Experimental limitation in extending the exciton series in 
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 towards higher principal quantum numbers

Heckötter, Julian; Janas, David Maximilian; Schwartz, Rico; Aßmann, Marc; Bayer, М.

doi:10.1103/physrevb.101.235207

Cited by 20 publications

(14 citation statements)

References 35 publications

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“…Recent studies discussed the sensitivity of highly excited Rydberg excitons with quantum numbers n > 10 to electric fields induced by charged impurities. [5,16] As even parity D states are 5 Þ ortho exciton, the highest one in the multiplet, and the dipole-allowed P 3=2 exciton versus principal quantum number. In both panels, the red crosses show the experimental data.…”

Section: Discussionmentioning

confidence: 99%

“…Since even parity D excitons are optically activated by electric fields, the details of their fine structure are of importance for the analysis of the high-n regime close to the bandgap, where OPA spectra are influenced by the presence of inherent electric fields induced by charged impurities. [5,16] Moreover, D excitons show characteristic absorption features in OPA on synthetic samples with a certain amount of disorder. [17] 2.…”

Section: Introductionmentioning

confidence: 99%

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Analysis of the Fine Structure of the D‐Exciton Shell in Cuprous Oxide

Heckötter

Rommel

Main

et al. 2021

Physica Rapid Research Ltrs

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The exciton states in cuprous oxide show a pronounced fine structure splitting associated with the crystal environment and the resulting electronic band structure. High‐resolution spectroscopy reveals an especially pronounced splitting of the yellow D excitons with one state pushed above any other state with the same principal quantum number. This large splitting offset is related to a strong mixing of these D states with the 1S exciton of the green series, as suggested by previously published calculations. Here, a detailed comparison of this theory with experimental data is given, which leads to a complete reassignment of the experimentally observed D exciton lines. The origin of different amounts of green admixture to D‐envelope states is deduced by analyzing the different terms of the Hamiltonian. The yellow–green mixing leads to level repulsion and induces an exchange interaction splitting to D‐envelope states, from which one of them becomes the highest state within each multiplet. Furthermore, the assignment of D exciton states according to their total angular momentum F is given and corrects an earlier description given in a former study.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Analysis of the Fine Structure of the D‐Exciton Shell in Cuprous Oxide

Heckötter

Rommel

Main

et al. 2021

Physica Rapid Research Ltrs

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“…Nevertheless, our results show there is clear scope for improvement. Previous studies have suggested that charged impurities set the ultimate limit on the highest observable n, as well as contributing a background electric field that causes the anomalous broadening of the resonances [6,59,60]. Using higherquality samples with strain-free mounting and careful surface treatment thus appears essential [18].…”

Section: Discussionmentioning

confidence: 99%

“…The observation of high principal quantum number Rydberg excitons in cuprous oxide [1] (Cu 2 O) has brought about renewed interest [2][3][4][5][6] in the material. A major motivation is the potential to combine long-range van der Waals interactions (which scale with principal quantum number, n, as n 11 ) between excitons with the quantum optical properties of exciton-polaritons [4,7,8].…”

Section: Introductionmentioning

confidence: 99%

“…The apparently abrupt cut-off of the SHG spectrum from of the even parity states has important implications for the utility of SHG and the even parity states in quantum optics applications. The factors governing the visibility of high-n Rydberg excitons have been extensively studied in absorption experiments on the nP series [18,20,32,58], and include Rydberg blockade [1], thermally or optically excited free carriers [20,59], charged defects [32,60,61], and local strain and disorder [18,20]. Therefore to gain further insight we carried out further experiments on the power dependence and spatial variation of the SHG spectrum.…”

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High resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu$_{2}$O

Rogers,

Gallagher,

Pizzey

et al. 2021

Preprint

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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 1.99 eV associated with an exceptional lifetime of 641 ± 7 µs. The near transform-limited excitation bandwidth enabled detailed 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.

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A Temperature Study of High‐n$n$ Rydberg States in Cu2O${\rm Cu}_2{\rm O}$

Heckötter,

Panda,

Brägelmann

et al. 2024

Adv Quantum Tech

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The temperature dependence of Rydberg excitons in with principal quantum numbers is investigated for bath temperatures between 1.3 and 50 K. The energy shift of Rydberg exciton lines allows us to perform a precise measurement of the band gap as a function of temperature. The phonon shows a dominant contribution to the temperature shift of the band gap. The optical properties of Rydberg excitons are analyzed for different temperatures and discussed in the context of phonon scattering as well as thermal ionization of impurities and compared to earlier descriptions in Ref. [1]. The maximum principal quantum number as a function of temperature in crystals of different quality is studied and compared. The observations are correlated to photoluminescence spectra of impurities at different temperatures.

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Experimental limitation in extending the exciton series in Cu2O towards higher principal quantum numbers

Cited by 20 publications

References 35 publications

Analysis of the Fine Structure of the D‐Exciton Shell in Cuprous Oxide

Analysis of the Fine Structure of the D‐Exciton Shell in Cuprous Oxide

High resolution nanosecond spectroscopy of even-parity Rydberg excitons in Cu$_{2}$O

A Temperature Study of High‐n$n$ Rydberg States in Cu2O${\rm Cu}_2{\rm O}$

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