High-Resolution Second Harmonic Generation Spectroscopy with Femtosecond Laser Pulses on Excitons in Cu${}_2$O

Abstract

We present a novel spectroscopic technique for second harmonic generation (SHG) using femtosecond laser pulses at 30~kHz repetition rate, which nevertheless provides high spectral resolution limited only by the spectrometer. The potential of this method is demonstrated by applying it to the yellow exciton series of Cu${}_2$O. Besides even parity states with $S-$ and $D-$ envelope, we also observe odd parity, $P-$ excitons with linewidths down to 100 $\mu$eV, despite of the broad excitation laser spectrum with a full width at half maximum of 14~meV. The underlying light-matter interaction mechanisms of SHG are elaborated by a group theoretical analysis which allows us to determine the linear and circular polarization dependences, in good agreement with experiment.

arXiv comment9 pages, 8 figures

References in corpus (7)

• Non-linear Optical Spectroscopy of Excited Exciton States for Efficient Valley Coherence Generation in WSe2 Monolayers
• Giant Rydberg Excitons in Cuprous Oxide
• Intrinsic exciton states mixing and non-linear optical properties in transition metal dichalcogenide monolayers
• Second harmonic generation spectroscopy of excitons in ZnO
• Observation of excitonic resonances in the second harmonic spectrum of MoS${}_2$
• High resolution study of the yellow excitons in Cu${}_2$O subject to an electric field
• The even exciton series in Cu${}_2$O

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• High resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu${}_2$O
• Second Harmonic Generation of cuprous oxide in magnetic fields
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• Fast Reflective Optic-Based Rotational Anisotropy Nonlinear Harmonic Generation Spectrometer
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