Recent developments in opto-optical modulation technique calls for improved temporal control of light modulation processes of coherent XUV light. This thesis project evaluates an experimental method aimed at achieving redirection and amplitude modulation of XUV-light, by using precise determination of decay times in states of noble gases that are deemed suitable for opto-optical control. It is possible to obtain a higher signal-to-noise ratio than previously possible when performing decay time measurements using a recently developed technique to obtain spatial phase control of the states that are being measured.
Recent developments in opto-optical modulation technique calls for improved temporal control of light modulation processes of coherent XUV light. This thesis project evaluates an experimental method aimed at achieving redirection and amplitude modulation of XUV-light, by using precise determination of decay times in states of noble gases that are deemed suitable for opto-optical control. It is possible to obtain a higher signal-to-noise ratio than previously possible when performing decay time measurements using a recently developed technique to obtain spatial phase control of the states that are being measured.
Extreme ultraviolet (XUV) light is a valuable frequency range for ultrafast optics experiments. The short wavelength is a requirement for ultrashort pulses, which are widely used to characterize fast dynamics. Additionally, the high photon energy enables quantum control of high frequency transitions in atoms. These transitions are of interest for ultrafast quantum control as the bandwidth of the control pulses needs to be less than the transition frequency. Presently, however, no good modulators exist for these frequencies, which significantly reduces the possible ultrafast optics experiments or applications in the XUV regime. This thesis addresses this problem and focuses on the control of XUV light in time and space. To enable control of XUV light a method is described which modulates the phase of XUV light emitted from a gas of noble atoms. The atoms are resonantly excited with a coherent XUV pulse generated through high order harmonic generation. After the excitation pulse has passed through the gas, the atoms will emit light in the absence of an external field, known as free induction. The phase of the emitted light is changed by shifting the resonance frequencies through the AC Stark shift with a non-resonant infrared control pulse. This phase-control of the emitting atoms also translates into a control of the phase of the emitted XUV field.With the method described in the previous paragraph, the direction of XUV light emitted from noble gases was controlled, and the temporal dynamics of the emission was studied. The redirection of the XUV emission, through the use of a spatially offset IR pulse, was found to change both with intensity of the control pulse and by changing the spatial offset between the pulses. By varying the delay between the excitation and the control pulse the time of redirection was controlled, which enabled high signal to noise study of the temporal dynamics of the emission. Furthermore, with two control pulses the emission was redirected twice, resulting in an XUV pulse shape with controlled duration emitted with a certain angle. Hopefully the presented work will result in more research into the development of this technique, to fully realize the possibility to shape the amplitude and phase of XUV pulses. Such a development would open the door for ultrafast XUV quantum control.
Abstract Ultrashort, coherent light pulses in the extreme ultraviolet (XUV) wavelength region are excellent tools for a wide range of experiments. These XUV pulses are in particular used to characterize electron dynamics. Additionally, the high photon energy enables quantum control of short-lived transitions in atoms. These transitions are of interest for ultrafast quantum control as the bandwidth of the control pulses needs to be less than the transition frequency. Coherent XUV pulses would be even more useful if the tools to control and manipulate them existed. Presently, however, no modulators exist for these frequencies, which significantly reduces the number of possible ultrafast optics experiments and applications in the XUV regime. This Ph.D. tutorial addresses this problem and focuses on the control of XUV light in time and space. To enable control of XUV light we have developed a method for opto-optical modulation (OOM), which modulates the phase of XUV light emitted from a gas of atoms. The atoms are resonantly excited with a coherent XUV pulse generated through high order harmonic generation and emit light after the excitation pulse passed. By shifting the resonance frequencies through the AC Stark shift with a non-resonant infrared control pulse, the phase of the emitted light, and therefore its wavefront, is controlled. With OOM the direction of XUV light emitted from noble gases has been controlled, and the temporal dynamics of the emission studied. By varying the delay between the excitation and the control pulse, the time of redirection was controlled, which enabled high signal to noise study of the temporal dynamics of the emission. Furthermore, a proof-of-principle experiment with two control pulses was performed, resulting in a shaped XUV pulse with controlled duration. The technique of OOM presented in this article is still at a very early stage and in order to obtain complete control of the amplitude and phase of the XUV pulses further development is necessary. Such development would present new opportunities for ultrafast XUV quantum control.
