# Is there a symmetry between absorption and amplification in disordered media?

Recent observations  of laser-like emission from dye solution emerged with TiO<sub>2</sub> nanoparticles have stimulated intensive theoretical efforts to investigate the properties of disordered media which are optically active. From considerations of enhanced optical paths through multiple scattering, random systems are expected to possess a reduced gain threshold for lasing. Correspondingly, one would expect the transmission in disordered systems to be enhanced with gain. The longer the system, the larger the enhancement. Surprisingly, numerical calculations based on time-independent wave equations showed that for large systems the wave propagation is still attenuated, indicating a localization of waves even with gain. The rate of the exponential attenuation is the same as if the system was absorbing. Such a symmetry between absorption and amplification was subsequently shown to hold for the time-independent wave equation.

Intuitively one would expect that the presence of amplification should facilitate wave propagation, not suppress it, even in disordered systems. The peculiar result of reduced transmission in gain media is also absent when wave propagation in disordered media is described by time dependent diffusion equations which always predict an increased output and a gain threshold above which the system become unstable. The diffusion equation neglects the phase coherence of the wave and is adequate only when the wavelength is much smaller than the mean free path. Thus it was proposed that the paradoxical phenomenon may indicate enhanced localization due to the amplification of coherent backscattering. However, amplification of backscattering does not necessarily imply a reduction in transmission since no conservation of the total photon flux is required in gain media. To fully understand the origin of this non-intuitive result, we will examine the validity of the solutions derived from the time-independent wave equation which has been commonly employed in describing the wave propagation in active media.

Linearized time-independent wave equations with a complex dielectric constant have been successfully utilized to find lasing modes by locating the poles in the complex frequency plane and to investigate the spontaneous emission noise below the lasing threshold in distributed feedback semiconductor lasers. Such equations are known to be inadequate to describe the actual lasing phenomena due to their simplicity in dealing with the interactions between radiation and matter. However, it is generally believed that the time-independent equation should suffice to describe the wave propagation in amplifying media, before any oscillations occur. We will unambiguously show that the so-called symmetry between amplification and absorption is an artifact due to the unphysical assumption of a finite output in solving the wave equations. We show that for each system, there is a frequency-dependent gain threshold above which both the total transmission and the total reflection become divergent. Solving the time-independent wave equations by incorrectly assuming a fixed output leads to unphysical solutions that does not correspond to the true behavior of the system.

To demonstrate our point, we take the simplest example of a uniform active media sandwiched between two mirrors as feedback (see the insert in Fig. 1), the classical Febry-Perot setup. Wave propagation within the active media is simply described with the following phenomenological wave equation,

$$\frac{d^2E(z)}{dz^2}+\frac{\omega ^2}{c^2}\epsilon (z)E(z)=0,$$
(1)   
where $`E(z)`$ is the electric field and the dielectric constant $`\epsilon (z)=\epsilon ^{}(z)i\epsilon ^{^{\prime \prime }}(z)`$ with the imaginary part signifying amplification ($`\epsilon ^{^{\prime \prime }}>0`$) or absorption ($`\epsilon ^{^{\prime \prime }}<0`$ ). We point out that in electromagnetic theory, the imaginary part of the dielectric constant is proportional to the conductivity of the material and thus cannot be negative. The negative dielectric constant is strictly speaking only an effective way to introduce coherent amplification . Complex potentials known as optical potential have long been employed in nuclear physics to describe nuclei scattering processes.

The transmission and the reflection amplitude can be easily obtained by solving Eq.(1) to yield:

$$t=\frac{t_1t_2e^{ikL}}{1r_1r_2e^{2ikL}}$$
(2)   
where $`t_1=2k/(k+k_0)`$, $`t_2=2k_0/(k+k_0)`$, and $`r_1=r_2=(kk_0)/(k+k_0)`$ are the transmission and reflection coefficients at the left and right two interfaces, respectively. $`k_0=\sqrt{\epsilon _0}\frac{2\pi }{\lambda }`$ and $`k=k^{}ik^{\prime \prime }=\sqrt{\epsilon ^{}i\epsilon ^{\prime \prime }}\frac{2\pi }{\lambda }`$ are the wavevectors outside and inside the system, $`L`$ is the distance between the mirrors (system size). The oscillation condition for lasing is correctly given by $`1r_1r_2e^{2ikL}=0`$ at which both the transmission and reflection coefficient diverge.

