# Femtosecond Coherent Dynamics of the Fermi Edge Singularity and Exciton Hybrid

## Abstract

We study theoretically the coherent nonlinear optical response of doped semiconductor quantum wells with several subbands. When the Fermi energy approaches the exciton level of an upper subband, the absorption spectrum acquires a characteristic double–peak shape originating from the interference between the Fermi–edge singularity and the exciton resonance. We demonstrate that, for off–resonant pump excitation, the pump/probe spectrum undergoes a striking transformation in the coherent regime, with a time–dependent exchange of oscillator strength between the Fermi edge singularity and exciton peaks. We show that this effect originates from the many–body electron–hole correlations which determine the dynamical response of the Fermi sea. Possible experimental applications are discussed.

Ultrafast nonlinear spectroscopy offers a unique perspective into the role of many–body effects in semiconductors. While the linear absorption spectrum provides information about static properties, ultrafast time–resolved spectroscopy allows one to probe the system on time scales shorter than those governing the interactions between the elementary excitations. In the coherent regime, the dynamics of many–body correlations plays an important role in the transient changes of the absorption spectrum. For example, in undoped semiconductors, exciton–exciton interactions were shown to play a dominant role in the optical response for specific sequences of the optical pulses.

In modulation–doped quantum wells (QW), the optical properties are dominated by the Fermi edge singularity (FES). Unlike in the undoped case, where the linear absorption exhibits discrete bound state peaks whose width is ultimately determined by the homogeneous broadening, the FES is a continuum resonance whose lineshape is governed by the Coulomb interactions of the photoexcited carriers with the low–lying Fermi sea (FS) excitations. In this letter we study the role of such many–body correlations in pump/probe measurements, where the strong “pump” pulse excites the system at time $`t=0`$, while the weak “probe” pulse measures the optical response at time $`t=\tau `$. In the doped systems, the interactions are screened and there are no discrete bound states. Therefore, the many–body correlations enter into the nonlinear response not via exciton–exciton interactions, but mainly through the dynamical response of the FS during the course of the optical excitation. Since such electron–hole (e–h) correlations come from the “dressing” of the photoexcited e–h pair by gapless FS excitations, the response of the FS to ultrashort optical pulses is intrinsically unadiabatic . For resonant pump excitation, the electron–electron (e–e) scattering also leads to strong variations of the dephasing and relaxation times, from a few ps close to the FES to $`10`$ fs away from the Fermi level. However, such incoherent relaxation effects are suppressed for off–resonant excitation, when the pump is tuned below the FES resonance, in which case coherent effects dominate. Furthermore, for negative ($`\tau <0`$) time delays, the pump/probe signal is due to the coherent interaction of the pump pulse with the polarization induced in the sample by the probe pulse and, again, the effects of incoherent processes are strongly attenuated . Therefore, the coherent dynamics studied below can be best observed under off–resonant conditions or when the probe precedes the pump.

Here we investigate the ultrafast pump/probe dynamics of the FES–exciton hybrid, which is formed in asymmetric QW’s with partially occupied subbands. In such structures, interband optical transitions from the valence band to several conduction subbands are allowed due to the finite overlap between the hole and electron envelope wave–functions. The many–body effects on the linear absorption spectrum have been described by using the simple two–subband Hamiltonian

$$H=H_0\underset{ij}{}\underset{\mathrm{𝐩𝐤𝐪}}{}v_{ij}(𝐪)a_{i𝐩+𝐪}^{}a_{j𝐩}b_{𝐤𝐪}^{}b_𝐤,$$
(1)   
with $`H_0=_{i𝐤}ϵ_{i𝐤}^ca_{i𝐤}^{}a_{i𝐤}+_𝐤(ϵ_𝐤^v+E_g)b_𝐤^{}b_𝐤`$. Here $`a_{i𝐤}^{}`$ and $`ϵ_{i𝐤}^c`$ are the creation operator and the energy of a conduction electron in the $`i`$th subband, $`b_𝐤^{}`$ and $`ϵ_𝐤^v`$ are those of a valence hole ($`E_g`$ is the bandgap), and $`v_{ij}(𝐪)`$ is the screened e–h interaction matrix with diagonal (off–diagonal) elements describing the intrasubband (intersubband) scattering. Due to the screening, the interaction potential is short–ranged and can be replaced by its s–wave component ; close to the Fermi surface, $`v_{ij}(𝐪)v_{ij}`$ . Here we consider the case where only the first subband is occupied, but the Fermi level is close to the exciton level (with binding energy $`E_B`$) below the bottom of the second subband \[see inset in Fig. 1(a)\]. For large values of the FES–exciton splitting $`\mathrm{\Delta }E_FE_B`$, where $`\mathrm{\Delta }`$ is the subband separation, the linear absorption spectrum consists of two well separated peaks, the lower corresponding to the FES from subband 1, and the higher corresponding to the Fano resonance from the exciton of subband 2 broadened by its coupling to the continuum of states in subband 1. With decreasing $`\mathrm{\Delta }E_FE_B`$, the FES and the exciton become hybridized due to the intersubband scattering arising from the Coulomb interaction. This results in the transfer of oscillator strength from the exciton to the FES and a strong enhancement of the absorption peak near the Fermi level due to the resonant scattering of the photoexcited electron by the exciton level.

