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Contactless quantum non-linear optics with cold Rydberg atoms

Hannes Busche

Published Jan 1, 2017• 2 citations
OpenAlex

Abstract

Rydberg quantum optics achieves optical non-linearities at the single-photon level by mapping the strong dipolar interactions between Rydberg atoms in cold atomic gases onto light fields using electromagnetically-induced transparency and photon storage. The non-linearities are a direct consequence of the long-range character of the interaction which allows a single photon to modify the optical response in a volume containing many atoms. In this thesis, the long-range character of the resulting effective photon-photon interaction is directly observed as photons propagating in non-overlapping optical modes are stored as collective Rydberg excitations in adjacent and non-overlapping microscopic clouds of 87Rb atoms. While stored, van-der-Waals interactions imprint spatially non-uniform phase shifts in the collective excitations. These distort the photons' retrieval modes resulting in anti-correlated retrieval between the original modes.In this first demonstration of contactless effective interactions between photons, these effects are observed between photons separated by more than 15 times their wavelength, well above the optical diffraction limit.This represents a promising step towards the implementation of scalable, multichannel quantum optical devices such as quantum gates. The experiments are enabled by a new, specialised experimental setup centred around a pair of in-vacuo aspheric lenses. These provide optical resolution of order 1 µm to optically trap and address the ensembles separated by distances well below the range of Rydberg interactions. The ensembles are prepared in approximately 100 ms thanks to efficient loading of a magneto-optical trap (MOT) from an atomic beam produced by a 2D MOT. Combined with the ability to recycle the ensembles > 20000 times, effective cycle times exceeding 100 kHz enable the acquisition of large datasets for the analysis of photon statistics within a matter of minutes.

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Using electromagnetically induced transparency and photon storage, the strong dipolar interactions between Rydberg atoms and the resulting dipole blockade can be mapped onto light fields to realise optical non-linearities and interactions at the single photon level. We report on the realisation of an experimental apparatus designed to study interactions between single photons stored as Rydberg excitations in optically trapped microscopic ensembles of ultracold 87Rb atoms. A pair of in-vacuum high numerical aperture lenses focus excitation and trapping beams down to 1 μm, well below the Rydberg blockade. Thanks to efficient magneto-optical trap (MOT) loading from an atomic beam generated by a 2D MOT and the ability to recycle the microscopic ensembles more than 20000 times without significant atom loss, we achieve effective repetition rates exceeding 110 kHz to obtain good photon counting statistics on reasonable time scales. To demonstrate the functionality of the setup, we present evidence of strong photon interactions including saturation of photon storage and the retrieval of non-classical light. Using in-vacuum antennae operating at up to 40 GHz, we perform microwave spectroscopy on photons stored as Rydberg excitations and observe an interaction induced change in lineshape depending on the number of stored photons.

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Photons are good candidates for carrying quantum information because they are very stable particles: they interact weakly with the medium and barely with each other. However, this has drawbacks when you want to process the information because, in this case, it is preferable to have photon-photon interactions. For example, for applications in quantum repeaters, such interactions would allow deterministic Bell state measurements, increasing the entanglement distribution rate between two remote nodes. Getting two photons to interact with each other efficiently requires mapping them into a nonlinear medium at the single-photon level, that is, a medium that reacts differently when it interacts with a single photon than when it does with two. Such strong nonlinearity has been demonstrated with Rydberg atoms, which are atoms excited to a state with a high principal quantum number. In this thesis we have performed nonlinear quantum optics experiments using an ensemble of cold Rydberg atoms, where we have studied the properties of the quantum light emitted by these atoms. First, we demonstrated nonlinearities at the single-photon level. To reach this stage, we made several improvements to the previous experimental setup available in the group, of which the implementation of a dipole trap was especially relevant. We evidence quantum nonlinearity by measuring photon antibunching for the transmitted light after interacting with the Rydberg state under electromagnetically induced transparency (EIT). We also showed the generation of single photons on-demand after storing weak coherent states of light pulses as collective Rydberg excitations. Then, we studied the variation of the light statistic throughout the output pulse after propagating through the medium as Rydberg polaritons, which are superposition states of light and Rydberg excitations. We showed that the properties at the beginning and the end of the pulse were different from those of the steady state. In particular, the light detected after the input pulse was abruptly turned off gave much stronger suppression of two-photon events. Then, we investigated how to exploit this effect to generate single photons on demand. To do this, we analyzed the quality of the single photons detected at the end of the pulse as a function of the detection probability and compared the results with those obtained by storing the input pulse as collective Rydberg excitations. We showed that the photons were generated more efficiently when increasing the detection window at the cost of deteriorating the single photons statistics. Finally, we investigated the indistinguishability of the photons emitted by our Rydberg atomic ensemble, a crucial property for using Rydberg atoms as nodes in quantum networks. We also compared the single photons generated after storage under EIT conditions with those obtained using a two-photon Raman excitation to the Rydberg state. We measured the indistinguishability by making them interfere with weak coherent states of light in a Hong-Ou-Mandel experiment. And we showed that, although we obtained better photon statistics under EIT conditions, the indistinguishability from those obtained with Raman excitation was significantly higher.

