## Abstract

We have switched GaAs/AlAs and AlGaAs/AlAs planar microcavities that operate in the “Original” (O) telecom band by exploiting the instantaneous electronic Kerr effect. We observe that the resonance frequency reversibly shifts within one picosecond when the nanostructure is pumped with low-energy photons. We investigate experimentally and theoretically the role of several parameters: the material backbone and its electronic bandgap, the quality factor, and the duration of the switch pulse. The magnitude of the frequency shift is reduced when the backbone of the central *λ*-layer has a greater electronic bandgap compared to the cavity resonance frequency and the frequency of the pump. This observation is caused by the fact that pumping with photon energies near the bandgap resonantly enhances the switched magnitude. We thus find that cavities operating in the telecom O-band are more amenable to ultrafast Kerr switching than those operating at lower frequencies, such as the C-band. Our results indicate that the large bandgap of AlGaAs/AlAs cavity allows to tune both the pump and the probe to the telecom range to perform Kerr switching without detrimental two-photon absorption. We observe that the magnitude of the resonance frequency shift decreases with increasing quality factor of the cavity. Our model shows that the magnitude of the resonance frequency shift depends on the pump pulse duration and is maximized when the duration matches the cavity storage time to within a factor two. In our experiments, we obtain a maximum shift of the cavity resonance relative to the cavity linewidth of 20%. We project that the shift of the cavity resonance can be increased twofold with a pump pulse duration that better matches the cavity storage time. We provide the essential parameter settings for different materials so that the frequency shift of the cavity resonance can be maximized using the electronic Kerr effect.

© 2016 Optical Society of America

## 1. Introduction

Fast optical switching rates are currently under demand by both optical information technologies [1–9 ] and by fundamental studies that aim to manipulate light-matter interactions at femtosecond time scales [10–13 ]. The electronic Kerr effect inherently provides the highest possible speed given its virtually instantaneous response nature [7, 14–20 ]. Using the Kerr effect the resonance of a microcavity has been switched within a duration as short as 300 fs [17], and repeated switching has been performed at unprecedented single-channel rates beyond one THz clock rate [20]. The electronic Kerr effect is a third-order nonlinear process and its magnitude increases linearly with the intensity of the pump laser pulse [14]. Increasing the intensity of the laser pulse, however, causes the excitation of free carriers that have a much slower speed and counteract the electronic Kerr effect [18, 21]. Fortunately, the excitation of free carriers through two-photon absorption process can be suppressed via the judicious selection of the photon energy and the intensity of the switching pulse [15–18 , 20].

Until now, however, only moderate switch amplitudes at most around quarter a mode linewidth have been reported [17, 18, 20]. In view of practical applications of Kerr switching, a shift of at least half a linewidth is highly desirable, to benefit from a large modulation of the reflectivity or transmission of the microcavity. To achieve this challenging goal, one has to delicately choose all parameters that play a role in frequency shift of the cavity resonance; 1) the intensity of the light pulses, 2) the backbone and the frequency of light relative to the backbone’s electronic bandgap, 3) the quality factor of the cavity, and 4) the duration of the switch pulse. Previously, we have investigated the effect of the pump intensity with emphasis on the competition between Kerr and free-carrier effects that occur at high pump intensities [18]. In this work, we explore, for the first time, the effect of the backbone, the frequency of the pump and the probe light relative to the backbone’s electronic bandgap, cavity storage time, and the duration of the pump pulse. As a result, we provide a set of crucial parameters that serve to maximize the resonance frequency shift induced by the electronic Kerr effect. Noticeably, we show that AlGaAs/AlAs microcavities designed to operate at telecom wavelength should enable near-instantaneous Kerr switching with both pump and probe tuned to telecom wavelengths.

## 2. Experimental details

#### 2.1. Samples

We have performed experiments on planar microcavities that consist of a GaAs *λ*-layer (*d* = 376 nm) sandwiched between two Bragg stacks consisting of *λ/*4-thick layers (*d _{GaAs}* = 94 nm) and AlAs (

*d*= 110 nm) that are grown on a GaAs wafer. Figure 1(b) shows a scanning electron micrograph (SEM) cross-section of a GaAs/AlAs sample. Since the bottom Bragg mirror is positioned on a GaAs wafer, there is a smaller refractive index contrast that results in a lower reflectivity. Therefore, a greater number of layers is required for the bottom Bragg stack to achieve a similar reflectivity as for the upper Bragg stack. The cavity resonance is designed to occur at

_{AlAs}*λ*

_{0}= 1280

*±*5 nm in the Original (

*O*) telecom band. For a

*λ*− microcavity the mode number is

*m*= 2 [22], hence the cavity quality factor readily gives the finesse. The cavity mode extends over about 1

*μ*m along the longitudinal direction of our samples.

In order to achieve a range of quality factors we prepared a large sample and cut it into smaller chips (5 mm*×*5 mm). Next, a number of layers is selectively removed from the top Bragg stack of one chosen chip by dry and wet etching techniques to obtain four asymmetric GaAs/AlAs cavities with sequentially reduced quality factors, see Table 1 for a list of all samples.

