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At least 1,693 records · Page 94

Substantial reduction of the anisotropy in the critical current densities J c of Ni-doped CaKFe 4 As 4 single crystals by chemical and irradiation-induced disorder

Here, we demonstrate that the anisotropy in the critical current densities, J c , of CaK(Fe 1–x Ni x ) 4 As 4 (x = 0, 0.015, 0.025, and 0.030) single crystals reduces with increasing chemical and irradiation-induced disorder. The magnetic field dependences of J c are analyzed by performing magnetization measurements with H applied parallel and perpendicular to the crystallographic c-axis. The results show that undoped crystals display large anisotropies in Jc due to an enhancement of the vortex pinning with H applied parallel to the crystallographic ab-planes. This anisotropy reduces substantially as Ni addition increases. Moreover, we found that random disorder introduced by proton irradiation enhances mainly the vortex pinning for H parallel to the c-axis. Consequently, using adequate fluencies, the vortex pinning at low temperatures in both undoped and doped samples becomes close to isotropic. These results make the CaKFe 4 As 4 system promising for applications that require isotropic J c under magnetic fields.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Influence of the number of orientational domains on avalanche criticality in ferroelastic transitions

In this work, we study the relationship between avalanche criticality and the number of orientational domains in ferroelastic transitions. To this end, we use a general Ginzburg-Landau model appropriate for displacive transitions of the square lattice. The model includes disorder as a quenched distribution of local transition temperatures. We focus on the square-to-rectangle and the square-to-oblique ferroelastic transitions, which have two and four orientational domains, respectively, which in turn determine the corresponding degeneracy of the ground state of the system. The phase transitions are driven by temperature under the assumption of a strict athermal behavior. That is, we assume that thermal fluctuations do not play any role. Numerical results are obtained using a purely relaxational dynamics, and it is shown that both the square-to-rectangle and the square-to-oblique transitions occur intermittently in the form of avalanches. Avalanche sizes and avalanche energies are found to display power-law distributions, which corroborates avalanche criticality. We compare and contrast the dependence of avalanche criticality on the number of orientational domains of the low-symmetry phase. It is found that the critical exponents depend on that number, in agreement with recent experimental results.

36 MATERIALS SCIENCE↗

Type-II Weyl nodes, flat bands, and evidence for a topological Hall-effect in the new ferromagnet FeCr 3 Te 6

The interplay between linearly dispersing, or Dirac-like, and flat electronic bands, for instance, in the kagome ferromagnets, has attracted attention due to a possible interplay between topology and electronic correlations. Here, we report the synthesis, structural, electrical, and magnetic properties of a single-crystalline ferromagnetic compound, namely Fe 1/3 ⁢CrTe 2 or FeCr 3 ⁢Te 6 , which crystallizes in the 𝑃$\overline{3}$⁢𝑚⁢1 space group instead of the 𝐼⁢2/𝑚 previously reported for FeCr 2 ⁢Te 4 . Electronic band structure calculations reveal type-II Dirac nodes and relatively flat bands near the Fermi level (ε 𝐹 ). This compound shows onset Curie temperature 𝑇 c ≃ 120K, followed by an additional ferromagnetic transition near 𝑇 c2 ∼ 92.5K. Below 𝑇 c , FeCr 3 ⁢Te 6 displays a pronounced anomalous Hall effect, as well as sizable coercive fields that exceed 𝜇 0 ⁢𝐻=1 T at low 𝑇⁢s. However, a scaling analysis indicates that the anomalous Hall effect results from a significant intrinsic contribution, as expected from the calculations, and also from the extrinsic mechanism, i.e., scattering. The extrinsic contribution probably results from occupational disorder at the 1b Fe-site within the van der Waals gap of the CrTe 2 host. We also observe evidence for a topological Hall component superimposed onto the overall Hall response, suggesting the presence of chiral spin textures akin to skyrmions in this centrosymmetric system. Their possible presence will require experimental confirmation.

