Microwave-optical coupling via Rydberg excitons in cuprous oxide

Gallagher, Liam A. P.; Rogers, Joshua; Pritchett, Jon D.; Mistry, Rajan A.; Pizzey, Danielle; Adams, Charles S.; Jones, Mike I; Grünwald, P.; Walther, Valentin; Hodges, Chris; Langbein, Wolfgang Werner; Lynch, Stephen Anthony

doi:10.1103/physrevresearch.4.013031

Cited by 21 publications

(14 citation statements)

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“…Lastly we note that the highly coherent, narrowband nature of the SHG produced in our experiment makes it very useful for applications, even within the currently observed range of principal quantum numbers. An example is the recent observation of the coherent modulation of the second harmonic by an applied microwave electric field [26].…”

Section: -10mentioning

confidence: 99%

“…The signal therefore vanishes above the bandgap of the material. These properties were essential to a recent demonstration of the microwave modulation of an optical carrier in cuprous oxide [26]. It is therefore an important question whether the even-parity spectrum may be resolved up to the same high principal quantum numbers (n > 25) observed in one-photon excitation of the nP series [1,18].…”

Section: Introductionmentioning

confidence: 99%

“…For SHG resonant with the even-parity states, the amplitude S n,L ∝ Q nl→VB M VB→nl [26]. Here Q nl→VB is the quadrupole matrix element between the Rydberg state and the valence band, which is predicted to scale as |Q nl→VB | 2 ∝ n −3 FIG.…”

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High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O

et al. 2022

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We present a study of even-parity Rydberg exciton states in cuprous oxide using second harmonic generation (SHG) spectroscopy. Excitonic states with principal quantum number n = 5 − 12 were excited by nanosecond pulses around 1143 nm. Using time-resolved single-photon counting, the coherently generated second harmonic was isolated both temporally and spectroscopically from inelastic emission due to lower-lying free and bound excitonic states, which included narrow resonances at 1.993 eV associated with a long lifetime of 641 ± 7 µs. The near transform-limited excitation bandwidth enabled high-resolution measurements of the exciton lineshape and position, from which we obtained values for the quantum defects of the S and D excitonic states associated with the appropriate crystal symmetries. Odd-parity P and F excitonic states were also observed, in accordance with predicted quadrupole-allowed two-photon excitation processes. We compared our measurements to conventional one-photon spectroscopy in the same sample, and find that the SHG spectrum is cut off at a lower principal quantum number (n = 12 vs n = 15). We attribute this effect to a combination of spatial inhomogeneities and local heating, and discuss the prospects for observing higher principal quantum number even-parity states in future experiments.

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Section: Introductionmentioning

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High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O

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“…Since signatures of coherence were observed [12], several theoretical studies focused on the optical nonlinearities of Rydberg excitons [13][14][15] in view of their potential for nonlinear quantum optics [6,7,16,17]. Experimental studies on Rydberg exciton nonlinearities are dominated by second harmonic generation (SHG) as a potent spectroscopic tool [18][19][20][21] and by investigating the blockadeinduced nonlinear absorption [8,22,23]. However, so far, no experimental study has looked at the giant Kerrtype optical nonlinearities expected from the sharp Rydberg resonances [13].…”

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“…Recent theoretical studies pave the way toward such goals [6,7], using both intra-series [17] and inter-series [38,39] Rydberg exciton transitions, including the non-trivial role of phonons [14]. With promising new results for intra-series coupling in the microwave domain [23] and recent advances in THz sources [40,41] enabling to explore transitions in the 1 ∼ 10 meV range, experimentally probing two-photon strategies is likely to soon yield important results for solid-state Rydberg physics.…”

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Self-Kerr effect across the yellow $\mathrm{Cu_2O}$ Rydberg series

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Tignon²,

Mangeney³

et al. 2022

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Probing Excitonic Rydberg States by Plasmon Enhanced Nonlinear Optical Spectroscopy in Monolayer WS₂ at Room Temperature

et al. 2022

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The optoelectronic properties of two-dimensional (2D) transition metal dichalcogenide (TMDC) monolayers such as WS 2 are largely dominated by excitons due to strong Coulomb interactions in these 2D confined monolayers, which lead to formation of Rydberg-like excitonic states below the free quasiparticle band gap. The precise knowledge of high order Rydberg excitonic states is of great importance for both fundamental understanding such as many-electron effects and device applications such as optical switching and quantum process information. Bright excitonic states could be probed by linear optical spectroscopy, while probing dark excitonic states generally requires nonlinear optical (NLO) spectroscopy. Conventional optical methods for probing high-order Rydberg excitonic states were generally performed at cryogenic temperatures to ensure enough signal-to-noise ratio (SNR) and narrow line width. Here we have designed a hybrid nanostructure of monolayer WS 2 integrated with a plasmonic cavity and investigated their NLO properties at the single particle level. Giant enhancement in NLO responses, stronger excitonic resonance effects, and narrowed line widths of NLO excitation spectra were observed when monolayer WS 2 was placed in our carefully designed plasmonic cavity. Optimum enhancement of 1000-, 3000-, and 3800-fold were achieved for two-photon photoluminescence (2PPL), second harmonic generation (SHG), and third-harmonic generation (THG), respectively, in the optimized cavity structure. The line width of SHG excitation spectra was reduced from 43 down to 15 meV. Plasmon enhanced NLO responses brought improved SNR and spectral resolution, which allowed us to distinguish discrete excitonic states with small energy differences at room temperature. By using three complementary NLO techniques in combination with linear optical spectroscopy, energies of Rydberg excitonic states of A (1s, 2s, 2p, 3s, 3p, 4s), B (1s), and C and D excitons of monolayer WS 2 have been accurately determined, which allow us to determine exciton binding energy and quasiparticle bandgap. It was interesting to find that the 2p lies 30 meV below 2s, which lends strong support to the theoretical prediction of nonlocal dielectric screening effects based on a non-hydrogenic model. Our results show that plasmon enhanced NLO spectroscopy could serve as a general method for probing high order Rydberg excitonic states of 2D materials.

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Microwave-optical coupling via Rydberg excitons in cuprous oxide

Cited by 21 publications

References 92 publications

High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O

High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O

Self-Kerr effect across the yellow $\mathrm{Cu_2O}$ Rydberg series

Probing Excitonic Rydberg States by Plasmon Enhanced Nonlinear Optical Spectroscopy in Monolayer WS₂ at Room Temperature

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Microwave-optical coupling via Rydberg excitons in cuprous oxide

Cited by 21 publications

References 92 publications

High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O

High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O

Self-Kerr effect across the yellow $\mathrm{Cu_2O}$ Rydberg series

Probing Excitonic Rydberg States by Plasmon Enhanced Nonlinear Optical Spectroscopy in Monolayer WS2 at Room Temperature

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Probing Excitonic Rydberg States by Plasmon Enhanced Nonlinear Optical Spectroscopy in Monolayer WS₂ at Room Temperature