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The high-order harmonic generation is theoretically studied when Rydberg state hydrogen atoms are interated with a linearly polarized three-color laser field along the z-axis. It is found that high-order harmonics show a super-continuum structure as well as extensive intensity enhancement. By time–frequency analyses, it is revealed that a large group of electronic density focused from the area outside the z-axis to the nucleus. This extraordinary behavior of Rydberg electron which is quite different from the previous study gives rise to the remarkable enhancement of the super-continuum. Further theoretical research based on semi-classical and quantum-mechanical technique displays the electronic focus effect caused by the combined action of the initial Rydberg orbital velocity and nuclear attraction of the core. This mechanism can apparently enhance the high-order harmonics, leading to remarkable attosecond pulse. [ABSTRACT FROM AUTHOR]

We discuss the possibility of localizing an electron in a highly excited Rydberg state. The second-order correlation of emitted photons is the tool for the determination of electron position. This second-order correlation of emitted radiation and, therefore, the correlation of operators describing the acceleration of the electron allows for a partial localization of the electron in its orbit. The correlation function is found by approximating the transition matrix elements by their values in the classical limit. It is shown that the second-order correlation, depending on two times, is a function of the time difference and is a periodic function of this argument with the period equal to the period of the corresponding classical motion. The function has sharp maxima corresponding to large electron acceleration in the vicinity of the “perihelion.” This allows the localization of the electron in its consecutive approach to the perihelion point. [ABSTRACT FROM AUTHOR]

Most of the previous TMDC-photon coupling devices were mainly based on A exciton due to its high oscillator strength and large exciton binding energy. Less effort has been focused on the modulation of the emission of B exciton and Rydberg states in TMDCs, especially in monolayer WS2. Here, we demonstrate that the photoluminescence (PL) emission of WS2-microcavity coupling devices can be tailored in a broad visible wavelength range (490 nm–720 nm). In contrast to the intrinsic PL emission of monolayer WS2, 25-fold enhanced B exciton emission and significant PL emission from the 2s Rydberg state can be observed. From the transient absorption (TA) measurements, the strongly coupled hybrid states based on B exciton can be remarkably fingerprinted. Furthermore, the strongly enhanced PL emission from the coupled B exciton has been demonstrated due to the strongly increased lower polariton (LP) state population and the internal conversion pathway being blocked in the strong coupling regime. Besides, the remarkable PL emission from the 2s Rydberg state is also revealed and confirmed by the additional ground state bleaching signal in TA spectra. These physical mechanisms about tailoring the PL emission in low dimensional TMDCs can provide significant references for constructing highly efficient optoelectronic devices.

Most of the previous TMDC-photon coupling devices were mainly based on A exciton due to its high oscillator strength and large exciton binding energy. Less effort has been focused on the modulation of the emission of B exciton and Rydberg states in TMDCs, especially in monolayer WS2. Here, we demonstrate that the photoluminescence (PL) emission of WS2-microcavity coupling devices can be tailored in a broad visible wavelength range (490 nm–720 nm). In contrast to the intrinsic PL emission of monolayer WS2, 25-fold enhanced B exciton emission and significant PL emission from the 2s Rydberg state can be observed. From the transient absorption (TA) measurements, the strongly coupled hybrid states based on B exciton can be remarkably fingerprinted. Furthermore, the strongly enhanced PL emission from the coupled B exciton has been demonstrated due to the strongly increased lower polariton (LP) state population and the internal conversion pathway being blocked in the strong coupling regime. Besides, the remarkable PL emission from the 2s Rydberg state is also revealed and confirmed by the additional ground state bleaching signal in TA spectra. These physical mechanisms about tailoring the PL emission in low dimensional TMDCs can provide significant references for constructing highly efficient optoelectronic devices. [ABSTRACT FROM AUTHOR]

