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Cardamom (small) - Production, Quality standards and grade specifications

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Cardamom (small) - Production, Quality standards and grade specifications


Cardamom (small)




1     Introduction Small  cardamom,  popularly  known  as  ‘Queen  of  Spices’,  is  the  dried  fruit  of  the  tall perennial  herbaceous  plant,  Elettaria  cardamomum  Maton,  belonging  to  the  family Zingiberaceae. It is a shade loving plant cultivated at an altitude of 600 to 1200 m above MSL with an annual rainfall of 1500 to 4000 mm and a temperature range of 10 to 35sC. Until recently India was the main producer and exporter of cardamom. Of late Guatemala has emerged as a keen competitor to Indian cardamom in the international spice market. Tanzania, Sri Lanka, El Salvador, Vietnam, Laos, Cambodia and Papua New Guinea are the other cardamom growing countries. In India, cardamom is cultivated in the southern states of Kerala, Karnataka and Tamil Nadu. Kerala accounts for 60% of the cultivation and  production  followed  by  Karnataka  30%  and  Tamil  Nadu  10%.  The  physical  and chemical characteristerics of cardamom from different growing regions in India is shown in Table 1.

Cardamom oil is used in food, perfumery and liquor and pharmaceutical industries as  a  flavour  and  a  carminative.  Its  use  in  the  food  industry  is  in  flavouring  pickles, meat and canned soups. However, the oil is reported to develop some off flavour in a few days when it contacts with air; its use is therefore restricted to fresh meat products and  foods  with  short  shelf-life.  Increasing  use  of  cardamom   oil  is  reported  in compounded  flavours  for  baked  goods,  sauces  and  condiments.  Cardamom  oil  is reported  to  be  gaining  increasing  use  in  perfumery,  with  a  trend  to  spicy  tones modifying  the  dominant  lavender  group  perfumes  for  women  (ITC,  Markets  for Essential Oils and Oleoresins 1974).

Cardamom is used as an adjuvant to carminative drugs. It is officially recognised in British  and  US  pharmacopoeias  and  used  as  an  aromatic  stimulant,  carminative  and flavouring  agent.  It  can  be  used  to  ease  cigarette  addiction.  Eating  a  few  seeds  of cardamom  can  safely  be  recommended  to  initially  minimise  the  number  of  cigarettes being  smoked,  and  slowly  the  smoker  may  give  up  the  chronic  addiction  to  chain smoking.


Table 1    Composition of cardamom

Region of   Weight Husk      Seed       Volatile   NVEE*   Starch          Fibre  Protein growth of 100  (%)      (%)      oil (%)            (%)      (%)        crude     (N   6.25)

capsules                                                                (%)      (%)

(g)

Karnataka

Mudigere   23–24  25.5–28.0   72.0–74.5   8.6–8.9    2.0–3.6    47.0–48.0   6.9–6.8    8.8–11.3

Coorg         23–25  26.0–27.0   73.0–74.0   1–4    2.2–3.1    47.7–48.0   6.7–2.7    10.5

Kerala

Wynard      20–22  28.0–38.0   62.0–72.0   7.5–10.0  2.2–2.4    31–43.7   8.4–3    7–14.0

Alleppey     23        27.7       72.3       4–6    2.2         37.8                

green

Tamil Nadu

Yercaud     23–26  27.0       73.0       4–6    2.4         45.5       7.0       8

Nelliampathy  12–18                         26.0–31.0   74.0          8.5–10.5  2.5–3.5    43.0–46.0   5–12.8  10.7–11.5

* NVEE non-volatile ether extracts.

Sources:   Kasturi and Iyer (1955), Krishnamurthy (1964) and Natarajan et al. (1968).

2     Description

Cardamom is indigenous to the evergreen rainforests of western ghats of Southern India from where it spread to other tropical countries such as Sri Lanka, Tanzania and a few Central  American  countries.  Presently it  is being cultivated in countries  lying  between

20s latitude north and south. Cardamom was an article of Greek trade during the fourth century BC. It was listed among the Indian spices liable to duty at Alexandria in AD  176

(Rosengarten 1969).

