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- ItemExcited-state relaxation of hydrated thymine and thymidine measured by liquid-jet photoelectron spectroscopy: experiment and simulation(Washington, DC : ACS Publications, 2015) Buchner, Franziska; Nakayama, Akira; Yamazaki, Shohei; Ritze, Hans-Hermann; Lübcke, AndreaTime-resolved photoelectron spectroscopy is performed on thymine and thymidine in aqueous solution to study the excited-state relaxation dynamics of these molecules. We find two contributions with sub-ps lifetimes in line with recent excited-state QM/MM molecular dynamics simulations (J. Chem. Phys.2013, 139, 214304). The temporal evolution of ionization energies for the excited ππ* state along the QM/MM molecular dynamics trajectories were calculated and are compatible with experimental results, where the two contributions correspond to the relaxation paths in the ππ* state involving different conical intersections with the ground state. Theoretical calculations also show that ionization from the nπ* state is possible at the given photon energies, but we have not found any experimental indication for signal from the nπ* state. In contrast to currently accepted relaxation mechanisms, we suggest that the nπ* state is not involved in the relaxation process of thymine in aqueous solution.
- ItemHigh-order parametric generation of coherent XUV radiation(Washington, DC : Soc., 2021) Hort, O.; Dubrouil, A.; Khokhlova, M.A.; Descamps, D.; Petit, S.; Burgy, F.; Mével, E.; Constant, E.; Strelkov, V.V.Extreme ultraviolet (XUV) radiation finds numerous applications in spectroscopy. When the XUV light is generated via high-order harmonic generation (HHG), it may be produced in the form of attosecond pulses, allowing access to unprecedented ultrafast phenomena. However, the HHG efficiency remains limited. Here we present an observation of a new regime of coherent XUV emission which has a potential to provide higher XUV intensity, vital for applications. We explain the process by high-order parametric generation, involving the combined emission of THz and XUV photons, where the phase matching is very robust against ionization. This introduces a way to use higher-energy driving pulses, thus generating more XUV photons.
- ItemDisparate ultrafast dynamics of itinerant and localized magnetic moments in gadolinium metal([London] : Nature Publishing Group UK, 2015) Frietsch, B.; Bowlan, J.; Carley, R.; Teichmann, M.; Wienholdt, S.; Hinzke, D.; Nowak, U.; Carva, K.; Oppeneer, P. M.; Weinelt, M.The Heisenberg–Dirac intra-atomic exchange coupling is responsible for the formation of the atomic spin moment and thus the strongest interaction in magnetism. Therefore, it is generally assumed that intra-atomic exchange leads to a quasi-instantaneous aligning process in the magnetic moment dynamics of spins in separate, on-site atomic orbitals. Following ultrashort optical excitation of gadolinium metal, we concurrently record in photoemission the 4f magnetic linear dichroism and 5d exchange splitting. Their dynamics differ by one order of magnitude, with decay constants of 14 versus 0.8 ps, respectively. Spin dynamics simulations based on an orbital-resolved Heisenberg Hamiltonian combined with first-principles calculations explain the particular dynamics of 5d and 4f spin moments well, and corroborate that the 5d exchange splitting traces closely the 5d spin-moment dynamics. Thus gadolinium shows disparate dynamics of the localized 4f and the itinerant 5d spin moments, demonstrating a breakdown of their intra-atomic exchange alignment on a picosecond timescale.
- ItemUniaxial stress flips the natural quantization axis of a quantum dot for integrated quantum photonics(London : Nature Publishing Group, 2018) Yuan, X.; Weyhausen-Brinkmann, F.; MartÃn-Sánchez, J.; Piredda, G.; Křápek, V.; Huo, Y.; Huang, H.; Schimpf, C.; Schmidt, O.G.; Edlinger, J.; Bester, G.; Trotta, R.; Rastelli, A.The optical selection rules in epitaxial quantum dots are strongly influenced by the orientation of their natural quantization axis, which is usually parallel to the growth direction. This configuration is well suited for vertically emitting devices, but not for planar photonic circuits because of the poorly controlled orientation of the transition dipoles in the growth plane. Here we show that the quantization axis of gallium arsenide dots can be flipped into the growth plane via moderate in-plane uniaxial stress. By using piezoelectric strain-actuators featuring strain amplification, we study the evolution of the selection rules and excitonic fine structure in a regime, in which quantum confinement can be regarded as a perturbation compared to strain in determining the symmetry-properties of the system. The experimental and computational results suggest that uniaxial stress may be the right tool to obtain quantum-light sources with ideally oriented transition dipoles and enhanced oscillator strengths for integrated quantum photonics.
- ItemHighly-efficient extraction of entangled photons from quantum dots using a broadband optical antenna(London : Nature Publishing Group, 2018) Chen, Y.; Zopf, M.; Keil, R.; Ding, F.; Schmidt, O.G.Many quantum photonic technologies require the efficient generation of entangled pairs of photons, but to date there have been few ways to produce them reliably. Sources based on parametric down conversion operate at very low efficiency per pulse due to the probabilistic generation process. Semiconductor quantum dots can emit single pairs of entangled photons deterministically but they fall short due to the extremely low-extraction efficiency. Strategies for extracting single photons from quantum dots, such as embedding them in narrowband optical cavities, are difficult to translate to entangled photons. Here, we build a broadband optical antenna with an extraction efficiency of 65% ± 4% and demonstrate a highly-efficient entangled-photon source by collecting strongly entangled photons (fidelity of 0.9) at a pair efficiency of 0.372 ± 0.002 per pulse. The high brightness achieved by our source represents a step forward in the development of optical quantum technologies.
