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1. Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity

   https://doi.org/10.1073/pnas.1909948116  

   Bao, Wei ; Liu, Xiaoze ; Xue, Fei ; Zheng, Fan ; Tao, Renjie ; Wang, Siqi ; Xia, Yang ; Zhao, Mervin ; Kim, Jeongmin ; Yang, Sui ; et al ( October 2019 , Proceedings of the National Academy of Sciences)

   The condensation of half-light half-matter exciton polaritons in semiconductor optical cavities is a striking example of macroscopic quantum coherence in a solid-state platform. Quantum coherence is possible only when there are strong interactions between the exciton polaritons provided by their excitonic constituents. Rydberg excitons with high principal value exhibit strong dipole–dipole interactions in cold atoms. However, polaritons with the excitonic constituent that is an excited state, namely Rydberg exciton polaritons (REPs), have not yet been experimentally observed. Here, we observe the formation of REPs in a single crystal CsPbBr 3 perovskite cavity without any external fields. These polaritons exhibit strongmore »nonlinear behavior that leads to a coherent polariton condensate with a prominent blue shift. Furthermore, the REPs in CsPbBr 3 are highly anisotropic and have a large extinction ratio, arising from the perovskite’s orthorhombic crystal structure. Our observation not only sheds light on the importance of many-body physics in coherent polariton systems involving higher-order excited states, but also paves the way for exploring these coherent interactions for solid-state quantum optical information processing.« less
2. Exciton-polaron Rydberg states in monolayer MoSe2 and WSe2

   https://doi.org/10.1038/s41467-021-26304-w  

   Liu, Erfu ; van Baren, Jeremiah ; Lu, Zhengguang ; Taniguchi, Takashi ; Watanabe, Kenji ; Smirnov, Dmitry ; Chang, Yia-Chung ; Lui, Chun Hung ( October 2021 , Nature Communications)

   Exciton polaron is a hypothetical many-body quasiparticle that involves an exciton dressed with a polarized electron-hole cloud in the Fermi sea. It has been evoked to explain the excitonic spectra of charged monolayer transition metal dichalcogenides, but the studies were limited to the ground state. Here we measure the reflection and photoluminescence of monolayer MoSe₂and WSe₂gating devices encapsulated by boron nitride. We observe gate-tunable exciton polarons associated with the 1 s–3 s exciton Rydberg states. The ground and excited exciton polarons exhibit comparable energy redshift (15~30 meV) from their respective bare excitons. The robust excited states contradict the trion picture because themore »trions are expected to dissociate in the excited states. When the Fermi sea expands, we observe increasingly severe suppression and steep energy shift from low to high exciton-polaron Rydberg states. Their gate-dependent energy shifts go beyond the trion description but match our exciton-polaron theory. Our experiment and theory demonstrate the exciton-polaron nature of both the ground and excited excitonic states in charged monolayer MoSe₂and WSe₂.

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3. Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2

   https://doi.org/10.1038/s41467-021-22537-x  

   Gu, Jie ; Walther, Valentin ; Waldecker, Lutz ; Rhodes, Daniel ; Raja, Archana ; Hone, James C. ; Heinz, Tony F. ; Kéna-Cohen, Stéphane ; Pohl, Thomas ; Menon, Vinod M. ( December 2021 , Nature Communications)

   Abstract 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 (WSe 2 ) embedded inmore »a microcavity. The realized excited-state polaritons exhibit an enhanced nonlinear response ∼ $${g}_{{pol}-{pol}}^{2s} \sim 46.4\pm 13.9\,\mu {eV}\mu {m}^{2}$$ g p o l − p o l 2 s ~ 46.4 ± 13.9 μ e V μ m 2 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.« less
4. Rotaxane rings promote oblique packing and extended lifetimes in DNA-templated molecular dye aggregates

   https://doi.org/10.1038/s42004-021-00456-8  

   Barclay, Matthew S. ; Roy, Simon K. ; Huff, Jonathan S. ; Mass, Olga A. ; Turner, Daniel B. ; Wilson, Christopher K. ; Kellis, Donald L. ; Terpetschnig, Ewald A. ; Lee, Jeunghoon ; Davis, Paul H. ; et al ( February 2021 , Communications Chemistry)