In typical QW’s, $`v_{12}`$ is much smaller than $`v_{ii}`$ (a value $`v_{12}/v_{11}0.2`$ was deduced from the fit to the linear absorption spectrum in ). In the absence of coupling ($`v_{12}=0`$), the different nature of the exciton and FES leads to distinct dynamics under ultrafast excitation. In the presence of coupling, one should expect new effects coming from the interplay of this difference and the intersubband scattering that hybridizes the two resonances. Indeed, we demonstrate that, at negative time delays, the pump/probe spectrum undergoes a drastic transformation due to a transient light–induced redistribution of the oscillator strength between the FES and the exciton. We show that such a redistribution is a result of the dynamical FS response to the pump pulse. In fact, the ultrafast pump/probe spectra of the FES–exciton hybrid can serve as an experimental test of the difference between the FES and exciton dynamics.

Theory.— The total Hamiltonian of the system is $`H+H_p(t)+H_s(t)`$, with $`H_\alpha (t)`$ ($`\alpha =p,s`$) describing the optical excitations,

$$H_\alpha (t)=_\alpha (t)\underset{i}{}\left[\mu _iU_i^{}e^{i\omega _pt+i𝐤_\alpha 𝐫}+\text{h.c.}\right],$$
(2)   
where $`U_i^{}=_𝐤a_{i𝐤}^{}b_{i𝐤}^{}`$ is the transition operator to the $`i`$th subband, $`\mu _i`$ is the dipole matrix element, and $`_\alpha (t)`$ are the amplitudes of the probe ($`\alpha =s`$) and pump ($`\alpha =p`$) electric fields, propagating in the directions $`𝐤_\alpha `$. In order to account for the e–h correlations that govern the dynamics of the hybrid, we use the multi–subband generalization of the method developed previously for the FES. The non–linear pump/probe spectrum of the system described by the “bare” Hamiltonian (1) represents the linear response to the probe alone of the system described by the Hamiltonian $`H+H_p(t)`$. In order to take advantage of the linear–response formalism, we adopt the “pump–dressed” effective Hamiltonian $`\stackrel{~}{H}(t)`$, which we derived from $`H+H_p(t)`$ using a time–dependent Schrieffer–Wolff transformation. In fact, such a treatment mimics nicely the spirit of the pump/probe experiments. The details will be published elsewhere, and here we present only the final expressions. Since the pump/probe signal is linear in the probe field, the essential physics can be captured by assuming a $`\delta `$–function probe pulse, $`_\tau (t)=_\tau e^{i\omega _p\tau }\delta (t\tau )`$, and a Gaussian pump pulse. The pump/probe polarization has the form ($`t>\tau `$)

$$P(t)=i_se^{i\omega _pt}\underset{ij}{}\mu _i\mu _j0|\stackrel{~}{U}_i(t)𝒦(t,\tau )\stackrel{~}{U}_j^{}(\tau )|0,$$
(3)   
where $`𝒦(t,\tau )`$ is the time–evolution operator for the effective Hamiltonian,

