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Delay and distortion of light pulses by exciton resonances in wide-gap semiconductors

T. V. Shubina, Николай Алексеевич Гиппиус, Михаил Михайлович Глазов, Alexey A. Toropov, Galia Pozina, Bo Monemar

Published Jan 1, 2012• 0 citations
OpenAlex

Abstract

Propagation of light pulses in wide-gap semiconductors, GaN and ZnO, has been studied by time-of-flight spectroscopy. It has been demonstrated that significant light delay exists near an exciton resonance and that this delay is accompanied by pulse distortion and attenuation. Simulation of the pulse shape in the time-energy plane has permitted us to refine excitonic parameters inherent for bulk materials. The time-of-flight studies done over a wide temperature range demonstrate the strong influence of resonant scattering by phonons on the light delay in polar semiconductors. Optical dispersion at exciton resonances in semiconductors results in a delay of light transfer, which is induced by the variation of the group velocity — a phenomenon studied long ago(1-3). Thisdelayhasbeenobservedbytime-of-flightspec- troscopy in different semiconductors (4-6). The current inter- estinsuchretardationisenhancedbecauseitisoneoftheways toobtaintheso-calledslowlight,whichisneededforoptical communication and data processing. Wide-gap semiconduc- tors, like ZnO and GaN, possess strong excitonic resonances thatmakesthemsuitableforsuchapplication. Lightvelocities as low as 6000 km/s in ZnO (4) and 2100 km/s in GaN (5) have been recently measured. In view of these findings, the distortion of a pulse shape has attracted special attention (7). It is worth mentioning that early experiments showed no sig- nificant changes in the shape of a light pulse at the excitonic resonances in GaAs (8) and GaP (9), while the optical dis- persion near the resonances implies a different group velocity and attenuation for the higher- and lower-energy edges of the pulses (10), that inevitably means their distortion in the time- energy plane. The optical pulse modification is also important for a set of optoelectronic devices — high-frequency ones or those, where the light should propagate a long distance. The

