Name: determination of the excitation and coupling rates between light emitters and surface plasmon polaritons
Uploaded: 2018-07-21T12:30:00
Description: Watch this Scientific Journal Video about Determination of the Excitation and Coupling Rates Between Light Emitters and Surface Plasmon Polaritons at JoVE.com

This research was supported by the Chinese University of Hong Kong through the Direct Grants 4053077 and 4441179, RGC Competitive Earmarked Research Grants, 402812 and 14304314, and Area of Excellence AoE/P-02/12.

1. Setup of Interference Lithography
NOTE: Interference lithography is used to fabricate the periodic arrays12. The schematic setup, as is shown in Figure 1, is built up as follows:
<ol>
	<li>Focus the 325 nm laser from a HeCd multimode laser to a 13X UV objective lens and pass it through a 50 &#956;m pinhole based spatial filter for mode cleaning.</li>
	<li>Place two 2.5 cm diameter irises 30 cm apart to further filter the central region...

<ol>
	<li>Okamoto, K., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Surface-plasmon-enhanced+light+emitters+based+on+InGaN+quantum+wells.">Surface-plasmon-enhanced light emitters based on InGaN quantum wells.</a> Nature Materials. 3 (9), 601-605 (2004).</li><li>Akselrod, G. M., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Leveraging+Nanocavity+Harmonics+for+Control+of+Optical+Processes+in+2D+Semiconductors.">Leveraging Nanocavity Harmonics for Control of Optical Processes in 2D Semiconductors.</a> Nano Letters. 15 (5), 3578-3584 (2015).</li><li>Gontijo, I., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Coupling+of+InGaN+quantum-well+photoluminescence+to+silver+surface+plasmons.">Coupling of InGaN quantum-well photoluminescence to silver surface plasmons.</a> Physical Review B. 60 (16), 11564 (1999).</li><li>Huang, K. C. Y., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Antenna+electrodes+for+controlling+electroluminescence.">Antenna electrodes for controlling electroluminescence.</a> Nature Communications. 3, 1005 (2012).</li><li>Atwater, H. A., Polman, A. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Plasmonics+for+improved+photovoltaic+devices.">Plasmonics for improved photovoltaic devices.</a> Nature Materials. 9 (3), 205-213 (2010).</li><li>Anker, J. N., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Biosensing+with+plasmonic+nanosensors.">Biosensing with plasmonic nanosensors.</a> Nature Materials. 7 (6), 442-453 (2008).</li><li>Chen, Y., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Excitation+enhancement+of+CdSe+quantum+dots+by+single+metal+nanoparticles.">Excitation enhancement of CdSe quantum dots by single metal nanoparticles.</a> Applied Physics Letters. 93 (5), 053106 (2008).</li><li>Birowosuto, M. D., Skipetrov, S. E., Vos, W. L., Mosk, A. P. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Observation+of+Spatial+Fluctuations+of+the+Local+Density+of+States+in+Random+Photonic+Media.">Observation of Spatial Fluctuations of the Local Density of States in Random Photonic Media.</a> Physical Review Letters. 105 (1), 013904 (2010).</li><li>Cao, Z. L., Ong, H. C. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Determination+of+coupling+rate+of+light+emitter+to+surface+plasmon+polaritons+supported+on+nanohole+array.">Determination of coupling rate of light emitter to surface plasmon polaritons supported on nanohole array.</a> Applied Physics Letters. 102 (24), 241109 (2013).</li><li>Lin, M., Cao, Z. L., Ong, H. C. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Determination+of+the+excitation+rate+of+quantum+dots+mediated+by+momentum-resolved+Bloch-like+surface+plasmon+polaritons.">Determination of the excitation rate of quantum dots mediated by momentum-resolved Bloch-like surface plasmon polaritons.</a> Optics Express. 25 (6), 6029-6103 (2017).</li><li>Nikolaev, I. S., Lodahl, P., Driel, A. F. V., Koenderink, A. F., Vos, W. L. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Strongly+nonexponential+time-resolved+fluorescence+of+quantum-dot+ensembles+in+three-dimensional+photonic+crystals.">Strongly nonexponential time-resolved fluorescence of quantum-dot ensembles in three-dimensional photonic crystals.</a> Physical Review B. 75 (11), 115302 (2007).</li><li>Cao, Z. L., Lo, H. Y., Ong, H. C. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=Determination+of+absorption+and+radiative+decay+rates+of+surface+plasmon+polaritons+from+nanohole+array.">Determination of absorption and radiative decay rates of surface plasmon polaritons from nanohole array.</a> Optics Letters. 37 (24), 5166-5168 (2012).</li><li>Haus, H. A. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed&cmd=Search&doptcmdl=Citation&defaultField=Title+Word&term=.">.</a> Waves and Fields in Optoelectronics. , (1984).</li></ol>

