Ultrafast control of strong light–matter coupling

Lange, Christoph; Cancellieri, E.; Panna, Dmitry; Whittaker, D. M.; Steger, Mark; Snoke, D. W.; Pfeiffer, L. N.; West, K. W.; Hayat, Alex

doi:10.1088/1367-2630/aa9fd0

Cited by 6 publications

(10 citation statements)

References 42 publications

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“…1c, d ), and the pulsewidth-limited signal indicates that the shift only occurs when the pump pulse is present. The lack of coherent oscillations before t = 0 confirms that the measurement is in the adiabatic limit of the Stark shift, which avoids additional Δ R / R spectral broadening 26 . When the pump and probe are cross-circularly polarized there is no significant signal near t = 0.…”

Section: Resultsmentioning

confidence: 56%

“…The expected Δ R / R signal shown in Fig. 1 d has the “double Lorentzian-derivative” shape that characterizes the experimental signature of the polaritonic optical Stark effect 25 , 26 . For a valley-selective polaritonic OSE, this Δ R / R spectrum only occurs when the pump and probe are co-polarized.…”

Section: Resultsmentioning

confidence: 69%

“…This dramatic polarization contrast suggests that for a particular circular polarization of the off-resonant pump, the Stark shift is isolated to polaritons in a single valley. The long-timescale background signal present for t > 0 in both polarization configurations is attributed to the generation of real carriers by two-photon absorption of the pump pulse 4,26,30 . Since the OSE signal here is polarization-selective, the background is removed for subsequent analysis by subtracting the crosspolarized signal from the co-polarized signal.…”

Section: Resultsmentioning

confidence: 90%

“…Transient reflectance spectroscopy measures the difference between the shifted and unshifted reflectance spectra ΔR, normalized by the unshifted reflectance R. The expected ΔR/R signal shown in Fig. 1d has the "double Lorentzian-derivative" shape that characterizes the experimental signature of the polaritonic optical Stark effect 25,26 . For a valley-selective polaritonic OSE, this ΔR/R spectrum only occurs when the pump and probe are co-polarized.…”

Section: Resultsmentioning

confidence: 98%

“…While the optical Stark effects of excitons have been measured in a variety of semiconductors, optical Stark effects in excitonpolaritons have so far only been measured in GaAs quantum wells [24][25][26][27] . Even in GaAs quantum wells, polarization-selective optical Stark shifts of polaritons have not yet been demonstrated.…”

mentioning

confidence: 99%

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Valley-selective optical Stark effect of exciton-polaritons in a monolayer semiconductor

et al. 2021

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Selective breaking of degenerate energy levels is a well-known tool for coherent manipulation of spin states. Though most simply achieved with magnetic fields, polarization-sensitive optical methods provide high-speed alternatives. Exploiting the optical selection rules of transition metal dichalcogenide monolayers, the optical Stark effect allows for ultrafast manipulation of valley-coherent excitons. Compared to excitons in these materials, microcavity exciton-polaritons offer a promising alternative for valley manipulation, with longer lifetimes, enhanced valley coherence, and operation across wider temperature ranges. Here, we show valley-selective control of polariton energies in WS2 using the optical Stark effect, extending coherent valley manipulation to the hybrid light-matter regime. Ultrafast pump-probe measurements reveal polariton spectra with strong polarization contrast originating from valley-selective energy shifts. This demonstration of valley degeneracy breaking at picosecond timescales establishes a method for coherent control of valley phenomena in exciton-polaritons.

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Section: Resultsmentioning

confidence: 56%

Section: Resultsmentioning

confidence: 69%

Section: Resultsmentioning

confidence: 90%

Section: Resultsmentioning

confidence: 98%

mentioning

confidence: 99%

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Valley-selective optical Stark effect of exciton-polaritons in a monolayer semiconductor

et al. 2021

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Multimode Vibrational Strong Coupling of Methyl Salicylate to a Fabry–Pérot Microcavity

et al. 2020

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The strong coupling of an IR-active molecular transition with an optical mode of the cavity results in vibrational polaritons, which opens a new way to control chemical reactivity via confined electromagnetic fields of the cavity. In this study, we design a voltagetunable open microcavity and we show the formation of multiple vibrational polaritons in methyl salicylate. A Rabi splitting and polariton anticrossing behavior is observed when the cavity mode hybridizes with the CO stretching vibration of methyl salicylate. Furthermore, the proposed theoretical model based on coupled harmonic oscillators reveals that the absorption of uncoupled molecules must also be considered to model the experimental spectra properly and that simultaneous coupling of multiple molecular vibrations to the same cavity mode has a significant influence on the transmission spectral profile.

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Inverted optical bistability and optical limiting in coherently driven exciton–polaritons

et al. 2023

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Exciton–polaritons in optical cavities exhibit strong nonlinearities predominantly because of the third-order Kerr-like interactions mediated by the excitonic component. Under quasi-resonant excitation, depending on the energy of the incident laser, it results in the optical limiting or bistable behavior. The latter phenomenon is manifested by the hysteresis loop observed in the input–output power characteristics, when a cavity is quasi-resonantly driven by a laser field. The direction of the loop is typically counterclockwise when increasing and subsequently decreasing the optical power. In this work, we demonstrate the optical bistability with an inverted hysteresis direction. It is observed in an exfoliated CdTe-based semiconductor microcavity when the frequency of the pumping laser is tuned slightly below the lower polariton mode. This unusual behavior is caused by the interplay of the suppression of strong coupling and the redshift of the lower polariton mode energy when increasing the incident power. We show that under these conditions, the polariton microcavity can be used as an optical limiter. All of the experimental observations, the shape and the direction of the hysteresis and the optical limiting behavior, are fully supported by a theoretical model.

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Ultrafast control of strong light–matter coupling

Cited by 6 publications

References 42 publications

Valley-selective optical Stark effect of exciton-polaritons in a monolayer semiconductor

Valley-selective optical Stark effect of exciton-polaritons in a monolayer semiconductor

Multimode Vibrational Strong Coupling of Methyl Salicylate to a Fabry–Pérot Microcavity

Inverted optical bistability and optical limiting in coherently driven exciton–polaritons

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