Abstract

We implement a versatile concept to time-resolve optical nonlinearities of semiconductors in amplitude and phase. A probe pulse transmitted through the optically pumped sample is superimposed with first subharmonic spectral components derived from the same laser source. This effective ω/2ω pulse pair induces a coherently controlled current in a time-integrating semiconductor detector. Current interferograms obtained by scanning the ω/2ω time delay then reveal the electric field of the 2ω part as well as its pump-induced modifications. As a paradigm we analyze the excitonic optical nonlinearity of a CdTe thin film at frequencies around 385 THz. We then move on to resolve the pump-induced amplitude- and phase-distortions of a probe pulse related to two-photon absorption and cross-phase modulation in ZnSe.

© 2012 Optical Society of America

Phase-resolved techniques are integral to modern optics. As an important example, time-domain THz spectroscopy is used to analyze phenomena ranging from exciton formation [1], the dynamics of an electron-hole plasma [2] to magnetic excitations [3]. While those techniques have been advanced to bandwidths beyond 100 THz [4,5], progress toward the visible is, e.g., hampered by the lack of sufficiently short probe pulses. For phase-retrieval at optical frequencies, therefore, alternative concepts are necessary, many of which rely on spectral interferometry [68]. In its common heterodyne embodiment, a signal pulse is superimposed with a local oscillator, which allows to trace the phase-difference with respect to such a reference. This concept is particularly useful to analyze the weak coherent response typical of, e.g., four-wave mixing experiments.

In this Letter, we demonstrate an alternative scheme of spectral interferometry. It proves versatile to detect transient amplitude and phase changes in ultrafast pump-probe type configurations. After transmission through the sample, a probe pulse of center frequency 2ω is superimposed with an ω pulse from the same laser source, and thereby generates an electrical signal reflecting ω/2ω quantum interference control of currents [9] in a semiconductor detector. A Fourier transform of the resulting two-color field cross-correlation reveals the electric field of the 2ω pulse as well as any pump-induced modifications of the 2ω field. We test these ideas for two examples of transient semiconductor optical phenomena. In particular, the excitonic resonance of bulk CdTe serves as a testbed for the transient response of a narrowband optical resonance. In addition, we study the mutual interaction of copropagating 2ω probe and optical pump pulses in ZnSe and extract field modifications related to two-photon absorption and cross-phase modulation.

The optical source is a 250 kHz regenerative amplifier (Coherent RegA 9040) delivering 40 fs, 7 μJ pulses at 1.55 eV (800 nm). While a portion of 2 μJ is reserved as an optical pump, the remainder is fed into an OPA to generate 60 fs, 0.8 eV (1550 nm) signal pulses referred to as fundamental pulse ω. This near-infrared light is frequency doubled in a BiBO crystal. As sketched in Fig. 1(a), the ω and 2ω pulses are passed through a two-color Michelson interferometer, which ensures full control over the relative timing of the co-polarized harmonically related components. Despite a compact design with 6 cm arms, it is possible to insert a microscope cryostat into the 2ω arm. Also the pump pulse is loosely focused onto the sample with an adjustable relative timing [cf. Fig. 1(a)]. As a result, we conceptionally perform 1.55 eV pump-2ω probe experiments as a function of the time tD elapsed since excitation. Performing such an experiment with the established approach, involving spectral resolution within the 2ω probe, would therefore extract a transmission change ΔT2ω(ν,tD). For the present interferometric technique, instead, the transmitted 2ω pulse is superimposed with a time-delayed ω pulse and focused onto a 50 μm wide bar of electrically contacted low temperature grown GaAs. Its room temperature bandgap EG=1.42eV satisfies ω<EG<2ω. Phase-stable superpositions of such ω and 2ω pulses induce a coherently controlled lateral electrical current according to [10]

