Masterson went on to become principal soprano with English National Opera, from 1971, singing a wide range of roles from Mozart to Wagner and Rossini to Puccini. Her successes there included Adèle in Rossini's Le comte Ory, Micaëla in Carmen, Violetta in La traviata and the title role in Massenet's Manon ("exquisitely sung and acted"). Her many other roles there included Woglinde and the Woodbird in the Ring and Sophie and the Marschallin in Der Rosenkavalier. She made her Royal Opera House, Covent Garden debut in 1974 and her French debut at Toulouse in 1975 as Manon. For three seasons, beginning in 1975, at the Aix-en-Provence Festival, she sang a variety of roles, including "a memorable Matilde in Elisabetta, regina d'Inghilterra". Other early roles included Mimì in La bohème and Pamina in The Magic Flute. She also sang in Strasbourg (Pamina), Rouen (Countess, Marriage of Figaro), and returned to Toulouse (Violetta).
There followed starring roles, over a career lasting more than 30 years, in major opera houses around the world. Her repertory extended from the earliest operas to late 20th century works. At Covent Garden she created the role of May in Hans Werner Henze's 1976 premiere of We Come to the River, and sang The Anne who Steals in Aulis Sallinen's 1984 opera The King Goes Forth to France, at the UK premiere on 1 April 1987. Of her 1983 Madame Lidoine in Dialogues des Carmélites, The Times wrote that Masterson "makes a sound so beautiful one wishes it could go on for ever. ... Life offers few pleasures like that of hearing Felicity Lott and Valerie Masterson singing on the same stage".
She made her debut at the Paris Opera in 1978, singing Drusilla in Monteverdi's 1642 work, The Coronation of Poppea. Soon afterwards, she sang Constanza in The Seraglio and Gilda in Rigoletto, and she continued to have success in Mozart roles, including in Così fan tutte, Don Giovanni and Idomeneo She sang both Susanna and the Countess in The Marriage of Figaro, appearing at the Prague National Theatre in 1993 as the Countess. She performed for two seasons at Geneva, as Gilda in 1981 and Mireille later that year. Masterson (singing Gilda) was a member of the English National Opera company that toured five cities in the U.S. in May and June 1984. She also sang roles in The Merry Widow and Lucia di Lammermoor, among others.
Masterson played a significant part in the reintroduction of Handel's operas to the mainstream repertoire. Her purity of line and facility for ornamentation, coupled with excellent diction, helped to bring to life his works which, as recently as the 1960s, were considered unperformable. In 1983, Masterson won a Laurence Olivier Award for her performance in the title role of Semele at Covent Garden. Her other Handel roles included Romilda in Xerxes for ENO, Cleopatra in Giulio Cesare opposite Janet Baker for ENO and later for Houston Grand Opera and San Francisco Opera, Berenice in Scipio for the Handel Opera Society at Sadler's Wells, and Morgana in Alcina at Aix en Provence. On the concert platform she sang the Queen of Sheba in Solomon.
Some of her greatest successes were in the French repertoire. Of her 1974 Manon for ENO, The Times commented, "The Coliseum has found a worthy successor to Elizabeth Harwood in the delectable form of Valerie Masterson, who has here her greatest success to date with the company. She looks at once charming, fragile and seductive, and she sings with light insouciance and easy forward tone." Her Marguerite in Gounod's Faust in Paris and London drew warm notices: "The jewel song has the girlish delight that Gounod wanted (but does not always get) delivered in the easy coloratura Miss Masterson first displayed in The Pirates of Penzance." She sang Juliet, in Romeo and Juliet, in London and internationally, Leila in The Pearl Fishers, and the title role in Louise.
As a home-grown British soprano with a charming personality and attractive appearance, Masterson became popular with wider British audiences through frequent contributions to the popular radio series Friday Night is Music Night and the TV programme The Good Old Days. She also participated in television broadcasts of several Gilbert and Sullivan operas and live relays from English National Opera.
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