Nondegenerate Pump-probe Spectroscopy Research Articles

Optical control of a dark exciton reservoir

Optically inactive or dark excitons play an important role in exciton and polariton devices. On one hand, they supply excitons to the light cone and feed the photoluminescence signal. On the other hand, they repel radiatively active excitons due to the exchange interaction and contribute to the formation of lateral potentials for exciton and polariton condensates. On top of this, they play an important role in scattering and energy relaxation dynamics of quasiparticles in semiconductors. So far, because of optical inaccessibility, studies were focused typically on one experimental technique, giving information about one quantity of dark excitons. Here we present a comprehensive study of the dark exciton reservoir in a high-quality 14-nm GaAs/AlGaAs quantum well using several experimental techniques. We develop a new method of nonradiative broadening spectroscopy of exciton resonances and combine it with nondegenerate pump-probe spectroscopy. The exciton and carrier dynamics in the reservoir is monitored via dynamic broadening of exciton resonances induced by exciton-exciton and exciton-carrier scattering. The dynamics is found to be strongly dependent on the optical excitation conditions. Based on the experimental results, we develop a model of dynamics in a reservoir of excitons and free carriers. The model allows us to describe the experimentally measured photoluminescence kinetics with no fitting parameters. We also demonstrate the optical control of the dark exciton density by means of an additional excitation that creates imbalance of free carriers depleting the reservoir. These results shed light onto the dynamics of the excitonic ``dark matter'' and pave the way to the high-precision engineering of optically induced potentials in exciton-polariton and integrated photonic devices. We expect that the observed results can be transferred also to other semiconductors so that the current quantum well serves as a high-quality model system.

Nanostructured amorphous gallium phosphide on silica for nonlinear and ultrafast nanophotonics.

Nanophotonics based on high refractive index dielectrics relies on appreciable contrast between the indices of designed nanostructures and their immediate surrounding, which can be achieved by the growth of thin films on low-index substrates. Here we propose the use of high index amorphous gallium phosphide (a-GaP), fabricated by radio-frequency sputter deposition, on top of a low refractive index glass substrate and thoroughly examine its nanophotonic properties. Spectral ellipsometry of the amorphous material demonstrates the optical properties to be considerably close to crystalline gallium phosphide (c-GaP), with low-loss transparency for wavelengths longer than 650 nm. When nanostructured into nanopatches, the second harmonic (SH) response of an individual a-GaP patch is characterized to be more than two orders of magnitude larger than the as-deposited unstructured film, with an anapole-like resonant behavior. Numerical simulations are in good agreement with the experimental results over a large spectral and geometrical range. Furthermore, by studying individual a-GaP nanopatches through non-degenerate pump-probe spectroscopy with sub-10 fs pulses, we find a more than 5% ultrafast modulation of the reflectivity that is accompanied by a slower decaying free carrier contribution, caused by absorption. Our investigations reveal a potential for a-GaP as an adequate inexpensive and CMOS-compatible material for nonlinear nanophotonic applications as well as for photocatalysis.

Ultrafast All-Optical Modulation in 2D Hybrid Perovskites.

Two-dimensional (2D) hybrid organic-inorganic Ruddlesden-Popper perovskites (RPPs) have been recently shown to exhibit large nonlinear optical properties due to the strong excitonic effects present in their multiple quantum wells. In this work, we use nondegenerate pump-probe spectroscopy in the 600-1000 nm wavelength range to study the influence of nonlinear effects on the ultrafast dynamics of 2D RPP thin flakes. We find that, under sub-bandgap excitation, ∼100 nm thick perovskite sheets allow up to ∼2% reflectivity modulation within a 20 fs period, due to the nonlinear optical Kerr effect and two-photon absorption, surpassing by a factor of ∼5 the reported nonlinear performance of photonic metasurfaces and single nanoantennas. When the excitation is resonant with the excitonic absorption, the ultrafast nature of the nonlinear response is lost due to the presence of linear absorption creating long-lived free carriers. Our results suggest that 2D RPPs are potential nanoscale all-optical modulators in the visible/near-infrared waveband for applications such as ultrafast information processing, optical data transmission, and high-performance computing.

Ultrafast Nanoimaging of the Photoinduced Phase Transition Dynamics in VO2.

Many phase transitions in correlated matter exhibit spatial inhomogeneities with expected yet unexplored effects on the associated ultrafast dynamics. Here we demonstrate the combination of ultrafast nondegenerate pump-probe spectroscopy with far from equilibrium excitation, and scattering scanning near-field optical microscopy (s-SNOM) for ultrafast nanoimaging. In a femtosecond near-field near-IR (NIR) pump and mid-IR (MIR) probe study, we investigate the photoinduced insulator-to-metal (IMT) transition in nominally homogeneous VO2 microcrystals. With pump fluences as high as 5 mJ/cm(2), we can reach three distinct excitation regimes. We observe a spatial heterogeneity on ∼50-100 nm length scales in the fluence-dependent IMT dynamics ranging from <100 fs to ∼1 ps. These results suggest a high sensitivity of the IMT with respect to small local variations in strain, doping, or defects that are difficult to discern microscopically. We provide a perspective with the distinct requirements and considerations of ultrafast spatiotemporal nanoimaging of phase transitions in quantum materials.

Ultrafast pump-probe spectroscopy in gallium arsenide at 25 T.

