# A simple formula for the L-gap width of a face-centered-cubic photonic crystal

## I Introduction

The propagation of light in a periodic dielectric medium has recently attracted much attention due to the possibility of opening a gap in the spectrum of electromagnetic waves for both polarizations and all directions of the incident waves . In such a medium, the density of states (DOS) can be, in a certain frequency interval, either reduced down to zero (photonic band gap) or enhanced with respect to the vacuum case. The changes in the DOS affect various physical quantities. The most transparent is the change in the spontaneous emission rate of embedded atoms and molecules which may have applications for semiconductor lasers, heterojunction bipolar transistors, and thresholdless lasers  or to create new sources of light for ultra-fast optical communication systems.

Existence of the full photonic band gap was first demonstrated at microwaves . Recently, thanks to the intense experimental effort, we have witnessed a significant progress in fabrication of complete photonic-bandgap structures at near-infrared . In two dimensions, complete photonic-bandgap structures have been fabricating for TM polarization . In three dimensions, a promissing structure has been fabricated by Sandia’s group . Nevertheless, in one direction this structure extends less than two unit cells and there is ongoing experimental search to improve its properties. One of the most promising candidates to achieve a complete photonic bandgap at optical wavelengths and fabricate large enough structures at near-infrared wavelengths are collodial systems of microspheres. Indeed, the latter can self-assemble into three-dimensional crystals with excellent long-range periodicity with the lattice constant well below infrared scale . This long-range periodicity gives rise to strong optical Bragg’s scattering clearly visible by the naked eye and already described in 1963 . Monodisperse collodial suspensions of microspheres crystalize either in a face-centered-cubic (fcc)  or (for small sphere filling fraction) in a body-centered-cubic (bcc) lattice . Using suspensions of microspheres of different sizes one can also prepare crystals with a complex unit cell (containing more than one scatterer). Both the case of “dense spheres”  and “air spheres”  when the dielectric constant of spheres $`\epsilon _s`$ is greater and smaller than the dielectric constant $`\epsilon _b`$ of the background medium, respectively, can be realized experimentally. There is a significant difference between the two cases, since, according to numerical calculations, simple dielectric lattices of homogeneous spheres  in air do not exhibit a full photonic band gap, while for air spheres a full band gap can open for a simple fcc lattice . Unfortunately, the required dielectric contrast $`\delta =\mathrm{max}(\epsilon _s/\epsilon _b,\epsilon _b/\epsilon _s)`$ for opening the full band gap, either $`\stackrel{>}{}8.4`$ obtained using the plane wave method , or, $`\stackrel{>}{}8.13`$ obtained by the photonic analoque of the Korringa-Kohn-Rostocker (KKR) method , is currently out of experimental reach at optical and near-infrared frequencies for photonic colloidal structures. The absence of a full gap in this frequency range in currently available collodial crystals of homogeneous and single size spheres does not mean the absence of interesting physics in this weak photonic region. For example, the change in the spontaneous emission rate of dye molecules in an fcc collodial crystal can be observed already at a relatively low $`\delta 1.2`$ .

In contrast to the full gap, Bragg’s reflection can be observed for arbitrarily small $`\delta `$ as long as a sample has sufficient long-range periodicity. Analysis of Bragg’s scattering might not only be useful to understand the physics of photonic crystals, but it has already found practical application in distributed feedback lasers in the visible region of the spectrum . The first Bragg’s peak can be characterized by the width of the (lowest) stop gap (gap at a fixed direction of the incident light) at a certain point on the boundary of the Brillouin zone. We focus here on the case of a simple fcc lattice of air spheres , which is among the most promising candidates to achieve a full photonic band gap. For an fcc lattice, it is convenient to consider Bragg’s scattering in the (111) direction which corresponds to the L direction of the Brillouin zone (see  for the classification of special points of three-dimensional lattices). Apart from numerous experimental data now available , there are at least two other reasons for this choice. First, the width of the first stop gap takes on its maximum at the L point and, second, experimental techniques make it possible to allow one to grow collodial crystals such that the L direction corresponds to normal incidence on the crystal surface.