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Propagation of light pulses in wide-gap semiconductors, GaN and ZnO, has been studied by time-of-flight spectroscopy. It has been demonstrated that significant light delay exists near an exciton resonance and that this delay is accompanied by pulse distortion and attenuation. Simulation of the pulse shape in the time-energy plane has permitted us to refine excitonic parameters inherent for bulk materials. The time-of-flight studies done over a wide temperature range demonstrate the strong influence of resonant scattering by phonons on the light delay in polar semiconductors. Optical dispersion at exciton resonances in semiconductors results in a delay of light transfer, which is induced by the variation of the group velocity — a phenomenon studied long ago(1-3). Thisdelayhasbeenobservedbytime-of-flightspec- troscopy in different semiconductors (4-6). The current inter- estinsuchretardationisenhancedbecauseitisoneoftheways toobtaintheso-calledslowlight,whichisneededforoptical communication and data processing. Wide-gap semiconduc- tors, like ZnO and GaN, possess strong excitonic resonances thatmakesthemsuitableforsuchapplication. Lightvelocities as low as 6000 km/s in ZnO (4) and 2100 km/s in GaN (5) have been recently measured. In view of these findings, the distortion of a pulse shape has attracted special attention (7). It is worth mentioning that early experiments showed no sig- nificant changes in the shape of a light pulse at the excitonic resonances in GaAs (8) and GaP (9), while the optical dis- persion near the resonances implies a different group velocity and attenuation for the higher- and lower-energy edges of the pulses (10), that inevitably means their distortion in the time- energy plane. The optical pulse modification is also important for a set of optoelectronic devices — high-frequency ones or those, where the light should propagate a long distance. The
We report on a strong delay in light propagation through bulk GaN, detected by time-of-flight spectroscopy. The delay increases resonantly as the photon energy approaches the energy of a neutral-donor bound exciton (BX), resulting in a velocity of light as low as 2100 km/s. In the close vicinity of the BX resonance, the transmitted light contains both ballistic and diffusive components. This phenomenon is quantitatively explained in terms of optical dispersion in a medium where resonant light scattering by the BX resonance takes place in addition to the polariton propagation.
Development of all-optical schemes of quantum communication and information processing implies a precise control of photon pulses—in particular, their spectral and temporal characteristics. Therefore “slow light”, propagating with a velocity much lower than the speed of light in vacuum, has been studied intensively in recent years. GaN and related materials are very promising for different applications in nanophotonics and optoelectronics. The advantages of time-of-flight spectroscopy to determine the parameters of bulk semiconductors, as well as investigation of the fine structure of an excitonic spectrum, are presented
We have identified several physical processes by which below-gap photons can modify excitonic absorption in GaAs quantum wells.1-3 These different phenomena can be distinguished by their temporal response times, which range from tens of nanoseconds to less than one picosecond. Our experiments also show that the relative contributions of these mechanisms to below-gap optical modulation of exciton absorption depend strongly on temperature as well as on the wavelength of the below-gap modulating beam. The size of the modulation indicates that a new class of absorptive and dispersive devices for optical signal processing is possible in which signals propagate in the transparent region of the crystal and experience negligible attenuation. In order to successfully interpret and calculate the magnitude of these exciting new effects, we show that it is necessary to take into account the special properties of two-dimensional excitons in semiconductor quantum wells.
The pulse distortion in GaAs quantum wells was studied by means of a light-gating technique. In the experiment, we used the incoherent picosecond pulse to observe accurately the changes of the coherent spike and its surrounding envelope. The experimental results clearly showed that the pulse is not anomalously delayed but is strongly distorted around the exciton resonance. We also compared the results with a computational simulation based on the absorption saturation mechanism. The simulated results agreed well with experimental results. The simulation showed that the recovery time of the exciton saturation is 90 ps around the tail part of the exciton absorption. We also observed a reduction of the coherent spike around the exciton resonance. Theoretical calculations indicate that the coherent-propagation effect in the linear absorber causes the reduction of the coherent spike.
This dissertation presents research on the propagation and manipulation of excitons in GaAs. There are three main aspects to be addressed. In the first part, we provide a comprehensive understanding of the slow- and fast-light propagation based on excitonic resonances. Propagation (or transit) times of optical pulses through a medium near an absorptive resonance with and without spatial dispersion are studied and contrasted. We show that, when the broadening of the resonance (i.e., dephasing rate) is below a critical value, a frequency range exists near resonance where the transit times are determined by interference between co-propagating exciton-polaritons and deviate strongly from expectations based on the group velocities of the individual exciton-polariton branches. Our theory puts the well-known slow- and fast-light effects in systems without spatial dispersion into a broader context by interpreting them as a limiting case of systems with spatial dispersion. An important ingredient of the exciton theory is the light-matter coupling that can be expressed either in terms of the dipole or the momentum matrix elements. We re-examine the validity of a frequently used relation between the interband momentum and dipole matrix elements ('p-r relation') in semiconductors. An additional correction term was obtained when we applied the 'p-r relation' to finite-volume crystals treated with periodic boundary conditions. The correction term does not vanish in the limit of infinite volume. We illustrate this with numerical examples for bulk GaAs and GaAs superlattices. For bulk GaAs, the correction term is found to be always important; while for a GaAs superlattice, the importance of the correction term for the transition depends strongly on the origin of the unit cell.As an example for manipulation of excitons, we consider mechanical deformations of GaAs nanomembranes. The nanomembranes with lateral sizes much larger than their thicknesses exhibit great flexibility in non-planar deformations and thus promise applications in flexible electronic and photonic devices. These non-planar deformations do not fit in the well-established theory for planar deformations induced by lattice mismatch. Our theory relates the general mechanical deformations (planar or non-planar) of nanomembranes to their excitonic spectra, and is numerically evaluated within the average-strain approximation.
The pulse velocity in the linear regime in samples of GaP: N with a laser tuned to the bound AAA-exciton line is measured with use of a picosecond time-of-flight technique. The pulse is seen to propagate through the material with little pulse-shape distortion, and with an envelope velocity given by the group velocity even when the group velocity exceeds 3\ifmmode\times\else\texttimes\fi{}1010{10}^{10}1010 cm/sec, $\mathrm{equals}\ifmmode\pm\else\textpm\fi{}\ensuremath{\infty}$, or becomes negative. The results verify the predictions of Garrett and McCumber.