United States Environmental Protection Agency Health Effects Research Laboratory Research Triangle Park NC 27711 Research and Development EPA/600/S1-87/002 Aug. 1987 Project Summary Millimeter-Wave Emissivity of Cellular Systems K. H. Illinger A general analysis is presented of the millimeter-wave and far-infrared spec- troscopic properties of in vivo cellular systems, and of the boson radiative equilibrium with steady-state nonequili- brium molecular systems. The frequency threshhold of spectroscopic properties associated with such nonequilibrium ef- fects is (roughly) estimated to be as low as ~100 GHz, if the Frbhlich vibrational model can be invoked for cellular- membrane systems. On this basis, the rationale for the specific experimental protocol employed was further to utilize the fact that in a photosynthetic pre- paration the onset and disappearance of the nonequilibrium state can be switched by modulating the optical- illumination input. The negative findings of the present V-band (50-75 GHz) radiometric study on in vivo chloralla pyrenoidosa algal cells appear to con- firm the absence of non-Planckian emissivity features in the total radio- metric study on saccharomyces cerevislae near 42 GHz (3), but does not negate totally the existence of non- equilibrium emissivity terms in the frequency range studied. Limitations of radiometer sensitivity, in spite of the S/N enhancement achieved through the AM-modulation technique, and/or damping of the non-Planckian emissivity features may have vitiated their detec- tion. More fundamentally, the frequency threshhold for such properties may indeed lie at higher frequencies, in the far-infrared region. An order of magni- tude of refinement in the theoretical models will be required to serve as a reliable guide for the prediction of such frequency threshholds. This Project Summary was developed by EPA's Health Effects Research Labo- ratory, Research Triangle Park, NC, to announce key findings of the research project that Is fully documented In a separate report of the same title (see Protect Report ordering Information at back). Discussion As a consequence of the existence of nonequilibrium thermodynamic subsys- tems in in vivo biological entities, in- cluding cellular systems, spectroscopic features may be expected to arise which differ from those exhibited by ordinary equilibrium thermodynamic systems. A detailed theoretical analysis identifies, in particular, the emissivity function as a targetable observable in this category. The emissivity function, t(w), is defined as the ratio of the aetuat emission in- tensity of the system under consideration, at a given frequency, to that of an ideal blackbody at the same temperature. The emission intensity is the photon energy emitted across a unit surface area, per unit time, into a solid angle of 2?r steradians, and is proportional to the value of the generalized distribution func- tion of photons over frequencies, n(o>), at the given frequency, characteristic of the thermodynamic system under considera- tion. If the system is an ideal blackbody, n(oj) is the Planck function and e(cu) is unity and frequency-independent. A general thermodynamic analysis shows that nonequilibrium systems should exhibit frequency-dependent fea- tures in t(tu). If the Froehlich vibrational model is applied to cellular systems and the cellular membrane is identified as the locus of nonequilibrium thermo- dynamic processes, a frequency regime as low as ~ 100 GHz is credible for the possible existence of non-Planckian fea- ------- tures. This study utilized in vivo photo- synthetic algal cells [chlorellapyrenoidosa (American Type Culture Collection, in the form of their strains ATCC 22521, 7516 and 11469)] as the experimental model system, since the photosynthetic ap- paratus is located in the cell membrane, and since photosynthetic processes lend themselves directly to external modula- tion. In consequence, the temporal onset and disappearance of these nonequili- brium processes are externally control- lable, and the opportunity is provided to improve the S/N ratio of measurements of the contribution of the nonequilibrium subsystem(s) to the total emissivity func- tion, the preponderant portion of which arises from the Planckian background from the remainder of the system. Millimeter-wave radiometry systems usually operate within the frequency regions encompassed by individual wavequide systems. This study employed V-band [WR-15], 50-75 GHz, to roughly approximate the frequency domain charted in the application of the Froehlich model to the photosynthetic chloroplast. The latter consists of a flat, double- membraned configuration, with a mem- brane thickness between 100-200 A, the site of the photosynthetic apparatus and the putative locus of longitudinal vibra- tions invoked in the model. A serious caveat in any generalization that might be made from the results of this type of study arises from the combination of the crudeness of the frequency-range esti- mate from theory and the inherent nar- row-bandedness of microwave and millimeter-wave waveguide systems. The emissivity of the cellular prepa- ration was measured using a 50-75 GHz radiometer, with its detection circuit phase-locked to the optical illumination of the sample in the wavelength range centered at 4900 A (±350 A), AM- modulated by a precision optical chopper at 100 Hz, to accomodate the response time constant of the photosynthetic ap- paratus of the preparation, and to