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1426 IEEE JOURNAL OF QUANTUM ELECTRONICS, VOL. 34, NO.

8, AUGUST 1998

Optical Characterization of Low-Temperature-Grown


GaAs for Ultrafast All-Optical Switching Devices
Hany S. Loka, Student Member, IEEE, Seldon D. Benjamin, and Peter W. E. Smith, Fellow, IEEE

Abstract— Low-temperature-grown GaAs (LT-GaAs) is a of 550 C–650 C. LT-GaAs is a high-quality single crystal
promising material for all-optical switching devices due to its with as much as 1%–2% excess arsenic incorporation [5],
outstanding optical characteristics. In this paper, we outline a which gives the material its unique properties. This excess
simplified model we have developed to describe the dynamics
of the carriers in this material. We also report the results of a arsenic is incorporated in the form of point defects [6]–[8].
series of measurements that we have performed to characterize Melloch et al. have shown that by annealing the LT-GaAs
the optical properties of the material. Specifically, we present the excess arsenic precipitates and forms arsenic clusters [9].
the first measurements of the two-photon absorption coefficient The number of point defects in the epilayers varies inversely
and the refractive index changes as a function of the growth
and annealing temperatures in LT-GaAs. Finally, we show how
with the growth and annealing temperatures [10]. On the
our model can be used to optimize the material for applications other hand, the size of the arsenic precipitates increases
in all-optical switching. with increasing annealing temperature and time [11], but the
Index Terms—Low-temperature-grown GaAs, nonlinear optics,
total amount of arsenic in the precipitates stays the same
optical materials, optical switches, time-resolved measurements. for the different annealing conditions. As-grown LT-GaAs
is conductive and it is only after annealing that LT-GaAs
becomes semi-insulating with resistivities up to 10 cm
I. INTRODUCTION [12]. There is considerable controversy surrounding the role

I N 1978, Mortani et al. were the first to investigate the


growth of GaAs by molecular beam epitaxy at temper-
atures lower than the regular material growth temperature
of point defects versus arsenic precipitates in explaining the
semi- insulating nature of annealed LT-GaAs [13], [14]. The
majority of the measurements done on LT-GaAs suggest
and predicted it to be a useful buffer layer for GaAs field- that the defect model dominates for as-grown and weakly
effect transistors (FET’s) [1]. Their experiments indicated annealed conditions, whereas the internal Schottky model
that the GaAs grown at 410 C can achieve a resistivity of tends to dominate for more strongly annealed materials [4].
3 10 cm. In this early work, however, they did not This continuous evolution from the point defect to the internal
adequately characterize the material to achieve the optimum Schottky model is accompanied by a smooth evolution of the
growth conditions. In 1988, Smith et al. successfully used optical and electrical properties.
GaAs grown at 200 C as a buffer layer in the fabrication of Several groups have shown that LT-GaAs can be tailored
GaAs FET’s and showed that this material eliminated backgat- to have subpicosecond carrier lifetimes [15]–[19]. As the
ing between devices [2]. Shortly thereafter, photoconductive intensity of the pump pulse is increased, a saturation of the trap
detectors fabricated with GaAs grown at 200 C and annealed states occurs. This saturation occurs from more electron–hole
at 600 C were shown to have switching speeds less than pairs being created than the number of trapping sites. The
500 fs with excellent sensitivity [3]. Since then there has been traps fill with electrons, and further removal of electrons
an increasing number of papers investigating the structural, from the conduction band can occur only after electrons in
optical, and electronic properties of GaAs grown by molecular the traps decay to the valence band. These ultrafast response
beam epitaxy (MBE) at very low substrate temperatures and measurements initiated our interest in investigating the optical
the processing and device applications of this material (for a characteristics of this material and its potential for ultrafast
recent review paper, see [4]). all-optical switching devices. In an earlier work, Benjamin et
The growth of low-temperature-grown GaAs (LT-GaAs) is al. [19] showed that LT-GaAs overcomes a tradeoff problem
performed at substrate temperatures between 200 C and 300 between sensitivity and response. They reported index changes
C at rates of 1 m/h. The growth temperatures are sub- as large as 0.1 with picosecond responses.
stantially lower than normal GaAs MBE growth temperatures In LT-GaAs the initial fast response is due to removal
of electrons from the conduction band, but it does not im-
Manuscript received December 11, 1997; revised April 22, 1998. This work ply electron–hole recombination. Recently, researchers have
was supported by Photonics Research Ontario and by the Natural Sciences and
Engineering Research Council of Canada. conducted experiments to measure the recombination times
H. S. Loka and P. W. E. Smith are with the Department of Electrical and in LT-GaAs [20]–[23]. The most extensive investigation was
Computer Engineering and Photonics Research Ontario, University of Toronto, done by Lochtefeld et al. [20], who looked at the role of point
Toronto, ON M5S 3G4, Canada.
S. D. Benjamin is with Corning Inc., Corning, NY 14831 USA. defects and arsenic precipitates on trapping and recombination
Publisher Item Identifier S 0018-9197(98)05409-8. times. In their measurements, they observed a saturation of
0018–9197/98$10.00  1998 IEEE
LOKA et al.: OPTICAL CHARACTERIZATION OF GaAs FOR ULTRAFAST SWITCHING DEVICES 1427

