Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Probing nonlocal correlations with ultralong-range Rydberg molecules

J. D. Whalen

Published Jun 14, 2021• 0 citations
OpenAlex

Abstract

Ultracold atomic systems provide pristine environments for creating and manipulating strongly-interacting quantum systems. The flexibility and utility of ultracold atomic systems comes at the cost of isolation of the quantum system away from environmental perturbations inside of an ultra-high vacuum chamber. This isolation reduces the number of ways that these systems can be probed, in particular, there are relatively few ways to probe correlations in these systems at mesoscopic length scales. In this thesis we present a new technique for probing correlations in ultracold atomic gases using ultralong-range Rydberg molecules. We will present a description of the relevant experimental apparatus and techniques developed for laser cooling and trapping ultracold mixtures of Sr, and a brief theoretical discussion on the relationship between the pair correlation function $g^{(2)}(R)$ and the excitation rates of ultralong-range Rydberg molecules. We present two publications: the first on using ultralong-range Rydberg molecules to probe $g^{(2)}(R)$ in thermal gases, and the second on the creation of heteronuclear ultralong-range Rydberg molecules from a strongly interacting Bose mixture of $^{88}$Sr and $^{84}$Sr. Finally, we will present conclusions and a brief outlook for the future experiments utilizing this method.

Related papers

Probing nonlocal spatial correlations in quantum gases with ultra-long-range Rydberg molecules

J. D. Whalen, S. K. Kanungo, Roger Ding +7 more

We present photoexcitation of ultra-long-range Rydberg molecules as a probe of spatial correlations in bosonic and fermionic quantum gases. Rydberg molecules can be created with well-defined internuclear spacing, set by the radius of the outer lobe of the Rydberg electron wave function ${R}_{n}$. By varying the principal quantum number $n$ of the target Rydberg state, the molecular excitation rate can be used to map the pair-correlation function of the trapped gas ${g}^{(2)}({R}_{n})$. We demonstrate this with ultracold Sr gases and probe pair-separation length scales in the range ${R}_{n}=1400--3200$ ${a}_{0}$, which are on the order of the thermal de Broglie wavelength for temperatures around 1 $\ensuremath{\mu}\mathrm{K}$. We observe bunching for a single-component Bose gas of ${}^{84}\mathrm{Sr}$ and antibunching due to Pauli exclusion at short distances for a polarized Fermi gas of ${}^{87}\mathrm{Sr}$, revealing the effects of quantum statistics.

arXiv:1903.11526•Physical Review A•Jul 22, 2019•35 citations

Nonlocal spatial correlations in an interacting atomic gas

C. Wang, Ang Li, Y. Lu +4 more

We report measurements of the nonlocal two-body spatial correlation function g ( 2 ) ( R ) in an ultracold Bose gas with strong interactions using photoassociation of ultra-long-range Rydberg molecules (ULRRMs) as a spatially selective probe. This technique provides access to g ( 2 ) ( R ) on length scales from 60 to 180 nm, bridging the gap between short-range and long-range correlation measurements. The large s -wave scattering length of Sr 86 ( a = 811 a 0 ) enables exploration of the universal regime where g ( 2 ) ( R ) is governed solely by two-body interactions. Comparison with a weakly interacting isotope, Sr 84 , highlights interaction-induced suppression of pair correlations. The measured correlation functions agree quantitatively with calculations based on the two-body reduced density matrix, without adjustable parameters. Our results establish Rydberg molecular photoassociation as a powerful tool for probing nonlocal correlations in strongly interacting quantum gases.

Physical Review A•Jan 13, 2026•0 citations

Studies in Ultracold Ground State Atom-Rydberg Atom Interactions

Samuel C. Markson

Collisions involving Rydberg atoms reveal detailed information on the state of a background medium and can be used as diagnostic probes of temperature and density distributions in a neutral or ionized gas. Spectroscopy of Rydberg atoms in highly excited states reveals the interaction of the Rydberg electron with core electrons, including relativistic effects, and can be used for precise determination of fundamental constants. The advent of ultracold trapping and cooling methods in the last three decades has ushered in a new paradigm in Rydberg physics control and manipulation. The concept of the Rydberg blockade, for instance, al- lows for precise control of long-range dipolar interaction between atoms, creation of correlated many-body wave functions, and realization of macroscopic quantum entanglement and quan- tum logic operations. The formation of a new class of Rydberg molecules arising from ground and Rydberg atom collisions can be used to manipulate electron-atom scattering phase shifts, form and manipulate molecules with enormous permanent electric dipole moments, study Ry- dberg chemistry at the ultracold, and realize macroscopic quantum polaronic systems. In this thesis, I will investigate charge transfer from covalent ground-Rydberg collisions to form heavy ion pair states. In another related study, I explore the formation of spin-mixed ultralong range Rydberg molecules, by accounting for spin-dependent relativistic fine and hyperfine interac- tion. Such studies help to not only explain experimental observations, but also point to how molecular reactions can be controlled using small electric or magnetic fields.

