Light-electron interactions generate synthetic momentum-space dynamics that can be used to engineer free electron quantum states. Here we develop coherent control protocols in which the optical phase acts as the controllable hopping phase of a Floquet-Bloch momentum lattice. Pontryagin optimization designs phase-only waveforms that prepare selected momentum populations and coherent few-sideband superpositions with programmable relative phases. In a complementary Bragg regime protocol, dynamical phase matching selectively couples neighboring sidebands and enables deterministic sequential state synthesis. Full wave-packet simulations based on the minimal-coupling Hamiltonian identify the tolerance window set by phase noise, detuning, and finite momentum spread. The two protocols expose a speed-selectivity tradeoff between ultrafast multilevel interference control and slower resonant engineering, establishing programmable free electron sidebands as a platform for ultrafast quantum state synthesis.
Light-electron interactions generate synthetic momentum-space dynamics that can be used to engineer free electron quantum states. Here we develop coherent control protocols in which the optical phase acts as the controllable hopping phase of a Floquet-Bloch momentum lattice. Pontryagin optimization designs phase-only waveforms that prepare selected momentum populations and coherent few-sideband superpositions with programmable relative phases. In a complementary Bragg regime protocol, dynamical phase matching selectively couples neighboring sidebands and enables deterministic sequential state synthesis. Full wave-packet simulations based on the minimal-coupling Hamiltonian identify the tolerance window set by phase noise, detuning, and finite momentum spread. The two protocols expose a speed-selectivity tradeoff between ultrafast multilevel interference control and slower resonant engineering, establishing programmable free electron sidebands as a platform for ultrafast quantum state synthesis.
The pursuit of programmable light sources with high coherence and spectral purity hinges on establishing a precise set of phase relationships in light-matter interactions. Here, we demonstrate that the quadratic dispersion of a freely propagating electron wave packet serves as a programmable quantum medium. Prepared in a coherent momentum-state ladder via a single laser interaction, the electron subsequently undergoes deterministic phase evolution during free propagation-an intrinsic process that compiles its quantum state into two distinct output channels. This mechanism, quantified by a quantum bunching factor, enables (i) Talbot-resonant bunching, where the electron density self-structures into subcycle combs with tunable harmonic selectivity, and (ii) coherent phase transfer of the programmed quadratic phase to light, generating nonclassical photon states such as multicomponent Schrödinger cat states via energy-resolved electron readout. This quadratic-phase programming provides a drift-section platform for Talbot-selected coherent short-wavelength emission and nonclassical light synthesis based on electron self-interference.
Coherent optical modulation of free-electron wavepackets offers a route to ultrafast beam steering, energy exchange, temporal compression, and quantum-state shaping. Recent advances in photon-induced near-field electron microscopy (PINEM), ultrafast Kapitza-Dirac effect (KDE) and dielectric laser acceleration (DLA) have demonstrated strong light-electron coupling, but longitudinal energy modulation, transverse momentum transfer, and wavepacket-dependent diffraction are still commonly described with separate models. Here, we develop a unified Light-Electron Modulation (LEM) framework that treats optical near fields as programmable phase modulators for free-electron wavepackets. Within this framework, we identify longitudinal and transverse modulation channels, analogous to electro-optic phase modulation and acousto-optic diffraction of light, respectively, and show how their operation depends on wavepacket extent, recoil, phase matching, and optical-field geometry. This formulation organizes PINEM, Raman-Nath and Bragg diffraction, DLA-like acceleration, and anomalous PINEM as limiting regimes of a common modulation picture. The resulting framework provides design principles for free-electron modulators that can control energy spectra, temporal density, transverse wavefronts, and electron-photon quantum interfaces, establishing LEM as a device-level platform for programmable femtosecond-to-attosecond matter-wave control.
