# Far infrared giant dipole resonances in neutral quantum dots

## I Introduction

A well-established result of Nuclear Physics is the presence of giant resonance modes related to collective excitations in nuclei. Particularly, collective states corresponding to giant electric dipole oscillations are known in nuclei long ago . They show themselves as very high peaks in photoabsorption at energies $`80A^{1/3}`$ MeV, where A is the mass number. An understanding of this phenomenon can be achieved by means of a simple hydrodynamic model in which one considers small density perturbations against the background nuclear density and computes the small-oscillation frequencies associated to dipole excitations . A second, microscopic, approach makes use of the nuclear shell model . It is shown that the giant dipole resonance (GDR) is a state coming from the splitting of a degenerate set of $`1^{}`$ states, which takes almost the whole strength of the $`1^{}`$ transition.

Collective states very similar to the GDR have been extensively studied, both experimentally and theoretically, in Atomic Physics. They are at the base of giant and broad atomic resonances in the photoionisation continuum . The photoabsorption cross section of metallic clusters  exhibits also the dominance of a collective oscillation mode at 2 - 3 eV . Theoretical calculations based on the Random Phase Approximation (RPA)  are shown to reproduce well the resonance position and dipole strength distribution.

In the present paper we show that, in electron-hole systems confined in a quantum dot, the energy-weighted photoabsorption sum rule is almost saturated by GDR-like states, in which the electronic cloud oscillates relatively to the hole cloud. This result is mainly related to the existence of positively and negatively charged particles, and not to a particular dot geometry. Thus, we will use a very simplified model of disk-shaped dot, in which the lateral confinement is ideally parabolic .

$`N`$ electron-hole pairs are supposed to be created in the dot by means of, e. g., laser pumping with a typical $``$ 2 eV energy, as corresponding to a semiconductor band gap. The created particles live hundreds of picoseconds and even more . We will study the linear absorption of a second far infrared (FIR), $``$ 5 meV, light wave by the $`N`$-pair cluster. The period of this signal is $`10^{13}`$s, thus the cluster may be considered as stable when studying absorption. We will use the dipole approximation for the interaction hamiltonian.

Experiments on FIR study of excitonic systems have been conducted for a long time . More recently, the modifications of the interband photoluminescence (PL) of quantum well excitons caused by the absorption of FIR radiation have been studied  by means of a technique baptised as ODR (optical detection of FIR resonances). These experiments are conducted at relatively small exciton densities, where many-body effects are not expected to play a significant role. To study the collective FIR absorption by a multi-exciton system, intense laser beams for the interband processes shall be used. Experimentally, densities as high as 10<sup>12</sup> electron-hole (e-h) pairs/cm<sup>2</sup> in GaAs wells have been achieved by using pulsed (5 ps long) dye lasers . The effective absorbed power is greater than 2 MW/cm<sup>2</sup>.

To our knowledge, however, the effect of FIR radiation on dense excitonic systems have not been experimentally studied so far, although intense enough laser beams and the ODR technique are available. For simplicity of the calculations, we confine the system in a quantum dot (qdot). This confinement makes the detection a little more cumbersome, but still experimentally achievable. Single qdot multi-excitonic PL has been isolated from the averaged PL by means of microscopy techniques (see, for example, Ref. \[\]). Thus, in principle, the ODR study of single qdots is also possible.

The organisation of the paper is as follows. In Section II, we present the model to be used in the paper. Next, the basic RPA equations are explicitly written in Section III. In the later two sections, the main results and a few concluding remarks are given.

