Ralf Röhlsberger

Collective Lamb Shift in Single-Photon Superradiance

All Together Now An atom, when excited, will typically decay with a characteristic decay time. An ensemble of atoms, collectively coupled together with just one of the atoms excited will conspire to decay much faster than the single atom case. This enhancement of light-matter interaction is known as superradiance. Röhlsberger et al. (p. 1248, published online 13 May; see the cover; see the Perspective by Scully and Svidzinsky) present the realization of an artificial superradiant system comprising resonant iron atoms embedded in a semiconductor cavity and excited by synchrotron radiation and report the signature collective Lamb shift expected from the cooperative interaction and enhanced decay rate. The availability of such a controlled system to look closer at this effect should shed light on its role in natural and complex light-harvesting systems, and possibly allow the production of more efficient solar cells. Superradiance is observed from an ensemble of iron atoms excited by synchrotron radiation. Superradiance, the cooperative spontaneous emission of photons from an ensemble of identical atoms, provides valuable insights into the many-body physics of photons and atoms. We show that an ensemble of resonant atoms embedded in the center of a planar cavity can be collectively excited by synchrotron radiation into a purely superradiant state. The collective coupling of the atoms via the radiation field leads to a substantial radiative shift of the transition energy, the collective Lamb shift. We simultaneously measured the temporal evolution of the superradiant decay and the collective Lamb shift of resonant 57Fe nuclei excited with 14.4–kilo–electron volt synchrotron radiation. Our experimental technique provides a simple method for spectroscopic analysis of the superradiant emission.

In Situ GISAXS Study of Gold Film Growth on Conducting Polymer Films

The growth of a thin gold film on a conducting polymer surface from nucleation to formation of a continuous layer with a thickness of several nanometers is investigated in situ with grazing incidence small-angle X-ray scattering (GISAXS). Time resolution is achieved by performing the experiment in cycles of gold deposition on poly(N-vinylcarbazole) (PVK) and subsequently recording the GISAXS data. The 2D GISAXS patterns are simulated, and morphological parameters of the gold film on PVK such as the cluster size, shape, and correlation distance are extracted. For the quantitative description of the cluster size evolution, scaling laws are applied. The time evolution of the cluster morphology is explained with a growth model, suggesting a cluster growth proceeding in four steps, each dominated by a characteristic kinetic process: nucleation, lateral growth, coarsening, and vertical growth. A very limited amount of 6.5 wt % gold is observed to be incorporated inside a 1.2-nm-thick enrichment layer in the PVK film.

Electromagnetically induced transparency with resonant nuclei in a cavity

The manipulation of light–matter interactions by quantum control of atomic levels has had a profound impact on optical sciences. Such manipulation has many applications, including nonlinear optics at the few-photon level, slow light, lasing without inversion and optical quantum information processing. The critical underlying technique is electromagnetically induced transparency, in which quantum interference between transitions in multilevel atoms renders an opaque medium transparent near an atomic resonance. With the advent of high-brilliance, accelerator-driven light sources such as storage rings or X-ray lasers, it has become attractive to extend the techniques of optical quantum control to the X-ray regime. Here we demonstrate electromagnetically induced transparency in the regime of hard X-rays, using the 14.4-kiloelectronvolt nuclear resonance of the Mössbauer isotope iron-57 (a two-level system). We exploit cooperative emission from ensembles of the nuclei, which are embedded in a low-finesse cavity and excited by synchrotron radiation. The spatial modulation of the photonic density of states in a cavity mode leads to the coexistence of superradiant and subradiant states of nuclei, respectively located at an antinode and a node of the cavity field. This scheme causes the nuclei to behave as effective three-level systems, with two degenerate levels in the excited state (one of which can be considered metastable). The radiative coupling of the nuclear ensembles by the cavity field establishes the atomic coherence necessary for the cancellation of resonant absorption. Because this technique does not require atomic systems with a metastable level, electromagnetically induced transparency and its applications can be transferred to the regime of nuclear resonances, establishing the field of nuclear quantum optics.

In situ GISAXS Investigation of Gold Sputtering onto a Polymer Template

Microphase-separation structures in mixed diblock-triblock copolymer thin films are used for the incorporation of gold atoms inside the polymer matrix via sputtering of gold. Polystyrene (PS) spheres are arranged in a liquidlike type with a well defined nearest neighbor distance inside a polyisoprene matrix acting as a template for directing the gold atoms. Sputtering conditions are selected with a very low sputtering rate to avoid clustering in the atmosphere so that gold reaches the polymer surface in its atomic state. Due to the mobility of the gold atoms and the selective interaction with the PS parts of the microphase separation structure, gold is accumulated inside the polymer film in the PS spheres, as probed in situ with grazing incidence small-angle X-ray scattering (GISAXS). Nominally 4.3 A of gold is deposited, which by diffusion is spread out vertically over a thickness of 280 nm. UV-vis spectroscopy reveals a small blue shift for the gold sputtered polymer film. Atomic force microscopy proves the absence of gold clusters on the film surface. For low sputtering rate, GISAXS proves good sensitivity for gold migration inside the polymer film and opens new possibilities for studying polymer-metal interaction.

