Journal of Photochemistry Photobiology B:Biology and www.elsevier.hi/ locate/jphotobiol ELSEVIER J. Photochem.Photobiol.B: Biol. 50 (1999) 149-158 Effects of changes of irradiance on the pigment composition of Gracilaria tenuistipitata var. liui Zhang et Xia E. Carnicas *, C. Jim6nez, F.X. Niell Department of Ecology, Faculty of Sciences, Universityof Mdlaga, E-29071 Malaga, Spain Received 2 February 1999; accepted 5 July 1999 Abstract In plants, excess irradiation can damage the photosynthetic apparatus, although some protective mechanisms exist. The excess energy can be dissipated as thermal energy, and pigments (i.e., carotenoids) also play an important role in protecting the photosynthetic apparatus by epoxidating reactions. Chromatographic analysis of pigment extracts of Gracilaria tenuistipitata shows that zeaxanthin is the major carotenoid in this alga, accounting for up to 82% of total carotenoids. Short-term (55 h) and long-term (10 days) response of the pigments shows that Chl a, 13-carotene and zeaxanthin degradation after light increase follows negative exponential trends, while the response of biliproteins is almost linear. Decreasing the irradiance results in a clear saturating response of the synthesis of Chl a and 13-carotene after one to two days. Biliprotein synthesis displays a double linear trend, the first one lasting for four days in the cases of both R-phycoerythrin (RPE) and Rphycocyanin (RPC). The response of zeaxanthin is always faster than that of Chl a or biliproteins to changes of irradiance. Our results might indicate the presence of two pools of zeaxanthin in this alga, with different acclimation responses to the changes in the photon flux density. © 1999 Elsevier Science S.A. All rights reserved. Keywords: Gracilaria tenuistipitata; Xantophyllcycle; Zeaxanthin; Pigmentcontent; HPLC 1. Introduc~on Light is the essential energy source for photosynthesis. Photosynthetic organisms are capable of operating a lightabsorbing pigment system over a wide range of photon flux densities (PFDs). However, excess solar energy can lead to photodestruction of the photosynthetic apparatus [ 1-3]. Irradiance levels are very high in some latitudes, reaching values around 2500 p~mol m -2 s -1 in the tropics. Typical sun algae become photosynthetically light-saturated at photon fluence rates around 500 p,mol m - 2 s - t and shade algae at 60-150 pLmol m - 2 s - ~ [4]. Algae, like higher plants, have developed mechanisms to adapt to excess sunlight, Macrophytes, in contrast to phytoplankton which are free to move vertically, are restricted to their site of growth and survive by developing internal mechanisms that increase the dissipation of excitation energy through non-photosynthetic metabolism. Therefore, components of the photosynthetic system of the chloroplast involved in light absorption, electron transport and carbon fixation undergo acclimation to the level of irradiance [5,6]. When an excess of light reaches the photosyn* Corresponding author. Tel.: + 34-952-131844; Fax: + 34-952-132000; E-mail: mecarnicas@uma.es thetic apparatus, an increased proportion of absorbed quanta is dissipated as thermal energy [7]. The irradiance level also has a pronounced effect on algal pigment composition. The chlorophylls do most of the light harvesting, whereas carotenoids play two important roles, one as light-harvesting pigments and another in protecting the photosynthetic apparatus against excess irradiance through epoxidating reactions [ 8-10]. Two main xanthophyll cycles have been described, acting as photoprotective mechanisms of the photosynthetic apparatus. The first one, called the 'violaxanthin cycle', has been reported in higher plants, green algae and in some brown algae. Under excess light, violaxanthin de-epoxidates through the intermediate antheraxanthin to form zeaxanthin [ 11 ]. Conversely, the action of an epoxidase transforms zeaxanthin to violaxanthin, via anteraxanthin. The 'diadinoxanthin cycle' is found in diatoms [ 12] and it involves similar reactions. Under high irradiance, diadinoxanthin de-epoxidates to diatoxanthin. In both cycles, the reverse epoxidating reactions occur under low irradiance. A third