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PubMed2002

An investigation of energy spectrum and lineal energy variations in mega-voltage photon beams used for radiotherapy.

Megavoltage photon beams are routinely used for external-beam radiotherapy. Recently, new treatment modalities based on dynamic and intensity modulated (IM), beam delivery systems are increasingly used in clinical practice. The purpose of this work is to investigate the energy spectrum and microdosimetric features of these photon beams. A Monte Carlo technique was first used to simulate beam lines of medical accelerators and to compute photon fluence and spectrum per unit dose-to-water inside the irradiated medium. Subsequently, a track structure code was used to compute the lineal energy and its distribution in a 1 micron sphere based on the individual photon spectrum. Results showed that the low energy photon component varied significantly with field size and location within the field due to the presence of the scattered photons. The calculated dose-mean lineal energy ranged from 2.3 keV.micron-1 at a depth of 1.5 cm along the central axis of a 4 cm x 4 cm field, to 3.7 keV.micron-1 at a depth of 20 cm of the field edge in a 10 cm x 10 cm field. In the tested IM fields at a depth of 10 cm, ranged from 2.6 to 3.5 keV.micron-1, which was inversely related to the dose intensity in the field. The values for the clinical photon beams were also significantly greater than that of a reference 60Co beam (1.8 keV.micron-1 from the calculation). The beam quality factor was estimated to vary within 20% due to the change of the energy spectrum for the radiotherapy photon fields.

Cobalt Radioisotopes↗
PubMed2004

Measurement of photon energy and dose rate.

According to ICRP 60, the radiation weighting factor for photon radiation is set equal to one, irrespective of photon energy and dose rate. However, it is well known that the relative biological effectiveness is not constant for all photon energies and also depends on the dose rate. If these dependencies are to be considered, both the photon energy and the dose rate should be measured. This paper describes the extent to which these quantities can be measured for photons with the available instruments. For individual monitoring the existing dosemeters are mainly used to measure the dose, and so values or estimates of both the dose rate and the photon energy are only available for specially designed instruments as additional information. Some passive dosemeters as well as a few direct reading electronic dosemeters can provide information on photon energy. In addition, some of the direct reading electronic dosemeters have the capability to provide dose rate information. For workplace monitoring the dose rate is the main measured quantity, and so dose rate values are always available. Moreover, there are some special instruments available in the market that are designed to measure photon energy.

Humans↗
PubMed2005

Are all photon radiations similar in large absorbers?--a comparison of electron spectra.

Conventional X rays, i.e. X rays generating voltage between roughly 150 and 300 kV, are used in many radio-diagnostic procedures and also in radiobiological experiments. They release less energetic and, therefore, more densely ionising electrons than the high-energy gamma rays from 60Co or from the A bombs. Accordingly, they are considered to be somewhat more effective, especially at low doses. Various radiobiological studies, especially studies on chromosome aberrations have confirmed this assumption, but epidemiological investigations, e.g. the comparison of the excess relative risk for mammary cancer in the X-ray exposed patients and in the gamma-ray exposed A bomb survivors, have not demonstrated a similar difference. In view of the missing epidemiological evidence and largely for the reasons of practicality in radiation protection, the ICRP has recommended the radiation weighting factor unity equally for all photon radiations. However, in the discussion preceding the 2005 Recommendations of the ICRP, the issue remains controversial. In a recent paper, Harder et al. argue--with reference to an assessment by the German Radiation Protection Commission (SSK)--that the use of the same weighting factor for different photon energies can be justified more directly. For high-energy incident photons, they present the degraded photon spectra at different depths in a phantom, and they conclude that much of the difference between high-energy gamma rays and conventional X rays disappears in a large phantom. The present assessment, which is more direct, compares the spectra of electrons released (through pair production, Compton effect and photo effect) in a small and in a very large receptor for the incident photons of 150 keV, 1 MeV and 6 MeV. For the 1 Mev and 6 MeV photons, there is a substantial shift towards smaller electron energies in the large receptor, but the electron spectra remain much harder than those from the 150 keV incident photons. Furthermore, it is seen--in agreement with earlier conclusions by Straume--that for the broad gamma-ray spectrum from the A bombs there is no shift at all to lower energies within the body, but rather some degree of hardening of the radiation. The assumption that distinct differences between high-energy gamma rays and conventional X rays are restricted to small samples must, thus, be rejected. The attribution of the same effective quality factor or radiation weighting factor to all photon energies remains, therefore, an issue that is based on the considerations beyond dosimetry.

