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AIPP Photonics in Chemical Physics

Quantum-Classical Mechanics: Principles, Applications, and Prospects

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MATERIALS FOR HUMANITY (MH 21)

MH 21 is arranged around 6 themes that focus attention on pressing needs that should be addressed to enhance the well-being of communities and provide a forum for presenting breakthrough discoveries.

poster

The field of photonics, broadly defined, ranges from basic physical work on lasers and ultrashort laser pulses to applications in healthcare, communications, and materials. With its increasingly diverse disciplines and subdisciplines, photonics has become a key component in modern society. The scientific program consists of cross-disciplinary researchers, including chemists, physicists, and engineers, in both theory and experimentation. These researchers will discuss this rapidly expanding field and cover topics that address the latest advances in photonics related research and debate the current needs and priorities, as well as the emerging areas.

To access the AIPP Photonics in Chemical Physics conference, [please remember to register.  ](https://services.aip.org/AIPPHorizons/?confID=3351210)

The field of photonics, broadly defined, ranges from basic physical work on lasers and ultrashort laser pulses to applications in healthcare, communications, and materials. With its increasingly diverse disciplines and subdisciplines, photonics has become a key component in modern society. 

Controlling light-matter interaction with molecular vibrations in mid-infrared resonators offers exciting new research opportunities in chemistry and physics [1]. Laboratory implementations use standard materials, operate at room temperature, and use traditional fabrication and detection techniques, yet they have deeply challenged our fundamental understanding on the connections between cavity quantum electrodynamics and chemistry. We have developed rigorous microscopic quantum theory to describe the optical and chemical properties of realistic molecular vibrations in infrared cavity resonators with non-perturbative light-matter interaction [2,3]. We can successfully describe the linear and nonlinear spectra of vibrational polaritons [4]—hybrid vibration-cavity eigenstates– and realistically study the dissociation dynamics of cavity-coupled molecular bonds under non-adiabatic conditions [5]. The role of symmetry of the ground state electronic density with respect to nuclear displacements in the dynamics of vibrational polaritons is discussed, and future applications of these systems for the generation of THz quantum light are suggested.

Strong light-matter coupling with molecular vibrations in infrared resonators

Trivalent europium ions (Eu(III)) exhibit high color purity, but their absorption coefficients are very small. Eu(III) complexes that utilize energy transfer from antenna ligands to a metal center have been developed to produce efficient luminescent materials. Nevertheless, their energy transfer mechanisms, which depend on the kinds of ligands and their configurations, are still elusive due to weak and complicated interactions between organic ligands and lanthanide ions. To elucidate the energy transfer mechanisms, we measured the temporal changes of emission and absorption spectra using time-resolved photoluminescence (TR-PL) and transient absorption (TA), respectively. We compared the intramolecular energy transfer of the mononuclear complex and the dinuclear complex. Although they have identical antenna chromophores, the dynamics of the two complexes are different. The lifetime of the ligand S1 state in the dinuclear complex is faster than in the mononuclear complex. By comparing molecular geometries between the complexes, we concluded that this difference originated from the difference in the relative configuration of the two triphenylenes. Our discovery helps to establish the design strategy of highly efficient luminescent lanthanide complexes in photofunctional materials.

Energy transfer dynamics in luminescent Eu(III) complexes with phosphine oxide ligands


In this study, optical deep-level transient spectroscopy (O-DLTS) has been employed to investigate trap properties in the p-GaN/AlGaN heterostructure, the key part of such a normally-off enhancement-mode III-N transistors. Three electron traps labeled as E1, E2, and E3 were extracted by O-DLTS. The temperature-enhanced emission process of E3 has been studied by isothermal mode O-DLTS.



Study of Traps in p-GaN Gate HEMT by Optical DLTS

The new trends in biosensing field involves fast and real-time identification of biomarkers for rapid diagnosis with less-invasive methods by means of low-cost miniaturized and portable point of care devices. The ability of plasmonic systems to confine the light at nanometer dimension and manipulate the light with size, shape and material features, makes these systems promising candidates for biomedical devices. In this work we demonstrate the sensing capability of compact arrays of 3D metal dielectric core-shell chiral nano helices-based metamaterial enabled by the engineering of many technological elements. On one hand, the intrinsic chiral geometry of these structures, realized by Focused Ion Beam Induced Deposition technology, makes the system unaffected by background interferences, allowing to work even in optically dense environments like body fluids. Moreover, the metal-dielectric architecture realized through a conformal coating of a functional polymeric layer, enhance the chiroptical plasmonic properties of the chiral metamaterial in the far and near- field, and offers a large surface to suitable for molecular immobilization, together with the extrusion along the third dimension. We recorded refractive index sensitivity of about 800nm/RIU and FOM= 1276 RIU-1 for different concentration of glycerol-water solution. We also demonstrated the detection abilities to surface-specific binding event with the Tar-Dna binding protein, TDP-43, currently under study as biomarker for early-stage detection of neurodegenerative diseases. We successfully tested the sensor at different molar concentrations ranging from 1pM down to 10 fM, and in different environment, like human serum. We believe that our finding provides new perspectives for novel diagnostic tools.

3D Helix-based Metamaterial Arrays for Femtomolar Biodetection

Stepwise two-photon absorption (2PA) processes are becoming an important technique because it can achieve high reductive photochemical reactions with visible and near infrared light and intensity-gated high spatiotemporal selectivity with much lower power thresholds than those of the simultaneous 2PA. However, excited states generated by stepwise 2PA (higher excited states and excited states of transient species) are so short-lived that the efficiency for the stepwise 2PA induced photochemical reactions is usually quite low, which limits the versatility for this technique. Here, we demonstrated that the electron of the higher excited state can be efficiently extracted in a nanohybrid of organic molecules and wide bandgap semiconductor nanocrystals (NCs).1 Using perylene bisimide (PBI)-coordinated CdS NCs as a model compound, we demonstrated that the electron of the higher excited state of PBI generated by stepwise 2PA can be extracted to the conduction band of CdS NCs with a quantum yield of ∼0.5–0.7. Moreover, the extracted electron survives at the conduction band of CdS NCs over nanoseconds, which is more than hundred times longer than the lifetime of the higher excited state of PBI. This method can be applied to other organic molecules and larger wide bandgap semiconductors, and therefore, will expand the versatility for the photochemical reactions utilizing the short-lived excited states.

Green and far-red-light induced electron injection from perylene bisimide to wide-bandgap semiconductor nanocrystals with stepwise two-photon absorption process

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Quantum-Classical Mechanics: Principles, Applications, and Prospects

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