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Optical control over transmission of terahertz radiation through

arrays of subwavelength holes of varying size

Citation for published version (APA):

Isaac, T. H., Gómez Rivas, J., & Hendry, E. (2009). Optical control over transmission of terahertz radiation through arrays of subwavelength holes of varying size. Physical Review B, 80(19), 193412-1/4. [193412]. https://doi.org/10.1103/PhysRevB.80.193412

DOI:

10.1103/PhysRevB.80.193412

Document status and date: Published: 01/01/2009

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Optical control over transmission of terahertz radiation through arrays

of subwavelength holes of varying size

T. H. Isaac,1 J. Gómez Rivas,2 and E. Hendry1

1School of Physics, University of Exeter, Stocker Road, Exeter EX4 4QL, United Kingdom

2FOM Institute for Atomic and Molecular Physics AMOLF, c/o Philips Research Laboratories, High Tech Campus 4,

5656 AE Eindhoven, The Netherlands

共Received 24 September 2009; revised manuscript received 27 October 2009; published 25 November 2009兲

We modulate the transmission of terahertz共THz兲 radiation through periodic arrays of subwavelength holes in a metallic film by using pulses of visible-wavelength light to photoexcite the semiconducting substrate of the hole arrays. By varying the photodoping level of the semiconductor we are able to switch off the resonant transmission of THz radiation through the array. By varying the size of the holes, we demonstrate the crucial role that surface modes play in the resonant transmission and ultimately in the photomodulation behavior of these structures. We demonstrate that the surface-wave transmission mechanism can allow for very efficient optical modulation of radiation transmission.

DOI:10.1103/PhysRevB.80.193412 PACS number共s兲: 71.45.Gm, 41.20.Jb, 84.40.⫺x

Photonic structures which incorporate some degree of dy-namic control over their electromagnetic properties1,2are

in-teresting for numerous reasons. Some structures have direct applications in proposed photonic devices; in others the dy-namic control can provide direct evidence for transmission pathways and for the role of material properties in determin-ing the behavior of a structure.3Manipulating material

prop-erties optically4–10is of particular interest, as changes to the

structure can be made on the same time scale as the transit of light pulses through the system.

One very fundamental photonic structure is an array of subwavelength holes perforated in a conducting screen. Such arrays can exhibit narrow transmission resonances11 for wavelengths determined by the periodicity of the array—this is known as extraordinary optical transmission or EOT. The mechanisms underlying EOT in these arrays have been the subject of considerable debate,12–14 however consensus has

gradually emerged that for many structures the transmission is mediated at least in part by electromagnetic surface modes at the interface between the perforated conducting screen and the dielectric layers by which it is bound.15,16

In this contribution we use pulses of visible light to modu-late the transmission of terahertz 共THz兲 radiation through periodic arrays of subwavelength holes in a metallic film fabricated at the interface of a substrate of crystalline silicon. By varying the photodoping level of the silicon we are able to switch off EOT of THz radiation through the array. By varying the size of the holes we are able to explain the pho-tomodulation effects in terms of the properties of the surface mode which mediates the enhanced transmission; in particu-lar, we can make a direct link between the lifetime of the surface mode and the magnitude of the photomodulation. We show that if we extend the surface-mode lifetime by mini-mizing losses and reducing the hole size it is possible to attain photomodulation levels which are orders of magnitude greater than those found for a plain silicon surface.

The hole-array structure we shall consider in this work 共Fig. 1兲 is formed from a 150-nm-thick film of gold on a

silicon substrate. The gold is perforated with a square lattice 共pitch 100 ␮m兲 of square subwavelength holes—the holes

have sides ranging in size from 25 to 85 ␮m. Previous works have shown6,17–19 that such hole-array structures

ex-hibit EOT at terahertz frequencies. The mechanism underly-ing the transmission can be considered as a Fano-type picture in which resonances arise from constructive interference be-tween radiation which has been transmitted straight through the holes, and radiation which has been transmitted after coupling to a surface mode on the metal-dielectric interface.16 The frequencies of the EOT resonances

r are

determined by the hole-array lattice pitch d and the permit-tivity of the dielectric substrate, ␧d and are approximately

