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| Open AccessProbing molecules in gas cells of subwavelength thickness with high frequency resolution
Using gas cells for spectroscopic studies opens possibility for miniaturized platforms that can be integrated with other optical components. Here the authors demonstrate molecular rovibrational spectroscopy by confining molecules in a cell of subwavelength thickness.
- Guadalupe Garcia Arellano
- , Joao Carlos de Aquino Carvalho
- & Athanasios Laliotis
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Article
| Open AccessRobust temporal adiabatic passage with perfect frequency conversion between detuned acoustic cavities
Phase matching is pivotal for realizing complete energy transfer for classical waves. Here, authors propose temporal quasi-phase matching method and realize robust and complete energy transfer between arbitrarily detuned acoustic cavities by combing the concept of stimulated Raman adiabatic passage.
- Zhao-Xian Chen
- , Yu-Gui Peng
- & Yan-Qing Lu
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Article
| Open AccessCollectively enhanced Ramsey readout by cavity sub- to superradiant transition
One of the ways excited-state atoms relax to ground state is by emitting radiation. Here the authors demonstrate sub- and super-radiant emission threshold from a cavity-mediated atomic ensemble of Sr atoms.
- Eliot A. Bohr
- , Sofus L. Kristensen
- & Jörg H. Müller
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| Open AccessFrom chiral laser pulses to femto- and attosecond electronic chirality flips in achiral molecules
Chirality is a unique property of certain molecules. Here the authors discuss method to induce and flip electronic chirality in oriented NaK molecules using circularly polarized laser pulses.
- Yunjiao Chen
- , Dietrich Haase
- & Yonggang Yang
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Article
| Open AccessSpatiotemporal imaging and shaping of electron wave functions using novel attoclock interferometry
Electrons detached from atoms by photoionization carry valuable information about light-atom interactions. Here, authors propose a novel attoclock interferometry to spatiotemporally shape and image the electron wave function, from which the quantum nature of strong-field ionization is identified.
- Peipei Ge
- , Yankun Dou
- & Yunquan Liu
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Article
| Open AccessSub-Doppler optical-optical double-resonance spectroscopy using a cavity-enhanced frequency comb probe
Probing molecules in excited vibrational states requires precise methods to extract the spectroscopic parameters. Here the authors demonstrate optical-optical double-resonance spectroscopy of excited-bands of methane using single pass high power continuous wave pump and cavity-enhanced frequency comb probe.
- Vinicius Silva de Oliveira
- , Isak Silander
- & Aleksandra Foltynowicz
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Article
| Open AccessInitial-site characterization of hydrogen migration following strong-field double-ionization of ethanol
Excitation of hydrogen-rich molecules often causes hydrogen migration, but characterisation of the individual sites is challenging. Here, the authors show that measurements of several isotopologues of ethanol can identify each hydrogen site’s contribution to the final products.
- Travis Severt
- , Eleanor Weckwerth
- & Itzik Ben-Itzhak
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Article
| Open AccessSubcycle surface electron emission driven by strong-field terahertz waveforms
THz-driven electron emission is predicted to yield a single burst, due to the single-cycle waveform. Here, the authors demonstrate the confinement of single-cycle THz-waveform-driven electron emission to one of the two half cycles and the control of the active half cycle by changing the field polarity.
- Shaoxian Li
- , Ashutosh Sharma
- & József A. Fülöp
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Article
| Open AccessAcoustic frequency atomic spin oscillator in the quantum regime
Realising a quantum-backaction-limited oscillator in the acoustic frequency range would have applications in sensing and metrology. Here, the authors reach this goal by demonstrating destructive interference between quantum back-action noise and shot noise down to sub-kHz range in a warm atomic vapor cell.
- Jun Jia
- , Valeriy Novikov
- & Eugene S. Polzik
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Article
| Open AccessMachine learning assisted vector atomic magnetometry
Multiparameter sensors in quantum optics are often complex due to use of external fields. Here the authors demonstrate a simple single-shot all-optical vector atomic magnetometer based on machine learning for the correspondence of the measured signals and the magnetic field.
