Abstract Interaction between light and matter results in new quantum states whose energetics can modify chemical kinetics. In the regime of ensemble vibrational strong coupling (VSC), a macroscopic number$$N$$ of molecular transitions couple to each resonant cavity mode, yielding two hybrid light–matter (polariton) modes and a reservoir of$$N-1$$ dark states whose chemical dynamics are essentially those of the bare molecules. This fact is seemingly in opposition to the recently reported modification of thermally activated ground electronic state reactions under VSC. Here we provide a VSC Marcus–Levich–Jortner electron transfer model that potentially addresses this paradox: although entropy favors the transit through dark-state channels, the chemical kinetics can be dictated by a few polaritonic channels with smaller activation energies. The effects of catalytic VSC are maximal at light–matter resonance, in agreement with experimental observations.
more »
« less
Cavity induced collective behavior in the polaritonic ground state
Cavity quantum electrodynamics provides an ideal platform to engineer and control light-matter interactions with polariton quasiparticles. In this work, we investigate collective phenomena in a system of many particles in a harmonic trap coupled to a homogeneous cavity vacuum field. The system couples collectively to the cavity field, through its center of mass, and collective polariton states emerge. The cavity field mediates pairwise long-range interactions and enhances the effective mass of the particles. This leads to an enhancement of localization in the matter ground state density, which features a maximum when light and matter are on resonance, and demonstrates a Dicke-like, collective behavior with the particle number. The light-matter interaction also modifies the photonic properties of the polariton system, as the ground state is populated with bunched photons. In addition, it is shown that the diamagneticA^2 term is necessary for the stability of the system, as otherwise the superradiant ground state instability occurs. We demonstrate that coherent transfer of polaritonic population is possible with an external magnetic field and by monitoring the Landau-Zener transition probability.
more »
« less
- Award ID(s):
- 2116679
- PAR ID:
- 10516808
- Publisher / Repository:
- SciPost
- Date Published:
- Journal Name:
- SciPost Physics
- Volume:
- 14
- Issue:
- 6
- ISSN:
- 2542-4653
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract We investigate electroabsorption (EA) in organic semiconductor microcavities to understand whether strong light-matter coupling non-trivially alters their nonlinear optical [$${\chi }^{(3)}\left(\omega,{{{{\mathrm{0,0}}}}}\right)$$ ] response. Focusing on strongly-absorbing squaraine (SQ) molecules dispersed in a wide-gap host matrix, we find that classical transfer matrix modeling accurately captures the EA response of low concentration SQ microcavities with a vacuum Rabi splitting of$$\hslash \Omega \approx 200$$ meV, but fails for high concentration cavities with$$\hslash \Omega \approx 420$$ meV. Rather than new physics in the ultrastrong coupling regime, however, we attribute the discrepancy at high SQ concentration to a nearly dark H-aggregate state below the SQ exciton transition, which goes undetected in the optical constant dispersion on which the transfer matrix model is based, but nonetheless interacts with and enhances the EA response of the lower polariton mode. These results indicate that strong coupling can be used to manipulate EA (and presumably other optical nonlinearities) from organic microcavities by controlling the energy of polariton modes relative to other states in the system, but it does not alter the intrinsic optical nonlinearity of the organic semiconductor inside the cavity.more » « less
-
Abstract The nature of dark matter remains unresolved in fundamental physics. Weakly Interacting Massive Particles (WIMPs), which could explain the nature of dark matter, can be captured by celestial bodies like the Sun or Earth, leading to enhanced self-annihilation into Standard Model particles including neutrinos detectable by neutrino telescopes such as the IceCube Neutrino Observatory. This article presents a search for muon neutrinos from the center of the Earth performed with 10 years of IceCube data using a track-like event selection. We considered a number of WIMP annihilation channels ($$\chi \chi \rightarrow \tau ^+\tau ^-$$ /$$W^+W^-$$ /$$b\bar{b}$$ ) and masses ranging from 10 GeV to 10 TeV. No significant excess over background due to a dark matter signal was found while the most significant result corresponds to the annihilation channel$$\chi \chi \rightarrow b\bar{b}$$ for the mass$$m_{\chi }=250$$ GeV with a post-trial significance of$$1.06\sigma $$ . Our results are competitive with previous such searches and direct detection experiments. Our upper limits on the spin-independent WIMP scattering are world-leading among neutrino telescopes for WIMP masses$$m_{\chi }>100$$ GeV.more » « less
-
Abstract A model based on a$$U(1)_{T^3_R}$$ extension of the Standard Model can address the mass hierarchy between generations of fermions, explain thermal dark matter abundance, and the muon$$g - 2$$ ,$$R_{(D)}$$ , and$$R_{(D^*)}$$ anomalies. The model contains a light scalar boson$$\phi '$$ and a heavy vector-like quark$$\chi _\textrm{u}$$ that can be probed at CERN’s large hadron collider (LHC). We perform a phenomenology study on the production of$$\phi '$$ and$${\chi }_u$$ particles from proton–proton$$(\textrm{pp})$$ collisions at the LHC at$$\sqrt{s}=13.6$$ TeV, primarily through$$g{-g}$$ and$$t{-\chi _\textrm{u}}$$ fusion. We work under a simplified model approach and directly take the$$\chi _\textrm{u}$$ and$$\phi '$$ masses as free parameters. We perform a phenomenological analysis considering$$\chi _\textrm{u}$$ final states to b-quarks, muons, and neutrinos, and$$\phi '$$ decays to$$\mu ^+\mu ^-$$ . A machine learning algorithm is used to maximize the signal sensitivity, considering an integrated luminosity of 3000$$\text {fb}^{-1}$$ . The proposed methodology can be a key mode for discovery over a large mass range, including low masses, traditionally considered difficult due to experimental constraints.more » « less
-
Abstract Ultra-pure NaI(Tl) crystals are the key element for a model-independent verification of the long standing DAMA result and a powerful means to search for the annual modulation signature of dark matter interactions. The SABRE collaboration has been developing cutting-edge techniques for the reduction of intrinsic backgrounds over several years. In this paper we report the first characterization of a 3.4 kg crystal, named NaI-33, performed in an underground passive shielding setup at LNGS. NaI-33 has a record low$$^{39}$$ K contamination of 4.3 ± 0.2 ppb as determined by mass spectrometry. We measured a light yield of 11.1 ± 0.2 photoelectrons/keV and an energy resolution of 13.2% (FWHM/E) at 59.5 keV. We evaluated the activities of$$^{226}$$ Ra and$$^{228}$$ Th inside the crystal to be$$5.9\pm 0.6~\upmu $$ Bq/kg and$$1.6\pm 0.3~\upmu $$ Bq/kg, respectively, which would indicate a contamination from$$^{238}$$ U and$$^{232}$$ Th at part-per-trillion level. We measured an activity of 0.51 ± 0.02 mBq/kg due to$$^{210}$$ Pb out of equilibrium and a$$\alpha $$ quenching factor of 0.63 ± 0.01 at 5304 keV. We illustrate the analyses techniques developed to reject electronic noise in the lower part of the energy spectrum. A cut-based strategy and a multivariate approach indicated a rate, attributed to the intrinsic radioactivity of the crystal, of$$\sim $$ 1 count/day/kg/keV in the [5–20] keV region.more » « less
An official website of the United States government

