We propose and demonstrate a versatile technique to measure the lifetime of the one-phonon Fock state using two-color pump-probe Raman scattering and spectrally resolved, time-correlated photon counting. Following pulsed laser excitation, the n=1 phonon Fock state is probabilistically prepared by projective measurement of a single Stokes photon. The detection of an anti-Stokes photon generated by a second, time-delayed laser pulse probes the phonon population with subpicosecond time resolution. We observe strongly nonclassical Stokes-anti-Stokes correlations, whose decay maps the single phonon dynamics. Our scheme can be applied to any Raman-active vibrational mode. It can be modified to measure the lifetime of n≥1 Fock states or the phonon quantum coherences through the preparation and detection of two-mode entangled vibrational states.

A single quantum of excitation of a mechanical oscillator is a textbook example of the principles of quantum physics. But mechanical oscillators, despite their pervasive presence in nature and modern technology, do not generically exist in an excited Fock state. In the past few years, careful isolation of gigahertz-frequency nanoscale oscillators has allowed experimenters to prepare such states at millikelvin temperatures. These developments illustrate the tension between the basic predictions of quantum mechanics-which should apply to all mechanical oscillators even at ambient conditions-and the extreme conditions required to observe those predictions. We resolve the tension by creating a single Fock state of a 40-THz vibrational mode in a crystal at room temperature and atmospheric pressure. After exciting a bulk diamond with a femtosecond laser pulse and detecting a Stokes-shifted photon, the Ramanactive vibrational mode is prepared in the Fock state j1i with 98.5% probability. The vibrational state is then mapped onto the anti-Stokes sideband of a subsequent pulse, which when subjected to a Hanbury Brown-Twiss intensity correlation measurement reveals the sub-Poisson number statistics of the vibrational mode. By controlling the delay between the two pulses, we are able to witness the decay of the vibrational Fock state over its 3.9-ps lifetime at ambient conditions. Our technique is agnostic to specific selection rules, and should thus be applicable to any Raman-active medium, opening a new general approach to the experimental study of quantum effects related to vibrational degrees of freedom in molecules and solidstate systems.

The observation of photoconduction and nonlinear optical absorption on functionalized multiwall carbon nanotubes decorated with platinum is reported. The samples were prepared by a chemical vapor deposition method. The electrical conductivity of the carbon nanotubes seems to be decreased by the functionalization process; but this property is strongly enhanced after the incorporation of platinum particles. Nonresonant photoconductive experiments at 532 nm and 445 nm wavelengths allow us to detect a selective participation of the platinum to the photoelectrical response. A mechanooptic effect based on Fresnel reflection was obtained through a photoconductive modulation induced by the rotation of a silica substrate where the samples were deposited as a thin film. A two-photon absorption process was identified as the main physical mechanism responsible for the nonlinear optical absorption. We consider that important changes in the nonlinear photon interactions with carbon nanotubes can be related to the population losses derived from phonons and the detuning of the frequency originated by functionalization.

Time-resolved Raman spectroscopy techniques offer various ways to study the dynamics of molecular vibrations in liquids or gases and optical phonons in crystals. While these techniques give access to the coherence time of the vibrational modes, they are not able to reveal the fragile quantum correlations that are spontaneously created between light and vibration during the Raman interaction. Here, we present a scheme leveraging universal properties of spontaneous Raman scattering to demonstrate Bell correlations between light and a collective molecular vibration. We measure the decay of these hybrid photon-phonon Bell correlations with sub-picosecond time resolution and find that they survive over several hundred oscillations at ambient conditions. Our method offers a universal approach to generate entanglement between light and molecular vibrations. Moreover, our results pave the way for the study of quantum correlations in more complex solid-state and molecular systems in their natural state.

Spontaneous vibrational Raman scattering is a ubiquitous form of light–matter interaction whose description necessitates quantization of the electromagnetic field. It is usually considered as an incoherent process because the scattered field lacks any predictable phase relationship with the incoming field. When probing an ensemble of molecules, the question therefore arises: What quantum state should be used to describe the molecular ensemble following spontaneous Stokes scattering? We experimentally address this question by measuring time-resolved Stokes–anti-Stokes two-photon coincidences on a molecular liquid consisting of several sub-ensembles with slightly different vibrational frequencies. When spontaneously scattered Stokes photons and subsequent anti-Stokes photons are detected into a single spatiotemporal mode, the observed dynamics is inconsistent with a statistical mixture of individually excited molecules. Instead, we show that the data are reproduced if Stokes–anti-Stokes correlations are mediated by a collective vibrational quantum, i.e. a coherent superposition of all molecules interacting with light. Our results demonstrate that the degree of coherence in the vibrational state of the liquid is not an intrinsic property of the material system, but rather depends on the optical excitation and detection geometry.