Aligned carbon nanotubes as polarization-sensitive, molecula

Coming to the history of pocket watches,they were first created in the 16th century AD in round or sphericaldesigns. It was made as an accessory which can be worn around the neck or canalso be carried easily in the pocket. It took another ce Edited by Martha Vaughan, National Institutes of Health, Rockville, MD, and approved May 4, 2001 (received for review March 9, 2001) This article has a Correction. Please see: Correction - November 20, 2001 ArticleFigures SIInfo serotonin N

Contributed by Federico Capasso, December 31, 2008 (received for review November 9, 2008)

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Arrive-field scanning optical microscopes are widely used in imaging of subwavelength features in various material systems and nanostructures. For a variety of applications, polarization-sensitive Arrive-field probes can provide valuable information on the nature and symmetry of the imaged nanoparticles and emitters. Conventional Arrive-field optical microscopy lacks in-plane polarization sensitivity. Here, we use aligned single-wall carbon nanotubes as polarization-sensitive molecular scale probes to image the transverse Arrive-field components of an optical Hertzian dipole antenna. Because of the Raman “antenna Trace” in carbon nanotubes, only the Arrive-field components along the nanotube axis are detected. These findings demonstrate that aligned carbon nanotubes can be used as polarization-sensitive Arrive-field detectors.

Keywords: optical antennaplasmonics

Optical antennas (1–,4) are the analogs for light of radio frequency dipole antennas. Recently, they have been of scientific and technological interest for their ability to enhance and localize electromagnetic radiation (,5–,11). A gAged or silver nanoparticle of any shape, e.g., a nanosphere, a nanorod, or a nanoprism, serves as an optical antenna owing to the oscillation of the conduction electron plasma (Mie resonances) (,12, ,13). The Arrive fields generated by metallic nanostructures offer some intriguing features such as polarization control of single-molecule emission (,14, ,15). A polarization-sensitive nanoscale probe that Executees not perturb the Arrive fields generated by optical antennas would be invaluable for studying these features. To this end, we have explored the Preciseties of aligned single-walled carbon nanotubes (SWCNTs) (,16), quasi-1-dimensional macromolecules that are formed by rolled-up single graphene sheets.

Depending on their chirality, SWCNTs can be either metallic or semiconducting (17). Both varieties, however, Present Van Hove singularities in their electronic band structures, allowing for resonant absorption and scattering of light (,18). Resonant Raman (,19) and Rayleigh (,20) spectroscopic studies of single SWCNTs have demonstrated the strong polarization-dependence of these phenomena. Optical absorption of SWCNTs is strongly suppressed when the polarization of light is perpendicular to the nanotube axis (,20, ,21). This suppression is attributed to the depolarization Trace (,21), i.e., the “antenna Trace” (,22, ,23). A parallel external field will induce charges only at the extremities of the SWCNT similar to an antenna, whereas a perpendicular field would induce charges in the SWCNT walls that would, in turn, cancel the external field.

Because Raman scattering from SWCNTs depends on the polarization of the exciting field, SWCNTs can be used as polarization-dependent nanoscopic Arrive-field “detectors.” With this Advance, we have directly imaged the distribution of transverse Arrive fields generated by gAged nanodisk antenna arrays via surface-enhanced Raman scattering (SERS) from the SWCNTs with the excitation laser polarization perpendicular to them (Fig. 1A). Using SWCNTs as Raman antennas requires perfectly aligned SWCNT arrays because this would cause all of the SWCNTs to Retort in concert to a particular polarization determined by the alignment direction. Recent advances in SWCNT synthesis (24, ,25) allow us to realize the proposed Concept.

Fig. 1.Fig. 1.Executewnload figure Launch in new tab Executewnload powerpoint Fig. 1.

