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The downscaling of nonlinear optical devices is significantly hindered by the inherently weak nonlinearity in regular materials. Here, we report a giant third-harmonic generation discovered in epitaxial thin films of V-VI chalcogenide topological insulators. Using a tailored substrate and capping layer, a single reflection from a 13 nm film can produce a nonlinear conversion efficiency of nearly 0.01%, a performance that rivals micron-scale waveguides made from conventional materials or metasurfaces with far more complex structures. Such strong nonlinear optical emission, absent from the topologically trivial member in the same compound family, is found to be generated by the same bulk band characteristics that are responsible for producing the band inversion and the nontrivial topological ordering. This finding reveals the possibility of obtaining superior optical nonlinearity by examining the large pool of newly discovered topological materials with similar band characteristics.

Delafossites are promising candidates for photocatalysis applications because of their chemical stability and absorption in the solar region of the electromagnetic spectrum. For example, CuAlO2 has...

Solar-driven production of renewable energy (e.g., H2) has been investigated for decades. To date, the applications are limited by low efficiency due to rapid charge recombination (both radiative and nonradiative modes) and slow reaction rates. Tremendous efforts have been focused on reducing the radiative recombination and enhancing the interfacial charge transfer by engineering the geometric and electronic structure of the photocatalysts. However, fine-tuning of nonradiative recombination processes and optimization of target reaction paths still lack effective control. Here we show that minimizing the nonradiative relaxation and the adsorption energy of photogenerated surface-adsorbed hydrogen atoms are essential to achieve a longer lifetime of the charge carriers and a faster reaction rate, respectively. Such control results in a 16-fold enhancement in photocatalytic H2 evolution and a 15-fold increase in photocurrent of the crystalline g-C3N4 compared to that of the amorphous g-C3N4.

As optical two-dimensional coherent spectroscopy (2DCS) is extended to a broader range of applications, it is critical to improve the detection sensitivity of optical 2DCS. We developed a fast phase-cycling scheme in a non-collinear optical 2DCS implementation by using liquid crystal phase retarders to modulate the phases of two excitation pulses. The background in the signal can be eliminated by combining either two or four interferograms measured with a proper phase configuration. The effectiveness of this method was validated in optical 2DCS measurements of an atomic vapor. This fast phase-cycling scheme will enable optical 2DCS in novel emerging applications that require enhanced detection sensitivity., 4 pages, 3 figures, 1 table

La0.7Sr0.3MnO3 is a strongly correlated complex oxide. There is limited information about La0.7Sr0.3MnO3 thin films’ transient reflectivity (TR), where differences in ultra-fast dynamics due to surface and interface effects are expected. By decreasing the film thickness, additional energy states emerge, providing extra relaxation channels. Due to the reduced absorption in thin films, observing the effects of these extra states in TR signal is challenging, especially in a hole doped system such as La0.7Sr0.3MnO3. Moreover, in lower thicknesses, sinusoidal behavior superimposed on the TR signal is not analyzable by Fourier transforms. Wavelet transforms are perfect tools to analyze these fast-vanishing oscillations.

Multidimensional coherent spectra are presented for exciton-polaritons in a semiconductor microcavity at cryogenic temperatures as a function of mixing time. A decrease in vacuum Rabi splitting is observed along with spectral phase shifts.

We demonstrate temperature-dependent refraction, absorption, electron-phonon coupling, AC conductivity and mobility in bulk chalcopyrite semiconductors using THz-TDs. The measured optical and electronic properties are significantly influenced by temperature that affects the underlying carrier scattering mechanism.

We apply Linear Prediction from Singular Value Decomposition (LPSVD) to two-dimensional complex optical data in the time-domain to generate spectra with advantages over discrete Fourier transformation (DFT). LPSVD is a non-iterative procedure that fits time-domain complex data to the sum of damped sinusoids, or Lorentzian peaks in the spectral domain. Because the fitting is linear, it is not necessary to give initial guess parameters as in nonlinear fits. Although LPSVD is a one-dimensional algorithm, it can be performed column-wise on two-dimensional data. The method has been extensively used in 2D NMR spectroscopy, where spectral peaks are typically nearly ideal Lorentzians, but to our knowledge has not been applied in the analogous optical technique, where peaks can be far from Lorentzian. We apply LPSVD to the analysis of zero, one, and two quantum electronic two-dimensional spectra from a semiconductor microcavity. The spectra consist of non-ideal, often overlapping peaks. We find that LPSVD achieves a very good fit even on non-ideal data. It reduces noise and eliminates discrete distortions inherent in the DFT. We also use it to isolate and analyze weak features of interest.

