Optical clocks at sea.

Deployed optical clocks will improve positioning for navigational autonomy, provide remote time standards for geophysical monitoring and distributed coherent sensing, allow time synchronization of remote quantum networks and provide operational redundancy for national time standards. Although laboratory optical clocks now reach fractional inaccuracies below 10 (refs. ), transportable versions of these high-performing clocks have limited utility because of their size, environmental sensitivity and cost.

Modal analysis for noise characterization and propagation in a femtosecond oscillator.

We study noise propagation dynamics in a femtosecond oscillator by injecting external noise on the pump intensity. We utilize a spectrally resolved homodyne detection technique that enables simultaneous measurement of amplitude and phase quadrature noises of different spectral bands of the oscillator. We perform a modal analysis of the oscillator noise in which each mode corresponds to a particular temporal/spectral shape of the pulsed light.

Tomography and Purification of the Temporal-Mode Structure of Quantum Light.

High-dimensional quantum information processing promises capabilities beyond the current state of the art, but addressing individual information-carrying modes presents a significant experimental challenge. Here we demonstrate effective high-dimensional operations in the time-frequency domain of nonclassical light. We generate heralded photons with tailored temporal-mode structures through the pulse shaping of a broadband parametric down-conversion pump.

Spectral noise correlations of an ultrafast frequency comb.

Cavity-based noise detection schemes are combined with ultrafast pulse shaping as a means to diagnose the spectral correlations of both the amplitude and phase noise of an ultrafast frequency comb. The comb is divided into ten spectral regions, and the distribution of noise as well as the correlations between all pairs of spectral regions are measured against the quantum limit. These correlations are then represented in the form of classical noise matrices, which furnish a complete description of the underlying comb dynamics.

Efficient retrieval of landscape Hessian: forced optimal covariance adaptive learning.

Knowledge of the Hessian matrix at the landscape optimum of a controlled physical observable offers valuable information about the system robustness to control noise. The Hessian can also assist in physical landscape characterization, which is of particular interest in quantum system control experiments. The recently developed landscape theoretical analysis motivated the compilation of an automated method to learn the Hessian matrix about the global optimum without derivative measurements from noisy data.

Dynamic dimensionality identification for quantum control.

The control of quantum systems with shaped laser pulses presents a paradox since the relative ease with which solutions are discovered appears incompatible with the enormous variety of pulse shapes accessible with a standard pulse shaper. Quantum landscape theory indicates that the relevant search dimensionality is not dictated by the number of pulse shaper elements, but rather is related to the number of states participating in the controlled dynamics. The actual dimensionality is encoded within the sensitivity of the observed yield to all of the pulse shaper elements.

Discriminating biomolecules with coherent control strategies.

The activity of the GAP-Biophotonics research group at the University of Geneva in the field of coherent control for discriminating similar biomolecules, such as flavins, proteins and DNA bases, is presented and future developments are discussed.

Control of nitromethane photoionization efficiency with shaped femtosecond pulses.

The applicability of adaptive femtosecond pulse shaping is studied for achieving selectivity in the photoionization of low-density polyatomic targets. In particular, optimal dynamic discrimination (ODD) techniques exploit intermediate molecular electronic resonances that allow a significant increase in the photoionization efficiency of nitromethane with shaped near-infrared femtosecond pulses. The intensity bias typical of high-photon number, nonresonant ionization is accounted for by reference to a strictly intensity-dependent process.

Resolution of strongly competitive product channels with optimal dynamic discrimination: application to flavins.

Fundamental molecular selectivity limits are probed by exploiting laser-controlled quantum interferences for the creation of distinct spectral signatures in two flavin molecules, erstwhile nearly indistinguishable via steady-state methods. Optimal dynamic discrimination (ODD) uses optimally shaped laser fields to transiently amplify minute molecular variations that would otherwise go unnoticed with linear absorption and fluorescence techniques. ODD is experimentally demonstrated by combining an optimally shaped UV pump pulse with a time-delayed, fluorescence-depleting IR pulse for discrimination amongst riboflavin and flavin mononucleotide in aqueous solution, which are structurally and spectroscopically very similar.

How shaped light discriminates nearly identical biochromophores.

We present a general mechanism for successful discrimination of spectroscopically indistinguishable biochromophores by shaped light. For this purpose we use nonadiabatic dynamics in excited electronic states in the frame of the field-induced surface hopping method driven by the experimentally shaped laser fields. Our findings show that optimal laser fields drive low-frequency vibrational modes localized in the side chains of two biochromophores, thus selecting the parts of their potential energy surfaces characterized by different transition dipole moments leading to different ionization probabilities.

Quantum control of tightly competitive product channels.

Fundamental selectivity limits of quantum control are pushed by introducing laser driven optimal dynamic discrimination to create distinguishing excitations on two nearly identical flavin molecules. Even with modest spectral resources, significant specificity is achieved with optimal pulse shapes, which amplify small molecular differences to create distinct, identifying signals. Rather than being a hindrance, system complexity appears to aid the control process and augments control field capability, which bodes well for implementation of quantum control in a variety of demanding applications.