Analysis of complex multidimensional optical spectra by linear prediction.

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.

Automated polarization-dependent multidimensional coherent spectroscopy phased using transient absorption.

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.

Application of wavelet analysis on transient reflectivity in ultra-thin films.

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.

Stimulated two-photon emission in bulk CdSe.

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.

Broadband terahertz pulse emission from ZnGeP2.

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.

A versatile ultrastable platform for optical multidimensional Fourier-transform spectroscopy.

The JILA multidimensional optical nonlinear spectrometer (JILA-MONSTR) is a robust, ultrastable platform consisting of nested and folded Michelson interferometers that can be actively phase stabilized. This platform generates a square of identical laser pulses that can be adjusted to have arbitrary time delay between them while maintaining phase stability. The JILA-MONSTR provides output pulses for nonlinear excitation of materials and phase-stabilized reference pulses for heterodyne detection of the induced signal. This arrangement is ideal for performing coherent optical experiments, such as multidimensional Fourier-transform spectroscopy, which records the phase of the nonlinear signal as a function of the time delay between several of the excitation pulses. The resulting multidimensional spectrum is obtained from a Fourier transform. This spectrum can resolve, separate, and isolate coherent contributions to the light-matter interactions associated with electronic excitation at optical frequencies. To show the versatility of the JILA-MONSTR, several demonstrations of two-dimensional Fourier-transform spectroscopy are presented, including an example of a phase-cycling scheme that reduces noise. Also shown is a spectrum that accesses two-quantum coherences, where all excitation pulses require phase locking for detection of the signal.

Enhanced all-optical tuning of leaky eigenmodes in photonic crystal waveguides.

We demonstrate all-optical switching in an active two-dimensional photonic crystal waveguide, observing as large as 16 nm blueshifts of a leaky eigenmode at 839 nm and switching ratios of almost 70%. These results are larger than those previously observed in similar experiments performed on passive photonic crystal waveguides; the enhancement is due to resonant photogeneration of carriers by In(0.12)Al(0.2)Ga(0.68)As quantum wells in the core of the waveguide. The effective change in the refractive index of the structure is approximately10(-2), with a rise time of approximately1 ps and a decay time of approximately10 ps, potentially allowing high-speed switching and fast modulation rates.