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Journal articleRuberti M, Patchkovskii S, Averbukh V, 2022,
Quantum coherence in molecular photoionization
, PHYSICAL CHEMISTRY CHEMICAL PHYSICS, Vol: 24, Pages: 19673-19686, ISSN: 1463-9076- Author Web Link
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- Citations: 6
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Journal articleMaimaris M, Pettipher AJ, Azzouzi M, et al., 2022,
Sub-10-fs observation of bound exciton formation in organic optoelectronic devices
, Nature Communications, Vol: 13, ISSN: 2041-1723Fundamental mechanisms underlying exciton formation in organic semiconductors are complex and elusive as it occurs on ultrashort sub-100-fs timescales. Some fundamental aspects of this process, such as the evolution of exciton binding energy, have not been resolved in time experimentally. Here, we apply a combination of sub-10-fs Pump-Push-Photocurrent, Pump-Push-Photoluminescence, and Pump-Probe spectroscopies to polyfluorene devices to track the ultrafast formation of excitons. While Pump-Probe is sensitive to the total concentration of excited states, Pump-Push-Photocurrent and Pump-Push-Photoluminescence are sensitive to bound states only, providing access to exciton binding dynamics. We find that excitons created by near-absorption-edge photons are intrinsically bound states, or become such within 10 fs after excitation. Meanwhile, excitons with a modest >0.3 eV excess energy can dissociate spontaneously within 50 fs before acquiring bound character. These conclusions are supported by excited-state molecular dynamics simulations and a global kinetic model which quantitatively reproduce experimental data.
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Journal articleLiu X, Wang W, Wright SC, et al., 2022,
The chemistry of AlF and CaF production in buffer gas sources
, JOURNAL OF CHEMICAL PHYSICS, Vol: 157, ISSN: 0021-9606 -
Journal articleTarrant J, Khokhlova M, Averbukh V, 2022,
Interferometry of quantum revivals
, JOURNAL OF CHEMICAL PHYSICS, Vol: 157, ISSN: 0021-9606- Author Web Link
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- Citations: 1
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Journal articleSauvage F, Mintert F, 2022,
Optimal Control of Families of Quantum Gates
, PHYSICAL REVIEW LETTERS, Vol: 129, ISSN: 0031-9007- Author Web Link
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- Citations: 4
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Journal articleLi Z-P, Wang Y-T, Yu S, et al., 2022,
Experimental investigation of high-efficiency weak-value amplification of nonunitary evolution
, PHYSICAL REVIEW A, Vol: 106, ISSN: 2469-9926 -
Journal articleMa Y, Pace MCC, Kim MS, 2022,
Unifying the sorensen-molmer gate and the milburn gate with an optomechanical example
, Physical Review A: Atomic, Molecular and Optical Physics, Vol: 106, ISSN: 1050-2947The Sørensen-Mølmer gate and Milburn gate are two geometric phase gates, generating nonlinear self-interaction of a target mode via its interaction with an auxiliary mechanical mode, in the continuous- and pulsed-interaction regimes, respectively. In this paper we aim at unifying the two gates by demonstrating that the Sørensen-Mølmer gate is the continuous limit of the Milburn gate, emphasizing the geometrical interpretation in the mechanical phase space. We explicitly consider imperfect gate parameters, focusing on relative errors in time for the Sørensen-Mølmer gate and in phase angle increment for the Milburn gate. We find that, although the purities of the final states increase for the two gates upon reducing the interaction strength together with traversing the mechanical phase space multiple times, the fidelities behave differently. We point out that the difference exists because the interaction strength depends on the relative error when taking the continuous limit from the pulsed regime, thereby unifying the mathematical framework of the two gates. We demonstrate this unification in the example of an optomechanical system, where mechanical dissipation is also considered. We highlight that the unified framework facilitates our method of deriving the dynamics of the continuous-interaction regime without solving differential equations.
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Journal articleKanari-Naish LA, Clarke J, Qvarfort S, et al., 2022,
Two-mode Schrodinger-cat states with nonlinear optomechanics: generation and verification of non-Gaussian mechanical entanglement
, QUANTUM SCIENCE AND TECHNOLOGY, Vol: 7, ISSN: 2058-9565- Author Web Link
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- Citations: 2
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Journal articleDanilov D, Tran T, Bearpark MJJ, et al., 2022,
How electronic superpositions drive nuclear motion following the creation of a localized hole in the glycine radical cation
, JOURNAL OF CHEMICAL PHYSICS, Vol: 156, ISSN: 0021-9606- Author Web Link
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- Citations: 3
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Journal articleGarratt D, Misiekis L, Wood D, et al., 2022,
Direct observation of ultrafast exciton localization in an organic semiconductor with soft X-ray transient absorption spectroscopy
, Nature Communications, Vol: 13, ISSN: 2041-1723The localization dynamics of excitons in organic semiconductors influence the efficiency of charge transfer and separation in these materials. Here we apply time-resolved X-ray absorption spectroscopy to track photoinduced dynamics of a paradigmatic crystalline conjugated polymer: poly(3-hexylthiophene) (P3HT) commonly used in solar cell devices. The π→π* transition, the first step of solar energy conversion, is pumped with a 15 fs optical pulse and the dynamics are probed by an attosecond soft X-ray pulse at the carbon K-edge. We observe X-ray spectroscopic signatures of the initially hot excitonic state, indicating that it is delocalized over multiple polymer chains. This undergoes a rapid evolution on a sub 50 fs timescale which can be directly associated with cooling and localization to form either a localized exciton or polaron pair.