36 MATERIALS SCIENCE↗

Plasma Treated Active Carbon for Capacitive Deionization of Saline Water

The plasma treatment on commercial active carbon (AC) was carried out in a capacitively coupled plasma system using Ar + 10% O 2 at pressure of 4.0 Torr. The RF plasma power ranged from 50 W to 100 W and the processing time was 10 min. The carbon film electrode was fabricated by electrophoretic deposition. Micro-Raman spectroscopy revealed the highly increased disorder of sp 2 C lattice for the AC treated at 75 W. An electrosorption capacity of 6.15 mg/g was recorded for the carbon treated at 75 W in a 0.1 mM NaCl solution when 1.5 V was applied for 5 hours, while the capacity of the untreated AC was 1.0 mg/g. The plasma treatment led to 5.09 times increase in the absorption capacity. The jump of electrosorption capacity by plasma treatment was consistent with the Raman spectra and electrochemical double layer capacitance. This work demonstrated that plasma treatment was a potentially efficient approach to activating biochar to serve as electrode material for capacitive deionization (CDI).

36 MATERIALS SCIENCE↗

Lipoprotein Particles in Cerebrospinal Fluid

The brain is the most lipid-rich organ in the body, and the intricate interplay between lipid metabolism and pathologies associated with neurodegenerative disorders is being increasingly recognized. The brain is bathed in cerebrospinal fluid (CSF), which, like plasma, contains lipid-protein complexes called lipoproteins that are responsible for extracellular lipid transport. Multiple CSF lipoprotein populations exist, some of which are produced de novo in the central nervous system and others that appear to be generated from protein constituents that are produced in the periphery. These CSF lipoproteins are thought to play key roles in maintaining lipid homeostasis in the central nervous system, while little else is known due to their limited accessibility and their low abundance in CSF. Recent work has provided new insights into the compositional complexity of CSF lipoprotein families and their metabolism in cerebral circulation. Finally, the purpose of this review is to summarize our current state of knowledge on the composition, origin, and metabolism of CSF lipoproteins.

59 BASIC BIOLOGICAL SCIENCES↗

Auditory and Vestibular Issues Related to Human Spaceflight

Human spaceflight provides unique opportunities to study human vestibular and auditory systems. This session will discuss 1) vestibular adaptive processes reflected by pronounced perceptual and motor coordination problems during, and after, space missions; 2) vestibular diagnostic and rehabilitative techniques (used to promote recovery after living in altered gravity environments) that may be relevant to treatment of vestibular disorders on earth; and 3) unique acoustical challenges to hearing loss prevention and crew performance during spaceflight missions.

Danielson, Richard W.↗

PrP{sup C} displays an essential protective role from oxidative stress in an astrocyte cell line derived from PrP{sup C} knockout mice

Highlights: Black-Right-Pointing-Pointer PrP{sup C} in solution acts as a radical scavenger. Black-Right-Pointing-Pointer PrP{sup C} reduces hydrogen peroxide toxicity in astrocytes. Black-Right-Pointing-Pointer Increase in ROS disrupted the cell cycle in the PrP{sup C}-knockout astrocytes. Black-Right-Pointing-Pointer PrP{sup C} prevents the cell death independently of an SOD-like activity. -- Abstract: The PrP{sup C} protein, which is especially present in the cellular membrane of nervous system cells, has been extensively studied for its controversial antioxidant activity. In this study, we elucidated the free radical scavenger activity of purified murine PrP{sup C} in solution and its participation as a cell protector in astrocytes that were subjected to treatment with an oxidant. In vitro and using an EPR spin-trapping technique, we observed that PrP{sup C} decreased the oxidation of the DMPO trap in a Fenton reaction system (Cu{sup 2+}/ascorbate/H{sub 2}O{sub 2}), which was demonstrated by approximately 70% less DMPO/OH{sup {center_dot}}. In cultured PrP{sup C}-knockout astrocytes from mice, the absence of PrP{sup C} caused an increase in intracellular ROS (reactive oxygen species) generation during the first 3 h of H{sub 2}O{sub 2} treatment. This rapid increase in ROS disrupted the cell cycle in the PrP{sup C}-knockout astrocytes, which increased the population of cells in the sub-G1 phase when compared with cultured wild-type astrocytes. We conclude that PrP{sup C} in solution acts as a radical scavenger, and in astrocytes, it is essential for protection from oxidative stress caused by an external chemical agent, which is a likely condition in human neurodegenerative CNS disorders and pathological conditions such as ischemia.

