Margaret Gregory, Paul Hockett, Albert Stolow, Varun Makhija
arXiv:2012.04561, Dec. 2020
The application of a matrix-based reconstruction protocol for obtaining Molecular Frame (MF) photoelectron angular distributions (MFPADs) from laboratory frame (LF) measurements (LFPADs) is explored. Similarly to other recent works on the topic of MF reconstruction, this protocol makes use of time-resolved LF measurements, in which a rotational wavepacket is prepared and probed via photoionization, followed by a numerical reconstruction routine; however, in contrast to other methodologies, the protocol developed herein does not require determination of photoionization matrix elements, and consequently takes a relatively simple numerical form (matrix transform making use of the Moore-Penrose inverse). Significantly, the simplicity allows application of the method to the successful reconstruction of MFPADs for polyatomic molecules. The scheme is demonstrated numerically for two realistic cases, N2 and C2H4. The new technique is expected to be generally applicable for a range of MF reconstruction problems involving photoionization of polyatomic molecules.
Update July 2020: now published as Appl. Phys. Lett. 117, 044001 (2020); https://doi.org/10.1063/5.0012429
[Submitted on 1 May 2020]
Peter Svihra, Yingwen Zhang, Paul Hockett, Steven Ferrante, Benjamin Sussman, Duncan England, Andrei Nomerotski
We describe a simple multivariate technique of likelihood ratios for improved discrimination of signal and background in multi-dimensional quantum target detection. The technique combines two independent variables, time difference and summed energy, of a photon pair from the spontaneous parametric down-conversion source into an optimal discriminant. The discriminant performance was studied in experimental data and in Monte-Carlo modelling with clear improvement shown compared to previous techniques. As novel detectors become available, we expect this type of multivariate analysis to become increasingly important in multi-dimensional quantum optics.
Yusong Liu, Spencer L. Horton, Jie Yang, J. Pedro F. Nunes, Xiaozhe Shen, Thomas J. A. Wolf, Ruaridh Forbes, Chuan Cheng, Bryan Moore, Martin Centurion, Kareem Hegazy, Renkai Li, Ming-Fu Lin, Albert Stolow, Paul Hockett, Tamás Rozgonyi, Philipp Marquetand, Xijie Wang, and Thomas Weinacht
Pump-probe measurements aim to capture the motion of electrons and nuclei on their natural timescales (femtoseconds to attoseconds) as chemical and physical transformations take place, effectively making “molecular movies” with short light pulses. However, the quantum dynamics of interest are filtered by the coordinate-dependent matrix elements of the chosen experimental observable. Thus, it is only through a combination of experimental measurements and theoretical calculations that one can gain insight into the internal dynamics. Here, we report on a combination of structural (relativistic ultrafast electron diffraction, or UED) and spectroscopic (time-resolved photoelectron spectroscopy, or TRPES) measurements to follow the coupled electronic and nuclear dynamics involved in the internal conversion and photodissociation of the polyatomic molecule, diiodomethane (CH2I2). While UED directly probes the 3D nuclear dynamics, TRPES only serves as an indirect probe of nuclear dynamics via Franck-Condon factors, but it is sensitive to electronic energies and configurations, via Koopmans’ correlations and photoelectron angular distributions. These two measurements are interpreted with trajectory surface hopping calculations, which are capable of simulating the observables for both measurements from the same dynamics calculations. The measurements highlight the nonlocal dynamics captured by different groups of trajectories in the calculations. For the first time, both UED and TRPES are combined with theory capable of calculating the observables in both cases, yielding a direct view of the structural and nonadiabatic dynamics involved.
Update Jan 2020: collected results are now online at ePSdata, which supersedes the previous OSF pages. This now includes DOIs for each dataset from Zenodo, and post-processing with the new python version of ePSproc.
An OSF project, collecting photoionization calculations (ePolyScat), and notes, is now available. This will be an ongoing resource for researchers in photoelectron spectroscopy, interferometry and related areas, and is part of our Open Science initiative.
