Transform-Limited Photon Emission from a Lead-Vacancy Center in Diamond above 10 K.

Transform-limited photon emission from quantum emitters is essential for high-fidelity entanglement generation. In this Letter, we report the coherent optical property of a single negatively charged lead-vacancy (PbV) center in diamond. Photoluminescence excitation measurements reveal stable fluorescence with a linewidth of 39 MHz at 6 K, close to the transform limit estimated from the lifetime measurement. We observe 4 orders of magnitude different linewidths of the two zero-phonon lines, and find that the phonon-induced relaxation in the ground state contributes to this huge difference in the linewidth. Because of the suppressed phonon absorption in the PbV center, we observe nearly transform-limited photon emission up to 16 K, demonstrating its high temperature robustness compared to other color centers in diamond.

Revealing the Origin of Fast Delayed Fluorescence in a Donor Functionalized Bisterpyridine.

A new carbazole-substituted bisterpyridine with pronounced delayed fluorescence is presented. While the molecular donor-acceptor-donor design suggests the origin of this to be thermally activated delayed fluorescence (TADF), results from various photophysical characterizations, OLED characteristics, temperature-dependent NMR spectroscopy, and DFT calculations all point against the involvement of triplet states. The molecule exhibits blue emission at about 440 nm with two or more fast decay channels in the lower nanosecond range in both solution and thin films. The delayed emission is proposed to be caused by rotational vibrational modes. We suggest that these results are generally applicable, especially for more complex molecules, and should be considered as alternative or competitive emissive relaxation pathways in the field of organic light emitting materials.

Ionization potentials of MgN (N = 7-56) clusters formed by spontaneous collapse of magnesium foam in helium nanodroplets.

The ionization potentials of magnesium clusters (MgN, N = 7-56) are determined by doping ultracold helium nanodroplets (HeM, M ≈ 52 000) with Mg atoms. Inspecting the particle size distributions resulting from non-resonant, short-wavelength, single-photon ionization gives evidence that beyond a certain ensemble size, the developing foam structure undergoes a spontaneous collapse on the way to the laser interaction region. As a result, hot Mg clusters form in the relaxation process. The spontaneous collapse manifests in a substantial change in the size distributions, when recording mass spectra at wavelengths shorter than 272 nm. Tracing individual MgN signals as a function of laser photon energy allows extraction of size-specific ionization potentials, which for small clusters show a good agreement with results obtained from density functional theory simulations. The further development is compared to calculations based on the liquid drop model. However, even when quantum effects are included, the simple scaling law is not able to reproduce the development of the ionization potentials. The results suggest that small neutral magnesium clusters behave as non-metallic. The comparison to electron affinities and band gaps obtained from photoemission experiments on MgN- provides information on the charge state dependence of the non-metal-to-metal transition and properties like the Mulliken electron negativity.

Phase-of-the-Phase Electron Momentum Spectroscopy on Single Metal Atoms in Helium Nanodroplets.

Magnesium atoms fully embedded in helium nanodroplets are exposed to two-color laser pulses, which trigger multiphoton above-threshold ionization (ATI). This allows exemplary study of the contribution of a dense, neutral, and finite medium on single electron propagation. The angular-resolved photoelectron spectra show striking differences with respect to results obtained on free atoms. Scattering of the individual Mg photoelectrons, when traversing the neutral helium environment, causes the angular distribution to become almost isotropic. Furthermore, the appearance of higher-energy electrons is observed, indicating the impact of the droplet on the concerted emission process. Phase-of-the-phase spectroscopy, however, reveals a marked loss in the 2ω-ω phase dependence of the electron signal. Taking into account sideband formation on a quantitative level, a Monte Carlo simulation which includes laser-assisted electron scattering can reproduce the experimental spectra and give insights into the strong-field-induced electron emission from disordered systems.

Photoelectron Spectroscopy on Magnesium Ensembles in Helium Nanodroplets.

The electronic properties of magnesium embedded in helium nanodroplets are investigated as a function of the doping level by combining resonant two-photon ionization with photoelectron spectroscopy. Photon absorption near the atomic 31P1 ← 31S0 transition triggers the dynamics, which is probed on a nanosecond timescale by the subsequent absorption of the ionizing photon. Striking similarities in the photoelectron spectra for different doping levels and the population of atomic states well beyond 31P1 evidence an energy release process being relevant for a wide range of droplet sizes and doping conditions. From the statistical analysis, one can infer that instead of a single compact cluster size, a loosely bound Mg atom ensemble is responsible for the resulting spectra.

Comparison of Electron and Ion Emission from Xenon Cluster-Induced Ignition of Helium Nanodroplets.

The charging dynamics of helium droplets driven by embedded xenon cluster ignition in strong laser fields is studied by comparing the abundances of helium and highly charged Xe ions to the electron signal. Femtosecond pump-probe experiments show that near the optimal delay for highly charged xenon the electron yield increases, especially at low energies. The electron signature can be traced back to the ionization of the helium environment by Xe seed electrons. Accompanying molecular dynamics simulations suggest a two-step ionization scenario in the Xe-He core-shell system. In contrast to xenon, the experimental signal of the helium ions, as well as low-energy electron emission show a deviating delay dependence, indicating differences in the temporal and spacial development of the charge state distribution of Xe core and He surrounding. From the pump-probe dependence of the electron emission, effective temperatures can be extracted, indicating the nanoplasma decay.

Efficient laser-driven proton acceleration from cylindrical and planar cryogenic hydrogen jets.

We report on recent experimental results deploying a continuous cryogenic hydrogen jet as a debris-free, renewable laser-driven source of pure proton beams generated at the 150 TW ultrashort pulse laser Draco. Efficient proton acceleration reaching cut-off energies of up to 20 MeV with particle numbers exceeding 109 particles per MeV per steradian is demonstrated, showing for the first time that the acceleration performance is comparable to solid foil targets with thicknesses in the micrometer range. Two different target geometries are presented and their proton beam deliverance characterized: cylindrical (∅ 5 µm) and planar (20 µm × 2 µm). In both cases typical Target Normal Sheath Acceleration emission patterns with exponential proton energy spectra are detected. Significantly higher proton numbers in laser-forward direction are observed when deploying the planar jet as compared to the cylindrical jet case. This is confirmed by two-dimensional Particle-in-Cell (2D3V PIC) simulations, which demonstrate that the planar jet proves favorable as its geometry leads to more optimized acceleration conditions.

Formation of coherent rotational wavepackets in small molecule-helium clusters using impulsive alignment.

We show that rotational line spectra of molecular clusters with near zero permanent dipole moments can be observed using impulsive alignment. Aligned rotational wavepackets were generated by non-resonant interaction with intense femtosecond laser pump pulses and then probed using Coulomb explosion by a second, time-delayed femtosecond laser pulse. By means of a Fourier transform a rich spectrum of rotational eigenstates was derived. For the smallest cluster, C(2)H(2)-He, we were able to establish essentially all rotational eigenstates up to the dissociation threshold on the basis of theoretical level predictions. The C(2)H(2)-He complex is found to exhibit distinct features of large amplitude motion and very early onset of free internal rotor energy level structure.