60 APPLIED LIFE SCIENCES↗

Transient Studies of Nonequilibrium Transport in Two-Dimensional Semiconductors

The overarching objective of research under DOE support has been to investigate emergent carrier phenomena in different two-dimensional (2D) systems, under conditions where they are driven far from equilibrium. The description of nonequilibrium transport has long represented one of the most enduring challenges in condensed-matter physics, in large part due to the need to invoke the role of complex many-body phenomena (electron-phonon and electron-electron coupling) in this regime. In this project, we have explored aspects of this problem in a variety of different two-dimensional systems. These include the modulation-doped two-dimensional electrons gas, or 2DEG, in GaAs/AlGaAs heterostructures; the electron and hole systems in graphene and its related hetero-structures, and; the strongly-confined electron layers in transition-metal dichalcogenide (MoS 2 and WS 2 ) and trichalcogenide (TiS 3 ) materials. Significant understanding has been achieved in a number of different areas, as we elaborate upon in subsequent sections of this proposal: Nanoscale spectroscopy of defect-related barriers in MoS2 Negative differential conductance due to inter-valley scattering in WS 2 under high fields Incipient localization due to scattering from frozen-phonon disorder in quantum point contacts High-field transient transport in graphene/hexagonal BN heterostructures Universal voltage scaling of quantum corrections in graphene under nonequilibrium A defining feature of much of this research has been an approach to problem solving in which novel experimental techniques (such as transient electrical pulsing and scanning-probe microscopy) are combined with the development (in collaboration with colleagues from condensed-matter theory) of sophisticated models, a strategy that we propose to continue in our future research. In recent years, we have developed an increasing capacity for handling atomically-thin materials, and their van der Waals systems, a capacity that is reflected in the balance of topics listed above.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ternary aluminides R{sub 0.67}Ni{sub 2}Al{sub 6} (R=Sc, Y, Gd-Lu) with partly disordered structures

Ten rare-earth nickel aluminides R{sub 0.67}Ni{sub 2}Al{sub 6} (R=Sc, Y, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu) were synthesized by arc melting and their crystal structures studied by X-ray powder diffraction. They crystallize in the hexagonal structure type Yb{sub 0.67}Ni{sub 2}Al{sub 6}: Pearson symbol hP11-2.33, space group P-6m2, a=4.18904(2), c=9.09816(6) A, which can be decomposed into three kinds of layer. The sequence of layers along [001] is Yb{sub 0.67}Al-NiAl{sub 2}-Al-NiAl{sub 2}, but stacking faults appear due to relative shifts of consecutive Yb{sub 0.67}Al layers containing two rare-earth metal atoms for one Al-atom triangle. An ordered superstructure is the type ErNi{sub 3}Al{sub 9} (Pearson symbol hR78, space group R32, a={radical}(3)a{sub 0}, c=3c{sub 0}), refined on single crystals. The physical properties of the R{sub 0.67}Ni{sub 2}Al{sub 6} (R=Tb, Er, Tm, Yb, and Lu) compounds were determined by means of magnetic and electrical transport measurements. All these materials but Lu{sub 0.67}Ni{sub 2}Al{sub 6} exhibit Curie-Weiss paramagnetic behavior due to the trivalent R ions, and order magnetically at low temperatures. They show good metallic conductivity. The Yb-containing compound is a dense Kondo system with distinct features in the paramagnetic state of the interplay between Kondo and crystalline electric field interactions. - Graphical abstract: Stacking of layers along [001] in the Yb{sub 0.67}Ni{sub 2}Al{sub 6}-type structure. Highlights: Black-Right-Pointing-Pointer The aluminides R{sub 0.67}Ni{sub 2}Al{sub 6} (R=Sc, Y, Gd-Lu) adopt a partly disordered structure. Black-Right-Pointing-Pointer The structure is characterized by R{sub 2}Al{sub 3} layers with two R atoms for one Al{sub 3} triangle. Black-Right-Pointing-Pointer The compounds with R=Tb, Er, Tm are paramagnets at rt and order magnetically at lt. Black-Right-Pointing-Pointer The Yb-compound exhibits a magnetically ordered Kondo lattice with strong CEF effect.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Morphological Phase Behavior of Poly(RTIL)-Containing Diblock Copolymer Melts