J˙Eω2E2ωsin(2ΦωΦ2ω).
Here Eω,2ω denote the electric fields of the pulses and Φω,2ω their phases. For Eq. (1) we assume a frequency (ν) independent 2ΦωΦ2ω which is, e.g., valid for transform limited pulses. Recently, we have extracted amplitude and phase information about the 2ω pulse by detecting current interferograms with varying ω/2ω delay time τ [11]. Here, we briefly recap the theory and apply it to the embodiment of transient spectroscopy. We interferometrically scan the ω/2ω time delay τ and detect the coherently controlled current induced in an electrically contacted detector. As a result, we measure a current I(τ,tD)Eω2(tτ)E2ω(t,tD)dt. For pump-probe experiments, the field E2ω(t,tD) (and thus I(τ,tD)) also depends on the delay time tD elapsed since photoexcitation of any sample the 2ω is transmitted through. The Fourier transform of I(τ,tD) scales as:
I(ν,tD)[Eω(ν)]2E2ω(ν,tD).
Most importantly, the spectral density I(ν,tD) contains the Fourier transform of the 2ω electric field for a given delay time tD. In the experiment, we simultaneously measure the interferograms I(τ,tD) (I0(τ)) of the optically pumped (unperturbed) sample. This parallel detection is achieved by mechanically chopping the pump pulse and detecting I(τ,tD)I0(τ) with a lock-in amplifier. The average value (I(τ,tD)+I0(τ))/2 is detected with a second lock-in amplifier referenced to the 250 kHz repetition rate. By straightforward Fourier transformation we construct the spectral densities I(ν,tD) and I0(ν) related to an optically pumped and unperturbed sample, respectively. As evident from Eq. (2), their ratio reads: I(ν,tD)/I0(ν)=E2ω(ν,tD)/E2ω,0(ν). It therefore contains the frequency- and tD-dependent change of the complex field transmission. In particular, the real and imaginary part reveal the transmission change E(ν,tD)/E0(ν) as well as the refractive index modulation Δn(ν,tD)Φ(ν,tD)Φ0(ν) within the 2ω spectrum.

 figure: Fig. 1.

Fig. 1. (a) Experimental setup: the RegA output is split up for use as a pump and as a seed of an OPA generating the ω pulse. A BiBO generates 2ω while a two-color interferometer controls the ω/2ω time delay τ. Another delay line adjusts the pump-2ω delay tD. (b) Photocurrent signal of a contacted LT-GaAs bar upon interferometric variation of τ while 2ω is transmitted through a CdTe thin film (T=7K). Inset: closeup at τ200fs. (c) Spectral domain results derived from a comparison of the data in (b) to a measurement without a sample. The CdTe has a field transmission ΔE/E(ν) (black) and induces a phase retardation ΔΦ(ν) (blue).

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To demonstrate the capabilities of the method, we analyze two classes of semiconductor optical nonlinearities. We start with the excitonic resonance of bulk CdTe and its pump induced transient changes. CdTe is chosen as its excitonic interband transitions conveniently lie within the 2ω spectrum. A 370 nm thin CdTe specimen glued to a fused silica substrate is cooled to T=7K in a cryostat positioned in the 2ω interferometer arm. Figure 1(b) shows the current interferogram for the CdTe sample without optical excitation. Remarkably, we still detect interferometric oscillations of the photocurrent beyond τ=100fs where no temporal overlap between ω and 2ω is expected. This finding reflects the free induction decay of the excitonic polarization induced by the 2ω pulse. By comparison with a reference interferogram IS(τ) when the 2ω beam is transmitted through the substrate only, we derive the CdTe induced changes to the 2ω field [cf. Fig. 1(c)]. The relative field amplitude change ΔE/E=E2ω,0(ν)/E2ω,S(ν)1 (black curve) shows a prominent dip around ω=384THz (ω=1.587eV) reflecting the ground state exciton transition. Around the same frequency, the phase change ΔΦ=Φ2ω,0(ν)Φ2ω,S(ν) (blue) shows a dispersive lineshape as expected from such a resonance.

