Excitation-induced Dephasing Research Articles

Many-Exciton Quantum Dynamics in a Ruddlesden-Popper Tin Iodide.

We present a study on the many-body exciton interactions in a Ruddlesden-Popper tin halide, namely, (PEA)2SnI4 (PEA = phenylethylammonium), using coherent two-dimensional electronic spectroscopy. The optical dephasing times of the third-order polarization observed in these systems are determined by exciton many-body interactions and lattice fluctuations. We investigate the excitation-induced dephasing (EID) and observe a significant reduction of the dephasing time with increasing excitation density as compared to its lead counterpart (PEA)2PbI4, which we have previously reported in a separate publication [J. Chem. Phys.2020, 153, 164706]. Surprisingly, we find that the EID interaction parameter is four orders of magnitude higher in (PEA)2SnI4 than that in (PEA)2PbI4. This increase in the EID rate may be due to exciton localization arising from a more statically disordered lattice in the tin derivative. This is supported by the observation of multiple closely spaced exciton states and the broadening of the linewidth with increasing population time (spectral diffusion), which suggests a static disordered structure relative to the highly dynamic lead-halide. Additionally, we find that the exciton nonlinear coherent lineshape shows evidence of a biexcitonic state with low binding energy (<10 meV) not observed in the lead system. We model the lineshapes based on a stochastic scattering theory that accounts for the interaction with a nonstationary population of dark background excitations. Our study provides evidence of differences in the exciton quantum dynamics between tin- and lead-based Ruddlesden-Popper metal halides (RPMHs) and links them to the exciton-exciton interaction strength and the static disorder aspect of the crystalline structure.

Notch-filtered adiabatic rapid passage for optically driven quantum light sources

We present a driving scheme for solid-state quantum emitters, referred to as Notch-filtered Adiabatic Rapid Passage (NARP), that utilizes frequency-swept pulses containing a spectral hole resonant with the optical transition in the emitter. NARP enables high-fidelity state inversion and exhibits robustness to variations in the laser pulse parameters, benefits that are derived from the insensitivity of the condition for adiabatic evolution. NARP also offers the advantage of immunity to phonon-mediated excitation-induced dephasing when positively chirped control pulses are used. Our resonant driving approach could be combined with spectral filtering of the scattered pump light and photonic devices for enhanced collection efficiency to realize simultaneous high indistinguishability and brightness in single photon source applications.

Photon echo from free excitons in a CH3NH3PbI3 halide perovskite single crystal

Halide perovskites show great potential for a variety of optoelectronic applications. The presence of robust exciton resonance in these materials makes them promising for use in information photonics. In this paper, we demonstrate the possibility of writing and delayed reading of the optical coherence in halide perovskite by the spontaneous (two-pulse) photon echo in ${\mathrm{MAPbI}}_{3}$ (${\mathrm{MA}}^{+}$ = ${\mathrm{CH}}_{3}{\mathrm{NH}}_{3}^{+}$) lead-halide perovskite single crystal on picosecond time scales. The spectral and polarimetric measurements of the photon echo signal confirm the free excitonic origin of the excitation under study. Observed relatively long dephasing time, high exciton oscillator strength, and weakly pronounced excitation-induced dephasing make halide perovskites a promising media for applications.

Using the Autler-Townes and ac Stark effects to optically tune the frequency of indistinguishable single photons from an on-demand source

We describe how a coherent optical drive that is near resonant with the upper rungs of a three-level ladder system, in conjunction with a short-pulse excitation, can be used to provide a frequency-tunable source of on-demand single photons. Using an intuitive master equation model, we identify two distinct regimes of device operation: (i) for a resonant drive, the source operates using the Autler-Townes effect, and (ii) for an off-resonant drive, the source exploits the ac Stark effect. The former regime allows for a large frequency-tuning range but coherence suffers from timing jitter effects, while the latter allows for high indistinguishability and efficiency, but with a restricted tuning bandwidth due to high required drive strengths and detunings. We show how both these negative effects can be mitigated by using an optical cavity to increase the collection rate of the desired photons. We apply our general theory to semiconductor quantum dots, which have proven to be excellent single-photon sources, and find that scattering of acoustic phonons leads to excitation-induced dephasing and increased population of the higher-energy level which limits the bandwidth of frequency tuning achievable while retaining high indistinguishability. Despite this, for realistic cavity and quantum dot parameters, indistinguishabilities of over $90%$ are achievable for energy shifts of up to hundreds of $\ensuremath{\mu}\mathrm{eV}$, and near-unity indistinguishabilities for energy shifts up to tens of $\ensuremath{\mu}\mathrm{eV}$. Additionally, we clarify the often-overlooked differences between an idealized Hong-Ou-Mandel two-photon interference experiment and its usual implementation with an unbalanced Mach-Zehnder interferometer, pointing out the subtle differences in the single-photon visibility associated with these different setups.

