Dielectric Fano Nanoantennas for Enabling Sub-Nanosecond Lifetimes in NV-based Single Photon Emitters

doi:10.21203/rs.3.rs-4723409/v1

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Dielectric Fano Nanoantennas for Enabling Sub-Nanosecond Lifetimes in NV-based Single Photon Emitters

https://doi.org/10.21203/rs.3.rs-4723409/v1

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Solid-state quantum emitters are essential sources of single photons, and enhancing their emission rates is of paramount importance for applications in quantum communications, computing and metrology. One approach is to couple quantum emitters with resonant photonic nanostructures, where the emission rate is enhanced due to the Purcell effect. Dielectric nanoantennas are promising as they provide strong emission enhancement compared to plasmonic ones, which suffer from high Ohmic loss. Here,we designed and fabricated a dielectric Fano resonator based on a pair of silicon (Si) ellipses and a disk, which supports the mode hybridization between quasi-bound-states-in-the-continuum (quasi-BIC) and Mie resonance. We demonstrated the performance of the developed resonant system by interfacing it with single photon emitters (SPEs) based on nitrogen vacancy (NV) centers in nanodiamonds (NDs). We observed that the interfaced emitters have a Purcell enhancement factor of ~10, with sub-ns emission lifetime and a polarization contrast of 9. Our results indicate a promising method for developing efficient and compact single-photon sources for integrated quantum photonics applications.

Physical sciences/Optics and photonics/Optical physics/Quantum optics

Physical sciences/Optics and photonics/Optical physics/Nanophotonics and plasmonics

Dielectric metasurfaces

Fano resonance

Single photon emitter

NV center

Purcell Enhancement

Bright single photon emitters (SPEs) are essential elements for quantum communications, quantum-enhanced metrology and quantum computing.^1–3 While many efforts are dedicated to the development of the bright SPEs based on new material systems, another approach relies upon improving emission properties of the existing ones by interfacing them with resonant photonic nanostructures and benefiting in enhanced brightness of emitters due to the Purcell effect.^{4, 5} Moreover, this approach provides additional control over the spatial and polarization degrees of freedom of the SPE emission. Many successful attempts have already been demonstrated with hyperbolic metamaterials and plasmonic nanoantennas, as well as dielectric thin film platforms (i.e., TiO₂, AlN, Si₃N₄).^6–13

Different platforms have their own pros and cons. Hyperbolic metamaterials benefit in broad range of supported wavelengths, and some remarkable results with photoluminescence enhancement and lifetime reduction have been demonstrated.^{14, 15} Nevertheless, their interfacing with SPEs is still very limited even with sophisticated fabrication process.^{15, 16} Plasmonic nanoantennas provide significant field enhancement with demonstrated record level lifetime reduction.^17–19 However, their high optical absorption brings a significant non-radiative contribution to the total decay rate. On the contrary, dielectric nanoantennas are free from such strong non-radiative contributions, while maintaining the advantage of tunability of resonant wavelength.^{8, 20, 21} Additionally, many prominent dielectric material platforms (Si, Si₃N₄) are CMOS-compatible, which is important for the potential large-scale fabrication.

In this work, we designed and fabricated an all-dielectric silicon metasurface that has a sharp Fano resonance in the visible range to achieve strong a Purcell enhancement factor. We tested the performance of the Fano nanoantennas with nanodiamonds (NDs) hosting negatively charged nitrogen vacancy (NV^-) centers, which are fluorescent atomic defects commonly used as SPEs due to their remarkable optical properties as well as the convenience and scalability of solid-state host system.^{13, 22, 23} They are stable under room temperature operation, facilitating the rapid characterization and therefore development of practical quantum communication systems.²⁴ However, they suffer from poor polarization selection, low brightness and long fluorescence lifetime,^{25, 26} which is typically around 10 to 30 ns.^{27, 28} Thus, its limited emission rate poses a challenge for their integration into high-speed quantum devices. Correspondingly, a significant improvement of their emission properties upon interfacing with our Fano metasurface would mark successful realization of our system as promising candidate for quantum photonics.