- ItemCharge transfer to ground-state ions produces free electrons([London] : Nature Publishing Group UK, 2017) You, D.; Fukuzawa, H.; Sakakibara, Y.; Takanashi, T.; Ito, Y.; Maliyar, G G.; Motomura, K.; Nagaya, K.; Nishiyama, T.; Asa, K.; Sato, Y.; Saito, N.; Oura, M.; Schöffler, M.; Kastirke, G.; Hergenhahn, U.; Stumpf, V.; Gokhberg, K.; Kuleff, A.I.; Cederbaum, L.S.; Ueda, KInner-shell ionization of an isolated atom typically leads to Auger decay. In an environment, for example, a liquid or a van der Waals bonded system, this process will be modified, and becomes part of a complex cascade of relaxation steps. Understanding these steps is important, as they determine the production of slow electrons and singly charged radicals, the most abundant products in radiation chemistry. In this communication, we present experimental evidence for a so-far unobserved, but potentially very important step in such relaxation cascades: Multiply charged ionic states after Auger decay may partially be neutralized by electron transfer, simultaneously evoking the creation of a low-energy free electron (electron transfer-mediated decay). This process is effective even after Auger decay into the dicationic ground state. In our experiment, we observe the decay of Ne2+ produced after Ne 1s photoionization in Ne-Kr mixed clusters.
- ItemRaman gas self-organizing into deep nano-trap lattice([London] : Nature Publishing Group UK, 2016) Alharbi, M.; Husakou, A.; Chafer, M.; Debord, B.; Gérôme, F.; Benabid, F.Trapping or cooling molecules has rallied a long-standing effort for its impact in exploring new frontiers in physics and in finding new phase of matter for quantum technologies. Here we demonstrate a system for light-trapping molecules and stimulated Raman scattering based on optically self-nanostructured molecular hydrogen in hollow-core photonic crystal fibre. A lattice is formed by a periodic and ultra-deep potential caused by a spatially modulated Raman saturation, where Raman-active molecules are strongly localized in a one-dimensional array of nanometre-wide sections. Only these trapped molecules participate in stimulated Raman scattering, generating high-power forward and backward Stokes continuous-wave laser radiation in the Lamb-Dicke regime with sub-Doppler emission spectrum. The spectrum exhibits a central line with a sub-recoil linewidth as low as ∼14 kHz, more than five orders of magnitude narrower than conventional-Raman pressure-broadened linewidth, and sidebands comprising Mollow triplet, motional sidebands and four-wave mixing.
- ItemSolid-state ensemble of highly entangled photon sources at rubidium atomic transitions(London : Nature Publishing Group, 2017) Keil, R.; Zopf, M.; Chen, Y.; Höfer, B.; Zhang, J.; Ding, F.; Schmidt, O.G.Semiconductor InAs/GaAs quantum dots grown by the Stranski-Krastanov method are among the leading candidates for the deterministic generation of polarization-entangled photon pairs. Despite remarkable progress in the past 20 years, many challenges still remain for this material, such as the extremely low yield, the low degree of entanglement and the large wavelength distribution. Here, we show that with an emerging family of GaAs/AlGaAs quantum dots grown by droplet etching and nanohole infilling, it is possible to obtain a large ensemble of polarization-entangled photon emitters on a wafer without any post-growth tuning. Under pulsed resonant two-photon excitation, all measured quantum dots emit single pairs of entangled photons with ultra-high purity, high degree of entanglement and ultra-narrow wavelength distribution at rubidium transitions. Therefore, this material system is an attractive candidate for the realization of a solid-state quantum repeater - among many other key enabling quantum photonic elements.
- ItemX-ray imaging of chemically active valence electrons during a pericyclic reaction(London : Nature Publishing Group, 2014) Bredtmann, T.; Ivanov, M.; Dixit, G.Time-resolved imaging of chemically active valence electron densities is a long-sought goal, as these electrons dictate the course of chemical reactions. However, X-ray scattering is always dominated by the core and inert valence electrons, making time-resolved X-ray imaging of chemically active valence electron densities extremely challenging. Here we demonstrate an effective and robust method, which emphasizes the information encoded in weakly scattered photons, to image chemically active valence electron densities. The degenerate Cope rearrangement of semibullvalene, a pericyclic reaction, is used as an example to visually illustrate our approach. Our work also provides experimental access to the long-standing problem of synchronous versus asynchronous bond formation and breaking during pericyclic reactions.
- ItemHighly indistinguishable and strongly entangled photons from symmetric GaAs quantum dots(London : Nature Publishing Group, 2017) Huber, D.; Reindl, M.; Huo, Y.; Huang, H.; Wildmann, J.S.; Schmidt, O.G.; Rastelli, A.; Trotta, R.The development of scalable sources of non-classical light is fundamental to unlocking the technological potential of quantum photonics. Semiconductor quantum dots are emerging as near-optimal sources of indistinguishable single photons. However, their performance as sources of entangled-photon pairs are still modest compared to parametric down converters. Photons emitted from conventional Stranski-Krastanov InGaAs quantum dots have shown non-optimal levels of entanglement and indistinguishability. For quantum networks, both criteria must be met simultaneously. Here, we show that this is possible with a system that has received limited attention so far: GaAs quantum dots. They can emit triggered polarization-entangled photons with high purity (g (2) (0) = 0.002±0.002), high indistinguishability (0.93±0.07 for 2 ns pulse separation) and high entanglement fidelity (0.94±0.01). Our results show that GaAs might be the material of choice for quantum-dot entanglement sources in future quantum technologies.