We now turn to results for transient spectroscopy of the exciton. The sample is excited with 0.5 μJ, 1.55 eV pump pulses to generate carrier densities of 2×1018cm3 mainly by absorption of the high-energy tail of this broadband pulse. The resulting pump induced changes are shown in Fig. 2 for various positive and negative tD. The signal ΔI(τ) [cf. Fig. 2(a) and 2(d)] decays on a timescale of 130fs related to the exciton dephasing time. This fast decoherence is probably connected to the elevated carrier density excited by 2ω and the pump as well as considerable strain of the CdTe thin film mounted on fused silica. The Fourier transform results show a pump induced bleaching of the exciton transition in the field transmission [Fig. 2(b)] and in the phase data [Fig. 2(c)]. The decay of the bleaching strength for increasing positive tD is mainly related to carrier recombination. In contrast, pronounced spectral oscillations are observed at slightly negative delay times tD where 2ω precedes the pump [cf. Fig. 2(e) and 2(f)]. Here the probe induced free induction decay is perturbed by the pump as previously studied, e.g., in bulk GaAs [12]. Intuitively, a pump induced dephasing of the excitonic polarization starting at a certain delay |tD| induces spectral oscillations with a period of Δν=1/|tD|. Spectral oscillations of the same frequency are also well resolved in the phase response [cf. Fig. 2(f)]. While the latter result is not unexpected, it previously remained unresolved.

 figure: Fig. 2.

Fig. 2. Transient spectroscopy of CdTe (T=7K). (a) pump induced photocurrent change ΔI(τ). (b), (c) Fourier transform results for the pump induced change of the field transmission ΔE/E(ν) and phase retardation ΔΦ(ν) for various positive pump-2ω delay times tD. Panels (d) to (f) display the corresponding results for several negative tD.

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Finally, we present results for 1.55 eV pump, 2ω probe experiments in 2 mm thick ZnSe at room temperature. While its bandgap EG=2.7eV satisfies 2ω<EG, transient signals during time-overlap can be expected due to two-photon absorption involving one pump and one probe photon. In addition, group velocity dispersion and cross-phase modulation affect the interaction. The pump induced amplitude and phase change of a weak 2ω field in ZnSe at various pump delay times and a pump intensity of IP10GW/cm2 are shown in Fig. 3. For pulses overlapping at the sample surface (tD=0) we observe a pronounced pump induced absorption especially for the low energy components within the 2ω spectrum centered at 387 THz. This negative going signal is much less pronounced on the high frequency wing beyond 395 THz because the group velocity mismatch to the pump at 375 THz effectively reduces the interaction length. Instead we detect a positive ΔE/E for slightly positive tD. It reveals a slight blue-shift of the 2ω spectrum related to cross-phase modulation induced by the pump (note that for tD>0 the probe overlaps with the trailing edge of the pump so that dIP/dt<0). In line with the amplitude data in Fig. 3(a), also the pump induced phase changes in panel (b) are most pronounced for the low frequency components around tD0. Simulations based on the nonlinear propagation equation for Gaussian pulses reproduce many aspects of the experiment with reasonable values of the nonlinear refractive index (γ=1.7×1018m2/W) and a two-photon absorption coefficient of β=3.5cm/GW. From the simulations we learn that the amplitude changes are mainly related to two-photon absorption while the phase change is predominantly governed by cross-phase modulation. The group velocity mismatch and dispersion effects in ZnSe lead to the larger influence of the pump on the low energy part of the 2ω probe spectrum for all delay times.

 figure: Fig. 3.

Fig. 3. Transient spectroscopy of 2 mm bulk ZnSe at room temperature. Pump induced amplitude (a) and phase changes (b) for different delay times tD observed for a 1.55 eV pump irradiance of IP10GW/cm2. The grey shaded area in (a) shows the 2ω spectrum in arbitrary units.

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In conclusion, we combine amplitude- and phase-resolution at optical frequencies with femtosecond time-resolution to sensitively trace transient semiconductor optical nonlinearities. The use of other modelocked laser sources and/or detector crystals can easily extend the concept to other optical frequencies. Future studies will focus on optical nonlinearities that mainly manifest as transient phase-retardations—phenomena inaccessible with conventional time-resolved spectroscopy.

