Brillouin–Mandelstam scattering is one of the most accessible nonlinear optical phenomena and has been widely studied since its theoretical discovery one hundred years ago. The scattering mechanism is a three-wave-mixing process between two optical fields and one acoustic field and has found a broad range of applications spanning microscopy to ultra-narrow-linewidth lasers. Building on the success of utilizing this nonlinearity at a classical level, a rich avenue is now being opened to explore Brillouin scattering within the paradigm of quantum optics. Here, we take a key step in this direction by employing quantum optical techniques yet to be utilized for Brillouin scattering to characterize the second-order coherence of Stokes scattering across the Brillouin lasing threshold. We use a silica microsphere resonator and single-photon counters to observe the expected transition from bunched statistics of thermal light below the lasing threshold to Poissonian statistics of coherent light above the threshold. Notably, at powers approaching the lasing threshold, we also observe super-thermal statistics, which arise due to instability and a “flickering” in and out of lasing as the pump field is transiently depleted. The statistics observed across the transition, including the “flickering,” are a result of the full nonlinear three-wave-mixing process and cannot be captured by a linearized model. These measurements are in good agreement with numerical solutions of the three-wave Langevin equations and are well demarcated by analytical expressions for the instability and the lasing thresholds. These results demonstrate that applying second-order-coherence and photon-counting measurements to Brillouin scattering provides new methods to advance our understanding of Brillouin scattering itself and progress toward quantum-state preparation and characterization of acoustic modes.
Brillouin–Mandelstam scattering is one of the most accessible nonlinear optical phenomena and has been widely studied since its theoretical discovery one hundred years ago. The scattering mechanism is a three-wave-mixing process between two optical fields and one acoustic field and has found a broad range of applications spanning microscopy to ultra-narrow-linewidth lasers. Building on the success of utilizing this nonlinearity at a classical level, a rich avenue is now being opened to explore Brillouin scattering within the paradigm of quantum optics. Here, we take a key step in this direction by employing quantum optical techniques yet to be utilized for Brillouin scattering to characterize the second-order coherence of Stokes scattering across the Brillouin lasing threshold. We use a silica microsphere resonator and single-photon counters to observe the expected transition from bunched statistics of thermal light below the lasing threshold to Poissonian statistics of coherent light above the threshold. Notably, at powers approaching the lasing threshold, we also observe super-thermal statistics, which arise due to instability and a “flickering” in and out of lasing as the pump field is transiently depleted. The statistics observed across the transition, including the “flickering,” are a result of the full nonlinear three-wave-mixing process and cannot be captured by a linearized model. These measurements are in good agreement with numerical solutions of the three-wave Langevin equations and are well demarcated by analytical expressions for the instability and the lasing thresholds. These results demonstrate that applying second-order-coherence and photon-counting measurements to Brillouin scattering provides new methods to advance our understanding of Brillouin scattering itself and progress toward quantum-state preparation and characterization of acoustic modes.
Brillouin-Mandelstam scattering offers several favourable properties to control sound with light at a quantum mechanical level. In particular, the high acoustic frequencies, acoustic mode selectivity, and low optical absorption provide a promising route towards this goal whilst also overcoming several current hindrances within optomechanics. Utilizing these properties, some of our main results in this direction include: the first observation of Brillouin optomechanical strong coupling, studying the second-order coherence across the Brillouin lasing threshold, and, we’ve performed heralded single-phonon addition and subtraction to a thermal state of the acoustic field observing the resulting non-Gaussianity with a precision that advanced the forefront of opticsbased mechanical state tomography. More recently, we’ve demonstrated that laser cooling may be enhanced via zero-photon detection, and we’ve characterized the Brillouin scattering response in optical fibre at millikelvin temperatures. This talk will cover these results, what they enable, and the broader direction of our lab including the prospects of this platform for quantum science and technology.