Body Burden↗
PubMed2003

Micronucleus response of human glioblastoma and neuroblastoma cells toward low-LET photon and high-LET p(66)/Be neutron irradiation.

The identification of photon resistant tumors that are sensitive to neutrons is still an unresolved problem, and no radiobiological criteria have been developed that could help the selection of patients for neutron therapy. The micronucleus (MN) assay has been evaluated for this purpose in a panel of human glioblastoma and neuroblastoma cell lines spanning a wide range of photon sensitivities defined by mean inactivation doses ([Latin capital letter D with macron above][gamma]) of 1.25-3.21 Gy. We show that the relative biologic effectiveness (RBE) of the p(66)/Be neutrons is significantly correlated with inherent photon sensitivity (r = 0.89, p < 0.01), indicating that the panel of cell lines used is suitable to study the differential biologic response to neutrons and photons. We find that p(66)/Be neutrons are 1.43 to 5.29 times more effective per unit dose in inducing micronuclei than 60Co [gamma]-rays. Surprisingly, cells that are inherently photon resistant tend to show a higher yield of micronuclei following exposure to either photons or neutrons, but no significant correlation could be demonstrated. However, RBE values based on micronucleus yield were found to strongly correlate with RBE values derived from cell survival data (r = 0.91, p < 0.01). It is concluded that although micronucleus yield does not reflect intrinsic sensitivity to either photons or neutrons, the strong correlation between RBE calculated from micronucleus formation and RBE derived from cell survival demonstrates that the micronucleus endpoint has a potential for detecting photon resistant cells that show increased sensitivity to neutrons.

Cell Line, Tumor↗
PubMed1995

On the possibility of calcium imaging using Indo-1 with three-photon excitation.

We show that the calcium fluorophore Indo-1 can be excited by simultaneous absorption of three-photons at 885 nm, a wavelength readily available from Ti:sapphire lasers. Three-photon excitation was demonstrated by the emission intensity of Indo-1 which depended on the cube of the laser power, and by a higher anisotropy than was observed for two-photon excitation. Excitation of Indo-1 becomes a two-photon process when the wavelength is decreased to 820 nm. Three-photon excitation was accomplished at a low 17 microM concentration of Indo-1. Examination of the spatial profile of the excited Indo-1 showed a smaller volume for three- versus two-photon excitation. These results suggest that three-photon excitation may be useful in fluorescence microscopy using the long wavelength output of Ti:sapphire lasers, and may provide higher spatial resolution than available using two-photon excitation.

Calcium↗
PubMed2001

Two-photon microscopy and spectroscopy based on a compact confocal scanning head.

We have combined a confocal laser scanning head modified for TPE (two-photon excitation) microscopy with some spectroscopic modules to study single molecules and molecular aggregates. The behavior of the TPE microscope unit has been characterized by means of point spread function measurements and of the demonstration of its micropatterning abilities. One-photon and two-photon mode can be simply accomplished by switching from a mono-mode optical fiber (one-photon) coupled to conventional laser sources to an optical module that allows IR laser beam (two-photon/TPE) delivery to the confocal laser scanning head. We have then described the characterization of the two-photon microscope for spectroscopic applications: fluorescence correlation, lifetime and fluorescence polarization anisotropy measurements. We describe the measurement of the response of the two-photon microscope to the light polarization and discuss fluorescence polarization anisotropy measurements on Rhodamine 6G as a function of the viscosity and on a globular protein, the Beta-lactoglobulin B labeled with Alexa 532 at very high dilutions. The average rotational and translational diffusion coefficients measured with fluorescence polarization anisotropy and fluorescence correlation methods are in good agreement with the protein size, therefore validating the use of the microscope for two-photon spectroscopy on biomolecules.