UPDATE May 2020 – now in PRA: Phys. Rev. A 101, 053808 – Published 4 May 2020
Sept. 2019 – New on arXiv
(Submitted on 20 Sep 2019)
Quantum illumination (QI) is a quantum sensing technique, employing the strong correlation between entangled photon pairs, which is capable of significantly improving sensitivity in remote target detection under noisy background conditions when compared to classical sensing schemes. The amount of enhancement is directly proportional to the number of measurable correlated modes between the photon pairs. QI had been demonstrated using degrees of freedoms such as temporal correlations and photon number correlations, but never a combination of two or more such continuous variables. In this work, we utilize both temporal and spectral correlation of entangled photon pairs in QI. We achieved over an order of magnitude reduction to the background noise when compared to utilizing only temporal modes. This work represents an important step in realizing a practical, real-time QI system. The demonstrated technique will also be of importance in many other quantum sensing applications and quantum communications.
Phys. Rev. A 101, 053808 – Published 4 May 2020
Update March 2019 – now in Optics Letters, DOI: 10.1364/OL.44.001427
June 2018 – New on arXiv.
(Submitted on 4 Jun 2018 (v1
), last revised 12 Jun 2018 (this version, v2))
Optically induced ultrafast switching of single photons is demonstrated by rotating the photon polarization via the Kerr effect in a commercially available single mode fiber. A switching efficiency of 97\% is achieved with a ∼1.7\,ps switching time, and signal-to-noise ratio of ∼800. Preservation of the quantum state is confirmed by measuring no significant increase in the second-order autocorrelation function g(2)(0). These values are attained with only nanojoule level pump energies that are produced by a laser oscillator with 80\,MHz repetition rate. The results highlight a simple switching device capable of both high-bandwidth operations and preservation of single-photon properties for applications in photonic quantum processing and ultrafast time-gating or switching.
We investigate the use of correlated photon pair sources for the improved quantum-level detection of a target in the presence of a noise background. Photon pairs are generated by spontaneous four-wave mixing, one photon from each pair (the herald) is measured locally while the other (the signal) is sent to illuminate the target. Following diffuse reflection from the target, the signal photons are detected by a receiver and non-classical timing correlations between the signal and herald are measured in the presence of a configurable background noise source. Quantum correlations from the photon pair source can be used to provide an enhanced signal-to-noise ratio when compared to a classical light source of the same intensity.
Phys. Rev. A 99, 023828 – Published 19 February 2019
arXiv 1811.04113 – Submitted on 9 Nov 2018
Feb 2019: New article in Quantum Science and Technology
Canada ranks among the world’s leading nations in quantum research, building on investments of more than $1 billion in the past decade alone. Canada’s amassed research expertise, growing private-sector impact, and government commitments to innovation and competitiveness, place the country in a strong position, as scientific advances drive quantum technology development. Here, we summarize the steps Canada has taken to build quantum research excellence and to support a growing quantum industrial base. We also discuss Canadian quantum community efforts to solidify and build the nation’s leadership, as the technology revolution unfolds.
Ben Sussman, Paul Corkum, Alexandre Blais, David Cory and Andrea Damascelli
2019 Quantum Sci. Technol. 4 020503
UPDATE June 2018 – Now published in Phys. Rev. A 97, 063417, 2018, DOI: 10.1103/PhysRevA.97.063417
… and in Kaleidoscope.
March 2018: New on arXiv
(1803.01081, Submitted on 3 Mar 2018)
Time-resolved pump-probe measurements of Xe, pumped at 133~nm and probed at 266~nm, are presented. The pump pulse prepared a long-lived hyperfine wavepacket, in the Xe 5p5(2P∘1/2)6s 2[1/2]∘1 manifold (E=77185 cm−1=9.57 eV). The wavepacket was monitored via single-photon ionization, and photoelectron images measured. The images provide angle- and time-resolved data which, when obtained over a large time-window (900~ps), constitute a precision quantum beat spectroscopy measurement of the hyperfine state splittings. Additionally, analysis of the full photoelectron image stack provides a quantum beat imaging modality, in which the Fourier components of the photoelectron images correlated with specific beat components can be obtained. This may also permit the extraction of isotope-resolved photoelectron images in the frequency domain, in cases where nuclear spins (hence beat components) can be uniquely assigned to specific isotopes (as herein), and also provides phase information. The information content of both raw, and inverted, image stacks is investigated, suggesting the utility of the Fourier analysis methodology in cases where images cannot be inverted.
Also available on Authorea.
Full data, code & analysis notes on OSF.
Our work in JCP has the (dubious?) honour of being selected as their Christmas card.
For more details of the work, see the press release (April 2017) and the original article (Feb 2017).