E.  Cardamomum  exhibits  considerable  variation  under  cultivation  and  the  naming  of commercial types after the places of production has led to confusion regarding the identity of the varieties. Two varieties based on the size of the fruits are recognized. They are : (1) E.cardamomum var. Major Thw. comprising the ‘wild’ indigenous cardamom of Ceylon or Greater oblong cardamom or long cardamom and (2) E.cardamomum var. minor comprising all the cultivated races, particularly those included under the names Malabar and Mysore cardamoms. Var. major is the more primitive variety from which the cultivated var. minor is derived. All the varieties and races are interfertile and the observed variations are probably due  to  natural  crossing.  The  genus  belongs  to  the  natural  order  Scitaminae,  family Zingiberaceae under monocotyledons with diploid chromosome number, 2n = 48.

2     Production

2.1     Harvesting

The  peak  period  of  harvest  is  October–November.  The  average  yield  of  cardamom  is around 150 kg (dry)/ha; however, record yield of 695 kg/ha (average of 9 crop seasons) was  obtained  by  adopting  high  production  technology  directly  in  farmers plantations

(Korikanthimath  1995).  Just  ripened  fruits  or  physiologically  ripened  are  generally harvested.   More   splitting   of   capsules   was   observed   in   over-matured   capsules


(Korikanthimath and Naidu 1986). Percentage of dry recovery was highest (29%) in the fully ripened capsules followed by the one harvested at physiological maturity (24%) and in immature stage (14%). Capsules may be washed in water to remove the adhering soil and a treatment with 2% washing soda (alkali) for 10 minutes enables  retention  of the green colour and prevents growth of mould.

3.2     Curing

In curing, moisture  of green cardamom  is reduced from 80% to 12% (wet basis) at an optimum temperature (50s) so as to retain its green colour to the maximum extent.

   Natural (sun) drying. This requires 5–6 days and the green colour is bleached by this method.

   Electrical drier. Fifty kg capsules can be dried in 10–12 hrs at 45–50sC retaining the green colour.

   Flue  pipe  curing. This is  the  convenient  method  of  curing  from  which  high-quality green cardamom  can be obtained. The structure consists of walls made of bricks or stones and tiled roof with ceiling. A pipe made of iron or zinc sheet starting from the furnace passes through the chamber and opens outside the roof. The heated air current generated in the furnace passes through the pipe and increases the temperature of the room.  The  fans  located  either  sides  of  the  wall  uniformly  spread  the  temperature. Inside the room the cardamom to be dried is kept in wooden/aluminium trays arranged in racks. The fire in the furnace is adjusted to maintain the temperature between 45–

50sC. Drying takes about 18 to 22 hours (Korikanthimath 1993).

3.3     Bleached cardamom

Bleached  cardamom  is  creamy  white  or  golden  yellow  in  colour.  It  can  be  done  with either  the  dried  capsule  or  freshly  harvested  capsules.  It  is  prepared  using  sulphur dioxide,  potassium metabisulphite  (25% containing  1% HCl for 30 min) and hydrogen peroxide (4–6% at pH 4.0). However bleached cardamom tends to lose more volatile oil.

3.4     Ground cardamom

A large portion of the cardamom imported into western countries is to meet industrial and institutional  requirements  for  bulk  supply  of  ground  cardamom  (Survey  of  the  World Market, 1977).

Proper maturity reflected by deep brown, shining seeds with satisfactory weight per litre  specifications  and  good  characteristic  aroma  are  the  factors  necessary  for  making good  quality  ground  cardamom.  In  cardamom,  the  presence  of  the  oil  cells  near  the surface  which  contains  aroma-significant  components  like  1,8-cineole  poses  special problems due to the high temperatures produced in attrition and grinding. To overcome the loss of volatiles, prechilling and reduced temperature grinding are used (Anon. 1975). A new innovation for idealized grinding of spices is freeze-grinding (   70sC) which has many  advantages;  increased  retention  of  volatiles,  minimizing  oxidation  of  volatiles, increased  throughput  and  improved  functional  properties  of  dispersability  of  the  fine ground material in food preparation (Russo 1976).



Ground spice deteriorates in its aroma quality both by rapid loss of volatile and by the action of oxygen in the head space on the terpenic and lipid components of the spice. This


loss  could  be  controlled  by  careful  selection  of  packaging  materials.  Gerhardt  (1972) found that of the different packaging material studied, lacquered cans, PVDC and HDPE gave the smallest loss of ethereal oils in powdered cardamom. Koller (1976) found that among   several   factors   influencing   flavour   quality   of   vacuum-packaged   ground cardamom,  temperature  not  exceeding  +5sC  was  the  most  important.  Cardamom  in powder   form   could   be   stored   vacuum-packed   in   laminater   such   as   polyamide/ polyethylene or cellophane or lacquered can for 12 months at                                                       18sC.