xanthophyll cycle, which involves the xanthophylls lutein and taraxanthin (5,6 diepoxilutein), has been described in Dunaliella tertiolecta [ 13]. Up to the present, no xanthophyU cycles have been described in red algae. In addition to this photoprotective function, in some marine organisms 1011-1344/99/$ - see front matter © 1999 Elsevier Science S.A. All rights reserved. PIISIO1 1-1344(99)00086-X 150 E. Carnicas et al. / J. Photochem. Photobiol. B: Biol. 50 (1999) 149-158 carotenoids also contribute significantly to light harvesting [141. Changes in pigment composition and in the different components of the xanthophyll cycle under luminous stress have been widely studied in higher plants [ 15-18 ] and green algae [8,19]. In contrast, the effects of irradiance on the concentration of Chl a and phycobiliproteins in red algae have been studied by several authors [20--231, but less work has been done concerning the xanthophyll composition and the change in carotenoid concentration under different irradiances [ 9]. In this study we analyse the pigment composition of a Rhodophyta, Gracilaria tenuistipitata, when thalli are submitted to drastic changes of the irradiance level. To perform the experiments, G. tenuistipitata was kept in a controlled system in which light was the only variable that was modified. The pigment response dynamic to light intensity is presumed to be vary with time, e.g., it has been demonstrated to be very fluctuating in the first hours in other red algae [21,23]. So, the acclimation of G. tenuistipitata to a luminous change was studied in short-term (55 h) and long-term ( 11 days) experiments. A detailed analysis of carotenoid composition was made in order to establish the xanthophyll composition of this rhodophyta, as well as the possible photoprotective mechanisms when the plants were exposed to excess light. 60 A 0 350 -~ 400 i 450 t 500 550 Wavelength t 600 r 650 i 700 i 750 (nm) Fig. 1. Spectrumof the halogenlamp used as a light sourcein the two sets of experiments. and once a day for 10 days after the starting day in the longterm acclimation experiments. In the second set of experiments, the light treatment was the reverse. The algae were kept at a relatively high irradiance (500 ixmol m -2 s- l) for one month and then were exposed to 40 ixmol m -2 s -1 for 55 h or for i0 days, following the same sampling strategy as in the experiment above. Experiments were repeated several times; samples were taken in triplicate. 2.3. Pigment analysis 2. Materials and methods 2.1. Organism and culture conditions G. tenuistipitata Zhang et Xia (1983) [24] was obtained from the Institute of Plant Physiology of the University of Uppsala (Sweden). The algae were cultivated in 41 cylinders at a temperature of 25°C and a plant density of 3 g 1-1. The culture medium consisted of filtered natural sea water (Whatman GF/F), enriched with Provasoli's solution [25]. The final concentrations of nitrate and phosphate were 820 and 30 IxM, respectively. It was renewed every three days and the cultures were bubbled with air at a rate of 4.4 1 min -1 [2628 ]. White light was continuously provided by halogen lamps (Mazda MAIH/400 W) (see spectrum in Fig. 1). 2.2. Experimental design Two sets of experiments were performed for the description of the acclimation of the photosynthetic pigments of G. tenuistipitata to short-term (55 h) and long-term ( 10 days) changes of the PFD. In the first one, the algae were grown at a PFD of 40 ixmol m-2 s - 1 for one month to acclimate to low irradiance. After this period, the plants were suddenly transferred to a higher PFD (500 Ixmol m -2 s - l) for 55 h or 10 days and the pigment composition ofG. tenuistipitata was analysed. Samples were taken three times a day during the first three days after the change of irradiance in the 55 h experiments (starting time, 4, 7, 24, 28, 31, 48, 52 and 55 h) The pigment composition of G. tenuistipitata was determined using two different techniques: spectrophotometry to obtain a fast although coarse result and high-performance liquid chromatography (HPLC) to obtain more accurate results. Whole plants were randomly taken from the cultures and water was removed to