Transient reflectivity (TR) measurements for La0.7Sr0.3MnO3 thin films indicate enhanced surface recombination of charge carriers for thinner films (d < 20 nm). Wavelet analysis of residual TR shows abrupt oscillatory modes with close energy ranges.

Automated, polarization-controlled 2D coherent spectroscopy is shown based on liquid-crystal variable retarders. Polarization-dependent rephasing spectra are recorded in a single scan, with absolute phase determined by a single auxiliary measurement.

Hot electrons established by the absorption of high-energy photons typically thermalize on a picosecond time scale in a semiconductor, dissipating energy via various phonon-mediated relaxation pathways. Here it is shown that a strong hot carrier distribution can be produced using a type-II quantum well structure. In such systems it is shown that the dominant hot carrier thermalization process is limited by the radiative recombination lifetime of electrons with reduced wavefunction overlap with holes. It is proposed that the subsequent reabsorption of acoustic and optical phonons is facilitated by a mismatch in phonon dispersions at the InAs-AlAsSb interface and serves to further stabilize hot electrons in this system. This lengthens the time scale for thermalization to nanoseconds and results in a hot electron distribution with a temperature of 490 K for a quantum well structure under steady-state illumination at room temperature.

In Forster resonance energy transfer (FRET), energy non-radiatively transfers from a blue-shifted emitter to a red-shifted absorber by dipole–dipole coupling. This study shows that plasmonics enables the opposite transfer direction, transferring the plasmonic energy towards the short-wavelength direction to induce charge separation in a semiconductor. Plasmon-induced resonance energy transfer (PIRET) differs from FRET because of the lack of a Stoke's shift, non-local absorption effects and a strong dependence on the plasmon's dephasing rate and dipole moment. PIRET non-radiatively transfers energy through an insulating spacer layer, which prevents interfacial charge recombination losses and dephasing of the plasmon from hot-electron transfer. The distance dependence of dipole–dipole coupling is mapped out for a range of detuning across the plasmon resonance. PIRET can efficiently harvest visible and near-infrared sunlight with energy below the semiconductor band edge to help overcome the constraints of band-edge energetics for single semiconductors in photoelectrochemical cells, photocatalysts and photovoltaics. Plasmon-induced resonance energy transfer is revealed and explored for solar energy harvesting from visible and near-infrared light.

Plasmonic metals can excite charge carriers in semiconductors through plasmon-induced resonance energy transfer (PIRET) and hot electron injection processes. Transient absorption spectroscopy reveals that the presence of plasmon-induced charge separation mechanisms in metal@TiO2 core–shell nanoparticles can be controlled by tailoring the spectral overlap and the physical contact between the metal and the semiconductor. In Ag@SiO2@TiO2 sandwich nanoparticles, the localized surface plasmon resonance band is overlapped with the absorption band edge of TiO2, enabling PIRET, while the SiO2 barrier prevents hot electron transfer. In Au@TiO2, hot electron injection occurs, but the lack of spectral overlap disables PIRET. In Ag@TiO2, both hot electron transfer and PIRET take place. In Au@SiO2@TiO2, photoconversion in TiO2 is not enhanced by the plasmon despite strong light absorption by Au.

Doping a semiconductor can extend the light absorption range, however, it usually introduces mid-gap states, reducing the charge carrier lifetime. This report shows that doping lanthanum dititinate (La2Ti2O7) with nitrogen extends the valence band edge by creating a continuum of dopant states, increasing the light absorption edge from 380 nm to 550 nm without adding mid-gap states. The dopant states are experimentally resolved in the excited state by correlating transient absorption spectroscopy with a supercontinuum probe and DFT prediction. The lack of mid-gap states is further confirmed by measuring the excited state lifetimes, which reveal the shifted band edge only increased carrier thermalization rates to the band edge and not interband charge recombination under both ultraviolet and visible excitation. Terahertz (time-domain) spectroscopy also reveals that the conduction mechanism remains unchanged after doping, suggesting the states are delocalized.