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Photons are ideal carriers of quantum information: they are fast, low-loss, and compatible with mature photonic infrastructure.Linear optical quantum computing exploits these properties but relies on probabilistic measurements and post-selection, incurring an exponential resource overhead that limits scalability [1].Circumventing this bottleneck requires deterministic quantum logic gates, which in turn demand strong, controllable interactions between individual photons.Photons do not interact in free space or in linear optical media.The standard route to attain effective photonphoton interactions is to hybridise photons with interacting matter excitations, forming polaritons.The matter component introduces an interaction-induced anharmonic level shift U into the ladder of polariton states: when one polariton occupies a mode, the next photon sees a shifted resonance (Fig. 1a).The key figure of merit is U/γ, where γ is the total polariton decoherence rate.For U/γ ≪ 1 the nonlinearity is classical; for U/γ ≳ 1 the system enters the quantum nonlinear regime, enabling photon blockade, large conditional phase shifts, and deterministic photonic gates.Atomic Rydberg systems have provided the clearest demonstration of this regime.Atoms excited to Rydberg states -electronic states with large principal quantum numbers n ≫ 1 -possess unique properties [2].Their lifetimes scale as 1/γ ∝ n 3 and transition dipole moments as µ ∝ n 2 , leading to strong dipole-dipole (U ∝ n 4 /r 3 ) or van der Waals (U ∝ n 11 /r 6 ) interactions over long distances r.These interactions can be imprinted onto photons via electromagnetically induced transparency (EIT) [3]: photons hybridise with collective atomic excitations to form slowly propagating Rydberg polaritons that strongly interact with each other over distances of up to tens of micrometres [4].This mechanism has produced photon blockade [5]