The development of nanostructured polymeric systems containing directionally continuous poly(ionic liquid) (poly(IL)) domains has considerable implications toward a range of transport-dependent, energy-based technology applications. The controlled, synthetic integration of poly(IL)s into block copolymer (BCP) architectures provides a promising means to this end, based on their inherent ability to self-assemble into a range of defined, periodic morphologies. In this work, we report the melt-state phase behavior of an imidazolium-containing alkyl-ionic BCP system, derived from the sequential ring-opening metathesis polymerization (ROMP) of imidazolium- and alkyl-substituted norbornene monomer derivatives. A series of 16 BCP samples were synthesized, varying both the relative volume fraction of the poly(norbornene dodecyl ester) block (f{sub DOD} = 0.42-0.96) and the overall molecular weights of the block copolymers (M{sub n} values from 5000-20,100 g mol{sup -1}). Through a combination of small-angle X-ray scattering (SAXS) and dynamic rheology, we were able to delineate clear compositional phase boundaries for each of the classic BCP phases, including lamellae (Lam), hexagonally packed cylinders (Hex), and spheres on a body-centered-cubic lattice (S{sub BCC}). Additionally, a liquid-like packing (LLP) of spheres was found for samples located in the extreme asymmetric region of the phase diagram, and a persistent coexistence of Lam and Hex domains was found in lieu of the bicontinuous cubic gyroid phase for samples located at the intersection of Hex and Lam regions. Thermal disordering was opposed even in very low molecular weight samples, detected only when the composition was highly asymmetric (f{sub DOD} = 0.96). Annealing experiments on samples exhibiting Lam and Hex coexistence revealed the presence of extremely slow transition kinetics, ultimately selective for one or the other but not the more complex gyroid phase. In fact, no evidence of the bicontinuous network was detected over a 2 month annealing period. The ramifications of these results for transport-dependent applications targeting the use of highly segregated poly(IL)-containing BCP systems are carefully considered.

36 MATERIALS SCIENCE↗

Physics of Hard Spheres Experiment: Significant and Quantitative Findings Made

Direct examination of atomic interactions is difficult. One powerful approach to visualizing atomic interactions is to study near-index-matched colloidal dispersions of microscopic plastic spheres, which can be probed by visible light. Such spheres interact through hydrodynamic and Brownian forces, but they feel no direct force before an infinite repulsion at contact. Through the microgravity flight of the Physics of Hard Spheres Experiment (PHaSE), researchers have sought a more complete understanding of the entropically driven disorder-order transition in hard-sphere colloidal dispersions. The experiment was conceived by Professors Paul M. Chaikin and William B. Russel of Princeton University. Microgravity was required because, on Earth, index-matched colloidal dispersions often cannot be density matched, resulting in significant settling over the crystallization period. This settling makes them a poor model of the equilibrium atomic system, where the effect of gravity is truly negligible. For this purpose, a customized light-scattering instrument was designed, built, and flown by the NASA Glenn Research Center at Lewis Field on the space shuttle (shuttle missions STS 83 and STS 94). This instrument performed both static and dynamic light scattering, with sample oscillation for determining rheological properties. Scattered light from a 532- nm laser was recorded either by a 10-bit charge-coupled discharge (CCD) camera from a concentric screen covering angles of 0 to 60 or by sensitive avalanche photodiode detectors, which convert the photons into binary data from which two correlators compute autocorrelation functions. The sample cell was driven by a direct-current servomotor to allow sinusoidal oscillation for the measurement of rheological properties. Significant microgravity research findings include the observation of beautiful dendritic crystals, the crystallization of a "glassy phase" sample in microgravity that did not crystallize for over 1 year in 1g (Earth's gravity), and the emergence of face-centered-cubic (FCC) crystals late in the coarsening process (as small crystallites lost particles to the slow ripening of large crystallites). Significant quantitative findings from the microgravity experiments have been developed describing complex interactions among crystallites during the growth process, as concentration fields overlap in the surrounding disordered phase. Time-resolved Bragg scattering under microgravity captures one effect of these interactions quite conclusively for the sample at a volume fraction of 0.528. From the earliest time until the sample is almost fully crystalline, the size and overall crystallinity grow monotonically, but the number of crystallites per unit volume (number density) falls. Apparently nucleation is slower than the loss of crystallites because of the transfer of particles from small to large crystals. Thus, coarsening occurs simultaneously with growth, rather than following the completion of nucleation and growth as is generally assumed. In the same sample, an interesting signature appears in the apparent number density of crystallites and the volume fraction within the crystallites shortly before full crystallinity is reached. A brief upturn in both indicates the creation of more domains of the size of the average crystallite simultaneous with the compression of the crystallites. Only the emergence of dendritic arms offers a reasonable explanation. The arms would be "seen" by the light scattering as separate domains whose smaller radii of curvature would compress the interior phase. In fiscal year 1999, numerous papers, a doctoral dissertation, and the PHaSE final report were produced. Although this flight project has been completed, plans are in place for a follow-on colloid experiment by Chaikin and Russel that employs a light microscope within Glenn's Fluids and Combustion Facility on the International Space Station. PHaSE is providing us with a deeper understanding of the nure of phase transitions. The knowledge derived has added to the understanding of condensed matter. In addition, the burgeoning study of the dynamics of colloidal self-assembly may lead to the development of a range of photonic materials that control the desirable properties of light. Thus, applications of ordered colloidal structures include not only ultrastructure ceramics, but also photonic crystals and photothermal nanosecond light-switching devices. Industries dealing with semiconductors, electro-optics, ceramics, and composites stand to benefit from such advancements.