Animals↗
PubMed2003

Comparison of dose calculation algorithms with Monte Carlo methods for photon arcs.

The objective of this study is to seek an accurate and efficient method to calculate the dose distribution of a photon arc. The algorithms tested include Monte Carlo, pencil beam kernel (PK), and collapsed cone convolution (CCC). For the Monte Carlo dose calculation, EGS4/DOSXYZ was used. The SRCXYZ source code associated with the DOSXYZ was modified so that the gantry angle of a photon beam would be sampled uniformly within the arc range about an isocenter to simulate a photon arc. Specifically, photon beams (6/18 MV, 4 x 4 and 10 x 10 cm2) described by a phase space file generated by BEAM (MCPHS), or by two point sources with different photon energy spectra (MCDIV) were used. These methods were used to calculate three-dimensional (3-D) distributions in a PMMA phantom, a cylindrical water phantom, and a phantom with lung inhomogeneity. A commercial treatment planning system was also used to calculate dose distributions in these phantoms using equivalent tissue air ratio (ETAR), PK and CCC algorithms for inhomogeneity corrections. Dose distributions for a photon arc in these phantoms were measured using a RK ion chamber and radiographic films. For homogeneous phantoms, the measured results agreed well (approximately 2% error) with predictions by the Monte Carlo simulations (MCPHS and MCDIV) and the treatment planning system for the 180 degrees and 360 degrees photon arcs. For the dose distribution in the phantom with lung inhomogeneity with a 90 degrees photon arc, the Monte Carlo calculations agreed with the measurements within 2%, while the treatment planning system using ETAR, PK and CCC underestimated or overestimated the dose inside the lung inhomogeneity from 6% to 12%.

Algorithms↗
PubMed2005

Dosimetric characteristics of a new unshielded silicon diode and its application in clinical photon and electron beams.

Shielded p-silicon diodes, frequently applied in general photon-beam dosimetry, show certain imperfections when applied in the small photon fields occurring in stereotactic or intensity modulated radiotherapy (IMRT), in electron beams and in the buildup region of photon beam dose distributions. Using as a study object the shielded p-silicon diode PTW 60008, well known for its reliable performance in general photon dosimetry, we have identified these imperfections as effects of electron scattering at the metallic parts of the shielding. In order to overcome these difficulties a new, unshielded diode PTW 60012 has been designed and manufactured by PTW Freiburg. By comparison with reference detectors, such as thimble and plane-parallel ionization chambers and a diamond detector, we could show the absence of these imperfections. An excellent performance of the new unshielded diode for the special dosimetric tasks in small photon fields, electron beams and build-up regions of photon beams has been observed. The new diode also has an improved angular response. However, due to its over-response to low-energy scattered photons, its recommended range of use does not include output factor measurements in large photon fields, although this effect can be compensated by a thin auxiliary lead shield.

Biophysical Phenomena↗
PubMed2006

Efficient photon beam dose calculations using DOSXYZnrc with BEAMnrc.