To investigate the effect of the bandgap of the backbone on Kerr switching, we have also studied a planar microcavity made of a Al_{0.3}Ga_{0.7}As *λ*-layer (*d* = 400 nm) sandwiched between two Bragg stacks made of 9 and 16 pairs of *λ/*4-thick layers of Al_{0.3}Ga_{0.7}As (*d _{AlGaAs}* = 100.2 nm) and AlAs (

*d*= 111.7 nm), respectively, and grown on a GaAs wafer. The AlGaAs/AlAs cavity is designed to resonate at

_{AlAs}*λ*

_{0}= 1280

*±*5 nm and has a quality factor of

*Q*= 210.

#### 2.2. Setup

A versatile ultrafast pump-probe setup is used to Kerr-switch our microcavity [23]. The setup is shown in Fig. 1(a) and consists of two independently tunable optical parametric amplifiers (OPA, Light Conversion Topas) pumped by a 1 kHz oscillator (Hurricane, Spectra Physics) that are the sources of the pump and probe beams. The pulse duration of both OPAs is *τ _{P}* = 140

*±*10 fs. The time delay Δ

*t*between the pump and the probe pulse is set by a delay stage with a resolution of 15 fs. The measured transient reflectivity contains information on the cavity resonance during the cavity storage time and it should thus not be confused with the instantaneous reflectivity at the delay Δ

*t*, see Appendix A.

The cavity is switched with the electronic Kerr effect by judicious tuning of the pump and the probe frequencies relative to the semiconductor bandgap of the cavity backbone [15, 16]. The probe frequency *ω _{pr}* is set by the cavity resonance in the telecom range (see Table 1). Furthermore, the photon energy of the pump light is chosen to lie below half of the semiconductor bandgap energy of both GaAs and AlGaAs
$({E}_{pu}<\frac{1}{2}{E}_{gap})$ to avoid two pump-photon excitation of free carriers. Therefore, the pump frequency is centered at

*ω*= 4165 cm

_{pu}^{−1}(

*λ*= 2400nm). The frequency of the pump and the probe light is kept the same for the GaAs and AlGaAs cavities to directly compare the effect of photon energy relative to the electronic bandgap. The probe fluence is set to

_{pu}*I*= 0.18

_{pr}*±*0.02 pJ

*/μ*m

^{2}while the average pump fluence is set to

*I*= 65 ± 20 pJ

_{pu}*/μ*m

^{2}. The fluences are chosen such that they yield an as large as possible Kerr effect without unwanted free carrier excitation in GaAs [18]. The fluence of the pulses is determined from the average laser power at the sample position and is converted to peak power assuming a Gaussian pulse shape. The pump beam has a larger Gaussian focus (2

*r*= 70

_{pu}*μ*m) than the probe beam (2

*r*= 30

_{pr}*μ*m) to ensure that only the central flat part of the pump focus is probed and that the probed region is spatially homogeneously pumped [24]. The induced resonance frequency shift with the electronic Kerr effect is determined by the pump-probe delay (Δ

*t*) and the spatial overlap of the pump and the probe beams. For this reason, once we fix the spatial alignment of the pump and probe beams we successively perform switching of the different cavities to allow for the best possible comparison.

## 3. Results and discussions

#### 3.1. Basic observables

Figure 2(a) shows the resonance frequency versus pump-probe time delay Δ*t* for the GaAs/AlAs cavity with *Q* = 390 *±* 60. The resonance is taken as the minimum of the transient reflectivity trough. The resonance quickly shifts by 5.6 cm^{−}^{1} to a lower frequency at pump-probe overlap (Δ*t* = 0) and quickly returns to the starting frequency within 1 ps. The shift of the cavity resonance to a lower frequency is due to the increased refractive index of GaAs, shown on the right ordinate. Our dynamic model (see Appendix B) predicts the frequency shift during the instantaneous switching of the cavity in excellent agreement with our experimental results.

Figure 2(a) shows that the minimum of the resonance trough appears at a higher frequency when the probe pulse arrives before the pump pulse (Δ*t* < −500 fs) even though the refractive index only increases. The apparent blue shift is the result of interference between probe light that reflects from the top Bragg mirror and probe light that is confined to the cavity, is frequency modulated, and then escapes. While the instantaneous cavity resonance tracks the refractive index change and only red-shifts (Fig. 2(a)), the minimum of the cavity trough is apparently blue shifted. The apparent blue shift of the cavity trough is a result of the asymmetric cavity design. In the asymmetric cavities the top Bragg mirror consist of fewer layers than the bottom Bragg mirror. This results in more leakage from the top Bragg mirror. As a result, the interference between the probe light that escapes from the cavity (where it is modulated by the pump pulse) and the probe light that has directly reflected from the top mirror increases. Given the increased modulation, the resonance trough seems to appear at a higher frequency, even though the refractive index does not yet change and certainly does not decrease [25].

