Paper on Photon-photon interactions in Rydberg-atom arrays

L. Zhang, V. Walther, K. Mølmer, T. Pohl

We investigate the interaction of weak light fields with two-dimensional lattices of atoms, in which two-photon coupling establishes conditions of electromagnetically induced transparency and excites high lying atomic Rydberg states. This system features different interactions that act on disparate length scales, from zero-range defect scattering of atomic excitations and finite-range dipole exchange interactions to long-range Rydberg-state interactions that span the entire array. Analyzing their interplay, we identify conditions that yield a nonlinear quantum mirror which coherently splits incident fields into correlated photon-pairs in a single transverse mode, while transmitting single photons unaffected. Such strong photon-photon interactions in the absence of otherwise detrimental photon losses in Rydberg-EIT arrays opens up a promising approach for the generation and manipulation of quantum light, and the exploration of many-body phenomena with interacting photons.

Paper on Nonclassical Light from Exciton Interactions in a Two-Dimensional Quantum Mirror

V. Walther, L. Zhang, S. F. Yelin, and T. Pohl

Excitons in a semiconductor monolayer form a collective resonance that can reflect resonant light with extraordinarily high efficiency. Here, we investigate the nonlinear optical properties of such atomistically thin mirrors and show that finite-range interactions between excitons can lead to the generation of highly non-classical light. We describe two scenarios, in which optical nonlinearities arise either from direct photon coupling to excitons in excited Rydberg states or from resonant two-photon excitation of Rydberg excitons with finite-range interactions. The latter case yields conditions of electromagnetically induced transparency and thereby provides an efficient mechanism for single-photon switching between high transmission and reflectance of the monolayer, with a tunable dynamical timescale of the emerging photon-photon interactions. Remarkably, it turns out that the resulting high degree of photon correlations remains virtually unaffected by Rydberg-state decoherence, in excess of non-radiative decoherence observed for ground-state excitons in two-dimensional semiconductors. This robustness to imperfections suggests a promising new approach to quantum photonics at the level of individual photons.

Paper on Polariton Exchange Interactions in Multichannel Optical Networks

Physical Review Letters 123, 113605 (2019)

M. Khazali, C. R. Murray, and T. Pohl

We examine the dynamics of Rydberg polaritons with dipolar interactions that propagate in multiple spatial modes. The dipolar excitation exchange between different Rydberg states mediates an effective exchange between polaritons that enables photons to hop across different spatial channels. Remarkably, the efficiency of this photon exchange process can increase with the channel distance and becomes optimal at a finite rail separation. Based on this mechanism, we design a simple photonic network that realizes a two photon quantum gate with a robust π phase, protected by the symmetries of the underlying photon interaction and the geometry of the network. These capabilities expand the scope of Rydberg electromagnetically induced transparency towards multidimensional geometries for nonlinear optical networks and explorations of photonic many-body physics.

Paper on Polariton dynamics in strongly interacting quantum many-body systems

Physical Review Research 2, 023102 (2020)

A. Camacho-Guardian, K. K. Nielsen, T. Pohl, and G. M. Bruun

We develop a theory for light propagating in an atomic Bose-Einstein condensate in the presence of strong interactions. The resulting many-body correlations are shown to have profound effects on the optical properties of this interacting medium. For weak atom-light coupling, there is a well-defined quasiparticle, the polaron-polariton, supporting light propagation with spectral features differing significantly from the noninteracting case. The damping of the polaron-polariton depends nonmonotonically on the light-matter coupling strength, initially increasing and then decreasing. This gives rise to an interesting crossover between two quasiparticles: a bare polariton and a polaron-polariton, separated by a complex and lossy mixture of light and matter.

Paper on Superfluid flow of polaron polaritons above Landau’s critical velocity

Physical Review Letters 125, 035301 (2020)

K. K. Nielsen, A. Camacho-Guardian, G. M. Bruun, and T. Pohl

We develop a theory for the interaction of light with superfluid optical media, describing the motion of quantum impurities that are created and dragged through the liquid by propagating photons. It is well known that a mobile impurity suffers dissipation due to phonon emission as soon as it moves faster than the speed of sound in the superfluid—Landau’s critical velocity. Surprisingly we find that in the present hybrid light-matter setting, polaritonic impurities can be protected against environmental decoherence and be allowed to propagate well above the Landau velocity without jeopardizing the superfluid response of the medium.

