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At least 253 records · Page 14

Improved semiclassical model for real-time evaporation of matrix black holes

In this paper, we study real-time classical matrix mechanics of a simplified 2 × 2 matrix model inspired by the black hole evaporation problem. This is a step towards making a quantitative model of real-time evaporation of a black hole, which is realized as a bound state of D0-branes in string theory. The model we study is the reduction of Yang–Mills in 2 + 1 dimension to 0 + 1 dimensions, which has been corrected with an additional potential that can be interpreted as a zero-point energy for fermions. Our goal is to understand the lifetime of such a classical bound state object in the classical regime. To do so, we pay particular attention to when D-particles separate to check that the “off-diagonal modes” of the matrices become adiabatic and use that information to improve on existing models of evaporation. It turns out that the naive expectation value of the lifetime with the fermionic correction is infinite. This is a logarithmic divergence that arises from very large excursions in the separation between the branes near the threshold for classical evaporation. The adiabatic behavior lets us get some analytic control of the dynamics in this regime to get this estimate. This divergence is cutoff in the quantum theory due to quantization of the adiabatic parameter, resulting in a long lifetime of the bound state, with a parametric dependence of order log(1/ℏ).

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Pines’ demon observed as a 3D acoustic plasmon in Sr2RuO4

Abstract The characteristic excitation of a metal is its plasmon, which is a quantized collective oscillation of its electron density. In 1956, David Pines predicted that a distinct type of plasmon, dubbed a ‘demon’, could exist in three-dimensional (3D) metals containing more than one species of charge carrier 1 . Consisting of out-of-phase movement of electrons in different bands, demons are acoustic, electrically neutral and do not couple to light, so have never been detected in an equilibrium, 3D metal. Nevertheless, demons are believed to be critical for diverse phenomena including phase transitions in mixed-valence semimetals 2 , optical properties of metal nanoparticles 3 , soundarons in Weyl semimetals 4 and high-temperature superconductivity in, for example, metal hydrides 3,5–7 . Here, we present evidence for a demon in Sr 2 RuO 4 from momentum-resolved electron energy-loss spectroscopy. Formed of electrons in the β and γ bands, the demon is gapless with critical momentum q c = 0.08 reciprocal lattice units and room-temperature velocity v = (1.065 ± 0.12) × 10 5 m s −1 that undergoes a 31% renormalization upon cooling to 30 K because of coupling to the particle–hole continuum. The momentum dependence of the intensity of the demon confirms its neutral character. Our study confirms a 67-year old prediction and indicates that demons may be a pervasive feature of multiband metals.

Science & Technology - Other Topics↗

Interfaces and the extended Hilbert space of Chern-Simons theory

The low energy effective field theories of (2 + 1) dimensional topological phases of matter provide powerful avenues for investigating entanglement in their ground states. In [1] the entanglement between distinct Abelian topological phases was investigated through Abelian Chern-Simons theories equipped with a set of topological boundary conditions (TBCs). In the present paper we extend the notion of a TBC to non-Abelian Chern-Simons theories, providing an effective description for a class of gapped interfaces across non-Abelian topological phases. These boundary conditions furnish a defining relation for the extended Hilbert space of the quantum theory and allow the calculation of entanglement directly in the gauge theory. Because we allow for trivial interfaces, this includes a generic construction of the extended Hilbert space in any (compact) Chern-Simons theory quantized on a Riemann surface. Additionally, this provides a constructive and principled definition for the Hilbert space of effective ground states of gapped phases of matter glued along gapped interfaces. Lastly, we describe a generalized notion of surgery, adding a powerful tool from topological field theory to the gapped interface toolbox.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

A unified realization of electrical quantities from the quantum International System of Units

In the revised International System of Units (SI), the ohm and the volt are realized from the von Klitzing constant and the Josephson constant, and a practical realization of the ampere is possible by applying Ohm’s law directly to the quantum Hall and Josephson effects. As a result, it is possible to create an instrument capable of realizing all three primary electrical units, but the development of such a system remains challenging. Here, in this study, we report a unified realization of the volt, ohm and ampere by integrating a quantum anomalous Hall resistor (QAHR) and a programmable Josephson voltage standard (PJVS) in a single cryostat. Our system has a quantum voltage output that ranges from 0.24 mV to 6.5 mV with combined relative uncertainties down to 3 μV V −1 . The QAHR provides a realization of the ohm at zero magnetic field with uncertainties near 1 μΩ Ω −1 . We use the QAHR to convert a longitudinal current to a quantized Hall voltage and then directly compare that against the PJVS to realize the ampere. We determine currents in the range of 9.33–252 nA, and our lowest uncertainty is 4.3 μA A −1 at 83.9 nA. For other current values, a systematic error that ranges from −10 μA A −1 to −30 μA A −1 is present due to the imperfect isolation of the PJVS microwave bias.