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Journal articleVoges KK, Gersema P, Hartmann T, et al., 2022,
Hyperfine dependent atom-molecule loss analyzed by the analytic solution of few-body loss equations
, PHYSICAL REVIEW RESEARCH, Vol: 4 -
Journal articleZhao H, Mintert F, Knolle J, et al., 2022,
Localization persisting under aperiodic driving
, PHYSICAL REVIEW B, Vol: 105, ISSN: 2469-9950- Author Web Link
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- Citations: 2
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Journal articleSchwickert D, Ruberti M, Kolorenc P, et al., 2022,
Electronic quantum coherence in glycine molecules probed with ultrashort x-ray pulses in real time
, SCIENCE ADVANCES, Vol: 8, ISSN: 2375-2548- Author Web Link
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- Citations: 10
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Journal articleChevalier H, Kwon H, Khosla KE, et al., 2022,
Many-body probes for quantum features of spacetime
, AVS Quantum Science, Vol: 4, Pages: 1-10, ISSN: 2639-0213Many theories of quantum gravity can be understood as imposing a minimum length scale the signatures of which can potentially be seen in precise table top experiments. In this work, we inspect the capacity for correlated many-body systems to probe non-classicalities of spacetime through modifications of the commutation relations. We find an analytic derivation of the dynamics for a single mode light field interacting with a single mechanical oscillator and with coupled oscillators to first order corrections to the commutation relations. Our solution is valid for any coupling function as we work out the full Magnus expansion. We numerically show that it is possible to have superquadratic scaling of a nonstandard phase term, arising from the modification to the commutation relations, with coupled mechanical oscillators.
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Working paperSun B, Morozko F, Salter PS, et al., 2022,
On-chip beam rotators, polarizers and adiabatic mode converters through low-loss waveguides with variable cross-sections
, Publisher: ArXivPhotonics integrated circuitry would benefit considerably from the ability toarbitrarily control waveguide cross-sections with high precision and low loss,in order to provide more degrees of freedom in manipulating propagating light.Here, we report on a new optical-fibres-compatible glass waveguide byfemtosecond laser writing, namely spherical phase induced multi-core waveguide(SPIM-WG), which addresses this challenging task with three dimensional on-chiplight control. Precise deformation of cross-sections is achievable along thewaveguide, with shapes and sizes finely controllable of high resolution in bothhorizontal and vertical transversal directions. We observed that thesewaveguides have high refractive index contrast of 0.017, low propagation lossof 0.14 dB/cm, and very low coupling loss of 0.19 dB coupled from a single modefibre. SPIM-WG devices were easily fabricated that were able to perform on-chipbeam rotation through varying angles, or manipulate polarization state ofpropagating light for target wavelengths. We also demonstrated SPIM-WG modeconverters that provide arbitrary adiabatic mode conversion with highefficiency between symmetric and asymmetric non-uniform modes; examples includecircular, elliptical modes and asymmetric modes from ppKTP waveguides which aregenerally applied in frequency conversion and quantum light sources. Createdinside optical glass, these waveguides and devices have the capability tooperate across ultra-broad bands from visible to infrared wavelengths. Thecompatibility with optical fibre also paves the way toward packaged photonicintegrated circuitry, which usually needs input and output fibre connections.
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Working paperSempere-Llagostera S, Patel RB, Walmsley IA, et al., 2022,
Experimentally finding dense subgraphs using a time-bin encoded Gaussian boson sampling device
, Publisher: ArxivGaussian Boson Sampling (GBS) is a quantum computing concept based on drawingsamples from a multimode nonclassical Gaussian state using photon-numberresolving detectors. It was initially posed as a near-term approach aiming toachieve quantum advantage, but several applications have been proposed eversince, such as the calculation of graph features or molecular vibronic spectra,among others. For the first time, we use a time-bin encoded interferometer toimplement GBS experimentally and extract samples to enhance the search fordense subgraphs in a graph. Our results indicate an improvement over classicalmethods for subgraphs of sizes three and four in a graph containing ten nodes.In addition, we numerically explore the role of imperfections in the opticalcircuit and on the performance of the algorithm.
