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arXiv:2112.01100 · Physical review. B./Physical review. B

Coherent contributions to population dynamics in a semiconductor microcavity

Jagannath Paul, Hendrik Rose, Ethan Swagel, T. Meier, Jared K. Wahlstrand, Alan D. Bristow

Published Mar 29, 2022• 6 citations
arXivHTMLPDF

Abstract

Multidimensional coherent spectroscopy (MDCS) is used to separate coherent and incoherent nonlinear contributions to the population-time dynamics in a GaAs-based semiconductor microcavity encapsulating a single InGaAs quantum well. In a three-pulse four-wave-mixing scheme, the second delay time is the population time that in MDCS probes excited-state coherences and population dynamics. Nonlinear optical interactions can mix these contributions, which are isolated here for the lower- and upper-exciton polariton through the self- and mutual-interaction features. Results show fast decays and oscillations arising from the coherent response, including a broad stripe along the absorption energy axis, and longer time mutual-interaction features that do not obey a simple population decay model. These results are qualitatively replicated by Bloch equation simulations for the $1s$ exciton strongly coupled to the intracavity field. The simulations allow for separation of coherent and incoherent Pauli-blocking and Coulomb interaction terms within the ${\ensuremath{\chi}}^{(3)}$-limit, and a direct comparison of each feature in one-quantum rephasing and zero-quantum spectra.