Quantum metrology↗

Lifting the Garage Door on Spawn, An Open-Source BEM-Controls Engine

Spawn is the latest whole-building energy simulation engine developed by the US Department of Energy, National Labs and industry. Whereas EnergyPlus was designed as a successor to DOE-2, Spawn is not a direct successor of–nor is it intended as an imminent replacement for– EnergyPlus. Instead, Spawn reuses parts of EnergyPlus while supporting new use cases in HVAC and controls. Spawn is intended to provide several capabilities that significantly advance beyond EnergyPlus. It is intended to support the evaluation of novel HVAC and district energy systems in a more physically realistic way. Critically, it can model control in a physically realistic way, using portable specifications that can be compiled for execution on control platforms. Spawn is also intended to support co-simulation in an intrinsic way to enable integration with third-party models. This paper describes the software architecture of Spawn from model authoring to compilation and simulation. It explains how Spawn reuses the envelope and daylighting modules of EnergyPlus and couples them to HVAC and control models from the Modelica Buildings Library using the Functional Mockup Interface (FMI) standard. It presents a number of examples that: i) validate Spawn’s coupled simulation approach by comparing its results to those of EnergyPlus, ii) illustrate the Spawn methodology for modeling and simulating HVAC systems, and iii) evaluate the performance of Spawn’s Quantized State System (QSS) time integration algorithms

Wetter, Michael↗

Cascade Error Projection: A Learning Algorithm for Hardware Implementation

In this paper, we workout a detailed mathematical analysis for a new learning algorithm termed Cascade Error Projection (CEP) and a general learning frame work. This frame work can be used to obtain the cascade correlation learning algorithm by choosing a particular set of parameters. Furthermore, CEP learning algorithm is operated only on one layer, whereas the other set of weights can be calculated deterministically. In association with the dynamical stepsize change concept to convert the weight update from infinite space into a finite space, the relation between the current stepsize and the previous energy level is also given and the estimation procedure for optimal stepsize is used for validation of our proposed technique. The weight values of zero are used for starting the learning for every layer, and a single hidden unit is applied instead of using a pool of candidate hidden units similar to cascade correlation scheme. Therefore, simplicity in hardware implementation is also obtained. Furthermore, this analysis allows us to select from other methods (such as the conjugate gradient descent or the Newton's second order) one of which will be a good candidate for the learning technique. The choice of learning technique depends on the constraints of the problem (e.g., speed, performance, and hardware implementation); one technique may be more suitable than others. Moreover, for a discrete weight space, the theoretical analysis presents the capability of learning with limited weight quantization. Finally, 5- to 8-bit parity and chaotic time series prediction problems are investigated; the simulation results demonstrate that 4-bit or more weight quantization is sufficient for learning neural network using CEP. In addition, it is demonstrated that this technique is able to compensate for less bit weight resolution by incorporating additional hidden units. However, generation result may suffer somewhat with lower bit weight quantization.

Duong, Tuan A.↗

Waveform processing using neural network algorithms on the front-end electronics

In a multi-channel radiation detector readout system, waveform sampling, digitization, and raw data transmission to the data acquisition system constitute a conventional processing chain. The deposited energy on the sensor is estimated by extracting peak amplitudes, area under pulse envelopes from the raw data, and starting times of signals or time of arrivals. However, such quantities can be estimated using machine learning algorithms on the front-end Application-Specific Integrated Circuits (ASICs), often termed as “edge computing”. Edge computation offers enormous benefits, especially when the analytical forms are not fully known or the registered waveform suffers from noise and imperfections of practical implementations. In this work, we aim to predict peak amplitude from a single waveform snippet whose rising and falling edges containing only 3 to 4 samples. We thoroughly studied two well-accepted neural network algorithms, Multi-Layer Perceptron (MLP) and Convolutional Neural Network (CNN) by varying their model sizes. Further, to better fit front-end electronics, neural network model reduction techniques, such as network pruning methods and variable-bit quantization approaches, were also studied. By combining pruning and quantization, our best performing model has the size of 1.5 KB, reduced from 16.6 KB of its full model counterpart. It can reach mean absolute error of 0.034 comparing to that of a naive baseline of 0.135. Such parameter-efficient and predictive neural network models established feasibility and practicality of their deployment on front-end ASICs.