$$\stackrel{~}{H}(t)=\underset{ij𝐤}{}ϵ_{ij𝐤}^c(t)a_{i𝐤}^{}a_{j𝐤}+\underset{𝐤}{}ϵ_𝐤^v(t)b_𝐤^{}b_𝐤+V_{eh}(t)+V_{ee}(t),$$
(4)   
where $`V_{eh}`$ and $`V_{ee}`$ are the effective e-h and e-e interactions and $`\stackrel{~}{U}_i^{}(t)`$ is the effective transition operator given below. Here $`ϵ_{ij𝐤}^c(t)=\delta _{ij}ϵ_{i𝐤}^c+\mathrm{\Delta }ϵ_{ij𝐤}^c(t)`$, and $`ϵ_𝐤^v(t)=ϵ_𝐤^v+\mathrm{\Omega }+\mathrm{\Delta }ϵ_𝐤^v(t)`$ are the band dispersions with pump–induced self–energies: $`\mathrm{\Delta }ϵ_{ij𝐤}^c(t)=_p(t)[\mu _ip_{j𝐤}^{}(t)+\mu _jp_{i𝐤}(t)]/2`$, and $`\mathrm{\Delta }ϵ_𝐤^v(t)=_p(t)\mathrm{Re}_i\mu _ip_{i𝐤}(t)`$, with $`p_{i𝐤}(t)`$ satisfying

$$i\frac{p_{i𝐤}(t)}{t}=(ϵ_{i𝐤}^c+ϵ_𝐤^v+\mathrm{\Omega })p_{i𝐤}(t)\underset{j𝐪}{}v_{ij}p_{j𝐪}(t)\mu _i(t),$$
(5)   
where $`\mathrm{\Omega }`$ is the detuning of $`\omega _p`$ measured from the Fermi level . Since $`p_{i𝐤}(t)`$ are linear in $`_p(t)`$, the self–energies are quadratic in the pump field. Note that (i) the time–dependence of the self–energies lasts for the duration of the pump, and (ii) that the pump induces additional intersubband scattering, described by $`\mathrm{\Delta }ϵ_{12𝐤}^c(t)`$. The effective transition operator appearing in Eq. (3) is $`\stackrel{~}{U}_i^{}(t)=_{j𝐤}\varphi _{ij𝐤}(t)a_{j𝐤}^{}b_𝐤^{}`$, with

$$\varphi _{ij𝐤}(t)=\delta _{ij}\left[1\frac{1}{2}\underset{l}{}|p_{l𝐤}(t)|^2\right]\frac{1}{2}p_{i𝐤}(t)p_{j𝐤}^{}(t).$$
(6)   
In the single–subband case, Eq. (6) takes a familiar form $`\varphi _𝐤(t)=1|p_𝐤(t)|^2`$ — the usual Pauli blocking factor in the coherent limit; in a multi–subband case, the latter is a matrix.

Eqs. (36) are used here to study the pump/probe signal of the multi-subband QW during negative time delays ($`\tau <0`$) and for off-resonant excitation with detuning $`\mathrm{\Omega }E_F`$, in which case the coherent effects dominate. Similar to the single–subband case, the above expressions apply for $`\mu _i_p/\mathrm{\Omega }1`$ (or $`t_p`$, $`\mu _i_pt_p1`$ for short pump pulse duration). For $`\mathrm{\Omega }E_M`$ (or for $`E_Mt_p1`$), $`E_ME_F`$ being the characteristic Coulomb energy of the FS excitations, the corrections to the above effective parameters due to pair–pair and pair–FS interactions  can be neglected for simplicity since they are perturbative in the screened interactions. One can also show  that, due to the FS Pauli blocking and the screening, the pump-induced corrections in the interaction potentials in (4) are suppressed, as compared to the self-energies, by a factor $`(E_M/\mathrm{\Omega })^2`$ (or $`(E_Mt_p)^2`$ for short pump duration) and can therefore be neglected in the excitation regime of interest here. Finally, similar to the linear absorption calculations, the effects of $`V_{ee}`$ can be taken into account via a screened e–h potential in $`V_{eh}`$ and by treating the e-e scattering within the dephasing time approximation ; indeed, for off-resonant excitation the e-e scattering is suppressed, while at the same time, due to high FS electron density, the build–up of screening in doped QW’s occurs during time scales shorter than the typical pulse duration $``$ 100 fs.

Thus, in the coherent limit, the effective Hamiltonian (4) has the same operator form as the “bare” Hamiltonian (1), but with time–dependent band dispersions. To calculate the polarization (3), we adopt the multi-subband generalization of the coupled cluster expansion method (CCE) for time–dependent Hamiltonians . We consider the physically relevant limit of large hole mass and include the hole recoil broadening in the dephasing time. Under such conditions, the CCE provides an exact description of the dynamics arising from the effective Hamiltonian (4) and thus accounts for the e–h correlations leading to the unadiabadic response of the FS to the pump pulse nonperturbatively \[beyond the Hartree–Fock approximation (HFA)\].

