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Physical review. B, Condensed matter

Transient excited-state absorption measurements in chromium-doped forsterite

Nickolay Zhavoronkov, Valentin P. Petrov, FRANK NOACK

Published Jan 15, 2000• 3 citations
Publisher

Abstract

The nonradiative transition dynamics between the excited ${}^{3}{A}^{\ensuremath{''}}{[}^{3}{E(}^{3}{T}_{1a})]$ state and the metastable ${}^{3}{A}^{\ensuremath{''}}{[}^{3}{E(}^{3}{T}_{2})]$ storage state of the tetravalent chromium ion $({\mathrm{Cr}}^{4+})$ in forsterite is investigated using femtosecond excite-and-probe technique. Following excitation to ${}^{3}{T}_{1a}$ with pump pulses at 750 or 773 nm the induced excited state absorption was probed with femtosecond pulses in the ultraviolet (306 nm), visible (650 nm), and infrared (1500 nm). The nonradiative decay time from ${}^{3}{T}_{1a}$ to ${}^{3}{T}_{2}$ was estimated from the rise time of the excited state absorption at 1500 nm using a rate equations model and its value at room temperature is only 3\ifmmode\pm\else\textpm\fi{}1 ps.

DOI
10.1103/physrevb.61.1866

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The nonradiative transition dynamics between the excited 3A\ensuremath′′[3E(3T1a)]{}^{3}{A}^{\ensuremath{''}}{[}^{3}{E(}^{3}{T}_{1a})]3A\ensuremath′′[3E(3T1a​)] state and the metastable 3A\ensuremath′′[3E(3T2)]{}^{3}{A}^{\ensuremath{''}}{[}^{3}{E(}^{3}{T}_{2})]3A\ensuremath′′[3E(3T2​)] storage state of the tetravalent chromium ion (Cr4+)({\mathrm{Cr}}^{4+})(Cr4+) in forsterite is investigated using femtosecond excite-and-probe technique. Following excitation to 3T1a{}^{3}{T}_{1a}3T1a​ with pump pulses at 750 or 773 nm the induced excited state absorption was probed with femtosecond pulses in the ultraviolet (306 nm), visible (650 nm), and infrared (1500 nm). The nonradiative decay time from 3T1a{}^{3}{T}_{1a}3T1a​ to 3T2{}^{3}{T}_{2}3T2​ was estimated from the rise time of the excited state absorption at 1500 nm using a rate equations model and its value at room temperature is only 3\ifmmode\pm\else\textpm\fi{}1 ps.
The gain dynamics of photoexcited chromium-doped forsterite (Cr4+:Mg2SiO4) were measured by means of a pulsed excite-and-probe technique. The nonradiative relaxation time within the 3T2 vibronic state was determined by measuring the change in the induced gain of the probe pulse as a function of the pumpprobe delay. A 30 ps, 1.064 m pulse from a mode-locked Nd:YAG laser was split into two beams. The first beam provided the pump pulse to populate the 3T2 manifold. The other beam was focused in a calcite crystal to generate a 1.2 m probe pulse by means of stimulated Raman scattering. The transient gain was determined from the measured ratio of the transmitted probe intensity for unpumped and pumped cases as a function of the pumpprobe delay. The rise time (time for growth of the gain from 10% to 90%) was calculated to be 50 ps. A rate-equation analysis of population in the various states was used to extract a value for the vibrational relaxation time from the experimental data under the assumption of Gaussian pump and probe pulses. The best fit to the experimental data of gain as a function of time yields a value of 10 5 ps for the intra-3T2-state vibrational relaxation time.
The optical absorption, temperature dependences of the luminescence intensity and decay time, and the transient absorption spectra of a Cr 4+ : Gd 2 SiO 5 crystal were determined by the picosecond excitation and probing method. An analysis of the results showed that the induced absorption observed in the 600–650 nm range was due to 3 T 2 ( 3 F ) → 3 T 1 ( 3 P ) transitions from the excited state. The lifetimes of the 3 T 2 ( 3 F ) and 3 T 1 ( 3 F ) levels were estimated to be 15 ns and 12 ps, respectively. The cross section for absorption from the first excited state at the wavelength of 616 nm was (1.1 ± 0.6)×10 -18 cm 2 and that for absorption from the ground state at λ = 540 nm was (2.2 ± 1.1)×10 -18 cm 2 .
The absorption cross sections of the Cr3+{\mathrm{Cr}}^{3+}Cr3+ ion in the metastable states 2E(E‾and2A‾)^{2}E (\overline{E} \mathrm{and} 2\overline{A})2E(Eand2A) of lightly doped ruby (\ensuremath{\sim}0.01%) have been measured as a function of polarization at temperatures of 30, 105, and 296\ifmmode^\circ\else\textdegree\fi{}K in the region from 2300 to 7000 \AA{}. The lifetime of these states was measured by observing the decay rate of the excited-state absorption, and agreed with the value of the measured fluorescence decay rate at various temperatures. The population of the excited states was measured by the change of the area under the first two vibronic sidebands at low temperatures. At room temperature the population was measured by the change of transmitted intensity of a ruby laser.
We describe a systematic, rigorous procedure for the determination of the optical absorption saturation parameters for Cr4+:YAG and Cr4+:forsterite crystals at 1064 nm. A rate-equation approach was used to analyze the cw and pulsed transmission data of several crystals by accounting for the transverse as well as longitudinal variation of the beam intensity, saturation effects, and excited-state absorption. Use of an iterative procedure whereby the cw and pulsed data were simultaneously analyzed led to a considerable reduction in the error for the determination of cross sections. The average value of the absorption cross section sigmaa and the normalized excited-state absorption cross section fp=sigmaesa/sigmaa were determined to be 6.13×10−19 cm2 and 0.45, respectively, for Cr4+:forsterite and 19.6×10−19 cm2 and 0.06, respectively, for Cr4+:YAG. Detailed comparison was also made with previous saturation measurements in the literature. Our results further show that lumped models based on the thin-length approximation should be used with caution in the determination of cross sections, especially when the pump beam is tightly focused inside the absorber.
The negatively charged nitrogen vacancy ($\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$) defect in diamond serves as a popular platform for manipulating and exploiting long-lived coherent spin dynamics at room temperature combined with optical readout. The required spin polarization of the spin triplet 3A2^{3}A_{2}3A2​ electronic ground state occurs through a cycle of repetitious optical photoexcitation events to the 3E^{3}E3E electronic excited state that is accompanied by a series of electronic transitions to a 1A1^{1}A_{1}1A1​ and a 1E^{1}E1E electronic state, and back to the 3A2^{3}A_{2}3A2​ state. The timescales of these transitions are largely known, yet for the relaxation time of the $^{1}A_{1}\ensuremath{\rightarrow}^{1}E$ infrared transition, which predominantly occurs via nonradiative recombination, only an upper limit of 1 ns could be determined so far. Here, we employ ultrafast transient absorption spectroscopy to probe the dynamics of the nonradiative relaxation from the 1A1^{1}A_{1}1A1​ to the 1E^{1}E1E state after photoexcitation of the 3E^{3}E3E state and find a relaxation time of 100 ps at a temperature of 78 K.