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Improved analytical fit of gold dispersion: Application to the modeling of extinction spectra

with a finite-difference time-domain method

Alexandre Vial,* Anne-Sophie Grimault, Demetrio Macas, Dominique Barchiesi, and Marc Lamy de la Chapelle

Laboratoire de Nanotechnologie et dInstrumentation Optique - CNRS FRE 2671, Universit de Technologie de Troyes,

12 rue Marie Curie, BP-2060 F-10010 Troyes Cedex, France

sReceived 13 July 2004; revised manuscript received 14 October 2004; published 23 February 2005d

We propose an accurate description for the dispersion of gold in the range of 1.242.48 eV. We implement

this improved model in an FDTD algorithm and evaluate its efciency by comparison with an analytical

method. Extinction spectra of gold nanoparticle arrays are then calculated.

I. INTRODUCTION vD2

e Ds v d = e ` , s1d

The employment of the nite-difference time-domain v s v + i g Dd

sFDTDd method in the study of different electromagnetic

where vD is the plasma frequency and gD is the damping

phenomena has raised constantly increasing interest over the

coefcient. Nevertheless, if frequencies within the range of

past 15 years. Since then, an extensive number of references

the visible spectrum are required for a specic study, the

describing the principles of the method have been published;

model in Eq. s1d may not be complete enough to provide

see, e.g., Refs. 1 and 2. Also, a wide variety of software

accurate results. To illustrate this fact, we try to t the rela-

based on this technique has been developed and is commer-

tive permittivity of gold eJC, tabulated by Johnson and

cially, and noncommercially, available elsewhere.

Christy12 through the optimization of e`, vD, and gD for

Due to the fact that accurate results for a full spectrum

energies between 1.24 and 2.48 eV swavelengths between

can be obtained in a single run of the program, the FDTD has

500 and 1000 nmd. In order to determine the best set of

proven to be well adapted for different kinds of spectro-

parameters, we dene a tness function ssometimes called an

scopic studies.3 Nevertheless, a strong limitation is the re-

objective functiond F as

quirement of an analytical model of dispersion. Typical

laws used for FDTD simulations are the Debye, Lorentz, or

Drude dispersion models.36 Also, a modied Debye law can

F= o

v

hRefeJCsv jd eDsv jdgj2 + hImfeJCsv jd eDsv jdgj2 ,

j

be used.7 At least in principle, any dispersion law could be

s2d

described in terms of a linear combination of Debye and

Lorentz laws.2 Surprisingly, this property has not been used where v j are the discrete values of the frequency v

in studies using the FDTD method. Rather, it has been suc- = 2pc / l for which the permittivity is calculated. The real

cessfully applied to the description of optical functions for 11 and imaginary parts of a complex value z are, respectively,

metals over a wide spectrum,8 or to a calculation of the re- Reszd and Imszd. The minimization of F is performed em-

ectance of single wall nanotubes.9 In this paper, we will ploying the simulated annealing procedure described in Ref.

employ a scheme similar to the one that appears in this last 13, and results are presented in the rst row of Table I.

reference for the study of the optical response of gold nano- The real and imaginary parts of the permittivity eDsvd,

structures. calculated with the Drude model, are, respectively, plotted

The structure of this work is as follows. In Sec. II, we with a dotted line in Figs. 1 and 2.

show the results obtained from the implementation of two It can be seen that neither ReseJCd nor ImseJCd are well

classic dispersion models employing the FDTD method. In described for energies above 2.2 and 1.9 eV, respectively. To

order to validate the numerical approaches, we apply them to emphasize this difference, we also plot in Figs. 1 and 2 the

the case of a simple structure and compare the results with relative errors on ReseDd and ImseDd. The existence of a

those obtained using the analytical method described in Ref. strong discrepancy for energies above 1.9 eV when using the

10. In Sec. III, we employ our FDTD-based implementation single Drude model is evident.

of the Drude-Lorentz model to the calculation of extinction Due to the inability of the Drude model to describe the

spectra. In Sec. IV, we present our main conclusions and permittivity of metals over a wide range of frequencies,

nal remarks. some of the authors working with the FDTD restrict their

studies to a zone of the spectrum where the Drude model is

II. MODELS OF DISPERSION valid sRef. 7 for a gold tip, Refs. 14 and 15 for silver and

aluminum structures; it should be noted that for these two

A. The Drude model

metals, the Drude model alone works well for the optical

It is well known that in the near infrared, the relative wavelengthsd. Others try to t the permittivity in the range of

permittivity of several metals can be described by means of interest by modifying the values of the parameters e`, vD,

the Drude model,11 and gD of the model, as shown in Ref. 5 for the case of silver

VIAL et al. PHYSICAL REVIEW B 71, 085416 s2005d

TABLE I. Values of the parameters used for the optimization of the Drude and the Drude-Lorentz models.

