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Register a new userBroadband sensitive pump-probe setup for ultrafast optical switching of photonic nanostructures and semiconductors
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We describe an ultrafast time resolved pump-probe spectroscopy setup aimed at studying the switching of nanophotonic structures. Both fs pump and probe pulses can be independently tuned over broad frequency range between 3850 and 21050 cm$^{-1}$. A broad pump scan range allows a large optical penetration depth, while a broad probe scan range is crucial to study strongly photonic crystals. A new data acquisition method allows for sensitive pump-probe measurements, and corrects for fluctuations in probe intensity and pump stray light. We observe a tenfold improvement of the precision of the setup compared to laser fluctuations, allowing a measurement accuracy of better than $Delta$R= 0.07% in a 1 s measurement time. Demonstrations of the improved technique are presented for a bulk Si wafer, a 3D Si inverse opal photonic bandgap crystal, and z-scan measurements of the two-photon absorption coefficient of Si, GaAs, and the three-photon absorption coefficient of GaP in the infrared wavelength range.
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We report here an experimental setup to perform three-pulse pump-probe measurements over a wide wavelength and temperature range. By combining two pump pulses in the visible (650-900 nm) and mid-IR (5-20 $mu$m) range, with a broadband supercontinuum white-light probe, our apparatus enables both the combined selective excitation of different material degrees of freedom and a full time-dependent reconstruction of the non-equilibrium dielectric function of the sample. We describe here the optical setup, the cryogenic sample environment and the custom-made acquisition electronics capable of referenced single-pulse detection of broadband spectra at the maximum repetition rate of 50 kHz, achieving a sensitivity of the order of 10$^{-4}$ over an integration time of 1 s. We demonstrate the performance of the setup by reporting data on mid-IR pump, optical push and broadband probe in a single-crystal of Bi$_2$Sr$_2$Y$_{0.08}$Ca$_{0.92}$Cu$_2$O$_{8+delta}$ across the superconducting and pseudogap phases.
The functionalities of a wide range of optical and opto-electronic devices are based on resonance effects and active tuning of the amplitude and wavelength response is often essential. Plasmonic nanostructures are an efficient way to create optical resonances, a prominent example is the extraordinary optical transmission (EOT) through arrays of nanoholes patterned in a metallic film. Tuning of resonances by heating, applying electrical or optical signals has proven to be more elusive, due to the lack of materials that can induce modulation over a broad spectral range and/or at high speeds. Here we show that nanopatterned metals combined with phase change materials (PCMs) can overcome this limitation due to the large change in optical constants which can be induced thermally or on an ultrafast timescale. We demonstrate resonance wavelength shifts as large as 385 nm - an order of magnitude higher than previously reported - by combining properly designed Au EOT nanostructures with Ge2Sb2Te5 (GST). Moreover, we show, through pump probe measurements, repeatable and reversible, large amplitude modulations in the resonances, especially at telecommunication wavelengths, over ps time scales and at powers far below those needed to produce a permanent phase transition. Our findings open a pathway to the design of hybrid metal PCM nanostructures with ultrafast and widely tuneable resonance responses, which hold potential impact on active nanophotonic devices such as tuneable optical filters, smart windows, biosensors and reconfigurable memories.
We present ultrafast optical switching experiments on 3D photonic band gap crystals. Switching the Si inverse opal is achieved by optically exciting free carriers by a two-photon process. We probe reflectivity in the frequency range of second order Bragg diffraction where the photonic band gap is predicted. We find good experimental switching conditions for free-carrier plasma frequencies between 0.3 and 0.7 times the optical frequency: we thus observe a large frequency shift of up to D omega/omega= 1.5% of all spectral features including the peak that corresponds to the photonic band gap. We deduce a corresponding large refractive index change of Dn_Si/n_Si= 2.0% and an induced absorption length that is longer than the sample thickness. We observe a fast decay time of 21 ps, which implies that switching could potentially be repeated at GHz rates. Such a high switching rate is relevant to future switching and modulation applications.
We present ultrafast all-optical switching measurements of Si woodpile photonic band gap crystals. The crystals are spatially homogeneously excited, and probed by measuring reflectivity over an octave in frequency (including the telecom range) as a function of time. After 300 fs, the complete stop band has shifted to higher frequencies as a result of optically excited free carriers. The switched state relaxes quickly with a time constant of 18 ps. We present a quantitative analysis of switched spectra with theory for finite photonic crystals. The induced changes in refractive index are well described by a Drude model with a carrier relaxation time of 10 fs. We briefly discuss possible applications of high-repetition rate switching of photonic crystal cavities.
Sculpting sub-cycle temporal structures of optical waveforms allows one to image and even control electronic clouds in atoms, molecules and solids. Here we show how the transverse spin component arising upon spatial confinement of such optical waveforms enables extremely efficient chiral recognition and control of ultrafast chiral dynamics. When an intense few-cycle, linearly polarized laser pulse is tightly focused into a medium of randomly oriented chiral molecules, the medium generates light which is elliptically polarized, with opposite helicities and opposite rotations of the polarization ellipse in media of opposite handedness. In contrast to conventional optical activity of chiral media, this new nonlinear optical activity is driven by purely electric-dipole interactions and leads to giant enantio-sensitivity in the near VIS-UV domain, where optical instrumentation is readily available. Adding a polarizer turns rotation of the polarization ellipse into highly enantio-sensitive intensity of the nonlinear-optical response. Sub-cycle optical control of the incident light wave enables full control over the enantio-sensitive response. The proposed all-optical method not only enables extremely efficient chiral discrimination, but also ultrafast imaging and control of chiral dynamics with commercially available optical technology.
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