47 OTHER INSTRUMENTATION↗

Analytic and numerical vibronic spectra from quasi-classical trajectory ensembles

The truncated Wigner approximation to quantum dynamics in phase space is explored in the context of computing vibronic line shapes for monomer linear optical spectra. We consider multiple model potential forms including a shifted harmonic oscillator with both equal and unequal frequencies on the ground and excited state potentials as well as a shifted Morse potential model. For the equal-frequency shifted harmonic oscillator model, we derive an analytic expression for the exact vibronic line shape that emphasizes the importance of using a quantum mechanical distribution of phase space initial conditions. For the unequal-frequency shifted harmonic oscillator model, we are no longer able to obtain an exact expression for the vibronic line shape in terms of independent deterministic classical trajectories. We show how one can rigorously account for corrections to the truncated Wigner approximation through nonlinear responses of the line shape function to momentum fluctuations along a classical trajectory and demonstrate the qualitative improvement in the resulting spectrum when the leading-order quantum correction is included. Finally, we numerically simulate absorption spectra of a highly anharmonic shifted Morse potential model. We find that, while finite quantization and the dissociation limit are captured with reasonable accuracy, there is a qualitative breakdown of the quasi-classical trajectory ensemble’s ability to describe the vibronic line shape when the relative shift in Morse potentials becomes large. The work presented here provides clarity on the origin of unphysical negative features known to contaminate absorption spectra computed with quasi-classical trajectory ensembles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spectroscopic Investigation of Catalyst Inks and Thin Films Toward the Development of Ionomer Quality Control

As the production of polymer electrolyte fuel cells expands, novel quality control methods must be invented or adapted in order to support expected rates of production. Ensuring the quality of deposited catalyst layers is an essential step in the fuel cell manufacturing process, as the efficiency of a fuel cell is reliant on the catalyst layer being uniform at both the target platinum loading and the target ionomer content. Implementing a quality control method that is sensitive to these aspects is imperative, as wasting precious metals and other catalyst materials is expensive, and represents a potential barrier to entry into the field for manufacturers experimenting with novel deposition processes. In this work, we analyzed catalyst inks to determine if their ionomer content could be quantized spectroscopically. Attenuated total reflection (ATR) Fourier transform infrared spectroscopic technique was investigated producing a signal proportional to the ionomer content. ATR spectroscopy was able to quantitatively differentiate samples in which the ionomer to carbon mass ratio (I/C) varied between 0.9 and 3.0. The I/C ratio was correlated to the measured ATR signal near the CF 2 vibrational bands located between 1100 cm −1 and 1400 cm −1 . The experimental results obtained constitute a step toward the development of novel quality control methodologies for catalyst inks utilized by the fuel cell industry.

30 DIRECT ENERGY CONVERSION↗

Field control of quasiparticle decay in a quantum antiferromagnet

Dynamics in a quantum material is described by quantized collective motion: a quasiparticle. The single-quasiparticle description is useful for a basic understanding of the system, whereas a phenomenon beyond the simple description such as quasiparticle decay which affects the current carried by the quasiparticle is an intriguing topic. The instability of the quasiparticle is phenomenologically determined by the magnitude of the repulsive interaction between a single quasiparticle and the two-quasiparticle continuum. Although the phenomenon has been studied in several materials, thermodynamic tuning of the quasiparticle decay in a single material has not yet been investigated. Here we show, by using neutron scattering, magnetic field control of the magnon decay in a quantum antiferromagnet RbFeCl 3 , where the interaction between the magnon and continuum is tuned by the field. At low fields where the interaction is small, the single magnon decay process is observed. In contrast, at high fields where the interaction exceeds a critical magnitude, the magnon is pushed downwards in energy and its lifetime increases. Our study demonstrates that field control of quasiparticle decay is possible in the system where the two-quasiparticle continuum covers wide momentum-energy space, and the phenomenon of the magnon avoiding decay is ubiquitous.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Magnon damping in the zigzag phase of the Kitaev-Heisenberg- Γ model on a honeycomb lattice

