在1908年夏季,荀伯克的妻子瑪蒂爾德離開他數月,與一位年輕的奧地利畫家里夏德·格斯特爾(英語:Richard Gerstl)(後來在瑪蒂爾德回到婚姻後於同年11月自殺)發生了關係。這一時期標誌着荀伯克作品的明顯變化。在妻子離開期間,他創作了《你靠在一棵銀柳樹上》(德語:Du lehnest wider eine Silberweide),這是他改編自德國神秘主義詩人施特凡·格奧爾格同名詩集的套曲《懸園之書(英語:The Book of the Hanging Gardens)》(德語:Das Buch der hängenden Gärten,作品15)中的第13首。這是他的第一首完全沒有調參照的作品。[10]
第一次世界大戰給他的發展帶來了危機。當他42歲時,兵役打亂了他的生活。他無法持續、不受打擾地工作,結果留下了許多未完成的作品和未發展的「開端」。有一次,一位上級軍官問他是否「就是臭名昭著的荀伯克」,荀伯克回答說:「報告,先生,是的。沒有人想要成為他,有人必須成為他,所以我成了他。」[12]據諾曼·萊布雷希特說,這是指荀伯克作為「不和諧的解放(英語:Emancipation of the dissonance)者」的明顯「命運」。[13]
當代作曲家與公眾之間關係的惡化導致他在1918年在維也納成立了私人音樂演出協會(德語:Verein für musikalische Privataufführungen)。他試圖提供一個論壇,以便現代音樂作品能夠經過精心準備和排練,並在受到時尚和商業壓力影響的條件下仍得到適當的演出。從成立到1921年因經濟原因結束為止,該協會向付費會員呈現了353場演出,有時每周一場。在最初的一年半中,荀伯克沒有讓自己的任何作品被演出。[15]協會音樂會的聽眾而是聽到了斯克里亞賓、德彪西、馬勒、魏本、貝爾格、雷格等20世紀音樂早期的重要人物的複雜當代作品。[16]
在這一最後時期,他創作了幾部重要的作品,包括小提琴協奏曲(作品36號,1934/36年)、為合唱和管弦樂團而作的《誓約》(Kol Nidre,作品39號,1938年)、《拿破崙·波拿巴頌》(Ode to Napoleon Buonaparte,作品41號,1942年)、鋼琴協奏曲(英語:Piano Concerto (Schoenberg))(作品42號,1942年),以及獻給大屠殺受害者的紀念作品《華沙倖存者(英語:A Survivor from Warsaw)》(作品46號,1947年)。他未能完成自己的歌劇《摩西與亞倫》(1932/33年),該作品是最早完全採用十二音技法創作的歌劇之一。除了十二音音樂,荀伯克在最後一個時期還回歸了調性,創作了G大調弦樂組曲(1935年)、降E小調第2號室內交響曲(英語:Chamber Symphony No. 2 (Schoenberg))(作品38號,始於1906年,於1939年完成)、D小調宣敘調變奏曲(作品40號,1941年)。在這個時期,他的著名學生包括約翰·凱奇和盧·哈里森。
在1920年代初,荀伯克致力於發展一種能夠使音樂織體更簡單、更清晰的秩序方式。這導致了「以只與彼此相關的十二個音符進行作曲的方法」[48],其中八度音階內的十二個音高(在作曲中並未實現)被視為相等,沒有任何一個音符或音調被賦予古典和聲中所佔據的重要性。他認為這一理論的重要性等同於物理中阿爾伯特·愛因斯坦的相對論的地位。荀伯克在與朋友約瑟夫·魯費爾(英語:Josef Rufer)散步時以他典型的方式宣佈了這一發現,當時他說:「我已經做出了一個發現,它將確保德國音樂在未來一百年中仍佔主導地位。」[49]這個時期的作品包括《為樂團而作的變奏曲》(作品31號,1928年);伴奏音樂《電影場景配樂(英語:Begleitungsmusik zu einer Lichtspielscene)》(作品34,1930年);《鋼琴作品》(作品Op. 33a/b號,1931年)以及鋼琴協奏曲(作品42號,1942年)。人們普遍認為荀伯克作曲方法嚴謹,但他對這種技巧的使用因每個獨立作品的要求而各不相同。因此,他未完成的歌劇《摩西與亞倫》的結構與他的《為小提琴與鋼琴而作的幻想曲》(作品47號,1949年)不同。
「《政治、宗教和文化利益周刊》(德語:Wochenschrift für politische, religiöse und Cultur-Interessen)刊登了通告《來自布拉格的保琳·納霍德小姐與來自普雷斯堡的塞繆爾·荀伯克的婚禮》。這些信息與宗教社區發佈的公告不符:1872年3月17日,12時30分,塞繆爾·荀伯克,來自塞切尼的商人,亞伯拉罕先生和特麗西婭女士的兒子,出生於1838年9月15日,住址為塔博爾街4號;保琳·納霍德,來自普雷斯堡,約瑟夫先生和卡羅琳娜女士的女兒,出生於1843年3月8日,住址為塔博爾街4號。宣佈姻緣並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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