This study examines the efficiencies of doses calculated using DOSXYZnrc for 18 MV (10 X 10 cm2 field size) and 6 MV (10 X 10 cm2 and 20 X 20 cm2 field sizes) photon beams simulated using BEAMnrc. Both phase-space sources and full BEAMnrc simulation sources are used in the DOSXYZnrc calculations. BEAMnrc simulation sources consist of a BEAMnrc accelerator simulation compiled as a shared library and run by the user code (DOSXYZnrc in this case) to generate source particles. Their main advantage is in eliminating the need to store intermediate phase-space files. In addition, the efficiency improvements due to photon splitting and particle recycling in the DOSXYZnrc simulation are examined. It is found that photon splitting increases dose calculation efficiency by a factor of up to 6.5, depending on beam energy, field size, voxel size, and the type of secondary collimation used in the BEAMnrc simulation (multileaf collimator vs photon jaws). The optimum efficiency with photon splitting is approximately 55% higher than that with particle recycling, indicating that, while most of the gain is due to time saved by reusing source particle data, there is significant gain due to the uniform distribution of interaction sites and faster DOSXYZnrc simulation time when photon splitting is employed. Use of optimized directional bremsstrahlung splitting in the BEAMnrc simulation sources increases the efficiency of photon beam simulations sufficiently that the peak efficiencies (i.e., with optimum setting of the photon splitting number) of DOSXYZnrc simulations using these sources are only 3-13% lower than those with phase-space file sources. This points towards eliminating the need for storing intermediate phase-space files.

Body Burden↗
PubMed2006

Dosimetric characterization of radionuclides for systemic tumor therapy: influence of particle range, photon emission, and subcellular distribution.

Various radionuclides have been proposed for systemic tumor therapy. However, in most dosimetric analysis of proposed radionuclides the charged particles are taken into consideration while the potential photons are ignored. The photons will cause undesirable irradiation of normal tissue, and increase the probability of toxicity in, e.g., the bone marrow. The aim of this study was to investigate the dosimetric properties according to particle range, photon emission, and subcellular radionuclide distribution, of a selection of radionuclides used or proposed for radionuclide therapy, and to investigate the possibility of dividing radionuclides into groups according to their dosimetric properties. The absorbed dose rate to the tumors divided by the absorbed dose rate to the normal tissue (TND) was estimated for different tumor sizes in a mathematical model of the human body. The body was simulated as a 70-kg ellipsoid and the tumors as spheres of different sizes (1 ng-100 g). The radionuclides were either assumed to be uniformly distributed throughout the entire tumor and normal tissue, or located in the nucleus or the cytoplasm of the tumor cells and on the cell membrane of the normal cells. Fifty-nine radionuclides were studied together with monoenergetic electrons, positrons, and alpha particles. The tumor and normal tissue were assumed to be of water density. The activity concentration ratio between the tumor and normal tissue was assumed to be 25. The radionuclides emitting low-energy electrons combined with a low photon contribution, and the alpha emitters showed high TND values for most tumor sizes. Electrons with higher energy gave reduced TND values for small tumors, while a higher photon contribution reduced the TND values for large tumors. Radionuclides with high photon contributions showed low TND value for all tumor sizes studied. The radionuclides studied could be divided into four main groups according to their TND values: beta emitters, Auger electron emitters, photon emitters, and alpha emitters. The TND values of the beta emitters were not affected by the subcellular distribution of the radionuclide. The TND values of the Auger electron emitters were affected by the subcellular radionuclide distribution. The photon emitters showed low TND values that were only slightly affected by the subcellular radionuclide distribution. The alpha emitters showed high TND values that were only slightly affected by the subcellular radionuclide distribution. This dosimetric characterization of radionuclides may be valuable in choosing the appropriate radionuclides for specific therapeutic applications.

Body Burden↗
PubMed1998

Electron contamination in 8 and 18 MV photon beams.