Since the apparent blue-shift is the result of interference involving light escaping from the cavity, we verify the magnitude of the apparent blue-shift by calculating it for cavities with a decreased escaping intensity from the top mirror. Therefore, we have performed calculations for cavities with sequentially increased number of top Bragg layers as shown in Fig. 2(b). With increasing number of top layers the cavity becomes more symmetric and at the same time the quality factor of the cavity increases. In Fig. 2(b) we observe that the apparent blue shift of the cavity resonance at Δ*t* < 0 decreases for increasingly symmetric cavities. In Fig. 2(b) the red shift of the cavity resonance at Δ*t* = 0 decreases with increasing quality factor, which will be discussed in section 3.3. We summarize our observations that the reversible red shift of the cavity resonance corresponds to the derived electric Kerr effect, whereas the apparent blue-shift is the result of an spatial interference.

#### 3.2. The effect of the backbone’s electronic bandgap

To compare the effect of the backbone’s electronic bandgap we have performed Kerr switching experiments on cavities that has similar quality factors and consist of GaAs/AlAs (*Q* = 390) and AlGaAs/AlAs (*Q* = 210). Figure 3(a) and 3(c) shows the resonance frequency versus time delay for these GaAs/AlAs and AlGaAs/AlAs microcavities, respectively. The cavity resonance for the AlGaAs cavity shifts by 1.8 cm^{−1}, which is less than 4.7 cm^{−1} of the GaAs cavity. To understand this lower frequency shift with the AlGaAs/AlAs cavity we consider how the third order susceptibility depends on material parameters.

Figure 4 shows the nondegenerate dispersion (*G*
_{2}) curve of the electronic Kerr effect for probe frequency *ω _{pr}* within the original (

*O*) and conventional (

*C*) telecom bands. The function

*G*

_{2}determines the dispersion of the nonlinear index coefficient

*n*

_{2}as follows [26]:

*K*is a constant,

*E*the Kane energy (≃ 21

_{p}*eV*),

*E*the bandgap, and

_{gap}*n*

_{0}

*,*

_{pr}*n*

_{0}

*are the linear refractive indices at probe (*

_{pu}*ω*) and pump frequency (

_{pr}*ω*), respectively. The dispersion function is obtained by the Kramers-Kronig transformation of the interband absorption change [26]. The dispersion of the nonlinear refractive index coefficient

_{pu}*n*

_{2}has been also validated experimentally [27–30 ]. We calculate the dispersion function

*G*

_{2}from Sheik-Bahae et. al. [26], Table 2. In Fig. 4 we see that the nonlinear index coefficient is maximized near the non-degenerate two photon absorption edge [28,29]. Our cavities are designed to operate within the original (

*O*) telecom band, which corresponds to a reduced probe frequency

*ħω*= 0.65. We set the pump frequency to

_{pr}/E_{gap}*ħω*= 0.35 in order to suppress degenerate free carrier excitation, see Fig. 3(b1). The non-degenerate free carrier excitation (pump and probe, Fig. 3(b2)) is suppressed since the probe fluence is much smaller than the pump fluence. At this setting of the pump frequency, the non-degenerate sum of pump and of probe frequency are tuned close to the electronic bandgap of the material. As a result, the nonlinear index coefficient is close to the maximum, as shown in Fig. 4. We use the same frequency of the pump and of the probe light for the AlGaAs/AlAs cavity. In this case we operate away from the electronic bandgap of AlGaAs both for degenerate two-pump photon excitation (Fig. 3(d1)) and for non-degenerate pump and probe photon excitation (Fig. 3(d2)). Consequently, we observe less refractive index change due to a smaller nonlinear refractive index coefficient, see Fig. 4, which explains the smaller shift of the cavity resonance in Fig. 3(c).

_{pu}/E_{gap}
Figure 4 also shows the dependence of the nonlinear index coefficient versus pump frequency when the cavity resonance *ω _{pr}* is set to operate within the

*C*-band (1530 – 1565 nm). In this case, we see that the electronic Kerr effect is maximized when the pump frequency is tuned to

*ħω*= 0.5 (

_{pu}/E_{gap}*λ*≃ 1700 nm for GaAs). At this pump frequency, however, the probability for the excitation of free carriers via two pump photons will be strong, which will hinder the electronic Kerr effect [18]. In contrast, cavities operating within

_{pu}*O*-band (1260 – 1360 nm) are more amenable than in the

*C*-band for ultrafast switching using the electronic Kerr effect, since the greater probe frequency can be combined with a lower pump frequency to profit from the maximized nonlinear index. Simultaneously, a lower pump frequency will much less likely induce unwanted two-photon excitation of free carriers.

