Abstract

Single-photon emitters (SPEs) in two-dimensional materials are promising candidates for the future generation of quantum photonic technologies. In this work, we experimentally determine the quantum efficiency (QE) of SPEs in few-layer hexagonal boron nitride (h-BN). We employ a metal hemisphere that is attached to the tip of an atomic force microscope to directly measure the lifetime variation of the SPEs as the tip approaches the h-BN. This technique enables nondestructive, yet direct and absolute measurement of the QE of SPEs. We find that the emitters exhibit very high QEs approaching (87±7)% at wavelengths of 580nm, which is among the highest QEs recorded for a solid-state SPE.

© 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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    [Crossref]

2019 (6)

B. Urbaszek and A. Srivastava, “Materials in flatland twist and shine,” Nature 567, 39–40 (2019).
[Crossref]

M. Toth and I. Aharonovich, “Single photon sources in atomically thin materials,” Annu. Rev. Phys. Chem. 70, 123–142 (2019).
[Crossref]

D. Wigger, R. Schmidt, O. Del Pozo-Zamudio, J. A. Preuß, P. Tonndorf, R. Schneider, P. Steeger, J. Kern, Y. Khodaei, J. Sperling, S. M. de Vasconcellos, R. Bratschitsch, and T. Kuhn, “Phonon-assisted emission and absorption of individual color centers in hexagonal boron nitride,” 2D Mater. 6, 035006 (2019).
[Crossref]

M. A. Feldman, A. Puretzky, L. Lindsay, E. Tucker, D. P. Briggs, P. G. Evans, R. F. Haglund, and B. J. Lawrie, “Phonon-induced multicolor correlations in hBN single-photon emitters,” Phys. Rev. B 99, 020101 (2019).
[Crossref]

N. Mendelson, Z.-Q. Xu, T. T. Tran, M. Kianinia, J. Scott, C. Bradac, I. Aharonovich, and M. Toth, “Engineering and tuning of quantum emitters in few-layer hexagonal boron nitride,” ACS Nano 13, 3132–3140 (2019).
[Crossref]

J. Comtet, E. Glushkov, V. Navikas, J. Feng, V. Babenko, S. Hofmann, K. Watanabe, T. Taniguchi, and A. Radenovic, “Wide-field spectral super-resolution mapping of optically active defects in hexagonal boron nitride,” Nano Lett. 19, 2516–2523 (2019).
[Crossref]

2018 (8)

H. N. My Duong, M. A. P. Nguyen, M. Kianinia, T. Ohshima, H. Abe, K. Watanabe, T. Taniguchi, J. H. Edgar, I. Aharonovich, and M. Toth, “Effects of high-energy electron irradiation on quantum emitters in hexagonal boron nitride,” ACS Appl. Mater. Interfaces 10, 24886–24891 (2018).
[Crossref]

T. Vogl, G. Campbell, B. C. Buchler, Y. Lu, and P. K. Lam, “Fabrication and deterministic transfer of high-quality quantum emitters in hexagonal boron nitride,” ACS Photon. 5, 2305–2312 (2018).
[Crossref]

Z.-Q. Xu, C. Elbadawi, T. T. Tran, M. Kianinia, X. Li, D. Liu, T. B. Hoffman, M. Nguyen, S. Kim, J. H. Edgar, X. Wu, L. Song, S. Ali, M. Ford, M. Toth, and I. Aharonovich, “Single photon emission from plasma treated 2D hexagonal boron nitride,” Nanoscale 10, 7957–7965 (2018).
[Crossref]

A. W. Schell, M. Svedendahl, and R. Quidant, “Quantum emitters in hexagonal boron nitride have spectrally tunable quantum efficiency,” Adv. Mater. 30, 1704237 (2018).
[Crossref]

M. Nguyen, S. Kim, T. T. Tran, Z.-Q. Xu, M. Kianinia, M. Toth, and I. Aharonovich, “Nanoassembly of quantum emitters in hexagonal boron nitride and gold nanospheres,” Nanoscale 10, 2267–2274 (2018).
[Crossref]

N. V. Proscia, Z. Shotan, H. Jayakumar, P. Reddy, C. Cohen, M. Dollar, A. Alkauskas, M. Doherty, C. A. Meriles, and V. M. Menon, “Near-deterministic activation of room-temperature quantum emitters in hexagonal boron nitride,” Optica 5, 1128–1134 (2018).
[Crossref]

S. Kim, J. E. Fröch, J. Christian, M. Straw, J. Bishop, D. Totonjian, K. Watanabe, T. Taniguchi, M. Toth, and I. Aharonovich, “Photonic crystal cavities from hexagonal boron nitride,” Nat. Commun. 9, 2623 (2018).
[Crossref]