The contribution from contaminant electrons in the buildup region of a photon beam must be separated when calculating the dose using a photon convolution kernel. Their contribution can be extrapolated from fractional depth dose (FDD) data using the fractional depth kerma (or the "equilibrium dose") derived from measured quantities such as beam attenuation with depth, phantom scatter factor as a function of field size and depth, and inverse-square law for the incident photon beam. Good agreement is observed between the extrapolated and the EGS4 Monte Carlo simulated, primary dose-to-kerma ratios in the surface region for the photon beams, excluding electron contamination. The FDD was measured using a Scanditronix photon diode and was normalized to a reference depth far beyond maximum range of contaminant electrons. An analysis for the 8 and 18 MV photon beams from a Varian 2100CD indicates that at a source-to-surface distance (SSD) of 100 cm, the maximum electron contaminant dose (relative to its maximum FDD) varies from 1% to 33% for 8 MV and 2% to 44% for 18 MV, for square collimator settings ranging from 5 to 40 cm (defined at 100 cm from the source). This value at a depth of maximum dose (2 cm for 8 MV and 3.5 cm for 18 MV) can reach 1% for 8 MV and 2.3% for 18 MV. This contaminant electron dose is almost independent of SSD for 8 MV and starts to fall off for 18 MV at SSDs larger than 120 cm. Compared with the open beam, the contaminant electron dose increases when a solid tray is used, and the magnitude of increase increases with field size, reaching 19% and 16% for a 40 x 40 cm2 field for 8 and 18 MV photons, respectively. The contaminant electron dose increases slightly for a blocked beam compared with an open beam of the same field size if a tray is used in both cases. The contaminant electron dose for the wedged field is less than that for an open field. However, the reduction is less significant at larger collimator settings (c = 20 cm) and may increase slightly for 8 MV photons.

Electrons↗
PubMed1998

On compensator design for photon beam intensity-modulated conformal therapy.

Recently the compensator has been shown to be an in expensive and reliable dose delivery device for photon beam intensity-modulated radiation therapy (IMRT). The goal of IMRT compensator design is to produce an optimized primary fluence profile at the patient's surface obtained from the optimization procedure. In this paper some of the problems associated with IMRT compensator design, specifically the beam perturbations caused by the compensator, are discussed. A simple formula is derived to calculate the optimal compensator thickness profile from an optimized primary fluence profile. The change of characteristics of a 6 MV beam caused by the introduction of cerrobend compensators in the beam is investigated using OMEGA Monte Carlo codes. It is found that the compensator significantly changes the energy spectrum and the mean energy of the primary photons at the patient's surface. However, beam hardening does not have as significant an effect on the percent depth dose as it does on the energy spectrum. We conclude that in most situations the beam hardening effect can be ignored during compensator design and dose calculation. The influence of the compensator on the contaminant electron buildup dose is found to be small and independent of the compensator thickness of interest. Therefore, it can be ignored in the compensator design and included as a correction into the final dose distribution. The scattered photons from the compensator are found to have no effect on the surface dose. These photons produce a uniform low fluence distribution at the patient's surface, which is independent of compensator shape. This is also true for very large fields and extremely asymmetric and nonuniform compensator thickness profiles. Compared to the primary photons, the scattered photons have much larger angular spread and similar energy spectrum at the patient's surface. These characteristics allow the compensator thickness profile and the dose distribution to be calculated from the optimized fluence profile of primary photons, without considering the scattered photons.

Calibration↗
PubMed1999

Matching photon and electron fields with dynamic intensity modulation.

A technique was developed to reduce the size and magnitude of the hot and cold spots in the abutting regions of photon and electron fields. The photon and electron fields were set up such that the photon field extended approximately 2 cm into the electron field in the abutting region. The region of the photon beam that overlapped the electron field was modulated using a multileaf collimator, effectively broadening the photon penumbra to make it complimentary to the electron penumbra. The computer calculations were verified using film measurements for abutting a 6 MV photon beam with a 9 MeV electron beam. A uniform dose was achieved at a prespecified depth of 2 cm, and dose uniformity was improved at the specified depth and beyond compared with unmodulated photon beams. A slight increase in dose inhomogeneity was seen at shallower depths. The overall areas of the hot and cold spots were significantly reduced. The technique also reduced the sensitivity of dose homogeneity to setup errors such that the magnitudes of the hot and cold spots were about half of those produced with unmodulated photon beam when an overlap or gap of 4 mm was introduced. The technique was applied to the treatment of a head and neck cancer and a lymphoma involving the right pleura with markedly reduced dose inhomogeneity in the abutting regions.

