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Birth and death of a single quantum of vibration

Santiago Tarrago Velez, Kilian Seibold, Nils Kipfer, Mitchell D. Anderson, Vivishek Sudhir, Christophe Galland

Published Nov 7, 2018• 0 citations
OpenAlex

Abstract

A single quantum of excitation of a mechanical oscillator is a textbook example of the principles of quantum physics. 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 GHz-frequency nano-scale oscillators has allowed experimenters to prepare such states at milli-Kelvin temperatures. These developments illustrate the tension between the basic predictions of quantum mechanics that should apply to all mechanical oscillators existing even at ambient conditions, and the complex experiments in extreme conditions required to observe those predictions. We resolve the tension by creating a single Fock state of a vibration mode of a crystal at room temperature using a technique that can be applied to any Raman-active system. After exciting a bulk diamond with a femtosecond laser pulse and detecting a Stokes-shifted photon, the 40~THz Raman-active internal vibrational mode is prepared in the Fock state $|1>$ with $98.5\%$ probability. The vibrational state is read out by 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 room temperature. Our technique is agnostic to specific selection rules, and should thus be applicable to any Raman-active medium, opening a new generic approach to the experimental study of quantum effects related to vibrational degrees of freedom in molecules and solid-state systems.

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A single quantum of excitation of a mechanical oscillator is a textbook example of the principles of quantum physics. 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 GHz-frequency nano-scale oscillators has allowed experimenters to prepare such states at milli-Kelvin temperatures. These developments illustrate the tension between the basic predictions of quantum mechanics that should apply to all mechanical oscillators existing even at ambient conditions, and the complex experiments in extreme conditions required to observe those predictions. We resolve the tension by creating a single Fock state of a vibration mode of a crystal at room temperature using a technique that can be applied to any Raman-active system. After exciting a bulk diamond with a femtosecond laser pulse and detecting a Stokes-shifted photon, the 40~THz Raman-active internal vibrational mode is prepared in the Fock state ∣1>|1>∣1> with 98.5%98.5\%98.5% probability. The vibrational state is read out by 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 3.93.93.9 ps lifetime at room temperature. Our technique is agnostic to specific selection rules, and should thus be applicable to any Raman-active medium, opening a new generic approach to the experimental study of quantum effects related to vibrational degrees of freedom in molecules and solid-state systems.
Measurement induced nonlinearity is a powerful tool in quantum optics to prepare non-classical states of light. We apply this concept to prepare a vibrational mode in a non-classical state with sub-Poissonian statistics in a diamond crystal at room temperature, using a scheme that is applicable to any Raman active mode. Upon detection of a single Stokes-shifted photon under pulsed excitation, quantum mechanics predicts that the wave-function describing the correlated vibrational mode collapses into its first excited energy eigenstate (Fock state n=1n=1n=1). We prove this by mapping the vibrational state onto an anti-Stokes photon, on which we perform a Hanbury-Brown and Twiss intensity interference measurement. Our data reveals deep sub-Poissonian statistics conditioned on the success of the Stokes measurement, and provides the first demonstration of this effect with a mechanical vibration in ambient conditions. Our work is also a proof-of-principle demonstration of a broadly tunable heralded single photon source with integrated short-lived quantum memory.
With the development of quantum optics, photon correlations acquired a prominent role as a tool to test our understanding of physics, and played a key role in verifying the validity of quantum mechanics. The spatial and temporal correlations in a light field also reveal information about its origin, and allow us to probe the nature of the physical systems interacting with it. Additionally, with the advent of quantum technologies, they have acquired technological relevance, as they are expected to play an important role in quantum communication and quantum information processing. This thesis develops techniques that combine spontaneous Raman scattering with Time Correlated Single Photon Counting, and uses them to study the quantum mechanical nature of high frequency vibrations in crystals and molecules. We demonstrate photon bunching in the Stokes and anti-Stokes fields scattered from two ultrafast laser pulses, and use their cross-correlation to measure the 3.9 ps decay time of the optical phonon in diamond. We then employ this method to measure molecular vibrations in CS2, where we are able to excite the respective vibrational modes of the two isotopic species present in the sample in a coherent superposition, and observe quantum beating between the two signals. Stokes scattering, when combined with a projective measurement, leads to a well defined quantum state. We demonstrate this by measuring the second order correlation function of the anti-Stokes field conditional on detecting one or more photons in the Stokes field, which allows us to observe a phonon modeâ s transition form a thermal state into the first excited Fock state, and measure its decay over the characteristic phonon lifetime. Finally, we use this technique to prepare a highly entangled photon-phonon state, which violates a Bell-type inequality. We measure S = 2.360 ± 0.025, violating the CHSH inequality, compatible with the non-locality of the state. The techniques we developed open the door to the study of a broad range of physical systems, where spectroscopic information is obtained with the preparation of specific quantum states. They also hold potential for future technological use, and promote vibrational Raman scattering to a resource in nonlinear quantum optics -- where it used to be considered as a source of noise instead.
Nano- and micromechanical solid-state quantum devices have become a focus of attention. Reliably generating nonclassical states of their motion is of interest both for addressing fundamental questions about macroscopic quantum phenomena and for developing quantum technologies in the domains of sensing and transduction. We used quantum optical control techniques to conditionally generate single-phonon Fock states of a nanomechanical resonator. We performed a Hanbury Brown and Twiss-type experiment that verified the nonclassical nature of the phonon state without requiring full state reconstruction. Our result establishes purely optical quantum control of a mechanical oscillator at the single-phonon level.
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.
The preparation of pure quantum states with high degrees of macroscopicity is a central goal of ongoing experimental efforts to control quantum systems. We present a state preparation protocol which renders a mechanical oscillator with an arbitrarily large coherent amplitude in a manifestly nonclassical state. The protocol relies on coherent-state preparation followed by a projective measurement of a single Raman scattered photon, making it particularly suitable for cavity optomechanics. The nonclassicality of the state is reflected by sub-Poissonian phonon statistics, which can be accessed by measuring the statistics of subsequently emitted Raman sideband photons. The proposed protocol would facilitate the observation of nonclassicality of a mechanical oscillator that moves macroscopically relative to motion at the single-phonon level.