At cryogenic temperature and at the single emitter level, the optical properties of single-wall carbon nanotubes depart drastically from that of a one-dimensional (1D) object. In fact, the (usually ...unintentional) localization of excitons in local potential wells leads to nearly 0D behaviors such as photon antibunching, spectral diffusion, inhomogeneous broadening, etc. Here, we present a hyperspectral imaging of this spontaneous exciton localization effect at the single nanotube level using a super-resolved optical microscopy approach. We report on the statistical distribution of the trap localization, depth, and width. We use a quasi-resonant photoluminescence excitation approach to probe the confined quantum states. Numerical simulations of the quantum states and exciton diffusion show that the excitonic states are deeply modified by the interface disorder inducing a remarkable discretization of the excitonic absorption spectrum and a quenching of the free 1D exciton absorption.
The narrow emission of a single carbon nanotube at low temperature is coupled to the optical mode of a fiber microcavity using the built-in spatial and spectral matching brought by this flexible ...geometry. A thorough cw and time-resolved investigation of the very same emitter both in free space and in cavity shows an efficient funneling of the emission into the cavity mode together with a strong emission enhancement corresponding to a Purcell factor of up to 5. At the same time, the emitted photons retain a strong sub-Poissonian statistics. By exploiting the cavity feeding effect on the phonon wings, we locked the emission of the nanotube at the cavity resonance frequency, which allowed us to tune the frequency over a 4 THz band while keeping an almost perfect antibunching. By choosing the nanotube diameter appropriately, this study paves the way to the development of carbon-based tunable single-photon sources in the telecom bands.
The performance of hybrid organic perovskite (HOP) for solar energy conversion is driving a renewed interest in their light emitting properties. The recent observation of broad visible emission in ...layered HOP highlights their potential as white-light emitters. Improvement of the efficiency of the material requires a better understanding of its photophysical properties. We present in-depth experimental investigations of white-light (WL) emission in thin films of the (C6H11NH3)2PbBr4. The broadband, strongly Stokes shifted emission presents a maximum at 90 K when excited at 3.815 eV, and below this temperature coexists with an excitonic edge emission. X-rays and calorimetry measurements exclude the existence of a phase transition as an origin of the thermal behavior of the WL luminescence. The free excitonic emission quenches at low temperature, despite a binding energy estimated to 280 meV. Time-resolved photoluminescence spectroscopy reveals the multicomponent nature of the broad emission. We analyzed the dependence of these components as a function of temperature and excitation energy. The results are consistent with the existence of self-trapped states. The quenching of the free exciton and the thermal evolution of the WL luminescence decay time are explained by the existence of an energy barrier against self-trapping, estimated to ∼10 meV.
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 microcavity, 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.
The performance of hybrid organic perovskite (HOP) for solar energy conversion is driving a renewed interest in their light emitting properties. The recent observation of broad visible emission in ...layered HOP highlights their potential as white-light emitters. Improvement of the efficiency of the material requires a better understanding of its photophysical properties. We present in-depth experimental investigations of white-light (WL) emission in thin films of the (C6H11NH3)(2)PbBr4. The broadband, strongly Stokes shifted emission presents a maximum at 90 K when excited at 3.815 eV, and below this temperature coexists with an excitonic edge emission. X-rays and calorimetry measurements exclude the existence of a phase transition as an origin of the thermal behavior of the WL luminescence. The free excitonic emission quenches at low temperature, despite a binding energy estimated to 280 meV. Time-resolved photoluminescence spectroscopy reveals the multicomponent nature of the broad emission. We analyzed the dependence of these components as a function of temperature and excitation energy. The results are consistent with the existence of self-trapped states. The quenching of the free exciton and the thermal evolution of the WL luminescence decay time are explained by the existence of an energy barrier against self-trapping, estimated to similar to 10 meV.
We present evidence of near-infrared photoluminescence (PL) signature of nitrogen vacancy centers (N sub(C) V sub(Si))? in silicon carbide (SiC). This center exhibits an S=1 ground state spin similar ...to the NV? center in diamond. We have performed photoluminescence excitation measurements at cryogenic temperature and demonstrated efficient photoexcitation of distinct photoluminescence from (N sub(C) V sub(Si))? in 4H-SiC. Furthermore, by correlating the energies of measured zero phonon lines (ZPLs) with theoretical values derived from hybrid density functional theory each of the ZPLs has been associated to the respective occupation of hexagonal (h) and quasicubic (k) lattice sites in close analogy to neutral divacancy centers (V sub(C) V sub(Si)) super(0) in the same material. Finally, with the appropriate choice of excitation energy we demonstrated the selective excitation of (N sub(C) V sub(Si))? PL with no contamination by (VCVSi)0 PL, thereby opening the way towards the optical detection of (N sub(C) V sub(Si))? electron spin resonance.
At low temperature the photoluminescence of single-wall carbon nanotubes show a large variety of spectral profiles ranging from ultranarrow 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, multipeak luminescence profiles with specific temperature dependence show the presence of confined phonon modes.
Single-walled carbon nanotubes provide an ideal system for studying the properties of one-dimensional (1D) materials, where strong electron-electron interactions are expected. Optical measurements ...have recently reported the existence of excitons in semiconducting nanotubes, revealing the importance of many-body effects. Surprisingly, pioneering electronic structure calculations and scanning tunnelling spectroscopy (STS) experiments report the same gap values as optical experiments. Here, an experimental STS study of the bandgap of single-walled semiconducting nanotubes, demonstrates a continuous transition from the gap reduced by the screening resulting from the metal substrate to the intrinsic gap dominated by many-body interactions. These results provide a deeper knowledge of many-body interactions in these 1D systems and a better understanding of their electronic properties, which is a prerequisite for any application of nanotubes in the ultimate device miniaturization for molecular electronics, or spintronics.
The Electron Ion Collider (EIC) collaboration and future experiment is a unique scientific ecosystem within Nuclear Physics as the experiment starts right off as a crosscollaboration between ...Brookhaven National Lab (BNL) & Jefferson Lab (JLab). As a result, this muti-lab computing model tries at best to provide services accessible from anywhere by anyone who is part of the collaboration. While the computing model for the EIC is not finalized, it is anticipated that the computational and storage resources will be made accessible to a wide range of collaborators across the world. The use of federated ID seems to be a critical element to the strategy of providing such services, allowing seamless access to each lab site computing resources. However, providing Federated access to a Federated storage is not a trivial matter and has its share of technical challenges. In this contribution, we focus on the steps we took towards the deployment of a distributed object storage system that integrates with Amazon S3 and Federated ID. We will first cover for and explain the first stage storage solutions provided to the EIC during the detector design phase. Our initial test deployment consisted of Lustre storage using MinIO, hence providing an S3 interface. High Availability load balancers were added later to provide the initial scalability it lacked. Performance of that system will be shown. While this embryonic solution worked well, it had many limitations. Looking ahead, the Ceph object storage is considered a top-of-the-line solution in the storage community - since the Ceph Object Gateway is compatible with the Amazon S3 API out of the box, our next phase will use a native S3 storage. Our Ceph deployment will consist of erasure coded storage nodes to maximize storage potential along with multiple Ceph Object Gateways for redundant access. We will compare performance of our next stage implementations. Finally, we will present how to leverage OpenID Connect with the Ceph Object Gateway’s to enable Federated ID access. We hope this contribution will serve the community needs as we move forward with cross-lab collaborations and the need for Federated ID access to distributed compute facilities.
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