Let $`\epsilon (𝐫)`$ be the dielectric constant of an fcc photonic crystal. One has $`\epsilon (𝐫)=\epsilon _s`$ if $`𝐫`$ is inside the sphere and $`\epsilon (𝐫)=\epsilon _b`$ otherwise. Let $`f`$ be the sphere filling fraction, i.e., volume of the sphere(s) in the unit cell per unit cell volume. Once $`f`$ is fixed, the spectrum is only a function of the dielectric contrast $`\delta `$. By a suitable rescaling, one can always set $`\epsilon _s=1`$ for the case of “air” spheres ($`\epsilon _b=1`$ for the case of “dense” spheres). As $`\delta `$ and $`f`$ are varied, both the absolute L-gap width $`\mathrm{}_L`$ and the L-midgap frequency $`\nu _c`$ change. As a function of $`\delta `$, $`\mathrm{}_L(\delta )`$ takes on its maximum at some $`\delta =\delta _m(f)`$ while $`\nu _c(\delta )`$ monotonically decreases. We address the question of whether the width $`\mathrm{}_L`$ can be understood in terms of simple quantities, namely, the volume averaged dielectric constant,

$$\overline{\epsilon }=f\epsilon _s+(1f)\epsilon _b,$$

the volume averaged $`\epsilon ^2(𝐫)`$,

$$\overline{\epsilon ^2}=[f\epsilon _s^2+(1f)\epsilon _b^2],$$

and the effective dielectric constant $`\epsilon _{eff}`$. The latter characterizes optical properties of the crystal in the long-wavelength limit and is (theoretically) determined by the slope of the linear part of the band structure, $`\epsilon _{eff}^{1/2}=lim_{k0}d\omega /(cdk)`$. Note that due to the vector character of electromagnetic waves, $`\epsilon _{eff}`$ differs from $`\overline{\epsilon }`$, in contrast to the scalar case where $`\epsilon _{eff}=\overline{\epsilon }`$ . One can show that for any $`f`$, $`\epsilon _b`$, and $`\epsilon _s`$,

$$\epsilon _{eff}\overline{\epsilon }\sqrt{\overline{\epsilon ^2}}.$$
(1)   
Equality in (1) occurs if and only if either $`f=0`$ or $`f=1`$, or, if $`\delta =1`$, i.e., if $`\epsilon _b=\epsilon _s`$. The effective dielectric constant can be well approximated  by Maxwell-Garnett’s formula ,

$$\epsilon _{eff}\epsilon _{eff}^{MG}=\epsilon _b(1+2f\alpha )/(1f\alpha ),$$
(2)   
where, for a homogeneous sphere, the polarizability factor $`\alpha =(\epsilon _s\epsilon _b)/(\epsilon _s+2\epsilon _b)`$. Note, however, that in the case of air (dense) spheres $`\epsilon _{eff}^{MG}`$ slightly overestimates (underestimates) the exact value of $`\epsilon _{eff}`$ as calculated from the band structure .

## II Results

Obtaining exact analytic results for dielectric lattices turns out to be notoriously difficult and numerics has been the main tool to understand photonic gaps so far . A simple analytical formula, if any, may be a good starting point for obtaining a better insight into the problem. It was rather surprising to find out that such a formula can be found for the L-gap width $`\mathrm{}_L`$. Namely, in the case for air spheres, $`\mathrm{}_L`$ can be approximated by the formula (see Fig. 1)

$$\mathrm{}_LCg=C\left(\sqrt{\overline{\epsilon ^2}}\epsilon _{eff}\right)^{1/2}/\overline{\epsilon }.$$
(3)   
For a given filling fraction $`f`$, the constant $`C=C(f)`$ was determined by taking the average over $`\mathrm{}_L/g`$ where $`\mathrm{}_L`$ is the L-gap width calculated numerically using a photonic analogue  of the KKR method . The latter method gives results which are in excellent agreement with experimental values .

