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Coulomb-mediated interactions between intersubband excitations of electrons in GaAs/AIGaAs double quantum wells and longitudinal optical phonons are studied by two-dimensional spectroscopy in the terahertz frequency range. The multitude of diagonal and off-diagonal peaks in the 2D spectrum gives evidence of strong polaronic signatures in the nonlinear response. A quantitative theoretical analysis reveals a dipole coupling of electrons to the polar lattice that is much stronger than in bulk GaAs, due to a dynamic localization of the electron wave function by scattering processes. [ABSTRACT FROM AUTHOR]

Femtosecond x-ray absorption spectroscopy with a laser-driven high-harmonic source is used to map ultrafast changes of x-ray absorption by femtometer-scale coherent phonon displacements. In LiBH4, displacements along an Ag phonon mode at 10 THz are induced by impulsive Raman excitation and give rise to oscillatory changes of x-ray absorption at the Li K edge. Electron density maps from femtosecond x-ray diffraction data show that the electric field of the pump pulse induces a charge transfer from the BH4- to neighboring Li+ ions, resulting in a differential Coulomb force that drives lattice vibrations in this virtual transition state. [ABSTRACT FROM AUTHOR]

The terahertz (THz) response of the ferroelectric prototype material lithium niobate (LiNbO3) is studied in the nonperturbative regime of light-matter interaction. Applying two-dimensional THz spectroscopy with few-cycle pulses of an amplitude E≈100??kV/cm and a center frequency of 2 THz, we dissect the overall nonlinear response into different orders in the electric field. The underlying nonlinear current is of interband character and consists of a strong low-frequency shift current (SC) and higher harmonics of the THz fundamental. The SC component originates from the lack of inversion symmetry and the strong interband decoherence for long electron trajectories in k space as shown by theoretical calculations. [ABSTRACT FROM AUTHOR]

The nonlinear dynamics of electrons in multilayer epitaxial graphene is investigated by time-resolved terahertz (THz) spectroscopy in a regime where the interaction of electrons with the external field dominates over scattering processes. The predominantly coherent electron response to the THz field involves both intra- and interband currents, leading to coherently driven interband transitions of carriers and to the generation of higher harmonics of the THz carrier frequency. The overall behavior of the graphene layers is always absorptive, even after generation of an initial electron-hole distribution by femtosecond midinfrared excitation. The results are in agreement with theoretical calculations of the nonperturbative THz response. [ABSTRACT FROM AUTHOR]

Transient polarizations connected with a spatial redistribution of electronic charge in a mixed quantum state are induced by optical fields of high amplitude. We determine for the first time the related transient electron density maps, applying femtosecond x-ray powder diffraction as a structure probe. The prototype ionic material LiBH4 driven nonresonantly by an intense sub-40 fs optical pulse displays a large-amplitude fully reversible electron transfer from the BH4- anion to the Li+ cation during excitation. Our results establish this mechanism as the source of the strong optical polarization which agrees quantitatively with theoretical estimates. [ABSTRACT FROM AUTHOR]

Charge transpor t in an electron-hole plasma driven by high-field terahertz (THz) pulses is strongly influenced by electron-hole interactions, as has been shown in a recent publication [P. Bowlan et al, Phys. Rev. Lett. 107, 256602 (2011)]. We introduce a picture of high-field THz transport which accounts for the roles of both types of carriers including their interactions. While holes make a negligible contribution to the current, they are heated by absorbing energy from the driving THz field and introduce a friction force for the electrons over a period of about 500 fs. Our model uses an extended version of the loss-function concept to calculate the time-dependent friction. The local field that drives the electrons differs from the incident THz field by screening due to Coulomb correlations in the plasma. We illustrate how spatial correlations between charged particles (electrons, holes, impurities) create a significant local-field correction to the THz driving field. The dominant contribution stems from Coulomb-correlated heavy-hole wave packets, which are strongly polarizable via inter-valence-band transitions [ABSTRACT FROM AUTHOR]

The nonlinear polaronic response of electrons solvated in liquid 2-propanol is studied by two-dimensional terahertz spectroscopy. Solvated electrons with a concentration of c_{e}≈800  μM are generated by femtosecond photoionization of alcohol molecules. Electron relaxation to a localized ground state impulsively excites coherent polaron oscillations with a frequency of 3.9 THz. Off-resonant perturbation of the terahertz coherence by a pulse centered at 1.5 THz modifies the polaron oscillation phase. This nonlinear change of electron polarizability is reproduced by theoretical calculations.

The impact of coherent phonon excitations on the valence charge distribution in cubic boron nitride is mapped by femtosecond x-ray powder diffraction. Zone-edge transverse acoustic (TA) two-phonon excitations generated by an impulsive Raman process induce a steplike increase of diffracted x-ray intensity. Charge density maps derived from transient diffraction patterns reveal a spatial transfer of valence charge from the interstitial region onto boron and nitrogen atoms. This transfer is modulated with a frequency of 250 GHz due to a coherent superposition of TA phonons related to the ^{10}B and ^{11}B isotopes. Nuclear and electronic degrees of freedom couple through many-body Coulomb interactions.

