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

Rogers, Joshua P., Gallagher, Liam A. P., Pizzey, Danielle, Pritchett, Jon D., Adams, Charles S., Jones, Matthew P. A., Hodges, Chris ORCID:, Langbein, Wolfgang ORCID: and Lynch, Stephen A. ORCID: 2022. High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O. Physical Review B 105 (11) , 115206. 10.1103/PhysRevB.105.115206

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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 n m . 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 e V associated with a long lifetime of 641 ± 7 μ s . 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.

Item Type: Article
Date Type: Published Online
Status: Published
Schools: Physics and Astronomy
Publisher: American Physical Society
ISSN: 2469-9950
Funders: EPSRC
Date of First Compliant Deposit: 31 March 2022
Date of Acceptance: 14 March 2022
Last Modified: 03 May 2023 12:31

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