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Author

Tomasz Jakubczyk

Bio: Tomasz Jakubczyk is an academic researcher from University of Grenoble. The author has contributed to research in topics: Quantum dot & Exciton. The author has an hindex of 13, co-authored 46 publications receiving 584 citations. Previous affiliations of Tomasz Jakubczyk include University of Warsaw & University of Bremen.


Papers
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Journal ArticleDOI
TL;DR: By implementing four-wave mixing (FWM) microspectroscopy, coherence and population dynamics of the exciton transitions in monolayers of MoSe2 are measured, revealing their dephasing times T2 and radiative lifetime T1 in a subpicosecond range and indicating radiatively limited dephase at a temperature of 6 K.
Abstract: By implementing four-wave mixing (FWM) microspectroscopy, we measure coherence and population dynamics of the exciton transitions in monolayers of MoSe2. We reveal their dephasing times T2 and radiative lifetime T1 in a subpicosecond (ps) range, approaching T2 = 2T1 and thus indicating radiatively limited dephasing at a temperature of 6 K. We elucidate the dephasing mechanisms by varying the temperature and by probing various locations on the flake exhibiting a different local disorder. At the nanosecond range, we observe the residual FWM produced by the incoherent excitons, which initially disperse toward the dark states but then relax back to the optically active states within the light cone. By introducing polarization-resolved excitation, we infer intervalley exciton dynamics, revealing an initial polarization degree of around 30%, constant during the initial subpicosecond decay, followed by the depolarization on a picosecond time scale. The FWM hyperspectral imaging reveals the doped and undoped area...

153 citations

Journal ArticleDOI
30 Apr 2018
TL;DR: In this article, a WS2 monolayer of transition metal dichalcogenides (TMDs) was studied and the dynamics of the exciton coherence was shown to be lost due to interaction with phonons and relaxation processes towards optically dark excitonic states.
Abstract: Scientific curiosity to uncover original optical properties and functionalities of atomically thin semiconductors, stemming from unusual Coulomb interactions in the two-dimensional geometry and multi-valley band structure, drives the research on monolayers of transition metal dichalcogenides (TMDs). While recent works ascertained the exotic energetic schemes of exciton complexes in TMDs, we here infer their unusual coherent dynamics occurring on subpicosecond time scale. The dynamics is largely affected by the disorder landscape on the submicron scale, thus can be uncovered using four-wave mixing in the frequency domain, which enables microscopic investigations and imaging. Focusing on a WS2 monolayer, we observe that exciton coherence is lost primarily due to interaction with phonons and relaxation processes towards optically dark excitonic states. Notably, when temperature is low and disorder weak, excitons large coherence volume results in enhanced oscillator strength, allowing to reach the regime of radiatively limited dephasing. Additionally, we observe long valley coherence for the negatively charged exciton complex. We therefore elucidate the crucial role of exciton environment in the TMDs on its dynamics and show that revealed mechanisms are ubiquitous within this family.

46 citations

Journal ArticleDOI
TL;DR: This work deterministically fabricates microlenses above selected InAs quantum dots, achieving their efficient coupling to the external light field, and consistently explains the initial coherence decay, the zero-phonon line fraction, and the line shape of the phonon-assisted PL using realistic quantum dot geometries.
Abstract: Optimized light–matter coupling in semiconductor nanostructures is a key to understand their optical properties and can be enabled by advanced fabrication techniques Using in situ electron beam lithography combined with a low-temperature cathodoluminescence imaging, we deterministically fabricate microlenses above selected InAs quantum dots (QDs), achieving their efficient coupling to the external light field This enables performing four-wave mixing microspectroscopy of single QD excitons, revealing the exciton population and coherence dynamics We infer the temperature dependence of the dephasing in order to address the impact of phonons on the decoherence of confined excitons The loss of the coherence over the first picoseconds is associated with the emission of a phonon wave packet, also governing the phonon background in photoluminescence (PL) spectra Using theory based on the independent boson model, we consistently explain the initial coherence decay, the zero-phonon line fraction, and the line

46 citations

Journal ArticleDOI
TL;DR: In this article, a radiative recombination channel of dark excitons in self-assembled quantum dots was demonstrated, which is due to a light hole admixture in the excitonic ground state.
Abstract: We demonstrate evidence for a radiative recombination channel of dark excitons in self-assembled quantum dots. This channel is due to a light hole admixture in the excitonic ground state. Its presence was experimentally confirmed by a direct observation of the dark exciton photoluminescence from a cleaved edge of the sample. The polarization-resolved measurements revealed that a photon created from the dark exciton recombination is emitted only in the direction perpendicular to the growth axis. Strong correlation between the dark exciton lifetime and the in-plane hole $g$ factor enabled us to show that the radiative recombination is a dominant decay channel of the dark excitons in CdTe/ZnTe quantum dots.

41 citations

Journal ArticleDOI
08 Feb 2019-ACS Nano
TL;DR: It is found that the exciton dynamics is governed by microscopic disorder on top of the ideal crystal properties, which provides stable monolayer samples with low disorder, avoiding surface contaminations and the resulting exciton broadening and modifications of the dynamics.
Abstract: 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 ar...

