Browse
Submit Data
Databases
API
Help

Dataset Information

25 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Quantum electrodynamics at room temperature coupling a single vibrating molecule with a plasmonic nanocavity.

ABSTRACT: Interactions between a single emitter and cavity provide the archetypical system for fundamental quantum electrodynamics. Here we show that a single molecule of Atto647 aligned using DNA origami interacts coherently with a sub-wavelength plasmonic nanocavity, approaching the cooperative regime even at room temperature. Power-dependent pulsed excitation reveals Rabi oscillations, arising from the coupling of the oscillating electric field between the ground and excited states. The observed single-molecule fluorescent emission is split into two modes resulting from anti-crossing with the plasmonic mode, indicating the molecule is strongly coupled to the cavity. The second-order correlation function of the photon emission statistics is found to be pump wavelength dependent, varying from g(2)(0) = 0.4 to 1.45, highlighting the influence of vibrational relaxation on the Jaynes-Cummings ladder. Our results show that cavity quantum electrodynamic effects can be observed in molecular systems at ambient conditions, opening significant potential for device applications.

SUBMITTER: Ojambati OS

PROVIDER: S-EPMC6400948 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Single-molecule strong coupling at room temperature in plasmonic nanocavities.

Project description:Photon emitters placed in an optical cavity experience an environment that changes how they are coupled to the surrounding light field. In the weak-coupling regime, the extraction of light from the emitter is enhanced. But more profound effects emerge when single-emitter strong coupling occurs: mixed states are produced that are part light, part matter1, 2, forming building blocks for quantum information systems and for ultralow-power switches and lasers. Such cavity quantum electrodynamics has until now been the preserve of low temperatures and complicated fabrication methods, compromising its use. Here, by scaling the cavity volume to less than 40 cubic nanometres and using host–guest chemistry to align one to ten protectively isolated methylene-blue molecules, we reach the strong-coupling regime at room temperature and in ambient conditions. Dispersion curves from more than 50 such plasmonic nanocavities display characteristic light–matter mixing, with Rabi frequencies of 300 millielectronvolts for ten methylene-blue molecules, decreasing to 90 millielectronvolts for single molecules—matching quantitative models. Statistical analysis of vibrational spectroscopy time series and dark-field scattering spectra provides evidence of single-molecule strong coupling. This dressing of molecules with light can modify photochemistry, opening up the exploration of complex natural processes such as photosynthesis and the possibility of manipulating chemical bonds.

| S-EPMC4947385 | biostudies-literature

Ultrastrong Coupling of a Single Molecule to a Plasmonic Nanocavity: A First-Principles Study.

Project description:Ultrastrong coupling (USC) is a distinct regime of light-matter interaction in which the coupling strength is comparable to the resonance energy of the cavity or emitter. In the USC regime, common approximations to quantum optical Hamiltonians, such as the rotating wave approximation, break down as the ground state of the coupled system gains photonic character due to admixing of vacuum states with higher excited states, leading to ground-state energy changes. USC is usually achieved by collective coherent coupling of many quantum emitters to a single mode cavity, whereas USC with a single molecule remains challenging. Here, we show by time-dependent density functional theory (TDDFT) calculations that a single organic molecule can reach USC with a plasmonic dimer, consisting of a few hundred atoms. In this context, we discuss the capacity of TDDFT to represent strong coupling and its connection to the quantum optical Hamiltonian. We find that USC leads to appreciable ground-state energy modifications accounting for a non-negligible part of the total interaction energy, comparable to k B T at room temperature.

| S-EPMC8931765 | biostudies-literature

Strong vibrational coupling in room temperature plasmonic resonators.

Project description:Strong vibrational coupling has been realized in a variety of mechanical systems. However, there have been no experimental observations of strong coupling of the acoustic modes of plasmonic nanostructures, due to rapid energy dissipation in these systems. Here we realized strong vibrational coupling in ultra-high frequency plasmonic nanoresonators by increasing the vibrational quality factors by an order of magnitude. We achieved the highest frequency quality factor products of f × Q = 1.0 × 1013 Hz for the fundamental mechanical modes, which exceeds the value of 0.6 × 1013 Hz required for ground state cooling. Avoided crossing was observed between vibrational modes of two plasmonic nanoresonators with a coupling rate of g = 7.5 ± 1.2 GHz, an order of magnitude larger than the dissipation rates. The intermodal strong coupling was consistent with theoretical calculations using a coupled oscillator model. Our results enabled a platform for future observation and control of the quantum behavior of phonon modes in metallic nanoparticles.

| S-EPMC6449381 | biostudies-literature

A Programmable DNA-Silicification-Based Nanocavity for Single-Molecule Plasmonic Sensing.