- Xin Meng
- , Youwei Zhang
- & Yanhong Xiao
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Article
| Open AccessMultiple-core-hole resonance spectroscopy with ultraintense X-ray pulses
Intense light pulses can create nonlinear ionization processes in atoms and molecules. Here the authors study the photoionization of xenon atoms using intense free-electron laser pulses that can create extremely high charge states and produce hollow atoms, featuring up to six simultaneous core-holes.
- Aljoscha Rörig
- , Sang-Kil Son
- & Rebecca Boll
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Article
| Open AccessDirectly imaging excited state-resolved transient structures of water induced by valence and inner-shell ionisation
Capturing the detailed structural evolution of electronic excited states is a challenging but critical step to understand and control ultrafast molecular dynamics. Here, combining a Coulomb explosion imaging approach and molecular dynamics simulations, the authors retrieve the transient geometry of the ground and excited states of D2O mono- and dication with few femtosecond, few picometre accuracy.
- Zhenzhen Wang
- , Xiaoqing Hu
- & Dajun Ding
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Article
| Open AccessH2 formation via non-Born-Oppenheimer hydrogen migration in photoionized ethane
Uncovering the mechanism behind neutral H2 formation from ionised hydrocarbon molecules still poses severe challenges. Here, based on the orbital fingerprints in the photoelectron momentum distributions, the authors were able to resolve the contributions of the ground and excited ionic states to the H2 formation channel.
- Yizhang Yang
- , Hao Ren
- & Dajun Ding
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Article
| Open AccessTwo-dimensional Kβ-Kα fluorescence spectrum by nonlinear resonant inelastic X-ray scattering
X-ray fluorescence spectroscopy is a powerful tool to investigate atomic properties. Here the authors report a two-dimensional fluorescence spectrum of copper metal using X-ray nonlinear scattering and find two-hole satellite feature resulting from atomic transitions.
- Kenji Tamasaku
- , Munetaka Taguchi
- & Tetsuya Ishikawa
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| Open AccessDirect observation of coherence transfer and rotational-to-vibrational energy exchange in optically centrifuged CO2 super-rotors
In this work the authors use coherent anti-Stokes Raman scattering to study collisional vibrational excitation in highly rotationally excited CO2 molecules prepared in an optical centrifuge.
- Timothy Y. Chen
- , Scott A. Steinmetz
- & Christopher J. Kliewer
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Article
| Open AccessPhotonic integrated beam delivery for a rubidium 3D magneto-optical trap
Ultracold atoms are generated in the lab using optical trapping and cooling. Here the authors implement a fiber-coupled photonic integrated circuit for a beam delivery to a three-dimensional magneto-optical trap where greater than 1 million rubidium atoms are cooled near 200 μK.
- Andrei Isichenko
- , Nitesh Chauhan
- & Daniel J. Blumenthal
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Article
| Open AccessMeasurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid
Spontaneous Raman scattering is classically understood as an incoherent process. Here, the authors demonstrate that macroscopic quantum coherence among billions of vibrating molecules in a liquid is generated when single photon detection and single spatio-temporal mode excitation are implemented.
- Valeria Vento
- , Santiago Tarrago Velez
- & Christophe Galland
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Article
| Open AccessQuantum dynamical effects of vibrational strong coupling in chemical reactivity
Experiments suggest that placing molecules in an infrared cavity alters their reactivity, an effect lacking a clear theoretical explanation. Here, the authors show that the key to understanding this process may lie in quantum light-matter interactions.
- Lachlan P. Lindoy
- , Arkajit Mandal
- & David R. Reichman
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| Open AccessInducing transient enantiomeric excess in a molecular quantum racemic mixture with microwave fields
There is growing interest in controlling and manipulating molecules using external field. Here the authors demonstrate microwave induced transient enantiomeric excess in a state-selective benzyl alcohol using microwave six-wave mixing.
- Wenhao Sun
- , Denis S. Tikhonov
- & Melanie Schnell
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Article
| Open AccessObservation of site-selective chemical bond changes via ultrafast chemical shifts
X-ray photoelectron spectroscopy probes the chemical environment in a molecule at a specific atomic site. Here the authors extend this concept with a site selective trigger to follow chemical bond changes as they occur on the femtosecond time scale.