Our dielectric Fano resonance was realized by mode hybridization between a pair of Si ellipses supporting quasi-bound-states-in-the-continuum (quasiBIC) and a Si nanodisk, which supports Mie resonance.^29–31 Numerical simulations were performed to optimize the geometric parameters of the Fano nanoantenna to ensure a good spectral overlap between its resonance and the emission of NV^- centers. Afterwards, the NV^- centers were integrated on the metasurface and tested by measuring second-order autocorrelation function g⁽²⁾(0), to be quantum emitters (i.e., g⁽²⁾(0) < 1) and/or SPEs (i.e., g⁽²⁾(0) < 0.5). Their measured emission lifetimes were significantly reduced to 0.93 ns, which is one order of magnitude shorter as compared to the ones on flat substrate region. To the best of our knowledge, the achieved Purcell factor of ~ 10 is the one of the highest reported values so far for quantum emitters interfaced with all-dielectric metasurfaces.^{32, 33} Additionally, it was proved that our nanoantenna arrays enable the SPE with polarization control. We believe that our findings provide a significant step towards the practical implementation of bright single photon sources for integrated quantum technologies.

To achieve the bright and polarized quantum light sources with enhanced emission rates via the Purcell effect, we introduce a metasurface based on Si nanoantennas with Fano resonance, composed of a pair of ellipses and a disk in the middle, as shown in Fig. 1a. The Si ellipses have a length (l) of 176 nm, a width (w) of 64 nm, and is rotated 48° with respect to the x-axis, thus introducing asymmetry for achieving the quasi-BIC resonances.³⁴ The disk with diameter (d) of 120 nm is displaced 75 nm in the positive direction of the y-axis direction. The height (h) of the nanostructure was designed to be fixed at 240 nm, with a pitch size of 327 and 324 nm along x and y axis, respectively. Here, a dip-coating method was carried out to deposit the NDs onto the metasurface.

To elaborate the mechanism of the Fano resonance, the simulated reflectance spectrum under y-polarized incident light and the corresponding electric field intensity distributions were shown in Figs. 1b and 1c, respectively. The quality factor of resonance at 671 nm was evaluated to be ~ 200, while the measured reflectance spectrum is shown in the supplementary information (Fig. S1). The resonance can be further explained by the electric field intensity changes in Fig. 1c and magnetic field intensity distribution (see SI, Fig. S2). At the dip of the reflectance spectra (indicated by the star symbol in Fig. 1b), the strongest electric field intensity occurs at the nanogaps between disk and two ellipses, also called hotspot, where an electric intensity enhancement factor (|E|²/|E₀|²) of 230 is obtained. When an in-plane electric dipole (oriented as indicated by the black arrow in the inset of Fig. 1d) is placed in the nanogap, the sharp resonance results in a high simulated Purcell factor of up to 23 (Fig. 1d). The position of ND with NV⁻ center emitter is confirmed by SEM image shown in Fig. 1e, where a single ND with a diameter of 35 nm is clearly visible at the nanogap.

Figure 1f presents the benchmarking summary of our NV⁻ SPEs integrated with dielectric nanoantenna being compared with respect to previous experimental works in terms of lifetime and Purcell factor.^{6, 27, 35–38} To the best of our knowledge, our work outperforms over the other dielectric nanoantenna enabled NV center-based SPEs in terms of emission lifetime reduction, highlighting the significance of achieving high Purcell factor when using the Fano resonance.

Figure 2 presents the basic principle of mode hybridization for the designed dielectric Fano nanoantenna. Here, we consider the dielectric material to be lossless Si with a refractive index of 3.74, thereby eliminating the influence of dispersion and Ohmic loss. As shown in Fig. 2a, both the disk and ellipse pair exhibit transverse magnetic modes (i.e., H_z is negligible). The disk supports a non-radiative electric dipole oriented along z-axis at the wavelength of 561 nm, denoted as \(\:\left|{\varvec{p}}_{\varvec{z}}⟩\right.\), generating an in-plane magnetic loop with the magnetic field H circulating in the xy-plane (Fig. 2b). The ellipses pair with a radiative quasi-BIC mode induces two in-plane magnetic dipoles \(\:\left|{\varvec{m}}_{\parallel\:}⟩\right.\) at the wavelength of 660 nm (Fig. 2c). The x-components of two magnetic dipoles \(\:\left|{\varvec{m}}_{\parallel\:}⟩\right.\) are aligned in the same direction, thereby reinforcing each other along the x-axis; meanwhile, the ycomponents of magnetic dipoles are oriented in opposite directions, thus cancelling each other out. In other words, this quasi-BIC mode can be readily excited when the incident optical field is y-polarized with a dominating magnetic field being x-polarized.