Apparently, for sufficiently high $`\delta \delta _m(f)`$, our formula captures the asymptotic behaviour of the absolute gap width $`\mathrm{}_L`$ exactly. The standard deviation $`\sigma `$ steadily decreases well below $`1\%`$ as one investigates region $`\delta \delta _c`$ for higher and higher $`\delta _c`$. For $`\delta 20`$ one has $`\sigma <0.1\%`$ for $`f=0.2`$, $`\sigma <0.4\%`$ for $`f=0.1`$, and $`\sigma <0.3\%`$ for $`f=0.4`$ (see, for example, Fig. 1). For $`\delta 36`$ and $`f=0.6`$, $`\sigma <0.5\%`$, while for the close-packed case, $`\sigma 1\%`$. If, however, in the latter case $`\delta 50`$, $`\sigma `$ drops below $`0.7\%`$.

For $`\delta (1,100]`$, our formula (3) still describes $`\mathrm{}_L`$ with a reasonable accuracy ranging from $`3.3\%`$ to $`6.5\%`$ (depending on the filling fraction). The values of $`C`$, their standard quadratic deviation $`\sigma `$, and the relative error $`\sigma _r=\sigma /C`$ are shown in Tab. I. Approximately thirty values of the dielectric contrast within the interval $`\delta (1,100]`$ were taken for every filling fraction considered. For a given filling fraction, the main part of the error is picked up

TABLE I. The values of $`C`$, their standard quadratic deviation $`\sigma `$, and the relative error $`\sigma _r=\sigma /C`$ for different filling fractions and $`\delta (1,100]`$.

|  | $`f=0.1`$ | $`f=0.2`$ | $`f=0.4`$ | $`f=0.6`$ | $`f=0.74`$ |
| --- | --- | --- | --- | --- | --- |
| $`C`$ | 0.762 | 0.868 | 0.875 | 0.808 | 0.736 |
| $`\sigma `$ | $`0.031`$ | $`0.03`$ | $`0.029`$ | $`0.038`$ | $`0.048`$ |
| $`\sigma _r`$ | $`4.1\%`$ | $`3.4\%`$ | $`3.3\%`$ | $`4.7\%`$ | $`6.5\%`$ |

around $`\delta =\delta _m(f)`$ for which $`\mathrm{}_L`$ takes on its maximum. At the maximum of the L-gap width $`\mathrm{}_L`$ our formula (3) gives persistently a slightly lower value for $`\mathrm{}_L`$. Note that for moderate $`\delta `$ Maxwell-Garnett overestimates $`\epsilon _{eff}`$ for the case of air spheres . Therefore, using the exact $`\epsilon _{eff}`$ may reduce errors further.

According to Tab. I, the quantity $`C`$ shows a weak dependence on $`f`$ which can be approximated with high accuracy (relative error 2.5%) by the formula

$$C(f)=C_0+0.14f(2f_mf)/f_m^2.$$
(4)   
Here $`C_00.74`$ is the minimal value of $`C`$ and $`f_m`$ is the filling fraction for which $`C`$ takes on its maximal value. Table I indicates that $`C`$ takes on its minimal value $`C_0`$ at the extreme filling fractions $`f=0`$ and $`f=0.74`$, and its maximal value is $`C_m0.88`$ at $`f_m0.74/2`$. The factor $`0.14`$ in the interpolation formula (4) is the difference $`C_mC_0`$. Using $`C(f)`$ in (3) does not raise the relative error $`\sigma _r`$ more than $`0.4\%`$ for intermediate filling fractions. Fig. 1 shows approximations to the L-gap width for $`f=0.4`$ using formula (3) with optimized $`C`$ taken from Tab. I and with $`C(f)`$ given by the formula (4). As the dielectric contrast $`\delta `$ increases, $`\mathrm{}_L`$ first increases to its maximal value and then slowly decreases as $`\delta ^{1/2}`$. This behavior is well reflected by our formula (3) which in the limit $`\delta 1`$ yields