We calculate dispersions and damping of the magnetic excitations in the model that is relevant to a description of the magnetic properties of iridium oxides α-Li 2 IrO 3 and Na 2 IrO 3 , and Ru-based materials such as α-RuCl 3 . Focusing on the parameter regime with the zigzag spin pattern in the ground state that is consistent with experiments, we are able to obtain explicit analytical expressions for magnon energies and eigenstates and go beyond the standard linear spin-wave theory approximation by calculating magnon damping and demonstrating its role in the dynamical structure factor. Here, we show that the magnon damping effects in both Born and self-consistent approximations are very significant, underscoring the importance of nonlinear magnon coupling in interpreting broad features in the neutron-scattering spectra.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Inducing Circularly Polarized Single-Photon Emission via Chiral-Induced Spin Selectivity

One of the central aims of the field of spintronics is the control of individual electron spins to effectively manage the transmission of quantized data. One well-known mechanism for controlling electronic spin transport is the chiral-induced spin-selectivity (CISS) effect in which a helical nanostructure imparts a preferential spin orientation on the electronic transport. One potential application of the CISS effect is as a transduction pathway between electronic spin and circularly polarized light within nonreciprocal photonic devices. Here in this work, we identify and quantify the degree of chiral-induced spin-selective electronic transport in helical polyaniline films using magnetoconductive atomic force microscopy (mcAFM). We then induce circularly polarized quantum light emission from CdSe/CdS core/shell quantum dots placed on these films, demonstrating a degree of circular polarization of up to ~21%. Utilizing time-resolved photoluminescence microscopy, we measure the radiative lifetime difference associated with left- and right-handed circular polarizations of single emitters. These lifetime differences, in combination with Kelvin probe mapping of the variation of surface potential with magnetization of the substrate, help establish an energy level diagram describing the spin-dependent transport pathways that enable the circularly polarized photoluminescence.

36 MATERIALS SCIENCE↗

Hydrogen Detection Strategies to Support H2@SCALE - The NREL Sensor Laboratory

Hydrogen represents a major pathway to decarbonize and stabilize the national and international energy industry and select manufacturing markets. To facilitate the development of hydrogen markets, the US Department of Energy initiated H2@Scale to bring together stakeholders to advance affordable hydrogen production, transport, storage, and utilization to increase revenue opportunities in multiple energy sectors. One major impediment to hydrogen implementation is cost. To expedite the use of hydrogen in energy and other markets, the United States announced in 2021 the Hydrogen Shot, which seeks to reduce the cost of clean hydrogen by 80% to $1 per 1 kilogram in 1 decade ("1 1 1"). As the cost of hydrogen drops, new applications will emerge that will require unique configurations of existing equipment and infrastructure, and eventually lead to advances in the generation and utilization of hydrogen. As the hydrogen economy expands, sensors and detection methods will need to adapt to changing infrastructure demands to address the primary targets of health & safety, emissions monitoring, and process control. The NREL Sensor Laboratory is playing a pivotal role in advancing the use of hydrogen sensors and detection methodologies in each of these categories to support DOE's mission for safe and efficient utilization in emerging markets. Health & safety monitors are required to ensure that operators and facilities can react to unintended hydrogen releases, either as GH2, LH2, or as a constituent of blends (e.g., natural gas or ammonia). Current detection methodologies focus on safety applications to detect near its lower flammable limit (4 vol %), and typically include point sensors in applications such as fixed or mobile detectors (e.g., personal gas monitors). Methodologies amenable for area detection include acoustic, emerging optical imaging methods, and flame detectors. Comparable detection strategies can be utilized for emissions monitoring and quantization, however few methods can simultaneously cover both low (emissions) and high (health & safety) levels. Deployment of emission level detectors will be required to 1) reduce product loss through small but potentially significant leaks from an environmental or cost perspective, 2) reduce downtime of high demand systems by early identification of eminent system failures (leaks through pump or compressor seals indicative of impending failure), and 3) address potential emission monitoring requirements that may be set by regulating bodies. The first two points should be adopted by industry to reduce the cost-of-goods-sold. The third main category for hydrogen detection relates to process control and may be advantageous for many existing applications. Two main applications are emerging. For example, the purity requirements for hydrogen that is dispensed from refueling systems for hydrogen fuel cell electric vehicles (FCEV) is rigorously regulated by the Standard SAE J2719, which prescribes maximum allowable levels of multiple impurities in the hydrogen fuel and must be verified by a regulatory body. Hydrogen contaminant detectors (HCD) integrated to the fueling station can assure this compliance. HCDs must be able operate in 100% H2 backgrounds and be able to distinguish between multiple contaminants at low ppm to low ppb levels. Secondly, as a strategy to decarbonize the natural gas grid, there are proposals to blend hydrogen with natural gas. This blending will affect transport applications (pipeline infrastructure), stationary combustion systems (turbines), and consumer and commercial appliances. In the short-term, hydrogen levels up to 20% are proposed. Variations in the hydrogen level can have dramatic impact on the combustion process and on the potential response of safety sensors. These mixtures may be regulated so that the concentration at a delivery point must be monitored with high precision. However, routine maintenance may introduce background gases such as ambient air (with water) or maintenance gases (introduced with welding processes or adhesive outgassing.) Therefore, the detection methodology must be robust enough to recover or respond to various contaminants. Several reviews can be found in literature addressing sensing and detection technologies, including their limitations and applications. However, for most applications, limitations can be alleviated by combining various detection techniques either through system integration or implementation of machine learning methods (artificial intelligence). In this presentation, we will discuss several applications, highlight their current approach for hydrogen detection, and suggest detection strategies to supplement their limitations.