- Andre Al-Haddad
- , Solène Oberli
- & Christoph Bostedt
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| Open AccessControlling Floquet states on ultrashort time scales
Floquet engineering aims at inducing new properties in materials with light. Here the authors have used pulses of variable durations, to investigate its applicability in the femtosecond domain. Surprisingly, they found that it holds to the few-cycle limit.
- Matteo Lucchini
- , Fabio Medeghini
- & Mauro Nisoli
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| Open AccessAbsolute frequency metrology of buffer-gas-cooled molecular spectra at 1 kHz accuracy level
High-resolution molecular spectroscopy with cryogenic setups is hampered by the lack of a skilled interrogation tool. Here, the authors demonstrate absolute metrology of cold rovibrational spectra at 1 kHz accuracy level, by coupling a Lamb-dip saturated-absorption cavity ring-down spectrometer to a buffer-gas cooling source.
- Roberto Aiello
- , Valentina Di Sarno
- & Pasquale Maddaloni
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Article
| Open AccessPauli blocking of stimulated emission in a degenerate Fermi gas
Pauli exclusion principle has fundamental and practical consequences to the structure of matter and particle interaction. Here the authors demonstrate Pauli blocking in a coherently driven system using trapped 3He degenerate Fermi gases.
- Raphael Jannin
- , Yuri van der Werf
- & Kjeld S. E. Eikema
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Article
| Open AccessHigh-precision electron affinity of oxygen
High-precision measurements are useful to find isotopic shifts and electron correlation. Here the authors measure electron affinity and hyperfine splitting of atomic oxygen with higher precision than previous studies.
- Moa K. Kristiansson
- , Kiattichart Chartkunchand
- & Dag Hanstorp
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Article
| Open AccessSub-optical-cycle light-matter energy transfer in molecular vibrational spectroscopy
Energy transfer between the electromagnetic field and atoms or molecules is fundamentally interesting. Here the authors demonstrate stepwise energy transfer between broadband mid-infrared optical pulses and vibrating methylsulfonylmethane molecules in aqueous solution.
- Martin T. Peschel
- , Maximilian Högner
- & Ioachim Pupeza
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| Open AccessStep-by-step state-selective tracking of fragmentation dynamics of water dications by momentum imaging
Determining the time evolution of reactions at the quantum mechanical level improves our understanding of molecular dynamics. Here, authors separate the breakup of water, one bond at a time, from other processes leading to the same final products and experimentally identify, separate, and follow step by step two breakup paths of the transient OD+ fragment.
- Travis Severt
- , Zachary L. Streeter
- & Itzik Ben-Itzhak
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Article
| Open AccessA compact cold-atom interferometer with a high data-rate grating magneto-optical trap and a photonic-integrated-circuit-compatible laser system
Cold-atom interferometers have been miniaturized towards fieldable quantum inertial sensing applications. Here the authors demonstrate a compact cold-atom interferometer using microfabricated gratings and discuss the possible use of photonic integrated circuits for laser systems.
- Jongmin Lee
- , Roger Ding
- & Peter D. D. Schwindt
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Article
| Open AccessA non-Hermitian optical atomic mirror
Here the authors provide a theoretical description of non-Hermitian topological phenomena in an atomic mirror. They find out diverse and unexpected phenomena by constructing an ad-hoc theoretical model. In particular, exceptional points, dispersive bulk Fermi arcs, and non-Hermitian geometry-dependent skin effect.
- Yi-Cheng Wang
- , Jhih-Shih You
- & H. H. Jen
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Article
| Open AccessUltraviolet supercontinuum generation driven by ionic coherence in a strong laser field
Supercontinuum generation can be utilized for light source development. Here the authors demonstrate ultraviolet supercontinuum generation from ions due to strong field ionization and multiphoton resonance effect.