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Journal articleWalter N, Seifert J, Truppe S, et al., 2022,
Spectroscopic characterization of singlet-triplet doorway states of aluminum monofluoride
, JOURNAL OF CHEMICAL PHYSICS, Vol: 156, ISSN: 0021-9606 -
Journal articleJoseph D, Martinez AJ, Ling C, et al., 2022,
Quantum mean-value approximator for hard integer-value problems
, PHYSICAL REVIEW A, Vol: 105, ISSN: 2469-9926- Author Web Link
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- Citations: 1
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Journal articleThekkadath G, Sempere-Llagostera S, Bell B, et al., 2022,
Experimental demonstration of Gaussian boson sampling with displacement
, PRX Quantum, Vol: 3, ISSN: 2691-3399Gaussian boson sampling (GBS) is a quantum sampling task in which one has to draw samples from the photon-number distribution of a large-dimensional nonclassical squeezed state of light. In an effort to make this task intractable for a classical computer, experiments building GBS machines have mainly focused on increasing the dimensionality and squeezing strength of the nonclassical light. However, no experiment has yet demonstrated the ability to displace the squeezed state in phase space, which is generally required for practical applications of GBS. In this work, we build a GBS machine that achieves the displacement by injecting a laser beam alongside a two-mode squeezed vacuum state into a 15-mode interferometer. We focus on two new capabilities. Firstly, we use the displacement to reconstruct the multimode Gaussian state at the output of the interferometer. Our reconstruction technique is in situ and requires only three measurement settings regardless of the state dimension. Secondly, we study how the addition of classical laser light in our GBS machine affects the complexity of sampling its output photon statistics. We introduce and validate approximate semiclassical models that reduce the computational cost when a significant fraction of the detected light is classical.
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Journal articleDoppelbauer M, Wright SC, Hofsaess S, et al., 2022,
Hyperfine-resolved optical spectroscopy of the A<SUP>2</SUP>? ? X<SUP>2</SUP>S<SUP>+</SUP> transition in MgF
, JOURNAL OF CHEMICAL PHYSICS, Vol: 156, ISSN: 0021-9606 -
Journal articleBarrett TJ, Evans W, Gadge A, et al., 2022,
An environmental monitoring network for quantum gas experiments and devices
, QUANTUM SCIENCE AND TECHNOLOGY, Vol: 7, ISSN: 2058-9565 -
Journal articleSong W, Lim Y, Jeong K, et al., 2022,
Quantum solvability of noisy linear problems by divide-and-conquer strategy
, Quantum Science and Technology, Vol: 7, ISSN: 2058-9565Noisy linear problems have been studied in various science and engineering disciplines. A class of 'hard' noisy linear problems can be formulated as follows: Given a matrix $\hat{A}$ and a vector b constructed using a finite set of samples, a hidden vector or structure involved in b is obtained by solving a noise-corrupted linear equation $\hat{A}\mathbf{x}\approx \mathbf{b}+\boldsymbol{\eta }$, where η is a noise vector that cannot be identified. For solving such a noisy linear problem, we consider a quantum algorithm based on a divide-and-conquer strategy, wherein a large core process is divided into smaller subprocesses. The algorithm appropriately reduces both the computational complexities and size of a quantum sample. More specifically, if a quantum computer can access a particular reduced form of the quantum samples, polynomial quantum-sample and time complexities are achieved in the main computation. The size of a quantum sample and its executing system can be reduced, e.g., from exponential to sub-exponential with respect to the problem length, which is better than other results we are aware. We analyse the noise model conditions for such a quantum advantage, and show when the divide-and-conquer strategy can be beneficial for quantum noisy linear problems.
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Journal articleZhang C, Zhang C, Cheng L, et al., 2022,
Inner-shell excitation in the YbF molecule and its impact on laser cooling
, Journal of Molecular Spectroscopy, Vol: 386, ISSN: 0022-2852The YbF molecule is a sensitive system for measuring the electron’s electric dipole moment. The precision ofthis measurement can be improved by direct laser cooling of the molecules to ultracold temperature. However,low-lying electronic states arising from excitation of a 4f electron may hinder laser cooling. One set of these ‘‘4fhole’’ states lies below the 𝐴2𝛱1∕2 excited state used for laser cooling, and radiative decay to these intermediatelevels, even with branching ratios as small as 10−5, can be a hindrance. Other 4f hole states lie very close tothe 𝐴2𝛱1∕2 state, and a perturbation results in states of mixed character that are involved in the laser coolingcycle. This perturbation may enhance the loss of molecules to states outside of the laser cooling cycle. Wemodel the perturbation of the 𝐴2𝛱1∕2 state to determine the strength of the coupling between the states, thede-perturbed potential energy curves, and the radiative branching ratios to various vibrational levels of theground state, 𝑋2𝛴+. We use electronic structure calculations to characterize the 4f hole states and the strengthsof transitions between these states and the 𝐴2𝛱1∕2 and 𝑋2𝛴+ states. We identify a leak out of the cooling cyclewith a branching ratio of roughly 5 × 10−4, dominated by the contribution of the ground state configurationin a 4f hole state. Finally, we assess the impact of these results for laser cooling of YbF and molecules withsimilar structure.
