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Physical Review A

Suppression of excited-state absorption: A path to ultraviolet tunable solid-state lasers

Elena Kuznetsova, Roman L. Kolesov, Olga A. Kocharovskaya

Published Oct 4, 2004• 17 citations
Publisher

Abstract

A method of suppression of losses due to excited-state absorption (ESA) in laser crystals is proposed, based on the well-known phenomenon of electromagnetically induced transparency. Typical situations in which ESA prevents lasing are considered. Theoretical analysis shows that by using an additional driving laser field one can inhibit ESA and make lasing possible. On the basis of available spectroscopic information estimates for rare-earth-ion-doped laser materials are presented. They show the feasibility of obtaining optical gain at parity-allowed $4{f}^{n}\ensuremath{\leftrightarrow}4{f}^{n\ensuremath{-}1}5d$ transitions of rare-earth ions in the ultraviolet spectral region after suppression of ESA at an emission wavelength into the conduction band of a host material.

DOI
10.1103/physreva.70.043801

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Physical Review A•Apr 19, 2005•3 citations
A method of suppression of losses due to excited-state absorption (ESA) in laser crystals is proposed, based on the well-known phenomenon of electromagnetically induced transparency. Typical situations in which ESA prevents lasing are considered. Theoretical analysis shows that by using an additional driving laser field one can inhibit ESA and make lasing possible. On the basis of available spectroscopic information estimates for rare-earth-ion-doped laser materials are presented. They show the feasibility of obtaining optical gain at parity-allowed 4fn\ensuremath↔4fn\ensuremath−15d4{f}^{n}\ensuremath{\leftrightarrow}4{f}^{n\ensuremath{-}1}5d4fn\ensuremath↔4fn\ensuremath−15d transitions of rare-earth ions in the ultraviolet spectral region after suppression of ESA at an emission wavelength into the conduction band of a host material.
The optical-absorption transitions originating from the lowest 4f5d excited state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y3{\mathrm{Y}}_{3}Y3​Al5{\mathrm{Al}}_{5}Al5​O12{\mathrm{O}}_{12}O12​ have been studied. The experimental arrangement uses a 7-ns 266-nm light pulse to populate the lowest 4f5d state, and a spatially overlapped, time-sequenced pulse from a frequency-tunable dye laser to induce transitions from that excited state. The excited-state-absorption (ESA) spectrum covering the 900--300-nm probe wavelength range is characterized by two broad peaks centered at 700 and 350 nm on a slowly rising background. The peak ESA cross section at 355 nm is (1\ifmmode\pm\else\textpm\fi{}0.1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}17}$ cm2{\mathrm{cm}}^{2}cm2. The position, shape, and strength of the spectrum suggest that the terminal states of the ESA transitions are the second 4f5d state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ and the conduction band of the host lattice. The ESA measurements have been extended to transitions from the 3^{3}3P0{\mathit{P}}_{0}P0​ and 1^{1}1D2{\mathit{D}}_{2}D2​ excited states of the 4f2{\mathit{f}}^{2}f2 configuration of Pr3+{\mathrm{Pr}}^{3+}Pr3+ as well. The ESA cross sections at a probe wavelength of 532 nm are (8\ifmmode\pm\else\textpm\fi{}1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ cm2{\mathrm{cm}}^{2}cm2 and (5.7\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ cm2{\mathrm{cm}}^{2}cm2 for transitions from the 3^{3}3P0{\mathit{P}}_{0}P0​ and 1^{1}1D2{\mathit{D}}_{2}D2​ excited states, respectively. The terminal state of ESA transitions from these two levels is the lowest 4f5d state. The strong ESA completely inhibits the potential laser action based on emission from these states in this crystal.
Broad bandwidth 5d→4f transitions in Ce3+ have been considered for tunable laser action. In this letter, optical probe measurements of excited Ce3+ ions in Y3Al5O12 show that stimulated emission in the 550–610-nm region is not possible at 295 K because of excited-state absorption. Transient measurements demonstrate that part of this loss has ≈75-ns lifetime and is associated with absorption from the lowest 5d level; a longer-lifetime loss is also observed. The excited-state-absorption loss is reduced at lower temperatures.
The impact of photodynamic processes induced by pump radiation in crystals doped with rare-earth (RE) ions on the possibility of generating stimulated radiation in the UV and VUV spectral ranges is analyzed. It is shown that, in addition to objective factors, one of the main causes preventing the lasing effect from being obtained using the interconfigurational 4ƒ n−15d-4ƒ n transitions of RE ions is insufficient consideration of the photodynamic processes involved in experiments. It is proposed to correct laser test techniques and “pumpprobe” experiments aimed at investigating active media appropriate for lasing in the UV and VUV ranges. Extended criteria oriented to search for new solid-state UV and VUV active media are formulated.
Index of refraction characterizes the linear response of a medium and hence it is strongly enhanced near atomic resonance. However, it is accompanied by either resonant absorption or gain preventing the use of high index. We show that these problems may be overcome using coherent control of excited state absorption (ESA), i.e. absorption from the populated excited electronic state. The idea is to compensate gain at the lower operating transition via partially suppressed ESA at the frequency of the probe field tuned to the maximum refractive index of the ESA transition. It results in resonant enhancement of refractive index without absorption in the absence of any neighboring amplification regions.
Propagation of a short pulse in an amplifier with excited-state absorption (ESA) is considered. As is shown both analytically and numerically, if the stimulated emission cross section exceeds the ESA cross section, a steady-state pulse of a dissipative soliton type can exist. The parameters of the soliton, i.e., its width, amplitude, and velocity, are calculated. In the opposite case, amplification is inhibited unless ESA is suppressed using an additional control field applied to a transition adjacent to the ESA one [Phys. Rev. A 70, 043801 (2004)]. Propagation and amplification dynamics of a probe pulse in the presence of a strong control field is analyzed. In the limit of a continuous wave control field, a dissipative soliton solution forms, which is a pair of pulses similar to adiabatons. In the case of a pulsed control field, amplification of the probe pulse is transient. Conditions for optimal amplification are derived. Estimates of soliton parameters are made for rare-earth and transition-metal ion-activated laser crystals.