Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light

We derive here a highly selective photoelectron-based chirality-sensing technique that utilizes “locally chiral” laser pulses. We show that this approach results in strong chiral discrimination, where the standard forwards/backwards asymmetry of photoelectron circular dichroism (PECD) is lifted. The resulting dichroism is larger and more robust than conventional PECD (especially in the high-energy part of the spectrum), is found in all hemispheres, and is not symmetric or antisymmetric with respect to any symmetry operator. Remarkably, chiral dichroism of up to 10% survives in the angularly integrated above-threshold ionization (ATI) spectra, and chiral dichroism of up to 5% survives in the total ionization rates. We demonstrate these results through ab initio calculations in the chiral molecules bromochlorofluoromethane, limonene, fenchone, and camphor. We also explore the parameter space of the locally chiral field and show that the observed dichroism is strongly correlated to the degree of chirality of the light, validating it as a measure for chiral-interaction strengths. Our results pave the way for highly selective probing of ultrafast chirality in ATI and motivate the use of locally chiral light for enhancing ultrafast spectroscopies. Most importantly, the technique can be implemented to achieve all-optical enantiopurification of chiral samples

Tracking electron motion within and outside of Floquet bands from attosecond pulse trains in time-resolved ARPES

Floquet engineering has recently emerged as a technique for controlling material properties with light. Floquet phases can be probed with time- and angle-resolved photoelectron spectroscopy (Tr-ARPES), providing direct access to the laser-dressed electronic bands. Applications of Tr-ARPES to date focused on observing the Floquet-Bloch bands themselves, and their build-up and dephasing on sub-laser-cycle timescales. However, momentum and energy resolved sub-laser-cycle dynamics between Floquet bands have not been analyzed. Given that Floquet theory strictly applies in time-periodic conditions, the notion of resolving sub-laser-cycle dynamics between Floquet states seems contradictory-it requires probe pulse durations below a laser cycle that inherently cannot discern the time-periodic nature of the light-matter system. Here we propose to employ attosecond pulse train probes with the same temporal periodicity as the Floquet-dressing pump pulse, allowing both attosecond sub-laser-cycle resolution and a proper projection of Tr-ARPES spectra on the Floquet-Bloch bands. We formulate and employ this approach in ab-initio calculations in light-driven graphene. Our calculations predict significant sub-laser-cycle dynamics occurring within the Floquet phase with the majority of electrons moving within and in-between Floquet bands, and a small portion residing and moving outside of them in what we denote as 'non-Floquet' bands. We establish that non-Floquet bands arise from the pump laser envelope that induces non-adiabatic electronic excitations during the pulse turn-on and turn-off. By performing calculations in systems with poly-chromatic pumps we also show that Floquet states are not formed on a sub-laser-cycle level. This work indicates that the Floquet-Bloch states are generally not a complete basis set for sub-laser-cycle dynamics in steady-state phases of matter

Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light

We derive here a highly selective photoelectron-based chirality-sensing technique that utilizes "locally chiral"laser pulses. We show that this approach results in strong chiral discrimination, where the standard forwards/backwards asymmetry of photoelectron circular dichroism (PECD) is lifted. The resulting dichroism is larger and more robust than conventional PECD (especially in the high-energy part of the spectrum), is found in all hemispheres, and is not symmetric or antisymmetric with respect to any symmetry operator. Remarkably, chiral dichroism of up to 10% survives in the angularly integrated above-threshold ionization (ATI) spectra, and chiral dichroism of up to 5% survives in the total ionization rates. We demonstrate these results through ab initio calculations in the chiral molecules bromochlorofluoromethane, limonene, fenchone, and camphor. We also explore the parameter space of the locally chiral field and show that the observed dichroism is strongly correlated to the degree of chirality of the light, validating it as a measure for chiral-interaction strengths. Our results pave the way for highly selective probing of ultrafast chirality in ATI and motivate the use of locally chiral light for enhancing ultrafast spectroscopies. Most importantly, the technique can be implemented to achieve all-optical enantiopurification of chiral samples