provide selectivity and S/N ratio enhancement of the radiometer signal arising from pro- cesses associated with the photosynthetic apparatus. The source of the optical illumination was a 1000W Xe lamp, fol- lowed by standard components of an optical train, including a (distilled-H20) broadband infrared filter and optical filters selected to tailor the illumination to the wavelength response function of the cellular preparation. Millimeter-wave emission from the sample was measured at an angle of 90° to the optical-illumina- tion axis, with the cell preparation con- tained in a quartz cuvette, transparent to both visible light and millimeter-wave emission. In the context of the present experiments, the task of the radiometer was to detect any response, phase-locked to the optical illumination, within a primary-illumination ra nge of 200-1OOOW total (regulated and calibrated) power, of the cell preparation. The local-oscillator (LO) arm of the radiometer originated in a set of three klystron oscillators spanning the 50-75 GHz range, and was coupled to the sample arm and the detection-system arm via broadband (50-75 GHz) ferrite isolators. The frequency axis of the radiometer signal was provided by measurement of the LO frequency by means of a mil- limeter-wave electronic counter and sub- sequent conversion of its frequency output via a digital/analog (D/A) con- verter to a voltage analog signal to com- prise the Y-axis of an X/Y recorder output. Under typical experimental conditions, frequency resolution thus obtained is equal to or better than 0.1 MHz, over the entire V-band frequency range, and frequency tracking of the LO is automatic. A separate power-measurement loop permits determination of the LO relative power across a given klystron mode, as a function of LO frequency. The primary element of the radiometer detection system is a broadband (50-75 GHz) harmonic mixer matched to an inter- mediate-frequency (IF) amplifier, the latter rejecting IF signals below ~ 500 MHz and above ~ 1500 MHz. Electronic tuning of the LO, by means of its reflector voltage, moves the center of this IF detec- tion window (bandwidth ~ 1000 MHz) across the klystron mode. Director moni- toring of radiometer performance is ac- complished by feeding the output of the IF amplifier directly into a (0-2 GHz) spectrum analyzer. Radiometry of the sample preparation is achieved by entering the output of the IF amplifier into a microwave video detector, thus, converting that output into a dc voltage. The phase-lock synchronization loop, externally synchronized to the precision optical chopper, is engaged via a phase- sensitive lock-in amplifier which accepts the dc radiometer-output signal. Finally, the radiometer-signal axis, from the out- put of the lock-in amplifier, is combined with the frequency axis, from the elec- tronic counter and D/A converter, to present the radiometry data on an X/Y recorder. The present study failed to detect any (non-artifactual) frequency-dependent features m the radiometry signal phase- locked to the optical illumination of th« photosynthetic algal-cell preparation Among the possible explanations for sucf a finding, two are salient. The centra modality of the radiometer experimen (direct AM-modulation of the photosyn thetic process) may have been vitiated b> insufficiently favorable S/N ratio char acteristics of any non-Planckian features in the emissivity. This would render the sensitivity of the current radiometei design incapable of detecting such fea- tures, in a manner which excludes arti- facts of millimeter-wave waveguide circuits. From a mechanistic standpoint, any of three (heuristic) parameters ma\ have contributed to such a possibility, (a the low concentration of subsystems which undergo nonequilibrium processes, per unit volume, compared to the (bulk; system near equilibrium; (b) low absolute emission intensity associated with any non-Planckian features; and/or (c) damping of any non-Planckian emissivity features, with an attendant reduction in S/N ratio, within a given frequency interval. The second case arises from the central question, to which existing theory is only a very rough guide, concerning the low- frequency threshhold, w,, of non- Planckian features. If (n 01,/«T) -4 1 is inadmissible as an assumption for cellular systems, no non-Planckian features are expected in the frequency range studied, with Ts300°K, and their absence in the present study is not inconsistent with the thermodynamic or the generalized Froeh- lich model, but would imply that definitive refinement in the theory is required for the prediction of their (frequency) range of existence. ------- K. H. Illinger is with Tufts University. Medford, MA 02155. Jamas R. Rabinowitz is the EPA Project Officer (see below). The complete report, entitled "Millimeter- Wave Emissivity of Cellular Systems," (Order No. PB 87-175 840; Cost: $ 11.95, subject to change) will be available only from: National Technical Information Service 5285 Port Royal Road Springfield, VA 22161 Telephone: 703-487-4650 The EPA Project Officer can be contacted at: Health Effects Research Laboratory U.S. Environmental Protection Agency Research Triangle Park, NC 27711 United States Environmental Protection Agency Center for Environmental Research Information Cincinnati OH 45268 ; : 0 2 1.: Official Business Penalty for Private Use $300 EPA/600/S1-87/002 0000329 PS U $ ENVIR PROTECTION AGENCY REGION 5 LIBRARY 230 $ DEARBORM STREET CHICAGO IL 60604 ------- |