## II The model

We will study a quasi-planar quantum dot, i. e. very narrow in the growth direction (the $`z`$ axis), in such a way that the first quantum well sub-band approximation works, and no significant modifications of Coulomb interactions due to $`z`$-averaging arise. A direct band-gap material and high barriers for both electrons and holes in the $`z`$ direction are assumed to exist. Confinement makes also the hole sub-bands to split. Thus, only one e and one h bands will be considered. e-h exchange will be neglected. As mentioned above, the lateral confinement will be modelled by an ideal parabolic potential. Finally, for simplicity, we take $`m_e=m_h`$. This is a non realistic assumption, justified only by the absence of experimental results. In a GaAs dot, for example, 8 nm wide in the $`z`$ direction, the ratio of the in plane heavy hole to electron masses is around 2. The equal-mass simplification makes calculations more easy, giving nevertheless a qualitatively correct picture of what is happening.

The second-quantised Hamiltonian for the two-dimensional motion of electrons and holes is written in oscillator units as

$`H`$ $`=`$ $`{\displaystyle \underset{i}{}}ϵ_i(\widehat{e}_i^{}\widehat{e}_i+\widehat{h}_i^{}\widehat{h}_i)+{\displaystyle \frac{\beta }{2}}{\displaystyle \underset{i,j,k,l}{}}i,j|1/r|k,l\widehat{e}_i^{}\widehat{e}_j^{}\widehat{e}_l\widehat{e}_k`$ (2)   
$`+{\displaystyle \frac{\beta }{2}}{\displaystyle \underset{i,j,k,l}{}}i,j|1/r|k,l\widehat{h}_i^{}\widehat{h}_j^{}\widehat{h}_l\widehat{h}_k\beta {\displaystyle \underset{i,j,k,l}{}}i,j|1/r|k,l\widehat{h}_i^{}\widehat{e}_j^{}\widehat{e}_l\widehat{h}_k,`$   
where $`\widehat{e}_i`$($`\widehat{h}_i`$) are electron (hole) operators, $`\beta =\sqrt{(\frac{m_ee^4}{\kappa ^2\mathrm{}^2})/(\mathrm{}\omega )}`$, $`\kappa `$ is the dielectric constant, and $`\omega `$ is the dot frequency. The Coulomb matrix elements are defined as

$`i,j|1/r|k,l`$ $`=`$ $`\delta (s_{zi},s_{zk})\delta (s_{zj},s_{zl}){\displaystyle \frac{\mathrm{d}^2r_1\mathrm{d}^2r_2}{|\stackrel{}{r}_1\stackrel{}{r}_2|}\varphi _i^{}(\stackrel{}{r}_1)\varphi _j^{}(\stackrel{}{r}_2)\varphi _k(\stackrel{}{r}_1)\varphi _l(\stackrel{}{r}_2)},`$ (3)   
and the explicit form of the harmonic-oscillator orbitals is the following

$$\varphi _j=C_{n_j,m_j}r^{|m_j|}L_{n_j}^{|m_j|}(r^2)e^{r^2/2}e^{im_j\theta },$$
(4)   
where $`n_j`$ and $`m_j`$ are oscillator quantum numbers, and $`C_{n,|m|}=\sqrt{n!/[\pi (n+|m|)!]}`$. The one-particle energies in the quadratic potential are $`ϵ_j=1+2n_j+|m_j|`$.

We consider the dot in the strong-confinement regime, where the one-particle energy dominates the total energy. It means, $`\beta <\beta _c`$, where $`\beta _c`$ may be estimated  from the breakdown of perturbation theory or from the onset of BCS pairing to be $`\beta _c0.58N^{1/4}`$. The associated value of density is $`\rho _c4/(\pi a_B^2)`$. For GaAs, the Bohr radius is $`a_B14`$ nm, thus $`\rho _c510^{11}`$ pairs/cm<sup>2</sup>.

For simplicity, we study closed-shell quantum dots. The number of electrons is equal to the number of holes, and is given by the expression $`N=N_s(N_s+1)`$, where $`N_s`$ is the last harmonic-oscillator filled shell. The zeroth-order ground state-function is a product of Slater determinants for electrons and holes. The total angular momentum, total electron spin and total hole spin are all equal to zero for this state.