time to reach the bottom of the conduction band . Both the


carrier trapping times ( and ) and the trap emptying time
are strongly affected by material growth and annealing
conditions. The model can be applied irrespective of the details
of the processes responsible for the carrier trapping and recom-
bination. For unannealed LT-GaAs and LT-GaAs subjected to
weak anneals, the dynamics are dominated by As point defects.
For stronger anneals, the As clusters that are formed begin to
dominate the dynamics. The details of the trapping mechanism
are not critical since they can be all folded into a single
trapping time for a given material. We are phenomenologically
Fig. 1. Band diagram for low-temperature-grown GaAs showing the differ- describing the mechanism as due to midgap states with effec-
ent processes in the rate equation model.
tive trapping times ( and ) and trap emptying time .
Transitions between the valence band and the conduction
the trap states as the intensity of the pump pulse is increased band as well as the midgap states to the conduction band
(i.e., more electron–hole pairs are created than the number form the main contributions to the total population of excited
of recombination centers). The investigation by Siegner et al. carriers. We neglect the valence band to midgap states transi-
[21] was limited to unannealed samples and suggested that tion since the absorption cross section of the valence band to
electrons and holes are trapped in different point defects. Note midgap states is about an order of magnitude lower than the
that both groups used optical excitation at energy larger than one for the midgap states to the conduction band [27].
the bandgap of the material. Under those conditions they are In order to apply the rate-equation model to the study of the
probing the transients of the carriers in the conduction band dynamics of the optical properties of this material, we make
and are not directly probing the carriers in the midgap states the following assumptions: 1) , the number of carriers at the
where the recombination occurs. Even with a wavelength a few bottom of the conduction band and , the number of carriers
nanometers longer than the absorption edge, one will still be excited to higher states in the conduction band, both contribute
probing the carriers in the conduction band and the localized to refractive index changes; 2) , the number of carriers in
states below the conduction band and above the valence band the midgap states contribute to induced absorption; and 3)
contributing to the large absorption tail [23], [24]. Smith et , the carriers excited at the bottom of the conduction band
al. [23] investigated the recombination process by probing the contribute to absorption saturation. The equations describing
carriers in the midgap states using a wavelength well below the the time dynamics of the carriers in LT-GaAs are given by
band edge. They also showed that for probing at wavelengths
closer to the band edge one must take into account the large
absorption tail. In this paper, we will review our work on LT- (1)
GaAs and its applications in ultrafast all-optical devices. We
develop a phenomenological rate equation model to describe
the dynamics of the carriers in the material. We present the where is the band-to-band absorption coefficient, is the
experiments we used to optically characterize the material intensity of incident light with photon energy
for all-optical device applications. We also present the first
measurements of the two-photon absorption coefficient and (2)
refractive index changes and their dependence on growth and
annealing temperatures in LT-GaAs. Finally, we use the rate
equation model to demonstrate how to tailor the material for where is the absorption coefficient from the traps to excited
an optimum ultrafast all-optical switching device and consider states in the conduction band, and
the tradeoffs affecting the device performance.

II. RATE-EQUATION MODEL (3)


We have previously developed a rate-equation model for
optically induced effects in LT-GaAs, which we have shown where is the two-photon absorption coefficient. In all cases
to accurately predict the carrier dynamics over a wide range the decay times refer to the relaxation processes indicated in
of time frames, optical intensities, and wavelengths [25], [26]. Fig. 1. The total absorption is given by
Fig. 1 shows schematically the important excitation and decay
processes for excitation with optical signals having energies
larger than the bandgap. In this model, we assume a large (4)
density of midgap trap states. Carriers trapped in these midgap
states can be excited high in the conduction band by absorption where is the cross section for the band-to-band transitions,
of incident radiation. Our measurements showed that is the saturation carrier density, and is the cross section
for most conditions, carriers excited to states high in the for absorption from the traps to the excited states in the
conduction band will decay to trap states before they have conduction band.
1428 IEEE JOURNAL OF QUANTUM ELECTRONICS, VOL. 34, NO. 8, AUGUST 1998

