Browse
Submit Data
Databases
API
Help

Dataset Information

0 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Quantum Beats and Coherence Decay in Degenerate States Split by Solvation.

ABSTRACT: Coherent dynamics of degenerate quantum states symmetry-broken on the femtosecond timescale is found to exhibit the phenomenon of quantum beats. Frequency-resolved and polarization-selective heterodyned transient grating spectroscopy enabled us to retrieve the oscillation pattern characteristic of the beating in systems undergoing ultrafast dynamical processes. This methodology applies to the general phenomena of coherence dynamics which is important in any ultrafast multidimensional spectroscopy. A particular application to the vibrational spectroscopy of coherence in the degenerate normal modes of the tricyanomethanide anion solvated in water is explored in this study. The relaxation of the cross-polarization transient grating anisotropy is shown to reflect the loss of the vibrational coherence, which is caused by ultrafast dynamics of the water solvation shell.

SUBMITTER: Chuntonov L

PROVIDER: S-EPMC3743118 | biostudies-literature | 2013 Jun

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Publications

Quantum Beats and Coherence Decay in Degenerate States Split by Solvation.

Chuntonov Lev L Kuroda Daniel G DG Ghosh Ayanjeet A Ma Jianqiang J Hochstrasser Robin M RM

The journal of physical chemistry letters 20130601 11

Coherent dynamics of degenerate quantum states symmetry-broken on the femtosecond timescale is found to exhibit the phenomenon of quantum beats. Frequency-resolved and polarization-selective heterodyned transient grating spectroscopy enabled us to retrieve the oscillation pattern characteristic of the beating in systems undergoing ultrafast dynamical processes. This methodology applies to the general phenomena of coherence dynamics which is important in any ultrafast multidimensional spectroscop ...[more]

PMID: 23956817

Similar Datasets

Quantum coherence of steered states.

Project description:Lying at the heart of quantum mechanics, coherence has recently been studied as a key resource in quantum information theory. Quantum steering, a fundamental notion originally considered by Schödinger, has also recently received much attention. When Alice and Bob share a correlated quantum system, Alice can perform a local measurement to 'steer' Bob's reduced state. We introduce the maximal steered coherence as a measure describing the extent to which steering can remotely create coherence; more precisely, we find the maximal coherence of Bob's steered state in the eigenbasis of his original reduced state, where maximization is performed over all positive-operator valued measurements for Alice. We prove that maximal steered coherence vanishes for quantum-classical states whilst reaching a maximum for pure entangled states with full Schmidt rank. Although invariant under local unitary operations, maximal steered coherence may be increased when Bob performs a channel. For a two-qubit state we find that Bob's channel can increase maximal steered coherence if and only if it is neither unital nor semi-classical, which coincides with the condition for increasing discord. Our results show that the power of steering for coherence generation, though related to discord, is distinct from existing measures of quantum correlation.

| S-EPMC4726079 | biostudies-other

Observation of Ultrafast Coherence Transfer and Degenerate States with Polarization-Controlled Two-Dimensional Electronic Spectroscopy.

Project description:Optical spectroscopy is a powerful tool to interrogate quantum states of matter. We present simulation results for the cross-polarized two-dimensional electronic spectra of the light-harvesting system LH2 of purple bacteria. We identify a spectral feature on the diagonal, which we assign to ultrafast coherence transfer between degenerate states. The implication for the interpretation of previous experiments on different systems and the potential use of this feature are discussed. In particular, we foresee that this kind of feature will be useful for identifying mixed degenerate states and for identifying the origin of symmetry breaking disorder in systems like LH2. Furthermore, this may help identify both vibrational and electronic states in biological systems such as proteins and solid-state materials such as hybrid perovskites.

| S-EPMC7586392 | biostudies-literature

Odd Integer Quantum Hall States with Interlayer Coherence in Twisted Bilayer Graphene.

Project description:We report on the quantum Hall effect in two stacked graphene layers rotated by 2°. The tunneling strength among the layers can be varied from very weak to strong via the mechanism of magnetic breakdown when tuning the density. Odd-integer quantum Hall physics is not anticipated in the regime of suppressed tunneling for balanced layer densities, yet it is observed. We interpret this as a signature of Coulomb interaction induced interlayer coherence and Bose-Einstein condensation of excitons that form at half filling of each layer. A density imbalance gives rise to reentrant behavior due to a phase transition from the interlayer coherent state to incompressible behavior caused by simultaneous condensation of both layers in different quantum Hall states. With increasing overall density, magnetic breakdown gains the upper hand. As a consequence of the enhanced interlayer tunneling, the interlayer coherent state and the phase transition vanish.

| S-EPMC8289309 | biostudies-literature

Ultrafast quantum beats of anisotropic excitons in atomically thin ReS2.

Project description:Quantum beats, periodic oscillations arising from coherent superposition states, have enabled exploration of novel coherent phenomena. Originating from strong Coulomb interactions and reduced dielectric screening, two-dimensional transition metal dichalcogenides exhibit strongly bound excitons either in a single structure or hetero-counterpart; however, quantum coherence between excitons is barely known to date. Here we observe exciton quantum beats in atomically thin ReS2 and further modulate the intensity of the quantum beats signal. Surprisingly, linearly polarized excitons behave like a coherently coupled three-level system exhibiting quantum beats, even though they exhibit anisotropic exciton orientations and optical selection rules. Theoretical studies are also provided to clarify that the observed quantum beats originate from pure quantum coherence, not from classical interference. Furthermore, we modulate on/off quantum beats only by laser polarization. This work provides an ideal laboratory toward polarization-controlled exciton quantum beats in two-dimensional materials.

| S-EPMC5783952 | biostudies-literature

Fermi-edge superfluorescence from a quantum-degenerate electron-hole gas.

