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[ACS Symposium Series] Raman Spectroscopy in the Undergraduate Curriculum Volume 1305 || Investigating the Similarities and Differences among UV/Vis, Infrared, Fluorescence, and Raman Spectroscopies through Discussion of Light–Matter Interactions
摘要： Spectroscopy is an invaluable tool in chemistry and is introduced throughout the undergraduate curriculum. At the fundamental level, spectroscopy measures the interactions between electromagnetic radiation and matter. Usually, students practice measuring spectra to characterize molecules and analyze experimental results. However, too often, little emphasis is placed on the specific interactions of the electromagnetic radiation with matter, which leads to a lack of differentiation and understanding of applicability among spectroscopic techniques. Here, a discussion of scattering, absorption, and emission processes is used to assist in the understanding of different spectroscopic techniques such as infrared and UV/vis (absorption), fluorescence (emission), and Raman (scattering). The purpose is to provide instructors with different visual frameworks and exercises for the introduction of spectroscopy in the undergraduate classroom and laboratory. The intended outcome is for students to understand the experimental spectroscopic techniques at a deeper level, giving rise to improved critical thinking skills in regards to scientific processes.
关键词： Raman,UV/Vis,Fluorescence,Light–Matter Interactions,Infrared,Spectroscopy
更新于2025-09-23 15:21:01
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Ultrastrong-coupling regime of nondipolar light-matter interactions
摘要： We present a circuit-QED scheme which makes it possible to reach the ultrastrong-coupling regime of a nondipolar interaction between a single qubit and a quantum resonator. We show that the system Hamiltonian is well approximated by a two-photon quantum Rabi model and propose a simple scattering experiment to probe its fundamental properties. In particular, we identify a driving scheme that reveals the change in selection rules characterizing the breakdown of the rotating-wave approximation and the transition from strong to ultrastrong two-photon interactions. Finally, we show that a frequency crowding in a narrow spectral region is observable in the output fluorescence spectrum as the coupling strength approaches the collapse point, paving the way to the direct observation of the onset of the spectral collapse in a solid-state device.
关键词： nondipolar light-matter interactions,spectral collapse,two-photon quantum Rabi model,ultrastrong-coupling regime,circuit-QED
更新于2025-09-23 15:21:01
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Nanoscale lighta??matter interactions in metala??organic frameworks cladding optical fibers
摘要： The utilization of refractive index (RI) change due to guest–host interactions between the guest volatile organic compound vapor and porous metal–organic frameworks (vapor–MOF interactions) is promising in photonic vapor sensors. Therefore, the study of light–matter interactions in nanoporous metal–organic frameworks (MOFs) is fundamental and essential for MOF-based photonic devices. In this work, the manipulation of light in MOFs to investigate the vapor–MOF interactions by using optical fiber devices is demonstrated. The vapor–MOF interactions and the light–vapor interactions (light in MOFs to sense the RI changes resulting from the vapor–MOF interactions) are investigated. The cladding mode is excited by a long-period fiber grating (LPFG) for evanescent field sensing in a ZIF-8 sensitive coating. The experimental results combining quantum chemical calculations and optical simulations reveal the relationships between the microscopic energy of vapor desorption, RI changes and evanescent field enhancement in ZIF-8 during the vapor–MOF interactions. With exceptionally large RI changes, the evanescent field of cladding mode in ZIF-8 is greatly enhanced to sense the vapor–MOF interactions. As a proof-of-concept, a LPFG sensor with ZIF-8 coating showed a high sensitivity of 1.33 pm ppm?1 in the linear range from 9.8 ppm to 540 ppm for the sensing of ethanol vapor. The investigation of light–matter interactions in ZIF-8 provides a useful guideline for the design and fabrication of MOF-based optical waveguide/fiber sensors.
关键词： Nanoscale,metal–organic frameworks,light–matter interactions,vapor sensing,optical fibers
更新于2025-09-19 17:13:59
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Coherent light matter interactions in nanostructure based active semiconductor waveguides operating at room temperature
摘要： Light matter coherent interactions require that the coherent state induced in the matter be maintained for the duration of the observation. The only way to induce and observe such interactions in room temperature semiconductors, where the coherence time is of the order of a few hundred femtoseconds, is to use ultrashort pulse excitations and an ultrafast characterization technique. For media comprising an ensemble of nanostructure semiconductors such as self-assembled quantum dots, the gain broadening inhomogeneity also affects the interaction. Moreover, when gain media in the form of an active waveguide, such as optical amplifiers, are used, the interaction is distributed and includes nonresonant incoherent phenomena that occur simultaneously with the coherent effects. Such a complex system can exhibit, nevertheless, clear coherent interactions even at room temperature. Using InAs/InP quantum dot and wirelike quantum dash amplifiers, Rabi oscillations, self-induced transparency, coherent control using spectral pulse shaping, Ramsey interference, and photon echo have been demonstrated. The characterization employed cross frequency resolved optical gating, and the experiments were accompanied by a comprehensive finite difference time domain model that solves the Maxwell and Lindblad equations. This work has major implications on the understanding of the details of dynamical processes in active semiconductor devices, on short pulse generation from semiconductor lasers, and on various future quantum devices.