Sulphur-bearing molecules in diffuse molecular clouds: new results from SOFIA/GREAT and the IRAM 30 m telescope

We have observed five sulphur-bearing molecules in foreground diffuse molecular clouds lying along the sight-lines to five bright continuum sources. We have used the GREAT instrument on SOFIA to observe the 1383 GHz $^2\Pi_{3/2} J=5/2-3/2$ transitions of SH towards the star-forming regions W31C, G29.96-0.02, G34.3+0.1, W49N and W51, detecting foreground absorption towards all five sources; and the EMIR receivers on the IRAM 30m telescope at Pico Veleta to detect the H$_2$S 1(10)-1(01), CS J=2-1 and SO 3(2)-2(1) transitions. In nine foreground absorption components detected towards these sources, the inferred column densities of the four detected molecules showed relatively constant ratios, with N(SH)/N(H$_2$S) in the range 1.1 - 3.0, N(CS)/N(H$_2$S) in the range 0.32 - 0.61, and N(SO)/N(H$_2$S) in the range 0.08 - 0.30. The observed SH/H$_2$ ratios - in the range (0.5-2.6) $\times 10^{-8}$ - indicate that SH (and other sulphur-bearing molecules) account for << 1% of the gas-phase sulphur nuclei. The observed abundances of sulphur-bearing molecules, however, greatly exceed those predicted by standard models of cold diffuse molecular clouds, providing further evidence for the enhancement of endothermic reaction rates by elevated temperatures or ion-neutral drift. We have considered the observed abundance ratios in the context of shock and turbulent dissipation region (TDR) models. Using the TDR model, we find that the turbulent energy available at large scale in the diffuse ISM is sufficient to explain the observed column densities of SH and CS. Standard shock and TDR models, however, fail to reproduce the column densities of H$_2$S and SO by a factor of about 10; more elaborate shock models - in which account is taken of the velocity drift, relative to H$_2$, of SH molecules produced by the dissociative recombination of H$_3$S$^+$ - reduce this discrepancy to a factor ~ 3.Comment: 30 pages, accepted for publication in A&

Light-Driven Extremely Nonlinear Bulk Photogalvanic Currents

We predict the generation of bulk photocurrents in materials driven by bichromatic fields that are circularly polarized and corotating. The nonlinear photocurrents have a fully controllable directionality and amplitude without requiring carrier-envelope-phase stabilization or few-cycle pulses, and can be generated with photon energies much smaller than the band gap (reducing heating in the photoconversion process). We demonstrate with ab initio calculations that the photocurrent generation mechanism is universal and arises in gaped materials (Si, diamond, MgO, hBN), in semimetals (graphene), and in two- and three-dimensional systems. Photocurrents are shown to rely on sub-laser-cycle asymmetries in the nonlinear response that build-up coherently from cycle to cycle as the conduction band is populated. Importantly, the photocurrents are always transverse to the major axis of the co-circular lasers regardless of the material's structure and orientation (analogously to a Hall current), which we find originates from a generalized time-reversal symmetry in the driven system. At high laser powers (∼1013 W/cm2) this symmetry can be spontaneously broken by vast electronic excitations, which is accompanied by an onset of carrier-envelope-phase sensitivity and ultrafast many-body effects. Our results are directly applicable for efficient light-driven control of electronics, and for enhancing sub-band-gap bulk photogalvanic effects

Attosecond magnetization dynamics in non-magnetic materials driven by intense femtosecond lasers