- Hongbin Lei
- , Jinping Yao
- & Zengxiu Zhao
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Article
| Open AccessPhotonic-circuited resonance fluorescence of single molecules with an ultrastable lifetime-limited transition
Single molecules can generate high-quality single photons for quantum technologies, but coupling to waveguides is difficult. Here, the authors show on-chip background-free resonance fluorescence generation and routing from single molecules with lifetime-limited transition and waveguide-aligned dipoles.
- Penglong Ren
- , Shangming Wei
- & Xue-Wen Chen
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Article
| Open AccessAssembly and coherent control of a register of nuclear spin qubits
In large qubit registers, long coherence times and individual qubit control are difficult to achieve at the same time. Here, the authors assemble a 2D register of qubits in an array of fermionic alkaline-earth atoms, where tailored pulses can be applied to subsets of individual qubits in parallel.
- Katrina Barnes
- , Peter Battaglino
- & Michael Yarwood
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Article
| Open AccessUniversality of Dicke superradiance in arrays of quantum emitters
Dicke superradiance is an important collective quantum phenomenon, but its analysis is hindered by the exponential growth of the state space with atom number. Here, the authors develop a theoretical framework that overcomes this, and predict a critical distance below which superradiant decay can be observed in large ordered arrays.
- Stuart J. Masson
- & Ana Asenjo-Garcia
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Article
| Open AccessDeep learning enhanced Rydberg multifrequency microwave recognition
Rydberg atoms are sensitive to microwave signals and hence can be used to detect them. Here the authors demonstrate a Rydberg receiver enhanced by deep learning, Rydberg atoms acting as antennae, to receive, extract, and decode the multi-frequency microwave signal effectively.
- Zong-Kai Liu
- , Li-Hua Zhang
- & Bao-Sen Shi
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Article
| Open AccessAmmonia dimer: extremely fluxional but still hydrogen bonded
The long-standing question whether ammonia dimer is hydrogen bonded is solved by first-principles quantum mechanical calculations. The authors show that the dimer is extremely fluxional, but the probability of hydrogen-bonded configurations prevails.
- Jing Aling
- , Krzysztof Szalewicz
- & Ad van der Avoird
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Article
| Open AccessSelection rules in symmetry-broken systems by symmetries in synthetic dimensions
The authors introduce the concept of real-synthetic symmetries and use it as a tool to derive selection rules in seemingly symmetry-broken strong-field interactions. These symmetries and their corresponding selection rules can be applied in various systems form harmonic generation to topological photonics
- Matan Even Tzur
- , Ofer Neufeld
- & Oren Cohen
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| Open AccessPhotoinduced bond oscillations in ironpentacarbonyl give delayed synchronous bursts of carbonmonoxide release
The photodissociation of transition metal carbonyls is involved in catalysis and synthetic processes. Here the authors, using semi-classical excited state molecular dynamics, observe details of the early stage dynamics in the photodissociation of Fe(CO)5, including synchronous bursts of CO at periodic intervals of 90 femtoseconds.
- Ambar Banerjee
- , Michael R. Coates
- & Michael Odelius
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| Open AccessRealizing topological edge states with Rydberg-atom synthetic dimensions
Synthetic dimensions, states of a system engineered to act as if they were a reconfigurable extra spatial dimension, have been demonstrated with different systems previously. Here the authors create a synthetic dimension using Rydberg atoms and configure it to support topological edge states.
- S. K. Kanungo
- , J. D. Whalen
- & T. C. Killian
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| Open AccessInternal Stark effect of single-molecule fluorescence
The internal Stark effect, a shift of the spectral lines of a chromophore induced by electrostatic fields in its close environment, plays an important role in nature. Here the authors observe a Stark shift in the fluorescence spectrum of a phthalocyanine molecule upon charge modifications within the molecule itself, achieved by sequential removal of the central protons with a STM tip.
- Kirill Vasilev
- , Benjamin Doppagne
- & Guillaume Schull
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| Open AccessFollowing excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
Imaging the charge flow in photoexcited molecules would provide key information on photophysical and photochemical processes. Here the authors demonstrate tracking in real time after photoexcitation the change in charge density at a specific site of 2-thiouracil using time-resolved X-ray photoelectron spectroscopy.