III. EXPERIMENTAL MEASUREMENTS


Our previous measurements [19], [25], [26], [28] were
obtained using samples with different growth temperatures
and annealing conditions than the samples reported here,
which have a broader range of annealing conditions. Since
the samples were grown in different reactors and since the
determination of the substrate temperature is inaccurate at
these temperatures, it is difficult to directly compare this work
with our previous work. The trends observed are consistent
and the model can be used to predict the dynamics of the
optical properties of samples from either set equally well.
The samples characterized in this work were grown on a n-
type (n 10 cm ) GaAs substrate by MBE, and consisted
of a 500-Å AlAs lift off layer; and a 1.5- m LT-GaAs layer (a)
grown at 270 C or a 1.07- m LT-GaAs layer grown at 220
C. Because of the inevitable uncertainty associated with the
accurate determination of the substrate temperature at such
low values, the amount of excess arsenic incorporated in the
material is used as the true measure to compare material
grown by different systems. The amount of excess arsenic
can be estimated by using the X-ray diffraction measurement
along with the expression derived by Liu et al. relating the
X-ray splitting to the concentration of arsenic antisite (As )
defects [29]. The X-ray diffraction measurements for the two
samples showed a splitting of 80 and 110 corresponding
to (As ) concentration of 4.83 10 cm and 6.64 10
cm for the 270 C and 220 C, respectively.
The two samples were cleaved into pieces 4 10 mm then (b)
rapid thermal annealed for 30 s at temperatures from 500 C Fig. 2. Normalized transmittance as a function of sample position (z -scan
to 900 C with steps of 100 C. To avoid effusion of As =
data) at  900 nm for (a) a sample grown at 220  C and annealed at 800
during annealing, the samples were placed upside down onto a 
 C using a 150-fs pulse with average power 9 W and spot size 2 m 
and (b) sample grown at 270  C and annealed at 700  C using a 150-fs pulse
GaAs wafer. The LT-GaAs layer is then lifted off the substrate  
with average power 13 W and spot size 1.6 m. The solid lines are
[30], cemented onto a glass slide, and antireflection coated on the theoretical results and were fit with (a) = 34 cm/GW and (b) =
one side to eliminate Fabry–Perot resonances. The following 35 cm/GW.
measurements were obtained using a mode-locked Ti:sapphire
laser as the excitation source. The -scan signature for the TPA is opposite to the single-
photon absorption (SPA) (direct band-to-band absorption or
A. Model Constants a two-step midgap state mediated process). For TPA, the
In this section we determine the constants needed for the rate transmitted power decreases with increasing incident power
equation model in order to use it to describe our experimental and is minimum at the beam focus as shown in
results. Fig. 2, whereas for SPA the transmitted power increases with
1) Two-Photon Absorption (TPA) Measurements: We demon- increasing incident power (absorption saturation).
strate the first direct measurement of the two-photon absorp- By fitting the simulations (the TPA coefficient is the only
tion (TPA) coefficient in LT-GaAs and show how it varies with unknown) to the experiments, we can obtain the values for the
growth and annealing temperatures. When the incident field TPA coefficient. In Fig. 2 we show the normalized transmit-
wavelength is such that , electrons make tance as a function of sample position for the sample grown
the transition from the valence band to the conduction band at 220 C and annealed at 800 C and the sample grown at
by simultaneously absorbing two photons. The strength of this 270 C and annealed at 700 C at 900 nm. The best fit
process is described by the TPA coefficient . for the two samples was achieved by using a TPA coefficient
To estimate the TPA coefficient we used a -scan [31] setup equal to 34 and 35 cm/GW, respectively.
(single beam measurement) and measured the light transmitted In Fig. 3 we show that the samples annealed at low tempera-
through the sample. The transmitted power through the sample tures have a TPA coefficient almost double the values reported
is measured as a function of the sample position. Although for regular GaAs [32]. The TPA coefficient decreases with
the input power is kept constant, the sample experiences increasing annealing temperatures and approaches the values
different incident intensities at different positions. Since we for regular GaAs ( 26 cm/GW [32]) under substantial anneal-
are using high input power and operating at the band tail, ing. We also observed that the value of the TPA coefficient is
we expect TPA to dominate over single photon absorption. smaller for higher growth temperatures, as shown in Fig. 3.
LOKA et al.: OPTICAL CHARACTERIZATION OF GaAs FOR ULTRAFAST SWITCHING DEVICES 1429

(a)
Fig. 3. Experimental measurements of the TPA coefficient as a function of
growth and annealing temperatures for LT-GaAs grown at 220  C and 270
 C and annealed at different temperatures.

We verified that the measured TPA coefficient is independent


of the excitation spot size.
The large TPA coefficient measured in LT-GaAs could be
used to advantage in optical limiting [32] and autocorrelation
devices [33].
2) Trapping Times: The electron trapping time is mea-
sured with a typical pump-probe experiment [34]. Carriers at
the bottom of the conduction band are created by a pump
at a wavelength resonant with the bandgap (870 nm), while
the probe (at the same wavelength) is used to monitor the (b)
dynamics of the carriers at the bottom of the conduction band.
Fig. 4. Normalized dynamic transmission changes after excitation with a
This technique is sensitive to the electron population in the =
150-fs pulse at a wavelength ( 870 nm) resonant with bandgap for (a) the
conduction band due to the much larger density of states in the sample grown at 220  C and (b) the sample grown at 270  C. The optically
valence band. The pump beam is chopped at 2 kHz and focused excited carrier density is 1018 cm03 .

to a 14- m-diameter spot on the samples and the delayed probe
beam is focused to a slightly smaller area inside the pump representing the trapping of the carriers at the bottom of the
spot. Pump and probe average power levels are 1 mW and conduction band . Another observation is the induced
4 W, respectively. Changes in the transmitted probe power absorption for the unannealed sample and this
that are caused by the presence of photogenerated carriers from is attributed to a build up of population in the trap states.
the pump beam are recorded using a lock in amplifier as a The slow decay from the trap states leads to a large excess
function of the time delay between the pump and probe pulses. population of trapped carriers ( annealed samples), which
The photocarrier lifetime for the material is defined as can build up as a result of the fast trapping process.
the time it takes the transmission change to drop to its 3) Trap Emptying Times: Rapid trap emptying times are
maximum value. essential for any application which requires not only a material
From Fig. 4(a) and (b) we see that the trapping rates that has a fast response but also one that recovers to its
increase with lower growth and annealing temperatures. These equilibrium state rapidly. To measure the trap emptying times,
measurements are consistent with what has been reported we used the same pump–probe experimental setup [34] but at
in the literature [15]–[19]. For lower growth temperatures, a longer wavelength (970 nm) where the sample is transparent
the amount of excess As (point defects and As clusters) and thus does not exhibit the absorption saturation observed
incorporated into the material is increased leading to an for the bandgap resonant pumping. By using a high-intensity
increased trapping rate. Under higher temperature anneals, pump, we can excite carriers in the conduction band primarily
the number of point defects decreases and the number of As through TPA. These carriers have high excess energy and are
precipitates decreases as they coarsen, leading to a reduced rapidly trapped into the midgap states. This build-up of
probability of the carriers being trapped and a longer carrier population in the midgap states results in an increase in the
lifetime. trap related absorption, which subsequently decays with the
Two features are observed in the measurements shown in time constant (recombination time for the trapped carriers).
Fig. 4(b) for the sample grown at 270 C. For the annealed From Fig. 5, it can be seen that with the different annealing
samples the initial fast decay for times less than 1 ps is due temperatures the trap emptying times vary from 2 to 10
to redistribution of the carriers out of their initial states by ps. For the more strongly annealed samples, the trap emptying
carrier–carrier scattering. This is followed by a longer decay times are slower, and this can be understood in terms of the
1430 IEEE JOURNAL OF QUANTUM ELECTRONICS, VOL. 34, NO. 8, AUGUST 1998

Fig. 7. Absorption coefficient of the sample grown at 270  C and annealed


at different temperatures as a function of the wavelength.