Our approach has a straightforward physical interpretation. The photoexcited e–h state $`𝒦(t,\tau )\stackrel{~}{U}_i^{}(\tau )|0`$, entering into (3), can be viewed as describing the propagation of the e–h pair with amplitude $`\mathrm{\Phi }_{ij}(𝐤,t)`$ excited by the probe pulse at time $`\tau `$, dressed by the scattering of the FS excitations (dynamical FS response). The latter leads to a dynamical broadening described by the amplitude $`s_{ij}(𝐩,𝐤,t)`$ that satisfies the differential equation

$`i{\displaystyle \frac{s_{ij}(𝐩,𝐤,t)}{t}}=(ϵ_{i𝐩}^cϵ_{j𝐤}^c)s_{ij}(𝐩,𝐤,t)`$ $`+{\displaystyle \underset{l}{}}[\mathrm{\Delta }ϵ_{il𝐩}^c(t)s_{lj}(𝐩,𝐤,t)\mathrm{\Delta }ϵ_{lj𝐤}^c(t)s_{il}(𝐩,𝐤,t)]`$ (8)   
$`{\displaystyle \underset{l}{}}\stackrel{~}{v}_{il}(𝐩,t)[\delta _{lj}+{\displaystyle \underset{q>k_F}{}}s_{lj}(𝐪,𝐤,t)],`$   
with initial condition $`s_{ij}(𝐩,𝐤,\tau )=0`$, and p and k labeling respectively the ($`i`$th subband) FS electron and the ($`j`$th subband) FS hole. Since only the first subband is occupied, the only non–zero components of $`s_{ij}`$ are $`s_{11}(𝐩,𝐤,t)`$ and $`s_{21}(𝐩,𝐤,t)`$, which describe the intra and intersubband FS excitations respectively. The photoexcited e–h pair wavefunction $`\mathrm{\Phi }_{ij}(𝐤,t,\tau )`$ satisfies the Wannier–like equation

$`i{\displaystyle \frac{\mathrm{\Phi }_{ij}(𝐤,t)}{t}}={\displaystyle \underset{l}{}}[ϵ_{il𝐤}^c(t)+\delta _{lj}[ϵ_𝐤^v(t)+ϵ_A(t)]i\mathrm{\Gamma }]\mathrm{\Phi }_{lj}(𝐤,t){\displaystyle \underset{l,q>k_F}{}}\stackrel{~}{v}_{il}(𝐤,t)\mathrm{\Phi }_{lj}(𝐪,t)`$ (9)   
with initial condition $`\mathrm{\Phi }_{ij}(𝐤,\tau )=\varphi _{ij𝐤}(\tau )`$, where $`ϵ_A(t)=_{k^{}<k_F}[v_{11}+_{p^{}>k_F}s_{11}(𝐩^{},𝐤^{},t)v_{11}]`$ is the self–energy due to the readjustment of the FS to the photoexcitation of a hole and $`\mathrm{\Gamma }`$ is the inverse dephasing time due to all the processes not included in $`H`$. In Eqs. (8) and (9), $`\stackrel{~}{v}_{ij}(𝐤,t)=v_{ij}_{l,k^{}<k_F}s_{il}(𝐤,𝐤^{},t)v_{lj}`$ is the effective e–h potential whose time–dependence is due to the dynamical FS response . Note that it is the interplay between this effective potential and the pump-induced self-energies that gives rise to the unadiabatic FS response to the pump field. In terms of $`\mathrm{\Phi }_{ij}(𝐤,t)`$, the polarization (3) takes the simple form ($`t>\tau `$)

$$P(t)=i_se^{i\omega _pt}\underset{ijl}{}\mu _i\mu _j\underset{k>k_F}{}\mathrm{\Phi }_{il}(𝐤,t)\varphi _{ij𝐤}^{}(t),$$
(10)   
with $`\varphi _{ij}(𝐤,t)`$ given by (6). The nonlinear absorption spectrum is then proportional to $`\mathrm{Im}P(\omega )`$, where $`P(\omega )`$ is the Fourier transform of the rhs of (10).