We acknowledge helpful discussions with A. W. Holleitner and E. Sternemann and thank D. Schuh and W. Wegscheider for providing the GaAs material. This work is supported by the DFG priority program SPP1391 “Ultrafast Nanooptics”.

References

1. R. A. Kaindl, M. A. Carnahan, D. Hägele, R. Lövenich, and D. S. Chemla, Nature 423, 734 (2003). [CrossRef]  

2. R. Huber, F. Tauser, A. Brodschelm, M. Bichler, G. Abstreiter, and A. Leitenstorfer, Nature 414, 286 (2001). [CrossRef]  

3. T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011). [CrossRef]  

4. C. Kübler, R. Huber, S. Tübel, and A. Leitenstorfer, Appl. Phys. Lett. 85, 3360 (2004). [CrossRef]  

5. A. Sell, R. Scheu, A. Leitenstorfer, and R. Huber, Appl. Phys. Lett. 93, 251107 (2008). [CrossRef]  

6. W. J. Walecki, D. N. Fittinghoff, A. L. Smirl, and R. Trebino, Opt. Lett. 22, 81 (1997). [CrossRef]  

7. D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010). [CrossRef]  

8. M. E. Siemens, G. Moody, H. B. Li, A. D. Bristow, and S. T. Cundiff, Opt. Express 18, 17699 (2010). [CrossRef]  

9. R. Atanasov, A. Haché, J. L. P. Hughes, H. M. van Driel, and J. E. Sipe, Phys. Rev. Lett. 76, 1703 (1996). [CrossRef]  

10. A. Haché, Y. Kostoulas, R. Atanasov, J. L. P. Hughes, J. E. Sipe, and H. M. van Driel, Phys. Rev. Lett. 78, 306 (1997). [CrossRef]  

11. S. Thunich, C. Ruppert, A. W. Holleitner, and M. Betz, Opt. Lett. 36, 1791 (2011). [CrossRef]  

12. M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit a la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988). [CrossRef]  

References

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  1. R. A. Kaindl, M. A. Carnahan, D. Hägele, R. Lövenich, and D. S. Chemla, Nature 423, 734 (2003).
    [Crossref]
  2. R. Huber, F. Tauser, A. Brodschelm, M. Bichler, G. Abstreiter, and A. Leitenstorfer, Nature 414, 286 (2001).
    [Crossref]
  3. T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
    [Crossref]
  4. C. Kübler, R. Huber, S. Tübel, and A. Leitenstorfer, Appl. Phys. Lett. 85, 3360 (2004).
    [Crossref]
  5. A. Sell, R. Scheu, A. Leitenstorfer, and R. Huber, Appl. Phys. Lett. 93, 251107 (2008).
    [Crossref]
  6. W. J. Walecki, D. N. Fittinghoff, A. L. Smirl, and R. Trebino, Opt. Lett. 22, 81 (1997).
    [Crossref]
  7. D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010).
    [Crossref]
  8. M. E. Siemens, G. Moody, H. B. Li, A. D. Bristow, and S. T. Cundiff, Opt. Express 18, 17699 (2010).
    [Crossref]
  9. R. Atanasov, A. Haché, J. L. P. Hughes, H. M. van Driel, and J. E. Sipe, Phys. Rev. Lett. 76, 1703 (1996).
    [Crossref]
  10. A. Haché, Y. Kostoulas, R. Atanasov, J. L. P. Hughes, J. E. Sipe, and H. M. van Driel, Phys. Rev. Lett. 78, 306 (1997).
    [Crossref]
  11. S. Thunich, C. Ruppert, A. W. Holleitner, and M. Betz, Opt. Lett. 36, 1791 (2011).
    [Crossref]
  12. M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit a la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988).
    [Crossref]

2011 (2)