•Jan 1, 2017•0 citations

Excitation of Rydberg Molecules in Ultracold Quantum Gases

Carsten Lippe, Tanita Eichert, Oliver Thomas +2 more

Recent experiments in our group on the excitation of Rydberg molecules in ultracold quantum gases have been reviewed. Quantum gases are a well‐suited environment to excite Rydberg molecules, due to the high atomic density and the perfect control of the internal spin degrees of freedom and the center of mass motion of the atoms. In parallel, the coupling to Rydberg molecules can be used to probe and manipulate the interaction in ultracold quantum gases. In this Feature Article, a comprehensive introduction to the field of Rydberg molecules, including ultralong‐range molecules and butterfly molecules is given. The Rydberg molecules have been characterized spectroscopically and their internal spin structure is discussed. Then, it is shown how these Rydberg molecules work as a tool to monitor the double occupancy in optical lattice experiments and to change the inter‐particle interaction with the help of a so‐called optical Feshbach resonance.

physica status solidi (b)•Mar 8, 2019•7 citations

Measuring nonlocal three-body spatial correlations with Rydberg trimers in ultracold quantum gases

S. K. Kanungo, Y. Lu, F. B. Dunning +3 more

We measure nonlocal third-order spatial correlations in nondegenerate ultracold gases of bosonic ($^{84}\mathrm{Sr}$) and spin-polarized fermionic ($^{87}\mathrm{Sr}$) strontium through studies of the formation rates for ultralong-range trimer Rydberg molecules. The trimer production rate is observed to be very sensitive to the effects of quantum statistics with a strong enhancement of up to a factor of 6 (3!), in the case of bosonic $^{84}\mathrm{Sr}$ due to bunching and a marked reduction for spin-polarized fermionic $^{87}\mathrm{Sr}$ due to antibunching. The experimental results are compared to theoretical predictions and good agreement is observed. The present approach opens the way to in situ studies of higher-order nonlocal spatial correlations in a wide array of ultracold atomic-gas systems.

arXiv:2301.00871•Physical Review A•Mar 20, 2023•14 citations

Heteronuclear Rydberg molecules

J. D. Whalen, S. K. Kanungo, Y. Lu +4 more

In this work, the authors report on the observation of heteronuclear ultralong-range Rydberg molecules, together with a detailed theoretical analysis of the experimental data. Such heteronuclear Rydberg molecules are expected to present many new opportunities for studying quantum systems, such as probing interparticle and interspecies pair correlation functions in multicomponent many-body systems, exploring the sensitivity of the isotope shift to the mass polarization energy for Rydberg trimers or larger molecules, or studying new types of Rydberg impurities in quantum gases.

