Johannes Feist

Delay in Photoemission

Defining Time-Zero When a high-energy photon hits an atom and is absorbed, the result can be the excitation and emission of an electron. This photoemission, or photoelectric effect, is generally assumed to occur instantaneously, and represents the definition of “time-zero” in clocking such ultrafast events. Schultze et al. (p. 1658, see the cover; see the Perspective by van der Hart) use ultrafast spectroscopy, with light pulses on the time scale of several tens of attoseconds, to test this assumption directly. They excite neon atoms with 100 eV photons and find that there is a small (20-attosecond) time delay between the emission of electrons from the 2s and 2p orbitals of the atoms. These results should have implications in modeling electron dynamics occurring on ultrafast time scales. Ultrafast metrology reveals a 20-attosecond delay between photoemission from different electronic orbitals in neon atoms. Photoemission from atoms is assumed to occur instantly in response to incident radiation and provides the basis for setting the zero of time in clocking atomic-scale electron motion. We used attosecond metrology to reveal a delay of 21±5 attoseconds in the emission of electrons liberated from the 2p orbitals of neon atoms with respect to those released from the 2s orbital by the same 100–electron volt light pulse. Small differences in the timing of photoemission from different quantum states provide a probe for modeling many-electron dynamics. Theoretical models refined with the help of attosecond timing metrology may provide insight into electron correlations and allow the setting of the zero of time in atomic-scale chronoscopy with a precision of a few attoseconds.

Coupling a Single Trapped Atom to a Nanoscale Optical Cavity

Trapped and Coupled Trapped single atoms are ideal for storing and manipulating quantum information. Thompson et al. (p. 1202, published online 25 April; see the Perspective by Keller) were able to control single atoms interacting coherently with a field mode of a photonic crystal cavity. An optical tweezer was used to trap the single atom, which enabled positioning of the atom in close proximity to the photonic crystal waveguide, coupling the atom to the optical mode of the cavity. Such coupling should prove useful in quantum measurement, sensing, and information processing. A single rubidium atom is positioned in close proximity to an optical cavity so they can interact. [Also see Perspective by Keller] Hybrid quantum devices, in which dissimilar quantum systems are combined in order to attain qualities not available with either system alone, may enable far-reaching control in quantum measurement, sensing, and information processing. A paradigmatic example is trapped ultracold atoms, which offer excellent quantum coherent properties, coupled to nanoscale solid-state systems, which allow for strong interactions. We demonstrate a deterministic interface between a single trapped rubidium atom and a nanoscale photonic crystal cavity. Precise control over the atoms position allows us to probe the cavity near-field with a resolution below the diffraction limit and to observe large atom-photon coupling. This approach may enable the realization of integrated, strongly coupled quantum nano-optical circuits.

Radiative heat transfer in the extreme near field

Radiative transfer of energy at the nanometre length scale is of great importance to a variety of technologies including heat-assisted magnetic recording, near-field thermophotovoltaics and lithography. Although experimental advances have enabled elucidation of near-field radiative heat transfer in gaps as small as 20–30 nanometres (refs 4, 5, 6), quantitative analysis in the extreme near field (less than 10 nanometres) has been greatly limited by experimental challenges. Moreover, the results of pioneering measurements differed from theoretical predictions by orders of magnitude. Here we use custom-fabricated scanning probes with embedded thermocouples, in conjunction with new microdevices capable of periodic temperature modulation, to measure radiative heat transfer down to gaps as small as two nanometres. For our experiments we deposited suitably chosen metal or dielectric layers on the scanning probes and microdevices, enabling direct study of extreme near-field radiation between silica–silica, silicon nitride–silicon nitride and gold–gold surfaces to reveal marked, gap-size-dependent enhancements of radiative heat transfer. Furthermore, our state-of-the-art calculations of radiative heat transfer, performed within the theoretical framework of fluctuational electrodynamics, are in excellent agreement with our experimental results, providing unambiguous evidence that confirms the validity of this theory for modelling radiative heat transfer in gaps as small as a few nanometres. This work lays the foundations required for the rational design of novel technologies that leverage nanoscale radiative heat transfer.