Interacting plexcitons for designed ultrafast optical nonlinearity in a monolayer semiconductor

Searching for ideal materials with strong effective optical nonlinear responses is a long-term task enabling remarkable breakthroughs in contemporary quantum and nonlinear optics. Polaritons, hybridized light-matter quasiparticles, are an appealing candidate to realize such nonlinearities. Here, we explore a class of peculiar polaritons, named plasmon–exciton polaritons (plexcitons), in a hybrid system composed of silver nanodisk arrays and monolayer tungsten-disulfide (WS2), which shows giant room-temperature nonlinearity due to their deep-subwavelength localized nature. Specifically, comprehensive ultrafast pump–probe measurements reveal that plexciton nonlinearity is dominated by the saturation and higher-order excitation-induced dephasing interactions, rather than the well-known exchange interaction in traditional microcavity polaritons. Furthermore, we demonstrate this giant nonlinearity can be exploited to manipulate the ultrafast nonlinear absorption properties of the solid-state system. Our findings suggest that plexcitons are intrinsically strongly interacting, thereby pioneering new horizons for practical implementations such as energy-efficient ultrafast all-optical switching and information processing.

Local field effects in ultrafast light–matter interaction measured by pump-probe spectroscopy of monolayer MoSe2

Abstract Using ultrafast resonant pump-probe spectroscopy in an unconventional experimental setup we investigate the spectral shape and dynamics of absorption features related to the A exciton in an hexagonal boron nitride (hBN)/MoSe2/hBN van der Waals heterostructure. While in a pure two-level system a pump-probe experiment measures the occupation or the polarization dynamics, depending on the time ordering of the pulse pair, in the transition metal dichalcogenide (TMD) system both quantities get thoroughly mixed by strong exciton–exciton interaction. We find that for short positive delays the spectral lines experience pronounced changes in their shape and energy and they relax to the original situation on a picosecond time scale. For negative delays, distinctive spectral oscillations appear indicating the first-time observation of perturbed free induction decay for a TMD system. The comparison between co-circular and cross-circular excitation schemes further allows us to investigate the rapid inter-valley scattering. By considering a three-level system as a minimal model including the local field effect, excitation-induced dephasing (EID), and scattering between the excited states we explain all phenomena observed in the experiment with excellent consistency. Our handy model can be even further reduced to two levels in the case of a co-circular excitation, for which we derive analytic expressions to describe the detected signals. This allows us to trace back the spectral shapes and shifts to the impact of local field effect and EID thus fully reproducing the complex behavior of the observed effects.

Van der Waals heterostructure polaritons with moiré-induced nonlinearity.

Controlling matter-light interactions with cavities is of fundamental importance in modern science and technology1. This is exemplified in the strong-coupling regime, where matter-light hybrid modes form, with properties that are controllable by optical-wavelength photons2,3. By contrast, matter excitations on the nanometre scale are harder to access. In two-dimensional van der Waals heterostructures, a tunable moiré lattice potential for electronic excitations may form4, enabling the generation of correlated electron gases in the lattice potentials5-9. Excitons confined in moiré lattices have also been reported10,11, but no cooperative effects have been observed and interactions with light have remained perturbative12-15. Here, by integrating MoSe2-WS2 heterobilayers in a microcavity, we establish cooperative coupling between moiré-lattice excitons and microcavity photons up to the temperature of liquid nitrogen, thereby integrating versatile control of both matter and light into one platform. The density dependence of the moiré polaritons reveals strong nonlinearity due to exciton blockade, suppressed exciton energy shift and suppressed excitation-induced dephasing, all of which are consistent with the quantum confined nature of the moiré excitons. Such a moiré polariton system combines strong nonlinearity and microscopic-scale tuning of matter excitations using cavity engineering and long-range light coherence, providing a platform with which to study collective phenomena from tunable arrays of quantum emitters.