Fig. 5. Normalized dynamic absorption changes after excitation with a


=
150-fs pulse at a wavelength ( 970 nm) well below the band gap for the increase is primarily due to the existence of localized (shallow)
sample grown at 270  C. The optically excited carrier density is 1018 cm03 .
 states formed by potential fluctuations, which are weakly cou-
pled to their respective bands and the midgap states. We would
expect carriers in these states to have relatively long lifetimes
and absorption saturation due to carriers in these states to be
relatively long lasting [23], [24]. Thus, we interpret the long
absorption saturation tails seen near the band edge in weakly
annealed samples (Figs. 5 and 6) to carriers excited to these
shallow states by one-photon absorption from the pump pulse.
For the stronger (higher temperature) annealed samples, the
decay process is nonexponential and has a long tail of
induced absorption. In these samples the arsenic clusters have
to be considered. From Nolte’s calculations [35], the arsenic
(metallic) clusters contribute to an extra absorption component,
which is proportional to cube of the diameter of the arsenic
clusters.
The absorption measurements in Fig. 7 also show that for
photon energies above the bandgap, the defect absorption is
Fig. 6. Normalized dynamic absorption changes after excitation with a
150-fs pulse at a wavelength ( =
905 nm) well below the bandgap
strongly reduced by annealing due to the reduction of the
for the sample grown at 270  C. The optically excited carrier density is point defects, which is similar to the measurements reported
23 1018 cm03 . by Streb et al. [36]. For the lightly annealed samples, we
observe smearing of the band edge due to the substantial
reduced number of midgap states present in the more strongly concentration of defects, resulting in a significant increase
annealed samples. in one-photon absorption from these defects, and only at
For the weakly annealed samples (30 s at 500 C and annealing temperatures above 600 C we see clear indication
600 C), absorption increases in a time on the order of the 150- of a band edge structure.
fs pump pulse, indicating that carriers high in the conduction For the strongly annealed temperatures (800 C and 900
band are trapped rapidly compared to those near the C), the band edge structure becomes more pronounced and
bottom of the band which are trapped in 1 ps or more for it starts to approach the sharpness of regular GaAs. Similar
these same samples. The strongly annealed samples (30 s at features were observed in the absorption measurements on the
800 C and 900 C) show a pronounced rising edge (with a sample grown at 220 C.
time constant of 0.6 and 1 ps, respectively) to the onset of We have also shown how the number of carriers excited
the induced absorption which indicates that the trapping time can affect the trap emptying process [23]. For the sample
of carriers placed high in the conduction band also increases grown at 270 C and annealed at 800 C, carrier densities
with stronger anneals. higher than 10 cm present a bottleneck and the trap
For wavelengths closer to the band edge, significant long emptying time approaches 100 ps [23]. There is a tradeoff
time constant phenomena are observed, as shown in Fig. 6. For between long lasting carriers in the shallow states in weakly
the weak (low-temperature) annealing samples, a substantial annealed material and the reduced number of midgap states
longterm absorption saturation component is observed. This and the effect of the clusters in the strongly annealed material.
can be understood by taking into account the large absorption Therefore, optimum growth and annealing temperatures have
increase, which extends over the whole wavelength’s range for to be considered to reduce the localized states and to avoid
weakly annealed samples, as shown in Fig. 7. This absorption the bottleneck due to the reduced number of midgap states.
LOKA et al.: OPTICAL CHARACTERIZATION OF GaAs FOR ULTRAFAST SWITCHING DEVICES 1431

TABLE I
N
SATURATION CARRIER DENSITY o CHANGE WITH WAVELENGTH FOR THE
SAMPLE GROWN AT 270  C AND ANNEALED AT 800  C OBTAINED FROM THE
SIMULATIONS USED TO FIT THE QUASI-STEADY-STATE MEASUREMENTS

Fig. 8. Average absorption coefficient as a function of average light intensity


in a sample grown at 270  C and annealed at 800  C during the passage of
3-ps pulses at various wavelengths. Solid curve is from computer simulation
based on rate equations.