avoid a progressive reduction in plant density during the experiments. The extraction of hydrosoluble pigments (R-phycoerythrin, RPE, and R-phycocyanin, RPC) was performed by grinding the plants (50 mg fresh weight (FW)) in phosphate buffer (0.1 M, pH 6.5) at 4°C. After 12 h, the extracts were centrifuged for 15 min at 19 000g at 4°C (Heraeus 17-SB) and the supernatant was used to determine the phycobiliprotein concentration, according to Ref. [29]. In order to determine the concentration of liposoluble pigments, samples of around 100 mg FW were extracted in 4 ml dimethylformamide (DMF) and kept overnight at 4°C. This method avoids grinding the plants and has previously been used efficiently in algae [30] and higher plants [31]. Pigments were then transferred to a more volatile solvent by adding 2 ml of diethylether and 2 ml of bidistilled water to the extracts. A short centrifugation pulse of 1 min at 1000g was given after sample mixing and the diethylether phase containing the pigments was transferred to a 2 ml glass container and kept at - 2 0 ° C until HPLC analysis (less than one week). If the DMF/water fraction was still coloured, the process was repeated until it became totally transparent. Before injection in the chromatograph, the diethylether was evaporated under a nitrogen flow and pigments were finally resuspended in 20 Ixl of terbutylmethylether. E. Carnicas et al. / J. Photochem. Photobiol. B: Biol. 50 (1999) 149-158 A Hewlett-Packard HP-1090 system equipped with a reverse-phase VYDAC 201TP54 C-18 column (25 cm × 4.6 mm, 5 Ixm particle size) was used. Elution was performed in a two-solvent gradient system. The solvents were a mixture of acetonitrile (75%), methanol (15%) and tetrahydrofuran (10%) (solvent A) and 100% bidistilled water (solvent B). The gradient system was as follows: initial 80% A + 20% B; 0-30 min linear gradient to 100% A; 30-40 min isocratic 100% A; 40-50 min linear gradient to 80% A + 2 0 % B; 5060 min isocratic 80% A + 20% B for column stabilization before next injection, at a flow of 1.0 ml m i n - 1. A programmable photodiode array detector was used for pigment detection, at 445 and 412 nm. Identification of chromatographic peaks was carried out by injection of commercial standards (Sigma, St Louis); zeaxanthin was kindly provided by Dr Olimpio Montero (Instituto de Ciencias Marinas de Andaluc{a, Puerto Real, C{tdiz) and by comparison with several spectral and chromatographic characteristics reported in the literature [32]. As the relationship between fresh and dry weight may vary at different irradiances, pigment content was expressed on a dry weight basis. 2.4. Statistics Experiments were repeated several times, and samples for HPLC were analysed in triplicate in each experiment. Results presented here correspond to one representative experiment for each of the treatments. Two different statistical tests were employed. A Student's t test was used to establish significant differences between initial and final pigment concentrations. An ANOVA was performed to determine the significance of the changes in the pigment concentration of G. tenuistipitata during the experiments [33]. 3. Results G. tenuistipitata, like all the Rhodophyta, contains Chi a, and carotenoids and phycobiliproteins (RPE and RPC) as major accessory pigments. Fig. 2 shows the chromatograms of plants acclimated to PFDs of 40 and 500 I~mol m - 2 s - 1. Four main liposoluble pigments were identified: Chl a, 13carotene ([3-CT), zeaxanthin (Z) and lutein (L), but neither violaxanthin nor anteraxanthin. The percentage zeaxanthin concentration (on a total carotenoid basis) represented 76.7 and 75.7% at 40 and 500 ixmol m -2 s - 1 respectively, and it did not vary significantly among the plants acclimated to low and high irradiance. In the first set of experiments, the change in the pigment composition of G. tenuistipitata was followed after an increase of the PFD from 40 up to 500 ixmol m - 2 s - 1. When plants that were acclimated to 40 Ixmol m -2 s-~ were exposed to a higher irradiance for 55 h, the concentration of all pigments decreased markedly (Fig. 3). Chl a concentration decreased from an initial value of 5.26 mg g - 1dry