Article
Chemistry, Physical
Joel Creutzberg, Wojciech Skomorowski, Thomas-C. Jagau
Summary: In this study, we compute the autoionization widths of various Rydberg states of neon and N2 using equation-of-motion coupled-cluster theory combined with complex scaling and complex basis functions. This study represents the first application of complex-variable methods to Rydberg states represented in Gaussian basis sets. A new computational protocol based on Kaufmann basis functions is designed to make these methods applicable to atomic and molecular Rydberg states. The results demonstrate a decrease in the decay width with increasing angular momentum and principal quantum number within both Rydberg series.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Physics, Multidisciplinary
Marcin Kalinowski, Nishad Maskara, Mikhail D. Lukin
Summary: Understanding topological matter is a difficult task in physical science, but programmable quantum simulators have emerged as a powerful tool for studying these systems. This study introduces and analyzes a new method for simulating topological matter using periodic driving. The researchers show that this approach can efficiently explore topological phases of matter and provide insights for further research on materials and lattice gauge theories by utilizing programmable quantum simulators.
Article
Materials Science, Multidisciplinary
Stefanie Czischek, M. Schuyler Moss, Matthew Radzihovsky, Ejaaz Merali, Roger G. Melko
Summary: Rydberg atom arrays are programmable quantum simulators that can prepare various quantum states. Pretraining modern RNNs significantly reduces the convergence time for variational optimization of the wave function, even with small amounts of data.
Article
Physics, Multidisciplinary
D. P. Ornelas-Huerta, Przemyslaw Bienias, Alexander N. Craddock, Michael J. Gullans, Andrew J. Hachtel, Marcin Kalinowski, Mary E. Lyon, Alexey Gorshkov, S. L. Rolston, J. Porto
Summary: Long-range Rydberg interactions combined with EIT can produce strongly interacting photons with tunable and controllable strength, sign, and form of the interactions, allowing for the generation of novel few-photon states. It has been shown that in the Rydberg-EIT system, three-body interactions can be as strong or stronger than two-body interactions. The observed features in the outgoing photonic correlations are strongly suggested to be caused by the resonant enhancement of three-body losses based on numerical simulations and analytical estimates.
PHYSICAL REVIEW LETTERS
(2021)
Article
Engineering, Electrical & Electronic
Danijela Danilovic, Dusan K. Bozanic, Gustavo A. Garcia, Laurent Nahon, Una Stamenovic, Vesna V. Vodnik, Vladimir Djokovic
Summary: The angle-resolved photoelectron spectroscopy of isolated silver sulfide nanoparticles was conducted using velocity map imaging technique. The results show the maximum energy of the valance band and the minimum energy of the conduction band of the nanoparticles, and the onset of inelastic scattering at around 1 eV.
OPTICAL AND QUANTUM ELECTRONICS
(2022)
Article
Chemistry, Multidisciplinary
Ignacio R. Sola, Vladimir S. Malinovsky, Jaewook Ahn, Seokmin Shin, Bo Y. Chang
Summary: By controlling the temporal and spatial features of light, we propose a novel protocol for preparing entangling gates on trapped atoms. The protocol is robust to variations in pulse areas and atom positions, and it uses structured light. We analyze the gate fidelity map and propose generalizations for multi-pulse sequences.
Article
Chemistry, Multidisciplinary
Shoma Hoshino, Kento Ishii, Koichi Tsukiyama
Summary: We investigated the predissociation dynamics of the Rydberg states of Br2 and found the existence of predissociation pathways through ion-pair states and core Rydberg states.
Article
Physics, Multidisciplinary
Rosario Gonzalez-Ferez, Janine Shertzer, H. R. Sadeghpour
Summary: It is predicted that ultralong-range Rydberg bimolecules will form in collisions between polar molecules in cold and ultracold settings, with high energy and permanent electric dipole moments. The Rydberg bimolecules have rotational constants in the MHz range, allowing for microwave spectroscopy and achieving considerable orientation. These molecules hold promise for studying a special class of long-range bimolecular interactions.
PHYSICAL REVIEW LETTERS
(2021)
Article
Multidisciplinary Sciences
Jacob DeLange, Kinjol Barua, Anindya Sundar Paul, Hamid Ohadi, Val Zwiller, Stephan Steinhauer, Hadiseh Alaeian
Summary: Cuprous oxide (Cu2O) is a promising material in solid-state quantum technology due to its excitonic Rydberg states. This study demonstrates the successful synthesis of a Cu2O thin film on a transparent substrate, showcasing Rydberg excitons suitable for photonic device fabrications. These findings mark a significant advancement towards scalable and on-chip integrable Rydberg quantum technologies.