- D. Mayer
- , F. Lever
- & M. Gühr
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Article
| Open AccessInfluence of shape resonances on the angular dependence of molecular photoionization delays
It is an interesting topic to find the time it takes for an electron to escape an atom or a molecule after photoionization. Here the authors measure the angular dependence of photoionization time delay in the molecular frame and discuss the role of shape resonances.
- F. Holzmeier
- , J. Joseph
- & R. R. Lucchese
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Article
| Open AccessMeasuring the photoelectron emission delay in the molecular frame
Measuring photoionization time delays is an interesting and challenging topic. Here the authors demonstrate a method to measure the photoionization time delays using inner-shell ionization of CO molecule.
- Jonas Rist
- , Kim Klyssek
- & Till Jahnke
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Article
| Open AccessSympathetic cooling of positrons to cryogenic temperatures for antihydrogen production
Positrons are key to the production of cold antihydrogen. Here the authors report the sympathetic cooling of positrons by interacting them with laser-cooled Be+ ions resulting in a three-fold reduction of the temperature of positrons for antihydrogen synthesis.
- C. J. Baker
- , W. Bertsche
- & J. S. Wurtele
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Article
| Open AccessTime-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast XUV-IR regime
Polycyclic aromatic hydrocarbons play an important role in interstellar chemistry, where interaction with high energy photons can induce ionization and fragmentation reactions. Here the authors, with XUV-IR pump-probe experiments, investigate the ultrafast photoinduced dynamics of fluorene, phenanthrene and pyrene, providing insight into their preferred reaction channels.
- J. W. L. Lee
- , D. S. Tikhonov
- & M. Schnell
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Article
| Open AccessControlled multi-photon subtraction with cascaded Rydberg superatoms as single-photon absorbers
Interaction of photons with Rydberg atoms can be used to modify quantum states of light. Here the authors demonstrate a controlled nonlinear quantum behavior of multi-photon subtraction in a cascaded system based on Rydberg superatoms.
- Nina Stiesdal
- , Hannes Busche
- & Sebastian Hofferberth
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Article
| Open AccessUltrafast imaging of spontaneous symmetry breaking in a photoionized molecular system
The Jahn-Teller effect is the spontaneous symmetry breaking of the molecular structure caused by the coupling of electrons and nuclei. Here the authors use ultrafast Coulomb explosion imaging to map the evolution of the fundamental symmetry lowering process in photoionized methane within around 20fs.
- Min Li
- , Ming Zhang
- & Peixiang Lu
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Article
| Open AccessObservation of laser-assisted electron scattering in superfluid helium
Laser-assisted electron scattering (LAES) is a commonly observed strong field process in gas phase systems. Here the authors use helium droplets with core atoms and molecules to observe increased electron energy due to multiple LAES events within the droplets.
- Leonhard Treiber
- , Bernhard Thaler
- & Markus Koch
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Article
| Open AccessFast-field-cycling ultralow-field nuclear magnetic relaxation dispersion
Nuclear spin polarization and relaxation can be studied using nuclear magnetic resonance (NMR). Here the authors demonstrate a combination of fast-field cycling and optical magnetometry techniques, to realize a NMR sensor that operates in the region of very low frequency and high relaxation rate.
- Sven Bodenstedt
- , Morgan W. Mitchell
- & Michael C. D. Tayler
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Article
| Open AccessRoom-temperature single-photon source with near-millisecond built-in memory
Room-temperature single photon sources with memory capabilities are promising for quantum information processing, but are currently limited in their memory time or photon purity. Here, the authors report single photon emission with good antibunching from an atomic vapour cell source with 0.68 ms memory time.
- Karsten B. Dideriksen
- , Rebecca Schmieg
- & Eugene S. Polzik
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Article
| Open AccessPrecisely spun super rotors
Optical pulses can be useful to create and control molecules in higher quantum states. Here the authors use optical pumping to create rotationally excited states of SiO+ molecular ion into super rotor ensemble.
- Ivan O. Antonov
- , Patrick R. Stollenwerk
- & Brian C. Odom