weight 151 (DW) to a final value of 2.94 mg g - 1 DW (Fig. 3 (A) ); this decrease fitted a negative logarithmic function (r 2= 0.92). [3-Carotene decreased in a similar way, from 0.12 to 0.05 mg g - 1DW (Fig. 3 ( B ) ) (r 2 = 0.94 ). The long-term acclimation of G. tenuistipitata after the increase in irradiance was also studied (Fig. 4). When the algae were exposed to 500 ~mol m - 2 S- 1 for 10 days, the concentration of Chl a decreased from 5.71 to 2.63 mg g - 1 DW and the logarithmic trend of the decay was maintained during the whole period (Fig. 4 ( A ) ) . The results obtained for 13-carotene were different (Fig. 4 ( B ) ) . As described above, its concentration decreased during the first 55 h but it increased sharply to the initial value during the third day. Then it decayed continuously during the rest of the experiment, reaching a final value of 0.047 mg g - 1 DW. Two main xanthophyUs were identified in G. tenuistipitata, zeaxanthin and lutein (Fig. 2). Zeaxanthin was found to be the major carotenoid in G. tenuistipitata, with concentrations four to six times higher than that of lutein and three to five times higher than 13-carotene. The changes of the two xanthophylls were markedly different from the logarithmic trends described for Chl a and 13-carotene (Fig. 3(C), ( D ) ) . Zeaxanthin concentration (Fig. 3 ( C ) ) decreased sharply during the first 7 h of exposure to 500 Ixmol m - 2 s - ~. During this time, its concentration dropped to half of the initial value (0.45 to 0.22 mg g - 1 D W ) . Then, it fluctuated between 0.22 and 0.30 mg g - ~DW. The concentration of zeaxanthin over 10 days behaved in a similar way to that of [3-carotene (Fig. 4(C). It decreased during the first two days from an initial value of 0.62 to 0.53 mg g - 1 D W , increasing sharply on day three to a value of 0.68 mg g-~ DW and finally decaying during the rest of the experiment, reaching a final value of 0.45 mg g - 1 DW. The change in lutein concentration (Fig. 3 ( D ) ) was very irregular during the first 55 h the plants were exposed to high irradiance. Its concentration decreased sharply in 7 h, from an initial value of 0.08 mg g - 1 DW to a value of 0.042 mg g-- 1 D W , and it continued decreasing to a minimum of 0.035 mg g-1 DW after 24 h. Then it rose to 0.07 mg g-1 DW, with a final decay to the end of the experiments (0.05 mg g - ~ DW). Changes of the lutein content over 10 days were also significant (Fig. 4(D) ), with an initiai decay from 0.08 to 0.043 mg g - 1 DW during the first three days, followed by daily fluctuations ranging between 0.03 and 0.05 mg g-1 DW. G. tenuistipitata contains both RPE and RPC as accessory light-harvesting pigments. The RPE concentration was 2.52.6 times higher than that of RPC. Both pigments decreased when plants acclimated to 40 txmol m - 2 s - 1 were exposed to 500 ixmol m - 2 s - 1. The RPE concentration decreased from an initial value of 22.05 to 13.96 mg g-~ DW at the end of the experiment (55 h) (Fig. 3 ( E ) ) . The experimental results were also fitted to a negative logarithmic curve (r2=0.92). In contrast, the RPC concentration decreased from 8.84 to 5.89 mg g - 1 DW following a linear behaviour (Fig. 3 ( F ) ) . Changes in the concentration of phycobilipro- 152 E. Carnicas et al. / J. Photochem. Photobiol. B: Biol. 50 (1999) 149-158 ]SO0- A 4 3" 1100 - v TN- ,,R 3 n.i, -IN I S I I J0 I 1S Z0 1 2$ 1 30 I 35 i ~0 I 4S I SO I SS I 60 Time (min) l|oo* B IN- ~D So0. ..B. Z00. 3 n.i. -100 1 i | r I I I f I I I I I 5 10 J$ 20 2S 30 3S qO 4S SO 5S 60 Time (min) Fig. 2. HPLC chromatograms of G. tenuistipitata cultured at two irradiances, 40 ixmol m 2 s - 1 (A) and 500 ~mol m -2 s - t (B). The following pigments were identified: lutein (peak 1 ), zeaxanthin (peak 2), Chl a (peaks 3, 3' and 3") and 13-carotene (peak 4), n.J. not identified. E. Carnicas et al. / J. Photochem. Photobiol. B: Biol. 50 (1999) 149-158 153 0.13~ 0.11- 5 ~ 0.08m u ~ 0.06J . 