arXiv:2004.14585•Physical Review A•Jun 24, 2020•17 citations
Ultracold atomic systems provide pristine environments for creating and manipulating strongly-interacting quantum systems. The flexibility and utility of ultracold atomic systems comes at the cost of isolation of the quantum system away from environmental perturbations inside of an ultra-high vacuum chamber. This isolation reduces the number of ways that these systems can be probed, in particular, there are relatively few ways to probe correlations in these systems at mesoscopic length scales. In this thesis we present a new technique for probing correlations in ultracold atomic gases using ultralong-range Rydberg molecules. We will present a description of the relevant experimental apparatus and techniques developed for laser cooling and trapping ultracold mixtures of Sr, and a brief theoretical discussion on the relationship between the pair correlation function g(2)(R)g^{(2)}(R)g(2)(R) and the excitation rates of ultralong-range Rydberg molecules. We present two publications: the first on using ultralong-range Rydberg molecules to probe g(2)(R)g^{(2)}(R)g(2)(R) in thermal gases, and the second on the creation of heteronuclear ultralong-range Rydberg molecules from a strongly interacting Bose mixture of 88^{88}88Sr and 84^{84}84Sr. Finally, we will present conclusions and a brief outlook for the future experiments utilizing this method.
We present photoexcitation of ultra-long-range Rydberg molecules as a probe of spatial correlations in bosonic and fermionic quantum gases. Rydberg molecules can be created with well-defined internuclear spacing, set by the radius of the outer lobe of the Rydberg electron wave function Rn{R}_{n}Rn​. By varying the principal quantum number nnn of the target Rydberg state, the molecular excitation rate can be used to map the pair-correlation function of the trapped gas g(2)(Rn){g}^{(2)}({R}_{n})g(2)(Rn​). We demonstrate this with ultracold Sr gases and probe pair-separation length scales in the range Rn=1400−−3200{R}_{n}=1400--3200Rn​=1400−−3200 a0{a}_{0}a0​, which are on the order of the thermal de Broglie wavelength for temperatures around 1 $\ensuremath{\mu}\mathrm{K}$. We observe bunching for a single-component Bose gas of 84Sr{}^{84}\mathrm{Sr}84Sr and antibunching due to Pauli exclusion at short distances for a polarized Fermi gas of 87Sr{}^{87}\mathrm{Sr}87Sr, revealing the effects of quantum statistics.
We report measurements of the nonlocal two-body spatial correlation function g ( 2 ) ( R ) in an ultracold Bose gas with strong interactions using photoassociation of ultra-long-range Rydberg molecules (ULRRMs) as a spatially selective probe. This technique provides access to g ( 2 ) ( R ) on length scales from 60 to 180 nm, bridging the gap between short-range and long-range correlation measurements. The large s -wave scattering length of Sr 86 ( a = 811 a 0 ) enables exploration of the universal regime where g ( 2 ) ( R ) is governed solely by two-body interactions. Comparison with a weakly interacting isotope, Sr 84 , highlights interaction-induced suppression of pair correlations. The measured correlation functions agree quantitatively with calculations based on the two-body reduced density matrix, without adjustable parameters. Our results establish Rydberg molecular photoassociation as a powerful tool for probing nonlocal correlations in strongly interacting quantum gases.
Collisions involving Rydberg atoms reveal detailed information on the state of a background medium and can be used as diagnostic probes of temperature and density distributions in a neutral or ionized gas. Spectroscopy of Rydberg atoms in highly excited states reveals the interaction of the Rydberg electron with core electrons, including relativistic effects, and can be used for precise determination of fundamental constants. The advent of ultracold trapping and cooling methods in the last three decades has ushered in a new paradigm in Rydberg physics control and manipulation. The concept of the Rydberg blockade, for instance, al- lows for precise control of long-range dipolar interaction between atoms, creation of correlated many-body wave functions, and realization of macroscopic quantum entanglement and quan- tum logic operations. The formation of a new class of Rydberg molecules arising from ground and Rydberg atom collisions can be used to manipulate electron-atom scattering phase shifts, form and manipulate molecules with enormous permanent electric dipole moments, study Ry- dberg chemistry at the ultracold, and realize macroscopic quantum polaronic systems. In this thesis, I will investigate charge transfer from covalent ground-Rydberg collisions to form heavy ion pair states. In another related study, I explore the formation of spin-mixed ultralong range Rydberg molecules, by accounting for spin-dependent relativistic fine and hyperfine interac- tion. Such studies help to not only explain experimental observations, but also point to how molecular reactions can be controlled using small electric or magnetic fields.
Recent experiments in our group on the excitation of Rydberg molecules in ultracold quantum gases have been reviewed. Quantum gases are a well‐suited environment to excite Rydberg molecules, due to the high atomic density and the perfect control of the internal spin degrees of freedom and the center of mass motion of the atoms. In parallel, the coupling to Rydberg molecules can be used to probe and manipulate the interaction in ultracold quantum gases. In this Feature Article, a comprehensive introduction to the field of Rydberg molecules, including ultralong‐range molecules and butterfly molecules is given. The Rydberg molecules have been characterized spectroscopically and their internal spin structure is discussed. Then, it is shown how these Rydberg molecules work as a tool to monitor the double occupancy in optical lattice experiments and to change the inter‐particle interaction with the help of a so‐called optical Feshbach resonance.
We measure nonlocal third-order spatial correlations in nondegenerate ultracold gases of bosonic (84Sr^{84}\mathrm{Sr}84Sr) and spin-polarized fermionic (87Sr^{87}\mathrm{Sr}87Sr) strontium through studies of the formation rates for ultralong-range trimer Rydberg molecules. The trimer production rate is observed to be very sensitive to the effects of quantum statistics with a strong enhancement of up to a factor of 6 (3!), in the case of bosonic 84Sr^{84}\mathrm{Sr}84Sr due to bunching and a marked reduction for spin-polarized fermionic 87Sr^{87}\mathrm{Sr}87Sr due to antibunching. The experimental results are compared to theoretical predictions and good agreement is observed. The present approach opens the way to in situ studies of higher-order nonlocal spatial correlations in a wide array of ultracold atomic-gas systems.
In this work, the authors report on the observation of heteronuclear ultralong-range Rydberg molecules, together with a detailed theoretical analysis of the experimental data. Such heteronuclear Rydberg molecules are expected to present many new opportunities for studying quantum systems, such as probing interparticle and interspecies pair correlation functions in multicomponent many-body systems, exploring the sensitivity of the isotope shift to the mass polarization energy for Rydberg trimers or larger molecules, or studying new types of Rydberg impurities in quantum gases.