Engineering Papers⌕ Search

Engineering topics

Lienau, Christoph

Publications and source records attributed to Lienau, Christoph.

6 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Plasmon mediated coherent population oscillations in molecular aggregates

The strong coherent coupling of quantum emitters to vacuum fluctuations of the light field offers opportunities for manipulating the optical and transport properties of nanomaterials, with potential applications ranging from ultrasensitive all-optical switching to creating polariton condensates. Often, ubiquitous decoherence processes at ambient conditions limit these couplings to such short time scales that the quantum dynamics of the interacting system remains elusive. Prominent examples are strongly coupled exciton-plasmon systems, which, so far, have mostly been investigated by linear optical spectroscopy. Here, we use ultrafast two-dimensional electronic spectroscopy to probe the quantum dynamics of J-aggregate excitons collectively coupled to the spatially structured plasmonic fields of a gold nanoslit array. We observe rich coherent Rabi oscillation dynamics reflecting a plasmon-driven coherent exciton population transfer over mesoscopic distances at room temperature. This opens up new opportunities to manipulate the coherent transport of matter excitations by coupling to vacuum fields.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Charge Delocalization and Vibronic Couplings in Quadrupolar Squaraine Dyes

Squaraines are prototypical quadrupolar charge-transfer chromophores that have recently attracted much attention as building blocks for solution-processed photovoltaics, fluorescent probes with large two-photon absorption cross sections, and aggregates with large circular dichroism. Their optical properties are often rationalized in terms of phenomenological essential state models, considering the coupling of two zwitterionic excited states to a neutral ground state. As a result, optical transitions to the lowest S 1 excited state are one-photon allowed, whereas the next higher S 2 state can only be accessed by two-photon transitions. A further implication of these models is a substantial reduction of vibronic coupling to the ubiquitous high-frequency vinyl-stretching modes of organic materials. Here, in this study, we combine time-resolved vibrational spectroscopy, two-dimensional electronic spectroscopy, and quantum-chemical simulations to test and rationalize these predictions for nonaggregated molecules. We find small Huang–Rhys factors below 0.01 for the high-frequency, 1500 cm –1 modes in particular, as well as a noticeable reduction for those of lower frequency modes in general for the electronic S 0 → S 1 transition. The two-photon allowed state S 2 is well separated energetically from S 1 and has weak vibronic signatures as well. Thus, the resulting pronounced concentration of the oscillator strength in a narrow region relevant to the lowest electronic transition makes squaraines and their aggregates exceptionally interesting for strong and ultrastrong coupling of excitons to localized light modes in external resonators with chiral properties that can largely be controlled by the molecular architecture.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Roadmap on plasmonics

Explore the source record for details and available documents.

solar (photovoltaic), solid state lighting, phonon↗
DOE OSTI2015

Near-infrared emitting In-rich InGaN layers grown directly on Si: Towards the whole composition range

The authors report compact and chemically homogeneous In-rich InGaN layers directly grown on Si (111) by plasma-assisted molecular beam epitaxy. High structural and optical quality is evidenced by transmission electron microscopy, near-field scanning optical microscopy, and X-ray diffraction. Photoluminescence emission in the near-infrared is observed up to room temperature covering the important 1.3 and 1.55 μm telecom wavelength bands. The n-InGaN/p-Si interface is ohmic due to the absence of any insulating buffer layers. This qualitatively extends the application fields of III-nitrides and allows their integration with established Si technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Stranski-Krastanov InN/InGaN quantum dots grown directly on Si(111)

The authors discuss and demonstrate the growth of InN surface quantum dots on a high-In-content In{sub 0.73}Ga{sub 0.27}N layer, directly on a Si(111) substrate by plasma-assisted molecular beam epitaxy. Atomic force microscopy and transmission electron microscopy reveal uniformly distributed quantum dots with diameters of 10–40 nm, heights of 2–4 nm, and a relatively low density of ∼7 × 10{sup 9} cm{sup −2}. A thin InN wetting layer below the quantum dots proves the Stranski-Krastanov growth mode. Near-field scanning optical microscopy shows distinct and spatially well localized near-infrared emission from single surface quantum dots. This holds promise for future telecommunication and sensing devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