4) Absorption Cross-Section Measurements: Absolute mea-


surements of the changes in probe absorption observed in the
previous experiment are used to characterize the strength of the
cross section for absorption from the trap states back into the
conduction band. This additional absorption is described by
(5)
where is the absorption cross section for the midgap states.
To measure the strength of the absorption cross section for
(a)
the sample grown at 270 C and annealed at 700 C and 800
C, we used an intense pump at 880 nm to pump carriers
via TPA high in the conduction band producing 10 cm
carriers. These carriers get trapped in the midgap states in
less than 1 ps, generating carrier concentration in the midgap
states 10 cm . For the weak probe at 880 nm, we
measured at this carrier density of 4600 cm , giving a
corresponding 5 10 cm from (5).
From our measurements, along with the simulations using
the rate equation model, we found that is not affected by the
annealing temperatures. We believe this is because the amount
of excess arsenic is the same (either in the form of point defects
or arsenic clusters) for a specific growth temperature. For the
samples grown at 220 C, the absorption cross section was
(b)
measured to be 3 10 cm .
Fig. 9. Average absorption coefficient changes induced by 3-ps pulses as a
=
function of average light intensity at a wavelength  870 nm in (a) samples
grown at 270  C and annealed at 700  C, 800  C, 900  C, and (b) a sample
B. Model Validation grown at 220  C and annealed at 900  C. Solid curve is from computer
simulation of rate equations.
In this section, we present measurements of the nonlinear
optical properties that are most critical for device design and
use these measurements to validate our model. bottom of the conduction band is close to a linear function of
1) Quasi-Steady-State Experiments: In these measurements, the wavelength, as shown in Table I.
a steady-state population distribution is assumed to be reached Absorption saturation for longer wavelengths can be
during the 3-ps pump pulse. All measurements are averaged achieved at lower powers since less photons are needed to
over the pulse duration. saturate the reduced number of states available at the bottom
a) Absorption saturation: As shown in Fig. 8, we mea- of the conduction band for these wavelengths.
sured in a sample grown at 270 C and annealed at 800 C the In Fig. 9 we show how different growth and annealing
absorption coefficient as a function of light intensity from a conditions affect the absorption saturation in LT-GaAs. The
wavelength resonant with the bandgap (870 nm) to excitation measurements were done at a wavelength resonant with the
energies higher than the energy gap of the material (830 nm). bandgap (870 nm) for the samples grown at 270 C and
From the absorption measurements and the fits with the model annealed at 700 C, 800 C, and 900 C and the sample grown
we found that the absorption saturation carrier density at the at 220 C and annealed at 900 C.
1432 IEEE JOURNAL OF QUANTUM ELECTRONICS, VOL. 34, NO. 8, AUGUST 1998

TABLE II
COMPARISON OF THE TIME CONSTANTS FOR THE SAMPLES GROWN AT 270  C AND ANNEALED AT
 
700 C, 800 C, AND 900 C AND THE SAMPLE GROWN AT 220  C AND ANNEALED AT 900  C


Sample grown at 270  C and annealed for 30 s at Sample grown at 220  C and anneled for 30 s at

700  C 800  C 900  C 900  C


1 2 ps 4.5 ps 7 ps 2.5 ps
2
1 1 1 1
6.4 ps 9.5 ps 15.4 ps 9 ps
3
4 0.3 ps 0.6 ps 1.1 ps 0.1 ps

For the measurements in Figs. 8 and 9, the absorption


saturation is only partial, in contrast to the complete saturation
observed in regular GaAs [37]. The incomplete absorption
saturation in LT-GaAs is due to the large number of midgap
states. We also observe that the change in absorption is
increased for the samples grown and annealed at higher tem-
peratures since the concentration of midgap states is decreased.
But still the absorption saturation is incomplete for the strongly
annealed samples resulting from the excess residual absorption
due to optical absorption in a composite material of dilute
spherical particles embedded in an absorbing medium [35].
In Figs. 8 and 9, no variations with respect to time in our
model (1)–(3) are assumed to obtain the steady-state carrier (a)
densities. These values along with the assumption of no TPA
are then used in (4) to calculate the absorption.
b) Refractive index changes: In Fig. 10, we show the
results of measurements, using the -scan technique [31], of
the average index change induced in the material during the
time the pulse is passing through the samples, as a function
of the incident light intensity. In previous measurements for
different growth conditions we have observed the largest
known refractive index changes (three times larger than regular
GaAs [37]) with picosecond response [19]. For the growth and
annealing conditions used in this paper, we measure index
changes that are approximately two times larger than those
observed for regular-temperature-grown GaAs [37]. The index (b)
changes measured are not caused by thermal effects because Fig. 10. Average refractive index changes induced by 3-ps pulses of varying
the -scan signature is opposite for a thermal nonlinearity =
light intensity at a wavelength  870 nm in (a) samples grown at 270  C
(positive) and the laser pulse repetition rate was reduced to and annealed at 700 C, 800  C, and 900  C, and (b) sample grown at 220
 C and annealed at 900  C. Solid curve is from computer simulation of rate
4 kHz to minimize any possible thermal problems. equations.
From Fig. 10 and earlier measurements reported in [28], it
appears that the refractive index changes for a given light
intensity increase with growth temperatures increase up to the rate equation model for steady-state conditions. Then
an optimum growth value and then it starts decreasing ap- we calculate the carrier-induced refractive index changes by
proaching regular GaAs index changes. It also appears that the using the theory of Banyai and Koch [39] for GaAs which
refractive index changes increase with annealing temperatures takes into account exciton effects, band filling, and bandgap
increase except for the sample grown at 270 C and annealed at renormalization. We believe that using the Banyai and Koch
900 C. Liliental-Weber et al. [38] have shown a degradation theory reasonably depicts the refractive index changes in LT-
in the quality of LT-GaAs annealed at high temperatures due to GaAs due to the material’s good crystalline quality.
As effusion. Some indication for the degradation of the sample Good agreement is found between the quasi-CW experimen-
grown at 270 C and annealed at 900 C can be seen in the tal measurements (absorption saturation and refractive index
absorption measurements shown in Fig. 7, where we obtain changes) and the predictions of the model at steady state for
a higher value for the absorption coefficient over the whole the conditions shown in Table II.
wavelength range. Still, for this sample, the pronounced band 2) Ultrafast Dynamic Measurements: Here we are using a
edge structure is obtained with a slight red shift. 150-fs pump-probe setup to reveal the detailed ultrafast dy-
For the theoretical simulations we calculate the total number namics and for each case our rate-equation model is fitted
of carriers excited in the conduction band by using to the experimental data. Initial experiments with a relatively
LOKA et al.: OPTICAL CHARACTERIZATION OF GaAs FOR ULTRAFAST SWITCHING DEVICES 1433

TABLE III
COMPARISON OF THE TIME CONSTANTS USED TO FIT RATE-EQUATION MODEL TO
EXPERIMENTAL DATA FOR GAAS GROWN AT 270  C AND ANNEALED AT 800  C
EXCITED AT 870 NM WITH (A) 3-PS PULSES (QUASI-CW) AND (B) 150-FS PULSES