36 citations


Cited by
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Journal ArticleDOI
01 Jan 1977-Nature
TL;DR: Bergh and P.J.Dean as discussed by the authors proposed a light-emitting diode (LEDD) for light-aware Diodes, which was shown to have promising performance.
Abstract: Light-Emitting Diodes. (Monographs in Electrical and Electronic Engineering.) By A. A. Bergh and P. J. Dean. Pp. viii+591. (Clarendon: Oxford; Oxford University: London, 1976.) £22.

1,560 citations

Journal ArticleDOI
TL;DR: In this article, the authors reviewed recent progress in understanding of the excitonic properties in monolayer transition metal dichalcogenides (TMDs) and future challenges are laid out.
Abstract: Atomically thin materials such as graphene and monolayer transition metal dichalcogenides (TMDs) exhibit remarkable physical properties resulting from their reduced dimensionality and crystal symmetry. The family of semiconducting transition metal dichalcogenides is an especially promising platform for fundamental studies of two-dimensional (2D) systems, with potential applications in optoelectronics and valleytronics due to their direct band gap in the monolayer limit and highly efficient light-matter coupling. A crystal lattice with broken inversion symmetry combined with strong spin-orbit interactions leads to a unique combination of the spin and valley degrees of freedom. In addition, the 2D character of the monolayers and weak dielectric screening from the environment yield a significant enhancement of the Coulomb interaction. The resulting formation of bound electron-hole pairs, or excitons, dominates the optical and spin properties of the material. Here recent progress in understanding of the excitonic properties in monolayer TMDs is reviewed and future challenges are laid out. Discussed are the consequences of the strong direct and exchange Coulomb interaction, exciton light-matter coupling, and influence of finite carrier and electron-hole pair densities on the exciton properties in TMDs. Finally, the impact on valley polarization is described and the tuning of the energies and polarization observed in applied electric and magnetic fields is summarized.

1,234 citations

Journal Article
TL;DR: This work shows that the spectral distribution and time-dependent decay of light emitted from excitons confined in the quantum dots are controlled by the host photonic crystal, providing a basis for all-solid-state dynamic control of optical quantum systems.
Abstract: Control of spontaneously emitted light lies at the heart of quantum optics. It is essential for diverse applications ranging from miniature lasers and light-emitting diodes, to single-photon sources for quantum information, and to solar energy harvesting. To explore such new quantum optics applications, a suitably tailored dielectric environment is required in which the vacuum fluctuations that control spontaneous emission can be manipulated. Photonic crystals provide such an environment: they strongly modify the vacuum fluctuations, causing the decay of emitted light to be accelerated or slowed down, to reveal unusual statistics, or to be completely inhibited in the ideal case of a photonic bandgap. Here we study spontaneous emission from semiconductor quantum dots embedded in inverse opal photonic crystals. We show that the spectral distribution and time-dependent decay of light emitted from excitons confined in the quantum dots are controlled by the host photonic crystal. Modified emission is observed over large frequency bandwidths of 10%, orders of magnitude larger than reported for resonant optical microcavities. Both inhibited and enhanced decay rates are observed depending on the optical emission frequency, and they are controlled by the crystals’ lattice parameter. Our experimental results provide a basis for all-solid-state dynamic control of optical quantum systems.

1,019 citations

Journal ArticleDOI
TL;DR: The latest quantum dot-based single-Photon sources are edging closer to the ideal single-photon source, and have opened new possibilities for quantum technologies.
Abstract: Single photons are a fundamental element of most quantum optical technologies. The ideal single-photon source is an on-demand, deterministic, single-photon source delivering light pulses in a well-defined polarization and spatiotemporal mode, and containing exactly one photon. In addition, for many applications, there is a quantum advantage if the single photons are indistinguishable in all their degrees of freedom. Single-photon sources based on parametric down-conversion are currently used, and while excellent in many ways, scaling to large quantum optical systems remains challenging. In 2000, semiconductor quantum dots were shown to emit single photons, opening a path towards integrated single-photon sources. Here, we review the progress achieved in the past few years, and discuss remaining challenges. The latest quantum dot-based single-photon sources are edging closer to the ideal single-photon source, and have opened new possibilities for quantum technologies.

828 citations

Journal ArticleDOI
TL;DR: In this article, the authors show that encapsulation of monolayer MoS2 in hexagonal boron nitride can efficiently suppress the inhomogeneous contribution to the exciton linewidth, as they measure in photoluminescence and reflectivity a FWHM down to 2 meV at T=4
Abstract: The strong light-matter interaction and the valley selective optical selection rules make monolayer (ML) MoS2 an exciting 2D material for fundamental physics and optoelectronics applications. But, so far, optical transition linewidths even at low temperature are typically as large as a few tens of meV and contain homogeneous and inhomogeneous contributions. This prevented in-depth studies, in contrast to the better-characterized ML materials MoSe2 and WSe2. In this work, we show that encapsulation of ML MoS2 in hexagonal boron nitride can efficiently suppress the inhomogeneous contribution to the exciton linewidth, as we measure in photoluminescence and reflectivity a FWHM down to 2 meV at T=4 K. Narrow optical transition linewidths are also observed in encapsulated WS2, WSe2, and MoSe2 MLs. This indicates that surface protection and substrate flatness are key ingredients for obtaining stable, high-quality samples. Among the new possibilities offered by the well-defined optical transitions, we measure the homogeneous broadening induced by the interaction with phonons in temperature-dependent experiments. We uncover new information on spin and valley physics and present the rotation of valley coherence in applied magnetic fields perpendicular to the ML.

540 citations