151 research outputs found
Exploiting one-dimensional exciton-phonon coupling for tunable and efficient single-photon generation with a carbon nanotube
Condensed-matter emitters offer enriched cavity quantum electrodynamical
effects due to the coupling to external degrees of freedom. In the case of
carbon nanotubes a very peculiar coupling between localized excitons and the
one-dimensional acoustic phonon modes can be achieved, which gives rise to
pronounced phonon wings in the luminescence spectrum. By coupling an individual
nanotube to a tunable optical micro-cavity, we show that this peculiar
exciton-phonon coupling is a valuable resource to enlarge the tuning range of
the single-photon source while keeping an excellent exciton-photon coupling
efficiency and spectral purity. Using the unique flexibility of our scanning
fiber cavity, we are able to measure the efficiency spectrum of the very same
nanotube in the Purcell regime for several mode volumes. Whereas this
efficiency spectrum looks very much like the free-space luminescence spectrum
when the Purcell factor is small (large mode volume), we show that the
deformation of this spectrum at lower mode volumes can be traced back to the
strength of the exciton-photon coupling. It shows an enhanced efficiency on the
red wing that arises from the asymmetry of the incoherent energy exchange
processes between the exciton and the cavity. This allows us to obtain a tuning
range up to several hundred times the spectral width of the source
Unifying the low-temperature photoluminescence spectra of carbon nanotubes: the role of acoustic phonon confinement
At low temperature the photoluminescence of single-wall carbon nanotubes show
a large variety of spectral profiles ranging from ultra narrow lines in
suspended nanotubes to broad and asymmetrical line-shapes that puzzle the
current interpretation in terms of exciton-phonon coupling. Here, we present a
complete set of photoluminescence profiles in matrix embedded nanotubes
including unprecedented narrow emission lines. We demonstrate that the
diversity of the low-temperature luminescence profiles in nanotubes originates
in tiny modifications of their low-energy acoustic phonon modes. When low
energy modes are locally suppressed, a sharp photoluminescence line as narrow
as 0.7 meV is restored. Furthermore, multi-peak luminescence profiles with
specific temperature dependence show the presence of confined phonon modes
Measuring many-body effects in carbon nanotubes with a scanning tunneling microscope
Electron-electron interactions and excitons in carbon nanotubes are locally
measured by combining Scanning tunneling spectroscopy and optical absorption in
bundles of nanotubes. The largest gap deduced from measurements at the top of
the bundle is found to be related to the intrinsic quasi-particle gap. From the
difference with optical transitions, we deduced exciton binding energies of 0.4
eV for the gap and 0.7 eV for the second Van Hove singularity. This provides
the first experimental evidence of substrate-induced gap renormalization on
SWNTs
Chirality dependence of the absorption cross-section of carbon nanotubes
The variation of the optical absorption of carbon nanotubes with their
geometry has been a long standing question at the heart of both metrological
and applicative issues, in particular because optical spectroscopy is one of
the primary tools for the assessment of the chiral species abundance of
samples. Here, we tackle the chirality dependence of the optical absorption
with an original method involving ultra-efficient energy transfer in
porphyrin/nanotube compounds that allows uniform photo-excitation of all chiral
species. We measure the absolute absorption cross-section of a wide range of
semiconducting nanotubes at their S22 transition and show that it varies by up
to a factor of 2.2 with the chiral angle, with type I nanotubes showing a
larger absorption. In contrast, the luminescence quantum yield remains almost
constant
Environmental effect on the carrier dynamics in carbon nanotubes
Carrier dynamics is investigated in both luminescent and non luminescent samples of single wall carbon nanotubes -obtained by laser ablation- by means of two-color pump-probe experiments. The recombination dynamics is monitored by probing the transient photobleaching observed on the interband transitions of semi-conducting nanotubes. Interband and inter-subband relaxation times are about one order of magnitude slower in isolated nanotubes than in ropes of nanotubes bringing evidence of the environment influence on the carrier dynamics. The relaxation dynamics is non-exponential and is interpreted as a consequence of the inhomogeneity of the sample. Slow components up to 250 ps are measured which is significantly greater than values previoulsy reported in HiPCo nanotubes. These observations show the great dependence of the electronic properties of carbon nanotubes on the synthesis method and on their environment
Solid-State Physics Perspective on Hybrid Perovskite Semiconductors
International audienceIn this review we examine recent theoretical investigations on 2D and 3D hybrid perovskites (HOP) that combine classical solid-state physics concepts and density functional theory (DFT) simulations as a tool for studying their optoelectronic properties. Such an approach allows one to define a new class of semiconductors, where the pseudocubic high temperature perovskite structure plays a central role. Bloch states and k.p Hamiltonians yield new insight into the influence of lattice distortions, including loss of inversion symmetry, as well as spin-orbit coupling. Electronic band folding and degeneracy, effective masses and optical absorption are analyzed. Concepts of Bloch and envelope functions, as well as confinement potential are discussed in the context of layered HOP and 3D HOP heterostructures. Screening and dielectric confinements are important for room temperature optical properties of 3D and layered HOP, respectively. Non-radiative Auger effects are analyzed for the first time close to the electronic band gap of 3D hybrid perovskites
Elastic exciton-exciton scattering in photoexcited carbon nanotubes
International audienceWe report on original nonlinear spectral hole-burning experiments in single wall carbon nanotubes that bring evidence of pure dephasing induced by exciton-exciton scattering. We show that the collision-induced broadening in carbon nanotubes is controlled by exciton-exciton scattering as for Wannier excitons in inorganic semiconductors, while the population relaxation is driven by exciton-exciton annihilation as for Frenkel excitons in organic materials. We demonstrate that this singular behavior originates from the intrinsic one-dimensionality of excitons in carbon nanotubes, which display unique hybrid features of organic and inorganic systems
Ultrafast carrier dynamics in single-wall carbon nanotubes
Time-resolved carrier dynamics in single wall carbon nanotubes is investigated by means of two-color pump-probe experiments. The recombination dynamics is monitored by probing the transient photo-bleaching observed on the first interband transition of the semi-conducting tubes. The carrier dynamics takes place on a one picosecond time scale which is one order of magnitude slower than in graphite. Transient photo-induced absorption is observed with exactly the same dynamics for non-resonant probe conditions and is interpreted as a global red shift of the plasmon resonance. We show that the opening of the band gap in semi-conducting carbon nanotubes determines the non-linear response dynamics over the whole visible and near-infrared spectrum
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