Does entanglement enhance single-molecule pulsed biphoton spectroscopy?
arXiv:2307.02204 · doi:10.1088/2058-9565/ad331b
Abstract
It depends. For a single molecule interacting with one mode of a biphoton probe, we show that the spectroscopic information has three contributions, only one of which is a genuine two-photon contribution. When all the scattered light can be measured, solely this contribution exists and can be fully extracted using unentangled measurements. Furthermore, this two-photon contribution can, in principle, be matched by an optimised but unentangled single-photon probe. When the matter system spontaneously emits into inaccessible modes, an advantage due to entanglement can not be ruled out. In practice, time-frequency entanglement does enhance spectroscopic performance of the oft-studied weakly-pumped spontaneous parametric down conversion (PDC) probes. For two-level systems and coupled dimers, more entangled PDC probes yield more spectroscopic information, even in the presence of emission into inaccessible modes. Moreover, simple, unentangled measurements can capture between 60% - 90% of the spectroscopic information. We thus establish that biphoton spectroscopy using source-engineered PDC probes and unentangled measurements can provide tangible quantum enhancement. Our work underscores the intricate role of entanglement in single-molecule spectroscopy using quantum light.
arXiv comment18+14 pages, 12+14 figures, 1+0 tables
References in corpus (39)
- Quantum entanglement
- Quantum Fisher information matrix and multiparameter estimation
- Heralded Generation of Ultrafast Single Photons in Pure Quantum States
- Progressive field-state collapse and quantum non-demolition photon counting
- Nonlinear optical signals and spectroscopy with quantum light
- A Quantum Pulse Gate based on Spectrally Engineered Sum Frequency Generation
- Teleportation of Nonclassical Wave Packets of light
- A high-efficiency quantum non-demolition single photon number resolving detector
- Generation of polarization entangled photon pairs and violation of Bell's inequality using spontaneous four-wave mixing in fiber loop
- Heralding Single Photons from Pulsed Parametric Down-Conversion
- Spectroscopy by frequency entangled photon pairs
- Quantum Fisher information for density matrices with arbitrary ranks
- Heralded single-photon source utilizing highly nondegenerate, spectrally factorable spontaneous parametric downconversion
- Setting bounds on two-photon absorption cross-sections in common fluorophores with entangled photon pair excitation
- Quantum-limited time-frequency estimation through mode-selective photon measurement
- Flexible resources for quantum metrology
- Quantum-limited loss sensing: Multiparameter estimation and Bures distance between loss channels
- Entangled Two-Photon Absorption by Atoms and Molecules: A Quantum Optics Tutorial
- Achieving the ultimate quantum timing resolution
- Quantum Metrology: Extended Convexity of Quantum Fisher Information
- Entanglement-Assisted Absorption Spectroscopy
- Quantum spectroscopy of plasmonic nanostructures
- Direct generation of tailored pulse-mode entanglement
- Dealing with entanglement of continuous variables: Schmidt decomposition with discrete sets of orthogonal functions
- Saturating the quantum Cramér-Rao bound using LOCC
- Measurement noise susceptibility in quantum estimation
- Generation of pulsed bipartite entanglement using four-wave mixing
- Quantum enhanced spectroscopy with entangled multi-photon states
- Nonlinear Interferometry for Quantum-Enhanced Measurements of Multiphoton Absorption
- Fundamental limits of pulsed quantum light spectroscopy: Dipole moment estimation
- Effects of coherence on temporal resolution
- Dynamics of photosynthetic light harvesting systems interacting with N-photon Fock states
- Nondestructive photon counting in waveguide QED
- Nonlinear quantum interferometric spectroscopy with entangled photon pairs
- Photonic temporal-mode multiplexing by quantum frequency conversion in a dichroic-finesse cavity
- Probing exciton dynamics with spectral selectivity through the use of quantum entangled photons
- Towards a Spectroscopic Protocol for Unambiguous Detection of Quantum Coherence in Excitonic Energy Transport
- Performing quantum entangled biphoton spectroscopy using classical light pulses
- Model-Independent Simulation Complexity of Complex Quantum Dynamics
Cited by in corpus (6)
- Pathway selectivity in time-resolved spectroscopy using two-photon coincidence counting with quantum entangled photons
- A tensor network approach to sensing quantum light-matter interactions
- On the role of chirping in pulsed single photon spectroscopy
- Sensing with Quantum Light: A perspective
- Two-dimensional fluorescence spectroscopy with quantum entangled photons and time- and frequency-resolved two-photon coincidence detection
- Optimal quantum spectroscopy using single-photon pulses