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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Spectroscopic Hole Burning In Saturable Dyes

David L. Stockman

Published May 17, 1969• 0 citations
Publisher

Abstract

The results of frequency locking experiments with coupled ruby lasers are presented. The single axial mode characteristics of an individual saturable dye-switched laser can be understood without requiring spectroscopic hole burning in the dye. For coupled lasers in which frequency locking is observed, the existence of a spectroscopic hole seems necessary to explain the experimental results. The widths of the holes are inferred to be about 0.10 cm-1 using pyridine and 0.04 cm-1 using cyclohexanol as solvents. A relatively slow time dependent perturbation of the dye by thermal density fluctuations in the solvent yields a fluctuation in the transition energy of about 0.12 cm-1, which is in qualitative agreement with the inferred widths.

DOI
10.1117/12.946872

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Physical review. B, Condensed matter•Dec 1, 1991•48 citations
The results of frequency locking experiments with coupled ruby lasers are presented. The single axial mode characteristics of an individual saturable dye-switched laser can be understood without requiring spectroscopic hole burning in the dye. For coupled lasers in which frequency locking is observed, the existence of a spectroscopic hole seems necessary to explain the experimental results. The widths of the holes are inferred to be about 0.10 cm-1 using pyridine and 0.04 cm-1 using cyclohexanol as solvents. A relatively slow time dependent perturbation of the dye by thermal density fluctuations in the solvent yields a fluctuation in the transition energy of about 0.12 cm-1, which is in qualitative agreement with the inferred widths.
Using picopulses generated by a mode-locked ruby laser, we have measured the 3-8-Å bandwidth of a hole burned in the 0-0 transition of cryptocyanine in methanol and demonstrated the inhomogeneous chatacter of this transition. The population-rate equations are written for an inhomogeneous transition with two and four energy levels interacting with continuous or pulsed excitation. Using the numerical solutions of this model together with the experimental result we determine a transverse relaxation timeT_{2} = 0.6-1ps for cryptocyanine in methanol.
Saturation spectroscopy of Iodine is used to lock the frequency of a Coherent 699-21 Ring Dye laser. Without an external reference the laser frequency drifts several tens of MHz per hour. With the system presented in this thesis the drift has been reduced to a maximum of ±lMHz. Theoretical description of saturation spectroscopy and hole burning is given and the experiments are presented. In preparation for future experiments in quantum computing hole burning in rare-earth-ion-doped crystals and broadening of the hole by excitation of ions at different intervals have also been studied in this master's thesis.
The interaction between waves in an idealized saturable absorber is discussed. It is shown that the presence of a strong wave will cause the line to appear to be ``hole-burned'' when probed by a second wave, even though the broadening mechanisms are conventionally homogeneous. This effect would be expected to work against the tendency of dye-switched ruby lasers to operate in a single mode. Related effects should play a role in optical pulse generators and in other devices using saturable absorbers.
By using an Ar+ ion laser, a tunable Rh 6G dye laser(Linewidth : 0.5 cm(-1)) and a Coherent 899-21 dye laser as light sources and using a monochromator and a phase-locking amplifier, the optical properties of Eu3+ : Y2SiO5 crystal were detected. Persistent spectral hole burning (PSHB) were also observed in (5)Do-(7)Fo transition in the crystal at the temperature of 16 K. For 15 mW dye laser (Wavelength : 579.62 nm) burning the crystal for 0.1 s a spectral hole with about 80 MHz hole width were detected and the hole can been keep for longer than 10 h.
At very low temperatures, the spread in the different environments of matrix embedded dye molecules results in an inhomogeneously broadened S1 ← S0 band. Spectroscopic techniques based on the appearence of optical zero phonon lines, such as fluorescence line narrowing, spectral hole-burning, and single molecule spectroscopy provide an experimental resolution limited by the homogeneous linewidth. From the investigation of the homogeneous line width as a function of different parameters (time, temperature) information on the guest host interactions responsible for the observed linewidth is obtained. Spectrally narrow features are extremely sensitive probes for external perturbations, such as electric fields, magnetic fields, or hydrostatic pressure.
Frequency-domain optical hole burning of the R1{\mathit{R}}_{1}R1​ line [4{[}^{4}[4A2{\mathit{A}}_{2}A2​(-1/2)\ensuremath{\leftrightarrows}E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) transition] in dilute ruby is studied at 2 K and with a field of 3.6 kG applied along the c axis. A pump-probe (PP) technique is used with precise probe-frequency shifting obtained by an acousto-optic modulator. For sufficiently short PP pulses (50 \ensuremath{\mu}s), two holes (narrow and wide) are observed. The narrow (\ensuremath{\sim}20 kHz half width at half maximum at low power) hole-width dependence on Rabi frequency approximately agrees with that inferred from free-induction-decay measurements. For the present concentration (0.0034 wt. % Cr2{\mathrm{Cr}}_{2}Cr2​O3{\mathrm{O}}_{3}O3​) and field, the narrow hole width is determined by fluctuating fields produced by Cr-Cr spin flips [A. Szabo, T. Muramoto, and R. Kaarli, Phys. Rev. B 42, 7769 (1990)]. When the PP delay time is varied, the amplitude of the narrow hole decays with a 1/e time constant of \ensuremath{\sim}300 \ensuremath{\mu}s compared to the E\ifmmode\bar\else\textasciimacron\fi{} fluorescence lifetime of 4 ms. The wide hole (\ensuremath{\sim}500 kHz half width at half maximum) is due to Al-Cr superhyperfine interactions and is created by a spectral diffusion mechanism driven by Al-spin flipping in the host lattice.