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Physical Review Letters

Two-photon absorption spectroscopy in GaAs quantum wells

Kuochou Tai, A. Mysyrowicz, R. Fischer, Richard E. Slusher, A.Y. Cho

Published Apr 10, 1989• 74 citations
Publisher

Abstract

Two-photon absorption spectroscopy was performed in GaAs quantum wells with photon energy \ensuremath{\Elzxh}\ensuremath{\omega} near half the band gap ${\mathrm{E}}_{\mathrm{g}}$. For the case of incident light polarized perpendicular to the confinement direction \ensuremath{\epsilon}^\ensuremath{\perp}z^, the onset of two-photon absorption occurs at the 2P state of the lowest-energy heavy-hole exciton and the absorption increases linearly with 2\ensuremath{\Elzxh}\ensuremath{\omega}-${\mathrm{E}}_{\mathrm{g}}$. For \ensuremath{\epsilon}^\ensuremath{\parallel}z^, the two-photon spectrum is stepped with superpositions of sharp 1S exciton features at odd \ensuremath{\Delta}N light-hole--conduction-band transitions. These results are used to accurately determine exciton binding energy, successive subband energy splittings, and band offsets.

DOI
10.1103/physrevlett.62.1784

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Two-photon absorption spectroscopy was performed in GaAs quantum wells with photon energy \ensuremath{\Elzxh}\ensuremath{\omega} near half the band gap Eg{\mathrm{E}}_{\mathrm{g}}Eg​. For the case of incident light polarized perpendicular to the confinement direction \ensuremath{\epsilon}^\ensuremath{\perp}z^, the onset of two-photon absorption occurs at the 2P state of the lowest-energy heavy-hole exciton and the absorption increases linearly with 2\ensuremath{\Elzxh}\ensuremath{\omega}-Eg{\mathrm{E}}_{\mathrm{g}}Eg​. For \ensuremath{\epsilon}^\ensuremath{\parallel}z^, the two-photon spectrum is stepped with superpositions of sharp 1S exciton features at odd \ensuremath{\Delta}N light-hole--conduction-band transitions. These results are used to accurately determine exciton binding energy, successive subband energy splittings, and band offsets.
Photoconductivity measurements revealing two-photon absorption in GaAs/AlGaAs multiple quantum wells are presented. It is shown that both the forbidden 1S and the allowed 2P excitons can be observed. The energy separation between 1S and 2P excitons is determined directly from the absorption spectra to high accuracy. The data give evidence for two different absorption mechanisms: One is the two-photon absorption and the other one is the absorption of the second-harmonic wave which is generated inside the sample by nonlinear optical processes. By means of this additional absorption mechanism, the observation of the 1S excitions in two-phonon absorption spectra can be explained qualitatively.
We have measured two-photon-absorption spectra of GaAs/Al 0.4 Ga 0.6 As quantum-well structures in a static electric field for photon energies near half the band gap energy, and found drastic field-induced-changes in the spectra. The two-photon-absorption peak at half the energy of the lowest light-hole exciton is induced by the static electric field normal to the quantum well layers, in agreement with a theory that takes account of quasi-two-dimensional exciton effects. With increasing the electric field, however, this peak grows more drastically than the theoretical prediction, and it approaches a large value predicted by another simplified theory based on a two-level model.
We have investigated the polarization-dependent two-photon absorption in GaAs/AlGaAs quantum wires. The anisotropic selection rules of the multiphoton absorption process are exploited to study the one-dimensional 2p exciton states and the transitions between quantum wire subbands of different quantum numbers (\ensuremath{\Delta}ny{\mathit{n}}_{\mathit{y}}ny​\ensuremath{\ne}0 selection rule). The deviations from the selection rules derived for the strict one-dimensional case are discussed, and depend on the actual quasi-one-dimensional character of the excitonic wave functions.
Optical interband excitonic absorption of semiconductor quantum wells (QW’s) driven by a coherent pump field is investigated on the basis of semiconductor Bloch equations. The pump field has a photon energy close to the intersubband spacing between the first two conduction subbands in the QW’s. An external weak optical field probes the interband transition. The excitonic effects and pump-induced population redistribution within the conduction subbands in the QW system are included. When the density of the electron–hole pairs in the QW structure is low, the pump field induces an Autler–Townes splitting of the exciton absorption spectrum. The split size and the peak positions of the absorption doublet depend not only on the pump frequency and intensity but also on the carrier density. As the density of the electron–hole pairs is increased, the split contrast (the ratio between the maximum and the minimum values) is decreased, because the exciton effect is suppressed at higher densities owing to the many-body screening.
The dependence of the excitonic two-photon absorption on the quantum correlations (entanglement) of exciting biphotons by a semiconductor quantum well is studied. We show that entangled photon absorption can display very unusual features depending on space-time-polarization biphoton parameters and absorber density of states for both bound exciton states as well as for unbound electron-hole pairs. We report on the connection between biphoton entanglement, as quantified by the Schmidt number, and absorption by a semiconductor quantum well. Comparison between frequency-anti-correlated, unentangled and frequency-correlated biphoton absorption is addressed. We found that exciton oscillator strengths are highly increased when photons arrive almost simultaneously in an entangled state. Two-photon-absorption becomes a highly sensitive probe of photon quantum correlations when narrow semiconductor quantum wells are used as two-photon absorbers.