Emission dynamics of optically driven aluminum nitride quantum emitters

Open Access

Emission dynamics of optically driven aluminum nitride quantum emitters

Yanzhao Guo, John P. Hadden, Rachel N. Clark, Samuel G. Bishop, and Anthony J. Bennett

Phys. Rev. B 110, 014109 – Published 22 July 2024

Abstract

Aluminum nitride is a technologically important wide band-gap semiconductor which has been shown to host bright quantum emitters. We use photon emission correlation spectroscopy (PECS), time-resolved photoluminescence (TRPL), and state-population dynamic simulations to probe the dynamics of emission under continuous wave (CW) and pulsed optical excitation. We infer that there are at least four dark shelving states, which govern the TRPL, bunching, and saturation of the optical transition. We study in detail the emission dynamics of two quantum emitters (QEs) with differing power-dependent shelving processes, hypothesized to result from charge ionization and recombination. These results demonstrate that photon bunching caused by shelving the system in a dark state inherently limits the saturation rate of the photon source. In emitters where increasing optical power deshelves the dark states, we observe an increased photon emission intensity.

Received 9 October 2023
Revised 26 April 2024
Accepted 28 June 2024

DOI:https://doi.org/10.1103/PhysRevB.110.014109

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Physics Subject Headings (PhySH)

Color centers Point defects Quantum communication Quantum information processing

Wide band gap systems

Fluorescence Photoluminescence Photon counting Time-resolved photoluminescence

Condensed Matter, Materials & Applied PhysicsQuantum Information, Science & Technology

Authors & Affiliations

Yanzhao Guo , John P. Hadden , Rachel N. Clark , Samuel G. Bishop , and Anthony J. Bennett ^*

Translational Research Hub, Cardiff University, Maindy Road, Cardiff, CF24 4HQ, United Kingdom and School of Engineering, Cardiff University, Queen's Buildings, The Parade, Cardiff, CF24 3AA, United Kingdom

^*Contact author: BennettA19@cardiff.ac.uk

Article Text

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Issue

Vol. 110, Iss. 1 — 1 July 2024

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Images

Figure 1
Characterization of two quantum emitters in AlN at room temperature: QE A (first row) and QE B (second row). (a) and (e) show the spectra between 532 and $650 n m$ . (b) and (f) are the photon emission correlation histograms, normalized, without background correction (black points), and fit using an empirical model discussed in the text (red line). Error bars represent Poissonian uncertainties based on the photon counts in each bin. (c) and (g) are the CW-PL saturation behaviors (black points) as a function of laser power, fit using Eq. (1). (d) and (h) show the excited-state lifetime measurement, fit with a single exponential (red line).
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Figure 2
Photon emission correlation spectroscopy (PECS). Black lines in (a) and (b) are the PECS of QE A and QE B, fit using empirical equation (2) for $N$ = 2, 3, 4, and 5. (c) and (d) are the corresponding residuals from the fits to QE A and QE B, respectively. The raw data between 22– $35 n s$ is masked to hide reflections from the APDs' backflash.
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Figure 3
Double pulse laser excitation. (a) and (b) are the TRPL of QE A and QE B under double pulse laser excitation. The inset in (a) is the train of the laser pulses. (c) and (d) represent the PL revival behavior under the second pulse excitation in (a) and (b) fitted by single exponential and double exponential equations.
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Figure 4
Power-dependent PECS from (a) QE A and (b) QE B. Each autocorrelation is fitted with Eq. (2) and $N = 5$ . (c) and (d) are amplitudes $C_{i}$ and rates $r_{i}$ arising from fitting Eq. (2) for QE A and QE B, respectively.
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Figure 5
Power-dependent TRPL with square excitation pulses. (a) QE A, (b) QE B, with insert showing the pulse sequence. (c) and (d) are the normalized PL saturation behaviours of the steady states. (e) and (f) are the TRPL decay rates observed in (a) and (b).
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Figure 6
State population dynamics simulation. (a) PECS and (b) TRPL simulation results for shelving model I and model II with transition rates from Table 1. The inset in (a) is the proposed three-energy level shelving models I and II which include radiative emission (red arrow), optically pumped transitions (green arrows), and nonradiative transitions with a fixed spontaneous decay rate (dotted grey arrows). (c)–(e) are the best-fit parameters $r_{1}$ , $C_{2}$ , and $r_{2}$ determined by fitting simulated $g^{(2)} (τ$ ) data using Eq. (2) with $N = 2$ . (f) is the steady-state PL saturation behavior fitted by Eq. (1). The results are plotted as a function of $k_{12} / k_{21}$ , where $k_{21} =$ $200 M Hz$ is a fixed parameter as the spontaneous emission decay rate.
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