The terahertz (THz) response of solvated electrons in liquid water is studied in nonlinear ultrafast pump-probe experiments. Free electrons with concentrations from c_{e}=4 to 140×10^{-6} moles/liter are generated by high-field THz or near-infrared multiphoton excitation. The time-resolved change of the dielectric function as mapped by broadband THz pulses exhibits pronounced oscillations persisting up to 30 ps. Their frequency increases with electron concentration from 0.2 to 1.5 THz. The oscillatory response is assigned to impulsively excited coherent polarons involving coupled electron and water shell motions with a frequency set by the local electric field.

The impact of transient electric currents on the transverse optical (TO) phonon resonance is studied after excitation by two femtosecond near-infrared pulses via the fourth-order nonlinear terahertz emission. Nonlinear signals due to interband shift currents and heavy-hole-light-hole polarizations are separated from Raman-induced TO phonon coherences. The latter display a frequency upshift by some 100 GHz upon interband excitation of an electron-hole plasma. The frequency shift is caused by transverse electronic shift currents, which modify the dielectric function. A local-field model based on microscopic current densities reproduces the observed frequency upshift.

We demonstrate amplification of longitudinal optical (LO) phonons by polar-optical interaction with an electron plasma in a GaAs structure coupled to a metallic metasurface using two-color two-dimensional spectroscopy. In a novel scheme, the metamaterial resonator enhances broadband terahertz fields, which generate coherent LO phonons and drive free electrons in the conduction band of GaAs. The time evolution of the LO phonon amplitude is monitored with midinfrared pulses via the LO-phonon-induced Kerr nonlinearity of the sample, showing an amplification of the LO phonon amplitude by up to a factor of 10, in agreement with a theoretical estimate.

The second-order nonlinear response of bulk GaAs in the terahertz (THz) range is mapped via the THz field emitted after near-infrared interband excitation. Phase-resolved THz detection reveals three nonlinear processes occurring in parallel, the Raman excitation of transverse optical phonons, the creation of coherent polarizations on heavy-hole-light-hole transitions, and the generation of displacive shift currents with a THz spectrum controlled by the near-infrared optical phase. Theoretical calculations reproduce the data and demonstrate the interband character of shift currents.

The nonlinear response of soft-mode excitations in polycrystalline acetylsalicylic acid (aspirin) is studied with two-dimensional terahertz spectroscopy. We demonstrate that the correlation of CH_{3} rotational modes with collective oscillations of π electrons drives the system into the nonperturbative regime of light-matter interaction, even for a moderate strength of the THz driving field on the order of 50  kV/cm. Nonlinear absorption around 1.1 THz leads to a blueshifted coherent emission at 1.7 THz, revealing the dynamic breakup of the strong electron-phonon correlations. The observed behavior is reproduced by theoretical calculations including dynamic local-field correlations.

We report the first observation of two-phonon quantum coherences in a semiconductor. Two-dimensional terahertz (THz) spectra recorded with a sequence of three THz pulses display strong two-phonon signals, clearly distinguished from signals due to interband two-photon absorption and electron tunneling. The two-phonon coherences originate from impulsive off-resonant excitation in the nonperturbative regime of light-matter interaction. A theoretical analysis provides the relevant Liouville pathways, showing that nonlinear interactions using the large interband dipole moment generate stronger two-phonon excitations than linear interactions.

Sound amplification in an electrically biased superlattice (SL) is studied in optical experiments with 100 fs time resolution. Coherent SL phonons with frequencies of 40, 375, and 410 GHz give rise to oscillatory reflectivity changes. With currents from 0.5 to 1.3 A, the Fourier amplitude of the 410 GHz phonon increases by more than a factor of 2 over a 200 ps period. This amplification is due to stimulated Čerenkov phonon emission by electrons undergoing intraminiband transport. The gain coefficient of 8×10^{3}  cm^{-1} is reproduced by theoretical calculations and holds potential for novel sub-THz phonon emitters.

Longitudinal bulk plasmons in an n-doped ZnO layer system are studied by two-color femtosecond pump-probe spectroscopy in the midinfrared. The optical bulk plasmon resonance identified in linear reflectivity spectra undergoes a strong redshift and a limited broadening upon intraband excitation of electrons. The nonlinear changes of plasmon absorption decay on a time scale of 2 ps and originate from the intraband redistribution of electrons. Theoretical calculations explain the plasmon redshift by the transient increase of the ensemble-averaged electron mass and the concomitantly reduced plasma frequency in the hot electron plasma. The observed bulk plasmon nonlinearity holds strong potential for applications in plasmonics.

We study the quasi-instantaneous change of electron density in the unit cells of LiH and NaBH4 in response to a nonresonant strong optical field. We determine for the first time the related transient electron density maps, applying femtosecond x-ray powder diffraction as a structure probe. The light-induced charge relocation in NaBH4 exhibits an electron transfer from the anion (BH(4)(-)) to the Na(+) cation. In contrast, LiH displays the opposite behavior, i.e., an increase of the ionicity of LiH in the presence of the strong electric field. This behavior originates from strong electron correlations in LiH, as is evident from a comparison with quasiparticle band structures calculated within the Coulomb-hole-plus-screened-exchange formalism.