When integrating an ellipse pair and a disk in a single unit cell, two hybrid modes are generated at 534 and 671 nm, respectively, due to the coupling between \(\:\left|{\varvec{p}}_{\varvec{z}}⟩\right.\) and \(\:\left|{\varvec{m}}_{\parallel\:}⟩\right.\). To be more precise, the upper hybridized mode (\(\:\left|{\varvec{m}}_{\parallel\:},-{\varvec{p}}_{\varvec{z}}⟩\right.\)) arises from the coupling between \(\:\left|{\varvec{m}}_{\parallel\:}⟩\right.\) along + x axis and \(\:\left|{\varvec{p}}_{\varvec{z}}⟩\right.\), where its corresponding electric and magnetic field distributions are shown in Fig. S3. On the other hand, the lower one (\(\:\left|{\varvec{m}}_{\parallel\:},{\varvec{p}}_{\varvec{z}}⟩\right.\)) is due to the interaction of \(\:\left|{\varvec{m}}_{\parallel\:}⟩\right.\) and \(\:-\left|{\varvec{p}}_{\varvec{z}}⟩\right.\) (see Fig. 2d). Consequently, a narrow dip emerges in the reflection spectrum, as shown in Fig. 1b, where this mode is able to achieve a strongly enhanced optical field at the nanogap region between disk and ellipse, especially at the plane of z = 25 nm above substrate for strong Purcell enhancement (see the electric and magnetic field distributions at Fig. S4). Moreover, we have also investigated the dependence of this hybridized mode on the nanogap size, which is a key parameter to engineer the ultimate field enhancement factor and Purcell effect (see Fig. S5). In addition, the resonances depend on the disk diameters (see Fig. S6), and we chose the design where the resonance matches well with the NV spectrum (a measured PL spectrum is shown in Fig. S7)

Figure 3a presents the home-built confocal microscope setup, which was able to measure the lifetime and secondorder correlation function, g⁽²⁾(τ), for the characterization of SPEs. The excitation was performed by a 515-nm laser, which is capable to operate either in continuous wave (CW) or pulsed modes (110 ps). A photoluminescence (PL) intensity map was first measured to determine the emitter locations on the metasurface (see Fig. S8 for details). To verify the emission of single photons, we performed the g⁽²⁾(τ) measurement for a representative single NV⁻ center coupled to Fano resonance using a Hanbury-Brown and Twiss (HBT) system. The collected photon was directed to a fiber-based beam splitter and avalanche photodiodes (APDs) via single mode fiber. The correlation function shown in Fig. 3b exhibits a distinctive dip at τ = 0 with g⁽²⁾ (0) = 0.24, proving the antibunching behaviour of the emitted single photons.

Figure 3c depicts a comparison of the lifetime between the SPEs on Si metasurface and on flat substrate region. Notably, the emission lifetime of SPE on metasurface is significantly reduced to 0.93 ns (blue curve); in comparison, the emitter at the flat substrate region has a lifetime of 9.56 ns, revealing a Purcell factor of ~ 10. The significant reduction of lifetime is a direct consequence of the higher densityof-opticalstates in the nanogap between disks and the ellipses, which leads to enhanced radiative emission (Purcell effect). This experimental result verifies the simulation investigation (Fig. 1d) on the peak Purcell factor. The difference in simulated and observed Purcell enhancement is explained by the fact that emission linewidth of NV⁻ centers is larger rather than width of the resonance, which makes enhancement less efficient and thus reduces the effective Purcell factor.⁴⁰ Similar decay dynamics were observed from other 5 coupled and 5 uncoupled single photon and quantum emitters, and their extracted lifetime are summarized in Fig. 3d and detailed in Table S1. These results confirm that the metasurface with Fano resonance could reduce the lifetime of the NV⁻ center emitter effectively. Additionally, we measured the emission rate I as a function of the pump power shown in Fig. 3e. The data fits well to a saturation behaviour given by \(\:I\left(P\right)={I}_{sat}\times\:P/(P+{P}_{sat})\),⁴¹ where P is the pump power, \(\:{I}_{sat}\) and \(\:{P}_{sat}\) represent fitting parameters that denote the saturation intensity and saturation power, respectively. From the measured pump dependence, we found that the enhancement of the emission rate constituted 7.5 times in the linear regime. The measured emission rate enhancement agrees well with the lifetime reduction, proving the absence of Ohmic dissipation loss in dielectric nanostructures.