   Molecular excitons play a central role in natural and artificial light harvesting, organic electronics, and nanoscale computing. The structure and dynamics of molecular excitons, critical to each application, are sensitively governed by molecular packing. Deoxyribonucleic acid (DNA) templating is a powerful approach that enables controlled aggregation via sub-nanometer positioning of molecular dyes. However, finer sub-Angstrom control of dye packing is needed to tailor excitonic properties for specific applications. Here, we show that adding rotaxane rings to squaraine dyes templated with DNA promotes an elusive oblique packing arrangement with highly desirable optical properties. Specifically, dimers of these squaraine:rotaxanes exhibit anmore »absorption spectrum with near-equal intensity excitonically split absorption bands. Theoretical analysis indicates that the transitions are mostly electronic in nature and only have similar intensities over a narrow range of packing angles. Compared with squaraine dimers, squaraine:rotaxane dimers also exhibit extended excited-state lifetimes and less structural heterogeneity. The approach proposed here may be generally useful for optimizing excitonic materials for a variety of applications ranging from solar energy conversion to quantum information science.

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5. Roadmap on STIRAP applications

   https://doi.org/10.1088/1361-6455/ab3995  

   Bergmann, Klaas ; Nägerl, Hanns-Christoph ; Panda, Cristian ; Gabrielse, Gerald ; Miloglyadov, Eduard ; Quack, Martin ; Seyfang, Georg ; Wichmann, Gunther ; Ospelkaus, Silke ; Kuhn, Axel ; et al ( September 2019 , Journal of Physics B: Atomic, Molecular and Optical Physics)

   STIRAP (stimulated Raman adiabatic passage) is a powerful laser-based method, usually involving two photons, for efficient and selective transfer of populations between quantum states. A particularly interesting feature is the fact that the coupling between the initial and the final quantum states is via an intermediate state, even though the lifetime of the latter can be much shorter than the interaction time with the laser radiation. Nevertheless, spontaneous emission from the intermediate state is prevented by quantum interference. Maintaining the coherence between the initial and final state throughout the transfer process is crucial. STIRAP was initially developed with applicationsmore »in chemical dynamics in mind. That is why the original paper of 1990 was published inThe Journal of Chemical Physics. However, from about the year 2000, the unique capabilities of STIRAP and its robustness with respect to small variations in some experimental parameters stimulated many researchers to apply the scheme to a variety of other fields of physics. The successes of these efforts are documented in this collection of articles. In Part A the experimental success of STIRAP in manipulating or controlling molecules, photons, ions or even quantum systems in a solid-state environment is documented. After a brief introduction to the basic physics of STIRAP, the central role of the method in the formation of ultracold molecules is discussed, followed by a presentation of how precision experiments (measurement of the upper limit of the electric dipole moment of the electron or detecting the consequences of parity violation in chiral molecules) or chemical dynamics studies at ultralow temperatures benefit from STIRAP. Next comes the STIRAP-based control of photons in cavities followed by a group of three contributions which highlight the potential of the STIRAP concept in classical physics by presenting data on the transfer of waves (photonic, magnonic and phononic) between respective waveguides. The works on ions or ion strings discuss options for applications, e.g. in quantum information. Finally, the success of STIRAP in the controlled manipulation of quantum states in solid-state systems, which are usually hostile towards coherent processes, is presented, dealing with data storage in rare-earth ion doped crystals and in nitrogen vacancy (NV) centers or even in superconducting quantum circuits. The works on ions and those involving solid-state systems emphasize the relevance of the results for quantum information protocols. Part B deals with theoretical work, including further concepts relevant to quantum information or invoking STIRAP for the manipulation of matter waves. The subsequent articles discuss the experiments underway to demonstrate the potential of STIRAP for populating otherwise inaccessible high-lying Rydberg states of molecules, or controlling and cooling the translational motion of particles in a molecular beam or the polarization of angular-momentum states. The series of articles concludes with a more speculative application of STIRAP in nuclear physics, which, if suitable radiation fields become available, could lead to spectacular results.

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