given by ␯r= ␻r 2␲⬇ c冑i2+ j2 d冑d , 共1兲

where i and j are integers indicating the diffracted order coupling to the surface mode. We determine that the hole arrays under investigation have two EOT resonances in the measured frequency range of 0.4–1.4 THz, labeled as the 具1,0典 and 具1,1典. Both are due to surface modes on the inter-face between the silicon substrate and the gold film共modes on the opposing gold-air interface lie outside the spectral range of the incident terahertz pulse, above 3 THz兲. In this work we chiefly discuss the lowest-frequency 共具1,0典兲 reso-nance as changes to the relative coupling intensity between the higher-order modes are complex and highly dependent on sample geometry.19 The amplitudes and widths of the trans-mission resonances are determined by the lifetime of the sur-face mode mediating the transmission.20 For a hole array

made from lossless materials the lifetime of the surface mode is entirely determined by phase retardation across the width of the holes; i.e., arrays with larger holes exhibit a shorter mode lifetime.19,20 Through photoexcitation of the silicon

surface in these samples one can effectively control this surface-mode-mediated element of the EOT transmission and alter the amplitude of the EOT resonances.6

In Fig. 1共a兲 we show a schematic of the experimental measurement. Two pulses 共both arriving at a repetition rate of 1.05 kHz兲 separated by a 40 ps optical delay illuminate

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the hole-array structure at the air-gold interface. The first pulse to arrive is a 100 fs, 400 nm pump pulse, which pho-toexcites the silicon exposed in the holes关Fig.1共b兲兴. The 400

nm beam is expanded to a circle of 3 cm diameter to ensure that the region of photoexcitation is homogeneous across the 2 cm square-sided sample area. The region of silicon photo-excited is very thin, as the penetration depth of the 400 nm light in the silicon is submicron.21 The relaxation time for photoexcited charge carriers in silicon at room temperature is on the order of microseconds22and so a 40 ps interval after

the arrival of the pump pulse the silicon is in a steady, fully photoexcited state, i.e., we have essentially formed a thin film of extra charge carriers on the silicon interface under-neath the holes. By fitting a Drude response to the measured permittivity of these carriers,23 we determine that our most

intense photoexcitation beam produces a charge density in the silicon of approximately 2.8⫻1024 m−1, corresponding

to a plasma frequency of 30 THz. After the 40 ps interval the THz probe pulse arrives in a 1 cm diameter collimated beam. We detect the terahertz pulse which has transmitted through the sample in the far field using a terahertz spectrometer similar to the one described in Ref.24. In this technique we measure the electric fields of the transmitted terahertz pulses as time-domain spectra;19these can be converted to

transmis-sion intensity spectra by taking the Fourier transform of the time-domain pulses, squaring the field amplitude, and nor-malizing by a reference spectrum.

In Fig.2 we show transmission spectra taken through ar-rays of 45 ␮m holes for varying fluence of the 400 nm pump pulses. The two expected resonances 共具1,0典 and 具1,1典兲 are labeled. As we add an increasing fluence of 400 nm pulses we observe a distinct quenching of transmitted terahertz in-tensity at resonance. The quenching effect at the resonance peak is much higher than the quenching of the nonresonant transmission 共which is dominant at lower frequencies兲. At

the 具1,0典 resonance peak a pump fluence of 0.054 J/m2 re-duces the THz intensity by a factor of 0.69 whereas at 0.6 THz, just below the resonance frequency, transmission inten-sity reduces by a factor of only 0.88. In order to evaluate this enhancement in photomodulation, we can define a photo-modulation ratio, P, as P =共I0− Ipm兲/I0, where I0is the peak

THz transmission intensity with no photoexcitation and Ipm

is the peak THz transmission intensity after 400 nm photo-excitation.

We compare these photomodulation levels directly in Fig.

3共a兲. In this figure we plot the photomodulation ratio P at 0.86 THz 共the peak of the 具1,0典 resonance兲 as a function of the fluence of 400 nm pulses for various hole sizes. As a reference we also evaluate the photomodulation measured for a plain, unstructured silicon surface. We expect the plain silicon surface to exhibit the same amount of photomodula-tion as the nonresonant component of the hole-array trans-mission, as in both cases the transmission pathways can be described by wave vectors perpendicular to the interface. The hole-array structures will introduce surface modes to the transmission—these surface modes have wave vectors

paral-lel to the gold silicon interface. For this reason we expect the

transmission resonances to be more strongly modulated than the transmission through the plain silicon interface; this ef-fect can be seen in Fig.3共a兲as the traces for the hole arrays all lie above that for the unstructured silicon.

