Many-body interactions and correlations in atomic ensembles are fundamental in understanding many-body effects such as collective and emergent phenomena and also play an important role in various atom-based applications. Optical two-dimensional coherent spectroscopy (2DCS) provides a powerful tool to measure many-body interactions and correlations. Here, we present the study of many-body dipole-dipole interactions and correlations in potassium and rubidium atomic vapors by using double-quantum and multi-quantum 2DCS. The results show that double-quantum 2DCS provides sensitive and background-free detection of weak dipole-dipole interaction between atoms with a mean separation up to about 16 μm, and multi-quantum 2DCS can excite and detect multi-atom states (Dicke states) with up to eight correlated atoms. The technique of optical 2DCS can provide a new approach to study many-body physics in atomic ensembles and can be potentially implemented to measure many-body effects in cold atoms and other atomic/molecular systems.
Optical two-dimensional coherent spectroscopy (2DCS) has become a powerful tool for studying energy-level structure, dynamics, and coupling in many systems including atomic ensembles. Various types of two-dimensional (2D) spectra, including the so-called single-quantum, zero-quantum, and double-quantum 2D spectra, of both
D lines (
D1 and
D2 transitions) of potassium (K) atoms have been reported previously. For rubidium (Rb), a major difference is that the
D lines are about 15 nm apart as opposed to only about 3 nm for K. Simultaneously exciting both
D lines of Rb atoms requires a broader laser bandwidth for the experiment. Here, we report a broadband optical 2DCS experiment in a Rb atomic vapor. A complete set of single-quantum, zero-quantum, and double-quantum 2D spectra including both
D lines of Rb atoms were obtained. The experimental spectra were reproduced by simulated 2D spectra based on the perturbation solutions to the optical Bloch equations. This work in Rb atoms complements previous 2DCS studies of K and Rb with a narrower bandwidth that covers two
D lines of K or only a single
D line of Rb. The broadband excitation enables the capability to perform double-quantum and multiquantum 2DCS of both
D lines of Rb to study many-body interactions and correlations in comparison with K atoms.
Collective resonance of interacting particles has important implications in many-body quantum systems and their applications. Strong interactions can lead to a blockade that prohibits the excitation of a collective resonance of two or more nearby atoms. However, a collective resonance can be excited with the presence of weak interaction and has been observed for atoms in the first excited state (P state). Here, we report the observation of collective resonance of rubidium atoms in a higher excited state (D state) in addition to the first excited state. The collective resonance is excited by a double-quantum four-pulse excitation sequence. The resulting double-quantum two-dimensional (2D) spectrum displays well-isolated peaks that can be attributed to collective resonances of atoms in P and D states. The experimental one-quantum and double-quantum 2D spectra can be reproduced by a simulation based on the perturbative solutions to the optical Bloch equations, confirming collective resonances as the origin of the measured spectra. The experimental technique provides a new approach for preparing and probing collective resonances of atoms in highly excited states.
We report a novel, to the best of our knowledge, double-quantum-zero-quantum two-dimensional coherent spectroscopy (2DCS) that allows direct detection of the quantum coherence between multiparticle collective states. Through correlating the double-quantum coherence and the zero-quantum coherence, signatures for coherence between collective states can be well isolated as side peaks and readily identified in the 2D spectrum. The experiment is implemented in a vapor of rubidium atoms in a collinear 2DCS setup. Good agreement with a theoretical simulation using density matrix confirms the essential role of the interatomic correlation effect in generating the side peak signals. This 2D spectrum technique paves a new avenue for studying the coherent coupling of highly excited states and many-body properties.
is the Bohr radius. The experimental results confirm the long range nature of the dipole-dipole interaction, which is critical for understanding many-body physics in atoms/molecules. The long range interaction also has implications in atom-based applications involving many-body interactions. Additionally, we demonstrated that double-quantum 2DCS is sufficiently sensitive to probe dipole-dipole interaction at densities that can be achieved with cold atom in a magneto-optical trap, paving the way for double-quantum 2DCS studies of cold atoms and molecules. The method can also open a new avenue to study long-range interactions in solid state systems such as quantum dots and color centers in diamonds.