This paper presents a sandwich-structured CdS-Au-TiO2 nanorod array as the photoanode in a photoelectrochemical cell (PEC) for hydrogen generation via splitting water. The gold nanoparticles sandwiched between the TiO2 nanorod and the CdS quantum dot (QD) layer play a dual role in enhancing the solar-to-chemical energy conversion efficiency. First, the Au nanoparticles serve as an electron relay, which facilitates the charge transfer between CdS and TiO2 when the CdS QDs are photoexcited by wavelengths shorter than 525 nm. Second, the Au nanoparticles act as a plasmonic photosensitizer, which enables the solar-to-hydrogen conversion at wavelengths longer than the band edge of CdS, extending the photoconversion wavelength from 525 to 725 nm. The dual role of Au leads to a photocurrent of 4.07 mA/cm(2) at 0 V (vs Ag|AgCl) under full solar spectrum irradiation and a maximum solar-to-chemical energy conversion efficiency of 2.8%. An inversion analysis is applied to the transient absorption spectroscopy data, tracking the transfer of electrons and holes in the heterostructure, relating the relaxation dynamics to the underlying coupled rate equation and revealing that trap-state Auger recombination is a dominant factor in interfacial charge transfer. It is found that addition of Au nanoparticles increases the charge-transfer lifetime, reduces the trap-state Auger rate, suppresses the long-time scale back transfer, and partially compensates the negative effects of the surface trap states. Finally, the plasmonic energy-transfer mechanism is identified as direct transfer of the plasmonic hot carriers, and the interfacial Schottky barrier height is shown to modulate the plasmonic hot electron transfer and back transfer. Transient absorption characterization of the charge transfer shows defect states cannot be ignored when designing QD-sensitized solar cells. This facile sandwich structure combines both the electrical and the optical functions of Au nanoparticles into a single structure, which has implications for the design of efficient solar-energy-harvesting devices.

Optical injection and detection of charge currents is an alternative to conventional transport and photoemission measurements, avoiding the necessity of invasive contact that may disturb the system being examined. This is a particular concern for analyzing the surface states of topological insulators. In this work one- and two-color sources of photocurrents are isolated and examined in epitaxial thin films of Bisub2/subSesub3/sub. We demonstrate that optical excitation and terahertz detection simultaneously captures one- and two-color photocurrent contributions, which has not been required for other material systems. A method is devised to extract the two components, and in doing so each can be related to surface or bulk excitations through symmetry. The separation of such photocurrents in topological insulators opens a new avenue for studying these materials by all-optical methods.

An experimental apparatus is described for multidimensional optical spectroscopy with fully automated polarization control, based on liquid crystal variable retarders. Polarization dependence of rephasing two-dimensional coherent spectra are measured in a single scan, with absolute phasing performed for all polarization configurations through a single automated auxiliary measurement at the beginning of the scan. A factor of three improvement in acquisition time is demonstrated, compared to the apparatus without automated polarization control. Results are presented for a GaAs quantum well sample and an InGaAs quantum well embedded in a microcavity.

Optical rectification of near-infrared laser pulses generates broadband terahertz radiation in chalcopyrite crystals CdGeP2, ZnGeP2 and CdSiP2. The emission is characterized using linear-polarized excitation from 0.8 eV to 1.55 eV (1550 nm – 800 nm). All three crystals are (110)-cut and polished to 0.5 mm, thinner than the coherence length across most of the excitation photon energy range, such that they all produce a bandwidth ~2.5 THz when excited with ~100 fs pulses. It is found that CdGeP2 produced the strongest emission at telecoms wavelengths, while CdSiP2 is generally the strongest source. Pump-intensity dependence provides the nonlinear coefficients for each crystal.

