Observation of Forbidden Exciton Transitions Mediated by Coulomb Interactions in Photoexcited Semiconductor Quantum Wells

Rice, William; Kono, Junichiro; Zybell, S.; Winnerl, Stephan; Bhattacharyya, Jayeeta; Schneider, Harald; Helm, M.; Ewers, Benjamin; Chernikov, A.; Koch, Martin; Chatterjee, Sangam; Khitrova, G.; Gibbs, H. M.; Schneebeli, L.; Breddermann, B.; Kira, M.; Koch, S. W.

doi:10.1103/physrevlett.110.137404

Cited by 30 publications

(10 citation statements)

References 36 publications

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“…[25]. When they are defined either from microscopic computations [129,25,28] or experiments [137,138], one can indeed explain nontrivial details of the experimentally observed quantum-kinetic phenomena, as long the effects depend directly on polarization and density dynamics. Naturally, this approximation scheme should not be used when one studies direct effects of higher-order clusters.…”

Section: Dephasing In the Hbesmentioning

confidence: 99%

Hyperbolic Bloch equations: Atom-cluster kinetics of an interacting Bose gas

Kira

2015

Annals of Physics

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Experiments with ultracold Bose gases can already produce so strong atom-atom interactions that one can observe intriguing many-body dynamics between the Bose-Einstein condensate (BEC) and the normal component. The excitation picture is applied to uniquely express the many-body state uniquely in terms of correlated atom clusters within the normal component alone. Implicit notation formalism is developed to explicitly derive the quantum kinetics of all atom clusters. The clusters are shown to build up sequentially, from smaller to larger ones, which is utilized to nonperturbatively describe the interacting BEC with as few clusters as possible. This yields the hyperbolic Bloch equations (HBEs) that not only generalize the Hartree-Fock Bogoliubov approach but also are analogous to the semiconductor Bloch equations (SBEs). This connection is utilized to apply sophisticated many-body techniques of semiconductor quantum optics to BEC investigations. Here, the HBEs are implemented to determine how a strongly interacting Bose gas reacts to a fast switching from weak to strong interactions, often referred to as unitarity. The computations for 35 Rb demonstrate that molecular states (dimers) depend on atom density, and that the many-body interactions create coherent transients on a 100 µs time scale converting BEC into normal state via quantum depletion.

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Section: Dephasing In the Hbesmentioning

confidence: 99%

Hyperbolic Bloch equations: Atom-cluster kinetics of an interacting Bose gas

Kira

2015

Annals of Physics

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“…The TeraHertz (THz, 3-330 cm −1 , 0.1-10 THz), or farinfrared, region of the electromagnetic spectrum is one such frontier that offers novel probes of a variety of condensedmatter systems such as charge transport in semiconductors, 1,2 the biophysics of vision, 3 and the coherent control of molecular reactions. 4 Of particular interest to physical chemistry, the THz-active degrees of freedom correspond to soft, largeamplitude modes of a liquid that participate directly in the molecular dynamics.…”

Section: Introductionmentioning

confidence: 99%

Nonlinear terahertz coherent excitation of vibrational modes of liquids

Allodi

Finneran

Blake

2015

The Journal of Chemical Physics

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We report the first coherent excitation of intramolecular vibrational modes via the nonlinear interaction of a TeraHertz (THz) light field with molecular liquids. A TeraHertz-TeraHertz-Raman pulse sequence prepares the coherences with a broadband, high-energy, (sub)picosecond TeraHertz pulse, that are then measured in a TeraHertz Kerr effect spectrometer via phase-sensitive, heterodyne detection with an optical pulse. The spectrometer reported here has broader TeraHertz frequency coverage, and an increased sensitivity relative to previously reported TeraHertz Kerr effect experiments. Vibrational coherences are observed in liquid diiodomethane at 3.66 THz (122 cm −1 ), and in carbon tetrachloride at 6.50 THz (217 cm −1 ), in exact agreement with literature values of those intramolecular modes. This work opens the door to 2D spectroscopies, nonlinear in TeraHertz field, that can study the dynamics of condensed-phase molecular systems, as well as coherent control at TeraHertz frequencies.

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“…EPs demonstrate remarkable physical phenomena such as Bose–Einstein condensation (BEC) and single-photon nonlinearity, which are extremely difficult in solid-state materials. , These phenomena are all determined by the EP relaxation dynamics to ground states (lowest polariton band) once they are excited, involving various competing mechanisms with the thermalization process. , Depending on the relaxation efficiency, the final population distribution of EPs with respect to the ground states could enable various exotic quantum properties for polariton condensation and nonlinear optics. , However, distinct relaxation dynamics would be introduced to develop the conventional understanding of key processes for EP physical phenomena, when EP excited states (higher energy bands) are involved. These excited states introduce unique fundamental properties, such as different parity symmetry and quantum coherence, − leading to abundant QED with distinct light–matter interactions, including coherent energy exchange, , ultrafast terahertz transitions, , and optical selection rules. ,,− …”

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confidence: 95%

Nonlinear Optics at Excited States of Exciton Polaritons in Two-Dimensional Atomic Crystals

Liu

et al. 2020

Nano Lett.

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Exciton polaritons (EPs) are partial-light partialmatter quasiparticles in semiconductors demonstrating striking quantum phenomena such as Bose−Einstein condensation and single-photon nonlinearity. In these phenomena, the governing process is the EP relaxation into the ground states upon excitation, where various mechanisms are extensively investigated with thermodynamic limits. However, the relaxation process becomes drastically different and could significantly advance the understanding of EP dynamics for these quantum phenomena, when excited states of EPs are involved. Here, for the first time, we observe nonlinear optical responses at the EP excited states in a monolayer tungsten disulfide (WS 2 ) microcavity, including dark excited states and dynamically metastable upper polariton bands. The nonlinear optics leads to unique emissions of ground states with prominent valley degree of freedom (DOF) via an anomalous relaxation process, which is applicable to a wide range of semiconductors from monolayer transition metal dichalcogenides (TMDs) to emerging halide perovskites. This work promises possible approaches to challenging experiments such as valley polariton condensation. Moreover, it also constructs a valleydependent solid-state three-level system for terahertz photonics and stimulated Raman adiabatic passage.

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Observation of Forbidden Exciton Transitions Mediated by Coulomb Interactions in Photoexcited Semiconductor Quantum Wells

Cited by 30 publications

References 36 publications

Hyperbolic Bloch equations: Atom-cluster kinetics of an interacting Bose gas

Hyperbolic Bloch equations: Atom-cluster kinetics of an interacting Bose gas

Nonlinear terahertz coherent excitation of vibrational modes of liquids

Nonlinear Optics at Excited States of Exciton Polaritons in Two-Dimensional Atomic Crystals

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