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

Daniel Turner, Patrick Wen, Dylan H. Arias, Keith A. Nelson

Research output: Contribution to journalArticle

Abstract

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 line shapes. 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.

Original languageEnglish (US)
Article number165321
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume84
Issue number16
DOIs
StatePublished - Oct 21 2011

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Excitons
fluence
excitons
Spectroscopy
optical polarization
Light polarization
electronics
Linewidth
spectroscopy
line shape
Spectrometers
Nanostructures
interactions
spectrometers
Semiconductor materials
Lasers
pulses
lasers
simulation
LDS 751

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Electronic, Optical and Magnetic Materials

Cite this

Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy. / Turner, Daniel; Wen, Patrick; Arias, Dylan H.; Nelson, Keith A.

In: Physical Review B - Condensed Matter and Materials Physics, Vol. 84, No. 16, 165321, 21.10.2011.

Research output: Contribution to journalArticle

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