Direct evidence of exciton condensation in semiconductor heterostructures remains elusive. Here we propose charge transport of doped carriers as a probe of exciton condensation in transition-metal dichalcogenide heterostructures and identify distinct experimental signatures. First, condensation suppresses the phase space for carrier scattering, leading to a reduction in resistivity, that provides a general diagnostic of exciton condensation. Second, in heterostructures with a tunable solid-state Feshbach resonance, condensate-induced hybridization between doped carriers and trion bound states qualitatively modifies transport. In particular, near resonance, this hybridization yields a negative effective mass and a corresponding sign reversal of the Hall resistivity. These results establish charge transport as a promising route for detecting and characterizing exciton condensation in semiconductor heterostructures.
Direct evidence of exciton condensation in semiconductor heterostructures remains elusive. Here we propose charge transport of doped carriers as a probe of exciton condensation in transition-metal dichalcogenide heterostructures and identify distinct experimental signatures. First, condensation suppresses the phase space for carrier scattering, leading to a reduction in resistivity, that provides a general diagnostic of exciton condensation. Second, in heterostructures with a tunable solid-state Feshbach resonance, condensate-induced hybridization between doped carriers and trion bound states qualitatively modifies transport. In particular, near resonance, this hybridization yields a negative effective mass and a corresponding sign reversal of the Hall resistivity. These results establish charge transport as a promising route for detecting and characterizing exciton condensation in semiconductor heterostructures.
The study of the nonlinear optical response of excitons in semiconductors is important for both scientific and technological applications. Although the nonlinear optical properties of bulk semiconductors and heterostructures have been studied for almost three decades, with most of the research focusing on heterostructures, the mechanisms leading to the nonlinearities in these systems are not completely understood. Determining these mechanisms and developing a theoretical picture which describes the most dominant effects remains a challenge and an active area of study. Although optical interactions in semiconductors is a genuine many-body problem, a description of this system similar to the optical Bloch equations used in atomic studies has shown some success, but more work is needed to make this model complete. Experimental work, particularly in the bulk system uncomplicated by the interface disorder present in heterostructures, will provide the guidance to extend this formalism. In this dissertation, the frequency domain resonant nonlinear optical response of excitons in bulk gallium arsenide at low density is studied to gain insight into the dominant mechanisms leading to the response, as well as the dynamics of the nominally three-dimensional excitonic system. Specifically, the nonlinear response was probed with differential transmission (DT) and four-wave mixing (FWM) experiments, which measure to lowest order the third-order susceptibility, $\chi\sp{(3)}.$ Using these various tools, three specific areas were studied and the results will be presented. First, the role of the biexciton, the state of two bound excitons, in determining the bulk nonlinear response was explored. The observation of a red-shifted nonlinear resonance suggests the importance of this state at moderate densities. Second, a new response, characterized by a resonant increase in exciton absorption induced by optical pumping with initial superlinear growth and a transition to behavior described by simple line broadening with increased pump intensity, was studied in detail. A model considering increased polariton absorption with increased exciton-exciton interactions explains these effects. Finally, nonlinear optical spectroscopy was used to study exciton transport, where near-ballistic behavior was revealed. The effect of exciton transport, thermalization and radiative recombination on the nonlinear optical response was explored.
The realization of Coulomb coupled electron-hole double layers in 2D semiconductor heterostructures has enabled the thermodynamic and transport studies of equilibrium exciton fluids without a magnetic field. By doping the exciton fluid with additional electrons/holes, an equilibrium fluid of trions - three particle bound states of electrons and holes - further emerge, providing the platform to explore new transport phenomena associated with such composite particles. Here we report the observation of a Hall effect for trions in MoSe2/WSe2 heterobilayers, which support Coulomb-coupled electron and hole fluids with tunable densities. The Hall effect arises from a Lorentz force on trions under a perpendicular magnetic field. It is manifested in both Hall drag measurements and standard Hall effect measurements on just one of the semiconductor layers. For negatively charged trions, an electron Hall effect is observed even in a hole doped WSe2 monolayer due to the presence of trion drags. The trion Hall effect also disappears when the trions are ionized at elevated temperatures and/or high trion densities. Our work opens the door for realizing quantum oscillations and the quantum Hall effect for trions.
