Effects of coherent polarization interactions on time-resolved degenerate four-wave mixing

Leo, K.; Wegener, Martin; Shah, Jagdeep; Chemla, Denis; Eo, Göbel; Tc, Damen; Schmitt‐Rink, S.; Schäfer, W.

doi:10.1103/physrevlett.65.1340

Cited by 279 publications

(122 citation statements)

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“…The first and most prominent was a signal for the ''wrong'' time delay in a two-pulse TFWM experiment. Theoretically, such signals could arise from several effects including local fields (3,4), biexcitons (5), excitation-induced dephasing (6, 7), or excitation-induced shift (8). Time resolving the signal also provided evidence for many-body contributions (9,10), although it did not resolve the ambiguity regarding the underlying phenomena.…”

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confidence: 99%

Polarization-dependent optical 2D Fourier transform spectroscopy of semiconductors

Zhang

Кузнецова

Meier

et al. 2007

Proc. Natl. Acad. Sci. U.S.A.

118

113

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Optical 2D Fourier transform spectroscopy (2DFTS) provides insight into the many-body interactions in direct gap semiconductors by separating the contributions to the coherent nonlinear optical response. We demonstrate these features of optical 2DFTS by studying the heavy-hole and light-hole excitonic resonances in a gallium arsenide quantum well at low temperature. Varying the polarization of the incident beams exploits selection rules to achieve further separation. Calculations using a full many-body theory agree well with experimental results and unambiguously demonstrate the dominance of many-body physics.excitons ͉ many-body effects ͉ ultrafast O ptical excitation of a direct gap semiconductor, such as gallium arsenide (GaAs), produces electron-hole pairs. The Coulomb attraction between the electron and hole can result in a bound state, known as an exciton, with a hydrogenic wavefunction for the relative coordinate. Excitons have a large oscillator strength because of the proximity of the electron and hole and thus can dominate the absorption spectrum close to the fundamental band gap. In GaAs heterostructures, the exciton binding energy is of order 10 meV; thus, excitonic resonances appear only at low temperatures. Excitons and unbound electron-hole pairs exhibit dynamics on a femtosecond-to-picosecond time scale. These timescales, combined with the strong interaction with light, make ultrafast spectroscopy an ideal tool for studying carrier dynamics in semiconductors.Over the last two decades, excitonic resonances in semiconductors have been studied extensively by using ultrafast spectroscopy, primarily transient four-wave-mixing (TFWM) (1, 2). The measurements clearly showed signatures of many-body effects. The first and most prominent was a signal for the ''wrong'' time delay in a two-pulse TFWM experiment. Theoretically, such signals could arise from several effects including local fields (3, 4), biexcitons (5), excitation-induced dephasing (6, 7), or excitation-induced shift (8). Time resolving the signal also provided evidence for many-body contributions (9, 10), although it did not resolve the ambiguity regarding the underlying phenomena.Recent results using optical 2D Fourier transform spectroscopy (2DFTS) to study the exciton resonances have shown that much more information is obtained, promising a more stringent test of the theory (11). 2DFTS traces its roots to NMR (12). Recently, there has been significant progress in translating multidimensional NMR techniques into the infrared and optical domains for the study of vibrations (13) and electronic excitations (14-16) in molecules. Although the usefulness of adding a second dimension was recognized in TWFM studies of semiconductors (17-20), only the intensity of the emitted signal, not the phase-resolved electric field, was measured. The transient absorption experiments clearly show that detecting only the real part of the emitted field is advantageous (21, 22), but the effects of inhomogeneous broadening cannot be removed. 2DFTS combines the best...

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confidence: 99%

Polarization-dependent optical 2D Fourier transform spectroscopy of semiconductors

Zhang

Кузнецова

Meier

et al. 2007

Proc. Natl. Acad. Sci. U.S.A.

118

113

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“…Phase-coherent nonlinear spectroscopic measurements such as four-wave-mixing are sensitive to the changes that occur when excitons interact through Coulomb forces [5] or local fields [6]. Early nonlinear 'self-diffraction' measurements revealed a signal at 'negative' delays due to many-body interactions (MBIs) [6][7][8], but since the exciton coherence frequencies could not be correlated with the emitted coherence frequencies, the contributions due to MBIs such as excitationinduced dephasing (EID) [9], excitation-induced energy shift (EIS) [10], and local field effects (LFEs) [6] could not be distinguished. EID and EIS result in density-dependent collisional broadening and renormalization of the exciton energy, respectively.…”

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confidence: 99%

Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy

et al. 2011

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We use fifth-order two-dimensional electronic spectroscopy to measure coherent four-particle dynamics in a semiconductor nanostructure. By using optical polarization control in two-quantum measurements enabled by the COLBERT spectrometer, we separate coherent signals due to bound biexcitons and unbound two-exciton correlations. The rephasing nature of the measurement allows us to separate homogeneous from inhomogeneous contributions to the two-quantum lineshapes. We find that, unlike the bound biexciton state, the energy of the unbound pair and its homogeneous linewidth depend on the laser fluence. Simulations using an extended phenomenological model help determine the primary interaction mechanism that leads to the formation of the unbound exciton pair; the model also indicates that seventh-order interactions contribute to the measured spectra under high pulse fluences.

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“…In conclusion we have demonstrated that our theoretical approach is able to describe the microscopic dynamics of laser-excited semiconductors quantitatively for all excitation densities at the (3) level. This is achieved by accounting on the same footing for two important effects: ͑i͒ scattering with free carriers as the most effective dephasing process and ͑ii͒ screening of the Coulomb interaction that controls correlation effects.…”

Section: Discussionmentioning

confidence: 98%

“…Indeed it is now possible to perform experiments with time resolution shorter than the scattering time scales of the fundamental elementary excitations and with interferometric control of the excitation density and energy. 1,2 However, most of the work, experimental or theoretical, concentrates on either one of two completely different experimental situations, involving, respectively, coherently driven states [3][4][5][6][7] or incoherently relaxing distributions. [8][9][10][11][12][13][14] In real life this distinction is artificial since an initially coherently driven system naturally relaxes and eventually reaches thermodynamic equilibrium.…”

Section: Introductionmentioning

confidence: 99%

“…9,[21][22][23] To obtain a thorough understanding of the evolution of e-h pair systems from initial coherently driven states to relaxed ones it is important to have at hand a theoretical description that can bridge the two cases. Recently progress in that direction has been made at the level of the lowest ( (3) ) nonlinearity. A many-particle theory has been developed, representing an approximation scheme that contains the NGF and the DCTS as limiting cases and provides a natural interpolation between these limits.…”

Section: →10mentioning

confidence: 99%

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Semiconductor polarization dynamics from the coherent to the incoherent regime: Theory and experiment

et al. 2002

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We explore the capability of a many-particle approach to the polarization dynamics of optically excited semiconductors. The theory contains the well-established theories for the coherent low excitation and incoherent high excitation regimes as limiting cases. The approach shows excellent agreement with four-wave mixing experiments where an incoherent background of carriers is created by a cw beam allowing to investigate the full range between the limiting cases.

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Effects of coherent polarization interactions on time-resolved degenerate four-wave mixing

Cited by 279 publications

References 12 publications

Polarization-dependent optical 2D Fourier transform spectroscopy of semiconductors

Polarization-dependent optical 2D Fourier transform spectroscopy of semiconductors

Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy

Semiconductor polarization dynamics from the coherent to the incoherent regime: Theory and experiment

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