DOI
10.1103/physrevb.105.115307

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Multidimensional coherent spectroscopy (MDCS) is used to separate coherent and incoherent nonlinear contributions to the population-time dynamics in a GaAs-based semiconductor microcavity encapsulating a single InGaAs quantum well. In a three-pulse four-wave-mixing scheme, the second delay time is the population time that in MDCS probes excited-state coherences and population dynamics. Nonlinear optical interactions can mix these contributions, which are isolated here for the lower- and upper-exciton polariton through the self- and mutual-interaction features. Results show fast decays and oscillations arising from the coherent response, including a broad stripe along the absorption energy axis, and longer time mutual-interaction features that do not obey a simple population decay model. These results are qualitatively replicated by Bloch equation simulations for the 1s1s1s exciton strongly coupled to the intracavity field. The simulations allow for separation of coherent and incoherent Pauli-blocking and Coulomb interaction terms within the \ensuremathχ(3){\ensuremath{\chi}}^{(3)}\ensuremathχ(3)-limit, and a direct comparison of each feature in one-quantum rephasing and zero-quantum spectra.
Light-matter interactions associated with excitons and exciton related complexes are explored in bulk GaAs and semiconductor microcavities using multidimensional coherent spectroscopy (MDCS). This approach provides rich spectra determining quantum excitation pathways, structural influences on the excitons, and coherence times.;Polarization, excitation density, and temperature-dependent MDCS is performed on excitons in strained bulk GaAs layers, probing the coherent response for differing amounts of strain. Biaxial tensile strain lifts the degeneracy of heavy-hole and light-hole valence states, leading to an observed splitting of the associated excitons at low temperature. Increasing the strain increases the magnitude of the heavy-/light- hole exciton peak splitting, induces an asymmetry in the off-diagonal interaction coherences, increases the difference in the heavy- and light- hole exciton homogenous linewidths, and increases the inhomogeneous broadening of both exciton species. All results arise from strain-induced variations in the local electronic environment, which is not uniform along the growth direction of the thin layers. For cross-linear polarized excitation, wherein excitonic signals give way to biexcitonic signals, the high-strain sample shows evidence of bound light-, heavy- and mixed- hole biexcitons.;2DCS maps the anticrossing associated with normal mode splitting in a semiconductor microcavity. For a detuning range near zero, it is observed that there are two diagonal features related to the intra-action of exciton-polariton branches and two off-diagonal features related to coherent interaction between the polaritons. At negative detuning, the line shape properties of the diagonal intra-action features are distinguishable and can be associated with cavity-like and exciton-like modes. A biexcitonic companion feature is observed, shifted from the exciton feature by the biexciton binding energy. Closer to zero detuning, all features are enhanced and the diagonal intra-action features become nearly equal in amplitude and linewidth. At positive detuning the exciton-like and cavity-like characteristics return to the diagonal intra-action features. Off-diagonal interaction features exhibit asymmetry in their amplitudes throughout the detuning range. The amplitudes are strongly modulated as the lower polariton branch crosses the bound biexciton energy determined from negatively detuned spectra.
Abstract Multidimensional coherent optical spectroscopy (MDCS) is an elegant and versatile tool to measure the ultrafast nonlinear optical response of materials. Of particular interest for semiconductor nanostructures, MDCS enables the separation of homogeneous and inhomogeneous linewidths, reveals the nature of coupling between resonances, and is able to identify the signatures of many-body interactions. As an extension of transient four-wave mixing (FWM) experiments, MDCS can be implemented in various geometries, in which different strategies can be used to isolate the FWM signal and measure its phase. I review and compare different practical implementations of MDCS experiments adapted to the study of semiconductor materials. The power of MDCS is illustrated by discussing experimental results obtained on semiconductor nanostructures such as quantum dots, quantum wells, microcavities, and layered semiconductors.
Multidimensional coherent spectroscopy maps the detuning dependence of the upper (UP) and lower (LP) excitonpolariton branches1 in a wedged microcavity with a single InGaAs quantum well at 5 K. Features on the diagonal correspond to intra-action coherences of the UP and LP branches. Off-diagonal peaks are interaction coherences between the UP and LP branches. With increasing detuning (Δ), all peaks move to higher energy, the exciton-like (EEX) and cavity-like (Eγ) modes swap position and have maximum intensity near the anti-crossing at Δ=0. An isolated biexciton (B) is only seen at Δ<0, separated by a binding energy of approximately 2 meV. For Δ>0, the spectral weight of the off-diagonal features swap, as the LP and B come into resonance. This indicates that the off-diagonal features are sensitive to the interactions including two-quantum contributions and that a situation similar to a Feshbach resonance exists.2 Polarization of two-quantum contributions show spin sensitive two-polariton and new biexciton correlations. The latter likely influence the Feshbach resonance between biexcitons and two-polariton states. The two-quantum signatures also demonstate that biexcitons perturb the light-matter coupling in the microcavity to reduce the mixed two-polariton contributions. Detuning dependence of zero-quantum contributions show Raman-like coherences that are enhanced near zero detuning. Asymmetry of the Raman coherences are indicative of many-body interactions, which also grow stronger as the light-matter interactions are enhanced near zero deuning.
Multi-dimensional coherent spectroscopy (MDCS) has become an extremely versatile and sensitive technique for elucidating the structure, composition, and dynamics of condensed matter, atomic, and molecular systems. The appeal of MDCS lies in its ability to resolve both individual-emitter and ensemble-averaged dynamics of optically created excitations in disordered systems. When applied to semiconductors, MDCS enables unambiguous separation of homogeneous and inhomogeneous contributions to the optical linewidth, pinpoints the nature of coupling between resonances, and reveals signatures of many-body interactions. In this review, we discuss the implementation of MDCS to measure the nonlinear optical response of excitonic transitions in semiconductor nanostructures. Capabilities of the technique are illustrated with recent experimental studies that advance our understanding of optical decoherence and dissipation, energy transfer, and many-body phenomena in quantum dots and quantum wells, semiconductor microcavities, layered semiconductors, and photovoltaic materials.
In article number 1800171, Christopher L. Smallwood and Steven T. Cundiff introduce a multidimensional coherent spectroscopy (MDCS) probe of the dynamics of excitons in an asymmetric In0.05Ga0.95As/GaAs double quantum well. Spectral information here is plotted as a correlation between the frequency of a first-order optical excitation interaction (ωτ) and a third-order emission interaction (ωt) at various intermediate-state mixing times (T), providing a window into a semiconductor's inhomogeneity, many-body interactions, and coherent coupling dynamics at femtosecond timescales. Image credit: Brad Baxley, Part to Whole.