Nonlinear optical effects where quantum mechanical predictions are at variance with the results of classical calculations are studied. Certain initial conditions, those of unstable equilibrium or those that lead to unstable equilibrium, classically, give rise to an aperiodicity in the intensity of the emitted radiation. One example of such a system is second-harmonic generation, which is studied in detail because of the potential amenability of the aperiodicity to experimental observation. Numerical and analytic predictions for the evolution of the intensity and photon statistics of the second harmonic light are presented. The photon statistics of the second harmonic light are predicted to undergo a sharp transition following the first maximum of the intensity.
Nonlinear optical effects where quantum mechanical predictions are at variance with the results of classical calculations are studied. Certain initial conditions, those of unstable equilibrium or those that lead to unstable equilibrium, classically, give rise to an aperiodicity in the intensity of the emitted radiation. One example of such a system is second-harmonic generation, which is studied in detail because of the potential amenability of the aperiodicity to experimental observation. Numerical and analytic predictions for the evolution of the intensity and photon statistics of the second harmonic light are presented. The photon statistics of the second harmonic light are predicted to undergo a sharp transition following the first maximum of the intensity.
The effect of the quantum properties of light on nonlinear processes has been well studied theoretically. It has been shown that the efficiency of n-photon nonlinear processes in many cases scales as the normalized n-th order correlation function. For light with high intensity correlation function, the efficiency of the n-th harmonic generation will be considerably higher than for coherent light. The experimental observation of this effect remained difficult until recently, because of the absence of bright sources with strong and fast intensity fluctuations. For the experimental demonstration of statistical effects in optical harmonic generation we use as a pump the radiation of high-gain parametric down conversion. Such light shows quantum properties (e.g. quadrature or two-mode squeezing) and has large number of photons in one mode. The normalized n-th order correlation function for this light is (2n - 1)!!, which makes it more attractive for nonlinear processes than both coherent and thermal light. For the generation of optical harmonics we used broadband parametric down conversion around frequency-degeneracy (1600 nm) produced in 1cm BBO crystal from Ti:Sapphire laser (800 nm, 1.6ps, 5kHz, 3W mean intensity). Due to spectral filtering and post-selection technique we could vary the statistics of light from coherent to super-bunched, which allowed us to demonstrate the efficiency enhancement for second-, third-, and fourth-harmonic generation. The obtained experimental results show a good agreement with the theory.
Nonlinear optics is the study of the response of dielectric media to strong optical fields. The fields are sufficiently strong that the response of the medium is, as its name implies, nonlinear. That is, the polarization, which is the dipole moment per unit volume in the medium, is not a linear function of the applied electric field. In the equation for the polarization, there is a linear term, but, in addition, there are terms containing higher powers of the electric field. This leads to significant new types of behavior, one of the most notable being that frequencies different from that of the incident electromagnetic wave, such as harmonics or subharmonics, can be generated. Linear media do not change the frequency of light incident upon them. The first observation of a nonlinear optical effect was, in fact, second-harmonic generation – a laser beam entering a nonlinear medium produced a second beam at twice the frequency of the original. Another type of behavior that becomes possible in nonlinear media is that the index of refraction, rather than being a constant, is a function of the intensity of the light. For a light beam with a nonuniform intensity profile, this can lead to self-focusing of the beam. Most nonlinear optical effects can be described using classical electromagnetic fields, and, in fact, the initial theory of nonlinear optics was formulated assuming the fields were classical. When the fields are quantized, however, a number of new effects emerge. Quantized fields are necessary if we want to describe fields that originate from spontaneous emission. For example, in a process known as spontaneous parametric down-conversion, a beam of light at one frequency, the pump, produces a beam at half the original frequency, the signal. This second beam is a result of spontaneous emission.
Effects of extreme nonlinear optics, such as high harmonic generation (HHG), are conventionally modeled with classical electromagnetic fields: both the driving and emitted fields are treated classically. We present the fully quantum electrodynamical theory of extreme nonlinear optics and use it to predict new quantum effects in HHG. The quantum description shows new effects in both the spectral and statistical properties of HHG. We also describe how the HHG process changes in the single-atom regime and discuss experiments that can test our various predictions. Revealing the quantum-optical nature of HHG could lead to novel sources of attosecond light having intrinsically quantum statistics, such as squeezing and entanglement.