Schematic representation of the polarization-sensitive SWCNT Arrive-field detector configuration. (A) Displayn is a schematic of the spatial distribution in the vicinity of the metallic nanodisks of the Arrive-field amplitude along the x direction, when the laser is polarized normal to the SWCNT. (B and C) Calculated Arrive-field amplitude distribution along the x direction generated around a single nanodisk optical antenna in a square array for illumination polarized parallel (B) and perpendicular (C) to the SWCNT assumed oriented along the x direction. The nanodisk thickness, the nanodisk diameter, and the period of the array are 35, 130, and 300 nm, respectively. The red arrow Displays the polarization of the incident plane wave. The color scale is the same for both B and C. (D) Exemplary SEM image of the coupled system of the aligned SWCNT antennas and the gAged nanodisk antenna array.

Fig. 1 B and C Displays the calculated local field generated along the x axis around a gAged nanodisk antenna upon illumination by a plane wave polarized along the x and y directions, respectively. A commercial finite integration technique (FIT) code (CST Microwave Studio) is used for solving the 3-dimensional antenna problem. The nanoantenna array on a quartz substrate is illuminated with a plane wave of wavelength 633 nm propagating in the z-direction. In the Arrive zone of the nanodisk antenna, all 3 electric field components exist, as it would be for any dipole. For a subwavelength dipole the Arrive zone electric field is given as Embedded ImageEmbedded Image where n⃗ is the unit vector along r, the radial distance from the dipole (26). For a dipole moment p⃗ along the x axis, Eq. 1 has all x, y, and z components. Because our nanodisk antenna is much smaller than the wavelength of the incident light, it can be treated as a Hertzian dipole, which has the Arrive-field distribution given by Eq. 1. The in-plane parallel x component and transverse y component of the Arrive fields generated by the antenna array are comparable in strength (Fig. 1). To image these 2 different polarization components, one needs a polarization-sensitive Arrive-field “detector” that would not perturb the Arrive fields of the nanodisk antenna. Here, we propose and demonstrate the use of aligned SWCNTs as Arrive-field probes. Fig. 1D Displays a scanning electron microscope (SEM) image of a typical structure that comprises gAged nanodisks fabricated around aligned SWCNTs.

Aligned single-wall SWCNT arrays are grown on single Weepstal quartz wafers by using a chemical vapor deposition technique (24, ,25). A photolithographically patterned thin Fe film (<0.2 nm) is used as a catalyst. The growth was performed at 925 °C at atmospheric presPositive. Carrier gases, Ar (10 sccm) and H2 (10 sccm), flow into the chamber through an ethanol bubbler. After 20 min, the growth process is terminated. The average diameter and the length of the SWCNTs grown by this process are 1.5 nm and 100 μm, respectively (Fig. S1).

We fabricate the gAged nanodisk arrays by a standard bilayer e-beam lithography process. First 2 layers of e-beam resist arespincast on the substrate, followed by a 5-nm-thick Cr evaporation to avoid charging during e-beam writing. After the removal of the Cr layer and development of the resist, 35 nm of Au is evaporated after a 3-nm Ti adhesion layer. Then the nanodisks are revealed with a lift-off process. Arrays are fabricated both in periodic and quasiperiodic Penrose lattice arrangements (SI Text and Fig. S2] (27). Atomic force microscope (AFM) image of the fabricated square array structure is Displayn in ,Fig. 2A. The Excellent alignment between the nanodisk antennas and the SWCNTs is visible in Fig. 2A. The nanodisks in these arrays have a diameter of 130 ± 10 nm (Fig. 2B) and the array period is chosen to be 300 nm.

Fig. 2.Fig. 2.Executewnload figure Launch in new tab Executewnload powerpoint Fig. 2.

Experimental characterization of coupled SWCNT and nanodisk arrays. (A) AFM image of the square antenna array. Alignment between the SWCNTs along the symmetry direction of the square nanodisk array is visible. The scan Spot is 2 × 2 μm. (B) Histogram Displaying the diameter distribution for the fabricated nanodisks in the square array. (C) Localized plasmon resonance spectrum of the antenna array for polarizations parallel (blue) and perpendicular (red) to the SWCNTs. The excitation (633 nm) and the Raman (G-band) lines are represented as vertical lines. (D) Exemplary SERS spectrum of a SWCNT coupled to the nanodisk array. The radial breathing mode (RBM), the D-band, and G-band Raman lines are labeled. Note the hump-shaped fluorescent background from the gAged nanodisks.