Stochastic scattering theory for excitation-induced dephasing: Time-dependent nonlinear coherent exciton lineshapes.

We develop a stochastic theory that treats time-dependent exciton-exciton s-wave scattering and that accounts for dynamic Coulomb screening, which we describe within a mean-field limit. With this theory, we model excitation-induced dephasing effects on time-resolved two-dimensional coherent optical lineshapes and we identify a number of features that can be attributed to the many-body dynamics occurring in the background of the exciton, including dynamic line narrowing, mixing of real and imaginary spectral components, and multi-quantum states. We test the model by means of multidimensional coherent spectroscopy on a two-dimensional metal-halide semiconductor that hosts tightly bound excitons and biexcitons that feature strong polaronic character. We find that the exciton nonlinear coherent lineshape reflects many-body correlations that give rise to excitation-induced dephasing. Furthermore, we observe that the exciton lineshape evolves with the population time over time windows in which the population itself is static in a manner that reveals the evolution of the multi-exciton many-body couplings. Specifically, the dephasing dynamics slow down with time, at a rate that is governed by the strength of exciton many-body interactions and on the dynamic Coulomb screening potential. The real part of the coherent optical lineshape displays strong dispersive character at zero time, which transforms to an absorptive lineshape on the dissipation timescale of excitation-induced dephasing effects, while the imaginary part displays converse behavior. Our microscopic theoretical approach is sufficiently flexible to allow for a wide exploration of how system-bath dynamics contribute to linear and non-linear time-resolved spectral behavior.

Stochastic scattering theory for excitation-induced dephasing: Comparison to the Anderson-Kubo lineshape.

In this paper, we present a quantum stochastic model for spectroscopic lineshapes in the presence of a co-evolving and non-stationary background population of excitations. Starting from a field theory description for interacting bosonic excitons, we derive a reduced model whereby optical excitons are coupled to an incoherent background via scattering as mediated by their screened Coulomb coupling. The Heisenberg equations of motion for the optical excitons are then driven by an auxiliary stochastic population variable, which we take to be the solution of an Ornstein-Uhlenbeck process. Itô's lemma then allows us to easily construct and evaluate correlation functions and response functions. Focusing on the linear response, we compare our model to the classic Anderson-Kubo model. While similar in motivation, there are differences in the predicted lineshapes, notably in terms of asymmetry, and variation with the increasing background population.

Exciton-Scattering-Induced Dephasing in Two-Dimensional Semiconductors.

Enhanced Coulomb interactions in monolayer transition metal dichalcogenides cause tightly bound electron-hole pairs (excitons) that dominate their linear and nonlinear optical response. The latter includes bleaching, energy renormalizations, and higher-order Coulomb correlation effects like biexcitons and excitation-induced dephasing. While the first three are extensively studied, no theoretical footing for excitation-induced dephasing in exciton-dominated semiconductors is available so far. In this Letter, we present microscopic calculations based on excitonic Heisenberg equations of motion and identify the coupling of optically pumped excitons to exciton-exciton scattering continua as the leading mechanism responsible for an optical-power-dependent linewidth broadening (excitation-induced dephasing) and sideband formation. Performing time-, momentum-, and energy-resolved simulations, we quantitatively evaluate the exciton-induced dephasing for the most common monolayer transition metal dichalcogenides and find an excellent agreement with recent experiments.

Difference in the behavior of the photon echo of excitons in InGaAs/GaAs quantum wells from the predictions of the model of two-level system ensemble

In this work, we studied the photon echo from heavy-hole excitons in a thin InGaAs/GaAs quantum well. To analyze the results, we used the model of an ensemble of two-level systems. The model allows us to describe the temporal profile and the moment of arrival of the echo signal, as well as the echo amplitude decay with increasing delay between pulses. In addition, excitation-induced dephasing effect was observed, that was beyond the limits of applicability of the model.

Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites

In two-dimensional hybrid organic-inorganic metal-halide perovskites, the intrinsic optical lineshape reflects multiple excitons with distinct binding energies, each dressed differently by the hybrid lattice. Given this complexity, a fundamentally far-reaching issue is how Coulomb-mediated many-body interactions --- elastic scattering such as excitation-induced dephasing, inelastic exciton bimolecular scattering, and multi-exciton binding --- depend upon the specific exciton-lattice coupling. We report the intrinsic and density-dependent exciton pure dephasing rates and their dependence on temperature by means of a coherent nonlinear spectroscopy. We find exceptionally strong screening effects on multi-exciton scattering relative to other two-dimensional single-atomic-layer semiconductors. Importantly, the exciton-density dependence of the dephasing rates is markedly different for distinct excitons. These findings establish the consequences of particular lattice dressing on exciton many-body quantum dynamics, which critically define fundamental optical properties that underpin photonics and quantum optoelectronics in relevant exciton density regimes.

Spatially asymmetric transients of propagating exciton-polariton modes in a planar CdZnTe/CdMgTe guiding structure

We report on ultrafast time-resolved pump-probe studies in a CdZnTe/CdMgTe planar guiding structure covered with a metallic grating. The one-dimensional periodic gold structure allows for efficient coupling into the guiding layer for $p$-polarized 30 fs optical pulses with a large spectral bandwidth of about 60 nm. The resulting spectral width of optical pulses propagating inside the guiding layer corresponds to 20--30 nm. We demonstrate that the excitation of exciton-polariton modes in the guiding layer leads to a modulation of the optical response in the vicinity of the excitonic resonance. Spatially resolved pump-probe measurements show an asymmetric behavior in the optical response when the relative position of the pump and probe spots is varied on the scale of ten micrometers perpendicular to the metal ridges. This is attributed to the excitation of resonant and off-resonant exciton-polariton modes which propagate in opposite directions inside the guiding layer in accordance with their dispersion relations. Two main mechanisms are considered and evaluated, namely, Pauli blocking and excitation-induced dephasing, which are shown to be responsible for the pump-induced changes in the exciton absorption spectrum. While both of these processes lead to the generation of photoexcited carriers in the guiding layer, their impact on the optical properties (transmission and reflection) are different which leads to the asymmetric behavior of the spatially resolved transients.

Control of the filament dynamics of 10 µm pulses via designer pulse trains

Atmospheric low-loss delivery of high-energy long wavelength picosecond duration pulses over multiple Rayleigh ranges will be dominated by the recently identified many-body coherent excitation-induced dephasing and avalanche based memory effects. We numerically illustrate this physics with pulse trains where prepulses gradually accumulate plasma preparing the medium for the main high-power pulse. The control over the nonlinear dynamics makes it possible to effectively avoid pulse splitting in the first few hundred meters, and deliver a wave packet with an improved spatiotemporal profile downstream.

Coherent dynamics of localized excitons and trions in ZnO/(Zn,Mg)O quantum wells studied by photon echoes

We study optically the coherent evolution of trions and excitons in a $\delta$-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 $\chi^{(3)}$ 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 trion energy: more strongly localized trions reveal longer coherence dynamics. The localized neutral excitons decay on the picosecond timescale with coherence times up to $T_2=4.5$~ps. The coherent dynamics of the X$_\text{B}$ exciton and T$_\text{B}$ trion are very short ($T_2<1$~ps), which is attributed to the fast energy relaxation from the trion and exciton B states to the respective A states. The trion population dynamics is characterized by the decay time $T_1$, rising from 30~ps to 100~ps with decreasing trion energy.

Damping of Rabi oscillations in intensity-dependent photon echoes from exciton complexes in a CdTe/(Cd,Mg)Te single quantum well