High harmonic generation (HHG) is an extremely nonlinear effect generating coherent broadband radiation and pulse durations reaching attosecond timescales. Conventional models of HHG that treat the driving and emitted fields classically are usually very successful but inherently cannot capture the quantum-optical nature of the process. Although prior work considered quantum HHG, it remains unknown in what conditions the spectral and statistical properties of the radiation depart considerably from the known phenomenology of HHG. The discovery of such conditions could lead to novel sources of attosecond light having squeezing and entanglement. Here, we present a fully-quantum theory of extreme nonlinear optics, predicting quantum effects that alter both the spectrum and photon statistics of HHG, thus departing from all previous approaches. We predict the emission of shifted frequency combs and identify spectral features arising from the breakdown of the dipole approximation for the emission. Our results show that each frequency component of HHG can be bunched and squeezed and that each emitted photon is a superposition of all frequencies in the spectrum, i.e., each photon is a comb. Our general approach is applicable to a wide range of nonlinear optical processes, paving the way towards novel quantum phenomena in extreme nonlinear optics.
The main scope of this thesis is the investigation of quantum properties of nonlinear, dissipative, optical and condensed matter systems. Compared with previous studies on this subjects, we reached several milestone of general interests for the theoretical and experimental community. \nThe main experimental platform we refer to in this thesis is microcavity polaritons: polaritons arise from the coupling of light with excitons in a quantum well, i.e., a 2D semiconductor material embedded in the microcavity. They have attracted the interest of the scientific community for their rich physics. Polaritons can form out-of-equilibrium Bose-Einstein condensates, they can experience superfluid phase transition and, due to their interaction via the excitonic component, they show a variety of phenomena which are typical of nonlinear physics, such as bistability and parametric scattering. \nIn particular, motivated by recent proposals about the generation of single photons from weakly nonlinear system, like the unconventional photon blockade, and by the production of squeezed states in polariton systems, we studied the possibility of obtaining antibunched light and other quantum states (like squeezed states and entangled states), when the nonlinear system shows some peculiar features: in particular we consider polariton soliton and cascade systems. \nFinally, when considering nonlinear incoherent processes, we investigate the effect of the PT-symmetry and the PT-symmetry breaking on the quantum state of the emitted light. \nHence, this research work has two main objectives: first, from the fundamental physics point of view, to understand the interplay between nonlinear phenomena and quantum optics, second to provide useful tools for future technological applications. Specifically, for the latter case, we demonstrate a theorem that links the measurement of intensity correlations with the occurrence of certain phase transitions, and we propose a setup to maximize the non-classicality of the light emitted by weakly non-linear systems via a cascade configuration. \n \n \n
The topic of this thesis is a theoretical study of nonequilibrium transitions and quantum statistical properties of nonlinear quantum optical systems driven by an external radiation source. In certain limiting cases, a comparison is made between these transitions and the phase transitions found in equilibrium physical systems. In chapters one and two, the mathematical tools are introduced. In operator terms, the time development is described by a Markovian master equation in the interaction picture. This is equivalent to a corresponding time development equation or Fokker-Planck equation in a vector space of c-numbers. In order to deal with the type of Fokker-Planck equation that results, we introduce a quantum classical correspondence resulting in a distribution function over a complex phase-space, which is a generalisation of the Glauber-Sudarshan P-function. In chapter three this is applied to a model of a coherently driven mode with nonlinear dispersion and absorption. We find in the limit of zero temperature, that the spectrum is symmetric relative to the input frequency, and an exact solution is obtained for the distribution function. For a detuned driving field and nonlinear dispersion, optical bistability can occur. In chapter four a model of sub/second harmonic generation is introduced. This has several non-equilibrium transitions, including dispersive optical bistability, and bistable behaviour with coherent phase-locked input to both modes. Exact solutions occur in the limit of zero temperature and adiabatic elimination of one mode. In both chapters three and four, steady-state photon anti-bunching occurs with an absorptive nonlinearity. In chapter five we include interactions between the radiation mode and a fluorescent atomic system. In this case different behaviour occurs depending on the relative decay rates of the individual atoms and of the radiation mode. In the case of a high-Q interferometer, the atomic variables can be adiabatically eliminated. Both dispersive and absorptive bistability can occur. We show by analytic and numerical calculations (in the case of inhomogeneous broadening) that dispersive operation has advantages in requiring a lower atomic density and input field to observe bistability. When the input field has Gaussian (rather than coherent) photon statistics, there is no bistability, but enhanced photon bunching occurs. Finally, there is a different type of behaviour when the field mode decays rapidly and can be adiabatically eliminated. Within the cooperation lifetime the system can be described by a J²-invariant Hamiltonian, giving the special case of only collective damping. The result is a new type of critical point transition in the thermodynamic limit, with the appearance of a family of solutions like Lotka-Volterra cycles for a coherent driving field above threshold.