In Fig.3共b兲we plot the modulation as a function of hole size for various fluences, as well as for the unstructured sili-con interface. We see a marked increase in the modulation as we decrease the hole size from 85 to 45 ␮m for all fluences, indicating that as we decrease the hole size the surface mode is predominating in the transmission. However, for the very smallest holes, the trend is reversed and the resonant trans-mission for the 25 and 35 ␮m holes is clearly less strongly modulated than for the 45 ␮m holes. In a lossless hole array, one might expect that the photomodulation effect would be greatly enhanced for arrays of very small holes, as the life-time of the surface mode is increased. Indeed, in Fig.3共c兲we plot the results of finite-element numerical modeling25 of

hole arrays on a lossless silicon substrate共blue dashed line兲. This simple, lossless model predicts that P increases mono-tonically upon decreasing the hole size; example transmis-sion spectra shown as an inset in Fig. 3共c兲indicate that we

Photoexcited silicon (~ 125 nm) Silicon substrate 100 µm pitch 40ps delay a d 400nm pump pulse THz probe pulse

Hole array structure (section) Silicon wafer substrate Transmitted THz pulse (a) (b) size aHole 150nm Au film

FIG. 1.共Color online兲 共a兲 Diagram of the experimental measure-ment. A visible pump pulse with center wavelength 400 nm illumi-nates an array of holes in a gold film on substrate of silicon. 40 ps after the arrival of the pump pulse, a probe pulse in the THz range is transmitted through the hole array and subsequently detected in the far field.共b兲 Side profile of the photoexcited structure, indicat-ing the 100 ␮m array pitch and hole size a.

0 . 2 0 0 . 1 5 0 . 1 0 0 . 0 5 0 . 0 0 Tr an sm is si on in te ns it y 1 . 4 1 . 2 1 . 0 0 . 8 0 . 6 0 . 4 F r e q u e n c y ( T H z ) P u m p f l u e n c e ( J / m 2) 0 . 1 9 7 0 . 1 0 7 0 . 0 5 4 0 . 0 1 9 0 < 1 , 0 > < 1 , 1 >

FIG. 2. 共Color online兲 THz transmission spectra through arrays of 45 ␮m holes with various fluences of 400 nm pump beam. Pho-toexcitation quenches the EOT resonances, indicated as the 具1,0典 and具1,1典 peaks.

BRIEF REPORTS PHYSICAL REVIEW B 80, 193412共2009兲

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see a similar resonance-quenching effect upon photoexcita-tion of the silicon substrate as we have observed in the ex-perimental measurement. The nonmonotonic trend of photo-modulation with hole size seen in our experiment is due to intrinsic losses within our silicon substrate; a low concentra-tion of impurity charge carriers in the crystalline silicon con-tribute an imaginary component to the permittivity of the substrate, which reduces the surface-mode lifetime. In the 25 and 35 ␮m holes the surface-mode lifetime is not limited by phase retardation across the holes but instead by absorption in the silicon substrate—this in turn limits the interaction of the surface modes with the photoexcited silicon. By

intro-ducing an imaginary component to the dielectric constant of the silicon substrate in our model of 0.56i at 0.85 THz 共de-termined by phase-resolved THz transmission measurements through the silicon substrate兲 we can accurately reproduce the experimental results as the solid red line in Fig.3共c兲. The model incorporating loss exhibits the nonmonotonic trend in photomodulation with hole size seen in the experiment, and further demonstrates the role of surface-mode lifetime in de-termining the modulation. The modeled modulation for the given fluence is actually slightly higher than that measured in experiment; this is because we do not fully recover the nar-row mode width for transmission through the smallest holes—the instrumental frequency resolution of the terahertz spectrometer is limited by reflections within the silicon substrate.19

Our results suggest that if one could limit the intrinsic losses in an array of very small holes fabricated on a semi-conductor, the photomodulation effect could become ex-tremely efficient. Our modeling in Fig.3共c兲indicates that for an array of 25 ␮m holes on a lossless silicon substrate a fluence of less than 0.2 J/m2 will produce a

photomodula-tion ratio of near unity. This photomodulaphotomodula-tion ratio corre-sponds to the intensity 共I0/Ipm兲 changing by a factor of 600,

compared to a factor of only 1.5 for the unstructured plain silicon surface. If we compare this to other reports of photo-modulation of terahertz in literature using silicon with simi-lar densities of photoexcited charge carriers, a silicon-based photonic crystal structure has been shown10to modulate

tera-hertz intensity by a factor of approximately 12, and a silicon-based waveguide structure26gives an intensity change of 1.4

under a continuous-wave excitation. In our lossy experimen-tal system, the maximum intensity change attained共with the 55 ␮m hole array兲 is a factor of 2.6, very comparable with other measured photomodulation measurements in hole-array structures.4,6In order to approach the modeled factor of 600

one would need to reduce the levels of scattering and loss in the system—this can be achieved by using ultrahigh-purity semiconductor substrates and cooling to cryogenic temperatures.19 Additionally, the photoexcited carrier

life-time in silicon is relatively long; for modulation by a pseudocontinuous-wave light source this long carrier lifetime is useful, as one can build up a high carrier density with a relatively weak light source. However, in pulsed applications the long lifetime imposes a maximum repetition rate of switching. This constraint could be avoided by using direct band-gap semiconductors such as GaAs instead of silicon.8