A schematic diagram of the conformational dynamics of Rydberg excited TMPDA. [Display omitted] • The charge transfer process linked to structural motions of the Rydberg excited TMPDA has been monitored in real time. • TSI and TBI are found to coexist to drive charge transfer. • Flexible three-carbon skeleton provide more opportunities for the two electron lone pairs to overlap in space. Flexible three-carbon skeleton makes N, N, N′, N′-tetramethyl-1,3-propanediamine (TMPDA) an important diamine system to investigate the conformation-dependent electron lone pair interactions and charge delocalization. The charge transfer process linked to structural motions of the three-carbon skeleton has been monitored in real time by the Rydberg electron binding energy (BE) spectra of TMPDA coupled with quantum chemical calculations. Optical excitation to the 3p state with a 200 nm pump pulse initially generated a localized charge on one of the two nitrogen atoms that may partially transfer to the other one. Rapid internal conversion (IC) from the 3p to 3s state occurred within 430 fs, resulting in an initial charge delocalized 3s_h/3s_l population ratio of 23.6 %/76.4 %. A final 3s_h/3s_l (51.9 %/48.1 %) equilibrium proceeded within about 2.64 ps. The 3s_h (TTTT+, GG′TG+ and G′GG′G+) and 3s_l (GG′GG′+ and GG′G′G+) (see text for structure definitions) are identified as the extended and folded conformers, respectively. Two types of electron lone pair interactions, i.e., through-space interaction (TSI) and through-bond interaction (TBI), are found to coexist in TMPDA to drive charge transfer. The GG′GG′+ and GG′G′G+ structures exhibit TSI, while the TTTT+ structure shows TBI. The GG′TG+ and G′GG′G+ structures exhibit both TSI and TBI. Flexible three-carbon skeleton provide more opportunities for the two N-electron lone pairs to overlap in space (i.e., TSI), making TMPDA to be favorable for the most stably folded conformation. [ABSTRACT FROM AUTHOR]

Conformational dynamics has been well observed in the 3s Rydberg state of amines, whereas its observation in higher-energy, non-equilibrium 3p Rydberg states is very rare, especially for a reversible conformational transition that could compete with other non-adiabatic transitions. Herein, we report the observation of a reversible conformational interconversion phenomenon in the 3p Rydberg excited-state dynamics of N,N-dimethylethylamine (DMEA). Upon electronic excitation, a forward and backward interconversion between the initially prepared 3p_l and 3p_h conformers accompanied by 3p internal conversions occurs, resulting in a 3p_l/3p_h equilibrium ratio of 61 %/39 % within ∼1.5 ps. The ensuing parallel internal conversions from the 3p_l to 3s_l and 3p_h to 3s_h deposit about 1.80 eV of vibrational energy into the 3s state, enabling a fast conformational interconversion between the 3s_h and 3s_l conformers to proceed within ∼2.0 ps. The final 3s_l/3s_h equilibrium ratio was determined to be 76 %/24 %. This work presents a real-time observation of the entire conformational interconversion process initiating from the higher-energy 3p states and finally reaching an equilibrium on the lower-energy 3s state., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

We report generation of directional far-infrared emission between Rydberg states of NO in the gas phase initiated by the absorption of black body radiation at room temperature. All the transitions detected are assignable to the nf → (n − 1)g and n′g → (n′ − 1)f transitions. The longest wavelength observed in the present experiment was ~ 112 µm (2.7 THz) which corresponds to the 14f → 13g transition. The laser-prepared population in the 14s and 15s states is transferred to the 13f and 14f states located energetically higher, respectively, which generates the subsequent emission of 13f → 12g at ~ 88 µm and 14f → 13g at ~ 112 µm. Collisions of Rydberg molecules with the surrounding ground state molecules are considered to responsible for the upward population flow. The population in the 14p and 15p states is transported to the 13f and 14f states located energetically lower, respectively, which gives rise to the subsequent emission of 13f → 12g at ~ 88 µm and 14f → 13g at ~ 112 µm. [ABSTRACT FROM AUTHOR]

