Stokes–anti-Stokes correlations in diamond

Kasperczyk, Mark; Jório, Ado; Neu, Elke; Maletinsky, Patrick; Novotny, Lukas

doi:10.1364/ol.40.002393

Cited by 45 publications

(44 citation statements)

References 19 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The excitation laser power dependence for

g_{S, a S}^{(2)} true(normalΔ t = 0 true)

, I SaS (Δ t = 0), and

{\overset{true¯}{I}}_{S a S} true(normalΔ t \neq 0 true)

in the real SaS process in diamond has been published in ref. . As predicted in ref.…”

Section: Resultssupporting

confidence: 87%

“…Equation (1) is valid in resonance with the vibrational transition, i.e., I S,aS is measured at energies matching the S,aS vibrational Raman shifts. [5] This correlated SaS light scattering phenomenon involving the exchange of real phonons has been studied recently in diamond [6][7][8][9] and graphene, [2,8] evidencing a time correlation at zero delay beyond the maximum classical correlation given by the Cauchy-Schwars inequality, indicating that this phenomenon has no classical analog.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Physical Properties of Photonic Cooper Pairs Generated via Correlated Stokes–anti‐Stokes Raman Scattering

Júnior

Monken

Santos³

et al. 2019

Physica Status Solidi (b)

Self Cite

View full text Add to dashboard Cite

The theoretical and experimental background for the creation of photonic Cooper pairs (PCPs) via correlated Stokes–anti‐Stokes Raman scattering is introduced, followed by experimental results on the second‐order photon time correlation g2(0) in diamond. It is shown how g2(0) changes with energy (Stokes–anti‐Stokes Raman shift), momentum (scattering angle) and excitation laser power. Both real and virtual phonon‐mediated scattering processes are addressed.

show abstract

“…The excitation laser power dependence for

g_{S, a S}^{(2)} true(normalΔ t = 0 true)

, I SaS (Δ t = 0), and

{\overset{true¯}{I}}_{S a S} true(normalΔ t \neq 0 true)

in the real SaS process in diamond has been published in ref. . As predicted in ref.…”

Section: Resultssupporting

confidence: 87%

Section: Introductionmentioning

confidence: 99%

Physical Properties of Photonic Cooper Pairs Generated via Correlated Stokes–anti‐Stokes Raman Scattering

Júnior

Monken

Santos³

et al. 2019

Physica Status Solidi (b)

Self Cite

View full text Add to dashboard Cite

show abstract

“…Recently, Kasperczyk et al 53 and Parra-Murillo et al, 54 have analyzed an idealized version of such detection setup, in which the detection probabilities P (S) and P (aS) are proportional to the respective intensities of the Raman intensities S(ω S ) and S(ω aS ), respectively. They showed that if all anti-Stokes photons are produced as part of correlated pairs of Stokes and anti-Stokes photons emitted from the cavity (as represented pictorially in Fig.…”

Section: Dependence Of Stokes-anti-stokes Correlations On the Parametmentioning

confidence: 99%

Quantum Mechanical Description of Raman Scattering from Molecules in Plasmonic Cavities

et al. 2016

View full text Add to dashboard Cite

Plasmon-enhanced Raman scattering can push single-molecule vibrational spectroscopy beyond a regime addressable by classical electrodynamics. We employ a quantum electrodynamics (QED) description of the coherent interaction of plasmons and molecular vibrations that reveal the emergence of nonlinearities in the inelastic response of the system. For realistic situations, we predict the onset of phonon-stimulated Raman scattering and a counterintuitive dependence of the anti-Stokes emission on the frequency of excitation. We further show that this QED framework opens a venue to analyze the correlations of photons emitted from a plasmonic cavity.Surface Enhanced Raman Scattering (SERS) is a spectroscopic technique in which the inelastic scattering from a molecule is increased by placing it in a hotspot of a plasmonic cavity, where the electric fields associated with the incident and the scattered photons are strongly enhanced (see the schematic in Fig. 1(a)). 1 The difference between the energy of those two photons provides a fingerprint of the molecule, i.e., detailed chemical information about its vibrational structure. Since the initial observation of Raman scattering from single molecules, 2,3 the use of a variety of plasmonic structures that act as effective optical nanoantennas over the last decades has allowed a tremendous advance of this molecular spectroscopy 4 . Metallic particles such as nanoshells 5,6 , nanorings 7 , nanorods 8 , nanowires 9 , or nano stars 10 , as well as plasmonic nanogap structures formed in particle dimers [11][12][13] , nanoparticle-on-a-mirror morphologies [14][15][16][17] , or nanoclusters 18 , are among the variety of structures that offer huge and controllable enhancements of the field intensity in their hotspots, boosting the inherently weak Raman scattering intensity, 1,19 and ultimately enabling the chemical identification and imaging of particular vibrational modes of a molecule with subnanometer resolution. 20 These results suggest that some experiments might have reached the regime where the quantum-mechanical nature of both the molecular vibrations and the plasmonic cavity emerges, 21 and call for an adequate theoretical description that goes beyond the classical treatment of the electric fields produced in plasmonic cavities. 1,22,23 In this work we address the underlying quantummechanical nature of Raman scattering processes by quantizing as bosonic excitations both the vibrations of the molecule and the electromagnetic field of a plasmonic cavity. The description of the vibrations through bosonic operators can be justified by considering the harmonic approximation to the energy landscape of the molecule along a generalized atomic coordinate ( Fig. 1(b)), such as the length of a molecular bond, e.g., C=O. 21,22 These vibrations interact with the cavity photons through a nonlinear Hamiltonian, reminiscent of that found in optomechanical systems. 24 In this description, the large enhancement of the Raman scattering from a molecule in the plasmonic cavity occurs thanks to ...

