Leigh S. Martin

Attosecond vacuum UV coherent control of molecular dynamics

Significance We show that we can precisely control molecular dynamics on both nuclear (i.e., femtosecond) and electronic (i.e., attosecond) timescales. By using attosecond vacuum UV light pulse trains that are tunable in the frequency domain, we show that it is possible to switch population between electronically excited states of a neutral molecule on attosecond time scales, and use this ability to coherently control excitation and ionization through specific pathways. This paper represents a milestone advance because almost two decades after attosecond physics was demonstrated, attosecond chemistry has not yet been fully established because the wavelength and bandwidth of attosecond pulses did not well match molecular quantum states. The richness and complexity of the dynamics, even in a simple molecule, is remarkable and daunting. High harmonic light sources make it possible to access attosecond timescales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics, the concept of attosecond chemistry has not yet been realized; this is because excitation and manipulation of molecular orbitals requires precisely controlled attosecond waveforms in the deep UV, which have not yet been synthesized. Here, we present a unique approach using attosecond vacuum UV pulse-trains to coherently excite and control the outcome of a simple chemical reaction in a deuterium molecule in a non-Born–Oppenheimer regime. By controlling the interfering pathways of electron wave packets in the excited neutral and singly ionized molecule, we unambiguously show that we can switch the excited electronic state on attosecond timescales, coherently guide the nuclear wave packets to dictate the way a neutral molecule vibrates, and steer and manipulate the ionization and dissociation channels. Furthermore, through advanced theory, we succeed in rigorously modeling multiscale electron and nuclear quantum control in a molecule. The observed richness and complexity of the dynamics, even in this very simplest of molecules, is both remarkable and daunting, and presents intriguing new possibilities for bridging the gap between attosecond physics and attochemistry.

High numerical aperture reflection mode coherent diffraction microscopy using off-axis apertured illumination.

We extend coherent diffraction imaging (CDI) to a high numerical aperture reflection mode geometry for the first time. We derive a coordinate transform that allows us to rewrite the recorded far-field scatter pattern from a tilted object as a uniformly spaced Fourier transform. Using this approach, FFTs in standard iterative phase retrieval algorithms can be used to significantly speed up the image reconstruction times. Moreover, we avoid the isolated sample requirement by imaging a pinhole onto the specimen, in a technique termed apertured illumination CDI. By combining the new coordinate transformation with apertured illumination CDI, we demonstrate rapid high numerical aperture imaging of samples illuminated by visible laser light. Finally, we demonstrate future promise for this technique by using high harmonic beams for high numerical aperture reflection mode imaging.

Quantum dynamics of simultaneously measured non-commuting observables

In quantum mechanics, measurements cause wavefunction collapse that yields precise outcomes, whereas for non-commuting observables such as position and momentum Heisenberg’s uncertainty principle limits the intrinsic precision of a state. Although theoretical work has demonstrated that it should be possible to perform simultaneous non-commuting measurements and has revealed the limits on measurement outcomes, only recently has the dynamics of the quantum state been discussed. To realize this unexplored regime, we simultaneously apply two continuous quantum non-demolition probes of non-commuting observables to a superconducting qubit. We implement multiple readout channels by coupling the qubit to multiple modes of a cavity. To control the measurement observables, we implement a ‘single quadrature’ measurement by driving the qubit and applying cavity sidebands with a relative phase that sets the observable. Here, we use this approach to show that the uncertainty principle governs the dynamics of the wavefunction by enforcing a lower bound on the measurement-induced disturbance. Consequently, as we transition from measuring identical to measuring non-commuting observables, the dynamics make a smooth transition from standard wavefunction collapse to localized persistent diffusion and then to isotropic persistent diffusion. Although the evolution of the state differs markedly from that of a conventional measurement, information about both non-commuting observables is extracted by keeping track of the time ordering of the measurement record, enabling quantum state tomography without alternating measurements. Our work creates novel capabilities for quantum control, including rapid state purification, adaptive measurement, measurement-based state steering and continuous quantum error correction. As physical systems often interact continuously with their environment via non-commuting degrees of freedom, our work offers a way to study how notions of contemporary quantum foundations arise in such settings.

Stabilizing Entanglement via Symmetry-Selective Bath Engineering in Superconducting Qubits.

Bath engineering, which utilizes coupling to lossy modes in a quantum system to generate nontrivial steady states, is a tantalizing alternative to gate- and measurement-based quantum science. Here, we demonstrate dissipative stabilization of entanglement between two superconducting transmon qubits in a symmetry-selective manner. We utilize the engineered symmetries of the dissipative environment to stabilize a target Bell state; we further demonstrate suppression of the Bell state of opposite symmetry due to parity selection rules. This implementation is resource efficient, achieves a steady-state fidelity F=0.70, and is scalable to multiple qubits.

A generalization for optimized phase retrieval algorithms

In this work, we demonstrate an improved method for iterative phase retrieval with application to coherent diffractive imaging. By introducing additional operations inside the support term of existing iterated projection algorithms, we demonstrate improved convergence speed, higher success rate and, in some cases, improved reconstruction quality. New algorithms take a particularly simple form with the introduction of a generalized projection-based reflector. Numerical simulations verify that these new algorithms surpass the current standards without adding complexity to the reconstruction process. Thus the introduction of this new class of algorithms offers a new array of methods for efficiently deconvolving intricate data.

Incoherent Qubit Control Using the Quantum Zeno Effect

The quantum Zeno effect is the suppression of Hamiltonian evolution by repeated observation, which pins the system to an eigenstate of the measurement observable. Using measurement alone, control of the state can be achieved if the observable is slowly varied, so that the state tracks the now time-dependent eigenstate. We demonstrate this using a circuit-QED readout technique that couples to a dynamically controllable observable of a qubit. Continuous monitoring of the measurement record allows us to detect an escape from the eigenstate, thus serving as a built-in form of error detection. We show this by postselecting on realizations with high fidelity with respect to the target state. Our dynamical measurement operator technique offers a new tool for numerous forms of quantum feedback protocols, including adaptive measurements and rapid state purification.

Attosecond Coherent Control of Single and Double Photoionization in Argon

Ultrafast high harmonic beams provide new opportunities for coherently controlling excitation and ionization processes in atoms, molecules, and materials on attosecond time scales by employing multiphoton two-pathway electron-wave-packet quantum interferences. Here we use spectrally tailored and frequency tuned vacuum and extreme ultraviolet harmonic combs, together with two phase-locked infrared laser fields, to show how the total single and double photoionization yields of argon can be coherently modulated by controlling the relative phases of both optical and electronic-wave-packet quantum interferences. This Letter is the first to apply quantum control techniques to double photoionization, which is a fundamental process where a single, high-energy photon ionizes two electrons simultaneously from an atom.

Mapping ultrafast dynamics of highly excited D2+ by ultrashort XUV pump - IR probe radiation

An ultrashort XUV laser pulse ionizes the D2 molecule creating an electronic and nuclear wave packet, with the dominant contributions from the 2sσg and 2pπu ionic states. A delayed interaction with a 780 nm IR field ejects the second electron, leading to the Coulomb explosion of the molecule, whose nuclear fragments, recorded in coincidence, map the dynamics associated to those two ionic excited states. By varying the orientation of the light polarization, one can control the molecular dynamics by modifying the ratio between the ionic states. Experimental and ab initio theoretical data are jointly reported.

Coherent diffraction imaging with an apertured illumination support

We demonstrate coherent diffraction imaging (CDI) using the projected image of an aperture as a support. This method is strikingly simple and allows CDI imaging of non-isolated objects in transmission and reflection.