SCIENTIFIC REPORTS
(2023)
Article
Physics, Multidisciplinary
Alexander Guttridge, Daniel K. Ruttley, Archie C. Baldock, Rosario Gonzalez-Ferez, H. R. Sadeghpour, C. S. Adams, Simon L. Cornish
Summary: We demonstrate Rydberg blockade between a single Rb atom and a single RbCs molecule confined in optical tweezers due to charge-dipole interaction. The molecule is efficiently transferred to the rovibrational ground state and the separation between the atom and molecule is controlled using species-specific tweezers. Excitation dynamics are observed to be consistent with simulated interaction potentials, opening up possibilities for transferring quantum information between individually trapped molecules using Rydberg atoms.
PHYSICAL REVIEW LETTERS
(2023)
Article
Physics, Multidisciplinary
Rui Li, Shuang He, Zhi-Jun Meng, Zhao Jin, Wei-Jiang Gong
Summary: We propose a scheme to actively engineer a steady bipartite Knill-Laflamme-Milburn (KLM) entangled state by exploiting the spontaneous emission of excited Rydberg states and coherent population trapping in a neutral atom system. Instead of using antiblockade dynamics, we utilize the Rydberg-Rydberg interaction as the pumping source to drive undesired states without needing to satisfy a specific laser detuning. Numerical simulations show that the fidelity and purity above 98% can be achieved with current feasible parameters, and the steady-state fidelity is robust to variations in the dynamical parameters.
CHINESE PHYSICS LETTERS
(2023)
Article
Physics, Multidisciplinary
Rhine Samajdar, Darshan G. Joshi, Yanting Teng, Subir Sachdev
Summary: Strongly interacting arrays of Rydberg atoms provide versatile platforms for exploring exotic many-body phases and dynamics of correlated quantum systems. Motivated by recent experimental advances, we show that the combination of Rydberg interactions and appropriate lattice geometries naturally leads to emergent Z(2) gauge theories endowed with matter fields. We also discuss the natures of the fractionalized excitations of these Z(2) spin liquid states using both fermionic and bosonic parton theories and illustrate their rich interplay with proximate solid phases.
PHYSICAL REVIEW LETTERS
(2023)
Article
Chemistry, Physical
Mizuho Fushitani, Stephen T. Pratt, Daehyun You, Shu Saito, Yu Luo, Kiyoshi Ueda, Hikaru Fujise, Akiyoshi Hishikawa, Heide Ibrahim, Francois Legare, Per Johnsson, Jasper Peschel, Emma R. Simpson, Anna Olofsson, Johan Mauritsson, Paolo Antonio Carpeggiani, Praveen Kumar Maroju, Matteo Moioli, Dominik Ertel, Ronak Shah, Giuseppe Sansone, Tamas Csizmadia, Mathieu Dumergue, N. G. Harshitha, Sergei Kuhn, Carlo Callegari, Oksana Plekan, Michele Di Fraia, Miltcho B. Danailov, Alexander Demidovich, Luca Giannessi, Lorenzo Raimondi, Marco Zangrando, Giovanni De Ninno, Kevin C. Prince
Summary: By performing time-resolved photoelectron imaging experiments on a group of complex resonances near 15.38 eV in the absorption spectrum of molecular nitrogen, time-dependent oscillations in photoelectron yields and angular distributions have been observed, providing insight into interactions among the resonant intermediate states and their influence on photoelectron production. The exponential decay of photoelectron yields, dependent on the ionic final state, can be rationalized by the different lifetimes of intermediate states contributing to specific ionization channels. Individual photoelectron final states and their angular dependence allow for the identification and differentiation of quantum pathways within this complex system.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Physics, Multidisciplinary
Frederic Hummel, Matthew T. Eiles, Peter Schmelcher
Summary: This study observed a series of conical intersections in the potential energy curves governing both the collision between a Rydberg atom and a ground-state atom and the structure of Rydberg molecules. By using the electronic energy of the Rydberg atom as a synthetic dimension, the von Neumann-Wigner theorem was circumvented. These conical intersections can occur when certain conditions are met, and have a significant impact on the rate of ultracold l-changing collisions.
PHYSICAL REVIEW LETTERS
(2021)
Article
Physics, Multidisciplinary
V. Bharti, S. Sugawa, M. Mizoguchi, M. Kunimi, Y. Zhang, S. de Leseleuc, T. Tomita, T. Franz, M. Weidemueller, K. Ohmori
Summary: This study reports the observation and control of ultrafast many-body dynamics of electrons in ultracold Rydberg-excited atoms. The emergence of many-body correlations and the crucial role of quantum fluctuations in the observed dynamics are deduced from time-domain Ramsey interferometry in the picosecond timescale.
