Electric dipole radiation can be controlled by coherent optical feedback, as has previously been studied by modulating the photonic environment for point dipoles placed both in optical cavities and near metal mirrors. In experiments involving fluorescent molecules, trapped ions and quantum dots the point nature of the dipole, its sub-unity quantum efficiency, and decoherence rate conspire to severely limit any change in total linewidth. Here we show that the transverse coherence of exciton emission in the monolayer two-dimensional (2D) material MoSe${}_2$ removes many of the fundamental physical limitations present in previous experiments. The coherent interaction between excitons and a photonic mode localized between the MoSe${}_2$ and a nearby planar mirror depends interferometrically on mirror position, enabling full control over the radiative coupling rate from near-zero to 1.8 meV and a corresponding change in exciton total linewidth from 0.9 to 2.3 meV. The highly radiatively broadened exciton resonance (a ratio of up to $3:1$ in our samples) necessary to observe this modulation is made possible by recent advances in 2D materials sample fabrication. Our method of mirror translation is free of any coupling to strain or DC electric field in the monolayer, which allows a fundamental study of this photonic effect. The weak coherent driving field in our experiments yields a mean excitation occupation number of ${\sim} 10^{-3}$ such that our experiments correspond to probing radiative reaction in the regime of perturbative quantum electrodynamics. This system will serve as a testbed for exploring new excitonic physics and quantum nonlinear optical effects.
We analyse the interaction of exciton and exciton-polariton condensates in semiconductor microcavity with a coherent acoustic wave. An analytical solution for the dispersion of excitations of coupled condensate-phonon system is found in the approximation of k-independent interactions. Accounting for k-dependence results in a stronger modification of the dispersion, and even in the appearance of the "roton instability" region.
Coherent excitation of materials via ultrafast laser pulses can have interesting, observable dynamics in time-resolved photoemission measurements. The broad spectral width of ultrafast pump pulses can coherently excite multiple exciton energy levels. When such coherently excited states are probed by means of photoemission spectroscopy, interference between the polarization of different exciton levels can lead to observable coherent exciton beats. Here, we present the theoretical formalism for evaluating the Time- and Angle- Resolved Photoemission Spectra (tr-ARPES) arising from the coherently …
Dark excitons are of fundamental importance in a broad range of contexts, but are difficult to study using conventional optical spectroscopy due to their weak interaction with light. We show how coherent multidimensional spectroscopy can reveal and characterize dark states. Using this approach, we identify different types of dark excitons in InGaAs/GaAs quantum wells and determine details regarding lifetimes, homogeneous and inhomogeneous linewidths, broadening mechanisms and coupling strengths. The observations of coherent coupling between bright and dark excitons hint at a role for a multi-s…
Coherent coupling between excitons is at the heart of many-body interactions with transition metal dichalcogenide (TMD) heterostructures as an emergent platform for the investigation of these interactions. We employ multi-dimensional coherent spectroscopy on monolayer MoSe\textsubscript{2}/WSe\textsubscript{2} heterostructures and observe coherent coupling between excitons spatially localized in monolayer MoSe$_2$ and WSe$_2$. Through many-body spectroscopy, we further observe the absorption state arising from free interlayer electron-hole pairs. This observation yields a spectroscopic measure…
Chirality is a fundamental asymmetry phenomenon, with chiral optical elements exhibiting asymmetric response in reflection or absorption of circularly polarized light. Recent realizations of such elements include nanoplasmonic systems with broken mirror symmetry and polarization-contrasting optical absorption known as circular dichroism. An alternative route to circular dichroism is provided by spin-valley polarized excitons in atomically thin semiconductors. In the presence of magnetic fields, they exhibit an imbalanced coupling to circularly polarized photons and thus circular dichroism. Her…
The use of ultra-short laser pulses to pump and probe materials activates a wealth of processes which involve the coherent and non coherent dynamics of interacting electrons out of equilibrium. Non equilibrium (NEQ) many body perturbation theory (MBPT) offers an equation of motion for the density-matrix of the system which well describes both coherent and non coherent processes. In the non correlated case there is a clear relation between these two regimes and the matrix elements of the density-matrix. The same is not true for the correlated case, where the potential binding of electrons and h…