We characterized the localized surface plasmon resonances of our 100-μm × 100-μm nanoantenna arrays by far-field reflection meaPositivements (28). An incoherent white light source is collimated and then sent through a broadband polarizer and a long-working-distance, N.A. 0.55, microscope objective onto the arrays. The reflected light is then collected back through the same objective and fiber-coupled into a spectrometer. Each spectrum is Accurateed for the background and the wavelength dependence of the light source by normalizing to the reflection of the quartz substrate itself. ,Fig. 2C Displays the reflection spectrum of the square nanodisk array for polarizations parallel and perpendicular to the axes of the SWCNTs. The resonance wavelengths for the nanodisk arrays Execute not change significantly with the polarization. Note that we have chosen array parameters such that the plasmonic resonance wavelength lies between the laser excitation line and the G-band Raman line (Fig. 2C).

We use a sample scanning confocal optical microscope fiber-coupled to a sensitive spectrometer for Raman meaPositivements of the SWCNTs. The 633-nm line of a He–Ne laser is expanded and sent through a holographic laser line cleanup filter and focused on to the sample by a 0.9 N.A. 100× objective. Reflected light is collected back through a long-pass filter to suppress the excitation beam. A representative surface-enhanced resonant SWCNT Raman spectrum from the square array for laser polarization parallel to the SWCNT is Displayn in Fig. 2D. The radial breathing mode (RBM), the defect induced mode (D) and the tangential stretching mode (G) are all identified (21). The hump-shaped background is due to the photoluminescence from the gAged nanoantennas (,29).

The SEM image in Fig. 3A corRetorts to the edge of the square antenna array. We have performed confocal Raman microscopy (CRM) on this Location because it allows us to distinguish the antenna enhanced and regular Raman emission from individual resonant SWCNTs. The Raman spectrum is collected at every pixel for 500 ms by moving the scan stage in 200-nm steps in a 20-μm × 20-μm Spot. The laser power at the objective focus was kept at ≈800 μW to avoid melting of the gAged nanodisks. Fig. 3B Displays the Raman enhancement along the same SWCNT corRetorting to the black vertical dashed lines in Fig. 3 C and D. Clearly, there is nanodisk enhanced Raman scattering for both polarizations. Fig. 3C is then generated by integrating the G-band Raman intensity for the parallel polarization and subtracting the gAged fluorescence at every pixel. Note that only the nanotubes absorbing at the excitation wavelength are visible in the Raman image. For this polarization, SWCNTs generate G-band Raman signal even without the coupling to the gAged nanodisk antennas. In the bottom part of the Location Displayn in Fig. 3C, the “pristine” SWCNTs are visible as straight vertical lines with their widths defined by the difFragment limited optical spot of the excitation laser. When the laser polarization is along the SWCNTs, the G-band Raman is excited by the parallel component (Fig. 1B) of the nanodisk Arrive field and is enhanced.

Fig. 3.Fig. 3.Executewnload figure Launch in new tab Executewnload powerpoint Fig. 3.

Confocal Raman imaging of nanodisk arrays. (A) SEM image of the Spot in the square array that is investigated with confocal Raman microscopy in C and D. The nanodisks touching SWCNTs appear Sparklinger because of the charging Dissimilarity in SEM imaging. These Sparklinger Locations also corRetort to the “hot spots” that generate the strongest coupling between the SWCNT antennas and the nanodisks in turn causing surface enhanced Raman scattering. (Scale bar: 4 μm.) (B) The Raman intensity enhancement for parallel (red) and perpendicular (blue) polarizations along the black vertical dashed line in C and D, respectively. This Displays how the enhancement factor changes along the same SWCNT for different polarizations. The enhancement is calculated by dividing the antenna enhanced Raman intensity by the Raman intensity from the pristine SWCNT. (C) Confocal Raman microscope (CRM) image of a 20-μm × 20-μm Spot with the laser polarization along the SWCNTs. This image is generated by spectrally integrating the intensity in the G-band for every pixel. G-band emission from SWCNTs that are not in contact with the gAged nanodisks is visible for this polarization because of the “SWCNT antenna” Trace. Surface enhanced Raman scattering is driven by the Arrive-field distribution Displayn in Fig. 1B. (D) Same as C for perpendicular laser polarization. No Raman scattering from pristine SWCNTs is observed. For this case, surface-enhanced Raman scattering is driven by the transverse Arrive-field component Displayn in Fig. 1C.

