Polarization dependence of semiconductor exciton and biexciton contributions to phase-resolved optical two-dimensional Fourier-transform spectra

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 communicatio

All-optical retrieval of the global phase for two-dimensional Fourier-transform spectroscopy

A combination of spatial interference patterns and spectral interferometry are used to find the global phase for non-collinear two-dimensional Fourier-transform (2DFT) spectra. Results are compared with those using the spectrally resolved transient absorption (STRA) method to find the global phase when excitation is with co-linear polarization. Additionally cross-linear polarized 2DFT spectra are correctly phased using the all-optical technique, where the SRTA is not applicable.Comment: 6 pages, 7 figures, journal publicatio

Optical Detection of a Single Nuclear Spin

We propose a method to optically detect the spin state of a 31-P nucleus embedded in a 28-Si matrix. The nuclear-electron hyperfine splitting of the 31-P neutral-donor ground state can be resolved via a direct frequency discrimination measurement of the 31-P bound exciton photoluminescence using single photon detectors. The measurement time is expected to be shorter than the lifetime of the nuclear spin at 4 K and 10 T.Comment: 4 pages, 3 figure

Coherent two-dimensional Fourier transform spectroscopy using a 25 Tesla resistive magnet.

We performed nonlinear optical two-dimensional Fourier transform spectroscopy measurements using an optical resistive high-field magnet on GaAs quantum wells. Magnetic fields up to 25 T can be achieved using the split helix resistive magnet. Two-dimensional spectroscopy measurements based on the coherent four-wave mixing signal require phase stability. Therefore, these measurements are difficult to perform in environments prone to mechanical vibrations. Large resistive magnets use extensive quantities of cooling water, which causes mechanical vibrations, making two-dimensional Fourier transform spectroscopy very challenging. Here, we report on the strategies we used to overcome these challenges and maintain the required phase-stability throughout the measurement. A self-contained portable platform was used to set up the experiments within the time frame provided by a user facility. Furthermore, this platform was floated above the optical table in order to isolate it from vibrations originating from the resistive magnet. Finally, we present two-dimensional Fourier transform spectra obtained from GaAs quantum wells at magnetic fields up to 25 T and demonstrate the utility of this technique in providing important details, which are obscured in one dimensional spectroscopy

Electron-Phonon Interaction in Tetrahedral Semiconductors

Effects of electron-phonon interactions on the band structure can be experimentally investigated in detail by measuring the temperature dependence of energy gaps or critical points (van Hove singularities) of the optical excitation spectra. These studies have been complemented in recent years by observing the dependence of such spectra on isotopic mass whenever different stable isotopes of a given atom are available at affordable prices. In crystals composed of different atoms, the effect of the vibration of each separate atom can thus be investigated by isotopic substitution. Because of the zero-point vibrations, such effects are present even at zero temperature (T = 0). In this paper we discuss state-of-the-art calculations of the dielectric function spectra and compare them with experimental results, with emphasis on the differences introduced by the electron-phonon interaction. The temperature dependence of various optical parameters will be described by means of one or two (in a few cases three) Einstein oscillators, except at the lowest temperatures where the T4 law (contrary to the Varshini T2 result) will be shown to apply. Increasing an isotopic mass increases the energy gaps, except in the case of monovalent Cu (e.g., CuCl) and possibly Ag (e.g., AgGaS2). It will be shown that the gaps of tetrahedral materials containing an element of the first row of the periodic table (C,N,O) are strongly affected by the electron-phonon interaction. It will be conjectured that this effect is related to the superconductivity recently observed in heavily boron-doped carbon.Comment: 17 pages, 17 fifure

Electron-phonon renormalization of the absorption edge of the cuprous halides

Compared to most tetrahedral semiconductors, the temperature dependence of the absorption edges of the cuprous halides (CuCl, CuBr, CuI) is very small. CuCl and CuBr show a small increase of the gap $E_0$ with increasing temperature, with a change in the slope of $E_0$ vs. $T$ at around 150 K: above this temperature, the variation of $E_0$ with $T$ becomes even smaller. This unusual behavior has been clarified for CuCl by measurements of the low temperature gap vs. the isotopic masses of both constituents, yielding an anomalous negative shift with increasing copper mass. Here we report the isotope effects of Cu and Br on the gap of CuBr, and that of Cu on the gap of CuI. The measured isotope effects allow us to understand the corresponding temperature dependences, which we also report, to our knowledge for the first time, in the case of CuI. These results enable us to develop a more quantitative understanding of the phenomena mentioned for the three halides, and to interpret other anomalies reported for the temperature dependence of the absorption gap in copper and silver chalcogenides; similarities to the behavior observed for the copper chalcopyrites are also pointed out.Comment: 14 pages, 5 figures, submitted to Phys. Rev.

Probing Interband Coulomb Interactions in Semiconductor Nanocrystals with 2D Double-Quantum Coherence Spectroscopy

Using previously developed exciton scattering model accounting for the interband, i.e., exciton-biexciton, Coulomb interactions in semiconductor nanocrystals (NCs), we derive a closed set of equations for 2D double-quantum coherence signal. The signal depends on the Liouville space pathways which include both the interband scattering processes and the inter- and intraband optical transitions. These processes correspond to the formation of different cross-peaks in the 2D spectra. We further report on our numerical calculations of the 2D signal using reduced level scheme parameterized for PbSe NCs. Two different NC excitation regimes considered and unique spectroscopic features associated with the interband Coulomb interactions are identified.Comment: 11 pages, 5 figure