Paper on Plasma-Enhanced Interaction and Optical Nonlinearities of Rydberg Excitons

Physical Review Letters 125, 097401 (2020)

V. Walther and T. Pohl

We theoretically investigate the nonlinear optical transmission through a cuprous oxide crystal for wavelengths that cover the series of highly excited excitons, observed in recent experiments. Since such Rydberg excitons have strong van der Waals interactions, they can dynamically break the conditions for resonant exciton creation and dramatically modify the refractive index of the material in a nonlinear manner. We explore this mechanism theoretically and determine its effects on the optical properties of a semiconductor for the case of degenerate pair-state asymptotes of Rydberg excitons in Cu_{2}O. Upon analyzing the additional effects of a dilute residual electron-hole plasma, we find quantitative agreement with previous transmission measurements, which provides strong indications for the enhancement of Rydberg-induced nonlinearities by surrounding free charges.

Paper on Controlling exciton-phonon interactions via electromagnetically induced transparency

Physical Review Letters 125, 173601 (2020)

V. Walther, P. Grünwald, and T. Pohl

Highly excited Rydberg states of excitons in Cu2O semiconductors provide a promising approach to explore and control strong particle interactions in a solid-state environment. A major obstacle has been the substantial absorption background that stems from exciton-phonon coupling and lies under the Rydberg excitation spectrum, weakening the effects of exciton interactions. Here, we demonstrate that two-photon excitation of Rydberg excitons under conditions of electromagnetically induced transparency (EIT) can be used to control this background. Based on a microscopic theory that describes the known single-photon absorption spectrum, we analyze the conditions under which two-photon EIT permits separating the optical Rydberg excitation from the phonon-induced absorption background, and even suppressing it entir7ely. Our findings thereby pave the way for the exploitation of Rydberg blockade with Cu2O excitons in nonlinear optics and other applications.

Paper on Self-bound droplet clusters in laser-driven Bose-Einstein condensates

Phys. Rev. A 103, 023308 (2021)

Y.-C. Zhang, V. Walther, and T. Pohl

We investigate a two-dimensional Bose-Einstein condensate that is optically driven via a retro-reflecting mirror, forming a single optical feedback loop. This induces a peculiar type of long-range atomic interaction with highly oscillatory behavior, and we show here how the sign of the underlying interaction potential can be controlled by additional optical elements and external fields. This additional tunability enriches the behavior of the system substantially and gives rise to a surprising range of ground states of the condensate. In particular, we find the emergence of self-bound crystals of quantum droplets with various lattice structures, from simple and familiar triangular arrays to complex superlattice structures and crystals with entirely broken rotational symmetry. This includes mesoscopic clusters composed of small numbers of quantum droplets as well as extended crystalline structures. Importantly, such ordered states are entirely self-bound and stable without any external in-plane confinement, having no counterpart to other quantum-gas settings with long-range atomic interactions.

Paper on Strongly Correlated States of Light and Repulsive Photons in Chiral Chains of Three-Level Quantum Emitters

Phys. Rev. Lett. 126, 083605 (2021)

Ole A. Iversen and Thomas Pohl

We study the correlated transport of photons through a chain of three-level emitters that are coupled chirally to a photonic mode of a waveguide. It is found that this system can transfer a weak classical input into a strongly correlated state of light in a unitary manner. Our analysis reveals two-photon scattering eigenstates, that are akin to Fano resonances or shape resonances in particle collisions and facilitate the emergence of antibunched light with long-range correlations upon crossing a critical length of the chain. By operating close to conditions of electromagnetically induced transparency of the three-level medium, a high degree of antibunching and photon transmission can be maintained in the presence of moderate losses. These features suggest a promising mechanism for single-photon generation and may open the door to exploring correlated quantum many-body states of light with repulsively interacting photons.

Paper on Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2

Nature Communications 12, 2269 (2021)

J. Gu, V. Walther, L. Waldecker, D. Rhodes, A. Raja, J. C. Hone, T. F. Heinz, S. Kéna-Cohen, T. Pohl and V. M. Menon 

Strong optical nonlinearities play a central role in realizing quantum photonic technologies. Exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such interactions is generally not sufficient to reach the regime of quantum nonlinear optics. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities. Here we demonstrate the formation of exciton-polaritons using excited excitonic states in monolayer tungsten diselenide (WSe2) embedded in a microcavity. The realized excited-state polaritons exhibit an enhanced nonlinear response ∼𝑔2𝑠𝑝𝑜𝑙−𝑝𝑜𝑙∼46.4±13.9𝜇𝑒𝑉𝜇𝑚2gpol−pol2s∼46.4±13.9μeVμm2 which is ∼4.6 times that for the ground-state exciton. The demonstration of enhanced nonlinear response from excited exciton-polaritons presents the potential of generating strong exciton-polariton interactions, a necessary building block for solid-state quantum photonic technologies.