In this protocol, there are several critical steps. First, mechanical stability is crucial in sample preparation. The standing wave generated by Lloyd&#39;s setup is sensitive to the phase difference between two illumination beams. Therefore, any vibration during the exposure time will degrade the uniformity and edge sharpness of the nanohole. It is highly recommended to operate in a vibration-free environment, e.g., an optical table with vibration isolation supports. In addition, high power laser is also desire...

Surface plasmon mediated fluorescence (SPMF) has received considerable attention recently1,2,3,4,5,6. When light emitters are placed in close proximity to a plasmonic system, energy can be transferred between the emitters and surface plasmon polaritons (SPPs). In general, the strong plasmonic fields can strongly enhance the excitation of the emitters2. At the same time, the emission rate is also increased because of the large density-of-states created by SPPs, yielding the well-known Purcell effect3. These two processes work hand in hand in producing the SPMF. As SPMF has stimulated numerous applications in solid-state lighting1,4, energy harvesting5, and bio-detection6, it is currently under intensive investigation. In particular, the knowledge of the energy transfer rates from the SPPs to the emitters and vice versa, i.e., the excitation and coupling rates, is of great importance. However, the excitation and emission processes are usually entangled together, study on this aspect is still lacking. For example, most of the studies only determine the excitation efficiency ratio, which simply compares the emission with and without SPPs7. The exact measurement of the excitation rate is still missing. On the other hand, conventional time-resolved techniques such as fluorescence lifetime spectroscopy are routinely used for studying the dynamics of the emission process, but they are unable to separate the coupling rate from the total decay rate8. Here, we describe how one can determine them by combining the rate equation model and the temporal coupled mode theory9,10. Remarkably, we find that the excitation and coupling rates can be expressed in terms of measurable quantities, which can be accessed by performing angle- and polarization-resolved reflectivity and photoluminescence spectroscopy. We will first outline the formulation and then describe the instrumentation in detail. This approach is entirely frequency domain based and it does not require any time-resolved accessories such as ultra-fast lasers and time-correlated single-photon counters, which are expensive and sometimes difficult to implement8,11. We anticipate this technique to be an enabling technology for determining the excitation and coupling rates between light emitters and resonant cavities.
The SPMF in periodic systems is briefed here. For a periodic plasmonic system where Bloch-like SPPs can be generated, other than direct excitation and emission, which are characterized by the excitation efficiency&#160;&#951; and spontaneous emission rate &#915;r, the emitters can be excited by incoming SPPs and decay via outgoing SPPs. In other words, under resonance excitation, incoming SPPs are generated to create strong plasmonic fields that energize the emitters. Once the emitters are excited, energy from them can be transferred to outgoing SPPs, which subsequently radiatively dissipate to far-field, giving rise to enhanced emission. They define SPMF. For simple two-level emitters, the excitation refers to the increased transition of electrons from the ground to the excited states whereas the emission defines the decay of electrons back to the ground states, accompanied by photon emission at wavelengths defined by the energy difference between the excited and ground states. The excitation and emission conditions for the SPMF are required to fulfill the well-known phase matching equation to excite the incoming and outgoing SPPs9
<img alt="Equation 1" src="/files/ftp_upload/56735/56735eq1.jpg" /> (1)
where &#949;a and &#949;m are the dielectric constants of the dielectrics and the metal,&#160;&#952; and&#160;&#966; are the incident and azimuthal angles, P is the period of the array,&#160;&#955; is the excitation or emission wavelength, and m and n are the integers specifying the order of SPPs. For excitation, the in-plane wavevector of the laser beam will be Bragg scattered to momentum match with the incoming SPPs and the &#952; and&#160;&#966; together define the specified incident configuration for exciting the SPPs to enhance the electronic absorption at the excitation wavelength &#955;ex. Likewise, for the emission, the outgoing SPPs will be reversely Bragg scattered to match with the light line and the angles now represent the possible emission channels at the emission wavelength &#955;em. However, it is noted that as the emitters can couple their energy to vectorial propagating SPPs with <img alt="Equation 2" src="/files/ftp_upload/56735/56735eq2.jpg" /> that has the same magnitude <img alt="Equation 3" src="/files/ftp_upload/56735/56735eq3.jpg" /> but different directions, the SPPs can decay via various combination of (m,n) to far-field following Eq. (1).
By using the rate equation model and temporal coupled mode theory (CMT), we find that the excitation rate &#915;ex, i.e., the energy transfer rate from SPPs to emitters, can be expressed as9,12,13
<img alt="Equation 4" src="/files/ftp_upload/56735/56735eq4.jpg" /> (2)
where &#951; is the aforementioned direct excitation rate in the absence of the incoming SPPs, &#915;tot is the total decay rate of the incoming SPPs&#160;<img alt="Equation 5" src="/files/ftp_upload/56735/56735eq5.jpg" /> in which &#915;abs and &#915;rad are the Ohmic absorption and radiative decay rates of SPPs, and&#160;<img alt="Equation 6" src="/files/ftp_upload/56735/56735eq6.jpg" /> is the photoluminescence power ratio with and without the incoming SPPs. On the other hand, the coupling rate &#915;c, i.e., the energy transfer rate from emitters to SPPs, can be written as:
<img alt="Equation 7" src="/files/ftp_upload/56735/56735eq7.jpg" /> (3)
where &#915;r is the direct emission rate, <img alt="Equation 8" src="/files/ftp_upload/56735/56735eq8.jpg" /> is the photoluminescence power ratio between the &#945;th SPP mediated decay and direct ports, and &#915;rad&#945; and &#915;tot are the radiative decay rates for the &#945;th port and the total decay rates. We will see that while all the SPP decay rates can be measured by reflectivity spectroscopy, the emission power ratio can be determined by photoluminescence spectroscopy. Details of the formulations can be found in reference9,10.