Whenever scientific tools are significantly advanced; new discoveries soon follow. My thesis work relies on advances in ultrafast laser technology that allow precise control over the shape of sub 20-fs laser pulses. This laser system enabled many new experiments that yielded significant advances in attosecond science, atomic physics; extreme nonlinear optics, quantum chemistry, coherent control, molecular physics, ultrafast optical phase modulation, EUV coherent imagines, and EUV radiation sources. By using an automated learning control algorithm coupled to our deformable mirror pulse shaper; we have demonstrated the control of a process on an attosecond time-scale for the first time. We demonstrate the manipulation of the phase of an electron wave packet, allowing us to tailor the EUV spectrum generated by high-order harmonic generation. These optimal fields were discovered by a learning algorithm that both found an unknown optimal solution; but also discovered an unknown phase-matching mechanism that occurs in the interaction of a single atom and light pulse. We control molecular vibrational and rotational coherences with the same learning algorithm; demonstrating selective control in room temperature molecules at atmospheric pressures. Moreover, we demonstrate that modifications to the algorithm can help automatically uncover the physics of the control mechanism found by the learning algorithm. We also demonstrate a new pulse-compression technique using rotational phase modulation, where optical pulses were compressed by an order of magnitude after phase modulation by a molecular rotational coherence and subsequent propagation through a transparent window. This technique will enable efficient pulse compression in the deep-UV. Finally, we measure the coherence of EUV light generated by high-harmonic upconversion of a femtosecond laser. In phase-matched hollow-fiber geometry, the EUV light exhibits the highest inherent spatial coherence of any source in this region of the spectrum. We use this source to demonstrate the coherent image with first table-top EUV radiation. Since this source exhibits full spatial coherence at very short wavelength, this light source represents has smallest inherent effective source-size of any light source yet created. We also demonstrate that the spectrum of an optical field can be determined by measuring the interference of a double-slit pattern.
Creating and controlling well-defined single-photon states is important for many quantum enhanced technologies. Information can be encoded in any degree of freedom associated with a single-photon field excitation, for example in the polarization or transverse spatial mode structure. The ability to encode multiple qubits in these states is desirable for high data transmission rates and increased information processing capacity. The spectral-temporal domain offers a large Hilbert space for encoding information, well suited to integrated optical architectures owing to the low cross-talk between channels. Indeed, time-frequency encoding is an integral component of existing information technologies infrastructure. Thus, complete, coherent control of the spectral-temporal mode structure of light is essential to advancing optical quantum technologies. Arbitrary control of single-photon states has been demonstrated in the polarization and spatial-momentum degrees of freedom however, is yet to be established in the spectral-temporal domain. Recently it was shown that spectral-temporal pulse shaping is experimentally feasible using nonlinear optical methods. However, such techniques can introduce noise photons, are challenging to implement deterministically and require specially prepared auxiliary pump pulses. Furthermore, they are typically only possible at relatively low repetition rates to avoid damage of nonlinear optical materials. Here, we demonstrate deterministic pulse shaping of single-photon wave packets by introducing a time-varying phase. Applying linear or quadratic phase to the wave packet introduces a spectral shift or spectral broadening, respectively. Achieving significant spectral manipulation requires temporal-phase modulation on the order of π. The phase must also vary on the same time scale as the optical pulses, approximately 1 ps in duration here. This relatively rapid phase variation is achieved using a fast electro-optic phase modulator. The modulator is driven by a time-varying voltage that is synchronized with a pulse train of single-photon wave packets for accurate temporal phase control. In this thesis, we experimentally demonstrate control of the spectral-temporal state of single-photon wave packets using this method. Heralded single-photon wave packets are generated by spontaneous parametric down conversion pumped by a frequency-doubled Titanium-Sapphire laser oscillator with 80 MHz repetition rate. To achieve significant modulation of single-photon pulses a 10 V peak-to-peak radio-frequency signal of 40 GHz drives the phase modulator, which requires approximately 3.6 V to achieve a π phase shift. The signal is synchronized with the oscillator pulse train using custom designed electronics. Details of these electronics are presented, resulting in a robust phase and amplitude controllable 40 GHz voltage source, phase locked to the single-photon pulse train. To demonstrate the utility of this pulse-shaping method we experimentally show spectral shearing of almost 1 nm for single-photon wave packets with 830 nm central wavelength and 1 nm bandwidth. Measurement of the second-order intensity correlation before and after the wave-packet manipulation remains constant within uncertainty of the measurement, showing that the quantum nature of the single-photon source is not deteriorated by the modulator. Preservation of the wave-packet coherence is verified by two-photon interference between spectrally sheared and non-modulated single-photons.