Next, we explored the polarization properties of single photon emission. We simulated the Purcell factor under various dipole excitations (Fig. 4a). It is observed that positioning a dipole at a 45-degree angle results in a Purcell factor as high as 23, indicating significant radiation enhancement. In contrast, setting the dipole at a 135-degree angle leads to a Purcell factor of only 0.95, demonstrating radiation suppression. We thus obtain a simulated degree of polarization (DOP) of 0.92. To verify the emission polarization experimentally, an analyser composed of a half-wave plate followed by a linear polarizer was put before collection single mode fiber and then sent to spectrometer. The collected photons exhibit the largest contrast with a ratio of 9 at the wavelength of 680 nm, which matches well with the simulation result (Fig. 4b). These observations clearly demonstrate strongly polarized single photon emission.

In this paper, we have successfully designed a Fano dielectric nanoantenna to enhance the spontaneous emission rate of quantum emitters. We demonstrate the functionality of our platform by integrating it with NV^- center in NDs and achieving an experimental Purcell enhancement factor of ~ 10 fold, confirmed by measurements of lifetime reduction and emission rate enhancement. Furthermore, the polarization contrast of SPEs induced by metasurface was demonstrated to be 9, providing a linearly polarized SPE. We believe that our work will contribute to the development of more efficient and scalable quantum light sources for quantum computation and communication systems.

Sample Fabrication. The process began by thinning the Si layer thickness on commercially purchased silicon-on-sapphire (SOS, Silicon Valley Microelectronics, Inc.) wafers from 300 to 240 nm, using chlorine (Cl₂)-based inductively-coupled-plasma reactive-ion etching (ICP RIE, Oxford Instruments Plasmalab System 100). Next, 6% HSQ was spin coated on the SOS sample at a speed of 5000 rpm for 60 s to form a layer of 70 nm thickness. After that, an array of ellipses with disks nanopatterns were fabricated on the SOS substrate using electron beam lithography (EBL), where the size of the patterning area was 50 × 50 µm². In the EBL process, an acceleration voltage of 100 keV and a beam current of 500 pA, with an exposure dosage of ~ 25 mC/cm² was used. The Si metasurface was then completed by etching down to sapphire substrate.

Nitrogen-vacancy (NV ^- ) centers in Nanodiamonds (NDs) and Sample Dip-coating. The NDs with a diameter of 40 nm (Adamas Nanotechnologies) were suspended in isopropanol with a concentration of 0.1 Millimoles/L. Before the deposition process, we carried out a surface treatment process via O₂ plasma using RIE (Oxford Plasmalab 80) with a pressure of 10 mTorr, a power of 50 watts and an O₂ flow rate of 50 sccm for 2 minutes. Subsequently, the sample was dip-coated inside the ND suspension at a rate of 0.1 mm/min within a nitrogen-filled glove box at room temperature.⁴²

Numerical Simulations. The reflectance spectra were obtained using Lumerical 3D finite difference time-domain (3D-FDTD) software. The elliptical nanostructures with disk were positioned in a unit cell measuring 327 nm × 324 nm × 1500 nm, with a 2.5 nm × 2.5 nm × 2.5 nm mesh surrounding them. This unit cell featured a perfectly matched layer (PML) along the z direction and periodic boundary conditions along the x and y directions. The reflectance spectrum was recorded under normal incidence conditions using a monitor placed above a plane wave source. The incident light wave was polarized along either the x- or y-axis. The refractive index (n) and extinction coefficient (k) values for crystalline Si were obtained from ellipsometer measurements³¹. The Purcell factor was calculated using the software's built-in method, based on the ratio of dipole emission power to total emitted power. The domain was constrained by PML boundary conditions. A point dipole source was positioned within a 13 × 13 array of nanostructures, specifically at the location of the highest field enhancement in the center nanoellipse. The emission center was set at 680 nm with a 100 nm span, and the simulation results of overall Purcell factor were averaged from orthogonal dipole orientations along the x-, y-, and z-axes.