3.5     Cardamom volatile oil The most functionally important constituent of cardamom is the volatile oil. The volatile oil content of seeds varies from 6.6–10.6% for the two types of cardamom (cv. Mysore and   Malabar)   grown   in   India   (Krishnamurthy   1964;   Krishnamurthy   et   al.   1967; Korikanthimath et al. 1999). In immature capsules the volatile oil content is low, in the order of 4–5%. The husk is reported to yield 0.2% volatile oil, having properties similar to those of seed oil (Rao et al. 1925). Yields of the volatile oil varied over a wide range: for seeds from 3.4 to 8.6% and for dried capsules from 5.2 to 11.3%.

Many  developing  countries  have  been  producing  different  aromatic  volatile  oils  by steam  distillation  over  a  long  period.  Among  the  different  distillation  methods,  steam distillation  is  the  preferred  method.  Esters  have  been  known  to  be  important  for cardamom  aroma.  Other  important  control  factors  for  obtaining  uniform  and  typical aroma  quality  of  the  oil  are  the  rate  and  time  of  distillation.  Use  of  top  grades  of cardamom for distillation of oil is not economical. Lower grades which are good from the point  of  view  of  flavour,  but  do  not  command  high  prices  as  dry  capsules  because  of defects in appearance, are generally used. The less mature, pale brown seeds contain less oil and flavour quality is also different.

The specifications of the Essential Oils Association (EOA), US, which are generally accepted by all countries are given in Table 2.

Nambudiri  et  al.  (1968)  described  a  stainless  steel  still,  consisting  of  a  material holding  cage,  condenser  and  receiver  for  steam  distillators  and  the  conditions  of distillation for obtaining acceptable quality oil. Selected material from the lower grades containing seeds of good maturity are first dehusked by shear in a disk mill with wide distances between disks and seeds separated by vibrating sieves. The seeds are again put through the same mill, but closing the distance between the disks to crush the seeds into a coarse powder. The essential oil glands are in a single layer below the epidermal  layer and  fine  milling  will  result  in  loss  of  volatile  oil.  Freshly  powdered  coarse  grains  of cardamom are uniformly and loosely packed into the holding chamber with a perforated bottom. When the cover of the distillation vessel is fitted securely and connected to the tabular  condenser,  steam  at  low  pressure  is  let  in  through  a  perforated  manifold.  For efficient  distillation,  the  design  of  the  retort  and  packing  of  the  powdered  cardamom should ensure that the steam passes through the bed uniformly without passing the cage or channelling. Other important controls are the rate and total time of distillation. It was recommended that the distillation be continued for two to three hours.

The large volume of condensate was collected in a cylindrical oil trap which siphoned off the excess water continuously, which if allowed to accumulate, could result in loss of oil by saturation and also cause compositional variation due to differential dissolution of the components. It was found that it is better to keep the condensate warm to get a better separation  of  volatile  oil.  The  oil  floating  at  the  top  was  collected  by  lapping  through another conical vessel which functioned as a second separator of any residual moisture.


Table 2    Specifications for cardamom volatile oil

Definition                Volatile oil distilled from the seeds E.cardamomum Maton

Source                     Family Zingiberaceace

Cardamom grown in South India, Ceylon, Guatemala, Indonesia, Thailand and South China.

Physical and chemical constants

Appearance:            Colourless to very pale yellow liquid.

Odour and taste:     Aromatic, penetrating, somewhat camphoraceous odour of cardamom:

persistently pungent, strongly aromatic taste. Specific gravity:   0.917 to 0.947 at 25oC

Optical rotation:      + 22o  to + 44o

Refractive index:     1.463 to 1.466 at 20oC

Descriptive characteristics

Solubility

70% alcohol: in five volumes: occasional opalescence

Benzylalcohol: in all proportions Deithyl phthalate: in all proportions Fixed oil: in all proportions Glycerine: insoluble

Mineral oil: soluble with opalescence

Propylene glycol: insoluble

Stability: unstable in presence of strong alkali and strong acids

Containers and storage

Glass, aluminium or suitably lined containers.