The low-lying Ω states of bismuth monofluoride (BiF) below 50000 cm−1 have been theoretically studied using the multi-reference configuration interaction and the equation-of-motion coupled-cluster methods, where the spin–orbit coupling (SOC) effects are respectively considered perturbatively or variationally. Since the perturbative treatment of SOC is not a good approximation for the heavy atom Bi, the latter method exhibits higher accuracy and better agreements with the experimental spectroscopic constants. Our results show that the second 3 Π state of BiF is due to the occupation on the Rydberg 7 s -shell of Bi, which gives rise to the so-called "triplet C " state and its sub-states reported in the early literatures. With the help of our theoretical results, some experimentally assigned spectral bands with considerable confusion have also been clarified and reassigned. [Display omitted] • The SOC effects have been included through perturbative and variational ways. • All the valence and Redberg Ω states below 50000 cm-1 have been investigated. • Some uncertain spectral transitions in the literatures have been reassigned. • The dissociation energy is calculated to be 4.09 eV at the complete basis set limit. [ABSTRACT FROM AUTHOR]

Photodissociation dynamics of acetone in gas phase were, for the first time, investigated using the pump‐probe technique of femtosecond transient absorption. To obtain a genuine time profile of nR state, we employed 200‐nm and 400‐nm pulses for two‐photon excitation and three‐photon excitation, respectively. In gas phase of acetone, the extraordinarily stable nR state originated from nR states in the Franck–Condon region, whose decay time constant was 350 ± 10 fs, was observed after excitation by three‐photon absorption of 400‐nm pulses. In the low‐power case of 267 nm, the photodissociation dynamics in the S1 state by one‐photon absorption showed that acetone was completely dissociated into two methyl radicals and C=O via an acetyl radical intermediate with a lifetime of 200 ± 10 fs. In the high‐power case of 267‐nm light, we interpreted the transient, although this is a subject of ongoing debate, as caused by both the photodissociation dynamics of the S1 state for a fast component and the dynamics of nR states for long‐lived species. [ABSTRACT FROM AUTHOR]

Alkaline-earth-like (AEL) atoms with two valence electrons and a nonzero nuclear spin can be excited to Rydberg state for quantum computing. Typical AEL ground states possess no hyperfine splitting, but unfortunately a GHz-scale splitting seems necessary for Rydberg excitation. Though strong magnetic fields can induce a GHz-scale splitting, weak fields are desirable to avoid noise in experiments. Here, we provide two solutions to this outstanding challenge with realistic data of well-studied AEL isotopes. In the first theory, the two nuclear spin qubit states ∣0〉 and ∣1〉 are excited to Rydberg states ∣r〉 with detuning Δ and 0, respectively, where a MHz-scale detuning Δ arises from a weak magnetic field on the order of 1 G. With a proper ratio between Δ and Ω, the qubit state ∣1〉 can be fully excited to the Rydberg state while ∣0〉 remains there. In the second theory, we show that by choosing appropriate intermediate states a two-photon Rydberg excitation can proceed with only one nuclear spin qubit state. The second theory is applicable whatever the magnitude of the magnetic field is. These theories bring a versatile means for quantum computation by combining the broad applicability of Rydberg blockade and the incomparable advantages of nuclear-spin quantum memory in two-electron neutral atoms. [ABSTRACT FROM AUTHOR]

We report on recent progress regarding the theoretical treatment of doubly-excited Rydberg states of atoms with two valence electrons. Building upon state-of-the-art techniques, we demonstrate that an approach based on configuration interaction with exterior complex scaling (CI-ECS) is capable of describing high Rydberg states ( n ∼ 100) and does not rely on the assumptions of R-matrix multichannel quantum-defect theory. We show that CI-ECS allows the simultaneous, accurate treatment of a range of doubly-excited Rydberg states broader than previously possible. The implementation of the method with numerical basis functions is explained in detail. As an example, CI-ECS calculations of the doubly-excited states of Mg and Sr are presented, and excellent agreement is found with available experimental data. The CI-ECS method opens new perspectives for studying collective two-electron dynamics in doubly-excited Rydberg states of alkaline-earth metal atoms, and is also of interest for the field of Rydberg-based quantum simulation. [ABSTRACT FROM AUTHOR]