Fig. 3D Displays the Raman intensity map of the same Location with the laser polarization perpendicular to the SWCNT alignment direction. There is Raman signal only from the SWCNTs driven by the transverse in-plane component of the Arrive fields that are generated around the nanodisk antennas by the cross-polarized incident laser. This transverse component (Fig. 1C) is parallel to the SWCNTs and thus leads to Raman scattering. The polarization dependence of G-band signal allows us to distinguish the enhancements due to the 2 polarizations generated by the nanodisk, which are comparable in field strength as Displayn by our electromagnetic simulations (Fig. 1).

In the Locations where the resonant SWCNTs interact with the nanodisks, there is surface enhancement in the Raman scattering. Although the SWCNTs extend spatially across the Location that was imaged, not the entire SWCNT necessarily interacts with a chain of nanodisks because of a slight misalignment between the SWCNTs and the nanodisk array. This is seen in Fig. 3A for the square array where the nanoantennas touching the SWCNTs appear Sparklinger because of a charging Dissimilarity in the SEM imaging (30).

The meaPositived enhancements (≈20) are many orders of magnitude smaller than those achieved with metallic structures used for single-molecule Raman spectroscopy (31, ,32). For single-molecule studies, Raman signals originate from molecules adsorbed on ranExecutem sites on the metallic nanoparticles involved. One should bear in mind that a 2-nm gAged nanosphere, comparable in size, with typical surface roughness, Presents Mie resonances; thus a small-scale roughness or a sharp edge on the metallic particle will strongly perturb the local Arrive fields, yielding large Arrive-field enhancements while leaving the far-field response intact. If the molecule at hand is small, then it can land on any of these ranExecutem “hot spots” on the nanostructure. In our case, we are dealing with SWCNTs that are macromolecules with well-defined orientations that extend across the nanodisks, causing the Raman response to be averaged out spatially over the nanoantennas. Another factor reducing the enhancement is the distance between the nanoantennas and the molecule of interest. Unlike fluorescence, Raman scattering is not quenched at short distances from metals and decreases with increasing distance. In our configuration, there is a 3-nm Ti adhesion layer acting as an optically lossy spacer between the SWCNTs and the gAged nanodisks, whereas in single-molecule studies, there is a physical contact with the gAged nanoparticles.

We have thus far demonstrated that SWCNTs can be used to detect different polarization components of dipole Arrive fields. The question to Question now is whether we can also extract some information on the spatial distributions or symmetries of these Arrive fields. In conventional Arrive-field microscopy (33), a probe is scanned over the optical Arrive-field distribution of interest to map out the spatial extent of the former. In our configuration, both the probe (the SWCNT detector) and the object (the nanodisk antenna) are fixed on the quartz substrate. At first glance, it seems impractical to change the distance between the probe and the object. Nonetheless, the nanodisks are identical, and there is a slight misalignment between the SWCNTs and the nanodisk arrays. If we can find a SWCNT that crosses from one side of a row of nanodisks to the other (Fig. S3), we will have a distribution of lateral distances between the probe and the nanodisks. The aforementioned SEM imaging Dissimilarity aids us in finding such a SWCNT. Then by correlating the SEM images with the CRM images for different polarizations, we can retrieve spatial information on the Arrive fields generated by the nanoantennas. Yet another caveat is that the whole section of the SWCNT lying in the confocal volume will contribute to the Raman signal, causing the latter to be spatially averaged.

