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. 2023 Nov 21;23(23):10901–10907. doi: 10.1021/acs.nanolett.3c03145

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© 2023 The Authors. Published by American Chemical Society

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Repump-free photoluminescence excitation (crf-PLE) of SiV^– in diamond parabolic reflectors and charge-state stabilization with 445 nm laser light. (a) Top: crf-PLE measurement averaged over 500 single sweeps across the resonance while collecting (PSB) counts. A Lorentzian fit (yellow) to the data reports an inhomogeneously broadened linewidth of 211.5 ± 0.5 MHz, within a factor of 2.15 of the lifetime limit (98.9 ± 0.9 MHz) for this particular emitter. The inset illustrates how we conduct crf-PLE experiments with constant laser intensity while modulating the laser frequency. Bottom: Trace of the PLE measurement, showing 500 single sweeps. A dashed black line acts as a guide to the eye for zero detuning. (b) Diagram illustrating the additional populations of SiV^–, classified by their behavior in crf-PLE (see main text). Populations 2 and 3 can be stabilized by applying high-powered (>5 mW) 445 nm laser light for extended durations (>1 h). (c) Top panel: Histogram of single sweep Lorentzian linewidths Δν of an SiV^– initially in population 3, which was mapped to population 1. Green bars are results from 515 nm charge-repump PLE (cr-PLE) and blue from crf-PLE after the SiV^– is exposed to the 445 nm laser. This representative data set shows that 445 nm exposure decreases single sweep linewidths compared to 515 nm cr-PLE. Middle panel: Center frequency spread extracted from the same PLE measurements, revealing that line stability is dramatically improved in crf-PLE. Bottom panel: Excitation power normalized peak intensity I_PLE comparison for 515 nm cr-PLE and crf-PLE. (d) Lorentzian fitted PLE linewidths Δν as a function of the number of sweeps over which the PLE spectrum is averaged for three representative SiV^–, comparing standard 515 nm cr-PLE (in green) and crf-PLE after 445 nm (in blue) illumination, exemplifying the distinct behavior between the measurement schemes. While crf-PLE converges to an average linewidth, linewidths measured during cr-PLE diverge [c.f. SI Figure S8 for more data sets]. Data sets corresponding to the same SiV^– are drawn with the same linestyle. The shaded area signifies the standard error. (e) Center frequency deviation σ(ν₀) comparison between crf-PLE on the y-axis and cr-PLE on the x-axis. The data point corresponding to the histograms in (c) is marked. A dashed black line denotes y = x. Markers denote the three populations introduced in (a) and (b). (f) Comparison between 515 nm cr- and crf-PLE excitation power normalized peak intensity for the three populations as in (e), with the dashed black line denoting y = x.

Inline graphic — Repump-free photoluminescence excitation (crf-PLE) of SiV^– in diamond parabolic reflectors and charge-state stabilization with 445 nm laser light. (a) Top: crf-PLE measurement averaged over 500 single sweeps across the resonance while collecting (PSB) counts. A Lorentzian fit (yellow) to the data reports an inhomogeneously broadened linewidth of 211.5 ± 0.5 MHz, within a factor of 2.15 of the lifetime limit (98.9 ± 0.9 MHz) for this particular emitter. The inset illustrates how we conduct crf-PLE experiments with constant laser intensity while modulating the laser frequency. Bottom: Trace of the PLE measurement, showing 500 single sweeps. A dashed black line acts as a guide to the eye for zero detuning. (b) Diagram illustrating the additional populations of SiV^–, classified by their behavior in crf-PLE (see main text). Populations 2 and 3 can be stabilized by applying high-powered (>5 mW) 445 nm laser light for extended durations (>1 h). (c) Top panel: Histogram of single sweep Lorentzian linewidths Δν of an SiV^– initially in population 3, which was mapped to population 1. Green bars are results from 515 nm charge-repump PLE (cr-PLE) and blue from crf-PLE after the SiV^– is exposed to the 445 nm laser. This representative data set shows that 445 nm exposure decreases single sweep linewidths compared to 515 nm cr-PLE. Middle panel: Center frequency spread extracted from the same PLE measurements, revealing that line stability is dramatically improved in crf-PLE. Bottom panel: Excitation power normalized peak intensity I_PLE comparison for 515 nm cr-PLE and crf-PLE. (d) Lorentzian fitted PLE linewidths Δν as a function of the number of sweeps over which the PLE spectrum is averaged for three representative SiV^–, comparing standard 515 nm cr-PLE (in green) and crf-PLE after 445 nm (in blue) illumination, exemplifying the distinct behavior between the measurement schemes. While crf-PLE converges to an average linewidth, linewidths measured during cr-PLE diverge [c.f. SI Figure S8 for more data sets]. Data sets corresponding to the same SiV^– are drawn with the same linestyle. The shaded area signifies the standard error. (e) Center frequency deviation σ(ν₀) comparison between crf-PLE on the y-axis and cr-PLE on the x-axis. The data point corresponding to the histograms in (c) is marked. A dashed black line denotes y = x. Markers denote the three populations introduced in (a) and (b). (f) Comparison between 515 nm cr- and crf-PLE excitation power normalized peak intensity for the three populations as in (e), with the dashed black line denoting y = x.