In this paper, we proposed a model based on Rydberg atoms for controlling the optical bistability (OB) and optical multistability (OM) in a ring cavity. The atoms interact with an elliptical polarized probe light and a strong coupling light in the presence of external magnetic field. We realized that the threshold of OB can be controlled by elliptical polarized parameter when the first excited states of the atoms interact with Rydberg state. Also, we found that by adjusting the elliptical parameter of probe light, the switching from OB to OM is possible when we consider the strong coupling between Rydberg level and first excited state of the atomic system. We find that when the probe light becomes linearly the OB and OM disappear due to Rydberg electromagnetically induced transparency. However, by adjusting the polarized parameter of the probe light the threshold of OB can be controlled due to Rydberg electromagnetically absorption. Our proposed model can be used as an all-optical device for switching between OB and OM with potential applications in optical communication. [ABSTRACT FROM AUTHOR]

The diverse nature of optoelectronic properties of few-layer or monolayer MoS 2 is generally dominated by A and B excitons. Occasionally, strong Coulombic interactions within the 2D monolayer led to the creation of hydrogen-like Rydberg states of excitons in MoS 2 similar to other 2D monolayers. In this paper, a simple process is used to convert trilayer MoS 2 films to a monolayer by introducing H 2 gas during chemical vapor deposition. Remarkably, alongside the usual A, B excitons, and A - trion, the appearance of the Rydberg states is evidenced by photoluminescence spectra even at room temperature; also, there is an increase in their areal percentage with an increase in H 2 content. The s-type excited Rydberg states up to the fourth order ( n = 5) and third order ( n = 4) of A and B excitons, respectively, have been probed from the photoluminescence spectra at 93 K. Unprecedentedly, the first-order derivative of room-temperature photocurrent spectrum reveals the Rydberg states concurrently and elaboratively. Furthermore, the large-area MoS 2 films exhibit photoresponse in a broad UV to visible region with excellent photosensitivity (∼10 2 ) toward both UV and visible lights. Not only does this provide a profound understanding of the excitonic Rydberg states but also highlights the considerable potential of large-area monolayer MoS 2 overcoming the difficulty of tiny flake-related 2D device endeavors.

In this paper, we have suggested a configuration based on Rydberg atoms for adjusting properties of optical bistability (OB) and optical multistability (OM) via spontaneously generated coherence (SGC) in a unidirectional ring cavity. The Rydberg atoms consist of four energy levels interacts by a weak probe and a strong coupling fields, respectively. We have found that due to presence of SGC, threshold of OB and OM can be controlled when the strong light coupled the intermediate levels to the Rydberg state. [ABSTRACT FROM AUTHOR]

Abstract We present a theoretical study on probe field propagation through a three-level Ξ type system formed in an atomic vapour medium in presence of a strong control field. The model is based on density matrix method and is solved analytically, without neglecting any term in any power of probe and control Rabi frequencies, to find out the probe response under Doppler free condition as well as at room temperature. The probe response for a four-level Ξ type system is also determined analytically. Electromagnetically induced transparency is formed in the simulated probe response for both the level schemes. We also present the switching of probe field propagation from subluminal to superluminal as a function of probe detuning for different control transitions, one of which is to a Rydberg state. The switching window becomes asymmetric under detuned control field with the asymmetry depending on the wavelength mismatching factor between the control field and the probe field. Under strong probe regime probe propagation switches from superluminal to subluminal on resonance when the wavelength mismatch between the probe and the control field is increased, an effect which can be explained with the help of the analytical model that is free from any perturbative treatment. [ABSTRACT FROM AUTHOR]

A potential scheme to produce the water window single attosecond pulses (SAPs) from the multi-cycle mid-infrared (MIR) laser field has been investigated with the help of the chirp gating modulation. It is found that with the introduction of the laser chirp (i.e. up-chirp or down-chirp modulation), the extension of the harmonic cutoff can be achieved and the single harmonic radiation peak (HRP) can be selected during the harmonic emission process. Moreover, the chirp gating modulation on the high-order harmonic generation (HHG) is sensitive to the few-cycle pulse duration, but it is not very sensitive to the multi-cycle pulse duration. Moreover, a larger extension of the harmonic cutoff covering the whole water window region can be found with the help of the multi-cycle down-chirp modulation. Further, by properly choosing the coherent superposition of the ground state and the high Rydberg state as the initial state, the efficiency of HHG can be enhanced by 5 orders of magnitude. Finally, a series of high-intensity sub-40as pulses covering the water window region can be obtained. [ABSTRACT FROM AUTHOR]