Applications of wavelet analysis in ultra-thin film transient reflectivity (TR) measurements have been investigated. Advantages of utilizing different localized wavelet bases, in position and time, have been addressed on the residual TR signals. Morse wavelets have been used to obtain information from the abrupt oscillatory modes in the signal, which are not distinguishable with conventional methods such as Fourier transforms. These abrupt oscillatory modes are caused by the surface, interface, or any short-lived oscillatory modes which are suppressed in the TR signal in ultra-thin films. It is demonstrated that by choosing different Morse wavelets, information regarding different oscillatory modes in the TR signal of a heterostructure thin film is achievable. Moreover, by performing wavelet analysis on multiferroic heterostructures, oscillatory modes with very close energy ranges are easily distinguishable. For illustration, residuals of the TR signals have been obtained by a pump-probe setup in reflectivity mode on La0.7Sr0.3MnO3/SrTiO3 and BaTiO3/La0.7Sr0.3MnO3/SrTiO3 samples, where sufficient signal to noise ratios have been achieved by taking multiple scans. The residual signals have been analyzed with Morse wavelets, and multiple oscillatory modes with close energy ranges have been observed and distinguished. This approach can isolate the location of various oscillatory modes at the surface, interface and in the bulk of the heterostructure sample.

Compared to pristine Cu2O nanoparticles (NPs), Ag@Cu2O core-shell NPs exhibit photocatalytic activity over an extended wavelength range because of the presence of localized surface plasmon resonance (LSPR) in the Ag core. The photocatalysis action spectra and transient absorption measurements show that the plasmonic energy is transferred from the metal to the semiconductor via plasmon-induced resonant energy transfer (PIRET) and direct electron transfer (DET) simultaneously, generating electron–hole pairs in the semiconductor. The LSPR band of Ag@Cu2O core-shell NPs shows a red-shift with an increase in the Cu2O shell thickness, extending the light absorption of Ag@Cu2O heterostructures to longer wavelengths. As a result, the photocatalytic activity of the Ag@Cu2O core-shell NPs is varied by modulation of the shell thickness on the nanometer scale. This work has demonstrated that the Ag@Cu2O core-shell heterostructure is an efficient visible-light plasmonic photocatalyst, which allows for tunable light ab...

Optical 2-D Fourier transform spectroscopy is a powerful technique for studying resonant light-matter interactions, determining the transition structure and monitoring dynamics of optically created excitations. The ability to separate homogeneous and inhomogeneous broadening is one important capability. In this paper, we discuss the use of this technique to study excitonic transitions in semiconductor nanostructures. In quantum wells, the effects of structural disorder is observed as inhomogeneous broadening of the exciton resonances. In quantum dots, the temperature dependence of the homogeneous width gives insight into the nature of the dephasing processes.

While two-photon emission processes are firmly established in atomic physics, their observation and use in semiconductor physics remains elusive. Here, we experimentally investigate stimulated two-photon emission in photoexcited bulk CdSe and identify requirements for the observation of stimulated two-photon emission. In particular, this process requires population inversion as well as two-photon transition energies close to the bandgap energy. In any regime investigated in the present study, net optical gain is not achieved, as the free-carrier absorption intrinsically linked to the photoexcitation completely masks the two-photon gain. The results are well in line with a recent study on nondegenerate versions of two-photon emission in GaAs and place clear limits for the practical use of two-photon emission in optically excited semiconductors.