Computer Simulation↗
PubMed1993

[The mixed fractionated radiotherapy of R1H tumors in the rat using neutrons and photons].

A number of experimental investigations has demonstrated, that tumor growth delay due to a mixed fractionated treatment schedule with photons and neutrons can be prolonged compared to pure photon treatment. That question after the mechanisms remains undissolved. In the presented study of the R1H tumor of the rat 30 fractions using 2 Gy of photons in 39 days are compared to results of mixed fractionated treatment schedules with neutrons and photons. Neither a prolonged net growth delay (NGD) was found nor does the sequence in which neutrons and photons are given influence the outcome when replacing photons by neutrons in twelve of 30 fractions (RBE 2.5). In contrast, hypofractionated schedules (five fractions/total dose 40 Gy/four days) have a considerable longer NGD when replacing two fractions of photons by neutrons (RBE 2.5) (p < 0.01). This could be explained if 8 Gy photons/fraction destroyed all euoxic tumor cells, a 24 hour interval was too short for reoxygenation and thus make hypoxia to a major problem in 8 Gy/fraction photon treatment.

Animals↗
PubMed1998

Photon energy recovery: a method to improve the effective energy resolution of gamma cameras.

UNLABELLED: One of the major limitations of gamma cameras is their relatively poor energy resolution. The main practical consequence of this is that the detection of both scattered and unscattered photons in the photopeak energy window, affecting image contrast and resolution, makes the data inconsistent with the assumption of scatter-free projection data in reconstruction and attenuation correction algorithms. Here, we proposed a method to improve the effective energy resolution of scintigraphic acquisitions. This method is called photon energy recovery (PER). METHODS: Photon energy recovery is based on a spectral deconvolution analysis and uses iterative recurrent linear regressions. In practice, PER only required splitting the photopeak energy window into several subwindows and did not need list mode acquisitions. The method was fully automated. Photon energy recovery was quantitatively validated on 99mTc planar images using a Monte Carlo simulation and a real phantom and was illustrated by a bone study. RESULTS: The Monte Carlo simulation demonstrated that convergence was reached within relatively few (10-15) iterations. Photon energy recovery led to a considerable quantitative improvement because the mean error between the photopeak energy window image and the true unscattered image was equal to 8.72 s.d. (the mean error between one image and the true image was the mean of the differences between the two images; the difference is expressed as several s.d., where s.d. was the square root of the true value), whereas the mean error between the 140-keV PER image and the true unscattered image was only equal to 2.70. Moreover, the true and PER spectra were highly correlated. The real phantom data pointed out that the counts in the 140-keV PER image calculated from the images acquired "with scatter" were not very different from the true counts given by the "scatter-free" reference image. Planar pelvic bone scintigraphy demonstrated the advantages of PER because contrast increased when only unscattered photons were selected. CONCLUSION: Photon energy recovery is a stable and automated method that allows recovery of the correct value of the photon energy after a scintigraphic acquisition. Its ability to separate scattered from unscattered events has been quantitatively validated.

Algorithms↗
PubMed1996

Radiation therapy for glottic cancer using 6-MV photons.