The value of the tness function is given in the last column.

Drude-Lorentz 5.9673 2113.6 15.92 650.07 104.86 1.09 14.521

reference, Drude parameters are actually adapted for several eDLsvd = e` 2 , s3d

vsv + igDd sv VL2 d + iGLv

particular wavelengths.

One way to overcome the limitations of the Drude model where VL and GL, respectively, stand for the oscillator

could be to split the spectrum in several zones and use a strength and the spectral width of the Lorentz oscillators, and

different set of parameters for each of these parts in order to De can be interpreted as a weighting factor.

get the best t. However, a drawback of this solution is that In order to nd the best set of parameters and the best t

a whole new computation is required for each set of param- of eJCsvd, we employ the same optimization scheme as we

eters. did for the Drude model. The new parameters are presented

in the second row of Table I.

B. Extended Drude model In order to facilitate the comparison with the results ob-

tained employing the single Drude model, we depict with a

Another way to overcome the limitations of the Drude solid line in Figs. 1 and 2 the real and imaginary parts cal-

model for gold in the 1.242.48 eV range, and also to take culated with the Drude-Lorentz model. The agreement be-

into account the interband transitions, is suggested in Ref. tween the experimental values and the ones described by Eq.

11. It consists in the addition of one or several Lorentzian s3d is quite good for the whole spectrum. The initial discrep-

terms to Eq. s1d. This approach was used in Ref. 8, where ancies present for energies above 1.9 eV, when using the

ve Lorentzian terms were added in order to t the permit- Drude model, have been removed. This effect is illustrated

tivity of 11 metals for energies between 0.1 and 5 eV. Nev- further when we plot the relative errors on ReseDLd and

ertheless, as the authors acknowledge themselves, the Drude- ImseDLd.

Lorentz model does not t very well experimental values The improved law of dispersion in Eq. s3d is now imple-

around 2 eV for gold, even with additional terms. Moreover, mented in our FDTD code through the recursive convolution

we aim to implement our improved dispersion law in an method described in Ref. 1 for validation. Details on the

FDTD code, and the memory requirements increase linearly numerical implementation are given in an Appendix at the

with the number of terms used for the dispersion law. For end of this paper.

these reasons, we decided to restrict our model of dispersion C. Validation of the new approach

to only one additional Lorentzian term. Thus, we write the

permittivity of gold as In order to evaluate the performance of our approach, we

will compare its results with those obtained employing an

FIG. 1. Real part of the permittivity of gold as published in Ref. FIG. 2. Imaginary part of the permittivity of gold as published

12, calculated with the single Drude model and calculated with the in Ref. 12, calculated with the single Drude model and calculated

Drude-Lorentz model. with the Drude-Lorentz model.

085416-2

IMPROVED ANALYTICAL FIT OF GOLD PHYSICAL REVIEW B 71, 085416 s2005d

FIG. 3. Coefcient of transmission through a layer of 20 nm of

gold, respectively, calculated analytically, with the simple Drude

gold, respectively, calculated analytically, with the simple Drude

model and with the Drude-Lorentz model. The relative error on utu

model and with the Drude-Lorentz model. The relative error on utu

by comparison with the analytical result is also depicted.

by comparison with the analytical result is also depicted.

analytical method. For simplicity, the structure we will con- drawn. In this case, the maximal error achieved when using

sider for our tests consists of a thin layer of gold surrounded the Drude-Lorentz model is 5.2%, and the Drude model per-

by air. We will calculate the coefcient of transmission in forms worse only for energies above 2.34 eV swavelengths

amplitude for the electric eld using the formulas that appear below 530 nmd. If now we still consider the threshold previ-

in Ref. 10 for an absorbing lm on a transparent substrate. ously dened smaximal error of 2.7%d, then the Drude-

In Fig. 3, we present the results obtained considering a Lorentz model can be accepted for energies below 2.39 eV

thin lm of thickness e = 20 nm. The absolute values of the swavelengths greater than 520 nmd, whereas the Drude

transmission coefcients utu, computed through the FDTD model is only acceptable for energies below 1.78 eV swave-

implementations of Drude and Drude-Lorentz models, are, lengths above 697 nmd and in a narrow zone between 2.08

respectively, depicted with a dashed and a thick solid curve. and 2.24 eV s555 and 596 nmd.