Energy renormalizations of resident carriers and excitons are studied theoretically, and compared with recent experiments of electrostatically-doped WSe2 monolayers. The calculated energy renormalization of resident carriers, subjected to strong out-of-plane magnetic field, reveals the importance of dynamical screening in transition metal dichalcogenides. The energy renormalization of tightly bound excitons is analyzed through the exchange interaction between the electron (or hole) component of the exciton and resident carriers that share the same spin and valley quantum numbers. Our theory explains the weak energy shift of excitonic resonances despite the strong energy renormalization of resident carriers. We identify the dependence of the energy renormalization on the envelope function of a tightly-bound exciton, showing that unlike free electron-hole pairs, this energy renormalization is not the added renormalizations of a resident electron and resident hole.
I report on the effect of a moderate excess electron population on nonlinearities in modulation-doped CdTe quantum wells. I show that the electron population does not qualitatively affect the nature of correlations between excitons. In this respect, I bring strong evidence of the existence of unbound and bound (stable) two-exciton states in the presence of electrons and charged excitons (trions). In time-resolved pump and probe experiment, they lead to the observation of electromagnetically induced transparency and optical Stark shift of the exciton resonance. Rabi flopping of excitons within a sea of electrons is also clearly evidenced through ac Stark splitting and gain without inversion. The quantum coherence is more robust to electron induced dephasing than what would have been expected. I demonstrate third and higher-order exciton correlations in the presence of electrons, which manifest, for increasing exciton densities, through the blue-shift of counter-polarized exciton resonance, the red-shift of the biexciton resonance and the exciton to biexciton crossover. I also evidence correlated behavior of excitons and trions under excitation which manifests itself by crossed trion-exciton effects. I observe a wealth of phenomena encompassing bleaching, crossed bleaching, induced-absorption and energy shifts of the resonances. Significant differences are found between the nonlinear optical effects induced by an exciton and a trion population. Electron scattering with electron and exciton is shown to strongly broaden the high energy tail of exciton and trion resonance lineshapes. Variations of electron density result in a clear modification of both resonance lineshapes. The dynamics of the formation of trions is also studied. I propose a two-channel mechanism for their formation; they are formed through bi- and tri-molecular processes. This implies that both negatively and positively charged excitons coexist in a quantum well, even in the absence of excess carriers. The model is applied to a time-resolved photoluminescence experiment performed on a very high quality InGaAs quantum well sample, in which the photoluminescence contributions at the energy of the trion, exciton and at the band edge can be clearly separated and traced over a broad range of times and densities. The unresolved discrepancy between the theoretical and experimental radiative decay time of the exciton in a doped semiconductor is explained.
Type-II quantum well heterostructures are considered high-potential candidates for next-generation active semiconductor devices. They promise low fundamental transition energies and suppressed Auger scattering as well as temperature stability in device performance. Understanding their fundamental properties, such as scattering and diffusion, and revealing intricate differences from type-I quantum structures are important steps towards optimized structure design. Using degenerate four-wave mixing spectroscopy, we investigate the phase coherence of excitonic polarizations in a (Ga,In)As/GaAs/Ga(As,Sb) type-II double-quantum-well structure. It is designed to exhibit spectrally isolated resonances in its linear absorption spectrum including a well-resolved charge-transfer exciton resonance. This allows us to study the coherent dynamics of the unperturbed charge-transfer exciton polarization. In addition, the effects of many-body interactions with free charge carriers as well as excitons that are injected by an optical prepulse are revealed. Scattering of charge-transfer excitons with free charge carriers is three times more efficient than scattering of charge-transfer excitons with each other. The comparison with Wannier excitons in a type-I quantum well structure shows that the interaction strength between charge-transfer excitons is about twice as large as for excitons in a type-I quantum well structure.
The bilayer Hubbard model with electron-hole doping is an ideal platform to study excitonic orders due to suppressed recombination via spatial separation of electrons and holes. However, suffering from the sign problem, previous quantum Monte Carlo studies could not arrive at an unequivocal conclusion regarding the presence of phases with clear signatures of excitonic condensation in bilayer Hubbard models. Here, we develop a determinant quantum Monte Carlo algorithm for the bilayer Hubbard model that is sign-problem-free for equal and opposite doping in the two layers and study excitonic order and charge and spin density modulations as a function of chemical potential difference between the two layers, on-site Coulomb repulsion, and interlayer interaction. In the intermediate coupling regime and in proximity to the SU(4)-symmetric point, we find a biexcitonic condensate phase at finite electron-hole doping, as well as a competing (π,π) charge density wave state. We extract the Berezinskii-Kosterlitz-Thouless transition temperature from superfluid density and a finite-size scaling analysis of the correlation functions and explain our results in terms of an effective biexcitonic hard-core boson model.