B. van Dam, C. I. Osorio, M. A. Hink, R. Muller, A. F. Koenderink, and K. Dohnalova, “High internal emission efficiency of silicon nanoparticles emitting in the visible range,” ACS Photon. 5, 2129–2136 (2018).
[Crossref]

2017 (7)

X.-L. Chu, S. Götzinger, and V. Sandoghdar, “A single molecule as a high-fidelity photon gun for producing intensity-squeezed light,” Nat. Photonics 11, 58–62 (2017).
[Crossref]

G. Grosso, H. Moon, B. Lienhard, S. Ali, D. K. Efetov, M. M. Furchi, P. Jarillo-Herrero, M. J. Ford, I. Aharonovich, and D. Englund, “Tunable and high-purity room temperature single-photon emission from atomic defects in hexagonal boron nitride,” Nat. Commun. 8, 705 (2017).
[Crossref]

S. A. Tawfik, S. Ali, M. Fronzi, M. Kianinia, T. T. Tran, C. Stampfl, I. Aharonovich, M. Toth, and M. J. Ford, “First-principles investigation of quantum emission from hBN defects,” Nanoscale 9, 13575–13582 (2017).
[Crossref]

N. R. Jungwirth and G. D. Fuchs, “Optical absorption and emission mechanisms of single defects in hexagonal boron nitride,” Phys. Rev. Lett. 119, 057401 (2017).
[Crossref]

B. Sontheimer, M. Braun, N. Nikolay, N. Sadzak, I. Aharonovich, and O. Benson, “Photodynamics of quantum emitters in hexagonal boron nitride revealed by low-temperature spectroscopy,” Phys. Rev. B 96, 121202 (2017).
[Crossref]

W.-H. Lin, V. W. Brar, D. Jariwala, M. C. Sherrott, W.-S. Tseng, C.-I. Wu, N.-C. Yeh, and H. A. Atwater, “Atomic-scale structural and chemical characterization of hexagonal boron nitride layers synthesized at the wafer-scale with monolayer thickness control,” Chem. Mater. 29, 4700–4707 (2017).
[Crossref]

M. Kianinia, B. Regan, S. A. Tawfik, T. T. Tran, M. J. Ford, I. Aharonovich, and M. Toth, “Robust solid-state quantum system operating at 800  K,” ACS Photon. 4, 768–773 (2017).
[Crossref]

2016 (4)

N. R. Jungwirth, B. Calderon, Y. Ji, M. G. Spencer, M. E. Flatté, and G. D. Fuchs, “Temperature dependence of wavelength selectable zero-phonon emission from single defects in hexagonal boron nitride,” Nano Lett. 16, 6052–6057 (2016).
[Crossref]

T. T. Tran, K. Bray, M. J. Ford, M. Toth, and I. Aharonovich, “Quantum emission from hexagonal boron nitride monolayers,” Nat. Nanotechnol. 11, 37–41 (2016).
[Crossref]

K. S. Novoselov, A. Mishchenko, A. Carvalho, and A. H. C. Neto, “2D materials and van der Waals heterostructures,” Science 353, aac9439 (2016).
[Crossref]

K. F. Mak and J. Shan, “Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides,” Nat. Photonics 10, 216–226 (2016).
[Crossref]

2015 (2)

Q. Li, H. Wei, and H. Xu, “Quantum yield of single surface plasmons generated by a quantum dot coupled with a silver nanowire,” Nano Lett. 15, 8181–8187 (2015).
[Crossref]

P. Rivera, J. R. Schaibley, A. M. Jones, J. S. Ross, S. Wu, G. Aivazian, P. Klement, K. Seyler, G. Clark, N. J. Ghimire, J. Yan, D. G. Mandrus, W. Yao, and X. Xu, “Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures,” Nat. Commun. 6, 6242 (2015).
[Crossref]

2014 (2)

C. Lethiec, J. Laverdant, H. Vallon, C. Javaux, B. Dubertret, J.-M. Frigerio, C. Schwob, L. Coolen, and A. Maître, “Measurement of three-dimensional dipole orientation of a single fluorescent nanoemitter by emission polarization analysis,” Phys. Rev. X 4, 021037 (2014).
[Crossref]

A. W. Schell, P. Engel, J. F. M. Werra, C. Wolff, K. Busch, and O. Benson, “Scanning single quantum emitter fluorescence lifetime imaging: quantitative analysis of the local density of photonic states,” Nano Lett. 14, 2623–2627 (2014).
[Crossref]

2013 (3)

R. Beams, D. Smith, T. W. Johnson, S.-H. Oh, L. Novotny, and A. N. Vamivakas, “Nanoscale fluorescence lifetime imaging of an optical antenna with a single diamond NV center,” Nano Lett. 13, 3807–3811 (2013).
[Crossref]