The thin solid curve corresponds to the analytical result. The As a last test, we compute the intensity 5 nm above an

values of the permittivity used for the analytical calculation innite gold cylinder of radius 15 nm illuminated with a

are the ones published in Ref. 12 and not the values tted by plane wave, the incident eld being polarized perpendicu-

the Drude-Lorentz model. larly with the axis of the cylinder. Results are compared with

It can be observed in Fig. 3 that the agreement between the Mie theory and presented in Fig. 5. It is conrmed that

the Drude model and the analytical one decreases for ener- the Drude-Lorentz models perform better than the single

gies above 1.8 eV swavelength below 700 nmd. On the other Drude model, which is unable to predict the peak of absorp-

hand, the agreement between the Drude-Lorentz model and tion around 2.4 eV. Nevertheless, the error calculated in this

the analytical one is quite good. This behavior can be visu- case is higher than previously observed, mainly due to the

alized further by plotting the relative error on the values of utu difculty to accurately describe a circle using an orthogonal

for the two models used with the FDTD method. It is obvi- mesh. For this calculation, in order to rene the description

ous from Fig. 3 that the Drude-Lorentz model not only per- of the shape of the cylinder, a spatial discretization of 0.5 nm

forms better than the Drude model, but also that it leads to a was used, instead of 5 nm for the thin-layer cases.

very small error on a wide spectrum. The maximal relative Once we have veried that an improvement can be ob-

error obtained with the Drude-Lorentz model is 2.7%, and if served not only on the description of the permittivity e, but

we consider this value as a threshold for the validity of the also on the calculation of transmission coefcients, we feel

model, the Drude model is only valid for energies below 1.97 condent to apply our new dispersion model to a more com-

eV swavelengths greater than 630 nmd. plicated case, namely the calculation of extinction spectra

According to Figs. 1 and 2, it is clear that the imaginary above gold nanostructures arrays.

part of the permittivity is less well described than the real

one even with the Drude-Lorentz model, thus we can check

results obtained for utu when considering a layer of thickness III. APPLICATION TO THE CALCULATION

e = 50 nm sFig. 4d in order to verify that we still get satisfy- OF EXTINCTION SPECTRA

ing results. It can be seen that both the transmission coef-

cients utu and the relative errors present a behavior analogous Recently, several experimental results obtained with gold

to the one shown in Fig. 3, and similar conclusions can be nanoparticle arrays have been published.1621 Various sizes,

085416-3

VIAL et al. PHYSICAL REVIEW B 71, 085416 s2005d

FIG. 5. Intensity transmitted above a gold cylinder of radius 15 elliptical basis: the height is 60 nm, the grating constant is 300 nm,

nm, respectively, calculated analytically sMie theoryd, with the and the major and minor axes are, respectively, 100 nm and 100 nm

simple Drude model and with the Drude-Lorentz model. The rela- sstructure Ad, 125 nm and 100 nm sstructure Bd, and 150 nm and

tive error by comparison with the analytical result is also depicted. 100 nm sstructure Cd. Calculations performed with the Drude-

Lorentz model are depicted with a thick line. Calculations per-

formed with the Drude model are depicted with a thin line. Peak

shapes, and periodicities are used in order to tune the posi-

positions for structures A, B, and C are, respectively, l = 637 nm,

tion of the extinction, and the inuence of these parameters l = 680 nm, and l = 712 nm with the Drude-Lorentz model, and l

was reviewed in Ref. 22. These experiments are mainly fo- = 637 nm, l = 683 nm, and l = 715 nm for the Drude model.

cused on the development and the improvement of surface

enhanced Raman spectroscopy sSERSd active substrate.

