interaction-induced inhomogeneous effects and spontaneous emission, which are intrinsic features of interacting disordered arrays in free space. Published by the American Physical Society 2024
Collective coupling between dipoles can dramatically modify the optical response of a medium. Such effects depend strongly on the geometry of the medium and the polarization of the light. Using a classical coupled dipole model, here we investigate the simplest case of one-dimensional arrays of interacting atomic dipoles driven by a weak laser field. Changing the polarization and direction of the driving field allows us to separately address superradiant, subradiant, redshifted, and blueshifted eigenmodes, as well as observe strong Fano-like interferences between different modes. The cooperative eigenvectors can be characterized by the phase difference between nearest-neighbor dipoles, ranging from all oscillating in phase to all oscillating out of phase with their nearest neighbors. Investigating the eigenvalue behavior as a function of atom number and lattice spacing, we find that certain eigenmodes of an infinite atomic chain have the same decay rate as a single atom between two mirrors. The effects we observe provide a framework for collective control of the optical response of a medium, giving insight into the behavior of more complicated geometries, as well as providing further evidence for the dipolar analog of cavity QED.
Ordered atomic arrays feature an enhanced collective optical response compared to random atomic ensembles due to constructive interference in resonant dipole-dipole interactions. One consequence of this is the existence of a large shift of the transition with respect to the bare atomic frequency. In the linear optics regime (low light intensity), one observes a spectroscopic shift of the Lorentzian atomic line often called the collective Lamb shift. For stronger driving, many excitations are present in the system rendering the calculation of this shift theoretically challenging, but its understanding is important for instance when performing Ramsey spectroscopy in optical clocks. Here we report on the study of the collective optical response of a one-dimensional array of 30 dysprosium atoms. We drive the atoms on the narrow intercombination transition isolating a two-level system, and measure the atomic state with single-shot state readout using a broad transition. In the linear optics regime, we measure the shift of the resonance in steady state due to dipole interactions, and measure how this shift depends on the interatomic distance. We further resolve at the single atom level how the excitation is distributed over the array. Then, on the same transition we perform Ramsey spectroscopy i.e., away from the linear regime. We observe a time-dependent shift, that allows us to draw the connection between the collective Lamb shift observed in the linear optics regime and in the large-excitation case.
We study the collective emission of a disordered array of N excited two-level atoms into a one-dimensional photonic waveguide. In the perfectly ordered case, where atoms are spaced by exact integer multiples of the wavelength, the system exhibits the characteristic superradiant burst with a peak emission rate scaling as N 2 . Using large-scale semiclassical simulations, we find that this key signature of superradiance remains asymptotically robust under strong spatial and spectral disorder, but also exhibits subtle finite-size scaling toward this limit. To explain our observations, we provide an analytical variational estimate for the maximal decay rate, which tightly bounds the numerical results and reveals how disorder shapes the collective decay. Specifically, we find that even in the presence of strong disorder, the spins tend to self-organize spontaneously according to their locations, which overall optimizes constructive interference effects and explains the emergence of mirror-asymmetric correlations in superradiant decay. These findings resolve important open questions regarding the existence and nature of superradiance in strongly disordered arrays and offer valuable insights for understanding collective quantum optical phenomena in realistic systems.
Energy and lifetime of collective optical excitations in regular arrays of atoms and molecules are significantly influenced by dipole-dipole interaction. While the dynamics of closely positioned atoms can be approximated well by the Dicke superradiance model, the situation of finite regular configurations is hard to access analytically. Most treatments use an exciton based description limited to the lowest excitation manifold. We present a general approach studying the complete decay cascade of a finite regular array of atoms from the fully inverted to the ground state. We explicitly calculate all energy shifts and decay rates for two generic cases of a three-atom linear chain and an equilateral triangle. In numerical calculations we show that despite fairly weak dipole-dipole interactions, collective vacuum coupling allows for superradiant emission as well as subradiant states in larger arrays through multi-particle interference. This induces extra dephasing and modified decay as important limitations for Ramsey experiments in lattice atomic clock setups as well as for the gain and frequency stability of superradiant lasers.