P. Lunnemann, F. T. Rabouw, R. J. A. Van Dijk-Moes, F. Pietra, D. Vanmaekelbergh, and A. F. Koenderink, “Calibrating and controlling the quantum efficiency distribution of inhomogeneously broadened quantum rods by using a mirror ball,” ACS Nano 7, 5984–5992 (2013).
[Crossref]

S. Karaveli, A. J. Weinstein, and R. Zia, “Direct modulation of lanthanide emission at sub-lifetime scales,” Nano Lett. 13, 2264–2269 (2013).
[Crossref]

2012 (1)

A. Kwadrin and A. F. Koenderink, “Gray-tone lithography implementation of Drexhage’s method for calibrating radiative and nonradiative decay constants of fluorophores,” J. Phys. Chem. C 116, 16666–16673 (2012).
[Crossref]

2010 (1)

S. Castelletto, I. Aharonovich, B. C. Gibson, B. C. Johnson, and S. Prawer, “Imaging and quantum-efficiency measurement of chromium emitters in diamond,” Phys. Rev. Lett. 105, 217403 (2010).
[Crossref]

2006 (1)

P. Anger, P. Bharadwaj, and L. Novotny, “Enhancement and quenching of single-molecule fluorescence,” Phys. Rev. Lett. 96, 113002 (2006).
[Crossref]

2005 (1)

B. C. Buchler, T. Kalkbrenner, C. Hettich, and V. Sandoghdar, “Measuring the quantum efficiency of the optical emission of single radiating dipoles using a scanning mirror,” Phys. Rev. Lett. 95, 63003 (2005).
[Crossref]

2004 (1)

X. Brokmann, L. Coolen, M. Dahan, and J. P. Hermier, “Measurement of the radiative and nonradiative decay rates of single CdSe nanocrystals through a controlled modification of their spontaneous emission,” Phys. Rev. Lett. 93, 107403 (2004).
[Crossref]

1998 (1)

W. L. Barnes, “Fluorescence near interfaces: the role of photonic mode density,” J. Mod. Opt. 45, 661–699 (1998).
[Crossref]

1997 (1)

R. M. Amos and W. L. Barnes, “Modification of the spontaneous emission rate of Eu3+ ions close to a thin metal mirror,” Phys. Rev. B 55, 7249–7254 (1997).
[Crossref]

1970 (1)

K. H. Drexhage, “Influence of a dielectric interface on fluorescence decay time,” J. Lumin. 1-2, 693–701 (1970).
[Crossref]

Abe, H.

H. N. My Duong, M. A. P. Nguyen, M. Kianinia, T. Ohshima, H. Abe, K. Watanabe, T. Taniguchi, J. H. Edgar, I. Aharonovich, and M. Toth, “Effects of high-energy electron irradiation on quantum emitters in hexagonal boron nitride,” ACS Appl. Mater. Interfaces 10, 24886–24891 (2018).
[Crossref]

Aharonovich, I.

N. Mendelson, Z.-Q. Xu, T. T. Tran, M. Kianinia, J. Scott, C. Bradac, I. Aharonovich, and M. Toth, “Engineering and tuning of quantum emitters in few-layer hexagonal boron nitride,” ACS Nano 13, 3132–3140 (2019).
[Crossref]

M. Toth and I. Aharonovich, “Single photon sources in atomically thin materials,” Annu. Rev. Phys. Chem. 70, 123–142 (2019).
[Crossref]

Z.-Q. Xu, C. Elbadawi, T. T. Tran, M. Kianinia, X. Li, D. Liu, T. B. Hoffman, M. Nguyen, S. Kim, J. H. Edgar, X. Wu, L. Song, S. Ali, M. Ford, M. Toth, and I. Aharonovich, “Single photon emission from plasma treated 2D hexagonal boron nitride,” Nanoscale 10, 7957–7965 (2018).
[Crossref]

M. Nguyen, S. Kim, T. T. Tran, Z.-Q. Xu, M. Kianinia, M. Toth, and I. Aharonovich, “Nanoassembly of quantum emitters in hexagonal boron nitride and gold nanospheres,” Nanoscale 10, 2267–2274 (2018).
[Crossref]

H. N. My Duong, M. A. P. Nguyen, M. Kianinia, T. Ohshima, H. Abe, K. Watanabe, T. Taniguchi, J. H. Edgar, I. Aharonovich, and M. Toth, “Effects of high-energy electron irradiation on quantum emitters in hexagonal boron nitride,” ACS Appl. Mater. Interfaces 10, 24886–24891 (2018).
[Crossref]

