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

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
Date Modified
5 January 2022, 11:01:14
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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
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User N. Syrotiuk has updated High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O [dataset] 5 months ago
User N. Syrotiuk has updated High-resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu2O [dataset] 5 months ago