Numerical results.— Below we present our results for the evolution of the pump/probe spectra of the FES–exciton hybrid. The spectra were obtained by the numerical solution of the coupled equations (9) and (8), with the time–dependent band dispersions $`ϵ_{ij𝐤}^c(t)`$ and $`ϵ_𝐤^v(t)`$. The calculations were performed at zero temperature for below–resonant pump with detuning $`\mathrm{\Omega }E_F`$ and duration $`t_pE_F/\mathrm{}=2.0`$, and by adopting the typical values of parameters $`v_{12}/v_{11}=0.2`$, $`\mathrm{\Gamma }=0.1E_F`$, and $`v_{11}𝒩=0.3`$, $`𝒩`$ being the density of states, previously extracted from fits to the linear absorption spectra  ($`E_F1520`$ meV in typical GaAs/GaAlAs QW’s). Note, however, that similar results were also obtained for a broad range of parameter values. In Fig. 1(a) we plot the nonlinear absorption spectra at different negative time delays $`\tau <0`$. For better visibility, the curves are shifted vertically with decreasing $`|\tau |`$ (the highest curve represents the linear absorption spectrum). For the chosen value of $`\mathrm{\Delta }`$, the FES and excitonic components of the hybrid are distinguishable in the linear absorption spectrum, with the FES peak carrying larger oscillator strength. It can be seen that, at short $`\tau <0`$, the oscillator strength is first transferred to the exciton and then, with further increase in $`|\tau |`$, back to the FES. At the same time, both peaks experience a blueshift, which is larger for the FES than for the exciton peak because the ac–Stark effect for the exciton is weaker due to the subband separation $`\mathrm{\Delta }`$.

The transient exchange of oscillator strength originates from the different nature of the FES and exciton components of the hybrid. At negative time delays, the time–evolution of the exciton is governed by its dephasing time, which is essentially determined by the homogeneous broadening $`\mathrm{\Gamma }`$ (in doped systems the exciton–exciton correlations do not play a significant role due to the screening). The pump pulse first leads to a bleaching of the exciton peak, which then recovers its strength at $`|\tau |\mathrm{}/\mathrm{\Gamma }`$. On the other hand, since the FES is a many–body continuum resonance, (i) the bleaching of the FES peak is stronger, and (ii) the polarization decay of the FES is determined not by $`\mathrm{\Gamma }`$, but by the scattering with the low–lying FS excitations. This leads to much faster dynamics, roughly determined by the inverse Coulomb energy $`E_M`$ . However, the time–evolution of the hybrid spectrum is not a simple superposition of the dynamics of its components. Indeed, the pump-induced self-energies lead to the flattening of the subbands or, to the first approximation, to a time–dependent increase in the effective mass (and hence the density of states), which in turn increases the e–h scattering. Important is, however, that, due to the subband separation and different nature of the resonances, such an increase is stronger for the FES. Therefore, the effect of the pump is to reduce the excitonic enhancement of the FES peak (coming from the resonant scattering of the photoexcited electron by the exciton level) as compared to the linear absorption case, resulting in the oscillator strength transfer from the FES back to exciton. In fact, such a transfer is strong even for smaller $`\mathrm{\Delta }`$ \[see Fig. 1(b)\]. It should be emphasized that the above feature cannot be captured within the HFA. Indeed, the latter approximates the FES by a bound state and thus neglects the difference between the FES and exciton dynamics originating from the unadiabatic response of the FS to the change in the e–h correlations. This is demonstrated in Fig. 1(c) where we show the spectra obtained without the FS dynamical response, i.e., by setting $`s_{ij}=0`$. Although in that case both peaks show blue shift and broadening, there is no significant transfer of oscillator strength

In conclusion, we investigated theoretically the coherent nonlinear optical response of the FES–exciton hybrid in a QW with partially occupied subbands. We found a strong redistribution of the oscillator strength between the FES and exciton peaks which is caused by the different dynamics of the FES and exciton components of the hybrid as well as by their coupling due to the e–h correlations. This originates from the dynamical Fermi sea response and leads to a strong transient changes in the pump/probe spectra. Such systems can be used to probe the role of the many–body correlations in the Fermi liquid versus bound states dynamics.

This work was supported by the NSF grant ECS-9703453, and by HARL, Hitachi Ltd. The work of D.S.C. was supported by the Director, Office of Energy Research, Office of Basic Energy Sciences, Division of Material Sciences of the U.S. Department of Energy, under Contract No. DE-AC03-76SF00098.

FIG. 1