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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	<tbody>
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			<td height="21" style="height:21px;width:319px;">SU-8</td>
			<td style="width:213px;">MicroChem</td>
			<td style="width:119px;">SU-8 2000.5</td>
			<td style="width:167px;"></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;">Adhesion solution</td>
			<td style="width:213px;">MicroChem</td>
			<td style="width:119px;">Omnicoat</td>
			<td></td>
		</tr>
		<tr height="20">
			<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>
			<td></td>
		</tr>
		<tr height="21">
			<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>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Spin Coater</td>
			<td style="width:213px;">Chemat Technology</td>
			<td style="width:119px;">KW-4A</td>
			<td></td>
		</tr>
		<tr height="21">
			<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>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Shutter</td>
			<td style="width:213px;">Thorlabs</td>
			<td style="width:119px;">SH05</td>
			<td></td>
		</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>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Pinhole</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">PNH-50</td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Iris</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">M-DI47.50</td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Prism</td>
			<td style="width:213px;">Thorlabs</td>
			<td style="width:119px;">PS611</td>
			<td></td>
		</tr>
		<tr height="21">
			<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>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Supttering Deposition System</td>
			<td style="width:213px;">Homemade</td>
			<td style="width:119px;"></td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Rotation Stage 1</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">URM80ACC</td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Rotation Stage 2</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">RV120PP</td>
			<td></td>
		</tr>
		<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>
			<td></td>
		</tr>
		<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>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Quartz lamp</td>
			<td style="width:213px;">Newport</td>
			<td align="right" style="width:119px;">66884</td>
			<td></td>
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			<td height="21" style="height:21px;width:319px;">Fiber Bundle</td>
			<td style="width:213px;">Newport</td>
			<td align="right" style="width:119px;">77578</td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Objective for measurement</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">M-5X &#38; M-60X</td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Polarizer &#38; Analyzer</td>
			<td style="width:213px;">Thorlabs</td>
			<td style="width:119px;">GT15</td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Multimode Fiber</td>
			<td style="width:213px;">Thorlabs</td>
			<td style="width:119px;">BFL105LS02</td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Spectrometer</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">MS260i</td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">CCD</td>
			<td style="width:213px;">Andor</td>
			<td style="width:119px;">DV420-OE</td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">514nm Argon Ion Laser</td>
			<td style="width:213px;">Spectra-Physics</td>
			<td style="width:119px;">177-G01</td>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">633nm HeNe Laser</td>
			<td style="width:213px;">Newport</td>
			<td style="width:119px;">R-32413</td>
			<td></td>
		</tr>
		<tr height="21">
			<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>
			<td></td>
		</tr>
		<tr height="21">
			<td height="21" style="height:21px;width:319px;">Polyvinyl alcohol polymer (PVA)</td>
			<td style="width:213px;">SIGMA-ALDRICH</td>
			<td align="right" style="width:119px;">363073</td>
			<td></td>
		</tr>
		<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 ...

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