#### 3.3. The effect of the cavity storage time

We have performed switching experiments on cavities with different quality factors to investigate the effect of the cavity storage time *τ _{c}* on the Kerr-induced resonance frequency change. Figure 5 shows the relative cavity resonance frequency shift versus both the quality factor

*Q*and the storage time

*τ*of the cavity. We observe that the shift of the cavity resonance frequency (

_{c}*δω*) relative to the cavity linewidth (Δ

*ω*) is maximal when the storage time is matched to the pump pulse duration

*τ*. We see both in our measurements and in our model (for the model see Appendix B) that increasing the storage time

_{P}*τ*of the cavity not only decreases the switching speed but also decreases the induced frequency shift induced via the Kerr effect. This can be understood since the magnitude of the observed frequency shift (

_{c}*δω*) is given by the time-overlap integral of the pump and probe light that is stored in the cavity [17]. The decreasing frequency shift with increasing quality factor is caused by the decreased temporal overlap of pump and probe as the cavity-stored probe pulse becomes much longer than the pump pulse (

*τ*≫

_{cav}*τ*).

_{P}In qualitative agreement with our experiments, our model in Fig. 5 shows that a greater resonance frequency shift is observed for a cavity that matches the switch pulse duration during the Kerr switching of a cavity. The relative shift of the resonance frequency is maximal at *τ _{c}* = 140 fs, reaching a value close to 40%, when the duration of the cavity-stored probe matches the pump duration (

*τ*≃

_{c}*τ*). Our model predicts a greater resonance frequency shift compared to our experiments. Our model employed in Fig. 5 is an improvement over our earlier work since it contains explicit time dependency, as opposed to the time-independent model we presented earlier [18]. In our previous study [18] we have investigated the effect of the cavity enhancement and found that the effect of the counteracting free carriers is more pronounced for high quality factor cavities. In a cavity with a high quality factor the probe light intensity is enhanced and thereby the probability of degenerate and non-degenerate two-photon excitation of free carriers is increased [18]. Therefore, the difference between our dynamic model and our experiments is larger for high quality factor cavities since we can currently not include free carrier effects in the model. In cavities with a short storage time the excited free carrier density is reduced and the temporal overlap of the pump pulse with the cavity-stored probe light is increased (

_{P}*τ*≃

_{c}*τ*), which even allows to Kerr switch a cavity resonance at exhilarating THz clock rates [20].

_{P}
Figure 6 schematically illustrates the effect of the storage time of the cavity on the Kerr switching of a microcavity in real time. We plot situations where the delay Δ*t* is such that the overlap of the pump and cavity-stored probe is maximal, and we assume the observed cavity resonance *ω _{avg}* to be averaged over the whole pulse duration in view of the relatively slow detection (

*t*), see section 2.2. For a high quality factor cavity, see Fig. 6(a) and 6(b), there is no pump light during a long fraction of the probe pulse in the cavity since

_{int}> τ_{pr}*τ*≫

_{c}*τ*. As a result, the average resonance frequency shift

_{P}*ω*is small. Given the same refractive index change, one would naively expect to observe a greater relative shift of the cavity resonance for a high quality factor cavity. However, this is only true if the switch duration is longer than the cavity storage time (

_{avg}*τ*). Since the Kerr switching of the cavity is performed within the pump pulse duration, one has to consider the overlap integral in time to get the average resonance frequency shift. This overlap is determined both by the duration of the pump pulse and the quality factor of the cavity that affects the duration of the cavity-stored probe pulse. Consequently, at similar switch conditions a cavity with a shorter storage time will reveal a greater shift of the time averaged resonance

_{c}< τ_{P}*ω*since the instantaneous cavity resonance shift

_{avg}*ω*′ has a larger weight. As illustrated in Fig. 6(c) and 6(d), a larger portion of the cavity-stored probe light overlaps with the short pump pulse in a cavity that has a short storage time, close to the pump pulse duration (

*τ*≃

_{c}*τ*).

_{P}#### 3.4. The effect of the pump pulse duration

To investigate the effect of the pump pulse duration on Kerr-induced cavity resonance frequency switching, we have performed calculations on a switched cavity using our dynamic model as a function of the pump pulse duration. Similar to our experiments, the microcavity in our calculations has 7 pairs of GaAs/AlAs layers in the top mirror and 19 pairs of GaAs/AlAs layers in the bottom mirror and is surrounded by air. For the modeled nanostructure we get a quality factor *Q* = 450 in our calculations whereas the closest cavity in our experiments has a quality factor *Q* = 390. The difference in measured and calculated quality factors are due to absence of loss mechanisms in the model, such as slight deviations of the layer thicknesses versus the nominal design. Moreover, in our model we do not include the GaAs wafer that also increases the quality factor, given the increased contrast between air and the bottom Bragg mirror. Figure 7 shows the cavity resonance frequency shift relative to the resonance linewidth (*δω/*Δ*ω*) versus the pump pulse duration at a pump-probe delay Δ*t* = 0 fs. The maximum shift (*δω*) reaches 32% when the pump pulse duration is set to *τ _{P}* = 550 fs for this particular cavity. Beyond