The lowest excitations against the ground state are one-particle excitations from the last filled shell to the next empty shell. The states with total angular momentum, $`M=\pm 1`$, and electron and hole total spins, $`S_e=S_h=0`$, are the candidates among which we shall look for the GDR. To be definite, we will consider $`M=1`$. Notice that there are $`N_s`$ orbitals in the last shell, that is $`2N_s`$ electrons and, thus, $`2N_s`$ wave functions with $`M=1`$. There are also $`2N_s`$ functions corresponding to hole excitations. It makes a total of $`4N_s`$ many-particle states.

The Coulomb interaction breaks the oscillator degeneracy. The collective nature of the GDR is manifested in two facts: (i) it acquires the highest excitation energy in the multiplet, and (ii) the electric dipole transition probability from the ground state is strongly enhanced . We will present RPA calculations in support of these statements.

## III The random phase approximation

In the RPA , we allow a general correlated ground state, $`|RPA`$, and the excited states are looked for in the form

$$\mathrm{\Psi }=Q^{}|RPA,$$
(5)   
where the $`Q^{}`$ operator is given by the expression

$$Q^{}=\underset{\sigma ,\lambda }{}(X_{\sigma \lambda }^ee_\sigma ^{}e_\lambda +X_{\sigma \lambda }^hh_\sigma ^{}h_\lambda Y_{\sigma \lambda }^ee_\lambda ^{}e_\sigma Y_{\sigma \lambda }^hh_\lambda ^{}h_\sigma ).$$
(6)   
The index $`\lambda `$ runs over the last Hartree-Fock (HF) filled shell, and $`\sigma `$ runs over the first unfilled shell. The $`X`$ coefficients are nonzero only for “up” transitions, i.e. for which the angular momentum values satisfy $`m_\sigma m_\lambda =1`$, and the $`Y`$ coefficients are nonzero only for “down” transitions, i.e. $`\lambda `$ and $`\sigma `$ satisfying $`m_\lambda m_\sigma =1`$. They are obtained from the RPA equations

$`\left(\begin{array}{cc}A& B\\ B^t& A^d\end{array}\right)\left(\begin{array}{c}X\\ Y\end{array}\right)=\mathrm{\Delta }E\left(\begin{array}{c}X\\ Y\end{array}\right),`$ (7)   
in which the $`A`$ matrix is given by

$`\left(\begin{array}{cc}A^{ee}& A^{eh}\\ A^{he}& A^{hh}\end{array}\right),`$ (8)   
and its matrix elements are the following

$`A_{\sigma \lambda ,\tau \mu }^{ee}`$ $`=`$ $`(ϵ_\sigma ^{HF}ϵ_\lambda ^{HF})\delta _{\sigma \tau }\delta _{\lambda \mu }+\beta \left(\sigma ,\mu |1/r|\lambda ,\tau \sigma ,\mu |1/r|\tau ,\lambda \right),`$ (9)   
$`A_{\sigma \lambda ,\tau \mu }^{eh}`$ $`=`$ $`\beta \sigma ,\mu |1/r|\lambda ,\tau .`$ (10)   
$`A^{hh}=A^{ee}`$, $`A^{he}=A^{eh}`$ because of the electron-hole symmetry of our hamiltonian. $`\tau `$ and $`\mu `$ are indexes similar to $`\sigma `$ and $`\lambda `$, respectively. The $`B`$ matrix has a similar structure. Its matrix elements, calculated between up and down transitions, are given by

$`B_{\sigma \lambda ,\tau \mu }^{ee}`$ $`=`$ $`\beta (\sigma ,\tau |1/r|\lambda ,\mu \sigma ,\tau |1/r|\mu ,\lambda ),`$ (11)   
$`B_{\sigma \lambda ,\tau \mu }^{eh}`$ $`=`$ $`\beta \sigma ,\tau |1/r|\lambda ,\mu .`$ (12)   
$`B^{hh}=B^{ee}`$ and $`B^{he}=B^{eh}`$. $`B^t`$ is the transpose of the numerical matrix $`B`$, and the $`A^d`$ matrix is calculated from (9,10) between down transitions. Usually, positive (physical) and negative (unphysical) excitation energies of equal magnitude come from (7). The physical solutions annihilate the RPA ground state