2 8 10 20 3'0 4'0 5'0 Time (hours) 0"71 i 0.04 6O o 1'o 2~0 3'0 4~0 5'0 0'0 5~0 8'0 Time (hours) 0.09" C ~ 0.07. ~ O. 5 .,~ ,u o . o s - 0.4 i 8.3 ~ 0.03- o.2 0.1 ~ 0 10 20 30 40 Time (hours) 50 35- 1'0 2'0 3~0 4]0 Time (hours) lit 30- ~ 25'7~o ~u 20- 10- 5 0.01 60 F 4- 1'0 2'0 3'0 4'0 5'0 6'0 Time (hourS) 2 0 i 10 i 20 i 30 i 40 i 50 6'0 Time (hours) Fig. 3. Changes in pigment concentrations (rag g - ~ DW) of G. tenuistipitata when plants acclimated to low irradiance (40 I~mol m -2 s - l ) were exposed for 55 h to 500 is.rnol m - 2 s - ]. The extracts were analysed using HPLC and mean values with their standard deviation are shown (n = 34). teins were also studied over 10 days after increasing the irradiance level. RPE decreased from an initial value of 32.67 mg g - ] DW to a final value of 7.92 mg g - ~ DW, while the RPC concentration decayed from 11.3 to 2.79 mg g - 1 DW (Fig. 4(E), ( F ) ) . Both responses followed clear negative logarithmic patterns. In the second set of experiments, cultures of G. tenuistipitata that were acclimated to high irradiance (500 Ixmol m - 2 s -~) were transferred to a lower one (40 p~mol m -2 s - ] ) during the same time periods as above, 55 h and 10 days. As expected, the concentrations of all pigments increased during the experiments. The concentration of Chl a (Fig. 5 ( A ) ) rose from 1.62 to 2.87 mg g - ~ DW after 55 h of exposure. When the experiments were extended over 10 days, the concentration of Chl a continued to increase, reaching a final concentration of 3.62 mg g-1 DW. Changes in 13-carotene concentration are shown in Fig. 5 (B). The initial concentration (0.034 mg g-~ DW) increased to a value of 0.072 mg g - ] DW after 55 h. In contrast to Chl a, the I~-carotene concentration did not significantly vary from day three to the end of the experiment. Both Chl a and 13-carotene concentrations increased following a logarithmic pattern over the 10 days (r 2 = 0.72 and r 2 = 0.75, respectively). In plants acclimated to high irradiance, the concentration of zeaxanthin was around six to eight times higher than that of lutein and five to six times higher than that of 13-carotene. The change in zeaxanthin and lutein concentrations is shown in Fig. 5(C, D). When plants acclimated to high irradiance were exposed to a lower photon flux density for 55 h, the zeaxanthin content increased from an initial value of 0.21 mg g - ] DW to a final value of 0.35 mg g - 1DW with a maximum of 0.45 mg g - ] DW after 24 h. The lutein concentration increased in a similar way, from 0.035 to 0.049 mg g - 1DW, showing a peak of 0.055 mg g - ~ DW, also after 24 h. This behaviour totally changed when exposure to 40 Ixmol m - a s - t was extended for 10 days. The concentration of both xanthophylls fluctuated widely and the final zeaxanthin content was not significantly different from the initial value (0.27 mg g-1 DW), while lutein increased to a final value of 0.054 mg g - 1 DW. The change in the concentration of RPE and RPC is shown in Fig. 5(E, F). The concentration of both pigments continuously increased after the shift, although they did it in a different way from the rest of the pigments. The amount of RPE (Fig. 5 ( E ) ) rose from an initial value of 5.41 mg g - i DW to a value of 10.5 mg g - 1 DW in 55 h, while the con- E. Carnicas et al. / J. Photochem. Photobiol. B: Biol. 50 (1999) 149-158 154 0.14- A B ~ 0.12~ a 0.1- ~ 0.08- ~ ;--'L'.--,a~..~_l ~ 0.060.04 Time (days) Time (days) 0.7- 0.09- 0.60.07- 0.5- ~ 0.2 0.40.3- ~ o.o3. 0.20.1 0.01 0 Time (days) ~ ~ ~' i'o ~ d d lb Time (days) 35- 14. E 30- 12- 25- \ ~ 10- ~ 6- 2015105 4 6I Time (days) 8' 1; 2 Time (days) Fig. 4. Changes in the concentrations ( m g g - 1 D W ) of pigments when plants grown at 40 ~ m o l m -2 s - 1 were exposed to 500 Ixmol m -2 s - ] for 10 days. Mean values with their standard deviations are shown (n = 22). centration of RPC increased from 2.1 to 3.2 mg g-~ DW (Fig. 5 ( F ) ) . In both cases, the upward trend was linear, in contrast to the logarithmic trend of the liposoluble pigments. The ratio between these two pigments was similar to that obtained in the experiment described above (2.5-2.8). Longer exposure to low irradiance ( 10 days) induced a further linear increase of the concentration of phycobiliproteins, but at a lower rate. Table 1 shows the changes in the proportions of pigments (final concentration/initial concentration) at different times when the incident PFD was changed