Irradiating solids with ultrashort laser pulses is known to initiate femtosecond timescale magnetization dynamics. However, sub-femtosecond spin dynamics have not yet been observed or predicted. Here, we explore ultrafast light-driven spin dynamics in a highly non-resonant strong-field regime. Through state-of-the-art ab-initio calculations, we predict that a non-magnetic material can be transiently transformed into a magnetic one via dynamical extremely nonlinear spin-flipping processes, which occur on attosecond timescales and are mediated by a combination of multi-photon and spin-orbit interactions. These are non-perturbative non-resonant analogues to the inverse Faraday effect that build up from cycle-to-cycle as electrons gain angular momentum. Remarkably, we show that even for linearly polarized driving, where one does not intuitively expect any magnetic response, the magnetization transiently oscillates as the system interacts with light. This oscillating response is enabled by transverse anomalous light-driven currents in the solid, and typically occurs on timescales of ~500 attoseconds. We further demonstrate that the speed of magnetization can be controlled by tuning the laser wavelength and intensity. An experimental set-up capable of measuring these dynamics through pump-probe transient absorption spectroscopy is outlined and simulated. Our results pave the way for new regimes of ultrafast manipulation of magnetism

Time- and angle-resolved photoelectron spectroscopy of strong-field light-dressed solids: Prevalence of the adiabatic band picture

In recent years, strong-field physics in condensed matter was pioneered as a potential approach for controlling material properties through laser dressing, as well as for ultrafast spectroscopy via nonlinear light-matter interactions (e.g., harmonic generation). A potential controversy arising from these advancements is that it is sometimes vague which band picture should be used to interpret strong-field experiments: The field-free bands, the adiabatic (instantaneous) field-dressed bands, Floquet bands, or some other intermediate picture. Here, we try to resolve this issue by performing theoretical experiments of time- and angle-resolved photoelectron spectroscopy (Tr-ARPES) for a strong-field laser-pumped solid, which should give access to the actual observable bands of the irradiated material. To our surprise, we find that the adiabatic band picture survives quite well up to high field intensities (∼1012W/cm2) and in a wide frequency range (driving wavelengths of 4000 to 800 nm, with Keldysh parameters ranging up to ∼7). We conclude that, to first order, the adiabatic instantaneous bands should be the standard blueprint for interpreting ultrafast electron dynamics in solids when the field is highly off resonant with characteristic energy scales of the material. We then discuss weaker effects of modifications of the bands beyond this picture that are nonadiabatic, showing that by using bichromatic fields the deviations from the standard picture can be probed with enhanced sensitivity. In this paper, we outline a clear band picture for the physics of strong-field interactions in solids, which should be useful for designing and analyzing strong-field experimental observables and to formulate simpler semi-empirical models

Four-point correlator constraints on electromagnetic chiral parameters and resonance effective Lagrangians

We pursue the analysis of a set of generalized DGMLY sum rules for the electromagnetic chiral parameters at order $e^2p^2$ and discuss implications for effective Lagrangians with resonances. We exploit a formalism in which charge spurions are introduced and treated as sources. We show that no inconsistency arises from anomalies up to quadratic order in the spurions. We focus on the sum rules associated with QCD 4-point correlators which were not analyzed in detail before. Convergence properties of the sum rules are deduced from a general analysis of the form of the counterterms in the presence of electromagnetic spurions. Following the approach in which vector and axial-vector resonances are described with antisymmetric tensor fields and have a chiral order, we show that the convergence constraints are violated at chiral order four and can be satisfied by introducing a set of terms of order six. The relevant couplings get completely and uniquely determined from a set of generalized Weinberg sum-rule relations. An update on the corrections to Dashen's low-energy theorem is given.Comment: 42 pages, 1 figure. v2: references adde