We analyze the quantum statistical properties of light scattered by an acousto-optic modulator. From the perspective of quantum mechanics, the acousto-optic effect arises from a nonlinear interaction between three bosonic fields: the laser light, the Brillouin-scattered light, and an acoustic wave. The Hamiltonian coincides with that of sum-frequency generation, where the sum-frequency mode is known to exhibit sub-Poissonian statistics. We calculate the free temporal evolution of the Fano factor for Brillouin backscattered light and determine that sub-Poissonian statistics are obtained when faint laser light is scattered by a counter-propagating coherent acoustic wave with low average phonon number. The use of sub-Poissonian light would lead to an increase of the security for quantum key distribution.
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.
Four-wave mixing mediated by Brillouin scattering in the transient regime exhibits an instability which results in large phase conjugate reflectivities [A. M. Scott and K. D. Ridley, IEEE J Quantum Electron. QE-25, 438 (1989)]. In this paper we compare measurements of the threshold for the instability both as a function of the ratio of the second pump beam to the first pump beam and as a function of the phase mismatch. Phase conjugation in Brillouin enhanced four-wave mixing occurs through the interaction of a signal with two counterpropagating pump beams. In our experiments, the frequencies of all three input beams are different, and a small phase mismatch results. The magnitude of this mismatch was varied both by changing one of the input frequencies and the interaction length. The frequency of the second pump beam was changed by using stimulated Brillouin scattering in various mixtures. Thus we were able to vary the phase mismatch from four to thirteen resulting in a 50% change in the threshold intensity, in agreement with theoretical models. The ratio of the backward-to-forward pump beam intensities also affects the threshold, and measurements of this agree with the model.
Abstract A new approach for analytically solving quantum nonlinear Langevin equations is proposed and applied to calculations of spectra of superradiant lasers where collective effects play an important role. We calculate lasing spectra for arbitrary pump rates and recover well-known results such as the pump dependence of the laser linewidth across the threshold region. We predict new sideband peaks in the spectrum of superradiant lasers with large relaxation oscillations as well as new nonlinear structures in the lasing spectra for weak pump rates. Our approach sheds new light on the importance of population fluctuations in the narrowing of the laser linewidth, in the structure of the lasing spectrum, and in the transition to coherent operation.
In the first part of this thesis, a detailed analysis of lasing in random multiple-light-scattering media with gain is presented. Random laser emission is analyzed using a time-dependent diffusion model for light propagating in the medium containing active atoms. We demonstrate the effects of scatterers to narrow the emission spectral linewidth and to shorten the emitted pulse duration at a specific threshold pump intensity. This threshold pump intensity decreases with scatterer density and excitation spot diameter, in excellent agreement with experimental results. The coherence properties of the random laser are studied using a generalized master equation. The random laser medium is treated as a collection of low quality-factor cavities, coupled by random photon diffusion. Laser-like coherence, on average, is demonstrated above a specific pumping threshold. We demonstrate that with stronger scattering, the pumping threshold for the transition from chaotic to isotropic coherent light emission decreases and enhanced optical coherence for the emitted light is achieved above threshold. The second part of this thesis presents a study of lasing in photonic crystals (PCs). The emission from an incoherently pumped atomic system in interaction with the electro-magnetic reservoir of a PC is analyzed using a set of generalized semiclassical Maxwell-Bloch equations. We demonstrate that the photonic band edge facilitates the enhancement of stimulated emission and the reduction of internal losses, leading to an important lowering of the laser threshold. In addition, an increase of the laser output at a photonic band edge is demonstrated. We next develop a detailed quantum theory of a coherently pumped two-level atom in a photonic band gap material, coupled to both a multi-mode wave-guide channel and a high-quality micro-cavity embedded within the PC. The cavity field characteristics are highly distinct from that of a corresponding high-Q cavity in ordinary vacuum. We demonstrate enhanced, inversionless, and nearly coherent light generation when the photon density of states (DOS) jump between the Mollow spectral components of atomic resonance fluorescence is large. In the case of a vanishing photon DOS on the lower Mollow sideband and no dipolar dephasing, the emitted photon statistics is Poissonian and the cavity field exhibits quadrature coherence.