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			<td height="20" style="height:21px;width:319px;">SU-8 Thinner (Gamma-Butyrolactone)</td>
			<td style="width:213px;">MicroChem</td>
			<td style="width:119px;">SU-8 2000 Thinner</td>
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			<td height="21" style="height:21px;width:319px;">SU-8 Developer</td>
			<td style="width:213px;">MicroChem</td>
			<td style="width:119px;">SU-8 Developer</td>
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			<td height="21" style="height:21px;width:319px;">Spin Coater</td>
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			<td height="21" style="height:21px;width:319px;">HeCd laser</td>
			<td style="width:213px;">KIMMON KOHA CO., LTd</td>
			<td style="width:119px;">IK3552R-G</td>
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			<td height="21" style="height:21px;width:319px;">Shutter</td>
			<td style="width:213px;">Thorlabs</td>
			<td style="width:119px;">SH05</td>
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		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Objective for sample preparation</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">U-13X</td>
			<td></td>
		</tr>
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			<td height="21" style="height:21px;width:319px;">Pinhole</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">PNH-50</td>
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			<td height="21" style="height:21px;width:319px;">Iris</td>
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			<td height="21" style="height:21px;width:319px;">Prism</td>
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			<td style="width:119px;">PS611</td>
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			<td height="21" style="height:21px;width:319px;">Rotation stage for sample preparation</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">481-A</td>
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			<td height="21" style="height:21px;width:319px;">Rotation Stage 1</td>
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			<td style="width:119px;">URM80ACC</td>
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			<td height="21" style="height:21px;width:319px;">Rotation Stage 2</td>
			<td style="width:213px;">Newport</td>
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		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Rotation Stage 3</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">SR50PP</td>
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		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Detection arm</td>
			<td style="width:213px;">Homemade</td>
			<td style="width:119px;"></td>
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			<td height="21" style="height:21px;width:319px;">Quartz lamp</td>
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			<td height="21" style="height:21px;width:319px;">Polarizer &#38; Analyzer</td>
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			<td style="width:119px;">GT15</td>
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			<td height="21" style="height:21px;width:319px;">CdSeTe quantum dot</td>
			<td style="width:213px;">Thermo Fisher Scientific</td>
			<td style="width:119px;">q21061mp</td>
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			<td height="21" style="height:21px;width:319px;">Polyvinyl alcohol polymer (PVA)</td>
			<td style="width:213px;">SIGMA-ALDRICH</td>
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		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Control program</td>
			<td style="width:213px;">National Instruments</td>
			<td style="width:119px;">LabVIEW</td>
			<td></td>
		</tr>
	</tbody>
</table>