BACKGROUND: It has been recommended that cobalt-60 or 4-MV photons be used when treating glottic cancer with radiation therapy. Underdosing may occur when using higher energy photons, particularly when the anterior commissure is involved. The authors report their experience using higher energy photons (6 MV) for the treatment of glottic cancer. METHODS: Between January 1975 and July 1991, 73 patients with Tis, T1, T2, or T3 glottic tumors underwent radiation therapy with curative intent. Cobalt-60 or 4-MV photons were used to treat the cancers of 30 patients, and 6-MV photons were used to treat 43 patients. Clinical records were reviewed retrospectively to determine patterns of treatment failure, cancer deaths, and local tumor control in the 43 patients receiving treatment with 6-MV photons. Patients were followed until death or for a minimum of two years. RESULTS: Treatment failures were: local recurrence, one patient; local recurrence and distant metastasis, one patient; delayed neck metastasis, two patients; and delayed neck metastasis with distant metastasis, one patient. Three patients who had treatment failure are alive and free of cancer after salvage treatment. Two patients died of neck and distant metastases. The 2-year initial local tumor control rate was 94.8%. CONCLUSIONS: Glottic cancer can be treated successfully with 6-MV photons. Local tumor control is similar to that reported using cobalt-60 or 4-MV photons.

Adult↗
PubMed2006

o-nitrobenzyl photolabile protecting groups with red-shifted absorption: syntheses and uncaging cross-sections for one- and two-photon excitation.

We evaluated the o-nitrobenzyl platform for designing photolabile protecting groups with red-shifted absorption that could be photolyzed upon one- and two-photon excitation. Several synthetic pathways to build different conjugated o-nitrobenzyl backbones, as well as to vary the benzylic position, are reported. Relative to the reference 4,5-dimethoxy-2-nitrobenzyl group, several o-nitrobenzyl derivatives exhibit a large and red-shifted one-photon absorption within the near-UV range. Uncaging after one-photon excitation was studied by measuring UV-visible absorption and steady-state fluorescence emission on model caged ethers and esters. In the whole series investigated, the caged substrates were released cleanly upon photolysis. Quantum yields of uncaging after one-photon absorption lie within the 0.1-1 % range. We observed that these drop as the maximum wavelength absorption of the o-nitrobenzyl protecting group is increased. A new method based on fluorescence correlation spectroscopy (FCS) after two-photon excitation was used to measure the action uncaging cross section for two-photon excitation. The series of o-nitrobenzyl caged fluorescent coumarins investigated exhibit values within the 0.1-0.01 Goeppert-Mayer (GM) range. Such results are in line with the low quantum yields of uncaging associated with cross-sections of 1-50 GM for two-photon absorption. Although the cross-sections for one- and two-photon absorption of o-nitrobenzyl photolabile protecting groups can be readily improved, we emphasize the difficulty in enlarging the corresponding action uncaging cross-sections in view of the observed trend of their quantum yield of uncaging.

Journal Article↗
PubMed1996

Multiple-Photon Dynamics in Molecules: A New Approach to High Resolution Spectroscopy of Highly Excited Vibrational States

Multi-photon transitions with two simultaneously interacting IR laser fields lead to final excited states with frequencies nnu = n1nu1 + n2nu2, with n the total number of photons absorbed and (n, n1, n2) = (2, 1, 1), (3, 2, 1), (4, 1, 3), etc. The nature of the actual transition is determined by shift measurements, where the lasers are frequency-tuned by deltanui in opposite directions keeping the sum frequency, nnu, resonant with the molecular transition. This technique opens a new spectral range for multi-photon transitions and a unique identification of the observed features. For n1 and n2 both positive the excitation will lead to a "normal" up-up multi-photon transition. Many three- and four-photon transitions in the nu3 vibrational ladder of SF6 could be resolved with a resolution of 1 MHz, as well as four new two-photon transitions. As long as n1 + n2 >/= 0, one of the two ni may be negative resulting in an, e.g., up-down excitation pathway with its particular selection rules. The up-down excitations are demonstrated both for one- and two-photon transitions using the frequency shift technique. The different possible excitation schemes which meet the resonance condition for these transitions lead to interference effects and local couplings to highly excited states. Changes in resonance frequency for a one-photon transition (n = 1), due to these effects, are demonstrated. Evidently, the radiative coupling of participating levels to high-lying or quasi-continuum states may drastically change for different deltanui leading both to ac Stark shift and transition probability variations.

Journal Article↗