We investigate the dissociation dynamics of hydrogen molecular ions driven by nonclassical light by solving the time-dependent Schrödinger equation. The driving field is composed of horizontally polarized 400 nm coherent light and vertically polarized 800 nm quantum squeezed light. Our results reveal that the photon quantum fluctuations encoded in the squeezing parameter influence the kinetic energy release spectra and modulate the relative yields of competing dissociation channels. In particular, the photon-number statistics and phase uncertainty introduced by the quadrature-squeezed light can selectively enhance or suppress specific dissociation pathways. These findings highlight the potential of quantum light as a tunable resource for manipulating and probing the molecular dynamics. This Letter has implications on ultrafast chemistry with quantum light.
We investigate the dissociation dynamics of hydrogen molecular ions driven by nonclassical light by solving the time-dependent Schrödinger equation. The driving field is composed of horizontally polarized 400 nm coherent light and vertically polarized 800 nm quantum squeezed light. Our results reveal that the photon quantum fluctuations encoded in the squeezing parameter influence the kinetic energy release spectra and modulate the relative yields of competing dissociation channels. In particular, the photon-number statistics and phase uncertainty introduced by the quadrature-squeezed light can selectively enhance or suppress specific dissociation pathways. These findings highlight the potential of quantum light as a tunable resource for manipulating and probing the molecular dynamics. This Letter has implications on ultrafast chemistry with quantum light.
Squeezed coherent quantum light is described by the complex squeeze parameter ζ = s e i ϑ and the coherent-state displacement parameter β = | β | e i ϕ β . Our study of strong-field ionization [D. Habibović and D. B. Milošević, ], which focused on bright squeezed vacuum quantum light with β = 0 and s ≫ 1 , is extended to ionization by squeezed coherent light. It is shown that the amplitudes s and | β | strongly influence the ionization process, whereas phases ϑ and ϕ β play a less significant role. The present work provides a unified treatment of coherent, squeezed vacuum, and squeezed coherent light within a single theoretical framework. The quantum nature of the driving field is incorporated by averaging the strong-field ionization probability over the Husimi-Kano phase-space distribution. Using neon as a representative target, we analyze how the parameters characterizing squeezed coherent light modify photoelectron spectra and intensity-dependent enhancements. We show that nonclassical photon statistics can lead to a pronounced steepening of the rescattering plateau and, at low mean intensities, to an effective suppression of the nominal high-energy cutoff. These effects originate from the reduced weight of high-intensity field components inherent to squeezed states and have no analog in strong-field ionization driven by a coherent light. Our results highlight the potential for quantum-statistical control of strong-field ionization and provide a foundation for exploring laser-matter interactions driven by quantum light.
Autler–Townes splitting (ATS) is a hallmark phenomenon of strong light–matter interaction, in which the resonant photoelectron energy spectrum splits into distinct peaks when driven by a strong electromagnetic field. We investigate the Autler–Townes Splitting (ATS) in K 2 molecules with quantum light. The triple splitting structures originating from three-photon ionization are analyzed under different types of driving fields, including bright squeezed vacuum (BSV), phase-squeezed coherent (PSC) light and amplitude-squeezed coherent (ASC) light by numerically solving the time-dependent Schrödinger equation. Compared with the results with the coherent-state (classical) light drive, we show that the ATS dynamics is sensitive with the squeezing parameter of quantum light, leading to modifications of the subband structures and splitting magnitudes. In particular, a BSV pulse exhibits a higher splitting efficiency than a classical pulse of the same mean intensity. This work has implications on ultrafast coherent control of molecular reactions with quantum light.
Recently, the intersection of quantum optics and attosecond physics has attracted growing interest. Here, we study the quantum optical signatures of high-harmonic generation (HHG) from solid-state material driven by squeezed coherent states. We find that squeezed coherent states can either enhance or suppress the HHG yields compared to that driven by coherent light, depending on the photon bunching or antibunching characteristics of driving light. The analysis on semiclassical trajectories indicates that the amplitude fluctuation alters the recombination energy, while the phase fluctuation affects the birth and recombination time of electron-hole pairs. By calculating the Husimi Q distributions of HHG, we demonstrate that the squeezing of the two conjugate quadratures of driving light asymmetrically influence the squeezing phase of harmonics. Surprisingly, we find that even under coherent driving, the harmonics still exhibit squeezing due to the highly nonlinear response of solid-state HHG, which was overlooked previously. Numerical calculations of the Mandel parameter are performed to characterize the photon statistics of emitted HHG arising from different microscopic mechanisms. The results indicate that intraband radiation can exhibit a super-Poissonian distribution, while interband emission exhibits sub-Poissonian distribution under coherent driving.
Quantum Dynamics of H2+ in Orthogonal Two-Color Fields
We present full-dimensional quantum simulations of H2+ dissociative ionization driven by strong orthogonal laser fields. We consider equal-frequency orthogonal components, which generate elliptical or circular polarization depending on their relative phase and amplitude, as well as orthogonal 800- and 400-nm two-color fields. These two-dimensional fields strongly modify the fragmentation dynamics. Most notably, we identify a high-energy peak in the proton kinetic-energy-release (KER) spectrum at approximately 4−5 eV that is absent from the corresponding single-color, linearly polarized calculations. The yield of this peak can be coherently controlled by varying the relative carrier-envelope phase of the perpendicular field component. The perpendicular field also disrupts the clear electron-proton energy-sharing pattern observed in the main 3−3.5 eV dissociation channel, indicating more complex multichannel dynamics. Time-dependent state projections and calculations initiated from individual excited states attribute the additional peak to laser-induced vibrational excitation of H2+. Furthermore, the perpendicular field rotates the fragment angular distributions, causing the most probable proton and electron emission directions to deviate substantially from the principal z axis. These findings demonstrate that the spatial and temporal geometry of orthogonal laser fields provides an additional degree of freedom for controlling ultrafast electron-nuclear dynamics.
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.
In the last 20 years, advancements in laser technology have allowed for the production of intense laser pulses with durations in the femtosecond (10⁻¹⁵ second) regime, giving scientists the ability to probe nuclear dynamics on their natural time scale. Study of the dissociated fragments created by these intense fields can be used to learn about the molecular structure and dynamics. The work presented in this thesis focuses on controlling this light–molecule interaction in such a way that we can preferentially dissociate the molecule to a desired final product. The hydrogen molecular ion, HD⁺, as well as LiF serve as simple systems that can be studied theoretically for a broad range of laser parameters. Our goal in using these relatively simple systems is to capture the essential physics of the light–molecule interaction and develop general methods to describe these interactions in more complex systems.