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Register a new userVisible pump -- mid infrared pump -- broadband probe: development and characterization of a three-pulse setup for single-shot ultrafast spectroscopy at 50 kHz
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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.
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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.
We present a novel microscopic technique to access local transient optical constants and carrier motion in thin-film materials in three dimensions, with sub-10 nm spatial precision and sub-15 fs temporal resolution. Our experimental scheme is based on imaging a traditionally defocussed plane in an interferometrically enhanced femtosecond pump-probe microscope, combining the amplitude and phase contrast between the perturbed and unperturbed probe due to the local photoinduced complex refractive index change. We find that our experimental approach is well described by a simple optical model based on a radially averaged Gaussian photoexcitation approximation, which we benchmark using finite-difference time-domain calculations. Measurements on the organic semiconductor pentacene reveal an unexpected sub-1 ps out-of-plane motion of the correlated triplet-triplet exciton. Our approach is applicable to thin film materials in any pump-probe experiment, and holds promise for quantitative studies of three-dimensional transport in semiconductors, especially relevant to next-generation functional materials.
Time- and angle-resolved photoelectron spectroscopy (trARPES) is a powerful method to track the ultrafast dynamics of quasiparticles and electronic bands in energy and momentum space. We present a setup for trARPES with 22.3 eV extreme-ultraviolet (XUV) femtosecond pulses at 50-kHz repetition rate, which enables fast data acquisition and access to dynamics across momentum space with high sensitivity. The design and operation of the XUV beamline, pump-probe setup, and UHV endstation are described in detail. By characterizing the effect of space-charge broadening, we determine an ultimate source-limited energy resolution of 60 meV, with typically 80-100 meV obtained at 1-2e10 photons/s probe flux on the sample. The instrument capabilities are demonstrated via both equilibrium and time-resolved ARPES studies of transition-metal dichalcogenides. The 50-kHz repetition rate enables sensitive measurements of quasiparticles at low excitation fluences in semiconducting MoSe$_2$, with an instrumental time resolution of 65 fs. Moreover, photo-induced phase transitions can be driven with the available pump fluence, as shown by charge density wave melting in 1T-TiSe$_2$. The high repetition-rate setup thus provides a versatile platform for sensitive XUV trARPES, from quenching of electronic phases down to the perturbative limit.
We investigate the valley related carrier dynamics in monolayer MoS2 using helicity resolved non-degenerate ultrafast pump-probe spectroscopy at the vicinity of the high-symmetry K point under the temperature down to 78 K. Monolayer MoS2 shows remarkable transient reflection signals, in stark contrast to bilayer and bulk MoS2 due to the enhancement of many-body effect at reduced dimensionality. The helicity resolved ultrafast time-resolved result shows that the valley polarization is preserved for only several ps before scattering process makes it undistinguishable. We suggest that the dynamical degradation of valley polarization is attributable primarily to the exciton trapping by defect states in the exfoliated MoS2 samples. Our experiment and a tight-binding model analysis also show that the perfect valley CD selectivity is fairly robust against disorder at the K point, but quickly decays from the high-symmetry point in the momentum space in the presence of disorder.
The parkerite-type ternary chalcogenide Bi$_2$Rh$_3$Se$_2$ was discovered to be a charge density wave (CDW) superconductor. However, there was a debate on whether the observed phase transition at 240 K could be attributed to the formation of CDW order. To address the issue, we performed optical spectroscopy and ultrafast pump-probe measurements on single crystal samples of Bi$_2$Rh$_3$Se$_2$. Our optical conductivity measurement reveals clearly the formation of an energy gap with associated spectral change only at low energies, yielding strong evidence for a CDW phase transition at 240 K. Time resolved pump-probe measurement provides further support for the CDW phase transition. The amplitude and relaxation time of quasiparticles extracted from the photoinduced reflectivity show strong enhancement near transition temperature, yielding further evidence for the CDW energy gap formation. Additionally, a collective mode is identified from the oscillations in the pump-probe time delay at low temperature. This mode, whose frequency decreases gradually at elevated temperature, could be naturally attributed to the amplitude mode of CDW state.
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