*τ*= 1 ps the cavity resonance frequency shift decreases with increasing pump pulse duration. When we compare the optimum pump pulse duration (

_{P}*τ*= 550 fs) to the cavity storage time (

_{P}*τ*= 300 fs for

_{c}*Q*= 450, see Fig. 5) we observe that they are of comparable magnitude, as is to be expected. It is noteworthy that the times are not exactly equal as

*τ*= 1.8. The difference of unity is probably related to subtle issues of pulse shapes that determine the detailed temporal overlap of the pump and probe fields. Although, the effect of the cavity storage time is similar to pump pulse duration we see in Fig. 7 that at

_{P}/τ_{c}*τ*= 140 fs the resonance frequency shift is smaller than the results shown in Fig. 5. This is because in Fig. 5 the resonance frequency shift is calculated Δ

_{P}*t*= −100 fs, at which delay the resonance frequency shift reaches its maximum [20], whereas at Δ

*t*= 0 fs the resonance shift is smaller on the probe pulse has already partially escaped from the cavity. This time delay was chosen here so that we can calculate the effect of the pump pulse duration that is shorter than the cavity storage time.

To interpret the behavior versus pulse duration, we schematically depict in Fig. 8 the probe pulse that is in resonance with the cavity and the pump pulse versus real time. The resonance frequency of the cavity shifts from *ω*
_{0} to *ω*′ due to the instantaneous change of the refractive index. Given the time averaging of the detector, we observe an average resonance frequency shift *ω _{avg}* that is smaller than the instantaneous shift. For a short pump pulse duration (

*τ*) illustrated in Fig. 8(a) the cavity-averaged frequency shift is small, see Fig. 8(b). As the pump pulse gets longer in time (Fig. 8(c)) the weight of instantaneous shift increases in the time-averaged resonance frequency shift. As a result, a greater shift of the cavity resonance is observed, see Fig. 8(d). Stretching the pump pulse to be much longer than the cavity storage time tomographically samples the probe light in the cavity, see Fig. 8(e) and 8(f). The average resonance frequency shift decreases when

_{P}< τ_{c}*τ*≫

_{P}*τ*since the magnitude of the frequency shift

_{c}*δω*is given by the overlap integral of the pump and probe. We conclude that the storage time of the cavity and the duration of the pump pulse have similar consequences in resonance frequency shift of the cavity [17].

Our dynamic calculations have shown that the relative resonance frequency shift can be increased by 1.7*×*, by increasing the pump pulse duration from *τ _{P}* = 140 fs to

*τ*= 550 fs. As a result, we project that the resonance frequency shift we experimentally obtain 5.6 cm

_{P}^{−1}can be increased to 9.5 cm

^{−1}, which is half a linewidth.

## 4. Summary and conclusion

We have studied the ultrafast all-optical switching of GaAs/AlAs and AlGaAs/AlAs semiconductor microcavities at telecom wavelengths using the electronic Kerr effect. We investigate the effect of the pump pulse duration, the cavity storage time, backbone material, and the frequency of the pump and the probe relative to the electronic bandgap of the backbone material. We show that the refractive index change induced by the electronic Kerr effect is increased when the cavity storage time match the pump pulse duration. Our results indicate that cavities with AlGaAs backbone hold the advantage that both the pump and the probe can be at telecom wavelengths. In this case, for a cavity operating at *O*-band, the pump frequency should be set to about 7280 cm^{−1}(1370 nm) to maximize the non-degenerate nonlinear index coefficient. Two-photon excitation of free carriers via degenerate pump photons will still be suppressed at this photon energy since AlGaAs has a larger bandgap. Our results indicate that an additional twofold increase of the nonlinear index coefficient can be expected with this setting of the cavity resonance and the pump frequency for AlGaAs cavity.

## Appendix A Transient reflectivity

We explain the transient reflectivity using the description given in earlier studies [23, 31, 32]. In the absence of spectral filtering, the measured signal J, neglecting electronic amplification factors, is equal to the magnitude of the time- and space-integrated Poynting vector S [23,31]:

*Ẽ*(

*t*) of FWHM

*τ*and amplitude

_{P}*Ẽ*

_{0}that is multiplied by sinusoidal component with a carrier frequency

*ω*

_{0}in rad/s. This slowly varying envelope approximation (SVEA, see [33]) can be applied to pulses where

*τ*>> 1

_{P}*/ω*

_{0}, and where

*ω*

_{0}does not change over

*t*, in other words, for bandwidth limited pulses. For pulses whose envelope is broadened by the interaction with a cavity, the analytic expression (Eq. (4)) is not valid, but the approximation of the integration limits remains the same. The beam is collimated and has radius

*r*,

*ε*

_{0}and

*μ*

_{0}denote the permitivity and permeability of free space, respectively. Since the integration time

*t*of the InGaAs line array detector is much longer than any probe interaction time

_{int}*τ*, we essentially integrate all probe light that is stored or reflected by the cavity, given a pump-probe time delay Δ

_{pr}*t*. The probe interaction time is either

*τ*=

_{pr}*τ*or

_{P}*τ*=

_{pr}*Q/ω*

_{0}, whichever is greater, and it is in the 100 fs to 1 ps range. Therefore, the boundaries of time integral in Eq. (2) can be taken to be infinity because

*t*. The squared oscillating term can then be integrated separately and yields 1/2. In Eq. (3) we approximate the peak intensity for a focussed Gaussian pulse as $I=4\sqrt{ln2}G/({\pi}^{3/2}{r}^{2}{\tau}_{P})$, where r is the waist radius at the focus and G the energy per pulse. Eq. (3) reveals that it is not the instantaneous transmission or reflection that is measured, but the integrated intensity.