Aluminium cans were fitted to the top with the oil to avoid head space, closed tightly and stored in cold chambers.

4     Chemical structure

The early work of several authors, summarized by Guenther (1975), shows the presence of 1,8-cineole, d-   -terphenol, terpinyl acetate, limonene, sabinene and borneol. The first detailed  analysis of the volatile oil of cardamom was reported by Nigam et al. (1965). They used gas chromatography under isothermal conditions and analyzed both the total oil and fractions obtained by fractional distillation and alumina column chromatography. They  confirmed  and  quantified  all  the  hydrocarbon  and  oxygenated  compounds.  1,8- cineole  and      -terpinyl  acetate are  the  major  components  in the  cardamom  volatile  oil. Besides  the  usual  terpene  hydrocarbon  and  alcohols  as  minor  compounds  and  the dominance of 1,8-cineole and    -terpinyl acetate, it is significant that methyl eugenol also has  been  identified  (Lawrence  1979).  The  basic  cardamom  aroma  produced  by  a combination   of   the   major   components,                                 -terpinyl   acetate   and   1,8-cineole.   The percentages  of  the  main  components  given  by  Lawrence  (1979)  are  as  follows:        - pinene  (1.5%),         -pinene  (0.2%),  sabinene  (2.8%),  myrcene  (1.6%),                 -phellandrene

(0.2%),  limonene  (11.6%),  1,8-cineole  (36.3%),                                        -terpinene  (0.7%),  p-cymene  (0.1%), terpinolene  (0.5%),  linalool  (3.0%),  linalyl  acetate  (2.5%),  terpinen-4-01  (0.9%),        -


terpineol  (2.6%),      -terpinyl  acetate  (31.3%),  citronellol  (0.3%),  nerd  (0.5%),  geraniol

(0.5%), methyl eugenol (0.2%), trans-nerolidol (2.7%). When  the  spice  is  chewed,  it  does  have  a  slight  astringent  and  pungent  taste.  The astringent sensation could arise from intense release of many components of the volatile oil when seeds are chewed and or from phenolics that are usually present in seeds. Pungency stimuli have been identified in other spices belonging to the family Zingiberaceae to which cardamom belongs, e.g. gingerols and shogaols in ginger and also the saturated compound

(6)-paradol from the seeds of the related spices, the Aframomum meleguta (Connell 1970). The  most  significant  component  of  cardamom,  as  spice,  is  the  volatile  oil  with  its characteristic  aroma,  described  generally  as  comphory,  sweet,  aromatic  spicy.  The cardamom oil has few mono- or sesquiterpenic hydrocarbons and is predominantly made up of oxygenated compounds, all of which are potential aroma compounds. While many of the identified compounds alcohols, esters and aldehydes are commonly found in many spice oils (or even volatiles of many different foods), the dominance of the ether,



1,8-cineole and the esters,    -terpinyl  and linalyl  acetates  in the composition, make the cardamom volatiles a unique combination. The aroma differences in different sources of cardamom are attributed to the proportion of the esters and 1,8-cineole (Lewis et al. 1966; Salzer 1975; Wijesekera and Jayawardena 1973; Korikanthimath et al. 1997).

Volatile  oil  from  cardamom  (E.cardamomum Maton  var. Minisula  Barhill) contains few hydrocarbons and large amounts of 1,8-cineole and                          -cineole and         -terpinyl acetate, while   that   from   E.   cardamomum   Maton   var,   major   Thewaites   (the   Ceylon   wild cardamom)  is  high  in  monoterpenes  and  very  poor  in  the  above  two  oxygenated compounds.  The  oils  from  the  Ammomum  species  are  all  much  higher  in  1,8-cineole, around  60  to  75%,  and  some  have  relatively  large  amounts  of  comphor  and  borneol. Thus,   a   complete   dominance   of   1,8-cineole,   camphor,   or   borneol   among   the oxygenerated compounds could be identified with the comphory smell.

The flavour characteristics of important volatile components in cardamom are listed in

Table 3, and the structure of some of the important aroma compounds are shown in Fig.

1.

5     Quality standards and grade specifications

Dried cardamom require cleaning to remove all stalks and dried remains of floral parts. This should be done by rubbing dried cardamom over a coarse surface of wire-mesh or bamboo trays. This is best carried out while the cardamom is still hot.