The electric and magnetic field distributions in Fig. 2 were obtained with finite-element method in Electromagnetic Waves Frequency Domain module of COMSOL Multiphysics. All modal analysis were investigated using eigenfrequency solver. In all cases, periodic boundaries were applied to x and y axis, while scattering boundaries are applied on both + z and -z boundaries. A Tetrahedral mesh with local refinement around fine structures was employed. The refractive index of sapphire was set as 1.76. The structural parameters were set based on the SEM of as-fabricated nanostructures. Due to some dimensional tolerance in SEM measurements (about ± 5 nm), the parameters were adjusted within a reasonable range according to the comparison between simulated and measured spectra.

Lifetime and g ⁽²⁾ (τ) Measurement. The measurements were performed with a home-built confocal microscope setup, where the 515 nm pump laser (Omicron) was scanned by steering mirror (Newport) and projected to the sample by 4f lens system and 100x microscope objective (Olympus, NA = 0.9). The pump laser can operate in either continuous-wave (CW) or pulsed modes.

For lifetime measurements, the pump laser was operated in pulsed mode (110 ps pulse duration, 2 MHz repetition rate). The emitted photons were spectrally filtered (Semrock 680/42 filter), collected into a single-mode fiber, and detected by a single-photon avalanche diode (SPAD) (Excilatas). The correlations between the emission detected by SPAD and the laser pulses were measured using a time-to-digital converter (QuTools quTau), with a resolution of 81 ps. The fluorescence decay curve was fitted to a single exponential model to extract the lifetime.

For g⁽²⁾(τ) measurements, the pump laser was operated in the CW mode. The emission was selected by Semrock filter 675/150 and split between two SPADs by the fiber beamsplitter (Thorlabs) in a Hanbury-Brown and Twiss (HBT) configuration. The same time-to-digital converter (QuTools quTau) recorded photon arrival time differences to calculate g⁽²⁾(τ), with g⁽²⁾(0) < 0.5, indicating single-photon emission. The spectrometer measurements were performed by sending the collected emission into the spectrometer a spectrometer (Princeton Instruments, IsoPlane160, 0.13 nm max resolution). Calibration was performed using known standards, and error analysis accounted for uncertainty sources such as photon counting statistics and detector noise.

Acknowledgements

This work is supported by the funding support of Agency for Science, Technology and Research (A*STAR) with the Project No. C230917005. In addition, Z.D. also would like to acknowledge the funding support from A*STAR under its Career Development Award grant (Project No. C210112019), MTC IRG (Project No. M21K2c0116 and M22K2c0088), the Quantum Engineering Programme 2.0 (Award No. NRF2021-QEP2-03-P09), and National Research Foundation via Grant No. NRF-CRP30-2023-0003.

Author contributions

S.A., Z.D., C.-W.Q., D.K. and V.L. conceived the concept, designed the experiments. S.A. did the electron beam lithography, developed the fabrication processes, and performed the simulations and optical reflectance measurements. D.K. measured the lifetimes and second-order correlation function of the emitters. W.S. performed the simulation analysis. Z.M. prepared the ND suspension and optimized the dip coating process to deposit the NDs. A.B.C. helped with the SEM image and interpretation. Y.L. provided support on the mechanism analysis. J.W., D.Z. and W.G. participated in discussions and provided suggestions to improve the work. Z.D., C.-W.Q. and V.L. supervised the project. All authors analyzed the data, read and corrected the manuscript before the submission.

Data availability

All data in the paper and the supplementary materials are available.

Competing interests

The authors declare no competing interests.

Supplementary information The online version contains supplementary material available on the website.

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