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Multiple-quantum 2D spectroscopy of many-body correlations in GaAs quantum wells

Keith Adam Nelson, Dylan H. Arias, Wen, Patrick, Katherine W. Stone, Daniel B. Turner

Published Jan 1, 2010• 0 citations
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Abstract

Multiple-quantum two-dimensional Fourier transform optical (2D FTOPT) spectroscopy was developed and conducted on GaAs quantum wells. Spatiotemporal femtosecond pulse shaping was used to control the optical phases and time delays of ultrashort pulses in multiple non-collinear beams so that fully coherent four-wave and higher-order mixing measurements could be conducted without delay stages, multiple interferometers, or any active phase control. Coherences of biexcitons, unbound but correlated exciton pairs, and excitons undergoing rephasing were observed directly.

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arXiv:cond-mat/0701424•Physical Review B•Mar 2, 2007•65 citations
Multiple-quantum two-dimensional Fourier transform optical (2D FTOPT) spectroscopy was developed and conducted on GaAs quantum wells. Spatiotemporal femtosecond pulse shaping was used to control the optical phases and time delays of ultrashort pulses in multiple non-collinear beams so that fully coherent four-wave and higher-order mixing measurements could be conducted without delay stages, multiple interferometers, or any active phase control. Coherences of biexcitons, unbound but correlated exciton pairs, and excitons undergoing rephasing were observed directly.
Multiple-quantum two-dimensional Fourier transform optical (2D FTOPT) spectroscopy was developed and conducted on GaAs quantum wells. Spatiotemporal femtosecond pulse shaping was used to control the optical phases and time delays of ultrashort pulses in multiple non-collinear beams so that fully coherent four-wave and higher-order mixing measurements could be conducted without delay stages, multiple interferometers, or any active phase control. Coherences of biexcitons, unbound but correlated exciton pairs, and excitons undergoing rephasing were observed directly.
Electronic structure and dynamics are captured by optical 2D-Fourier-transform (2DFT) spectroscopy, which tracks the phase of the nonlinear signal during two time delays of a multi-pulse excitation sequence. These Fourier-transformed spectra separate and isolate overlapping and competing contributions to the coherent response. We have developed an ultra-stable platform consisting of nested interferometers with active phase control, allowing for exploration of single- and two-quantum coherences. Phase-resolved spectra are retrieved by all-optical determination of experimental phase ambiguities. GaAs quantum wells show suppression of many-body interactions in cross-linear polarized 2DFT spectra and many-body two-quantum coherences. Potassium vapor also shows unexpected two-quantum coherences.
We demonstrate three-dimensional (3D) electronic Fourier transform spectroscopy of GaAs quantum wells using four fully phase-coherent, noncollinear optical fields. Since the full complex signal field is measured as a function of all three time intervals, nearly every peak in the resulting 3D spectral solid arises from a distinguishable sequence of transitions represented by a single Feynman pathway. We use the 3D spectral peaks to separate two pathways involving weakly bound mixed biexcitons generated in different time orders. In the process, we reveal a peak that was previously obscured by a correlated but unbound exciton pair coherence. We also demonstrate a calibration procedure for the carrier frequency which yields biexciton binding energy values with high accuracy.
Multidimensional analysis of coherent signals is commonly used in nuclear magnetic resonance to study correlations among spins. These techniques were recently extended to the femtosecond regime and applied to chemical, biological and semiconductor systems. In this work, we apply a two-dimensional correlation spectroscopy technique which employs double-quantum-coherence to investigate many-body effects in a semiconductor quantum well. The signal is detected along the direction k(1)+ k(2)- k(3), where k(1), k(2) and k(3) are the pulse wave vectors in chronological order. We show that this signal is particularly sensitive to many-body correlations which are missed by time-dependent Hartree-Fock approximation. The correlation energy of two-exciton can be probed with a very high resolution arising from a two-dimensional correlation spectrum, where two-exciton couplings spread the cross peaks along both axes of the 2D spectrum to create a characteristic highly resolved pattern. This level of detail is not available from conventional one-dimensional four-wave mixing or other two-dimensional correlation spectroscopy signals such as the photo echo (-k(1)+ k(2)+ k(3)).