We perform coherent nonlinear spectroscopy of excitons in single-layers of MoSe$_2$ and WSe$_2$ encapsulated between thin films of hexagonal boron nitride. Employing four-wave mixing microscopy we identify virtually disorder free areas, generating exciton optical response at the homogeneous limit. Focussing on such areas, we measure exciton homogeneous broadening as a function of environmental factors, namely temperature and exciton density. Exploiting FWM imaging, we find that at such locations, nonlinear absorption of the exciton excited states and their coherent couplings can be observed. U…
Quantifying and controlling the coherent dynamics and couplings of optically active excitations in solids is of paramount importance in fundamental research in condensed matter optics and for their prospective optoelectronic applications in quantum technologies. Here, we perform ultrafast coherent nonlinear spectroscopy of a charge-tunable MoSe$_2$ monolayer. The experiments show that the homogeneous and inhomogeneous line width and the population decay of exciton complexes hosted by this material can be directly tuned by an applied gate bias, which governs the Fermi level and therefore the fr…
We develop a model of the coherent exciton spin-valley dynamics in two-dimensional transition metal dichalcogenides under elastic strain. The strain splits the exciton radiative doublet in linearly polarized states. Consequently, it induces an effective magnetic field acting on the exciton pseudospin and causes its precession. As a result, under circularly polarized excitation, the circular polarization of excitons oscillates with time, also a time-oscillating linear polarization appears. We study competition of the strain-induced effective magnetic field with the field caused by the exciton l…
Quantifying the spin-spin interactions which influence electronic transitions in organic semiconductors is crucial for understanding their magneto-optoelectronic properties. By combining a theoretical model for three spin interactions in the coherent regime with pulsed electrically detected magnetic resonance experiments on MEH-PPV diodes, we quantify the spin-coupling within complexes comprising three spin-half particles. We determine that these particles form triplet-exciton:polaron pairs, where the polaron:exciton exchange is over 5 orders of magnitude weaker (less than 170 MHz) than that w…
Polarization-dependent two-dimensional Fourier-transform spectroscopy (2DFTS) 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 (HH) and light-hole (LH) valence states, leading to an observed splitting of the associated excitons at low temperature. Increasing the strain increases the magnitude of the HH/LH exciton peak splitting, induces an asymmetry in the off-diagonal coherences, increases the difference in the HH and LH exciton homogenous linewidths, and increases the…
The possibility of electrical manipulation and detection of charged exciton (trion) before its radiative recombination makes it promising for excitonic devices. Using a few-layer graphene/monolayer WS$_{2}$/monolayer graphene vertical heterojunction, we report inter-layer charge transport from top few-layer graphene to bottom monolayer graphene, mediated by coherently formed trion state. This is achieved by using a resonant excitation and varying the sample temperature, the resulting change in the WS$_{2}$ bandgap allows us to scan the excitation around the exciton-trion spectral overlap with …
Increasing the speed limits of conventional electronics requires innovative approaches to manipulate other quantum properties of electrons besides their charge. An alternative approach utilizes the valley degree of freedom in low-dimensional semiconductors. Here we demonstrate that the valley degeneracy of exciton energies in transition metal dichalcogenide monolayers may be lifted by coherent optical interactions on timescales corresponding to few tens of femtoseconds. The optical Stark and Bloch-Siegert effects generated by strong nonresonant circularly-polarized light induce valley-selectiv…
In this study we analyze the transmission spectrum of a thin plate of Cuprous Oxide in the range of the absorption of the yellow exciton states with the coherent transfer matrix method. We demonstrate that, in contrast to the usual analysis using Beer's law, which turns out to be a rather good approximation only in the spectral region of high principal quantum numbers, a consistent quantitative description over the whole spectral range under consideration is possible. This leads to new and more accurate parameters not only for the Rydberg exciton states, but also for the strengths of indirect …
We propose a theory of interference contributions to the two-dimensional exciton diffusion coefficient. The theory takes into account four spin states of the heavy-hole exciton. An interplay of the single particle, electron and hole, spin splittings with the electron-hole exchange interaction gives rise to either localization or antilocalization behavior of excitons depending on the system parameters. Possible experimental manifestations of exciton interference are discussed.