Cobalt nanoparticles growth on a block copolymer thin film: a time-resolved GISAXS study.

Cobalt sputter deposition on a nanostructured polystyrene-block-poly(ethylene oxide), P(S-b-EO), template is followed in real time with grazing incidence small-angle X-ray scattering (GISAXS). The polymer template consists of highly oriented parallel crystalline poly(ethylene oxide) (PEO) domains that are sandwiched between two polystyrene (PS) domains. In-situ GISAXS shows that cobalt atoms selectively decorate the PS domains of the microphase-separated polymer film and then aggregate to form surface metal nanopatterns. The polymer template is acting as a directing agent where cobalt metal nanowires are formed. At high metal load, the characteristic selectivity of the template is lost, and a uniform metal layer forms on the polymer surface. During the early stage of cobalt metal deposition, a highly asymmetric nanoparticles agglomeration is dominating structure formation. The cobalt nanoparticles mobility in combination with the high tendency of the nanoparticles to coalescence and to form immobile large-sized particles at the PS domains are discussed as mechanisms of structure formation.

Growth and morphology of sputtered aluminum thin films on P3HT surfaces.

Growth and morphology of an aluminum (Al) contact on a poly(3-hexylthiophene) (P3HT) thin film are investigated with X-ray methods and related to the interactions at the Al:P3HT interface. Grazing incidence small-angle scattering (GISAXS) is applied in situ during Al sputter deposition to monitor the growth of the layer. A growth mode is found, in which the polymer surface is wetted and rapidly covered with a continuous layer. This growth type results in a homogeneous film without voids and is explained by the strong chemical interaction between Al and P3HT, which suppresses the formation of three-dimensional cluster structures. A corresponding three stage growth model (surface bonding, agglomeration, and layer growth) is derived. X-ray reflectivity shows the penetration of Al atoms into the P3HT film during deposition and the presence of a 2 nm thick intermixing layer at the Al:P3HT interface.

Vacuum-assisted generation and control of atomic coherences at x-ray energies.

The control of light-matter interaction at the quantum level usually requires coherent laser fields. But already an exchange of virtual photons with the electromagnetic vacuum field alone can lead to quantum coherences, which subsequently suppress spontaneous emission. We demonstrate such spontaneously generated coherences (SGC) in a large ensemble of nuclei operating in the x-ray regime, resonantly coupled to a common cavity environment. The observed SGC originates from two fundamentally different mechanisms related to cooperative emission and magnetically controlled anisotropy of the cavity vacuum. This approach opens new perspectives for quantum control, quantum state engineering and simulation of quantum many-body physics in an essentially decoherence-free setting.

Phonon damping in thin films of Fe

The phonon density of states (DOS) in thin films of polycrystalline α-Fe was measured by inelastic nuclear resonant scattering of synchrotron radiation. The thin-film DOS exhibits significant deviations from the DOS of bulk Fe, which we attribute to phonon lifetime broadening in the confined geometry. The measured DOS can be described with a damped harmonic oscillator model for the phonons with different quality factors Q=25(2) and Q=13(1) for layer thicknesses of 28 and 13 nm, respectively.

X-ray quantum optics

Quantum optics with X-rays has long been a somewhat exotic activity, but it is now rapidly becoming relevant as precision x-ray optics and novel X-ray light sources, and high-intensity lasers are becoming available. This article gives an overview of the current state of the field and an outlook to future prospects.

Technical Report: PETRA III: DESY's New High Brilliance Third Generation Synchrotron Radiation Source

At present, the storage ring DORIS III (4.5 GeV, 150 mA) serves as the main source for synchrotron radiation experiments at DESY. DORIS III is a second generation storage ring with a rather large emittance of 404 nmrad, thus producing high flux X-ray beams of comparatively low brilliance. In order to follow the increasing user request for high brilliance beams, DESY will rebuild the storage ring PETRA into a very low emittance synchrotron radiation source called PETRA III. PETRA (positron electron tandem ring accelerator) is a storage ring with 2.304 km circumference, which was built in 1976 as an e+ - e− collider. Currently PETRA is used as a pre-accelerator for the proton-lepton collider HERA. In parallel it also serves one undulator beamline in parasitic mode.