Letter pubs.acs.org/journal/apchd5
Nanofabrication of Plasmonic Circuits Containing Single Photon Sources Hamidreza Siampour,* Shailesh Kumar, and Sergey I. Bozhevolnyi* Centre for Nano Optics, University of Southern Denmark, Campusvej 55, DK-5230 Odense M, Denmark S Supporting Information *
ABSTRACT: Nanofabrication of photonic components based on dielectric loaded surface plasmon polariton waveguides (DLSPPWs) excited by single nitrogen vacancy (NV) centers in nanodiamonds is demonstrated. DLSPPW circuits are built around NV containing nanodiamonds, which are certified to be single-photon emitters, using electron-beam lithography of hydrogen silsesquioxane (HSQ) resist on silver-coated silicon substrates. A propagation length of 20 ± 5 μm for the NV single-photon emission is measured with DLSPPWs. A 5-fold enhancement in the total decay rate, and 58% coupling efficiency to the DLSPPW mode is achieved, indicating significant mode confinement. Finally, we demonstrate routing of single plasmons with DLSPPW-based directional couplers, revealing the potential of our approach for on-chip realization of quantum-optical networks. KEYWORDS: nanofabrication, dielectric-loaded surface plasmon polariton (DLSPP) waveguide, single-photon sources, nitrogen vacancy (NV) center, quantum-optical networks, quantum information technologies
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In this Letter, we propose and experimentally demonstrate a top-down fabrication technique for deterministic positioning of DLSPP waveguides to incorporate nanodiamonds that are precharacterized to contain a single nitrogen vacancy (NV) center, that is, to be a single photon source. NV centers are known to be stable and bright single-photon sources,26−29 that also have an optically accessible electron and nuclear spin that can be used as qubits.26 DLSPP waveguides are built with nanometer precision around precharacterized nanodiamonds, whose locations are related to specifically designed and fabricated coordinate markers, using electron-beam lithography of hydrogen silsesquioxane (HSQ) resist spin-coated on silvercoated silicon substrates (Figure 1).30 We have experimentally observed a decay rate enhancement by a factor of ∼5 on average for the NV centers in nanodiamonds coupled to DLSPP waveguides, when compared to the NV centers in nanodiamonds spin coated on a fused silica glass substrate. Also, β factor, defined as the fraction of total emission into the plasmonic mode, is estimated to be 0.58 ± 0.03. The propagation distance measured for the fabricated DLSPPWs is 20 ± 5 μm. Therefore, a figure of merit (FOM) defined as the product of the propagation length, total decay rate enhancement and β-factor, normalized by the operation wavelength, as proposed in ref 7, is 83 ± 15 for our coupled system. This value is higher than previously reported FOM values.7 In addition to the excitation of DLSPP waveguides with
trongly confined surface plasmon-polariton (SPP) modes can be efficiently excited by quantum emitters.1−8 Moreover, the quantum information encryption survives the photonto-plasmon conversion, plasmon propagation and plasmon-tophoton conversions.9−11 This has been demonstrated for single photons, entangled photons and quadrature squeezed light. Plasmonic circuitry has also been utilized for quantum interference and observation of Hong-Ou-Mandel effect.12 The most important challenge in exploiting plasmonic circuitry for quantum-optical networks is inevitable SPP propagation loss by absorption (ohmic loss).13−15 High transparency of dielectric waveguides facilitates information transport over long distances but the corresponding waveguide modes are diffraction-limited in their cross sections.13 Dielectric-loaded surface plasmon polariton (DLSPP) waveguides that confine SPPs laterally by using dielectric ridge waveguides patterned on a flat metal film support guided modes and can also serve as a bridge between nanoplasmonic components and dielectric waveguides.16−19 Furthermore, DLSPP waveguides can be fabricated using standard lithography process, as opposed to V-groove based plasmonic waveguides supporting channel plasmon polaritons or wedge waveguides that can have similar low losses, but require advanced fabrication techniques, such as focused ion beam milling.7,20,21 Furthermore, to accurately position quantum emitters in the vicinity of plasmonic structures or high-index dielectric waveguides, scanning probe manipulation is often used, which can be time-consuming and difficult in incorporation of several single emitters in an integrated circuit.5−7,22−25 © XXXX American Chemical Society
Received: April 12, 2017 Published: August 3, 2017 A
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electron beam lithography onto the nanodiamond, which is found to be a single photon emitter. An atomic force microscope (AFM) image of the fabricated waveguide is illustrated in Figure 2b. Postfabrication charge coupled device (CCD) camera image shows the coupling of the emitter to the DLSPP waveguide and subsequent emission from the gratings at the two ends (Figure 2c), when the NV center is excited. Antibunching dip observed in the second-order correlation function of the NV-center both before (Figure 2d) and after (Figure 2e) fabrication of the waveguide indicates a single photon emitter (g(2)(0) < 0.5). The measured data is fitted with a model presented in ref 29. The cross-correlation (featuring g(2)(0) < 0.5) between the out-coupled emission at the end B and the emission collected from the NV-center shows that the source of emission at ND spot and end B is the same, and that it is a single photon emitter (Figure 2f). This also means that the emission from NV center creates single plasmons in the guided mode that propagate to the ends of the waveguide and are scattered to the far field as single photons. Figure 2g shows the emission spectra of the NV-center taken before and after coupling, as well as the spectrum of the out-coupled light from the grating end A. In Figure 2h, lifetime of the NV-center before and after coupling is presented. A lifetime reduction (from ∼10 ns to ∼6 ns) is observed for the coupled NV-center. The lifetimes are obtained by tail fitting of the measured data with a single exponential. First few ns of the data is avoided in the fitting, as it arises from background fluorescence. We have observed lifetime changes in the range 1.5 to 3.1, and on average, the lifetime decreased by a factor of ∼2.5 (see Figures S2 and S3 in the Supporting Information). On average, the lifetime of NV centers decreased by a factor of 2 due to a silver plane surface, from ∼18 ns on fused silica substrate to ∼9 ns on silver surface.