中国科学通报:英文版•Sep 8, 2026•0 citations
Rydberg quantum optics achieves optical non-linearities at the single-photon level by mapping the strong dipolar interactions between Rydberg atoms in cold atomic gases onto light fields using electromagnetically-induced transparency and photon storage. The non-linearities are a direct consequence of the long-range character of the interaction which allows a single photon to modify the optical response in a volume containing many atoms. In this thesis, the long-range character of the resulting effective photon-photon interaction is directly observed as photons propagating in non-overlapping optical modes are stored as collective Rydberg excitations in adjacent and non-overlapping microscopic clouds of 87Rb atoms. While stored, van-der-Waals interactions imprint spatially non-uniform phase shifts in the collective excitations. These distort the photons' retrieval modes resulting in anti-correlated retrieval between the original modes.In this first demonstration of contactless effective interactions between photons, these effects are observed between photons separated by more than 15 times their wavelength, well above the optical diffraction limit.This represents a promising step towards the implementation of scalable, multichannel quantum optical devices such as quantum gates. The experiments are enabled by a new, specialised experimental setup centred around a pair of in-vacuo aspheric lenses. These provide optical resolution of order 1 µm to optically trap and address the ensembles separated by distances well below the range of Rydberg interactions. The ensembles are prepared in approximately 100 ms thanks to efficient loading of a magneto-optical trap (MOT) from an atomic beam produced by a 2D MOT. Combined with the ability to recycle the ensembles > 20000 times, effective cycle times exceeding 100 kHz enable the acquisition of large datasets for the analysis of photon statistics within a matter of minutes.
High optical nonlinearities can be achieved at the single photon level by coupling the photon states to strongly interacting Rydberg excitations under the conditions of electromagnetically induced transparency. The nonlinear response in Rydberg quantum optics comes as a direct result of the long range dipole-dipole interactions via Rydberg blockade and interaction induced dephasing. In this thesis, Rydberg quantum optics experiments are performed with two spatially separated mediums with a nonlinear response at the single photon level. Two ultracold rubidium atomic clouds are tightly confined by a pair of in-vacuo aspheric lenses such that only a few Rydberg excitations can exist in each one of the clouds simultaneously. The long range character of the dipole-dipole interactions leads to the generation of quantum states of light. The effective photon-photon interactions are directly observed as an anti-correlation in the simultaneous photon retrieval as a result of the non resonant van der Waals interactions. The collective Rydberg excitations, stored in the non-overlapping mediums, experience an additional spatial non-uniform phase. In addition, we experimentally characterize the cooperative optical response of a cold atomic medium at a single photon level. This aims to exploit the enhancement of the spontaneous emissions decay rate (superradiance) as a dependence of the number of atoms involved in the ensemble. The observed atomic response in two different regimes gives a further understanding of the system dynamics and unlocks a promising potential route towards the implementation in scalable, multichannel quantum optical devices.
Using electromagnetically induced transparency and photon storage, the strong dipolar interactions between Rydberg atoms and the resulting dipole blockade can be mapped onto light fields to realise optical non-linearities and interactions at the single photon level. We report on the realisation of an experimental apparatus designed to study interactions between single photons stored as Rydberg excitations in optically trapped microscopic ensembles of ultracold 87Rb atoms. A pair of in-vacuum high numerical aperture lenses focus excitation and trapping beams down to 1 μm, well below the Rydberg blockade. Thanks to efficient magneto-optical trap (MOT) loading from an atomic beam generated by a 2D MOT and the ability to recycle the microscopic ensembles more than 20000 times without significant atom loss, we achieve effective repetition rates exceeding 110 kHz to obtain good photon counting statistics on reasonable time scales. To demonstrate the functionality of the setup, we present evidence of strong photon interactions including saturation of photon storage and the retrieval of non-classical light. Using in-vacuum antennae operating at up to 40 GHz, we perform microwave spectroscopy on photons stored as Rydberg excitations and observe an interaction induced change in lineshape depending on the number of stored photons.
Interacting Rydberg excitations in cold atomic ensembles can exhibit large quantum nonlinearities that enable engineering of strong interactions between individual photons. Consequently, Rydberg ensembles are a promising platform for quantum information applications and the study of more fundamental physics of few- and many-body phenomena with interacting photons. This thesis presents a series of experiments that study and exploit different regimes of Rydberg-mediated interactions. We report the realization of an efficient on-demand single-photon source. The strong long-range Rydberg interactions allow the excitation of only a single collective Rydberg state within the entire atomic medium. The collective excitation can be subsequently retrieved as a single-photon. We use this scheme to generate highly pure and highly indistinguishable photons, which are suitable for scalable quantum information applications. These photons can be compatible with other atomic systems due to their narrow bandwidth, which makes building practical hybrid quantum systems feasible. Here, we demonstrate high visibility two-photon quantum interference between our Rydberg-produced photons, and photons emitted by a remote single-trapped ion. We also study Rydberg atoms under electromagnetically induced transparency conditions, where coherent superpostions of photons and Rydberg excitations propagate through the atomic medium as lossless dark-state polaritons. In the experiment, we use the external control fields to tune the interactions to a many-body regime where we can observe resonant scattering of dark-state polaritons to lossy channels. We show that the enhanced scattering process arises as a pure three-body effect.
