Travis M. Autry

Multidimensional coherent photocurrent spectroscopy of a semiconductor nanostructure

Multidimensional Coherent Optical Photocurrent Spectroscopy (MD-COPS) is implemented using unstabilized interferometers. Photocurrent from a semiconductor sample is generated using a sequence of four excitation pulses in a collinear geometry. Each pulse is frequency shifted by a unique radio frequency through acousto-optical modulation; the Four-Wave Mixing (FWM) signal is then selected in the frequency domain. The interference of an auxiliary continuous wave laser, which is sent through the same interferometers as the excitation pulses, is used to synthesize reference frequencies for lock-in detection of the photocurrent FWM signal. This scheme enables the partial compensation of mechanical fluctuations in the setup, achieving sufficient phase stability without the need for active stabilization. The method intrinsically provides both the real and imaginary parts of the FWM signal as a function of inter-pulse delays. This signal is subsequently Fourier transformed to create a multi-dimensional spectrum. Measurements made on the excitonic resonance in a double InGaAs quantum well embedded in a p-i-n diode demonstrate the technique.

Coherent excitonic coupling in an asymmetric double InGaAs quantum well arises from many-body effects.

We study an asymmetric double InGaAs quantum well using optical two-dimensional coherent spectroscopy. The collection of zero-quantum, one-quantum, and two-quantum two-dimensional spectra provides a unique and comprehensive picture of the double well coherent optical response. Coherent and incoherent contributions to the coupling between the two quantum well excitons are clearly separated. An excellent agreement with density matrix calculations reveals that coherent interwell coupling originates from many-body interactions.

Multi-dimensional coherent optical spectroscopy of semiconductor nanostructures: Collinear and non-collinear approaches

We review our recent work on multi-dimensional coherent optical spectroscopy (MDCS) of semiconductor nanostructures. Two approaches, appropriate for the study of semiconductor materials, are presented and compared. A first method is based on a non-collinear geometry, where the Four-Wave-Mixing (FWM) signal is detected in the form of a radiated optical field. This approach works for samples with translational symmetry, such as Quantum Wells (QWs) or large and dense ensembles of Quantum Dots (QDs). A second method detects the FWM in the form of a photocurrent in a collinear geometry. This second approach extends the horizon of MDCS to sub-diffraction nanostructures, such as single QDs, nanowires, or nanotubes, and small ensembles thereof. Examples of experimental results obtained on semiconductor QW structures are given for each method. In particular, it is shown how MDCS can assess coupling between excitons confined in separated QWs.

Analytical solutions to the finite-pulse Bloch model for multidimensional coherent spectroscopy

We present perturbative analytical solutions to the optical Bloch equations at third order, with finite duration Gaussian pulse envelopes. We find that a given double-sided Feynman diagram in this approximation can be conveniently described in the frequency domain as a product of the expression in the impulsive limit and a finite-pulse factor. Finite-pulse effects are Feynman-diagram-dependent, however, and include nontrivial phase corrections that can occur even in the case of transform-limited pulses. The results constitute a practical framework for modeling phenomena in multidimensional coherent spectroscopy that cannot easily be captured in the impulsive limit, including the roles of bandwidth, resonance, and pulse chirp.

Direct imaging of surface plasmon polariton dispersion in gold and silver thin films

We image the dispersion of surface plasmon polaritons in gold and silver thin films of 30 and 50 nm thickness, using angle-resolved white light spectroscopy in the Kretschmann geometry. Calibrated dispersion curves are obtained over a wavelength range spanning from 550 to 900 nm. We obtain good qualitative agreement with calculated dispersion curves that take into account the thickness of the thin film.

Many-body interactions between excitons in GaAs quantum wells quantified using two-dimensional coherent spectroscopy

We have quantified excitonic many-body interaction energies in GaAs quantum wells using two-dimensional coherent spectroscopy. The anharmonic oscillator model for excitons is used to extract the inter- and intra-mode interaction energies from 2D spectra.

Measurement of nonlinear polariton dispersion curves reveals the Tavis-Cummings quantum ladder

The nonlinear dispersion curves of the Tavis-Cummings quantum ladder are measured for exciton-polaritons. This quantum ladder remixes the exciton-cavity system in a manner analogous to a quantum beam splitter, realizing a light-matter n=2 nOOn state.

Observation of the Excitation Ladder in a Microcavity Diode Using Multi-quantum Coherent Optical Photocurrent Spectroscopy

Light-matter coupling in a cavity results in a ladder of states with splittings determined by the coupling strength. We observe the higher ladder rungs in a semiconductor microcavity using multiquantum coherent optical photocurrent spectroscopy.

Optical two-dimensional coherent spectroscopy of semiconductor nanostructures

Our recent work on optical two-dimensional coherent spectroscopy (2DCS) of semiconductor materials is reviewed. We present and compare two approaches that are appropriate for the study of semiconductor nanostructures. The first one is based on a non-collinear geometry, where the Four-Wave-Mixing (FWM) signal is detected in the form of a radiated optical field. This approach works for samples with translational symmetry, such as Quantum Wells (QWs), or large and dense ensembles of Quantum Dots (QDs). The second method is based on a collinear geometry, where the FWM is detected in the form of a photocurrent. This second approach enables 2DCS of samples where translational symmetry is broken, such as single QDs, nanowires, or nanotubes, and small ensembles thereof. For each method, we provide an example of experimental results obtained on semiconductor QWs. In particular, it is shown how 2DCS can reveal coherent excitonic coupling between adjacent QWs.

Coupling in InGaAs double quantum wells studied with 2D Fourier transform spectroscopy

We study asymmetric double InGaAs quantum well samples, featuring three different barrier widths, using optical two-dimensional Fourier transform spectroscopy. Depending on the barrier width, we observe different coupling mechanisms between the two wells.