Project description:Plasmonic nanocavities are highly desirable for optical sensing because of their singular ability to confine light into deep subwavelength volumes. Yet, it remains profoundly challenging to fabricate structurally resilient nanocavities with high fidelity, and to obtain direct, noninvasive visualization of the plasmonic hotspots within such constructs. Herein, highly precise and robust nanocavities, entitled DNA-silicified template for Raman optical beacon (DNA-STROBE), are engineered by using silicified DNA scaffolds for spatial organization of discrete plasmonic nanoparticles. In addition to substantially enhancing structural stability and chemical inertness, DNA silicification significantly improves nanogap control, resulting simultaneously in large and controlled local electromagnetic field enhancement. The ultrasmall mode volume of the DNA-STROBE constructs promotes single-molecule occupancy enabling surface-enhanced Raman spectroscopy (SERS) observations of single-molecule activity even at elevated background concentration, significantly relaxing the restrictive pico- to nanomolar molecular concentration condition typically required for such investigations. Additionally, leveraging super-resolution SERS measurements allows noninvasive and diffraction-unlimited spatial profiling of otherwise unresolvable plasmonic hotspots. The highly programmable and reproducible nature of the DNA-STROBE, coupled with its quantitative label-free molecular readouts, provides a versatile platform with applications across the spectrum of nanophotonics and biomedical sciences.

| S-EPMC8275373 | biostudies-literature

Quantum interference effects at room temperature in OPV-based single-molecule junctions.

Project description:Interference effects on charge transport through an individual molecule can lead to a notable modulation and suppression on its conductance. In this letter, we report the observation of quantum interference effects occurring at room temperature in single-molecule junctions based on oligo(3)-phenylenevinylene (OPV3) derivatives, in which the central benzene ring is coupled to either para- or meta-positions. Using the break-junction technique, we find that the conductance for a single meta-OPV3 molecule wired between gold electrodes is one order of magnitude smaller than that of a para-OPV3 molecule. Theoretical calculations confirm the occurrence of constructive and destructive interference in the para- and meta-OPV3 molecules respectively, which arises from the phase difference of the transmission coefficients through the molecular orbitals.

| S-EPMC3663707 | biostudies-literature

Colloidal quantum dot molecules manifesting quantum coupling at room temperature.

Project description:Coupling of atoms is the basis of chemistry, yielding the beauty and richness of molecules. We utilize semiconductor nanocrystals as artificial atoms to form nanocrystal molecules that are structurally and electronically coupled. CdSe/CdS core/shell nanocrystals are linked to form dimers which are then fused via constrained oriented attachment. The possible nanocrystal facets in which such fusion takes place are analyzed with atomic resolution revealing the distribution of possible crystal fusion scenarios. Coherent coupling and wave-function hybridization are manifested by a redshift of the band gap, in agreement with quantum mechanical simulations. Single nanoparticle spectroscopy unravels the attributes of coupled nanocrystal dimers related to the unique combination of quantum mechanical tunneling and energy transfer mechanisms. This sets the stage for nanocrystal chemistry to yield a diverse selection of coupled nanocrystal molecules constructed from controlled core/shell nanocrystal building blocks. These are of direct relevance for numerous applications in displays, sensing, biological tagging and emerging quantum technologies.

| S-EPMC6915722 | biostudies-literature

Single molecule quantum-confined Stark effect measurements of semiconductor nanoparticles at room temperature.