Doherty, Michael P.↗

Reversible differentiation of myofibroblasts by MyoD

Myofibroblasts participate in tissue repair processes in diverse mammalian organ systems. The deactivation of myofibroblasts is critical for termination of the reparative response and restoration of tissue structure and function. The current paradigm on normal tissue repair is the apoptotic clearance of terminally differentiated myofibroblasts; while, the accumulation of activated myofibroblasts is associated with progressive human fibrotic disorders. The capacity of myofibroblasts to undergo de-differentiation as a potential mechanism for myofibroblast deactivation has not been examined. In this report, we have uncovered a role for MyoD in the induction of myofibroblast differentiation by transforming growth factor-{beta}1 (TGF-{beta}1). Myofibroblasts demonstrate the capacity for de-differentiation and proliferation by modulation of endogenous levels of MyoD. We propose a model of reciprocal signaling between TGF-{beta}1/ALK5/MyoD and mitogen(s)/ERK-MAPK/CDKs that regulate myofibroblast differentiation and de-differentiation, respectively. Our studies provide the first evidence for MyoD in controlling myofibroblast activation and deactivation. Restricted capacity for de-differentiation of myofibroblasts may underlie the progressive nature of recalcitrant human fibrotic disorders.

60 APPLIED LIFE SCIENCES↗

The development of methods for primary mast cells in vitro and ex vivo: An historical review

Highlights: • Mast cells form a first-line defense of immune system against various challenges. • Over the past few decades, technologies for acquiring mast cells have been continually optimized. • The advantages and applicability of diverse mast cell models evaluated. • It is important to choose a proper cell source for mast cell-related experiments. Mast cells (MCs) are tissue-based stationary effector cells that form the immune system's first-line defense against various challenges. They are developed from the bone marrow-derived progenitors to complete their differentiation and maturation in the tissues where they eventually establish residence. MCs have been implicated in many diseases, such as allergy, parasitic infection, and neoplastic disorders. Immortalized MC lines, such as RBL-2H3, HMC-1, and LAD-2, are useful for investigating the biological functions of MC only to some extents due to the restriction of degranulation evaluation, in vivo injection and other factors. Over the past few decades, technologies for acquiring primarily MCs have been continually optimized, and novel protocols have been proposed. However, no relevant publications have analyzed and summarized these techniques. In this review, the classical approaches for extracting MCs are generalized, and new methods with potential values are introduced. We also evaluate the advantages and applicability of diverse MC models. Since MCs exhibit substantial plasticity and functional diversity due to different origins, it is both necessary and urgent to select a reliable and suitable source of MCs for a particular study.

60 APPLIED LIFE SCIENCES↗

Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction

Electrochemical nitrate reduction (NO 3 RR) has attracted attention as an emerging approach to mitigate nitrate pollution in groundwater. Here, we report that a highly ordered PdCu alloy-based electrocatalyst exhibits selective (91% N 2 ), stable (480 h), and near complete (94%) removal of nitrate without loss of catalyst. In situ and ex situ XAS provide evidence that structural ordering between Pd and Cu improves long-term catalyst stability during NO 3 RR. In contrast, we also report that a disordered PdCu alloy-based electrocatalyst exhibits non-selective (44% N 2 and 49% NH 4 + ), unstable, and incomplete removal of nitrate. The copper within disordered PdCu alloy is vulnerable to accepting electrons from hydrogenated neighboring Pd atoms. This resulted in copper catalyst losses which were 10× greater than that of the ordered catalyst. The design of stable catalysts is imperative for water treatment because loss of the catalyst adds to the system cost and environmental impacts.