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Journal articleWalter N, Doppelbauer M, Marx S, et al., 2022,
Spectroscopic characterization of the a3Π state of aluminum monofluoride.
, J Chem Phys, Vol: 156Spectroscopic studies of aluminum monofluoride (AlF) have revealed its highly favorable properties for direct laser cooling. All Q lines of the strong A1Π ← X1Σ+ transition around 227 nm are rotationally closed and thereby suitable for the main cooling cycle. The same holds for the narrow, spin-forbidden a3Π ← X1Σ+ transition around 367 nm, which has a recoil limit in the µK range. We here report on the spectroscopic characterization of the lowest rotational levels in the a3Π state of AlF for v = 0-8 using a jet-cooled, pulsed molecular beam. An accidental AC Stark shift is observed on the a3Π0, v = 4 ← X1Σ+, v = 4 band. By using time-delayed ionization for state-selective detection of the molecules in the metastable a3Π state at different points along the molecular beam, the radiative lifetime of the a3Π1, v = 0, J = 1 level is experimentally determined as τ = 1.89 ± 0.15 ms. A laser/radio frequency multiple resonance ionization scheme is employed to determine the hyperfine splittings in the a3Π1, v = 5 level. The experimentally derived hyperfine parameters are compared to the outcome of quantum chemistry calculations. A spectral line with a width of 1.27 kHz is recorded between hyperfine levels in the a3Π, v = 0 state. These measurements benchmark the electronic potential of the a3Π state and yield accurate values for the photon scattering rate and for the elements of the Franck-Condon matrix of the a3Π-X1Σ+ system.
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Journal articleWill C, Bohman M, Driscoll T, et al., 2022,
Sympathetic cooling schemes for separately trapped ions coupled via image currents
, NEW JOURNAL OF PHYSICS, Vol: 24, ISSN: 1367-2630 -
Journal articleSchofield RC, Burdekin P, Fasoulakis A, et al., 2022,
Narrow and Stable Single Photon Emission from Dibenzoterrylene in <i>para</i>-Terphenyl Nanocrystals
, CHEMPHYSCHEM, Vol: 23, ISSN: 1439-4235- Author Web Link
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- Citations: 1
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Journal articleKarra M, Cretu MT, Friedrich B, et al., 2022,
Dynamics of translational and rotational thermalization of AlF molecules via collisions with cryogenic helium
, Physical Review A, Vol: 105, ISSN: 2469-9926 -
Journal articleTang H, Banchi L, Wang T-Y, et al., 2022,
Generating Haar-uniform randomness using stochastic quantum walks on a photonic chip
, Physical Review Letters, Vol: 128, ISSN: 0031-9007As random operations for quantum systems are intensively used in various quantum information tasks, a trustworthy measure of the randomness in quantum operations is highly demanded. The Haar measure of randomness is a useful tool with wide applications, such as boson sampling. Recently, a theoretical protocol was proposed to combine quantum control theory and driven stochastic quantum walks to generate Haar-uniform random operations. This opens up a promising route to converting classical randomness to quantum randomness. Here, we implement a two-dimensional stochastic quantum walk on the integrated photonic chip and demonstrate that the average of all distribution profiles converges to the even distribution when the evolution length increases, suggesting the 1-pad Haar-uniform randomness. We further show that our two-dimensional array outperforms the one-dimensional array of the same number of waveguide for the speed of convergence. Our Letter demonstrates a scalable and robust way to generate Haar-uniform randomness that can provide useful building blocks to boost future quantum information techniques.
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Journal articleLi S, Driver T, Rosenberger P, et al., 2022,
Attosecond coherent electron motion in Auger-Meitner decay
, SCIENCE, Vol: 375, Pages: 285-+, ISSN: 0036-8075- Author Web Link
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- Citations: 17
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Journal articleMoroney N, Del Bino L, Zhang S, et al., 2022,
A Kerr polarization controller
, NATURE COMMUNICATIONS, Vol: 13- Author Web Link
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- Citations: 5
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