_{int}>> τ_{P}In our study, we use a spectrometer to frequency resolve the reflected transient signal. The reflected signal from the cavity is spectrally filtered with a spectrometer (Acton) and detected with a nitrogen cooled InGaAs line array detector (Princeton Instruments). Therefore, the observed spectrum, without amplification and conversion factors, is a Fourier transform of *E*(*t*) [31,32]

*R*(

^{t}*ω*) =

*J*(

*ω*)

*(*

_{sample}/J*ω*)

*exceeds unity at the new frequency components. In this sense, the transient reflectivity differs from the reflectivity measured in a CW experiment that is necessarily always bounded to 100%. The measured transient reflectivity*

_{ref}*R*(

^{t}*ω*) is a result of the probe light that impinges at delay Δ

*t*, circulates in the cavity during on average the storage time

*τ*, escapes, and is then integrated by the detector. Therefore, we call the measured signal the transient reflectivity or the transient transmission.

_{c}## Appendix B Model to calculate time-resolved spectra

The model that we employ to calculate the time-resolved transient reflectivity *R ^{t}* spectra has previously been introduced by by Harding et. al. [25]. The probe field is calculated in the time domain at every position in a one-dimensional planar microcavity that experiences a time-dependent refractive index. To account for the induced refractive index change

*n*(

*t*), we consider here the positive non-degenerate Kerr coefficient of GaAs [18]. We start with a Gaussian probe pulse at position

*z*=

*z*

_{0}:

_{0}is the amplitude of the probe field

*E*and

_{pr}*ω*the angular frequency,

*t*running time and

*t*

_{0}is the launch time of the probe pulse. In our calculations we chose a short duration for the probe pulse (

*τ*= 10 fs) to obtain a broad spectral bandwidth and thus a flat response within the spectral region of the cavity resonance. The field that starts from position

_{pr}*z*=

*z*

_{0}travels in homogeneous medium with a time dependent refractive index

*n*(

*t*). The time that it takes for the field to travel from position

*z*

_{0}to

*z*is then equal to

*t*=

*n*(

*t*)·(

*z*−

*z*

_{0})

*/c*. As a result, the Gaussian pulse at position

*z*is given by

Similar to our experiments the structure that we describe in our model consists of air, the top Bragg mirror, the *λ*-layer, the bottom Bragg mirror, and air after the cavity structure, as shown in Fig. 9. Since the thickness of the GaAs wafer is not exactly known, we exclude it in our model. The Bragg mirrors consist of AlAs and GaAs layers with unswitched refractive indices n_{AlAs} and
${\mathrm{n}}_{\text{GaAs}}^{0}$, respectively. During the switching of our microcavity we take the refractive index of AlAs and air to be constant in time, whereas the refractive index of GaAs is time dependent. Since the change of the refractive index of AlAs is five times smaller [15] we safely treat its refractive index as a constant. The refractive index of GaAs changes with the time delay Δ*t* between the pump and the probe pulses due to the electronic Kerr effect. Hence, we define a position- and time-dependent refractive index for the structure as follows:

*χ*

^{(3)}is the third-order susceptibility of GaAs,

*I*the peak intensity of the pump pulse,

_{pu}*τ*the duration of the pump pulse, and Δ

_{pu}*t*the time delay between pump and the probe. In our calculations we neglect the refractive index change induced by the probe light since the intensity of the probe is much lower than the pump intensity. Since the probe field propagates through the microcavity structure that consists of many different materials with different refractive indices, the field encounters many interfaces. The field that impinges on an interface is partly reflected and partly transmitted, as given by the Fresnel coefficients [34]. The reflected $(\mathfrak{r})$ and transmitted $(\mathfrak{t})$ amplitude coefficients at normal incidence from any interface are equal to

*n*

_{1}(

*z,t*) and

*n*

_{2}(

*z,t*) are the time-dependent refractive indices of the first and the second medium, respectively. Due to the transmission and reflection from an interface, there are fields travelling in opposite directions. Part of the field transmitted by interface

*i*is reflected from the next interface

*i*+ 1 and thus interferes with the incident field. As a result, at a given position

*z*inside the microcavity, the field is equal to

For convenience we take the direction of the transmission as the positive direction. Since the microcavity structure consists of *N* interfaces, we have generalized Eq. (10) to N total number of interfaces and mark Fresnel coefficients
${\mathfrak{r}}^{i}$ and
${\mathfrak{t}}^{i}$ with the index *i*, which represent the interface number.