Enhancement of near-field radiative heat transfer using polar dielectric thin films

Thermal radiative emission from a hot surface to a cold surface plays an important role in many applications, including energy conversion, thermal management, lithography, data storage and thermal microscopy. Recent studies on bulk materials have confirmed long-standing theoretical predictions indicating that when the gap between the surfaces is reduced to tens of nanometres, well below the peak wavelength of the blackbody emission spectrum, the radiative heat flux increases by orders of magnitude. However, despite recent attempts, whether such enhancements can be obtained in nanoscale dielectric films thinner than the penetration depth of thermal radiation, as suggested by theory, remains experimentally unknown. Here, using an experimental platform that comprises a heat-flow calorimeter with a resolution of about 100 pW (ref. 7), we experimentally demonstrate a dramatic increase in near-field radiative heat transfer, comparable to that obtained between bulk materials, even for very thin dielectric films (50-100 nm) when the spatial separation between the hot and cold surfaces is comparable to the film thickness. We explain these results by analysing the spectral characteristics and mode shapes of surface phonon polaritons, which dominate near-field radiative heat transport in polar dielectric thin films.

Extraordinary Exciton Conductance Induced by Strong Coupling

We demonstrate that exciton conductance in organic materials can be enhanced by several orders of magnitude when the molecules are strongly coupled to an electromagnetic mode. Using a 1D model system, we show how the formation of a collective polaritonic mode allows excitons to bypass the disordered array of molecules and jump directly from one end of the structure to the other. This finding could have important implications in the fields of exciton transistors, heat transport, photosynthesis, and biological systems in which exciton transport plays a key role.

Ab initio nanoplasmonics: The impact of atomic structure

We present an ab-initio study of the hybridization of localized surface plasmons in a metal nanoparticle dimer. The atomic structure, which is often neglected in theoretical studies of quantum nanoplasmonics, has a strong impact on the optical absorption properties when sub-nanometric gaps between the nanoparticles are considered. We demonstrate that this influences the hybridization of optical resonances of the dimer, and leads to significantly smaller electric field enhancements as compared to the standard jellium model. In addition we show that the corrugation of the metal surface at a microscopic scale becomes as important as other well-known quantum corrections to the plasmonic response, implying that the atomic structure has to be taken into account to obtain quantitative predictions for realistic nanoplasmonic devices.

Nanoplasmonic Lattices for Ultracold Atoms

We propose to use subwavelength confinement of light associated with the near field of plasmonic systems to create nanoscale optical lattices for ultracold atoms. Our approach combines the unique coherence properties of isolated atoms with the subwavelength manipulation and strong light-matter interaction associated with nanoplasmonic systems. It allows one to considerably increase the energy scales in the realization of Hubbard models and to engineer effective long-range interactions in coherent and dissipative many-body dynamics. Realistic imperfections and potential applications are discussed.

Cavity-induced modifications of molecular structure in the strong coupling regime

In most theoretical descriptions of collective strong coupling of organic molecules to a cavity mode, the molecules are modeled as simple two-level systems. This picture fails to describe the rich structure provided by their internal rovibrational (nuclear) degrees of freedom. We investigate a first-principles model that fully takes into account both electronic and nuclear degrees of freedom, allowing an exploration of the phenomenon of strong coupling from an entirely new perspective. First, we demonstrate the limitations of applicability of the Born-Oppenheimer approximation in strongly coupled molecule-cavity structures. For the case of two molecules, we also show how dark states, which within the two-level picture are effectively decoupled from the cavity, are indeed affected by the formation of collective strong coupling. Finally, we discuss ground-state modifications in the ultra-strong coupling regime and show that some molecular observables are affected by the collective coupling strength, while others only depend on the single-molecule coupling constant.

Thermalization and cooling of plasmon-exciton polaritons : towards quantum condensation

We present indications of thermalization and cooling of quasiparticles, a precursor for quantum condensation, in a plasmonic nanoparticle array. We investigate a periodic array of metallic nanorods covered by a polymer layer doped with an organic dye at room temperature. Surface lattice resonances of the array--hybridized plasmonic-photonic modes--couple strongly to excitons in the dye, and bosonic quasiparticles which we call plasmon-exciton polaritons (PEPs) are formed. By increasing the PEP density through optical pumping, we observe thermalization and cooling of the strongly coupled PEP band in the light emission dispersion diagram. For increased pumping, we observe saturation of the strong coupling and emission in a new weakly coupled band, which again shows signatures of thermalization and cooling.

Suppressing photochemical reactions with quantized light fields

Photoisomerization, that is, a photochemical reaction leading to a change of molecular structure after absorption of a photon, can have detrimental effects such as leading to DNA damage under solar irradiation, or as a limiting factor for the efficiency of solar cells. Here, we show that strong coupling of organic molecules to a confined light mode can be used to strongly suppress photoisomerization, as well as other photochemical reactions, and thus convert molecules that normally show fast photodegradation into photostable forms. We find this to be especially efficient in the case of collective strong coupling, where the distribution of a single excitation over many molecules and the light mode leads to a collective protection effect that almost completely suppresses the photochemical reaction.