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High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O [dataset] Open Access

We present a study of even-parity Rydberg exciton states in cuprous oxide using time-resolved second harmonic generation (SHG). 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 an long lifetime of 641 +/- 7 us. 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.

Descriptions

Resource type

Dataset

Contributors

Creator: Rogers, Joshua P. ¹
Contact person: Rogers, Joshua P. ¹
Data collector: Rogers, Joshua P. ¹
Data curator: Rogers, Joshua P. ¹
Data collector: Gallagher, Liam A. P. ¹
Contact person: Jones, Matthew P. A. ¹
Data collector: Pritchett, Jon D. ¹
Contact person: Adams, Charles S. ¹
Data collector: Pizzey, Danielle ¹
Contact person: Lynch, Stephen A. ²
Contact person: Langbein, Wolfgang W. ²
Contact person: Hodges, Chris ²

¹ Department of Physics, University of Durham, UK
² School of Physics and Astronomy, Cardiff University, UK

Funder

Engineering and Physical Sciences Research Council

Research methods

Experimental spectroscopy of cryogenically cooled cuprous oxide gemstone.

Other description

The raw data for the paper entitled 'High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O'

Keyword

SHG spectroscopy
Cuprous oxide
Rydberg excitons

Subject

High resolution spectroscopy
Laser spectroscopy--Research
Laser spectroscopy
Time-resolved spectroscopy
Nonlinear optical spectroscopy

Location

Department of Physics, University of Durham, UK

Language

English

Cited in

arxiv:2111.13062

Identifier

ark:/32150/r1t435gd034
doi:10.15128/r1t435gd034

Rights

Creative Commons Attribution 4.0 International (CC BY)

Publisher

Durham University

Date Created

2021-12-15

File Details

Depositor

J.P. Rogers

Date Uploaded

15 December 2021, 14:12:04

Date Modified

5 January 2022, 11:01:14

Audit Status

Audits have not yet been run on this file.

Characterization

File format: zip (ZIP Format)

Mime type: application/zip

File size: 6912562

Last modified: 2021:12:15 14:10:05+00:00

Filename: High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O.zip

Original checksum: 222b7932fb7ece2bd08ac2828b709827