We study Rabi oscillations detected in the coherent optical response from various exciton complexes in a 20~nm-thick CdTe/(Cd,Mg)Te quantum well using time-resolved photon echoes. In order to evaluate the role of exciton localization and inhomogeneous broadening we use selective excitation with spectrally narrow ps-pulses. We demonstrate that the transient profile of the photon echo from the localized trion (X$^-$) and the donor-bound exciton (D$^0$X) transitions strongly depends on the strength of the first pulse. It acquires a non-Gaussian shape and experiences significant advancement for pulse areas larger than $\pi$ due to non-negligible inhomogeneity-induced dephasing of the oscillators during the optical excitation. Next, we observe that an increase of the area of either the first (excitation) or the second (rephasing) pulse leads to a significant damping of the photon echo signal, which is strongest for the neutral excitons and less pronounced for the donor-bound exciton complex (D$^0$X). The measurements are analyzed using a theoretical model based on the optical Bloch equations which accounts for the inhomogeneity of optical transitions in order to reproduce the complex shape of the photon echo transients. In addition, the spreading of Rabi frequencies within the ensemble due to the spatial variation of the intensity of the focused Gaussian beams and excitation-induced dephasing are required to explain the fading and damping of Rabi oscillations. By analyzing the results of the simulation for the X$^-$ and the D$^0$X complexes we are able to establish a correlation between the degree of localization and the transition dipole moments determined as $\mu($X$^-$)=73~D and $\mu($D$^0$X)=58~D.

Four-Wave Mixing in Perovskite Photovoltaic Materials Reveals Long Dephasing Times and Weaker Many-Body Interactions than GaAs

Perovksite semiconductors have shown promise for low-cost solar cells, lasers and photodetectors, yet their fundamental photophysical properties are not well understood. Recent observations of a low ($\sim$few meV) exciton binding energy and evidence of hot phonon effects in the room temperature phase suggest that perovskites are much closer to inorganic semiconductors than the absorber layers in traditional organic photovoltaics, signaling the need for experiments that shed light on the placement of perovskite materials within the spectrum of semiconductors used in optoelectronics and photovoltaics. Here we use four-wave mixing (FWM) to contrast the coherent optical response of CH$_3$NH$_3$PbI$_3$ thin films and crystalline GaAs. At carrier densities relevant for solar cell operation, our results show that carriers interact surprisingly weakly via the Coulomb interaction in perovskite, much weaker than in inorganic semiconductors. These weak many-body effects lead to a dephasing time in CH$_3$NH$_3$PbI$_3$ $\sim$3 times longer than in GaAs. Our results also show that the strong enhancement of the exciton FWM signal tied to excitation-induced dephasing in GaAs and other III-V semiconductors does not occur in perovskite due to weak exciton-carrier scattering interactions.

Signatures of four-particle correlations associated with exciton-carrier interactions in coherent spectroscopy on bulk GaAs

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 transitions high above band gap. Simulations using a multilevel model augmented by many-body effects provide excellent agreement with the 2DFTS experiments and indicate that excitation-induced dephasing (EID) and excitation-induced shift (EIS) affect degenerate and nondegenerate interactions equivalently, with stronger exciton-carrier coupling relative to exciton-exciton coupling by approximately an order of magnitude. These simulations also indicate that EID effects are three times stronger than EIS in contributing to the coherent response of the semiconductor.

Ultrafast dynamical response of the lower exciton-polariton branch in CdZnTe

We investigate the transient optical response in high-quality ${\mathrm{Cd}}_{0.88}{\mathrm{Zn}}_{0.12}\mathrm{Te}$ crystals in the regime of slow light propagation on the lower exciton-polariton branch. Femtosecond photoexcitation leads to very substantial transmission changes in a $\ensuremath{\sim}10$-meV broad spectral range within the transparency window of the unexcited semiconductor. These nonlinear optical signatures decay on picosecond time scales governed by carrier thermalization and recombination. The temporal and spectral dependence indicate the dynamical optical response as arising from excitation-induced dephasing and perturbed free induction decay. Model simulations for the optical response taking into account the actual exciton-polariton dispersion and excitation-induced dephasing of a nonlinearly driven two-level system support this interpretation.

Optical excitation dependent emission properties of InGaN quantum wells

Fully microscopic many-body calculations are used to study the carrier and polarization dynamics in optically excited InGaN quantum wells. For long-pulse or stationary (CW) optical excitation conditions, it is shown that the strong excitation-induced dephasing due to the excited charge carriers leads to an effective spectral width of the created polarization in the range of several hundred meV. The subsequent polarization to population conversion results in broad carrier distributions spreading over energy regions well above and below the central excitation energy. Without invoking Auger transitions, it is shown that this model can explain experiments observing ultraviolet quantum-well photoluminescence after resonant CW excitation of a neighboring green emitting quantum well Binder et al. (Appl. Phys. Lett. 103:071108, 2013).