ENERGY STORAGE,HYDROGEN↗

Casimir force on a light front

Depending on the point of view, the Casimir force arises from variation in the energy of the quantum vacuum as boundary conditions are altered or as an interaction between atoms in the materials that form these boundary conditions. Standard analyses of such configurations are usually done in terms of ordinary, equal-time (Minkowski) coordinates. However, physics is independent of the coordinate choice, and an analysis based on light-front coordinates, where x + ≡ t + z / c plays the role of time, is equally valid. After a brief historical introduction, we illustrate and compare equal-time and light-front calculations of the Casimir force.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Electrochemical and Optical Spectroscopic Probing of Transition–Sized Au 130 (SR) 50 Nanoclusters

Ultrasmall metal nanoclusters (NCs) exhibit a quantized conduction band, hence, a distinct HOMO-LUMO gap (E g ). Such a quantized electronic structure gives rise to multiple discrete peaks in the optical absorption spectrum of the NCs. As the size grows to 130 gold atoms (Au 130 protected by ligands), electrical charging and optical behaviors seem to show certain metal-like features (hence, transition-sizes). To probe such behaviors, especially the potential ligand effect, we have devised the synthesis of Au 130 NCs protected by phenylethanethiolate and naphthalenethiolate, respectively, with the former having a nonconjugated separation between the aromatic molecular group and the metal core while the latter being in direct bonding. A careful comparison of these two Au 130 nanoclusters with the earlier reported analogues is carried out, including the structurally characterized Au 130 (pMBT) 50 and the aqueous counterpart. While all of these nanoclusters possess the same 80 free electron counts in the core, some notable differences in electrochemical and optical properties are found, which are attributed to the ligand effects. The obtained insights may stimulate further interest in the transition-sized nanoclusters and also promote their applications in optics, energy conversion, and biomedicine.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interplay of superconducting, metallic, and crystalline states of composite fermions at 𝜈 = $\frac{1}{6}$ in wide quantum wells

Evidence for developing fractional quantum Hall effect (FQHE) at filling fraction 𝜈 = 1/6 and 1/8 was recently reported in wide GaAs quantum wells [Wang et al., Phys. Rev. Lett. 134, 046502 (2025)]. In this article, we theoretically investigate the nature of the state at 𝜈 = 1/6 as a function of the quantum well width and the density by considering composite-fermion (CF) crystals, CF Fermi sea, and various kinds of paired CF states. The 𝑓-wave paired state has the lowest energy among the paired CF states. However, for parameters of interest, the energies of the CF crystal, the CF Fermi liquid, and the 𝑓-wave paired CF state are too close to distinguish. We, therefore, predict that 𝑖𝑓 the FQHE at 𝜈 = 1/6 is experimentally confirmed, this state would be an 𝑓-wave paired state of CFs, which can be verified by measurement of its thermal Hall conductance. Exact diagonalization studies on clean systems with up to eight electrons show that the ground states at 𝜈 = 𝑛/(6⁢𝑛 ± 1) are incompressible for all widths and densities we have considered, and are well described by the corresponding Laughlin and Jain states. We propose a phase diagram for large quantum well widths and densities in which at zero disorder, incompressible FQHE states are stabilized at 𝜈 = 𝑛/(6⁢𝑛 ± 1) and 𝜈 = 1/6, but in between these fillings the CF crystal is stabilized. We also present a qualitative discussion on the effects of disorder and propose a schematic phase diagram based on it. With disorder, which creates a spatial variation in the filling factor, two regimes are identified: (i) for small disorder, when the incompressible states percolate at the special fillings, FQHE with quantized Hall plateaus and vanishing longitudinal resistance should occur; and (ii) for larger disorder, when the CF crystal percolates, the longitudinal resistance rises with decreasing temperature but the domains of FQHE liquid produce minima at the special filling factors. Here, experiments are consistent with the latter scenario. We also mention a possible connection of the phase diagram presented here to a puzzling behavior observed for the fractional quantum anomalous Hall effect in pentalayer graphene.