In conclusion, we have shown how photomodulation of the EOT in our hole-array structures is governed by the ef-fects of surface-mode propagation. By adding a metal hole-array structure to the surface of a silicon substrate we are able to enhance the response of the silicon to photoexcita-tion. In particular, we find that when surface-mode lifetime is limited 共such as by intrinsic loss in the substrate兲 the photo-modulation enhancement is similarly limited. However our modeling shows that by following the strategies for loss re-duction and increasing the surface-mode lifetime extremely high efficiencies for optical modulation could be achieved using this scheme. Such efficient optical modulators could find applications as nonlinear switches in optical circuitry and related systems.

0 . 2 0 0 . 1 5 0 . 1 0 0 . 0 5 0 . 0 0 P u m p b e a m f l u e n c e ( J / m 2) 0 . 6 0 . 4 0 . 2 0 . 0 Ph ot om od ul at io n ra tio (P ) H o l e s i z e s3 5 µ m 4 5 µ m 8 5 µ m S i l i c o n 1 . 0 0 . 8 0 . 6 0 . 4 0 . 2 0 . 0 Ph ot om od ul at io n ra tio (P ) 2 5 3 5 4 5 5 5 6 5 7 5 8 5 H o l e s i z e ( µ m ) N u m e r i c a l m o d e l w i t h : N o l o s s L o s s Si lic on re fe re nc e 1 . 0 0 . 8 0 . 6 0 . 4 0 . 2 0 . 0 Ph ot om od ul at io n ra tio (P ) 2 5 3 5 4 5 5 5 6 5 7 5 8 5 H o l e s i z e ( µ m ) P u m p f l u e n c e ( J / m 2) 0 . 1 9 7 0 . 1 5 6 0 . 1 0 7 0 . 0 6 9 0 . 0 5 4 0 . 0 2 7 0 . 0 1 9 0 Si lic on re fe re nc e a ) b ) ( c ) 0 . 6 0 . 4 0 . 2 0 . 0 T ra ns m iss io n in te ns ity 0 . 8 8 0 . 8 6 0 . 8 4 0 . 8 2 F r e q u e n c y ( T H z ) F l u e n c e 0 . 1 9 7 J / m 2 0

FIG. 3. 共Color online兲 共a兲 Photomodulation versus fluence of 400 nm pump pulses for three sizes of hole and a reference surface of silicon. 共b兲 Experimentally measured photomodulation vs hole size for various fluence of 400 nm pump pulses. For the 25 ␮m holes it was not possible to measure photomodulation for the lowest fluences due to the low level of transmitted THz signal.共c兲 Numeri-cally modeled photomodulation of the THz transmission at reso-nance as a function of hole size at a 400 nm pump fluence of 0.197 J/m2, with and without loss in the silicon substrate. Inset:

Modeled transmission spectra through 55 ␮m holes in a lossless substrate, with and without photoexcitation.

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T.H.I. and E.H. acknowledge the support of the EPSRC 共U.K.兲; E.H. also acknowledges the RCUK 共U.K.兲. This work is part of the research program of the Stichting voor Fundamenteel Onderzoek der Materie 共FOM兲, which is

financially supported by the Nederlandse organisatie voor Wetenschappelijk Onderzoek共NWO兲 and is part of an indus-trial partnership program between Philips and FOM.

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25We model the hole array using the Ansoft HFSS v.11

finite-element modeling package, approximating the gold layer as per-fect electrical conductor, modeling the silicon as a dielectric with complex permittivity of ␧s= 11.85+ 0.56i. We model the photoexcited silicon as a 125-nm-thick region in the substrate immediately below the hole, with a dielectric function deter-mined through phase-resolved direct transmission measurements of the photoexcited silicon. We define the modulation P in the same way as for the experimental measurements, P

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BRIEF REPORTS PHYSICAL REVIEW B 80, 193412共2009兲

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