S. Kim, J. E. Fröch, J. Christian, M. Straw, J. Bishop, D. Totonjian, K. Watanabe, T. Taniguchi, M. Toth, and I. Aharonovich, “Photonic crystal cavities from hexagonal boron nitride,” Nat. Commun. 9, 2623 (2018).
[Crossref]

G. Grosso, H. Moon, B. Lienhard, S. Ali, D. K. Efetov, M. M. Furchi, P. Jarillo-Herrero, M. J. Ford, I. Aharonovich, and D. Englund, “Tunable and high-purity room temperature single-photon emission from atomic defects in hexagonal boron nitride,” Nat. Commun. 8, 705 (2017).
[Crossref]

S. A. Tawfik, S. Ali, M. Fronzi, M. Kianinia, T. T. Tran, C. Stampfl, I. Aharonovich, M. Toth, and M. J. Ford, “First-principles investigation of quantum emission from hBN defects,” Nanoscale 9, 13575–13582 (2017).
[Crossref]

B. Sontheimer, M. Braun, N. Nikolay, N. Sadzak, I. Aharonovich, and O. Benson, “Photodynamics of quantum emitters in hexagonal boron nitride revealed by low-temperature spectroscopy,” Phys. Rev. B 96, 121202 (2017).
[Crossref]

M. Kianinia, B. Regan, S. A. Tawfik, T. T. Tran, M. J. Ford, I. Aharonovich, and M. Toth, “Robust solid-state quantum system operating at 800  K,” ACS Photon. 4, 768–773 (2017).
[Crossref]

T. T. Tran, K. Bray, M. J. Ford, M. Toth, and I. Aharonovich, “Quantum emission from hexagonal boron nitride monolayers,” Nat. Nanotechnol. 11, 37–41 (2016).
[Crossref]

S. Castelletto, I. Aharonovich, B. C. Gibson, B. C. Johnson, and S. Prawer, “Imaging and quantum-efficiency measurement of chromium emitters in diamond,” Phys. Rev. Lett. 105, 217403 (2010).
[Crossref]

Aivazian, G.

P. Rivera, J. R. Schaibley, A. M. Jones, J. S. Ross, S. Wu, G. Aivazian, P. Klement, K. Seyler, G. Clark, N. J. Ghimire, J. Yan, D. G. Mandrus, W. Yao, and X. Xu, “Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures,” Nat. Commun. 6, 6242 (2015).
[Crossref]

Ali, S.

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Supplementary Material (1)

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Figures (4)

Fig. 1.
Fig. 1. Schematic representation of the experiment and two representative spectra of both investigated emitter families. (a) An AFM equipped with a gold-coated hemispherical tip with a diameter of 5.5 μm is aligned with an SPE in h-BN and held at a distance d. An oil-immersion objective lens excites the SPE and collects its emission from below the glass substrate. (b) Representative spectra of a typical SPE from each emitter family showing a pronounced ZPL at 595nm and 660 nm and a phonon sideband, respectively.
Fig. 2.
Fig. 2. Simulated fluorescence intensity, simulated wavelength, and distance-dependent lifetimes together with measured quantum efficiency data. (a) A simulation of the experimental scenario showing the intensity distribution of a horizontally polarized dipole (mimicking the h-BN emitter), emitting at 600 nm placed in the center of a 10-nm-thick h-BN layer, on top of a glass substrate at a distance of 1240 nm from the gold hemisphere. (b) Changes of the lifetime as a function of the distance between the AFM tip and an SPE simulated for a range of ZPL positions. The values were extracted from simulations similar to (a). This map is used to fit the experimental data. c) A typical distance-dependent lifetime measurement (dots) fitted by Eq. (1) (blue solid line) determines the QE. A function with a QE of 1.0 is shown for reference by the green solid line. d) A repeated measurement of the QE (dots) is shown, together with the average (solid line) and the standard deviation (shaded area) of these measurements. Another consecutive measurement is shown in Fig. S3 of Supplement 1.
Fig. 3.
Fig. 3. Excitation wavelength and power dependence. (a) The QE relative to the excitation wavelength shows an insignificant modulation. (b) QE relative to the excitation power. Error bars are given by the statistical error shown in Fig. 2(d).
Fig. 4.
Fig. 4. QE dependence on ZPL width and central wavelength. (a) QE of 17 emitters plotted against their central ZPL position. (b) The same 17 emitters plotted against their respective ZPL linewidth. In both plots, green marks the 12 emitters with central wavelengths below 640 nm and blue above 640 nm. The two circles in (a) are placed at the averaged position of each family, and the width and height represent the respective standard deviation, given by λ580=(597±11)nm and λ660=(661±4)nm. Error bars are given by the statistical error shown in Fig. 2(d).

Equations (2)

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τ(d)=τ()1+η(ρ(d)ρ()1),
ρ(d)/ρ()=P(d)/P(),

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