Project description:We measured the quantum-confined Stark effect (QCSE) of several types of fluorescent colloidal semiconductor quantum dots and nanorods at the single molecule level at room temperature. These measurements demonstrate the possible utility of these nanoparticles for local electric field (voltage) sensing on the nanoscale. Here we show that charge separation across one (or more) heterostructure interface(s) with type-II band alignment (and the associated induced dipole) is crucial for an enhanced QCSE. To further gain insight into the experimental results, we numerically solved the Schrödinger and Poisson equations under self-consistent field approximation, including dielectric inhomogeneities. Both calculations and experiments suggest that the degree of initial charge separation (and the associated exciton binding energy) determines the magnitude of the QCSE in these structures.

| S-EPMC3507316 | biostudies-literature

Room-Temperature Strong Coupling of CdSe Nanoplatelets and Plasmonic Hole Arrays.

Project description:Exciton polaritons are hybrid light-matter quasiparticles that can serve as coherent light sources. Motivated by applications, room-temperature realization of polaritons requires narrow, excitonic transitions with large transition dipoles. Such transitions must then be strongly coupled to an electromagnetic mode confined in a small volume. While much work has explored polaritons in organic materials, semiconductor nanocrystals present an alternative excitonic system with enhanced photostability and spectral tunability. In particular, quasi-two-dimensional nanocrystals known as nanoplatelets (NPLs) exhibit intense, spectrally narrow excitonic transitions useful for polariton formation. Here, we place CdSe NPLs on silver hole arrays to demonstrate exciton-plasmon polaritons at room temperature. Angle-resolved reflection spectra reveal Rabi splittings up to 149 meV for the polariton states. We observe bright, polarized emission arising from the lowest polariton state. Furthermore, we assess the dependence of the Rabi splitting on the hole-array pitch and the number N of NPLs. While the pitch determines the in-plane momentum for which strong coupling is observed, it does not affect the size of the splitting. The Rabi splitting first increases with NPL film thickness before eventually saturating. Instead of the commonly used [Formula: see text] dependence, we develop an analytical expression that includes the transverse confinement of the plasmon modes to describe the measured Rabi splitting as a function of NPL film thickness.

| S-EPMC6578340 | biostudies-literature

Strong coupling and induced transparency at room temperature with single quantum dots and gap plasmons.

Project description:Coherent coupling between plasmons and transition dipole moments in emitters can lead to two distinct spectral effects: vacuum Rabi splitting at strong coupling strengths, and induced transparency (also known as Fano interference) at intermediate coupling strengths. Achieving either strong or intermediate coupling between a single emitter and a localized plasmon resonance has the potential to enable single-photon nonlinearities and other extreme light-matter interactions, at room temperature and on the nanometer scale. Both effects produce two peaks in the spectrum of scattering from the plasmon resonance, and can thus be confused if scattering measurements alone are performed. Here we report measurements of scattering and photoluminescence from individual coupled plasmon-emitter systems that consist of a single colloidal quantum dot in the gap between a gold nanoparticle and a silver film. The measurements unambiguously demonstrate weak coupling (the Purcell effect), intermediate coupling (Fano interference), and strong coupling (Rabi splitting) at room temperature.

| S-EPMC6167320 | biostudies-literature

A Single Hydrogen Molecule as an Intensity Chopper in an Electrically Driven Plasmonic Nanocavity.

Project description:Photon statistics is a powerful tool for characterizing the emission dynamics of nanoscopic systems and their photophysics. Recent advances that combine correlation spectroscopy with scanning tunneling microscopy induced luminescence (STML) have allowed the measurement of the emission dynamics from individual molecules and defects, demonstrating their nature as single-photon emitters. The application of correlation spectroscopy to the analysis of the dynamics of a well-characterized adsorbate system in an ultrahigh vacuum remained to be demonstrated. Here, we combine single-photon time correlations with STML to measure the dynamics of individual H2 molecules between a gold tip and an Au(111) surface. An adsorbed H2 molecule performs recurrent excursions below the tip apex. We use the fact that the presence of the H2 molecule in the junction modifies plasmon emission to study the adsorbate dynamics. Using the H2 molecule as a chopper for STM-induced optical emission intensity, we demonstrate bunching in the plasmonic photon train in a single measurement over 6 orders of magnitude in the time domain (from microseconds to seconds) that takes only a few seconds. Our findings illustrate the power of using photon statistics to measure the diffusion dynamics of adsorbates with STML.

| S-EPMC6517280 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data