The optical Stark effect is a tell-tale signature of coherent light-matter interaction in excitonic systems, wherein an irradiating light beam tunes exciton transition frequencies. Here we show that, when excitons are placed in a nanophotonic cavity, the excitonic Stark effect can become highly nonlinear, exhibiting multi-valued and hysteretic Stark shifts that depend on the history of the irradiating light. This multistable Stark effect (MSE) arises from feedback between the cavity mode occupation and excitonic population, mediated by the Stark-induced mutual tuning of the cavity and excitonic resonances. Strikingly, the MSE manifests even for very dilute exciton concentrations and can yield discontinuous Stark shift jumps of order meV. We expect that the MSE can be realized in readily available transition metal dichalcogenide excitonic systems placed in planar photonic cavities, at modest pump intensities. This phenomenon can provide new means to engineer coupled states of light and matter that can persist even in the single exciton limit.
We report on the observation of spin dependent optically dressed states and optical Stark effect on an individual Mn spin in a semiconductor quantum dot. The vacuum-to-exciton or the exciton-to-biexciton transitions in a Mn-doped quantum dot are optically dressed by a strong laser field and the resulting spectral signature is measured in photoluminescence. We demonstrate that the energy of any spin state of a Mn atom can be independently tuned using the optical Stark effect induced by a control laser. High resolution spectroscopy reveals a power, polarization and detuning dependent Autler-Town…
We show that two initially non-resonant quantum dots may be brought into resonance by the application of a single detuned laser. This allows for control of the inter-dot interactions and the generation of highly entangled excitonic states on the picosecond timescale. Along with arbitrary single qubit manipulations, this system would be sufficient for the demonstration of a prototype excitonic quantum computer.
Monolayer transition metal dichalcogenide semiconductors host strongly bound two-dimensional excitonic complexes, and form an excellent platform for probing many-body physics through manipulation of Coulomb interaction. Quantum confined Stark effect is one of the routes to dynamically tune the emission line of these excitonic complexes. In this work, using a high quality graphene/hBN/WS$_2$/hBN/Au vertical heterojunction, we demonstrate for the first time, an out-of-plane electric field driven change in the sign of the Stark shift from blue to red for four different excitonic species, namely, …
We theoretically investigate excitons in MoS$_2$ monolayers in an applied in-plane electric field. Tight-binding and Bethe-Salpeter equation calculations predict a quadratic Stark shift, of the order of a few meV for fields of 10 V/$μ$m, in the linear absorption spectra. The spectral weight of the main exciton peaks decreases by a few percent with an increasing electric field due to the exciton field ionization into free carriers as reflected in the exciton wave functions. Subpicosecond exciton decay lifetimes at fields of a few tens of V/$μ$m could be utilized in solar energy harvesting and p…
We present studies on Coulomb interactions in single self-assembled CdTe quantum dots. We use a field effect structure to tune the charge state of the dot and investigate the impact of the charge state on carrier wave functions. The analysis of the quantum confined Stark shifts of four excitonic complexes allows us to conclude that the hole wave function is softer than electron wave function, i. e. it is subject to stronger modifications upon changing of the dot charge state. These conclusions are corroborated by time-resolved photoluminescence studies of recombination lifetimes of different e…
We calculate the excitonic spectrum of few-layer black phosphorus by direct diagonalization of the effective mass Hamiltonian in the presence of an applied in-plane electric field. The strong attractive interaction between electrons and holes in this system allows one to investigate the Stark effect up to very high ionizing fields, including also the excited states. Our results show that the band anisotropy in black phosphorus becomes evident in the direction dependent field induced polarizability of the exciton.
The Dynamical Franz-Keldysh Effect is exposed by exploring near-bandgap absorption in the presence of intense THz electric fields. It bridges the gap between the DC Franz- Keldysh effect and multi-photon absorption and competes with the THz AC Stark Effect in shifting the energy of the excitonic resonance. A theoretical model which includes the strong THz field non-perturbatively via a non-equilibrium Green Functions technique is able to describe the Dynamical Franz-Keldysh Effect in the presence of excitonic absorption.