Coherent light-matter interactions of direct-gap semiconductor nanostructures provide a great test system for fundamental research into quantum electronics and many-body physics. The understanding gained from studying these interactions can facilitate the design of optoelectronic devices. Recently, we have used optical two-dimensional Fourier-transform spectroscopy to explore coherent light-matter interactions in semiconductor quantum wells. Using three laser pulses to generate a four-wave-mixing signal, we acquire spectra by tracking the phase of the signal with respect to two time axes and then Fourier transforming them. In this Account, we show several two-dimensional projections and demonstrate techniques to isolate different contributions to the coherent response of semiconductors. The low-temperature spectrum of semiconductor quantum wells is dominated by excitons, which are electron-hole pairs bound through Coulombic interactions. Excitons are sensitive to their electronic and structural environment, which influences their optical resonance energies and line widths. In near perfect quantum wells, a small fluctuation of the quantum well thickness leads to spatial localization of the center-of-mass wave function of the excitons and inhomogeneous broadening of the optical resonance. The inhomogeneous broadening often masks the homogeneous line widths associated with the scattering of the excitons. In addition to forming excitons, Coulombic correlations also form excitonic molecules, called biexcitons. Therefore, the coherent response of the quantum wells encompasses the intra-action and interaction of both excitons and biexcitons in the presence of inhomogeneous broadening. Transient four-wave-mixing studies combined with microscopic theories have determined that many-body interactions dominate the strong coherent response from quantum wells. Although the numerous competing interactions cannot be easily separated in either the spectral or temporal domains, they can be separated using two-dimensional Fourier transform spectroscopy. The most common two-dimensional Fourier spectra are S(I)(omega(tau),T,omega(t)) in which the second time period is held fixed. The result is a spectrum that unfolds congested one-dimensional spectra, separates excitonic pathways, and shows which excitons are coherently coupled. This method also separates the biexciton contributions and isolates the homogeneous and inhomogeneous line widths. For semiconductor excitons, the line shape in the real part of the spectrum is sensitive to the many-body interactions, which we can suppress by exploiting polarization selection rules. In an alternative two-dimensional projection, S(I)(tau,omega(Tau),omega(t)), the nonradiative Raman coherent interactions are isolated. Finally, we show S(III)(tau,omega(Tau),omega(t)) spectra that isolate the two-quantum coherences associated with the biexciton. These spectra reveal previously unobserved many-body correlations.

Silicon has been the dominant material in electronics since the invention of the integrated transistor. In contrast, silicon’s indirect bandgap and vanishing second-order optical nonlinearity limit its applications in optoelectronics1. Although all-optical components such as Raman lasers2, parametric amplifiers3 and electro-optic modulators4,5 have recently been reported, control over charge motion in silicon has only ever been achieved electronically. Here, we report all-optical generation of ultrafast ballistic electrical currents in clean, unbiased, bulk silicon at room temperature. This current injection, which provides new insights into optical processes in silicon, results from quantum interference between one- and two-photon absorption pathways across the indirect bandgap despite phonon participation and the multi-valley conduction band. The transient currents induced by 150 fs pulses are detected via the emitted THz radiation. The efficiency of this third-order optical process is surprisingly large for fundamental wavelengths in the 1,420–1,800 nm range.

Plasmonics can enhance solar energy conversion in semiconductors by light trapping, hot electron transfer, and plasmon-induced resonance energy transfer (PIRET). The multifaceted response of the plasmon and multiple interaction pathways with the semiconductor makes optimization challenging, hindering design of efficient plasmonic architectures. Therefore, in this paper we use a density matrix model to capture the interplay between scattering, hot electrons, and dipole–dipole coupling through the plasmon's dephasing, including both the coherent and incoherent dynamics necessary for interactions on the plasmon's timescale. The model is extended to Shockley–Queisser limit calculations for both photovoltaics and solar-to-chemical conversion, revealing the optimal application of each enhancement mechanism based on plasmon energy, semiconductor energy, and plasmon dephasing. The results guide application of plasmonic solar-energy harvesting, showing which enhancement mechanism is most appropriate for a given semiconductor's weakness, and what nanostructures can achieve the maximum enhancement.

Efficient solar energy conversion in photovoltaics and solar to chemical conversion is hindered by large band gaps and poor absorption in thin films. The easily tunable absorption and scattering cross section of localized surface plasmon resonance (LSPR) make it an ideal solution to capturing lost light. For above band edge light, scattering and light trapping can be used to increase absorption in thin semiconductor films, improving photoconversion without sacrificing recombination times. Below the band edge, plasmonic hot electrons can transfer to the semiconductor directly or resonant energy transfer can non-radiatively induce charge separation, allowing photoconversion where the semiconductor cannot absorb. In this brief review, we explore the mechanisms and efficiency of light recovery in plasmonics. Surface plasmon polaritons are used to increase light trapping in semiconductor nanowires using a metal nanohole array. Metal-semiconductor nanostructures with varying energy alignment, insulating barrier thickness, and spectral overlap are systematically varied to differentiate hot electron and resonant energy transfer. Transient absorption spectroscopy and action spectrum analysis are applied to track plasmonic charge creation and transfer, linking short and long time scale behavior. Guidelines are given for achieving optimal plasmonic light capturing and enhancement across the solar spectrum.