(a) The long process can be understood as a manifestation


of the phonon bottleneck effects in LT-GaAs reported in [41].
For the sample grown at 270 C and annealed at 800 C,
Table III compares the time constants found from the rate
equation fits for the dynamic data with the quasi-CW data.
It can be seen that very good agreement is obtained, even
though, for the 150-fs case, TPA effects play an important
role, and no assumptions of steady-state carrier concentrations
under the optical excitation are made.
In the simulations for the rate-equation model in both the
quasi-steady-state and ultrafast dynamic cases,
and were used as fitting parameters. With our rate-equation
model, we succeeded in fitting experimental measurements
obtained with different pulsewidths and wavelengths. This
(b) gives us confidence in the validity of our model since a good fit
cannot be obtained if any of the fitting parameters are varied
Fig. 11. (a) Probe transmission change versus delay from pump for GaAs
grown at 270  C and annealed for 30 s at 800  C at a wavelength  = by more than 10%.
870 nm. (b) Normalized dynamic absorption change versus delay from pump
for GaAs grown at 270  C and annealed for 30 s at 800 C at a wavelength
=
 970 nm. The continuous line is the dynamic behavior predicted by our IV. MATERIAL OPTIMIZATION FOR ALL-OPTICAL SWITCHING
rate-equation model.
In this section we will use the model we have developed to
show how material parameters can be optimized and tailored
for device applications. We will investigate the design of two
weak saturating pulse at a wavelength resonant with the band types of all-optical switching devices using LT-GaAs.
gap ( 870 nm) exhibit a fast rise followed by a single
exponential decay of absorption saturation (due to band filling) A. Refractive Index Change-Based Device
providing a direct measurement of the trapping time , as For an ultrafast compact all-optical waveguide-based device,
seen in Fig. 11(a). an ideal material would have a large nonlinear refractive index
In Fig. 11(b), we show different pump-probe dynamics change, fast response time, no competing effects (e.g., thermal
where we are measuring the increase in absorption at a effects). It should also be compatible with other technolo-
longer wavelength (970 nm). The initial fast rise in absorption gies with which it must interface and have low loss at the
increase is due to the fast trapping of the carriers excited wavelength of interest. For the nonlinear optical materials that
high in the conduction band and the slow exponential decay are currently available, there is a tradeoff between sensitivity
represents the recombination (trap emptying) process . For and speed. We have shown that with LT-GaAs, it is possible
this case ( 970 nm), the carriers pumped via the TPA to obtain both large nonlinear effects and ultrafast response.
mechanism will be excited lower in the conduction band (i.e., This material exhibits an enhanced bandgap resonant index
lower carrier velocity) than the previous case ( 870 nm). change with recovery time 1 ps. LT-GaAs satisfies many
We would expect the trapping time to be longer at longer of the requirements of an ideal material for ultrafast all-
pump wavelengths, since we expect the carrier trapping time optical device applications except for the substantial loss due
by the midgap states to be inversely proportional to the carrier to the unsaturated absorption even for the highly annealed
velocity [40]. In the model fit we used a trapping time material, as shown in Fig. 6. For waveguide-based devices
1 ps which is longer then measured for the 870-nm case using a resonant nonlinearity, there is a tradeoff between the
( 0.5 ps). We extrapolated the value for the saturation absorptive loss and the index change and accordingly the
carrier density at 970 nm ( 1.2 10 cm ) from the data excitation beam for a single wavelength operation has to be
in Table I. detuned below the bandgap energy. For our case, we will
1434 IEEE JOURNAL OF QUANTUM ELECTRONICS, VOL. 34, NO. 8, AUGUST 1998

operate at 900 nm since starting at this wavelength


the unsaturated absorption is constant and by moving to a
longer wavelength the refractive index change is reduced.
On the other hand, by moving to a shorter wavelength,
we will incur the higher absorption losses. Thus we expect
optimum operation (minimum loss and maximum refractive
index change) will occur in the region around 900 nm.
We will use our model to investigate the dynamic behavior
of the various absorption mechanisms in LT-GaAs and try to
tailor the material to minimize the unsaturated absorption. We
used our model to investigate the effect of changing the values
of the different constants for the sample grown at 270 C and
annealed at 800 C on the optical properties of the material.
We found that changing the values for and does not (a)
substantially affect the absorption saturation. But changing
has a pronounced effect on the amount of absorption
saturation as seen in Fig. 12(a). Fig. 12(b) and (c) show
the behavior of the various pertinent absorption mechanisms
using the parameters measured for the sample grown at 270
C and annealed at 800 C for different pulsewidths and
input intensities, respectively. From Fig. 12, we see that the
total absorption near the pulse maximum is 50 cm . This
absorption saturation occurs for a peak power of 10 W,
assuming a cross-sectional area of 1 m in a waveguide.
The maximum waveguide length is limited by the absorption
length to 200 m. For the conditions of Fig. 12, the total
carrier concentration generated in the conduction band of the
LT-GaAs is approximately 10 cm , which corresponds to
an average refractive index change of 0.025. With this index
change, we can produce a nonlinear phase change of several
(b)
times 2 in our maximum waveguide length.
Various figures of merit have been used in the literature to
compare nonlinear optical materials. In the case where both
the one-and the two-photon absorption processes affect the
absorption length, a figure of merit is defined by [42]

