KEYWORDSPerovskite, nanocrystals, quantum dots, four wave mixing, photon echo, coherence, T2, phonons, lead halide, heterodyne detection 2 ABSTRACT Fully-inorganic cesium lead halide perovskite nanocrystals (NCs) have shown to exhibit outstanding optical properties such as wide spectral tunability, high quantum yield, high oscillator strength as well as blinking-free single photon emission and low spectral diffusion. Here, we report measurements of the coherent and incoherent exciton dynamics on the 100 fs to 10 ns timescale, determining dephasing and density decay rates in these NCs. The experiments are performed on CsPbBr2Cl NCs using transient resonant three-pulse four-wave mixing (FWM) in heterodyne detection at temperatures ranging from 5 K to 50 K. We found a low-temperature exciton dephasing time of 24.5±1.0 ps, inferred from the decay of the photon-echo amplitude at 5 K, corresponding to a homogeneous linewidth (FWHM) of 54±5 eV. Furthermore, oscillations in the photon-echo signal on a picosecond timescale are observed and attributed to coherent coupling of the exciton to a quantized phonon mode with 3.45 meV energy. TEXT Recently, a new type of colloidal nanocrystals (NCs) has emerged for opto-electronic applications which combines simplicity in synthesis with great spectral flexibility and exceptional optical properties. Fully inorganic cesium lead halide perovskite NCs (CsPbX3, where X = Cl, Br, I or mixture thereof) 1,2 have shown outstanding optical properties such as wide spectral tunability and high oscillator strength. 3 These NCs can be synthesized with precise compositional and size control, and show room-temperature photoluminescence (PL) quantum yields (QY) of 60 -90% (ref. 1). Moreover, perovskite NCs have attracted a lot of interest due to their large absorption coefficient and gain for optically pumped lasing devices. 4 At cryogenic temperatures, the PL decay is mostly radiative with lifetimes in the few hundred picosecond range, depending on size and

We measure the coherent nonlinear response of excitons in a single layer of molybdenum disulfide embedded in hexagonal boron nitride, forming a h-BN/MoS2/h-BN heterostructure. Using four-wave mixing microscopy and imaging, we correlate the exciton inhomogeneous broadening with the homogeneous one and population lifetime. We find that the exciton dynamics is governed by microscopic disorder on top of the ideal crystal properties. Analyzing the exciton ultrafast density dynamics using amplitude and phase of the response, we investigate the relaxation pathways of the resonantly driven exciton population. The surface protection via encapsulation provides stable monolayer samples with low disorder, avoiding surface contaminations and the resulting exciton broadening and modifications of the dynamics. We identify areas localized to a few microns where the optical response is totally dominated by homogeneous broadening. Across the sample of tens of micrometers, weak inhomogeneous broadening and strain effects are observed, attributed to the remaining interaction with the h-BN and imperfections in the encapsulation process.

We report on the exciton and trion density dynamics in a single layer of MoSe2, resonantly excited and probed using three-pulse four-wave mixing (FWM), at temperatures from 300 K to 77 K . A multi-exponential third-order response function for amplitude and phase of the heterodyne-detected FWM signal including four decay processes is used to model the data. We provide a consistent interpretation within the intrinsic band structure, not requiring the inclusion of extrinsic effects. We find an exciton radiative lifetime in the sub-picosecond range consistent to what has been recently reported 1 . After the dominating radiative decay, the remaining exciton density, which has been scattered from the initially excited bright radiative state into dark states of different nature by exciton-phonon scattering or disorder scattering, shows a slower dynamics, covering 10ps to 10ns timescales. This includes direct bright transitions with larger in-plane momentum, as well as indirect dark transitions to indirect dark states. We find that exciton-exciton annihilation is not relevant in the observed dynamics, in variance from previous finding under non-resonant excitation. The trion density at 77 K reveals a decay of the order of 1 ps, similar to what is observed for the exciton. After few tens of picoseconds, the trion dynamics resembles the one of the exciton, indicating that trion ionization occurs on this timescale.

The fine structure of exciton states in colloidal quantum dots (QDs) results from the compound effect of anisotropy and electron-hole exchange. By means of single-dot photoluminescence spectroscopy, we show that the emission of photo-excited InP/ZnSe QDs originates from radiative recombination of such fine-structure exciton states. Depending on the excitation power, we identify a bright exciton doublet, a trion singlet and a biexciton doublet line that all show a pronounced polarization. Fluorescence line 1 narrowing spectra of an ensemble of InP/ZnSe QDs in magnetic fields demonstrate that the bright exciton effectively consists of three states. The Zeeman splitting of these states is well described by an isotropic exciton model, where the fine structure is dominated by electron-hole exchange and shape anisotropy only leads to a minor splitting of the F = 1 triplet. We argue that excitons in InP-based QDs are nearly isotropic because the particular ratio of light and heavy hole masses in InP makes the exciton fine structure insensitive to shape anisotropy.

Spontaneous emission from excitonic transitions in InAs/GaAs quantum dots embedded in photonic crystal waveguides at 5 K into non-guided and guided modes is determined by direct hyperspectral imaging. This enables measurement of the absolute coupling efficiency into the guided modes, the beta factor, directly, without assumptions on decay rates used previously. Notably, we found beta factors above 90% over a wide spectral range of 40 meV in the fast light regime, reaching a maximum of (99 ± 1)%. We measure the directional emission of the circularly polarized transitions in a magnetic field into counter-propagating guided modes, to deduce the mode circularity at the quantum dot sites. We find that points of high directionality, up to 97%, correlate with a reduced beta factor consistent with their positions away from the mode field antinode. By comparison with calibrated finite-difference time-domain simulations, we use the emission energy, mode circularity and beta factor to estimate the quantum dot position inside the photonic crystal waveguide unit cell.

Decoherence or dephasing of the exciton is a central characteristic of a quantum dot (QD) that determines the minimum width of the exciton emission line and the purity of indistinguishable photon emission during exciton recombination. Here, we analyze exciton dephasing in colloidal InP/ ZnSe QDs using transient four-wave mixing spectroscopy. We obtain a dephasing time of 23 ps at a temperature of 5 K, which agrees with the smallest line width of 50 μeV we measure for the exciton emission of single InP/ZnSe QDs at 5 K. By determining the dephasing time as a function of temperature, we find that exciton decoherence can be described as a phononinduced, thermally activated process. The deduced activation energy of 0.32 meV corresponds to the small splitting within the nearly isotropic bright exciton triplet of InP/ZnSe QDs, suggesting that the dephasing is dominated by phonon-induced scattering within the bright exciton triplet.

No abstract

No abstract