Robert A. Kaindl

Generation, shaping, and characterization of intense femtosecond pulses tunable from 3 to 20 µm

We report on an intense mid-infrared light source that provides femtosecond pulses on a microjoule energy level, broadly tunable in the 3–20-µm wavelength range with pulse durations as short as 50 fs at 5 µm. The pulses are generated by phase-matched difference-frequency mixing in GaSe of near-infrared signal and idler pulses of a parametric device based on a 1-kHz Ti:sapphire amplifier system. Pulse durations are characterized with different techniques including autocorrelation measurements in AgGaS2, two-photon absorption in InSb, and cross-correlation measurements with near-infrared pulses in a thin GaSe crystal. A subsequent zero-dispersion stretcher of high transmission allows for optimum pulse compression, a more detailed amplitude and phase characterization and, ultimately, amplitude shaping of the mid-infrared pulses.

Ultrafast terahertz probes of transient conducting and insulating phases in an electron–hole gas

Many-body systems in nature exhibit complexity and self-organization arising from seemingly simple laws. For example, the long-range Coulomb interaction between electrical charges has a simple form, yet is responsible for a plethora of bound states in matter, ranging from the hydrogen atom to complex biochemical structures. Semiconductors form an ideal laboratory for studying many-body interactions of electronic quasiparticles among themselves and with lattice vibrations and light. Oppositely charged electron and hole quasiparticles can coexist in an ionized but correlated plasma, or form bound hydrogen-like pairs called excitons. The pathways between such states, however, remain elusive in near-visible optical experiments that detect a subset of excitons with vanishing centre-of-mass momenta. In contrast, transitions between internal exciton levels, which occur in the far-infrared at terahertz (1012 s-1) frequencies, are independent of this restriction, suggesting their use as a probe of electron–hole pair dynamics. Here we employ an ultrafast terahertz probe to investigate directly the dynamical interplay of optically-generated excitons and unbound electron–hole pairs in GaAs quantum wells. Our observations reveal an unexpected quasi-instantaneous excitonic enhancement, the formation of insulating excitons on a 100-ps timescale, and the conditions under which excitonic populations prevail.

Broadband electromagnetic response and ultrafast dynamics of few-layer epitaxial graphene

We study the broadband optical conductivity and ultrafast carrier dynamics of epitaxial graphene in the few-layer limit. Equilibrium spectra of nominally buffer, monolayer, and multilayer graphene exhibit significant terahertz and near-infrared absorption, consistent with a model of intra- and interband transitions in a dense Dirac electron plasma. Non-equilibrium terahertz transmission changes after photoexcitation are shown to be dominated by excess hole carriers, with a 1.2-ps mono-exponential decay that refects the minority-carrier recombination time.

Broadband phase-matched difference frequency mixing of femtosecond pulses in GaSe: Experiment and theory

Phase-matched difference frequency mixing within the broad spectrum of single 13 fs pulses from a cavity-dumped, mode-locked Ti:sapphire laser in a GaSe crystal allows the generation of femtosecond mid-infrared pulses, continuously tunable in the wavelength range from 7 to 20 μm. Pulse durations down to 95 fs at 9.3 μm are directly measured. Model calculations including the full dispersion of GaSe show that the chirp of the pump pulses allows to change both the pulse duration and conversion efficiency obtained in the nonlinear process, in agreement with the experiment.

Femtosecond infrared pulses tunable from 9 to 18??µm at an 88-MHz repetition rate

Femtosecond mid-infrared laser pulses that are continuously tunable in the wavelength range from 9 to 18mum are demonstrated. These nearly bandwidth-limited pulses are generated by phase-matched difference-frequency mixing within the broad spectrum of 20-fs pulses from a mode-locked Ti:sapphire laser in GaSe. A direct determination of the pulse duration at 11.5mum gives a value of 140 fs. The average mid-infrared power of 1muW is ~100 times greater than that for infrared generation by non-phase-matched optical rectification.

Far-infrared optical conductivity gap in superconducting MgB2 films

We report the first study of the optical conductivity of MgB2 covering the range of its lowest-energy superconducting gap. Terahertz time-domain spectroscopy is utilized to determine the complex, frequency-dependent conductivity sigma(omega) of thin films. The imaginary part reveals an inductive response due to the emergence of the superconducting condensate. The real part exhibits a strong depletion of oscillator strength near 5 meV resulting from the opening of a superconducting energy gap. The gap ratio of 2Delta0/k(B)TC approximately 1.9 is well below the weak-coupling value, pointing to complex behavior in this novel superconductor.

Transient terahertz spectroscopy of excitons and unbound carriers in quasi two-dimensional electron-hole gases

We report a comprehensive experimental study and detailed model analysis of the terahertz (THz) dielectric response and density kinetics of excitons and unbound electron-hole pairs in GaAs quantum wells. A compact expression is given, in absolute units, for the complex-valued THz dielectric function of intra-excitonic transitions between the 1s and higher-energy exciton and continuum levels. It closely describes the THz spectra of resonantly generated excitons. Exciton ionization and formation are further explored, where the THz response exhibits both intra-excitonic and Drude features. Utilizing a two-component dielectric function, we derive the underlying exciton and unbound pair densities. In the ionized state, excellent agreement is found with the Saha thermodynamic equilibrium, which provides experimental verification of the two-component analysis and density scaling. During exciton formation, in turn, the pair kinetics is quantitatively described by a Saha equilibrium that follows the carrier cooling dynamics. The THz-derived kinetics is, moreover, consistent with time-resolved luminescence measured for comparison. Our study establishes a basis for tracking pair densities via transient THz spectroscopy of photoexcited quasi-2D electron-hole gases.

Controlled shaping of ultrafast electric field transients in the mid-infrared spectral range

We experimentally demonstrate amplitude and phase shaping of femtosecond mid-infrared pulses in a range centered about 14 mum . Single pulses with a tailored optical phase and phase-locked double pulses are generated by phase-matched difference-frequency mixing in a GaSe crystal of near-infrared pulses shaped with a liquid-crystal modulator. The electric field transients are directly measured by free-space electro-optic sampling, yielding pulse durations of 200-300 fs. Our data are in good agreement with a model that describes phase-matched optical rectification.

Atomic-scale perspective of ultrafast charge transfer at a dye-semiconductor interface

Understanding interfacial charge-transfer processes on the atomic level is crucial to support the rational design of energy-challenge relevant systems such as solar cells, batteries, and photocatalysts. A femtosecond time-resolved core-level photoelectron spectroscopy study is performed that probes the electronic structure of the interface between ruthenium-based N3 dye molecules and ZnO nanocrystals within the first picosecond after photoexcitation and from the unique perspective of the Ru reporter atom at the center of the dye. A transient chemical shift of the Ru 3d inner-shell photolines by (2.3 ± 0.2) eV to higher binding energies is observed 500 fs after photoexcitation of the dye. The experimental results are interpreted with the aid of ab initio calculations using constrained density functional theory. Strong indications for the formation of an interfacial charge-transfer state are presented, providing direct insight into a transient electronic configuration that may limit the efficiency of photoinduced free charge-carrier generation.

Nodal quasiparticle meltdown in ultrahigh-resolution pump–probe angle-resolved photoemission

Where a superconductor has a node, or a zero, in the superconducting gap, low-energy excitations exist that are similar to those in normal metals and are thought to be unaffected by superconductivity. However, excitation of superconductors with a near infrared pulse reveals there is a link between these excitations and superconductivity.