We calculate the field at any position *z* in the multilayer structure by inserting the time-dependent refractive index of GaAs and the time-independent refractive indices of AlAs and air in *n*(*z,t*) from Eq. (8) into Eq. (10). Equation (10) can be generalized to a case where both the refractive indicies of GaAs and AlAs are time-dependent. If the field is, for instance, at GaAs and AlAs interface, the time-dependent index of GaAs and AlAs should be inserted in *n*
_{1}(*z,t*) and *n*
_{2}(*z,t*) in Eq. (9), respectively. To calculate the transient reflectivity spectrum we include all interfaces, see Fig. 9, to obtain the total time-resolved field
${\mathcal{E}}_{pr}(z,t)$. Next, we perform a discrete Fourier transform on such a field in reflection geometry

*R*spectra. In Eq. (11)

^{t}*δt*represents the time step.

## Acknowledgments

We thank Allard Mosk and Henri Thyrrestrup for useful discussions. This research was supported by FOM-NWO, the NWO-Nano program, ERC-Pharos Project No. 279248, and STW.

## References and links

**1. **A. Kan’an, P. LiKamWa, M. Dutta, and J. Pamulapati, “1.7-ps consecutive switching in an integrated multiple-quantum-well Y-junction optical switch,” IEEE Photon. Technol. Lett. **8**, 1641–1643 (1996). [CrossRef]

**2. **J. P. Mondia, H. W. Tan, S. Linden, and H. M. van Driel, “Ultrafast tuning of two-dimensional planar photonic-crystal waveguides via free-carrier injection and the optical Kerr effect,” J. Opt. Soc. Am. B **22**, 2480–2486 (2005). [CrossRef]

**3. **H. Altug, D. Englund, and J. Vučković, “Ultrafast photonic crystal nanocavity laser,” Nat. Phys. **2**, 484–488 (2006). [CrossRef]

**4. **I. Fushman, E. Waks, D. Englund, N. Stoltz, P. Petroff, and J. Vučković, “Ultrafast nonlinear optical tuning of photonic crystal cavities,” Appl. Phys. Lett. **90**, 091118 (2007). [CrossRef]

**5. **P. J. Harding, T. G. Euser, Y. Nowicki-Bringuier, J.-M. Gérard, and W. L. Vos, “Dynamical ultrafast all-optical switching of planar GaAs/AlAs photonic microcavities,” Appl. Phys. Lett. **91**, 111103 (2007). [CrossRef]

**6. **C. Husko, A. de Rossi, S. Combrié, Q. V. Tran, F. Raineri, and C. W. Wong, “Ultrafast all-optical modulation in GaAs photonic crystal cavities,” Appl. Phys. Lett. **94**, 021111 (2009). [CrossRef]

**7. **C.-Y. Jin and O. Wada, “Photonic switching devices based on semiconductor nano-structures,” J. Phys. D Appl. Phys. **47**, 133001 (2014). [CrossRef]

**8. **A. Pejkic, R. R. Nissim, E. Myslivets, A. O. J. Wiberg, N. Alic, and S. Radic, “All-optical switching in a highly efficient parametric fiber mixer: design study,” Opt. Express **22**, 23512–23527 (2014). [CrossRef] [PubMed]

**9. **X. Xia, J. Xu, and Y. Yang, “Controllable optical bistability of an asymmetric cavity containing a single two-level atom,” Phys. Rev. A **90**, 043857 (2014). [CrossRef]

**10. **P. M. Johnson, A. F. Koenderink, and W. L. Vos, “Ultrafast switching of photonic density of states in photonic crystals,” Phys. Rev. B **66**, 081102(2002). [CrossRef]

**11. **M. F. Yanik and S. Fan, “Stopping light all optically,” Phys. Rev. Lett. **92**, 083901 (2004). [CrossRef] [PubMed]

**12. **H. Thyrrestrup, A. Hartsuiker, J.-M. Gérard, and W. L. Vos, “Switching the decay rate of an emitter inside a cavity in the time domain,” Opt. Express **21**, 23130–23144 (2013). [CrossRef] [PubMed]

**13. **R. Johne, R. Schutjens, S. F. Poor, C.-Y. Jin, and A. Fiore, “Control of the electromagnetic environment of a quantum emitter by shaping the vacuum field in a coupled-cavity system,” Phys. Rev. A **91**, 063807 (2015). [CrossRef]

**14. **R. Boyd, *Nonlinear Optics*, 3rd ed.(Academic, 2008).

**15. **A. Hartsuiker, P. J. Harding, Y. Nowicki-Bringuier, J.-M. Gérard, and W. L. Vos, “Kerr and free carrier ultrafast all-optical switching of GaAs/AlAs nanostructures near the three photon edge of GaAs,” J. Appl. Phys. **104**, 083105 (2008). [CrossRef]