Composite fermions↗

Quantum Information for Fusion Energy Sciences (Final Technical Report)

The simulation of plasma dynamics is a critical area of Fusion Energy Sciences (FES) due to it’s usefulness in predicting, controlling, and confining plasmas in the context of potential fusion reactors. The simulation of plasmas is a computationally difficult problem in both classical and quantum physics, motivating investigation into the potential of quantum computers to simulate these systems. This project took several concrete steps towards this goal by developing tools for improving the control, characterization, and calibration of quantum gates on a superconducting quantum computer, developing error suppression and mitigation tools to reduce errors on the quantum computer, and utilizing these advancements to simulate reduced models of plasma dynamics on the quantum computer. In order to efficiently simulate plasma physics, an optimal control method which synthesizes, directly at the pulse level, any quantum gate on qubit and qutrit systems was developed. Using four superconducting transmon quantum processors at Rigetti and LLNL, it was demonstrated that any arbitrary quantum gate on qubits and qutrits could be implemented with high fidelity, leading to a significantly reduced length of a gate sequence. A problem of interest in FES is the nonlinear optical process of laser pulse compression within a plasma. Since quantum physics is linear, simulating nonlinear operations is not naturally feasible on a quantum computer, however it is possible to simulated a quantized version of the nonlinear process. A quantization approach to convert nonlinear wave-wave interaction problems to Hamiltonian simulation problems was developed and demonstrated using two qubits on a Rigetti device. In this experiment, a number of error suppression and mitigation techniques were investigated to determine how best to utilize the finite quantum resources. This study provides an example of how plasma problems may be solved on near-term, noisy quantum computing platforms and identified a promising set of techniques. Building on the insights of these experiments, the investigation turned to linear electron-plasma wave physics. A connection was identified between a local one-dimensional lattice spin model and linear wave phenomena, allowing a plasma physics problem to be efficiently mapped to the quantum computer. In this framework, reflection and transmission of plasma waves at a sharp boundary was studied, as well as the propagation of waves through an inhomogeneous plasma medium. In addition to the suite of error suppression and mitigation techniques developed, this experiment introduced the use of a digital-analog gate scheme designed to efficiently simulate the plasma Hamiltonian. With hardware available at the conclusion of the project, simulation at the scale of 9 qubits and 15 timesteps (60 entangling layers) was achieved.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Analytic rate theory of polariton relaxation that explains long polariton lifetime

Hybridization of a molecular exciton with a quantized photon creates a polariton. Despite extensive experimental investigations, the apparent lifetime of the exciton–polariton is not well-understood. For this work, we examined the steady-state population dynamics for a Holstein–Tavis–Cumming Hamiltonian to illuminate the long-term polaritonic dynamics and lifetime of the exciton–polariton in an optical cavity. For a realistic description of polariton relaxation, cavity loss and various exciton decay channels are included in the model. We found that in the presence of weak but finite exciton loss, the apparent lifetime of the lower polariton coincides with the out-of-cavity exciton lifetime and is independent of cavity-matter detuning. This is a simple explanation for the experimentally observed lifetimes for exciton polaritons and theoretically justifies the dark state reservoir hypothesis. Furthermore, if the upper polariton is initially populated, the system reaches the steady state very quickly, leading to single-exponential polariton relaxation. Starting from the lower polariton leads to a longer pre-steady-state time period, leading to double-exponential relaxation. Finally, we considered the effect of site orientational disorders and the exciton frequency disorderers. Under the collective limit, the effects of this disorder can be included in Fermi’s golden rule population dynamics without explicit sampling. For the exciton energy disorders, numerical calculations are needed. Our theoretical framework is applicable to interpret exciton–polariton experiments, especially related to the measured apparent lifetime of polaritons.

Chemical dynamics↗