show abstract

“…Correlation measurements, as performed in Refs. are not possible here due to the strong hot luminescence .…”

Section: Resultsmentioning

confidence: 98%

“…However, for the pulsed ML excitation, the behaviour is super‐linear. It has been shown already that this super‐linear behaviour is due to the correlated SaS scattering . As the SaS is a non‐linear process, the ultra‐high intensities within a laser pulse are needed to produce the effect in diamond.…”

Section: Resultsmentioning

confidence: 99%

Stokes and anti-Stokes Raman spectra of the high-energy C-C stretching modes in graphene and diamond

Jório

Kasperczyk

Clark

et al. 2015

Phys. Status Solidi B

Self Cite

View full text Add to dashboard Cite

The Stokes and the anti-Stokes Raman spectra from the high energy carbon-carbon stretching modes in graphene and diamond are studied, with focus on their intensity dependence on the excitation laser power. For diamond, the experiment was performed on a 50m slice of chemical vapour deposition grown single crystal, using a 785nm laser, both in the continuous wave (CW) and pulsed mode locked (ML -130fs pulses) excitation regimes. For graphene, the experiments were performed on suspended samples, including single layer, bilayer with AB-Staking, twisted bi-layer, and a sample with 4-6 layers, using a =532nm and a =633nm laser. The Stokes and anti-Stokes intensities vary largely from sample to sample, and the anti-Stokes/Stokes intensity ratio shows different excitation laser power behaviours. These differences can be explained on the basis of laser heating or correlated Stokes-antiStokes scattering phenomena.1 Introduction Phonons are quantum states of the harmonic oscillators, having their increase and decrease in number n described by creation (a † ) and annihilation (a) operators. The action of these operators on an eigenstate |n introduces normalization factors given by a † |n = (n+1) ½ |n+1 and a † |n = n ½ |n-1. In the inelastic scattering of light by phonons, a photon creates or annihilates a phonon, in the so-called Stokes or anti-Stokes Raman scattering process. The intensity ratio between the Stoke and antiStokes components (IaS/IS) are, therefore, usually determined by the quantum mechanics normalization factors, IaS/IS = n/(n+1) [1,2].The thermal population of phonons is given by the Bose-Einstein distribution function n0 = [exp(Eq/kBT)-1] -1 , where Eq and kBT are the phonon and thermal energies, respectively. Replacing n by n0 in the anti-Stokes/Stokes intensity ratio gives IaS/IS = (n0+1)/n0 = Cexp(Eq/kBT). This equation can be inverted to obtain the effective phonon temperature in a material by measuring their Stokes and anti-Stokes Raman spectra, given by T = Eq/{kB[lnCln(IaS/IS)]}. This procedure has been largely used in the literature to study the phonon population dependence of dif-

show abstract

Stokes–anti-Stokes correlations in diamond

Cited by 45 publications

References 19 publications

Physical Properties of Photonic Cooper Pairs Generated via Correlated Stokes–anti‐Stokes Raman Scattering

Physical Properties of Photonic Cooper Pairs Generated via Correlated Stokes–anti‐Stokes Raman Scattering

Quantum Mechanical Description of Raman Scattering from Molecules in Plasmonic Cavities

Stokes and anti-Stokes Raman spectra of the high-energy C-C stretching modes in graphene and diamond

Contact Info

Product

Resources

About