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The European Physical Journal Applied Physics

Interaction between infrared laser modes in Rydberg Matter: redshifted modes in reflection and blueshifted in transmission

Leif Holmlid

Published Mar 16, 2004• 4 citations
Publisher

Abstract

When an almost single-mode IR laser beam is reflected from an IR window with a deposit of Rydberg Matter on the inner, vacuum face, the laser modes appear red-shifted; thus their maxima are observed at lower laser current. This effect is complementary to the previously reported blue-shifts of IR laser modes in transmission through Rydberg Matter. Both types of shifts are due to interaction between the laser modes, now proved by using only two isolated modes both in reflection and transmission. The general process is stimulated Raman scattering. Rydberg Matter is here formed from Rydberg states of K atoms and nitrogen molecules inside a vacuum chamber. A theoretical description is given that involves slow decay or increase in the energy of the photons interacting with the Rydberg Matter, depending on the temperature of this matter. This means that the two isolated modes studied may become almost resonant within certain frequency ranges. The energy increase (frequency blue-shifting) of photons passing hot Rydberg Matter has been reported previously. The description used explains both the red-shifted reflection and the blue-shifted transmission results.

DOI
10.1051/epjap:2004019

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Wave-number blueshifts of single-mode laser light in low-density Rydberg matter are found to be due to stimulated Raman processes. The Rydberg matter is mainly formed from Rydberg states of K atoms. The lasers used are mW continuous-wave lasers in the ir, lead-salt tunable diode lasers. Of special significance is the blueshifting observed as shifts of Fabry-Perot etalon fringes of the order of 0.05 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$. This blueshifting is explained as due to complete conversion to anti-Stokes radiation through higher-order stimulated Raman shifting by extremely small quanta from the near continuum of energy levels in the metallic Rydberg matter phase. Complicated strong shifts of intensity to larger wave numbers in the laser modes are also observed, due to coupling of laser side modes to the anti-Stokes waves. The high efficiency of the stimulated Raman process is partly due to the weak coupling to other degrees of freedom.