We propose a coherent control scheme based on the optical Stark effect in optically generated excitons in quantum dot molecules (QDMs). We show that, by the combined action of voltage bias detuning sweeps and Rosen-Zener pulsed interactions, it is possible to dynamically generate and modify an anticrossing gap that emerges between the dressed energy levels of long-lived, spatially indirect excitons. We perform numerical and analytic non-perturbative calculations based on the Bloch-Feshbach formalism, which demonstrate that this effect induces a mechanism of coherent population trapping of indi…
Coherent interaction between matter and periodic light field induces both optical Stark effect (OSE) and Bloch-Siegert shift (BSS). Observing the BSS has been historically challenging, not only because it is weak but it is often accompanied by a much stronger OSE. Herein, by controlling the light helicity, we can largely restrict the OSE and BSS to different spin-transitions in CsPbI3 perovskite quantum dots, achieving room-temperature BSS as strong as 4 meV with near-infrared pulses. The ratio between the BSS and OSE magnitudes is however systematically higher than the prediction by the non-i…
The $k\cdot p$ effective mass approximation (EMA) predicts large, nearly size-independent exciton oscillator strengths in quantum confined semiconductors. Yet, experimental reports have concluded that the total oscillator strength of the lowest-energy (1S$_{3/2}$1S$_{\text{e}}$) excitons in strongly confined CdSe NQDs is small and strongly size-dependent. Using the optical Stark effect, we show that the oscillator strength of the 1S$_{3/2}$1S$_{\text{e}}$ excitonic absorption peak in CdSe NQDs follows the predictions of the EMA. These oscillator strengths enable helicity-selective unsaturated …
This letter assigns the Faraday rotation in photoexcited semiconductors to ``Pauli interactions'', \emph{i}. \emph{e}., carrier exchanges, between the real excitons present in the sample and the virtual excitons coupled to the $σ_{\pm}$ parts of a linearly polarized light. While \emph{direct Coulomb} interactions scatter bright excitons into bright excitons, whatever their spins are, \emph{Pauli} interactions do it for bright excitons \emph{with same spin only}. This makes these Pauli interactions entirely responsible for the refractive index difference, which comes from processes in which the…
Transition metal dichalcogenides (TMDs) constitute a versatile platform for atomically thin optoelectronics devices and spin-valley memory applications. In monolayers optical absorption is strong, but the transition energy is not tunable as the neutral exciton has essentially no out-of-plane electric dipole. In contrast, interlayer exciton transitions in heterobilayers are widely tunable in applied electric fields, but their coupling to light is considerably reduced. Here, we show tuning over 120 meV of interlayer excitons with high oscillator strength in bilayer MoS2. These shifts are due to …
We report experimental evidence of excitonic spin-splitting, in addition to the conventional Zeeman effect, produced by a combination of the Rashba spin-orbit interaction, Stark shift and charge screening. The electric-field-induced modulation of the spin-splitting are studied during the charging and discharging processes of p-type GaAs/AlAs double barrier resonant tunneling diodes (RTD) under applied bias and magnetic field. The abrupt changes in the photoluminescence, with the applied bias, provide information of the charge accumulation effects on the device.