Ground-state ammonia and water in absorption towards Sgr B2

We have used the Odin submillimetre-wave satellite telescope to observe the ground state transitions of ortho-ammonia and ortho-water, including their 15N, 18O, and 17O isotopologues, towards Sgr B2. The extensive simultaneous velocity coverage of the observations, >500 km/s, ensures that we can probe the conditions of both the warm, dense gas of the molecular cloud Sgr B2 near the Galactic centre, and the more diffuse gas in the Galactic disk clouds along the line-of-sight. We present ground-state NH3 absorption in seven distinct velocity features along the line-of-sight towards Sgr B2. We find a nearly linear correlation between the column densities of NH3 and CS, and a square-root relation to N2H+. The ammonia abundance in these diffuse Galactic disk clouds is estimated to be about (0.5-1)e-8, similar to that observed for diffuse clouds in the outer Galaxy. On the basis of the detection of H218O absorption in the 3 kpc arm, and the absence of such a feature in the H217O spectrum, we conclude that the water abundance is around 1e-7, compared to ~1e-8 for NH3. The Sgr B2 molecular cloud itself is seen in absorption in NH3, 15NH3, H2O, H218O, and H217O, with emission superimposed on the absorption in the main isotopologues. The non-LTE excitation of NH3 in the environment of Sgr B2 can be explained without invoking an unusually hot (500 K) molecular layer. A hot layer is similarly not required to explain the line profiles of the 1_{1,0}-1_{0,1} transition from H2O and its isotopologues. The relatively weak 15NH3 absorption in the Sgr B2 molecular cloud indicates a high [14N/15N] isotopic ratio >600. The abundance ratio of H218O and H217O is found to be relatively low, 2.5--3. These results together indicate that the dominant nucleosynthesis process in the Galactic centre is CNO hydrogen burning.Comment: 10 pages, 5 figure

Beam test results of silicon sensor module prototypes for the Phase-2 Upgrade of the CMS Outer Tracker

The start of the High-Luminosity LHC (HL-LHC) in 2027 requires upgrades to the Compact Muon Solenoid (CMS) Experiment. In the scope of the upgrade program the complete silicon tracking detector will be replaced. The new CMS Tracker will be equipped with silicon pixel detectors in the inner layers closest to the interaction point and silicon strip detectors in the outer layers. The new CMS Outer Tracker will consist of two different kinds of detector modules called PS and 2S modules. Each module will be made of two parallel silicon sensors (a macro-pixel sensor and a strip sensor for the PS modules and two strip sensors for the 2S modules). Combining the hit information of both sensor layers it is possible to estimate the transverse momentum of particles in the magnetic field of 3.8 T at the full bunch-crossing rate of 40 MHz directly on the module. This information will be used as an input for the first trigger stage of CMS. It is necessary to validate the Outer Tracker module functionality before installing the modules in the CMS experiment. Besides laboratory-based tests several 2S module prototypes have been studied at test beam facilities at CERN, DESY and FNAL. This article concentrates on the beam tests at DESY during which the functionality of the module concept was investigated using the full final readout chain for the first time. Additionally the performance of a 2S module assembled with irradiated sensors was studied. By choosing an irradiation fluence expected for 2S modules at the end of HL-LHC operation, it was possible to investigate the particle detection efficiency and study the trigger capabilities of the module at the beginning and end of runtime of the CMS experiment.The start of the High-Luminosity LHC (HL-LHC) in 2027 requires upgrades to the Compact Muon Solenoid (CMS) experiment. In the scope of the upgrade program the complete silicon tracking detector will be replaced. The new CMS Tracker will be equipped with silicon pixel detectors in the inner layers closest to the interaction point and silicon strip detectors in the outer layers. The new CMS Outer Tracker will consist of two different kinds of detector modules called PS and 2S modules. Each module will be made of two parallel silicon sensors (a macro-pixel sensor and a strip sensor for the PS modules and two strip sensors for the 2S modules). Combining the hit information of both sensor layers, it is possible to estimate the transverse momentum of particles in the magnetic field of 3.8 T at the full bunch-crossing rate of 40 MHz directly on the module. This information will be used as an input for the first trigger stage of CMS. It is necessary to validate the Outer Tracker module functionality before installing the modules in the CMS experiment. Besides laboratory-based tests several 2S module prototypes have been studied at test beam facilities at CERN, DESY and FNAL. This article concentrates on the beam tests at DESY during which the functionality of the module concept was investigated using the full final readout chain for the first time. Additionally the performance of a 2S module assembled with irradiated sensors was studied. By choosing an irradiation fluence expected for 2S modules at the end of HL-LHC operation, it was possible to investigate the particle detection efficiency and study the trigger capabilities of the module at the beginning and end of the runtime of the CMS experiment