Mapping the strong interaction between Rydberg excitations in ultra-cold atomic ensembles onto single photons enables the realization of optical nonlinearities which can modify light on the level of individual photons.This novel approach forms the basis of a growing Rydberg quantum optics toolbox, which already contains photonic logic building-blocks such as single-photon sources, switches, transistors, and conditional π-phase shifts.This thesis reports on two experiments investigating strong photon-photon interactions mediated by Rydberg interactions.First, applying a ladder-type EIT scheme to Rydberg atoms in D-states with high principal quantum number results in the Rydberg interaction mediated nonlinearity accompanied by a time-dependent decay of transmission of probe light through the medium.In a joint experimental and theoretical analysis, this effect is attributed to the dephasing of propagating polaritons into stationary Rydberg excitations caused by the state mixing interaction occurring with Rydberg D-state atoms.Second, via a two-photon Raman excitation scheme Rydberg atoms are efficiently excited in a small atomic cloud.As the size of the Rydberg blockade exceeds the dimension of the medium, only a single Rydberg excitation can be present at a time.By fast engineered dephasing this Rydberg excitation is decoupled from the light field.Measurement of the transmitted light and the amount of excited Rydberg atoms gives evidence for the realization of a deterministic single-photon absorber.
Photons are good candidates for carrying quantum information because they are very stable particles: they interact weakly with the medium and barely with each other. However, this has drawbacks when you want to process the information because, in this case, it is preferable to have photon-photon interactions. For example, for applications in quantum repeaters, such interactions would allow deterministic Bell state measurements, increasing the entanglement distribution rate between two remote nodes. Getting two photons to interact with each other efficiently requires mapping them into a nonlinear medium at the single-photon level, that is, a medium that reacts differently when it interacts with a single photon than when it does with two. Such strong nonlinearity has been demonstrated with Rydberg atoms, which are atoms excited to a state with a high principal quantum number. In this thesis we have performed nonlinear quantum optics experiments using an ensemble of cold Rydberg atoms, where we have studied the properties of the quantum light emitted by these atoms. First, we demonstrated nonlinearities at the single-photon level. To reach this stage, we made several improvements to the previous experimental setup available in the group, of which the implementation of a dipole trap was especially relevant. We evidence quantum nonlinearity by measuring photon antibunching for the transmitted light after interacting with the Rydberg state under electromagnetically induced transparency (EIT). We also showed the generation of single photons on-demand after storing weak coherent states of light pulses as collective Rydberg excitations. Then, we studied the variation of the light statistic throughout the output pulse after propagating through the medium as Rydberg polaritons, which are superposition states of light and Rydberg excitations. We showed that the properties at the beginning and the end of the pulse were different from those of the steady state. In particular, the light detected after the input pulse was abruptly turned off gave much stronger suppression of two-photon events. Then, we investigated how to exploit this effect to generate single photons on demand. To do this, we analyzed the quality of the single photons detected at the end of the pulse as a function of the detection probability and compared the results with those obtained by storing the input pulse as collective Rydberg excitations. We showed that the photons were generated more efficiently when increasing the detection window at the cost of deteriorating the single photons statistics. Finally, we investigated the indistinguishability of the photons emitted by our Rydberg atomic ensemble, a crucial property for using Rydberg atoms as nodes in quantum networks. We also compared the single photons generated after storage under EIT conditions with those obtained using a two-photon Raman excitation to the Rydberg state. We measured the indistinguishability by making them interfere with weak coherent states of light in a Hong-Ou-Mandel experiment. And we showed that, although we obtained better photon statistics under EIT conditions, the indistinguishability from those obtained with Raman excitation was significantly higher.
Photons are ideal carriers of quantum information: they are fast, low-loss, and compatible with mature photonic infrastructure.Linear optical quantum computing exploits these properties but relies on probabilistic measurements and post-selection, incurring an exponential resource overhead that limits scalability [1].Circumventing this bottleneck requires deterministic quantum logic gates, which in turn demand strong, controllable interactions between individual photons.Photons do not interact in free space or in linear optical media.The standard route to attain effective photonphoton interactions is to hybridise photons with interacting matter excitations, forming polaritons.The matter component introduces an interaction-induced anharmonic level shift U into the ladder of polariton states: when one polariton occupies a mode, the next photon sees a shifted resonance (Fig. 1a).The key figure of merit is U/γ, where γ is the total polariton decoherence rate.For U/γ ≪ 1 the nonlinearity is classical; for U/γ ≳ 1 the system enters the quantum nonlinear regime, enabling photon blockade, large conditional phase shifts, and deterministic photonic gates.Atomic Rydberg systems have provided the clearest demonstration of this regime.Atoms excited to Rydberg states -electronic states with large principal quantum numbers n ≫ 1 -possess unique properties [2].Their lifetimes scale as 1/γ ∝ n 3 and transition dipole moments as µ ∝ n 2 , leading to strong dipole-dipole (U ∝ n 4 /r 3 ) or van der Waals (U ∝ n 11 /r 6 ) interactions over long distances r.These interactions can be imprinted onto photons via electromagnetically induced transparency (EIT) [3]: photons hybridise with collective atomic excitations to form slowly propagating Rydberg polaritons that strongly interact with each other over distances of up to tens of micrometres [4].This mechanism has produced photon blockade [5]