关键词： active semiconductor waveguides,coherent control,self-induced transparency,Rabi oscillations,coherent light matter interactions,nanostructure,Ramsey interference,photon echo,room temperature
更新于2025-09-16 10:30:52
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Manipulating Light–Matter Interactions in Plasmonic Nanoparticle Lattices
摘要： Rationally assembled nanostructures exhibit distinct physical and chemical properties beyond their individual units. Developments in nanofabrication techniques have enabled the patterning of a wide range of nanomaterial designs over macroscale (>in.2) areas. Periodic metal nanostructures show long-range diffractive interactions when the lattice spacing is close to the wavelength of the incident light. The collective coupling between metal nanoparticles in a lattice introduces sharp and intense plasmonic surface lattice resonances, in contrast to the broad localized resonances from single nanoparticles. Plasmonic nanoparticle lattices exhibit strongly enhanced optical fields within the subwavelength vicinity of the nanoparticle unit cells that are 2 orders of magnitude higher than that of individual units. These intense electromagnetic fields can manipulate nanoscale processes such as photocatalysis, optical spectroscopy, nonlinear optics, and light harvesting. This Account focuses on advances in exciton?plasmon coupling and light?matter interactions with plasmonic nanoparticle lattices. First, we introduce the fundamentals of ultrasharp surface lattice resonances; these resonances arise from the coupling of the localized surface plasmons of a nanoparticle to the diffraction mode from the lattice. Second, we discuss how integrating dye molecules with plasmonic nanoparticle lattices can result in an architecture for nanoscale lasing at room temperature. The lasing emission wavelength can be tuned in real time by adjusting the refractive index environment or varying the lattice spacing. Third, we describe how manipulating either the shape of the unit cell or the lattice geometry can control the lasing emission properties. Low-symmetry plasmonic nanoparticle lasing responses, and multiscale plasmonic superlattices—finite patches of lattices can show polarization-dependent nanoparticles grouped into microscale arrays—can support multiple plasmon resonances for controlled multimodal nanolasing. Fourth, we discuss how the assembly of photoactive emitters on the nanocavity arrays behaves as a hybrid materials system with enhanced exciton?plasmon coupling. Positioning metal?organic framework materials around nanoparticles produces mixed photon modes with strongly enhanced photoluminescence at wavelengths determined by the lattice. Deterministic coupling of quantum emitters in two-dimensional materials to plasmonic lattices leads to preserved single-photon emission and reduced decay lifetimes. Finally, we highlight emerging applications of nanoparticle lattices from compact, fully reconfigurable imaging devices to solid-state emitter structures. Plasmonic nanoparticle lattices are a versatile, scalable platform for tunable flat optics, nontrivial topological photonics, and modified chemical reactivities.
关键词： nanoscale lasing,surface lattice resonances,exciton?plasmon coupling,light?matter interactions,plasmonic nanoparticle lattices
更新于2025-09-16 10:30:52
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Understanding the nature of mean-field semiclassical light-matter dynamics: An investigation of energy transfer, electron-electron correlations, external driving, and long-time detailed balance
摘要： Semiclassical electrodynamics (with quantum matter plus classical electrodynamics fields) is an appealing approach for studying light-matter interactions, especially for realistic molecular systems. However, there is no unique semiclassical scheme. On the one hand, intermolecular interactions can be described instantaneously by static two-body interactions connecting two different molecules, while a classical transverse E field acts as a spectator at short distance; we will call this Hamiltonian no. I. On the other hand, intermolecular interactions can also be described as effects that are mediated exclusively through a classical one-body E field without any quantum effects at all (assuming we ignore electronic exchange); we will call this Hamiltonian no. II. Moreover, one can also mix these two different Hamiltonians into a third, hybrid Hamiltonian, which preserves quantum electron-electron correlations for lower excitations but describes higher excitations in a mean-field way. To investigate which semiclassical scheme is most reliable for practical use, here we study the real-time dynamics of a minimalistic many-site model—a pair of identical two-level systems (TLSs)—undergoing either resonance energy transfer (RET) or collectively driven dynamics. While both approaches (no. 1 and no. 2) perform reasonably well when there is no strong external excitation, we find that no single approach is perfect for all conditions (and all methods fail when a strong external field is applied). Each method has its own distinct problems: Hamiltonian no. I performs best for RET but behaves in a complicated manner for driven dynamics; Hamiltonian no. II is always stable, but obviously fails for RET at short distances. One key finding is that, for externally driven dynamics, a full configuration-interaction description of Hamiltonian no. I strongly overestimates the long-time electronic energy, highlighting the not obvious fact that, if one plans to merge quantum molecules with classical light, a full, exact treatment of electron-electron correlations can actually lead to worse results than a simple mean-field electronic structure treatment. Future work will need to investigate (i) how these algorithms behave in the context of more than a pair of TLSs and (ii) whether or not these algorithms can be improved in general by including crucial aspects of spontaneous emission.