Figure of merit

where is the light-induced index change, is the total


absorption, and is the incident light wavelength. For
0.025, 50 cm , and 900 nm, the figure of merit
is equal to 5.5. This value was calculated at the peak of
the control pulse assuming constant absorption and refractive
index change values along the guiding medium. In reality, this
is not the case and the waveguide has to be divided into shorter (c)
sections, then the rate equation can be applied separately for Fig. 12. Calculated total absorption at  = 900 nm due to single-photon
each division with the results of the previous section as the band-to-band absorption, traps-to-band absorption, and TPA processes using
the time constants of GaAs grown at 270  C and annealed for 30 s at 800  C
new initial conditions. By performing a crude calculation of
after excitation by a 1-ps pulse and Ii= 2 3 109 W/cm2 showing the effect
propagating the pulse along the guide, we found that only 10% of changing (a) 1 , (b) incident pulsewidth, and (c) incident intensity.
throughput for the maximum absorption length 200 m was
obtained. Also, the figure of merit will decrease along the
waveguide from 5.5 to 0.5. On the other hand, we could not region since the input power will only drop by a factor of
increase the input power in order to keep the absorption and three and we find that the figure of merit will only decrease to
index change values in the saturation region because the TPA 3.0. It should be noted that a shorter waveguide device may
effect will then increase dramatically. One way to overcome be harder to fabricate.
this problem is to use a shorter waveguide. With a 100- m- The figures of merit calculated show that LT-GaAs can be
long waveguide, we will be mostly operating in the saturation used in a waveguide device. But with the inherent problem of
LOKA et al.: OPTICAL CHARACTERIZATION OF GaAs FOR ULTRAFAST SWITCHING DEVICES 1435

unsaturated absorption in the material, the device operation is The trapping and trap emptying (recombination) times increase
not efficient and the powers needed are impractical. with increasing the growth and annealing temperatures due
We have investigated a more practical all-optical switching to the reduced number of midgap states. Both processes are
device for this material where we can accommodate high affected by the number of excited carriers and are drastically
absorption values and make use of the high absorption changes slowed down at carrier concentrations larger than 10 cm .
obtained in LT-GaAs. The control of growth and annealing temperatures can be
used to tailor the material to fulfill the requirements for
B. Absorption Saturation-Based Device different ultrafast all-optical devices. For example, the large
We have investigated the use of LT-GaAs in an asymmetric TPA coefficient can be used in advantage for optical limiting
and autocorrelation devices. Finally, we have discussed the
Fabry–Perot (AFP) device operating in the reflection mode
use of LT-GaAs in ultrafast all-optical switching and have
with a low-reflectivity front mirror ( 2%) on one side
and a high-reflectivity back mirror ( 100%) on the other shown that the absorption-based device is more suitable than
side. We have operated the device in reflection rather than the index change-based device for this material.
transmission so we can accommodate higher absorption in the
active layer. Absorption reduces the absolute transmission but ACKNOWLEDGMENT
need not lead to either a low maximum reflection or to a small
difference between maximum and minimum reflectivity [43]. The authors would like to thank Prof. D. Thompson and
Also, by operating in reflection the critical switching energy Dr. B. Robinson at McMaster University for growing the LT-
is reduced [43]. GaAs samples, Prof. P. Mascher of McMaster University for
Mathematically, if the cavity has no loss and the bottom the AR coatings, and Prof. H. E. Ruda of the University of
mirror has reflectivity of one, the reflectivity of the AFP is Toronto for annealing the samples.
unity. The off level is provided by increasing the loss in the
cavity so that the effective reflection from the bottom mirror
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[23] P. W. E. Smith, S. D. Benjamin, and H. S. Loka, “Tailoring of trap-
related carrier dynamics in low-temperature-grown GaAs,” Appl. Phys. Hany S. Loka (S’98) was born in Cairo, Egypt, on
Lett., vol. 71, pp. 1156–1158, 1997. November 6, 1966. He received the B.Sc. degree
[24] G. Segschneider, T. Dekorsy, H. Kurz, R. Hey, and K. Ploog, “Energy (distinction with honors) in communications and
resolved ultrafast relaxation dynamics close to the band edge of low- electronics engineering and the M.Sc. degree in
temperature grown GaAs,” Appl. Phys. Lett., vol. 71, pp. 2779–2781, engineering physics from Cairo University in 1989
1997. and 1993, respectively. He is currently working
[25] S. D. Benjamin, H. S. Loka, A. Othonos, and P. W. E. Smith, “Ultrafast toward the Ph.D. degree in electrical and computer
dynamics of nonlinear absorption in low-temperature-grown GaAs,” engineering at the University of Toronto, Toronto,
Appl. Phys. Lett., vol. 68, pp. 2544–2546, 1996. ON, Canada.
[26] S. D. Benjamin, H. S. Loka, and P. W. E. Smith, “Tailoring of low- He is currently working on the optical charac-
temperature-MBE-grown GaAs for ultrafast photonic devices,” Can. J. terization of low-temperature-grown GaAs and the
Phys. (Suppl.), vol. 74, pp. 685–689, 1996. design of all-optical switching devices. From 1989 to 1993, he worked as an
[27] P. Silverberg, P. Omling, and L. Samuelson, “Hole photoionization cross Assistant Lecturer in the Faculty of Engineering at Cairo University. From
sections of EL2 in GaAs,” Appl. Phys. Lett., vol. 52, pp. 1689–1691, 1990 to 1993, he was in the automatic control department at Eletech (Siemens
1988. AG sole agent in Egypt), where he worked on implementing Siemens PLC’s
[28] P. W. E. Smith and S. D. Benjamin, “Materials for all-optical devices,” in new factories, updating old PLC systems, and training engineers in charge
Opt. Eng., vol. 34, pp. 189–194, 1995. of these systems. His research interests are characterization of semiconductor
[29] X. Liu, A. Prasad, E. R. Weber, Z. Liliental-Weber, and W. Walukiewicz, materials for ultrafast all-optical signal processing, fiber gratings, and fiber
“Native point defects in low-temperature-grown GaAs,” Appl. Phys. optic sensors.
Lett., vol. 67, pp. 279–281, 1995. Mr. Loka is a member of the Optical Society of America and a member of
[30] E. Yablonovich, T. Gmitter, J. P. Harbison, and R. Bhat, “Extreme the Egyptian Society of Engineers (ESE).
selectivity in the lift-off of epitaxial GaAs films,” Appl. Phys. Lett.,
vol. 51, pp. 2222–2224, 1987.
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Stryland, “Sensitive measurement of optical nonlinearities using a single
beam,” IEEE J. Quantum Electron., vol. 26, pp. 760–769, 1990.
[32] T. F. Boggess, Jr., A. L. Smirl, S. C. Moss, I. W. Boyd, and E. W. Van
Stryland, “Optical limiting in GaAs,” IEEE J. Quantum Electron., vol.
QE-21, pp. 488–494, 1985.
[33] N. M. Karkhanehchi, C. J. Hamilton, and J. H. Marsh, “Autocorrelation
measurements of modelocked Nd:YLF laser pulses using two-photon
absorption waveguide autocorrelator,” IEEE Photon. Technol. Lett., vol. Seldon D. Benjamin was born in Fox River, Nova
9, pp. 645–647, 1997. Scotia, Canada on February 11, 1962. He received
[34] F. E. Doany, D. Rischkowsky, and C. C. Chi, “Carrier lifetime versus the B.S. degree in electrical engineering from Rens-
ion-implantation dose in silicon on sapphire,” Appl. Phys. Lett., vol. 50, selaer Polytechnic Institute, Troy, NY, in 1986, and
pp. 460–462, 1987. the M.S. and Ph.D. degrees in electrical engineering
[35] D. D. Nolte, “Optical scattering and absorption by metal nanoclusters from North Carolina State University in 1988 and
in GaAs,” J. Appl. Phys., vol. 76, pp. 3740–3745, 1994. 1991, respectively.
[36] D. Streb, M. Ruff, S. U. Dankowski, P. Kiesel, M. Kneissl, S. Malzer, U. From 1992 to 1997 he worked as a Senior Re-
D. Keil, and G. H. Döhler, “Optical characterization of low temperature search Associate in the Department of Electrical and
grown GaAs by transmission measurements above the band gap,” J. Computer Engineering at the University of Toronto,
Vac. Sci. Technol. B, vol. 14, pp. 2275–2277, 1996. Toronto, ON, Canada. He is currently with Corning
[37] Y. H. Lee, A. Chavez-Pirson, S. W. Koch, H. M. Gibbs, S. H. Park, Inc., Corning, NY. His research interests include materials and devices for
J. Morhange, A. Jeffrey, N. Peyghambarian, L. Banyai, A. C. Gossard, ultrafast photonic switching, ultrafast laser sources, and fiber amplifiers.
LOKA et al.: OPTICAL CHARACTERIZATION OF GaAs FOR ULTRAFAST SWITCHING DEVICES 1437