determination of the excitation and coupling rates between light emitters and surface plasmon polaritons

We have developed a unique method to measure the excitation and coupling rates between the light emitters and surface plasmon polaritons (SPPs) arising from metallic periodic arrays without involving time-resolved techniques. We have formulated the rates by quantities that can be measured by simple optical measurements. The instrumentation based on angle- and polarization-resolved reflectivity and photoluminescence spectroscopy will be described in detail here. Our approach is intriguing due to its simplicity, which requires routine optics and several mechanical stages, and thus is highly affordable to most of the research laboratories.

An example of an Au periodic array is given in the inset of Figure 4a8. The plane view SEM image shows that the sample is a 2D square lattice circular hole array with a period of 510 nm, a hole depth of 280 nm, and a hole diameter of 140 nm. The p-polarized reflectivity mapping taken along the &#915;-X direction is shown in Figure 4a. The dash line is calculated by the phase matching equation Eq. (1) indic...

Watch this Scientific Journal Video about Determination of the Excitation and Coupling Rates Between Light Emitters and Surface Plasmon Polaritons at JoVE.com

Determination of the Excitation and Coupling Rates Between Light Emitters and Surface Plasmon Polaritons

This protocol describes the instrumentation for determining the excitation and coupling rates between light emitters and Bloch-like surface plasmon polaritons arising from periodic arrays.

We have developed a unique method to measure the excitation and coupling rates between the light emitters and surface plasmon polaritons (SPPs) arising ...