Figure 1. (a) Schematic of a DLSPP waveguide coupled to a nanodiamond containing single photon emitter. (b) Scanning electron micrograph of a HSQ waveguide, with 250 nm width and 180 nm height, fabricated on silver-coated silicon substrate (grating period = 550 nm).
NV-center emission, we also demonstrate routing of single plasmons between two DLSPP waveguides. In the experiment, a silicon sample is coated with a silver film of 250 nm thickness, on which gold markers are made, and subsequently, nanodiamonds (Microdiamant MSY 0−0.05 μm GAF) are spin coated. The sample is then characterized by scanning in a fluorescence confocal microscope. A detailed description of the experimental setup is available in the Supporting Information (Figure S1). In Figure 2a, markers (+) and a preselected nanodiamond can be observed from the fluorescence image obtained from confocal microscopy. Lifetime, spectrum, and correlation measurements are taken for the nanodiamonds. HSQ e-beam resist (Dow Corning XR1541−006) is then spin coated (1200 rpm, 1 min) to make a 180 nm film on the silver surface. Waveguide is fabricated using
Figure 2. (a) Fluorescence scan map of nanodiamonds spin coated on a sample with markers of gold fabricated on silver surface. Structure indicates the nanodiamond and its position on the sample relative to the markers. (b) AFM image of the fabricated waveguide. The inset shows thickness profile across the gray arrow and indicates a 180 nm height for the waveguide. (c) CCD camera image of the whole structure where the nanodiamond is excited and a fluorescence image of the focal plane is taken, is presented. Emission from the gratings at the ends of the waveguide, when nanodiamond is excited, confirms the coupling of NV center to the waveguide mode. Autocorrelation for the NV center before (d) and after (e) coupling to the waveguide, and cross-correction between the outcoupled emission from the end B and the emission collected directly from the NV center (f). In the correlation figures, τ denotes time delay. (g) Spectrum taken from uncoupled NV (blue), coupled NV (red), and outcoupled light through the grating end A (green). (h) Lifetime of the NV center before (blue) and after (red) coupling. B
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This gives a ∼5-fold enhancement in total decay rate (Γtot), which is in good agreement with the simulated Γpl and Γtot (discussed in detail later in this Letter). We measure propagation characteristics of the DLSPP waveguide for several waveguide samples of different lengths by comparing the attenuation of fluorescence signals PA and PB at the two ends of waveguides and their corresponding propagation distances LA and LB from coupled NV centers. The 1/e propagation length, LP, is extracted from the fluorescence signals at the two ends using PA/PB = exp[(LA − LB)/LP], where we assume symmetric coupling in two directions, uniform losses across the waveguide and the same out-coupling efficiency at the grating ends. The collected data are fitted to obtain the propagation length of 20 ± 5 μm for the DLSPP waveguide. We calculate the emitter’s decay rate into the plasmonic mode (Γpl) guided by the DLSPP waveguide using twodimensional (2D) finite-element modeling (FEM) method.31 Normalized by the spontaneous emission decay rate in the vacuum (Γ0), a 3-fold emission enhancement due to the plasmonic excitation is obtained (Figure 3a). Emission coupling
coupled emitter, as explained in refs 31 and 32. The coupling for a vertically oriented quantum emitter with a DLSPP waveguide is studied for two cases: (1) the distance of the emitter to the silver surface is fixed to 35 nm, and the emitter is moved along x (Figure 3b); and (2) the emitter is moved upward from the surface of the metal along y-axis (Figure 3c). Γ