$$Q|RPA=0,$$
(13)   
and satisfy the normalisation condition

$$1=\underset{\sigma ,\lambda }{}\{(X_{\sigma \lambda })^2(Y_{\sigma \lambda })^2\}.$$
(14)   
The FIR radiation to be absorbed is assumed to be linearly polarised, with the electric field vibrating along the $`y`$ direction. The dipole matrix elements are computed from

$$\mathrm{\Psi }|D|RPA=\underset{\sigma ,\lambda }{}\{(X_{\sigma \lambda }^hX_{\sigma \lambda }^e)\sigma |y|\lambda +(Y_{\sigma \lambda }^hY_{\sigma \lambda }^e)\lambda |y|\sigma \}.$$
(15)   
The calculated dipole elements fulfil the energy-weighted sum rule 

$`{\displaystyle \underset{\mathrm{\Psi }}{}}\mathrm{\Delta }E|\mathrm{\Psi }|D|RPA|^2={\displaystyle \underset{\mathrm{\Psi }_0}{}}\mathrm{\Delta }E_0|\mathrm{\Psi }_0|D|0|^2=N/2,`$ (16)   
where 0 indexes refer to the noninteracting $`\beta =0`$ case.

The HF energies and one-particle wave functions were obtained selfconsistently by means of an iterative scheme. We write

$$|\alpha =\underset{i}{}C_{\alpha i}|i,$$
(17)   
where latin indexes refer to harmonic oscillator orbitals. 272 orbitals, i. e. 16 harmonic oscillator shells where included in the calculations. The HF equations read

$$\underset{j}{}\{ϵ_i\delta _{ij}\beta \underset{\mu F}{}\underset{k,l}{}C_{\mu k}C_{\mu l}i,k|1/r|l,j\}C_{\alpha j}=ϵ_\alpha C_{\alpha i},$$
(18)   
and the starting approximation is $`C_{\alpha i}=\delta _{\alpha i}`$. $`F`$ denotes the Fermi level. A few iterations are enough to reach convergence at very low $`\beta `$ values, while at $`\beta 1`$, 15 iterations are needed.

## IV Results

Excitation energies and dipole strength distributions were computed for $`N`$ ranging between 2 and 110, and $`\beta `$ in the interval $`0\beta 0.6N^{1/4}`$. For larger values of $`\beta `$, pairing becomes very important , and should be taken into account more properly. Let us stress, however, that pairing should reinforce the picture of GDR dominance of photoabsorption, leading to an increase of the excitation energy and, consequently, to a decrease in the same proportion of the dipole element squared.

The results for $`N=110`$ pairs at $`\beta =1`$ are shown in Fig. 1, where dipole matrix elements squared vs excitation energies are shown. The fraction of the sum rule (16) accounted for the GDR state is close to 100 %. Notice that only collective states, for which $`X^e=X^h`$, are represented in the figure. The rest of the states show a threefold degeneracy and give practically zero dipole matrix elements. Let us note that the energy gap is increased ($`\mathrm{\Delta }E>1`$) after the Coulomb interaction is switched on. This is a signal that the overall interaction among particles is attractive.

We draw in Fig. 2a the GDR excitation energies at $`\beta =1`$ as a function of $`N^{1/4}`$. Notice the approximate dependence $`\mathrm{\Delta }E_{gdr}10.7+0.4N^{1/4}`$. At $`\beta 1`$, the dependence is $`\mathrm{\Delta }E_{gdr}1(0.7+0.4N^{1/4})\beta `$. Turning back to ordinary units, we get an excitation energy

$$\mathrm{\Delta }E_{gdr}(1+0.7\beta )\mathrm{}\omega +0.4\frac{\mathrm{}^2}{ma_B}\sqrt{2\pi /3}\rho ^{1/2},$$
(19)   
where $`\rho 3N^{1/2}m\omega /(2\pi \mathrm{})`$ is the density of pairs. For large enough $`N`$, and $`\omega 0`$ in order to preserve a constant density, $`\mathrm{\Delta }E_{gdr}0.6\mathrm{}^2\rho ^{1/2}/(ma_B)`$, leading for example to $`\mathrm{\Delta }E_{gdr}4.5`$ meV for typical values of the constants in GaAs and $`\rho 510^{11}`$ pairs/cm<sup>2</sup>.