PHYSICAL REVIEW LETTERS
(2023)
Article
Chemistry, Physical
Chris Sparling, Dave Townsend
Summary: This article discusses examples of extracting meaningful information from image projection data using tomographic reconstruction techniques, and introduces alternative strategies for photochemical imaging. The article demonstrates the advantages of these strategies and how they can outperform current commonly used methods. Notably, the Hankel Transform Reconstruction (HTR) provides a bound for the minimum number of projections needed to reliably reconstruct 3D photoproduct distributions.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
D. M. P. Holland, D. A. Shaw, D. Townsend, I Powis
Summary: The absolute photoabsorption cross section of imidazole and 1-methylimidazole was measured using synchrotron radiation, and the absorption spectra were analyzed. It was found that the spectra exhibited several broad bands and sharp structures associated with Rydberg states. Assignments were made for some of the observed absorption bands based on calculated transition energies and oscillator strengths, guided by quantum defect analyses. Natural transition orbital plots indicated a mixed Rydberg/valence character for many of the electronically excited states. The irregularities in transition energies and relative intensities of the absorption bands assigned to Rydberg states were attributed to this mixing. Vibrational progressions of some Rydberg states were interpreted using simulations based on the Franck-Condon model.
Article
Chemistry, Multidisciplinary
Jiangping Liu, Andrew W. Prentice, Guy J. Clarkson, Jack M. Woolley, Vasilios G. Stavros, Martin J. Paterson, Peter J. Sadler
Summary: This study reports a Ru(II) polypyridyl prodrug, RuAzNM, functionalized with azo and nitrogen mustard, which exhibits multimodal theranostic properties towards hypoxic cancer cells. Reduction of the azo group in hypoxic cell microenvironments leads to the generation of reactive oxygen species and mtDNA crosslinking, while the resulting phosphorescent RuNH2 serves as a diagnostic signal and activates phototherapy. This unique strategy allows controlled multimodal theranostics to be realized in hypoxic cells, making RuAzNM a highly selective and effective cancer-cell-selective theranostic agent.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Luca Craciunescu, Eirik M. Liane, Adam Kirrander, Martin J. Paterson
Summary: In this study, the excited state van der Waals (vdW) potential energy surfaces (PESs) of the NO A(2)Sigma(+) + CO2 X-1 Sigma(+)(g) system were thoroughly investigated using advanced computational methods. The results show that the employed methods are efficient and cost-effective in predicting the depth of vdW wells. Furthermore, the study highlights the influence of multi-reference effects and long-range vdW surfaces on rotational energy transfer.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Xiao Peng Mi, Hui Lu, Tianlv Xu, Herbert Fruchtl, Tanja van Mourik, Martin J. Paterson, Steven R. Kirk, Samantha Jenkins
Summary: A study using simulated circularly polarized laser pulses on ethane showed that the mechanical properties, particularly bond-flexing and bond-torsion, increase depending on the plane of polarization. These properties may increase or decrease after the laser pulses are switched off, depending on the polarization plane, due to directionally-dependent effects of excited states' long-lasting superpositions. The chiral properties of ethane were found to be formally achiral. The study briefly discusses future investigations using ultra-fast circularly polarized lasers.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Physics, Atomic, Molecular & Chemical
Dave Townsend
Summary: Laser-based experiments provide various strategies to study the dynamics of excited states in molecules. These experiments can be separated into frequency- and time-resolved variants, and a combination of different approaches is typically required to reveal a complete mechanistic picture. Narrow linewidth lasers can provide detailed information about the starting and ending points of photochemical reactions. However, direct observation of intermediate pathways connecting these points is often not possible due to the long duration of laser pulses. Therefore, time-resolved pump-probe experiments using ultrafast laser pulses are used to monitor real-time evolution along the reaction coordinate.