This method can help answer key questions in fluorescence enhancement, such as surface plasmon-mediated fluorescence. The main advantage of this technique is that it differentiates the excitation and the decay processes of surface plasmon-mediated fluorescence entirely in frequency domain. Prepare a substrate for the periodic array.For this experiment, use a one square centimeter piece of glass. Clean it in ultrasonic baths of methanol and acetone for 10 minutes each. When done, place it on a 200 degree Celsius hotplate for one hour.For the spin coating steps, dilute native photoresist with a thinner, and have adhesion solution ready. Move the glass substrate to a spin coater, and dispense three to five drops of adhesion solution onto it. Spin the substrate at 600 rpm for 10 seconds, then 3, 600 rpm for one minute.Next, place five to seven drops of diluted photoresist on the substrate. Spin coat the substrate at 600 rpm for 10 seconds, then 3, 600 rpm for one minute. When done, move the spin coated sample to a 65 degree Celsius hotplate, and leave it there for one minute.Then, transfer the sample to a 95 degree Celsius hotplate, and leave it for another minute. From the hotplate, take the sample to mount on a Lloyd's interferometer. The set-up has a prism for a sample holder, with a mirror perpendicular to it.Use a drop of refractive index matching oil on the sample to attach it to the prism. Position the sample as close to the mirror as possible. Expose the sample in this initial orientation.Then, to create a two dimensional square lattice, rotate the sample 90 degrees on the prism. Use the same exposure time for a second exposure. Return the sample to the 65 degree Celsius hotplate for two minutes.Then, place it on the 95 degree Celsius hotplate for two minutes. Next, immerse the sample in developer for two minutes with continuous agitation. Retrieve the sample and immerse it in isopropyl alcohol for one minute, to rinse residuals.Work with an RF sputtering deposition system to put a 100 nanometer gold film on the sample. Once the sample is ready, take it and a styryl 8 dye preparation to a spin coater. Dispense 0.2 milliliters, or three to five drops, of the solution onto the sample.Spin coat this to produce a thickness of about 80 nanometers. For the reflectivity measurements, use a goniometer. This system uses broadband white light from a quartz lamp.A multi-mode fiber bundle transmits the light to face-to-face objective lenses for collimation. A polarizer and shutter are next in the path. The light illuminates a sample on a sample stage with three independent rotation stages.A detection analyzer is after the sample stage. Another multi-mode fiber collects the specular reflection from the sample, to transmit it to a spectrometer and CCD camera. After aligning and calibrating the set-up, set up an automated system to collect data.Use the automation to step through different incident angles and collect the reflection spectra. For these measurements, the step size of the incident angle is 0.5 degrees. The wavelength resolution is 0.66 nanometers.To measure the orthogonal reflectivity, alter the set-up. Set the incident polarizer to 45 degrees with respect to the incident plane. Set the analyzer to negative 45 degrees with respect to the incident plane.Proceed with another automated measurement. Photoluminescence measurements require another change to the set-up. Replace the broadband light source with a 633 nanometer helium neon laser.Place a laser line filter before the polarizer. Also, place a half wave plate after the shutter. Complete the set-up by substituting a notch filter for the analyzer before the spectrometer.Conduct automated incident scans by fixing the detection angle, and varying the incident angle with respect to the sample normal. The surface plasmon polaritons are incident angle dependent, and are selectively excited. Next, conduct a detection scans by fixing the incident angle with respect to the sample normal, and varying the detection angle.This is the P-polarized reflectivity mapping taken along the gamma X direction of the gold array in the inset. The dashed line is calculated using the phase matching equation, and implies that the M equals negative one and N equals zero surface plasma polaritons are excited. This reflectivity map is from when the polarizer and analyser are at orthogonal positions.The background is now zero, as indicated by the blue of the color map. The reflectivity profiles have peaks in green, instead of dips, as only the surface plasma polaritons remain after removing the background. This is the P-polarized reflectivity mapping and the orthogonal reflectivity mapping along the gamma X for cadmium, selenium, telluride, quantum dot doped PVA polymer, spin coated on the array.In addition, here are data for the incident and detection angle photoluminescence measurements. The data can be used to determine the excitation and coupling rates between light emitters and resident cavities. Though this method can provide insight into fluorescence enhancement from periodic arrays, it can be also applied to other systems, such as metamaterials and photonic crystals.Once mastered, this technique can be done in three hours, if it is performed properly. While attempting this procedure, it is important to remember to check the alignment of the array set-up, and the polarization and angles of the reflectivity spectrography. After its development, this technique paved the way for researchers in the field of photoluminescences to explore surface plasma-enhanced fluorescence in the field of resins enhancement.After watching this video, you should have a good understanding of how to determine the excitation and the coupling rate between light emitters and the surface plasma polaritons arising from periodic arrays.

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Nuclear reaction analysis (NRA) via the resonant 1H(15N,&#945;&#947;)12C reaction is a highly effective method of depth profiling that quantitatively and ...

Emission Spectroscopic Boundary Layer Investigation during Ablative Material Testing in Plasmatron

Ablative Thermal Protection Systems (TPS) allowed the first humans to safely return to Earth from the moon and are still considered as the only solution ...

Measurement of Outgassing Rates of Steels

Steels are commonly used materials in the fabrication of vacuum systems because of their good mechanical, corrosion, and vacuum properties. A variety of ...

Synchrotron X-ray Microdiffraction and Fluorescence Imaging of Mineral and Rock Samples

In this report, we describe a detailed procedure for acquiring and processing&#160;x-ray microfluorescence (&#956;XRF), and Laue and powder ...

Excitation-Scanning Hyperspectral Imaging Microscopy to Efficiently Discriminate Fluorescence Signals

Several techniques rely on detection of fluorescence signals to identify or study phenomena or to elucidate functions. Separation of these fluorescence ...

Accurate Determination of the Equilibrium Surface Tension Values with Area Perturbation Tests

We demonstrate two robust protocols for determining the equilibrium surface tension (EST) values with area perturbation tests. The EST values should be ...