We report on the experimental and theoretical investigation of magnetic-field-induced second harmonic generation (SHG) and two-photon absorption (TPA) of excited exciton states ($n \geq 3$) of the yellow series in Cu$_2$O. In this centrosymmetric material, SHG can occur due to constructive interplay of electric dipole and electric quadrupole/magnetic dipole transitions for light propagating along the low-symmetry directions [111] or [112]. By application of a magnetic field in Voigt configuration, SHG gets also allowed for excitation along the [110]-axis and even the high-symmetry cubic direct…
We investigate and compare experimental and numerical excitonic spectra of the yellow series in cuprous oxide Cu$_2$O in the Voigt configuration and thus partially extend the results from Schweiner et al. [Phys. Rev. B 95, 035202 (2017)], who only considered the Faraday configuration. The main difference between the configurations is given by an additional effective electric field in the Voigt configuration, caused by the motion of the exciton through the magnetic field. This Magneto-Stark effect was already postulated by Gross et al. and Thomas et al. in 1961 [Sov. Phys. Solid State 3, 221 (1…
Demonstrating the quantum-confined Stark effect (QCSE) in silicon nanocrystals (NCs) embedded in oxide has been rather elusive, unlike the other materials. Here, the recent experimental data from ion-implanted Si NCs is unambiguously explained within the context of QCSE using an atomistic pseudopotential theory. This further reveals that the majority of the Stark shift comes from the valence states which undergo a level crossing that leads to a nonmonotonic radiative recombination behavior with respect to the applied field. The polarizability of embedded Si NCs including the excitonic effects …
We show how to compute the optical functions of Wide Parabolic Quantum Wells (WPQWs) exposed to uniform electric F applied in the growth direction, in the excitonic energy region. The effect of the coherence between the electron-hole pair and the electromagnetic field of the propagating wave including the electron-hole screened Coulomb potential is adopted, and the valence band structure is taken into account in the cylindrical approximation. The role of the interaction potential and of the applied electric field, which mix the energy states according to different quantum numbers and create sy…
The study of two-dimensional (2D) van der Waals materials has been an active field of research in the development of new optoelectronics and photonic applications over the last decade. Organic-inorganic layered perovskites are currently some of the most promising 2D van der Waals materials, due to their exceptional optical brightness and enhanced excitonic effects. However, low crystal quality and spectral diffusion usually broaden the exciton linewidth, obscuring the fine structure of the exciton in conventional photoluminescence experiments. Here, we propose a mechanical approach for reducin…
In 1H monolayer transition metal dichalcogenide, the inversion symmetry is broken, while the reflection symmetry is maintained. On the contrary, in the bilayer, the inversion symmetry is restored, but the reflection symmetry is broken. As a consequence of these contrasting symmetries, here we show that bilayer WS$_2$ exhibits a quantum confined Stark effect (QCSE) that is linear with the applied out-of-plane electric field, in contrary to a quadratic one for a monolayer. The interplay between the unique layer degree of freedom in the bilayer and the field driven partial inter-conversion betwee…
We systematically measure the dielectric function of atomically thin MoS2 films with different layer numbers and demonstrate that excitonic effects play a dominant role in the dielectric function when the films are less than 5-7 layers thick. The dielectric function shows an anomalous dependence on the layer number. It decreases with the layer number increasing when the films are less than 5-7 layers thick but turns to increase with the layer number for thicker films. We show that this is because the excitonic effect is very strong in the thin MoS2 films and its contribution to the dielectric …
We investigate the magneto-optical properties of excitons bound to single stacking faults in high-purity GaAs. We find that the two-dimensional stacking fault potential binds an exciton composed of an electron and a heavy-hole, and confirm a vanishing in-plane hole $g$-factor, consistent with the atomic-scale symmetry of the system. The unprecedented homogeneity of the stacking-fault potential leads to ultra-narrow photoluminescence emission lines (with full-width at half maximum ${\lesssim 80~μ\text{eV} }$) and reveals a large magnetic non-reciprocity effect that originates from the magneto-S…
The Berry phase of Bloch states can have profound effects on electron dynamics lead to novel transport phenomena, such as the anomalous Hall effect and the valley Hall effect. Recently, it was predicted that the Berry phase effect can also modify the exciton states in transition metal dichalcogenide monolayers, and lift the energy degeneracy of exciton states with opposite angular momentum through an effective valley-orbital coupling. Here, we report the first observation and control of the Berry-phase induced splitting of the 2p-exciton states in monolayer molybdenum diselenide using the intr…
Photogenerated excitonic ensembles confined in coupled GaAs quantum wells are probed by a complementary approach of emission spectroscopy and resonant inelastic light scattering. Lateral electrostatic trap geometries are used to create dense systems of spatially indirect excitons and excess holes with similar densities in the order of 10$^{11}$ cm$^{-2}$. Inelastic light scattering spectra reveal a very sharp low-lying collective mode that is identified at an energy of 0.44 meV and a FWHM of only ~50 $μ$eV. This mode is interpreted as a plasmon excitation of the excess hole system coupled to t…