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•Jan 1, 1997•1 citation
When an almost single-mode IR laser beam is reflected from an IR window with a deposit of Rydberg Matter on the inner, vacuum face, the laser modes appear red-shifted; thus their maxima are observed at lower laser current. This effect is complementary to the previously reported blue-shifts of IR laser modes in transmission through Rydberg Matter. Both types of shifts are due to interaction between the laser modes, now proved by using only two isolated modes both in reflection and transmission. The general process is stimulated Raman scattering. Rydberg Matter is here formed from Rydberg states of K atoms and nitrogen molecules inside a vacuum chamber. A theoretical description is given that involves slow decay or increase in the energy of the photons interacting with the Rydberg Matter, depending on the temperature of this matter. This means that the two isolated modes studied may become almost resonant within certain frequency ranges. The energy increase (frequency blue-shifting) of photons passing hot Rydberg Matter has been reported previously. The description used explains both the red-shifted reflection and the blue-shifted transmission results.
Wave-number blueshifts of single-mode laser light in low-density Rydberg matter are found to be due to stimulated Raman processes. The Rydberg matter is mainly formed from Rydberg states of K atoms. The lasers used are mW continuous-wave lasers in the ir, lead-salt tunable diode lasers. Of special significance is the blueshifting observed as shifts of Fabry-Perot etalon fringes of the order of 0.05 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$. This blueshifting is explained as due to complete conversion to anti-Stokes radiation through higher-order stimulated Raman shifting by extremely small quanta from the near continuum of energy levels in the metallic Rydberg matter phase. Complicated strong shifts of intensity to larger wave numbers in the laser modes are also observed, due to coupling of laser side modes to the anti-Stokes waves. The high efficiency of the stimulated Raman process is partly due to the weak coupling to other degrees of freedom.
The interaction between Rydberg systems [Rydberg atoms (RA) gas or Rydberg matter (RM)] and coherent light in various frequency bands is considered. It is shown why Rydberg systems possess a greater polarizabilities and, accordingly, linear and nonlinear susceptibilities and strong sensitive to high-1 (circular) Rydberg states in RA and RM. Quantum theory of physical and chemical properties of RA and RM are related with recent obtained results on the optical spectroscopy. The experimental data of Raman processes, wave mixing effects in gas of RA, and their clusters of RM are analyzed. Problem of blueshifts and stimulated electronic laser Raman processes, as well as four wave mixing in RM are discussed.
We have observed the process $\mathrm{Rb}ns+\mathrm{Rb}\phantom{\rule{4pt}{0ex}}ns+2h\ensuremath{\nu}\ensuremath{\rightarrow}\mathrm{Rb}\phantom{\rule{4pt}{0ex}}n{p}_{1/2}+\mathrm{Rb}\phantom{\rule{4pt}{0ex}}n{p}_{3/2}$ from n=34n=34n=34 to n=40n=40n=40 in a frozen gas of Rb Rydberg atoms. It is resonant when the microwave frequency is halfway between the $ns\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}n{p}_{1/2}$ and $ns\ensuremath{\rightarrow}n{p}_{3/2}$ frequencies, which range from 57 to 106 GHz. The process cannot occur in isolated atoms, nor can it occur if the magnetic quantum numbers are unchanged, an implicit assumption of one-dimensional models. A Floquet-Forster model shows that the coupling between the initial and final states involves the absorption of two microwave photons and the dipole-dipole interaction, which leads to a coupling proportional to the product of the density, the microwave field squared, and n∗14{n}^{*14}n∗14, where n∗{n}^{*}n∗ is the effective quantum number of the np3/2n{p}_{3/2}np3/2​ state. We have experimentally verified these dependences. The observed resonances are asymmetric, with a low-frequency tail, which we attribute to the van der Waals shift of the final np1/2np3/2n{p}_{1/2}n{p}_{3/2}np1/2​np3/2​ state due to its dipole-dipole interaction with the nearby ns(n+1)sns(n+1)sns(n+1)s state. While the van der Waals shift is negligible for most of the atoms in the Rydberg gas, it is not for the pairs of close atoms which undergo this transition.
A brief state-of-art review of the research into the interaction of laser radiation with Rydberg atoms and clusters of Rydberg atoms is provided. The dynamics of various Rydberg species in a high-frequency optical field is described with the use of the quantum-mechanical approach. Experimental data indicating the existence of Rydberg-state species (Rydberg clusters and Rydberg matter) are analyzed. A special emphasis is placed on Raman processes in Rydberg atoms and Rydberg matter created on solid surfaces.
Nonlinear optical phenomena in both semiconductor microcavities and sodium vapor are investigated. Systems displaying atomic and excitonic coupling are studied in detail in order to unravel underlying physical principles. Possible applications for these systems are evaluated where appropriate. Normal-mode coupling (NMC) in a semiconductor microcavity is achieved when a narrow-linewidth quantum well exciton resonance is coincident with the cavity mode of a high-finesse microcavity. This interaction leads to a double-peaked spectrum in either transmission, reflection, or photoluminescence (PL). The high-quality microcavities studied here at liquid-Helium temperatures reveal intensity dependent behavior that has not previously been observed. Nonlinear saturation of the exciton leads to a spectral broadening of the excitonic absorption without a significant loss in oscillator strength. This results in a reduction of the two transmission peaks with almost no change in the splitting between the peaks. Such behavior is easily explained using phenomenological nonlinear dispersion theory. In this nonlinear regime, the luminescence from the microcavity shows a gradual transition from the nonperturbative regime of NMC to lasing with increasing excitation. The observed behavior is explained by density-dependent changes in both the transmission of the microcavity and the bare-exciton emission, rather than a boson-condensation of excitons which has been previously proposed. An intermediate-finesse microcavity also modifies the emission distribution from a bulk-semiconductor at room temperature. Angularly resolved emission spectra and quantum efficiency measurements show the PL is strongly dependent on the reflectivity of the microcavity. Unfortunately, the enhancement in the decay rate of excitons due to high-reflectivity mirrors seen previously by our group does not result in an increased quantum efficiency. High-gain optical-wavefront amplification in atomic sodium vapor is demonstrated via both the three-photon effect and stimulated Raman scattering (SRS). In both cases, single-pass weak-field gain of nearly 400 is achieved with only 800 mW of pump power near 589 nm. In the case of SRS, phase preservation of the amplified wavefront, which is necessary in adaptive imaging applications, is also demonstrated.