However, Eq.(2) also predicts the exponential decrease of the transmission coefficient for large system sizes. In fact the term in the numerator with the $`exp(ikL)`$ increases exponentially as the length of the system $`L`$ increases because of the gain, but the term in the denominator with the $`exp(2ikL)`$ increases even faster, making the transmission coefficient decay asymptotically as $`|t||exp(ikL)|=exp(k^{\prime \prime }L)`$. This is clearly shown in Fig.1, where we plot the $`ln(T)`$ versus $`L`$ for a one-layer system. Notice that for large $`L`$, $`ln(T)`$ decreases as $`L`$ increases despite the fact that we have gain at here. Gain effectively becomes loss at large lengths! Remember the system is homogeneous thus disorder is definitely not responsible for this strange behavior. Thus the inhibition of wave propagation for large systems is clearly not a result of amplification in backscattering.

A clear picture of what is going on can be obtained from the path integral method . In such an approach, the total transmission coefficient can be obtained by adding the paths of the successive reflected and transmitted rays. In doing so, we obtain that

$$t=t_1t_2e^{ikL}[1+(r_1r_2e^{2ikL})+(r_1r_2e^{2ikL})^2+\mathrm{}]$$
(3)   
where the first term represents the direct transmission of the incoming wave, and the second term represents the wave which was reflected first by $`r_2`$ at right interface and then by $`r_1`$ at left interface and subsequently transmitted through. More terms from sequences of multiple transmissions and reflections from the two mirrors follow. It is clear Eq.(3) represents an infinite series whose sum reproduces Eq. (2), provided that the following condition is met,

$`|r_1r_2e^{2ik^{}L}e^{2k^{\prime \prime }L}|<1.`$ (4)   
When the condition given by Eq.(4) is violated, such as when the system size or the gain is large, the physical output represented by the sum diverges, even away from the oscillation pole.

We hope to note at here that the sum of right side of Eq.(3) include the phases of all paths, so that it includes all interference of scattering waves. We also note that the results of Eq.(3) are consistent with time-dependent theory because different terms of Eq.(3) can explain as outputs at different time from a same incidence or the output at same time from a series incidence at different time. By this way, the out-put of a system with gain much larger than the threshold will increase exponentially versus time after a plane wave incidence, but time-independent theory suppose a small output as if the system is of absorbing material. Base on time-dependent Maxwell equations, a well-developed FDTD (finite-difference time-domain) method can help us to see the obvious different behavior of transmission of two kind of systems versus time. We choose a plane wave with $`\lambda =800`$nm as the incidence from left to the setup of Fig.1 with $`L=4300`$nm. The dielectric constant is taken to be $`\epsilon _0=1`$ outside and $`Re(\epsilon )=\epsilon ^{}=9`$ inside. The threshold of this system is $`\epsilon ^{\prime \prime }=0.12`$ from Eq.(4). Our numerical results show that, after a short instantaneous state, the output of system will get to a stable value which is the transmission of the system if the system with under-threshold gain or with absorption. Unless the gain or the length is over the threshold, the results of time-independent theory are same as the time-dependent theory. But if the system with gain is above the threshold, the output of system will increase exponentially versus time as predicted by Eq.(3). In Fig. 2, we plot the logarithm of amplitudes of out-put at right side of system versus time for different gain, we can see the numerical results exactly same as we predicted. We also examined the slope of lines with the gain larger the threshold in Fig. 2, and found the slope is exactly same as we predict in Eq. (3), equal to $`log_{10}|r_1r_2e^{2k^{\prime \prime }L}|`$.

The divergence of the transmission above threshold even away from the oscillation pole is the key in understanding the failure of Eq.(2), which is conventionally derived from boundary condition by implicitly assuming that the output is finite. Normally the physical boundary condition is satisfied when $`t_1t_2e^{ikL}+r_1r_2e^{2ikL}t=t`$, resulting in Eq. (2). Obviously this condition lost its meaning when t is infinite. As a result, Eq. (2) becomes unphysical. For a lossy system, the condition given by Eq.(4) is always satisfied. Thus the divergence is a new phenomenon occurring only to systems with gain. The breakdown of the time-independent wave equation signals the large fluctuations of the transmission in time and calls for more sophisticated theories that can take into account the interaction between radiation and matter to correctly describe the response of the system.