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

S. Thunich, C. Ruppert, A. W. Holleitner, and M. Betz, Opt. Lett. 36, 1791 (2011).
[Crossref]

2010 (2)

D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010).
[Crossref]

M. E. Siemens, G. Moody, H. B. Li, A. D. Bristow, and S. T. Cundiff, Opt. Express 18, 17699 (2010).
[Crossref]

2008 (1)

A. Sell, R. Scheu, A. Leitenstorfer, and R. Huber, Appl. Phys. Lett. 93, 251107 (2008).
[Crossref]

2004 (1)

C. Kübler, R. Huber, S. Tübel, and A. Leitenstorfer, Appl. Phys. Lett. 85, 3360 (2004).
[Crossref]

2003 (1)

R. A. Kaindl, M. A. Carnahan, D. Hägele, R. Lövenich, and D. S. Chemla, Nature 423, 734 (2003).
[Crossref]

2001 (1)

R. Huber, F. Tauser, A. Brodschelm, M. Bichler, G. Abstreiter, and A. Leitenstorfer, Nature 414, 286 (2001).
[Crossref]

1997 (2)

W. J. Walecki, D. N. Fittinghoff, A. L. Smirl, and R. Trebino, Opt. Lett. 22, 81 (1997).
[Crossref]

A. Haché, Y. Kostoulas, R. Atanasov, J. L. P. Hughes, J. E. Sipe, and H. M. van Driel, Phys. Rev. Lett. 78, 306 (1997).
[Crossref]

1996 (1)

R. Atanasov, A. Haché, J. L. P. Hughes, H. M. van Driel, and J. E. Sipe, Phys. Rev. Lett. 76, 1703 (1996).
[Crossref]

1988 (1)

Abstreiter, G.

R. Huber, F. Tauser, A. Brodschelm, M. Bichler, G. Abstreiter, and A. Leitenstorfer, Nature 414, 286 (2001).
[Crossref]

Antonetti, A.

Atanasov, R.

A. Haché, Y. Kostoulas, R. Atanasov, J. L. P. Hughes, J. E. Sipe, and H. M. van Driel, Phys. Rev. Lett. 78, 306 (1997).
[Crossref]

R. Atanasov, A. Haché, J. L. P. Hughes, H. M. van Driel, and J. E. Sipe, Phys. Rev. Lett. 76, 1703 (1996).
[Crossref]

Benoit a la Guillaume, C.

Betz, M.

Bichler, M.

R. Huber, F. Tauser, A. Brodschelm, M. Bichler, G. Abstreiter, and A. Leitenstorfer, Nature 414, 286 (2001).
[Crossref]

Bristow, A. D.

D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010).
[Crossref]

M. E. Siemens, G. Moody, H. B. Li, A. D. Bristow, and S. T. Cundiff, Opt. Express 18, 17699 (2010).
[Crossref]

Brodschelm, A.

R. Huber, F. Tauser, A. Brodschelm, M. Bichler, G. Abstreiter, and A. Leitenstorfer, Nature 414, 286 (2001).
[Crossref]

Carnahan, M. A.

R. A. Kaindl, M. A. Carnahan, D. Hägele, R. Lövenich, and D. S. Chemla, Nature 423, 734 (2003).
[Crossref]

Chemla, D. S.

R. A. Kaindl, M. A. Carnahan, D. Hägele, R. Lövenich, and D. S. Chemla, Nature 423, 734 (2003).
[Crossref]

Cundiff, S. T.

M. E. Siemens, G. Moody, H. B. Li, A. D. Bristow, and S. T. Cundiff, Opt. Express 18, 17699 (2010).
[Crossref]

D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010).
[Crossref]

Dai, X. C.

D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010).
[Crossref]

Dekorsy, T.

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

Fiebig, M.

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

Fittinghoff, D. N.

Haché, A.

