在1908年夏季,勋伯格的妻子玛蒂尔德离开他数月,与一位年轻的奥地利画家里夏德·格斯特尔(英语:Richard Gerstl)(后来在玛蒂尔德回到婚姻后于同年11月自杀)发生了关系。这一时期标志着勋伯格作品的明显变化。在妻子离开期间,他创作了《你靠在一棵银柳树上》(德语:Du lehnest wider eine Silberweide),这是他改编自德国神秘主义诗人施特凡·格奥尔格同名诗集的套曲《悬园之书(英语:The Book of the Hanging Gardens)》(德语:Das Buch der hängenden Gärten,作品15)中的第13首。这是他的第一首完全没有调参照的作品。[10]
第一次世界大战给他的发展带来了危机。当他42岁时,兵役打乱了他的生活。他无法持续、不受打扰地工作,结果留下了许多未完成的作品和未发展的“开端”。有一次,一位上级军官问他是否“就是臭名昭著的勋伯格”,勋伯格回答说:“报告,先生,是的。没有人想要成为他,有人必须成为他,所以我成了他。”[12]据诺曼·莱布雷希特说,这是指勋伯格作为“不和谐的解放(英语:Emancipation of the dissonance)者”的明显“命运”。[13]
当代作曲家与公众之间关系的恶化导致他在1918年在维也纳成立了私人音乐演出协会(德语:Verein für musikalische Privataufführungen)。他试图提供一个论坛,以便现代音乐作品能够经过精心准备和排练,并在受到时尚和商业压力影响的条件下仍得到适当的演出。从成立到1921年因经济原因结束为止,该协会向付费会员呈现了353场演出,有时每周一场。在最初的一年半中,勋伯格没有让自己的任何作品被演出。[15]协会音乐会的听众而是听到了斯克里亚宾、德彪西、马勒、韦伯恩、贝尔格、雷格等20世纪音乐早期的重要人物的复杂当代作品。[16]
在这一最后时期,他创作了几部重要的作品,包括小提琴协奏曲(作品36号,1934/36年)、为合唱和管弦乐团而作的《誓约》(Kol Nidre,作品39号,1938年)、《拿破仑·波拿巴颂》(Ode to Napoleon Buonaparte,作品41号,1942年)、钢琴协奏曲(英语:Piano Concerto (Schoenberg))(作品42号,1942年),以及献给大屠杀受害者的纪念作品《华沙幸存者(英语:A Survivor from Warsaw)》(作品46号,1947年)。他未能完成自己的歌剧《摩西与亚伦》(1932/33年),该作品是最早完全采用十二音技法创作的歌剧之一。除了十二音音乐,勋伯格在最后一个时期还回归了调性,创作了G大调弦乐组曲(1935年)、降E小调第2号室内交响曲(英语:Chamber Symphony No. 2 (Schoenberg))(作品38号,始于1906年,于1939年完成)、D小调宣叙调变奏曲(作品40号,1941年)。在这个时期,他的著名学生包括约翰·凯奇和卢·哈里森。
在1920年代初,勋伯格致力于发展一种能够使音乐织体更简单、更清晰的秩序方式。这导致了“以只与彼此相关的十二个音符进行作曲的方法”[48],其中八度音阶内的十二个音高(在作曲中并未实现)被视为相等,没有任何一个音符或音调被赋予古典和声中所占据的重要性。他认为这一理论的重要性等同于物理中阿尔伯特·爱因斯坦的相对论的地位。勋伯格在与朋友约瑟夫·鲁费尔(英语:Josef Rufer)散步时以他典型的方式宣布了这一发现,当时他说:“我已经做出了一个发现,它将确保德国音乐在未来一百年中仍占主导地位。”[49]这个时期的作品包括《为乐团而作的变奏曲》(作品31号,1928年);伴奏音乐《电影场景配乐(英语:Begleitungsmusik zu einer Lichtspielscene)》(作品34,1930年);《钢琴作品》(作品Op. 33a/b号,1931年)以及钢琴协奏曲(作品42号,1942年)。人们普遍认为勋伯格作曲方法严谨,但他对这种技巧的使用因每个独立作品的要求而各不相同。因此,他未完成的歌剧《摩西与亚伦》的结构与他的《为小提琴与钢琴而作的幻想曲》(作品47号,1949年)不同。
“《政治、宗教和文化利益周刊》(德语:Wochenschrift für politische, religiöse und Cultur-Interessen)刊登了通告《来自布拉格的保琳·纳霍德小姐与来自普雷斯堡的塞缪尔·勋伯格的婚礼》。这些信息与宗教社区发布的公告不符:1872年3月17日,12时30分,塞缪尔·勋伯格,来自塞切尼的商人,亚伯拉罕先生和特丽西娅女士的儿子,出生于1838年9月15日,住址为塔博尔街4号;保琳·纳霍德,来自普雷斯堡,约瑟夫先生和卡罗琳娜女士的女儿,出生于1843年3月8日,住址为塔博尔街4号。宣布姻缘并代表出席的是普雷斯堡的代表,日期是1872年3月2日。”
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