$$\mathrm{}_LC(f)\frac{2}{\sqrt{(1f)(2+f)}}\left(\frac{2+f}{2\sqrt{1f}}1\right)^{1/2}\delta ^{1/2}.$$
(5)   
Since the L-midgap frequency $`\nu _c`$ changes as $`f`$ and $`\delta `$ are varied, an invariant characteristic of Bragg’s scattering is provided by the relative L-gap width

$$\mathrm{}_L^r=\mathrm{}_L/\nu _c.$$

$`\mathrm{}_L^r`$ increases monotonically as $`\delta `$ increases (see Fig. 3) and saturates very fast for $`\delta >\delta _m`$. Our observation here is that the L-midgap frequency $`\nu _c`$ can be well approximated by

$$\nu _cck_L/(2\pi n_{eff}^{MG}),$$
(6)   
where $`n_{eff}^{MG}=\sqrt{\epsilon _{eff}^{MG}}`$ and $`k_L`$ is the length of the Bloch vector at the L point. In units where the length of the side of the conventional unit cell of the cubic lattice  is $`A=2`$, one has $`k_L/\pi =\sqrt{0.75}`$. Recent measurements of $`\nu _c`$ for moderate $`\delta `$  agree well with formula (6) (see also Fig. 2). For all filling fractions considered $`\delta `$ within the range and $`1\delta 100`$, the maximal deviation of the L-midgap frequency given by formula (6) is less than $`8\%`$ with respect to the exact value. Therefore, the formula

$$\mathrm{}_L^r2\pi n_{eff}^{MG}\mathrm{}_L/k_L$$
(7)   
is a natural candidate to describe $`\mathrm{}_L^r`$. However, as shown in Fig. 2, formula (6) systematically overestimates the exact value of $`\nu _c`$ by a little bit. This systematic error is also apparent from Fig. 4. Due to the systematic error, the relative L-gap width $`\mathrm{}_L^r`$ is described by the formula (7) with a slightly larger relative error than is $`\mathrm{}_L`$ by the formula (3). There are now two main contributions to the errors, one around the maximum of $`\mathrm{}_L`$ and the other due to the systematic error. However, in the asymptotic region $`\delta \delta _m`$ the first contribution disappears whereas the systematic error saturates (see Fig. 2). As a result, in the asymptotic region, the relative error $`\stackrel{~}{\sigma }_r`$ is still within $`1\%`$. Fig. 4 shows that even at $`\delta =100`$ the error in $`\mathrm{}_L^r`$ is less than $`2\%`$.

For $`\delta (1,100]`$, our formula (3) still describes $`\mathrm{}_L`$ with a reasonable accuracy ranging from 4.1% to 8% (depending on the filling fraction) For a given filling fraction, the relative error $`\stackrel{~}{\sigma }_r=\stackrel{~}{\sigma }/\overline{R}`$ was determined by calculating the standard quadratic deviation $`\stackrel{~}{\sigma }`$ of the average value $`\overline{R}`$ of the ratio $`R=\mathrm{}_L^{r;exact}/\mathrm{}_L^{r;approx}`$, where $`\mathrm{}_L^{r;exact}`$ is the exact value of $`\mathrm{}_L^r`$ calculated numerically and $`\mathrm{}_L^{r;approx}`$ is its approximation calculated using Eq. (7). The values of $`\overline{R}`$, $`\stackrel{~}{\sigma }`$, and $`\stackrel{~}{\sigma }_r`$ are collected in Table II.

