The colored rings shown in figure 1 are a spectacular manifestation of one type of nonlinear optical frequency conversion: parametric amplification of quantum noise. The amplification in this case is produced by the propagation of an intense pulse of ultraviolet radiation through a crystal of barium borate. When intense electromagnetic radiation propagates through such a material, whose polarization response at optical frequencies manifests a strongly nonlinear dependence on electric field amplitude, nonlinear mixing of the input radiation generates new spectral components. We can exploit this phenomenon to generate coherent radiation at frequencies for which we have no convenient laser sources.
The colored rings shown in figure 1 are a spectacular manifestation of one type of nonlinear optical frequency conversion: parametric amplification of quantum noise. The amplification in this case is produced by the propagation of an intense pulse of ultraviolet radiation through a crystal of barium borate. When intense electromagnetic radiation propagates through such a material, whose polarization response at optical frequencies manifests a strongly nonlinear dependence on electric field amplitude, nonlinear mixing of the input radiation generates new spectral components. We can exploit this phenomenon to generate coherent radiation at frequencies for which we have no convenient laser sources.
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.
In the previous chapter we examined nonlinear propagation in a two-level medium, which leads to amplification or absorption of the radiation field. As we will see further on in this volume, when the medium is placed in an optical cavity one realizes a laser in the case of amplification or an optically bistable system in the absorptive configuration. On the other hand, the nonlinear response of the atomic polarization to the electric field leads to further fascinating scenarios [29, 51–60]. For example, a field with central ω 0 can generate harmonic components with central frequencies 2 ω 0 , 3 ω 0 etc., processes that are called second-harmonic generation, third-harmonic generation etc. Furthermore, the interaction of two fields with central frequencies ω 1 and ω 2 , with ω 1 > ω 2 , can generate components with central frequency ω 1 + ω 2 (sum-frequency generation) and ω 1 − ω 2 (difference-frequency generation). Such phenomena have not yet appeared in this volume because we have assumed that the electric field corresponds to a narrow frequency band around a central frequency ω 0 only, whereas to describe them it is necessary to assume that the electric field is the superposition of a number of frequency bands. In this chapter we will provide a description of the basic elements which are necessary to describe these phenomena and we will discuss a small number of them for the case of materials with a quadratic nonlinearity, referring to textbooks in nonlinear optics for the description of other phenomena. The following chapter is devoted, instead, to the case of materials with cubic nonlinearities. The starting point of nonlinear optics is the expansion of the atomic polarization in powers of the electric field, when the electric field is not too intense. In our treatment in Chapter 5 we saw that the expansion of the nonlinear susceptibility contains only even powers of the electric field (see Eq. (5.27)), and therefore the expansion of the polarization includes only odd powers.
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 dynamics provide an indispensable resource for creating quantum states of light, as well as other bosonic systems. Seminal work using second- and third-order nonlinear optical crystals, cavity quantum electrodynamics, and superconducting circuits, have enabled generating squeezed states, as well as various non-Gaussian quantum states (e.g., single photons, cat states) at both infrared and microwave frequencies. Nevertheless, it remains challenging to generate quantum states of light in broad portions of the electromagnetic spectrum: for example, at terahertz frequencies and at ultraviolet and X-ray frequencies. In this Perspective, I discuss a variety of emerging material platforms, as well as emerging theoretical and experimental tools, which enable overcoming these challenges. The main argument of this Perspective is that advances in driving nonlinear dynamics of material excitations, will enable generating quantum states of these material excitations as well as quantum states of light at new frequency ranges. I will further argue that in order to realize much of the promise of this nascent field, there is a need for innovation in the laser systems used to drive these nonlinear dynamics: specifically, innovations in realizing high-power laser sources that have very low noise, having quantum statistics similar to coherent states of light which describe lower intensity laser systems. I will highlight some experimental and theoretical work, in understanding quantum noise dynamics in complex laser systems, that can address these challenges.
This thesis presents a study of photon generation and conversion processes in nonlinear optics. Our results extend beyond the first order perturbative regime, in which only pairs of photons are generated in spontaneous parametric down-conversion or four wave mixing. They also allow us to identify the limiting factors for achieving unit efficiency frequency conversion, and to correctly account for the propagation of bright nonclassical photon states generated in the nonlinear material. This is done using the Magnus expansion, which allows us to incorporate corrections due to time-ordering effects in the time evolution of the state, while also respecting the quantum statistics associated with squeezed states (in photon generation) and single photons or coherent states (in photon conversion). We show more generally that this expansion should be the preferred strategy when dealing with any type of time-dependent Hamiltonian that is a quadratic form in the creation and annihilation operators of the fields involved. Using the Magnus expansion, simple figures of merit to estimate the relevance of these time-ordering corrections are obtained. These quantities depend on the group velocities of the modes involved in the nonlinear process and provide a very simple physical picture of the interactions between the photons at different times. These time-ordering effects are shown to be important only when the photons and pump beam overlap within the nonlinear material for a significant amount of time. We also discuss the possibility of preparing Fock states with many photons using parametric down-conversion sources and realistic photon-number-resolving detectors. After discussing photon generation processes, we study photon conversion processes in which a nonlinear material and a classical strong pump field are used modify the frequency of a second incoming low-intensity field. We show that time-ordering effects limit the efficiency of this conversion process, re-examine strategies to get around this problem, and show that it should be possible to have a clear observation of modified upconversion probabilities due to these effects, and thus have an experimental demonstration of time-ordering effects in nonlinear optics.
Nonlinear optical mixing of existing laser frequencies to access portions of the spectrum where lasing action is not easily obtainable is common practice today. Although nonlinear solid-state media are available [1] for frequency conversion from just under 200 nm in the ultraviolet to about a few microns in the infrared, the generation of widely-tunable laser radiation in the mid-to-far infrared and VUV regions typically requires four-frequency mixing in atomic vapors. In the past, frequency conversion in atomic vapors suffered from poor conversion efficiencies due to the small magnitude of the third-order nonlinear susceptibility and the difficulty in phasematching. We demonstrate a method [2] for performing four-frequency mixing which overcomes both of these shortcomings, allowing efficient frequency conversion with moderate pump intensities.