Epitaxial NbO2 (110) films, 20 nm thick, were grown by pulsed laser deposition on Al2O3 (0001) substrates. The Ar/O2 total pressure during growth was varied to demonstrate the gradual transformation between NbO2 and Nb2O5 phases, which was verified using x-ray diffraction, x-ray photoelectron spectroscopy, and optical absorption measurements. Electric resistance threshold switching characteristics were studied in a lateral geometry using interdigitated Pt top electrodes in order to preserve the epitaxial crystalline quality of the films. Volatile and reversible transitions between high and low resistance states were observed in epitaxial NbO2 films, while irreversible transitions were found in case of Nb2O5 phase. Electric field pulsed current measurements confirmed thermally-induced threshold switching., Comment: This is an author-created, un-copyedited version of an article accepted for publication in Journal of Physics D: Applied Physics. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at http://dx.doi.org/10.1088/0022-3727/48/33/335308

A one-dimensional photonic crystal is patterned into an active planar waveguide containing multiple InGaAs quantum wells. External coupling reflectivity is used to map out the photonic band structure, revealing a clear anti-crossing at ~1.37 eV in the 45° TM polarized spectrum. The band structure is compared to and confirmed by scattering-matrix calculations. Photoluminescence measurements are performed in the same geometry on the patterned and unpatterned regions of the sample. The latter shows conventional quantum-well emission and GaAs emission with increasing pump power. In contrast, the spectra from the patterned sample contain a sharp mode from the dielectric-like band of the anti-crossing, corresponding to the Brillouin zone edge. Power-dependent excitation shows this mode to be strongly super-linear, indicative of band edge lasing.

We have studied the power-dependent wavelength shift of photonic coupling resonances of a two-dimensional photonic crystal waveguide by reflection geometry pump-probe measurements. The quadratic response is indicative of two-photon induced carrier creation, which alters the refractive index of the semiconductor core of the photonic lattice. A free-carrier model is used to simulate the phenomenon, giving values of the change in refractive index per unit carrier density that satisfactorily compare to values calculated for bulk AlGaAs under similar conditions. Time-resolved spectra are also presented, showing relaxation times of

Strong resonant polarization conversion is observed in the reflectivity properties of one-dimensional (1-D) lattices of air trenches deeply etched in AlGaAs surface waveguides. The symmetry properties and the magnitudes of the observed effects are found to be in good agreement with the results of scattering matrix calculations.

We present compelling experimental results of the optical characteristics of transparent oxide CuGaO2 and related CuGa1-xFexO2 (with 0.00≤x≤0.05) alloys, whereby the forbidden electronic transitions for CuGaO2 become permissible in the presence of B-site (Ga sites) alloying with Fe. Our computational structural results imply a correlation between the global strain on the system and a decreased optical absorption edge. However, herein, we show that the relatively ordered CuGa1-xFexO2 (for 0.00≤x≤0.04) structures exhibit much weaker vis-absorption compared to the relatively disordered CuGa0.95Fe0.05O2.

The absorption of phase-related near-infrared fundamental (ω) and second harmonic (2ω) femtosecond pulses results in ballistic electrical currents in clean bulk silicon at room temperature. The ultrafast charge motion is directly monitored via a time-resolved analysis of the emitted THz bursts of radiation. The vector direction of the current is precisely controlled by the polarization of the two-color pump field and the relative phase ΔΦ = 2Φω – Φ2ω. The current generation process relies on a third order optical nonlinearity. Microscopically, current injection can be understood as arising from the quantum interference of one- and two-photon absorption processes. Surprisingly, the efficiency of the current injection is relatively high despite the multitude of possible phonon-assisted absorption channels in the multi-valley band structure. (© 2008 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