关键词： resonance energy transfer,semiclassical electrodynamics,mean-field dynamics,light-matter interactions,electron-electron correlations
更新于2025-09-12 10:27:22
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[IEEE 2019 Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC) - Munich, Germany (2019.6.23-2019.6.27)] 2019 Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC) - Generation of Broad-Band Circularly Polarised Supercontinuum in Chiral Photonic Crystal Fibre
摘要： Supercontinuum (SC) generation in solid-core photonic crystal fibres (PCFs) is well established and has diverse applications in science and technology [1,2]. In a conventional SC, the polarization state is not maintained over the whole spectrum due to cross-phase modulation and may in addition vary with power. Recently, it has been reported that continuously twisted PCFs exhibit circular birefringence [3,4]. Here we report the first experimental demonstration of a twisted PCF that robustly maintains circular polarization state across the whole spectrum, independent of power.
关键词： Supercontinuum generation,chiral light-matter interactions,photonic crystal fibres,circular polarization
更新于2025-09-12 10:27:22
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Observation of scalable sub-Poissonian-field lasing in a microlaser
摘要： Sub-Poisson field with much reduced fluctuations in a cavity can boost quantum precision measurements via cavity-enhanced light-matter interactions. Strong coupling between an atom and a cavity mode has been utilized to generate highly sub-Poisson fields. However, a macroscopic number of optical intracavity photons with more than 3 dB variance reduction has not been possible. Here, we report sub-Poisson field lasing in a microlaser operating with hundreds of atoms with well-regulated atom-cavity coupling and interaction time. Its photon-number variance was 4 dB below the standard quantum limit while the intracavity mean photon number scalable up to 600. The highly sub-Poisson photon statistics were not deteriorated by simultaneous interaction of a large number of atoms. Our finding suggests an effective pathway to widely scalable near-Fock-state lasing at the macroscopic scale.
关键词： microlaser,Sub-Poissonian-field lasing,cavity-enhanced light-matter interactions,quantum precision measurements,macroscopic sub-Poissonian field stabilization
更新于2025-09-11 14:15:04
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Exact Multipolar Decompositions with Applications in Nanophotonics
摘要： The multipolar decomposition of electromagnetic sources is an important tool for the study of light–matter interactions in general, and optical materials in particular. Here, a report is given on recent progress in the multipolar decomposition of electromagnetic sources. First, the exact and simple expressions for the multipolar moments of electric current density distributions are reviewed, and then, the results are extended to multipolar moments of magnetization current density distributions due to intrinsic spin. The consideration of both electric and magnetic sources allows to establish the conditions for sources of pure handedness. Scripts are provided that facilitate the computation of multipolar moments of arbitrary order. The work and the included examples of use are placed in the context of nanophotonics and metamaterials, and an outlook for applications in these and other fields is provided.
关键词： light–matter interactions,nanophotonics,multipole moments,optical antennas,theory
更新于2025-09-10 09:29:36
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Phase-modulated single-photon router
摘要： The single-photon routing properties in the system composed of two waveguides and two coupled cavities interacting with a two-level system are investigated theoretically. The phases of the coupling strengths are considered. The analytical expressions for the single-photon routing probabilities are obtained. The study shows that single-photon routing in a single waveguide or between two waveguides can be switched on or off by modulating the phase difference between the coupling constants. The analytical results also exhibit that the coupling between the two nanocavities plays an important role in the phase-dependent single-photon routing. We also show numerically the influence of the dissipation of cavities and atoms on routing properties. Our results may be useful in controlling and manipulating light-matter interactions based on waveguides at the single-photon level.
关键词： light-matter interactions,single-photon routing,phase modulation,waveguide QED
更新于2025-09-09 09:28:46