Probing many-body interactions in a disordered semiconductor quantum well with electronic two-dimensional Fourier transform spectroscopy

The interplay between disorder and Coulomb interactions ubiquitously affects the properties of condensed matter systems. We examine its role in the nonlinear optical response of semiconductor quantum wells. In particular, we investigate the coherent coupling strength between exciton resonances that are spectrally split by interface fluctuations. Previous studies yielded conflicting results. In light of rising interest in semiconductor devices that rely on spatial and/or temporal coherence, we revisit this problem by applying a newly developed spectroscopy method: electronic two-dimensional Fourier transform spectroscopy (2DFTS). 2DFTS is a powerful technique for revealing the presence of coupling and for distinguishing the (coherent or incoherent) nature of such coupling, especially in complex systems with several spectrally overlapping resonances. Even the most basic information about such complex systems, including the homogeneous and inhomogeneous linewidths of various resonances, cannot be extracted reliably using conventional spectroscopic tools. In these new 2DFTS measurements, we did not observe any clear cross peaks corresponding to coherent couplings between either heavy-hole or light-hole excitons. These measurements allow us to place a quantitative upper bound on the possible coupling strength in this prototypical system. A modified mean-field theory reveals a simple yet important relation that determines how the coherent coupling strength depends on the disorder correlation length and Coulomb interaction length.

[1]  Darius Abramavicius,et al.  Coherent Multidimensional Optical Spectroscopy of Excitons in Molecular Aggregates; Quasiparticle versus Supermolecule Perspectives , 2009 .

[2]  Alan D. Bristow,et al.  Polarization dependence of semiconductor exciton and biexciton contributions to phase-resolved optical two-dimensional Fourier-transform spectra , 2008, 0812.2914.

[3]  Thomas,et al.  Simultaneous influence of disorder and Coulomb interaction on photon echoes in semiconductors. , 1994, Physical review. B, Condensed matter.

[4]  M. Hofmann,et al.  COHERENT EXCITATION SPECTROSCOPY ON INHOMOGENEOUS EXCITON ENSEMBLES , 1999 .

[5]  Tianhao Zhang,et al.  Many-body interactions in semiconductors probed by optical two-dimensional fourier transform spectroscopy. , 2006, Physical review letters.

[6]  D. Jonas Two-dimensional femtosecond spectroscopy. , 2003, Annual review of physical chemistry.

[7]  R. Stephenson A and V , 1962, The British journal of ophthalmology.

[8]  Daniel B. Turner,et al.  Two-Quantum 2D FT Electronic Spectroscopy of Biexcitons in GaAs Quantum Wells , 2009, Science.

[9]  Jagdeep Shah,et al.  Many-body and correlation effects in semiconductors , 2001, Nature.

[10]  S. Mukamel,et al.  Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitations. , 2000, Annual review of physical chemistry.

[11]  W. Marsden I and J , 2012 .

[12]  Tianhao Zhang,et al.  Optical two-dimensional Fourier transform spectroscopy with active interferometric stabilization. , 2005, Optics express.

[13]  Manuel Joffre,et al.  Linear techniques of phase measurement by femtosecond spectral interferometry for applications in spectroscopy , 1995 .

[14]  Binder,et al.  Transient nonlinear optical response from excitation induced dephasing in GaAs. , 1993, Physical review letters.

[15]  Smith,et al.  Influence of exciton-exciton interactions on the coherent optical response in GaAs quantum wells. , 1993, Physical review. B, Condensed matter.

[16]  Temporally and spectrally resolved amplitude and phase of coherent four-wave-mixing emission from GaAs quantum wells , 1997 .

[17]  R. Hochstrasser,et al.  Two-dimensional spectroscopy at infrared and optical frequencies , 2007, Proceedings of the National Academy of Sciences.

[18]  D. Gammon,et al.  An All-Optical Quantum Gate in a Semiconductor Quantum Dot , 2003, Science.

[19]  T. Mančal,et al.  Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems , 2007, Nature.

[20]  Thomas,et al.  Coupling of exciton transitions associated with different quantum-well islands. , 1993, Physical review. B, Condensed matter.

[21]  J. Wilkins,et al.  Splitting of the excitonic peak in quantum wells with interfacial roughness , 1998 .

[22]  S. Cundiff,et al.  Role of excitation-induced shift in the coherent optical response of semiconductors , 2002 .

[23]  A. Zrenner,et al.  Coherent properties of a two-level system based on a quantum-dot photodiode , 2002, Nature.

[24]  Leo,et al.  Effects of coherent polarization interactions on time-resolved degenerate four-wave mixing. , 1990, Physical review letters.

[25]  Weiss,et al.  Instantaneous frequency dynamics of coherent wave mixing in semiconductor quantum wells. , 1993, Physical review letters.