TABLE II. The average value $`\overline{R}`$, the standard quadratic deviation $`\stackrel{~}{\sigma }`$, and the relative error $`\stackrel{~}{\sigma }_r`$ for $`\mathrm{}_L^r`$ approximated by Eq. (7) for different filling fractions and $`\delta (1,100]`$.

|  | $`f=0.1`$ | $`f=0.2`$ | $`f=0.4`$ | $`f=0.6`$ | $`f=0.74`$ |
| --- | --- | --- | --- | --- | --- |
| $`\overline{R}`$ | $`1.004`$ | $`1.012`$ | $`1.025`$ | $`1.030`$ | $`1.031`$ |
| $`\stackrel{~}{\sigma }`$ | $`0.044`$ | $`0.042`$ | $`0.052`$ | $`0.068`$ | $`0.082`$ |
| $`\stackrel{~}{\sigma }_r`$ | $`4.37\%`$ | $`4.17\%`$ | $`5.05\%`$ | $`6.61\%`$ | $`7.95\%`$ |

One expects a deviations \[of the order $`5\%`$ from the behavior described by the formula (7)\] only in a rare case when a Mie resonance crosses the edge of the L-gap .

## III Discussion

Formulas (3) \[together with (4)\], (6), and (7) are the main results of this work. They fit nicely experimental data on Bragg’s scattering in fcc photonic crystals of air spheres . Note that $`\mathrm{}_L`$ also characterizes the transmission of light through such a crystal (see  for microwaves). The fact that such simple relations can describe one of the photonic gaps has been completely unexpected. Indeed, the numerical calculation of photonic band structures is a great deal more involved than that in the case of scalar waves (including the case of electrons) where no analog of formulas (3) and (7) is known. Numerics has been the main tool to understand photonic gaps . This is also the case of two recent discussions of Bragg’s scattering in the (111) direction . A previous attempt to understand Bragg’s scattering in photonic crystals involved an introduction of a “photonic strength” parameter $`\mathrm{\Psi }=3f\alpha `$ . It was shown that the dynamical diffraction theory , which is well known in x-ray diffraction, already fails to describe Bragg’s scattering in a photonic crystal for $`\mathrm{\Psi }0.5`$ .

Formulas (3) and (7) immediately raise questions whether one can understand and derive them analytically. The L-gap width for fcc structures is a natural measure to characterize their scattering strength, because, in contrast to the full band gap, $`\mathrm{}_L0`$ for arbitrarily small $`f`$ and $`\delta `$. The latter suggests to take $`\mathrm{}_L^r`$ given by Eq. (7) as a natural “photonic strength” parameter for the air spheres case. Neither the parameter $`\mathrm{\Psi }`$ , nor the parameter $`\epsilon _r=\left(\overline{\epsilon ^2}\overline{\epsilon }^2\right)^{1/2}/\overline{\epsilon },`$ introduced in , are directly related to a gap width. However, it turns out that formulas (3) and (7) cannot be applied to the case of dense spheres. The simple fcc lattices of air and dense spheres have for the same dielectric contrast rather different behavior with respect to the full photonic band gap  and to the first Bragg’s peak . Our numerical calculation shows that, for dense spheres, $`\mathrm{}_L^r`$ does not increase monotonically with $`\delta `$ as in the case of air spheres. Instead $`\mathrm{}_L^r`$ first reaches a local maximum, then it returns to zero and only afterwards starts to increase monotonically . This behavior is reminiscent to that of the relative X-gap width $`\mathrm{}_X^r`$ (X is another special point of the Brillouin zone of an fcc lattice ) in the case of air spheres . It has been argued that the vanishing of $`\mathrm{}_X^r`$ is due to the vanishing of the scattering form-factors . Also, if $`\mathrm{}_L^r`$ is plotted against the filling fraction, one observes that the maximum of $`\mathrm{}_L^r`$ shifts to lower $`f`$ for dense spheres and towards close-packing for air spheres . It would be interesting to understand what causes this different behavior. The latter can be partially attributed to the fact that, for a lattice of spheres, $`\epsilon _b`$ no longer describes the dielectric constant of the surrounding medium, which is instead described by the effective dielectric constant $`\epsilon _{eff}`$. Therefore, the bare dielectric contrast $`\delta `$ is renormalized to $`\delta _{eff}=\mathrm{max}(\epsilon _s/\epsilon _{eff},\epsilon _{eff}/\epsilon _s)`$, where $`1<\epsilon _{eff}<\delta `$ for $`\epsilon _s\epsilon _b`$. Given the bare dielectric contrast $`\delta `$, one finds that the renormalized dielectric contrast $`\delta _{eff}^d=\epsilon _s/\epsilon _{eff}`$ in the case of dense spheres is always smaller than the renormalized dielectric contrast $`\delta _{eff}^a=\epsilon _{eff}`$ in the case of air spheres . The latter is easy to verify in the limit when the bare dielectric contrast $`\delta `$ tends to infinity, where the Maxwell-Garnett equation (2) implies