Fig. 1    Structure of important aroma compounds.


Table 3    Flavour characteristics of important volatile components in cardamom

Components  Flavour                    Effect in           Use level         Range of description         flavour use                                      concentration

(%) in cardamom oil

Esters

-terpinyl       Mildly herbaceous,  To stretch        1–15 ppm        34.6–52.5

acetate           sweet spicy,             cardamom, variation in odour,     herbal spice, warm, mild spicy     imitation taste.      citrus and

cherry, peach flavours

Linalyl           Sweet, floral,           Fresh, sweet     2–15 ppm        0.7–6.3

acetate           fruity odour and      modifier in taste, poor tenacity,    perfume and but stronger than           berry flavours terpinyl acetate.

Ethers

1,8-cineole    Fresh, comphoraceous,                    Refreshing       1–15 ppm 23–51

cool odour and taste,   effect and

very diffusive and   lift; extensively poor tenacity.      used in perfume

and flavours

Alcohol          Floral, woody with  Light to heavy 2–10 ppm        1.4–4.5

Linalool         citrus note;               perfume;

creamy floral taste   peculiar pleasant at low levels.    taste effect at

low levels.

-terpineol     Delicately floral,      Citrus and        5–40 ppm        1.4–3.3

sweet, lilac-like       spice compositions

Others

Methyl eugenol    Musty tea-like,   Tenacious, dry,

mildly spicy,            herbaceous      5–15 ppm        1.3

warm, slightly          spicy effect earthy.

Descriptions based on Bernhard et al. (1971) and American Spice Trade Association.

With regard to the quality of the dried product, larger, round and uniform pods having a good  dark green colour always  fetch  the  highest  price.  The  small  type  of cardamom with  creeping  panicles  produces  round  fruits  of  uniform  size  and  shape,  giving  a  very attractive product. The largest type of bulk gives different kinds of fruits varying in shape and size, from round to longish fruits of nearly an inch in length. This results in a product of mixed quality.

The Government of India and the  Indian Standards Institution (ISI) have  prescribed fairly   well-defined   grades,   popularly   known   as   Agmark’   grades   and   Indian specifications or standards on the basis of important  quality factors like colour, weight per unit volume, size and percentage of ‘empties’, malformed, shrivelled and immature capsules (Tables 4 and 5).


Table 4    Agmark grade designations of ‘true small cardamom

Quality                                    Grade               Trade name

Alleppey Green cardamom      AGEB              Cardamom Extra Bold

AGB                Cardamom Bold AGS            Cardamom superior AGS 1                        Shipment Green 1

AGS 2             Shipment Green 2

AGL                Light

Coorg Green Cardamom         CGEB              Extra Bold

CGB                Bold

CG 1               Superior

CG 2               Coorg Green Motta Green

CG 3               Shipment

CG 4               Light

Bleached and/or half               BL 1               

bleached cardamom

BL 2                – BL 3          

Bleached white cardamom      BW 1               Mysore/Mangalore Bleachable

Cardamom clipped

BW 2              Unclipped

BW 3              Bulk

BW 4              Bulk cardamom unclipped

Mixed cardamom                    MEB                Mixed Extra Bold

MB                  Mixed Bold

MS                  Mixed superior

MS 1               Mixed shipment 1

MS 2               Mixed shipment 2

ML                  Mixed light

Cardamom seeds                     CS 1                Prime

CS 2                Shipment

CS 3                Brokens

Table 5    Specifications for cardamom seeds, India (Indian Standards Institution, New Delhi)

Grade           Trade           Extraneous   Light            Weight         General

name           matter           seeds            (G/l - min)   characteristics

CS-1            Prime           0.5               3.0               675              Decorticated dry seeds

CS-2            Shipment     1.0               5.0               660              of any variety of Elettaria

CS-3            Brokens       2.0                                                   cardamomum


National and international standards are becoming more and more similar because of close association between the producer and user countries. Specifications for cardamom include the following (Wellner 1972).

1.   Cardamom  in  capsule  form  should  be  dried,  nearly  ripe  fruits  of  E.cardamomum Maton. The capsule should be from light green to brown in colour; oblong, rounded or three-cornered in shape; and have a ribbed appearance.

