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Diaries, 1901-1968; papers and photograph albums relating to the Boer War and photography in military reconnaissance, including an unpublished manuscript, 1897-1902, service in Northern Nigeria on the Anglo-French Boundary Commission, 1902-1904, West Africa, 1903, West Indies, 1902 and Ordnance Survey of Scotland, 1904-1909; papers relating to the introduction and use of chemical warfare during World War One, 1914-1918, and on the North West Frontier, India, 1919-1920 andphotographs taken on the Western Front, 1914-1915 and 1919; articles written as Director of Irish Propaganda during the Anglo-Irish War, 1921; papers concerning appointments as Colonel Commandant and Representative Colonel Commandant, 1937-1944; papers concerning writing and publication of 'Gas!' The story of the Special Brigade (Blackwoods, 1934) and Commonsense and ARP (C Arthur Pearson, 1939) and draft chapters and photographs concerning the unpublished manuscript 'Adventures of an Engineer Subaltern' dealing with military career, 1897-1903; personal correspondence and papers relating to memorial service, 1900-1981; glass and film negatives covering career, 1897-1920.

Papers, 1908-1974, including Wynne's letters home to his father from Germany, 1908-1911, including detailed descriptions of illegal duelling by students in Hannover, Germany and calling card of General Otto von Emmich, Commander, 10 Army Corps, Hannover, Germany, 1909-1915. Bound typescript account by Wynne, 29 Jul-4 Sep 1914, on his experiences in the BEF's (British Expeditionary Force's) retreat from Mons, Belgium, the Battle of Le Cateau, France, and capture by German forces during the Battle of Le Cateau, France, 26 Aug 1914, written as a POW in Germany, Sep-Oct 1914. Correspondence, press cutting, menus and Christmas cards relating to time as POW, Germany and Netherlands, 1914-1918, including letters written to parents from Portobello Barracks, Dublin, immediately before embarkation for France, Aug 1914; cutting from The Morning Post , 3 Sept 1914, listing Wynne as killed; letter home from POW camp, Magdeburg, Germany, 30 Dec 1914, referring to incorrect report of his death; menus, playing cards and Christmas cards with watercolours by Wynne and signatures of fellow POW's. Correspondence and papers relating to Wynne's work for the Historical Section, Cabinet Office, and to his publications, 1928-1958, including two letters from Maj Gen Sir Ernest (Dunlop) Swinton relating to German defence systems, 30 Sep 1939, and to Wynne's book, If Germany attacks. The battle in depth in the west (Faber and Faber, London, 1940), 2 Feb 1940; manuscript diary and typescript report by Wynne on an official visit to North Africa, 12 Apr-23 May 1943; letters to Wynne from Lt Gen Sir Kenneth Arthur Noel Anderson, General Officer Commanding 1 Army, North Africa, rebutting allegations reported to Wynne by troops of 8 Army of Anderson's poor handling of 1 Army in operations in North Africa, May 1943; three letters from Capt Basil Henry Liddell Hart, dated Jan-Jul 1958, relating to Wynne's article on the Schlieffen plan and The Schlieffen plan. Critique of a myth by Professor Gerhard Ritter (Oswald Wolff, London, 1958). Correspondence, 1939-1974, relating to Wynne's publications, including his book If Germany attacks. The battle in depth in the west (Faber and Faber, London, 1940). Also photograph of Wynne's father, General Sir Arthur Singleton Wynne, c.1914.