Project description:Nonequilibrium can be a source of order. This rather counterintuitive statement has been proven to be true through a variety of fluctuation-driven, self-organization behaviors exhibited by out-of-equilibrium, many-body systems in nature (physical, chemical, and biological), resulting in the spontaneous appearance of macroscopic coherence. Here, we report on the observation of spontaneous bursts of coherent radiation from a quantum-degenerate gas of nonequilibrium electron-hole pairs in semiconductor quantum wells. Unlike typical spontaneous emission from semiconductors, which occurs at the band edge, the observed emission occurs at the quasi-Fermi edge of the carrier distribution. As the carriers are consumed by recombination, the quasi-Fermi energy goes down toward the band edge, and we observe a continuously red-shifting streak. We interpret this emission as cooperative spontaneous recombination of electron-hole pairs, or superfluorescence (SF), which is enhanced by Coulomb interactions near the Fermi edge. This novel many-body enhancement allows the magnitude of the spontaneously developed macroscopic polarization to exceed the maximum value for ordinary SF, making electron-hole SF even more "super" than atomic SF.

| S-EPMC3836032 | biostudies-literature

Persistent Inter-Excitonic Quantum Coherence in CdSe Quantum Dots.

Project description:The creation and manipulation of quantum superpositions is a fundamental goal for the development of materials with novel optoelectronic properties. In this letter, we report persistent (~80 fs lifetime) quantum coherence between the 1S and 1P excitonic states in zinc-blende colloidal CdSe quantum dots at room temperature, measured using Two-Dimensional Electronic Spectroscopy. We demonstrate that this quantum coherence manifests as an intradot phenomenon, the frequency of which depends on the size of the dot excited within the ensemble of QDs. We model the lifetime of the coherence and demonstrate that correlated interexcitonic fluctuations preserve relative phase between excitonic states. These observations suggest an avenue for engineering long-lived interexcitonic quantum coherence in colloidal quantum dots.

| S-EPMC3976995 | biostudies-literature

Low-temperature thermodynamics with quantum coherence.

Project description:Thermal operations are an operational model of non-equilibrium quantum thermodynamics. In the absence of coherence between energy levels, exact state transition conditions under thermal operations are known in terms of a mathematical relation called thermo-majorization. But incorporating coherence has turned out to be challenging, even under the relatively tractable model wherein all Gibbs state-preserving quantum channels are included. Here we find a mathematical generalization of thermal operations at low temperatures, 'cooling maps', for which we derive the necessary and sufficient state transition condition. Cooling maps that saturate recently discovered bounds on coherence transfer are realizable as thermal operations, motivating us to conjecture that all cooling maps are thermal operations. Cooling maps, though a less-conservative generalization to thermal operations, are more tractable than Gibbs-preserving operations, suggesting that cooling map-like models at general temperatures could be of use in gaining insight about thermal operations.

| S-EPMC4506506 | biostudies-literature

Revealing Ultrafast Population Transfer between Nearly Degenerate Electronic States.

Project description:The response of a molecule to photoexcitation is governed by the coupling of its electronic states. However, if the energetic spacing between the electronically excited states at the Franck-Condon window becomes sufficiently small, it is infeasible to selectively excite and monitor individual states with conventional time-resolved spectroscopy, preventing insight into the energy transfer and relaxation dynamics of the molecule. Here, we demonstrate how the combination of time-resolved spectroscopy and extensive surface hopping dynamics simulations with a global fit approach on individually excited ensembles overcomes this limitation and resolves the dynamics in the n3p Rydberg states in acetone. Photoelectron transients of the three closely spaced states n3px, n3py, and n3pz are used to validate the theoretical results, which in turn allow retrieving a comprehensive kinetic model describing the mutual interactions of these states for the first time.

| S-EPMC7052817 | biostudies-literature

Real single ion solvation free energies with quantum mechanical simulation.

Project description:Single ion solvation free energies are one of the most important properties of electrolyte solutions and yet there is ongoing debate about what these values are. Only the values for neutral ion pairs are known. Here, we use DFT interaction potentials with molecular dynamics simulation (DFT-MD) combined with a modified version of the quasi-chemical theory (QCT) to calculate these energies for the lithium and fluoride ions. A method to correct for the error in the DFT functional is developed and very good agreement with the experimental value for the lithium fluoride pair is obtained. Moreover, this method partitions the energies into physically intuitive terms such as surface potential, cavity and charging energies which are amenable to descriptions with reduced models. Our research suggests that lithium's solvation free energy is dominated by the free energetics of a charged hard sphere, whereas fluoride exhibits significant quantum mechanical behavior that cannot be simply described with a reduced model.

| S-EPMC5625628 | biostudies-literature

Quantum coherence and quantum phase transitions.

Project description:We study the connections between local quantum coherence (LQC) based on Wigner-Yanase skew information and quantum phase transitions (QPTs). When applied on the one-dimensional Hubbard, XY spin chain with three-spin interaction, and Su-Schrieffer-Heeger models, the LQC and its derivatives are used successfully to detect different types of QPTs in these spin and fermionic systems. Furthermore, the LQC is effective as the quantum discord (QD) in detecting QPTs at finite temperatures, where the entanglement has lost its effectiveness. We also demonstrate that the LQC can exhibit different behaviors in many forms compared with the QD.

| S-EPMC4872232 | biostudies-other

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