We have performed high-fluence, nondegenerate pump-probe spectroscopy in the Split Florida-Helix magnet at 25 T and 15 K. The electronic component of our ultrafast differential reflectivity can be described with a simplified four-level approximation to determine the scattering and recombination rates. Ultrafast oscillations are well described by a coherent acoustic phonon model. Our free-space ultrafast spectroscopic technique will permit future experimental investigations to study novel photoinduced phase transitions and complex interactions in correlated electron systems, which will require the high pulse energies of our free-space alternative.

Ultrafast ablation dynamics in fused silica with a white light beam probe

This study demonstrates a non-degenerate pump-probe spectroscopy with a white light beam probe based on a regenerative, amplified, mode-locked, Ti:sapphire laser. This white light beam probe is produced by supercontinuum generation of sapphire crystal after ultra-short pulse excitation. To implement the pump-probe experimental operation, the ablation dynamics with and without fresh spot measurements in fused silica samples are demonstrated. Combining the time-resolved differential reflection profiles in the white light range and X-ray photoelectron spectroscopy spectra of fused silica, the following ablation dynamics processes can be observed: Without fresh spot measurements, once carriers are excited, first, the three absorption bands of the intrinsic defect sites are observed within 750 fs. Then, a fast recovery is observed. This recovery comes from defect-trapped carriers excited to conduction bands through hot-carrier-phonon interactions. In the final step, a rapidly rising signal is observed after 800 fs. This signal rise comes from the creation of free-electron plasma, the density of which increases with increasing excitation energy accumulation. With fresh spot measurements, time delay of carrier dynamics among the three bands can be identified clearly within 750 fs. The intrinsic defect sites of fused silica play the key role during the ultrafast laser ablation process.

Identification of competing ultrafast all-optical switching mechanisms in Si woodpile photonic crystals

We present a systematic study of ultrafast all-optical switching of Si photonic bandgap woodpile crystals using broadband tunable nondegenerate pump-probe spectroscopy. At pump-probe coincidence, we investigate the behavior of the differential reflectivity at the blue edge of the stop band for a wide range of pump and probe frequencies. Both dispersive and absorptive features are observed from the probe spectra at coincidence. As the pump frequency is tuned through half the electronic bandgap of Si, the magnitude of both these features increases. For the first time, to the best of our knowledge, we unambiguously identify this dispersive effect with the electronic Kerr effect in photonic crystals and attribute the absorptive features to nondegenerate two photon absorption. The dispersive and absorptive nonlinear coefficients are extracted and are found to agree well with the literature. Finally, we propose a nondegenerate figure of merit, which defines the quality of switching for all nondegenerate optical switching processes.

Femtosecond pump-probe spectroscopy and time-resolved photoluminescence of anInxGa1−xN/GaNdouble heterostructure

We report a study of the carrier dynamics in an ${\mathrm{In}}_{0.18}{\mathrm{Ga}}_{0.82}\mathrm{N}$ thin film photoexcited well above the band gap using nondegenerate pump-probe spectroscopy and time-resolved photoluminescence (TRPL) for carrier densities ranging from ${10}^{17}$ to ${10}^{19} {\mathrm{cm}}^{\ensuremath{-}3}$ at 10 K. At carrier densities greater than $4\ifmmode\times\else\texttimes\fi{}{10}^{18} {\mathrm{cm}}^{\ensuremath{-}3},$ optical gain occurs across the entire band tail region after $\ensuremath{\sim}2.5 \mathrm{ps}$ time delay, when the hot carriers completely fill these states. From TRPL measurements performed in the surface emission geometry, we observed stimulated emission (SE) with a $\ensuremath{\sim}28 \mathrm{ps}$ decay time. Since this SE has a threshold density of $1\ifmmode\times\else\texttimes\fi{}{10}^{18} {\mathrm{cm}}^{\ensuremath{-}3},$ which is larger than the total density of localized states, and the SE spectra at early time delays are quite different from the spontaneous emission spectra, we attribute the SE to the recombination of an electron-hole plasma from renormalized band-to-band transitions.

Ultrafast all-optical modulation by near-infrared intersubband transition in n-doped InGaAs/AlAsSb quantum wells

We demonstrate the ultrafast modulation of interband (IB)-resonant light (1.0–1.1 μm) by near-infrared intersubband (ISB)-resonant light (1.55–1.9 μm) in n-doped InGaAs/AlAsSb multiple quantum wells (QWs) using non-degenerate pump–probe spectroscopy. A modulation with an absorption recovery time of 1.0–2.0 ps has been observed in a planer-type modulation device due to ultrafast ISB relaxation of the carriers. The IB carrier relaxation process in the absence of an ISB-resonant light has also been investigated by time-resolved photoluminescence (PL) measurement. The modulation speed is determined by the inter- and intra-subband relaxation of the carriers in the conduction subband. The modulation speed at 1.1 μm due to an ISB-resonant pump light at 1.95 μm has been observed to be 1.4 ps at excitation energy of 500 fJ/μm2.

Gain components in the Autler-Townes doublet from quantum interferences in decay channels

We consider non-degenerate pump-probe spectroscopy of V-systems under conditions such that interference among decay channels is important. We demonstrate how this interference can result in new gain features instead of the usual absorption features. We relate this gain to the existence of a new vacuum induced quasi-trapped-state. We further show how this also results in large refractive index with low absorption.