The GDR dipole elements squared at $`\beta =1`$ as a function of $`N`$ are shown in Fig. 2b. The points fit a linear dependence $`0.17N`$. For $`\beta 1`$, the saturation of the sum rule implies that $`D^2N/(2\mathrm{\Delta }E_{gdr})N/(2+(1.4+0.8N^{1/4})\beta )`$.

Finally, we draw in Fig. 3 the fraction of the energy-weighted sum rule (16), the $`S1`$ sum rule, corresponding to the transition to the GDR state. This fraction is higher than 98% for any of the systems shown in Figs. 3a and 3b. (We got a slight violation, fraction=1.01, for $`N=110`$ at $`\beta =1`$, but this is an artifact related to the finiteness of the basis used to construct the HF states).

## V Conclusions

We have shown that the far infrared absorption spectrum of neutral confined systems of electrons and holes is dominated by a giant dipole resonance which accounts for more than 98% of the energy-weighted photoabsorption sum rule. Calculations were done in a very simplified two-band model with $`m_e=m_h`$ and a disk-shaped parabolic dot. The qualitative conclusions are, however, expected to be valid for realistic systems since they are mainly related to the existence of positively and negatively charged particles in the system, which causes the enhancement of dipole oscillations.

For the resonance position at intermediate $`N`$, we obtained the fit, $`\mathrm{\Delta }E_{gdr}=\{1+(0.7+0.4N^{1/4})\beta \}\mathrm{}\omega `$. In terms of the density, we obtain $`\mathrm{\Delta }E_{gdr}(1+0.7\beta )\mathrm{}\omega +0.4\sqrt{2\pi /3}\mathrm{}^2\rho ^{1/2}/(ma_B)`$. The dipole strength scales with $`N`$: $`D^2N`$, at small $`N`$ values, and $`D^2N^{3/4}`$ at larger values of $`N`$.

The GDR state we found is the analogue in a finite two-dimensional system of the out-of-phase plasma frequency in the two-component plasma . The term proportional to $`\mathrm{}\omega `$ in the excitation energy is a shell effect of the external harmonic-oscillator potential.

We worked in the strong-confinement regime, $`\beta <0.6N^{1/4}`$. For still higher values of $`\beta `$, BCS pairing should be explicitly included in the calculations. Recently, we have computed the ground-state energy of the confined $`N`$-pair system by using a BCS trial function . The effect of pairing in $`\mathrm{\Delta }E_{gdr}`$ could be taken into account by means of a quasiparticle RPA scheme , which may be taken as the analogue for a finite system of the Gor’kov’s pairing approximation in the excitonic insulator phase . At relatively high densities we expect, qualitatively, a shift of the resonance position in accordance to the opening of the gap at the Fermi level:

$$\mathrm{\Delta }E_{gdr}=\sqrt{(2\mathrm{\Delta }_F)^2+\left((1+0.7\beta )\mathrm{}\omega +0.4\sqrt{2\pi /3}\mathrm{}^2\rho ^{1/2}/(ma_B)\right)^2},$$
(20)   
where $`\mathrm{\Delta }_F`$ is the gap function at the Fermi energy. The dipole strength shall decrease in the same proportion, as dictated by (16).

###### Acknowledgements.

A. D. and R. C. acknowledge support from the Universidad de Antioquia (where part of this work was done) and from the Caribbean Network for Theoretical Physics.