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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, Langbein, Wolfgang and Lynch, Stephen A. 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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Abstract

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: 01 Apr 2022 14:30
URI: https://orca.cardiff.ac.uk/id/eprint/149006

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