In this section, we will present computations of extinction illuminated from the z , 0 region at normal incidence. The

spectra on two kinds of gold nanoparticle arrays. As most of value of the electric eld is recorded after each time step of

the gures published in previously cited papers show the the calculation on a plane above the particles. Once we have

spectra as a function of the wavelength, the following gures checked that the Gaussian pulse has vanished and that no

will maintain the same convention. electric eld remains in the computing window, we stop the

computation, and it is then straightforward to calculate the

extinction spectrum of the structure by performing a Fourier

A. Geometry of the problem transform of the eld.1,2 The results presented in the follow-

The typical shape of the structures used for SERS experi- ing subsections are computed with spatial discretization Dx

ments is depicted in Fig. 6. It consists of a substrate made of = 5 nm, and the time step Dt is dened as Dt = Dx / s2cd with

glass on which gold nanoparticles are deposited. For our c the speed of light in vacuum.

forthcoming calculations, the incident eld is assumed to be

a plane wave with a Gaussian temporal shape. The sample is

B. Numerical results

an elliptical basis and a height of 60 nm. One of the axes of

the ellipse has a constant length sm = 100 nmd, whereas the

length of the second axis is variable sstructure A: M

= 100 nm; structure B: M = 125 nm; structure C: M

= 150 nmd. The periodicity of the array along the x and y

directions is px = py = 300 nm. The incident light is polarized

along the x axis. The exinction spectra obtained for struc-

tures A, B, and C are plotted in Fig. 7 with thick solid or

dashed curves.

These results are in good agreement with those published

in Ref. 20, where increasing the size of the major axis of the

ellipse induced a strong redshift of the peak. Results ob-

tained with the Drude model are also depicted in Fig. 7 with

FIG. 6. Geometry of the structure studied for the calculation of thin solid or dashed lines. It can be observed that the posi-

the extinction spectrum. tions of the peaks are almost the same, but oscillations are

085416-4

IMPROVED ANALYTICAL FIT OF GOLD PHYSICAL REVIEW B 71, 085416 s2005d

17, as it gives the right direction for the shift of the peak.

The benet of using Eq. s2d instead of the standard Drude

model given in Eq. s1d can be seen by comparing results

obtained with the single Drude model depicted with thin

lines in Fig. 8. Positions of the peaks are still almost the

same, but strong oscillations are present on the left part of

the spectrum for all structures.

IV. CONCLUSION

model, we were able to t the dispersion curve of gold over

a spectrum wider than possible with the single Drude model.

This improved dispersion law was then implemented in a

FDTD code and applied to the calculation of gold nanopar-

ticle arrays extinction spectra. Calculations are in good

agreement with experimental results. When calculations are

FIG. 8. Extinction spectra calculated for gold cylinders: the

made with the original Drude model, only a small shift of the

height is 60 nm, the diameter is 100 nm, and grating contants are,

respectively, 200 nm sstructure Ad, 250 nm sstructure Bd, and 300

absorption peak may be observed for some structures, but

nm sstructure Cd. Calculations performed with the Drude-Lorentz strong oscillations in the spectrum are visible for wave-

model are depicted with a thick line. Calculations performed with lengths below the resonance. This behavior is an indication

the Drude model are depicted with a thin line. Peak positions for that intensities calculated above or inside the metallic struc-

structures A, B, and C are, respectively, l = 625 nm, l = 630 nm, ture would then be wrong, leading to inexact estimations of

and l = 638 nm with the Drude-Lorentz model, and l = 628 nm, l the SERS gain.

= 630 nm, and l = 638 nm for the Drude model. Further work is still required in order to be able to t the

permittivity of gold over the full visible spectrum. This could

present on the spectrum calculated with the Drude model for be achieved by adding at least one more Lorentzian term.

structure A. Moreover, other metals often used for the design of nano-

In the second case, particles are cylinders with a diameter structures, like silver or aluminum, should be studied too.

of 100 nm and a height of 60 nm, and the periodicity of the

array is changed sstructure A: px = py = 200 nm; structure B: ACKNOWLEDGMENTS

px = py = 250 nm; structure C: px = py = 300 nmd. Results are

presented in Fig. 8 with thick solid or dashed lines. D.M. acknowledges Le Ministre de la Jeunesse, de

The behavior of the curves in Fig. 8 is consistent with that lEducation Nationale et de la Recherche as well as the Con-

of the experimental results published in Ref. 17, where a seil Rgional de ChampagneArdennes for nancial support.

small shift to the red was observed when increasing the pe- A.-S. Grimault acknowledges the Conseil Rgional de

riod of the grating. Moreover, our model gives better results ChampagneArdennes for nancial support.