A. Haché, Y. Kostoulas, R. Atanasov, J. L. P. Hughes, J. E. Sipe, and H. M. van Driel, Phys. Rev. Lett. 78, 306 (1997).
[Crossref]

R. Atanasov, A. Haché, J. L. P. Hughes, H. M. van Driel, and J. E. Sipe, Phys. Rev. Lett. 76, 1703 (1996).
[Crossref]

Hägele, D.

R. A. Kaindl, M. A. Carnahan, D. Hägele, R. Lövenich, and D. S. Chemla, Nature 423, 734 (2003).
[Crossref]

Holleitner, A. W.

Huber, R.

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

A. Sell, R. Scheu, A. Leitenstorfer, and R. Huber, Appl. Phys. Lett. 93, 251107 (2008).
[Crossref]

C. Kübler, R. Huber, S. Tübel, and A. Leitenstorfer, Appl. Phys. Lett. 85, 3360 (2004).
[Crossref]

R. Huber, F. Tauser, A. Brodschelm, M. Bichler, G. Abstreiter, and A. Leitenstorfer, Nature 414, 286 (2001).
[Crossref]

Hughes, J. L. P.

A. Haché, Y. Kostoulas, R. Atanasov, J. L. P. Hughes, J. E. Sipe, and H. M. van Driel, Phys. Rev. Lett. 78, 306 (1997).
[Crossref]

R. Atanasov, A. Haché, J. L. P. Hughes, H. M. van Driel, and J. E. Sipe, Phys. Rev. Lett. 76, 1703 (1996).
[Crossref]

Hulin, D.

Joffre, M.

Kaindl, R. A.

R. A. Kaindl, M. A. Carnahan, D. Hägele, R. Lövenich, and D. S. Chemla, Nature 423, 734 (2003).
[Crossref]

Kampfrath, T.

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

Karaiskaj, D.

D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010).
[Crossref]

Klatt, G.

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

Koch, S. W.

Kostoulas, Y.

A. Haché, Y. Kostoulas, R. Atanasov, J. L. P. Hughes, J. E. Sipe, and H. M. van Driel, Phys. Rev. Lett. 78, 306 (1997).
[Crossref]

Kübler, C.

C. Kübler, R. Huber, S. Tübel, and A. Leitenstorfer, Appl. Phys. Lett. 85, 3360 (2004).
[Crossref]

Leitenstorfer, A.

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

A. Sell, R. Scheu, A. Leitenstorfer, and R. Huber, Appl. Phys. Lett. 93, 251107 (2008).
[Crossref]

C. Kübler, R. Huber, S. Tübel, and A. Leitenstorfer, Appl. Phys. Lett. 85, 3360 (2004).
[Crossref]

R. Huber, F. Tauser, A. Brodschelm, M. Bichler, G. Abstreiter, and A. Leitenstorfer, Nature 414, 286 (2001).
[Crossref]

Li, H. B.

Lindberg, M.

Lövenich, R.

R. A. Kaindl, M. A. Carnahan, D. Hägele, R. Lövenich, and D. S. Chemla, Nature 423, 734 (2003).
[Crossref]

Mährlein, S.

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

Migus, A.

Mirin, R. P.

D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010).
[Crossref]

Moody, G.

Mukamel, S.

D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010).
[Crossref]

Pashkin, A.

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

Peyghambarian, N.

Ruppert, C.

Scheu, R.

A. Sell, R. Scheu, A. Leitenstorfer, and R. Huber, Appl. Phys. Lett. 93, 251107 (2008).
[Crossref]

Sell, A.

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

A. Sell, R. Scheu, A. Leitenstorfer, and R. Huber, Appl. Phys. Lett. 93, 251107 (2008).
[Crossref]

Siemens, M. E.

Sipe, J. E.

A. Haché, Y. Kostoulas, R. Atanasov, J. L. P. Hughes, J. E. Sipe, and H. M. van Driel, Phys. Rev. Lett. 78, 306 (1997).
[Crossref]

R. Atanasov, A. Haché, J. L. P. Hughes, H. M. van Driel, and J. E. Sipe, Phys. Rev. Lett. 76, 1703 (1996).
[Crossref]

Smirl, A. L.