Sum-over-states vs quasiparticle pictures of coherent correlation spectroscopy of excitons in semiconductors; femtosecond analogues of multidimensional NMR
The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron-hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton-trion coupling and conversion phenomena. In this work, we reveal the coherent and incoherent nature of exciton-trion coupling and the relevant timescales in monolayer MoSe2 using optical two-dimensional coherent spectroscopy. Coherent interaction between excitons a…
Two-dimensional (2D) magnetic semiconductors feature both tightly-bound excitons with large oscillator strength and potentially long-lived coherent magnons due to the presence of bandgap and spatial confinement. While magnons and excitons are energetically mismatched by orders of magnitude, their coupling can lead to efficient optical access to spin information. Here we report strong magnon-exciton coupling in the 2D van der Waals (vdW) antiferromagnetic (AFM) semiconductor CrSBr. Coherent magnons launched by above-gap excitation modulate the interlayer hybridization, which leads to dynamic mo…
In many physical systems, there are specific electronic states called dark state that are protected from the rapid radiative decay imposed by the system symmetry. Although their long-lived nature indicates their potential for quantum information and spintronic applications, their high stability comes at the expense of optical accessibility. Breaking the symmetry by using magnetic and electric fields has been employed to hybridize dark and bright states thus making them optically active, but high-frequency and on-chip operation remains to be developed. Here we demonstrate the strain-induced coh…
The recent accessibility of high quality, charge neutral monolayer transition metal dichalcogenides with narrow exciton linewidths at the homogeneous limit provides an ideal platform to study excitonic many-body interactions. In particular, the possibility to manipulate coherent exciton-exciton interactions, which govern the ultrafast nonlinear optical response, by applying an external magnetic field has not been considered so far. We address this discrepancy by presenting a nonlinear microscopic theory in the coherent limit for optical excitations in the presence of out-of-plane, in-plane, an…
The dephasing mechanisms of p-shell and s-shell excitons in an InAs self-assembled quantum dot ensemble are examined using two-dimensional coherent spectroscopy (2DCS). 2DCS provides a comprehensive picture of how the energy level structure of dots affects the exciton dephasing rates and recombination lifetimes. We find that at low temperatures, dephasing of s-shell excitons is lifetime limited, whereas p-shell excitons exhibit significant pure dephasing due to scattering between degenerate spin states. At elevated temperatures, quadratic exciton-phonon coupling plays an important role in both…
Nonreciprocal perfect Coulomb drag in electron-hole bilayers: coherent exciton superflow as a diode
Tsung-Dao Lee Institute & School of Physics and Astronomy, Shanghai Jiao Tong University（上海交大李政道研究所与物理与天文学院）；Shanghai Branch, Hefei National Laboratory（合肥国家实验室上海分部）
We review the topic of Bose-Einstein condensation of excitons in semiconductors, focusing on the signatures of the macroscopic order of the exciton condensate.
We report quantum coherent oscillations of photocapacitance of a double-barrier resonant tunneling heterostructure with bias at 10 K. Periodic presence and absence of sharp excitonic transitions in photocapacitance spectra with increasing bias demonstrate strong coupling between InAs quantum dots (0D) and triangular GaAs quantum well (2D). Coherent resonant tunneling in this 0D-2D heterostructure establishes the momentum space narrowing of excitonic Bose-Einstein Condensation. Drastic increase of indirect exciton densities below 70 K reveal that excitonic wave functions anchored with each InAs…
We study the coherent dynamics of localized excitons in 100-periods of 2.5 nm thick (In,Ga)N/GaN quantum wells with 7.5% indium concentration, measured with spectroscopic resolution through two-pulse and three-pulse photon echoes at the temperature of 1.5 K. A long-lived coherent exciton dynamics is observed in the (In,Ga)N quantum wells: When the laser photon energy is tuned across the 43 meV-wide inhomogeneously broadened resonance line, the coherence time T2 varies between 45 and 255 ps, increasing with stronger exciton localization. The corresponding narrow homogeneous linewidths ranging f…
Transient four-wave mixing studies of bulk GaAs under conditions of broad bandwidth excitation of primarily interband transitions have enabled four-particle correlations tied to degenerate (exciton-exciton) and nondegenerate (exciton-carrier) interactions to be studied. Real two-dimensional Fourier-transform spectroscopy (2DFTS) spectra reveal a complex response at the heavy-hole exciton emission energy that varies with the absorption energy, ranging from dispersive on the diagonal, through absorptive for low-energy interband transitions to dispersive with the opposite sign for interband trans…
Microwave-to-optical transduction using magnon-exciton coupling in a layered antiferromagnet
City College of New York（纽约市立学院）；Graduate Center of the City University of New York (CUNY)（纽约市立大学研究生中心）；CUNY Advanced Science Research Center（纽约市立大学高级科学研究中心）；University of Chemistry and Technology Prague（布拉格化工大学）；Columbia University（哥伦比亚大学）；University of Chicago（芝加哥大学）；Rheinland-Pfälzische Technische Universität（莱茵兰-普法尔茨科技大学）