Peter W. E. Smith (M’67–SM’76–F’78) was born


in London, England, on November 3, 1937. He re-
ceived the B.Sc. degree in mathematics and physics
in 1958 and the M.Sc. and Ph.D. degrees in physics
in 1961 and 1964, respectively, all from McGill
University, Montreal, PQ, Canada. His thesis work
was on paramagnetic relaxation of iron group ions
in dilute single crystals.
From 1958 to 1959, he was an Engineer at
the Canadian Marconi Company, Montreal, Canada,
where he worked on transistor circuitry. After ob-
taining the Ph.D. degree, he joined Bell Telephone Laboratories, Holmdel,
NJ, where he conducted research on laser mode selection and mode-locking,
pioneered the development of waveguide gas lasers, and demonstrated and
developed hybrid bistable optical devices. In 1970, he spent nine months
at the University of California, Berkeley, as Visiting Mackay Lecturer in
the Department of Electrical Engineering, and in 1978–1979, he was a
Visiting Research Scientist at the Laboratoire d’Optique Quantique, Ecole
Polytechnique, Palaiseau, France. From 1984 to 1992, he was with Bell
Communications Research, Red Bank, NJ, where from 1990 on he was
Division Manager of Photonic Science and Technology Research. In July
1992, he became Professor of Electrical and Computer Engineering at the
University of Toronto, Toronto, ON, Canada. From 1992 to 1995, he also
served as Executive Director of the Ontario Laser and Lightwave Research
Centre. His current research interests involve ultrafast optical switching and
photonics. He has published over 250 technical papers and holds 32 patents.
He was Associate Editor of Optics Letters from 1980 to 1982 and Editor
of Optics Letters from 1991 to 1995. He was the founder of the Photonic
Switching Conference and served as co-chair of the first two conferences in
1987 and 1989.
Dr. Smith is a fellow of the Optical Society of America and a member
of the American Physical Society, L’Association Canadienne-Française pour
l’Avancement des Sciences, and the Canadian Association of Physicists. He
has participated in numerous conference organizing committees and has been
Guest Editor for several special journal issues. He served as Associate Editor
of the IEEE JOURNAL OF QUANTUM ELECTRONICS from 1976 to 1979. From
1987 to 1991, he served as Editor-in-Chief of the IEEE Press book series
“Progress in Lasers and Electro-Optics.” He is currently a member of the
International Advisory Board of the Journal of Modern Optics. He served as
president of the IEEE Lasers and Electro-Optics Society in 1984. In 1986, he
was awarded the IEEE Quantum Electronics Award.

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