Monolayer fluctuations in the thickness of a semiconductor quantum well (QW) lead to the formation of spectrally resolved excitons located in the narrower, average, and thicker regions of the QW. Whether or not these excitons are coherently coupled via Coulomb interaction is a long-standing debate. We demonstrate that different types of disorder potential govern coherent coupling among excitons, and the coupling strength can be quantitatively measured using optical two-dimensional Fourier transform spectroscopy. Strong coherent coupling occurs between certain types of excitons but is missing between other types of excitons because the distinctive nature of excitons results in different spatial overlap. Our finding may be applicable to other disordered systems, such as photosynthesis and conjugated polymers, where exciton coupling plays a critical role in determining charge and energy transfer.

Collinear phase-matched optical rectification is studied in ZnGeP$_{2}$ pumped with near-infrared light. The pump-intensity dependence is presented for three crystal lengths (0.3, 1.0 and 3.0 mm) to determine the effects of linear optical absorption, nonlinear optical absorption and terahertz free-carrier absorption on the generation. Critical parameters such as the coherence length (for velocity matching), dispersion length (for linear pulse broadening) and nonlinear length (for self-phase modulation) are determined for this material. These parameters provide insight into the upper limit of pulse intensity and crystal length required to generate intense terahertz pulse without detriment to the pulse shape. It is found that for 1-mm thick ZnGeP$_{2}$(012), pumped at 1.28 micron with intensity of ~15 GW/cm2 will produce intense undistorted pulses, whereas longer crystals or larger intensities modify the pulse shape to varying degrees. Moreover, phase-matching dispersion maps are presented for the terahertz generation over a large tuning range (1.1-2.4 micron) in longer (3 mm) crystal, demonstrating the phase-matching bandwidth and phase mismatch that leads to fringing associated with multi-pulse interference. All observed results are simulated numerically showing good qualitative agreement., Comment: 7 pages, 4 figures, journal submission, version 2

We have used femtosecond pump-probe spectroscopy to study the ultrafast nonlinear response of AlGaAs two-dimensional photonic crystal waveguides in the near-infrared spectral region. The modulation of the reflectivity spectra due to the refractive index change produced by photogenerated carriers was measured. We observed an instantaneous pump-induced shift in the wavelength of a photonic resonance at 882 nm with a fast decay time of ≈8 ps. The magnitude of the reflectivity change was very large at wavelengths close to the photonic resonance, with a maximum value of ΔR/R>30% at 877 nm. These results confirm the excellent potential of photonic crystal waveguides in ultrafast nonlinear switching applications.

Plasmonic metal nanostructures have been incorporated into semiconductors to enhance the solar-light harvesting and the energy-conversion efficiency. So far the mechanism of energy transfer from the plasmonic metal to semiconductors remains unclear. Herein the underlying plasmonic energy-transfer mechanism is unambiguously determined in Au@SiO(2)@Cu(2)O sandwich nanostructures by transient-absorption and photocatalysis action spectrum measurement. The gold core converts the energy of incident photons into localized surface plasmon resonance oscillations and transfers the plasmonic energy to the Cu(2)O semiconductor shell via resonant energy transfer (RET). RET generates electron-hole pairs in the semiconductor by the dipole-dipole interaction between the plasmonic metal (donor) and semiconductor (acceptor), which greatly enhances the visible-light photocatalytic activity as compared to the semiconductor alone. RET from a plasmonic metal to a semiconductor is a viable and efficient mechanism that can be used to guide the design of photocatalysts, photovoltaics, and other optoelectronic devices.

Generation of terahertz pulses by optical rectification is demonstrated in chalcopyrite ZnGeP 2 (ZGP) as a function of pump intensity, wavelength and crystal orientation. For infrared excitation, ZGP emission exceeds that of GaAs and GaP.