Motivated by recent experimental measurement of the intrinsic excitonic wave-function in 2D Transition-metal dichalcogenides (TMDs) by angle-resolved photoemission spectroscopy (ARPES), we developed a theoretical study to resolve some characteristics of these excitons and some of the many open issues in these systems. The system is assumed to be embedded in an environment with average dielectric constant, below which electrostatic interactions in the corresponding TMD layer are screened. We adopt the long range approximation, which gives the electron-hole interaction in the Rytova - Keldysh fo…
We demonstrate theoretically and experimentally that the nonlinear interaction between excitations whose harmonic energies coincide gives rise to a strong coupling that opens a new coherent ultrafast energy relaxation path. Instead of an incoherent decay of excitations, that should take a finite time that depends on the energy difference between the initial state and the final state, the nonlinear interaction allows their coherent superposition and thus an instantaneous transfer of the excitation over energies as large as the electron-volt. Such a situation should be encountered in many system…
Strong spin-orbit coupling and inversion symmetry breaking in transition metal dichalcogenide monolayers yield the intriguing effects of valley-dependent optical selection rules. As such, it is possible to substantially polarize valley excitons with chiral light and furthermore create coherent superpositions of K and K- polarized states. Yet, at ambient conditions dephasing usually becomes too dominant, and valley coherence typically is not observable. Here, we demonstrate that valley coherence is, however, clearly observable for a single monolayer of WSe2, if it is strongly coupled to the opt…
Long-range and fast transport of coherent excitons is important for development of high-speed excitonic circuits and quantum computing applications. However, most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities, as there are large inhomogeneous broadening and dephasing effects on the exciton transport in their native states of the materials. Here, by confining coherent excitons at the 2D quantum limit, we firstly observed molecular aggregation enabled super-transport of excitons in atomically thin two-dimensional (2D) organic…
In this work we demonstrate theoretically how to use external laser field to control the population inversion of a single quantum dot exciton qubit in a nanocavity. We consider the Jaynes-Cummings model to describe the system, and the incoherent losses were take into account by using Lindblad operators. We have demonstrated how to prepare the initial state in a superposition of the exciton in the ground state and the cavity in a coherent state. The effects of exciton-cavity detuning, the laser-cavity detunings, the pulse area and losses over the qubit dynamics are analyzed. We also show how to…
Using femtosecond pump-probe spectroscopy, we identify excitation induced dephasing as a major mechanism responsible for the breaking of the strong-coupling between excitons and photons in a semiconductor microcavity. The effects of dephasing are observed on the transmitted probe pulse spectrum as a density dependent broadening of the exciton-polariton resonances and the emergence of a third resonance at high excitation density. A striking asymmetry in the energy shift between the upper and the lower polaritons is also evidenced. Using the excitonic Bloch equations, we quantify the respective …
We study optically the coherent evolution of trions and excitons in a $δ$-doped 3.5 nm-thick ZnO/Zn$_{0.91}$Mg$_{0.09}$O multiple quantum well by means of time-resolved four-wave mixing at temperature of 1.5~K. Employing spectrally narrow picosecond laser pulses in the $χ^{(3)}$ regime allows us to address differently localized trion and exciton states, thereby avoiding many-body interactions and excitation-induced dephasing. The signal in the form of photon echoes from the negatively charged A excitons (T$_\text{A}$, trions) decays with coherence times varying from 8 up to 60~ps, depending on…
The condensation of half-light half-matter exciton polaritons in semiconductor optical cavities is a striking example of macroscopic quantum coherence in a solid state platform. Quantum coherence is possible only when there are strong interactions between the exciton polaritons provided by their excitonic constituents. Rydberg excitons with high principle value exhibit strong dipole-dipole interactions in cold atoms. However, polaritons with the excitonic constituent that is an excited state, namely Rydberg exciton polaritons (REPs), have not yet been experimentally observed. Here, for the fir…
The collective decay of excitons from initial Bose-Einstein condensate state is investigated theoretically. As practically more interesting case we consider excitons of the yellow series in the semiconductor cuprous oxide where we have collective photon and phonon assisted decay of excitons. It is shown that because of intrinsic instability of recoilless two-boson decay of Bose-Einstein condensate, the spontaneously emitted bosonic pairs are amplified leading to an exponential buildup of a macroscopic population into the certain modes. The collective decay rate has a nonlinear dependence on th…
