Rotational-state-selective field ionization of molecular Rydberg states

Patel, Rupal; Jones, N J A; Fielding, Helen H.

doi:10.1103/physreva.76.043413

Cited by 10 publications

(5 citation statements)

References 62 publications

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“…Similar fields were used to ionize neutral Rydberg molecules for detection immediately after photoexcitation. To detect molecules in long-lived Rydberg states, slowly-rising pulsed ionization fields 31,59 (rise time ∼ 2 µs) were applied 126 µs after laser photoexcitation. In these measurements the electric field amplitude at the time of ionization was correlated with the electron signal detected at MCP2 to provide information on the internal quantum state populations.…”

Section: Electric Field Ionizationmentioning

confidence: 99%

“…High Rydberg states of NO have been the subject of numerous experimental and theoretical investigations (see, for example, Refs. 6,[20][21][22][23][24][25][26][27][28][29][30][31][32]. The work reported here builds on these detailed studies of the structure and dynamics of Rydberg states of NO, many of which were carried out in particular in the context of the development of ZEKE photoelectron spectroscopy, 6 and more recent studies of plasma formation in cold Rydberg gases.…”

Section: Introductionmentioning

confidence: 99%

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Excitation and characterization of long-lived hydrogenic Rydberg states of nitric oxide

Deller

Hogan

2020

The Journal of Chemical Physics

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High Rydberg states of nitric oxide (NO) with principal quantum numbers between 40 and 100 and lifetimes in excess of 10 µs have been prepared by resonance enhanced two-color two-photon laser excitation from the X 2 Π 1/2 ground state through the A 2 Σ + intermediate state. Molecules in these long-lived Rydberg states were detected and characterized 126 µs after laser photoexcitation by state-selective pulsed electric field ionization. The laser excitation and electric field ionization data were combined to construct two-dimensional spectral maps. These maps were used to identify the rotational states of the NO + ion core to which the observed series of long-lived hydrogenic Rydberg states converge. The results presented pave the way for Rydberg-Stark deceleration and electrostatic trapping experiments with NO, which are expected to shed further light on the decay dynamics of these long-lived excited states, and are of interest for studies of ion-molecule reactions at low temperatures. arXiv:2005.00090v1 [physics.chem-ph] 30 Apr 2020

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Section: Electric Field Ionizationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Excitation and characterization of long-lived hydrogenic Rydberg states of nitric oxide

Deller

Hogan

2020

The Journal of Chemical Physics

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“…For low density Rydberg gases, SFI has served as an exacting probe of the coupling of electron orbital angular momentum with core rotation. Studies of nitric oxide in particular have shown that nf (2) Rydberg states of NO traverse the Stark manifold to form NO + in rotational states N + = 2 and 0 [47]. These experiments operate in a diabatic regime, employing a slew rate of 0.7 V cm −1 ns −1 .…”

Section: Experimental Backgroundmentioning

confidence: 99%

Coupled rate-equation hydrodynamic simulation of a Rydberg gas Gaussian ellipsoid: Classical avalanche and evolution to molecular plasma

Haenel

Grant

2018

Chemical Physics

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An ellipsoidal volume of Rydberg molecules, entrained in a supersonic molecular beam, evolves on a nanosecond timescale to form a strongly coupled ultracold plasma. We present coupled rate-equation simulations that model the underlying kinetic processes and molecular dissociation channels in both a uniformly distributed plasma and under the conditions dictated by our experimental geometry. Simulations predict a fast electron-driven collisional avalanche to plasma followed by slow electron-ion recombination. Within 20 µs, release of Rydberg binding energy raises the electron temperature of a static plasma to T e = 100 K. Providing for a quasi-self-similar expansion, the hot electron gas drives ion radial motion, reducing T e . These simulations provide a classical baseline model from which to consider quantum effects in the evolution of charge gradients and ambipolar forces in an experimental system undergoing responsive avalanche dynamics.

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“…Many previous studies have recognized that the rate of predissociation, which depends sensitively on Rydberg orbital angular momentum, , limits transitions readily detected by ionization from A 2 Σ + N = 0 to those in the N = 1 nf Rydberg series that converges to the NO + rotational level, N + = 2 [61][62][63][64]68]. This hydrogenic series, n 0 f (2), defines a particular subset of nitric oxide Rydberg gas initial states that evolve to form a durable ultracold plasma.…”

Section: Discussionmentioning

confidence: 99%

mm-wave Rydberg-Rydberg resonances as a witness of intermolecular coupling in the arrested relaxation of a molecular ultracold plasma

Wang,

Sous,

Aghigh

et al. 2020

Preprint

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Out-of-equilibrium, strong correlation in a many-body system can trigger emergent properties that act in important ways to constrain the natural dissipation of energy and matter. Networks of atoms, intricately engineered to arrange positions and tune interaction energies, exhibit striking dynamics. But, strong correlation itself can also act to restrict available phase space. Relaxation confined by strong correlation gives rise to scale invariance and density distributions characteristic of self-organized criticality. For some time, we have observed signs of self-organization in the avalanche, bifurcation and quench of a state-selected Rydberg gas of nitric oxide to form an ultracold, strongly correlated ultracold plasma. The robust arrested relaxation of this system forms a disordered state with quantum-mechanical properties that appear to support a coherent destruction of transport. Work reported here focuses on initial stages of avalanche and quench, using the mm-wave spectroscopy of an embedded quantum probe to characterize the intermolecular interaction dynamics associated with the evolution to plasma. Double-resonance excitation prepares a Rydberg gas of nitric oxide composed of a single selected state, n0f (2) (referring to a particular principal quantum number from n0 = 30 to 70 in the f ( = 3) Rydberg series converging to the NO + rotational state, N + = 2). Penning ionization, followed by an avalanche of electron-Rydberg collisions, forms a plasma of NO + ions and weakly bound electrons, in which a residual population of n0 Rydberg molecules evolves to high-. Predissociation depletes the plasma of low-molecules. Relaxation ceases and n0 (2) molecules with ≥ 4 persist for very long times, evidently under collision-free conditions. At short times, excitation spectra of mm-wave Rydberg-Rydberg transitions, n0f (2) → (n0 ± 1)g(2) mark the rate of electron-collisional -mixing. At long times, n0 (2) → (n0 ± 1)d( 2) depletion resonances signal collision-free energy redistribution in the basis of central-field Rydberg states. The widths and asymmetries of Fano lineshapes witness the degree to which coupling to the arrested bath broadens the bright state as well as how bright-state predissociation mixes the network of levels in the localized ensemble.

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Rotational-state-selective field ionization of molecular Rydberg states

Cited by 10 publications

References 62 publications

Excitation and characterization of long-lived hydrogenic Rydberg states of nitric oxide

Excitation and characterization of long-lived hydrogenic Rydberg states of nitric oxide

Coupled rate-equation hydrodynamic simulation of a Rydberg gas Gaussian ellipsoid: Classical avalanche and evolution to molecular plasma

mm-wave Rydberg-Rydberg resonances as a witness of intermolecular coupling in the arrested relaxation of a molecular ultracold plasma

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