Tauser, F.

R. Huber, F. Tauser, A. Brodschelm, M. Bichler, G. Abstreiter, and A. Leitenstorfer, Nature 414, 286 (2001).
[Crossref]

Thunich, S.

Trebino, R.

Tübel, S.

C. Kübler, R. Huber, S. Tübel, and A. Leitenstorfer, Appl. Phys. Lett. 85, 3360 (2004).
[Crossref]

van Driel, H. M.

A. Haché, Y. Kostoulas, R. Atanasov, J. L. P. Hughes, J. E. Sipe, and H. M. van Driel, Phys. Rev. Lett. 78, 306 (1997).
[Crossref]

R. Atanasov, A. Haché, J. L. P. Hughes, H. M. van Driel, and J. E. Sipe, Phys. Rev. Lett. 76, 1703 (1996).
[Crossref]

Walecki, W. J.

Wolf, M.

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

Yang, L. J.

D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010).
[Crossref]

Appl. Phys. Lett. (2)

C. Kübler, R. Huber, S. Tübel, and A. Leitenstorfer, Appl. Phys. Lett. 85, 3360 (2004).
[Crossref]

A. Sell, R. Scheu, A. Leitenstorfer, and R. Huber, Appl. Phys. Lett. 93, 251107 (2008).
[Crossref]

Nature (2)

R. A. Kaindl, M. A. Carnahan, D. Hägele, R. Lövenich, and D. S. Chemla, Nature 423, 734 (2003).
[Crossref]

R. Huber, F. Tauser, A. Brodschelm, M. Bichler, G. Abstreiter, and A. Leitenstorfer, Nature 414, 286 (2001).
[Crossref]

Nature Photon. (1)

T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Nature Photon. 5, 31 (2011).
[Crossref]

Opt. Express (1)

Opt. Lett. (3)

Phys. Rev. Lett. (3)

D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, Phys. Rev. Lett. 104, 117401 (2010).
[Crossref]

R. Atanasov, A. Haché, J. L. P. Hughes, H. M. van Driel, and J. E. Sipe, Phys. Rev. Lett. 76, 1703 (1996).
[Crossref]

A. Haché, Y. Kostoulas, R. Atanasov, J. L. P. Hughes, J. E. Sipe, and H. M. van Driel, Phys. Rev. Lett. 78, 306 (1997).
[Crossref]

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Figures (3)

Fig. 1.
Fig. 1. (a) Experimental setup: the RegA output is split up for use as a pump and as a seed of an OPA generating the ω pulse. A BiBO generates 2ω while a two-color interferometer controls the ω/2ω time delay τ. Another delay line adjusts the pump-2ω delay tD. (b) Photocurrent signal of a contacted LT-GaAs bar upon interferometric variation of τ while 2ω is transmitted through a CdTe thin film (T=7K). Inset: closeup at τ200fs. (c) Spectral domain results derived from a comparison of the data in (b) to a measurement without a sample. The CdTe has a field transmission ΔE/E(ν) (black) and induces a phase retardation ΔΦ(ν) (blue).
Fig. 2.
Fig. 2. Transient spectroscopy of CdTe (T=7K). (a) pump induced photocurrent change ΔI(τ). (b), (c) Fourier transform results for the pump induced change of the field transmission ΔE/E(ν) and phase retardation ΔΦ(ν) for various positive pump-2ω delay times tD. Panels (d) to (f) display the corresponding results for several negative tD.
Fig. 3.
Fig. 3. Transient spectroscopy of 2 mm bulk ZnSe at room temperature. Pump induced amplitude (a) and phase changes (b) for different delay times tD observed for a 1.55 eV pump irradiance of IP10GW/cm2. The grey shaded area in (a) shows the 2ω spectrum in arbitrary units.

Equations (2)

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J˙Eω2E2ωsin(2ΦωΦ2ω).
I(ν,tD)[Eω(ν)]2E2ω(ν,tD).

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