To show that the exponentially attenuated results of time-independent theory with gain is not from the backscattering effect, but from a theoretical mistake, we also do the same numerical experiment to random system with gain. The system is made of 50 cells, each cell contains two kind layers with dielectric constant $`\epsilon _1=1`$ and $`\epsilon _2=4i\epsilon ^{\prime \prime }`$. To introduce disorder, we choose the width of first layer of the $`n`$th cell to be random variable $`a_n=a_0(1+W\gamma )`$,where $`a_0=95`$ nm, $`W`$ describes the strength of randomness which is 0.8 in our model and $`\gamma `$ is a random number between $`(0.5,0.5)`$. The width of second layer in $`n`$th cell is $`b_n=215nma_n`$. The wavelength of incident wave is $`\lambda =1200`$nm. In Fig.3, we plot the logarithm of output at right side of system versus time with plane wave incidence for different gain. We also get the same results as what we predicted, the exponential increase of the output versus time when the gain is over the threshold value, which are showed in Fig.3. The time-dependent results also show that the threshold of random system is quite small as previously predicted and showed experimentally . Actually all time-dependent theories about the system with the gain or the length over the threshold, such as Letokohov diffusion theory , Lamb theory , give the divergent output of the system. The physical meaning of the divergent output is that the rate of generating photons by the induced radiation is larger than the escaping rate of photons from the interfaces of the system. Now the field in the system will become stronger and stronger even if the frequency of the wave is not resonant frequency(at the resonant frequency, the system become a laser).

For multilayer systems, to see whether the results of transmission or reflection coefficients of the time-independent theory is physical, a simple approach is to check every layer of the system by the following method. When we examine one certain layer, such as m-th layer, in the multilayer system, we can assume that the left part of system forms an effective interface of the layer with transmission and reflection coefficients $`t_l`$ and $`r_l`$, and the right part forms the other effective interface with $`t_r`$ and $`r_r`$. Here we assume both right and left subsystems are below threshold. The convergence condition for every layer of the system is then given by Eq.(2), with ($`t_1`$, $`r_1`$), and ($`t_2`$, $`r_2`$) replaced by ($`t_l`$,$`r_l`$) and ($`t_r`$, $`r_r`$), respectively. For every layer, Eq.(2) gives us a line. The cusps are formed by the lowest limit out of all lines. Fig. 4 shows the results of such a calculation for a 40 layer system, which is formed by two kind of layers with widths $`L_1=95nm`$, $`L_2=120nm`$ and dielectric constants $`\epsilon _1^{}=1`$, $`\epsilon _2^{}=2`$ respectively . In reality, the curve only gives an indication of the magnitude of the gain above which the results from time-independent equation becomes suspect.

In solving the time-independent equations, it is difficult to know exactly when the solutions break down. One certainly cannot tell from the expression of the total transmission and the total reflection coefficient which are well behaved except exactly at the oscillation pole. However, a rough indication is that when the gain for a fixed system approaches the lasing threshold for nearby poles or when the system sizes exceed the threshold length, the solutions should not be trusted. However, the threshold condition is still given by the poles in the complex plane. A study of the distribution of these poles has been carried out through carefully locating the pole position by continuously tuning the gain up at a fixed frequency until the transmission coefficient diverges.

The implication of the analysis above is that the calculation of transmission and reflection coefficient with the traditional method become suspect once the gain or system size reaches a certain value. Care has to be taken to ensure that the system is not above threshold and the solution is physical. This remark, unfortunately, also pertains to the application of the powerful $`invariant`$ $`embedding`$ method . in which the finite reflection and transmission are assumed implicitly.

In summary, this note aims to bring attention to some peculiar aspects of the time-independent wave equation when the gain is above certain threshold for a fixed length, or equivalently, when the length of the system exceeds a certain value for a fixed gain. Thus some of the conclusions on the statistical properties of the reflection and the transmission coefficient in media with gain become suspicious at large system sizes. The time-independent equation is inadequate to describe the amplification of light under these conditions. Nevertheless, the simplicity of the time-independent equation can be used effectively to locate resonant conditions, even in disordered systems. A complete treatment of the wave propagation in gain media may require the construction of the time-dependent solution out of the continuous and discrete solutions of the time-independent equation . Unlike for the Hermitian system, the completeness of these solutions could not be proved easily  when the potential is complex.

Ames Laboratory is operated for the U.S. Department of Energy by Iowa State University under Contract No. W-7405-Eng-82. This work was supported by the director for Energy Research, Office of Basic Energy Sciences.