from 500 to 40 ixmol m -2 s - ~ and vice versa over 10 days. The ratio between the final and the initial concentrations of zeaxanthin and Chl a increased to 1.62 and 1.41, respectively, in 4 h, while that of RPE and RPC increased only to 1.22 and 1.19, respectively. When the experiments were extended to 10 days, it was found that Chl a was the pigment that underwent the widest range of variation, either when increasing or decreasing the irradiance. The ratio Chl a f / C h l a i rose to 3.22 when the irradiance was decreased, and dropped to 0.24 when it was increased. On the contrary, the variation of the zeaxanthin concentration was narrow, increasing to 1.25 after 10 days in low PFD and decreasing only to 0.72 after the same period in high PFD. It is also seen that while the phycobiliprotein and Chl a content increased gradually over the 10 days when the light level was reduced from 500 to 40 lxmol m - 2 s - l, the concentration of zeaxanthin increased sharply during the first hours and then decayed to the end of the experiments. A similar behaviour occurred when the irradiance was increased: the zeaxanthin concentration dropped sharply during the first 4 h, while the Chl a and phycobiliprotein concentrations decreased gradually. When algae were acclimated to low irradiance, the ratio between the phycobiliproteins ( R P E + R P C ) and Chl a (Table 2) was higher (7.7) than when the algae were grown at high irradiance (4.77). The ratio ( R P E + R P C ) / C h l a significantly decreased when the irradiance was increased from 40 to 500 ~mol m - 2 s-~, after an initial increase on day one. On the contrary, when the irradiance was decreased from 500 to 40 ~mol m -2 s -1, the ratio (RPE + RPC)/Chl a increased; nevertheless, an initial drop of this ratio was detected on the first day. 155 E. Carnicas et al. /J. Photochera. Photobiol. B: Biol. 50 (1999) 149-158 A 4.5- 0.11- B 43.53- el 0.0,. ................ ,u ~ 0.05- 2.52- 0.03 1.5 8 Time (days) 1'0 Time (days) 0.7- C 0.09- D 0.6~ 0.07' ~ 0.5- •~ 0.05- 0.4- o.a~0.03~0.20.1 ~ ~ ~; 1'o 0.01 Time (days) Time (days) 18- E • 7- 16~ 14~ ~ 12- 5- ~ 10~ 03- 6 j 4 F ~ ~ Time (days) Time (days) ~ 1'o Fig. 5. Increase of the pigment concentrations (mg g- 1 DW) after a decrease of the photon flux density of growth of G. tenuistipitata from 500 to 40 p,mol m- 2 s- t for 10 days. Samples were taken three times a day during the first three days ( days 0 to 2 ) and then once a day up to the 10th day ( n = 34). Table 1 Final concentration/initial concentration ratios of the main pigments of G. tenuistipitata, Chl a, zeaxanthin and the phycobiliproteins RPE and RPC, when the algae are exposed to a change of the irradiance level for 10 days Time (days) Chl af/Chl a i RPEf/RPE i RPCf/RPC i Decrease of irradiance from 500 to 40 ltmol m -2 s- t 0 1.0 1.0 1.0 0.17 1.41 1.22 1.19 1 1.84 1.48 1.25 2 1.97 1.84 1.7 2.3 1.77 1.94 1.54 4 2.43 2.11 1.66 7 2.77 2.27 2.12 Increase of irradiance from 40 to 500 p,mol m- 2 S--I 0 1.0 1.0 1.0 0.17 0.71 0.75 0.88 1 0.62 0.71 0.77 2 0.51 0.62 0.68 2.3 0.61 0.63 0.66 4 0.46 0.49 0.62 7 0.31 0.32 0.5 10 0.24 0.24 0.46 Zf/Z_q 1.0 1.62 1.9 1.86 1.62 1.49 1.06 1.0 0.61 0.65 0.7 0.63 0.84 0.76 0.72 4. D i s c u s s i o n T h e p i g m e n t c o m p o s i t i o n o f red algae shows s o m e differences related to other plants; the light-harvesting antennae consist o f large extrinsic protein c o m p l e x e s , the phycobilisomes, w h i c h are attached to the thylakoid m e m b r a n e s . In addition to this, only the p r e s e n c e o f chlorophyll a has b e e n clearly demonstrated as a chlorophyllic p i g m e n t [ 32]. All o f the c h l o r o p h y l l a and m o s t carotenoids are attached to a f e w specific proteins. 