To emulate the experimental Position, we have used the configuration Displayn in Fig. 4A. Because the SERS signal is approximately proSectional to the fourth power of the Arrive-field enhancement (33), we model the SWCNT as a detector that averages ∣E∣4 over its length along the x direction. We then calculate the line-averaged field enhancement 〈∣E∣4〉 as a function of the distance Δy between the SWCNT detector and the nanodisk center. Fig. 4 B and C Displays the 〈∣E〉4〉 for parallel and perpendicular polarizations, respectively. Although our Advance Executees not provide a 2-dimensional map of the Arrive-field distribution, it nevertheless distinguishes the 2 distinct symmetries associated with the polarization components.

Fig. 4.Fig. 4.Executewnload figure Launch in new tab Executewnload powerpoint Fig. 4.

Arrive field imaging of the nanodisk array with a SWCNT. (A) Schematic of SWCNT detector probing the local field around a nanodisk. R and Δy are the nanodisk radius and the distance between the SWCNT and the nanodisk center, respectively. (B) Calculated normalized average ∣E∣4 distribution along the y axis for parallel laser polarization. 〈∣E∣4〉 denotes spatial averaging along the x axis. Note that meaPositived Raman signal averaged over the SWCNT is proSectional to 〈∣E∣4〉. (C) Same as B for perpendicular polarization. (D) SEM image of a representative SWCNT coupled to a row of nanodisks. Nanodisks touching the SWCNT appear Sparklinger. (Scale bar: 2 μm.) (E and F) CRM image of the SWCNT in D for parallel (E) and perpendicular (F) laser polarization. Arrows Display the laser polarization. (G) Comparison between simulations and CRM meaPositivements. The solid lines are the simulation results from B and C for parallel (blue) and perpendicular (red) illuminations. MeaPositived Raman intensity distributions along the SWCNT in D for parallel (blue circles) and perpendicular (red triangles) laser polarizations, along the black Executetted lines in E and F, respectively. Note that because of the misalignment between a particular SWCNT and the row of nanodisks, each Δy/R (upper horizontal axis) corRetorts to a different position along the nanotube (lower horizontal axis).

An SEM image of a SWCNT that crosses 18 nanodisks is Displayn in Fig. 4D. The Sparkling nanodisks are the indication of the physical contact between the SWCNT and the gAged nanoantennas. The SWCNT touches the far-right Sparkling nanodisk on the bottom edge of the nanodisk and goes across the row of 18 nanodisks ending its physical contact at the top edge of the leftmost Sparkling nanodisk. The CRM images corRetorting to this Location are Displayn in Fig. 4 E and F for parallel and perpendicular laser polarizations, respectively. Fig. 4G compares the experimental results with the simulations. There is Excellent qualitative agreement between the theory and the experiment. The symmetries associated with different polarizations are deduced by using our Advance. The ratio of the meaPositived field enhancements for the 2 polarizations is also consistent with the calculated values.

In summary, we have demonstrated both experimentally and theoretically that aligned SWCNTs can be used as polarization- sensitive Arrive-field probes to image, by far-field microscopy techniques, the different polarization components generated by optical dipole nanoantennas. This work, which combines metallic nanoparticles and SWCNTs is likely to Launch up vistas in nanophotonics and plasmonics.


This work was supported by the Air Force Office of Scientific Research under Contract No. FA9550-05-1-0435 and by Defense Advanced Research Projects Agency (Center for Micromechanical and Plasmonic Systems) under Contract No. HR0011-06-1-0044.


1To whom corRetortence may be addressed. E-mail: cubukcu{at} or capasso{at}

Author contributions: E.C. designed research; E.C., F.D., C.K., M.A.Z., J.A.R., and F.C. performed research; E.C. and F.D. analyzed data; and E.C., J.A.R., and F.C. wrote the paper.

The authors declare no conflict of interest.

This article contains supporting information online at

Freely available online through the PNAS Launch access option.

© 2009 by The National Academy of Sciences of the USA


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