Sebastien Couet

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.

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.

BEOL compatible high tunnel magneto resistance perpendicular magnetic tunnel junctions using a sacrificial Mg layer as CoFeB free layer cap

Perpendicularly magnetized MgO-based tunnel junctions are envisaged for future generation spin-torque transfer magnetoresistive random access memory devices. Achieving a high tunnel magneto resistance and preserving it together with the perpendicular magnetic anisotropy during BEOL CMOS processing are key challenges to overcome. The industry standard technique to deposit the CoFeB/MgO/CoFeB tunnel junctions is physical vapor deposition. In this letter, we report on the use of an ultrathin Mg layer as free layer cap to protect the CoFeB free layer from sputtering induced damage during the Ta electrode deposition. When Ta is deposited directly on CoFeB, a fraction of the surface of the CoFeB is sputtered even when Ta is deposited with very low deposition rates. When depositing a thin Mg layer prior to Ta deposition, the sputtering of CoFeB is prevented. The ultra-thin Mg layer is sputtered completely after Ta deposition. Therefore, the Mg acts as a sacrificial layer that protects the CoFeB from sputter-indu...

Time-Resolved Ultrathin Cobalt Film Growth on a Colloidal Polymer Template

Cobalt (Co) sputter deposition onto a colloidal polymer template is investigated using grazing incidence small-angle X-ray scattering (GISAXS), scanning electron microscopy (SEM), and atomic force microscopy (AFM). SEM and AFM data picture the sample topography, GISAXS the surface and near-surface film structure. A two-phase model is proposed to describe the time evolution of the Co growth. The presence of the colloidal template results in the correlated deposition of an ultrathin Co film on the sample surface and thus in the creation of Co capped polystyrene (PS) colloids. Well below the percolation threshold, the radial growth is restricted and only height growth is observed.

A compact UHV deposition system for in situ study of ultrathin films via hard x-ray scattering and spectroscopy

We report on a compact ultrahigh vacuum deposition system developed for in situ experiments using hard x rays. The chamber can be mounted on various synchrotron beamlines for spectroscopic as well as scattering experiments in grazing incidence geometry. The deposition process is completely remotely controlled and an ellipsometer is available for online monitoring of the layer growth process. The unique sample position in the chamber allows one to perform deposition, grazing incidence x-ray experiments, and ellipsometry measurements at the same time, enabling to correlate the x-ray analysis with parameters of the growth process. Additionally, the setup can be used to study in situ chemical and structural changes in an element specific manner by x-ray absorption spectroscopy. The flexibility and versatility of the system brings new possibilities to study the chemistry and structure of surfaces and interfaces in thin films systems during their formation.

Thin Co/Ni-based bottom pinned spin-transfer torque magnetic random access memory stacks with high annealing tolerance

Spin-transfer torque magnetic random access memory (STT-MRAM) is considered as a replacement for next generation embedded and stand-alone memory applications. One of the main challenges in the STT-MRAM stack development is the compatibility of the stack with CMOS process flows in which thermal budgets up to 400 °C are applied. In this letter, we report on a perpendicularly magnetized MgO-based tunnel junction (p-MTJ) on a thin Co/Ni perpendicular synthetic antiferromagnetic layer with high annealing tolerance. Tunnel magneto resistance (TMR) loss after annealing occurs when the reference layer loses its perpendicular magnetic anisotropy due to reduction of the CoFeB/MgO interfacial anisotropy. A stable Co/Ni based p-MTJ stack with TMR values of 130% at resistance-area products of 9 Ω μm2 after 400 °C anneal is achieved via moment control of the Co/Ta/CoFeB reference layer. Thinning of the CoFeB polarizing layer down to 0.8 nm is the key enabler to achieve 400 °C compatibility with limited TMR loss. Thinning the Co below 0.6 nm leads to a loss of the antiferromagnetic interlayer exchange coupling strength through Ru. Insight into the thickness and moment engineering of the reference layer is displayed to obtain the best magnetic properties and high thermal stability for thin Co/Ni SAF-based STT-MRAM stacks.

Time-resolved spin-torque switching in MgO-based perpendicularly magnetized tunnel junctions

We study ns scale spin-torque-induced switching in perpendicularly magnetized tunnel junctions (pMTJ). Although the switching voltages match with the macrospin instability threshold, the electrical signatures of the reversal indicate the presence of domain walls in junctions of various sizes. In the antiparallel (AP) to parallel (P) switching, a nucleation phase is followed by an irreversible flow of a wall through the sample at an average velocity of 40 m/s with back and forth oscillation movements indicating a Walker propagation regime. A model with a single-wall locally responding to the spin-torque reproduces the essential dynamical signatures of the reversal. The P to AP transition has a complex dynamics with dynamical back-hopping whose probability increases with voltage. We attribute this back-hopping to the instability of the nominally fixed layers.