$$\delta _{eff}^d\delta (1f)/(1+2f)<\delta _{eff}^a\delta (1f)/(1+f/2).$$
(8)   
Nevertheless, a full understanding of the differences between the lattices of air and dense spheres still remains a theoretical challenge.

## IV Conclusion

To conclude we have found that, despite of the complexity of the problem of propagation of electromagnetic waves in a periodic dielectric medium, the absolute and the relative width of the first Bragg’s peak in the (111) direction for an fcc lattice of air spheres can be accurately described by the simple empirical formulas (3) and (7), respectively. Apparently, for sufficiently high $`\delta 1`$, our formula (3) captures the asymptotic behaviour of $`\mathrm{}_L`$ exactly. Indeed, the relative error $`\sigma _r`$ steadily decreases as one investigates region $`\delta \delta _c`$ for higher and higher $`\delta _c`$. For all filling fractions $`\sigma _r`$ falls well below $`1\%`$ if sufficciently high $`\delta `$ is taken. For example for $`\delta 20`$ one obtains $`\sigma _r<0.1\%`$ for $`f=0.2`$ and $`\sigma _r<0.3\%`$ for $`f=0.4`$. For $`\delta (1,100]`$ formula (3) still describes $`\mathrm{}_L`$ with a reasonable precision, namely, with the relative error ranging from 3.3% to 6.5% (depending on the filling fraction). The main contribution to the error is picked up around $`\delta =\delta _m(f)`$ for which $`\mathrm{}_L`$ takes on its maximum. At $`\delta =\delta _m`$, our formula (3) gives persistently a slightly lower value for $`\mathrm{}_L`$. The relative L-gap width $`\mathrm{}_L^r`$ is described by the formula (7) with a slightly larger relative error ranging from 4.1% to 8% (depending on the filling fraction). The reason is that there are now two main contributions to the error, that around the maximum of $`\mathrm{}_L`$ and the second systematic error due to the overestimation of the L-midgap frequency $`\nu _c`$ when using Eq. (6). All the formulas only involve the effective dielectric constant of the medium $`\epsilon _{eff}`$ approximated by Maxwell-Garnett’s formula (2), and volume averaged $`\epsilon (𝐫)`$ and $`\epsilon ^2(𝐫)`$ over the lattice unit cell. Since $`\overline{\epsilon }`$, $`\overline{\epsilon ^2}`$, and $`\epsilon _{eff}`$ have well-defined meaning for any lattice, this suggests that a similar gap behavior may occur for other lattices. It would be interesting to find out if the same is true for the width of the full photonic band gap .

I would like to thank A. van Blaaderen, A. Tip, and W. L. Vos for careful reading of the manuscript and useful comments, and other members of the photonic crystals interest group for discussion. This work is part of the research program by the Stichting voor Fundamenteel Onderzoek der Materie (Foundation for Fundamental Research on Matter) which was made possible by financial support from the Nederlandse Organisatie voor Wetenschappelijk Onderzoek (Netherlands Organization for Scientific Research). SARA computer facilities are also gratefully acknowledged.