13-Carotene is active in p h o t o s y s t e m I ( P S I ) , and probably in P S I I too [ 3 4 ] , and the presence o f a variable n u m b e r o f other carotenoids has b e e n described in red algae ( m a i n l y lutein, zeaxanthin, 13-cryptoxanthin and anteraxanthin), although their contribution to photosynthesis is not yet clear [ 3 5 ] . The c h r o m a t o g r a p h i c analysis o f p i g m e n t extracts f r o m G. t e n u i s t i p i t a t a shows a particular p i g m e n t c o m p o s i t i o n in w h i c h zeaxanthin and c h l o r o p h y l l a, along with R P E and R P C , are the m o s t abundant p i g m e n t s at both l o w and high irradiance. In fact, zeaxanthin concentrations are m u c h h i g h e r than those o f lutein or 13-carotene ( a p p r o x i m a t e d l y 75% o f 156 E. Carnicas et al. / J. Photochem. Photobiol. B: Biol. 50 (1999) 149-158 Table 2 Change in the accessory pigments (RPE and RPC)/Chl a ratios and in the percentage of zeaxanthin (on a zeaxanthin + lutein + [3-carotene basis) after a shift of irradiance. Standard deviations in brackets Time (days) 0 1 2 4 7 10 500 to 40 tzmol m -2 s - i 40 to 500 i~mol m -2 s -I (RPE + RPC)/Chl a %Z 7.77 8.04 6.98 5.84 4.75 4.07 76.7 77.9 80.4 81.7 82.4 82.1 (1.48) (0.7) (0.19) (0.3) (0.05) (0.16) total carotenoids). Thus, no components of the 'xanthophyll cycle' have been detected and zeaxanthin is the main carotenoid of G. tenuistipitata and not lutein or [3-carotene, as described in higher plants and other algae [ 32]. Several studies in higher plants point out the photoprotective role of the xanthophyll zeaxanthin, which is related to detoxification processes when plants are exposed to excess irradiation [3,11 ]. This photoprotective role of zeaxanthin via the 'xanthophyll cycle' has also been reported in macroand microalgae [8-10]. Under photoinhibiting irradiance, violaxanthin is converted to zeaxanthin via anteraxanthin, and zeaxanthin dissipates part of the absorbed energy via non-photochemical quenching of the light-harvesting complexes. In G. tenuistipitata zeaxanthin is the major carotenoid, but neither anteraxanthin nor violaxanthin has been found, indicating that the violaxanthin-anteraxanthin-zeaxanthin cycle is not operative in this Rhodophyta. Lutein has been found, but its concentration is very small compared with that of zeaxanthin. The first pigment to respond to a change of PFD is zeaxanthin. Its concentration increases or decreases proportionately more than the other pigments when light is reduced or increased, respectively, in a short period of time (4 h) (Table 1 ). The change of zeaxanthin concentration follows a similar pattern to the other liposoluble pigments in the short-term experiments, but when they were prolonged to 10 days, the results were different. When the irradiance level was lowered (500 to 40 ixmol m - 2 s - l ) the zeaxanthin concentration increased first and then decreased up to the end of the experiments, reaching similar values to the initial ones. In contrast, when plants were shifted to a higher irradiance, the zeaxanthin concentration decreased sharply in 24 h, then increased and finally reached values slightly lower than the initial ones. These two responses lead us to consider the possible presence of two pools of zeaxanthin, one acting as an accessory lightharvesting pigment and the other acting as a photoprotective pool. In groups that lack the xanthophyll cycle, e.g., cyanobacteria, the putative photoprotective function of zeaxanthin is not convincing [ 36] and zeaxanthin may still act as a lightharvesting pigment, transferring energy from its higherenergy excited state to chlorophyll a [37]. When the light irradiance is reduced, the zeaxanthin concentration increases first, indicating an adaptation of the photosynthetic apparatus (7%) (7%) (3.8%) (3.8%) (4%) (3.9%) ( R P E + RPC)/Chl a %Z 4.77 3.88 4.23 6.72 5.89 6.42 75.7 76.3 74.6 71.7 62.8 67.8 (0.28) (0.24) (0.26) (0.49) (0.84) (0.05) (2.5%) (9.6%) (3.8%) (13%) (9%) (18.2%) to low light. Then its concentration decreases, probably due to destruction of the photoprotective pool. In contrast, when light is increased, the zeaxanthin concentration falls rapidly as a result of an acclimative response of the light-harvesting pool. The sharp increase on day three may be due to an increase of the photoprotective pool as an acclimation to high irradiance. According to these results, the acclimative response of the light-harvesting zeaxanthin pool is faster than the response of the photoprotective pool. In spite of these changes, the amount of zeaxanthin did not vary much during the two sets of experiments performed (Table 2), indicating that the main changes of its concentration took place in a short period of time and that zeaxanthin would undergo a subsequent equilibrium. The probability of a harvesting role for zeaxanthin is very small and it is not generally accepted in the literature, although we think that it cannot be totally excluded in G. tenuistipitata, as zeaxanthin is the major carotenoid. However, further research on the photochemistry of zeaxanthin in this alga should be done before assuring the two proposed roles. After a decrease of PFD, the concentrations of all pigments increase in a logarithmic way except for the phycobiliproteins, which increase linearly. Chlorophyll a and carotenoids are closely related to the reaction centre and physically bound to the thylakoid membranes. The rise in the concentration of these pigments is limited by the free space in the membranes and, therefore, the kinetics is a saturation curve. In contrast, phycobilisomes are structures that are asociated with PSII and located on the thylakoid membranes. The phycobiliprotein localization does not depend on the strict spatial availability in the thylakoid membranes, as they form prominent structures, being the possible cause for these linear responses. The first response to a decrease of the irradiance is a rise in the concentration of pigments [ 20,21,38 ]. But this increase is not equal for all the pigments: accessory pigments increase faster than Chl a [39,40]. The Z/Chl a ratio over 10 days is presented in Fig. 6. When G. tenuistipitata was grown at high PFD (500 txmol m -2 s -1) and shifted to a lower one (40 Ixmol m -2 s - 1) for 10 days, the ratio Z/Chl a increased first and then decayed and reached a similar value to the initial one in two days. When the experiment was prolonged for 10 days, the ratio Z/Chl a continued to decay up to the end of the experiment. On the contrary, when the irradiance level E. Carnicas et al. / J. Photochem. Photobiol. B: BioL 50 (1999) 149-158 • fl Decrease of irradiance from 500 to 40 p.moles m "2 s "1 Increase of irradiance from 40 to 500 ~moles m "2 s "1 0.25,I 0.20.150.1- o os- Time (days) Fig. 6. Variation of the zeaxanthin/Chl a ratio following either an increase or a decrease of the photon flux density. was increased from 40 to 500 ixmol m -2 s-1, the Z/Chl a ratio decayed first and then increased progressively during the first two days. When the exposure to high PFD was extended, the Z/Chl a ratio showed a clear upward trend. Two hypotheses have been proposed to explain the changes of pigment proportions when plants are exposed to decreasing irradiance. One of them has been described in terrestrial plants, Chlorophyceae and Rhodophyceae, suggests a higher increase of accessory pigment proportions through changes in the accessory pigments/Chl a ratio [41-43 ]. As it stimulates the synthesis of the most efficient pigments, this strategy results in an energy saving economy for plants. The second hypothesis proposes an increase of all of the pigments, and it has been observed in diatoms and Phaeophyceae [44], some Cyanobacteria and in a Rhodophyta, Bostrychia binderii [45]. This strategy implies a higher energy consumption. In the case of G. tenuistipitata, the concentration of all pigments increased when light was lowered and vice versa. The accessory pigments ( R P E + R P C ) / C h l a ratio remained around 3.8-4.7 in the first two days and then started to increase. The acclimative strategy of G. tenuistipitata is probably the second one described above in a short period of time, with an increase of all the pigments. However, when algae were kept for 10 days at low irradiance this ratio increased, indicating that the phycobiliproteins were the last pigments to respond to a decrease of irradiance. Zeaxanthin could be an exception to this behaviour due to the possible presence of two pools of this xanthophyll with different acclimation response to changes in the PFD. Acknowledgements This work was supported by project AMB-96-0782 of the CICYT. E.C. was supported by a fellowship from the Spanish Minister of Education and Culture. References [ 1 ] B. 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