For a three-dimensional computation window, with a spatial discretization Dx and a temporal discretization Dt, we represent

the value of any eld U at position x = iDx, y = jDx, z = kDx and for the instant t = nDt by uUuni,j,k, and the standard recursion

equations in a nondispersive and nonmagnetic medium for the electric and magnetic elds are

Dt n

n+1/2

uHxui1/2,j+1,k+1 n1/2

= uHxui1/2,j+1,k+1 + usE u n

uEyui1/2,j+1,k+1/2 n

+ uEzui1/2,j+1/2,k+1 n

uEzui1/2,j+3/2,k+1 d, sA1d

m0Dx y i1/2,j+1,k+3/2

Dt n

n+1/2

uHyui,j+1/2,k+1 n1/2

= uHyui,j+1/2,k+1 + usE u n

uEzui1/2,j+1/2,k+1 n

+ uExui,j+1/2,k+1/2 n

uExui,j+1/2,k+3/2 d, sA2d

m0Dx z i+1/2,j+1/2,k+1

Dt n

n+1/2

uHzui,j+1,k+1/2 n1/2

= uHzui,j+1,k+1/2 + usE u n

uExui,j+1/2,k+1/2 n

+ uEyui1/2,j+1,k+1/2 n

uEyui+1/2,j+1,k+1/2 d, sA3d

m0Dx x i,j+3/2,k+1/2

Dt n+1/2

n+1

uExui,j+1/2,k+1/2 n

= uExui,j+1/2,k+1/2 + usHzui,j+1,k+1/2 uHzui,j,k+1/2

n+1/2 n+1/2

+ uHyui,j+1/2,k n+1/2

uHyui,j+1/2,k+1 d, sA4d

e0ei,j+1/2,k+1/2Dx

085416-5

VIAL et al. PHYSICAL REVIEW B 71, 085416 s2005d

Dt n+1/2

n+1

uEyui1/2,j+1,k+1/2 n

= uEyui1/2,j+1,k+1/2 + usHxui1/2,j+1,k+1 uHxui1/2,j+1,k

n+1/2 n+1/2

+ uHzui1,+1j,k+1/2 n+1/2

uHzui,j+1,k+1/2 d,

e0ei1/2,j+1,k+1/2Dx

sA5d

Dt n+1/2

n+1

uEzui1/2,j+1/2,k+1 n

= uEzui1/2,j+1/2,k+1 + usHyui,j+1/2,k+1 uHyui1,j+1/2,k+1

n+1/2 n+1/2

+ uHxui1/2,j,k+1 n+1/2

uHxui1/2,j+1,k+1 d.

e0ei1/2,j+1/2,k+1Dx

sA6d

Eq. s3d, we need to introduce two new vector elds CD and xL0 = i s1 esa+ibdDtd, sA12d

a ib

CL known as recursive acumulators and Eqs. sA4dsA6d

have to be replaced by the following three equations:

g

r

uCDun = uCD d n

CDun1 + uCD Eu , sA7d DxL0 = i s1 esa+ibdDtd2 . sA13d

a ib

uCLuni = uCLr CLun1 + uCLd Eun , sA8d Coefcients CLr and CLd can now be written as

CLr = esa+ibdDt , sA14d

uEun+1 = uCaEun + Cb 3 Hn+1/2 + Cg ResuCDun + uCLund,

sA9d CLd = DxL0 . sA15d

where the coefcients Ca, Cb, Cg, Cd, and Cr depend on the Finally, we dene x0 = xD0 + ResxL0 d, and the last three co-

coefcients of Eq. s3d. efcients needed are

0

For the Drude term, we dene de = svD / gDd2, xD

0 2 e`

= des1 egDDtd, DxD = des1 egDDtd2, and sD = vD / gD. Then Ca = , sA16d

the coefcients CD r d

and CD are dened as e` + x0 + sDDt

r

CD = egDDt , sA10d Dt

Cb = , sA17d

d 0

Dxe0se` + x0 + sDDtd

CD = DxD . sA11d

For the Lorentz term, we rst dene a = GL / 2, b 1

Cg = . sA18d

= VL2 a2, and g = DeVL2 / b. Then we dene e` + x0 + sDDt

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085416-7

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