The time evolution of high-field carrier transport in bulk GaAs is studied with intense femtosecond THz pulses. While ballistic transport of electrons occurs in an n-type sample, a transition from ballistic to driftlike motion is observed in an electron-hole plasma. This onset of friction is due to the holes, which are heated by THz absorption. Theoretical calculations, which reproduce the data quantitatively, show that both electron-hole scattering and local-field effects in the electron-hole plasma are essential for the time-dependent friction., (© 2011 American Physical Society)

We present a combined theoretical and experimental study of spatiotemporal propagation effects in terahertz (THz) generation in gases using two-color ionizing laser pulses. The observed strong broadening of the THz spectra with increasing gas pressure reveals the prominent role of spatiotemporal reshaping and of a plasma-induced blueshift of the pump pulses in the generation process. Results obtained from (3+1)-dimensional simulations are in good agreement with experimental findings and clarify the mechanisms responsible for THz emission.

Electrons in bulk n-doped GaAs at a lattice temperature of 300 K are driven by ultrashort high-field transients of up to 300 kV/cm in the terahertz frequency range. In the lowest conduction band the carriers show coherent ballistic motion, which is detected via the THz field emitted by them. This partial Bloch oscillation is reproduced by a quantum-kinetic theory of coherent transport on ultrafast time scales.

We report the first analysis of the polarization and lattice dynamics in a metal/ferroelectric/metal nanolayer system by femtosecond x-ray diffraction. Two Bragg reflections provide information on the coupled dynamics of the two relevant phonon modes for ferroelectricity in perovskites, the tetragonal distortion and the soft mode. Optical excitation of the SrRuO(3) metal layers generates giant stress (>1 GPa) compressing the PbZr(0.2)Ti(0.8)O(3) layers by up to 2%. The resulting change of tetragonality reaches a maximum after 1.3 ps. As a result, the ferroelectric polarization P is reduced by up to 100% with a slight delay that is due to the anharmonic coupling of the two modes.

Femtosecond photoexcitation of organic chromophores in a molecular crystal induces strong changes of the electronic dipole moment via intramolecular charge transfer as is evident from transient vibrational spectra. The structural response of the crystal to the dipole change is mapped directly for the first time by ultrafast x-ray diffraction or diffuse scattering. Changes of diffracted and transmitted x-ray intensity demonstrate an angular rearrangement of molecules around excited dipoles following the 10 ps kinetics of charge transfer and leaving lattice plane spacings unchanged. Transient x-ray scattering is governed by solvation, masking changes of the chromophore molecular structure.

Excitation of an n-type GaAs layer by intense ultrashort terahertz pulses causes coherent emission at 2 THz. Phase-resolved nonlinear propagation experiments show a picosecond decay of the emitted field, despite the ultrafast carrier-carrier scattering at a sample temperature of 300 K. While the linear THz response is in agreement with the Drude response of free electrons, the nonlinear response is dominated by the super-radiant decay of optically inverted impurity transitions. A quantum mechanical discrete state model using the potential of the disordered impurities accounts for all experimental observations.

We present the first evidence for a distinct optical phonon progression in the linear and nonlinear intersubband absorption spectra of electrons in a GaN/Al(0.8)Ga(0.2)N heterostructure. Femtosecond two-color pump-probe experiments in the midinfrared reveal spectral holes on different vibronic transitions separated by the LO-phonon frequency. These features wash out with a decay time of 80 fs due to spectral diffusion. The remaining nonlinear transmission changes decay with a time constant of 380 fs. All results observed are described by the independent boson model.

Strong electric-field transients resonant to intersubband transitions in n-type modulation-doped GaAs/AlGaAs quantum wells induce coherent Rabi oscillations, which are demonstrated by a phase-resolved measurement of the light emitted by the sample. The time evolution of the intersubband polarization is influenced by Coulomb-mediated many-body effects. The subpicosecond period and the phase of the Rabi oscillations are controlled by the properties of the midinfrared driving pulse.

Coherent electron transport is studied in an electrically driven quantum cascade structure. Ultrafast quantum transport from the injector into the upper laser state is investigated by midinfrared pump-probe experiments directly monitoring the femtosecond saturation and subsequent recovery of electrically induced optical gain. We demonstrate for the first time pronounced gain oscillations giving evidence for a coherent electron motion. The coexistence of a long dephasing time of quantum coherence and high Coulomb scattering rates in the injector points to the occurrence of scattering-induced coherence in electron transport.

We present the first study of ultrafast hole dynamics after resonant intersubband excitation in a quasi-two-dimensional semiconductor. p-type Si0.5Ge 0.5/Si multiple quantum wells are studied in pump-probe experiments with 150 fs midinfrared pulses. Intersubband scattering from the second heavy-hole back to the first heavy-hole subband occurs with a time constant of 250 fs, followed by intrasubband carrier heating within 1 ps. Such processes give rise to a strong reshaping of the intersubband absorption line, which is accounted for by calculations of the subband structure, optical spectra, and hole-phonon scattering rates.