Quantum opto-mechanics is a fast moving, broad research field which aims to investigate and control the interaction of light and the quantized motion of mechanical objects and the coupling between them. This allows one to engineer the mechanical quantum state by controlling and measuring the electromagnetic field, and conversely, to control the dynamical evolution of the optical field via its interaction with a mechanical system. Mechanical resonators are accessible in many different shapes and sizes, from kilogram scales in experiments that test gravitational theories to micro- and nano-scales in resolved sideband regime, where the frequency of the mechanical resonator is larger than the bandwidth of the optical cavity. In this regime, it is possible to cool the mechanical object to the ground state which allows a high degree of control and the ability to prepare interesting non-classical states, states that could aid in investigating the quantum dynamics of macroscopic objects. The field of quantum opto-mechanics is a promising testbed for quantum control technologies, such as fundamental tests of quantum mechanics, ultra-sensitive quantum sensors for precise measurements, phonon lasing, mechanical memories with long lifetime and quantum information processing. Furthermore, experiments are progressing toward strong opto-mechanical coupling regimes with single photons. This creates a platform that can take advantage of the nonlinear optical interactions to generate highly non-classical states in such light-matter interfaces. Photonic systems working in the single photon regime will be promising for low power applications and also for implementations of quantum information and computation. Motivated by these applications, this thesis consists of theoretical studies in the context of single photonics. This includes investigating non-classical mechanical state generation and mechanically controlling the dynamical evolution of optical fields in the strong coupling regime single photon opto-mechanics and furthermore, proposing a quantum sensor using single photonics. In this regard, we employ three important formalisms to treat and measure open quantum systems with non-Gaussian input fields: the conditional and unconditional cascaded master equations, Fock-state master equations and input-output Langevin equations. In the context of opto-mechanics, the system to be investigated is composed of two optical cavities with a coupling modulated via a mechanical resonator. In one case, a sequence of single photons are irreversibly sent to one of the optical cavities. After photons go through the opto-mechanical interaction, photon counting measurements are performed on the cavity output, conditionally steering the mechanical state to a highly non-classical Fock state. Numerical calculations are performed to predict the experimental parameters needed to generate a mechanical Fock state before the mechanical object is thermalized. In another case, the same opto-mechanical scheme is employed to conversely modify the state of the optical mode by engineering the state of the mechanical degree of freedom. In this case, it is shown that the opto-mechanical system operates as an effective beam splitter for the input single photons, with a transmission that can be controlled by tuning the number of excitations in the bulk mechanical resonator. When the mechanical resonator has a small coherent amplitude it acts as a quantum control, entangling the optical and mechanical degrees of freedom. As the coherent amplitude of the resonator increases, it acts as a classical control for the input photons. Finally, we propose a novel multi-purpose sensor architecture that can be used for force, refractive index and possibly local temperature detection. In this scheme, two coupled cavities behave as an effective beam splitter. This sensor is based on fourth order interference (the Hong-Ou-Mandel effect) and requires a sequence of single photon pulses and consequently has low pulse power. Changes in the parameter to be measured induce variations in the effective beam splitter reflectivity and result in changes to the visibility of interference. We propose that this generic scheme could be implemented with coupled L3 photonic crystal cavities and find that this system, which only relies on photon coincidence detection and does not need any spectral resolution, can estimate forces as small as 10-7 Newtons and can measure one part per million change in refractive index using a very low input power of 10-10 W.
Coherent control schemes are interference-based procedures for the control of quantum mechanical systems informed by a careful analysis of the physical conditions on interference. In this thesis, the coherent control approach is applied to experimental phase control in the condensed phase. Specifically, coherent control schemes are proposed as mechanisms for experimental manifestations of phase interference. First, a simulation of a ``black box'' feedback control experiment using realistic pulse shaping is shown to automatically find a specific, previously devised coherent control scheme. Qualitative features of experiments performed in this way are reproduced. Second, an analysis of interference in one-photon phase control yields an upper bound on the duration of phase effects. One-photon phase control was previously shown to be possible only over the transient (as opposed to steady-state) value of observables. The bound described here quantifies this statement and provide a rigorous definition of ``transient'' control. We propose that phase control beyond this bound, as reported in a number of weak-field experimental and computational studies, is the result of previously unaccounted for multiphoton effects. Third, we analyze a recent experiment showing phase control of the macroscopic current emanating from living brain cells photostimulated by two-photon absorption. We propose mechanisms for the phase dependence of the current that operate over fifteen orders of magnitude in time, from the femtosecond dynamics of light-matter interactions to the macroscopic dynamics of neuron current. Significantly, coherent control is extended to the case of systems repeatedly interacting with pulses of light; we show that macroscopic control is obtained, in this case, from the multi-pulse accumulation of small phase effects. Research into multiphoton control led to the development of a novel algorithm to compute higher order perturbation theory integrals, presented in the final chapter of this thesis. The Fourier-Laplace Inversion of the Perturbation Theory (FLIPT) method is a highly efficient, numerically exact, ``black box'' integration algorithm. The FLIPT method exploits the specific structure of the multidimensional perturbation theory integrals to obtain an exponential improvement in performance over standard quadrature.