2.   The aroma and taste of cardamom in capsules and seeds should be characteristic and fresh and free from foreign aroma and taste, including rancidity and mustiness.

3.   Cardamom capsules and seeds should be free from living insects and moulds. Marks on capsules due to thrips infestation should not be counted as insect infestation.

4.   Cardamom should be free from visible dirt or dust. Extraneous matter such as bits of calyx,  stalks  and  others  shall  not  be  more  than  5%  by  weight  in  cardamom  in capsules and 0.5 to 2% by weight in seeds.



5.   The proportions of empty or malformed capsules, from opening and examining 100

capsules taken from the sample, should not be more than 1 to 7% by count.

6.   The proportions of immature and shrivelled capsules should not be more than 2 to

7% (m/m).

7.   Capsules having black colour and those which are split open at the corners for more than half the length should not be found in the bold grades and not be more than 10 and 15% by count in the ‘shipment and ‘light grades.

8.   The  proportions  of  cardamom  seeds  which  are  light  brown,  broken  or  immature

(shrivelled), should not be more than 3 to 5% (m/m).

The importance attached to the different dimensions of quality varies with the primary raw material producer, the intermediary collector, the trader and exporter, the importer, the processor, the distributor and the final consumer. Product quality is generally related to safe moisture level and cleanliness. The content of substandard product and extraneous matter  is  important  to  the  producer  and  trader   appearance  and  colour  also  to  the exporter and importer. The extraction, volatile oil, and specific ingredients are valued by the processor; the interest is sensory quality and cost to the distributor and consumer.

5.1     Adulteration

Decorticated seeds can be adulterated with seeds from lower grades and also from large cardamom as they are of similar shape, size and colour. Pale brown coloured seeds would represent  immature  cardamom  which  are  low  in  volatiles  and  poor  in  quality  and intensity.  The  seeds  from  large  cardamom  have  lower  volatile  oil  content,  entirely different  composition  and  aroma.  Gross  adulteration  with  seeds  from  large  cardamom will show higher 1,8-cineole and higher terpene hydrocarbons, which are determinable by gas or thin-layer chromotography. However, examination of the surface of the seeds with a hand lens showed distinct differences: while the seed coat surface of true cardamom has clear furrows and ridges, the large cardamom has an almost smooth surface.

Adulteration of cardamom powder is possible with almost any material powdered to similar  size.  Cereal  and  pulse  flours  and  extracted  ginger  have  been  reported  as adulterants. These can be detected by microscopy by very different size and structure of the starch granules. Cardamom starch grains, unlike those of cereal  and other starches, are  very  small  (2  to  4 m).  Whole  cardamom  powder  can  be  distinguished  from  the cardamom seed powder by microscopy. The former can be recognized by the yellowish colour,   abundance   of   pitted   fibres,   spiral   cells   of   the   vascular   bundles,   empty


parenchymatous  cells  and  scattered  resin  cells  with  brownish  clumps  (Melchior  and

Kastner 1974).

6     References

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GERHARDT,  U.,  Changes  in  spice  constituents  due  to  the  influence  of  various  factors.

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KASTURI, T.R.  and IYER, B.H., Fixed oil from Elettaria cardamomum seeds, J. Indian Inst. Sci., 37A, 106, 1955.

KOLLER,   W.D.,   Die   Temperature,   ein   wesentlichen   Faktor   bei   der   Lagerung   von gemehlenen Naturgewurzen, Z. Lebensm. Unters. Forsch. 160(2), 143, 1976. KORIKANTHIMATH, V.S. and NAIDU, R., Influence of harvest on the recovery percentage of

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19(4), 1024–7, 1997.

KORIKANTHIMATH, V.S., RAVINDRA MULGE and JOHN ZACHARIAH, T., Variations in essential oil  constituents  in  high  yielding  selections  of  cardamom.  Journal  of  Plantation Crops, 27(3), 230–2, 199

KRISHNAMURTHY,  M.N.  PADMABAI,  R.   and  NATARAJAN,  C.P.,  Chemical  composition  of cardamom. J. Food Sci. Technol., 4, 170, 1967.

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NATARAJAN, C.P., KUPPUSWAMY, S.  and KRISHNAMURTHY, M.N.,  A study on the maturity, regional variations and retention of green colour of cardamom, J. Food Sci. Technol.,

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