Nonclassical states of light are central resources for quantum metrology and quantum information, yet most high performance squeezing platforms operate in narrowband or continuous-wave regimes where the quantum noise is effectively stationary. This work advances ultrafast quantum optics by demonstrating how squeezed states can be generated, measured, and engineered on femtosecond and attosecond time scales, so that quantum fluctuations become a controllable property of the optical waveform itself. In this work, broadband few-cycle coherent drivers are produced using the light field synthesizer (LFS) setup that coherently combines UV/VIS/NIR channels with independently adjustable delays and amplitudes. Ultrafast squeezed light is generated via degenerate four-wave mixing (DFWM) in fused silica using a three-beam interaction geometry, implemented as a quantum light field squeezer (QLFS) that enables quasi-collinear phase matching across a wide bandwidth. A metrology framework compatible with ultrashort pulses is developed: amplitude (intensity) uncertainty is extracted from shot-to-shot spectral statistics, while relative phase fluctuations are retrieved from spectral-interference fringes in channel-overlap regions. These observables are connected to a displaced squeezed state model by fitting variance expressions, enabling phase-space visualization through Wigner function reconstruction. Beyond static squeezing, the QLFS provides attosecond-resolved control of the generated quantum state by tuning inter-pulse delay and phase matching geometry, allowing the redistribution of uncertainty between conjugate quadratures and revealing time-dependent (sub-cycle) structure of the intensity uncertainty within the optical cycle. Finally, the work extends ultrafast quantum optics into solid-state systems by demonstrating squeezed light driven tunneling in a graphene-silicon-graphene phototransistor, where state-dependent modulation of current noise is observed alongside simultaneous optical uncertainty measurements. Together, these results establish a practical route to waveform-level quantum state engineering and motivate future ultrafast quantum metrology, strong field quantum optics control, and hybrid photonic electronic quantum technologies.
Coherent dynamics of interacting quantum particles plays a central role in the study of strongly correlated quantum matter and the pursuit of quantum information processors. Here, we present the state space of interacting Rydberg atoms as a synthetic landscape on which to control and observe coherent and correlated dynamics. With full control of the coupling strengths and energy offsets between the pairs of sites in a nine-site synthetic lattice, we realize quantum walks, Bloch oscillations, and dynamics in an Escher-type "continuous staircase." In the interacting regime, we observe correlated quantum walks, Bloch oscillations, and confinement of particle pairs. Additionally, we simultaneously tilt our lattice both up and down to achieve coherent pair oscillations. When combined with a few straightforward upgrades, this work establishes synthetic Rydberg lattices of interacting atom arrays as a promising platform for programmable quantum many-body dynamics with access to features that are difficult to realize in real-space lattices.
The scalable preparation of large photon-number (Fock) states is a long-standing frontier in quantum science, with direct implications for quantum metrology and bosonic quantum information processing. Despite substantial progress at small photon numbers, extending state generation to large photon numbers while maintaining high fidelity and operating deterministically remains a significant challenge. Here we demonstrate a scalable and experimentally accessible control protocol for generating large photon-number states using only native spin--oscillator operations. The protocol alternates Jaynes--Cummings interactions with phase-space displacements to imprint photon-number--dependent phases and convert them into selective interference in photon-number space. It already achieves high preparation fidelity unconditionally, while an optional final qubit projection removes residual qubit--field correlations and further enhances the fidelity. Conditioned on this final projection, photon-number state preparation with fidelities exceeding 0.95 is achieved for photon numbers in the few-hundred regime, with a success probability exceeding 0.90, placing the protocol in a near-deterministic operating regime. The resulting control sequences remain shallow and are robust against detuning, control noise, and experimentally relevant dissipation. Our results establish a practical route to scalable, high-fidelity photon-number state preparation at large photon numbers and provide a versatile interference-engineering toolbox for nonclassical bosonic state synthesis.
Experimental and theoretical work is presented on the control of wave packet dynamics in atomic and molecular systems. Using sequences of phase-locked optical pulses, the link between optical phase and quantum mechanical phase is explored in the Na atom and Naj dimer, representing a step towards the logical engineering of quantum states in more complicated systems. A novel apparatus, constructed to study and control the vibrational dynamics of vibrational wave packets on the Na ionic potential surface, is described in chapter 3. Theoretical simulations for proposed experiment are presented in chapter 4. Control is achieved by exploiting the phase-evolution of the constituent vibrational quantum states within the wave packet superposition. The phase relationship and the accumulated phase difference between the various components of the wave packet is determined, and a sequence of phase-locked optical pulses is employed to selectively enhance or depopulate specific vibrational states, or sets of vibrational states. The quantum state composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multi-pulse response of the time-dependent vibrational state populations. In chapter 5, the quantum interference between Rydberg electron wave packets in the Na atom is investigated using pairs of phase-locked wave packets, allowing manipulation of the total orbital angular momentum of Na Rydberg atoms. Initially the wave packet is composed of a superposition of s and d Rydberg series. Exploitation of the difference between the quantum defects of the two series allows specific angular momentum compositions within the resultant wave packet to be engineered. Experimentally, this final quantum state distribution is analysed in the frequency domain using state selective field ionisation, and in the time domain using the optical Ramsey method. The theoretical calculations show how the phase difference between pairs of optical pulses is linked to the corresponding Rydberg frequency spectrum, therefore enabling the control of the quantum state composition of the wave packets.