The distance dependence of the plasmonic decay rate ( pl ), and Γ0
β factor for an emitter coupled to a DLSPP waveguide with 250 nm width, 180 nm height, and dielectric refractive index of nd = 1.41, are calculated for both cases in Figure 3b and c, respectively. We used Palik’s handbook of optical constants33 for silver refractive index for making realistic modeling. With optimized distance of the emitter to the silver surface, the β factor can reach 63%. We calculate the apparent plasmonic coupling factor, βpl, using βpl ≃
[IA + IB] , [IA + IB + INV ]
where IA and IB are
the emission intensity collected by galvanometric mirror scan at the ends of the waveguide and INV is the emission intensity measured at the NV center position (i.e., free space emission not coupled to the DLSPP mode). Here, we have assumed same collection efficiency from the NV center as well as that from the ends, and have ignored the nonradiative decay, as the changes in observed lifetimes are not very high. An apparent coupling factor of 48% is found for the coupled DLSPP waveguide shown in Figure 2c. Taking the propagation length of the DLSPP waveguide into account, the corrected plasmonic coupling factor of 58% is obtained. This is in good agreement with the simulation result and predicts a satisfactory precision in deterministic positioning of the DLSPP waveguide onto the nanodiamond. The ability of such coupled system to achieve efficient longrange energy transfer can be quantified by a figure of merit (FOM) defined as the product of the propagation length, Purcell factor ( Γtot ) and β-factor, normalized by the operation Γ0
wavelength, as proposed in ref 7. The NV-DLSPP waveguide coupled system reaches a value of 83 ± 15 Γ ( Γtot = 5 ± 1, β = 0.58 ± 0.03, Lp = 20 ± 5 μm, λ = 0.7 0
μm) for FOM, which is significantly larger than the value of 6.6 ± 1.5 achieved for NV center coupled to V-groove waveguides (ref 7) or the value of 4.2 ± 1.9 for a colloidal quantum dotsilver nanowire system extracted from ref 3. Far-field characterization of the straight DLSPP waveguide using a super continuum source to excite one grating end and taking spectrum of the outcoupled light from other end is shown in Figure 4. In Figure 4a, one of the grating tapers is used for the DLSPP waveguide excitation, whereas the other one is used to monitor the transmission of the guided SPP mode through the structure. The transmission spectrum of the waveguide is taken and shown in Figure 4c (gray line). A directional coupler (DC) as a basic building block of plasmonic circuitry is designed based on DLSPP waveguides34 and fabricated as shown in Figure 4b (left). The DC consists of two DLSPP waveguides of rectangular cross-section with height h = 180 nm, width w = 250 nm, refractive index nd = 1.41, the separation gap at the parallel section is g = 200 nm, and the Sbends are based on cosine curves. The length of the parallel section (coupling length) is designed to impart a π phase shift at λ = 700 nm between the symmetric and antisymmetric DLSPP modes supported by the structure and calculated to be Lc = 5.3 μm. Design rationale for the structure is explained in the Supporting Information (Figure S4). In Figure 4b, one of
Figure 3. (a) Simulation result for plasmonic decay rate Γpl/Γ0 shows a 3-fold emission enhancement at the optimal position of the emitter. The inset illustrates the NV center inside the DLSPP waveguide in the cross-section. Distance dependence of the plasmonic decay rate and spontaneous emission β factor for DLSPP waveguide coupled NV emitter with a vertically oriented dipole (y-polarized). (b) Emitter moved along x direction outward from the middle of the waveguide (y = 35 nm). (c) Emitter moved along the y-axis outward from the silver surface.