**16. **P. J. Harding, T. G. Euser, and W. L. Vos, “Identification of competing ultrafast all-optical switching mechanisms in Si woodpile photonic crystals,” J. Opt. Soc. Am. B **28**, 610–619 (2009). [CrossRef]

**17. **G. Ctistis, E. Yüce, A. Hartsuiker, J. Claudon, M. Bazin, J.-M. Gérard, and W. L. Vos, “Ultimate fast optical switching of a planar microcavity in the telecom wavelength range,” Appl. Phys. Lett. **98**, 161114 (2011). [CrossRef]

**18. **E. Yüce, G. Ctistis, J. Claudon, E. Dupuy, K.-J. Boller, J.-M. Gérard, and W. L. Vos, “Competition between electronic Kerr and free carrier effects in an ultimate-fast optically switched semiconductor microcavity,” J. Opt. Soc. Am. B **29**, 2630–2642 (2012). [CrossRef]

**19. **V. Eckhouse, I. Cestier, G. Eisenstein, S. Combrié, G. Lehoucq, and A. D. Rossi, “Kerr-induced all-optical switching in a GaInP photonic crystal Fabry-Perot resonator,” Opt. Express **20**, 8524–8534 (2012). [CrossRef] [PubMed]

**20. **E. Yüce, G. Ctistis, J. Claudon, E. Dupuy, R. D. Buijs, B. de Ronde, A. P. Mosk, J.-M. Gérard, and W. L. Vos, “All-optical switching of a microcavity repeated at terahertz rates,” Opt. Lett. **38**, 374–376 (2013). [CrossRef] [PubMed]

**21. **J.-F. Wu and C. Li, “Similar role of transient Kerr effect and two-photon absorption in a nonlinear photonic crystal nanocavity,” IEEE Photon. J.1 **5**, 6100209 (2013). [CrossRef]

**22. **J.-M. Gérard, “Solid-state cavity-quantum electrodynamics with self-assembled quantum dots,” Top. Appl. Phys. **90**, 269–314 (2003). [CrossRef]

**23. **T. G. Euser, P. J. Harding, and W. L. Vos, “Broadband sensitive pump-probe setup for ultrafast optical switching of photonic nanostructures and semiconductors,” Rev. Sci. Instrum. **80**, 073104 (2009). [CrossRef] [PubMed]

**24. **T. G. Euser and W. L. Vos, “Spatial homogeneity of optically switched semiconductor photonic crystals and of bulk semiconductors,” J. Appl. Phys. **97**, 043102 (2005). [CrossRef]

**25. **P. J. Harding, H. J. Bakker, A. Hartsuiker, J. Claudon, A. P. Mosk, J. M. Gérard, and W. L. Vos, “Observation of a stronger-than-adiabatic change of light trapped in an ultrafast switched GaAs-AlAs microcavity,” J. Opt. Soc. Am. B **29**, A1–A5 (2012). [CrossRef]

**26. **M. Sheik-Bahae, J. Wang, and E. W. van Stryland, “Nondegenerate optical Kerr effect in semiconductors,” IEEE J. Quantum. Electron. **30**, 249–255 (1994). [CrossRef]

**27. **M. G. Kuzyk, R. A. Norwood, J. W. Wu, and A. F. Garito, “Frequency dependence of the optical Kerr effect and third-order electronic nonlinear-optical processes of organic liquids,” J. Opt. Soc. Am. B **6**, 154–164 (1989). [CrossRef]

**28. **M. Sheik-Bahae, D. J. Hagan, and E. W. van Stryland, “Dispersion and band-gap scaling of the electronic Kerr effect in solids associated with two-photon absorption,” Phys. Rev. Lett. **65**, 96–99 (1990). [CrossRef] [PubMed]

**29. **M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. van Stryland, “Dispersion of bound electron nonlinear refraction in solids,” IEEE J. Sel. Top. Quantum Electron. **27**, 1296–1309 (1991). [CrossRef]

**30. **W. C. Hurlbut, Y.-S. Lee, K. L. Vodopyanov, P. S. Kuo, and M. M. Fejer, “Multiphoton absorption and nonlinear refraction of GaAs in the mid-infrared,” Opt. Lett. **32**, 668–670 (2007). [CrossRef] [PubMed]

**31. **P. J. Harding, “Photonic crystals modified by optically resonant systems,” Ph.D. thesis, University of Twente (2008).

**32. **A. Hartsuiker, “Ultrafast all-optical switching and optical properties of microcavities and photonic crystals,” Ph.D. thesis, University of Twente (2009).

**33. **J. C. Diels and W. Rudolph, *Ultrashort Laser Pulse Phenomena: Fundamentals, Techniques, and Applications on a Femtosecond Time Scale*, 2nd ed.(Academic, 1996).

**34. **M. Born and E. Wolf, *Principles of Optics*, 7th ed.(Cambridge University, 2002).