Optical rectification is demonstrated in (110)-cut ZnGeP_2 (ZGP) providing broadband terahertz (THz) generation. The source is compared to both GaP and GaAs over a wavelength range of 1150 nm to 1600 nm and peak intensity range of 0.5 GW/cm^2 to 40 GW/cm^2. ZGP peak-to-peak field amplitude is larger than in the other materials due to either lower nonlinear absorption or larger second order nonlinearity. This material is well suited for broadband THz generation across a wide range of infrared excitation wavelengths., Comment: 4 pages, 3 figures, journal article

Optical multidimensional Fourier transform spectroscopy excites a sample with a sequence of ultrafast pulses. A spectrum is constructed by taking Fourier transforms with respect to pulse delays, which are interferometrically controlled.

Optical two-dimensional Fourier-transformed (2DFT) spectroscopy is used to study the coherent optical response of potassium vapor in a thin transmission cell. Rephasing and non-rephasing spectra of the D1 and D2 transitions are obtained and compared to numerical simulations. Calculations using the optical Bloch equations gives very good agreement with the experimental peak strengths and line shapes. Non-radiative Raman-like coherences are isolated using a different 2DFT projection. Density-dependent measurements show distortion of 2DFT spectra due to pulse propagation effects.

Electronic structure and dynamics are captured by optical 2D-Fourier-transform (2DFT) spectroscopy, which tracks the phase of the nonlinear signal during two time delays of a multi-pulse excitation sequence. These Fourier-transformed spectra separate and isolate overlapping and competing contributions to the coherent response. We have developed an ultra-stable platform consisting of nested interferometers with active phase control, allowing for exploration of single- and two-quantum coherences. Phase-resolved spectra are retrieved by all-optical determination of experimental phase ambiguities. GaAs quantum wells show suppression of many-body interactions in cross-linear polarized 2DFT spectra and many-body two-quantum coherences. Potassium vapor also shows unexpected two-quantum coherences.

We demonstrate optical two-dimensional Fourier transform spectroscopy of heavy- and light-hole excitons in GaAs quantum wells. This is enabled by active interferometric stabilization of the excitation pulse separation and of a reference pulse.

We present optical two-dimensional Fourier transform spectra for the pulse sequence sensitive to two-quantum coherences. In semiconductors, two-quantum coherences occur due to biexcitons and many-body effects, in a potassium vapor, they arise from atomic interactions.

Two-quantum coherences in two-dimensional Fourier-transform (2DFT) spectra are attributed to many-body interactions. 2DFT spectroscopy allows two-quantum coherences in semiconductors to be isolated. As a result, many-body coherences can be separated from bound biexciton coherences.

Optical two-dimensional Fourier transform spectroscopy is used to study excitonic resonances in semiconductor nanostructures. The spectra show the dominance of many-body contributions. Two-quantum coherences are observed due to both biexcitons and many-body states.

We present the experimental and simulation results of two-dimensional optical coherent correlation spectroscopy signals along the phase-matching direction k(I) = -k(1) + k(2) + k(3) projected on the two-dimensional (2D) (Omega(3),Omega(2)) plane corresponding to the second and third delay periods. Overlapping Raman coherences in the conventional (Omega(3),Omega(1)) 2D projection may now be clearly resolved. The linewidths of the heavy-hole (HH) and light-hole (LH) excitonic Raman coherence peaks are obtained. Further insights on the higher-order (beyond time-dependent Hartree-Fock) correlation effects among mixed (HH and LH) two excitons can be gained by using a cocircular pulse polarization configuration.

Quantum interference between single and two photon inter-band absorption processes can lead to injection of electrical currents in direct and indirect band gap semiconductors. When the optical excitation occurs through 100 fs optical pulses the transient electrical currents emit THz radiation that can be used as a probe of the ultrafast current dynamics.

We study the coherent light-matter interactions of GaAs quantum wells associated with excitons, biexcitons and many-body effects. For most polarization configurations, excitonic features dominate the phase-resolved two-dimensional Fourier-transform (2DFT) spectra and have dispersive lineshapes, indicating the presence of many-body interactions. For cross-linear excitation, excitonic features become weak and absorptive due to the strong suppression of many-body effects; a result that can not be directly determined in transient four-wave mixing experiments. The biexcitonic features do not weaken for cross-polarized excitation and thus are more important., Comment: 4 page, 3 figures, journal article - rapid communication