efficiency (β factor) to the DLSPP waveguide is defined as the probability that the quantum emitter excites a single plasmonic mode. It can be described by the fraction of the emitted energy that is coupled to the plasmonic mode, that is, β = Γpl/Γtot, where Γpl is the plasmonic decay rate obtained from the 2D simulation result shown in Figure 3a, and Γtot is the total decay rate, including radiative decay rate, nonradiative decay rate, and the plasmonic decay rate of the quantum emitter coupled to the DLSPP waveguide. A three-dimensional (3D) FEM model with scattering boundaries surrounding the computational domain is implemented using COMSOL Multiphysics software and the total decay rate is extracted from the total power dissipation of the C
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antisymmetric modes with effective refractive indices of n+eff = 1.23, and n−eff = 1.16, respectively (see Figure S4 in the Supporting Information). The difference between experimental measurement and simulation results can be due to the difference in metal layer refractive index that are not exactly the same in fabrication as the ones used for simulation. Following the same procedure, as for DLSPP waveguides, the DLSPPW-based DC is fabricated onto a nanodiamond containing a single emitter. SEM image of the fabricated DC is presented in Figure 5a, top. Postfabrication fluorescent emission imaged on a charge coupled device (CCD) camera, while the NV-center is excited, shows the coupling of the emitter to the structure, and subsequent emission from the grating at the three ends (Figure 5a, bottom). The antibunching dips in the second-order autocorrelation function of the coupled NV center, and in the cross correlation between the coupled NV center and the outcoupled end C are observed in the measurement results illustrated in Figure 5b. As indicated in Figure 5b (right), the antibunching dip for the crosscorrelation is g(2)(0) = 0.49 ± 0.02. This essentially means that the source of emission at all the emission spots (ND, A, B, and C) is the same single NV center. For emission at spot C, the emission from NV center creates single plasmons that first propagate in first waveguide, are routed to the second waveguide, propagate to end C, where it is scattered to the far field as single photons. A g(2)(0) = 0.49 ± 0.02 is high and it arises due to low signal-to-noise ratio at the waveguide end. We note that g(2)(0) values in this experiment, in general, can be improved with the use of single crystalline silver film, which can reduce background fluorescence.35−37 We have repeated the process of fabrication and measurement for DLSPPW-based DC a few times to verify the experimental results (see Supporting Information, Figure S5). Lifetime measurements of the NV center, taken before and after coupling, show a reduction from 12 to 5 ns due to the emission enhancement of the coupled NV center (Figure 5c). Emission spectra of the NV center (before and after coupling) and the outcoupled end C are shown in Figure 5d. Resonance
Figure 4. (a) Camera image of the straight DLSPP structure (right) when end A is illuminated with super continuum source and a microscope image of a DLSPP waveguide (left). (b) Camera image of the DLSPP-based directional coupler (right) when end A is illuminated with super continuum source and a microscope image of the structure (left) are shown. (c) Transmission spectra taken for the straight DLSPP waveguide (gray line), both outcoupled ends B and C of DC together (red line) and end C (cyan line) separately.
the grating tapers (A) is used for SPP excitation, whereas the other ones (B, C) are used to monitor the transmission of the guided DLSPP mode through the DC. The transmission spectra for both outcoupled ends together (B and C), and end C separately, are illustrated in Figure 4c. The spectrum of the end C shows a peak around λ = 650 nm (instead of λ = 700 nm that is designed by simulation) in which the corresponding coupling length, Lc = λ/2(n+eff − n−eff), imparts a π phase shift between the orthogonal symmetric and
Figure 5. (a) CCD camera image of the whole structure when the ND is excited with a continuous wave (532 nm) laser (bottom). SEM image of the fabricated DLSPP-based DC (top). (b) Autocorrelation from the uncoupled NV (blue), coupled NV (red), and cross-correlation taken between the coupled NV and outcoupled end C (b, right). (c) Lifetime measured before (blue) and after (red) fabrication of the DC. (d) Spectrum taken from the uncoupled NV (blue), the coupled NV (red), and outcoupled end C (cyan). D
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peaks observed in the spectrum of the outcoupled end C can be described using mλr = 2n±effLc, where λr denotes the resonance wavelength corresponding to the mth mode of the cavity length, which is equal to the coupling length of the DC, Lc, and n+eff and n−eff are the effective refractive indices of the symmetric and antisymmetric DLSPP modes propagating along parallel section of the DC. For the simulated parameters of n+eff = 1.23, n−eff = 1.16, and Lc = 5.3 μm, the corresponding resonance wavelengths are calculated to be close to 687 nm (m = 19) and 653 nm (m = 20), which fits well to the measured results in Figure 5d. In conclusion, we have demonstrated DLSPP waveguide as a basic building block for plasmonic circuitry containing single photon sources. An emission coupling efficiency of 58% and a 5-fold enhancement in total decay rate has been achieved due to the confined DLSPP mode. A large propagation length of 20 ± 5 μm has been observed experimentally that can be further enhanced by coupling of DLSPP waveguides into photonic waveguides. The DLSPP waveguides have been employed for making directional coupler and can be also used for other components such as cavities to provide a platform for on-chip processing of quantum information.
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ASSOCIATED CONTENT
S Supporting Information *
The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsphotonics.7b00374. Section S1: Optical set-up; Section S2: Excitation of DLSPP mode with a single NV center; Section S3: Routing of single plasmons in a DLSPPW based circuitry (PDF).
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AUTHOR INFORMATION
Corresponding Authors
*E-mail:
[email protected]. *E-mail:
[email protected]. ORCID
Hamidreza Siampour: 0000-0001-8476-0207 Sergey I. Bozhevolnyi: 0000-0002-0393-4859 Notes
The authors declare no competing financial interest.
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ACKNOWLEDGMENTS The authors acknowledge financial support from the European Research Council, Grant 341054 (PLAQNAP). REFERENCES
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