Skip to main content

Research Repository

Advanced Search

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; Lynch, Stephen A.

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


Authors

Joshua P. Rogers

Liam Gallagher liam.a.gallagher@durham.ac.uk
Post Doctoral Research Associate

Chris Hodges

Wolfgang Langbein

Stephen A. Lynch



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 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.

Citation

Rogers, J. P., Gallagher, L. A., Pizzey, D., Pritchett, J. D., Adams, C. S., Jones, M. P., …Lynch, S. A. (2022). High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O. Physical Review B, 105(11), Article 115206. https://doi.org/10.1103/physrevb.105.115206

Journal Article Type Article
Acceptance Date Mar 14, 2022
Online Publication Date Mar 31, 2022
Publication Date Mar 15, 2022
Deposit Date Jun 15, 2022
Publicly Available Date Jun 15, 2022
Journal Physical Review B
Print ISSN 2469-9950
Electronic ISSN 2469-9969
Publisher American Physical Society
Peer Reviewed Peer Reviewed
Volume 105
Issue 11
Article Number 115206
DOI https://doi.org/10.1103/physrevb.105.115206

Files

Published Journal Article (12.6 Mb)
PDF

Copyright Statement
Reprinted with permission from the American Physical Society: Rogers, Joshua P., Gallagher, Liam A. P., Pizzey, Danielle, Pritchett, Jon D., Adams, Charles S., Jones, Matthew P. A., Hodges, Chris, Langbein, Wolfgang & Lynch, Stephen A. (2022). High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O. Physical Review B 105(11): 115206. © (2022) by the American Physical Society. Readers may view, browse, and/or download material for temporary copying purposes only, provided these uses are for noncommercial personal purposes. Except as provided by law, this material may not be further reproduced, distributed, transmitted, modified, adapted, performed, displayed, published, or sold in whole or part, without prior written permission from the American Physical Society.





You might also like



Downloadable Citations