36 MATERIALS SCIENCE↗

Dynamic Behavior of Platinum Atoms and Clusters in the Native Oxide Layer of Aluminum Nanocrystals

Strong metal–support interactions (SMSIs) are well-known in the field of heterogeneous catalysis to induce the encapsulation of platinum (Pt) group metals by oxide supports through high temperature H 2 reduction. However, demonstrations of SMSI overlayers have largely been limited to reducible oxides, such as TiO 2 and Nb 2 O 5 . In this report we show that the amorphous native surface oxide of plasmonic aluminum nanocrystals (AlNCs) exhibits SMSI-induced encapsulation of Pt following reduction in H 2 in a Pt structure dependent manner. Reductive treatment in H 2 at 300 °C induces the formation of an AlO x SMSI overlayer on Pt clusters, leaving Pt single-atom sites (Ptiso) exposed available for catalysis. The remaining exposed Pt iso species possess a more uniform local coordination environment than has been observed on other forms of Al 2 O 3 , suggesting that the AlO x native oxide of AlNCs presents well-defined anchoring sites for individual Pt atoms. This observation extends our understanding of SMSIs by providing evidence that H 2 -induced encapsulation can occur for a wider variety of materials and should stimulate expanded studies of this effect to include nonreducible oxides with oxygen defects and the presence of disorder. It also suggests that the single-atom sites created in this manner, when combined with the plasmonic properties of the Al nanocrystal core, may allow for site-specific single-atom plasmonic photocatalysis, providing dynamic control over the light-driven reactivity in these systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Light quantum control of persisting Higgs modes in iron-based superconductors

The Higgs mechanism, i.e., spontaneous symmetry breaking of the quantum vacuum, is a cross-disciplinary principle, universal for understanding dark energy, antimatter and quantum materials, from superconductivity to magnetism. Unlike one-band superconductors (SCs), a conceptually distinct Higgs amplitude mode can arise in multi-band, unconventional superconductors via strong interband Coulomb interaction, but is yet to be accessed. Here we discover such hybrid Higgs mode and demonstrate its quantum control by light in iron-based high-temperature SCs. Using terahertz (THz) two-pulse coherent spectroscopy, we observe a tunable amplitude mode coherent oscillation of the complex order parameter from coupled lower and upper bands. The nonlinear dependence of the hybrid Higgs mode on the THz driving fields is distinct from any known SC results: we observe a large reversible modulation of resonance strength, yet with a persisting mode frequency. Together with quantum kinetic modeling of a hybrid Higgs mechanism, distinct from charge-density fluctuations and without invoking phonons or disorder, our result provides compelling evidence for a light-controlled coupling between the electron and hole amplitude modes assisted by strong interband quantum entanglement. Such light-control of Higgs hybridization can be extended to probe many-body entanglement and hidden symmetries in other complex systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Linear response of molecular polaritons

In this article, we show that the collective light–matter strong coupling regime where N molecular emitters couple to the photon mode of an optical cavity can be mapped to a quantum impurity model where the photon is the impurity that is coupled to a bath of anharmonic transitions. In the thermodynamic limit where N ≫ 1, we argue that the bath can be replaced with an effective harmonic bath, leading to a dramatic simplification of the problem into one of the coupled harmonic oscillators. We derive simple analytical expressions for linear optical spectra (transmission, reflection, and absorption) where the only molecular input required is the molecular linear susceptibility. This formalism is applied to a series of illustrative examples, showing the role of temperature, disorder, vibronic coupling, and optical saturation of the molecular ensemble, explaining that it is useful even when describing an important class of nonlinear optical experiments. For completeness, we provide Appendixes A–C that include a self-contained derivation of the relevant spectroscopic observables for arbitrary anharmonic systems (for both large and small N) within the rotating-wave approximation. While some of the presented results herein have already been reported in the literature, we provide a unified presentation of the results as well as new interpretations that connect powerful concepts in open quantum systems and linear response theory with molecular polaritonics.

Chemistry↗