JOURNAL OF MOLECULAR SPECTROSCOPY
(2023)
Article
Chemistry, Physical
Stuart W. Crane, Malcolm Garrow, Paul D. Lane, Kate Robertson, Alex Waugh, Jack M. Woolley, Vasilios G. Stavros, Martin J. Paterson, Stuart J. Greaves, Dave Townsend
Summary: Ultrafast transient absorption spectroscopy was used to investigate the excess energy redistribution dynamics in nitrobenzene under hexane and isopropanol solvation. The results were compared with a recent time-resolved photoelectron imaging study, revealing a 1/e lifetime in the TAS data that was absent in the TRPEI measurements. This discrepancy highlights the varying sensitivity of different spectroscopic techniques in capturing specific steps along the reaction coordinate.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Thomas F. M. Luxford, Thomas R. Sharples, Martin Fournier, Cleïment Soulie, Martin J. Paterson, Kenneth G. McKendrick, Matthew L. Costen
Summary: A crossed molecular beam velocity map ion imaging apparatus was used to investigate the rotationally inelastic scattering between NO and N2, CO, and O2. The results showed that for collisions with N2 and CO, a fraction of NO was scattered sideways and backward, with increasing rotational excitation and collision parameters. In contrast, collisions with O2 mainly resulted in forward scattering with little rotational excitation. This is consistent with the literature on NO-O2 interaction potential energy surfaces.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Organic
Emmanouil Broumidis, Christopher G. Thomson, Brendan Gallagher, Lia Sotorrios, Kenneth G. Mckendrick, Stuart A. Macgregor, Martin J. Paterson, Janet E. Lovett, Gareth O. Lloyd, Georgina M. Rosair, Andreas S. Kalogirou, Panayiotis A. Koutentis, Filipe Vilela
Summary: This study discovered that 1,2,6-thiadiazines can be converted into 1,2,5-thiadiazole 1-oxides using visible light and oxygen under ambient conditions, which was previously difficult to achieve. Experimental and theoretical studies revealed that 1,2,6-thiadiazines act as triplet photosensitizers and undergo a selective cycloaddition reaction to form an endoperoxide.
Article
Environmental Sciences
Aisling C. Stewart, Martin J. Paterson, Stuart J. Greaves
Summary: The role of organic aqueous aerosols in the atmosphere depends on their structures, which are influenced by both their components and the way they are packed together. In this study, the surface coverage of three C18 fatty acids was investigated to understand its impact on aerosol structure. Higher coverage leads to tighter packing and alignment along the surface normal. Surface analysis showed that CH3 and CH2 groups dominate at all coverages, but changes in the presence of HC=CH and COOH indicate when monolayer coverage is exceeded. The accessibility of different groups to ozone molecules was also assessed, providing insights into how organic surface coverage affects aerosol reactivity.
ENVIRONMENTAL SCIENCE-ATMOSPHERES
(2023)
Article
Chemistry, Multidisciplinary
Dominic Taylor, Thomas Malcomson, Adilet Zhakeyev, Georgina M. Rosair, Martin J. Paterson, Jose Marques-Hueso, Scott J. Dalgarno, Filipe Vilela
Summary: Regioselective stepwise phenylation of 4,7-diarylbenzo[c][1,2,5]thiadiazole fluorophores was achieved by a facile one-pot, three-step synthetic strategy involving sequential borylation, hydroxydechlorination, and Suzuki-Miyaura cross-coupling reactions. Selectivity was achieved by using BCl3 to install a boronic acid group in the ortho-position of only one of the diaryl groups. The introduction of ortho-phenyl groups through Suzuki-Miyaura cross-coupling resulted in twisted structures with hindered intramolecular rotation, allowing for adjustment of the fluorophore absorption and emission properties.
Article
Chemistry, Physical
Chris Sparling, Stuart W. Crane, Lewis Ireland, Ross Anderson, Omair Ghafur, Jason B. Greenwood, Dave Townsend
Summary: We demonstrate an initial Velocity-Map Imaging (VMI) experiment using a back-irradiation laser-based desorption source integrated into the electrode assembly. This allows for the use of high-density plumes of non-volatile molecular samples with the popular VMI approach. Phenylalanine molecule is used to illustrate this novel method, showing forward-backward emission asymmetries of approximately 7%.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Organic
Dominic Taylor, Thomas Malcomson, Adilet Zhakeyev, Shengxian Cheng, Georgina M. Rosair, Jose Marques-Hueso, Zhengtao Xu, Martin J. Paterson, Scott J. Dalgarno, Filipe Vilela
Summary: This study reports the synthesis, characterization, and application of a library of 26 donor-acceptor (D-A) compounds based on the benzo[c][1,2,5]thiadiazole (BTZ) motif. By varying the donor groups while keeping the BTZ acceptor group the same, the optoelectronic and photophysical properties of the photocatalysts were systematically modified. These photocatalysts were validated through a test reaction under both batch and continuous flow conditions.
ORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Multidisciplinary
Christopher Robertson, Martin J. Paterson
Summary: In this study, two potential energy models were used to investigate the reactive scattering of OH(sigma) + H-2 -> H2O(X) + H. By analyzing the quenching channels and generating velocity map images, the simulated results provided insights into the mechanisms behind some experimental observations.
CHEMICAL COMMUNICATIONS
(2022)